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The effect of microbial action on nuclear waste management: is there enhanced leaching from bitumen and.. Clegg, Bruce Campbell 1982-12-31

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EFFECT OF MICROBIAL ACTION ON NUCLEAR WASTE MANAGEMENT: THERE ENHANCED LEACHING FROM BITUMEN AND INCREASED RADIONUCLIDE MOVEMENT THROUGH GEOLOGIC MEDIA? by BRUCE CLELLAND CLEGG B.Sc, The University Of Alberta, 1979 A THESIS SUBMITTED IN PARTIAL FULFILMENT OF THE REQUIREMENTS FOR THE DEGREE OF MASTER OF APPLIED SCIENCE in THE FACULTY OF GRADUATE STUDIES Department Of Civil Engineering We accept this thesis as conforming to the required standard THE UNIVERSITY OF BRITISH COLUMBIA October 1982 © Bruce Clelland Clegg, 1982 In presenting this thesis in partial fulfilment of the requirements for an advanced degree at the University of British Columbia, I agree that the Library shall make it freely available for reference and study. I further agree that permission for extensive copying of this thesis for scholarly purposes may be granted by the Head of my Department or by his or her representatives. 'It is understood that copying or publication of this thesis for financial gain shall not be allowed without my written permission. Department of Civil Engineering The University of British Columbia 2075 Wesbrook Place Vancouver, Canada V6T 1W5 Date: 15 October 1979 Abstract Long-term management of nuclear wastes demands absolute physical isolation of noxious radionuclides from the biosphere until decay to safe levels has occurred. Due to the extremely long half-life of some isotopes, the required isolation may be on the order of millennia. Past research on radioactive wastes has centered on the physicochemical mechanisms that may effect a premature return of radionuclides to the environment. However, biological action in a radwaste disposal site may have two major effects: 1) physical destruction of the solidifying matrix through solubilization or oxidation; and/or 2) enhanced movement of radionuclides through (adsorbent) geologic media by production of various chelating agents. The work presented here is focused on both these microbiological processes. 60Co and 137Cs encapsulated in bitumen was allowed to undergo microbial attack by a selected hydrocarbonoclastic culture under idealized environmental conditions. The radionuclides released by this process were then evaluated for their ability to bind with selected geologic media. In order to compare the effect of reduced adsorption due to microbial action, synthetic chelating agents were used as a standard. The same hydrocarbonoclastic culture used for these experiments was also tested for its sensitivity to y-irradiation. iii Subsequent analysis showed microbial attack of bitumen did not enhance the release of the ions. However, a decreased adsorption to the geologic media was observed but the effect was much less than that observed for the synthetic chelating agents. The level of r-radiation expected in the final waste repository will not effect the viability of the organisms tested. Table of Contents Abstract ii List of Tables ... vList of Figures viAcknowledgement viiI. INTRODUCTION 1 1 . ' BACKGROUND2. THE CHALK RIVER NUCLEAR LABORATORIES' LOW AND INTERMEDIATE LEVEL WASTE PROGRAM 2 A. TREATMENT AND DISPOSAL OF LOW AND INTERMEDIATE LEVEL WASTES 4 i. Volume Reductionii. Immobilization 4 iii. Ultimate Disposal 6 iv. Natural Barriers3. MICROBIAL ANTAGONISATION OF RADWASTE ISOLATION ...7 A. MICROBIAL ACTIVITY AND LEACHING 7 B. MICROBIAL ACTIVITY AND SUBSURFACE NUCLIDE MOVEMENT 8 4. SCOPE OF THIS WORK 9 II. MICROBIAL DEGRADATION OF BITUMEN 10 1 . BACKGROUND 1A. ALIPHATICS 1 B. AROMATICS 2 C. POLYCYCLIC AROMATIC HYDROCARBONS 13 2. REPRESENTATIVE HYDROCARBONOCLASTIC BACTERIA 14 3. CONDITIONS FOR GROWTH AND PRELIMINARY IDENTIFICATION 15 A. GROWTH CONDITIONS 1B. IDENTIFICATION 6 C. GROWTH CURVES4. SELECTION OF A SUITABLE CULTURE AND GROUNDWATER .17 A. SELECTION OF A SUITABLE CULTURE 1B. SELECTION OF A SUITABLE GROUNDWATER SOLUTION .22 REMARKS 23 III. MICROBIAL RADIOSENSITIVITY 24 1 . BACKGROUND 2 4 2. METHODS  5 A. GROWTH MEDIA PREPARATION 25 B. CELL PREPARATION 2C. IRRADIATION AND ENUMERATION 6 3. RESULTS 27 IV. EVALUATION OF MICROBIALLY ENHANCED LEACHING 31 1. ENHANCED LEACHING 32 2. METHODS 44 A. ANALYSIS 6 3. RESULTS AND DISCUSSION 47 A. STATISTICAL EVALUATIONV B. CONCLUSION 49 V. EFFECT OF CHELATING AGENTS ON RADIONUCLIDE MIGRATION 50 1 . BACKGROUND 52. METHODS 3 3. ANALYSIS 4 4. RESULTS AND DISCUSSION 56 5. REMARKS 61 VI. CONCLUSION 2 BIBLIOGRAPHY 5 APPENDIX A - ONTARIO MINISTRY OF THE ENVIRONMENT ANALYSIS 71 APPENDIX B - SYNTHETIC GROUNDWATER SOLUTIONS 73 APPENDIX C - LEACH TEST DATA 77 APPENDIX D - LEACHANT CONDUCTIVITY AND PH 89 APPENDIX E - ANALYSIS OF VARIANCE OF 60Co AND 137Cs~ SAMPLE MEANS AT T>14DAYS 90 List of Tables I. MICROBIAL MINERAL SALTS SOLUTION 15 II. y-IRRADIATION TIMES USED FOR CULTURES A,B,C AND D ..27 III. 60Co ADSORPTION DATA 56 IV. 137Cs ADSORPTION DATAV. 85Sr ADSORPTION DATAVI. COMPETING ION ADSORPTION DATA 58 VII. ADSORPTION DATA FOR COMPETING IONS IN SELECTED GROUNDWATERS 5VIII. LEACHANT A ADSORPTION DATA 59 IX. ADSORPTION DATA FOR NUTRIENT MEDIA CONTROL 5X. LEACHANT D ADSORPTION DATA 60 XI. LEACH TEST DATA - TEST SET A1 - 60Co 77 XII. LEACH TEST DATA - TEST SET A2 - 60CoXIII. LEACH TEST DATA - TEST SET A3 - 60Co 78 XIV. LEACH TEST DATA - TEST SET B1 - 60Co -...7XV. LEACH TEST DATA - TEST SET B2 - 60Co 79 XVI. LEACH TEST DATA - TEST SET B3 - 60CoXVII. LEACH TEST DATA - TEST SET Cl - 60Co 80 XVIII. LEACH TEST DATA - TEST SET C2 - 60Co 80 XIX. LEACH TEST DATA - TEST SET C3 - 60Co 1 XX. LEACH TEST DATA - TEST SET D1 - 60Co 8XXI. LEACH TEST DATA - TEST SET D2 - 60Co 2 XXII. LEACH TEST DATA - TEST SET D3 - 60Co 8XXIII. LEACH TEST DATA - TEST SET A1 - 137Cs 83 XXIV. LEACH TEST DATA - TEST SET A2 - 137CsXXV. LEACH TEST DATA - TEST SET A3 - 137Cs 84 XXVI. LEACH TEST DATA - TEST SET B1 - 137CsXXVII. LEACH TEST DATA - TEST SET B2 - 137Cs 85 XXVI11. LEACH TEST DATA - TEST SET B3 - 137Cs 85 XXIX. LEACH TEST DATA - TEST SET C1 - 137Cs 6 XXX. : LEACH TEST DATA - TEST SET C2 - 137Cs 8XXXI. LEACH TEST DATA - TEST SET C3 - 137Cs 7 XXXII. LEACH TEST DATA - TEST SET D1 - 137Cs 87 XXXIII. LEACH TEST DATA - TEST SET D2 - 137Cs 88 XXXIV. LEACH TEST DATA - TEST SET D3 - 137Cs 88 vii List of Figures 1. Culture A - 11 Hour Growth Curve 18 2. Culture A - Standard Curve 13. Culture B - 12 Hour Growth Curve 9 4. Culture B - Standard Curve5. Culture C - 12 Hour Growth Curve 20 6. Culture C - Standard Curve 27. Culture D - 12 Hour Growth Curve 1 8. Culture D - Standard Curve9. Dose-Response of Culture A 29 10. Dose-Response of Culture B11. Dose-Response of Culture C 30 12. Dose-Response of Culture D13. Leaching profiles for sets A1,B1,C1 and D1 - 60Co ....35 14. Leaching profiles for sets A1,B1,C1 and D1 - 137Cs ...35 15. Leaching profiles for sets A2,B2,C2 and D2 - 60Co ....36 16. Leaching profiles for sets A2fB2,C2 and D2 - 137Cs ...36 17. Leaching profiles for sets A3,B3,C3 and D3 - 60Co ....37 18. Leaching profiles for sets A3,B3,C3 and D3 - 137Cs ...37 19. Leaching profiles for sets A1,A2 and A3 - 60Co 38 20. Leaching profiles for sets A1,A2 and.A3 •- 137Cs 38 21. Leaching profiles for sets B1,B2 and B3 - 60Co '.39 22. Leaching profiles for sets B1,B2 and B3 - 137Cs 39 23. Leaching profiles for sets C1,C2 and C3 - 60Co 40 24. Leaching profiles for sets C1,C2 and C3 .- 137Cs 40 25. Leaching profiles for sets D1,D2 and D3 - 60Co 41 26. Leaching profiles for sets D1,D2 and D3 - 137Cs 41 I viii Ac knowledgement It is with sincere gratitude that I would like to thank the engineers, scientists and technicians of the Chalk River Nuclear Laboratories. Their kind suggestions, helpful criticisms and general support has culminated in this thesis. I would like to thank in particular Dr.'s Norman Gentner and Douglas Champ for the generous use of their time and lab space. However, I would like to thank especially, Mr.Leo Buckley who's expert suggestions and weekends in the lab were an inspiration. 1 I. INTRODUCTION 1. BACKGROUND Full scale atomic energy research in Canada has culminated in a pressurized heavy water reactor known as CANDU* This reactor, one of Canada's great technical achievements, is one of three reactor designs on world commercial markets. The uniqueness of the reactor design is characterized by the use of 1) natural uranium; 2) deuterium oxide (heavy water) as moderator and coolant; 3) a multiple pressure tube configuration instead of a single large pressure vessel of other reactors; and 4) on power fueling (fuel bundle replacement during reactor operation). The commercial power reactor uses uranium with greater efficiency than the LWR** types. Because of its neutron economy the CANDU reactor also has the advantage of being adaptable to more efficient fuel cycles, such as the thorium fuel cycle without major * CANada Dueterium Uranium. **Light Water Reactor 2 modification of the existing design. This means it is possible to operate at or near breeding, making the CANDU reactor comparable to the fast breeder reactor. Thorium.is at least three times as abundant in the earth's crust as uranium thus the available nuclear fuel resource would be considerably increased. If this cycle is embraced, Canada will require a reprocessing facility in order to recover fissile materials contained in the spent fuels.1 The separated fission products will require safe permanent disposal. The Canadian waste management program was initiated to evaluate disposal options. Prior to 1971 all irradiated fuel was either processed abroad or sold.2 Since then, the spent fuel has been stored in water filled bays at the nuclear power stations. The fate of the spent fuels has not yet been decided, but either it will be reprocessed and the residues immobilized and disposed, or it will be disposed intact, most likely in mined cavities within granitic mineral free structures abundantly located in the Canadian Shield. 2. THE CHALK RIVER NUCLEAR LABORATORIES' LOW AND INTERMEDIATE  LEVEL WASTE PROGRAM Along with the high level wastes are less active wastes generated from daily operation of the nuclear power reactors. The broad categories including all low and intermediate level 3 radwastes encompass only 0.1% of the total "waste" radioactivity.3 Unfortunately, these wastes are substantial in volume and are chemically and radiologically heterogenous. Some of the various differences with Canada's low and intermediate level wastes are: 1) the production of 14C is much greater than in a LWR due to the much smaller LWR core size; 2) a high degree of system integrity minimizes losses containing fission and neutron activation products; and 3) tritium appears to be more abundant than in LWR's.4 Furthermore, the major sources of CANDU low and intermediate level wastes are associated with: 1) Routine operation and maintenance. 2) Purification in heavy and light water circuits (the majority of the radioisotopes are contained on spent ion-exchange resins and filters containing 60Co, 137Cs and 1"C (present as a carbonate on ion-exchange resins). 3) Equipment decontamination.5 The ultimate disposal of radwastes will incorporate a multiple barrier system in which a waste nuclide would have to breach a series of obstacles6 prior to recontact with the biosphere. These obstacles include a number of pretreatment and treatment steps discussed below. 4 A. TREATMENT AND DISPOSAL OF LOW AND INTERMEDIATE LEVEL  WASTES i. Volume Reduction All wastes that occur as incinerable solids will be incinerated to a stable ash. Both Ontario Hydro (Bruce Nuclear Power Development) and Atomic Energy of Canada Limited (AECL) at the Chalk River Nuclear Laboratory (CRNL) have incinerators operating for this purpose. Liquid wates may undergo a two-step procedure for volume reduct ion: 1) Reverse osmosis; and 2) Evaporation. Reverse osmosis concentrates solids by excluding water through a semipermeable membrane. A second step in volume reduction may utilize a vertical thin-film evaporator6 to further increase the percentage of total solids (up to 50% has been achieved with some wastes).7 i i. Immobilization The ultimate aim of immobilization of radwastes is the production of a durable leach-resistant solid. Compounds that have been used as a solidifying matrix include cement, urea-formaldehyde, polyester and bitumen.8 The selection of bitumen by CRNL's low and intermediate level waste program was due to its versatility, volume savings and leach resistance (highest 5 of those materials mentioned).9. Bitumen is chemically very heterogenous but its components may be grouped into four broad categories: saturated hydrocarbons, resins, cyclic hydrocarbons and asphaltenes.10 Other elements that may be present are oxygen(1 -17%), sulfur(1-9%) and/or nitrogen(1 %).11 At room temperature(20-25°) bitumen's physical state may be described as a complex colloidal system.12 Bitumen has been used to cement building materials (Babylon), caulk boats or as a water stop between brick walls in the the third millenium B.C.13 The establishment of bitumen as a solidifying matrix for nuclear wastes may be attributed to the Research Centre for Nuclear Energy at Mol, Belgium and the Plutonium Research Centre of Marcoule, France. The Belgium establishment was constructed and operated (on a small scale) from 1960-1964 while the Marcoule installation started operation in 1965. Canadian experience with bitumen has been limited to laboratory and pilot scale projects. The completion of CRNL's Waste Treatment Centre (WTC) has been slated for 1982. This complex will utilize volume reduction by incineration or reverse osmosis and evaporation, followed by bitumenization. 6 iii. Ultimate Disposal In order to ensure physical isolation of the radwaste from contact with the biosphere (until the waste radionuclides have decayed to acceptable limits) terminal disposal will be subterranean. The final waste repository will probably be located on the Canadian Shield in a geologically stable hard rock formation known as a pluton. Some of the obvious advantages for the selection of a pluton are that they are: "relatively homogeneous structures of high integrity and long stability" and "have remained undisturbed since early geologic times ie, for 200 to 2000 million years".1" iv. Natural Barriers Although the utmost consideration will be given to siting the repository in a hydrogeologically inactive zone, groundwater intrusion may occur. If intrusion does occur the deleterious effect of the groundwater flow may be twofold: leaching of the solidified waste with concomitant movement through the repository and the subsurface environment. In order to minimize the passage of leached radionuclides out of the repository, naturally occurring adsorbents may be used to backfill the repository environment. This method is in accordance with the multiple-barrier approach to nuclear waste management. If a strong adsorbent ie, bentonite is used, leached nuclide attenuation will be greatly enhanced. 7 3. MICROBIAL ANTAGONISATION OF RADWASTE ISOLATION Microbial activity may enhance the movement of radionuclides from a repository by effecting physical destruction of the solidified matrix or production of complexing agents that may decrease . the effectiveness of sorption reactions by backfill material. A. MICROBIAL ACTIVITY AND LEACHING The release of waste radionuclides encapsulated in bitumen may be envisioned as a process involving two mechanisms: 1) Matrix decay caused by direct microbial attack of the bitumen; and 2) Matrix solubilization effected through the production of alcohols, esters, ketones and other metabolic end-products.15 Although the result of each mechanism is assumed to be negligible over a few years, the effect may have significant consequences for a waste that must remain isolated for centuries.16 The effect of direct microbial attack on bitumen has been documented by previous investigators.17"23 However, investigations on microbial attack of nuclear wastes encapsulated in bitumen is virtually non-existent.2" The research that has been done was performed under the auspices of the Los Alamos Scientific Laboratory.25 Unfortunately, many of their findings do not have general applicability. The 8 experimental design and rationale focused on experiments that would yield information that pertained directly to the U.S. Waste Isolation Pilot Plant (WIPP). These studies included C02 gas evolution from (inactive) asphalt, microbial methylation of Pu, enumeration of WIPP microflora and general radiobiological studies. The geological environment of plutons and that expected for the WIPP (hard rock-salt) is dissimilar and therefore cross comparisons should only be made with caution. B. MICROBIAL ACTIVITY AND SUBSURFACE NUCLIDE MOVEMENT The ability of strong synthetic chelating agents to mitigate against radionuclide sorption to backfill material has been established elsewhere.26 Emery27, has shown that hydroxamate and polyhydroxamate chelating agents may be produced through microbial metabolism of organic materials. It follows logically, therefore, that microbially produced chelating agents may serve to enhance the movement of radionuclides through backfill material and the surrounding subsurface environment. The fate and migratory properties of nuclear waste elements in a natural geological environment has been evaluated by numerous methodologies. However, evaluation of the partitioning of the waste element between the solid media and liquid phase (groundwater) is the focal point of most studies. Various researchers have tried to illustrate the 9 destiny of escaped radionuclides under a myriad of conditions.28-30 4. SCOPE OF THIS WORK As mentioned earlier, microbial populations may have an adverse effect on nuclear waste management by direct attack of a bituminized waste package and/or production of chelating agents. The scope of this thesis will span these two issues. Unlike the Los Alamos work, this research should find general applicability throughout the nuclear industry. However, sundry details (choice of radionuclides, organisms and techniques) were chosen for their relevance to the Canadian nuclear program. 10 II. MICROBIAL DEGRADATION OF BITUMEN 1 . BACKGROUND Compared with glucose degradation, microbial oxidation of hydrocarbons poses a unique set of problems: they are insoluble in water and present problems of how they are solubilized or emulsified; they are chemically unreactive so require specialized enzymes for their initial oxidation, and, finally they reverse the metabolism of microorganisms from being glycolytic and lipogenic to being lypolytic and gluconeogenic.31 . Since metabolism of hydrocarbons is not as "energy-efficient" as degradation of common sugars, use of hydrocarbons as a substrate will only occur as a secondary mechanism.* As a result, adaptation and natural selection have evolved microorganisms with the ability to overcome or circumvent some of the constraints listed above. These adaptations have endowed organisms with the ability to: * Hydrocarbons will only be degraded in those cases where other more suitable substrates are lacking or absent. 11 produce surface-active agents for the emulsification of their hydrocarbon substrate; oxidize their reactant (usually to an alcohol or diol) thereby making them more prone to an enzymatic catabolism similar to fatty acid metabolism; produce simple sugars from fatty acids or other lipoidal precursors. Although the high substrate specificity of most microbial species limits the overall degradation of a heterogenous mixture of hydrocarbons, individual components may be attacked preferentially by a mixed culture of hydrocarbonoclastic bacteria. With respect to the major organic groups that compose bitumen, microbial degradation may occur in the following ways: A. ALIPHATICS According to Ratledge,32 the following characteristics apply to the degradation of aliphatic hydrocarbons: 1. Aliphatic hydrocarbons are assimilated by a wide variety of microorganisms. Other classes of compound, including aromatics, may be oxidised but are assimilated by only a few bacteria. 2. n-Alkanes of chain length shorter than n-nonane are not usually assimilated but may be oxidised. Only some bacteria have the ability to grow on alkanes shorter than n-octane. As the chain length of the alkane increases beyond C9 the yield factor increases but the rate of oxidation decreases. 3... Saturated compounds are degraded more readily than unsaturated ones. 4. Branched-chain compounds are degraded less readily than straight chain compounds. Although hydrocarbons of chain length <C9 are more 1 2 soluble and therefore more available to microorganisms they seem to illicit a toxic response.33 This toxicity may be attributed to a disruption of the cytoplasmic membrane with a concomitant loss in functional integrity.34 In addition to toxicity from short hydrocarbons, fatty acids may also be noxious. The deleterious effect of fatty acids is evident from their amphoteric nature by means of which they may act as an emulsif ier.3 5 The first step in the metabolism of aliphatic hydrocarbons is usually to a primary alcohol by one of two possible enzymes (cytochrome P-450 or rubredoxin). To convert the primary alcohol to its corresponding carboxylic acid, a second oxidation usually follows. After this conversion to a carboxylic acid is complete, final degradation can occur via normal biochemical catabolic pathways such as 0-oxidation. Although the initial mode of oxidation changes for alkenes and branched-chain substrates, the resultant product is usually similar, namely, a terminal carboxylic group. B. AROMATICS Not unlike the decomposition of an aliphatic compound -metabolism of an aromatic species requires oxidation of the initial substrate to a common product. In the case of most simple benzene-like compounds, the common product is usually a catechol. Chapman36 illustrates that 3 major products of an 13 initial oxidation sequence (catechol or 1,2-dihydroxybenzene, protocatechuic acid or 3,4-dihydroxybenzoic acid and gentistic acid or 2,5-dihdroxybenzoic acid) are "at the focal points of pathways for a wide range of compounds" and that "other substituted catechols or substituted parahydric phenols may serve as ring-fission substrates".37 The subsequent reaction step that follows conversion to a catechol is ring-fission. For catechols the ortho-fission (cleavage between the two carbons containing the hydroxy groups) pathway predominates, while substituted catechols may undergo meta-fission (cleavage of the bond between an hydroxy-bearing carbon and a carbon adjacent to it that is not hydroxy-substituted).38 Thus, following conversion to a catechol or a substituted catechol and ring-fission, central metabolic pathways function to cause complete oxidation. C. POLYCYCLIC AROMATIC HYDROCARBONS In comparison to degradation of the simple aromatic compounds, polycyclic aromatic hydrocarbons (PAH) are also dependent on conversion to a dihydrodiol before further metabolism may proceed. Although some genera (Aeromonas) appear to vary from this scheme through production of a 1-hydroxy-2-napthoic acid from phenanthrene, the general microbial attack seems to start with production of the diol. Again, dihydrodiol production is usually followed by ring-14 fission and then total degradation via various central metabolic pathways. The degradation of PAH's larger than 3 rings has not yet been unequivocally demonstrated. Although this may represent a lack of perseverence by experimenters in the field, the asphaltene fraction of bitumen may be resistant to microbial attack. In conclusion, microbial degradation of hydrocarbons is dependent on conversion of the substrate to a more reactive intermediate such as a carboxylic acid or an alcohol, this product in turn is completely degraded by intracellular systems that have a more general function. 2. REPRESENTATIVE HYDROCARBONOCLASTIC BACTERIA As mentioned earlier, the rate of microbial oxidation of hydrocarbons is usually extremely slow. Thus, to maximize the possible degradation of bitumen (containing waste radionuclides) fresh cultures of unidentified hydrocarbonoclastic microbes were obtained from: 1) Gemni Biochemical Research Limited - 1 mixed (Culture A) and 2 pure (Cultures B and C) cultures. 2) University of Calgary - 1 mixed culture (Culture D).* * Thanks to Dr.Ian Forrester and Mr.Cam Wyndham of Gemni Biochemical Research and the University of Calgary respectively for their kind donation of these cultures. 15 All four cultures had been located in the bitumen-rich Athabasca tarsands and were therefore well adapted to the task of utilizing a heterogenous mixture of hydrocarbons as a metabolic substrate. 3. CONDITIONS FOR GROWTH AND PRELIMINARY IDENTIFICATION A. GROWTH CONDITIONS All cultures were grown on a mineral salts solution that had been found to be satisfactory for microbial degradation of hydrocarbons. As described by Bushnell and Haas,39 the contents of this mixture are listed in Table I below: Distilled, deionized water 1000.0 mis MgSO„ 0.2 g CaCl2 0.02 g KH 2 PO„ 1.0 g K2HPO„ 0 g (NH„)2SO„ 1 .0 g FeCJ-3 2 drops cone. soln. Table I - MICROBIAL MINERAL SALTS SOLUTION To prevent precipitation of various inorganic species after sterilization (>20 minutes at 125°C), FeCl3 and CaCl2 were autoclaved separately and added after the main solution had cooled. In addition to the salts listed above, non-selective nutrients including 0.3 wt.% malt extract, 0.3 wt.% yeast extract and 0.5 wt.% peptone were added to the mineral salts 1 6 solution on the recommendation of Forrester."0 Temperature was maintained at close to ambient (20-25°C) and aeration was maximized through continous agitation of all cultures. B. IDENTIFICATION Cultures A,C and D contained gram negative rod-shaped cells that showed some motility at 30°C. An Ontario Ministry of The Environment analysis"1 (see Appendix A) report showed the 4 cultures may contain the following genera: Culture A - Pseudomonas Culture B - Bacillus Culture C - VE group* Culture D - Citrobacter, Pseudomonas C. GROWTH CURVES In conjuction with the Ontario Ministry of The Environment analysis (Appendix A), microbial growth profiles (Figures 1,3,5 and 7) were established by the following methods: 0.30 ml of fresh innoculum was added to 20 mis of the nutrient media salt solution (described earlier) and allowed to rotate(5-l0 RPM) at 25°C. Samples were taken from the reaction vessel every hour for at least 11 hours. Serial * Bacteria in the VE group share characteristics with the genera Pseudomonas, Xanthomenas and Chromobacterium and as yet are not well defined taxonomically."2 17 dilutions followed by media plating was used to determine the number of viable cells per sample."3 Standard curves (Figures 2,4,6 and 8) of absorbance vs cell concentration, were also obtained for each culture by taking absorbance readings of 0.5 to 1.0 ml aliquots of each hourly sample on a Gilford 240 spectrophotometer (wavelength=600nm). "These plots (Figures 1-8) illustrate that Culture D showed the most rapid initial growth. A second interesting observation of the culture D profile is its biphasic nature. This information coupled with that in Appendix A, confirms the multi-organism content of Culture D. 4. SELECTION OF A SUITABLE CULTURE AND GROUNDWATER A. SELECTION OF A SUITABLE CULTURE In order to isolate the mixed culture with the greatest bitumen degrading potential, the following procedure was followed: 1.0 g of bitumen(30-40 mesh of Sp-170)* was placed in 20.0 mis of deionized water (DIW) containing 0.1340 g Yeast Nitrogen Base (YNB)** and 0.1 wt.% peptone. This solution was then sterilized by r_irradiation (500 Krads). Two identical * "Sp-170" is the designation used by Husky Oil (the bitumen supplier) for this class of oxidized bitumen. **YNB is a non-selective source of non-carbon nutrients for microbial growth, including the following: (NHa) 2SOi, ( 75 wt.%), KH2P0,(15 wt.%), MgSOa(7 wt.%), NaClO wt.%), CaCl2(l wt.%) and selected vitamins and nutrients(<1 wt.%) 18 CULTURE A 11 HOUR GROWTH CURVE Figure 1 - Culture A - 11 Hour Growth Curve CULTURE A STANDARD CURVE-(ABS. VS CELL CONC.) Figure 2 - Culture A - Standard Curve 19 20 CULTURE C 12 HOUR GROWTH CURVE T 1 1 I 1 1 1 1 1 1 1 T~~ 1$ $jt HA ItM 14A t*M TIMM(EOURS) Figure 5 - Culture C - 12 Hour Growth Curve CULTURE C STANDARD CURVE-(ABS. VS CELL CONC.) CELL CONCENTRATION (CELLS/ML) (X10* ) Figure 6 - Culture C - Standard Curve 21 CULTURE D STANDARD CURVE-(ABS. VS CELL CONC.) ittt* tHM 144** IMA* CELL CONCENTRATION (CEILS/ML) (X10* ) Figure 8 - Culture D - Standard Curve 22 solutions were prepared following this procedure. To confirm that bitumen was the sole carbon source present in the test vessels, appropriate controls (sets a and b) were run. Also, to directly compare rate of growth on bitumen to rate of growth on a common carbon source a second set of controls were run (e and f) consisting of sucrose substituted for bitumen. Thus, six individual sets were run consisting of: a) YNB + Culture A b) YNB + Culture D c) YNB + Bitumen(1 g) + Culture A d) YNB + BitumenU g) + Culture D e) YNB + SucroseO g) + Culture A f) YNB + SucroseO g) + Culture D At T=46 hours, growth was found only for those sets containing Culture D and similarily, .the largest population L sizes were only found for sets d and f. B. SELECTION OF A SUITABLE GROUNDWATER SOLUTION Current work by the Applied Geoscience Branch of the Whiteshell Nuclear Research Establishment has established four synthetic groundwaters as appropriate for radionuclide adsorption studies.In order to simulate "real" repository conditions for subsequent experiments (Sections IV and V), selection of a synthetic groundwater that would not supress microbial growth was necessary. The four synthetic groundwater solutions were prepared according to the methods outlined in Appendix B. Growth of Culture D was tested through simple innoculation of each 23 groundwater solution containing 0.3 wt.% malt extract, 0.3 wt.% yeast extract and 0.5 wt.% peptone but no additional mineral salts other than those contained by the groundwater. After incubation at 25°C the solution containing WN-1 Saline Solution supported the best growth of Culture D. REMARKS Since the degradation of bitumen is extremely slow, all foreseeable inhibitors of microbial activity were eliminated (Section IV). On the basis of the rudimentary evaluations of growth mentioned above, Culture D and WN-1 Saline Solution were selected as the most appropriate culture and groundwater solution respectively, to provide a "worst case" approach. 24 III. MICROBIAL RADIOSENSITIVITY Since the final waste repository will be a continous source of low-level radiation (<10 R/hr), the effect of radiation on Cultures A,B,C and D has been evaluated. 1. BACKGROUND The majority of low-level waste radionuclides that may be encapsulated in bitumen emit r_radiation (ie 137Cs, 60Co etc.). The absorbed dose from these radionuclides has been cited as a potential area of concern with respect to radiolytic degradation of asphalt with concomitant gas generation."5 However, these same fields could be bacteriocidal; the relative resistivity of Culture A,B,C and D to low LET* radiation was evaluated through irradiation of each culture with a high energy (1330.0 KeV) r_source. In order to graphically illustrate the lethal effects on * LET or Linear Energy Transfer encompasses that fraction of the inherent energy associated with the radiation that is transferred to the target atoms - energy transmitted to the absorber per unit path length. 25 a population of each culture, percentage survival was determined over the range of 0-300 Krads. The results of this experiment will yield information that is important in the consideration of whether or not irradiation will effectively decrease or eliminate the rate of bitumen biodegradation. 2. METHODS A. GROWTH MEDIA PREPARATION Six litres of mineral salts solution were prepared as described earlier (Section II), with the exception of CaCl2. To prevent the precipitation of inorganic salts (during sterilization) a CaCl2 solution of 0.02 g/ml was prepared separately. Peptone, yeast and malt extract were added according to Forrester, accompanied by 2 wt.% agar. These two solutions (medium and CaCl2) were then sterilized separately and mixed upon termination of sterilization. Approximately 300 plates were prepared from this mixture and allowed to cool under intense UV irradiation. B. CELL PREPARATION A fresh solution of cells was prepared from each culture and allowed to incubate for approximately 72 hours. Due to this long incubation period all cell solutions were assumed to be in a stationary growth phase. 26 Cell washing was done three times by adding 1 ml of each fresh culture to Nalgene centrifuge tubes followed by 9-10 mis of PBS.* Each culture was then centrifuged at 9000 RPM for 5-10 minutes at 2°C. The supernatant was discarded and the pellet resuspended in 9-10 mis of PBS. C. IRRADIATION AND ENUMERATION Following washing, the pellets were vigorously agitated in PBS to yield a homogeneous cell solution. Immediately prior to and following each irradiation interval each culture was placed in ice to decrease the effect of enzymatically catylzed repair. Irradiation was performed with an AECL Gammacell-220 with a dead time** and dose rate of 2.4024 Krad and 0.4640 Krad/sec*** respectively.46 On the basis of this dead time and dose rate the cultures were irradiated directly in the centrifuge tubes according to Table II. * PBS- Phosphate Buffer Solution is a mixture of K2HPOa and KH2PO„ present in an appropriate molar ratio to yield a buffered pH of 7.50. ** Dead time is the residual radiation received by the sample prior to and upon termination of the dosing period. ***Dose rate and dead time are determined from the measured source (60Co) activity at some reference time, t=0. Thus, doses and dead time at time t can be calculated from the original activity, reference time and source half-life. 27 Dose(Krad) Sequent ial Time(sec) Cumulative Time(sec) 0 5 10 15 25 50 75 100 200 300 210.3 210.3 0.0 5.6 5.6 5.6 16.4 48.7 48.7 48.7 0.0 5.6 11.2 16.8 33.2 81 .9 130.6 179.3 389.6 600.2 Table II - y-IRRADIATION TIMES USED FOR CULTURES A,B,C AND D Upon receipt of the appropriate dose,. 0.5 mis of the culture was removed and serial dilutions of 10" 1 ,10"2,10"3 , 10"4 and the first four dilutions and at each dose listed in Table II. A fifth set of replicate plates was prepared for the 0 dose control. Since irradiation of the cultures was performed sequentially, 0.5 ml aliquots of the sample were diluted and plated after receipt of the appropriate dose. All plates were then allowed to incubate for 48 hours at 20°C prior to colony enumerat ion. 3. RESULTS Dose-response curves (Figures 9-12) were generated for cultures A,B,C and D. These curves illustrate that none of the cultures are capable of growth at a dose >75 Krads. At least half the population will die (LD50) after exposure to a dose exceeding 6 Krad. These results indicate that none of IO"5 were made. Replicate plates were prepared for each of 28 the cultures tested are radiosensitive (substantial cell death is only realized at >1000 rads) however, Culture A,C and D all showed survival curves characteristic of a Multitarget* mechanism for cellular inactivation.*7 This result may be expected since many bacterial species show this response to y-irradiation. In order to minimize the exposure to personnel and prevent severe radiolytic damage to the bitumen, the initial surface dose rate will be kept below 10 R/hr.a8 Except for 1"C, 137Cs and 60Co will be the most predominant radionuclides contained in the low level waste repository."9 These waste nuclides have a half-life of 5730, 30 and 5.3 years respectively. Thus, with an exponential decay, activity contributed by 137Cs and 60Co will have decreased to negligible levels within 300 years. Since each culture tested is relatively radio-insensitive and the bitumen waste block will contain predominately short lived radionuclides with a low initial activity - the radiological effect of the waste on these microbial species would be negligible. However, long-term exposure may increase the rate of mutation and/or increase the relative radiosensitivity of exposed organisms.50 * Multitarget theory assumes an organism death will result only after various intracellular "targets" are inactivated by the radiation source. 29 RADIATION DOSE RESPONSE PROFILE OF CULTURE A DOSE(KRAD) Figure 9 - Dose-Response of Culture A RADIATION DOSE RESPONSE PROFILE OF CULTURE B T 1 1 1 1 1 1 1 1 1 1 1 1 r 1t.O S4.0 MM 40.9 4IM MM $4M 71.0 tOJ> DOSE(KRAD) Figure 10 - Dose-Response of Culture B 30 RADIATION DOSE RESPONSE PROFILE OF CULTURE C 00.0 04J0 10J0 0OJ> DOSE(KRAD) Figure 11 - Dose-Response of Culture C RADIATION DOSE RESPONSE PROFILE OF CULTURE D i 1 i 1 1 1 1 1 1 1 1 r-i 1 i 1 1 1 1 1 1 1— 0J0 4.0 0J0 10.0 I0J0 00.0 04.0 00.0 00J0 00.0 40J0 DOSE (KRAD) Figure 12 - Dose-Response of Culture D 31 IV. EVALUATION OF MICROBIALLY ENHANCED LEACHING Leaching, the process by which a relatively insoluble species such as an inorganic salt is solubilized, is the primary mechanism for release. of encapsulated waste radionuclides. The process of leaching immobilized wastes has been shown51"'52 to be approximated by Fick's diffusion equations,53''5" and a plot of: Igj y. vs (tn)°-5 Eqt.IV. 1 A0 F will show linearity if the process is governed by diffusion.* If the cumulative fraction of activity leached is plotted against time the resultant curve (for a diffusion-mediated response) may be described as parabolic initially then tapering off to a straight line with slope "~0. This type of plot was used to illustrate the data presented in this Section. However, diffusion (and therefore leaching) will not * Where an =radioactivi_ty leached during the leachant renewal period,n;A0=radioactivity initally present in specimen;F=ex-posed surface area of specimen(cm2);V=specimen volume(cm3) and tn=duration(days) of leachant renewal period.5" 32 occur unless the solidified wastes are in contact with the leachant. An increase in any of the mechanisms that will allow greater availability of the encapsulated species with the leachant will therefore result in an increase in leaching. 1. ENHANCED LEACHING The pertinent factors with respect to bitumen that may result in enhanced leaching are: a) Mechanical abrasion, b) Temperature, c) Diffusion, d) Biodegradation. Since the final waste repository will be located in a geologically stable location, the effect of mechanical abrasion will elicit a negligible increase in contact of the immobilized waste radionuclides with native groundwaters. Unfortunately, the temperature characteristics of the repository are unknown. Initially the repository temperature is expected to be approximately 10°C however, waste heat from high-level radioactive decay may increase the overall repository temperature. If the increase is large enough, leaching may be enhanced as a result of the increased surface contact.55 The remaining two factors may result in the greatest increase in leaching under "repository conditions" and therefore deserve greater elaboration. 33 Diffusion The enhanced movement of ions from bitumen as the concentration gradient is decreased between the bitumen and solvent can be rationalized by a diffusion mediated phenomenon.51 The radionuclide - bitumen mixture will be essentially homogeneous thus, the waste solid may be considered an isotropic medium. In this case, a random uniform movement of ions between the bitumen surface and the surrounding media will occur. If the surrounding media has a low initial ionic concentration (ie DIW), a net increase in the ion content will be observed after contact with the bitumen block. The driving force for this steady-state movement is the difference in concentration between the bitumen and water, AC. As AC approaches 0, the net exchange between the isotropic solid and leachant will also become 0. Mathematically, diffusion may be described as: the rate of transfer of diffusing substance through unit area of a section is proportional to the concentration gradient measured normal to the section, ie F = -D\T. Eqt.IV.2 \X where F is the rate of transfer per unit area of section, C the concentration of diffusing substance, x the space coordinate measured normal to the section, and D is called the diffusion coef f icient.5 6 The resultant effect of this process will be an equilibrium state in which the concentration of ions in the 34 leachant approximates the concentration of ions in the bitumen. Unfortunately, equilibrium will only be attained in those cases in which the leachant is static. Groundwater flow in a "real" repository would represent a dynamic state that may afford infinite dilution provided a concentration gradient exists between the solid matrix and groundwater. This behaviour is clearly illustrated by Figures 13 to 26 in which the cumulative fraction leached (as a function of time) is still increasing for all cases in which an ionic counterbalance was not present (Set-A). Sets B,C, and D* however, all illustrate the case in which an equilibrium is being approached and slope—-K), due to the mitigating effects of ions present in solution prior to the initiation of the test. Biodegradation As previously mentioned both laboratory17"19 and in situ  21-23,57-60 attack has been adequately demonstrated. The effect of microbial attack of a bituminized waste may enhance leaching via: physical removal of the exposed layer of the bitumen as it is used as a microbial substrate; solubilization by metabolic intermediates, end-products15 or co-oxidative products61; or emulsification of the bitumen by microbially * Set A contained DIW only. However, B,C and D were composed primarily of the nutrient solution discussed in Section II. 0 35 SETS A1#1,C1J)1 - "Co LEACHED VS TIME —i— /ML0 TIME(DAYS) Figure 13 - Leaching profiles for sets Al,B1,C1 and D1 _ 6 0 Co' SETS A1,B1,C1J)1 - mCs LEACHED VS TIME a 1 e—© SET A-1 * • SET B-1 •—» SET C-t SET D-1 TIME (DAYS) Figure 14" - Leaching profiles for sets A1,B1,C1 and D1 - 137Cs 36 SETS A2tB2,C2tD2 - "Co LEACHED VS TIME ^ SETS A2tB2,C2tD2 - "Cs LEACHED VS TIME TIME(DAYS) Figure 16 - Leaching profiles for sets A2,B2,C2 and D2 - 137Cs 37 SETS A3£3,C3J)3 - ' Cs LEACHED VS TIME a—o SET A-3 < • SET B-3 • SET C-3 x—K SET D-3 f—~T" ? i *— ( 4 _ + • ^)t, ^ fi * x * *~~ —X M — K tJO tOM MM M.0 70.0 MM MM IMM 49M MM MM TIME(DAYS) Figure 18 - Leaching profiles for sets A3,B3,C3 and D3 - 137Cs 38 SETS A1A2A3 - mCs LEACHED VS TIME 39 i SETS B122.B3 - "Co LEACHED VS TIME o—e> SET B-1 < • SET B-2 *—• SET B-3 -i 1 1 r I IM TIME(DAYS) Figure 21 - Leaching profiles for sets B1,B2 and B3 - 60Co SETS B1,B2£3 - Cs LEACHED VS TIME 40 r SETS C1,C2,C3 - "Co LEACHED VS TIME SET C-1 SET C-2 SET C-3 T 1 1 50.0 00.0 i r 70.0 I r~ 00.0 —i 1 1 r 30.0 4CJO 1QQJ0 Figure TIME(DAYS) 23 - Leaching profiles for sets C1,C2 and C3 - 60Co SETS C1,C2,C3 - mCs LEACHED VS TIME o—o SIT C-1 * • SET C-2 *—» SET C-3 —i 1 1 1 1 r 40J) 80.0 80.0 TIME(DAYS) Figure 24 - Leaching profiles for sets C1,C2 and C3 IOOJO 137Cs 41 TIME(DAYS) Figure 25 - Leaching profiles for sets D1,D2 and D3 - 60Co SETS D 1J)2J)3 - mCs LEACHED VS TIME T 1 I0QJO TIME(DAYS) Figure 26 - "Leaching "profiles for sets D1,D2 and D3 - 137Cs 42 produced surface-active agents such as lipids, glycolipids and lipoproteins.62"65 Obviously, the latter two modes of microbially initiated radioactive waste release are dependent on the presence of the first if bitumen is the sole carbon source (a likely scenario in a deep waste repository). Furthermore, the presence of exogenous agents that may solubilize or emulsify the bitumen is not a relevant problem unless the repository containing the waste is in or adjacent to a geological formation containing petroleum. Until now, no investigators have undertaken to show increased release of radionuclides encapsulated in bitumen due to microbial action and only one study has reviewed microbial attack of asphalt containing inactive salts.66 In the past, investigators have utilized any available method to maximize the contact of the microbial biomass with the substrate in order to increase the rate of attack. Unfortunately, these techniques have usually disrupted (or destroyed) the structural integrity of the bitumen to such an extent as to preclude the possibility of their use in any satisfactory experiment designed to show enhanced leaching. In the experiment described in the following pages a standardized procedure67 was followed that should allow good intercomparison of results. The procedure was modified slightly for test Sets C and D (described in Section II). to allow for maximum growth of hydrocarbonoclastic bacteria. 43 Optimal nutrient, oxygen and temperature conditions were maintained to create an experimental system that could resolve any difference in mass leaching of radionuclides from bitumen that was or was not undergoing microbial attack. Although microbial growth was not dependent on the use of bitumen as a sole carbon source, after approximately 12 hours (see Section II) an endogenous growth phase had been reached for the mixed population and further growth was dependent on the use of bitumen as a carbon source. The objective of this investigation was simply to determine if a statistically significant difference existed between inoculated samples and their respective controls, irrespective of the mechanism (solubilization, emulsification or biodegradation) under conditions that were optimized for microbial growth. 44 2.• METHODS Twelve identical samples of Sp-170 (oxidized) bitumen containing 38 wt.% sodium nitrate, 4.914 »iCi/gm 60Co and 8.229 »iCi/gm 137Cs (New England Nuclear Ltd.) were prepared in a twin-screw extruder at a product flow rate of 2.163 kg/hr and a peak temperature of <170°C. The final homogeneous cylindrical product had a mean mass, volume and area of 21.2 gU=1.08), 15.7 cm3(tf=7.90 X IO"?) and 35.1 cm2U=1.05) resp ectively. While the leach samples cooled for four days at ambient temperature, four separate leachant solutions were prepared and consisted of the following: Leachant Solution A Distilled, demineralized water (conductivity <1.00 X 10"6Mho/cm). Leachant Solution B T5 Distilled, demineralized water (conductivity - as above). 2) Mineral salts solution as described earlier (Section II). 3) Microbial nutrient media consisting of: 0.3% malt extract, 0.3% yeast extract and 0.5% peptone. Leachant solution C T) Distilled, demineralized water(conductivity - as above). 2) Mineral salts solution as described earlier (Section II). 3) Microbial nutrient media consisting of: 0.3% malt extract, 0.3% yeast exctract and 0.5% peptone. 4) Hydrocarbonoclastic bacteria (Culture-D). Leachant Solution D Tl Distilled, demineralized water (conductivity - as above). 2) WN-1 Synthetic groundwater solution as described 45 earlier in Section II.* 3) Microbial nutrient media consisting of: 0.3% malt extract, 0.3% yeast extract and 0.5% peptone. 4) Hydrocarbonoclastic bacteria (Culture-D). The bitumen samples were placed in 250 ml Sybron/Nalge wide-mouth, straightside polymethylpentene jars with polypropylene screw closures. Three samples for each leachant solution were then immersed in 100 mis of leachant, in such a manner as to maximize the exposure between the leachant and sample surface (with not less than 5.0 mis covering the sample). To maintain good aeration of the microbial cultures but to minimize release of radionuclides as a result of mechanical agitation, all samples were agitated horizontally by a Lab-Line Junior Orbit Shaker at 100 RPM. The leachant solutions were changed according to the guidelines of Hespe67 - every 24 hours for the first 7 days and then once per week for the following 8 weeks. Prior to termination of the experiment a final sample was collected 30 days after the end of the 8 week sampling period. For the duration of the test all samples were maintained at an average temperature of 23.6°C (tf=1.64). In order to ensure microbial activity was at a maximum rate (exponential growth phase), all sterile leachant solutions (C and D) were innoculated 3-4 hours before * In keeping with a "worst-possible-case" philosophy, WN-1 synthetic groundwater was selected as a suitable example since this groundwater was shown earlier (Section II) to be the most conducive to growth of Culture-D. 46 the time in which they were to be changed (see Section II). A. ANALYSIS Immediately prior to each leachant change, 25.0 mis of spent leachant were withdrawn from the sample containers and transferred to polypropylene vials. The subsequent analysis employed a multi-channel y-spectrometer equipped with a Ge(Li)* detector. Counting took an average of 3 hours for each sample. Most samples averaged between 2-3 orders of magnitude above background (1 X 10" 12 Ci/ml) therefore background was not considered a significant factor in the resulting statistical analysis. Conductivity-and pH measurements were made with the use of Radiometer(Copenhagen) and Fisher Instruments (see Appendix D) . * Ge(Li) - Germanium, Lithium. 47 3. RESULTS AND DISCUSSION Visual interpretation of Figures 13 to 18 show only one consistent trend is evident in the profiles of: £an V vs (tr,)0-5 Eqt.IV. 1 A0 F (cumulative fraction leached vs time). Set A's slope is greatest in most cases at t>21 days in comparison to Sets B,C and D. These latter test sets all appear to be approaching a slope=0 (Figure 16). As mentioned earlier, justification for the leaching behaviour of set A can be explained by a high AC. In this case, diffusion will cause a net movement of radionuclides between the bitumen and DIW. Although all samples were virtually identical in terms of mass, volume and area, small surface imperfections would explain the initial differences in leaching behaviour of the samples. However, long term behaviour would be a function, ultimately, of the leachant rather than the sample. A. STATISTICAL EVALUATION Since only qualitative evaluations may be made by inspection of Figures 13 to 18, an Analysis of Variance (with one-independent variable) coupled with the Student-Newman-Keuls procedure68 was employed as a quantitative approach to 48 determine differences in sample means. Since slope~0 at t>14 days (see Figure 18), sample means were evaluated from the cumulative fraction leached from t=14 to t=93 days. All statistical tests were performed independently for the two isotopes used, at an c=0.05 significance level (see Appendix E for statistical results). Inspection of Appendix E shows that for 60Co the average means of Sets A and B were significantly different from the average means of Sets C and D at a=0.05, and for 137Cs Group A was significantly different from B,C and D. However, there was no significant difference between C and D and between B and D. Thus, the combined statistical analysis for 60Co and 137Cs illustrates only that the Set A average was significantly higher than sets C and D's average at a=0.05. Set B's mean was statistically homogeneous to Set A for 60Co as a result of the abnormally low leaching behaviour of 60Co for sample A1 (Figure 13). This is illustrated by the profiles of all other samples but especially Figure 21 in which A1 shows abnormally low leaching with respect to A2 and A3. Thus, it appears sample A1 could represent an anomaly in which the initial leaching (at Day 1,2 and 3) was unusually supressed. This abnormality, in turn, affects the statistical analysis for the entire test. 49 B. CONCLUSION After 93 days of leaching under optimal conditions, microbial attack did not enhance the release of 137Cs and 60Co from bitmen. Extrapolation of the data and/or plots presented here, would not provide a viable case for enhanced leaching of these representative radionuclides for the long-term (t>93 days). However, the cumulative fraction leached is a function of leachant conductivity (see Appendix C and D). This is certainly a consideration for real repository conditions in which the conductivity of native groundwaters are expected to be high. 50 V. EFFECT OF CHELATING AGENTS ON RADIONUCLIDE MIGRATION As a result of a "defense in depth"* philosophy adopted by many of the organizations contemplating land-burial of radwastes, naturally occurring geologic media is being considered as a potential radionuclide adsorbent. The media that may comprise this barrier will occur naturally in situ, or various materials with a high adsorption capacity (bentonite) may be used to augment the burial site's natural ability to attenuate radionuclide migration through its subsurface environment. 1. BACKGROUND Although numerous studies26" 3 0 , 6 9 "75 have been performed to date on the adsorption of radionuclides to soils, sands and gravels, few experiments have considered adsorption to these materials under non-idealized conditions. The prognosis for a * A "defence in depth" philosophy utilizes multiple barriers to arrest the return of escaped radionuclides to the biosphere. 51 radionuclide that has completely breached its solidifying matrix but abuts a well packed adsorbent is quite good. This adsorbent will tend to reduce the movement of the released radionuclide via two independent mechanisms: a) a well-packed, highly dense adsorbent of small particle size will drastically reduce the groundwater flow rate and therefore decrease the active particle's linear velocity; and b) the adsorbent will "tie-up" the escaped nuclides through various physicochemical mechanisms such as ion-exchange, van der Waals attraction, covalent bonding, etc. Unfortunately, numerous mitigating factors exist that may reduce the ability of the backfill material to bind released radionuclides. These factors have only received cursory attention. For instance, the ability of some dissolved compounds to have strong ionic, secondary or complex interactions with common fission products may serve to impair or neutralize the geologic media's ability to attenuate these radionuclides. Of potential concern to the Nuclear Industry are multidentate chelating agents such as ethylenediamine-tetraacetic acid (EDTA), diethylenetriaminepentaacetic acid (DTPA) or cyclohexanediaminetetraacetic acid (CDTA). Since many of these compounds are used in conjunction with detergents, their use for radioactive decontamination is essentially ubiquitous. A recent study26 has shown a 20,000 fold decrease in the 52 adsorptive capacity of Conasauga shale for 60Co due to the presence of extremely low concentrations of EDTA. As a result, many 60Co contaminant plumes showing abnormally high migration rates may be attributed to the decreased ability of the soil to bind complexed 60Co.26 In addition to the synthetic multidentate ligands mentioned above - many naturally occurring organics may act as complexing agents. These organics include humic and fulvic acids, many dicarboxylic acids, and various microbially-generated biochemicals such as hydroxamate and polyhydroxamate.27 Even glycine, the simplest amino acid, may serve to complex waste radionuclides. Due to this potential for enhanced migration of radionuclides through geologic media due to microbial action, the following set of experiments was designed to illustrate if there was an observable effect and if so, to determine its magnitude. Accompanying those runs that directly employed microbial populations were other experiments that would show the adsorption of 60Co, 137Cs and 85Sr to bentonite, gabbro and granite in the presence of EDTA, Turco (a common radioactive decontamination compound), SCSSS, Granite Groundwater* and deionized, demineralized water. In order to simulate real conditions, all solutions that contained * The composition of SCSSS (Standard Canadian Shield Saline Solution) and Granite Groundwater is discussed in Appendix B. 53 microbial populations were taken from the leachant solution (after 1 week's contact) mentioned in Section IV. From the combined results of, these experiments the effect of EDTA, Turco, microbes and the antagonistic (or enhanced) effect of competing cations (60Co-137Cs, 85Sr-137Cs) could be compared and interrelated. 2. METHODS Eight independent experimental runs were performed and are listed in Tables III-X following. For each determination, 1.0 g of adsorbent (Fisher-bentonite, 40-50 mesh gabbro or granite) was placed in an acid-washed (10 minutes in 6N HN03) polypropylene test tube and mixed with 14.8 mis of adsorbate consisting of "super Q"* water, SCSSS, Granite Groundwater,10"5M EDTA, Turco** or the leachant material (1 week's contact) of set A or D described earlier (see Section IV). Standard solutions of 6°Co,137Cs,85Sr or a combination of 60Co and 137Cs or 85Sr and 137Cs were then added (0.2 mis) to all samples not containing leachant material to yield an initial total activity not exceeding 1.05 X 10"1 uCi. Each tube was then sealed with parafilm and allowed to rotate on a * "Super Q" water is water that has been distilled, deionized, millipore filtered and passed through activated carbon. * Turco is a common decontamination solution containing 6.0 wt.% diammonium hydrogen citrate, 2.5 wt.% oxalic acid and 1.0 wt.% phenylthiourea. This solution was diluted to a diammonium hydrogen citrate concentration of 10"5M. 54 Scientific Industries Incorporated Model 151 rotater. Agitation was continued for 48 hours at 5 RPM to minimize grain abrasion.30 Temperature ranged from 20-25°C. Upon termination of each run adsprbate and adsorbent were separated via centrifugation at 15,000 RPM for 60 minutes. Appropriate controls (test radionuclide + liquid phase only) were run with each experimental group. To evaluate the effect nutrient media (composition reported in Section II) had on adsorptivity, an entire experimental run was set-up consisting of nutrient media spiked with 60Co and 137Cs. The results of this control group are shown in Table IX. 3. ANALYSIS Upon termination of centrifugation 6.0 mis of supernatant were collected, placed in polypropylene vials and counted on a multi-channel y-spectrometer as per Section IV. The y-activity background and count time remained unchanged (from that described in Section IV) for all analyses. According to convention,30176 the distribution coefficient, K^, was evaluated according to the following formula: KD (ml/g) = (Cn - Ce )(V) Eqt.V.1 (Ce )(M) Where C0 is the radionuclide concentration initially, Ce is the radionuclide concentration at equilibrium, V is the volume of liquid and M is the mass of adsorbent material. 55 Evaluation of this equation for every run yields a numerical expression for the distribution of each radionuclide between the liquid and solid phase. This method allows for good intercomparison of results as adsorbent or other experimental conditions change. The initial concentration of each radionuclide was evaluated through controls that contained components identical to the experimental sets except for an adsorbent. Unfortunately, it became evident from these runs that some radionuclide adsorption to the reaction vessel walls occurred. To minimize this effect, 10""5M EDTA was added to 60Co and 137Cs controls. The presence of EDTA in the control tubes decreased the adsorption of cobalt to the vessel walls. Since the net adsorption (as expressed by K6) of 60Co is greatly effected by C0 all KB's for 60Co were calculated from a C0 that contained EDTA. Since a microbial biomass may adsorb various species, all KD's of solutions containing active cultures were evaluated from a C0 of net available (unadsorbed) activity. Thus, the available activity of an active solution of leachant (from Section IV) was evaluated as that activity remaining free in solution.after the treatment described earlier in Methods but with no adsorbent. This alteration will resolve the difference between radionuclides adsorbed to the microbial population and the specific adsorbent. 56 4. RESULTS AND DISCUSSION Tables III-V indicate that adsorption of 60Co was higher than that of any other nuclide. However, the effect of EDTA was much more pronounced with cobalt and with a granite adsorbent, it elicits a 1900 fold decrease in K0. This result, although not as dramatic, is in accordance with that reported by Means and Crerar.26 As expected, EDTA had only a negligible effect on 137Cs adsorption but 85Sr had slightly decreased KD's due to EDTA. However, since EDTA does not form strong complexes with anything other than rare earths, transition metals or transuranics, this effect may be expected. The relative effect of Turco on decreasing KD was greatest for 85Sr in which an 11 fold decrease in adsorption to bentonite was observed. Sample 60CoUCi/ml) KD Bentonite 2.051 X IO"4 7.41 X Gabbro 4.508 X 10"3 3.23 X Granite 1.493 X 10'3 1.01 X Bentonite+EDTA 3.068 X 10"3 4.82 X Gabbro+EDTA 1.050 X 10-1 0.00 Granite+EDTA 9.813 X 10"2 5.25 X Bentonite+Turco 2.908 X l0-a 5.22 X Control 1.016 X 10"1 Table III - 60Co ADSORPTION DATA 57 Sample 137Cs(„Ci/ml) KD Bentonite 1.643 X 10-3 7.54 X 10 Gabbro 7.325 X 10"3 1 .57 X 10 Granite 4.615 X 10'3 2.59 X 10 Bentonite+EDTA 1.695 X 10"3 7.30 X 10 Gabbro+EDTA 7.513 X 10'3 1 .53 X 10 Granite+EDTA 3.154 X 10-3 3.85 X 1 0 Bentonite+Turco 1.899 X 10"3 6.50 X 10 Control 8.41.9 X 10"2 Table IV - 137Cs ADSORPTION DATA Sample 85Sr(„Ci/ml) 6.975 X 10"" K0 Bentonite 2.23 X Gabbro 3.164 X 10"2 3.44 X Granite 4.619 X 10"2 1 .88 X Bentonite+EDTA 7.931 X 10"" 1 .96 X Gabbro+EDTA 1.028 X 10" 1 2.02 X Granite+EDTA 1.036 X 10"1 8.51 X Bentonite+Turco 7.625 X 10'3 1 .90 X Control 1.042 X 10"1 Table V - 85Sr ADSORPTION DATA Sample e o CoUC i/ml) Co,Cs+Bentonite 1 . 757 X 10"" Sr,Cs+Bentonite Co,Cs+Gabbro 1 . 766 X 10"3 Sr,Cs+Gabbro Co,Cs+Granite 7. 181 X 10-" Sr,Cs+Granite Co,Cs(Control) 1 . 224 X I0"a Sr,Cs(Control) Sample 6 0 Co K0 Co,Cs+Bentonite 3. 50 X 1 O3 Sr,Cs+Bentonite Co,Cs+Gabbro 3. 35 X 102 Sr,Cs+Gabbro Co,Cs+Granite 8. 46 X 1 O2 Sr,Cs+Granite 1 37CsUCi/ml) 8 5Sr UCi/ml) 8 .650 X I0"a 8 .906 X 10-" 4 .199 X 10"" 2 .066 X 10"3 2 .481 X 10"3 1 .403 X 10'2 1 .824 X 10~3 2 .024 X 10"3 2 .141 X 10"2 2 .508 X 10"3 3 .658 X 10"2 1 .743 X 10"3 1 37Cs K0 8 5Sr K0 8 .71 X 102 8 .45 X 102 1 .83 X 103 3 .56 XJ02 2 .94 X 102 4 .03 X 101 4 .05 X 102 3 .64 X 102 2 .13 X 101 Table VI - COMPETING ION ADSORPTION DATA 58 Sample Co,Cs+Bentonite + Granite G/W Sr,Cs+Bentonite + Granite G/W Co,Cs+Granite + Granite G/W Sr,Cs+Granite + Granite G/W Co,Cs+Bentonite + SCSSS G/W Sr,Cs+Bentonite + SCSSS G/W Co,Cs+Granite + SCSSS G/W Sr,Cs+Granite + Granite G/W Sample Co,Cs+Bentonite + Granite G/W Sr,Cs+Bentonite + Granite Co,Cs+Granite + Granite G/W Sr,Cs+Granite + Granite Co,Cs+Bentonite + SCSSS G/W Sr,Cs+Bentonite + SCSSS G/W Co,Cs+Granite + SCSSS G/W Sr,Cs+Granite + Granite G/W 60Co(„Ci/ml) 1.774 X 10"" 7.550 X 10-" 8.181 X 10"4 2.236 X 10"2 60Co K0 3.47 X 103 8.04 X 102 7.40 X 102 1.26 X 102 37CsUCi/ml) 1 .086 X 10" 3 1 .033 X 10" 3 3 .408 X 10" 3 3 .859 X 10" 3 1 .084 X 10" 2 1 .091 X 10" 2 2 .084 X 10" 2 1 .969 X 10" 2 i 37Cs Ko 6. 91 X 102 7. 27 X 1 o2 2. 10 X 102 1 . 84 X 102 5. 57 X 101 5. 52 X 101 2. 18 X 101 2. 39 X 101 85Sr(„Ci/ml) 4.911 X 10"" 3.870 X 10"2 5.022 X 10"2 5.279 X 10"2  B5Sr KD 1.57 X 103 5.06 X 10° 4.55 X 10" 1 0.00 Table VII - ADSORPTION DATA FOR COMPETING IONS IN SELECTED GROUNDWATERS 59 Sample 60CoUCi/ml) 137Cs(„Ci/ml) Set A+Bentonite 3.955 X 10"a 7.763 X 10"" Set A+Gabbro 1.490 X 10"3 1 .902 X 1.0'3 Set A+Granite 4.411 X 10"" 9.788 X 10"" Set A (Control) 8.838 X 10"3 2.359 X 10~2 Sample 60CoKo 137CsK0 Set A+Bentonite 3.20 X 102 4.41 X 102 Set A+Gabbro 7.40 X 101 1.71 X 102 Set A+Granite 2.86 X 102 3.47 X 102 Table VIII - LEACHANT A ADSORPTION DATA Sample 6 °CoJJiCjVml) 13 7Cs (nCi/ml) Set C+Bentonite 2.001 X 10"3 1.867 X 10"3 Set C+Gabbro 5.815 X 10'3 1.278 X 10'2 Set C+Granite 6.030 X 10"3 1.249 X 10"2 Set C (Control) 5.631 X 10~3 1.299 X 10"2 Sample 60CoKD 137CsK0 Set C+Bentonite 2.72 X 101 8.93 X 101 Set C+Gabbro 0.00 2.44 X 10"1 Set C+Granite 0.00 5.97 X 10~1 Table IX - ADSORPTION DATA' FOR NUTRIENT MEDIA CONTROL Sample 6°Co(pCi/ml) 137Cs(„Ci/ml) Set D+Bentonite 1.949 X 10'3 6.519 X 10"J Set D+Gabbro 7.781 X 10"3 1.795 X 10~2 Set D+Granite 7.819 X 10"3 1.836 X 10~2 Set D (Control) 1.135 X 10"ft 3.062 X 10"U Sample 6°Co KD 137Cs K0 Set D+Bentonite 3.96 X 101 2.90 X 101 Set D+Gabbro 0.00 9.94 X 10"1 Set D+Granite 0.00 6.35 X 10"1 Table X - LEACHANT D ADSORPTION DATA 60 The competing effects of 60Co on 137Cs and 85Sr on 137Cs are reported in Table VI. In all cases bentonite showed the highest adsorptive capacity followed by granite (for 60Co and 137Cs) and gabbro. The relative difference in KD's for the three adsorbents decreased for each group of radionuclides from their non-competitive counterpart. As evidenced by the data in Table VI, the adsorptive capacity of bentonite was decreased by the competing ions while that for gabbro and granite was increased (perhaps due to a non-competitive mechanism for adsorption). Table VIII presents data relating to the effect of synthetic groundwaters on KB. In every case and for both adsorbents tested (bentonite and granite) the groundwater with the highest conductivity (SCSSS) has the greatest effect on decreasing K„. This higher figure is easily explained by the saturation of available active sites on the adsorbent by non-active ions present in the highly concentrated brine. Bentonite showed a greatly reduced adsorptivity for the leached radionuclides contained in leachant A and D. However, it appears that leachant A (JJIW) only slightly perturbed the adsorptive capacity of granite and gabbro. In the case of leachant A contacted with gabbro or granite, a < 2 fold reduction was found for KD's between this leachant and deionized, demineralized water containing 60Co and 137Cs. The effect of leachants C and D on the adsorption of these 61 radionuclides to granite or gabbro is significant. The adsorptivity of both gabbro and granite for the radionuclides contained in leachant C or D was decreased more than 100 times by the complexing agents present in the two solutions (as evidenced by the R0 values reported in Tables VI,IX and X). XXXIII and XXXIV. 5. REMARKS The effect of complexing agents (whether synthetic or otherwise) may cause a reduced attenuation of waste radionuclides leaching from a nuclear waste repository. As evidenced from the results, strong chelating agents present at 10"5M can decrease a RD by up to 3 orders of magnitude. Turco did not decrease K0's as much as EDTA, probably because its major constituent (diammonium hydrogen citrate) is not as strong a complexing agent as EDTA. 62 VI. CONCLUSION Throughout the course of these experiments, conditions for microbial growth were maintained at a level only possible under the idealized environment of a laboratory. The conditions expected in a full-scale low-level repository are as follows: a) a moderately low temperature (<20°C); b) a low oxygen atmosphere (approaching O.Oppm 02); and c) devoid of any microbial growth. Since it is assumed that water will fill the repository, the presence of an unusually high salt content may be expected that would be bacteriocidal or bacteriostatic for all but a few halophiles. In addition to the conditions listed above, a fourth constraint that may inhibit the microbial growth under repository conditions is the lack of an initial contaminating culture that is capable of utilizing various hydrocarbons as a 63 substrate. Also, the low temperature (<20°C), high pressure and lack of oxygen will serve to create a microbially hostile environment. Even if various organisms could survive under these conditions and utilize bitumen as their sole carbon source, the rate of their metabolism (and therefore rate of oxidation of bitumen) would be extremely slow. In addition to the conditions listed above, a fourth constraint that may inhibit the microbial growth under repository conditions is the lack of an initial contaminating culture that may utilize various hydrocarbons as a substrate. The solidification of waste radionuclides with bitumen requires a bitumen temperature of approximately 175°C. The molten bitumen-waste mixture will then be placed in a stainless steel container. The effect of both the molten bitumen and the impermeable container will: 1) kill any contaminating microbes on or near the bitumen; 2) volatilize the most easily metabolized components of the bitumen (light alkane fraction); 3) create an anhydrous environment; and 4) prevent microbial contamination during storage or final disposal. As illustrated by the results presented in Section III, the anticipated background radioactivity will not affect the net growth of a microbial population. Changes may occur to the overall genotype of the population as a result of an 64 increased rate of mutation. However, the number of viable organisms will not change due to the radiation expected under repository conditions. Although microbially enhanced leaching from bitumen was not found, a significant decrease in K0 was observed as a result of microbial action but its importance is secondary to complexation and/or chelation due to synthetic agents. Also, since microbial proliferation will be highly limited, any or all enhanced migration of a waste radionuclide due to microbial action would probably be "swamped" by migration of nuclides chelated prior to conditioning (provided the complex is not thermally labile). A secondary influence of a microbial population present in situ may be to utilize organic complexes as a metabolite. This in turn would serve to decrease enhanced radionuclide migration due to any previous chelation reactions. On the basis of these short-term experiments, the effect of microbial action on long-term radioactive waste disposal should be small. If microbial attack does occur, other factors such as diffusion or chelation (to synthetic chelating agents) would "swamp" this effect. 65 BIBLIOGRAPHY 1. Tomlinson,M., et al., "Management Of Radioactive Wastes From Nuclear Fuels And Power Plants In Canada", Atomic Energy of Canada Limited, Rep.AECL-5706 (1977), p.1-2. 2. 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Buckley,L.P.,Pettipas,W.H., "Bituminization of Reactor Wastes, Development, Design and Demonstration", Atomic Energy of Canada Limited, Rep.AECL-7338 (1981) p.5. 49. Charlesworth,D.H., op.cit., p.2. 50. Barnhart,B.J. et al., "Potential Microbial Impact on Transuranic Wastes Under Conditions Expected in the Waste Isolation Pilot Plant (WIPP), December 15,1978-March 15,1979", Los Alamos Scientific Laboratory, Rep.LA-7839-PR .(1979). L 51. Godbec,H.W., et al., "Diffusion of Radioisotopes Through Waste Solids", Transactions of the American Nuclear Society, Vol.12, (.1969) pp.450-451. 52. Dejonghe,P., et al., "Insolubilization of Radioactive Concentrates by Asphalt Coating, Final Report 2, 1st part, Concerning Proposal 167", Eur. Atomic Energy Commission,Rep.EURAEC-695 (1963). 53. Crank,J., The Mathematics Of Diffusion, 2nd ed. (London: Oxford University Press, 1975). 54. Hespe,E.D., "Leach Testing Of Immobilized Radioactive Waste Solids", Atomic Energy Review, Vol.9, No.1, (1971) pp.201. 55. Buckley,L.P., Personal Communication, June 1981. 56. Crank,J., op.cit., p.2. 57. Kulman,F.E., "Microbiological Deterioration of Buried Pipe and Cable Coatings", Corrosion, Vol.14, (1958) pp.21 3-222. 58. Martin,K.G., "Deterioration of Bituminous Roofing 69 Fabrics", Division of Building Research, Commonwealth Scientific and Industrial Research Organization, Melbourne, Rep.11 (1961). 59. Harris,J.O., "Soil Microorganisms in Relation to Cathodically Protected Pipe", Corrosion, Vol.16, (1960) pp.441t-448t. 60. Harris,J.O., "Microbiological Studies Reveal Significant Factor in Oil and Gas Pipeline Back-Filled Ditches", Kansas State University Agricultural Experiment Station, Rep.135 (1963). 61. Perry,J.J., "Microbial Cooxidation Involving Hydrocarbons", Microbiological Reviews, Vol.43, No.1, (1979) pp.59-72. 62. Gerson,D.F., Zajic,J.E., "Surfactant Production From Hydrocarbons by Corynebacterium lepus, sp.nov. and Pseudomonas asphaltenicus sp.nov.", Developments in Industrial Microbiology, Vol.19, (1978) pp.577-599. 63. Lupton,F.S., Marshall,K.C., "Effectiveness of Surfactants in the Microbial Degradation of Oil", Geomicrobiology Journal, Vol.1,No.3 (1978) pp.235-247. 64. Zajic,J.E., Supplisson,B., Emulsification and Degradation of Bunker-C Fuel Oil by Micro-organisms", Biotechnology and Bioengineering, Vol.14, (1972) pp.331-343. 65. Cooper,D.G., Zajic,J.E., "Surface-Active Compounds from Microorganisms", Advances In Applied Microbiology, Vol.26, (1980) pp.229-253. 66. Rodier,J.,et al., "Bitumen Coating of Radioactive Sludges from the Effluent Treatment Plant at the Marcoule Centre, Review of the Progress Reports 1,2,3 and 4", Rep.CEA-2331 (1963). 67. Hespe,E.D., op.cit pp.195-207. 68. Nie,N.H., et al., SPSS: Statistical Package for the  Social Sciences, 2nd ed. (New York: McGraw-Hill Book Company, 1975), p.428. 69. Means,J.L., et al., "Chemical Mechanisms of 60Co Transport in Ground Water from Intermediate-Level Liquid Waste Trench 7: Progress Report for Period Ending June 30, 1975", Oak Ridge National Laboratory, Env. Sc. 70 Div., Rep.940 (1976). 70. Fried,S., et al., "Retention of Plutonium and Americium by Rock", Science, Vol.196, (1977) pp.1087-1089. 71. de Marsily,G., et al., "Nuclear Waste Disposal: Can the Geologist Guarantee Isolation?", Science, Vol.197, No.4303, (1977) pp.519-527. 72. Seitz,M.G., et al., "Studies Of Nuclear-Waste Migration In Geologic Media, Annual Report, November 1976-October 1977", Argonne National Laboratory, Rep.ANL-78-8, (1978) 73. Means,J.L., et al., "Adsorption of Co and selected actinides by Mn and Fe oxides in soils and sediments", Geochimica and Cosmochimica Acta., Vol.42, (1978) pp.1763-1773. 74. Sheppard,J.C., et al., "Retention of Radionuclides by Mobile Humic Compounds and Soil Particles", Environmental Science and Technology, Vol.14, No.11, (1980) pp.1349-1353. 75. Walton,F.B., et al., "Determination of Nuclide -Geologic Media Reaction Kinetics Using Mixing - Cell Contractors", Submitted to Chemical Geology, June, 1981. 76. Wilding,M.W., et al., "Removal of Cesium and Strontium from Fuel Storage Basin Water" in Advances In Chemistry  Series 153 ed. M.H. Campbell (Washington: American Chemical Society, 1976), pp.134-151. 71 APPENDIX A - ONTARIO MINISTRY OF THE ENVIRONMENT ANALYSIS* TEST/COLONY A B C D1 D2 Gram stain - + - - -Shape Rod Rod Rod Rod Rod Spores - + - - -Motility 30°C + + + + -20°C -Catalase + + + + + Oxidase + — — — + Glucose OF (5 Day) — — — F -Growth 20°C + + + + TSA 30°C + + + 35°C + + Weak + 42°C + + - -MacConkey Agar 30°C Gr + No Gr No Gr Gr + Gr + LAC- LAC+ LAC-Skim Growth + + Weak + + Milk Pigment - - - - -Agar Caseinase - - - - -Flouresc. — — — — + Nitrate (5 Day) Reduction +(Gas) — +(N02) +(N02) — Gelat inase - + + -Arginine (5 Day) Dihydrolase — + Urease - - + Citrate + Growth 6.5% NaCl Weak + + -ONPG - + -"+" and "-" represent growth or no growth, respectively. * Independent analysis was performed for each of the two distinct species found in Culture D 72 Colony Morphology: TSA 30°C A - Tan, dry, wrinkled. B - Cream to white, irregular, spreading, margin. C - Tiny, cirular, smooth, pale yellow. D1- Circular, cream, convex, smooth, entire, margin. D2- Circular, cream, convex, smooth. 73 APPENDIX B - SYNTHETIC GROUNDWATER SOLUTIONS STANDARD SYNTHETIC GRANITE GROUNDWATER" 1) The following stock solutions were made up: a) 11.090 g MgSO,.7H20 /25ml b) 7.115 g MgCl2.6H20 /25mc) 1.512 g NaHC03 /25ml d) 1.965 g KOH /25me) 0.506 g KN03 /25mf) 0.291 g KF l 2) 0.10 ml of (a), (b), (c), (d), (e) and (f) were pipetted to a 2 L volumetric flask. 1.00 ml of (c) was added and the volume made up to 1700 mis with deionized water (DIW). 0.048 g Ca(OH)2 was added to a 200 ml volumetric flask filled with about 180 mis of DIW. C02 was bubbled through this mixture while stirring until the solution became clear. It was then filled to the mark with DIW and the contents of this 200 ml flask added to the 2 L volumetric flask. The final 100 ml of DIW was added to the volumetric flask to make the volume up to 2.00 L and the solution was stirred for 24 hours in contact with the atmosphere to bring the pH to "6.5 + 0.5. 74 STANDARD CANADIAN SHIELD SALINE SOLUTION (SCSSS)"" To 100.0 mis of DIW the following dry chemicals were added: a) 1.906 g KCl b) 1.216 g SrCl2.6H20 c) 3.080 g Na2Si03.9H20 d) 0.276 g NaHC03 e) 1.370 g NaN03 10.0 mis of this stock solution was added to a 2 L volumetric flask and made up to 2.0 litres. 110.050 g CaCl2.2H20, 4.056 g MgSO„.7H20 and 25.420 g NaCl were added and the entire mixture was stirred thoroughly. 75 BASALT GROUNDWATER4 * Stock Solution A The following was combined in a 200 ml volumetric flask: a) 100 ml DIW b) 8.000 g NaHC03 c) 5.485 g Na2SO„.10H20 d) 0.994 g MgSO,.7H20 e) 1.490 g KC1 f) 0.232 g KF This solution was stirred until dissolved and the volume made up to 200 mis. The following was then combined in a 2 L volumetric flask: a) 1800 ml DIW b) 0.0109 g CaS0„.l/2H20 and stirred until dissolved. Stock Solution B The following was then combined in a 200 ml volumetric flask: a) 180 ml DIW b) 1.871 g CaCl2.2H20 This was mixed until dissolved and the volume made up to 2 L. To the stirred 2 L volumetric flask the following was added: a) 4.0 ml Stock Solution A b) 4.0 ml Stock Solution B and made up to 2.0 litres, then stirred overnight. 76 WN-1 Saline-Solution** 1) The following stock solution was made-up in a 200 ml volumetric flask (filled to the mark with DIW) a) 0.537 g KCl b) 1.882 g NaHC03 c) 0.901 g NaN03 2) 20.0 mis of this stock solution was pipetted into a 2 L volumetric flask, the following dry chemicals added, then made up the mark with DIW. d) 0.056 g FeSO,.7H20 e) 0. 150 g SrCl2.6H20 f) 13.111 g CaCl2.2H20 g) 1 .232 g MgSOa.7H20 h) 9.520 g NaCl i) 1.282 g Ca(OH)2 77 APPENDIX C - LEACH TEST DATA TEST Al -TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT '• 0 686E-01 0 0623 2. 0 1G4E*00 0 1495 3 . 0 200E*00 0 1822 4 . 0 226E*00 0 2056 5 . 0 244E+00 0 2220 6 0 257E*00 0 2333 7 . 0 2G6E*00 0 2420 14 . 0 295E*00 0 2677 21 . 0 355E»00 0 3227 2B . 0 423E+00 0 3844 . 35 • 0 476E+0O 0 4324 42 . 0 541E*0O 0 4921 49. 0 G22E*00 0 5656 56. 0 717E*00 0 6515 63. 0 796E*00 0 7240 93. 0 1O8E*01 0 9800 " Table XI - LEACH 1-60 CUMULATIVE FRACTION INCREMENTAL LEACHED LEACH RATE CM CM/DAY 0 284E-03 0 284E-03 0 682E-03 0 397E-03 0 831E-03 0 149E-03 0 937E-03 0 106E-03 0 101E-02 0 751E-04 0 106E-02 0 512E-04 0 110E-02 0 399E-04 0 122E-02 0 167E-04 0 147E-02 0 358E-04 0 175E-02 0 402E-04 0 197E-02 O 312E-04 0 224E-02 0 389E-04 0 258E-02 0 479E-04 0 297E-02 0 559E-04 0 330E-02 0 472E-04 0 447E-02 0 389E-04 TEST DATA - TEST MASS DIFFUSION LEACH RATE G/CM"»2*DAY COEFFICIENT CM"2/SEC O.384E-03 0 734E-12 0.537E-03 0 211E- 1 1 0.201E-03 0 209E-11 0.144E-03 0 200E-1 1 0.101E-03 0 186E- 11 0.692E-04 0 171E- 1 1 0.539E-04 0 158E- 1 1 0. 226E-04 0 967E-12 0.484E-04 0 937E-12 0.543E-04 0 997E-12 0.422E-04 0 101E- 1 1 0.525E-04 0 109E- 1 1 0.647E-04 0 123E- 1 1 0.755E-04 0 143E- 11 0.638E-04 0 157E- 11 0.526E-04 0 195E- 11 SET A1 - 60Co TEST A2 - CO-60 TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL CUMULATIVE FRACTION RELEASED LEACHED PERCENT CM INCREMENTAL LEACH RATE CM/DAY MASS DIFFUSION LEACH RATE COEFFICIENT G/CM*-2*DAY CM**2/SEC 1 . 0. 125E+01 1.1811 0.532E-02 0 532E-02 0.719E-02 0 258E-09 2. 0. 155E + 01 1 . 4669 0.66 IE-02 0 129E-02 0.174E-02 0 199E-09 3 . 0. 159E+01 1 .4978 0.675E-02 O 139E-03 0. 188E-03 0 138E-09 4 . 0. 165E+01 1.5533 O.7OOE-02 0 250E-03 0.338E-03 0 111E-09 5. 0. 168E+01 1.5892 0.716E-02 0 162E-03 0.218E-03 0 933E- 10 6. 0 . 17 1 E+01 1.6148 0.728E-02 0 115E-03 0. 156E-03 0 802E-lO 7. 0 . 174E+01 1.6373 0.738E-02 0 101E-03 0.137E-03 0 707E-10 14 . 0. 185E+01 1.7446 0.786E-02 0 69 IE-04 0.933E-O4 0 401E-10 21 . 0. 199E+01 1.8778 0.846E-02 0 857E-04 0.116E-03 0 310E-10 28 . 0. 216E+01 2.0365 0.918E-02 0 102E-03 0. 138E-03 0 274E-10 35 . 0.232E+01 2.1920 0.988E-02 0 100E-03 0. 135E-03 0 253E-10 42. 0.253E*01 2.3856 0.108E-01 . 0 125E-03 0. 168E-03 0 250E-10 49 . 0.277E+01 2.6091 0.118E-01 0 144E-03 0. 194E-03 0 257E- 10 56 . 0.307E+01 2.893 1 0.130E-01 0 183E-03 0. 247E-03 0 276E-10 63 . 0.33 IE+01 3. 1262 0.141E-01 0 150E-03 0-203E-03 0 286E-10 93. 0.437E+01 4 . 1262 0.186E-01 0 I50E-03 0-203E-03 0 338E-10 Table XII - LEACH TEST"DATA - TEST SET A2 - 60Cc 78 TEST A3 - CO-60 TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT CUMULATIVE FRACTION LEACHED CM INCREMENTAL LEACH RATE CM/DAY MASS LEACH RATE G/CM"2*DAY DIFFUSION COEFFICIENT CM"2/SEC 1 . 0 126E*01 1.1856 0 534E-02 0 534E-02 0 722E-02 0 260E-09 2. 0 144E+01 1.3568 0 612E-02 0 770E-03 0 104E-02 0 170E-09 3. 0 I49E*01 1.4036 0 633E-02 0 211E-03 0 285E-03 0 121E-09 4. 0 162E+01 1.5266 0 688E-02 0 554E-03 0 748E-03 0 108E-09 5. 0 169E+01 1.5927 O 718E-02 0 298E-03 0 402E-03 0 937E- 10 6. 0 I73E+01 1.6280 0 734E-02 0 159E-03 0 2I5E-03 0 816E- 10 7 . 0 174E*OI 1.6430 0 741E-02 0 675E-04 0 911E-04 0 712E- 10 14 . . 0 181E+O1 1.7075 0 770E-02 0 415E-04 0 561E-04 0 385E-10 2 1 . 0 191E+01 1.7996 0 811E-02 0 593E-04 0 8COE-04 0 285E- 10 28. 0 202E+01 1.9047 0 858E-02 0 677E-04 0 913E-04 0 239E- 10 35. 0 218E+01 2.0570 0 927E-02 0 981E-04 0 132E-03 0 223E-10 42 . 0 243E*01 2.2887. 0 103E-01 0 149E-03 0 20 IE-03 0 230E-10 49. 0 270E*01 2.5511 0 115E-01 0 169E-03 0 228E-03 0 245E- 10 56 . 0 29GE*01 2.7932 0 126E-01 0 156E-03 0 210E-03 0 257E-10 S3. 0 323E+01 3 0503 0 137E-01 0 166E-03 0 224E-03 0 273E-10 93. 0 423E+01 3.9937 0 180E-O1 O 142E-03 0 191E-03 0 317E-10 Table XIII - LEACH TEST DATA - TEST SET A3 - 60Co TEST Bl - C0-60 TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL CUMULATIVE FRACTION RELEASED LEACHED PERCENT CM INCREMENTAL LEACH RATE CM/DAY MASS LEACH RATE G/CM**2*DAY DIFFUSION COEFFICIENT CM"2/SEC 1 . 0 492E*00 0.5415 0 229E-02 0 229E-02 0 309E -02 0 477E-10 2 . 0 608E+00 0.6689 0 283E-02 0 539E-03 0 727E-03 0 364E-10 3. 0 658E+00 0.7234 0 306E-02 0 231E-03 0 312E-03 0 284E-10 4 . 0 69SE*00 0.7674 0 324E-02 , 0 186E-03 0 25 IE-03 0 239E- 10 5. 0 729E*00 0.8022 0 339E-02 0 147E-03 0 199E-03 0 209E-10 6. 0 757E*00 0.8333 0 352E-02 0 131E-03 0 177E-03 0 188E-10 7 . 0 784E*00 0.8630 0 365E-02 0 125E-03 0 169E-03 0 173E-10 •14 . 0 960E+00 1.0565 0 447E-02 0 117E-03 0 158E-03 0 130E-10 2 1 . 0 113E+01 1.2446 0 526E-02 0 114E-03 0 153E-03 0 120E-10 28. 0 125E+01 1 . 3798 o 583E-02 0 817E-04 O 1 IOE-03 0 111E-10 35. 0 135E*01 1 .4806 o 626E-02 0 609E-04 O 822E-04 0 102E- 10 42. 0 144E+01 1.5856 0 670E-02 0 634E-04 0 857E-04 0 973E-11 49. 0 155E+01 1.7013 0 719E-02 0 699E-04 0 944E-04 0 960E-11 56. 0 165E+01 t.8130 0 767E-02 0 674E-04 0 911E-04 0 954E-1 1 63. 0 174E+01 1.9087 0 807E-02 0 578E-04 0 78 IE-04 0 940E-11 93 . 0 204E*01 2.2418 0 948E-02 0 470E-04 0 634E-04 0 678E-11 Table XIV - LEACH TEST DATA - TEST SET B1 - 60Co 79 TEST B2 - CO-60 TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT CUMULATIVE FRACTION LEACHED CM INCREMENTAL LEACH RATE CM/DAY MASS LEACH RATE G/CM**2*0AY DIFFUSION COEFFICIENT CM"2/SEC 1 . 0. 175E+01 1.6500 0.744E-02 0. 744E-02 0.100E-01 0. 503E-09 2. 0. 192E*01 1.8143 0.8 18E-02 0. 741E-03 0.100E-02 0. 304E-09 3 . 0. I99E*01 1.8815 0.848E-02 0. 302E-03 0.408E-03 0. 218E-09 4 . 0. 205E+01 1.9331 0.871E-02 0. 233E-03 0.314E-03 0. 173E-09 5 . 0. 207E*01 1.9550 0.881E-02 0. 987E-04 0. 133E-03 0. 141E-09 6. 0. 210E+01 1.9789 0.892E-02 0. 107E-03 0. 145E-03 0. 121E-09 7 . 0. 211E*0I 1.9943 0.899E-02 0. G98E-04 0.942E-04 0. 105E-09 14. 0. 219E+01 2.0678 0-932E-02 0. 473E-04 0.638E-04 0 564E-I0 2 1 . 0. 226E*01 2.1288 0.959E-02 0. , 393E-04 0.53 IE-04 0. 398E-10 28 . 0. 233E*01 2.1977 0.99 IE-02 0 444E-04 0. 599E-04 0. 319E-10 35. 0. 239E+01 2.2528 0.102E-01 0 355E-04 0. 479E-04 0. 268E-10 42. 0. 244E*0I 2.2993 0.104E-01 0 . 299E-04 0. 404E-04 0. 232E-10 49 . 0. 249E+01 2.3479 0.106E-01 0 .313E-04 0.423E-04 0. 2O8E-10 56 . 0. 253E*01 2.3878 0. 108E-01 0 . 257E-04 0.347E-04 0. 188E-10 63 . 0. 256E*01 2.4114 0.109E-01 0 . 152B-04 0.205E-04 0. 17OE-10 93 . 0. 263E*01 2.4770 0. 1 12E-01 0 984E-05 0. 133E-04 0. 122E- 10 Table XV - LEACH TEST DATA - TEST SET B2 - 60Co TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL MASS DIFFUSION TIME DAYS RELEASED MICROCURIES RELEASED PERCENT LEACHED CM LEACH RATE CM/DAY LEACH RATE G/CM*'2'DAY COEFFICIENT CM«*2/SEC 1 . 0. 145E+01 1.3054 0.599E-02 0 .599E-02 0 810E-02 0. 326E-09 2 . 0. 165E+01 1.4853 . 0.68 IE-02 0 825E-03 0 112E-02 0. 211E-09 3. 0. 175E+01 1 .5759 0.723E-02 0 415E-03 0. 562E-03 0. 158E-09 4 . 0. 179E+01 1 .6148 0.74 IE-02 0 .179E-03 0. 242E-03 0. 125E-09 5. O. 181E+01 ».6292 0. 747E-02 0 660E-04 0 893E-04 0. 102E-O9 6 . 0. 183E+01 1.6456 0.755E-02 0 .752E-04 0. 102E-03 0. 864E-10 7. 0.184E+01 1.6551 0.759E-02 0. 436E-04 0. 590E-04 0. 749E-10 14. 0.191E+01 1.7204 0.789E-02 0 428E-04 0. 580E-04 0. 405E-10 2 1 . 0.198E+01 1.78 13 0.817E-02 0. 399E-04 0. 540E-04 0. 2B9E-10 28 . O.203E*01 1.8332 0.841E-02 O. 340E-04 0. 460E-04 0. 230E-10 35. 0.207E+01 1 .8660 0.856E-02 0. 215E-04 0. 290E-04 0. 190E-10 42. 0. 214E+01 1.9284 0.885E-02 0. 409E-04 0. 553E-04 0. 169E- 10. 49. 0.220E+01 1.98 1 1 0.909E-02 0. 346E-04 0. 468E-04 0. 153E-10 56. 0.230E+01 2.0692 0.949E-02 0. 577E-04 0. 78 1E -04 0. 146E-10 63. 0.234E+01 2.1088 0.967E-02 0. 260E-04 0. 35 IE-04 0. 135E-10 93. 0.246E+01 2.2163 0.102E-01 0. 165E-04 0. 223E-04 0. 101E-10 Table XVI - LEACH TEST DATA - TEST SET B3 - 60Co 80 TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT CUMULATIVE FRACTION LEACHED CM INCREMENTAL LEACH RATE CM/DAY MASS LEACH RATE G/CM'"2'DAY DIFFUSION COEFFICIENT CM**2/SEC 1 . 0. 135E-KJ1 1.3196 0 586E-02 0 586E-02 0 79 IE-02 0 312E-09 2 . 0. 144E+01 1.4130 0 627E-02 0 414E-03 0 560E -03 0 179E-09 3 . 0. 149E+01 1.4627 0 649E-02 0 221E-03 O 298E-03 0 128E-09 4 . 0. 151E*01 1.4833 0 658E-02 0 917E-04 0 124E-03 0 985E-10 5 . 0. 153E*01 1.4965 0 664E-02 0 585E-04 0 790E-04 0 802E- 10 6. 0. 153E*01 1.5043 0 668F.-C2 0 343E-04 0 464E-04 0 67SE-10 7 . 0. 154E+01 1.5115 0 671E- 02 0 32 IE-04 0 434E-04 0 584E- 10 14 . 0. 157E*01 1 5398 0 683E-02 0 179E-04 0 242E-04 0 303E-10 21 . 0. 162E*01 1.5910 0 706E-02 0 325E-04 0 439E-04 0 216E-10 28. 0. 166E+01 1.6240 0 72 IE-02 0 209E-04 0 283E-04 0 169E- 10 35. 0. 168E+01 1.6498 0 732E-02 0 163E-04 0 220E-04 0 139E-10 42 . 0. 172E+01 1.6820 0 746E-02 0 205E-04 0 276E-04 0 121E-10 49 . 0. 175E*01 .1.7154 0 761E-02 0 212E-04 0 286E-04 0 108E- 10 56. 0. 179E+01 1.7580 0 780E-02 0 270E-04 0 365E-04 0 988E-11 63. 0. 1R3E*01 1.7971 0 798E-02 0 248E-04 0 335E-04 0 918E-11 93. 0. 190E+01 1.8661 0 828E-02 0 102E-04 0 138E-04 p_ 670E-11 Table XVII - LEACH TEST DATA - TEST SET C1 - 60Co TEST C2 - CO-60 TOTAL TIME DAYS TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL RELEASED RELEASED LEACHED LEACH RATE MICROCURIES PERCENT CM CM/DAY MASS LEACH RATE G/CM«-2*DAY DIFFUSION COEFFICIENT CM*'2/SEC 1 . 0.47OE+OO 0.4610 0.204E-02 0 204E-02 0.276E-02 0.378E-10 2 . 0.587E+0O 0.5757 0.255E-02 0 507E-03 0.686E-03 0.295E-10 3. 0.658E+00 0.6448 0.285E-02 0 305E-03 0.413E-03 O.246E-10 4 . 0.695E+00 0,68 14 0.301E-02 0 162E-03 0.219E-03 0.206E-10 5. O.724E+0O 0.7095 0.314E-02 0 124E-03 0.168E-03 0.179E-10 6 . 0.748E+00 0.7333 0.324E-02 0 105E-03 0.143E-03 0. 159E- 10 7 . 0.7G2E*O0 0.7475 0.331E-02 0 630E-04 0.852E-04 0.142E-10 14 . O.832E+00 0.8153 0.361E-02 0 4 28E;04 0.579E-04 0.844E- 1 1 21 . 0.9O3E+O0 0.8855 0. 392E-02 0 443E-04 0.600E-04 0.664E-11 28 . 0.969E+OO O.9504 0.4 20E-02 o 410E-04 0.555E-04 0.573E-11 35. 0.103E+01 1.0136 0.448E-02 0 400E-04 0.541E-04 0.522E-11 42 . 0.108E+01 1.0629 0.470E-02 0 311E-04 0.42 IE-04 0.47BE-11 49 . 0. 1 14E+01 1.1189 0.495E-02 0 354E-04 0.479E-04 0.454E-1 1 5G . 0.163E+01 1.6014 O.7O8E-02 o 305E-03 0.412E-03 0.814E-1 1 63. 0.169E+01 1.6600 O.734E-02 0 370E-04 0.501E-04 0.777E-1 1 93. 0.I87E+01 1.8366 0.812E-02 0 260E-04 0.352E-04 0.645E- 1 1 Table XVIII - LEACH TEST DATA - TEST SET C2 - 6 81 TEST C3 - CO-GO TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL CUMULATIVE FRACTION RELEASED LEACHED PERCENT CM INCREMENTAL LEACH RATE CM/DAY MASS LEACH RATE G/CM-»2*0AY DIFFUSION COEFFICIENT CM**2/SEC 1. 0. 108E+01 0.9899 0 451E-02 0 45 IE-02 0.610E-02 0 185E-09 2. 0. 119E+0I 1.0883 0 496E-02 0 448E-03 0.607E-03 0 112E-09 3. 0. 125E*01 1.1436 0 521E-02 0 252E-03 0.341E-03 0 822E-10 4 . 0. 127E*01 1.1666 0 531E-02 0 105E-03 0.141E-03 0 642E-10 5. 0. 128E+01 1.1772 0 536E-02 O 484E-04 0.655E-04 0 523E-10 6 . 0. 130E*01 1.1889 0 542E-02 0 535E-04 0.724E-04 0 444E-10 7 . 0. 131E+01 1 .2000 0 547E-02 0 504E-04 0.682E-04 0 388E-10 14 . 0. 135E*01 1.2378 0 564E-02 0 246E-04 0.333E-04 0 206E-10 21 . 0. 142E+01 1.3043 0 594E-02 0 432E-04 0.585E-04 0 153E-10 28. 0. 145E*01 1.3344 0 608E-02 0 196E-04 0.266E-04 0 120E-10 35 . 0. 149E*0I 1.3652 0 622E-02 0 200E-04 0.27 IE-04 0 100E- 10 42 . 0. 152E*01 1 . 3900 0 633E-02 0 162E-04 0.219E-04 0 868E-11 49. 0. 155E*0I 1.4196 0 647E-02 0 193E-04 0.261E-04 0 776E-11 56. 0 164E*01 1.5077 0 6B7E-02 0 573E-04 0.776E-04 0 766E-11 63. 0 167E+01 1 .5306 0 697E-02 0 149E-04 0. 202E-04 0 702E-11 93 n 171E+01 .1 .5707 0 716E-02 0 609E-05 0.824E-05 . 0 500E-11 Table XIX - LEACH" TEST DATA - TEST SET C3 - 60Co TEST Dl - CO-GO TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT CUMULATIVE FRACTION LEACHED CM INCREMENTAL LEACH RATE CM/OAY MASS LEACH RATE G/CM**2*DAY DIFFUSION COEFFICIENT CM'-2/SEC '• 0. 1 15E+01 1. 1 184 0. 498E-02 0.498E-02 0.672E-02 O.226E-09 2 . 0. I26E+01 1.2206 0. 544E-02 0.455E-03 0.613E-03 0.134E-09 3 . 0. 131E +01 1.27 1 1 0.566E-02 0.225E-03 0.303E-03 O.971E-10 4 . 0.133E+01 1 .2905 0. 575E-02 0.864E-04 0. 1 16E-03 0.751E-10 5. 0. 135E-»01 1.3109 0. 584E-02 0.91 IE-04 0. 123E-03 0.620E-10 6 . 0. 137E+01 1 .3313 0. 593E-02 0.908E-04 0. 122E-03 0.533E-1O 7 . 0. 139E*0t 1 .349 1 0.60 IE-02 O.792E-04 0.107E-03 0.469E-IO 14 . 0. 1-I5C + 01 1.4078 0.627E-02 0.373E-04 0.503E-04 0.255E-10 2 1 . 0. 152E<-01 1 . 4749 0.657E-02 0.427E-04 0.576E-04 0.187E-10 28 . 0. 15GE+01 1 .5 172 0.676E-02 0.269E-04 0.363E-04 0. 148E-10 35. O. 159E+01 1 . 5427 0.687E-02 0. 162E-04 0.219E-04 0. I23E- 10 42 . 0. 1G2E+01 1 .5767 0.702E-02 0.2 16E-04 0.291E-04 0.107E-10 49, 0.I65E+01 1.6065 0.716E-02 0. 190E-04 0. 256E-04 0.950E-( 1 56 . 0. 172E+01 1 .6667 6.742E-02 0.383E-04 0.517E-04 0.895E- 1 1 63 . 0.173E*01 1.6793 O.748E-02 0. 802E-05 0.108E-04 0.807E-11 93 . 0.178E+01 L 7 361 0.769E-02 (XG95E-05 0.937E-05 0.578E- 1 1 Table XX - LEACH TEST DATA" - TEST~ SET D1 - 60Co 82 TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL MASS DIFFUSION TIME DAYS RELEASED MICROCURIES RELEASED PERCENT LEACHED CM LEACH RATE CM/DAY LEACH RATE G/CM*'2*DAY COEFFICIENT CM**2/SEC 1 . 0. 120E*01 1.1558 0.515E-02 0 515E-02 0 697E-02 0 241E-09 2. 0. 135E+01 1.2984 0.579E-02 0 636E-03 0 860E-03 0 152E-09 3. 0. I42E*0I 1.3684 0.610E-02 0 312E-03 0 422E-03 0 113E-09 4 . 0. 145E*01 1.3980 O.623E-02 0 132E-03 0 178E-03 0 8B2E-10 5. 0. 150E+01 1.4386 0.64 IE-02 0 181E-03 0 245E-03 0 747E-10 6 . 0. 153E+01 1.4747 0.657E-02 0 161E-03 0 218E-03 0 655E-10 7 . 0. 155E*01 1.4924 0.665E-02 0 793E-04 0 107E-03 0 575E- 10 14 . 0. 163E*01 1.5681 0.699E-02 0 482E-04 0 65 IE-04 0 317E-10 21 . 0. 17 1E+01 1.6461 0.734E-02 0 497E-04 0 672E-04 0 233E-10 28 . 0. 177E+01 1.6993 0.757E-02 0 339E-04 0 458E-04 0 186E- 10 35. 0. 182E+01 1.7533 0.78 IE-02 0 343E-04 0 465E-04 0 159E-10 42 . 0. 186E+01 1.7920 0.799E-02 0 247E-04 0 334E-04 0 138E- 10 49. 0. I92E*01 1 .8500 0.825E-02 0 369E-04 0 50OE-O4 0 126E-10 56. 0. I96E*0I 1.8852 0.840E-02 0 224E-04 0 303E-04 0 115E-10 63. 0. 198E+01 1.9053 0.849E-02 0 128E-04 0 173E-04 0 104E-10 93. 0. 204E+01 1.9639 0.875E-02 0 870E-05 0 118E-04 0 749E-1 1 Table XXI - LEACH TEST DATA - TEST SET D2 - 6 0Cc TEST D3 - CO-60 TOTAL TIME OAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL CUMULATIVE FRACTION INCREMENTAL RELEASED LEACHED LEACH RATE PERCENT CM CM/DAY MASS LEACH RATE G/CM**2*0AY DIFFUSION COEFFICIENT CM"2/SEC 1 . 0 308E*00 0.3050 0. 135E.-02 0 135E-02 0 182E-02 0 165E-10 2. 0 391E+0O 0.3875 0. 171E-02 0 365E-03 0 491E-03 0 133E- 10 3. 0 432E*00 0.4280 0.189E-02 0 179E-03 0 241E-03 0 iq9E-10 4 . 0 451E+00 0.4470 0.198E-02 0 844E-04 0 114E-03 0 888E-11 5. 0 474E*00 0.4691 0.207E-02 0 977E-04 0 132E-03 0 782E-11 6. 0 499E+00 0.4945 0.219E-02 0 112E-03 0 151E-03 0 724E-11 7 . 0 533E+00 0.5278 0.233E-02 0 147E-03 0 198E-03 0 707E-11 14 . O 638E+00 0.6319 0.279E-02 0 658E-04 0 886E-04 0 507E-11 21 . 0 731E*00 0.7237 0.320E-02 0 580E-04 0 780E-04 0 443E-11 28. 0 807E+00 O.7994 0.353E-02 o 478E-04 0 644E-04 0 406E-11 35. 0 867E*00 0 8585 0.380E-02 0 374E-04 0 503E-04 0 374E-11 42. 0 933E+00 0.9234 0.408E-02 0 409E-04 0 551E-04 0 361E-11 49.. q 103E+01 1.0246 0.453E-02 0 640E-04 0 86 IE-04 0 381E- 11 56. 0 109E+01 1.0835 0.479E-02 0 372E-04 0 50 IE-04 0 373E-11 63. 0 1 13E*01 1.1161 0.494E-02 0 206E-04 0 277E-04 0 351E-11 0. 122E+01 1.2043 0.533E-02 0 130E-04 1 0 175E-04 q 277E-11 Table XXII - LEACH TEST DATA -• TEST SET D3 . 60( 83 TEST A1 - CS-137 TOTAL TIME DAYS TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL RELEASED RELEASED LEACHED LEACH RATE MICROCURIES PERCENT CM CM/DAY MASS LEACH RATE G/CM**2*DAY DIFFUSION COEFFICIENT CM"2/SEC 1 . 0. 2B9E*01 1.5712 0.716E-02 0 .716E-02 ' 0 968E-02 0 .466E-09 2 . 0. 316E*01 1 . 7194 0. 784E-02 0 676E-03 0 913E-03 0 .279E-09 3. 0. 326E+01 1 .7718 0.808E-02 0 .239E-03 0. 323E-03 0 . 198E-09 4 . 0. 332E*01 1.8022 0.82 IE-02 0 .138E-03 0. 187E-03 0 .153E-09 5. 0. 335E+01 1.8205 O.83OE-02 0 831E-04 0. 112E-03 0 . 125E-09 6 . 0. 337E+01 1.8329 0.835E-02 0 567E-04 0. 7G7E-04 0 . 106E-09 7 . 0. 339E+01 1.8427 0.840E-02 0 .448E-04 0. 606E-04 0 916E-10 14 . 0. 347E+01 1.8858 0.860E-02 0 .281E-04 0. 379E-04 0 480E-10 21 . 0. 363E+01 i .9703 0.898E-02 0 550E-04 0. 743E-04 0 349E-10 28. 0. 3B1E*01 2.0730 0.945E-02 0 669E-04 0. 904E-04 0. 290E-10 35. 0. 397E+01 2.1559 0.983E-02 0 540E-04 0. 729E-04 0. 251E-10 42 . 0. 414E*01 2.2477 0.102E-01 0 598E-04 0. 808E-04 0 227E-10 49. 0. 437E+01 2.3738 0.108E-01 0 821E-04 0. 111E-03 0. 217E-10 5G . 0. 463E*01 2.5165 0.115E-01 0 929E-04 0. 126E-03 0. 214E-10* 63. 0. 486E*01 2.64 17 0.120E-01 0. 816E-04 0. 110E-03 0. 209E-10 93. 0. 575E*01 3.1259 0.142E-01 0. 736E-04 0. 994E-04 0. 198E;10. . Table XXIII - LEACH TEST DATA - TEST SET A1 _ 1 3 TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL MASS DIFFUSION TIME RELEASED RELEASED LEACHED LEACH RATE LEACH RATE COEFFICIENT DAYS MICROCURIES PERCENT CM CM/DAY G/CM"2*DAV CM**2/SEC 1 . 0.681E+01 3. 8286 0. 173E-01 0. 173E-01 0. 233E-01 0. 27 IE-08 2. 0.761E+01 •4 , 2732 0. 193E-01 0. 200E-02 0. 270E-02 0. 169E-08 3 . 0.759E+01 4 4310 0. 200E-01 O. 71 IE-03 0. 960E-03 0. 121E-08 4 . 0.803E+01 4 , 5136 0. 203E-01 0. 372E-03 0. 503E-03 0. 940E-09 5. 0.812E+01 4 , 5631 0. 206E-01 0. 223E-03 0. 301E-03 0. 769E-09 6 . 0.818E+01 A .5959 0. 207E-01 0. 148E-03 0. 200E-03 0. 650E-09 7 . 0.825E+01 4 6363 0. 209E-01 0. 182E-03 0. 246E-03 0. 567E-09 14 . 0.858E+01 4 8206 0. 217E-01 0. 119E-03 0. 160E-03 0 307E-09 21 . 0.897E+01 5 .0373 0. 227E-01 0. 140E-03 0. 188E-03 0. 223E-09 28. 0.943E+01 5 . 2976 0. 239E-01 0. 168E-03 0. 226E-03 0. 185E-09 35 . o.anoE+oi 5 .5622 0. 251E-01 0. 170E-03 0. 230E-03 0. 163E-09 42 . 0.105E+02 5 .9154 0 267E-01 0. 227E-03 0. 307E-03 0. 154E-09 49. 0. 1 13E + 02 6 . 3448 0. 286E-01 0. 276E-03 0. 373E-03 0. 152E-09 56. 0.1P2E+02 6 . 8690 0 310E-0I 0. 337E-03 0. 456E-03 0. 156E-09 63 . O, UOE+02 7 . 3066 0. 329E-01 0. 282E-03 0. 380E-03 0. 156E-09 93. 0. 164E+02 9 . 2055 0. 415E-01 0 285E-03 0. 385E--9?. 0. 168E-09. Table XXIV - LEACH TEST DATA -- TEST SET A2 -. 13 7 84 TEST - A3 CS-137 TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT CUMULATIVE FRACTION LEACHED CM INCREMENTAL LEACH RATE CM/DAY MASS LEACH RATE G/CM*'2'DAY DIFFUSION COEFFICIENT CM"2/SEC 1 . 0 .421E+01 2 . 3652 0 .107E-01 0 .107E-01 0 .144E-01 0. 103E-08 2 . 0 .460E+01 2 .5825 0 .116E-01 0 .980E-03 0 .132E-02 0.616E-09 3. 0 . 47SEKM 2 .6685 0 .120E-01 0 .388E-03 0 . 523E-03 0.438E-09 4 . 0 .482E+01 2 .7080 0 .122E-OI 0. 178E-03 0 . 240E -03 0.339E-09 5 . 0 486E+01 2 .7309 0 . 123E-01 0. 103E-03 0 .139E-03 0.275E-09 6. 0 .489E+01 2 . 7490 0 .124E-01 0. 817E-04 0 .110E-03 0.233E-09 7 . 0 492E*01 2 7629 0 .125E-01 0. 627E-04 0. 846E-04 0.201E-O9 14. 0 507E*01 2 .8500 0 .128E-OI 0. 56 IE-04 0. 757E-04 0.107E-09 21 . 0. 530E*01 2 9800 0 .134E-01 0. 837E-04 0. 1 13E-03 0.781E-10 28 . 0. 555E*01 3. 1 178 0. 141E-0I 0. 887E-04 0. 120E-03 0.641E-10 35. 0. 594E+01 3 . 3347 0. 150E-01 0. MOE-03 0. 189E-03 0.587E-10 42 . 0. 667E*01 3. 7482 0. 169E-01 0. 266E-03 0. 359E-03 0.61BE-10 49. 0. 739E*OI 4 . 1528 0. 187E-01 0. 260E-03 0. 352E-03 0.650E-10 56. 0. 811E*01 4. 5547 0. 205E-01 0. 259E-03 0. 349E-03 0.684E-10 63. 0. 8S7E+01 4 . 9819 0. 225E-01 0. 275E-03 0. 37 IE-03 0.727E-10 93. 0. 117E*02 6 . 5802 0. 297E-01 0. 24OE-03 0. 324E-03 0.860E-10 Table XXV -LEACH TEST DATA - TEST SET A3 - 137Cs TEST Bt -CS-137 TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTIPN INCREMENTAL MASS DIFFUSION TIME DAYS RELEASED MICROCURIES RELEASED PERCENT LEACHED CM LEACH RATE CM/DAY LEACH RATE COEFFICIENT G/CM''2'DAY CM"2/SEC 1 . 0. 119E*01 0. 7822 0.331E-02 0. 331E-02 0. 447E-02 0.994E- 10 2 . 0. 144E+01 0.9477 0.4O1E-02 0. 700E-03 0. 945E-03 0.730E-10 3. 0. 159E+01 1.0438 0.44 1E-02 0.406E-03 0. 549E-03 0.590E-10 4 . 0. 169E+01 1.1087 O.469E-02 0. 275E-03 0. 37 IE-03 0.499E-10 5. 0. 17GE+01 1. 1555 0.489E-02 0. 198E-03 0. 267E-03 0.434E-10 6. 0. 182E+01 t.2005 0.508E-02 0.190E-03 0. 257E-03 0.390E-10 7 . 0. 189E+01 1 .2429 0.526E-02 0.180E-03 0. 242E-03 0.359E-10 14. O. 215E+01 1 .4 146 0.598E-02 0.104E-03 0. 140E-03 0.232E-10 21 . 0. 234E+01 1.5392 0.65 IE-02 0. 752E-04 0. 102E-03 0.183E-10 28 . 0-245E+01 1.6123 0.682E-02 0.442E-04 0. 59GE-04 0.151E-10 35 . 0. 253E+01 1 .6633 0.703E-02 0.308E-04 0. 416E-04 0.128E-10 42. 0. 262E+01 1 .7222 0.728E-02 0.356E-04 0. 481E-04 0.115E-10 49. 0. 272E+01 1.7916 0.758E-02 0.4I9E-04 0. 566E-04 0.106E-10 56 . 0. 23'OE+OI 1.8452 0.780E-02 0.324E-04 0. 437E-04 0.968E-11 63. 0-2B6E+01 1.8835 0.796E-02 0.23IE-04 0. 312E-04 0.9I5E-11 93. 0. 303E+01 1.9950 0.844E-02 0.157E-04 0. 212E-04 0.696E-11 Table XXVI - LEACH TEST DATA - TEST SET B1 _ 13 7 85 TEST B2 - CS-137 TOTAL TIME DAYS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT CUMULATIVE FRACTION LEACHEO CM INCREMENTAL LEACH RATE CM/OAY MASS LEACH RATE G/CM»*2"0AY DIFFUSION COEFFICIENT CM"2/SEC 1 . 0. 477E»01 2 . 6815 0. 121E-01 0. 121E-01 0. 163E-01 0. 133E-08 2 . 0. 521E+01 2. 9281 0. 132E-01 0. 1 1 1E-02 0. 150E-O2 0. 7926-09 3. 0. 540E+01 3. 0349 0. 137E-01 0. 48 IE-03 0. 650E-03 0. 567E-09 4 . 0. 552E+01 3. 1039 0. 140E-01 0. 311E-03 0. 420E-O3 0. 445E-09 5 . 0. 557E*01 3 . 1298 0. 141E-01 0. 116E-03 0. 157E-03 0. 362E-09 6 . 0. 563E+01 3 . 1628 0. 143E-01 0. 149E-03 0. 201E-03 0. 308E-09 7 . 0. 5G7E+01 3 1826 0. 143E-01 0. 892E-04 0. 120E-03 0. 267E-09 14 . 0. 587E+01 3 . 2998 0. 149E-01 0. 754E-04 0. 102E-03 0. 144E-09 21 . 0. 604E+01 3 . 3934 0. 153E-01 0. 603E-04 0. 814E-04 0 .101E-09 28 . 0. 624E+01 3 . 5029 0. 158E-01 0. 705E-04 O. 952E-04 0 .809E-10 ',35 • 0. 640E+01 3 .5947 0. 162E-01 0. 591E-04 0. 798E-04 0 .682E-10 42 . 0. 652E+01 3 .6644 0. 165E-01 0. 449E-04 0. 60GE-04 0 .590E-10 49. 0 6G4E+01 3 . 7 307 0. 168E-01 0. 426E-04 0. 576E-04 0 524E- 10 5G. 0 675E+01 3 . 7903 0. 171E-0I 0. 384E-04 0 519E-04 0 .474E-10 63 . 0 6R2E+01 3 .8289 0. 173E-01 0 248E-04 O 335E-04 0 .430E-10 93 . o 7O2E+01 3 .9463 0. 178E-01 0 176E-04 0 238E-04 0 .309E-10 Table XXVII - LEACH TEST DATA - TEST SET B2 1 3 7 TEST B3 - CS-137 TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL MASS DIFFUSION TIME RELEASED RELEASED LEACHED LEACH RATE LEACH RATE COEFFICIENT DAYS MICROCURIES PERCENT CM CM/DAY G/CM«-2-0AY CM»'2/SEC 1. 0 .388E+01 2 .0887 0. 958E-02 0 .958E-02 0 .130E-01 0 .835E-09 2. 0 .435E+01 2 .3396 O. 107E-01 0 . 1 15E-02 0 .156E-02 0 .524E-09 3. O 460E+01 2 .4752 0. 114E-01 0 -622E-03 0 .842E-03 0 .39 IE-09 4 . 0. 469E+01 2 .5195 0. 116E-01 0 .203E-03 0 .275E-03 0 .304E-09 5 . O .471E+01 2 .5336 0. 116E-01 0 .648E-04 0 .877E-04 0 .246E-09 6. 0 475E+01 2 .5538 0. 117E-01 0 925E-04 0 125E-03 0. 208E-09 7 . 0 477E+01 2 .5649 0. 118E-01 0. 510E-04 0. 691E-04 0. 180E-09 14 . 0 493E+01 2 .6480 0. 121E-01 0. 545E-04 0. 737E-04 0. 958E-10 2 1 . 0 507E+01 2 .7252 0. 125E-01 0. 506E-04 O. 685E-04 0. 677E- 10 28. 0. 519E+01 2 .7886 0. 128E-01 0. 415E-04 0. 562E-04 0. 531E-10 35. 0. 526E+01 2 .8272 0. I30E-01 0. 253E-04 0. 342E-04 0. 437E- 10 42. 0. 541E+01 2 9089 0. 133E-01 0. 535E-04 0. 724E-04 0. 385E-10 49. 0. 550E+01 2. 9581 0. 136E-01 0. 323E-04 0. 437E-04 0. 342E-10 56. 0. S74E+01 3 0841 0. 141E-01 0. 826E-04 0. 112E-03 0. 325E- 10 63. 0. 585E+01 3 1428 0. I44E-01 0. 384E-04 0. 520E-04 0. 300E- 10 93. 0. 621E+01 3. 3376 0. I53E-01 0. 298E-04 _ .0. 403E-04 0. 229E-10 Table XXVIII - LEACH TEST DATA - TEST SET B3 - 137 86 TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL MASS DIFFUSION TIME DAYS RELEASED MICROCURIES RELEASED PERCENT LEACHED CM LEACH RATE CM/DAY LEACH RATE G/CM*«2*DAY COEFFICIENT CM"2/SEC 1 . 0.290E>01 1.6936 0.752E-02 O 752E-02 0 I02E-0I 0.514E-O9 2 . 0.310E+01 1.81 12 0.804E-02 0 522E-03 0 705E-03 0.294E-09 3 . 0.320E*01 1.8719 0.83 IE-02 0 269E-03 0 364E-03 0.209E-09 4 . 0.324E+01 1.8951 0.84 IE-02 0 103E-03 0 140E-03 0.161E-09 5. 0.326E*01 1.9091 0.847E-02 0 621E-04 0 838E-04 0.131E-09 6 . 0.328E+01 1.9167 0.B51E-02 0 336E-04 0 454E-04 0. 1 10E-09 7 . 0. 329E+-01 1.9248 O.854E-02 0 359E-04 0 485E-04 0.948E-10 14 . 0. 335E*01 1.9610 0.870E-02 0 230E-04 0 310E-04 0.492E-10 2.1 . 0. 346E+01 2.0226 0.898E-02 0 39 IE-04 0 528E-04 0.349E-10 28. 0.354E*01 2.0700 0.919E-02 0 300E-04 0 406E-04 0.274E- 10 35. 0.360E+01 2.1065 0.935E-02 0 231E-04 0 312E-04 O.227E-10 42 . 0.368E+01 2.1524 0.955E-02 0 29 IE-04 0 394E-04 0.198E-10 49. 0.376E+01 2.2013 0.977E-O2 0 310E-04 0 419E-04 0.177E-10 56. 0. 387E+01 2 . 2628 0.100E-01 0 390E-04 0 526E-04 0.164E- 10 63. 0.397E+01 2.3199 0.103E-01 0 362E-04 0 489E-04 0.153E-10 93. 0.414E+01 Table XXIX 2.4199 - LEACH 0.107E-01 TEST DATA 0 148E-04 TEST 0.200E-04 SET Cl 0.113E-10 _ 13 7 TEST"C2 - CS-137"" • - • TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL MASS DIFFUSION TIME RELEASED RELEASED LEACHED LEACH RATE LEACH RATE COEFFICIENT DAYS MICROCURIES PERCENT CM CM/DAY G/CM**2*DAY CM-*2/SEC 1 . 0.103E+01 0.6035 0. 267E-02 0.267E-02 0.36 IE-02 0.647E-10 2 . 0.120E*01 0.704 7 0. 312E-02 0.447E-03 0.605E-03 0.441E-10 3. 0.130E+O1 0.7674 0.339E-02 0.277E-03 0. 375E-03 0.349E-10 4 . 0.t36E+01 0.7986 0.353E-02 0. 138E-03 0. 187E-03 0.283E-1O 5. 0.139E*01 0.8204 0.363E-02 0.963E-04 0. 130E-03 0.239E-10 6 . 0.143E+0I 0.84 19 0.372E-02 0.948E-04 0. 128E-03 0.210E-10 7 . 0.146E+01 O.8577 0.379E-02 0.7OOE-04 0.948E-04 0.187E-10 14 . 0.160E+01 0.9394 0.415E-02 0.516E-04 0.698E-04 0.112E-10 21 . 0.172E+01 1.0129 0. 448E-02 0.464E-04 0.628E-04 0.868E-11 28 . 0.182E+01 1.0721 0.474E-02 0.374E-04 0.506E-04 0.730E-11 35. 0.192E+01 1 . 1297 O.5OOE-02 0.364E-04 0.493E-04 0.648E-11 42 . 0.199E+01 1.17 11 0. 5 18E-02 0.262E-04 0.354E-04 0.580E-11 49 . 0.213E+01 1.2509 0.553E-O2 O.504E-O4 0.681E-04 0.568E-11 56. 0.233E*01 1 .37 13 0.606E-02 0.761E-04 0.103E-O3 0.597E- 1 1 63 . 0. 240E+01 1.4110 0.624E-02 0.250E-04 0.339E-04 0.562E- 1 1 93 . 0. 2T!8E*01 1 .5158 0.670E-02 0. 155E-04 0.209E-04 0.439E-1 1 Table XXX - LEACH TEST DATA -"TEST SET C2 _ 1 3 7 Q 87 TEST C3 - CS-137 TOTAL TIME OAVS TOTAL ACTIVITY RELEASED MICROCURIES FRACTIONAL RELEASED PERCENT CUMULATIVE FRACTION LEACHED CM INCREMENTAL LEACH RATE CM/DAY MASS LEACH RATE G/CM""2'DAY DIFFUSION COEFFICIENT CM**2/SEC 1 . 0. 288E+01 1.5732 0. 717E-02 0. 717E-02 0.970E-02 0. 467E-09 2. 0. 3 I7E+01 1.7305 0. 788E-02 0. 716E-03 0.970E-03 0. 282E-09 3. 0. 331E+01 1 .8105 0. 825E-02 0. 364E-03 0.493E-03 0. 206E-09 4. 0. 336E+01 1 .8379 0. 837E-02 0. 125E-03 0.169E-03 0. 159E-09 5. 0. 339E+01 1.8500 0. 843E-02 0. 551E-04 0.746E-04 0. 129E-09 6 . 0. 34IE+01 1.8631 0. 849E-02 0. 597E-04 0.809E -04 0. 109E-09 7 . 0. 343E+01 1.8767 0. 855E-02 0. 62 IE-04 0.84IE-04 0. 949E-10 14 . 0. 353E+01 1.9314 0. 880E-02 0. 355E-04 0.48 IE-04 0. 503E-10 21 . 0. 370E+01 2.0239 0. 922E-02 0. 6O2E-04 0.8I5E-04. 0. 368E-10 28. 0. 377E+01 2.0611 0 .939E-02 O .242E-04 0.328E-04 0 .286E-10 35 . 0. 3B5E+01 2.1038 0 .958E-02 0 .278E-04 0.376E-04 0 239E-10 42 . 0. 39 IE+01 2.1374 0 .974E-02 0 .219E-04 0.296E-O4 0 .205E-10 49. 0. 399E+01 2.1803 0 .993E-02 0 .279E-04 0.377E-04 0 .1B3E-10 56. 0 420E+01 2.2976 0 .105E-01 0 .764E-04 0.103E-03 0 .178E-10 63 . 0 427E+01 2.3319 0 .106E-01 0 .223E-04 O.302E-O4 0 . 163E- 10 93. 0 .438E+01 2.394 1 0 .109E-01 O .944E-05 0.128E-04 0 .11GE-10 Table XXXI - LEACH TEST DATA - TEST SET C3 _ 13 7 Cs TEST 01 - CS-137 TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL MASS DIFFUSION TIME RELEASEO RELEASED LEACHED LEACH RATE LEACH RATE COEFFICIENT DAYS MICROCURIES PERCENT CM CM/DAY G/CM"2'DAY CM"2/SEC 1. 0.3 1 IE + 01 1 .8064 0.805E-02 0. 805E-02 0. 108E-01 0. 588E-09 2 . 0.34 IE+01 1 .9822 0.883E-02 0. 783E-03 0. 106E-02 0. 354E-09 3 . 0.356E+01 2 .07 13 0.923E-02 0. 397E-03 0. 535E-03 0. 258E-09 4 . 0.363E+01 2 . 1131 0.94 IE-02 0. 186E-03 0. 25 IE-03 0. 20 IE-09 5. 0.369E+01 2 . 1463 0.956E-O2 0. 148E-03 0. 200E-03 0. 166E-09 6 . 0.372E+01 2 . 1644 0.964E-02 0. 803E-04 0. 108E-03 0. 141E-09 7 . 0.375E+01 2 . 1822 0.972E-02 0. 793E-04 0. 107E-03 0. 123E-09 14 . 0.3B9E+01 2 .2614 0.101E-01 0. 504E-04 0. 680E-04 0. 659E- 10 21 . 0.403E+01 2 . 3456 0.104E-01 0. 536E-04 0. 722E-04 0. 472E- 10 28 . 0.413E+01 2 .4003 0.107E-01 0. 348E-04 0. 469E-04 o. 371E-10 35. 0.420E+01 2 .4398 0.109E-01 0. 251E-04 0. 339E-04 0. 307E-10 42. 0.427E+01 2 .4851 0. 1 11E-01 0. 288E-04 0. 389E-04 0 265E-10 49. 0.435E+01 2 .5276 0.113E-01 0. 271E-04 0. 365E-04 0. 235E-10 56. 0.449E+01 2 .6091 0. 1 16E-01 0. 518E-04 0. 699E-04 0. 219E-10 63. 0.452E+01 2 .6254 0.117E-01 0. 104E-04 0. 140E-04 0. 197E-10 93 . 0^461E+01 2 .6796 0.119E-0I 0. 805E-05 0. 109E-04 0. 139E- 10 Table XXXII - LEACH TEST DATA - TEST SET D1 _ 1 3 yCs 88 TOTAL TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL TIME RELEASED RELEASED LEACHED LEACH RATE LEACH RATE COEFFICIENT OAYS MICROCURIES PERCENT CM CM/DAY G/CM«*2'DAY CM"2/SEC . 1 . 0 3G8E+01 2 1138 0 942E-02 0 942E-02 0 127E-01 0 807E-09 2 . 0 4 1 1E*01 2 3629 0 105E-01 0 111E-02 . 0 150E-02 0 504E-09 3. 0 434E+01 2 4947 0 111E-01 0 587E-03 0 794E-03 0 375E-09 4 . 0 44SE+01 2 5577 0 114E-01 0 281E-03 0 380E-03 0 295E-09 5. 0 456E+01 2 6 ISO 0 117E-01 0 269E-03 0 363E-03 0 248E-09 6. 0 4S0E+01 2 6447 0 118E-01 0 119E-03 0 161E-03 0 21 1E-09 7 . 0 464E+01' 2 6665 0 119E-01 0 971E-04 0 131E-03 0 183E-09 14. 0 484E+01 2 7815 0 124E-01 0 732E-04 0 990E -04 0 998E-10 21 . 0 505E+01- 2 9004 0 129E-01 0 757E-04 0 102E-O3 0 723E-10 26. 0 517E+01 2 9691 0 132E-01 0 437E-04 0 59 IE-04 0 569E- 10 35. 0 530E+01 3 0436 0 136E-01 0 474E-04 0 64 IE-04 0 478E-10 42 . 0 539E+01 3 0973 0 138E-01 0 342E-04 0 463E-04 0 412E-10 49. 0 553E+01 3 1764 0 142E-01 0 504E-04 0 682E-04 0 372E-10 56. 0 BSOE+OI 3 2207 0 144E7OI 0 282E-04 0 382E-04 0 335E- IO 63 . 0 5R5F.*01 3 2468 0 145E-01 0 166E-04 0 224E-04 0 302E-10 93. 0 5nOE*-01 3 3314 0 I48E-01 0 126E-04 0 170E-04 0 216E-10 Table XXXIII - LEACH TEST DATA - TEST SET D2 - 1 TEST D3 - CS-137 TOTAL TIME DAYS TOTAL ACTIVITY FRACTIONAL CUMULATIVE FRACTION INCREMENTAL RELEASED RELEASED LEACHED LEACH RATE MICROCURIES PERCENT CM CM/DAY MASS LEACH RATE G/CM"2'0AY DIFFUSION COEFFICIENT CM*»2/SEC 1 . 0 111E*01 0.6547 0.290E-02 0 290E-02 0 390E-02 0 762E-10 2. 0 136E*01 0.8022 0.355E-02 0 652E-03 O 878E-03 0 572E- 10 3. 0 14BE*0I 0.8709 0.385E-02 0 304E-03 0 409E-03 0 449E-10 4. 0 154E+01 0.9087 0.402E-02 0 167E-03 0 225E-03 6 367E-10 5 . 0 160E*01 0.9405 0.416E-02 0 141E-03 0 189E-03 0 314E-10 6. 0 164E+01 0.9647 0.427E-02 0 107E-03 0 145E-03 0 276E-10 7 . 0 I70E*01 1.0014 0.443E-02 0 162E-03 0 219E-03 0 255E-10 14 . 0 195E*01 t.1450 0.506E-02 0 907E-04 0 122E-03 0 166E-10 21 . 0 214E*01 1.2616 0.558E-02 0 736E-04 0 991E-04 0 135E-10 28 . 0 230E+01 1.3550 0.599E-02 0 590E-04 0 795E-04 0 117E-10 35. 0 243E*01 1.4309 0.633E-02 0 479E-04 0 645E-04 0 104E-10 42 . 0 25GE*01 1.5071 0.666E-02 0 482E-04 0 648E-04 0 961E-11 49. 0 278E+01 1.6351 0. 723E-02 0 808E-04 0 109E-03 0 970E-11 56. 0 289E*01 1.6986 0.751E-02 0 40 IE-04 0 540E-04 0 916E-11 63. 0 295E*01 1.7377 0.76BE-02 0 247E-04 0 333E-04 0 852E-11 0 313E+01 1.8440 0.815E-02 0 157E-04 0 211E-04 0 650E-11 Table XXXIV - LEACH TEST DATA - TEST SET D3 _ 13 7 89 APPENDIX D - LEACHANT CONDUCTIVITY AND PH Initial Final 1 Week's contact Set A pH 4.10 5.80 Conductivity 1.00 X lO-6Mho/cm 4.90 X 10""Mho/cm Set B pH 6.39 6.25 Conductivity 4.80 X l0"3Mho/cm 6.5 X l0-3Mho/cm Set C pH 6.39 5.65 Conductivity 4.80 X lO"3Mho/cm 5.5 X 10-3Mho/cm Set D ph 5.62 4.99 Conductivity 1.85 X lO-2Mho/cm 1.95 X 10"2Mho/cm 90 APPENDIX E - ANALYSIS OF VARIANCE OF 60Co AND 137Cs~SAMPLE MEANS AT T>14DAYS e o Co: Set Mean St Deviation St Error 95% Confidence Interval for Mean A B C D 0.0083 0.0087 0.0064 0.0064 0, 0. 0. 0, 0050 0018 0013 0018 0.0010 0.0003 0.0003 0.0003 0.0064 0.0080 0.0059 0.0057 0.0103 0.0094 0.0070 0.0071 F Ratio=4.856 Homogenous subsets: Subset 1 Group Set D Set C Mean 0.0064 0.0064 Subset 2 Group Set A Set B. Mean 0.0083 0.0087 1 3 7 Set A B C D Cs:  Mean 0.0190 0.0124 0.0083 0.0105 St Deviation St Error 95% Confidence Interval for Mean 0.0087 0.0040 0.0022 0.0031 0.0017 0.0008 0.0004 0.0006 0.0156 0.0108 0.0074 0.0093 0.0225 0.0140 0.0092 0.01.1 7 F Ratio=21.756 Homogenous Subsets: Subset 1 Group Mean Set C 0.0083 Set D 0.0105 Subset Group Mean Set D 0.0105 Set B 0.0124 Subset Group Mean Set A 0.0190 

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