-js-^ u( \ 
 
 COO-1 264-2 
 
 CIVIL ENGINEERING STUDIES 
 
 SANITARY ENGINEERING SERIES NO. 25 
 
 A SURVEY OF STABLE AND RADIOACTIVE ZINC 
 AND COBALT IN THE COLUMBIA RIVER 
 
 LOAN COPY 
 
 By 
 ROBERT H. WATSON 
 
 Property of 
 
 COLLEGE OF ENGINEERING DOCUMENTS CENTER 
 
 UNIVERSITY OF ILLINOIS 
 
 157 GFUi >BTi£jy 
 
 1301 WES .."5ELD AVENUE 
 
 URBAi^A, ILLINOIS 31801 USA 
 
 Supported by 
 
 DIVISION OF BIOLOGY AND MEDICINE 
 
 U.S. ATOMIC ENERGY COMMISSION 
 
 RESEARCH CONTRACT AT(1 1-1 )-l 264 
 
 DEPARTMENT OF CIVIL ENGINEERING 
 
 UNIVERSITY OF ILLINOIS 
 
 URBANA, ILLINOIS 
 
 JANUARY, 1965 
 
A SURVEY OF STABLE AND RADIOACTIVE ZINC AND COBALT 
 
 IN THE 
 COLUMBIA RIVER 
 
 by 
 Robert Henry Watson 
 
 Supported by the 
 
 United States Atomic Energy Commission 
 
 Research Grant US-AT -11-1-1264 
 
 Department of Civil Engineering 
 The University of Illinois 
 Urbana, Illinois 
 
 January, 1965 
 
Digitized by the Internet Archive 
 in 2013 
 
 http://archive.org/details/surveyofstablera25wats 
 
ABSTRACT 
 
 Data accumulated during a comprehensive review of the literature 
 on the occurrence of stable and radioactive zinc and cobalt in samples from 
 the aquatic and terrestrial environments is presented. Zinc and cobalt 
 radionuclides found in natural waters result from nuclear weapons testing 
 and nuclear reactor activities and commonly become the major radionuclides 
 associated with aquatic plant and animal life inhabiting these waters,, 
 
 In natural waters, the literature indicates that a dynamic 
 equilibrium exists between zinc ions in solution and zinc ions adsorbed on 
 the surfaces of living aquatic plant life and inorganic bottom sediments. 
 The degree of adsorption is high and the rate, rapid, at pH's above neu- 
 trality, Desorption is complete at pH's below four. 
 
 Analytical techniques were developed to determine the concentra- 
 tions in environmental samples of both total and radioactive zinc and 
 cobalt, stressing simplicity of procedure and analytical equipment. In 
 each sample, the desorbable zinc and cobalt were isolated by anion exchange 
 chromatography, the total zinc and total cobalt concentrations determined 
 by colorimetric procedures, and the radioactive zinc and radioactive cobalt 
 activities determined by gamma scintillation counting. 
 
 Four samples of water, four samples of plankton and twenty-four 
 samples of bottom sediments were obtained on August 14- and 15, 1963, from 
 a one-hundred mile reach of the Columbia River between just upstream of the 
 Hanford reactors and just downstream of McNary dam. The bottom sediment 
 samples were collected along the shorelines of the river at a time when 
 the water surface was receding from a flood peak which had occurred six 
 weeks previously. 
 
The following table indicates the minimum, maximum and average 
 concentrations of total and radioactive zinc and cobalt found in the 
 Columbia River samples „ 
 
 CONCENTRATIONS OF TOTAL AND RADIOACTIVE ZINC 
 AND COBALT IN COLUMBIA RIVER SAMPLES* 
 AUGUST 14 AND 15, 1963 
 
 Analysis 
 
 ZINC 
 
 (ug/g) 
 
 COBALT 
 ( Mg'/g )" 
 
 Water 
 
 SajmoleJIype 
 
 Plankton"-""" 
 
 Bottom Sediments 5 ""' 
 
 Mm 
 
 .048 
 
 Max 
 120 
 
 Ave 
 072 
 
 Min 
 
 Max 
 
 1060 1960 1660 
 
 00005 .00014 .00010 
 
 1.2 
 
 3o5 
 
 2 5 
 
 ZINC 
 
 65 
 
 (pc/g) 0013 .0199 .0084 4830 8060 5940 
 (pc/in2)t 
 
 COBALT 60 
 
 (pc/g) oOOOO 0014 0OOO8 
 
 (pc/in2)t 
 
 63 
 
 30 
 
 Min 
 
 Max 
 
 Ave 
 
 5 
 
 187 
 
 71 
 
 o00 
 
 o87 
 
 o28 
 
 .00 
 
 230 
 
 52 
 
 .0 
 
 5510 
 
 1060 
 
 oOO 
 
 13o0 
 
 2.1 
 
 oO 
 
 313 
 
 46 
 
 *based on analyses of 3 water, 4 plankton and 24 bottom sediment samples 
 ** as dry weights 
 t in2 ground surface area 
 
 The radioactivity of the zinc fractions of all samples was caused 
 
 65 
 
 by Zinc and the radioactivity of the cobalt fractions of all samples was 
 caused by Cobalt . Zinc was a major radionuclide associated with plankton 
 and bottom sediment samples and Cobalt was a minor radionuclide associated 
 with these samples. No relation was found between the Zinc ' and Cobalt 
 activities of the bottom sediments of the Columbia River and the total zinc 
 and cobalt concentrations of these sediments Total zinc concentrations of 
 the sediments were highest above the reactor area, along the reactor shore, 
 and decreased with distance downstream. Total cobalt concentrations of the 
 
sediments generally decreased with distance downstream throughout the study 
 reach „ The major portion of the Zinc ' and Cobalt activities associated 
 with bottom sediments collected along the shorelines of the Columbia River 
 occurred in a 40 to 50 mile reach extending through the Hanford reactor 
 area and downstream, and concentrated along the reactor shore „ 
 
 Zinc ' and Cobalt , in their present concentrations and locations 
 in bottom sediments of the Columbia River, do not represent a significant 
 public health hazard „ Continuous monitoring at the water treatment plants 
 of public water supplies taken from the Columbia River is, however, con- 
 sidered to be necessary as a safeguard against the consumption of water 
 containing excessive concentrations of radioactivity „ 
 
Ill 
 
 ACKNOWLEDGEMENTS 
 
 This report is submitted as a thesis in partial fulfillment of the 
 requirements for the degree of Master of Science in Sanitary Engineering 
 under the direction of Dr John T O'Connor, Associate Professor of Sanitary 
 Engineering, University of Illinois „ 
 
 The research was supported by Research Grant US-AT-11-1-1264, from 
 the Division of Biology and Medicine, United States Atomic Energy Commission, 
 and carried out at the Sanitary Engineering Laboratory of the University of 
 Illinoiso 
 
 The samples analyzed in this study were obtained by Dr„ Benjamin 
 B Ewing, Professor of Sanitary Engineering, University of Illinois, with 
 the permission and active support of Dr„ Richard F Foster, Manager, Environ- 
 mental Studies and Evaluation, Radiation Protection Operation, Hanford Atomic 
 Products Operation, General Electric Company, Richland, Washington „ 
 
 The author wishes to take this opportunity to thank Dr Ewing for 
 obtaining the samples on which the results of this study are based, and for 
 his constructive criticism during the course of the work, and Dr Foster for 
 his help in obtaining a large proportion of the reference data compiled in 
 this thesiso 
 
 Acknowledgements are gratefully extended to Sambhunath Ghosh, 
 Tsohsiong Fann and Emil Frein, for their help during various phases of the 
 experimental work, and to Josephine Lee and other members of the Sanitary 
 Engineering Laboratory who helped the author in connection with this research. 
 
 Above all, the author extends his deep gratitude to Dr John T 
 O'Connor for his enthusiastic assistance in performing this work, and for 
 the many hours spent in reviewing and guiding both the experimental work and 
 the preparation of this thesis „ 
 
IV 
 
 TABLE OF CONTENTS 
 
 Page 
 
 ACKNOWLEDGEMENTS iii 
 
 LIST OF TABLES viii 
 
 LIST OF FIGURES x 
 
 I, INTRODUCTION 1 
 
 THE HANFORD REACTORS AND THE COLUMBIA RIVER 1 
 
 ENVIRONMENTAL RADIATION EXPOSURE AND MONITORING IN THE 
 
 HANFORD AREA 4 
 
 ZINC 65 AND COBALT 50 7 
 
 OBJECTIVES OF THE STUDY 9 
 
 II o LITERATURE REVIEW 12 
 
 COLUMBIA RIVER AREA 13 
 
 Additional Data - Qualitative and Quantitative 14 
 
 THAMES RIVER, CONNECTICUT, AREA 15 
 
 SOUTH-WEST PACIFIC AREA 16 
 
 Additional Data - Qualitative and Quantitative 16 
 
 OTHER AREAS 18 
 
 Additional Data - Qualitative and Quantitative 18 
 
 III. A DISCUSSION OF ZINC 65 EQUILIBRIUM AND TRANSPORT IN 
 
 NATURAL WATERS 20 
 
 CHEMICAL FORCES 21 
 
 Solubility Limitations 21 
 
 Adsorption Phenomena 22 
 
 PHYSICAL FORCES 24 
 
 BIOLOGICAL FORCES 24 
 
 TRANSPORT OF ZINC 65 25 
 
TABLE OF CONTENTS (continued) 
 
 Page 
 
 65 
 
 FACTORS CAUSING THE RETURN OF ZINC TO SOLUTION 27 
 
 MATERIALS BALANCE 27 
 
 SUMMARY 28 
 
 IV o ANALYTICAL PROCEDURE 30 
 
 PHASE I 30 
 
 Water 30 
 
 Plankton 32 
 
 Bottom Sediments 33 
 
 PHASE II 34 
 
 PHASE III 35 
 
 Procedure for Separation and Isolation of Zinc and Cobalt 35 
 
 PHASE IV 35 
 
 ANALYSES FOR TOTAL ZINC AND FOR TOTAL COBALT 36 
 
 Analysis for Total Zinc 37 
 
 Analysis for Total Cobalt 38 
 
 V DISCUSSION OF ANALYTICAL PROCEDURE 39 
 
 PHASE I 39 
 
 Elution of Zinc and Cobalt from Dowex 50 Cation Exchange 
 
 Resin 39 
 
 Elution of Zinc and Cobalt from Plankton and Bottom 
 
 Sediment Samples 40 
 
 Counting for Total Gamma Activity 41 
 
 PHASE II 42 
 
 PHASE III 43 
 
 Separation and Isolation of Zinc and Cobalt by Anion 
 
 Exchange Chromatography 43 
 
VI 
 
 TABLE OF CONTENTS (continued) 
 
 Page 
 
 PHASE IV 51 
 
 Analysis for Total Zinc 51 
 
 Analysis for Total Cobalt 55 
 
 Determination of Radioactive Zinc and Radioactive Cobalt 56 
 
 Prevention of Contamination and Loss of Microgram 
 
 Quantities of Zinc and Cobalt 60 
 
 VI o SAMPLING SURVEY 62 
 
 WATER SAMPLES 62 
 
 PLANKTON SAMPLES 68 
 
 BOTTOM SEDIMENT SAMPLES 68 
 
 VII „ RESULTS OF ANALYSES 70 
 
 EXPLANATION OF CALCULATIONS FOR A TYPICAL SAMPLE: BOTTOM 
 
 SEDIMENT SAMPLE #13 77 
 
 Phase I 77 
 
 Phase II 77 
 
 Phase IV - Zinc and Zinc ' 79 
 
 Phase IV - Cobalt and Cobalt 81 
 
 RADIOACTIVITY RELATED TO SURFACE AREA 81 
 
 VIII o DISCUSSION OF RESULTS OF ANALYSES 83 
 
 QUALITATIVE PROOF OF ISOLATION OF ZINC 65 AND COBALT 60 83 
 
 PRECISION OF ANALYTICAL RESULTS 83 
 
 Zinc 83 
 
 Cobalt 83 
 
 „. 65 
 
 Zinc 85 
 
 fin 
 
 Cobalt 86 
 
 ACCURACY OF ANALYTICAL RESULTS 86 
 
TABLE OF CONTENTS (continued) 
 
 VII 
 
 Page 
 
 TOTAL GAMMA ACTIVITY 88 
 
 COMPARISON OF TOTAL GAMMA ACTIVITY WITH ZINC 65 AND COBALT 60 
 
 ACTIVITY 89 
 
 COMPARISON OF TOTAL ZINC AND TOTAL COBALT WITH ZINC 65 AND 
 
 COBALT 60 92 
 
 EFFECT OF LOCATION OF SAMPLES 93 
 
 Location of Bottom Sediment Samples Relative to the 
 
 Water Surface Level of the Columbia River 94 
 
 Location of Bottom Sediment Samples Relative to the 
 
 Flow Velocity of the Columbia River 94 
 
 Total Gamma Activity 95 
 
 Zinc and Cobalt 96 
 
 Zinc 65 and Cobalt 60 99 
 
 COMPARISON OF RESULTS WITH DATA OBTAINED BY OTHERS 104 
 
 Water 104 
 
 Plankton 105 
 
 Bottom Sediments 105 
 
 CONCENTRATION RATIOS 108 
 
 SIGNIFICANCE OF ZINC 65 AND COBALT 60 CONCENTRATIONS 109 
 
 IXo CONCLUSIONS 111 
 
 REFERENCES 114 
 
 APPENDIX 117 
 
 REFERENCES FOR APPENDIX 135 
 
 ADDITIONAL REFERENCES FOR APPENDIX 142 
 
Vlll 
 
 LIST OF TABLES 
 
 Table Page 
 
 5.1 Radionuclides Present in Reactor Effluent as it Enters 
 
 the Columbia River 46 
 
 5.2 Naturally Occurring Radionuclides 47 
 
 5.3 Significant Radionuclides 48 
 
 5.4 Test Results Used for Establishing the Standard Curve for 
 
 Total Zinc Determination 54 
 
 5.5 Range in Test Results Used for Establishing the Standard 
 
 Curve for Total Zinc Determination 54 
 
 5.6 Test Results Used for Establishing the Standard Curve 
 
 for Total Cobalt Determination 57 
 
 5.7 Range in Test Results Used for Establishing the Standard 
 
 Curve for Total Cobalt Determination 57 
 
 5.8 Establishment of Counting Efficiency for Zinc ' and Cobalt 59 
 
 6.1 Water Samples, Columbia River - August 14 & 15, 1963 64 
 
 6.2 Plankton Samples, Columbia River - August 14 & 15, 1963 64 
 
 6.3 Bottom Sediment Samples, Columbia River - August 14 & 15, 1963 65 
 
 7.1 Total Gamma Activity of Columbia River Samples 71 
 
 7.2 Total Zinc and Total Cobalt of Columbia River Samples 72 
 
 7.3 Radioactive Zinc and Radioactive Cobalt of Columbia River 
 Samples 73 
 
 7.4 Radioactivity of Columbia River Bottom Sediment Samples 
 
 Related to Surface Area 74 
 
 7.5 Summary of Results of Analyses of Columbia River Samples 75 
 
 8.1 Precision of Analytical Results 85 
 
 8.2 Concentration Ratios of Columbia River Plankton and Bottom 
 Sediment Samples to Columbia River Water 109 
 
 9.1 Concentrations of Total and Radioactive Zinc and Cobalt in 
 
 Columbia River Samples, August 14 and 15, 1963 112 
 
IX 
 
 LIST OF TABLES (continued) 
 
 Table Page 
 
 A-l Stable and Radioactive Zinc and Cobalt in Environmental 
 
 Samples Taken from the Columbia River Area 118 
 
 A-2 Columbia River Area - Data from Additional References 121 
 
 A-3 Zinc and Zinc ' in Environmental Samples Taken from the 
 
 Thames River, Connecticut, Area 125 
 
 A-4 Stable and Radioactive Zinc and Cobalt in Environmental 
 Samples Taken from the South-West Pacific Area, 1956-57, 
 Following the "Redwing" Shot Series 126 
 
 A-5 South-West Pacific Area - Data from Additional References 130 
 
 A-6 Stable and Radioactive Zinc and Cobalt in Environmental 
 Samples (Excluding the Columbia River, the South-West 
 Pacific and the Thames River, Connecticut, Areas) 131 
 
LIST OF FIGURES 
 
 Figure Page 
 
 101 Geographical Relationship of Hanford Works to Pacific 
 
 Northwest 2 
 
 1 2 Features of Hanford Project and Vicinity 3 
 
 65 
 
 1 3 Zinc in Columbia River Water at Pasco, Washington 5 
 
 4 1 Flow Diagram of Analytical Procedure 31 
 
 5 1 Adsorption Coefficients of the Elements on Dowex I Anion 
 
 Resin with Varying Concentrations of Hydrochloric Acid 49 
 
 6<,1 Location of Sampling Points 63 
 
 8 1 Comparison of Zinc ' and Cobalt Composite Samples with 
 Standards 84 
 
 8 2 Variation in Percent of Total Gamma Activity Eluted from 
 
 Bottom Sediments with Total Gamma Activity of Sample 91 
 
 65 
 8«3 Variation in Percent of Total Gamma Activity Due to Zinc 
 
 from Bottom Sediments with Total Gamma Activity 91 
 
 80*+ Variation of Total Zinc with Location of Bottom Sediments 97 
 
 80 5 Variation of Total Cobalt with Location of Bottom Sediments 98 
 
 806 Variation of Zinc ' with Location of Bottom Sediments - 
 
 Weight Basis, August 15, 1963 100 
 
 80 7 Variation of Zinc ' with Location of Bottom Sediments - 
 
 Surface Area Basis, August 15, 1963 101 
 
 8„8 Variation of Cobalt with Location of Bottom Sediments - 
 
 Weight Basis, August 15, 1963 102 
 
 80 9 Variation of Cobalt with Location of Bottom Sediments - 
 
 Surface Area Basis, August 15, 1963 103 
 
I„ INTRODUCTION 
 
 THE HANFORD REACTORS AND THE COLUMBIA RIVER 
 
 The Hanford Atomic Products Operation, or the Hanford Works, is 
 located in a United States Atomic Energy Commission reservation in the 
 southeastern section of the State of Washington, as shown in Figs, 1.1 and 
 l 2o The reservation includes an area of about five hundred square miles. 
 Plant operations commenced in 1944 and have expanded to the present complex 
 which includes eight production reactors , fuel fabrication plants , chemical 
 separation facilities and research and development laboratories The 
 installation is operated for the Atomic Energy Commission by the General 
 Electric Company The Columbia River flows through the reservation and 
 forms part of its eastern boundary , 
 
 The part of Washington in which Hanford Works is located is 
 semiarid, having an average annual rainfall of about eight inches, and thus 
 provides an excellent site for nuclear reactor operation,, The inclusion 
 of the Columbia River within the reservation is also advantageous, as it 
 has a minimum flow of about 50,000 cubic feet per second at Hanfordo This 
 considerable minimum flow provides both a continuous source of reactor 
 cooling water and also a means of disposing, by dilution, of large quanti- 
 ties of low-level radioactive wastes „ 
 
 Columbia River water has been used as a source of reactor cooling 
 water since the start of operations in 1944 „ Water is pumped from the 
 river and passes through a complete water treatment plant which includes 
 coagulation, sedimentation, filtration and chlorination Chromates are 
 added to the water to keep corrosion to a minimum The effluent from the 
 treatment plant Is maintained at less than o 01 units of turbidity „ The 
 cooling water passes once through a reactor and then into an open retention 
 
Fig. 1.1 
 
 GEOGRAPHICAL RELATIONSHIP OF 
 HANFORD WORKS TO PACIFIC NORTHWEST 
 
Fig. 1.2 
 
 FEATURES OF HANFORD PROJECT AND VICINITY 
 
4 
 tank where short-lived isotopes are allowed to decay before the water is 
 returned tc the Columbia River , 
 
 The Columbia River, as shown in Fig, 1,3, has a flow at Pasco, 
 Washington, ranging from 60,000 to more than 300,000 cubic feet per second „ 
 The flow at Hanford is slightly less, as the Yakima River joins the 
 Columbia between these two locations , The flow past Hanford is rapid. The 
 river water is of excellent quality, having a pH of between 7,5 and 9 o 
 with an average of 8 1, an alkalinity of between 43 and 170 mg/1 with an 
 average of 65 mg/1, and a very low turbidity. As the river passes Richland, 
 Washington, it enters the reservoir formed by McNary dam, and the current 
 velocity decreases. Sediments have been accumulating slowly in the impound- 
 ment since it was placed in operation in 1953, 
 
 In late summer and early fall, the water contains approximately 
 1 mg/1 dry weight of organic matter. The organic matter is composed mainly 
 of phytoplankton, with diatoms making up over 90 percent of the population 
 and the Cyclotella diatoms predominant during this period of the year, 
 
 ENVIRONMENTAL RADIATION EXPOSURE AND MONITORING IN THE HANFORD AREA 
 
 A fraction of the impurities remaining in the cooling water, after 
 treatment, is transformed into radioactive elements during passage through 
 the reactor and during retention in films which form on the surface of the 
 fuel channels and elements. The majority of the radionuclides are thus 
 
 formed by neutron activation rather than by fission. As the reactor effluent 
 
 *u n i u» d- »4- 4- • „ 56 . 64 M 24 . 51 „ 239 
 water enters the Columbia River, it contains: Mn , Cu , Na , Cr , Np , 
 
 As , Si , making up 90 percent of the total radioactivity; 13 other radio- 
 
 65 
 nuclides, including Zn , which make up 8 percent of the radioactivity; and 
 
 over 40 others, including Co 9 which make up the remaining 2 percent of 
 
8 
 
 ■P 
 (0 
 
 & 
 
 C 
 •H 
 
 in 
 
 ID 
 O 
 
 c 
 
 N bO 
 — 
 
 O Ou 
 
 a 
 o 
 •h 
 
 ■p 
 
 05 
 U 
 P 
 c 
 d) 
 o 
 
 (3 
 O 
 O 
 
 O 0) 
 
 H W 
 
 U. \ 
 
 P 
 
 k 0) 
 
 c o 
 
 •H 
 
 ITS X5 
 
 1 
 
 3 o 
 
 ■H O 
 
 O O 
 
 O .-I 
 
 500 — 
 
 400 
 
 300 — 
 
 200 — 
 
 100 
 
 in 
 
 to 
 
 200 
 
 o ^ 
 
 
 c >, 
 
 
 •H rfl 
 
 
 C<J t3 
 
 
 -v. 
 4h to 
 
 150 
 
 0) 
 
 
 •H 
 
 
 P & 
 
 
 fc 3 
 
 
 O V 
 
 100 
 
 CO 
 
 
 c c 
 
 
 fO o 
 
 
 & «H 
 
 
 H P 
 3 
 
 50 
 
 4h H 
 
 
 o o 
 
 
 CO 
 
 
 0) 
 
 
 P c 
 
 
 
 m -h 
 
 p2 
 
 
 Fig. 
 
 1.3 
 
 1958 
 
 1959 
 
 1960 
 
 1961 
 
 1962 
 
 1963 
 
 .65 
 
 ZINC IN COLUMBIA RIVER WATER AT PASCO, WASHINGTON 
 
65 
 the radioactivity. It should be noted that Zn ' is of minor importance and 
 
 Co only a trace radionuclide as the reactor effluent enters the Columbia 
 River o 
 
 The extensive monitoring program at Hanford and downstream in the 
 Columbia River has shown that natural background and world-wide fallout are 
 the primary sources of environmental radiation exposure for most persons 
 in the neighborhood of the Hanford reservation „ The principal Hanford 
 source of environmental exposure has been identified with the neutron in- 
 duced radionuclides present in reactor cooling water discharged to the 
 Columbia River „ The primary mechanisms of exposure from this source are 
 the drinking of water derived from the river and the consumption of fish 
 and water fowl which inhabit the river „ Consumption of products from farms 
 irrigated with Columbia River water provides an additional source of 
 exposure o 
 
 The composite annual exposure for a hypothetical individual whose 
 habits include consumption of locally caught fish, consumption of products 
 from farms irrigated with Columbia River water, consumption of water from 
 the Pasco sanitary system (which is derived from the Columbia River), and 
 who engage in swimming and boating on the river, has been estimated at 
 150 mrems to the GI tract, 70 mrems to the total body, and 30 percent of 
 the National Committee on Radiation Protection (NCRP) maximum permissible 
 rate of intake for bone seeking radionuclides A high rate of consumption 
 of certain marine organisms, such as oysters from the Willapa Bay, 
 Washington, area would increase the rate of intake 
 
 An extensive and continuous monitoring program developed by 
 Hanford assures the safety of the residents of Richland, Pasco and other 
 cities along the Columbia River from overdoses of environmental radiation 
 
ZINC 65 AND COBALT 60 
 
 65 oo. 
 
 Zinc constitutes only about one percent of the total radioactivity 
 
 fiO 
 
 discharged into the Columbia River „ Cobalt is present as a trace radio- 
 nuclide in the reactor effluent » Neither radionuclide would appear to be a 
 
 potential radiation exposure hazards However, Zinc has a half-life of 245 
 
 fin 
 days and Cobalt has a half-life of 5„27 years Due to their long half- 
 lives, the activity of these radionuclides does not decrease rapidly „ Only 
 a very small percentage of the activity would have decayed during the normal 
 flow time required to reach Pasco, Washington, about 4-0 river miles down- 
 stream from the reactors „ 
 
 fis 
 The flow in the Columbia, the concentration of Zinc ' in the water 
 
 55 
 and the rate of transport of Zinc have been monitored by the Hanford staff „ 
 
 Data resulting from monitoring at Pasco from 1958 to 1963, is presented in 
 
 65 
 
 Figo lo3 The data indicate that the rate of transport of Zinc ' has 
 
 decreased from an annual average of about 100 curies/day in 19 58 to an 
 
 annual average of about 55 curies/day in 1963 „ 
 
 65 
 The annual average Zinc activity in the Columbia River in 1963, 
 
 as reported by the Hanford staff, was 47 pc/g at Hanford Ferry, just 
 
 downstream from the reactors, o38 pc/g at Richland, 22 pc/g at Pasco and 
 
 06 pc/g at Vancouver, Washington, which is 260 miles downstream of the 
 
 65 
 
 reactors o These data indicate that 19 percent of the Zinc activity was 
 
 removed from the water by the time it reached Richland, 47 percent had been 
 removed by the time it reached Pasco and 87 percent by the time it reached 
 
 Vancouver c Other studies by the Hanford staff have shown that the removal 
 
 fin 
 of Cobalt activity from the Columbia River water in this reach compares 
 
 65 
 closely with Zinc „ Richland began using Columbia River water in 1963 and 
 
 65 
 was able to remove an average of 80 percent of the Zinc activity of the 
 
 river water in its water treatment plant „ Pasco, which has been using 
 
Columbia River water for many years, removes about 60 percent of the 
 Zinc activity of the river water in its treatment plant „ 
 
 The Hanford staff have concluded that Zinc is removed along 
 with particulate matter G The radionuclides may initially come in contact 
 with suspended particulate matter, or bottom sediments, or a combination 
 of these o Most of the suspended particulate matter eventually settles, 
 with the finer particles being carried as far downstream as McNary 
 reservoir,. The high degree of removal by the water treatment plants of 
 
 Richland and Pasco further indicates an affinity between the particulate 
 
 65 
 matter and Zinc „ 
 
 Some forms of biota, such as certain algae, have been shown to 
 
 65 
 concentrate Zinc ' thousands of times over the concentration found in the 
 
 surrounding water „ Whitefish caught between the reactor area and Pasco 
 
 65 
 contained an average Zinc ' concentration of 38 pc/g wet weight 8 in 1963 8 
 
 65 
 or more than one hundred times the concentration of Zinc in the sur~ 
 
 rounding water , However „ the biota is sparse in this section of the 
 
 Columbia River., The accumulation by the biota can thus account for only a 
 
 65 
 minor fraction of the depletion of Zinc in this reach „ 
 
 The Hanford staff analyzed five bottom sediment samples taken 
 
 along the shorelines of the Columbia River in the reach extending from 
 
 Ringoid to Richland, in March 8 1962 „ A sample from the river bank opposite 
 
 Ringold contained 310 pc/g of Zinc ' and 13 pc/g of Cobalt „ The four 
 
 remaining samples were from the shorelines of islands in the river between 
 
 Ringold and Richland „ The concentrations of Zinc ' and Cobalt were 
 
 found to decrease with distance downstream from the Hanford reactors Con- 
 
 centrations of Zinc % declined steadily from 880 to 170 pc/g 8 while 
 
 concentrations of Cobalt declined from 2h to 5 6 pc/g with the exception 
 
 fin 
 of one sample which contained 69 pc/g of Cobalt „ All data were expressed 
 
6 E 
 as grams dry weight of sediment Zinc " accounted for about one-third of 
 
 the total activity found in these samples „ 
 
 In core samples taken by the Hanford staff of the bottom sediments 
 
 in McNary reservoir in 1962, Zinc accounted for over two=thirds of the 
 
 fin 
 total radioactivity o Cobalt was also accumulated on the bottom sediments 
 
 From the average of seven core samples, it was estimated that the sediments 
 
 65 
 of the reservoir contained 1350 pc of Zinc per gram dry weight of sedi- 
 
 fin 
 ment, and 47 pc of Cobalt per gram dry weight of sediment, at the 
 
 sediment-water interface „ This concentration decreased rapidly with depth 
 
 to values of about three pc/g for each radionuclide at a depth of twelve 
 
 inches o It was estimated that the sediments contained a total of 57,000 pc 
 
 of Zinc ' and 2500 pc of Cobalt per square inch of sediment, or 230 
 
 curies of Zinc and 10 curies of Cobalt per square mile of sediment <> 
 
 Much of the information included in this introduction has been 
 
 gathered from various reports of the Hanford Environmental Studies and 
 
 Evaluation staff (7, 8, 14, 15) „ Other data have been gathered from a study 
 
 of the Columbia River made in 1954 by the United States Public Health 
 
 Service (22) and from personal discussions with Dr Benjamin B„ Ewing, 
 
 Professor of Sanitary Engineering, University of Illinois a 
 
 OBJECTIVES OF THE STUDY 
 
 The overall objective of a proposed comprehensive Columbia River 
 
 study is, as described by Dr Benjamin B G Ewing (5)i 
 
 "to determine the fate of certain radionuclides in 
 the Columbia River downstream of the Hanford reactors „ 
 This river offers a unique site for such a study in 
 that radionuclides have been discharged to the river 
 in reactor cooling water for many years While no 
 hazard of significance has been produced, the quan- 
 tities of radionuclides which have been put into the 
 river are greater than at any other site in the 
 United States „ 
 
10 
 "It is proposed that the study be confined to the 
 reaches of the river between Priest Rapids Dam 
 (upstream from the reactors) and Vancouver, 
 Washington., The approach is a material balance; 
 i e„j to compare the rate of input to any reach, 
 corrected for decay, with the rate of output from 
 the reach to ascertain the fraction depleted „ 
 Whenever a significant depletion is encountered, a 
 survey will be made to locate the places of storage „ 
 Such a study will provide information about the 
 mechanisms which remove radionuclides from river 
 water and the factors which influence these mecha- 
 nisms , the quantity of each radionuclide being 
 retained in various river reaches, location, and 
 nature of storage, the likelihood of translocation 
 and the potential hazard arising from a possible 
 translocation of stored radionuclides „ 
 
 "The results of this study are needed to provide a 
 better understanding of the fate of radionuclides 
 in a river in order to permit prediction of the 
 hazards which might result from a change of conditions 
 in this river at some future time, or which might be 
 encountered in other rivers under similar circum- 
 stances o" 
 
 The particular objectives of the current study were; 
 
 (a) to obtain, by an extensive literature search, a knowledge 
 of the occurrence of stable and radioactive zinc and cobalt in the aquatic 
 and terrestrial environments and an understanding of the fate of these two 
 elements when discharged into the aquatic environment; 
 
 (b) to develop analytical techniques for determining the concen- 
 trations in environmental samples of both the radioactive and the stable 
 fractions of zinc and cobalt, stressing simplicity of procedure and ana- 
 lytical equipment; 
 
 (c) to obtain and analyze samples of water, plankton and partic- 
 ularly bottom sediments , from a one-hundred-mile reach of the Columbia 
 River between just upstream of the Hanford reactors and just downstream of 
 McNary dam 
 
 The following Chapters consider each objective of the author's 
 study in the stated order Chapters II and III and the Appendix refer to 
 
11 
 
 objective (a), Chapters IV and V refer to objective (b), and Chapters VI, 
 VII and VIII refer to objective (c). 
 
12 
 II, LITERATURE REVIEW 
 
 Part of the first objective in this study was to obtain, by an 
 extensive literature search , a knowledge of the occurrence of stable and 
 radioactive zinc and cobalt in the aquatic and terrestrial environments. 
 The data compiled during this literature review are presented as an 
 Appendix to this thesis. 
 
 The data are divided into four separate sections , based on the 
 geographical location of the samples » Tables A-l and A-2 consist of data 
 obtained from the analysis of samples taken in the Columbia River area. 
 Table A-3 summarizes analyses of samples taken in the Thames River, 
 Connecticut area. Tables A-4 and A-5 report results obtained in the South- 
 west Pacific area, and Table A-6 contains the data found for all areas not 
 included in the preceding tables Each table is divided, where data are 
 available, into two major sections, "Aquatic Environment" and "Terrestrial 
 Environment o " Within each section, the data are tabulated as to sample 
 type in a general order of increasing physical or biological complexity , 
 Thus a typical table begins with data concerning water and ends with data 
 concerning either fish, if in the aquatic environment section, or man, if 
 in the terrestrial environment section, A complete list of the sources of 
 information for this data is included in the references section following 
 Table A-6, Additional references which do nor contain specific quantitative 
 data, but are of general interest, are included separately. 
 
 The quantitative data in these tables should be related to 
 allowable concentrations of these radionuclides in particular types of 
 samples, Eisenbud O) states that the United States Atomic Energy Commis- 
 sion's recommended limits (1961) are: 
 
13 
 Zinc ; 3000 pc/g occupational limit and 100 pc/g non-occupational 
 limit, in water; 400 pc/g in seafood when the population 
 
 obtains half its protein requirement from seafood 
 
 fin 
 Cobalt j 1000 pc/g occupational limit and 50 pc/g non-occupational 
 
 limit, in water; 100 pc/g in seafood when the population 
 
 receives half its protein requirement from seafood 
 
 The recommended limits provide a basis for understanding the significance 
 of the concentrations of Zinc ' and Cobalt reported in the tables. 
 
 It should be recognized that data on radioactivity are most 
 abundant in locations where a possible radiation hazard exists The con= 
 centrations of radioactive zinc and cobalt in environmental samples do not, 
 therefore, represent normal conditions „ 
 
 The concentrations of stable and radioactive zinc and cobalt have 
 been reported in the literature in several types of units , Where possible, 
 
 data in the tables have been converted to ppm (parts per million) or pc/g 
 
 -12 
 (pico OLO ' ) curies per gram), Weights have been recorded as either wet, 
 
 dry or ashed, whenever these data were given in the literature „ Thomas 
 
 etalo (28) has provided the following relationships between dry and wet 
 
 weights for environmental samples, as dry weight to wet weight ratios ; 
 
 "Fish* 10 samples; range ,162 to 262; ave ,200 
 Plants; 9 samples; range ,081 to o*+02; ave ,215 
 Invertebrates t 8 samples; range 125 to ,515; ave„ 238 n 
 
 COLUMBIA RIVER AREA 
 
 Tables A-i and A-2 contain data concerning the Columbia River area, 
 Table A=l is a brief summary of the results of very extensive monitoring of 
 the Hanford area and downstream along the Columbia River, by the Hanford 
 
14 
 staff o Table A=2 includes a broader range of sample types, but the sampling 
 is less intensive o 
 
 Additional Data - Qualitative and Quantitative 
 
 Ttrr r— ^i-r— ~*—r~ B— PM ~T rMrr" i i m i m i — I iM i a— iwiwn ■iiMTiairunn'irnr thii mi i~ i u~w I im wina 
 
 65 
 Pritchard and Joseph (1961) (20) found that Zinc was the most 
 
 abundant radionuclide found in shellfish near the mouth of the Columbia 
 
 River, and that it showed a marked decrease with distance seaward from the 
 
 mouth of the Columbia River for both shellfish and plankton „ 
 
 Osterberg et al (1964) (18) reported that samples of euphausiids 
 
 collected in the Pacific at Newport, Oregon, contained an average of 
 
 65 
 11 o0 pc/g dry weight of Zinc , and that background activities along the 
 
 Pacific coast of Alaska and California showed 1^0 to 1 4 pc/g dry weight of 
 
 65 
 Zinc ' in this organism „ The authors continue: 
 
 fi s 
 "High Zn values near the mouth of the Columbia River 
 
 in spring and somewhat increased values in the fall 
 
 correspond roughly to spring and fall plankton "blooms „" 
 
 The euphausiid studied,, Euphausia pacifia , grazes on 
 
 phytoplankton u c ofrom which it appears to obtain Zn65 000 
 
 fresh water and marine diatoms reach equilibrium with 
 
 reactor effluent water rapidly $ in a few hours 
 
 Euphausiids require a much longer period for maximum 
 
 concent rat ion „ " 
 
 Foster (1963) (6) states: 
 
 65 
 "Zn is the only radionuclide of reactor effluent 
 
 origin which has been found in sufficient abundance 
 beyond the mouth of the Columbia to be of radio- 
 logical interest o The oyster has been found to 
 contain more Zn"^ than other seafood organisms " 
 
 Watson et^ al„ (1961) (29) found, in addition, that the highest 
 
 65 
 levels of Zinc ' were found in plankton, algae and mollusks and that of the 
 
 human foods, oysters exhibited the highest levels: 
 
 65 
 "In these marine organisms, Zn was responsible for 
 
 up to 40% of the total radioactivity „ = oThis radionu= 
 
 elide is present in Hanford reactor effluents and is 
 
 one of the dominant radioisotopes in aquatic organisms 
 
 inhabiting the Columbia River downstream from the 
 
15 
 
 reactors c o oConcentrat ion of Zn in crabs, fish and 
 marine birds is approximately one-tenth that found 
 in algae and mollusks (in samples from the Oregon 
 and Washington coasts ) " 
 
 Palmer (19 58) (19) found that rats exposed to concentrated 
 Hanford reactor effluent for one year contained a concentration of Zinc 
 in the skeleton and soft tissue that was higher than any other radionuclide „ 
 
 Silker (1964) (25) measured the concentrations of zinc and cobalt 
 in Columbia River water just upstream of the Hanford reactors „ Samples 
 were taken during the period from January 5 to August 17, 1962 „ Zinc con- 
 centrations ranged from 2 h to 37*6 ppb and cobalt concentrations ranged 
 from oOOl to „087 ppb, during this period „ 
 
 THAMES RIVER, CONNECTICUT, AREA 
 
 Table A=3 contains data concerning the Thames River, Connecticut, 
 area Of particular interest in this table is the graphic result of a study 
 
 by Skauen (1964) (26) of the effect of nuclear submarine activities on the 
 
 65 
 Zinc concentration in oysters harvested from the Thames River near the 
 
 submarine base Whenever a submarine docked for an extended period, it 
 
 would shut down its power reactor „ The reactor cooling water decreased 
 
 slightly in volume as the water temperature decreased Before starting up 
 
 the reactor for another voyage , the reactor cooling water was "topped up" 
 
 to produce correct operating characteristics within the power reactor system. 
 
 However, as the reactor began to operate, the temperature of the cooling 
 
 water Increased, with a corresponding increase in volume, with the result 
 
 that the excess few gallons of contaminated water was discharged into the 
 
 river o It appears, from the table, that this practice was corrected by 
 
 July 10, 1961 o 
 
16 
 SOUTH-WEST PACIFIC AREA 
 
 Tables A-4 and A-5 contain data concerning the South-West Pacific 
 area Table A~4 summarizes the extensive monitoring of this area following 
 the "Redwing" shot series of 1956, as reported by Thomas et al „ (19 58) (28) 
 Table A-5 provides additional data concerning this geographical area 
 
 Addi-tiona .1 Dat:a - Qualitative and Quantitative 
 
 Watson et al (1961) (29) stated that! 
 
 "Zn^^si a nonfission product commonly formed by 
 nuclear detonations and nuclear reactors , was 
 found in pelagic fish collected in 19 54 near the 
 Pacific Proving Grounds after the 'Castle* series 
 of weapon tests It was subsequently reported in 
 tuna, marine plankton, mollusks and reef fishes 
 of the western Pacific „ In these marine organisms, 
 Zn^5 was responsible for up to 40% of the total 
 radioactivity and in most instances was more 
 abundant than any of the fission products ." 
 
 Held (1961) (10) reported that five years after contamination with 
 
 radioactive fallout which occurred due to a detonation at Bikini Atoll in 
 
 19 54, Zinc ' and Cobalt were found to be the most abundant radionuclides 
 
 in marine organisms, and in man, as a result of the consumption of marine 
 
 organisms o Birds which fed almost exclusively on marine organisms contained 
 
 mainly Zinc „ Zinc ' predominated in fish, with Cobalt present as well 
 
 Marine invertebrates contained Manganese , Cobalt * , Zinc , Strontium 
 
 144 65 60 
 
 and Cerium , with Zinc and Cobalt most prominent Corals contained 
 
 Cobalt o Clams contained mostly Zinc ' and Cobalt * „ Plankton con- 
 
 . . , M 54 _ , .57, 60 „. 65 „. . 95 _ .. , 106 
 tamed Manganese , Cobalt , Zinc , Zirconium , Ruthenium and 
 
 144 . 
 Cerium , all in minute amounts „ Marine algae contained principally 
 
 Cerium 
 
 Thomas et al , (1958) (28) noted that following the "Redwing" shot 
 
 series of 1956, Cobalt and Manganese were the predominant radionuclides 
 
17 
 
 65 oo... 
 
 in clams, Zinc was the major radioisotope in fish specimens, and radio- 
 active cobalt, manganese and zinc were the most universally detected 
 radionuclides with respect to all sample types „ The Cobalt concentration 
 in livers of clams increased for about ten months after the first shot of 
 the series, peaked at about 80 pc/g, then rapidly decreased Cobalt was 
 
 also found in clam mantle, gonad and muscle, but at lower concentrations 
 
 65 
 Zinc ' followed the same pattern, peaking at about 8 pc/g The authors 
 
 en cc. 
 
 concluded that the concentrations of Cobalt and Zinc ' for whole clams 
 
 would be about 20 to 25 percent of that of clam livers for the same sample „ 
 
 Donaldson (1961) (3) reported, with reference to the Eniwetok 
 
 test site, that? 
 
 "Available substances are rapidly taken up by the biota „ 
 Plankton acquire radioisotopes by absorption, adsorp- 
 tion, or botho The major initial concentration of 
 radioactive Isotopes probably occurs in the phytoplank- 
 ton and includes Zn 6 5 (12 to 47%), Co 57 » 58 » 6 ° (11 to 
 50%), Fe 55 » 59 (1 to 40%) and Zr S5 -Hb 95 (3 to 44%) 
 
 "The herbivorous and omnivorous fish tend to concentrate 
 the same isotopes found in plankton Zn^5 accounts for 
 more than 50% of the total radioactivity in the organs 
 of these fish and Fe55»59 comprises a major part of the 
 remaining activity „ The radioactive isotopes of cobalt 
 account for ? to 20% of the radioactivity*, 
 
 "The carnivorous fish such as tuna and bonito (mackeral), 
 caught In the cpen ocean, contain Zn^5 a t the highest 
 levels of any of the three groups of fish, Zn^5 accounts 
 for 75 to 92% of the total radioactivity; Fe 55 »~ 9 for 
 6 to 25% and the cobalt radioisotopes for 1 to 3% " 
 
 Lowman (1961) (13) observed in sea water contaminated with fission 
 
 65 
 products and neutron induced radionuclides that Zinc at 48 hours after a 
 
 detonation accounted for only ,02 percent of the activity in water samples, 
 
 and that by the end of six weeks accounted for ,84 percent of the activity „ 
 
 65 
 However, in plankton samples, at 48 hours, the Zinc accounted for per- 
 cent of the total radioactivity while at the end of six weeks, it accounted 
 for 25 o percent of the total activity „ Iron ' and Cobalt * * 
 
18 
 
 65 
 occur in concentrations almost identical with Zinc , in each of these two 
 
 types of samples, at each sampling time The author comments ; 
 
 "Plankton exhibit high concentration factors for a 
 few elements of which cobalt is one Since plankton 
 only equal about 1 ppm by weight in sea water, thus 
 they contain only a small fraction of the total 
 activity „ u Concentration factors exhibited by plankton 
 for cobalt are 100,000 at six weeks „" 
 
 In the food chain of water to plankton to omnivorous fish to 
 
 57 58 60 
 carnivorous fish, Lowman found that discrimination against Cobalt ' ' 
 
 was progressive throughout the trophic levels A large percentage of the 
 
 65 
 total radioactivity in the carnivorous fish was due to Zinc In the food 
 
 chain of water to plankton to omnivorous fish to birds, the birds did not 
 
 retain significant amounts of radioisotopes of cobalt, but did retain a 
 
 major part of the ingested Zinc , 
 
 that: 
 
 Rowe and Gloyna (1964) (23) found from a review of the literature 
 
 65 
 "The mean level of Zn in 200 male, adult Marshallese 
 
 in 1959 was 9,400 yuc/kg (9„4 pc/g) of body weight, 
 
 or about 100 times that of an inhabitant of the United 
 
 States o The exposure was the result of seven series 
 
 of tests involving the detonation of 59 nuclear devices 
 
 by the United States in the Marshall Islands between 
 
 July, 1946, and July, 1958," 
 
 OTHER AREAS 
 
 Table A-6 contains data for samples obtained from many areas of 
 the world, but excluding the Columbia River, the South-West Pacific and the 
 Thames River, Connecticut areas. 
 
 Addi~t iona l Dg'Cg^ ^ Qualitative an d Quant it at iye 
 
 Lomenick et al u (1963) (12) determined the concentrations of 
 
19 
 
 fin 
 
 Cobalt in the White Oak Creek drainage basin This basin was used from 
 1943 to 1955 as a final settling basin for low-level radioactive wastes 
 discharged from the Oak Ridge, Tennessee, reactors and laboratories «, The 
 detention provided by the impoundment furnished some dilution and a period 
 of decay for short-lived radionuclides before release to the Clinch River « 
 It also resulted in deposition and accumulation of contaminated sediments. 
 In samples taken in 1962, the authors found that the layer of sediment 
 
 extending from to 6 inches below the surface contained 119 curies of 
 
 fin 
 Cobalt , the layer from 6 to 12 inches contained 22 curies, the layer from 
 
 12 to 18 inches contained 8 curies, and the layer from 18 to 24 inches 
 
 fin 
 contained 3 curies, for a total of 152 curies of Cobalt » A preliminary 
 
 survey of the creek bed and its flood plain revealed that bottom sediments 
 
 to a depth of 18 inches, 2 3 miles downstream from the source of contami- 
 
 fin 
 nation 8 contained Cobalt in concentrations of 290 to 2200 pc/g dry 
 
 fin 
 weight o Cobalt was the major radionuclide present in these sediments „ 
 
20 
 
 III, A DISCUSSION OF ZINC 65 EQUILIBRIUM 
 AND TRANSPORT IN NATURAL WATERS 
 
 65 
 What happens to Zinc ' radionuclides discharged into a watercourse? 
 
 An understanding of the dynamic equilibrium in which zinc, and therefore 
 Zinc , exists in natural waters is a prerequisite to a reasonable evalua- 
 tion of the probability of radiation exposure to man caused by a discharge 
 
 . _. 65 
 of Zinc o 
 
 In natural systems, there is little difference between the behavior 
 of the stable and the radioactive isotopes of zinc The total zinc content 
 of the system must therefore be considered,, The addition of radioactive 
 zinc in the concentrations found in environmental samples amounts to a 
 negligible increase in the total zinc content of natural waters, 
 
 There are several paths through which this radionuclide may become 
 a source of radiation exposure to man. The most direct path, causing direct 
 
 c c 
 
 internal exposure, is the consumption of water containing Zinc „ Another 
 pathway is the consumption of food derived either from the aquatic environ- 
 ment or from areas irrigated with water from a contaminated watercourse 
 
 Direct external exposure may result from swimming, bathing and boatingo 
 
 65 
 Zinc radionuclides present on bottom or shoreline sediments, as well as 
 
 those present in the water 9 contribute to direct external exposure „ 
 
 The dynamic equilibrium existing may be defined as the balance 
 between forces active in removing the radionuclides from solution and the 
 forces active in returning them to solution. These forces may be categor- 
 ized as being of chemical, physical or biological nature „ Factors causing 
 the transport of zinc and Zinc adsorbed on sediments must also be con- 
 sidered o Within a reach of a river 9 or within a lake, or where a river 
 
21 
 enters an ocean, a materials balance between input to the area and output 
 from the area must be considered , The materials balance would permit an 
 estimation of the storage within the reach „ 
 
 CHEMICAL FORCES 
 
 Solubility Limitations 
 
 The solubility of zinc hydroxide and zinc carbonate place an upper 
 limit on the concentration of zinc to be found in natural waters „ The zinc 
 ion is considered to react with water in the following manners 
 
 Zn ++ + H 2 t ZnOH + + H + Z Zn(OH ) 2 + H + 
 
 The equilibrium constant derived from the mass action equation at 25°C is 
 
 (Zn0Ht)(Ht) = 2,45 x 10- 10 
 (Z„ ++ ) 
 
 Thus the Zn ion represents almost the entire quantity of ionic zinc at 
 pH values less than eight At pH"s greater than eight, the ZnOH ion becomes 
 significant and it becomes about 25 percent of the total ionic zinc at a pH 
 of nme 
 
 The solubility of zinc hydroxide at 25°C is governed by the 
 following solubility product; 
 
 (Zn ++ )(OH~) 2 = 4,5 x lCf 17 
 
 Thus, at a pH of eight or less, 290 ppb of Zn ion can exist in solution, 
 and at a pH of nine, 29 ppb of Zn ion can exist in solution without pre- 
 
 cipitating zinc hydroxide, 
 
22 
 The solubility of zinc carbonate at 25°C is governed by the 
 following solubility products 
 
 (Zn ++ )(C0 3 ~~) = 2 x 1(T 10 
 
 Since the carbonate-bicarbonate alkalinity equilibrium is dependent on pH, 
 the solubility of zinc carbonate is a function of both the alkalinity and 
 the pH of the water „ Rowe and Gloyna (1964) (23) state that at an alkalinity 
 of 100 mg/1 as CaCCL , or less, and at a pH of eight or less, 1360 ppb of 
 Zn ion can exist in solution without precipitating zinc carbonate „ If 
 the pH is raised to nine, the Zn ion solubility is decreased to 150 ppb<, 
 
 At an alkalinity of 250 mg/1 as CaCO , or lesSj, and a pH of eight or less, 
 
 ++ „ . . 
 
 150 ppb of Zn ion can exist in solution „ If the pH is raised to nine, 
 
 at this alkalinity concentration, the Zn ion solubility is decreased to 
 60 ppbo 
 
 From the data included in the Appendix, it can be concluded that 
 the total zinc concentration found in natural waters seldom exceeds 200 ppb 
 It can therefore be concluded that zinc hydroxide and zinc carbonate pre- 
 cipitates will not be found in significant amounts in natural waters <, 
 
 As a cation 8 zinc can occupy a position within the crystal lattice 
 structure of a clay particle, or may be attached to a negatively charged 
 site on the surface „ In the former case, the zinc is considered to be 
 unexchangeable since it is in dynamic equilibrium with the ions in solution „ 
 Suspended matter and bottom sediments, such as silts and clays, apparently 
 take up and release zinc by the mechanisms of adsorption and ion exchange 
 at the surfaces of the particles „ 
 
23 
 
 Tne concept of an ion exchange type of reaction is supported by 
 the results of studies by Bachman (1961) (2K Increasing the concentration 
 of other cations in solution decreased the uptake of zinc Bachman con- 
 cluded that this was due to a competition between these ions and zinc for 
 the available exchange sites The suspended materials and bottom sediments 
 in natural waters may thus behave as ion exchangers which are in a state 
 of dynamic equilibrium with the ions in solution „ However, 0'' Connor and 
 Renn (1964) (16) found that an increase in concentration of calcium ions 
 in solution, from 40 to 80 mg/1, had only a minor effect on the uptake of 
 
 zinc by sediments „ Rowe and Gloyna (1964) (23) reported that the uptake of 
 
 65 
 Zinc was independent of the concentration of Mg, Ca, Na and K ions. The 
 
 mechanism of uptake of zinc seems to be due largely to adsorption on the 
 
 surfaces of the suspended matter and bottom sediments,, 
 
 Further studies by Rowe and Gloyna with Lake Austin, Texas, 
 
 sediments , indicated that the clay fraction of the sediment was the main 
 
 65 
 
 sorbent of Zinc „ The effect of natural organic material in these sedi- 
 
 65 
 ments was small and suggested that an insignificant amount of Zinc was 
 
 associated with the organic material in the sediment „ 
 
 The influence of pH on uptake and release was also studied by 
 
 65 
 
 Rowe and Gloyna „ They concluded that Zinc ' uptake increased as the pH was 
 
 raised up to ten It was apparent that uptake was reduced as the pH was 
 lowered to a value of seven, and materially reduced at a pH of six Uptake 
 was negligible at a pH of five The lowering of the oxidation-reduction 
 potential of the water, producing reducing conditions, had an effect on the 
 release of adsorbed Zinc similar to that resulting from a reduction of 
 the pH of the water „ 
 
 O'Connor and Renn showed that in natural water systems the major 
 portion of the zinc in the system is adsorbed when equilibrium exists 
 
24 
 Removal from solution is effected mainly by the particulate matter in the 
 stream bed, with suspended matter usually of secondary quantitative impor- 
 tance o The pH had a very definite effect on zinc adsorption on particu- 
 late matter » indicating an exchange between zinc and the hydrogen ion 
 All of the zinc adsorbed on these particles could be readily returned to 
 solution by adjusting the pH to four or less. 
 
 Most natural waters such as rivers , impoundments and estuaries 
 contain suspended matter and sediments that are highly undersaturated with 
 respect to zinc Thus zinc is adsorbed rapidly upon entering the water- 
 course 
 
 PHYSICAL FORCES 
 
 When an industrial effluent or stream containing zinc enters a 
 watercourse, the most important physical forces influencing the ionic con- 
 centrations include temperature and density differences between the influent 
 stream and the receiving water, the velocity, turbulence and flow volume of 
 the receiving water, and the bottom shape characteristics of the receiving 
 water These forces affect the diffusion and mixing of the influent stream 
 and the distance the zinc ions may travel before reaching equilibrium with 
 the suspended particulate matter and the bottom sediments „ Diffusion and 
 mixing result in dilution, but it must be realized that dilution only 
 reduces the concentration of ions, and does not remove them from the envi- 
 ronment o Density differences and tidal movement must also be considered 
 
 e c 
 
 in estuarine and coastal waters. Radioactive decay influences the Zinc 
 concentrations but not the total zinc concentration 
 
 BIOLOGICAL FORCES 
 
 Zinc is present as an essential component of the protoplasm of 
 
25 
 
 living organisms, associated with enzymes which regulate cellular metabolism , 
 
 65 . . 
 
 Zinc and Zinc may therefore be assimilated by flora and fauna Adsorption 
 
 of the ions on surfaces of phytoplankton is also a known mechanism „ When 
 metabolized, the ion is not exchangeable, but when adsorbed, it is exchange- 
 able o The removal of zinc from solution by biological means may be con- 
 sidered analogous to removal by clay particles, with one difference When 
 the biological form dies and decays, the assimilated and adsorbed zinc will 
 
 return to solution or be adsorbed on surrounding sediments „ 
 
 65 
 Biological uptake and return of zinc and Zinc ' to solution are 
 
 usually not of very great significance, quantitatively, to the zinc equilib- 
 rium in natural waters, due to the low density of these organisms in the 
 
 65 
 water,, However, a portion of the Zinc adsorbed or assimilated by the 
 
 phytoplankton will be transferred through food chains to fish and thus to 
 
 man Bottom feeding commercial fin fish and bottom living shellfish take 
 
 65 
 up Zinc present on the bottom sediments and associated with plankton of 
 
 watercourses and shallow coastal areas When these fish are used for human 
 
 65 
 consumption, part of the Zinc present in the edible portions of the fish 
 
 will be retained by the consumer „ 
 
 65 
 TRANSPORT OF ZINC 
 
 Rowe and Gloyna (1964) (23) reported the results of an extensive 
 
 65 
 study to evaluate the transport of Zinc under simulated river conditions <> 
 
 65 
 They concluded that in a flowing system the greatest fraction of Zinc ' was 
 
 associated with the solution and suspended material and would be continu- 
 ously transported downstream „ In a non-flowing system such as a lake, the 
 
 65 
 Zinc would become associated mainly with the bottom sediment , Uptake of 
 
 Zinc by rooted and macroscopic plants was found to be independent of the 
 
26 
 
 flow velocity o Photosynthesis appeared to be the prime element in the 
 uptake and release of Zinc in these plants <, 
 
 They concluded in additions 
 
 65 
 "1 The transport of Zinc in a stream is affected 
 
 significantly by hydrodynamic characteristics, chemical 
 
 characteristics of bottom sediments, type and amount of 
 
 aquatic plants and the environmental factors affecting 
 
 their growth „ 
 
 2o The role of bottom sediment in the transport of 
 Zinc65 is limited by opportunities for contact, the 
 composition of the clay fraction, and the pH Under 
 sluggish stream conditions, contact is slight and 
 effectively reduces the role of the clay fraction , 
 The Zinc^S under short contact periods becomes asso- 
 ciated with only the top few millimeters of the sedi- 
 ment and comes into contact mainly with the organic 
 debris which has settled The sediment is sensitive 
 to pH for there is no uptake of Zinc°^ if the pH drops 
 below five Furthermore, there is an increase in 
 uptake if the pH levels are between five and ten. The 
 Zinc^ is released with time if the pH is increased 
 above ten* 
 
 3 If Zinc" is released in a stream and plants are 
 available, the Zinc" will become associated, initially 
 and probably preferentially, with the plants. However, 
 this initial association with the plants is of a tem- 
 porary nature and is controlled by the growth cycle , 
 Zinc" as an essential micronutrient is sorbed primarily 
 by the leaves and becomes involved in the metabolic 
 processes o When plants die and settle to the bottom, 
 the Zinc^S is released back to solution where it is 
 available for plant growth or it may be transported 
 hydrodynamically further downstream 
 
 to Environmental factors such as pH, dissolved oxygen, 
 oxidation-reduction potential, and light intensity 
 affect plant growth and therefore are related to the 
 transport of Zinc^S i n streams. Thus, a decrease in 
 plant growth will be accompanied by an increase in 
 Zinc^S transport* In a stream or river with abundant 
 plant growth, the transport of Zinc^S will be arrested „ 
 
 5 In a non- flowing ecological system such as a lake* 
 the Zinc^ will tend to become associated with the bottom 
 sediment due to prolonged contact , as evidenced by the 
 greater penetration into the sediment „ The Zinc" in the 
 sediment of a closed ecosystem tends to be non-exchangeable 
 and only a fraction remains available for plant growth „ 
 The pH of the sediment , provided it does not drop below the 
 neutral point or exceed ten, will not affect the transport 
 of Zinc 65 o" 
 
27 
 FACTORS CAUSING THE RETURN OF ZINC 6 ° TO SOLUTION 
 
 There are many factors which influence the return of zinc and 
 
 65 . 
 
 Zinc to solution o Some of these, such as a reduction in pH 9 a reduction 
 
 in oxidation-reduction potentials a reduction in plant growth and the decay 
 
 of rooted and suspended plants, have been mentioned previously 
 
 A change in chemical properties of the waste materials discharged 
 
 or of the receiving water itself may solubilize some of the previously 
 
 adsorbed ions A reduction of pH by an increase in the acidity of the 
 
 waste stream is an example „ The alkalinity of the receiving water will 
 
 65 
 eventually absorb the acidity 8 but in the process Zinc adsorbed on bottom 
 
 sediments will be solubilized and will flow downstream to a new adsorption 
 
 site 
 
 The release of increased quantities of stable zinc may reduce the 
 
 biological and chemical uptake of Zinc , Where Zinc ' is already adsorbed 8 
 
 the addition of such diluting stable materials may be responsible for the 
 
 65 
 return of Zinc to solution „ Upstream saturation of bottom sediment and 
 
 rooted plant surfaces will tend to cause subsequent contaminants to move 
 
 further downstream before being adsorbed. 
 
 It is also possible that when the levels of activity in the water 
 
 environment drop due to decreased releases or increased flows, the Zinc 
 
 adsorbed or exchangeable on bottom sediments and biological forms may be 
 
 released slowly back to the water 
 
 MATERIALS BALANCE 
 
 In studying the Zinc equilibrium and transport within a reach 
 of a river, or within a lake, or in an estuary formed when a river flows 
 into an ocean, a materials balance of Input and output is useful „ Data 
 obtained in this type of study may help to indicate what happens to the 
 
28 
 
 Zinc ' within the area Continuous monitoring of the Zinc ' concentrations 
 in the water will provide data which can be used to predict the changes in 
 
 concentration with seasonal changes in flow and water temperature The 
 
 65 
 probability of changes in concentrations of Zinc in municipal water sup= 
 
 plies taken from the contaminated water can be estimated,, 
 
 65 
 
 To establish the input into the area, the zinc and Zinc in 
 
 solution and adsorbed on the suspended matter upstream of the study area 
 must be monitored,, If the upstream reach is prone to scouring action during 
 
 floods, the bottom sediments must be analyzed „ Within the study area, the 
 
 65 
 input of Zinc ' from industrial effluents and from fallout must be monitored „ 
 
 Zinc and Zinc ' from tributary streams, if present in significant quantities 
 
 in solution, on suspended matter or from scoured bottom sediments, must be 
 
 accounted for Ground water flow and surface runoff from river banks and 
 
 adjacent drainage areas may also affect the total zinc concentration within 
 
 the area 
 
 Monitoring of output in solution, on suspended matter or on 
 
 scoured sediments either flowing out of the study area or being withdrawn 
 
 for industrial, agricultural or domestic use, is a necessity Groundwater 
 
 seepage may affect the total zinc and Zinc ' concentrations „ Radioactive 
 
 decay also constitutes a continuous decrease in Zinc 
 
 SUMMARY 
 
 Zinc is one of the isotopes of the element zinc The Zinc 
 
 equilibrium and transport in natural waters is therefore based on the total 
 zinc content of the aquatic environment „ The dynamic zinc equilibrium 
 existing in this environment may be thought of as the flux between the 
 different phases superimposed upon the movements of the phases themselves 
 
29 
 
 At the zinc concentration levels found in natural waters, insoluble zinc 
 
 compounds will not be formed „ Under pH conditions prevailing in most 
 
 ++ 
 natural waters, the soluble zinc will be found as the Zn ion„ The zinc 
 
 ion will establish an equilibrium with the zinc adsorbed on the surfaces 
 of suspended matter and bottom sediments , The clay fraction of the sus- 
 pended matter and sediments may be the main inorganic sorbent of zinc 
 Rooted aquatic plants and phytoplankton are the primary organic sorbents 
 of zinco However, the death of these living plants is followed by a release 
 of zinc associated with these plants „ The adsorption and desorption of zinc 
 is dependent on the pH of the waters The degree of adsorption is high and 
 the rate, rapid, at pH's above neutrality., Desorption is complete at pH's 
 below four 
 
 Much of the information included in this discussion has been 
 gathered from reports by Bachman (1961) (2), Donaldson (1960) (3), O'Connor 
 and Renn (1964) (16), Rowe and Gloyna (1964) (23), and Straub (1960) (27), 
 
30 
 
 IV. ANALYTICAL PROCEDURE 
 
 This chapter describes the analytical procedure developed for 
 the quantitative determination of total and radioactive zinc and cobalt in 
 samples of river water, plankton and bottom sediments collected from the 
 Columbia River on August 14 and 15, 1963. 
 
 The analysis of each sample was divided into four phases as 
 illustrated in Fig 4.1. Phase I began with the sample as received at the 
 laboratory o It included preliminary separations of each sample to change 
 it to a more suitable form for analysis. Phase II included analyses for 
 total zinc and cobalt and total gamma radioactivity . The third phase was 
 the separation and isolation of the elements, zinc and cobalt. In the 
 fourth phase, the zinc and cobalt fractions were quantitatively analyzed 
 for both radioactive and total zinc and cobalt. 
 
 It should be noted that this system provided a quantitative check 
 on the method used for separation and isolation of each of the two elements, 
 A qualitative check was provided by comparing the waveform of the isolated 
 samples on a single channel gamma ray spectrometer with that of standard 
 waveforms of these two elements. Any appreciable contamination or carry- 
 over would cause a discrepancy in the shape of the isolated samplers 
 waveform. 
 
 PHASE I 
 
 Water 
 
 Each water sample had been passed through a Dowex 50 hydrogen 
 cycle cation exchanger at the collection site. These exchangers were sealed 
 and delivered to the laboratory. The exchangers were made up of approxi- 
 mately 120 ml of exchange resin contained in a 150 ml columnar separatory 
 
PHASE I 
 
 PHASE IV 
 
 WATER 
 (in Dowex 50 cation 
 resin) 
 
 Eluted with 2N-HC1 
 i 
 
 PLANKTON 
 
 31 
 
 BOTTOM SEDIMENTS 
 
 1 
 
 ELUATE Concentrated 
 
 by Evaporation 
 H 
 
 Washed with 0.5N-HC1 Counted for Total 
 
 i 
 
 I 
 
 t 
 RESIDUE Dr ed and 
 
 Weighed | 
 
 i 
 I 
 ft 
 
 Counted for Tota 
 Gamma Acti vi ty 
 
 Gamma Activity 
 
 J 
 
 Dried and Weighed 
 
 Counted for Total _^ 
 
 Gamma Activity == ^ : =5^ Sample Taken for 
 PHASE II ||L Total Zinc and -____ Correction Made 
 
 .Total Cobalt =r " =rs=:S *-for Loss in 
 
 Remaining Sample 
 
 "^ 5s ^==^=S^ic === Tota 1 Cobalt = ~ = ^ ==: S*-for Los: 
 == ^ == " ;:?S: S^£ r - =::::::::: ^ Rema i n i i 
 
 PHASE III Zinc and Cobalt isolated by Anion Exchange Chromatography 
 
 Analysed for Total Zinc 
 
 It 
 
 Counted for Gamma Activity 
 'II 
 
 Composite Sample of Zinc 
 l| 
 
 i J 
 
 l|l 
 Concentrated by Evaporation 
 li 
 
 f 
 
 Gamma Spectrum Compared 
 with Standard 
 
 COBALT 
 Analysed for Total Cobalt 
 
 ! 
 
 Counted for Gamma Activity 
 
 I 
 
 Composite Sample of Cobalt 
 
 Conce 
 
 nt rat 
 
 ed by Evaporation 
 
 i 
 
 Gamma Spectrum Compared 
 with Standard 
 
 Fi fi» ■»•! 
 
 FLOW DIAGRAM OF ANALYTICAL PROCEDURE 
 
32 
 
 funnel „ The resin was held in place in the funnel with the aid of glass 
 wool plugs at each end of the funnel. When received at the laboratory, 
 each exchanger was unsealed, attached to a retort stand and a 500 ml sep- 
 aratory funnel reservoir was sealed to the ground glass inlet „ The 
 reservoir was filled with 2N-HC1 and the acid allowed to pass through the 
 cation resin at a rate of approximately .5 ml/sq cm /min. Ten resin 
 volumes of 2N-HC1 were passed through the resin „ The eluate was collected 
 in a 1000 ml volumetric flask and transferred, with washings of 5N-HC1, 
 to a 1000 ml beaker „ The glass wool filters used in the collection of 
 water samples were also washed with 2N-HC1 and the washings added to the 
 beaker o The beaker was then placed over a Bunsen flame in a hood. Three 
 "V" shaped pieces of glass tubing were placed on the top edge of the beaker 
 and a six-inch diameter watchglass, with its convex face pointed down, was 
 placed on top of the glass "V"s. This method resulted in rapid evaporation 
 without loss of sample or contamination., The eluate was evaporated to a 
 final volume of approximately 50 ml and stored, with washings, in a gradu- 
 ated glass bottle « The above method was used for all concentration steps 
 in the analyses , 
 
 Plankton 
 
 Each plankton sample was received at the laboratory in 250 ml 
 sealed glass bottles „ Each sample was shaken, unsealed and poured, with 
 washings of . 5N-HC1, onto a ,45 y membrane filter placed over a disc of 
 fiberglass window screening in a six-inch diameter Buchner funnel inserted 
 in a vacuum flask „ A vacuum was applied to the flask and the sample washed 
 with five 100 ml aliquots of „5N-HC1„ The residue was dried at 103 de- 
 grees Centigrade and weighed to determine the initial dry weight of the 
 plankton sample „ The residue was then placed in a plastic test tube and 
 
33 
 counted for total gamma activity. The eluate was concentrated to approxi- 
 mately 50 ml by evaporation and stored, with washings, in a graduated glass 
 bottle. 
 
 Bottom Sediments 
 
 Each bottom sediment sample was received in the laboratory in 
 sealed plastic containers which held about 1500 to 2000 grams of moist sedi- 
 ment. Each sample was thoroughly mixed on a large plexiglass plate, A 10 
 to 15 g dry weight representative sample was placed in a plastic test tube 
 and counted for total gamma activity. The contents of the test tube were 
 then placed on a glass dish, dried at 103 degrees Centigrade, and weighed, 
 
 A 250 to 350 g dry weight representative sample was taken from 
 the original sample and washed with five 200 ml aliquots of , 5N-HC1 to 
 remove the zinc and cobalt, using the same apparatus and procedure as was 
 used for the plankton samples. The residue was dried at 103 degrees Centi- 
 grade for 24 hours and weighed, A 10 to 15 g sample of the dry residue was 
 taken and counted for total gamma activity to determine what proportion of 
 gamma activity remained after the acid wash. The eluate from the acid wash 
 was concentrated to about 150 ml by evaporation. In this evaporation step 
 a yellow~amber gel formed when the eluate had been concentrated to about 
 150 ml. Care had to be exercised at this stage, as the gel had poor heat 
 transfer characteristics and tended to "pop," At this point the gel was 
 cooled and refiltered, using five 100 ml aliquots of , 5N-HC1 to remove the 
 zinc and cobalt from the gel, (After this treatment, the remaining gel was 
 white and opaque. Samples of the washed gel were counted and found to 
 contain negligible activity.) The eluate was finally concentrated to 
 approximately 50 ml and stored in a graduated glass bottle. 
 
34 
 
 PHASE II 
 
 At the beginning of Phase II, the zinc and cobalt separated from 
 each sample was in an aqueous phase and concentrated to approximately 50 ml 
 in volume . The samples were about 6N in HC1 (due to evaporation) and had 
 been stored in graduated glass bottles . 
 
 The original volume of the water samples were known. These 
 volumes could be converted to weight for future calculations „ The dry 
 weights of the plankton and bottom sediment samples were known, All data 
 for plankton and bottom sediments could thus be recorded in terms of dry 
 weight o The remaining portion of each bottom sediment sample was dried 
 and weighed in order to obtain data regarding bottom sediments in terms of 
 the surface area of the river bottom. 
 
 The initial step in Phase II was to take a 10 ml aliquot of each 
 sample from the graduated bottles and count each aliquot for total gamma 
 activity o This activity was recorded in terms of cpm per g of original 
 sample o Dry weights were used throughout the analyses for plankton and 
 bottom sediment samples. The 10 ml aliquots were then returned, with 
 washings of . 5N=HC1, to the graduated glass bottles. 
 
 Samples not exceeding 5 ml were taken for total zinc and total 
 cobalt analyses. These analyses were to be used only as checks for gross 
 error in the more accurate analyses performed after each element had been 
 isolated o They were also used to provide approximate solution concentra- 
 tions so that the samples would be within the correct range of allowable 
 concentrations when the final analyses were made. The procedures used for 
 these analyses are recorded at the end of this chapter. 
 
 Corrections were made for the volume of sample lost in this step. 
 Finally, 12N-HC1 was added to the remaining concentrated eluate until it 
 was at least 7N in HC1„ 
 
35 
 
 PHASE III 
 
 Fresh anion exchange columns were made up for each sample, con- 
 structed in the same manner as the water sampling exchangers „ but containing 
 about 30 ml of resin in a 50 ml columnar separatory funnels Dowex 1, 
 chloride cycle, 50 or 200 mesh anion resin was used for separating and 
 isolating and zinc and cobalt „ The flow rate through the anion exchange 
 column was approximately 2 ml/sq cm /min. The following procedure was 
 used? 
 
 Procedure for Separati on and Is olat ion of Zinc and Cobalt 
 I, Pass three resin volumes of 7N-HC1 through 30 ml of Dowex 1 
 anion resin in a column. 
 
 2 c, Make sample at least 7N in HC1 and three resin volumes in 
 volume and pass through resin „ 
 
 3o Pass ten resin volumes of 7N-HC1 through resin as a rinse „ 
 4„ Pass ten resin volumes of 4N-HC1 through resin and collect 
 eluate Concentrate eluate to approximately 50 ml by evaporation and store 
 in graduated glass bottles. This fraction contains the cobalt, pure and 
 4N in HClo 
 
 5 Pass ten resin volumes of >5N~HC1 through resin as a rinse 
 6 Pass ten resin volumes of „01N-HC1 through resin and concen- 
 trate as in step 4 This fraction contains the zinc, pure and 01N in HC1„ 
 7o Discard the used resin „ 
 
 PHASE IV 
 
 At the beginning of Phase IV, the zinc that had been separated 
 from the original sample had been isolated in a pure state and stored as a 
 liquid in a graduated glass bottle in dilute HClo The cobalt fraction was 
 
36 
 
 in a similar condition except that the normality of the acid in which it 
 was stored was much higher, at approximately 6N, due to evaporation. 
 Accurate values for radioactive zinc and for radioactive cobalt could now 
 be obtained by counting 10 ml aliquots of each sample Accurate values for 
 total zinc and total cobalt could also be obtained, using the procedures 
 described at the end of this chapter and by diluting or concentrating the 
 sampie to a proper volume, as ascertained by the previous analyses 8 to 
 place the concentration within the required range for analysis 
 
 A composite sample of zinc and another of cobalt were re-concentrated 
 until their activities were great enough to run a gamma spectrum of eacho 
 This spectrum was compared with that of a standard, at the same activity 
 level, to provide a qualitative check on the isolation procedure „ 
 
 ANALYSES FOR TOTAL ZINC AND FOR TOTAL COBALT 
 
 The analysis for total zinc was an adaptation of the method called 
 the "Mixed-Color Method" described on page 265 of the 11th edition of 
 Standard Methods for the Exa mination of Wat er and Wastewater (1) All 
 reagents were unchanged , The analysis for total cobalt was an adaptation 
 of the method called "Procedure B (Citrate-Phosphate-Borate Medium)" de- 
 scribed on page 419 of Colorimetric Determin ation of Trace s of Metals by 
 Eo B Q Sandell (19 59) (24). All reagents were unchanged. 
 
 The following procedures were used; 
 
37 
 
 Analysis f o^Tota l Zinc 
 
 lo Sample solution should contain between 1 and 15 ug of zinc, 
 have a volume of not greater than 10 ml and be neutral in pH, 
 
 2, Place sample in a 125 ml Squibb separatory funnel and bring 
 the volume up to 10 ml by adding zinc-free water. 
 
 3, Add 5,0 ml of acetate buffer and 1,0 ml of sodium thiosulfate 
 solution and mix, 
 
 Ho Add 10 ml of dithizone II solution, stopper and shake 
 vigorously for 1-2 minutes. Allow the layers to separate and allow the 
 lower layer to run into a 25 ml volumetric flask, 
 
 5o Repeat step 4 with an additional 10 ml of dithizone . 
 
 6, Repeat step 4 with an additional 5 ml of dithizone. During 
 this third extraction, the lower layer should be almost the same color as 
 the reference blank being used, 
 
 7 Bring the volume of the sample collected in the 25 ml volu- 
 metric flask up to exactly 25 ml with dithizone II solution and mix, 
 
 8, Set the spectrophotometer at: Wavelength = 510 my, 
 
 9, Measure absorbance of sample against a blank which has gone 
 through steps 2 to 7, 
 
 10, Compare results with standard curve for zinc, 
 
38 
 
 Analysis for Total Cobalt 
 
 1, Sample solution should contain between 1 and 35 ug of cobalt. 
 Place in a 50 ml erlenmeyer flask and slowly evaporate to dryness to 
 neutralize the sample,, 
 
 2 Add 2o5 ml of citric acid solution , 
 
 3, Add 3,0 ml of phosphate-boric acid buffer and mix g 
 
 4, Check pH by testing a small drop with cresol red. It should 
 be close to 8,0, If necessary, add dilute HC1 or dilute NH OH to adjust 
 the pH, The volume at the completion of step 4 should not exceed 10 ml, 
 
 5, Add exactly 1,0 ml of nitroso-R salt solution while stirring, 
 
 6, Boil for 1 minute, 
 
 7, Add 3,0 ml of reagent grade nitric acid, 
 
 8, Boil for 1 minute, 
 
 9, Cool in the dark, 
 
 10 o Transfer samples to a 25 ml volumetric flask and add repeated 
 washings to bring volume up to 25 ml, 
 
 11, Set the spectrophotometer at; Wavelength = 500 my, 
 
 12, Measure absorbance of sample against a blank that has gone 
 through steps 2 to 10, 
 
 13, Compare results with standard curve for cobalt. 
 
39 
 
 V„ DISCUSSION OF ANALYTICAL PROCEDURE 
 
 This discussion is presented to clarify the rationale for each 
 step of the analytical procedure „ 
 
 PHASE I 
 
 Elution of Zinc and Cobalt from Dowex 50 Cation Exchange Resin 
 
 Dowex 50 is a strongly acidic cation exchange resin which 
 operates on a hydrogen cycle „ When water is passed through the resin 9 at 
 near neutral pH 9 divalent metallic cations such as zinc and cobalt displace 
 hydrogen ions and are strongly held by the resin „ The passage of dilute 
 HC1 through the resin tends to displace the divalent ions due to the 
 increased concentration of hydrogen ions Q 
 
 A series of tests were run to ascertain that both zinc and cobalt 
 would be completely retained when passed through the Dowex 50 cation resin 
 in a neutral solution,, After the zinc or cobalt cations had been adsorbed 
 on the resin s each test was continued 9 using a different normality of HC1 8 
 to find the optimum normality to be used to elute these two cations from 
 
 the resin 
 
 65 
 In the first test series B a known amount of Zinc tracer - 9 in a 
 
 neutral solution 9 was passed through the resin at approximately 
 
 2 ml/sq cm/mino The eluate was counted in each test and contained no 
 
 65 
 measureable activity,, It was therefore certain that all of the Zinc ' had 
 
 been retained by the resin „ Elution was accomplished by the passage of 
 
 12N 9 8N 9 6N 9 4N 9 and 2N=HC1 through the resin 9 at approximately 
 
 o5 ml/sq cm/min 9 one normality of HC1 being used for each test 9 and new 
 
 resin also used for each test., The eluate was collected in .10 ml increments. 
 
 in plastic test tubes 9 and counted for gamma activity., It was found that 
 
40 
 the rate of elution became slightly more rapid as the normality of the 
 acid decreased, and that the length of the run was shortened,, Elution was 
 complete after the passage of seven resin volumes of 6N-NC1, or with the 
 passage of only five resin volumes of 2N-HClo There was considerably less 
 tailing off of the elution curve when 2N-HC1 was used These tests indi- 
 
 CiC. 
 
 cated that rapid and complete elution of Zinc ' is attained using 2N-HC1„ 
 
 A similar test was conducted using Cobalt tracer and 2N-HC1, 
 with similar results „ 
 
 It was concluded that complete elution of zinc and cobalt could 
 be obtained by the passage of ten resin volumes of 2N-HC1 through the 
 cation resin e A rate of ,5 ml/sq cm/min provided rapid elution without 
 short-circuiting through the resin bed„ A head of at least one-half an 
 inch of liquid was allowed to accumulate initially before the inlet 
 reservoir was sealed to the exchange column, in all ion exchange opera- 
 tions , to help prevent short-circuiting and to keep the entire ion 
 exchange bed submerged in liquid An air space between the top of the 
 liquid in the exchange column and the reservoir was also maintained, so 
 that fresh j, uncontaminated eluting liquid would be continually entering 
 the resin 
 
 All new cation resin was washed with 2N-HC1 and then with 
 deionized water before use All new anion resin was washed with deionized 
 water and then with 7N-HC1 before use„ These steps decontaminated the 
 resins and then acclimated them for their respective uses As an addi- 
 tional precaution, new resin was used for each sample analyzed « 
 
 Elution of Zinc and Cobalt_from plankton and Bottom Se diment 
 Samples 
 
 The plankton and bottom sediment samples collected from the 
 
41 
 Columbia River were initially at a pH of about 8„lo As the pH decreases, 
 zinc and cobalt are desorbed from these materials „ Desorption is report- 
 edly complete (16, 23) at pH 4 or less A „5N-HC1 solution, which has a 
 pH of about lo5 9 was therefore used to wash the plankton and bottom sedi- 
 ment samples o Five separate washings were considered to be quite adequate 
 to remove all of the zinc and cobalt which could be removed at this pH 
 The total contact time between the wash solution and the samples varied 
 from one to several hours „ 
 
 A 45 u membrane filter placed over a disc of fiberglass window 
 screening in a six-inch diameter Buchner funnel inserted in a vacuum 
 flask was used to separate the eluate and residue from acid washing of 
 samples of plankton and bottom sediments „ The filtering time varied with 
 the amount of clay sized particles in the bottom sediment samples „ The 
 vacuum in the flask was adjusted to provide a minimum contact time between 
 the wash solution and the sample of one hour 
 
 Countin g for To tal Gamma Activity 
 
 A NMC model GSS-1 Gamma-Scintillation Spectrometer with a two 
 inch by two inch cylindrical crystal of thallium activated sodium iodide 
 was used for all gamma count ing It was adjusted to 1000 volts spectral 
 energy and allowed to warm up for at least one hour before being usedo 
 At this spectral energy, a fairly flat plateau existed 9 so that the 
 voltage could vary slightly without markedly influencing the efficiency 
 of count ingo Five-minute counts of background radiation using a plastic 
 test tube containing 10 ml of deionized water as a blank were continued 
 until it was certain that the counter had stabilized „ Each sample was 
 counted several times, with the length of time for each count varying from 
 two to ten minutes, depending upon the activity of the sample,, Lower 
 
42 
 activities required longer counting times. Background was checked at 
 half -hour intervals or as often as necessary. Since the background for 
 this instrument was in the range of 250 to 350 cpm, it was more difficult 
 and time consuming to obtain reasonably precise results when the activity 
 of the sample was less than 100 cpm. All liquid samples were made up to 
 exactly 10 ml in volume and all solid samples to approximately this 
 volume o Tests using different volumes of tracer of known activity indi- 
 cated slight changes in counter efficiency as the volume was varied above 
 and below 10 ml, A volume of 10 ml was therefore used as a standard for 
 all counting work. Thin walled plastic test tubes were used throughout 
 the research as sample containers for gamma counting. 
 
 It was considered that the spectrometer might exhibit a different 
 efficiency when counting gamma scintillations emanating from a bottom sedi- 
 ment or solid sample instead of a liquid sample due to the greater density 
 of the solid, A known amount of tracer Zinc was placed on a 10 to 15 g 
 
 (10 ml volume) sample of sand which contained no other source of activity, 
 
 65 
 in a plastic test, tube. The same amount of tracer Zinc was placed in a 
 
 second test tube and the volume made up to 10 ml. The liquid in the test 
 
 tube containing the sand was allowed to evaporate and the two samples were 
 
 counted. The resulting counts indicated that the efficiency of the counter 
 
 was not measurably affected by replacing the liquid sample by a sand 
 
 sample , 
 
 PHASE II 
 
 At the beginning of Phase II, the eluates from each sample of 
 water, plankton or bottom sediments were in the same state and could hence- 
 forth be treated in a similar manner. Due to the vapor pressure system 
 for a mixture of HC1 and water, evaporation produces a final mixture that 
 
43 
 
 is 6N in HC1 Since all of the sample eluates were at least „5N in HC1 
 before evaporation was started, and were concentrated to about one-tenth 
 of the initial volume, it could be assumed that the normality approached 
 6N in HC1. 
 
 Since the concentrated eluates contained many elements, some of 
 which could possibly interfere with the analysis for total zinc or cobalt, 
 it was not expected that the results of these initial analyses would be as 
 precise as those made after the isolation of zinc and cobalt had been 
 completed. However, these initial values would indicate later whether 
 separation had been complete or only partial,, In the total cobalt analyses, 
 the concentration of cobalt was so low that many of these initial results 
 were in doubt It was quite apparent that interference had occurred in 
 some cases o 
 
 PHASE III 
 
 Separation and Isolation of Zinc and Cobalt by Anion Exchange 
 Chromatography 
 
 One of the objectives in this research was to make use only of 
 equipment that would be available to any laboratory having responsibility 
 for radiological health monitoring or control „ This equipment might 
 include a single-channel gamma-scintillation spectrometer but not an 
 expensive multi-channel instrument „ Therefore, in order to analyze 
 specific radionuclides, each radionuclide would have to be isolated „ Both 
 zinc and cobalt were isolated as a mixture of stable and radioactive iso- 
 topes of the particular element, and possibly including stable and radio- 
 active isotopes of certain other elements in minor quantities „ 
 
 c c. no 
 
 The element zinc has isotopes from Zn to Zn „ All of these 
 
 c c. 
 
 isotopes, with the exception of Zn with a half-life of 245 days, are 
 
44 
 either stable or have half -lives of two days or less The activity due to 
 
 radioactive zinc in the bottom sediments of the Columbia River could only 
 
 65 
 be due to the presence of the isotope Zn „ 
 
 51+ 64 
 Cobalt 8 which has isotopes from Co to Co , has the following 
 
 radioisotopes of interests Co with a half-life of 72 days; Co with a 
 
 half-life of 270 days; Co with a half-life of 72 days; and Co ' with a 
 
 half -life of 5„27 years „ Of these, only Cobalt has been found by the 
 
 Hanford staff in analyses of reactor effluent „ 
 
 Both zinc and cobalt 8 in ionic form, occur in the divalent state „ 
 This considerably simplifies isolation, as ion exchange chromatography is 
 very dependent on the valence of the ion 
 
 In order to determine the concentrations of radioactive zinc and 
 cobalt s it was necessary to consider what other radioactive elements might 
 be present o Radioactive elements in the Columbia River are from three 
 possible sources? from the reactor effluent 9 by irradiation; from fallout 9 
 by fission; and from natural background 9 through the three decay chains of 
 naturally occurring radioactive elements „ Of these three sources 9 the 
 reactor effluent source would predominate „ 
 
 A test was run in the laboratory using a sample of mixed fission 
 products to determine if these radionuclides would interfere with the 
 effectiveness of anion exchange chromatography for zinc and cobalt isola- 
 tion o The sample was made 12N in HC1 and passed through a Dowex 1 chloride 
 cycle anion exchange column „ The resin was rinsed by passing three addi- 
 tional resin volumes of 12N-HC1 through the column. At this point 9 
 96 o0 percent of the activity had been eluted The passage of three resin 
 volumes of 4N-HC1 and then chree resin volumes of 005N-HC1 failed to 
 elute any further activity,. From this test it was concluded that fission 
 product radionuclides present in the Columbia River due to fallout would 
 
45 
 
 not interfere with the separation scheme adopted „ 
 
 Table 5 1 lists the radionuclides presenx in the reactor effluent 
 as it enters the Columbia River 9 as stated by Hanford's Environmental 
 Studies and Evaluation staff (7)„ Table 5,2 lists the radionuclides 
 occurring in the three decay chains of naturally occurring radioactive 
 elements (9K Half-lives of each radionuclide have been included in these 
 tables „ In additions, the major gamma transitions of the radionuclides 
 having relatively long half-lives are given Half-lives and gamma transi- 
 tions are as listed in the Radiolog ical Health Handbook , 1957 (21)» 
 
 65 
 The major gamma transitions of Zn ' occur at .1.12 Mev and those 
 
 of Co occur at 1.17 and 1»33 Mev The efficiency of the gamma- 
 scintillation spectrometer decreases as the energy level of the gamma 
 transitions decreases „ It can therefore be assumed that trace elements 
 and background radiation due to naturally occurring radionuclides will not 
 cause significant interference if the energy level of the gamma transitions 
 is less than o 10 Mev„ All radionuclides having no gamma transitions can 9 
 of course 8 be neglected , The analyses for radioactive zinc and radioactive 
 cobalt were made several months after the samples were collected, thus any 
 activity exhibited by short-lived radionuclides would have disappeared., 
 Therefore s, all radionuclides having half=lives of less than a few days may 
 be neglected o The radionuclides of greatest significance are therefore 
 those having half-lives of more than a few days and also having gamma 
 transitions at an energy level greater than dO Mev as listed in Table 5 3„ 
 
 Figo 5 1 depicts the variation in adsorption coefficients for 
 various elements on Dowex 1 chloride cycle anion resin with concentration 
 of HClj as obtained by Kraus and Nelson (11)« If the sample is made 7N in 
 HC1 8 passed through the anion exchange column and thoroughly washed with 
 ten additional resin volumes of 7N-HC1 9 of the radionuclides listed in 
 
46 
 
 Table 5.1 
 
 RADIONUCLIDES PRESENT IN REACTOR EFFLUENT 
 AS IT ENTERS THE COLUMBIA RIVER 
 
 
 MAXTOR, 
 
 90^ 
 
 
 
 TRACE , 
 
 2* 
 
 Half- 
 
 
 Radio- 
 
 Half- 
 
 Gamma 
 
 Radio - 
 
 Half- 
 
 Gamma 
 
 Radio- 
 
 Gamma 
 
 nuclide 
 
 Life 
 
 Transi- 
 tions 
 
 nuclide 
 
 Life 
 
 Transi- 
 tions 
 
 nuclide 
 
 Life 
 
 Transi- 
 tions 
 
 
 15. lh 
 
 (Mev) 
 
 7 
 
 
 (Mev) 
 none 
 
 T 141 
 La 
 
 3,7h 
 
 (Mev) 
 
 T? 5 "" 
 
 12, 4y 
 
 _ 
 
 Si 31 
 
 2.62h 
 
 _ 
 
 c 1 " 
 
 5568y 
 
 none 
 
 Pr 1 * 2 
 
 19, 2h 
 
 _ 
 
 Cr 51 
 
 27.8d 
 
 .32 
 
 s 35 
 
 87. Id 
 
 none 
 
 Ce 1 " 3 
 
 34h 
 
 _ 
 
 u 56 
 
 Mn 
 
 2.58h 
 
 - 
 
 Oa" 
 
 152d 
 
 none 
 
 Pr 1 " 3 
 
 13, 7d 
 
 none 
 
 Cu 
 
 12.8h 
 
 - 
 
 So* 6 
 
 85d 
 
 ,89, 1.12 
 
 to"* 
 
 282d 
 
 .03-2,18 
 
 a 76 
 
 As 
 
 26.8h 
 
 _ 
 
 So" 
 
 3.43d 
 
 _ 
 
 Pr 
 
 17.5m 
 
 ^ 
 
 Np 239 
 
 2.3d 
 
 .01-. 33 
 
 Mn 5 " 
 
 310d 
 
 .84 
 
 Pr 145 
 
 4.5h 
 
 - 
 
 
 
 
 Fe 59 
 Co 60 
 Sr 85 
 
 45. Id 
 
 1.29, 1.10 
 
 Nd 147 
 
 D 147 
 Pm 
 
 149 
 Nd 
 
 11,3d 
 
 ,09~„53 
 
 
 MINOR, 
 
 8% 
 
 5.27y 
 65d 
 
 JLoOOo Xo X / 
 
 .51 
 
 2,6y 
 2, Oh 
 
 none 
 
 p 32 
 
 14.3d 
 
 none 
 
 • 
 
 Zn 65 
 
 245d 
 
 1.12 
 
 Sr 90 
 
 19. 9y 
 
 none 
 
 D 149 
 
 Pm 
 
 54h 
 
 aa 
 
 Zn 69 
 
 57m 
 
 _ 
 
 T 91 
 
 61d 
 
 1.2, .2 
 
 D 151 
 
 Pm 
 
 27, 5h 
 
 == 
 
 Ga 72 
 
 14. 3h 
 
 _ 
 
 Zr 95 
 
 65d 
 
 .73, .92 
 
 Eu 152 
 
 13y 
 
 ,12-1,09 
 
 Y 90 
 
 61h 
 
 m. 
 
 Mo 
 
 67h 
 
 = 
 
 Sm 153 
 
 47h 
 
 CO 
 
 Sr 91 
 
 9.7h 
 
 en, 
 
 . 103 
 Ru 
 
 40d 
 
 .50 
 
 _ 156 
 Eu 
 
 15,4d 
 
 2.0 
 
 Sr 92 
 
 2.7h 
 
 - 
 
 Ag 111 
 
 7„6d 
 
 .24, .34 
 
 e 156 
 Sm 
 
 lOh 
 
 « 
 
 92 
 Y^ 
 
 3.6h 
 
 =, 
 
 Cd 115 
 
 53h 
 
 _ 
 
 Eu 157 
 
 15, 4h 
 
 Mi 
 
 93 
 Y 
 
 10 .Oh 
 
 • 
 
 I 131 
 
 8„I4d 
 
 .08=. 36 
 
 Tb 16 ° 
 
 74d 
 
 .96-. 09 
 
 97 
 Nb 
 
 72m 
 
 _ 
 
 132 
 
 2.4h 
 
 _ 
 
 w 187 
 
 24,lh 
 
 — 
 
 133 
 
 2 Oh 
 
 „ 
 
 Cs 137 
 
 33y 
 
 .66 
 
 Po 210 
 
 138d 
 
 ,80 
 
 j.135 
 
 6.7h 
 
 _ 
 
 Pa 1 " 
 
 12. 8d 
 
 ,03-. 54 
 
 a 227 
 
 Ac 
 
 22y 
 
 ,04 
 
 u 239 
 
 23.5m 
 
 - 
 
 . 140 
 La 
 
 40h 
 
 m. 
 
 238 
 
 U 
 
 4x10 y 
 
 ,05 
 
 
 
 
 « 141 
 
 Ce 
 
 33d 
 
 ,14 
 
 D 239 
 
 Pu 
 
 2x10% 
 
 .04-. 38 
 
47 
 
 Table 5,2 
 
 NATURALLY OCCURRING RADIONUCLIDES 
 
 UR£ 
 
 >NIUM SERIES 
 Half- Gamma 
 
 THORIUM SERIES 
 Radio- Half- Gamma 
 
 ACTINIUM SERIES 
 
 Radio- 
 
 Radio- 
 
 Half- 
 
 Gamma 
 
 nuclide 
 
 Life 
 
 Transi- 
 tions 
 
 nuclide 
 
 Life 
 
 Transi- 
 tions 
 
 nuclide 
 
 Life 
 
 Transi- 
 tions 
 
 
 4,19m 
 
 (Mev) 
 
 ^208- 
 
 
 (Mev) 
 
 
 
 (Mev) 
 
 T1 206 
 
 3.1m 
 
 T1 207 
 
 4.79m 
 
 a. 
 
 T1 210 
 
 l 32m 
 
 _ 
 
 Pb 2 " 
 
 10. 6h 
 
 _ 
 
 Pb 211 
 
 36.1m 
 
 _ 
 
 Pb 210 
 
 22y 
 
 .05 
 
 Bi 212 
 
 60.5m 
 
 _ 
 
 Bi 211 
 
 2.2m 
 
 B 
 
 Bi 21C 
 
 5.0d 
 
 none 
 
 Po 212 
 
 10~ 7 s 
 
 _ 
 
 Po 211 
 
 .5s 
 
 _ 
 
 Po 210 
 
 138d 
 
 .80 
 
 Po 216 
 
 .16s 
 
 _ 
 
 Bi 215 
 
 8m 
 
 _ 
 
 Pb 21 " 
 
 26o8m 
 
 _ 
 
 At 216 
 
 _4 
 10 s 
 
 _ 
 
 Po 215 
 
 10" 3 s 
 
 _ 
 
 Bi 2W 
 
 19o7m 
 
 a. 
 
 En, 220 
 
 54s 
 
 _ 
 
 At 215 
 
 10" 4 s 
 
 ^ 
 
 _ 21t 
 Po 
 
 10" 4 s 
 
 _ 
 
 Ra 22 * 
 
 3„64d 
 
 _ 
 
 At 219 
 
 .9m 
 
 _ 
 
 Po 218 
 
 3o05m 
 
 _ 
 
 Ra 228 
 
 6.7y 
 
 .03 
 
 Em 219 
 
 3.9s 
 
 ,„ 
 
 At 218 
 
 2s 
 
 _ 
 
 Ac 228 
 
 6.13h 
 
 <_ 
 
 Fr 223 
 
 21m 
 
 = 
 
 Em 222 
 
 3.82d 
 
 • 
 
 Th 228 
 
 1.90y 
 
 .08 
 
 Ra 223 
 
 11, 2d 
 
 .14-. 34 
 
 Ra 226 
 
 1622y 
 
 .19 
 
 Th 232 
 
 lxl0 10 y 
 
 .05, .07 
 
 A 227 
 
 Ac 
 
 22. Oy 
 
 .04 
 
 Th 23 ° 
 
 8x10% 
 
 .07 
 
 
 
 
 227 
 Th 
 
 18„6d 
 
 .05-. 28 
 
 Th 234 
 
 24. Id 
 
 .09 
 
 
 
 
 Th 231 
 
 25. 6h 
 
 ^ 
 
 Pa 234 
 
 1.2m 
 
 — 
 
 
 
 
 Pa 231 
 
 3xl0 4 y 
 
 .03-, 38 
 
 u 234 
 
 2xl0 5 y 
 
 .05-.12 
 
 
 
 
 u 235 
 
 7x1 8 y 
 
 .09-. 39 
 
 u 238 
 
 4xl0 9 y 
 
 .05 
 
 
 
 
 
 
 
48 
 
 Table 5.3 
 
 SIGNIFICANT RADIONUCLIDES 
 
 Description 
 
 MAJOR 
 
 Radionuclide 
 
 Cr 
 Np 
 
 51 
 239 
 
 Half-Life 
 
 27o8d 
 2.3d 
 
 Gamma Transitions 
 (Mev) 
 
 .32 
 
 .01-. 33 
 
 MINOR 
 
 Zn 
 
 65 
 
 245d 
 
 1.12 
 
 TRACE 
 
 NATURALLY 
 OCCURRING 
 
 Sc 
 Mn 
 Fe 
 Co 
 
 46 
 54 
 59 
 
 60 
 
 Sr 
 „91 
 
 85 
 
 Zr 
 Ru 
 
 95 
 103 
 
 111 
 
 Ag 
 ,131 
 
 Cs 
 Ba 
 Ce 
 Ce 
 Nd 
 Eu 
 Eu 
 Tb 
 Po 
 Pu 
 
 137 
 140 
 141 
 144 
 147 
 152 
 156 
 160 
 210 
 239 
 
 Ra 
 Ra 
 
 Th 
 
 223 
 226 
 227 
 
 231 
 
 Pa 
 
 u 234 
 
 u 
 
 235 
 
 85d 
 
 310d 
 
 45. Id 
 
 5.27y 
 
 65d 
 
 61d 
 
 65d 
 
 40d 
 
 7.6d 
 
 8.14d 
 
 33y 
 
 12. 8d 
 
 33d 
 
 282d 
 
 11. 3d 
 
 13y 
 
 15. nd 
 
 74d 
 
 138.3d 
 
 24,300y 
 
 11. 2d 
 
 1622y 
 
 18. 6d 
 
 3.43x10% 
 
 2.48xl0 5 y 
 
 7.13xl0 8 y 
 
 «B9 j 
 
 1,12 
 
 .84 
 
 
 1.29 
 
 , 1.10 
 
 1.33 
 
 , 1.17 
 
 .51 
 
 
 1.2, 
 
 .2 
 
 .73, 
 
 .92 
 
 .50 
 
 
 .24, 
 
 .34 
 
 .08- 
 
 .36 
 
 .66 
 
 
 .03- 
 
 .54 
 
 .14 
 
 
 .03- 
 
 2.18 
 
 .09- 
 
 .53 
 
 .12-. 
 
 L.09 
 
 2.0 
 
 
 .96- 
 
 .09 
 
 .80 
 
 
 .04- 
 
 .38 
 
 .14- 
 
 a 34 
 
 .19 
 
 
 .05- 
 
 ,28 
 
 .03- 
 
 .38 
 
 .05- 
 
 ,12 
 
 ,09- 
 
 ,39 
 
— 1 — 
 
 i 
 
 — I- 
 
 — i — 
 
 1 
 
 — i — 
 
 1 
 
 i 
 
 1 
 
 — 1 — 
 
 — i — 
 
 — 1 — 
 / 
 
 — 1 — 
 
 — 1 — 
 
 1 
 
 
 H 
 
 - 
 
 
 - 
 
 O 
 
 l. 
 
 
 
 - 
 
 - 
 
 
 l& } 
 
 - 
 
 
 1-1/ - 
 / 
 
 - 
 
 
 - 
 
 
 LL. 
 
 
 , - 
 
 
 
 , - 
 
 CD 
 
 1 
 
 i 
 
 J- 
 
 1— 1 
 
 1 
 
 i -» 
 
 
 < 
 
 
 ! " 
 
 
 — 1 — 
 
 
 1 - 
 
 — 1 — 
 
 
 ' - 
 
 — 1 — 
 
 — i — 
 
 1 — 
 
 — 1 — 
 
 — 1—7 
 
 CO 
 
 ' - 
 
 1 
 
 1 J 1 
 
 CO 
 
 
 - 
 
 
 - 
 
 - 
 
 
 - 
 
 - 
 
 
 N N > 
 
 A 
 
 
 in 
 
 - 
 
 
 ^° 
 
 - 
 
 
 J3_ 
 
 
 - 
 
 -co 
 
 i 
 
 
 - 
 
 co 
 
 i 
 
 W 
 
 ' 
 
 V 
 
 1 
 
 - 
 
 
 
 1 
 
 (/ 
 
 1 
 
 
 1 
 
 
 ' - 
 
 , .,_ 
 
 
 - 
 
 — i — 
 
 i 
 
 l w 
 
 -p " 
 
 I 
 
 /' - 
 
 ..,_, 
 
 ' 
 
 /'" 
 
 
 - 
 
 
 - 
 
 - 
 
 
 - 
 
 
 
 B\ 
 
 
 
 - 
 
 
 ^ 
 
 r 
 
 
 ^_ 
 
 
 - 
 
 0_ 
 
 
 - 
 
 < 
 
 i 
 
 j 
 
 1 
 
 CO, N^ 
 
 
 5 , • 
 
 ^_ 
 
 ' 
 
 
 ■ '1 ■ 
 
 
 1 - 
 
 — i — 
 
 
 - 
 
 i 
 
 
 1 
 
 ■H 
 
 b 
 
 /'- 
 
 ■ ! 
 
 
 1 — 
 
 
 - 
 
 
 - 
 
 co 
 
 i 
 
 
 
 - 
 
 - 
 
 M 
 
 V 
 
 . fH 
 
 r 
 
 
 
 
 
 i3_ 
 
 
 , - 
 
 
 
 , - 
 
 
 i 
 
 ■ 
 
 CO 
 
 V 
 
 
 a. 
 
 1 
 
 , < 
 
 2 
 
 . ' 
 
 
 1 - 
 
 T 
 
 CO 
 
 ' - 
 
 i j 
 
 — i — 
 
 T — 
 
 — 1 — 
 
 1 
 
 7- 
 
 M 
 
 / 
 
 — l — 
 to " 
 
 h-t 
 CO 
 
 u 
 
 2 H 
 
 O »— ' 
 
 - 
 
 
 - 
 
 - 
 
 
 H O- 
 
 c 
 
 - 
 
 ° 1= 
 
 i 
 
 
 - 
 
 - 
 
 
 N /' 
 
 f=l 
 
 ' HH 
 
 - 
 
 H_ 
 
 ' 
 
 1 
 
 < 
 
 i 
 
 i 
 
 i 
 
 c 
 
 t-H 
 
 1 
 
 k 
 
 ^ 
 
 , 
 
 <o _ 
 
 1 
 
 
 """ o 
 
 X 
 
 1- 
 
 _J 
 o 
 
 1 
 
 i 
 
 -"/ 
 
 /'" 
 
 — 1 — 
 
 "~T 
 
 
 / 
 
 V 
 
 / 
 
 / ' - 
 
 2 Q 
 
 
 - 
 
 
 - 
 
 ^ 
 
 
 - 
 
 y 
 
 
 < M 
 
 
 N 
 
 c 
 
 -^J- 
 
 o 
 
 1 
 
 ( 
 
 
 *J 
 
 / 
 
 1 
 
 HH < 
 
 
 — i — 
 
 1 
 
 / 
 
 " 1 
 
 1 
 
 1 - 
 
 - 1 
 
 
 1 
 
 X 
 
 U l-H 
 
 S pi 
 
 C\J _ 
 
 - 
 
 l-H 
 
 A 
 
 - 
 
 l-H • " 
 
 
 - 
 
 
 
 5g ,. 
 
 3 
 
 , 
 
 f & 
 
 «. 
 
 
 ^ - 
 
 73 
 
 
 - 
 
 X 
 
 
 
 
 
 
 
 
 
 
 
 £^ A 
 
 l 
 
 1 ', 1 
 CO 
 
 1 
 
 1 
 
 /'- 
 
 1 
 
 J 
 
 
 
 
 ^ S! o* 
 
 - 
 
 « c 
 
 > 
 > — 
 
 - 
 
 s 
 
 / - 
 
 - 
 
 w 
 
 - 
 
 CO Q 
 
 v z 
 
 Z- 
 
 c 
 
 
 / 
 
 1 
 
 
 0. 
 
 7^ 
 
 - 
 
 2 X 
 U 
 
 s: tu 
 w 
 J 
 
 ° 2 z 
 o 2 
 
 — I — 
 
 — 1 — 
 
 r 
 
 1 
 
 I 
 a 
 
 c 
 
 
 - 
 
 — 1 — 
 
 J 
 
 ■ 1 
 
 - 
 
 1=1 \ 
 
 
 
 ^ 
 
 
 7 
 
 y 
 
 u co 
 2 
 
 r- ~ O 
 
 o 
 
 
 
 CO 
 
 "i 
 
 / 
 
 u 
 
 X M 
 
 0- en- £ 
 
 
 
 
 
 
 
 
 
 
 E- E- 
 < 
 
 u. a: 
 
 O E-" 
 
 2 
 
 CO u 
 E- O 
 
 ._ J, . 
 
 1 
 
 «\- 
 
 i 
 
 1 
 
 a / 
 
 /'- 
 
 1 
 
 d'l 
 
 1 
 
 ADSO 
 
 LIGHT A 
 0.3 < D < 
 
 TRONG A 
 
 t 
 
 i*Ss 
 
 3 - 
 
 
 ' - 
 
 - 
 
 7 
 
 - 
 
 
 3 ^ 
 
 1 
 
 
 
 
 CO 
 
 /, 
 
 
 
 
 
 
 
 
 
 
 
 1 
 
 1 
 
 W 
 
 1 
 
 I 
 
 1 
 
 - 
 
 1 
 
 1 
 
 ;- 
 
 
 2 2 
 
 M O 
 
 ^- co_ to 
 ■ i i 
 
 c — 
 
 
 - 
 
 P," 
 
 £ 
 
 / 
 
 - 
 
 °1 
 
 -> 
 
 / - 
 
 CJ 
 
 
 1 
 
 ■ 
 
 J 
 
 / 
 
 , - 
 
 1 
 
 
 U-, 2 
 Lm 1— 1 
 U >-" 
 O CC 
 
 ■o -o -o 
 
 O O o 
 
 1 1 .' 
 CO 
 
 - 1 ■ 
 
 co - 
 ■D — 
 O . 
 
 to - 
 
 i 
 
 — I - 
 
 1 r- 
 
 — r - 
 
 
 ■ -r— 
 
 - 
 
 IS 
 
 — 1 — 
 
 o _• iz 
 
 C to CO 
 
 - 1=1 
 
 CO 
 
 1 
 
 o — 
 
 Hi 
 
 . 
 
 - 
 
 ^ 
 
 \ - 
 
 - 
 
 1 
 
 % 
 
 CJ < 
 
 
 & 
 
 1 
 
 Vi 
 
 5, 
 
 
 ' 
 
 =>, 
 
 2 
 
 O X 
 
 
 — 1 — 
 
 co^ 
 -a — 
 o 
 
 — r™ 
 
 — 1 — 
 
 !-■ 
 
 1 - 
 
 — 1 — 
 
 — r— v — 1 — 
 
 1 
 
 V 
 
 
 M E- 
 E-. t-i 
 
 » 
 
 O 
 CO 
 Q 
 
 
 N . 
 
 J3 — 
 
 
 \ 
 
 - 
 
 ) 
 
 — 
 
 a. 
 
 1 
 
 X; 
 
 
 
 > 
 
 CO 
 
 1 
 
 i 
 
 /, - 
 
 h 
 
 
 / 
 
 
 
 1 1 l 
 
 gig!-- 
 
 LlJ < Q K 
 
 _i c <r> 
 w 1 o 
 
 1 1 
 
 1 
 
 ... r 
 
 ,. ,. . 
 
 CO 
 
 L TJ - 
 
 i ° 
 
 -&: 
 
 
 
 
 ' - 
 
 — j— 
 
 M 
 
 — 1 — 
 
 1 
 
 1 1 1 
 to 
 
 HI- 
 
 c 
 
 < 
 
 
 
 M 
 
 
 ^ 
 
 - 
 
 M 
 
 - 
 
 h 
 
 
 
 
 _M 
 
 
 
 - 
 
 - 
 
 X 
 
 
 
 
 
 1 
 
 
 
 
 
 
 
 
 
 
 
 
 i 
 
 CO 
 
 - 
 
 -0 
 
 
 
 
 c 
 1 
 
 
 - 
 
 
 CO 
 
 1 
 
 to 
 
 
 
 10 
 
 <J- C\J 
 
 o — 
 CO 
 
 
 3 
 
 - 
 
 
 - 
 
 - 
 
 5 
 
 O 
 
 O — 
 
 c 
 > 
 
 — 
 
 
 
 
 
 a "ddaoo 'disia oo 
 
 
 
 >- 
 
 
 - 
 
 UJ 
 DC 
 
 
 
 
 c 
 I 
 
 
 
 — i — 
 
 — 1— 
 
 CO 
 
 — r— 
 
 1 
 
 — 1 — 
 
 CO 
 
 ' - 
 
 ■■-i ■ 
 
 CO 
 
 — 1 — 
 
 - ' 
 
 O 
 
 O 
 
 c 
 
 
 1 - 
 
 1 
 
 CO 
 
 "O — 
 
 
 
 1 
 
 1 
 
 — 1 — 
 
 CO 
 
 
 
 CD 
 
 o 
 
 o ■ 
 
 c 
 1 
 
 
 ■ 
 
 "O 
 
 o 
 
 - 
 
 2._ 
 
 O 
 
 - 
 
 - 
 
 
 - 
 
 O 
 
 CD, 
 
 - 
 
 — 
 
 a 
 
 
 
 i 
 
 o 
 
 c 
 
 1 
 
 O 
 
 c 
 1 
 
 I 
 
 CO 
 
 
 - 
 
 c 
 
 1 
 
 
 
 c 
 1 
 
 
 m 
 
 m 
 
 •H 
 
 U, 
 
 
 — i — 
 
 — 1 — 
 
 CO 
 
 1 
 
 —\ — 
 
 — i — 
 
 CO 
 
 ■ 'I 
 
 — i — 
 
 — T 
 
 <o 
 
 ' - 
 
 — 1 — 
 
 ■ I 
 
 to 
 
 TO 
 O 
 
 O 
 
 c 
 
 
 ' - 
 
 — 1 — 
 
 CO 
 
 T3 — 
 O 
 
 O 
 
 C 
 
 — 1 — 
 
 ■ 1— 
 
 co 
 
 
 
 - 
 
 o 
 
 - 
 
 - 
 
 O 
 
 - 
 
 - 
 
 o 
 
 - 
 
 jQ 
 
 
 - 
 
 - 
 
 - 
 
 - 
 
 O 
 
 
 
 '3 
 
 c 
 1 
 
 , " 
 
 o 
 
 
 o 
 
 c 
 
 ' 
 
 *: 
 
 c 
 1 
 
 I 
 
 
 - 
 
 CO 
 
 1 
 
 
 c 
 
 1 1 
 
 , - 
 
 
 49 
 
50 
 
 54 „ 59 rj . , ^ „ 85 v 91 ^95 .. 137 _ 140 . 141 
 Table 5,3 , Mn , Fe (divalent ) 8 Sr , Y s Zr , Cs , Ba , Ce , 
 
 <*"*. Nd 1 " 7 , Eu 152 . Eu 156 , Tb i60 , Ra 223 . Ra 226 , and Th 227 pass through 
 
 the resin and are separated from the remaining radionuclides. The radio- 
 
 46 51 59 
 nuclides retained on the anion resin are Sc , Cr , Fe (trivalent) g 
 
 60 65 „ 103 , 111 T 131 n 210 _ 231 ..234 T ,235 „ 239 . _ 239 
 Co , Zn , Ru , Ag ,1 , Po , Pa 8 U , U 9 Np and Pu 
 
 Of these j, Sc is slightly adsorbed at all normalities of HC1, Cr in the 
 
 trivalent state is slightly adsorbed at all normalities of HC1 and strongly 
 
 210 . 
 adsorbed at all normalities if in the hexavalent state, and Po is 
 
 strongly adsorbed at all normalities of HC1„ As the normality of HC1 is 
 
 decreased to zero, the adsorption coefficients increase for the radio- 
 
 103 111 13 1 
 nuclides Ru , Ag and I -„ The normality of the HC1 may therefore be 
 
 adjusted between 7N and ON without eluting any of these radionuclides. It 
 
 should be noted that the adsorption curve for ruthenium, shown in Fig, 5,1, 
 
 has not been extended below 2N in HC1, so it is possible that this element 
 
 could be eluted with very dilute HC1, The remaining radionuclides are now 
 
 r- 59 /4. • i «.* n 60 n 65 _ 231 ..234 235 M 239 , _ 239 
 Fe (trivalent), Co , Zn , Pa , U , U , Np and Pu 
 
 At this point an eiution scheme was formulated. The sample was first 
 
 passed through the resin in 7N-HC1 and, secondly, washed with ten resin 
 
 volumes of 7N-HC1, Tests with tracer Cobalt under these conditions 
 
 indicated that cobalt is adsorbed and held on the resin without leakage. 
 
 As can be seen from Fig 5,1, cobalt might have leaked out of the resin in 
 
 a 7N-HC1 environment, but no leakage was observed with the passage of up 
 
 to ten resin volumes of wash 7N-HC1, Further tests indicated that the 
 
 eiution of cobalt was rapid and complete using 4N-HC1,- Still further tests 
 
 59 
 showed that tracer Fe ' was rapidly and completely eluted using 5N-HC1 
 
 but that no leakage occurred at 4N in HC1, Therefore the third step in 
 
 the process was to elute the cobalt with the passage of ten resin volumes 
 
 of 4N-HC1, Other tests indicated that the eiution of zinc was rapid and 
 
51 
 complete using uOlN-HCl and that no zinc leakage occurred using 5N=HC1 
 Therefore the fourth step in the separation was to elute the trivalent 
 iron s if any were presents, by the passage of ten resin volumes of „5N-HC1<, 
 The fifth and final step was to elute the zinc fraction with the passage 
 
 of ten resin volumes of o 01N-=HCl o 
 
 231 234 235 
 This procedure may. not separate the radionuclides Pa 9 U ' , U , 
 
 23q 239 231 
 Np * * 8 and Pu ' „ Pa , if presents would likely have been eluted with 
 
 the Fe . U and U , if presents, would have been eluted with the Co 
 
 59 
 if in the tetravalent state, or with the Fe ' if in the hexavalent state „ 
 
 239 239 
 The adsorption coefficients for Np and Pu were not known „ 
 
 The process of establishing a procedure for anion exchange chroma- 
 tography was time consuming, but the procedure, once established, was 
 quite simple and rapid „ 
 
 The flow rate of approximately „2 ml/sq cm/min was suggested by Kraus 
 and Nelson (11) 
 
 PHASE IV 
 
 Analysis for Total Zinc 
 
 The procedure for the analysis of total zinc was adapted from 
 the method called the "Mixed-Color Method," found on pages 265 to 268 of 
 the 11th edition of Standard Methods for_ the_Examination of Wat er and 
 Wastewat er ( 1 ) „ 
 
 Dithizone (diphenylthiocarbazone) forms complexes with nearly 
 twenty metals By selecting a specific set of conditions, it can be made 
 to react with only zinc However, if greater than moderate amounts of 
 interfering metals are present s some color interference may occur „ In the 
 initial zinc determinations made in Phase II of the procedure, the samples 
 might well have contained more than moderate amounts of interfering metals „ 
 
52 
 
 The results of these initial analyses can therefore not be considered to 
 
 be too reliable o Once the zinc fraction had been isolated 9 the possible 
 
 presence of minute quantities of other elements should not interfere with 
 
 the total zinc determination » 
 
 As discussed in Standar d Methods 9 the reaction between zinc and 
 
 dithizone is demonstrably slow and incomplete <, Using the single extraction 
 
 procedure advocated 9 the quantitative determination of zinc is to some 
 
 extent empirical 9 and it is necessary to carefully adhere to the prescribed 
 
 conditions o The duration and vigor of shaking 9 the volumes of sample 8 
 
 thiosulfate and dithizone, and the pH should all be kept constant In the 
 
 t 
 
 procedure adopted for this research 9 some of these sources of error were 
 eliminated, simply by replacing the single extraction procedure with a 
 triple extraction procedure „ 
 
 The initial pH of each sample was checked and adjusted to a neutral 
 value o A constant volume of thiosulfate was added to each sample „ The 
 triple extraction procedure eliminated the need to shake with constant 
 vigor for a constant period „ If the sample was within the range of allowable 
 concentrations, that is, between 1 and 15 yg 9 then the first extraction would 
 be from blue to pink in color,, The second extraction would be from green to 
 blue 9 indicating that it contained between and, perhaps, 3 yg of zinc 
 The third extraction was green and the cclor could not be distinguished 
 from that of the reference blank The addition of dithizone II to bring 
 the extracted volume to a constant value of 25 ml did not, therefore, cause 
 any inherent lack of precision in the procedure, and eliminated the need 
 for precise pipeting of dithizone during each extraction step Since 
 dithizone has a carbon tetrachloride base, and is thus quite volatile, 
 precise pipeting of this liquid is difficult „ 
 
 A Beckman DU model 24-00 Spectrophotometer with 10 mm rectangular 
 
53 
 
 glass absorption cells was used for the colorimetnc determination of the 
 concentration of zinc in each sample <> The wavelength used, 510 my, was 
 established by plotting percent transmittance against wavelength for various 
 concentrations of zinc in dithizone, using a pure CCl^ reference blank. Two 
 peaks were produced, one at 510 my, due to the green color of pure dithizonej 
 and another peak at about 580 my, due to the red color of the dithizone-zinc 
 complex o As the concentration of zinc was increased, the 510 my peak 
 diminished and the 580 my peak increased „ As the concentration of zinc 
 increased, the precision of detection decreased „ A spectrophotometer slit 
 opening of „ 5 mm allowed adequate sensitivity over the range from to 15 yg 
 of zinc in a 25 ml volume of dithizone „ 
 
 A series of ten sets of tests, using concentrations of 1, 2, 3, 
 4, 5, 7, and 10 yg of zinc per 25 ml volume of dithizone, were made The 
 results at each concentration level were averaged and a straight line 
 equation of absorbance (negative logarithm of percent transmittance) 
 against zinc concentration was produced, using the Method of Least Squares 
 The resulting equation of best fit was; 
 
 „, _ , » Absorbance = 001 
 Zinc Concentration (yg) = ohb ' i ' ' 
 
 Table 5 4 contains the 53 test results used for establishing the 
 standard curve or equation of best fit for total zinc determinations „ In 
 Table 5-5, the absorbance at each zinc concentration level has been calcu- 
 lated, using the equation of best fito The range in test results, presented 
 in Table 5,5, indicates the precision of the analytical technique „ In the 
 equation of best fit, an error of * o 004 units of absorbance results in an 
 error of *„1 yg of zinc Of the 53 test results shown in Table 5oU, only 
 one is not within ±,,020 units of absorbance, or * 5 yg of zinc, indicating 
 
54 
 
 Table 
 
 5.4 
 
 TE 
 
 ST RESULT 
 
 S USE 
 
 ;d for e 
 
 STABLISH 
 
 ING T? 
 
 IE STANI 
 
 )ARD 
 
 
 
 
 
 
 CURVE 
 
 FOR 
 
 TOTAL ZINC DETERMINATION 
 
 
 
 
 ZINCo 
 
 
 
 
 
 ABSORBANCE 
 
 
 
 
 
 
 CONCo 
 
 Set 
 
 Set 
 
 Set 
 
 Set 
 
 Set 
 
 Set 
 
 Set 
 
 Set 
 
 Set 
 
 Set 
 
 AVE. 
 
 (wg) 
 
 #1 
 
 J2_ 
 
 #3 
 
 J4 
 
 J.5 
 
 Jj_ 
 
 #7 
 
 J8 
 
 #9 
 
 flO 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 1 
 
 c035 
 
 .036 
 
 .040 
 
 .034 
 
 .035 
 
 - 
 
 - 
 
 - 
 
 .039 
 
 .041 
 
 .037 
 
 2 
 
 - 
 
 - 
 
 .082 
 
 .080 
 
 .083 
 
 .082 
 
 _ 
 
 - 
 
 - 
 
 - 
 
 .082 
 
 3 
 
 „125 
 
 .118 
 
 .125 
 
 .121 
 
 .130 
 
 =. 
 
 - 
 
 - 
 
 .132 
 
 . 
 
 .125 
 
 4 
 
 ol78 
 
 .177 
 
 .174 
 
 .153 
 
 .155 
 
 .163 
 .161 
 
 " 
 
 — 
 
 ~ 
 
 =, 
 
 .166 
 
 5 
 
 o212 
 
 .220 
 
 .203 
 
 - 
 
 .215 
 
 .225 
 
 - 
 
 - 
 
 .202 
 
 .209 
 
 .212 
 
 7 
 
 *■ 
 
 ™ 
 
 — 
 
 " 
 
 _ 
 
 •■ 
 
 .292 
 .280 
 
 .288 
 .278 
 
 .277 
 
 ,297 
 
 .285 
 
 10 
 
 
 
 
 
 
 
 .412 
 
 .398 
 .423 
 .398 
 
 .387 
 
 .419 
 
 .406 
 
 Table .5. 5 RANGE IN TEST RESULTS USED FOR 
 ESTABLISHING THE STANDARD CURVE 
 FOR TOTAL ZINC DETERMINATION 
 
 ZINC 
 
 CONC, 
 
 (Mg) 
 
 1 
 2 
 3 
 4 
 5 
 7 
 10 
 
 "ABSORBANCE^ 
 
 .042 
 .083 
 .124 
 165 
 .206 
 .287 
 .410 
 
 RANGE 
 IN TEST 
 RESULTS 
 
 (yg) 
 
 s.008 
 *.003 
 *.008 
 ±.013 
 *„019 
 *.010 
 *.023 
 
 ^Computed from least squares equation 
 
55 
 that there is a 98 percent probability that any s~.»gle analysis for total 
 zinc will be within ^5 yg of the true value The standard deviation for 
 any single analysis is ± o 0072 units of absorbance, or ^0 189 yg of zinc, 
 using the equation of best fito 
 
 Further tests for total zinc at concentrations up to 15 yg 
 indicated that the equation of best fit was still satisfactory at this 
 concentration of zinc in 25 ml of dithizone 
 
 The procedure for the determination of total zinc has an out- 
 standing advantage in that contamination of glassware and reagents can 
 readily be detected from the dithizone color change when washed with a few 
 ml of dithizone II solution,, An excellent evaluation of procedures for 
 the determination of zinc in natural waters is presented by O'Connor and 
 Renn (1963) (17) 
 
 Analysis for Total Cobalt 
 
 The procedure used for the analysis of total cobalt was adapted 
 from the method called "Procedure B (Citrate=Phosphate=Borate Medium)" on 
 pages 415 to 420 of Colorim etrie Determination o f Traces of Me tals B by 
 Eo Bo Sandell (1959) (24). 
 
 The procedure developed for the analysis of total cobalt was in 
 many ways similar to that used for total zinc Beth procedures are colori- 
 metrie o The same spectrophotometer and cells were usedo The wavelength 
 of 500 my was adopted from Sandell 6 but other spectrophotometer settings 
 were established using a procedure similar to that used for zinc 
 
 A series of three sets of tests 8 using concentrations of 5, 10 9 
 15, 20, 25 j 30 9 35, 40 B 45 and 50 yg of cobalt per 25 ml volume of solution 
 were made The scatter of values for concentrations greater than 35 yg 
 indicated that the test was reasonably precise within the range from to 
 
56 
 
 35 ug of cobalt per 25 ml of solution,, The resulxs, at each concentration 
 level within this range were averaged and a straight line equation of 
 absorbance against total cobalt concentration was computed, using the 
 Method of Least Squares , The resulting equation of best fit wass 
 
 „ , , ^. / x Absorbance - ,004 
 Cobalt Concentration (ug) = 00 92 9 6 "" " 
 
 Table 5,6 contains the 24 test results used for establishing the 
 standard curve or equation of best fit for total cobalt determinations , 
 In Table 5,7, the absorbance at each cobalt concentration level has been 
 calculated 8 using the equation of best fit. The range in test results, 
 presented in Table 5,7, indicates the precision of the analytical technique 
 In the equation of best fit, an error of *,009 units of absorbance results 
 in an error of *l o ug of cobalt , Of the 24 test results shown in Table 5,6, 
 only one is not within ± o 014 units of absorbance, or *1,6 ug of cobalt, 
 indicating that there is a 96 percent probability that any single analysis 
 for total cobalt will be within *1,6 ug of the true value. The standard 
 deviation for any single analysis is *„ 00602 units of absorbance, or 
 *,648 ug of cobalt, using the equation of best fit. 
 
 Determinat ion of Rad ioac tive Zinc and Radi oactive Co balt 
 The same procedure used for counting total gamma activities was 
 used for counting zinc and cobalt activities. In order to convert the 
 results for zinc and cobalt activities from cpm to pc/g, the counting effi- 
 ciency of the gamma scintillation counter had to be established, 
 
 65 
 A liquid Zinc ' standard was obtained from the United States 
 
 Department of Commerces, National Bureau of Standards, The National Bureau 
 
 of Standards had assayed the Zinc standard and found that it contained an 
 
57 
 
 Table 5,6 TEST RESULTS USED FOR ESTABLISHING 
 THE STANDARD CURVE FOR TOTAL COBALT 
 DETERMINATION 
 
 COBALT 
 
 
 ABSORBANCE 
 
 Set 
 
 AVE 
 
 CONCo 
 
 Set 
 
 Set 
 
 
 (yg) 
 
 #1 
 
 #2_ 
 
 #2 
 
 ^ ^ ^ ^ 
 
 
 
 
 
 
 
 
 
 
 
 5 
 
 ,046 
 
 ,048 
 
 O 053 
 
 ,049 
 
 10 
 
 O 098 
 
 olOO 
 
 ,104 
 
 ,101 
 
 15 
 
 ,147 
 
 ol57 
 
 ,155 
 
 ,153 
 
 20 
 
 .188 
 
 ,194 
 
 186 
 
 ,189 
 
 25 
 
 223 
 
 ,236 
 
 ,240 
 
 o233 
 
 30 
 
 288 
 
 ,284 
 
 c277 
 
 o283 
 
 35 
 
 c338 
 
 321 
 
 329 
 
 329 
 
 Table 5,7 RANGE IN TEST RESULTS USED FOR 
 ESTABLISHING THE STANDARD CURVE 
 FOR TOTAL COBALT DETERMINATION 
 
 COBALT 
 CONCo 
 
 (yg) 
 
 5 
 10 
 15 
 20 
 25 
 30 
 35 
 
 ABSORB ANCE- 
 
 „050 
 ,097 
 ,143 
 ,190 
 ,236 
 ,283 
 ,330 
 
 RANGE IN 
 TEST RESULTS 
 
 (yg) 
 
 *,004 
 * o 007 
 
 * o 014 
 
 *,004 
 * , 013 
 ±,006 
 ±,009 
 
 ^Computed from Least Squares equation 
 
58 
 
 5 a . . 
 
 activity of 7„20 x 10 dps e with a precision of *l o percent, on January 7 B 
 1963 „ The sample was carefully diluted to a volume of 100 ml„ Three 
 5=ml aliquots of the diluted standard were taken and each aliquot was 
 carefully diluted to 25 ml„ Three 1-mi aliquots of the second dilution 
 were taken and placed in separate counting tubes „ The volume in each 
 tube was increased to 10 ml with water and the tubes were counted „ The 
 true activity contained in each counting tube was calculated by multi- 
 plying the activity of the standard by a decay factor of ,546 for tubes 
 counted on August 9, 1963 8 a decay factor of 541 for tubes counted on 
 
 August 12, 1963, and by dividing the activity by a dilution factor of 
 
 65 
 500 o Table 5„8 contains the results from counting the nine Zinc samples, 
 
 The counting efficiency averaged 23 o percent The precision of the assay 
 resulted in a standard deviation of * 23 x l o - ^23 percent in the 
 estimation of counting efficiency,, The range of results for counting 
 efficiency produced a standard deviation of *o27 percent in counting effi- 
 ciency, for a total standard deviation of * 35 percent. The counting 
 
 65 
 
 efficiency for Zinc was therefore established at 23 o * 4 percent 
 
 A liquid Cobalt standard was obtained from the Nuclear=Chicago 
 
 Corporation, Standards Section The assay of the standard had shown an 
 
 5 
 
 activity of 9 65 x 10 dps, with a precision of ± 3 ^ percent, on 
 
 January 3, 1961 „ The gamma scintillation counter efficiency for counting 
 
 fin 
 Cobalt activity was established by following a procedure similar to 
 
 fi r 
 that used for establishing the efficiency for counting Zinc ' activity , 
 
 fin 
 Table 5„8 also contains the results from counting the Cobalt samples 
 
 The counting efficiency averaged 36 „ 7 percento The precision of the assay 
 
 plus the precision of the established counting efficiency resulted in a 
 
 fin 
 standard deviation of *1 2 percento The counting efficiency for Cobalt 
 
 was therefore 36 . 7 *1 2 percento 
 
59 
 
 Table 5o8 
 
 ESTABLISHMENT OF COUNTING EFFICIENCY FOR 
 ZINC 65 AND COBALT 60 
 
 SAMPLE 
 
 
 COUNTING 
 DATE 
 
 TRUE 
 ACTIVITY 
 (dpm) 
 
 COUNTED* 
 ACTIVITY 
 (cpjn) 
 
 EFFICIENCY 
 (percent) 
 
 _. 65 
 Zinc 
 
 1 
 2 
 3 
 
 8/9/63 
 
 47,200 
 
 10,990 
 10,921 
 11,075 
 
 
 23,2 
 23.1 
 23o4 
 
 rr- 65 
 
 Zinc 
 
 4 
 5 
 6 
 
 8/12/63 
 
 46,800 
 
 10,711 
 10,804 
 10,533 
 
 
 22 9 
 23.1 
 22o5 
 
 7 * 65 
 Zinc 
 
 7 
 8 
 9 
 
 8/12/63 
 
 46,800 
 
 10,584 
 10,753 
 10,809 
 
 Average 
 
 22.6 
 23.0 
 23.1 
 
 23.0 
 
 Cobalt 60 
 
 1 
 2 
 
 12/17/63 
 
 39,200 
 
 14,439 
 14,298 
 
 
 36.8 
 36.5 
 
 60 
 Cobalt 
 
 3 
 
 4 
 
 12/17/63 
 
 39,200 
 
 14,427 
 14,376 
 
 Average 
 
 36.8 
 36.6 
 
 36.7 
 
 '♦Average of three 2-minute counts minus background activity 
 
60 
 As the decay factors for these isolated radionuclides were known, 
 all activities were converted to pc/g on the date of collection of the 
 samples „ Total gamma activities had to be recorded on the date that the 
 activity of each sample was measured t since decay factors could not be 
 calculated for these mixtures of radionuclides,, 
 
 Prevention o f Contami nati on and Loss of Microg ram Quantities 
 of Zinc and Cobalt 
 
 When working with microgram quantities of zinc or cobalt, 
 adsorption on surfaces such as glass and plastic 8 must be considered,, 
 Leaching of metal contaminants from glassware can interfere with analyti- 
 cal accuracy,, Contamination of reagents is a distinct possibility,, 
 
 To avoid these possible sources of error in the analytical 
 procedure s a variety of precautions were taken „ All glassware and any 
 other materials that would come in contact with the sample during the 
 analysis were washed twice with dilute (approximately „1N) HC1 and then 
 twice with water which had been deionized by several passages through a 
 mixed resin ion exchange column „ Whenever there was doubt as to the 
 cleanliness of a piece of glassware B it was tested by swirling a few 
 ml of dithizone II solution in it„ Whenever a sample was transferred 
 from one glass container to another 9 the inside of the initial container 
 was washed with either „ 5N or dilute ( „iN) HC1 several timesj, and the 
 washings added to the sample „ As each sample was poured into the anion 
 exchange column 8 it was washed with 7N-HC1 and the washings added to the 
 exchange column „ This procedure eliminated adsorption on the glass and 
 plastic surfaces with which a sample came into contact „ Samples were 
 not allowed to come into contact with any material other than glass or 
 various forms of plastics „ 
 
61 
 
 Hydrochloric acid was used extensively throughout the analyses 
 All of the HC1 used had been decontaminated at a concentration of 12N by 
 passage through a Dowex 1 anion exchange column at a rate of approximately 
 <>2 ml/sq cm/min Under these conditions 9 any zinc or cobalt contained in 
 the acid would have been strongly adsorbed by the anion exchange resin „ 
 Other reagents used in the determination of total zinc were decontaminated 
 by extraction with dithizone II solution 9 as described in Standard Methods 
 for the Examination of Water and Wastewater No such simple purification 
 procedure was available for decontaminating reagents used in the determi- 
 nation of total cobalt o However 9 in both of these analyses 8 the use of 
 reference blanks compensated for errors due to minor contamination of 
 reagents o 
 
 The color forming reagents used in colorimetric analyses are 
 usually light and heat sensitive,. To prevent decompositions, the dithizone 
 solution was stored in a dark glass bottle and kept in a refrigerator „ 
 The nitroso=>R-salt solution used in the. cobalt test was light sensitive 
 but would not decompose at room temperature „ It was therefore stored in 
 a dark glass bottle and kept in a dark cabinet „ 
 
62 
 
 VI o SAMPLING SURVEY 
 
 On August 14 and 15 8 1963 8 four water, four plankton and twenty^ 
 four bottom sediment samples were collected from the Columbia River 9 from 
 a reach of the river extending from just upstream of ail of the Hanford 
 reactors downstream to the junction of the Umatilla River with the Columbia 9 
 a distance of 97 „ 8 river miles The location of each of the sampling points 
 is noted in Fig„ 6„1 and detailed in Tables 6 l s 6 2 and 6„3 
 
 Water samples were taken to determine whether Zinc and Cobalt 
 were being removed from the river water as it moved downstream 9 and if so 8 
 to determine how rapidly these two radionuclides were being removed 9 and 
 where the removal was occurring It should be noted that only four water 
 samples were taken and that the resulting data are therefore very limited 
 The Hanford staff have accumulated a wealth of data concerning the analysis 
 of water samples and have applied this data to fulfill the objectives 
 stated above o 
 
 Plankton samples were taken to ascertain the degree of concentra- 
 tion of Zinc and Cobalt exhibited by these aquatic organisms 8 and also 
 to show the effect of location aj,ong the river on the concentration of 
 these radionuclides in plankton „ 
 
 A series of bottom sediment samples were taken in order to 
 determine the concentration of Zinc and Cobalt along approximately 
 100 miles of the river from the reactors to below McNary dam„ 
 
 WATER SAMPLES 
 
 Water samples were taken at 15 to 33 „ 5 mile intervals along this 
 reach of the Columbia River, The first two samples were taken in the late 
 
-§3 
 
 PRIES"P 
 RAPIDS 
 
 
 1 $&< 
 
 ► 7 
 .8 
 
 N 
 
 I 
 
 HANFORD 9* 
 
 10 
 
 H2 
 
 
 
 J5 
 
 WASHINGTON 
 
 i* 
 
 : it*A 
 
 lRICHLANO 
 
 PASCO S 
 
 18. 
 
 „#(£ 
 
 Rl 
 
 y/£" 
 
 KENNEWICK 
 
 ,20 
 
 WASHINGTON 
 
 OREGON 
 
 C° 
 
 LU 
 
 MBit 
 
 Rl 
 
 v e* 
 
 PATERSON 
 
 OREGON 
 
 Approximate Scale In Miles 
 5 5 10 15 20 
 
 McNARY DAM 4 
 
 4» 23 2I 
 
 24<£VillMATILLA 
 
 7^ 
 
 21 
 
 LEGEND : 
 
 • Bottom Sediment Samples 
 — Water 8 Plankton Samples 
 
 Fig. 6,1 
 
 LOCATION OF SAMPLING POINTS 
 
64 
 
 Table 6.1 WATER SAMPLES 
 
 
 COLUMBIA 
 
 RIVER - AUGUST 14 & 15 9 1963* 
 
 Sample § 
 
 Volume 
 (liters) 
 
 44.64 
 44,87 
 44.02 
 43,95 
 
 Location 
 
 River Mile 
 
 1 
 2 
 3 
 4 
 
 Hanford Ferry 
 
 300 Area off PRTR Intake 
 
 Pasco below RR Bridge 
 
 1000 yards above McNary Dam 
 
 361.5 
 344.5 
 326.5 
 293 
 
 *A11 samples collected by Dr. Benjamin B, Ewing 2 Professor of Sanitary 
 Engineering, University of Illinois 
 
 Table 6.2 PLANKTON SAMPLES 
 
 
 
 COLUMBIA 
 
 RIVER - AUGUST 14 & 15, 1963* 
 
 
 Sample 
 
 1 
 
 Sampl ing 
 
 Time 
 (minutes) 
 
 30 
 
 Location 
 
 River Mile 
 
 1 
 
 
 Hanford Ferry 
 
 361.5 
 
 2 
 
 
 20 
 
 300 Area off PRTR Intake 
 
 344.5 
 
 3 
 
 
 15 
 
 Pasco below RR Bridge 
 
 326,5 
 
 4 
 
 
 30 
 
 1000 yards above McNary Dam 
 
 293 
 
 *A11 samples collected by Dr. Benjamin B. Ewing, Professor of Sanitary 
 Engineering^, University of Illinois 
 
65 
 
 Table 6.3 BOTTOM SEDIMENT SAMPLES 
 
 COLUMBIA RIVER - AUGUST 14 £ 15 9 1963* 
 
 Sample W° Area Depth Description^ of Loca t ion P * RTyer_M'ile 
 
 1 8" 4> 1" 100 yards above 100-B water 384,8 
 
 intake on south shore -=1/2 
 mile above first waste outfall 
 
 2 8"' $ 3/4" 75 yards above 100<=K water 382,3 
 
 intake on plant shore 
 
 Plant shore between KE and N 381 
 
 Hard packed clay bank under 375 . 5 
 bluff on far shore 
 
 Sand beach 50 yards above 100-H 373d 
 water intake on plant shore 
 
 Sandy beach 1.00 feet below White 369,7 
 Bluff Ferry landing on plant 
 shore between H Area and F Area 
 
 8" 4> 3/4" Sand and clay on far shore below 366 
 100-F Area 
 
 8" <t> 3/4" Sandy beach on far shore 365,5 
 
 9 8" <J> 3/4" Sandy beach on plant shore 100 361,5 
 
 feet above Hanford Ferry 
 
 8" <J> 3/4" Sand bank on far shore below 359,3 
 Hanford Ferry 
 
 3 
 
 8" * 
 
 3/4" 
 
 4 
 
 6"x4" 
 rectangle 
 
 1/2" 
 
 5 
 
 8" <J» 
 
 3/4" 
 
 6 
 
 8" * 
 
 3/4" 
 
 8" 
 
 * 
 
 3/4" 
 
 8" 
 
 * 
 
 3/4" 
 
 8" 
 
 * 
 
 3/4" 
 
 8" 
 
 * 
 
 3/4" 
 
 8" 
 
 ♦ 
 
 3/4" 
 
 8" 
 
 <P 
 
 3/4" 
 
 11 8" $ 3/4" Sandy beach en plant shore below 357,5 
 
 Hanford Ferry 
 
 12 8" <J> 3/4" Sandy beach below Ringold on 353„5 
 
 Ringoid shore 
 
 13 8" <p 3/4" Sand spot on rocky shore 1 mile 351,3 
 
 above Power Line crossing on 
 plant shore 
 
 1H 8" <J> 3/4" Sand beach on plant shore 3/4 349,3 
 
 mile below Power Line crossing 
 
 15 8" <f> 3/4" Beach on far shore just above 345,3 
 
 300 Area 
 
66 
 
 Table 6 „ 3 ( cont inued ) 
 
 Sample "W" Area Depth Descr iption_ of Location .^YJIE-?!!^ 
 
 16 8" <J> 3/4" Sand spot on rocky shore on 344 . 3 
 
 plant side just below PRTR 
 intake 
 
 17 8" <f> 3/4" Beach on Richland shore about 339 
 
 1 mile above Fire Station 
 
 18 8" $ 3/4" Sand beach on island below 326 
 
 Pasco RR bridge and 1/10 mile 
 above Power Line crossing 
 
 19 8" <j> 3/4" Sand behind barges on plant 321 
 
 shore 1/4 mile below Union 
 Pacific RR bridge 
 
 20 8" <|> 3/4" East shore of island 3/4 mile 320„5 
 
 below Union Pacific RR bridge 
 nearer Snake River shore 
 
 21 8" <j> 3/4" Sand beach at mouth of creek at 298 
 
 Hat Rock State Park on Oregon 
 shore 
 
 22 8" $ 3/4" Sand beach on Oregon shore 3 295 
 
 miles above McNary Dam 
 
 8" <J> 
 
 3/4" 
 
 8" <f> 
 
 3/4" 
 
 8" $ 
 
 3/4" 
 
 23 8" <f> 3/4" Sand beach 1000 yards above 293 
 
 McNary Dam on Oregon shore 
 
 24 8" 4> 3/4 Upstream side of mcuth of 287 
 
 Umatilla River at Umatilla on 
 Oregon shore 
 
 s1f All samples collected by Dr» Benjamin B Ewmg 9 Professor of Sanitary 
 Engineerings, University of Illinois 
 
67 
 
 morning and early afternoon of August 14 and the second two during the same 
 periods of August 15 8 1963 „ In order to reduce the volume and weight of 
 the water samples so that they could be economically transferred to the 
 laboratory 9 each was passed through a column of Dowex 50 cation exchange 
 resin o The column 8 containing the zinc and cobalt, and other cations t was 
 then shipped to the Sanitary Engineering Laboratory at the University of 
 Illinois o The sampling apparatus which came into contact with the sample 
 was made entirely of polyethylene with the exception of the ion exchange 
 column and reducer which were glass „ 
 
 Each water sample was collected in midstream in polyethylene 
 bottles and transferred to shore Each was then filtered through a glass= 
 wool wad in a funnel which drained into a 7170 ml polyethylene carboy. A 
 150 ml cylindrical glass separatory funnel containing 120 ml of Dowex 50 
 resin was attached and sealed 8 via a glass reducer 8 stopcock grease and 
 rubber bands 8 to the outlet tap at the bottom of the carboy „ The sample 
 was passed through the resin at a maximum rate of approximately 
 six mi/sq cm/min„ A small sample of eluate was tested occasionally with 
 total hardness indicator 5 ** to be certain that nc leakage of cations from 
 the resin had occurred „ Laboratory tests had shown that the 120 ml of 
 resin would completely remove the hardness from 74 liters of water contain- 
 ing 100 ppm total hardness as CaC0 3 at the above flow rate The hardness 
 of the Columbia River was not measured 8 but was assumed 8 from published 
 data (22) B to be less than 100 ppm„ No leakage of cations occurred when 
 approximately 45 liter samples were passed through the cation resin columns , 
 
 After each sample had been passed through the cation exchange 
 column 8 the column was sealed and shipped to the laboratory „ The fiberglass 
 
 "Univer II, Hach Chemical Co 09 Ames 9 Iowa 
 
68 
 filters used to strain each sample were placed in glass bottles , sealed 
 and also shipped to the laboratory „ 
 
 PLANKTON SAMPLES 
 
 Plankton samples were collected at the same location and time as 
 the water samples,, Each sample was collected in midstream with a #25 
 plankton net The net was suspended in the flowing water for a period of 
 from 15 to 30 minutes „ The plankton caught in the net were then transferred 
 to a glass jar j sealed, and shipped to the laboratory 
 
 Data resulting from the analyses of these plankton samples could 
 only be recorded in terms of dry weight of plankton, as neither the numbers 
 of plankton nor the volume of water from which the samples had been collected 
 was known „ 
 
 BOTTOM SEDIMENT SAMPLES 
 
 The Columbia River from the reactor area to Richland is a swift, 
 rocky-bottomed stream,, Bottom sediments in this reach are nearly always 
 limited to the near shore area and even there the sediments consist mainly 
 of sand or gravelo Silt and mud could only be found in a few backwater 
 areas „ Samples of bottom sediments were taken along the shore-line of the 
 river o 
 
 Bottom sediment samples were collected by inserting an eight-inch 
 inside diameter cylinder into the sediments, to a depth of three-quarters 
 of an inch,, The sediment within the cylinder was scooped into a plastic 
 bag until a three-quarter-inch disc of sediment had been removed „ Samples 
 #1 and #4 are exceptions „ Sample #1 was composed of a layer one inch thick „ 
 Sample #4 was obtained by cutting a six-inch by four-inch rectangle, three- 
 quarters of an inch thick, out of the sediment „ Each sample was placed in 
 
69 
 
 a plastic bag, sealed, placed in a cardboard container which was also 
 sealed, and shipped to the laboratory , 
 
 The samples were usually of clean, fine sand or silty sando A 
 few samples contained some clay sized material „ 
 
 The analytical procedure presented in Chapter IV and discussed 
 in Chapter V was used for the quantitative determination of the total and 
 radioactive zinc and cobalt in these samples „ 
 
70 
 
 VII RESULTS OF ANALYSES 
 
 The results of the analyses of the four water 8 four plankton and 
 twenty-four bottom sediment samples collected from the Columbia River on 
 August 14 and 15, 1963, are presented in Tables 7.1 to 7 5 o 
 
 The results of the analyses for total gamma activity are 
 presented in Table 7.1. The total gamma activity of plankton and bottom 
 sediment samples and the activities of the residue and eluate from the 
 acid washing of each of these samples is given The total gamma activities 
 of the water samples 8 as presented, are the activities of the cationic 
 fractions of these samples, since they were collected on cation exchange 
 resin at the site and eluted from the resin at the laboratory. The date of 
 measurement of the gamma activities of each sample is given. 
 
 Table 7.2 gives the results of the analyses for total zinc and 
 total cobalts, both before and after separation. The values obtained before 
 separation are approximate only. The results of the determinations of 
 radioactive zinc and radioactive cobalt 8 as Zinc ' and Cobalt , are pre- 
 sented in Table 7.3. Activities of these two radionuclides are given as of 
 the date of collection of the samples, August 15 8 1963. The percentages of 
 the total gamma activity due to Zinc and Cobalt in each sample and in 
 the eluate from the acid washing of each sample 8 as of the date of measure- 
 ment of the total gamma activities 8 are also presented in Table 7.3. 
 
 Table 7.4 summarizes the bottom sediment data included in Tables 
 7.1 and 7.3 8 relating activities to the ground surface area of each sample. 
 Table 7.5 is a summary of the results of analyses of the water, plankton 
 and bottom sediment samples. 
 
71 
 
 Table 
 
 TOTAL GAMMA ACTIVITY OF COLUMBIA RIVER SAMPLES 
 
 SAMPLE 
 
 TEST 
 DATE 
 
 
 TOTAL GAMMA ACTIVITY 
 
 
 PERCENT 
 
 DESCRIP- 
 
 Sample 
 
 Residue 
 
 Eluate 
 
 Sample 
 
 TOTAL GAMMA 
 
 TION 
 
 (*7 days) 
 
 (cpm/g) 
 
 (cpm/g) 
 
 (cpm/g) 
 
 Adjusted* 
 
 ACTIVITY 
 
 
 
 
 
 
 (cpm/g) 
 
 E LUTED** 
 
 WATER 
 
 
 
 
 
 
 1 
 
 10/10/63 
 
 o0690 
 
 - 
 
 - 
 
 - 
 
 - 
 
 2 
 
 10/17/63 
 
 0050 
 
 - 
 
 - 
 
 - 
 
 = 
 
 3 
 
 12/9/63 
 
 o0072 
 
 - 
 
 _ 
 
 » 
 
 - 
 
 4 
 
 12/9/63 
 
 o0192 
 
 - 
 
 - 
 
 - 
 
 - 
 
 PLANKTON 
 
 
 
 
 
 
 
 1 
 
 2/17/64 
 
 - 
 
 667 
 
 4300 
 
 4970 
 
 87 
 
 2 
 
 2/17/64 
 
 - 
 
 372 
 
 2870 
 
 324 
 
 89 
 
 3 
 
 2/17/64 
 
 - 
 
 542 
 
 2250 
 
 2790 
 
 81 
 
 4 
 
 2/17/64 
 
 - 
 
 193 
 
 2010 
 
 2200 
 
 91 
 
 BOTTOM 
 
 
 
 
 
 
 
 SEDIMENTS 
 
 
 
 
 
 
 
 1 
 
 11/11/63 
 
 13o9 
 
 llo4 
 
 3o90 
 
 14 o 6 
 
 27 
 
 2 
 
 11/11/63 
 
 llo9 
 
 10 7 
 
 5oi8 
 
 13 o 9 
 
 37 
 
 3 
 
 11/11/63 
 
 24 o 6 
 
 13 c 8 
 
 12 4 
 
 25„4 
 
 49 
 
 4 
 
 11/19/63 
 
 7,7 
 
 7o2 
 
 2o60 
 
 8o74 
 
 30 
 
 5 
 
 12/4/63 
 
 126 
 
 46o3 
 
 67o7 
 
 120 
 
 56 
 
 6 
 
 11/20/63 
 
 29o2 
 
 llo3 
 
 19o8 
 
 30,2 
 
 66 
 
 7 
 
 12/4/63 
 
 57 o 9 
 
 29cl 
 
 42 o 3 
 
 64 o 6 
 
 65 
 
 8 
 
 12/4/63 
 
 37„6 
 
 16o7 
 
 31o0 
 
 42o6 
 
 73 
 
 9 
 
 12/20/63 
 
 196 
 
 70 .1 
 
 162 
 
 214 
 
 76 
 
 10 
 
 12/20/63 
 
 15o0 
 
 10„9 
 
 llo3 
 
 18„6 
 
 61 
 
 11 
 
 12/20/63 
 
 124 
 
 40,1 
 
 102 
 
 133 
 
 • • 
 
 12 
 
 12/20/63 
 
 42 o 6 
 
 19 o 4 
 
 31 2 
 
 41 o 6 
 
 75 
 
 13 
 
 1/22/64 
 
 177 
 
 30o8 
 
 13 T 
 
 172 
 
 80 
 
 14 
 
 1/22/64 
 
 >_»...!_- 
 
 24 4 
 
 40 o 5 
 
 60o0 
 
 68 
 
 15 
 
 1/22/64 
 
 54 8 
 
 35,3 
 
 49 
 
 69 o 6 
 
 70 
 
 16 
 
 1/22/64 
 
 111 
 
 i?«7o « 
 
 70o9 
 
 110 
 
 54 
 
 17 
 
 1/25/64 
 
 75o2 
 
 22o8 
 
 65o2 
 
 81o6 
 
 80 
 
 18 
 
 1/25/64 
 
 17 o 2 
 
 6c8 
 
 10 o 4 
 
 17,2 
 
 60 
 
 19 
 
 1/25/64 
 
 10„1 
 
 6o9 
 
 4o22 
 
 10o6 
 
 40 
 
 20 
 
 1/25/64 
 
 16 5 
 
 Iw o - 
 
 3,75 
 
 16o8 
 
 22 
 
 21 
 
 1/25/64 
 
 4 o 
 
 5o5 
 
 o43 
 
 4o96 
 
 9 
 
 22 
 
 1/25/64 
 
 608 
 
 7 4 
 
 3o03 
 
 8o60 
 
 35 
 
 23 
 
 1/25/64 
 
 11 oO 
 
 7 7 
 
 6c95 
 
 12.8 
 
 54 
 
 24 
 
 1/28/64 
 
 15 5 
 
 lOcO 
 
 ^ 58 
 
 16o6 
 
 46 
 
 * Average of data for Initial Sample and data for Residue plus Eluate 
 ** Using Adjusted Sample and Eluate data 
 
72 
 
 Table 7.2 
 
 TOTAL ZINC AND TOTAL COBALT 
 OF COLUMBIA RIVER SAMPLES 
 
 SAMPLE 
 
 TOTAL 
 
 ZINC 
 
 TOTAL 
 
 COBALT 
 
 DESCRIPTION 
 
 Before 
 
 After 
 
 Before 
 
 After 
 
 
 Separation 
 
 Separation 
 
 Separation 
 
 Separation 
 
 
 (Approximate) 
 
 (yg/g) 
 
 (Approximate) 
 
 (yg/g) 
 
 
 (yg/g) 
 
 
 ^S/JLL. 
 
 
 WATER 
 
 
 
 
 
 1 
 
 _ 
 
 = 
 
 - 
 
 - 
 
 2 
 
 O 00593 
 
 oI20 
 
 - 
 
 .00011 
 
 3 
 
 »00506 
 
 o056 
 
 - 
 
 .00014 
 
 4 
 
 „00439 
 
 o048 
 
 - 
 
 .00005 
 
 PLANKTON 
 
 
 
 
 
 1 
 
 1620 
 
 1960 
 
 45 
 
 3o5 
 
 2 
 
 1300 
 
 1750 
 
 27 
 
 3.4 
 
 3 
 
 1700 
 
 1060 
 
 31 
 
 1.2 
 
 4 
 
 1900 
 
 1870 
 
 160 
 
 1.9 
 
 BOTTOM 
 
 
 
 
 
 SEDIMENTS 
 
 
 
 
 
 1 
 
 183 
 
 174 
 
 .31 
 
 .52 
 
 2 
 
 189 
 
 187 
 
 .24 
 
 .53 
 
 3 
 
 130 
 
 132 
 
 .06 
 
 .40 
 
 4 
 
 3o70 
 
 5o07 
 
 4.15 
 
 .87 
 
 5 
 
 166 
 
 177 
 
 o 06 
 
 .09 
 
 6 
 
 154 
 
 110 
 
 oil 
 
 .12 
 
 7 
 
 44 o 5 
 
 35o6 
 
 03 
 
 o07 
 
 8 
 
 69o5 
 
 43.5 
 
 .02 
 
 .04 
 
 9 
 
 151 
 
 98 o 4 
 
 .13 
 
 .00 
 
 10 
 
 133 
 
 90o5 
 
 .03 
 
 o01 
 
 11 
 
 108 
 
 WW o 
 
 .04 
 
 .00 
 
 12 
 
 13o8 
 
 21o 3 
 
 .00 
 
 .66 
 
 13 
 
 91 o 4 
 
 43 
 
 o06 
 
 .33 
 
 14 
 
 141 
 
 94 o 
 
 .14 
 
 82 
 
 15 
 
 224 
 
 137 
 
 .10 
 
 „72 
 
 16 
 
 33„6 
 
 24 2 
 
 .02 
 
 .22 
 
 17 
 
 93 6 
 
 110 
 
 .20 
 
 .18 
 
 18 
 
 16.0 
 
 56d 
 
 ,15 
 
 .01 
 
 19 
 
 2c20 
 
 8.22 
 
 .34 
 
 .14 
 
 20 
 
 5 o 76 
 
 18o4 
 
 .04 
 
 .32 
 
 21 
 
 o51 
 
 7o93 
 
 .33 
 
 ,18 
 
 22 
 
 3o85 
 
 9.77 
 
 .37 
 
 o ib 
 
 23 
 
 7 48 
 
 5o26 
 
 „28 
 
 <= 
 
 24 
 
 50ol 
 
 86o7 
 
 .20 
 
 .03 
 
73 
 
 Table 7.3 
 
 RADIOACTIVE ZINC AND RADIOACTIVE COBALT 
 OF COLUMBIA RIVER SAMPLES 
 
 SAMPLE 
 
 RADIOACTIVE ZINC AS 
 
 ZINC 65 
 
 RADIOACTIVE 
 
 COBALT AS 
 
 60 
 COBALT 
 
 DESCRIPTION 
 
 AUGU: 
 
 ST 15j 1963 
 
 AUGUST 15, 1963 
 
 
 
 Activity 
 
 Percent" 
 
 of Total 
 
 Activity 
 
 Percent" of Total 
 
 
 (pc/g) 
 
 Gamma Act 
 Sample 5 ' 4 " 
 
 :ivity of 
 Eluate 
 
 (pc/g) 
 
 Gamma Act: 
 Sample** 
 
 Lvity of 
 Eluate 
 
 WATER 
 1 
 2 
 
 
 
 
 
 .0199 
 
 160 
 
 = 
 
 „0011 
 
 16 
 
 _ 
 
 3 
 
 .0029 
 
 14 
 
 = 
 
 .0000 
 
 ,0 
 
 _ 
 
 4 
 
 ,0013 
 
 3 
 
 - 
 
 o0014 
 
 5.8 
 
 - 
 
 PLANKTON 
 
 
 
 
 
 
 
 1 
 
 8060 
 
 47 
 
 55 
 
 60 
 
 .9 
 
 1.0 
 
 2 
 
 5800 
 
 53 
 
 59 
 
 
 
 oO 
 
 .0 
 
 3 
 
 4830 
 
 50 
 
 63 
 
 63 
 
 1,7 
 
 2.1 
 
 4 
 
 5030 
 
 66 
 
 72 
 
 
 
 ,0 
 
 cO 
 
 BOTTOM 
 
 
 
 
 
 
 
 SEDIMENTS 
 
 
 
 
 
 
 
 1 
 
 „69 
 
 2 
 
 7 
 
 o34 
 
 1 o 8 
 
 6„8 
 
 2 
 
 5.13 
 
 14 
 
 38 
 
 o35 
 
 1.9 
 
 5.3 
 
 3 
 
 19 o 4 
 
 29 
 
 60 
 
 o55 
 
 X o / 
 
 3.4 
 
 4 
 
 3o07 
 
 12 
 
 40 
 
 33 
 
 3.0 
 
 10 
 
 5 
 
 111 
 
 33 
 
 60 
 
 Lo99 
 
 1.2 
 
 2.2 
 
 6 
 
 23.8 
 
 30 
 
 45 
 
 o94 
 
 2.3 
 
 3.5 
 
 7 
 
 62.0 
 
 35 
 
 54 
 
 loOO 
 
 1.2 
 
 1,8 
 
 8 
 
 30.9 
 
 27 
 
 36 
 
 1.10 
 
 2.0 
 
 2.7 
 
 9 
 
 201 
 
 32 
 
 42 
 
 S.50 
 
 3.3 
 
 4.4 
 
 10 
 
 13.0 
 
 25 
 
 40 
 
 .39 
 
 1.6 
 
 2.7 
 
 11 
 
 86o9 
 
 23 
 
 30 
 
 4o80 
 
 2 7 
 
 3.5 
 
 12 
 
 52.0 
 
 42 
 
 57 
 
 1.22 
 
 2.2 
 
 2.9 
 
 13 
 
 230 
 
 42 
 
 53 
 
 13o0 
 
 5 6 
 
 7„0 
 
 14 
 
 60o0 
 
 32 
 
 46 
 
 j. o 88 
 
 2.4 
 
 3.5 
 
 15 
 
 62o5 
 
 28 
 
 40 
 
 2o73 
 
 2.9 
 
 4„1 
 
 16 
 
 92„5 
 
 27 
 
 41 
 
 2.63 
 
 1.8 
 
 2.8 
 
 17 
 
 136 
 
 52 
 
 65 
 
 1.73 
 
 1 o 6 
 
 2.0 
 
 18 
 
 13„8 
 
 25 
 
 41 
 
 lo44 
 
 6.1 
 
 10 
 
 19 
 
 3.03 
 
 9 
 
 23 
 
 . 54 
 
 4.4 
 
 11 
 
 20 
 
 3 34 
 
 6 
 
 28 
 
 1.28 
 
 .6 
 
 26 
 
 21 
 
 oOO 
 
 
 
 
 
 .21 
 
 .3 
 
 37 
 
 22 
 
 4.67 
 
 16 
 
 48 
 
 o03 
 
 .2 
 
 .7 
 
 23 
 
 2o74 
 
 6 
 
 12 
 
 • 
 
 - 
 
 . 
 
 24 
 
 10„9 
 
 21 
 
 44 
 
 oOO 
 
 .0 
 
 oO 
 
 * On date of measurement of total gamma activity. 
 ** Using adjusted sample data. 
 
74 
 
 rd co 
 
 pa co 
 
 o o-. 
 
 O rH 
 
 «CM 
 
 in c 
 
 v^ 
 CO p. 
 
 W) 
 
 < 
 
 CJ 
 
 o 
 
 y C co 
 
 M tD 
 
 IS! cr. -g 
 ■H * 
 
 <D .*-■> 
 
 > «<N 
 
 Mm c 
 
 O \ 
 
 rO i-> 
 
 o w 
 
 H ^ 
 
 T3 bO 
 
 oi < 
 
 
 "2C 
 
 
 »;j 
 
 s^ 
 
 y=*\ 
 
 +JCN 
 
 °H 
 
 c 
 
 > 
 
 •H 
 
 'H 
 
 "■-«. 
 
 4-> 
 
 B 
 
 O 
 
 a! 
 
 < 
 
 o 
 
 
 ^-^ 
 
 C9 
 
 « ! 
 
 
 ^ 
 
 H 
 
 CD 
 
 id 
 
 Q | 
 
 P 
 
 1 
 
 o 
 
 ■*-• I 
 
 E- 
 
 W I 
 
 
 CD X 
 
 
 H I 
 
 +J y-N 
 
 tO CM 
 
 a* c 
 
 
 CO 
 
 
 ■p 
 
 CD 
 
 e c 
 
 iH 
 
 o <u 
 
 0. 
 
 ■m e 
 
 S 
 
 +J -H 
 
 <T3 
 
 O T> 
 
 to 
 
 cq a> 
 
 
 C/> 
 
 mcnd-ococncoE-- 
 
 (O^md-nifli^iDh 
 
 iotoa>rHtoaicnoorHr-oocotooococMco;i-i>-tn 
 
 rH CO rH rH rH rH iHCMiHCOmd-COCOiHCN 
 
 CM H CO 
 
 <n en co co 
 H cr co o 
 
 CO i-H 
 
 o :* o 
 
 o m o en 
 o cm to in 
 
 j 
 o 
 in cm in 
 
 CM 
 
 rH O 
 
 CO H 
 
 co in 
 
 in 
 
 o o o to en 
 
 j- d" J" to to 
 
 co in m co 
 
 H H CM 
 
 p- co 
 
 in o- 
 
 COCOt~-COOCnOJ-OOOCOOOOOO(OCMOOtOO(-( 
 
 E^iocoocMco:tCMLnt>tococotOcncMcoind-tocooor~ 
 
 CMCMJ-COCMlOCMI>-l>COO<OrHr-ldhCOin-3-CMCOrHCMCMCM 
 CN rH .j CO .3- r-\ ,-{ r-\ H 
 
 CO CO CO CO 
 
 CO 
 
 co co co co 
 
 tocoioiocotococotoioioto:* d-j-d-^-d-Jd-j-j-^ :* .d- 
 
 WW(DN,lO (OXN' — \U)lDlOlO«)(DtDlO(DiDlOlO 
 i— I H HI C7> -^ O \ -\ O O O 0'->^^'-^.\\\\ ^» \ "*^ ^ \ 
 
 HH^iHd-CMd- *(M(NWvNN(N(NCMirtinini/)iniflinco 
 
 \\S.X\XNN\SN\CNN(N(N(NCN(NOJCN(NCNM 
 rH H f-JH CM HCM CM CM tM (NCMVW\WNWW\ 
 HrHrHrHrHrHrHrHrHH-HHrHrHrHrHrHrHrHrHrHrHrHrH 
 
 oininoininininininmininmminininmininmmm 
 
 cooocoococococococococococococococotocococococo 
 
 ooo^toooooooooooooooooooo 
 ininincMtnininiominm in mm inmcnminm in mtn»n 
 
 ■M 
 
 
 
 
 
 
 
 
 
 A 
 
 H 
 
 CM 
 
 p- 
 
 in 
 
 H 
 
 it 
 
 CO 
 
 m 
 
 >> bO^ 
 
 zt 
 
 p- 
 
 to 
 
 3 
 
 co 
 
 to 
 
 CO 
 
 in 
 
 U -H bfl 
 
 cn 
 
 en 
 
 co 
 
 CO 
 
 cn 
 
 o 
 
 <7> 
 
 to 
 
 Q CD w 
 
 
 
 
 
 
 rH 
 
 
 
 3= 
 
 
 
 
 
 
 
 
 
 OCOCMIf-CMCOCMCMCM 
 
 o«ncoooj>cozfco 
 
 OrHCOCMCnOCOCncO 
 
 HI rH 1-4 H rH 
 
 lOh N J ID O 
 
 d- r» cm o *n cm 
 
 rH o CO cm o CO 
 
 H H rH rH H 
 
 rHCMcoj-intDf-oocn 
 
 O rH CM (O 
 
 rH rH rH H 
 
 j-intor->cocnorHCMcOif 
 
 rHHHrHrHrHCMCNCMCMCM 
 
 
 (0 
 
 
 
 
 
 u 
 
 
 nj 
 
 a> 
 
 0) 
 
 P 
 
 U 
 
 fl 
 
 ■d 
 
 E 
 
 Mh 
 
 H 
 
 u 
 
 X 
 
 3 
 
 o 
 
 B3 
 
 fc 
 
 
 D<CM 
 
 Gi 
 
 C 
 
 < 
 
 H 
 
75 
 
 CO 
 
 U 
 
 < 
 CO 
 
 os 
 w 
 > 
 
 M 
 OS 
 
 < 
 l-l 
 
 PQ 
 
 ►J 
 
 O 
 
 a 
 
 o 
 
 co 
 
 w 
 
 CO 
 
 r- 
 < 
 
 < 
 
 o 
 
 CO 
 
 H 
 
 CO 
 
 o 
 
 >- 
 
 OS 
 
 < 
 
 CD 
 CO 
 
 I I I I 
 
 II 
 
 m<T>^-r-oocnooc^ cd cn 
 toiDCDrHtocDCDcorHr-»oo 
 
 rH CO H rH rH rH rH CN 
 
 CN -H 
 
 H o d- 
 
 H O H 
 
 O O O 
 
 O O O 
 
 d-mmcocDd-ooocDOCM 
 
 nnmcooiaioHinncotN 
 
 o o 
 
 ID 
 
 00 o 
 ID 
 
 H H Ol 
 
 J" <-i 
 
 
 *1 
 
 
 'H 
 
 
 CM 
 
 
 C 
 
 o 
 
 'H 
 
 C co 
 
 V» 
 
 H CO 
 
 o 
 
 Cn] CD 
 
 rH 
 
 5 
 
 CO 
 
 
 > 
 
 -.*» 
 
 •H 
 
 in 
 
 P 
 
 <H 
 
 o 
 
 
 rd 
 
 4-> 
 
 o 
 
 to 
 
 »H 
 
 3 
 
 Tj 
 
 bO 
 
 rd 
 
 =1 
 
 OS 
 
 < 
 
 I 1 
 
 CT> 
 
 CNCDcoooozioinocDOrH 
 
 rHCDCOOtOOOCNtOinOtO 
 
 n-HowcNind-woco 
 
 CM iH J" CM 
 
 bO 
 
 CD CD CO 
 
 CD CN rH 
 
 rH O O 
 
 O O O 
 
 cn co r- 
 
 ID H If O 
 
 00 O CD 
 
 O CD O 
 
 O O O O 
 
 CD O CO CO 
 
 O CO CO O 
 
 CO lO J lO 
 
 inCDCOrHCOCNOrHCOtOCN 
 rH rHCMlDCOOrHCOiT) 
 
 H CN 
 
 bO 
 
 rH P 
 
 rt) rH 
 
 P rd 
 
 O XI M 
 
 H O 3. 
 
 <T3 
 
 O 
 
 bO 
 
 +-> 
 
 
 
 \ 
 
 O 
 
 ■H 
 
 bO 
 
 H 
 
 N 
 
 3 
 
 H J- m 
 
 rH H O 
 
 o o o 
 
 o o o 
 
 o o o 
 
 H m 
 
 o tD r- 
 
 CN lO J 
 
 rH O O 
 
 O IT) CN CN 
 IT) CO CM CD 
 
 CO CO rH rH 
 
 CNCOOr^CDC\ir~ltOrHO<D 
 iDinucOOrHOOOOOtO 
 
 o 
 
 to m J- m m co 
 
 •p 
 
 rH rC 
 
 rd bO -— • 
 
 P °H 60 
 
 O d)w 
 
 E- 3 
 
 o 
 
 O 
 
 o 
 
 o 
 
 3- 
 
 C* 
 
 CM 
 
 IT) 
 
 tD 
 
 CO 
 
 o 
 
 cn 
 
 =f 
 
 J- 
 
 J- 
 
 co 
 
 J" 
 
 3 
 
 3- 
 
 J- 
 
 o o o o 
 to m to c-» 
 cn r- o oo 
 
 m CN CD o 
 
 CN rH CN 00 
 
 tD CM rH CD 
 
 o o o o 
 
 rH CM CO 
 
 :3-r>-CMinc"-omcocoocOrH 
 r^ooco r-rHcod-CDCDcocM 
 
 H H rH rH H 
 
 
 rHCNC^mrHJ-OOintDOCOCN 
 J-|>tDJ-COtDtDinrHOmcO 
 CDCDOOCOCDOCDOOrHOrHOO 
 
 o 
 
 
 
 
 C 
 
 r- 
 
 
 a) 
 
 fc 
 
 o 
 
 
 
 rH 
 
 CD 
 
 p 
 
 0) 
 
 
 a 
 
 P rH CM co J- ^ 
 
 rH 
 
 
 E 
 
 rd 
 
 c 
 
 J=> 
 
 
 rd 
 
 3 
 
 rd 
 
 rrj 
 
 
 to 
 
 
 rH 
 
 H 
 
 
 
 
 P-, 
 
 rH CN CO J" 
 
 0) 
 
 p 
 
 c 
 
 e 
 
 H 
 X) 
 CO 
 
 CO 
 
 rHCMCOJ-intDt— OOCDOHCN 
 
 rH rH rH 
 
76 
 
 m 
 
 o 
 
 
 c 
 
 CO 
 
 •H 
 
 ID 
 
 Nl 
 
 CO 
 
 
 <H 
 
 <D 
 
 
 > 
 
 a 
 
 •H 
 
 in 
 
 ■M 
 
 rH 
 
 O 
 
 
 03 
 
 P 
 
 O 
 
 CO 
 
 -H 
 
 3 
 
 TJ 
 
 bfl 
 
 03 
 
 3 
 
 Pi 
 
 < 
 
 CM 
 
 G 
 H 
 
 .H P "-» 
 UH bO 
 
 O ^ M 
 H O 3- 
 
 n) o M 
 
 P C \ 
 
 O «H bO 
 
 H (SI 3. 
 
 
 •K P 
 
 
 h x: 
 
 /~\ 
 
 o3 b0'~» 
 
 TJ 
 
 +j °H bO 
 
 0) 
 
 0)'-' 
 
 3 
 
 E- tS 
 
 G 
 
 
 «H 
 
 
 P 
 
 
 G 
 
 
 
 
 
 O 
 
 
 cod-mjniomiD> 
 
 cococococMcos-r^m 
 
 rinm^tonricN 
 
 CO 
 
 OCDMO>JIONCNO 
 oooooooooo 
 
 CO H CM CM H <H rH 
 
 O 
 O 
 
 O 3" O Lf) 
 
 o o o o 
 
 OOOOOlDO^H H r- CO 
 
 rHlD3-3-3-lO<Dr>- h m o 
 
 in rH CO in in CO rH h 
 
 m H <H rH CM 
 
 co j- o r- 3- 
 co o ro o to r» 
 
 OOCMCMCOCOCOCO 
 CO (O (O CT) CO H 
 CM H 
 
 3" CM 
 
 CO CM CM CM CO H 3" 
 CO CO O CM rH O rH 
 
 CM CO CO 
 
 co H H 
 
 CO 
 
 o 
 
 O O CM 
 
 co 3- r- 3- o 
 
 3" CT> CO CM H 
 
 •H .H 
 
 CM 
 
 CM 
 
 co r— cd 
 
 CJl t> CM 
 
 <D CO CO f- CJ) in ID 
 
 in h co 
 
 t^CMCOCMCMCMtDt^CNJ-CDO 
 
 or-t^co^-coj-r^CMOincM 
 
 CNOlOOOOKOrlOOCMOtD 
 H H rHrHHrHHH 
 
 e 
 
 CO 
 
 to 
 
 P 
 
 c 
 a) 
 
 E 
 
 °H 
 
 <u 
 
 CO 
 
 3" 
 H 
 
 in id p» co a> o 
 
 HHrlHrlCN 
 
 rH CM CO 3" 
 CM CM CM CM 
 
 w 
 p 
 
 X 
 bO 
 •H 
 
 (1) 
 
 >> 
 
 (0 
 
 03 
 
 OT 
 
 p 
 
 c 
 a) 
 
 e 
 
 •H 
 TJ 
 CD 
 
 w 
 
 E 
 
 o 
 p 
 p 
 o 
 
 XI 
 
 G 
 
 m 
 
 G 
 
 o 
 
 p 
 
 AS 
 
 G 
 
 m 
 rH 
 
 a 
 
 03 
 
 o u 
 
 ip 03 
 
 W 0) 
 P o 
 X 03 
 
 bOMn 
 °H fc 
 
 0) 3 
 
 S 0) 
 
 r-iCM 
 
 H G 
 
 03 °H 
 
 P. 
 
 (1) 
 
 P 
 
 03 
 
 »P 
 
 O TJ 
 <U 
 
 ■H P 
 E 03 
 
 E 
 
 rH °H 
 P 
 
 lp W 
 O <U 
 
 P P 
 
 ,c x 
 
 bO bO 
 
 <H °H 
 II rH 
 
 nfl 
 bO P 
 
 o 
 
 rH P 
 
77 
 
 EXPLANATION OF CALCULATIONS FOR A TYPICAL SAMPLE? BOTTOM SEDIMENT 
 SAMPLE #13 
 
 The major calculations required in the analyses for a typical 
 
 sample, bottom sediment sample #13, are presented in the following para=» 
 
 graphs o Reference to Fig„ 4„1, the flow diagram for the analytical 
 
 procedure, will assist in following the stepwise explanation of these 
 
 calculations. 
 
 Phase I 
 
 A small, representative portion of the sample was counted for 
 total gamma activity on January 22, 1964 „ The count rate was 2463 cpm 
 The portion of the sample was then dried and weighed „ The dry weight, 
 13„9 g, indicated a total gamma activity of 177 cpm/g on January 22, 1964 
 
 A second representative portion of the sample was acid washed 
 and the eluate concentrated by evaporation to a volume of 45 ml„ The 
 residue was dried and found to weigh 351 g A portion of the residue was 
 weighed and counted in the gamma scintillation counter with a result of 
 404 cpm for a 14„1 g dry weight portion, or 30 8 cpm/g on January 22, 1964 
 
 The remaining sample was dried and weighed with a resulting dry 
 weight of 1207 g for the complete sample 
 
 Phase II 
 
 A 10 ml aliquot of the concentrated eluate had a gamma count rate 
 of 10,720 cpm, or 137 cpm/g dry weight of sediment, on January 22, 1964 
 
 4S ml 1 
 Activity (cpm/g) = 10,720 cpm x jfi-~£ X 35TT = 137 Cpnl/g 
 
78 
 The counted sample plus washings were then returned to the 
 remaining concentrated eluate j, increasing the volume to 52 ml 
 
 A one ml aliquot of the concentrated eluate was taken and diluted 
 to 100 ml with deionized water. One ml of the dilution was used for the 
 total zinc test 8 resulting in an absorbance of 253 and a total zinc con- 
 centration of 91 o^ yg/g dry weight of sediment „ 
 
 _ , . „ . , , Absorbance - „ 001 
 Total Zinc (yg) = — 
 
 „04086 
 
 253 - o001 
 
 „04086 
 
 = 6ol? yg in test aliquot 
 
 •v 4 i r,* t , \ a n 100 ml 52 ml 1 
 Total Zinc (yg/g) = 6„17 yg x -— «- — x ~TT x 
 
 1 ml 1 ml 351 g 
 = 91 o 4 Mg/g of sediment 
 
 A five ml aliquot of the concentrated eluate was used for the 
 total cobalt testj resulting in an absorbance of „024 and a total cobalt 
 concentration of o 06 yg/g dry weight of sediment „ An additional five ml of 
 the concentrated eluate was lost 
 
 rr 4. i n u 14. / \ Absorbance - o 004 
 Total Cobalt (yg) = o009296 
 
 _024 - o004 
 o009296 
 
79 
 = 2 16 yg in test aliquot 
 
 Total Cobalt (ug/g) = 2 16 ug x ~~ x -J— 
 
 = 0O6 ug/g of sediment 
 
 In the tests for total zinc and total cobalt , eleven ml of the 
 concentrated eluate had been used up A correction factor of 1 27 was 
 applied to sample volumes in succeeding tests, to account for this loss in 
 sample „ 
 
 Phase IV - Zinc and Zinc 
 
 The eluate from Phase III, containing the zinc fraction, was 
 concentrated to 38 ml Using the correction factor of 1„27 9 this volume 
 was equivalent to 48 2 ml„ 
 
 A one ml aliquot of this concentrated eluate was diluted to 100 ml 
 with deionized water „ One ml of the dilution was used for the total zinc 
 test j, resulting in an absorbance of 129 and a total zinc concentration of 
 43 ug/g dry weight of sediment „ The concentration was computed in a 
 manner similar to that used in Phase II s as described in a preceding para- 
 graph c 
 
 A ten ml aliquot of the concentrated eluate was counted for gamma 
 
 activity on February 7, 1964 „ It contained an activity of 4855 cpm $ or 
 
 65 
 66»8 cpm/g, or 139 pc/g as Zinc Applying a decay factor of O 606 9 this 
 
 activity became 230 pc/g as Zinc on the date of collection of the sample, 
 
 August 15 s 1963 „ 
 
80 
 
 , nrr 48 o 2 ml 1 
 
 Activity = 4855 cpm x 1Q ml x 3^ 
 
 = 66 o 8 cpm/g on February 7, 1964 
 
 . . 65 __ _ - 1 disintegrations 1 min 
 
 Activity as Zinc = 6608 cpm/g x - - -- '■■ • ••• >• » ■■ x _ n 
 
 J ,230 count 60 sec 
 
 = 5„14 dps/g 
 
 = 5 14 dps/g x E £ 
 
 = 2 
 3 7 x 10 dps 
 
 65 
 = 139 pc/g as Zinc on February 7, 1964 
 
 Decay Factor = ,-(.693/T 1/2 )(t) 
 
 65 
 where the half-life, T , , for Zinc = 245 days and t = 176 days 
 
 =(„693/245)(176) 
 = e 
 
 = „606 
 
 .65 
 Activity as Zinc on August 15, 1963 
 
 139 pc/g x -§- 
 
 230 pc/g dry weight of sediment 
 
Phase IV - Cobalt and Cobalt 
 
 81 
 
 60 
 
 The eluate from Phase III, containing the cobalt fraction, was 
 concentrated to 52 ml Using the correction factor of 1 27, this volume 
 was equivalent to 66 o ml„ 
 
 A twenty ml aliquot of this concentrated eluate was used for the 
 total cobalt test, resulting in an absorbance of 332 and a total cobalt 
 concentration of 33 pg/g dry weight of sediment The concentration was 
 computed in a manner similar to that used in Phase II, as described in a 
 preceding paragraph „ 
 
 A ten ml aliquot of the concentrated eluate containing the cobalt 
 fraction was counted for gamma activity on February 4, 1964 It contained 
 an activity of 504 cpm, or 9 48 cpm/g, or 12 2 pc/g as Cobalt „ Applying 
 a decay factor of „939, this activity became 13 o pc/g as Cobalt on the 
 
 date of collection of the sample, August 15, 1963 „ The calculations were 
 
 65 
 similar to those used to compute the Zinc ' activity The counter effi- 
 ciency factor was ,367 instead of „230, and the half -life was 5,27 years 
 instead of 245 days,, 
 
 RADIOACTIVITY RELATED TO SURFACE AREA 
 
 65 
 The total gamma activity^ the zinc activity as Zinc , and the 
 
 fif) 
 
 cobalt activity as Cobalt for bottom sediment samples related to ground 
 surface area, are presented in Table 7 4 
 
 A typical sample, bottom sediment sample #13, was composed of a 
 disc of sediment 75 in thick with a ground surface area of 50 3 in „ The 
 sample had a dry weight of 1207 g and a total gamma activity of 172 cpm/g, 
 
 as adjusted in Table 7 1, on January 22, 1964 It had a zinc activity of 
 
 65 
 230 pc/g as Zinc on August 15, 1963 8 and a cobalt activity of 13 „0 pc/g 
 
82 
 
 as Cobalt on August 15 , 1963 „ Each of these values has been multiplied 
 by the sample weight and divided by the area of the ground surface face of 
 the disc of sediment to obtain the values presented in Table 7<,4 
 
83 
 
 VIII o DISCUSSION OF RESULTS OF ANALYSES 
 
 QUALITATIVE PROOF OF ISOLATION OF ZINC 65 AND COBALT 60 
 
 Figo 8 1 is composed of six waveforms produced with the gamma 
 scintillation spectrometer „ A concentrated composite sample of the isolated 
 zinc fractions was scanned twice and compared with two scans of a standard 
 Zinc " sample o A concentrated composite sample of the cobalt fractions 
 was scanned and compared with a standard Cobalt sample „ The instrument 
 settings for each sample type were identical „ The activities of the com- 
 posite sample and the standard were similar, in both cases „ The resulting 
 waveforms are very similar From this qualitative check it can be con- 
 cluded that all of the measurable activity in the composite zinc sample was 
 caused by Zinc , and that all of the measurable activity in the composite 
 cobalt sample was caused by Cobalt 
 
 PRECISION OF ANALYTICAL RESULTS 
 
 Precision is a measure of the scatter around the mean The 
 precision of the analytical results is summarized in Table 8<,1» 
 
 Zinc 
 
 The standard deviation of the total zinc determination was 
 ± 189 yg/test aliquot „ The zinc concentrations of the test aliquots ranged 
 from five to fifteen yg The standard deviations of the total zinc deter- 
 minations would therefore range between *o9 and *2 6 percent, with an 
 average of approximately ±lo5 percent „ 
 
 Cobalt 
 
 The cobalt concentrations were generally quite low The precision 
 of the analytical results is therefore a function of the limit of detection 
 
84 
 
 
 1 miinruimufi i imnmnuiH— 1 ' ' """'..llllliljili 
 
 im . M - it— m - wan 
 
 
 
 
 lllll'lll Hill 
 
 
 
 1 kii ; J* 
 
 •1.. lm • 15 
 1 XV Il» -If »■ 
 
 ■iiiniiiiiiiiiiiiiiiii: i iiiim iiih Hiiiimiiiiiii 
 
 ■lllllllllllllllllllll! lilllllllllll: I1IIIIIIIIIIIIHIII 
 
 
 
 
 
 
 
 
 
 
 ill I ill! li 
 
 
 II 
 
 
 
 111 
 
 
 I I 
 
 1 
 
 
 ill 
 
 
 
 
 
 
 
 
 
 
 
 M 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 illinium;' ; 
 
 
 
 
 
 
 L 
 
 
 '"llllV'n,, 
 
 
 
 
 
 
 1 
 
 
 
 
 
 
 
 J-k'Sfil 
 
 illllllillllHi 
 llllllllillll;:;: 
 
 
 
 
 
 
 it 
 
 l%Wm 
 
 
 
 
 
 
 .1 
 
 H 111 
 
 
 
 
 
 
 
 1. J ,( 
 
 
 
 
 
 
 
 
 tor 
 
 
 
 
 
 
 
 r 
 
 1 II lllllllllll 
 
 
 lulllll 
 
 « m m m m m m .1 m 
 
 si m m m m m m .1 ■« 
 
 J J 4 1 .t • • t 14 UM M 
 1 1 4 4 4 J J J II UU ML. 
 
 
 liiiiiiiiiiiiiiiuiiiiiiiiiiiiiiiiiiiiiii 1 1 nil 
 
 1 UK - •» - ITMMM - MM #1 
 
 ■P" : ISii" * 
 
 1 »im» • 1 
 
 TIM IMIM< • If 
 
 1 am. fc-ir • )t» 
 »•■ «*rw • t» 
 
 1 Urn TIM ■ If ll> 
 
 ttt; ■ 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 II lllllllllilliil llllltllii 
 
 
 
 III' 
 
 
 
 
 
 
 
 iiiii Limn 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 IIIMIIIIIIIIWIH 
 
 
 
 
 
 
 
 
 
 ill 
 
 II! 
 Ill 
 
 
 
 
 
 
 
 
 
 lllllllllll 
 
 
 
 
 
 
 
 
 
 fnnmra 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 'TT 
 
 
 i! 
 
 
 
 
 
 I 19 I 
 
 
 
 
 
 
 
 1 IN. 
 
 
 Willi!!! 
 
 
 iniiiiiiiiiiiiiniiiiiiiiiiiiiiiiiinM 
 
 comit - to - inuuuu 
 
 1 II 
 
 ii 
 
 
 ii in IIJIll III | 
 
 
 
 liiiii 
 
 
 
 Activity - U» cf- 
 
 t**fa • IM 
 
 tfU4o. - S 
 TltTS (OIIIMI - » 
 HI*. IfWfT * » 
 *- fc-rjy - US 
 Sew T1» - IS !•■» 
 
 1 
 
 
 
 
 
 
 
 
 
 
 III lln 
 
 
 
 i L 
 
 
 
 
 
 f 1 fl i 1 [lliNillliTli IHitl ; 1 1 1 nln llaMi-lBtg 
 
 lm If 'III llifflNi ' 
 
 H 
 
 
 i 
 
 
 
 
 
 mi ii iiim i ; mn 1 iiiiiii 
 
 
 HlflllHi; 
 
 hi iI.iiii 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 'iiiiiifi 
 
 
 
 
 
 
 
 
 
 
 
 IJIJJIIJ It 
 
 11 
 
 
 
 
 
 
 ■ 
 
 ill 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 1 II 1 ' 1 31 111 
 
 
 
 
 
 
 
 
 
 
 
 Dill i 111 Ills 
 
 
 
 
 
 
 
 
 
 
 
 II li I II II 111 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 lllllllllilliil lllllllllll 
 
 i ii iiiiiniiirm 
 
 
 
 niiiiniiiiiiiHiiiiiiiiiiiiiiiiH 
 
 Mill 
 
 Jllil^WL 
 
 n 
 
 m 
 
 lllllllllll 
 
 IIIIIII 
 
 |l;l|i! 
 
 
 CMM.T - tO - OftWOtm IMU 
 
 Hi IIP 
 
 i lllllllllilliil 
 
 
 ' 
 
 ii 
 
 
 Aul.lty - 1» •-— 
 
 «-f - »• L 
 
 
 
 
 
 
 1 
 
 
 Tl» Cmium - 10 
 
 
 Pi 
 
 
 S««n Tl«« - IS Hi 
 
 i II 
 
 in inU lii 
 
 
 
 P'l 
 
 TUT i 
 
 ' ll|j!i| 
 
 
 
 
 
 
 
 Uiii.ii II 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 jjiyjll 
 
 
 
 I 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 tiffi 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 II M If 
 
 
 jlfflllli 
 
 
 
 
 
 
 
 ill IP 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 
 iiiiiiiiiiiiii™ 
 
 Fig. 8.1 
 
 COMPARISON OF ZINC 65 AND COBALT 60 COMPOSITE 
 SAMPLES WITH STANDARDS 
 
85 
 
 inherent in the determination and should be consid<.~ed in terms of yg/g 
 rather than in terms of percent . The standard deviation of the total 
 cobalt determination was ^0648 yg/test aliquot „ Approximately one=third 
 of each cobalt fraction (Phase IV) was used for the determination If the 
 total weight of each sample is considered 9 the resulting standard deviations 
 for total cobalt are approximately ± o 000 i + yg/g for water samples, 4 1.0 yg/g 
 for plankton samples and *. 006 yg/g for bottom sediment samples „ 
 
 Table 8 i 
 
 PRECISION OF ANALYTICAL RESULTS 
 
 Analysis 
 
 Total Zinc 
 
 Total Cobalt 
 
 Zinc 
 
 65 
 
 Cobalt 
 
 60 
 
 Sample Type 
 
 Water 
 
 Plankton 
 
 Bottom Sediments 
 
 Water 
 
 Planxton 
 
 Bottom Sediments 
 
 Water 
 
 Plankton 
 
 Bottom Sediments 
 
 Activity < 13 pc/g 
 Activity > 13 pc/g 
 
 Water 
 
 Plankton 
 
 Bottom Sediments 
 
 Precision 
 [ Standard Deviation) 
 
 ± 
 1 
 
 i 
 
 L 5% 
 1.5% 
 
 1 5% 
 
 ± 
 
 ± 
 
 oOOOU yg/g 
 1.0 yg/g 
 o 006 yg/g 
 
 i 
 i 
 
 o0C05 pc/g 
 1.5 pc/g 
 
 i 
 
 o2 pc/g 
 1.5% 
 
 i 
 A 
 1 
 
 .0005 pc/g 
 10 pc/g 
 .1 pc/g 
 
 65 
 
 65 
 
 The Zinc ' activities of the water samples were low and close to 
 the detection limit of the gamma scintillation counter. The standard 
 deviation of the counting precision 8 based on several five=minute counts 
 and based on samples containing activities close to backgrounds, is approxi- 
 mately *5 cpm. This precision is equivalent to a standard deviation of 
 
86 
 
 65 
 
 approximately ^0005 pc/g for Zinc activities in water samples, 
 
 Plankton samples contained high Zinc ' activities , The precision 
 of the results for plankton can therefore be based on the precision of the 
 estimation of efficiency of Zinc counting. The standard deviation for 
 plankton samples is therefore approximately ± 35 x 100/23,0 = *1,5 percent. 
 
 The Zinc activities of the bottom sediment samples ranged from 
 low to relatively high valueSo Samples with low activities would have a 
 standard deviation of *5 cpm 8 or a precision equivalent to a standard devia- 
 tion of approximately i 2 pc/g Samples containing activities greater than 
 13 pc/g have a standard deviation based on the precision of the estimation 
 of counter efficiency and would therefore have a standard deviation of 
 approximately *1„5 percent , 
 
 Cobalt 60 
 
 60 
 All of the samples contained low Cobalt activities. Based on a 
 
 standard deviation of *5 cpm for counting precisions, the standard deviations 
 
 fin 
 for Cobalt determinations are approximately i o 0005 pc/g for water samples, 
 
 i 10 pc/g for plankton samples 9 and *„! pc/g for bottom sediment samples. 
 
 ACCURACY OF ANALYTICAL RESULTS 
 
 The accuracy of experimental determinations is a measure of the 
 difference between the true values and the experimental values. 
 
 Losses in the elution of zinc and cobalt cations from the cation 
 
 and anion exchange resins would produce results lower than the true values, 
 
 65 60 
 
 Based on the results of tests made with Zinc and Cobalt tracers B losses 
 
 from these sources are considered to be negligible. Errors caused by con= 
 
 tamination of reagents and glassware and losses due to adsorption on glass 
 
 surfaces with which the samples came into contact are also considered to be 
 
87 
 small and to have a negligible effect on the accuracy of the results. All 
 
 determinations of zinc and cobalt were made using the same equipment, pro- 
 
 65 
 cedure and reagents used to produce the standard equations „ Zinc ' and 
 
 fin 
 Cobalt activities were measured using the same instrument settings, sample 
 
 sizes and sample containers used in establishing the gamma scintillation 
 
 counter efficiency for each radionuclide , 
 
 Table 7,2 contains the results of determinations of total zinc 
 and cobalt both before and after separation of each of these elements from 
 the samples o Both determinations, as made in Phase II, may have been sub- 
 ject to considerable error. Interference in color development caused by 
 the presence of relatively high concentrations of other ions is quite prob- 
 able o The presence of these ions could have reduced or increased the 
 absorbance of light at the particular wavelengths used in the determinations, 
 The presence of turbidity, as noticed in some of the Phase II cobalt deter- 
 minations, would produce erroneously high results. Because the water 
 samples were collected in cation exchange resin, the samples analyzed in 
 Phase II contained only cations and chloride anions. The plankton and 
 bottom sediment samples analyzed in Phase II contained everything that 
 would be eluted from the samples in the acid wash procedure The results 
 obtained after separation would not have been subject to interference from 
 other ions. Therefore, the results obtained in Phase II are considered to 
 be approximate only. The results obtained in Phase IV, for total zinc and 
 cobalt, are considered to be accurate. 
 
 The analyses for total gamma activity commenced approximately 
 three months after collection of samples and continued over a four=month 
 period, as shown in Table 7,1, In samples containing an unknown mixture 
 of radionuclides, the rate of decay cannot be calculated. The total gamma 
 
88 
 
 activities of these samples could not be converted to a constant date, as 
 was done with the Zinc ' and Cobalt fractions. Comparison of total 
 gamma activities with Zinc ' and Cobalt activities is therefore subject 
 to this lack of uniformity in time The efficiency of the gamma scintil- 
 lation counter for counting total gamma activity is also unknown „ The 
 
 efficiency has been approximated by using that of the major isotope, 
 
 „. 65 
 
 Zinc 
 
 TOTAL GAMMA ACTIVITY 
 
 The total gamma activities of the samples were measured primarily 
 to ascertain the proportion of the total activity of each sample caused by 
 Zinc ' and Cobalt , It was expected that samples having high total gamma 
 activities would have correspondingly high Zinc ' and Cobalt activities „ 
 The results of these analyses have been presented in Table 7„lo 
 
 Total gamma activities of the eluate plus the residue after acid 
 washing of each bottom sediment sample should have been equal to the total 
 gamma activity of each sample before acid washing „ Due to the natural 
 variation in a heterogeneous material such as bottom sediment 9 it was diffi- 
 cult to obtain representative portions , and the results fluctuate consid= 
 erably The sample and the residue data are based on 10 to 15 g portions, 
 whereas the eluate data is based on 250 to 350 g portions, both as dry 
 weights o The eluate data is therefore much more precise than the sample 
 and residue data,, 
 
 The percent elution of gamma activity by acid washing of plankton 
 samples varied from 81 to 91 percent „ The percent elution from bottom 
 sediment samples by this treatments as shown in Fig 8 2 8 varied from 
 between 9 and 61 percent for samples having activities less than 30 cpm/g, 
 to between 56 and 80 percent for samples having higher activities „ There 
 
89 
 is an apparent increase in degree of desorption with increasing concentra- 
 tion of total gamma activity, indicating that desorption in an acid medium 
 is a function of the concentration of ions causing gamma activity asso- 
 ciated with the sample o 
 
 It is assumed that assimilated ions producing gamma activity in 
 plankton are not eluted by acid washing, and that these ions when adsorbed 
 on the plankton surfaces are eluted by this treatment „ The results indicate 
 that adsorption of ions causing gamma activity is the major mechanism of 
 uptake by plankton „ However, these samples had been stored for several 
 months in sealed glass containers, and the results might have been quite 
 different if freshly collected samples had been analyzed „ 
 
 It is assumed that ions producing gamma activity occupying 
 positions within the crystal lattice structures of clay particles in the 
 bottom sediments, or incorporated into the sediments by other mechanisms, 
 are not eluted by the acid wash treatment „ It is also assumed that these 
 ions when adsorbed on the surfaces of the sediments, or attached to charged 
 sites on the surfaces of these particles, are eluted by acid washing of the 
 sediment o The results indicate that adsorption and attachment to charged 
 sites on the surfaces of the sediments, of ions causing gamma activity, are 
 the major mechanisms of uptake by the bottom sediments if these samples 
 contain high total gamma activities „ 
 
 COMPARISON OF TOTAL GAMMA ACTIVITY WITH ZINC 65 AND COBALT 60 ACTIVITY 
 
 Table 7„3 contains data concerning the percent of the total gamma 
 activity of each sample and of the eluate from acid washing of each sample, 
 on the date of measurement of the total gamma activity, caused by Zinc 
 and by Cobalt „ The total gamma activities of each sample and eluate have 
 been converted from cpm to pc/g by assuming a counting efficiency factor of 
 
90 
 
 65 
 
 ,230, based on that of the major radionuclide in tnese samples , Zinc , in 
 
 order to compute the percentages given in the table. 
 
 Three water samples were analyzed for Zinc ' and Cobalt „ The 
 
 activities of these samples were close to the detection limits of the 
 
 65 
 analytical equipment Results, although doubtful, indicate that Zinc 
 
 fin 
 and Cobalt each comprised less than ten percent of the cationic activity 
 
 of the water, several months after the samples were collected , The activity 
 
 caused by each radionuclide appeared to decrease as the total cationic 
 
 activity decreased „ These results indicate that Zinc ' and Cobalt would 
 
 not become major radionuclides in the water phase of the aquatic environment, 
 
 even after a decay period of several months „ 
 
 65 
 In the four plankton samples analyzed, the Zinc ' activities 
 
 ranged from 47 to 66 percent of the total gamma activities of the samples, 
 
 and from 55 to 72 percent of the total gamma activities eluted by the acid 
 
 fi s 
 
 wash treatment, at six months after sampling „ The Zinc ' activity appeared 
 
 to increase with decreasing total gamma activity. Cobalt activities were 
 
 very low and accounted for less than two percent of the total gamma activi- 
 
 65 
 ties at six months after sampling The results indicate that Zinc is the 
 
 major radionuclide associated with plankton at a period six months after 
 
 sampling, 
 
 6 S 
 Figo 8 3 indicates the relationships between the Zinc activities 
 
 and the total gamma activities of the samples and of the eluates from acid 
 
 washing, for bottom sediments. In the twenty-four bottom sediment samples 
 
 analyzed, the Zinc ' activities ranged from to 52 percent of the total 
 
 gamma activities of the samples, and from to 65 percent of the total gamma 
 
 activities eluted by the acid wash treatment. For all samples having total 
 
 gamma activities greater than 20 cpm/g, at least 23 percent of the activity 
 
 of each sample, and at least 30 percent of the activity of each eluate, was 
 
40 
 
 80 120 160 
 Total Gamma Activity - (cpm/g) 
 
 200 
 
 240 
 
 Fig. 8.2 VARIATION IN PERCENT OF TOTAL GAMMA ACTIVITY ELUTED FROM BOTTOM 
 
 SEDIMENTS WITH TOTAL GAMMA ACTIVITY OF SAMPLE 
 
 o 
 c: 
 
 n 60 
 
 40 
 
 20 
 
 - D 
 
 
 
 D 
 
 K) ft 
 
 D 
 
 d 
 
 CD 
 
 
 L o 
 
 D °° 
 
 o 
 n oo 
 
 D 
 
 oo 
 
 PO- 
 
 o 
 
 D 
 
 O 
 
 O 
 
 O 
 
 40 
 
 1 
 
 D O 
 
 O 
 
 Legend: 
 
 O Sample 
 
 DEluate 
 
 80 120 160 
 Total Gamma Activity - (cpm/g) 
 
 200 
 
 240 
 
 Fig. 8.3 
 
 VARIATION IN PERCENT OF TOTAL GAMMA ACTIVITY DUE TO ZINC 
 FROM BOTTOM SEDIMENTS WITH TOTAL GAMMA ACTIVITY 
 
 65 
 
92 
 caused by Zinc „ The total gamma activities of tL„ bottom sediment 
 samples were measured during a period of from three to five and a half 
 months after sampling „ The results indicate that for all sediments con- 
 taining an appreciable total gamma activity, Zinc ' is a major radionuclides, 
 during a period commencing several months after sampling „ 
 
 C A 
 
 The Cobalt activities of the bottom sediment samples were low, 
 but the determinations were reasonably precise „ The percentage of the total 
 activity caused by this radionuclide remained relatively constant, in a 
 range of from 1„2 to 5„6 percent of the total gamma activity of each sample 
 and from 1„8 to 10 percent of the total gamma activity of the eluate from 
 acid washing of each sample, within the reach of the Columbia River upstream 
 from McNary reservoir,, Within the reservoir, the activity increased to 
 6 1 percent and then dropped off to less than o percent of the total gamma 
 activity,, In this reach, the activity increased to 37 percent and then 
 
 dropped off to less than „0 percent of the total gamma activity of the 
 
 60 
 eluate from acid washing „ These data indicate that Cobalt is a minor 
 
 radionuclide in the sediments, but that within McNary reservoir , it may be 
 
 one of the major radionuclides that would be desorbed from the sediment 
 
 under acid conditions,. 
 
 COMPARISON OF TOTAL ZINC AND TOTAL COBALT WITH ZINC 55 AND COBALT 60 
 
 Table 7 5 contains the results of analyses of the Columbia River 
 
 c tr c a 
 
 samples for total zinc, total cobalt, Zinc and Cobalt 
 
 In the water and plankton samples, changes in total zinc concen- 
 
 . . 65 
 
 tration are accompanied by similar changes in Zinc activity „ This trend 
 
 65 
 is not followed by the bottom sediment samples „ The Zinc activity of the 
 
 sediments appears to be almost completely unrelated to the total zinc con- 
 
 RD 
 
 centration of the sediments , The Cobalt activities of all samples appear 
 
93 
 
 to be unrelated to the total cobalt concentrations of the samples „ 
 
 65 
 These data indicate that changes in Zinc ' concentration in the 
 
 soluble phase are a function of the total zinc concentration in the soluble 
 
 phase o It is possible that the plankton contain such a high concentration 
 
 of zinc adsorbed on their surfaces that the ions are loosely held, resulting 
 
 in a continuous flux of ions between the surfaces of the plankton and the 
 
 soluble phase o The total zinc concentration associated with the bottom 
 
 sediments may be far below saturation,, This condition would result in rapid 
 
 65 
 uptake of both zinc and Zinc „ The adsorbed ions may be tightly held by 
 
 the sediment o 
 
 60 
 The Cobalt activities of water and plankton samples were close 
 
 60 
 to the limit of detection and the results are doubt ful The Cobalt 
 
 activity of the bottom sediments may be unrelated to the total cobalt con- 
 centration of the sediments, for the same reasons as discussed for zinc 
 
 = 6 
 
 Of the total zinc, less than 6 x 10 percent was radioactive „ 
 
 -4 
 Of the total cobalt, less than 5 x 10 percent was radioactive „ Percent 
 
 radioactivity did not appear to be related to sample type as it was similar 
 
 in each of the water, plankton and bottom sediment types of samples „ 
 
 EFFECT OF LOCATION OF SAMPLES 
 
 The location of the water , plankton and bottom sediment samples 
 collected from the Columbia River has been shown in Fig 6 o l Location 
 details have been included in Tables 6„1 9 6„2 and 6 3 
 
 Water and plankton samples were taken in midstream from the 
 flowing water. Bottom sediment samples were collected along the shorelines 
 of the river in a reach extending from just upstream of the Hanford reactors 
 to just below McNary dam, a distance of almost one hundred river miles , 
 
94 
 
 Location of Bottom Sedi ment , ., Samples _ Relav ive ^ to the Water Surface 
 Level of t he Columbia River 
 
 As shown in Fig lo3 8 on the date of collection of the bottom 
 sediment samples, the flow of the Columbia River was receding from the peak 
 flow which occurred six weeks prior to sampling „ The flow at Pasco had 
 receded steadily from a peak of 290 , 000 cfs on July 1 to about 140,000 cfs 
 by August 15 o During the major part of preceding years, the flow had been 
 well below 140,000 cfs„ Bottom sediments located along the shorelines of 
 the river on August 15, 1963, had therefore likely been exposed to reactor 
 effluent contamination only during a few months of each year. They could 
 not have been continuously exposed to reactor effluent contamination unless 
 they had been translocated from sediments in the river bottom during the 
 high water period of June and July, 1963 „ Based on the preceding discussion, 
 it would be expected that the sediments collected in this study would con- 
 tain considerably less radioactivity than sediments collected along the 
 shorelines of the river during the low flow period of the year 
 
 Location o f Bottom Sediment Samples Re lat ive to the Flow Velocity 
 of the Col umbia Riv er 
 
 The Columbia is a swift flowing river throughout the reach from 
 
 the Hanford reactors to Richland In this reach a considerable amount of 
 
 translocation of bottom and shoreline sediments can be expected to have 
 
 occurred during the flood period just prior to sampling „ Sediments in one 
 
 location along the shoreline may have been there only a few weeks previous 
 
 to sampling and may have originated from a variety of upstream locations 
 
 Some of the sediments may not have been exposed to reactor effluent contam- 
 
 inated water during previous years Other patches of sediment along the 
 
 shoreline in the same reach of the river may have been deposited several 
 
 years or more in the past and been exposed to reactor effluent contaminated 
 
95 
 water for several months each year,, Still other seaxments may have been 
 translocated from areas which received continuous contact with reactor 
 
 effluent contaminated water „ The sediments from this reach can therefore 
 
 65 
 be expected to contain widely fluctuating concentrations of Zinc ' and 
 
 fin 
 Cobalt 
 
 Within McNary reservoir, downstream from Richland, scouring and 
 translocation of bottom sediments is not as likely, due to the reduced 
 flow velocity of the water „ Some of the sediments scoured from the upstream 
 reach during flood periods are transported in the water and deposited in the 
 reservoir Erratic values of Zinc and Cobalt activities within the 
 reservoir are not as likely to occur as would be expected within the up- 
 stream reach of the river „ 
 
 Total Gamma Activity 
 
 The total gamma activities of the cationic fractions of the water 
 samples collected near Richland, near Pasco and near McNary dam, were less 
 than 28 percent of the total gamma activity of the cationic fraction of the 
 sample collected near Hanford, indicating that the major portion of the 
 cations had rapidly been removed from the soluble phase „ However 9 the 
 total gamma activities of these samples did not decrease consistently with 
 distance downstream from the Hanford reactors „ The total gamma activities 
 of the plankton samples decreased consistently with distance downstream 
 from the Hanford reactor area Bottom sediment samples increased in total 
 gamma activity through the reactor area and then decreased with further 
 movement downstream The variation of the total gamma activity of the sedi- 
 ments with location closely followed the variation pattern of Zinc 
 activity with location „ 
 
96 
 
 Zinc and Cobalt 
 
 The total zinc and cobalt concentrations of water and plankton 
 samples decreased with distance downstream from the reactor area, except 
 for the plankton sample collected near McNary dam, which contained a higher 
 concentration of both zinc and cobalt than samples farther upstream „ The 
 variation in total zinc concentration with location of bottom sediment 
 samples is shown in Fig„ 8 Ho On the reactor shore , the concentration is 
 highest above the reactor area and decreases with distance downstreanu On 
 the opposite shore, the concentration of zinc is low in the reactor area 
 and increases to values similar to those found on the reactor shore, within 
 a few miles distance downstream from the reactor area The concentrations 
 along both shores then remain similar and decrease with distance, all the 
 way to McNary dam A sample taken below McNary dam was influenced by flow 
 from the Umatilla River „ 
 
 The results indicate that the total zinc concentration of the 
 sediments results from a source of zinc located upstream of the reactor 
 area, and is not affected by the reactor effluents „ The source of zinc may 
 be quite close to the reactor area, upstream, and on the reactor side of 
 the Columbia River , 
 
 The variation in total cobalt concentration with location of 
 bottom sediment samples is shown in Fig 8 5 The data indicate slowly 
 decreasing cobalt concentration with distance downstream, throughout the 
 study area, with the exception of a short reach between the reactor area 
 and the upstream end of McNary reservoir, in which a peak concentration 
 occurred o 
 
97 
 
 I E 
 
 z o 
 
 CO 
 
 o 
 
 
 £ 
 
 a> 
 
 en 
 
 l_ 
 
 
 o 
 
 
 .c 
 
 o 
 
 in 
 
 
 
 u 
 
 
 o 
 
 w. 
 
 (U 
 
 o 
 
 a: 
 
 u. 
 
 ■2 > 
 
 
 ■o 
 
 c 
 
 o 
 
 o 
 cu 
 
 Id 
 
 to 
 
 
 
 o 
 
 
 
 en 
 
 
 CO 
 
 SB 
 
 M 
 
 
 »«■% 
 
 a 
 
 
 w 
 
 w 
 
 
 H 
 
 CO 
 
 
 i 
 
 o 
 
 
 
 i 
 
 
 > 
 
 o 
 
 
 
 a 
 
 IT) 
 
 u. 
 
 CM 
 
 
 o 
 
 n 
 
 1 
 
 5= 
 
 
 c 
 
 o 
 
 
 o 
 
 M 
 
 
 •l-l 
 
 H 
 
 
 •M 
 
 < 
 
 
 f8 
 O 
 
 8 
 
 
 
 
 j 
 
 
 •J 
 
 X 
 
 
 0) 
 
 F- 
 
 
 H 
 
 M 
 
 
 C, 
 
 
 
 co 
 
 55 
 
 U"> 
 
 
 M 
 
 J" 
 
 •p 
 
 N 
 
 00 
 
 c 
 
 
 
 8 
 
 < 
 
 
 •H 
 
 f- 
 
 
 T3 
 
 O 
 
 
 <D 
 
 H 
 
 
 CO 
 
 u< 
 
 
 S 
 
 O 
 
 
 o 
 
 
 
 ■p 
 
 IS 
 
 
 +J 
 
 o 
 
 
 
 
 M 
 
 
 CQ 
 
 52 
 
 as 
 
 LO 
 
 
 < 
 
 UD 
 
 
 > 
 
 co 
 
 
 
 o 
 o 
 
 CN 
 
 (^8faM itap 2/Srt ) - oujz t«1<>1 
 
 ao 
 
 2* 
 
 Cm 
 
98 
 
 | > 
 
 I e 
 
 Z o 
 
 o 
 
 > 
 
 L. 
 
 0) 
 
 o: 
 
 a> 
 
 
 u. 
 
 
 O 
 
 
 JZ 
 
 a> 
 
 CO 
 
 t_ 
 
 
 o 
 
 
 .c 
 
 o 
 
 in 
 
 
 
 u 
 
 
 o 
 
 w 
 
 0) 
 
 O 
 
 a: 
 
 u_ 
 
 
 C a) 
 
 .-si: > 
 
 c 
 
 0) 
 
 UJ 
 
 CO 
 CM 
 
 o 
 
 n 
 
 > 
 
 C 
 
 o 
 
 .-I 
 
 *J 
 
 O 
 
 o 
 
 a. 
 
 L0 
 
 4-< 
 
 C 
 4) 
 F 
 
 <y 
 in 
 
 e 
 o 
 ■♦■■' 
 
 o 
 
 en 
 
 in 
 
 '-O 
 
 in 
 ao 
 
 (iq:-r^M Aap ?/2rt) - UPqoo tpioj. 
 
99 
 
 n- 65 A n v ^ 60 
 
 Zinc and Cobalt 
 
 65 
 The Zinc activities of the water samples decreased rapidly with 
 
 distance downstream from the reactor area,, The activity decreased 85 per= 
 
 cent in the 18<=mile reach between sample #2 and sample #3 8 and decreased 
 
 54 percent in the 33<,5~mile reach between sample #3 and sample #4 The 
 
 Zinc ' activities of the water samples were low and the data very limited, 
 
 but the data indicate rapid removal of Zinc ' from solution The Zinc 
 
 activity of the plankton samples decreased slowly with distance downstream 
 
 from the reactor area 
 
 65 
 Fig 'So 8 6 and 8„7 depict the variation in Zinc ' activity of 
 
 bottom sediments on a dry weight basis and on a ground surface area basis g 
 
 respectively,, The shapes of the curves in each figure are similar,, The 
 
 fi c 
 Zinc ' activity above the reactors is negligible „ The activity increases 
 
 through the reactor area and for about 40 miles downstream of the reactor 
 
 area,, and then decreases with distance downstream „ The activity on the 
 
 reactor shore of the river is much higher than on the far shore in the 
 
 reactor area and downstream to below Pasco „ In the reach below Pasco 8 the 
 
 65 
 Zinc activity is more evenly distributed along both shores of the Columbia 
 
 65 
 River The data indicate that the Zinc ' activity is not rapidly dispersed 
 
 across the width of the Columbia River and that the major portion of the 
 
 65 . . . 
 Zinc activity associated with the sediments 9 on a concentration per gram 
 
 dry weight or on a concentration per square inch of sediment basis 8 occurs 
 
 in a 40 to 50 mile reach of the Columbia River extending downstream from 
 
 the reactor area 
 
 fin 
 Fig' So 808 and 8 9 depict the variation in Cobalt activity with 
 
 location of bottom sediments on a weight basis and on a ground surface area 
 
 basis 8 respectively o The shapes of the curves in each figure are similar „ 
 
 60 
 The variation in Cobalt activity with location of sediments is similar to 
 
100 
 
 o ' 
 
 
 
 5 * 
 
 
 «\ 
 
 - Ei 
 
 
 \ 
 
 
 1 6 
 
 
 \ - 
 
 
 Z o 
 
 
 \ 
 
 
 2 
 
 
 
 
 
 1 
 t 
 
 ■ 
 
 
 0) 
 
 I _ 
 ■ 
 
 
 
 o 
 
 1 
 
 
 
 ■C 0) 
 
 
 
 
 en »- 
 
 
 
 
 
 o 
 
 
 
 >» 
 
 kp 
 
 ,_ -c 
 
 
 
 k. 
 
 o 
 
 o 
 
 > 
 
 5 to 
 
 
 
 z 
 
 i_ 
 
 o 
 
 
 
 u 
 
 0) 
 
 ° *- 
 
 
 ™ 
 
 2 
 
 (A 
 
 <D O 
 
 
 
 0> 
 
 <r u. 
 
 
 
 
 or 
 
 
 
 
 
 
 1 
 
 
 
 0> L. 
 
 
 1 
 
 ^7 
 
 _ 
 
 
 C 
 
 1 
 1 
 
 ^ /' ~ 
 
 
 
 cu 
 a> 
 
 ^ / 
 
 
 is 
 
 _) 
 
 ^ / 
 
 • - 
 
 Yoki 
 
 Riv 
 
 
 y^ / 
 
 
 1 
 
 
 / 
 
 
 
 \ / 
 
 
 
 ^\< 
 
 — 
 
 V 
 
 
 
 
 \ 
 
 
 
 ■ \ 
 
 -^ > 
 
 / 
 
 ■ 
 
 
 ~^^^ - 
 
 . 
 
 
 
 •*—- — " — " " \ 
 
 h_ 
 
 CO 
 
 
 •^zr \ 
 
 o 
 o 
 
 c 
 
 
 
 ^^^^^ n 
 
 o 
 
 r> 
 
 
 
 <D 
 
 •*- 
 
 
 
 or 
 
 UJ 
 
 
 
 i 
 
 r 
 
 1 
 
 1 1 
 
 ii i \ 
 
 o 
 
 O 
 
 o 
 
 o 
 
 o 
 
 o 
 
 •3- 
 
 O 
 
 lO 
 
 CM 
 
 co 
 
 3 
 
 CN 
 
 OJ 
 
 r-\ 
 
 »-t 
 
 
 
 ( iqSxaM Ajp 3/od) 
 
 S9 
 
 OUT 7. 
 
 Ul 
 
 
 
 CO 
 
 
 
 CM 
 
 
 n 
 
 CD 
 
 • 
 
 f- 
 
 u~> 
 
 
 O 
 
 o 
 
 
 3 
 
 ro 
 
 
 < 
 
 * 
 
 ►-< 
 
 
 ^■^ 
 
 < 
 
 
 <u 
 
 CQ 
 
 
 ^ 
 
 
 
 • H 
 
 H 
 
 
 E 
 
 X 
 
 
 h 
 
 n 
 
 
 a 
 
 U> 
 
 
 > 
 
 S 
 
 
 •H 
 
 
 
 l* 
 
 1 
 
 lT> 
 
 ^ 
 
 
 CNt 
 
 
 to 
 
 n 
 
 1 
 
 
 
 c 
 
 UJ 
 
 
 o 
 
 s: 
 
 
 •w 
 
 H 
 
 
 *-> 
 
 Q 
 
 
 TJ 
 
 U 
 
 
 o 
 
 CO 
 
 
 o 
 
 
 
 J 
 
 o 
 
 
 a) 
 
 f- 
 
 
 —i 
 
 H 
 
 
 a* 
 
 O 
 
 
 B 
 
 0Q 
 
 
 tJ 
 
 
 
 i/) 
 
 U, 
 
 in 
 
 
 O 
 
 j- 
 
 4-> 
 
 
 CO 
 
 c 
 
 2 
 
 
 0) 
 
 O 
 
 
 f= 
 
 i— < 
 
 
 •H 
 
 H 
 
 
 X) 
 
 < 
 
 
 0) 
 
 CJ 
 
 
 to 
 
 o 
 
 
 e 
 
 
 
 o 
 
 a: 
 
 
 4-> 
 
 H 
 
 
 ♦-» 
 
 t-t 
 
 
 o 
 
 rs 
 
 
 CO 
 
 in 
 CJ 
 
 in 
 
 
 2 
 
 lO 
 
 
 K-) 
 
 n 
 
 
 S3 
 
 u. 
 o 
 
 25 
 
 o 
 
 »-« 
 
 < 
 
 < 
 > 
 
 in 
 
 
 U3 
 
 00 
 
 
 ■♦ 
 
 ro 
 
 
 CO 
 
101 
 
 1 > 
 
 3 * 
 
 z O 
 
 O Q 
 
 2 
 
 CO 
 
 lO 
 
 m 
 
 o 
 
 o 
 
 o 
 
 o 
 
 o 
 
 o 
 
 o 
 
 o 
 
 c 
 
 o 
 
 o 
 
 o 
 
 00 
 
 o 
 
 <N 
 
 3- 
 
 t£> 
 
 00 
 
 J- 
 
 J 
 
 n 
 
 CN 
 
 •H 
 
 
 
 
 H 
 
 
 
 CO 
 
 
 
 o 
 
 
 
 a 
 
 
 
 n 
 
 
 
 < 
 
 ^n 
 
 
 
 O 
 
 
 • 
 
 n 
 
 
 CO 
 t— 1 
 CO 
 
 < 
 
 03 
 
 
 «•— ■* 
 
 < 
 
 
 <u 
 
 u 
 
 
 >H 
 
 Oi 
 
 
 •H 
 
 < 
 
 
 e 
 
 u 
 
 
 b 
 
 U 
 
 
 0) 
 
 < 
 
 
 > 
 
 u. 
 
 
 •H 
 
 C* 
 
 
 C 
 
 r> 
 
 iT) 
 
 ^ 
 
 CO 
 
 Tj 
 
 
 
 n 
 
 l 
 
 1 
 
 
 C 
 
 CO 
 
 
 O 
 
 f- 
 
 
 •H 
 
 2: 
 
 
 +-> 
 
 u 
 
 
 TJ 
 
 s 
 
 
 O 
 
 »— 1 
 
 
 o 
 
 c 
 
 
 ► J 
 
 CO 
 
 
 0) 
 
 
 
 ^ 
 
 s: 
 
 
 a 
 
 o 
 
 
 e 
 
 H 
 
 
 n3 
 
 E- 
 
 
 CO 
 
 C 
 
 ai 
 
 
 DQ 
 
 S 
 
 *-> 
 
 
 CO 
 
 c 
 
 U. 
 
 
 <u 
 
 o 
 
 
 E 
 
 
 
 • rH 
 
 2 
 
 
 T3 
 
 O 
 
 
 0) 
 
 ■ ' 
 
 
 L0 
 
 < 
 
 
 e 
 
 o 
 
 
 o 
 
 o 
 
 
 M 
 
 J 
 
 
 +-' 
 
 
 
 
 
 X 
 
 
 m 
 
 "J5 
 
 in 
 
 
 in 
 
 cl> 
 
 
 CO 
 
 n 
 
 
 2: 
 
 O 
 
 y. 
 o 
 <— < 
 f-- 
 < 
 
 ft. 
 < 
 
 in 
 
 
 
 CD 
 
 
 
 m 
 
 
 f- j 
 
 ( UT/Od) - OUT' 
 
 I '' ' S9 " 
 
102 
 
 £ 
 
 
 
 
 " "^^^1 ^ 
 
 
 
 1 
 
 Ij 
 
 
 
 5 o: 
 
 
 
 | 
 
 
 
 
 
 1 
 
 
 McNory 
 Dom 
 
 
 
 r - 
 1 
 
 
 
 
 
 1 _ 
 
 
 
 0) 
 
 o 
 
 1 
 
 >i 
 
 k. 
 
 CO «- 
 o 
 
 1 
 
 O 
 
 z 
 
 o 
 
 > 
 
 5 t/> 
 
 1 
 
 <_> 
 
 5 
 
 0) 
 
 <u o 
 a: u. 
 
 1 
 
 
 0> t- 
 
 
 1 
 1 
 
 it 
 
 _ 
 
 Snak 
 Rive 
 
 X) 
 
 c 
 
 1 
 1 
 
 i - 
 i 
 
 
 C~ *- 
 
 _i 
 
 
 i 
 
 • - 
 
 Yakin 
 Rive 
 
 
 
 i 
 
 
 ■ 
 
 
 
 il 
 
 
 
 
 i/ 
 
 
 
 
 \^ 
 
 
 
 
 y 
 
 > 
 / 
 
 ■ 
 
 
 
 ^^ ^^ 
 
 . 
 
 
 
 
 3^\ 
 
 u. 
 
 in 
 
 
 
 < \ 
 
 O 
 
 o 
 
 c 
 ai 
 
 
 
 X v 
 
 o 
 
 3 
 
 
 
 
 <1> 
 
 »*- 
 
 
 
 
 rr 
 
 **- 
 
 Ul 
 
 
 
 
 ■ 
 
 r 
 
 1 
 
 
 1 1 
 
 i i 1 1 
 
 en 
 
 09 
 
 
 
 H 
 
 
 
 00 
 
 
 
 :j 
 
 
 
 u 
 
 
 
 n 
 
 in 
 
 
 < 
 
 O 
 
 
 
 o 
 
 
 on 
 
 < 
 
 CO 
 
 
 a; 
 
 H 
 
 
 H 
 
 X 
 
 
 "4 
 
 c 
 
 
 G 
 
 (—1 
 
 
 U 
 
 •^ 
 
 
 <U 
 
 
 
 > 
 
 1 
 
 
 • -t 
 
 
 
 u 
 
 to 
 
 l/-> 
 
 V—* 
 
 H 
 
 CM 
 
 
 2 
 
 oo 
 
 1 
 
 
 
 c 
 
 ►-H 
 
 
 o 
 
 n 
 
 
 •H 
 
 ux 
 
 
 •M 
 
 00 
 
 
 m 
 
 
 
 u 
 
 jr 
 
 
 o 
 
 o 
 
 
 . 3 
 
 
 
 a> 
 
 O 
 
 
 . < 
 
 CD 
 
 
 (X 
 
 
 
 e 
 
 u. 
 
 
 m 
 
 C 
 
 
 00 
 
 
 iT) 
 
 
 2 
 
 3- 
 
 4-> 
 
 O 
 
 m 
 
 c 
 
 i—i 
 
 
 0) 
 
 H 
 
 
 F= 
 
 <f 
 
 
 ■ f-i 
 
 C_> 
 
 
 TJ 
 
 o 
 
 
 ID 
 
 wj 
 
 
 C/J 
 
 I 
 
 
 e 
 
 H 
 
 
 o 
 
 t— < 
 
 
 •M 
 
 s 
 
 
 M 
 
 
 
 o 
 
 o 
 
 
 m 
 
 to 
 
 H 
 .J 
 < 
 
 lO 
 
 
 m 
 
 OJ 
 
 
 o 
 
 n 
 
 
 CJ 
 
 u 
 
 o 
 
 f 1 
 < 
 
 < 
 > 
 
 in 
 
 
 
 n 
 
 
 ao J 
 
 oo 
 
 
 •H 1 
 
Loa 
 
 o 
 
 
 
 
 *"~ w 
 
 
 
 t 
 
 o « 
 
 
 
 
 e 2 
 
 
 
 1 
 
 3 * 
 
 
 
 
 
 
 
 
 1 
 
 
 1 >. 
 
 
 
 1 
 
 ■ 
 
 1 E 
 
 
 
 
 2 O 
 
 
 
 | 
 
 
 O Q 
 
 2 
 
 
 
 1 
 
 1 
 
 1 _ 
 / 
 
 • 
 
 
 1 
 
 1 
 
 ( 
 
 D 
 
 5 
 
 
 
 -c a> 
 
 / 
 
 
 
 00 >- 
 o 
 
 > 
 
 o 
 
 5 
 
 > 
 
 1 
 
 < 
 
 5 oo 
 
 / 
 
 2 
 
 w 
 
 1 
 
 3 
 
 / 
 
 o 
 
 0) 
 
 < 
 
 3 ^- 
 
 5 
 
 
 0) a 
 
 a: u. 
 
 / 
 
 
 
 
 1 
 
 / . 
 
 
 V k. 
 
 
 1 
 
 / / 
 
 
 -X « 
 
 
 ■ 
 
 
 
 
 •D 
 C 
 0) 
 
 o> 
 
 _J 
 
 1 
 
 1 
 
 i 
 
 'I 
 
 Yakirrx 
 River 
 
 
 
 1 
 1 
 
 
 
 
 1 I 
 
 ■ 
 
 
 
 \\ 
 
 
 
 \ 
 
 
 
 
 > 
 
 
 
 
 \ 
 
 1 
 
 ■ 
 
 
 
 ^^-^< 
 
 
 w 
 
 
 
 
 o 
 o 
 
 c 
 
 
 
 \ l 
 
 o 
 
 3 
 
 
 
 
 • 
 
 »•- 
 
 
 
 
 o: 
 
 LlI 
 
 
 
 
 i 
 
 
 
 
 1 1 II 
 
 - 1 *- 
 
 
 1 1 
 
 
 c 
 o 
 
 
 o 
 o 
 
 o 
 
 U-! 
 
 
 
 X 
 
 
 n 
 
 <N 
 
 
 o 
 -J 
 
 • 
 
 *~( 
 
 E- 
 
 - 
 
 • 
 < 
 
 - 
 
 
 * 
 
 O 
 
 
 ►— 1 
 
 m 
 
 
 id 
 
 < 
 
 < 
 
 
 -^ 
 
 3i 
 
 
 y 
 
 < 
 
 
 *-« 
 
 
 
 •<H 
 
 u 
 
 
 E 
 
 < 
 
 
 *« 
 
 Lm 
 
 
 1 
 
 a: 
 
 
 > 
 
 3 
 
 
 • — 
 
 w 
 
 
 S~ 
 
 
 .- 
 
 1 — . 
 
 i 
 
 r. 
 
 
 
 m 
 
 1 
 
 
 
 IZ 
 
 z: 
 
 
 o 
 
 u 
 
 
 • • 
 
 s 
 
 
 *-• 
 
 1 — 1 
 
 
 - 
 
 a 
 
 
 o 
 
 -: 
 
 
 - 
 
 tfl 
 
 
 ■ 
 
 s: 
 
 
 . 
 
 * 
 
 
 — 
 
 H 
 
 
 
 H 
 
 
 E 
 
 O 
 
 
 - 
 
 23 
 
 
 to 
 
 
 IT 
 
 
 U. 
 
 3 
 
 . 
 
 
 ci 
 
 c 
 
 
 
 1 
 
 12 
 
 
 E 
 
 
 
 - - 
 
 >~t 
 
 
 r 
 
 - * 
 
 
 a) 
 
 - 
 
 
 " 
 
 J 
 
 
 F 
 
 . 
 
 
 
 
 
 
 .- 
 
 — ; 
 
 
 +-> 
 
 - - 
 
 
 . 
 
 — 
 
 
 va 
 
 O 
 
 - 
 
 .- 
 
 
 
 
 
 o 
 z. 
 
 ( «! ^a) 
 
 39 
 
 "J 
 -i 
 
104 
 
 65 
 that found for Zinc except that the activity is much lower with the 
 
 result that the major portion of the Cobalt activity is adsorbed on the 
 sediments in a much shorter distance downstream from the reactor area. 
 
 COMPARISON OF RESULTS WITH DATA OBTAINED BY OTHERS 
 
 Water 
 
 O'Connor et al, (1964) (16) reported that of 34 samples of 
 Columbia River water analyzed by the United States Public Health Service 
 in 1952, 30 contained between 10 and 50 ppb of zinc, and the remaining four 
 contained between 50 and 130 ppb of zinc Silker (1964) (25) stated that 
 samples of water taken upstream of the Hanford reactors during the period 
 from January 5 to August 17, 1962, ranged from 2„4 to 37 „ 6 ppb of zinc and 
 001 to 087 ppb of cobalt o 
 
 The total zinc concentrations found in the three water samples 
 analyzed in this study ranged from „048 to „120 ug/g or from 48 to 120 ppb„ 
 The total cobalt concentrations of these samples ranged from , 00005 to 
 o 00011 yg/g or from 05 to »11 ppb„ The data is consistent with the con- 
 centrations reported by previous investigators 
 
 65 
 Figo 1 3 depicts the results of monitoring the Zinc activity in 
 
 Columbia River water at Pasco, from 1958 to 1963, by the Hanford staff, as 
 
 65 
 reported by Foster et al , (1964) (7) The Zinc activity at Pasco during 
 
 August, 1963, ranged from o 08 to l c 3 pc/g Foster et_ al „ also stated that 
 
 the average activity during 1963 was „47 pc/g at Hanford, 38 pc/g at 
 
 Richland and „22 pc/g at Pasco „ Data on Cobalt activity in Columbia River 
 
 water is not available 
 
 65 
 The Zinc ' activity of Columbia River water found in this study 
 
 varied from O 0199 pc/g near Richland, to „0013 pc/g near McNary dam The 
 
 sample collected near Pasco contained O 0029 pc of Zinc ' per gram of water 
 
105 
 
 65 
 Only three water samples were analyzed in this stu^-j , and the Zinc 
 
 activities of the samples were close to the detection limit of the gamma 
 
 scintillation counter,, The results are considerably lower than data 
 
 reported by Foster et al 
 
 fin 
 The Cobalt activity of Columbia River water was also close to 
 
 the detection limit of the gamma scintillation counter, but appeared to be 
 
 about oOOl pc/g of water o 
 
 Plankton 
 
 Davis (1963) (Appendix, 9) analyzed plankton samples collected 
 
 from the Columbia River near Hanford in 1957, and found an average of 
 
 65 
 7300 pc of Zinc per gram wet weight of plankton „ (Hanford, as shown on 
 
 Figo 6 1, is about ten miles downstream from the reactor area) Assuming 
 
 65 
 a dry to wet weight ratio of „2, the concentration of Zinc reported by 
 
 Davis is equivalent to 1460 pc/g dry weight of plankton „ Green algae 
 
 65 
 
 samples at this location contained approximately 2 8 500 pc of Zinc ' and 
 
 fin 
 30 pc of Cobalt per gram dry weight of plankton The green algae con- 
 tained less than 50 ug of zinc and less than 5 yg of cobalt per gram ashed 
 weight, as reported by Davis The reported concentrations of zinc and 
 cobalt would have been considerably less, if reported on a dry weight basis 
 instead of an ashed weight basis „ 
 
 In the present study, plankton samples contained from 1060 to 
 
 65 
 1960 yg of zinc, 1 2 to 3 5 yg of cobalt, 4830 to 8060 pc of Zinc ' and 
 
 to 63 pc of Cobalt , per gram dry weight of plankton With the exception 
 
 of the Cobalt data, the concentrations and activities of the plankton 
 
 samples were high enough to assure good analytical precision and accuracy „ 
 
 fi ^ 
 The data are consistent with that reported by Davis for Zinc ' activity 
 
 fin 
 and Cobalt activity The data reported by Davis for zinc and cobalt may 
 
106 
 not be accurate and are not very consistent with the concentrations of 
 zinc and cobalt found in this study 
 
 Bottom Sediments 
 
 Samples of bottom sediments were analyzed in March, 1962, by the 
 Hanford staff , These samples were collected from the shorelines of the 
 Columbia River between Hanford and Richland „ They were taken, as noted in 
 Chapter I, primarily from the shorelines of islands within this reach of 
 
 the Columbia River Zinc ' activities ranged from 170 to 880 pc/g and 
 
 fin 
 Cobalt activities ranged from 5 6 to 69 pc/g dry weight of sediment „ 
 
 Zinc ' caused one=third of the total radioactivity of these samples „ The 
 
 Hanford staff also took core samples from the bottom of McNary reservoir 
 
 65 
 in 1962, as noted in Chapter I These samples averaged 13 50 pc of Zinc 
 
 and 47 pc of Cobalt per gram dry weight of sediment, at the sediment-water 
 
 interface o 
 
 The variation in flow of the Columbia River has been shown in 
 Figo lo3 The flow had seldom been less than that which occurred in March, 
 1962 During low flow periods, the river surface level in the study reach 
 upstream from McNary reservoir fluctuates several feet daily, due to con- 
 trolled releases from the Priest Rapids dam, upstream from the Hanford 
 reactors o Sediments collected along the shorelines in March, 1962, could 
 have received daily exposure to reactor effluent contaminated water for 
 many months prior to sampling, and continuous exposure for the major portion 
 of many years prior to sampling,, 
 
 Sediments collected in the present study might contain lower 
 concentrations of radionuclides, due to the lower probability of exposure 
 of the sediments to reactor effluent contaminated water, as discussed pre- 
 viously Sediments collected from the shorelines of the river just after 
 
107 
 the flood period of the year would likely contain lower activity than those 
 collected along the shoreline prior to the flood period, as a result of 
 scouring and desorption by dilution 
 
 The core samples collected by the Hanford staff were taken from 
 the bottom of McNary reservoir, and the samples from this reach collected 
 for the present study were taken from the shoreline of the reservoir „ In a 
 reservoir, sedimentation tends to concentrate on the bottom rather than on 
 the shorelines o In McNary reservoir, the majority of the radioactivity 
 associated with the sediments may result from deposition of radioactive 
 sediments and not from adsorption of radioactive ions from the water, as 
 may be the case in the reach of the Columbia River between the reactor area 
 and Richland o Thus, sediments collected from the shorelines of McNary 
 reservoir for the present study might be expected to contain much lower 
 concentrations of Zinc ' and Cobalt than the concentrations found in the 
 core samples taken from the reservoir in 1962„ 
 
 Data on concentrations of zinc and cobalt in Columbia River 
 sediments are not available 
 
 The results of this study indicate a range of from 5 to 187 yg 
 of zinc and from „00 to „87 yg of cobalt per gram dry weight of sediment, 
 in the study reach of the Columbia River, as shown in Fig*s„ 8 C ^ and 8 5o 
 There appears to be an average concentration of 71 yg of zinc and „28 yg of 
 cobalt per gram dry weight of sediment, adsorbed or exchangeable on the 
 sediments of the study reach , 
 
 Fig' So 806 to 80 9 show the variation of Zinc ' and Cobalt 
 
 activities on bottom sediment samples along the study reach of the Columbia 
 
 65 
 River Zinc ' activities increased from 69 pc/g upstream of the reactor 
 
 area to 230 pc/g between Hanford and Richland, and then decreased to less 
 
 than 5 pc/g within McNary reservoir „ A sample taken below McNary dam 
 
108 
 contained 10 9 pc of Zinc ' per gram dry weight of sediment „ The highest 
 value obtained in McNary reservoir was 13 o 8 pc/g, and the sediments averaged 
 about 4 pc/g in the reservoir In the reach between the reactor area and 
 Richlandj, Zinc ' averaged approximately 90 pc/g Cobalt activities varied 
 from 34 pc/g upstream of the reactor area to 13 o pc/g between Hanford and 
 Richland and then decreased to less than 2 pc/g near McNary dam<, The 
 
 C A 
 
 highest value for Cobalt obtained in McNary reservoir was 1„44 pc/g, and 
 the sediments taken from the reservoir averaged less than 1„0 pc/g„ Cobalt 
 averaged approximately 3 pc/g in the reach between the reactor area and 
 
 Richland o 
 
 65 
 The Zinc activities obtained in this study for sediments in the 
 
 reach between Hanford and Richland average 24 percent of the activities 
 
 found by the Hanford staff in 1962 The concentrations of Zinc found in 
 
 McNary reservoir average 3 percent of the concentrations found in the 1962 
 
 study of the reservoir sediments „ The results indicate that sediments along 
 
 65 
 the shoreline of the reservoir contain much smaller concentrations of Zinc 
 
 than do the sediments in the bottom of the reservoir „ 
 
 C A 
 
 The Cobalt activities of sediments obtained in this study in 
 the reach between Hanford and Richland average 16 percent of the activities 
 found by the Hanford staff in 1962 <, The Cobalt activities obtained in 
 this study in McNary reservoir average approximately two percent of the 
 
 activities found in the 1962 study,, Both of these percentages are in the 
 
 65 
 same ranges as the percentages found for Zinc 
 
 CONCENTRATION RATIOS 
 
 The Columbia River water contained an average of O 072 yg of zinc 
 
 65 
 and „ 00010 pg of cobalt per gram of water The Zinc ' activity, as measured 
 
 by the Hanford staff on the date of sampling , was „11 pc/g at Pasco „ The 
 
109 
 Cobalt activity 8 as found in this study, averagea o 0008 pc/g of water, 
 
 Plankton samples collected from the study reach contained an 
 average of 1660 yg of zinc, 2 50 yg of cobalt, 5940 pc of Zinc and 30 pc 
 of Cobalt per gram dry weight of plankton „ Bottom sediment samples 
 collected from the study reach contained an average of 71 yg of zinc, 
 28 yg of cobalt, 52 pc of Zinc ' and 2 1 pc of Cobalt per gram dry 
 weight of sediment o The ratios of the concentrations found in plankton 
 and bottom sediments of zinc, cobalt, Zinc ' and Cobalt , to the concen- 
 trations of these elements and radionuclides in the surrounding water, 
 based on average values within the study reach of the Columbia River, are 
 presented in Table 8 2 
 
 Table 8 2 CONCENTRATION RATIOS OF COLUMBIA RIVER 
 PLANKTON AND BOTTOM SEDIMENT SAMPLES 
 TO COLUMBIA RIVER WATER 
 
 Analysis 
 
 Sample Type 
 
 Concentration Ratio 
 
 Total Zinc 
 
 Plankton 
 
 20,000 
 
 
 Bottom Sediments 
 
 1,000 
 
 Total Cobalt 
 
 Plankton 
 
 20,000 
 
 
 Bottom Sediments 
 
 3,000 
 
 „. 65 * 
 
 Zinc 
 
 Plankton 
 
 50,000 
 
 
 Bottom Sediments 
 
 400 
 
 Cobalt 60 
 
 Plankton 
 
 4 9 000 
 
 
 Bottom Sediments 
 
 300 
 
 based on Hanford staff evaluation of Zinc activity in water 
 
 SIGNIFICANCE OF ZINC 65 AND COBALT 60 CONCENTRATIONS 
 
 Eisenbud (1963) (4) has stated that the United States Atomic Energy 
 Commission's recommended maximum permissible concentrations in water for 
 non-occupational exposure are 100 pc of Zinc '' and 50 pc of Cobalt per gram 
 
110 
 
 of water o If all of the Zinc ' and Cobalt activity contained in the 
 plankton and bottom sediments of the Columbia River were somehow suddenly 
 released back into solution, the resulting concentration of these radio- 
 nuclides in the water would remain below these limits, because of dilution 
 by the large volume of water „ However, an industrial effluent containing 
 a high acidity and a greater density than the receiving water, discharged 
 into the Columbia River a few miles upstream from Richland or Pasco, could 
 accumulate high concentrations of Zinc and Cobalt , by desorption of 
 these radionuclides from bottom sediments „ It would be possible for this 
 density current to enter Richland or Pasco's municipal water supply intake, 
 It is therefore necessary for both of these cities to maintain continuous 
 monitoring of the radioactivity in the water at their water treatment 
 plants o An automatic alarm and by-pass system for water containing exces- 
 sive radioactivity is also necessary If continuous water monitoring and 
 automatic by-pass systems are maintained, the occurrence of Zinc " and 
 
 en 
 
 Cobalt in their present concentrations in the Columbia River water, 
 plankton and bottom sediments is very unlikely to produce a significant 
 radiation exposure hazard to the people using the Columbia River as a 
 source of drinking water <, 
 
Ill 
 
 IXo CONCLUSIONS 
 
 lo Zinc and cobalt radionuclides resulting from nuclear weapons 
 testing or nuclear reactor activities are commonly the major radionuclides 
 associated with aquatic plant and animal life 
 
 2 In natural waters, a dynamic equilibrium exists between zinc 
 ions in solution and zinc ions adsorbed on the surfaces of living aquatic 
 plant life and inorganic bottom sediments „ The degree of adsorption is 
 high and the rate, rapid, at pH v s above neutrality „ Desorpicion is complete 
 at pH°s below four,, 
 
 3 The desorbable zinc and cobalt fractions of environmental 
 samples, such as water 9 plankton and bottom sediments, can be isolated by 
 anion exchange chromatography u After isolation of each fraction, the total 
 zinc or cobalt concentration can be determined by colorimetric procedures, 
 and the radioactive zinc or cobalt activity can be determined by gamma 
 scintillation countingo 
 
 4 Table 9 1 indicates the minimum B maximum and average concen- 
 trations of total and radioactive zinc and cobalt in samples collected from 
 a one-hundred mile reach of the Columbia River between just upstream of the 
 Hanford reactors and just downstream of McNary dam 
 
 5 The radioactivity of the zinc fractions of all samples was 
 
 65 . . 
 
 caused by Zinc and the radioactivity of the cobalt fractions of all samples 
 
 was caused by Cobalt 
 
 65 
 6 Zinc ' was a major radionuclide associated with plankton and 
 
 bottom sediment samples and Cobalt was a minor radionuclide associated 
 
 with these samples 
 
 7 No relation was found between the Zinc ' and Cobalt activities 
 
112 
 
 of the bottom sediments of the Columbia River and the total zinc and cobalt 
 concentrations of these sediments . 
 
 8 Total zinc concentrations of the sediments were highest above 
 the reactor area, along the reactor shore, and decreased with distance 
 downstream Total cobalt concentrations of the sediments generally de- 
 creased with distance downstream throughout the study reach 
 
 Table 9.1 
 
 CONCENTRATIONS OF TOTAL AND RADIOACTIVE ZINC 
 AND COBALT IN COLUMBIA RIVER SAMPLES* 
 AUGUST 14 AND 15, 1963 
 
 Analysis 
 
 ZINC 
 
 (yg/g) 
 
 COBALT 
 
 H'lTl !"■■ 1 "ill" 
 
 (yg/g) 
 
 65 
 
 COBALT 
 
 60 
 
 Water 
 
 Plankton 
 
 SampleType 
 
 Mm 
 
 Max 
 
 Ave 
 
 Mm 
 
 Max 
 
 048 .120 072 1060 1960 1660 
 00005 .00014 .00010 1.2 3.5 
 
 ZINC 
 
 (pc/g) .0013 .0199 .0084 4830 8060 5940 
 (pc/in2)t 
 
 (pc/g) .0000 .0014 .0008 
 (pc/in 2 )t « 
 
 63 
 
 3G 
 
 Bottom Sediments*"*""' 
 
 i.'.t: 
 
 Ave Min 
 
 5 
 
 Max 
 
 187 
 2.5 .00 ,87 
 
 .00 230 
 .0 5510 
 
 .00 13.0 
 .0 313 
 
 Ave 
 71 
 
 28 
 
 52 
 
 1060 
 
 2,1 
 46 
 
 ""based on analyses of 3 water B 4 plankton and 24 bottom sediment samples 
 **as dry weights 
 tin 2 ground surface area 
 
 9. The major portion of the Zinc ' and Cobalt activities asso- 
 ciated with bottom sediments collected along the shorelines of the Columbia 
 River occurred in a 40 to 50 mile reach extending through the Hanford reactor 
 area and downstream, and concentrated along the reactor shore. 
 
 10. Zinc and Cobalt , in their present concentrations and 
 locations in bottom sediments of the Columbia River, do not represent a 
 
113 
 
 significant public health hazard Continuous monitoring at the water 
 treatment plants of public water supplies taken from the Columbia River 
 is g however, considered to be necessary as a safeguard against the consump- 
 tion of water containing excessive concentrations of radioactivity „ 
 
114 
 
 REFERENCES 
 
 Notes Abbreviations Used for Technical Reports 
 
 HWs U So Atomic Energy Commission Technical Reports; 
 Hanford Atomic Products Operation, General Electric 
 Company, Richland, Washington 
 
 ORNL ; Uo So Atomic Energy Commission Technical Reports; 
 Oak Ridge National Laboratory, Oak Ridge, Tennessee 
 
 RADIOECOLOGY: Proceedings of the First National Symposium 
 on Radioecology held at Colorado State University, Port 
 Collins, Colorado, Septo 10-15, 1961 s Uo Shultz and A W„ 
 Klement eds Reinhold, New York and The American Institute 
 of Biological Sciences, Washington, D C 746 pp (1961) 
 
 TIP ; Uo So Atomic Energy Commission Technical Reports 
 
 Ws Uo So Department of Health, Education and Welfare, 
 Public Health Service; The Robert A Taft Sanitary Engi- 
 neering Center Technical Reports, Cincinnati, Ohio 
 
 1 American Public Health Association et al„, Standard Methods for the 
 Examination ofWater and Wa s t e wa t er , 11th Edition, New York, 626 pp» 
 (i960) ' 
 
 65 
 2o Bachmann, R W , "Zinc ' in Studies of the Freshwater Zinc Cycle," 
 
 Radioecology , pp 485-499 (1961) 
 
 3» Donaldson, L R» , "Radiobiological Studies at the Eniwetok Test Site 
 and Adjacent Areas of the Western Pacific," W-60=3, pp 1-7 (1960) 
 
 4o Eisenbud, M , Eny iron mental Radioact ivi ty , McGraw-Hill, 430 pp (1963) 
 
 5 Ewing, Bo B , "Report on Proposed Research on Fate of Radionuclides 
 
 in the Columbia River 9 Hanford Atomic Products Operation," unpublished 
 draft, August 19, 1963 
 
 6 Foster, R„ F„ , "Relationships between the Concentration of Radionuclides 
 in the Columbia River Water and Fish," TID-7664, pp 269-288 (1963) 
 
 7o Foster, R F , et al , "Evaluation of Radiological Conditions in the 
 Vicinity of Hanford for 1963," R H Wilson ed , HW-80991, 198 pp 
 (1964) 
 
 8o Foster, R F„, et aloj "Evaluation of Radiological Conditions in the 
 Vicinity of Hanford for 1962," R„ H Wilson ed 0$ HW-76526, 183 pp 
 (1963) 
 
 9 Friedlander, G , and Kennedy, J W , Nuclear and Radiochemistry , John 
 Wiley and Sons, Inc, New York (1955) 
 
115 
 
 10o Held, Ec E,, "Qualitative Distribution of Radionuclides at Rongelap 
 Atoll," Radioecology, pp 167-171 (1961) 
 
 11, Kraus, K„ A , and Nelson, F , "Anion Exchange Studies of the Fission 
 
 Products," Proceedings of the International Conference on the Peaceful 
 Uses of Atomic Energy, Vol 7, p 113 „ Session 9B1, P/837, United 
 Nations (1956) 
 
 12 Lomenick, T F , et al , "Study of White Oak Creek Drainage Basin," 
 ORNL-3492, pp„ 51«62"Tl963) 
 
 13 o Lowman, F G„, "Radionuclides in Plankton and Tuna from the Central 
 Pacific," Radioecol ogy^, pp 145-150 (1961) 
 
 14 C McConnon, D , "Dose Rate Measurements of Beaches and Islands on the 
 Columbia River between Ringold and Richland," HW-72229 Rev , 21 pp„ 
 (1962) 
 
 15 Nielsen, J M , "Behavior of Radionuclides in the Columbia River," 
 TID-7664, pp 91-105 (1963) 
 
 16 o O'Connor, J T , and Renn, C E , "Soluble-Adsorbed Zinc Equilibrium in 
 Natural Waters," Journal Ameri can^Water Works Association , 56, pp 1055- 
 1061 (1964) 
 
 17 o O'Connor, J T , and Renn, C E„, "Evaluation of Procedures for the 
 
 Determination of Zinc," Journal American Wat er Works Association , 55, 
 pp 631-638 (1963) 
 
 18« Osterberg, C , Pattulo, J , and Pearcy, W , "Zinc-65 in Euphausiids as 
 Related to Columbia River Water off the Oregon Coast," Limnolo gy and 
 Oceanography, _9, PP° 249-257 (1964) 
 
 19o Palmer, R F 0£) "Accumulation of Radioisotopes by Rats Chronically 
 Exposed to Reactor Effluent Water," HW-53362, 16 pp„ (1958) 
 
 20 o Pritchard, D W , and Joseph, A B,, "Disposal of Radioactive Wastes; 
 Its History 5, Status and Possible Impact on the Environment," 
 Radioecology^ pp„ 27=34 (1961) 
 
 21 Rad iologi cal Heal th Handbook , 9 S Kinsman ed , U S Dept of Health, 
 
 Education and Welfare, Public Health Service, Bureau of State Services, 
 Division of Sanitary Engineering Services, Robert A Taft Sanitary 
 Engineering Center, Cincinnati, Ohio, 355 pp (1957) 
 
 22 o Robeck, G C„, Henderson, C , and Palange, R C , "Water Quality Studies 
 on the Columbia River 8 " U S Department of Health, Education and Wel- 
 fare, Public Health Service, Bureau of State Services, Division of 
 Sanitary Engineering Services, Robert A Taft Sanitary Engineering 
 Center, Cincinnati, Ohio, 99 pp plus 4 Appendices (1954) 
 
 23o Rowe, Do R , and Gloyna, E F„ , "Radioactivity Transport in Water - The 
 Transport of Zinc^S i n an Aqueous Environment," The University of Texas, 
 Department of Civil Engineering, Environmental Health Engineering 
 Laboratory Technical Report - 5 
 
116 
 
 24 6 Sandell, E„ B„, Colorimetric Determinations of Traces of Metals, 3rd 
 edition, New York and Interscience Publishers, 1032 pp„ (1959) 
 
 25„ Silker, W B„, "Variations in Elemental Concentrations in the Columbia 
 River," Limnology and Oceanography , 9_, pp» 540-545 (1964) 
 
 26 Skauen, D, M , "Radioactive Zinc-65 in Marine Organisms in Fisher's 
 
 Island Sound and its Estuaries <, Final Report, December 1, 1959 through 
 November 30, 1963," TID-19922, 50 pp, (1964) 
 
 27 <, Straub, C P<>, "Pollution Problems Caused by Power Reactors and Other 
 Uses of Atomic Energy," W-60-3, pp. 33-39 (1960) 
 
 28 6 Thomas, C E , Reid, D. L«, and Lust, L, F , "Radiochemical Analysis of 
 Marine Biological Samples Following the 'Redwing' Shot Series - 1956," 
 HW-58674, 81 pp„ (1958) 
 
 29, Watson, D„ G„, Davis, J t J«, and Hanson, W, C , "Zinc-65 in Marine 
 Organisms along the Oregon and Washington Coasts," Science , 133 , 
 pp, 1826-1828 (1961) 
 
117 
 
 APPENDIX 
 
 SUMMARY OF DATA ON THE OCCURRENCE OF 
 STABLE AND RADIOACTIVE ZINC AND COBALT IN THE 
 AQUATIC AND TERRESTRIAL ENVIRONMENTS 
 
118 
 
 o 
 
 CC 
 
 u. 
 
 
 
 *3 i 
 ■': 
 
 VV V V V v\ 
 
 VVVVVV VV 
 
 -"28 X 
 
 ■ - 8 
 
 ■-8-a- 
 
 < 
 
 UJ 
 
 -J 
 
 a. 
 
 SI 
 < 
 to 
 
 -o 
 
 5 
 
 £" 
 X 
 **- 
 
 o 
 
 :i 
 
 vv vv* 
 
 
 -*S 4" 
 
 < 
 
 ►- 
 Z 
 
 o < 
 
 a: ui 
 
 — cc 
 
 > < 
 
 c 
 o 
 > 
 a> 
 
 ■5 i 
 
 UJ 0£ — 
 
 UJ 
 
 Z > (/> 
 
 c 
 
 QC O 
 
 -J < 
 
 CO CO 
 
 o x: 
 <-> 3 
 
 _j 
 o o 
 z o 
 < 
 
 O 
 
 < 
 
 o 
 
 a 
 
 z 
 < 
 
 CO 
 
 < 
 
 I 
 
 < 
 
 jO 
 
 o 
 o 
 
 01 — 
 
 z 1- en 
 
 — o 
 
 isl — 
 
 cc an 
 
 O 5 
 
 (0 en 
 
 ■— O 
 
 0} Q. 
 > 
 
 UJ Q> 
 
 ; u 
 (0 
 
 .. to 
 
 (U — 
 
 U Z 
 
 C 3 
 0) 
 
 u •• 
 
 1) UJ 
 
 >+- H- 
 
 a) o 
 
 a: z 
 
 * 
 
 s 
 
 :i 
 
 S3 
 
 ; 
 
 tl 
 
 3 
 
 S3 
 
 *& i 
 
 S3 
 
 i 
 
 i 
 
 »S8 SS 
 
 *£2 S: 
 
 s*R 5a 
 
 sac i» 
 
 8SS Stf 
 
 ??I si 
 
 ill II 
 
 SS3S2 33 
 
 35ESS3 SS 232 
 
 *|fg|| as as 
 
 ~s; 
 
 « *«? st as s*a a» 
 
 isSS 2 2 s.|3 ss 
 
 "S3 — 8 "S£ 8 88 """" 2 
 
 sssss a agg s a? *ss a 
 
 :*I«2 
 "3A3? 
 
 SI I 
 I 
 
 §£!?? 
 
 I ! - l-| * ! 
 
 i'ErSfS if i^t if i^rsii it itl 1 Hit??! !\titl it ITiiiii i ftt \?i 
 
 I 
 
 I 
 
 
 _ 
 
 t 
 
 I 
 
 t 
 
 i 
 
 
 i 
 
 i 
 
 
 I 
 
 ! 
 
 1 
 
 I 
 
 3 
 
 i 
 
 * 
 
 I 1 
 
 2 1 
 
 I i 
 
 f ! f 
 
119 
 
 * i 
 
 en 
 < 
 
 fsS-SV A3i 
 
 a: 
 < 
 
 CD 
 
 ST 
 
 _l 
 O 
 <_) 
 
 -a 
 
 CD 
 
 C 
 
 * * 
 
 - i i 
 
 i % 
 
 i- 1 ! 
 
 i 3 t ii. 
 
 5 "5-2- 
 
I 
 
 < 
 
 03 
 
 
 \D 'ON CD < 
 
 <7\ •£) O (Ti 
 
 o o o o 
 
 120 
 
 ^ o tr»oo 
 '2 v v « J 
 
 CO 00 
 
 < 
 
 CO \D 
 
 cc 
 
 < 
 
 QQ 
 
 Z3 
 
 . (SI J ^ - 
 
 O 
 
 .5 2 
 
 o -J 
 
 ■ I 
 
 -5 1 
 
 3 
 C 
 
 «. < * < 
 
 S ■; 
 
 8 IS 
 
 £ C 8 £ 8 S 
 
 — — -O _i — J — TJ — _l — — J — 
 
 >>— > > — c — a > to 
 
 1- l. O i L l. t-OO'Ql-L. L.I.L. 
 
 « « o>v no) id (7' -■ > at u v v t) 
 
 > > C X >£ > C C -EC > r C 
 
 « L. * 
 
 8* iS* * S* ^ £ J J" 
 
 E - E 1 
 
 : o ot oc i 
 
 O O ot O i 
 
 5 3 
 
< 
 o 
 
 Q 
 Q 
 < 
 
 2! 
 O 
 CC 
 Li. 
 
 < 
 
 CC 
 < 
 
 *-: 
 
 121 
 
 l § § ! ~s 
 J s s ; 11 
 
 2 III 22 I 22 ! 
 I Hi ii i ii i 
 
 o 
 
 ■z. 
 
 LU 
 
 a: 
 
 UJ 
 
 u. 
 
 LU 
 
 cc 
 
 Vi \\ 
 
 \i :; : .1 ; 
 
 CC 
 
 < 
 
 ca 
 
 ,.■*..-'- .i - J- Tjcfc^trSc^a- o>^^ffio«a 
 
 O 
 
 o 
 
 11 
 
 lit I 
 
 !! -. 
 
 %i 
 
 CS4 
 I 
 
 < 
 
 i s 
 
 I .. ! I J 1 » I I _?! 
 
 " » I ° SS ' 5 J si- 
 
 4 s. £is:i£ -ii 
 
 3 -S 
 
 I s 13 
 
 ij 
 
 -O 
 
122 
 
 * * * * « 
 
 
 5 S S 5 % s s 
 
 S S * S « « £ 3 J 3 1 J J I ) J 3 
 
 II IS § S I I I SI r ! 
 il ii 33 3 33 33 i 
 
 * * -i 
 
 ski 
 
 s If? III? 
 
 i : : : 
 
 ■? * X x 
 
 - .; « x x t x 3 
 
 HI | | | | | 
 33 3 33 3 3 3 
 
 || || || | || || - 
 S3 33 11 i II ii J 
 
 < 
 
 LU 
 < 
 
 II 
 
 £s ^S? 5 
 
 < 
 
 CO 
 
 o 
 o 
 
 SI 
 
 Ii * t * * * * ? 
 
 R<r?.».^*.^ff-*.<j>*^»^> o-». *£<£^£;£9!I£X £ j^j 
 
 C 
 
 CM 
 < 
 
 I i I - 1 
 
 i * * 5, 
 
 iJ. 
 
 8-3-8- It 
 
 is 
 
 s | 'sis I il'111 I: i 
 
 I i 1181 J 8*8*5* ;-; i 
 
 si 1 |J i i 
 
 :a -J .'2 ii 
 
 * s is it ss 
 
 •• 11 
 
 
 sJ 
 
 4 
 
 Ii 1 
 
 s 
 
 ! 11 
 
 -si 
 
 I 1 3 
 
 : ? e=| ii 
 
 I I 
 
 5 
 
 I ii 
 
 1 1 Ii 
 
 - i 
 
 ii 
 
 Si 
 
 31 1= 
 
 r 
 
 s 
 Is 
 
 5 ; Ji . s; 
 
a: 
 < 
 
 cc 
 
 UJ 
 
 > 
 
 CC 
 
 < 
 
 O 
 
 o 
 
 i i 
 
 123 
 
 !•• * 
 
 CM 
 I 
 
 < 
 
 
 II 
 
 i t 
 
 o o o * 8 o o o o o o o 
 
 s s si!- sssssi & 
 
 * I * Ir% I *I * * I * 
 
 i ? ( ::s ;l il i ! ! * 
 
 t i i : i s 3 s 1 1 i I I i 
 
 ! \ 
 
 ■o 
 
 0) 
 
 C 
 
 C 
 
 o 
 u 
 
 i h-m Sis rs s ? m 
 
 s 3 s j : c - j 
 
 
 -Q 
 
Z — ' z 
 
 t) — — 
 
 o. oe oe 
 
 IS 
 
 S- 3- 
 
 -1 ~1 
 
 124 
 
 c <v c c c 
 
 « c <o c 
 
 « m 
 
 -» O f*>Op Q <N — CO - 
 
 in — -T ui O *M **\ J 1 wifti- 
 
 < 
 
 > 
 cc 
 
 < 
 
 III § 
 
 U t> f V 
 
 a a 5. a. 
 
 o o o o 
 
 o o o o 
 
 o 
 o 
 
 Z E 
 
 — a 
 *j a. 
 
 32 
 
 CKJ^ffl ON 
 
 ■a 
 
 3 
 C 
 
 CM 
 < 
 
 c >■ 
 
 a 
 
 a 
 
 o a a 
 
 x — 
 
 
 
 
 x t- 
 
 a» 
 
 a* 
 
 en an en 
 
 
 
 
 
 
 
 
 
 
 
 £. X. 
 
 
 u a. 
 
 * 3 
 
 1 
 
 *l 
 
 U! 
 
 gt 
 
 > 
 
 <0 > 
 
 > > > 
 
 
 
 
 
 
 
 
 
 
 
 > > > 
 
 
 « 
 
 > i 
 
 a a a: 
 
 |«SS 
 
 
 8 I I 
 
 22 $ 
 
 
 'fct-i » f (j »- w c C7>— u g t- fi • c >*- i 
 CifljfK-i o x -x — -o i £> 2 ~ — £. 2 * 
 
 n 
 
 a 
 
s s 
 
 125 
 
 3 3 3 
 
 3 3 3 
 
 i: 
 
 a: 
 < 
 
 o 
 
 I— 
 
 o 
 
 LU 
 
 > 
 
 CO 
 
 o 
 
 U. 
 
 < 
 
 I- 
 
 co 
 
 Q. 
 
 X. 
 
 < 
 
 CO 
 
 O 
 
 CJ 
 
 M 
 
 Q 
 
 z 
 
 < 
 
 CJ 
 
 z 
 
 CO 
 
 I 
 < 
 
 -Q 
 (0 
 
 * 5 
 
 3 a 
 
 O ooo — — o-»o^'*HMj-r«-irtr~-r».3J'«>i*-si> 3— o 
 
 — NNW^JJ^^ 
 
 o %A w\ a 
 
 ao f^_ ^> 
 
 ui — N« o 
 
 £ ... 
 
 Z O OOOOOOOQOOOOOOOOOOOO oo o 
 
 oc o> onoon n- — on cr« — — o«M.jr>*ooi-»— o> "v © *o ui 
 
 V> O OOO 
 
 F* f. O «~1 
 
 » — M 0> O 
 
 3 
 
 SO O O 
 
 oo — — , jj- ,_ 
 
 — — .* U% — •*> ~ IAU>N- 
 
 a 5 
 
 z 
 
 2 ° 
 
 uj O OQQQOOOOOQOOOOOOOOO 
 
 — vo cnco 3 co — «Nwj»^^3 ooo%oi^u\vo 
 _ — — _ 
 
 C 
 
 a. o 
 
 o <M 
 
 en 
 
 I 
 
 vO — — ______ — 
 
 M \0\flNiAU\CO W*CO 1/V4NO^O^OOO N — CM — O t* 
 
 O oOOWJr^<N*f».of«.<D — i^i* «M<D — o *« »n v\— o *•* «*"> 
 
 lA _ — ^ o 0> 
 
 O o <* o r» co 
 
 <•> o — w> o j o 
 
 Si"*> so ^c o CO IT 
 
 O (M O O O O 
 
 z 
 
 O O oc O GOOQOOOOOOOOOOOOOOOO QO o o o 
 
 O OO, < <** ffll^^5ff>N_J_ONMAi*PvJ^.^(MJN CO l/\ l/N (M O 
 
 <T- — t 00 OCOf^tNCriO^OO^-^D^O-J — — — ■ ON CO — — vO 0*vvO «J"* CO vO 
 
 3 — — - — 
 
 OOujO CTtOOOO 
 
 «NP>*OJ' N C\ CO — TO 
 
 < 
 
 SO O O O O O O 
 
 rt\ <J\ >r\ <X) (M UN O 
 
 £ ~ _* eo3 m *o M 
 
 «si rs O — — ~ — _______ _ _ — ^j jf r~. o — _ — — 
 
 O 
 
 ■ ■ — > _■ 
 
 _ im C _ > — — 
 
 \j — — 3«0— «%•— <M"T*£^ 
 
 « ■ i — » t5 z \o •_• \o _> — ' lTl 0"* 
 
 «« «*» oi_ — ImCQ m-«\coo"M!ONirtvOMh — vD © j- ■-- cr> fsij <w <jvo> cr>cr> <^ — — 
 
 * * S'Si .". ~ N ~." " """."■"*! ."g". '3'. ~". "."". " = 
 
 5 a v m a « 3 3 s uO« «3 * _jj 
 
 -> u. s: < r -» -» <« ozo ->n -» o« 
 
 ■D C 
 
 ■ I s 
 
 c c o o 
 
 J S " u s 
 
 • > ».>•— CCl-C 
 
 u t — — «.-— 0'0«C 
 
 > > — CO 
 
 -6 >c-cc*co-«>>c.-o 
 
 J 1 - I J I = i = 
 
 I 
 
 .^^ — • 
 
 "O ■« 3 
 
 • i M 
 
 £ X * 
 
 ■ • *< 
 
 5 t L 
 
 Si? 
 
 < O o 
 
 J HI > 
 
 s i s * 
 
 o * — — 
 
 >o < 
 
 1 1 
 
126 
 
 
 Ch r*\oo 
 
 \£ c»CO u"» 
 
 00 CO ir> J- 
 
 <M ci 
 
 — 
 
 f\ •— — -3" 
 
 V V 
 
 V 
 
 V V V V 
 
 CO o"l 
 
 
 — 0MA4 
 
 J- c^ 
 
 
 NMN U\ 
 
 V V 
 
 
 V V V V 
 
 \c- r^t 
 
 
 is o r^ 
 
 — r*\ 
 
 
 *v\ 
 
 rsi o no cm 
 
 4 1 - MM 
 
 3: oo 
 
 O LU 
 
 oc — 
 
 T3 
 
 c 
 
 o _i 
 o < 
 
 — — — CO CN — 
 
 — ro 
 
 U~l 
 
 < O 
 
 0) 
 
 X 
 
 _J C3 
 
 Q_ Z 
 
 s: — 
 
 < 3 
 
 (/> Q 
 
 UJ 
 
 -J CC 
 
 < r 
 
 Z LU 
 
 LU X 
 
 X 
 CD 
 
 o o 
 
 QC Z 
 
 z o 
 
 —i r-* 
 
 < un 
 
 0Q I 
 o \0 
 
 O LA 
 CT\ 
 Q — 
 Z 
 
 < - 
 < 
 
 O LU 
 Z QC 
 — < 
 
 O 
 
 2 
 cn 
 o 
 
 CL 
 
 0) 
 
 l_ 
 
 LU 
 
 o 
 
 o -i 
 
 oi 
 
 < 
 
 h- CJ 
 
 o < 
 
 < O. 
 O 
 
 — H- 
 
 Q (/> 
 
 2£ 
 
 Q X 
 
 Z I— 
 
 < =3 
 O 
 
 LU CO 
 _J 
 
 co lu 
 
 < x 
 l- h- 
 co 
 
 -3" 
 < 
 
 X> 
 <T5 
 
 00 
 LA 
 
 en 
 
 10 
 03 
 
 E 
 O 
 
 x 
 
 O 
 
 c 
 
 <D 
 
 u 
 <U 
 
 <U 
 CC 
 
 
 — — — 00 <M — N **\N N — 
 
 — CL — 
 
 NI/tON' 
 
 4) •— 4) 41 4) V 41 
 
 I- > — 1- u u u 
 
 4-« O W» 4-» *■» «■* 4J 
 
 C >* 3 C C C C 
 
 4> J £ t) 41 4> 41 
 
 5 5 
 
 O UJ 
 
 4) 4) 8 4) 41 4) V 
 
 ~U4IO«-'4>«"'o~ 
 
 «-•</>> -o c > c £x>c 
 
127 
 
 sitNOO— — oor^j-j-oo — CO CM O \£> — — — 00 
 
 _ v g •"'^S v v * v v v 
 
 vo at O cm r-. r^ r-». 
 
 00 Nrs — «— v. _ _- — _. _- ^_ 
 
 -j CT» '""v r*» v_> oo -J «*"*_*sOouacor-«ooo f-* -3"°S !0 
 
 cm r*- moo c^fMOO omacaoo vo-o^eo — vo ^ "7 
 
 <ffivO -^ tAOiA C\ON^ OC\- org ^\fi-' a; 
 
 fA-Nl^NOO • • ■ * 
 
 UJ ^JNJ- JOff\(T>- ^od'^'j! 
 
 > -3T CM f+\ tT\ r*» 0*l«40 U> U"\ CJ\ O N- N N WniM 4 ■— '"" -* 
 
 <__) < in — © r*.— — eg cm — v 
 en ^«* <M — — 
 
 a 
 
 Ot X 
 < UJ 
 
 *r* -** 
 
 -J -I 
 
 < 
 
 I CO 
 
 n ° «* 
 
 CO o — 
 
 UJ f 
 
 31 t/> 44. 
 
 o 
 
 CO 
 
 J- csj OJ <M — c^ clcsl — -^ <M 04*fl(CA0ffi Q v OJ N ff»- ^ <M 00 u"v m vo 
 
 vv vvvvvv S'^-SrC- 3 _ ~ N N ~ "* 
 
 f** OJ vA Lf\ 
 
 LA (M — CM 
 
 OJ _____ ___ __ — __(M_^_ CO 0O\O f~ . _ . 
 
 ■ r 
 s < 
 
 - . z ^ 
 
 c j: s £ _ i_ s 
 
 c 
 o 
 u 
 
 — wo 
 
 — V ID 
 
 >* y-s 
 
 <t "o— u*o— _.— *_?£*■ ^ 4 "" w ' 
 
 J_ "O -O 
 
 j ._ 5 3 — m 3 I fit-EC* 
 
 U) E — C7> E — E ^ 4» (U -. T! D ^ 
 
 o a> 
 
 c c — 
 
 00*- 
 
 __ J_ «/» ' 
 
 <Q 4> C 3 — 
 j_ _= — E — 
 
 —I V0> 4> <rt i/» — — <D S — ' CT> _» 
 
 O- l_U,U-0— I — JUUWUO)— I 
 
 _LJ *- —.-.CUB*- *_»— in C ^ <■' t- 1 HI 
 
 *n c c — 5 9. < i ae E E > o» — « uj 
 
 t» t» — Cn b J CO _C 
 
 f 
 
128 
 
 V V V V 
 
 \0 f» 
 
 - N l/lO — 
 
 V V V V V 
 
 00 vil 
 
 , — — — , i J-— CO — 
 
 — — .j — j- <nj rvj— — — 
 
 cc 
 
 < 
 
 • ~± co — 
 
 N CM/\rv 
 
 < 
 
 a. 
 
 
 CO 
 
 3 
 
 o 
 
 CO 
 
 tfs o 
 
 <r» 
 
 r* J- 
 
 \j\ — 
 
 so in 
 
 in a* 
 
 v£> 
 
 -tf m 
 
 r** 04 
 
 CO vD 
 
 f-» J- c\ r^ 
 
 V V V V 
 
 v£> vo 
 
 <M — C4 — — -* ■ 
 
 ■-* — — — eg — — — oi 
 
 — — OJ 
 
 3 
 
 c 
 
 o 
 u 
 
 I 
 
 < 
 
 
 8 § 
 
 O JJ i "D 
 
 CUV 
 
 to > u <0 
 D — 10 fi 
 
 a> a> *-< o 
 
 e — .o ^ 
 
 O U 4* -X T) 
 
 «A «A 4-* U 10 
 
 id a E «o *-• 
 
 — a — <o 
 
 <0 <0 >t J 10 — 
 
 a >- a. o a. => 
 
 — — 4) D 
 
 E $ 
 
 li 
 
 I 
 
 3 
 2 
 
 o o — e 
 
 & ID 
 
 i = 
 
 10 3 *D C « D — 
 © E © •- -C E > 
 
 »- .O -O Ul 
 
 <U -tf X) CD 
 
 > O fl> *-» 
 
 » V V c 
 
 - j) r .- 
 
 
 3 3 — 
 
 1 
 
 E E — 
 
 UJ 
 
 1 
 
 l/l 
 
 
 C^ 
 
 X 
 
 5 
 
 lA 
 
 * 
 
 U. 
 
129 
 
 O IANOQ0 — 
 
 — m vp \D «n ^ 
 v 
 
 V V V V V 
 
 V V V V V 
 
 s $ 
 
 — J- <T\ 
 
 <r> — «m 
 
 ON U> — 
 
 O -J 
 o < 
 
 — — SO — <M 
 
 < 
 
 < 
 
 UJ 
 
 3 
 O 
 to 
 
 N NvjOOOOO 
 J- — tM 
 
 V V V V V 
 
 ON WN 
 
 00 — 
 
 — — \C> — (Nj c-t 
 
 <1) 
 
 C 
 
 -3- 
 
 I 
 
 < 
 
 U V4- 
 «> — 
 
 « 0. 
 
 « T3 «-• J 
 
 k. I- L. > -O 
 TJ -O "D t C 
 
 -Q 
 
 M 01 0J 4t tf» 
 t) *■» L U V 
 > ~ — — > 
 
 >- 4) 
 
 V — >• 
 
 co lh 
 
 2 l §> i — 
 
130 
 
 < 
 
 ■z. 
 o 
 
 K 1 
 
 jf jfJT 3 * s 
 
 i i. ? 
 
 i I J 
 
 CO 
 LLl 
 
 a: 
 
 UJ 
 
 f 11 I 1 
 
 3 * 
 
 Q 
 
 < 
 
 O 
 
 < 
 Q 
 
 I 
 
 < 
 
 a: 
 
 < 
 
 < 
 a. 
 
 g S |i | 
 
 >n co O O 
 
 3 
 i 
 
 o 
 to 
 
 p 
 
 s » 
 
 S S^ 
 
 < 
 
 > > 
 
 « • *. 
 
 c c v 
 
 T> ^ ^- > 
 
 I • - I • 
 
 r >> oe 
 
 w« j 3 o © 
 
 S S s § 6 
 
 : ; J i ; 
 
 2 t- t 
 
 t I T i U 
 
 o ■ v> 5 v v 
 * x ^ - 11 
 
 5 5 
 
131 
 
 co 
 
 < 
 
 cc 
 
 < 
 
 23 
 
 
 ss c'SI!" 
 
 t, 9 t ?: S *■» f;- 
 
 i J £ i^b b ^J=TiJai^rii*rri mob bo b b o 
 
 2 
 
 ml 
 
 *i Sf !:j^ 
 
 SJJ *S SS«S*£*S S^fi! 
 
 co z 
 
 >- 
 
 
 
 LU O 
 
 _l 
 
 
 
 _i CJ 
 
 Z 
 
 
 £ 
 
 Q. 
 
 o 
 
 
 2 
 
 z: - 
 
 
 
 1 
 
 < cc 
 
 s_ 
 
 
 • 
 
 CO LU 
 
 <D 
 
 
 
 > 
 
 ■M 
 
 
 
 _J — 
 
 05 
 
 
 
 < OC 
 
 3 
 
 (/I 
 
 
 h- 
 
 
 <u 
 
 
 z co 
 
 fO 
 
 a. 
 
 
 LU LU 
 
 <D 
 
 >- 
 
 J" 
 
 s z: 
 
 co 
 
 Y- 
 
 £ 
 
 Z < 
 
 
 
 
 o x 
 
 T3 
 
 <U 
 
 i_ 
 
 o£ h- 
 
 C 
 
 
 -3 
 
 — 
 
 fU 
 
 C3. 
 
 
 > LU 
 
 
 E 
 
 
 Z X 
 
 1_ 
 
 (D 
 
 
 LU H- 
 
 <D 
 
 CO 
 
 J 
 
 
 +J 
 
 
 £ 
 
 Z Q 
 
 <D 
 
 1_ 
 
 
 — Z 
 
 3 
 
 <u 
 
 £ 
 
 < 
 
 
 -C 
 
 i 
 
 H 
 
 -C 
 
 ■M 
 
 
 _i o 
 
 I/) 
 
 o 
 
 
 < — 
 
 0) 
 
 
 
 CO Ll. 
 
 1_ 
 
 ,— 
 
 
 o — 
 
 Ll. 
 
 — 
 
 t 
 
 o o 
 
 
 < 
 
 
 < 
 
 i_ 
 
 
 s 
 
 Q Q. 
 
 O 
 
 s_ 
 
 1 
 
 z 
 
 4- 
 
 O 
 
 ° 
 
 < K 
 
 
 l+- 
 
 
 co 
 
 CT> 
 
 
 
 (_) LU 
 
 -* 
 
 cn 
 
 
 z 3 
 
 V. 
 
 ■">, 
 
 .? 
 
 — 1 
 
 u 
 
 o 
 
 ^ 
 
 M X 
 
 Ql 
 
 Q. 
 
 
 1- 
 
 
 
 *w 
 
 LU 13 
 
 -o 
 
 -o 
 
 - 
 
 > O 
 
 c 
 
 c 
 
 
 — CO 
 
 <0 
 
 <0 
 
 
 1- 
 
 
 
 
 <_> LU 
 
 -D 
 
 E 
 
 
 < x 
 
 a. 
 
 a. 
 
 5 
 
 O 1- 
 
 Q. 
 
 a. 
 
 
 ■« 
 
 
 
 ; 
 
 o « 
 
 <o 
 
 a) 
 
 M 
 
 5 cc 
 
 Cd LU 
 
 i_ 
 
 i_ 
 
 
 <D 
 
 <o 
 
 
 > 
 
 
 
 
 Q — 
 
 CO 
 
 CO 
 
 1 
 
 z cc 
 
 1- 
 
 H- 
 
 < 
 
 — 
 
 
 
 < 
 
 z 
 
 z 
 
 2 
 
 LU — 
 
 3 
 
 3 
 
 5 
 
 — 1 CO 
 
 
 
 
 co z: 
 
 
 
 
 < =3 
 
 LU 
 
 
 
 1 1 
 
 h- 
 
 
 
 co O 
 
 o 
 
 
 
 O 
 
 z 
 
 
 | 
 
 LU 
 
 
 
 5 
 
 X 
 
 
 
 
 K 
 
 
 
 
 C3 
 
 
 
 
 2 ; 
 
 s 
 
 3 I' 
 
 ft : t|j 5 1 j i ; - 
 
 ; i~- gs is: 
 
 | i 
 
 is > fSIJ 
 
 I 3" 
 8 "- 
 
 
 : ! I. 
 
 an 
 
 -u ^ a -j « » c — « J c - i — jo^t --a** u > n • , 
 
 I* - C "-C « £ i - * ^ u J 5 « - Ct.3>«L. M C — f - VI 
 
 J - ^ >. - * 3 t. * » c J * i - ~ , ■ -. * Q I ■ 5 , • ,. . 
 
 
 ;3,; ; ! ■ -■ i 
 
 J . 1 i ? .5 s'! 5 
 
 e " „ : i .»J,- 
 
 
 ;-•>';« mm 
 
 I 
 
 < 
 
 
 2 I 
 
 ^3 
 
132 
 
 o 
 o 
 
 |s£| iiii 
 £ I i 1 i i I } 
 
 * J H 
 
 I Mil lliltii Hi 
 
 
 i f 
 
 
 I l J 
 
 S : M 
 
 « : s ; 
 I I i 1 
 
 S ■ i i- 
 
 I- * ii ,1 
 
 I r jtj 
 
 J J Si J; 
 
 O 
 O 
 
 LU 
 
 S5 i »i? i* ?.ih Jill Si 
 
 I 5 ! 88 
 
 s s y I 
 
 5 ? :i H 
 
 i J. i. 
 
 CO 
 LU 
 
 < 
 
 Z Q 
 < Z 
 
 X < 
 
 o 
 
 Ct — 
 
 z I 
 I 
 
 o < 
 o. 
 
 CO 
 
 < h- 
 
 LU CO 
 
 OH LU 
 
 < 3 
 
 I 
 
 s a i m 
 
 o 
 
 CO 
 
 LU 
 
 X 
 
 A 
 
 cc 
 
 LU 
 
 > 
 a: 
 < 
 
 CD 
 
 o 
 
 *— .. o 
 
 0) LU 
 3 X 
 C (- 
 
 s * tilt 
 
 -. * 
 
 J ! 
 
 l"t 
 
 mi lf s J 
 
 i I 
 
 £?.*£o>&S £!v£r^Ji i"ij .'. 
 
 
 
 
 
 n n i 
 
 I* 3 5 5 - 
 
 * t 
 
 ■ . - - i . s 
 
 S {SI 
 
 , i i if :h 
 
 i • 1*5- 
 
 f j -.^ 
 
 * xs s* 
 
 
 P i j 
 
 3 ; s; 
 
 
 I 
 
 < 
 
 -O 
 (0 
 
I 
 
 < 
 
 I- llssiil il 
 
 133 
 
 LU 
 
 z 
 z 
 o 
 o 
 
 i* iiiill I 
 
 ^ 1 
 
 
 i I 
 
 Ss ii J 
 
 
 co 
 
 LU 
 
 < 
 
 Z Q 
 
 < Z 
 
 X < 
 
 I— 
 
 CC — 
 LU LU 
 
 X — 
 
 h- <_> 
 
 o < 
 
 a. 
 
 CO 
 
 < h- 
 
 LU CO 
 CC LU 
 
 < 3 
 
 I 
 
 X 
 
 o 
 
 CO 
 
 K * 
 
 I 
 
 s U till-Ili ii] 
 
 I J 
 
 i= S||S|i«i| 
 
 ii 
 
 s ; s 
 lit 
 
 is i 
 
 CC 
 
 LU 
 
 > 
 < 
 
 CO 
 
 2: 
 
 o 
 
 .— ^ o 
 
 d) LU 
 3 X 
 C h- 
 
 
 it i\ 
 
 J 1 
 
 SiSSSS ?*¥ St S>9 
 
 a |i{*;'~ 
 
 1 n 
 
 5 s J: 
 
 fV.i.fJ <?. 
 
 1 II 
 
 ; I. 
 
 Si I 1 i- 
 j-5 ? £ Si 
 
 * * * * 
 
 ill i 
 
 !•; 
 
 I J J 1 
 
 ! jj j* [| f' J' { 
 
 H II £ , 
 
 i.3 J 
 
 (TJ 
 
134 
 
 o 
 
 ij 
 
 \\ i 
 
 is 8 
 
 s * i:- - 
 
 
 O 
 
 o 
 
 a: 
 
 LU 
 
 CO 
 LU 
 
 1 
 
 i i Ij « si 
 
 ||SS£-I?-*3 
 
 < z 
 
 X < 
 
 I- 
 
 o 
 a: — 
 
 s 
 
 5 J 
 
 K <-> 
 O < 
 CL 
 to 
 
 < I- 
 UJ to 
 cc lu 
 
 < 3 
 
 i 
 
 ,' I 
 
 „«. »ts ».»=• ^a 
 
 s.J.siic; 
 
 O 
 to 
 
 0C 
 
 LU 
 
 > 
 
 < 
 
 CD 
 
 O 
 
 -a 
 
 a> LU 
 3 x 
 c.l- 
 
 Si 
 i§ 
 
 -M 
 
 2 H#* £ti ££S*3 S3 I ti t * * S3: £ £ 
 
 ] 
 
 I 1 
 
 !1* J* J 1 
 
 - > il- ? s ; ^ :3 : s i3 
 
 j i IjS 6 5 3 6 £ ^ 
 
 ,14? *»*•*•!* 
 
 _i* s -• s s -3 a 3 
 
 ?>* , ? 2s:... 
 
 « 5 1 ? S i 4 * 4 
 
 
 ! ? II 
 i ; i 
 
 s.r - • : 
 
 - 3 I? t 
 
 I £ **£ 
 
 5 ■;*! |3 
 
 s i i3 2 6 
 
 llilltiili Mn 
 
 u 
 
 i 
 
 ;8 
 
 I 
 
 < 
 
 
135 
 
 REFERENCES FOR APPENDIX 
 
 Note: Abbreviations Used for Technical Reports 
 
 A/Conf » 15 ; Proceedings of the Second International 
 Conference, United Nations Peaceful Uses of Atomic 
 Energy, Geneva, 1958 
 
 DPSPU ; U, So Atomic Energy Commission Technical Reports 
 
 HW and HW-SA ; U„ S Atomic Energy Commission Technical 
 Reports; Hanford Atomic Products Operation, General 
 Electric Company, Richland, Washington 
 
 LAMS ; Los Alamos Scientific Laboratory of the University 
 of California Technical Reports 
 
 NPs U„ S. Atomic Energy Commission Technical Reports 
 
 ORNL ; U» So Atomic Energy Commission Technical Reports; 
 Oak Ridge National Laboratory, Oak Ridge, Tennessee 
 
 RADIOECOLOGY: Proceedings of the First National Symposium 
 on Radioecology held at Colorado State University, Port 
 Collins, Colorado, September 10-15, 1961, U Shultz and 
 A, Wo Klement eds a , Reinhold, New York and The American 
 Institute of Biological Sciences, Washington, D, C, 
 746 pp (1961) 
 
 TIP ; U So Atomic Energy Commission Technical Reports 
 
 USNRDL ; Uo So Atomic Energy Commission Technical Reports 
 
 UWFL ; Uo So Atomic Energy Commission Technical Reports; 
 Applied Fisheries Laboratory, University of Washington, 
 Seattle, Washington 
 
 W; Uo So Department of Health, Education, and Welfare, 
 Public Health Service; The Robert A 8 Taft Sanitary Engi- 
 neering Center Technical Reports, Cincinnati, Ohio 
 
 65 
 1» Bachmann, R, W, , "Zinc in Studies of the Freshwater Zinc Cycle," 
 
 Radioecology , pp e 485-499 (1961) 
 
 2» Barranik, P„ I„, e t al . , "Zinc, Manganese, Cobalt and Iodine in the 
 Drinking Water from the Artesian Wells of Kiev," Gigiena i Sanit , 26, 
 ppo 95-96 (1961) 
 
 3o Bondarenko, G 6 P., "Seasonal Dynamics of Mobile Forms of Trace Elements 
 and Iron in Bottomland Soil of the Ramenskoe Widening of the Moscow 
 River," Nauchn._ Dpkl._ Vysshei Shkoly , Biolo Nauki , 1962, 4, pp 6 202-207 
 (1962) 
 
136 
 
 4 Brown, W H„ . and Fulton, R B., "Metal Content of Mine Waters," Symposium 
 of Geochemical Prospecting, I., Congr Geol„ Intern,, 20th, Mexico City, 
 1956, pp 189-197 (1958) 
 
 5o Carritt, D E , et^ al „ , "Studies of DuPont Spruance Plant Wastes and 
 the James River, 1951-52," 44 pp plus tables (1952, unpublished) 
 
 6„ Chipman, W A , Rice, T R. , and Price, J J,, "Uptake and Accumulation 
 of Radioactive Zinc by Marine Plankton, Fish and Shellfish," U„ So Fish 
 and Wildlife Service, Fishery Bulletin, 58, pp„ 279-292 (1958) 
 
 7„ Cohn, So Ho, Love, R A , and Gusmano, E A , "Zinc ' in Reactor Workers," 
 Science, 133, pp 1362-1363 (1961) 
 
 ■i r ii ii t ■*——■' —i- y - - -' * * 
 
 8 Cowser, K 6 E., Snyder, W S , and Cook, M Jo, "Preliminary Safety Analysis 
 of Radionuclide Release to the Clinch River," TID- 7664, pp 17-38 (1963) 
 
 9 Davis, Jo Jo, "Accumulation of Radionuclides by Aquatic Insects," HW-SA- 3050, 
 13 pp (1963) 
 
 10 o Davis, Jo Jo, Hanson, W G , and Watson, D, G , "Some Effects of Environ- 
 mental Factors upon Accumulation of World Wide Fallout in Natural 
 Populations," Radioecology , pp 35-38 (1961) 
 
 11a Davis, Jo Jo, et al , "Radioactive Materials in Aquatic and Terrestrial 
 Organisms Exposed to Reactor Effluent Water," United Nations Peaceful 
 Uses of Atomic Energy-Proceedings of the Second International Conference, 
 Geneva, September, 1958, pp 423-428 (1958) 
 
 12« Eisenbud, M , Enviro nmental Radioac t ivity , McGraw-Hill, 430 pp (1963) 
 
 13o Fabricand, B c P., et al , "Trace Metal Concentrations in the Ocean by 
 
 Atomic Absorption Spectroscopy," Geochern „ Co smochin , Acta , 26, pp» 1023- 
 1027 (1962) 
 
 65 
 
 14 o Fitzgerald, B W , Rankin, J S , and Skauen, D M , "Zinc Levels in 
 
 Oysters in the Thames River (Connecticut)," Science , 135, p 926 (1962-- 
 notes not 1961 as listed in tables) 
 
 15o Folsom, To Ro , and Mohanrao, G Jo, "Behavior and Significance of Certain 
 Radioactive Isotopes Found in Sewage-Treatment Plants of Various Cities, 
 II o Short-Term Variation and Behavior of Certain Gamma Activities in 
 the Hyperion Treatment Plant," TID-16466, Pto B , 54 pp (1962) 
 
 16 Folsom, To Ro , et al , "A Study of Certain Radioactive Isotopes in 
 
 Selected Waste Treatment Plants," Journal Water Pollution Control Feder- 
 ation, _35, pp 304-333 (1963) 
 
 17 Foster, R F , "Concentration of Radionuclides in Columbia River Water 
 at Hanford and Pasco, 1963," Private Correspondence, 2 pp (1964) 
 
 18o Foster, R F , et al , "Evaluation of Radiological Conditions in the 
 Vicinity of Hanford; Apr -June, 1963," R H Wilson, ed , HW-78395, 
 28 pp (1963) 
 
137 
 
 19 «, Foster, R F , et al , "Evaluation of Radiological Conditions in the 
 Vicinity of Hanford for 1962," R H Wilson, ed , HW-76526, 183 pp. 
 (1963) 
 
 20o Foster, R F , et al„, "Evaluation of Radiological Conditions in the 
 Vicinity of Hanford for 1961," I. Co Nelson, ed , HW-71999, 247 pp 
 (1962) 
 
 21 Foster, R F , et al , "Evaluation of Radiological Conditions in the 
 Vicinity of Hanford for 1960," I„ C„ Nelson, ed , HW-68435, 109 pp, 
 (1961) 
 
 22c Gericke, S„, "Effect of Thomas Phosphate on the Cobalt Content of 
 Meadow Hay," Phosphorsaeure , 22, pp„ 48-60 (1962) 
 
 23o Glebov, F M , and Kozarezenko, P M„ , "The Contents of Microelements 
 in the Water of Springs in and Around Kharkov," Mater ialy Naucho Konfo 
 Sanit o-Gigien Fak„ Khar'kov Med Insto, Posvyashchen. 40-Letiyu 
 Velikoi Oktyabr Sots Revolyutsii, Sbornik, 1958, pp„ 45-46 (1958) 
 
 24 Glebov, F M , and Kozarezenko, P„ M , "The Content of Copper and Zinc 
 in Mineral Waters of Berezovo and Mirgord," Materialy Nauch* Konfo 
 Sanit -Gigien Fak Khar'kov Med Insto, Posvyashchen 40-Letiyu 
 Velikoi 0ktyabr o SotSo Revolyutsh, Sbornik, 1958, pp, 47-48 (1958) 
 
 25 Gutknecht, J „ , "Zn ' Uptake by Benthic Marine Algae," Limnology and 
 Oceanography, £, pp„ 31-38 (1963) 
 
 26o Hanson, W C , et al , "Radioecology Studies in Northern Alaska," 
 HW-SA-3050, 10 pp "Tl963) 
 
 27 Harvey, R Scg "Uptake of Radionuclides by Fresh Water Algae and Fish," 
 DPSPU-63-30-3, 11 pp, (1963) 
 
 28 o Hayakawa, T 0!l "Amounts of Trace Elements Contained in Grass Produced in 
 Japan," Natl, Inst 0| Animal Health Quarto 2, pp 172-181 (1962) 
 
 29 Hayashi, A , "Biochemical Studies on the Trace Elements in Ostrea gigas, 
 II o Distribution in Different Parts of Meat," J Sci H irosh ima Univ, 
 Ser A-II, 25, pp 347-350 (1961) 
 
 30c Healy, J W , et al , "Radiation Exposure to People in the Environs of a 
 Major Production Atomic Energy Plant," United Nations Peaceful Uses of 
 Atomic Energy-Proceedings of the Second International Conference, Geneva, 
 September, 1958, 1£, pp 309-318 (1958) 
 
 31 o Heide, F„, and Singer, E , "The Copper and Zinc Content of the River 
 Saale," Naturwis senschaf ten , 41, pp 498-499 (1954) 
 
 32 o Hutchinson, G E Q , A Treatise on Limnolog y, John Wiley and Sons and 
 New York, 1015 pp (1957) 
 
 33 Junkins, et al , "Evaluation of Radiological Conditions in the Vicinity 
 of Hanford for 1959," HW-64371, 123 pp (1960) 
 
138 
 
 34 Kaye, S V„, and Dunaway, P B„, "Estimation of Dose Rate and Equilibrium 
 State from Bioaccumulation of Radionuclides by Mammals," Radioecology , 
 pp 107-112 (1961) 
 
 35 o Kehoe, R A , Cholak s J„, and Largent , E J,, "The Concentrations of 
 Certain Trace Metals in Drinking Water," Journa l American Water Works 
 Association, _36, pp« 637-644 (1944) 
 
 36o Kiermeier, F , and Winkelman, H„, "Determination and Occurrence of Cobalt 
 in Cow Milk," Z„ Leben sm-Untersucho Uo -Forsch, 115 , pp„ 309-322 (1961) 
 
 37 o Koval'skii, V V , and Letunova, S„ V , "The Role of Phyto and Zooplankton 
 of Water Bodies in Cobalt Migration," Zool Zhur , 40 , pp, 809-817 (1961) 
 
 38 Krainov e S R«, "New Data on Mineral Waters of the Marittime Territory," 
 Byulo Nauchn o -Te kn Inform,, Mi n Geolo i Okhrany Nedr SSSR 1961 , 2, 
 ppo 19-23 ('1961) " 
 
 39 Kreiger, H„ L„, Gilchrist, J E , and Gold, S , "Concentration of Radio- 
 activity and Detection of Cobalt 6° and Zinc 6 ^ in Rainout," Talanta , 6, 
 pp 254-264 (1960) 
 
 40a Kuroda, K„,< Bl Chem„ Soc Japan, 15, pp 88-92 (1940) 
 
 41 Lifshits, G M , "Trace Elements in Underground Waters of the Voronezh 
 Region," Tr Voro nezhsk Zoovetc Inst,, 17, pp 101-109 (1961) 
 
 42 Lifshits, G„ M , "Trace Elements in Waters of Certain Rivers of the 
 
 Voronezh Region," Tr, Voro nezhsko ^Zoovet^ Inst„ , 17, pp 111-117 (1961) 
 
 43o Lomenick, T F , et al , "Study of White Oak Creek Drainage Basin," 
 ORNL-3492, pp 51-62"Tl963) 
 
 44 o Lowman, F„ G„ , "Radionuclides in Plankton and Tuna from the Central 
 Pacific," Radioecology_ 9 pp„ 145-150 (1961) 
 
 45 Lowman, F G , "Iron and Cobalt in Ecology," Radioecology , pp„ 561-569, 
 (1961) 
 
 U6 Lowman, F G , "Radionuclides in Plankton near the Marshall Islands, 
 1956," UWFL-54, 31 pp , (1958) 
 
 47 o Lowman, F„ G , Palumbo, R F„ , and South, D„ J , "The Occurrence and 
 
 Distribution of Radioactive Non-Fission Products in Plants and Animals 
 of the Pacific Proving Ground," UWFL-51, 61 pp„ (1957) 
 
 Fin 
 48 o Marquez, L , da Costa, N Lo, and de Almeida, I„ G , "Cobalt from 
 
 Thermonuclear Tests in the Atmosphere," NP-7022, 10 pp (1958) 
 
 49o Marquez, L , da Costa, N L , and de Almeida, 1 G , "Radioisotopes from 
 Fusion in Rain Water: Co 57 , Mn 54 , and Co 50 ," A/Confo 15/ P/2285, 7 pp 
 (1958) 
 
139 
 
 50 McConnon, Do, "Dose Rate Measurements of Beaches and Islands on the 
 Columbia River between Ringold and Richland," HW-72229 Trb., 21 pp 
 (1962) 
 
 51 o Murakami, T„, et alo t "Inorganic Constituents in Marine Organisms, III, 
 Quantitative Determination of Molybdenum, Lead and Cobalt in Shellfish," 
 Himeji K ogyo Daigaku Ken kyu ^okoku, 13 , pp„ 98-108 (1961) 
 
 65 
 52 Murthy, G K , Goldwin, A S , and Campbell, J„ E , "Zinc in Foods," 
 
 Science ^ 130, pp„ 1255-1256 (1959) 
 
 53 Nagasawa, K , et al 09 "Radioactivity Contamination of Foods by Atomic 
 or Hydrogen Bomb Explosion, IX, Radiochemical Analysis of Radioactive 
 Elements Contaminating Fish Livers in 1958," Eisei Shikenjo Hokoku, 77, 
 pp 6 458-465 (1959) 
 
 54 Nielsen, J M , "Behavior of Radionuclides in the Columbia River," 
 TID-7664, pp 91-105 (1963) 
 
 55 Obukhova, Z D , et al„, "Content of Manganese, Iodine, Copper, and 
 
 Cobalt in Cereal Grain and Grass Fodder of Chuya Valley," Mikroelementy 
 v Zhivo tnovod styei Rastenievodst ve, A kad Nauk Kirg„ SSR 1962 , 1, 
 pp 71-106 {1962) " ' ~ 
 
 56 o O'Connor, J T , Renn, C E , "Soluble-Adsorbed Zinc Equilibrium in 
 
 Natural Waters," Journa l American Wat er Wo rks Association , 56, pp„ 1055- 
 1061 (1964) 
 
 57 6 O'Connor, J T,, Renn, C„ E , and Wintner, I „ , "Zinc Concentrations in 
 Rivers of the Chesapeake Bay Region," Journal American Water Works 
 Association, 56, pp„ 280=286 (1964) 
 
 58, 
 
 65 
 Osterberg, C oe "Zn Content of Salps and Euphausiids," Limnology and 
 
 Oceanography, 7^, pp„ 478-479 (1962) 
 
 59 Osterberg, C , Kulm, L D , and Byrne, J V , "Gamma Emitters in Marine 
 Sediments near the Columbia River," Science, 139 , pp 916-917 (1963) 
 
 60o Osterberg, C , Pattulo, J„, and Pearcy, W , "Zinc-65 in Euphausiids as 
 Related to Columbia River Water off the Oregon Coast," Limnology and 
 Oceanography, 9_, pp 249-257 (1964) 
 
 61 Palmer, R F„, "Accumulation of Radioisotopes by Rats Chronically Exposed 
 to Reactor Effluent Water," HW-53362, 16 pp„ (1958) 
 
 62o Parker, P L , "Zinc in a Texas Bay," Publ. Inst» of Marine Sc ience, 8, 
 ppo 75-79 (1962) 
 
 63, Parker, R A , and Hazelwood, Do H , "Some Possible Effects of Trace 
 Elements on Fresh=Water Microcrustacean Populations," Limnolo gy and 
 Oceanography , 7^, pp 344 = 347 (1962) 
 
 c c 
 
 64 Perkins, R W , and Nielsen, J M„ , "Zinc ' in Foods and People," 
 Science, 129, pp 94-95 (1959) 
 
140 
 
 65 Perkins, R W , Nielsen, J M. , Roesch, W„ C„, and McCall, R. C„, "Zinc 65 
 and Chromiurn-51 in Foods and People," Science , 132 , pp. 1895-1897 (1960) 
 
 66 o Report of the Government Chemist upon the work of his Department for the 
 
 year ending 31 March, 1957, H„ M„ Stationary Office, London, 36 pp. (1957) 
 
 67, Rice, T R„, "The Role of Phytoplankton in the Cycling of Radionuclides 
 in the Marine Environment," Radioecology , pp„ 179-187 (1961) 
 
 68c Rice, T R., "Review of Zinc in Ecology," Radioecology , pp. 619-633 (1961) 
 
 69o Roesch, W Co, McCall, R„ C , and Palmer, H E„, "Hanford Whole Body 
 Counter-1959 Activities," HW-67045, 50 pp„ (1960) 
 
 70o Rona, E , Hood, D W«, Muse, L„, and Buglio, B„, "Activation Analysis of 
 Manganese and Zinc in Sea Water," Limnology and Oceanography , 7, pp„ 201- 
 206 (1962) 
 
 71 Sameshima, M , and Saito, K„, "Radiological Contamination of Fish, Sea 
 Water and Plankton in the Southern Region of Kaigoshima Prefecture 
 during the period from November 1959 to December 1960," Kaigoshima 
 Daigaku Suisan Gakubu Kiyo , 10 , pp 15-22 (1961) 
 
 72 Seymour, A H„, "Radioactivity of Marine Organisms from Guam, Palau, and 
 the Gulf of Siam, 1958-1959," Radioecology^, pp 151-158 (1961) 
 
 73 Skauen, D„ M„ , "Radioactive Zinc-65 in Marine Organisms in Fisher's 
 
 Island Sound and its Estuaries t Final Report „ December 1, 1959 through 
 November 30, 1963," TID-19922, 50 pp (1964) 
 
 74„ Skauen, D M„ s "Radioactive Zinc-65 in Marine Organisms in Fisher's 
 
 Island Sound and its Estuaries: Progress Report," TID- 13509, 32 pp„ 
 (1961) 
 
 75 o Sprague, J„ B«, and Carson, W V„, "Chemical Conditions in the Northwest 
 Miramichi River during 1963," Fisheries Research Board of Canada, Bio- 
 logical Station, St Andrews, New Brunswick, Canada, 62 pp (1964) 
 
 76 Swanberg, Jr , F , "Quantitative Measurements of Some Gamma-Ray Emitting 
 Radionuclides in Nuclear Industrial Workers by Whole Body Counting 
 Techniques," Health Physics, 8_, pp 67-71 (1962) 
 
 77 6 Thomas, C W„, Reid, D L», and Lust, L F , "Radiochemical Analysis of 
 Marine Biological Samples Following the 'Redwing' Shot Series--1956," 
 HW-58674, 81 pp (1958) 
 
 78 o Thompson, T G , and Laevastu, T«, "Determination and Occurrence of 
 
 Cobalt in Sea-Water," Jou rnal of Marine R ese arch, 18 , pp 189-192 (1960) 
 
 79 Uzumasa, Y , and Akaiwa, H , "Chemical Investigations of Hot Springs of 
 Narugo, Miyagi Prefecture," Nippon K a yak u Zasshi, 81 , pp 912-915 (1960) 
 
 80. Van Dilla, M A., "Radioactivity in Nevada Cattle; 1959," LAMS- 2627, 
 pp. 226-233 (1961) 
 
141 
 
 81 Van Dilla, M A , "Zinc-65 and Zirconium-95 in Food," Science , 131 , 
 pp 659-660 (1960) 
 
 82o Van Dilla, M„ A,, and Engelke, M J , "Zinc-65 in Cyclotron Workers," 
 Science , 131, pp 830-832 (1960) 
 
 83 o Vekilova, F I„, et al„, "The Abundance of Cobalt in Natural Waters," 
 Iz vo Akado Navk A zerb. SSR, Ser Geol-Geogr.-Nauk i Nefti 1962 , 2, 
 pp. 43-52 (1962) " ' " 
 
 84 Vinogradova, Z. A , and Kovaljskii, V V,, "Element Composition of the 
 Black Sea Plankton," Dokl Akado Nauk SSSR , 147, pp 1458-1460 (1962) 
 
 85 Warren, H V , Delavault, R E., and Irish, R I., Bulletin Geological 
 Society of America, 62, pp„ 609-618 (1951) 
 
 86 o Watson, D G , and Davis, J Jo, "Concentration of Radioisotopes in 
 
 Columbia River Whitefish in the Vicinity of the Hanford Atomic Products 
 Operation," HW-48523, 136 pp (1957) 
 
 87 Watson, D Go, Davis, Jo Jo, and Hanson, W„ C , "Interspecies Differences 
 in Accumulation of Gamma Emitters by Marine Organisms near the Columbia 
 River Mouth," Limnology and Oceanography, 8_, pp 305-309 (1963) 
 
 88 Watson, D G„, Davis, Jo Jo, and Hanson, W„ C , "Zinc-65 in Marine 
 
 Organisms along the Oregon and Washington Coasts," Science , 133 , pp 1826- 
 1828 (1961) 
 
 89o Weiss, H V , and Reed, J A , "The Determination of Cobalt in Seawater," 
 USNRDL-TR-401, 9 pp (1960). Journal of Marine Research, 18, pp, 185- 
 188 (I960) 
 
 90» Weiss, Ho V , and Skipman, W H„, "Biological Concentration by Killer 
 
 Clams of Cobalt-60 and Radioactive Fallout," Science , 125, p 695 (1957) 
 
 91o Welander, A D , "Radiobiological Studies of the Fish Collected at 
 Rongelap and Ailinginae Atolls, July 1957," UWFL- 55, 29 pp (1958) 
 
 92o Young, R„ S , "Copper, Nickel and Cobalt Content of Oyster Shells," 
 Jour nal of Agriculture and Food Chemistry , 8_, pp 485-486 (1960) 
 
142 
 
 ADDITIONAL REFERENCES FOR APPENDIX 
 
 fin 
 la Abrunina, G A„, "Co Metabolism in Rats and Rabbits after Single 
 
 Administration and Calculation of Body Dose," The Toxicology of Radio- 
 acti ve Substances, 2, pp 14-29, The MacMillan Company, New York (1963) 
 
 2o Ballou, Jo Eo, "Metabolism of Zinc-65," HW-59500, pp. 81-86 (1960) 
 
 3 Bedrosian, P„ H , "Relationships of Certain Macroscopic Marine Algae 
 to Zn-65," Dissertation Abstract, 22; 3146, University of Florida, 
 Gainsville (1962) 
 
 4 Craig, F A , and Siegel, E,, "Distribution in Blood and Excretion of 
 Zn-65 in Man," Proceedings Society for Experimental Biology and Medi- 
 cine, 104 , pp„ 391-394 {i960) 
 
 5 Donaldson, L R« , "Radiobiological Studies at the Eniwetok Test Site 
 and Adjacent Areas of the Western Pacific," W-60-3, pp„ 1-7 (1960) 
 
 6« Donaldson, L. R« , "Panel Summary — Effects of the Discharge of Radioactive 
 Materials on Aquatic Life," W-60-3, pp 40-41 (1960) 
 
 7 Foster, R F , "Relationships between the Concentration of Radionuclides 
 in the Columbia River Water and Fish," TID-7664, pp 269-288 (1963) 
 
 8 Friend, A G , "The Aqueous Behavior of Strontium-85, Cesium-137, Zinc-65 
 and Cobalt-60 as Determined by Laboratory Type Studies," TID- 7664, 
 pp 43-56 (1963) 
 
 9 Frolova, L K , "Behavior of Radioactive Cobalt in Fish," Zhur Obshchei 
 Biola, 21, pp 301-305 (1960) 
 
 10o Gutknecht, J , "Mechanism of Radioactive Zinc Uptake by Ulya l actuca ," 
 Limnology and Oceano graphy , 6_, pp 426-431 (1961) 
 
 11a Hanson, W C , and Case, A C , "A Method of Measuring Waterfowl Disper- 
 sion Utilizing Phosphorous-32 and Zinc-65," Radioecology , pp 451-454, 
 (1961) 
 
 12» Held, Eo Eo, "Qualitative Distribution of Radionuclides at Rongelap 
 Atoll," Radioecology, pp 167-171 (1961) 
 
 13 o Lackey, J B , and Bennett, C F , "Micro-Organisms in Environments 
 Contaminated with Radioactivity," Radioecology , pp 175-177 (1961) 
 
 14 Ladd, E C , "Zinc Solubility in Shenandoah River," American Viscose 
 
 Corporation Memorandum, February 29, 1960 to J E Corr at Front Royal, 
 Va , 4 pp (1960) (unpublished) 
 
 15a Mauchline, J , Taylor, A M , and Ritsen, E B , "The Radioecology of a 
 Beach," Limnolog y and Oceanography, 9_, pp 187-194 (1964) 
 
143 
 
 16 o McKenney, J R , McClellan, R , and Bustard, L K„, "Early Uptake 
 
 and Dosimetry of Zn-65 in Sheep," Health P hysics , _8, pp„ 411-421 (1962), 
 HW-SA-2338, 10 pp„ (1962) 
 
 17 McKenney, J. Ro , et^ al c , "Metabolism of Zn-65 in Pregnant Ewes," HW-69500, 
 195 pp (1961) 
 
 18 Nakatani, R E , and Miller, W„ P., "Distribution of Zn-65 after Inges- 
 tion by Trout," HW-76000, pp<> 111-114 (1963) 
 
 19, Parker, F., "Clinch River Studies," TID°7664, pp 161-180 (1963) 
 
 20o Pritchard, D W , "Problems Related to Disposal of Radioactive Wastes 
 in Estuarine and Coastal Waters," W-60-3, pp„ 22-32 (1960) 
 
 21 o Richmond, C R , Furchner, J E , and Trafton, G„ A„, "Metabolism of 
 Zinc-65 in Mammals," LAMS- 2445, pp 80-89 (1959) 
 
 22 Rubini, M„ E , et al , "Metabolism of Zinc-65," American Journal of 
 Physiology , 200, pp 1345-1348 (1961) 
 
 23o Siegel, E , Craig, F A , Crystal, M M , and Siegel, E P., "Distribution 
 of Zn-65 in the Prostrate and Other Organs of Man," British Journal of 
 Cancer, 15, pp„ 647-664 (1961)