115 . . . - .:47 SAWERE D.. ALL LIEVE 1 . 1 ' " . T . 1 r. . . T . . PERTERET.'.. - 75 iti " 1 A . . .- F . "hi 1 TL RI :21 I I . . .. . . .. .! .. .. . . ' . . . . . TEXTO 1 . . :.. .47. LT . 7 2.1 .. . ... : : . i . . . . . ... : : 9. RI 1. .: .',. .:1 11HT. - . i . . wait ... Y... . . 2. .. .. T.... ' : in " . i ... 1'. .. : NH . . AT LA 7 ".D WENTY . .. TAL.-ROOLID án 1 : 7 1 T 7.ATADA " :* . : 1 ''L .. : L 1. STT . . . . ? , .. .. . .. * ' . WALA CLIEKTI : * St. - 4 4 4 :*:* :*: E FFY - THE Aynur UNCLASSIFIED ORNL Р. 1154 . . . T . : . :. ---- ity 24 OINI - AC-CIRICIAL 1112' usoodji - Tree i : LEGAL NOTICE – APR 27 86 " r" : 1 The report we prepared an account of Government O rd work. Watcher the United data, por the Courtoa, nor w pur og sett og blod Comindoni A. Maka may marteaty or reprezestadon, aprend w lap., Moroct to die noco- racy. capith, or totalment at the talordito contatud b to report, or out the w ol ay tuloration, apparte, wethod, or procu declared in the report any not to be printaly owned rtcu; of B. Awer my abilities with respect to the wwe of, for den su rezulthy fross the in day taformation, appuntua, bet ud, or procu daclound in this report As and b e bore, "persoa actag on all of the Cocaminator" tuctura ay na- ploys or contractor of the Commission, or employee of such sootractor, to the most chat much mployee or contructor of de Constanta, or employee of mucha contractor sopar, 1 dins butus, or provides noceo to, nay tafordato para DI M. employment of contract wobe De Coagularla, or his employment wild anica contractor, . 312 - ht . Ra, . t contract with the Union Carbide Corporation. *Research sponsored in part by the U. S. Atomic Energy Commission under (Sponsored by the European Nuclear Energy Agency of the 0.E.C.D.). Research Center of Grenoble, Grenoble, France, 15th - 18th June 1965 Symposium on Working Methods In High Activity Hot Laboratories, Nuclear To be presented (17 June 1965, 16:05-16:20 hr) at the International Vallecitos Atomic Labora Robert F. Stearns U.S. Naval Radiological Defense Laboratory Ross K. Fuller Los Alamos Scientific Laboratory Jerome E. Dummer Vallec Robe Acond St Laboratory IP (Formerly Hanford Laboratories) Pacific Northwest Laboratory Ernest A. Berreth Oak Ridge National Laboratory Clyde D. Watson RU ARE ON FILE IN THE RECEIVING SCHON THE PUBLIC IS APPROVED, PROCEDURES PATENT CLEARANCE OBTAINED. RELEASE TO ASI-AYNUO DECONTAMINATING 10T CELLS* POLICY AND PROCEDURES USED IN THE UNITED STATES PORTAL 1 Paper Communication No. 40 .3.6138 CONF-650604-3 " .-.-.-- ORNL - AEC - OFFICIAL ORML - AEC - OFFICIAL ., . . 1 . . Ch ". '. '. . ORNI - AI- OFFICIAL POLICY AND PROCEDURES USED IN THE UNITED STATES FOR DECONTAMINATING HOT CELLS Clyde D. Watson, Ernest A. Berreth, Jerome E. Dummer, Ross K. Fuller, and Robert F. Stearns Abstract In the United States, hot cells and equipment for handling radio- active solids or liquids are successfully decontaminated as required. The frequency varies from about three times a year to only once in three years for the larger pilot plant units. The normal time required to decontaminate a facility is about two to six weeks. Decontamination is usually done remotely, through appropriate design, precontamination application of protective coatings, expendable equipment, the proper choice of cleaning reagents (detergents, organic solvents, acids, alkalies, chelating agents and physical methods (grinding, ultrasonic cleaning, blasting, and abrading). Methods have been developed and are presented in this paper for decontaminating hot-ce118 and adjacent areas subjected to the uncon- trolled release of radioactivity. RÉGLEMENTS ET MÉTHODES EMPLOYÉCS AUX ÉTATS UNIS POUR LA DÉCONTAMINATION DE CELLULES CHAUDES Clyde D. Watson, Ernest A. Berreth, Jerome E. Dummer, Ross K. Fuller, and Robert F. Stearns. Résumé Aux Etats Unis les cellules chaudes à activité élevée et l'équipe- ment utilisé pour manipuler les éléments radioactifs sont décontaminées à la demande avec grand succes. La fréquence de décontamination varie de 3 fois par an à une fois seulement en 3 ans pour les grandes unités pilotes. Le temps normalement requis pour décontaminer une installation est de l'ordre de deux à six semaines. La décontamination est ordinaire. ment faite a distance grâce à une disposition appropriée de l'équipment, à l'emploi de recouvrements protecteurs avant contamination, et de pièces non réutilisables et grâce au choix de produits de nettoyage (détergents, solvants organiques, acides, bases et agents de chelation) et de méthodes physiques (broyage, ultrasons, nettoyage par jets et polissage). . : La présentation décrit des méthodes utilisées pour' décontaminer les cellules chaudes et les zones adjacentes ou la radioactivité peut involontairement s'étendre. mera ORNE L " LALO *. 13 .: . -2. INTRODUCTION 0111-ABC - OFFICIAL Research and development investigators using radioactive nuclides are confronted ultimately with the problem of removing and disposing of them. Decontamination is the practice or art of removing radioactive materials in the form of soils, chemical compounds and solutions, The tal fines, reaction products, etc., from valuable surfaces in order to: . 1. render such surfaces (hot cells, buildings, areas) harmless or safe to unprotected operators and the surrounding bic!og- ical environment; restore valuable production, research, development facilities, and equipnent to a condition suitable for reuse; or to 3. aid in safely removing unwanted radioactivity, contaminated materials, and equipment from an undesirable location to a more desirable one. Decontamination became a serious topic of interest soon after the Enrico Fermi Pile began operating, in December 1942. Early in 1943 at Oak Ridge National Laboratory, then Clinton Laboratories, the literature reports an investigation (1,2,3) of reagents for removing fission products from work areas and equipment used in processing plutonium. As the nuclear industry grew, each laboratory or site developed favorite methods, but no "universal" methods or "magic" solutions emerged. Consequently, decontamination as practiced in the United States varies from one site to another, depending on the nature of the work, age (design) of facilities, and convenience of waste disposal. Since 1943, the field has been extensively investigated and the results presented in numerous reports. Much of the information is contained in recent books (4,5,6,7). Commercial interest has grown sufficiently that several companies have entered the field in the past 10 to 15 years (8,9, 10, 11, 12, 13). Nuclear sites now depend more and more on commercial sources for chemical and physical methods. Generally, decontamination is considered to be a highly effective cleaning process (14, 15). In addition, the processes carry with them the associated problems of controlling the exposure of workers to ionizing radiation; preventing the contamination of workers and recontamination of areas; criticality considerations; the generation, 10 QINI-AEC - OFFICIAL - . . T SU- Jaro TRIO treatment, and disposal of various types of radioactive wastes; and the loss of use of work areas and equipment for extended times. This paper is a survey of current decontamination policy and basic procedures practiced throughout the United States for removing radio- active contaminants. The procedures reported here are specific for hot-laboratory operations, especially hot cells handling solids and, or, 11quido, and for supporting enclosures and other barriers used in conjunction with the cells. The practices range from spraying and mopping of solutions designed to decontaminate metals while only slightly affecting the inetals, themselves, to gross surface removal by grinding or blasting. In addition, some procedures are presented which were found effective in the decontamination of the structural and biological environmer. contaminated as the result of the uncontrolled release of radionuclides from hot-cell operations. GENERAL POLICY Decontamination work has undergone significant evolutionary changes . . during the past 20 years both in general policy and in procedures. When first tried, the nearly complete removal of radioactivity was attempted. However, it was soon realized that complete decontamination was not only costly and impractical but that the object or surface treated was either damaged or ruined. Most important, thorough decon- tamination cailed for close contact, a threat to the health of the worker. Thus, it became much more economical and safer to clean the inside of a hot cell remotely, even if fairly expensive equipment was required, than to use the "ce11-entry" or direct-worker method in high radiation fields. The present attitude may be summed up as, "Radioactive contamina- tion is a necessary evil best managed by avoiding it or by working around it." This is done by designing cells and equipment to minimize the need for decontamination. In addition, equipment is arranged so that it can be remotely maintained by replacement of parts of subassem- blies with manipulators. For example, equipment, tools, etc., where practicable, is inexpensive and commercially available. They are usually modified to make remote installation, operation, maintenance, . and removal easier. If worn out or if remote maintenance proves unsatisfactory, such equipment can be discarded. It is also advan- tageous to localize or limi'e the spread of contamination by placing ORNL - AEC - OFFICIAL -4. ORN - AEC - OFFICIAL shielding around the hottest sources, conducting the experiment in a box placed in the cell and by using other barriers, and trays (see Paper 52 of this Symposium, "u.s. Practices In The Control and Contain- ment of Radioactive Contamination," K. R. Ferguson). In addition to being protected by containment barriers, the cell walls and floors, equipment surfaces, and tools are further protected by surface treatments before contamination occurs. Radiation-resistant organic protective coatings, marking inks, water soluble paints, plas- tic sheeting, and tapes are commonly used. The u.s. policy is reflected in the Transur anium Processing Plant at ORNL, now being built, which is designed for completely remote maintenance and decontamination (16). All equipment, including the piping system, may be disconnected and replaced by in-cell manipulators.' Normally, complete decontamination of a cell for entry by workers should never be required here. The cell bank is designed so that all opera- tions can be isolated and so that transfers between the nine cells can be made in a sealed conveyor. This helps ensure that even a serious spill in one ce11 will have little effect on adjacent ones. Summarizing, in the U.S.A. today, we design hot cells to reduce the need for cleanup, and, when we do decontaminate them, it is done by remote manipulation and only to the extent required. Total decon- tamination is rarely required or accomplished. Insofar as possible, a similar policy is pursued in the older hot cells and large-scale engineering facilities, some of which ar: not equipped with mechanical ustnipulators. CONTAMINATION AND DECONTAMINATION MECHANI SMS com. It is generally accepted that contamination of a surface by radionuclides occurs through chemisorption, by ion exchange with free surface ions, and by physisorption or physical adhesion. A11 this is accompanied by migration of the nuclides into cracks and crevices. Only a few minutes is required for radioactive ions to become attached to the surfaces of metals and other structural materials (17). Experi- ence has shown that radioactive ions are fixed by the visible and invisible oxide films on metals; after extended contact times (months ), the contaminants diffuse into the parent metal and interact beneath ORNL - AEC - OFFICIAL the oxide films. -5- Decontamination (15) also includes chemical and physical mecha- nisms. The radioactive atoms which have combined with nonradioactive ones are dissolved by contacting them with a strong solvent while simultaneously preventing their redeposition. This 18 usually done with solutions of strong acids or alkalies which also contain com- plexing and chelating agents. The physical methods include the removal of loosely adhering surface scales, soils, salts, and particulate matter, and the abrading away of oxides and a surface layer of the material itself. Examples of the methods are: vacuum cleaning, swabbing, brushing, high-impact jet cleaning (with steam or water), sandblasting, and grinding. An ideal method would be one that leaves a surface in its original condi- tion of smoothness and utility, but this is rarely achieved. PROCEDURES To simplify the presentation of typical procedures, either chemi- cal or physical, two general types of hot-ce11 facilities are considered. Hot Cells in Which Solids are Handled Hot cells in which solids are handled are used primarily for conducting experiments that include mechanical processing or dis- mantling, and metallurgical operations, all of which generate partic- ulate matter (principally grindings, sawings, turnings, oxides, etc.). Although the cleaning sequence may vary from site to site, it is usually done in three phases. Phase I includes the general cell cleanup, in which loose, transferable or smearable activity is removed by remotely controlled. operations. Debris generated by the operation, itself, 18 collected . by sweeping or vacuum cleaning. Then it is removed from the cell (see Paper 30 of this Sympos lum, "Methods used in the U.S.A. for Transferring Materials Through Radiation Barriers," J. W. Schulte). Sticky tapes, treated paper, dusting cloths, damp sponges, or absorbent rags are used when vacuum cleaning fails. In the second part of phase I, visible deposits of more tightly held soil, rust, dried salts, and thin films of grease, and oil, etc. are removed from equipment, cell walls and floors. This is done with brushes, absorbent pads, sponges, and rags moistened in aqueous solutions of detergents and, or, complexing agents. Wet vacuum- ORNL - AEC - OFFICIAL ----- -6. ---08N1 - AEC - OSFICIAL cleaning devices like the "slurpper" (18, 19) are also useful. Manipulator-operated household floor polishers, fitted with a líquid supply line and coarse brushes or steel wool, are used for scrubbing floors, walls, and other flat working surfaces. Grease and oil are removed easiest with an organic solvent such as trichloroethylene (20). Some degreasers are obtainable in aerosol cans. Some sites remove loosely held radioactive matter with steam and water jets. Here, proper cell design and large disposal facilities for these liquid wastes are necessary. Other sites do both: Swab and clean with steam jets. Contamination that is smearable or that can easily be resuspended in air to form aerosols is sometimes fixed to the surface of equipment with glycerin or acrylic and vinyl lacquer (21). The fixing of radio- activity, along with other normal packaging precautions used in transferring equipment into temporary storage or to a nearby decon- tamination facility, prevents the spread of radioactivity and the recontamination of areas. The overall cleaning operation is best done by beginning high in. the cell, taking care not to flood electrical equipment and in-cell filters (some items can be covered with protective polyethylene mem- brane taped in place). Then one works downward to the floor. Clean- ing only a portion of a cell at a time is essential to prevent fogging the viewing windows. Rubber squeegees placed in the cell before jet cleaning are helpful for removing moisture from the windows. In phase II, the radioactivity level of the cell and equipment is measured and graphically charted, followed by more drastic measures for tenaciously held activity. A record is essential in following amer met the degree of decontamination and in determining which equipment can . . . IN .. be removed by remote manipulation to make access to the remaining equipment easier. In addition, it is necessary to determine when radiation levels in the cell are sufficiently low to permit entry by the operators. The hot spots in the cell are selectively attacked, beginning with the most contaminated areas; chemical and physical methods are used, according to the materials involved. Effective chemical decontaminants for various sur faces are listed in Table 1. More information can be found in a review of commercial procedures for cleaning metals. A recent book by Spring (22) 18 an excellent reference. -ORNL - AEC - OFFICIAL x LLERLE.L1.MA. . . Sw 1. . 121 . Table 1. Chemical Decontaminants for Removing Mixed Fission Products From Various Types of Surfaces 02115 ~ AEC - OFFICIAL .. . . . . .. -- . .. edi . .. . . ..... - . . 6 M - c. . 1. Stainless Steel 3. Aluminum a. Oxalic acid, 0.5 M (33); a. Use solution 2a. hydrogen peroxide, 0.3 M; sodium or ammonium fluoride, | b. Turco (8) and others as in lc. 0.1 M; Temp., 85-95°C 4. Lead Contact time, about 1 hr a. Dilute nitric acid chosen for Can be destroyed by adding desired degree of attack H2O2 and heating • Concentrated hydrochloric Oxalic acid, 0.4 M (23); acid hydrogen peroxide, 0.5 M; c. Turco (8) and others as in lc. ammonium citrate, 0. sodium or ammonium fluoride, 0.05 M; 5. Copper, Brass Raise to pH 4 with NH OH; a. Dilute nitric acid Temp., 85-95°C b. Turco (8) and others as in lc. Contact time, about 1 hr This version less corrosive Household and industrial to nearby carbon steel; cleaners for brass, copper Can be destroyed as in la. (25) Turco Products (8): 4306-B, 4306-C 6. Glassware Consult Turco and others a. Ultrasonic cleaning using (9, 10, 11, 12, 13) Turco 4234 d. Nitric acid, 1.5 M (24); b. Automatic household dish- sodium fluoride, 0.02 M washers and their cleaning e. Sulfuric acid, 1.5 M (23); agents hydrogen peroxide, 0.1 M; 7. Painted Surfaces Temp., 85-95°C Contact time, about 1 hr a. Commercial paint cleaners such as Oakite (26) and 2. Carbon Steel others a. Oxalic acid, 0.4 M (33); b. Steam-water and detergent hydrogen peroxide, 0.34 M; I c. Solvents and paint strippers citric acid, 0.16 M Ad just to pH 4 with NH4OH or 8. A11 Surfaces suitable mixture of salts Temp., 85-95°C a. Steam-water and detergent Contact time, about 1 hr b. Turco (8) and others as in lc. Can be destroyed as in la. Removes rust and inhibits future rusting 9. Special Equipment b. Turco Products (8): See (8, 9, 10, 11, 12, 13) and 4518, 4512, 4324 (27 28) Consult Turco and others, as in lc. . . . . . . . . . . . . . . . .,' . .. . . : 1. . ... - ORNL - AEC - OFFICIAL -- . -.. . C. Commercial rust removers 02:11 HIC - OFFICIAL : Physical methods for cleaning hot spots include ultrasonic clean- ing (for tools, etc.), chipping, scraping, grinding with an abrasive disc mounted on a flexible shaft, filing, scouring with coarse stainless-steel wool, with wet pumice, or with wet-dry emery cloth and toothbrush-size brushes fitted with stainless-steel bristles. The surfaces on the coll and equipment are repeatedly subjected to chemical and physical treatments until they are no longer effective or until tolerable levels of radioactivity are reached. Equipment that can be removed by remote handling is selectively taken out of the cell as decontamination progresses. In phase III, operators enter the cell to (a) assist in removing the remaining equipment, (b) continue the decontamination of remain- ing hot spots, and (c) install new equipment for future work. All this may be done by the cell operators or by an independent group specializing in this kind of work. As equipment is removed from the cell, workers are usually required to cut lines not easily cut by manipulators remotely. They often use power tools or hydraulic shears. Initial encry is made by workers wearing two suits of coveralls sealed with masking tape, shoes or boots covered with two pairs of shoe covers, two pairs of rubber gloves, an assault mask and hood, or a plastic air suit. After smears are taken and the extent and type of contamination has been established, later entries may be made by workers wearing plastic rain gear over the coveralls. In addition, an assault mask or plastic air mask is worn. After all equipment has been removed, the remaining hot spots are cleaned remotely or directly by in-cell workers as re- quired. The radioactivity levels should now be no higher than 10 to 100 mc/hr. Generally, as new equipment is installed, all cell entries can be made by workers clad in a single suit of clothing and wearing the assault mask. A full-vision plastic face mask supplied with fresh air by a hose has replaced the assault mask at some sites. IČ usually takes two to six weeks to drcontaminate typical facil. . ities, from the smallest to the largest. An exception is found in specialized box-in-cell facilities, which may require only one to three days. There is no apparent practical limit to the number of times a hot cell can be cleaned if it is suitably protected or lined with . . . - --------OR1L-AEC - OFFICIAL -9- O:;! - AIC - 0:1101;!.. stainless steel. Decontamination, however, may become more difficult each successive time because of the surface defects produced by previous efforts. Hot Cells in Which Solutions are Handled The primary source of contamination in cells in which radioactive solutions are used arises from spills and dried salts. Typical opera- tions include the isolation and purification of radioisotopes, the deve lopment of chemical processing methods for recovering spent nuclear fuels, and radiation chemistry in general. The cell equipment is usually not purely mechanical, consisting principally of tanks, piping, pumps, valves, glassware, and instrument lines. Yet, decontamination is similar in many respects to that for cells in which solids are handled. The principal difference is that the interiors of tanks, vessels, piping, pumps, instrument lines, etc., must be cleaned. Therefore, much larger volumes of decontaminating solutions are required. The procedure used in a typical cell consists of six steps, the first two of which are: 1. The interior of the cell is surveyed with remotely operated radiation-detection instruments, and a graphic chart of the radiation levels associated with equipment, walls, floors, etc., is prepared. 2. Sequential flushing of piping, tanks, and external surfaces are repeated until there is little or no change in radiation levels. The cleaning solutions used are varied, but the usual approach includes a general spray of jet washdown with water and detergent. This is followed by an oxidation-reduction treatment with appropriate reagents. Three examples of step 2 follow: A. At the ORNL Fission Product Development Laboratory (29), the normal sequence of solutions steam-jetted or pumped through the vessels and lines is: water plus detergent; 5% HNO3; water; 5% NaOH; water; 0.1 M Versene;* water; 5% NaOH; water. The sequence is repeated until radioactivity measurements on the washings show no further decline. After decontamination of vessels and piping, the cells are opened, and . the exterior surfaces are spray-washed to remove soluble matter. The normal sequence here is: water; Turco 4502 (8); 5% oxalic acid; water; and sometimes, 5% NaOH washes. However, in FPDL cells contaminated ORNI-MEC - OFFICIAL". *Ethylenediamine tetraacetic acid -10- by insoluble fission product compounds (e.8., strontium-90 titanate, cerium-144 oxide, cesium-137 glass), a different approach is used. Here, most of the decontamination calls for the use of detergents, water, and mechanical removal of insoluble particles. Acids and alkalies are ineffective. Surfaces are cleaned by pressure spraying with water, steam, and detergents. Manipulator held fiber brushes, adhesive strips, sponges, polishing wheels with cloth or fiber pads, and cellulose wipes are also used. Highly contaminated spots may be cleaned with household abrasives. B. The High Level Radiochemistry Facility at Hanford uses a sequence of alkaline permanganate and oxalic acid or ammonium citrate solutions containing inhibitors, and wetting agents. Turco solutions of similar composition are also used. Solutions are not recirculated. About two to three gallons of solution for each cubic foot of cell. volume is used for each decontamination. C. The Radiochemical Processing Pilot Plant at Oak Ridge (30) used a sequence of solutions presented in Table 2 for cleaning equip- ment contacted by mixed fission products and plutonium during processing of spent nuclear fuels. About 5.25 gallons oë total liquid was used per cubic foot of cell space. After the level of radiation in a cell has been reduced to reasonable levels (see steps 1 and 2 and examples A, B, and C above) the following is done: 3. Equipment is dismantled remotely, encased and removed, if necessary in shielded casks, for burial. A11 equipment is discarded, with but few exceptions. 4. After preparation for cell entry by high-pressure steam cleaning at the point of entry, the cell is entered, and equipment dismantling is continued. Dismantling is done with long-handled bolt cutters for cutting connections to stainless-steel tubing, piping, etc. Sabre saws or abrasive cutoff wheels are used on angle iron frames and piping. 5. Local decontamination, dismantling, and discarding, in that order, are continued until all equipment is removed. 6. Local hot spots are then decontaminated, and the cell is ready for installation of equipment. Some typical radiation levels encountered during a decontamina- tion cycle for mixed fission products are: -11- Table 2. Sequence of Decontamination Solutions Used to Remove Plutonium and Mixed Fission Products and Plutonium Solution Conc. (8/liter) 1.5 Commercial detergent: Fab, Tide, etc. Laundry detergent: Turco 4324 Degreasing solution: NaOH Trisodium phosphate Sodium carbonate 2.2 4.5 6.49 Detergent Oxalic acid 1.0 2.2 9.7 1.5 M 0.02 M Undiluted 360 27 100 Nitric acid Sodium fluoride Turco 4501 (8) Tucco 4502 Turco 4306-B Turco 4518 Sodium hydroxide Sodium hydroxide Oxalate-peroxide solution: Sodium oxalate, 4% Hydrogen peroxide, 3% Oxalic acid, 0.7% Water . . : -12- General Level Local Level Before contamination begins 400 rads/hr 3500 rads/hr After flushing, washdown, chemi- cal and physical treatment 1 rad/hr 100 rads/hr During contact removal of equip- ment, continued physical and chemical attack <1 rad/hr 50 rads/hr After equipment removal <25 millirads/hr (25 millirads/hr Final (after removal of hot spots). <10 millirads/hr <10 millirads/hr At the Savannah River Operations site, extremely-high-pressure jets (31) are successfully used to decontaminate the exteriors of large ves- sels and other equipment. Impact is so great that insulation and paint. are removed, but the tightly held metal oxides are not. Protective Surfaces Experience has shown that the decontamination of hot cells can be accomplished much easier if all surfaces are protected with a barrier film or protective coating before contact with radioactive materials. Parrott (30) concluded that decontamination of the ORNL Processing Pilot Plant was made much more difficult in areas where there were no protective surfaces. In general, all sites use anticontamination barriers. These consist of plastic membranes and tapes such as poly- ethylene, polyvinyl chloride, Saran, and protective coatings on walls and other working surfaces. Tools and small pieces of equipment are commonly coated with grease or oil, marking ink (32), plastic tape, or corrosion resistant protective coatings. Strippable plastic coat- ings also protect well but almost all sites report that they too are difficult to maintain and to remove. Waler-soluble paints such as billboard paint, polyvinyl acetate, etc., are worthwhile and effective but deteriorate if the humidity is high. In general, the more costly protective coatings, such as the vinyls and epoxies, offer the most protection and are easiest to clean. They are radiation resistant and can tolerate 5.0 x 109 r to 1010 r. (33,34) yet are much easier to decontaminate by washing than stainless steel, concrete, etc. However, in contact with volatile radioactive elements, the vinyls fix more iodine than the epoxies and retallic surfaces (35). -13- Nuclides The uncontrolled release of radioactive materials from normal confines is an uncommon event. Nevertheless, a few such instances have occurred, resulting in very costly cleanups. For this reason, it was felt proper to include a section dealing with this subject. When up-to-curie amounts of radionuclides escape from hot cells (or reactors or shipping cantainers) in uncontrolled and unexpected ways, the interiors and exteriors of the supporting facilities (shops, offices, etc.), surrounding grounds, and adjacent buildings are all likely to become contaminated.' Such a release may contaminate an unprotected area as large as several hundred to several thousand square meters. Here, decontamination cannot be done by remote manipulation or accord- ing to a standard procedure, as for hot cells. Some experience, however, indicates a general plan, which consists of an emergency phase, ar. operational recovery phase, and a final phase. The emergency phase is the perico immediately following the uncontrolled release. During this time, work areas are vacated. Then, the extent of the contaminated area is measured, and the intensity and toxicity of the nuclides are determined or estimated. An exclusion area is marked off, usually as an area larger than the contaminated one because a buffer zone is needed to prevent the transfer or migration of radioactivity outside of the contaminated area. The outer perimeter of the buffer zone is secured, and uncontrolled entrance is prevented by temporary fences and by plant guards. The effort during the operational recovery phase is directed toward the decontamination of the area to a point where rea recovery phase may extend over a period of months. During this period, crews restore the area so normal safety precautions and control can prevail. After an uncontrolled release of plutonium (30,36), it was first fixed to the roadways, paved areas, roofing, etc., with asphalt. Also, structures, vehicles, and some lawn areas were spray painted. The pavement and grounds were then excavated to a depth of about 3 inches, and the top soil was hauled away and buried. Decontamination then proceeded (Table 3) at a cost of thousands of man hours and dollars. -14- Table 3. Summary of Decontamination Treatments for Various Types of Surfaces After an Uncontrolled Release of Mixed Fission Products and Plutonium --. AEC - OFFICIAL Cleanup Rate (ft2/ man-hr). Character of Contamination Primary Treatment Surface Other Treatment . • 27 A11 (walls, floor, ceiling) Transferrable Scrubbed or sponged with detergent Dusty areas vacuumed . Fixed 4 Painted metal (walls and ceiling) Paint removed with paint remover and scrapers; surface scrubbed with soap and water Outer layer of paint removed with sandpaper Fixed 5 Concrete (floor) Ground with terrazzo-floor- grinding machine Hot spots chipped out, and verti- cal surfaces washed with dilute hydro- chloric acid Fixed : Bare metal (stainless steel piping and tanks ) Rinsed with dilute nitric acid and scrubbed with steel wool Surfaces abraded with emery paper Fixed Bare metal (other than stainless steel) Abraded with emery paper or ground to remove pits Fixed Lead shielding Rinsed with dilute nitric acid Fixed - Oil-coated metal (pumps ) Washed with "Gunk", a commercial solvent for de- greasing For the more general case, where the contamination need not be fixed, decontamination may be done faster (Table 4). The special characteristics of each incident will determine which sequence and combination of wet, dry, or land reclamation OBNL - AEC - OFFICIAL OFFICIAL -15 - Table 4. Methods for Decontaminating Outdoor Surfaces Where the Radioactivity Need Not Be Fixed (27 38) ORNI ~ hi Rate No. (1000 ft2 of man-hr) Men Effectiveness (fraction of radiation remaining) Method Surface Firehosing Roof 2.8 2 40 53 3 2-3 1. 1 0.02 to 0.08(39) 0.01 to 0.04(39) 0.02(40) 0.01 to 0.10(32) 1.2 1 0.05(39) ing 7.2 '1 0.10 to 0.30(41) Firehosing Pavement Motorized Pavement flushing Motorized Horizontal concrete sweeping or asphalt (e.g., streets) Hand sweep - Horizontal concrete or asphalt (e.g., streets) Motorized Horizontal concrete vacuum or asphalt (e.g., sweeping streets) Motor • Unplowed soil grading Motor Lawn grading Tractor Unp lowed soil scraping Tractor Plowed soil scraping Tractor Lawn scraping Hand shovel Lawn 14.40 0.01 3.34 0 0.1 1.07 0.1 3.44 0.1 1.86 0.1 0.1 0.16 0.33 Hand shovel Flower beds 0.1 metoa *Land reclamation methods usually call for the removal of the upper 1 to 3 in. (2 to 8 cm) of the soil and its burial at an approved site. Note: Sandblasting is effectively used on metallic or painted surfaces, but its use is generally avoided because of the radioactive aerosuls it generates. ***a * ORNL - AEC - OFFICIAL ............... methods will be most effective. The general sequence of decontamina- tion methods would be: (1) sweeping of large paved areas with a motorized street sweeper or motorized vacuum sweeper; (2) sweeping of -16. Oai - AEC - OFFICIAL sidewalks and small paved areas that are inaccessible to mechanized equipment, by hand; (3) flushing of large paved areas with a motorized street flusher or with manually held fire hoses; (4) firehosing of roofs and sides of buildings and structures; (5) application of land reclamation procedures to unpaved areas; (6) hand or motorized brushing and scrubbing on surfaces with detergents, followed by rinsing; and (7) surface -removal techniques as required, followed by resurfacing. This entire sequence may be changed as required; also, several opera- tions can be conducted concurrently. There are several excellent plans for the recovery of contaminated areas, the most comprehensive being "Fallout and Radiological Counter- measures" (42). "Estimating Cost and Effectiveness of Land Targets", (43) developed in 1959, is a theoretical model for planning the recovery of a residential target complex that has been contaminated by fallout. The plan, however, is useful in planning the recovery of any area (industrial or residential) contaminated by radioactive material. The basic concepts in ref (43) were verified, and an improved pre-recovery planning procedure was developed as reported in "Radiological Recovery of Land Target Components - Complex I an. Complex II" (21). Further refinement of planning factors are reported in "Radiological Recovery of Land Target Components - Complex III" CONCLUSIONS Hot-cells can be decontaminated and recovered for use an unlimited number of times. However, each succeeding cleanup may be more diffi- cult than the preceding one if protective films are not applied. Decontamination is now recognized as playing a vital and important role in the continued and economic operation of costly shielded facil- ities, and this new recognition is being reflected in the improved design of new facilities. New chemical solutions have been developed which are superior to nitric acid and sodium hydroxide for decontamination work. The oxalic acid solutions of Table 1 are notable in this respect. Solutions of this type are not only excellent decontaminants but offer the additional advantage of being easily destroyed to simplify waste disposal. To obtain best results, decontamination must be directed by trained ORAL-AEC - OFFICIAL workers. -17- ORNI ~ AEC - OFFICIAL A protective film applied prior to contamination is one of the best aids to decontamination. There is a breakeven point beyond which it may be less costly to discard equipment rather than to continue decontamination. Areas around hot cells such as buildings, offices, lawns, roadways can be decontaminated as satisfactorily as hot-cell facilities, but a much greater effort (manpower, money) 18 required. REFERENCES ܪ _ ܩܶܙܩܺ ܨܲܪ ܦ݁ܕ݁ܺܦܶܬ݁ ܦ݁ ; 1. M. D. Peterson, Equipment Decontamination-Survey Report, Clinton Laboratories, CN-1617 (May 1944). M. D. Peterson, 2. J. Reber, N. R. Glarum, and D. C. Overholt, Equipment Decontamination - Progress Report, Clinton Laboratories, CN-1869 (August 1944). 3. N. R. Glarum, D. C. Overholt, E. J. Reber, W. H. Baldwin, and M. D. Peterson, Equipment Decontamination - Final Report, Clinton Laboratories, CN-2208 (January 1945). 4. A. B. Meservey, "Progress in Nuclear Energy," Chap 5, Technology, Engineering and Safety, Series IV, Vol 4, Pergamon Press (1961). Reactor Technology, Vol 3, p. 189-210, Pergamon Press, 1962. A. B. Meservey, "Decontamination and Film Removal," Chap 7, J. A. Ayres, editor, Decontamination of Nuclear Reactors and Equipment 1965-1966, OTI, USAEC, in press. D. C. Layman, and Gunnar Thornton, Remote Handling of Mobile Nuclear Systems, Chap 5, OTI, USAEC, 1965 (in pre88). Turco Products, Inc., Wilmington, Dealware. Atomic Products Corp., Long Island, New York. Wyandotte Chemical Co., Wyandotte, Michigan. 1. Penn Salt Chemical Co., Los Angeles, California. Gray Co., Minneapolis, Minnesota. 3. Dow Chemical Co., Midland, Michigan. D. G. Stevensor, "Detergency in the Atomic Energy Industry," pp 140- 56 in Surface Phenomena in Chemistry and Biology, ed. J. F. Danielli et al., Pergamon Pre88, 1958. D. G. Stevenson, "Radiological Decontamination," Research Applied in Industry, vol XIII, pp 383-89, Butterworths, 1960. W. D. Burch, personal conmunication, Oak Ridge National Laboratory, Jan. 17, 1965. 0. M. Bízzeli, P. C. Tompkins, and C. D. Watson, "Practical Aspects of Surface Decontamination," Nucleonics, 7(2), pp 42-54, 87 (1950). P. J. Peterson, et al., A Recirculating wet Vacuum Cleaning and Scrubbing System for Decontamination, Proceedings of the Eleventh Conference on Hot Laboratories and Equipment, pp 281-84, American Nuclear Society 19. C. C. Burwe 11 et al., The Los Alamos "Wing 9" Alpha-Gamma Box System, Proceedings of the Twelfth Conference on Remote Systems Technolygy, pp 329-35, American Nuclear Society (1964). D. S. Irwin, and T. C. Johnson, Comparison of Solvents For Cleaning Metal Surfaces, RFP-469 (November 1964). W. B. Doe, personal communication, Argonne National Laboratory, Feb. 4, 1965. é ; ܟܲܕ ܝܼܲ ORNI - AEC - OFFICIAL -18- .ORNL-ALCOLLCML PL 2. Samel Spring, Metal cleaning, Reinhold, A. B. Meservey, Peroxide-Inhibited Decontamination Solution for Carbon Steel and Other Metals in the Gas-Cooled Reactor Program: Progress Report, November 1959-July 1962, ORNL -3308. M. R. Bennett, Evaluation of Reagent Decontamination, ORNL-CF- 51-11-123 (November 1951). C. D. Watson, Decontaminable Surfaces and Procedures for Hot Cells, Proceedings of the Fifth Hot Laboratories and Equipment Conference, ORNL-CF-57-3-159. Oakite Products, Inc., 19 Rector St., New York, N. Y. C. J. MacFarlane and R. J. Beal, Special Equipment for Decontamina- tion and Control of Radiation Hazards at Chalk River, CRRIS -1071 (March 1962). Sellers Injector Corp., 1600 Hamilton St., Philadelphia, Pa. F. N. Case, personal communication, Isotope Division, Oak Ridge National Laboratory, Jan. 17, 1965. J. R. Parrott, Decontamination of Ce11s 6 and 7 Building 3019 Following Plutonium-Release Incident, ORNL-3100, pp 28, 33-39 (Aug. 25, 1961). A. J. Hill, Jr., personal communication, Savannah River Operations, Jan. 27, 1965 (a report is in preparation). 2. J. W. Schulte, F. J. Fitzgibbon, and D. S. Shaffer, The Use of Solvent-Soluble Films in Decontamination, Proceedings of the Eighth Conference on Hot Laboratories and Equipment, OTI, USAEC, (1960). 3. G. A. West, and C. D. Watson, Gamma Radiation Damage and Decontamina- tion Evaluation of Protective Coatings and Other Materials for Hot Laboratory and Fuel Processing Facilities, ORNL-3589 (January 1965). 34. G. A. West, and C. D. Watson, Decontamination Testing of Highly Contaminated Protective Coatings, ORNL-2811 April 1960). · W. B. Parsley, personal communication, Oak Ridge National Laboratory, Nuclear Safety Pilot Plant, February 1965. L. J. King, and W. T. McCarley, Plutonium Release Incident of November 20, 1959, ORNL-2989 (Feb. 1, 1961). W. L. Owen, and J. D. Sartor, Radiological Recovery of Land Target Components - Complex I and Complex II, USNRDL-TR-570 (1962). W. L. Owen, and J. D. Sartor, Radiological Recovery of Land Target Components - Complex III, USNRDL-TR-700 (Nov. 20, 1963). L. Minvielle, and W. H. Van Horn, Recovery of Petroleum Refineries Contaminated by Fallout, USNRDL-TR-656 (June 24, 1963). D. E. Clark, Jr., and W. C. Cobbin, Removal Effectiveness of Simulated Dry Fallout From Paved Areas by Motorized Street Flusher, USNRDL-TR-797 (1965). D. E. Clark, Jr., and W. C. Cobbin, Removal Effectiveness of Simulated Dry Fallout From Paved Areas by Motorized and Vacuumized Street Sweepers, USNRDL-TR-746 (Aug. 8, C. F. Miller, Fallout and Radiological Countermeasures, Vols I and II, Standord Research Instutute, Menlo Park, California (January 1963) H. Lee, "Estimating Cost and Effectiveness of Decontaminating Land Targets," Vol 1, Estimating Procedure and Computational Techniques, USNRDL-TR-435 (June 6, 1960). w ..", . . ... ..... . 21.. . -- ORNL - AEC - OFFICIAL .. . I. 2 1 1, 2 1 | | 11. ' DATE FILMED 6 / 10 65 . . 1 . . . Arx . . 24 - EGAL NOTICE This report was prepared as an account of Government sponsored work. Neither the United States, nor the Commission, nor any person acting on bebalf of the Commission: A. Makes any warranty or representation, expressed or implied, with respect to the accu- racy, completeness, or usefulness of the information contained in this report, or that the use of any information, apparatus, method, or process disclosed in this report may not infringe privately owned rights; or B. Assumes any liabilities with respect to the use of, or for damages resulting from the use of any information, apparatus, method, or process disclosed in this report. As used in the above, person acting on behalf of the Commission” includes any em- ployee or contractor of the Commission, or employee of such contractor, to the extent that such employee or contractor of the Commission, or employee of such contractor prepares, disseminates, or provides access to, any information pursuant to his employment or contract with the Commission, or his employment with such contractor. END NE 277 IV.