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

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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 U n i v e r s i t y Of A l b e r t a , 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 C i v i l E n g i n e e r i n g  We accept t h i s t h e s i s as conforming t o the r e q u i r e d  standard  THE UNIVERSITY OF BRITISH COLUMBIA October  ©  1982  Bruce C l e l l a n d C l e g g , 1982  In  presenting  this  requirements  for  British  Columbia,  freely  available  that  permission  scholarly or  by  copying not  be  or  for  may  her  be  15  October  granted  by  this  thesis  my  written  Columbia  the  Library  and  Engineering  1979  at  study.  copying  of  The U n i v e r s i t y of B r i t i s h 2 0 7 5 Wesbrook P l a c e Vancouver, Canada V6T 1W5  Date:  the  representatives.  without  fulfilment  degree  that  extensive  Civil  partial  reference  publication  of  in  advanced  I agree  for  or  allowed  Department  an  purposes  his  thesis  of  the  'It for  of  make  further  this  Head  thesis my  of it  agree for  Department  i s understood  f i n a n c i a l gain  permission.  the  University  shall I  of  that shall  Abstract L o n g - t e r m management o f n u c l e a r physical until long on  isolation  the order Past  research  Due t o t h e e x t r e m e l y  the required  i s o l a t i o n may be  on t h e  m e c h a n i s m s t h a t may e f f e c t a p r e m a t u r e  return  to  the  environment.  However,  biological  i n a r a d w a s t e d i s p o s a l s i t e may h a v e two m a j o r  solubilization radionuclides of v a r i o u s  or  of  the  oxidation;  through  chelating  solidifying  6 0  Co  and  1 3 7  Cs  culture  under  m e d i a by  agents.  presented  The  work  encapsulated  released  their ability  t o bind  compare  action,  by  idealized  radionuclides  matrix  (adsorbent) geologic  undergo m i c r o b i a l a t t a c k  experiments  a  selected  irradiation.  here  is  to  hydrocarbonoclastic  environmental  conditions.  The  by t h i s p r o c e s s were t h e n e v a l u a t e d f o r with  selected geologic  hydrocarbonoclastic also  production  i n b i t u m e n was a l l o w e d  the e f f e c t of reduced adsorption  was  through  processes.  media.  tested  culture for  In  order  due t o m i c r o b i a l  s y n t h e t i c c h e l a t i n g a g e n t s were u s e d a s  same  effects:  a n d / o r 2) e n h a n c e d movement o f  f o c u s e d on b o t h t h e s e m i c r o b i o l o g i c a l  The  from t h e b i o s p h e r e  on r a d i o a c t i v e w a s t e s h a s c e n t e r e d  1) p h y s i c a l d e s t r u c t i o n  to  absolute  of m i l l e n n i a .  radionuclides  action  l e v e l s has occurred.  o f some i s o t o p e s ,  physicochemical of  demands  of noxious r a d i o n u c l i d e s  decay t o safe half-life  wastes  used  a  standard. for  i t s sensitivity  to  these y-  iii  Subsequent did  analysis  m i c r o b i a l a t t a c k of bitumen  not enhance the r e l e a s e of the i o n s .  a d s o r p t i o n t o the g e o l o g i c was  showed  much  agents.  media was observed but  the  l e s s than t h a t observed f o r the s y n t h e t i c  will  not  effect  the  effect  chelating  The l e v e l of r - r a d i a t i o n e x p e c t e d i n the f i n a l  repository tested.  However, a d e c r e a s e d  waste  v i a b i l i t y of the organisms  Table  of  Contents  Abstract i i L i s t of Tables ... v i L i s t of Figures v i i Acknowledgement viii I. INTRODUCTION 1 1. ' BACKGROUND 1 2. T H E CHALK R I V E R NUCLEAR L A B O R A T O R I E S ' LOW AND I N T E R M E D I A T E L E V E L WASTE PROGRAM 2 A. T R E A T M E N T AND D I S P O S A L OF LOW AND I N T E R M E D I A T E L E V E L WASTES 4 i. Volume R e d u c t i o n 4 i i . Immobilization 4 i i i . Ultimate Disposal 6 iv. Natural Barriers 6 3. M I C R O B I A L A N T A G O N I S A T I O N OF RADWASTE I S O L A T I O N ...7 A. M I C R O B I A L A C T I V I T Y AND L E A C H I N G 7 B. M I C R O B I A L A C T I V I T Y AND S U B S U R F A C E N U C L I D E MOVEMENT 8 4. S C O P E OF T H I S WORK 9 II. M I C R O B I A L DEGRADATION OF B I T U M E N 10 1. BACKGROUND 10 A. ALIPHATICS 11 B. AROMATICS 12 C. P O L Y C Y C L I C AROMATIC HYDROCARBONS 13 2. R E P R E S E N T A T I V E HYDROCARBONOCLASTIC BACTERIA 14 3. C O N D I T I O N S FOR GROWTH AND P R E L I M I N A R Y IDENTIFICATION 15 A. GROWTH C O N D I T I O N S 15 B. IDENTIFICATION 16 C. GROWTH CURVES 16 4. S E L E C T I O N OF A S U I T A B L E C U L T U R E AND GROUNDWATER .17 A. S E L E C T I O N OF A S U I T A B L E C U L T U R E 17 B. S E L E C T I O N OF A S U I T A B L E GROUNDWATER S O L U T I O N .22 REMARKS 23 III. MICROBIAL RADIOSENSITIVITY 24 1. BACKGROUND 24 2. METHODS 25 A. GROWTH MEDIA P R E P A R A T I O N 25 B. C E L L PREPARATION 25 C. I R R A D I A T I O N AND ENUMERATION 26 3. RESULTS 27 IV. E V A L U A T I O N OF M I C R O B I A L L Y ENHANCED L E A C H I N G 31 1. ENHANCED L E A C H I N G 32 2. METHODS 44 A. ANALYSIS 46 3. R E S U L T S AND D I S C U S S I O N 47 A. S T A T I S T I C A L EVALUATION 47  V  B. CONCLUSION E F F E C T OF C H E L A T I N G A G E N T S  V. 1. 2. 3. 4. 5.  BACKGROUND METHODS ANALYSIS R E S U L T S AND REMARKS VI. CONCLUSION BIBLIOGRAPHY A P P E N D I X A - ONTARIO  49 ON  RADIONUCLIDE  MIGRATION 50 50 53 54 56 61 62 65  DISCUSSION  MINISTRY  OF  T H E ENVIRONMENT  A P P E N D I X B - S Y N T H E T I C GROUNDWATER S O L U T I O N S A P P E N D I X C - L E A C H T E S T DATA A P P E N D I X D - L E A C H A N T C O N D U C T I V I T Y AND PH A P P E N D I X E - A N A L Y S I S OF V A R I A N C E OF C o AND SAMPLE MEANS A T T>14DAYS 6 0  ANALYSIS 71 73 77 89  1 3 7  Cs~ 90  List  I. II. III. IV. V. VI. VII.  of Tables  MICROBIAL MINERAL SALTS SOLUTION 15 y - I R R A D I A T I O N T I M E S USED FOR C U L T U R E S A , B , C AND D ..27 C o A D S O R P T I O N DATA 56 C s A D S O R P T I O N DATA 57 S r A D S O R P T I O N DATA 57 C O M P E T I N G ION A D S O R P T I O N DATA 58 A D S O R P T I O N DATA FOR C O M P E T I N G IONS I N S E L E C T E D GROUNDWATERS 58 L E A C H A N T A A D S O R P T I O N DATA 59 A D S O R P T I O N DATA FOR N U T R I E N T MEDIA CONTROL 59 L E A C H A N T D A D S O R P T I O N DATA 60 L E A C H T E S T DATA - T E S T S E T A1 Co 77 L E A C H T E S T DATA - T E S T S E T A2 Co 77 L E A C H T E S T DATA - T E S T S E T A3 Co 78 L E A C H T E S T DATA - T E S T S E T B1 Co -...78 L E A C H T E S T DATA - T E S T S E T B2 Co 79 L E A C H T E S T DATA - T E S T S E T B3 Co 79 L E A C H T E S T DATA - T E S T S E T C l Co 80  6 0  1  3  8  5  VIII. IX. X. XI. XII. XIII. XIV. XV. XVI. XVII. XVIII.  7  6 0  6 0  6 0  6 0  6 0  6 0  6 0  LEACH LEACH LEACH LEACH LEACH  T E S T DATA T E S T DATA T E S T DATA T E S T DATA T E S T DATA  -  TEST TEST TEST TEST TEST  SET SET SET SET SET  C2 C3 D1 D2 D3  -  LEACH LEACH LEACH LEACH  TEST TEST TEST TEST  DATA DATA DATA DATA  -  TEST TEST TEST TEST  SET SET SET SET  A1 A2 A3 B1  -  1  3  7  1  3  7  1  3  7  1  3  7  LEACH TEST XXVI11. LEACH TEST XXIX. LEACH TEST XXX. L E A C H T E S T XXXI. LEACH TEST XXXII. LEACH TEST XXXIII. LEACH TEST XXXIV. LEACH TEST  DATA  - TEST  S E T B2 -  1  3  7  XIX. XX. XXI. XXII. XXIII. XXIV. XXV. XXVI. XXVII.  :  DATA DATA DATA DATA -  T E S T S E T B3 T E S T S E T C1 T E S T S E T C2 T E S T S E T C3  -  Co Co Co Co Co  6 0  6 0  6 0  6 0  6 0  1  s s s s  83 83 84 84  Cs  85  Cs Cs Cs Cs  85 86 86 87  1  3  7  1  3  7  3  7  1  3  7  C C C C  80 81 81 82 82  DATA  - TEST  S E T D1  -  1  3  7  Cs  87  DATA  - TEST  S E T D2 -  1  3  7  Cs  88  DATA  - TEST  S E T D3 -  1  3  7  Cs  88  vii  List  1. 2. 3. 4. 5. 6. 7. 8. 9. 10. 11. 12. 13. 14. 15. 16. 17. 18. 19. 20. 21. 22. 23. 24. 25. 26.  of  C u l t u r e A - 11 H o u r G r o w t h Culture A - Standard Curve C u l t u r e B - 12 H o u r G r o w t h Culture B - Standard Curve C u l t u r e C - 12 H o u r G r o w t h Culture C - Standard Curve C u l t u r e D - 12 H o u r G r o w t h Culture D - Standard Curve Dose-Response of C u l t u r e A Dose-Response of C u l t u r e B Dose-Response of C u l t u r e C Dose-Response of C u l t u r e D Leaching p r o f i l e s for sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets Leaching p r o f i l e s f o r sets  Figures  Curve Curve Curve Curve  A1,B1,C1 a n d A1,B1,C1 a n d A2,B2,C2 a n d A2 B2,C2 and A3,B3,C3 and A3,B3,C3 and A 1 , A 2 a n d A3 A1,A2 a n d . A 3 B1,B2 a n d B3 B1,B2 a n d B3 C 1 , C 2 a n d C3 C 1 , C 2 a n d C3 D1,D2 a n d D3 D1,D2 a n d D3 f  D1 D1 D2 D2 D3 D3 •.-  18 18 19 19 20 20 21 21 29 29 30 30 C o ....35 Cs ...35 C o ....36 Cs ...36 Co ....37 Cs ...37 Co 38 Cs 38 Co '.39 Cs 39 Co 40 Cs 40 Co 41 Cs 41 6 0  1  3  7  6 0  1  3  7  6 0  1  6 0  1  3  6 0  1  3  6 0  1  3  6 0  1  3  7  7  7  7  3  7  I  viii  Ac k n o w l e d g e m e n t  It  i s with  thank the  sincere  the  Chalk  engineers, River  suggestions, has  Champ space.  the  Mr.Leo  Buckley  in  l a b were  the  thesis.  Dr.'s  I would  who's an  and  use like  expert  and I  Norman  generous  However,  I  would  of to  Their  general would  Gentner their thank  suggestions  inspiration.  like  to  t e c h n i c i a n s of  Laboratories.  criticisms  in this  in particular for  scientists  Nuclear  helpful  culminated  thank  gratitude that  support like  and time  kind  to  Douglas and  lab  especially, and  weekends  1  I.  1.  BACKGROUND Full  scale  culminated CANDU*  in  This  commercial  a  energy  pressurized  is  one  markets.  characterized oxide  atomic  reactor,  achievements,  one of  research heavy  of  vessel  three  replacement reactor types.  reactors;  during  great  operation).  Because of i t s neutron  as  the  * CANada D u e t e r i u m U r a n i u m . * * L i g h t Water R e a c t o r  has  known a s technical  designs  on  world  design 2)  deuterium  3)  a  multiple  fueling  pressure  (fuel  bundle  The c o m m e r c i a l  efficiency  than  the  economy t h e CANDU r e a c t o r  adaptable thorium  to  fuel  is  uranium;  of a s i n g l e l a r g e  a n d 4 ) on power  uses uranium w i t h g r e a t e r  such  reactor  and c o o l a n t ;  instead  reactor  the advantage of being  cycles,  reactor  Canada  The u n i q u e n e s s o f t h e r e a c t o r  tube c o n f i g u r a t i o n  of other  water  t h e use o f 1 ) n a t u r a l  by  in  Canada's  (heavy w a t e r ) a s m o d e r a t o r  pressure  has  INTRODUCTION  more cycle  efficient without  power LWR** also fuel major  2  modification  of  possible  operate  reactor least thus  to  the  comparable  three  times  existing at  or  to the as  the a v a i l a b l e  near  fast  abundant  nuclear  design.  This  breeding,  breeder  making  reactor.  in the earth's  fuel  means  resource  the  be  as  is  CANDU  Thorium.is  crust  would  i t  at  uranium  considerably  increased. If  this  reprocessing contained will  i n the  management  or  to  sold.  filled spent  will  be  has  THE  LEVEL  and  y e t been  the  free  fuel  power  most  disposal  been  stored  either  immobilized likely  structures  The  and  i n mined  in  fate i t  abroad water of  will  disposed, cavities  abundantly  waste  options.  processed  stations. but  products  Canadian  either  a  materials  fission  The  has  decided,  residues  intact,  separated  was  require  fissile  to evaluate  fuel  spent  will  located  the be  or i t within i n the  Shield.  CHALK  WASTE  Along generated The  not  mineral  Canadian  the  recover  The  1  initiated  the nuclear  disposed  granitic  2.  then,  at  reprocessed  was  to  Canada  disposal.  a l l irradiated  Since  fuels  fuels.  permanent  program  bays  embraced,  i n order  spent  safe  1971  2  is  facility  require  Prior  cycle  broad  RIVER  NUCLEAR  LABORATORIES'  LOW  AND  INTERMEDIATE  PROGRAM  with from  the high daily  categories  level  operation including  wastes of  are  less  the nuclear  a l l low  and  active power  wastes  reactors.  intermediate  level  3  radwastes  encompass  radioactivity. volume Some  and of  are  intermediate much  greater 2)  size;  a  containing tritium  Unfortunately,  3  the  0.1%  only  chemically  various level  than  to  with  of system  be  t h e major  level  are associated  total  sources  heterogenous.  Canada's  low  the production smaller  integrity  activation  more  of  minimizes  low  than  1 4  C i s core  losses 3)  and  in  and  and  LWR  products;  abundant  o f CANDU  "waste"  are substantial in  d u e t o t h e much  Furthermore, wastes  wastes  1)  are:  and neutron  appears  the  and r a d i o l o g i c a l l y  wastes  degree  fission  these  differences  i n a LWR  high  of  LWR's.  intermediate  with:  1)  Routine  2)  P u r i f i c a t i o n i n heavy and l i g h t water c i r c u i t s ( t h e m a j o r i t y o f t h e r a d i o i s o t o p e s a r e c o n t a i n e d on s p e n t ion-exchange r e s i n s and f i l t e r s c o n t a i n i n g Co, C s and "C ( p r e s e n t as a c a r b o n a t e on i o n exchange r e s i n s ) . Equipment decontamination.  operation  4  and maintenance.  6 0  1  3)  3  7  1  5  The  ultimate  multiple  barrier  breach  series  a  biosphere. and  treatment  disposal  system  i n which  of o b s t a c l e s  These steps  of  6  radwastes a waste  prior  obstacles  include  discussed  below.  to  will  nuclide  incorporate would  recontact  a number  of  a  have t o  with  the  pretreatment  4  A.  T R E A T M E N T AND  DISPOSAL  OF  LOW  AND  INTERMEDIATE  LEVEL  WASTES  i.  Volume  All  wastes  incinerated Nuclear (AECL)  that  to  Power at  Reduction  Liquid  as  stable  and  Chalk  River  operating  for  wates  undergo  may  incinerable  ash.  Development)  the  incinerators  a  occur  Both  Atomic  Nuclear this  solids  Ontario  Energy  of  will  Hydro Canada  Laboratory  be  (Bruce Limited  (CRNL)  have  purpose. a  two-step  procedure  for  volume  excluding  water  reduct ion: 1) 2)  Reverse  through  a  reduction  been  osmosis  may  achieved  The production been  concentrates  semipermeable utilize  increase  i i.  have  and  Evaporation.  Reverse  further  osmosis;  the  with  a  membrane. vertical  percentage  some  solids  of  wastes).  by  A  second  thin-film total  step  in  volume  evaporator  solids  (up  to  to  6  50%  has  7  Immobilization  ultimate of used  formaldehyde, low  a  aim  durable as  a  CRNL's  and  its  versatility,  immobilization  leach-resistant  solidifying  polyester  by  of  and  bitumen.  intermediate  volume  matrix  savings  8  level and  of  solid. include  The  is  Compounds cement,  selection  waste  leach  radwastes  program  of was  resistance  the that  ureabitumen due  to  (highest  5  of  those  materials  Bitumen  mentioned). . 9  is  chemically  components  may  saturated  hydrocarbons,  asphaltenes.  be  grouped  Other  1 0  oxygen(1 - 1 7 % ) ,  as  a  complex  been  used  to  caulk  boats  in  the  third  millenium B.C.  as  a  to  the  the  solidifying Research  Plutonium  Belgium scale)  from  to  by by  for  1965.  CRNL's  1982.  incineration bitumenization.  This or  water 1 3  Centre  The  Waste  reverse  At  1  and are room  be  described  building  materials  wastes  Energy of  may  brick  and  be  at Mol,  Marcoule,  walls bitumen  attributed  Belgium France.  operated  (on a  installation bitumen  pilot  projects.  scale  will  osmosis  Centre  utilize and  (WTC)  volume  evaporation,  and The small  started  experience with  Treatment  complex  1  e s t a b l i s h m e n t of  the Marcoule  and  may  s t o p between  constructed  Canadian  present  nitrogen(1 % ) .  for nuclear  while  laboratory of  a  be  state  i t s  categories:  hydrocarbons  may  cement  for Nuclear  Research  1960-1964 in  completion slated  Centre  e s t a b l i s h m e n t was  operation limited  matrix  as  but  1 2  (Babylon), the  or  that  physical  system.  broad  cyclic  and/or  bitumen's  has  heterogenous  four  resins,  elements  colloidal  Bitumen  into  sulfur(1-9%)  temperature(20-25°)  very  has  has  been The been  reduction followed  6  iii.  Ultimate  In o r d e r from c o n t a c t have  to ensure p h y s i c a l with  decayed  rock  on  the  biosphere  to acceptable  subterranean. located  Disposal  The the  formation  final  isolation (until  limits)  waste  a  Some  for  "relatively  homogeneous s t r u c t u r e s of h i g h  times  and  iv.  Natural  Although the  of  the  through  the  in  a may of  the  repository  the  accordance management. leached  If  that they  are:  and  long  geologic  1  groundwater  and  with  the  t h e p a s s a g e of  given  leached  strong  to  siting  inactive  zone,  does o c c u r  f l o w may  be  concomitant  subsurface  In  r a d i o n u c l i d e s out  of  environment.  method  nuclide attenuation w i l l  be  twofold:  environment.  may  This  be  used  to  is  in  approach to nuclear  adsorbent  the  movement  o c c u r r i n g adsorbents  the m u l t i p l e - b a r r i e r a  be  If i n t r u s i o n  waste  repository  with  hard  years". "  occur.  repository, naturally  backfill  be  obvious  since early  hydrogeologically  solidified  to minimize  the  integrity  utmost c o n s i d e r a t i o n w i l l  effect  leaching  stable  be  Barriers  intrusion  deleterious  the  to 2 0 0 0 m i l l i o n  repository  groundwater  order  the  probably  of  of a p l u t o n a r e  "have r e m a i n e d u n d i s t u r b e d  i e , for 200  will  in a geologically  pluton.  selection  radwaste  terminal disposal w i l l  advantages  stability"  the  as  the  waste r a d i o n u c l i d e s  repository  Canadian S h i e l d known  the  of  i e , bentonite  g r e a t l y enhanced.  waste  i s used,  7  3.  MICROBIAL  ANTAGONISATION  Microbial radionuclides destruction  sorption A.  may  from  repository  a  the  agents  that  may  by  MICROBIAL  ACTIVITY  release  bitumen  may  be  movement  effecting  matrix  or  of  physical  production  . the  of  effectiveness  of  material.  AND  waste  the  by  decrease  backfill  of  ISOLATION  enhance  solidified  reactions  The  RADWASTE  activity  of  complexing  OF  LEACHING  radionuclides  envisioned  as  a  encapsulated  process  in  involving  two  mechanisms: 1)  Matrix  decay  bitumen;  2)  and  production  of  the  over  consequences  has  been  1 6  Matrix  a  esters,  The  a  waste  that  effect  on  of  by  research  has  been  of  their  and  of  the  through  other  previous  Scientific  findings  do  not  must  the  metabolic  of  Laboratory.  to  isolated  1  on 7  "  2  3  However, wastes  non-existent. " 2  2 5  general  the  for  bitumen  nuclear  under  be  significant  attack  investigators.  performed  have  have  microbial  virtually  was  i s assumed  remain  attack  is  done  mechanism  e f f e c t may  direct  microbial bitumen  Alamos  each  the  in  Los  of  years,  encapsulated  the  attack  effected  ketones  few  for  investigations  of  microbial  solubilization  result  documented  that  direct  1 5  Although  centuries.  by  alcohols,  end-products.  negligible  caused  The  auspices  Unfortunately, applicability.  many The  8  experimental would  design  yield  information  Waste  Isolation  C0  gas  2  Pilot  dissimilar  and therefore  MICROBIAL  The mitigate  ability against  been  produced  f o r the cross  studies  geological WIPP  included  asphalt,  microbial  and  general  environment  of  rock-salt)  i s  (hard  comparisons  should  only  elements  b e made  synthetic sorption  elsewhere.  microbial  may  through  to  serve  backfill  2 7  ,  to  material  h a s shown agents  of organic  that  agents to  backfill  chelating  metabolism  therefore,  chelating  Emery  2 6  MOVEMENT  may  material  the  and  be  materials.  microbially  enhance  that  produced  movement  the  of  surrounding  environment. fate in  evaluated  by  and a  liquid  migratory  natural numerous  partitioning  studies.  SUBSURFACE NUCLIDE  polyhydroxamate  agents  subsurface  AND  strong  logically,  radionuclides  and  These  that  t o t h e U.S.  o f WIPP m i c r o f l o r a  radionuclide  through  follows  The  of  and  chelating  the  directly  (inactive)  The  ACTIVITY  established  hydroxamate  It  from  expected  on e x p e r i m e n t s  caution. B.  has  (WIPP).  studies.  and that  focused  pertained  o f Pu, e n u m e r a t i o n  radiobiological  with  that  Plant  evolution  methylation  plutons  and r a t i o n a l e  Various  geological  element  (groundwater) researchers  have  of  nuclear  environment  methodologies.  of t h e waste  phase  properties  i s  However, between  to  has  been  evaluation  the solid  the focal  tried  waste  point  of  media o f most  illustrate  the  9  destiny  of  conditions. 4.  2  S C O P E OF  As adverse a  escaped 8  -  3  Unlike  earlier,  effect  nuclear  the  on  waste  scope  Los  nuclear  microbial populations waste  were  program.  management  package this work,  (choice chosen  and/or  thesis will  throughout  details  techniques)  of  Alamos  applicability sundry  a  myriad  of  have  an  attack  of  T H I S WORK  mentioned  The  under  0  bituminized  agents.  radionuclides  by  may  direct  production  of  chelating  span  two  issues.  these  this  research  should  the  nuclear  industry.  of for  radionuclides, their  relevance  find  general However,  organisms to  the  and  Canadian  10  II.  1 .  MICROBIAL  DEGRADATION  OF  BITUMEN  BACKGROUND  Compared hydrocarbons  with  glucose  poses  a  degradation,  unique  set  of  microbial oxidation  of  problems:  they a r e i n s o l u b l e i n water and p r e s e n t problems of how they are solubilized or e m u l s i f i e d ; they are c h e m i c a l l y u n r e a c t i v e so r e q u i r e s p e c i a l i z e d enzymes for their initial oxidation, and, finally they reverse the m e t a b o l i s m of m i c r o o r g a n i s m s from b e i n g g l y c o l y t i c and lipogenic to being lypolytic and gluconeogenic. 3 1  . Since  metabolism  efficient"  as  hydrocarbons mechanism.* evolved  adaptations  *  a  a  some have  of  substrate  result,  of  the  endowed  with  is  common will  adaptation  microorganisms  circumvent  hydrocarbons  degradation as  As  of  only and  the  as  sugars, occur  natural  ability  constraints organisms  not  use a  of  secondary  selection  to  listed with  as  "energy-  have  overcome above.  the  H y d r o c a r b o n s w i l l o n l y be d e g r a d e d i n t h o s e c a s e s more s u i t a b l e s u b s t r a t e s a r e l a c k i n g o r absent.  ability  where  or  These to:  other  11  produce  s u r f a c e - a c t i v e agents  hydrocarbon  substrate;  alcohol  diol)  or  enzymatic simple  sugars  Although  the  species  limits  mixture  of  from  high  A.  to  by  With  acids  their  fatty or  reactant  them  more  degradation  mixed  the  microbial  of  components  culture  to  prone  lipoidal of  of  their  ( u s u a l l y to  a c i d metabolism;  other  individual  respect  e m u l s i f i c a t i o n of  specificity  overall  a  bitumen,  to  an an  produce  precursors.  most a  microbial  heterogenous  may  be  attacked  hydrocarbonoclastic  major  organic  degradation  may  groups  occur  in  that the  ways:  ALIPHATICS  According apply  to  substrate  hydrocarbons,  bacteria.  following  fatty  the  making  similar  the  preferentially  compose  oxidize  thereby  catabolism  for  the  to  Ratledge,  degradation  of  3 2  the  following  aliphatic  characteristics  hydrocarbons:  1. A l i p h a t i c h y d r o c a r b o n s a r e a s s i m i l a t e d by a w i d e variety of microorganisms. Other classes of compound, including a r o m a t i c s , may be o x i d i s e d b u t a r e a s s i m i l a t e d by o n l y a few b a c t e r i a . 2. n-Alkanes of c h a i n l e n g t h s h o r t e r than n-nonane are not usually a s s i m i l a t e d b u t may be o x i d i s e d . O n l y some b a c t e r i a have the ability to grow on alkanes shorter than n-octane. As t h e c h a i n length of the alkane i n c r e a s e s beyond C the yield factor i n c r e a s e s but the r a t e of o x i d a t i o n decreases. 3... Saturated compounds a r e d e g r a d e d more r e a d i l y than unsaturated ones. 4. Branched-chain compounds are degraded less r e a d i l y than s t r a i g h t c h a i n compounds. 9  Although  hydrocarbons  of  chain  length  <C  9  are  more  1 2  soluble seem  and  to  therefore  i l l i c i t  attributed  to  concomitant toxicity  a  a  toxic  in  short  The  from  amphoteric  an  emulsif i e r . The  possible the  second  normal  is  acid  is  and  usually  B.  of  means  toxicity  In  4  acids fatty  of  which  may  be  with  a  addition  to  membrane 3  they  may  also  be  acids  is  evident  they  may  act  as  to  P-450  follows.  i s complete,  final  catabolic  or  branched-chain  mode  substrates,  namely,  a  terminal  aliphatic  by  rubredoxin).  one To  carboxylic this  degradation  of  of  alcohol  After  pathways  initial  similar,  primary  i t s corresponding  usually  the  a  metabolism  such  as  can  two  convert acid,  conversion  a  to  occur  a  via  0-oxidation.  oxidation the  of  changes  resultant  carboxylic  for  product  group.  AROMATICS  Not  unlike  metabolism initial simple  to  biochemical  alkenes  fatty  the  (cytochrome  alcohol  Although  by  in  usually  oxidation  carboxylic  integrity.  effect  nature  This  3 3  cytoplasmic  functional  step  enzymes  primary  the  microorganisms  5  first  hydrocarbons  of  deleterious  3  to  response.  hydrocarbons,  noxious. their  available  disruption  loss  from  more  of  an  the  aromatic  substrate  to  benzene-like  catechol.  decomposition  Chapman  a  species common  compounds, 3 6  an  a l i p h a t i c compound  requires product.  the  illustrates  of  common  that  oxidation In  the  product  3 major  case  of  the  of  most  is usually  products  -  of  a an  13  initial  oxidation  protocatechuic acid  sequence  acid  (catechol  for  substituted serve  a  wide  catechols  subsequent  catechol  i s  (cleavage  between  groups)  substrates".  the  meta-fission  bearing  carbon  two  and  a  or a substituted pathways  POLYCYCLIC  In  comparison  to  conversion  metabolism  may  proceed.  hydroxy-2-napthoic microbial Again,  attack  dihydrodiol  acid seems  to  i t  hydroxy  catechols an  may  hydroxy-  that  i s not  conversion  ring-fission,  the  hydrocarbons a  to  a  central  oxidation.  to start i s  some through  simple (PAH)  dihydrodiol  scheme  from  production  to  of  Although this  the  between  complete  degradation  on  from  the ortho-fission  following and  to a  HYDROCARBONS  dependent  vary  may  conversion  substituted  adjacent  p o l y c y c l i c aromatic  to  while  o f t h e bond  compounds,  appear  of  "other  phenols  containing  t o cause  AROMATIC  follows  catechols  catechol  function  C.  that  Thus,  3 8  points  and that  parahydric  carbons  carbon  and g e n t i s t i c  3 7  For  (cleavage  hydroxy-substituted).  metabolic  step  predominates,  undergo  compounds"  or s u b s t i t u t e d  reaction  acid  are "at the focal  of  ring-fission.  pathway  catechol  acid)  range  as r i n g - f i s s i o n The  1,2-dihydroxybenzene,  or 3,4-dihydroxybenzoic  or 2,5-dihdroxybenzoic  pathways  or  aromatic are  before  genera  also  further  (Aeromonas)  production  of a  1-  phenanthrene,  the  with  of the d i o l .  production  usually  followed  general  by  ring-  14  fission  and  metabolic  pathways.  The been a  then  total  degradation  unequivocally  lack  o f PAH's  larger  demonstrated.  of perseverence  asphaltene  degradation  fraction  by  via  than  3 rings  Although  experimenters  of bitumen  may  various  this  in  central  has not may  the  yet  represent  field,  the  be r e s i s t a n t t o m i c r o b i a l  attack. In  conclusion,  dependent  on  conversion  intermediate  such  product  in  turn  systems  that  have  2.  microbial  as a c a r b o x y l i c is  mentioned  hydrocarbons  acid  completely  a more  general  possible  earlier,  i s usually  hydrocarbonoclastic 1) G e m n i  A) a n d 2 p u r e 2) U n i v e r s i t y  Thus,  were  Research  -  waste  unidentified  from:  Limited  1 mixed  of  t o maximize the  of  obtained  B a n d C)  oxidation  (containing  cultures  of Calgary  intracellular  of microbial  bitumen  (Cultures  this  BACTERIA  of  Biochemical  reactive  alcohol,  by  is  function.  slow.  microbes  an  degraded  the rate  fresh  hydrocarbons t o a more  or  extremely  degradation  radionuclides)  of  of the substrate  R E P R E S E N T A T I V E HYDROCARBONOCLASTIC  As  *  degradation  -  1 mixed  (Culture  cultures. culture  (Culture D).*  Thanks to Dr.Ian Forrester and Mr.Cam Wyndham of Gemni Biochemical Research and the University of Calgary r e s p e c t i v e l y f o r t h e i r kind donation of these c u l t u r e s .  15  All rich to  four  Athabasca the  task  hydrocarbons  3.  had  CONDITIONS  GROWTH  All  cultures found  of  a n d were  utilizing  as a metabolic  a  located therefore  were  As  of this  grown  heterogenous  for  by  Bushnell  are listed  deionized  water  2  2  had  MINERAL  precipitation  sterilization autoclaved  degradation Haas,  of  (>20 m i n u t e s  separately  SALTS  the  inorganic  a t 125°C), after  cone.  soln.  SOLUTION  various  and added  3 9  of  I below:  0.2 g 0.02 g 1.0 g 1.0 g 1 .0 g 2 drops  I - MICROBIAL  that  1000.0 m i s  2  were  mixture of  solution  and  i n Table  2  after  salts  microbial  MgSO„ CaCl KH P O „ K HPO„ (NH„) SO„ FeCJ-3  prevent  adapted  IDENTIFICATION  on a m i n e r a l  described  mixture  Distilled,  To  well  substrate.  t o be s a t i s f a c t o r y  Table  i n the bitumen-  CONDITIONS  hydrocarbons. contents  tarsands  had been  FOR GROWTH AND P R E L I M I N A R Y  A.  been  cultures  FeCl  the  species and C a C l  3  main  2  solution  cooled. In  nutrients extract  addition including and  to  the  salts  0.3 w t . %  0.5 w t . % p e p t o n e  malt were  listed  above,  extract, added  0.3  non-selective wt.%  yeast  to the mineral  salts  1 6  solution  on  maintained maximized  B.  t h e recommendation at close  (20-25°C)  A,C  showed  of  The  the  4 cultures  and  D  gram  some m o t i l i t y a t 3 0 ° C .  Environment may  analysis"  contain  was was  B  -  Bacillus  Culture  C  -  VE  Culture  D  -  Citrobacter,  and  7)  0.30 m l o f f r e s h  nutrient  media  vessel  salt  the  (Appendix  methods:  rotate(5-l0  report  showed  genera:  group*  with  analysis  1,3,5  A)  Ministry  Pseudomonas  CURVES  conjuction  Environment  rod-shaped  An O n t a r i o  the following  Culture  GROWTH  negative  (see Appendix  1  Pseudomonas  reaction  aeration  contained  -  to  and  of a l l c u l t u r e s .  A  (Figures  Temperature  agitation  Culture  In  0  IDENTIFICATION  that  C.  *  ambient  through continous  Cultures cells  to  of F o r r e s t e r . "  at  every hour  established  i n n o c u l u m was (described  25°C. for  Ministry  A), microbial  were  solution  RPM)  Ontario  by  added  the  least  were 11  The  profiles following  t o 20 m i s o f t h e  earlier)  Samples at  growth  of  and  allowed  taken  from t h e  hours.  Serial  B a c t e r i a i n t h e VE g r o u p s h a r e c h a r a c t e r i s t i c s w i t h t h e g e n e r a Pseudomonas, Xanthomenas and Chromobacterium and as yet are not w e l l d e f i n e d taxonomically." 2  17  dilutions  followed  by m e d i a  number  of viable c e l l s  2,4,6  and  obtained to  8)  per sample."  of absorbance  f o r each  culture  spectrophotometer  showed  observation This  4.  SELECTION  A.  In  followed:  degrading  then  Base  that  on  were  readings a  also  o f 0.5  Gilford  240  (YNB)**  nature.  A, c o n f i r m s  the  GROUNDWATER  culture  with  the  following  mesh  (DIW) c o n t a i n i n g  (500 K r a d s ) .  greatest  procedure  of Sp-170)*  a n d 0.1 w t . % p e p t o n e .  _  D  interesting  i s i t sb i p h a s i c  AND  the  by r i r r a d i a t i o n  Culture  CULTURE  t h e mixed  water  second  i n Appendix  CULTURE  potential,  A  that  D.  g of bitumen(30-40  sterilized  (Figures  concentration,  growth.  OF A S U I T A B L E  20.0 m i s o f d e i o n i z e d  Nitrogen  curves  illustrate  of Culture  to isolate  1.0  Standard  absorbance  D profile  with  OF A S U I T A B L E  SELECTION  bitumen  in  coupled  content  order  t o determine the  sample  1-8)  initial  of the culture  multi-organism  hourly  (Figures  rapid  information  vs c e l l  was u s e d  (wavelength=600nm).  plots  t h e most  3  by t a k i n g  1.0 m l a l i q u o t s o f e a c h  "These  plating  was  0.1340  This Two  was  placed g  Yeast  s o l u t i o n was identical  *  "Sp-170" i s t h e d e s i g n a t i o n u s e d by Husky O i l ( t h e bitumen s u p p l i e r ) f o r t h i s c l a s s of o x i d i z e d bitumen. **YNB i s a n o n - s e l e c t i v e source of non-carbon nutrients for microbial g r o w t h , i n c l u d i n g t h e f o l l o w i n g : ( N H ) 2 SOi, ( 75 w t . % ) , KH P0,(15 wt.%), MgSO (7 wt.%), N a C l O wt.%), CaCl (l wt.%) and s e l e c t e d v i t a m i n s a n d n u t r i e n t s ( < 1 wt.%) a  2  a  2  18  CULTURE  Figure  CULTURE  A  1 -  11 HOUR  Culture  A STANDARD  Figure  2 -  A -  GROWTH  11 H o u r  CURVE-(ABS.  Culture  A -  CURVE  Growth  Curve  VS  CELL  Standard  Curve  CONC.)  19  20  CULTURE  C 12 HOUR  T  GROWTH  1  1  1$  I  $jt  1  CURVE  1  HA  1  1  ItM  1  1 1 T~~ 14A t*M  TIMM(EOURS)  Figure  CULTURE  5 - Culture  C STANDARD  C -  12 H o u r  Growth  CURVE-(ABS.  CELL CONCENTRATION (CELLS/ML)  Figure  6 - Culture  C -  Curve  VS CELL  (X10*  Standard  )  Curve  CONC.)  21  CULTURE  D STANDARD  CURVE-(ABS.  VS CELL  ittt* CELL  Figure  CONCENTRATION (CEILS/ML)  t H M 144** (X10* )  8 - C u l t u r e D - Standard Curve  CONC.)  IMA*  22  solutions that  were  bitumen  vessels, to  run Thus,  was  on  compare  a common f)  (e a n d  following  the sole  appropriate  directly  growth  prepared  carbon  controls of  rate carbon  six individual  (sets  growth  of  sets  a  present  a a n d b) on  substituted  a)  YNB  +  Culture  b) c) d) e)  YNB YNB YNB YNB  + + + +  Culture D B i t u m e n ( 1 g) B i t u m e n U g) S u c r o s e O g)  + + +  Culture Culture Culture  A D A  f)  YNB  +  SucroseO  +  Culture  D  At  T=46  hours,  containing  confirm  the  test  run. to  Also,  rate  controls for  of were  bitumen.  of:  A  g)  growth  Culture  were  set of  run c o n s i s t i n g  To  in  bitumen  second  sucrose  were  procedure.  source  source  consisting  this  D  was  and  found  only  for  those  s i m i l a r i l y , .the l a r g e s t  sets  population L  sizes  were B.  only  found  SELECTION  Current Whiteshell synthetic  work  by  Nuclear  A  sets  the  conditions  s t u d i e s . I n for  selection  of a  microbial  growth  The  four  according  was  was  of  the  has e s t a b l i s h e d  four  appropriate  order  to simulate  experiments  groundwater  that  Branch  for  radionuclide  "real"  repository  (Sections  IV and V ) ,  would  not  supress  solutions  were  prepared  necessary.  synthetic  t o t h e methods D  SOLUTION  Geoscience  Establishment as  subsequent  synthetic  GROUNDWATER  Applied  Research  f.  d and  SUITABLE  groundwaters  adsorption  Culture  OF  for  tested  groundwater outlined  i n Appendix  through  simple  B.  Growth  innoculation  of  of each  23  groundwater wt.%  solution  yeast  mineral After  extract  salts  other  incubation  Solution  containing and than  at  supported  0.5 those  25°C  the  the  best  0.3  wt.%  malt  wt.%  peptone  contained solution  growth  of  by  extract,  but  no  the  additional  groundwater.  containing  Culture  0.3  WN-1  Saline  D.  REMARKS  Since  the  foreseeable (Section growth were  IV).  inhibitors On  mentioned  selected  solution  degradation  as  the  of  basis  above, the  of  most  respectively,  to  bitumen  microbial of  the  activity  rudimentary  Culture  D  appropriate provide  is extremely  a  and  WN-1  culture "worst  slow,  were  eliminated  evaluations Saline and  case"  a l l  of  Solution  groundwater approach.  24  III.  Since source  of  on  waste  repository  radiation  Cultures  majority  encapsulated  of  in  A,B,C  and  The  absorbed  cited  as  a  radiolytic generation."  each  LET*  culture In  dose  potential  degradation  (<10 D  will  be  R/hr),  has  the  from area of  been  the  a  continous effect  of  evaluated.  with  order  to  a  high  radionuclides  r radiation _  these of  asphalt these  relative  r a d i a t i o n was  waste  emit  However,  5  bacteriocidal; low  low-level  bitumen  etc.).  to  RADIOSENSITIVITY  BACKGROUND  The  *  final  low-level  radiation 1.  the  MICROBIAL  radionuclides concern  energy  with  with  fields of  Culture  through  (1330.0  graphically illustrate  1 3 7  may  Cs,  be  6 0  has  Co  been  respect  concomitant  same  resistivity evaluated  (ie  that  KeV) the  gas  could A,B,C  to  be and  irradiation  D of  r source. _  lethal  effects  LET or L i n e a r E n e r g y T r a n s f e r encompasses t h a t f r a c t i o n of inherent energy associated with the radiation that transferred to the t a r g e t atoms - energy t r a n s m i t t e d t o absorber per u n i t path length.  on  the is the  25  a  population  determined  of  over  experiment  decrease 2.  yield  percentage  o f 0-300  Krads.  information  of whether  or eliminate  The r e s u l t s  that  of bitumen  will  was  of  i s important  or not i r r a d i a t i o n  the rate  survival  this  i n the  effectively  biodegradation.  METHODS  A.  GROWTH MEDIA  Six described To  PREPARATION  litres  of  earlier  (Section  prevent  the  sterilization) separately.  mineral  a CaCl Peptone,  yeast  solutions  (medium  mixed  300  plates  under  upon were  A  CELL  fresh  and  allowed  this  long  in a  the exception inorganic  of  0.02  and  were  2  were  of  malt  accompanied  and C a C l )  solution  prepared  from  this  prepared of  g/ml  were  sterilized  mixture  (during prepared  by 2 wt.% a g a r .  then  2  was  extract  as  CaCl .  salts  termination of s t e r i l i z a t i o n .  i n t e n s e UV  B.  I I ) , with  solution  2  to Forrester,  and  salts  precipitation  according  be  culture,  t h e range  will  consideration  each  added  These  two  separately  Approximately  and allowed  to  cool  irradiation.  PREPARATION  solution to  of c e l l s  incubate  growth  prepared  for approximately  incubation period  stationary  was  a l l cell  phase.  from  each  72 h o u r s .  solutions  were  culture Due t o  assumed  to  26  Cell fresh  washing  culture  PBS.*  Each  10  minutes  at  culture 2°C.  in  PBS  prior was  and  placed  catylzed  in  and  0.4640  dead  time  in  the  a  and  following ice to  a  the  each  dead  rate tubes  1 ml  followed at  of  by  9000  each  9-10  RPM  mis  for  5-  was  discarded  and  the  were  vigorously  agitated  PBS.  ENUMERATION  pellets cell  solution.  irradiation  decrease  Krad/sec*** dose  of  the  Irradiation  with  centrifuge  *  AND  mis  adding  centrifuged  homogeneous  repair.  Gammacell-220  then  by  tubes  supernatant  washing,  to yield to  centrifuge  i n 9-10  IRRADIATION  Following  three times  was  The  resuspended  C.  done  to Nalgene  of  pellet  was  time**  was and  the  cultures  according to  interval  effect  of  performed dose  respectively.  4 6  were  Immediately  rate On  the  each  culture  enzymatically with of  an  AECL  2.4024  Krad  basis  irradiated  of  this  directly  Table I I .  PBSPhosphate Buffer Solution is a m i x t u r e of K HPO and KH PO„ present in an appropriate molar ratio to yield a b u f f e r e d pH o f 7.50. ** D e a d t i m e i s t h e r e s i d u a l r a d i a t i o n r e c e i v e d by the sample p r i o r t o and upon t e r m i n a t i o n o f t h e d o s i n g p e r i o d . ***Dose r a t e and dead time are determined from the measured source ( Co) activity at some r e f e r e n c e t i m e , t = 0 . Thus, d o s e s and dead time a t time t can be calculated from the o r i g i n a l a c t i v i t y , r e f e r e n c e time and source h a l f - l i f e . 2  2  6 0  a  27  Dose(Krad) 0 5 10 15 25 50 75 100 200 300 Table  Upon was IO"  Time(sec) 0.0 5.6 5.6 5.6 16.4 48.7 48.7 48.7  y-IRRADIATION  receipt  were  5  first fifth  of  then  serial  dilutions  Replicate  of  receipt  allowed  to  aliquots of  2  listed  irradiation ml  1  dose  plates  was of  prepared the  the appropriate  for  hours  a t 20°C  4  and  f o r each  the was  were  dose.  D  culture  , 10"  3  AND  of  in Table I I .  cultures  of t h e sample  i n c u b a t e f o r 48  the  10" , 1 0 " , 1 0 " prepared  replicate  A,B,C  of  were  s e t of  0.5  mis  plates  and a t each  Since  CULTURES  d o s e , . 0.5  dilutions  after  Time(sec) 0.0 5.6 11.2 16.8 33.2 81 .9 130.6 179.3 389.6 600.2  U S E D FOR  four  sequentially, plated  TIMES  the a p p r o p r i a t e  made.  control.  Cumulative  210.3 210.3  removed and  the A  II -  Sequent i a l  0  dose  performed  diluted  and  A l l plates  were  prior  to colony  enumerat i o n .  3.  RESULTS  Dose-response cultures the  cultures  least dose  A,B,C  half  curves  and  (Figures  D.  are capable  These of  the population  exceeding  6 Krad.  curves  growth will  These  9-12)  generated  illustrate  at a  die (LD  results  were  dose 5 0  )  >75  after  indicate  that  for  none  of  Krads.  At  exposure  to a  that  none  of  28  the is  cultures only  tested  are  r e a l i z e d at  showed  survival  mechanism expected  for since  radiosensitive  >1000  rads)  (substantial cell  however,  Culture  curves  characteristic  cellular  inactivation.*  many  b a c t e r i a l species  of  A,C  a  show  and  D a l l  Multitarget*  This  7  death  r e s u l t may  this  response  to  be y-  irradiation. In  order  prevent  severe  surface 1  "C,  1  3  7  to  dose Cs  rate  and  6 0  will will low  in  the  nuclides  have  a  negligible Since and lived  the  by  bitumen  the  1 3 7  Cs  rate  and  culture waste  radionuclides  be  effect  negligible. of  radiosensitivity  the  most waste of  with  block  of  the  10  R/hr.  Except  predominant  30  have  initial for  radionuclides  repository."  will  is  will  relatively contain  a  low  the  waste  However,  9  and  These  waste  5.3  years  decay,  activity  decreased  to  on  these  long-term  and/or  of  organisms.  short-  activity microbial  exposure  increase  M u l t i t a r g e t t h e o r y a s s u m e s an o r g a n i s m after various intracellular "targets" radiation source.  radio-insensitive  predominately  initial  mutation exposed  a 8  and  years.  tested  with  personnel  bitumen,  exponential  Co  300  to  the  5730,  an 6 0  to  below  level  levels within each  kept  be  exposure  damage  half-life  Thus,  radiological would  be  Co  contained  contributed  the  radiolytic  respectively.  *  minimize  may  the  -  the  species increase relative  5 0  death w i l l r e s u l t only a r e i n a c t i v a t e d by the  29  RADIATION  DOSE  RESPONSE  PROFILE  OF CULTURE  A  DOSE(KRAD)  Figure  RADIATION  DOSE  1  T  1t.O  9 - Dose-Response  RESPONSE  1  1  S4.0  Figure  1  1  of Culture A  PROFILE  1  1  1  1  MM 40.9 4IM DOSE(KRAD)  1  OF CULTURE  1  MM  10 - D o s e - R e s p o n s e  1  r  $4M  71.0  of Culture B  tOJ>  B  30  RADIATION  DOSE  RESPONSE  PROFILE  OF  00.0  04J0  CULTURE  C  10J0 0OJ>  DOSE(KRAD)  Figure  RADIATION  i  1  0J0  i  1  4.0  DOSE  1 1  1  0J0  11 - D o s e - R e s p o n s e  RESPONSE  1 1  10.0  Figure  1 1 r - i  of C u l t u r e C  PROFILE  1  i  I0J0 00.0 04.0 DOSE (KRAD)  OF CULTURE  1 1  00.0  12 - D o s e - R e s p o n s e  1 00J0  1 1  1 1—  00.0 40J0  of Culture D  D  31  IV.  EVALUATION  Leaching, species  such  primary  the  as  equations,  will If  against  y.  A  F  0  linearity cumulative  time  tapering  the  off  was  to  used  a  plot  be a  However,  is  a  approximated  LEACHING  relatively  insoluble  solubilized,  of  leaching  is  encapsulated immobilized by  the waste  wastes  Fick's  has  diffusion  of: Eqt.IV. 1  vs  (t )°-  i f the  process  5  n  fraction  of  curve  described  straight to  which  salt  of  resultant  may  Section.  *  and  be  ENHANCED  release.  process  to  5 2  5  response)  plot  "'  '' "  5 3  for  The  Igj  show the  5 1  by  inorganic  mechanism  shown  MICROBIALLY  process  an  radionuclides. been  OF  i s governed  leached  (for  diffusion-mediated  as  a  parabolic  with  slope  illustrate  the  data  (and  diffusion.*  activity  line  diffusion  by  therefore  is  plotted  initially  "~0.  This  then  type  presented  in  leaching)  will  of this not  Where a =radioactivi_ty leached d u r i n g the leachant renewal period,n;A =radioactivity i n i t a l l y present in specimen;F=exposed s u r f a c e a r e a of s p e c i m e n ( c m ) ; V = s p e c i m e n v o l u m e ( c m ) and tn=duration(days) of l e a c h a n t renewal p e r i o d . " n  0  2  3  5  32  occur  unless  leachant. allow  the An  greater  solidified increase  leachant  will  1.  ENHANCED  LEACHING  The result  enhanced  b)  Temperature,  final  geologically  immobilized  waste  elicit waste  a  are  unknown.  is  to  expected  high-level  greatest and  that  will  the  encapsulated in  with  an  species  increase  respect  to  in  with  leaching.  bitumen  that  may  are:  be  repository  temperature. be The  enhanced remaining  increase  therefore  If  in  deserve  the  as  a  the  factors  leaching greater  of  under  is  may  the  of  the  heat  from  the  overall  large  enough,  increased result  "repository  elaboration.  of  temperature  waste  increase  increase  a  groundwaters.  repository  may  in  mechanical  in contact  however,  result  two  of  native  the  10°C  decay  located  characteristics  Initially  approximately  be  effect  with  temperature  radioactive  may  will  the  radionuclides  repository  5 5  mechanisms  of  negligible increase  the  contact.  the  any  location,  Unfortunately,  leaching  with  abrasion,  stable  will  repository  the  contact  Biodegradation.  the  abrasion  in  Diffusion,  d) Since  leaching  Mechanical  are  result  factors  a)  c)  of  therefore  pertinent  in  in  availability  the  wastes  surface in  the  conditions"  33  Diffusion The  enhanced  concentration solvent  be  considered  the  ion  bitumen movement  of ions  media  initial  ionic  will  block.  by  thus,  between  The  the  and water,  between  the isotropic  Mathematically,  A s AC solid  this  ( i e DIW),  surface  force in  for  net  0,  contact  the  will  may  be  a  random  and  the has a  with  in the  steady-state between net  also  be d e s c r i b e d  be  increase  this  and  will  media  concentration  approaches  may  a  after  and leachant  diffusion  case,  If the surrounding  driving  AC.  solid  the bitumen  observed  difference  bitumen  In  the  mediated  mixture  waste  as  the bitumen  diffusion  - bitumen  medium.  be  bitumen  between a  the  occur.  will  from  decreased  concentration  content  i s  ions  radionuclide  isotropic  movement  surrounding low  i s  homogeneous an  of  rationalized The  5 1  essentially  uniform  gradient  can  phenomenon.  movement  the  exchange  become  0.  as:  the rate of t r a n s f e r of d i f f u s i n g substance through unit area of a section i s proportional to the concentration gradient measured normal to the section, ie F = -D\T. Eqt.IV.2  \X where F i s t h e r a t e o f t r a n s f e r per unit area of s e c t i o n , C the c o n c e n t r a t i o n of d i f f u s i n g substance, x the space coordinate measured normal to the section, and D is called the diffusion coef f i c i e n t . 5  The equilibrium  resultant state  6  effect  i n which  of  this  process  the concentration  of  will ions  be in  an the  34  leachant  approximates  bitumen.  Unfortunately,  those  cases  in  a  may  afford  "real"  exists  between  still  being ions  for  was  and  in  provided matrix by  only  case  slope—-K),  a  13  in  in which  solution prior  to  to  state  that  gradient  Sets an  This in  which  time)  which  the  the  26  of  in flow  groundwater.  function  to  the  attained  dynamic  (Set-A).  due  be  in  Groundwater  Figures a  ions  concentration  cases  present the  a and  (as  a l l  not  a l l illustrate  present  represent  leached  of  is static.  illustrated  fraction  approached  would  solid  increasing  however,  leachant  dilution  the  counterbalance  of  the  is clearly  cumulative  concentration  equilibrium will  repository  infinite  behaviour the  in which  the  an  B,C,  is  ionic and  D*  equilibrium  mitigating initiation  is  effects of  the  in  situ  test.  Biodegradation As 2  1  -  2  3  ,  5  previously 7  effect leaching bitumen by  6  0  of  attack  has  microbial  as  i t i s used  6 1  ;  or  been  attack  via: physical  metabolic  products  *  -  mentioned  of  removal as  a  both  adequately a of  the  the  "  1 9  waste  exposed substrate;  end-products  e m u l s i f i c a t i o n of  1 7  and  demonstrated.  bituminized  microbial  intermediates,  Set A c o n t a i n e d p r i m a r i l y of the  laboratory  layer  enhance of  the  solubilization or  1 5  may  The  co-oxidative  bitumen  by  microbially  DIW only. H o w e v e r , B,C a n d nutrient solution discussed  D in  were composed Section II.  0  35  SETS  A1#1,C1J)1  -  "Co LEACHED  VS  TIME  —i—  /ML0  TIME(DAYS)  Figure  13 - L e a c h i n g  SETS  profiles  A1,B1,C1J)1  -  m  f o r sets  Al,B1,C1  C s LEACHED  VS  _ a n d D1  6 0  Co'  TIME  e—©  a 1  SET A-1 * • SET B-1 •—» SET C-t SET D-1  TIME (DAYS)  Figure  14" - L e a c h i n g  profiles  f o rsets  A1,B1,C1  a n d D1 -  1 3 7  Cs  36  SETS  ^  SETS  A2 B2,C2 D2 t  t  A2 B2,C2 D2 t  t  - "Co  LEACHED  "Cs  LEACHED  -  VS  VS  TIME  TIME  TIME(DAYS)  Figure  16 - L e a c h i n g  profiles  f o r sets  A 2 , B 2 , C 2 a n d D2  -  1 3 7  Cs  37  SETS a—o  SET • SET • SET x — K SET <  A3£3,C3J)3  tJO  )  t  ,  ^  tOM  LEACHED  VS  TIME  A-3 B-3 C-3 D-3  f—~T"  ^  - ' Cs  fi  MM  ?  i  *  x  M.0  *—  *  49M  (  MM  +  •  —  M  —X *~~  MM  _  4  70.0  MM  K  MM  IMM  TIME(DAYS)  Figure  18 - Leaching p r o f i l e s f o r sets A3,B3,C3 and D3 -  1 3 7  Cs  38  SETS  A1A2A3  -  Cs  m  LEACHED  VS  TIME  39  SETS  i  B122.B3  -  "Co  LEACHED  VS  TIME  o—e> SET B-1 < *—•  • SET SET  B-2 B-3  -i  1  1  r  I I M  TIME(DAYS)  Figure  21  - Leaching  SETS  B1,B2£3  profiles  -  f o r sets  B 1 , B 2 a n d B3 -  Cs LEACHED  VS  TIME  6 0  Co  40  SETS  r  SET SET SET  C1,C2,C3  1  - Leaching  SETS  1  r  T  50.0  1  TIME  profiles  C1,C2,C3  -  m  00.0  r~  1QQJ0  70.0  f o r sets  Cs  I  ir  1  00.0  4CJO TIME(DAYS)  30.0  23  VS  C-1 C-2 C-3  —i Figure  - "Co LEACHED  C1,C2 a n d C3 -  LEACHED  VS  6 0  Co  TIME  o—o S I T  C-1 * • SET C-2 *—» SET C-3  —i  1  40J)  1  1  80.0  1  r  80.0  IOOJO  TIME(DAYS)  Figure  24 - L e a c h i n g  profiles  f o r sets  C1,C2 a n d C3  1 3 7  Cs  41  TIME(DAYS)  Figure  25 - L e a c h i n g  SETS  profiles  D 1J)2J)3  -  for sets  Cs  m  D1,D2  LEACHED  a n d D3 -  VS  T  26 - " L e a c h i n g " p r o f i l e s  for sets  Co  TIME  1 I0QJO  TIME(DAYS)  Figure  6 0  D1,D2  a n d D3 -  1 3 7  Cs  42  produced  surface-active agents  lipoproteins. microbially on  6  (a  Obviously,  5  or  the repository  Until increased  attack  of  asphalt  investigators  have  the  of  order  to increase  techniques structural preclude  In  have  the experiment  intercomparison slightly allow  for  of test  f o r maximum  6 7  growth  with  of  problem  or  adjacent  t o show  i n bitumen  6  6  due  microbial  In the past, to  maximize  the substrate  (or  t o such  in  an  in  these  destroyed) extent  use i n any  the  as  to  satisfactory  leaching. the  followed  C and D  may  Unfortunately,  their  The  that  has reviewed  attack.  enhanced  was  carbon  undertaken  disrupted  results. Sets  i s in  encapsulated  biomass  described  procedure  sole  relevant  inactive salts.  of  t o show  the  agents  have  of the bitumen  possibility  designed  standardized  of  of  a r e dependent  any a v a i l a b l e method  usually  integrity the  experiment  the rate  modes  petroleum.  study  microbial  and  waste r e p o s i t o r y ) .  t h e waste  one  containing  the  is  i s not a  investigators  utilized  release  deep  containing  and o n l y  two  exogenous  of r a d i o n u c l i d e s  action  contact  of  containing  no  release  a  the bitumen  formation  now,  microbial  in  glycolipids  latter  i f bitumen  presence  emulsify  a geological  the  scenario  the  as l i p i d s ,  r a d i o a c t i v e waste  of the f i r s t  likely  solubilize unless  6  initiated  Furthermore,  to  "  the presence  source  to  2  such  following  that  should  procedure  (described  was  pages allow  good  modified  in Section  hydrocarbonoclastic  a  II). t o  bacteria.  43  Optimal  nutrient,  maintained any  was  microbial sole II)  to create  difference  that  as  The  and a  i f  a  of  growth.  system  conditions that  radionuclides  undergoing microbial dependent  after  on  the  approximately  phase  had  growth  been was  12  could  resolve  from  bitumen  attack.  use  of  were  Although  bitumen  hours  (see  on  a  Section  reached f o r the dependent  as  mixed  the use  of  source. of  this  investigation  samples  under  significant  and  the mechanism  biodegradation)  microbial  of  statistically  inoculated  irrespective  not  further  carbon  temperature  leaching  growth  objective  determine  or  source,  and  experimental  not  was  endogenous  bitumen  between  was  growth  population  an  i n mass  or  carbon an  oxygen  their  was  difference  respective  (solubilization,  conditions  that  simply  were  to  existed  controls,  emulsification optimized  for  44  2.•  METHODS  Twelve containing »iCi/gm  1  3  7  identical 38  Cs  (New  twin-screw a  peak  England at  temperature  gU=1.08),  product 15.7  ectively.  prepared  sodium  extruder  cylindrical  ambient  wt.%  Leachant  Nuclear  a  <170°C.  had  a  t f  the  Solution  of  Sp-170 4.914  flow  X  IO"?)  samples  separate the  were rate  The  and  (oxidized)  »iCi/gm  Ltd.)  mean m a s s ,  leach  four  consisted  product  of  3  temperature,  of  nitrate,  cm ( =7.90  While  and  samples  6 0  2.163  final  35.1  and  8.229  prepared  of  volume  Co  bitumen  and  in  kg/hr  area  of  leachant  four  21.2 resp-  2  for  and  homogeneous  cm U=1.05)  cooled  a  days  solutions  at  were  following:  A  Distilled, demineralized <1.00 X 10" Mho/cm).  water  (conductivity  6  Leachant Solution B T5 Distilled, demineralized water ( c o n d u c t i v i t y - as above). 2) Mineral s a l t s s o l u t i o n as d e s c r i b e d e a r l i e r (Section II). 3) M i c r o b i a l n u t r i e n t media consisting of: 0.3% malt e x t r a c t , 0.3% y e a s t e x t r a c t a n d 0.5% peptone. Leachant solution C T) Distilled, demineralized water(conductivity - as above). 2) M i n e r a l s a l t s s o l u t i o n as d e s c r i b e d earlier (Section II). 3) Microbial nutrient media consisting o f : 0.3% malt e x t r a c t , 0.3% y e a s t e x c t r a c t a n d 0.5% peptone. 4) H y d r o c a r b o n o c l a s t i c bacteria (Culture-D). Leachant Solution D Tl Distilled, demineralized water ( c o n d u c t i v i t y - as above). 2) WN-1 Synthetic groundwater solution as described  45  earlier in Section I I . * 3) Microbial nutrient media consisting o f : 0.3% e x t r a c t , 0.3% y e a s t e x t r a c t a n d 0.5% p e p t o n e . 4)  Hydrocarbonoclastic  The  bitumen  wide-mouth,  samples  screw  solution  then  were  sample  as  but  to minimize  Hespe per the  were  - every  6 7  week  end  of  test  a l l samples  a  the  final  8 week  maximum  rate  solutions  5.0  Shaker  were  according  sample  sampling  8 weeks. was  (C a n d D)  were  7 days  collected  cultures of  horizontally The  leachant  guidelines then  of once  to termination 30 d a y s  after  For the duration  microbial  growth  the  result  and  a t an a v e r a g e  to ensure  a  the  Prior  period.  (exponential  as  activity  innoculated  3-4  a l l hours  of the  of the  temperature  phase),  a and  covering  RPM.  to  leachant  the leachant  agitated  a t 100  with  i n such  of the m i c r o b i a l  f o r the f i r s t  In o r d e r  jars  mis  radionuclides  were m a i n t a i n e d  (tf=1.64).  leachant  of  changed  a  Sybron/Nalge  f o r each  between  than  a l l samples  24 h o u r s  ml  samples  aeration  f o r the following  experiment  23.6°C  good  Orbit  250  i n 100 m i s o f l e a c h a n t ,  less  release  Junior  Three  the exposure  not  agitation,  a Lab-Line  solutions  *  (with  in  polymethylpentene  immersed  maximize  (Culture-D).  placed  closures.  To m a i n t a i n  mechanical by  to  surface  sample).  were  straightside  polypropylene  manner  bacteria  malt  of  was a t sterile before  In keeping with a "worst-possible-case" philosophy, WN-1 s y n t h e t i c g r o u n d w a t e r was s e l e c t e d a s a s u i t a b l e e x a m p l e s i n c e t h i s g r o u n d w a t e r was s h o w n e a r l i e r ( S e c t i o n I I ) t o be t h e most conducive t o growth of C u l t u r e - D .  46  the  time  i n which  A.  ANALYSIS  Immediately spent  leachant  transferred employed  each  prior were  sample. above  background resulting  each  was  Most  -  the  statistical  Germanium,  sample  The  25.0  mis  of  containers  and  subsequent  analysis  took  of  an  average  averaged  background not  change,  equipped  samples  (1  considered  X  10"  a  between 1 2  3  hours  2-3  Ci/ml)  significant  with  a for  o r d e r s of therefore  factor  in  the  analysis. pH  Radiometer(Copenhagen)  Ge(Li)  from  (see S e c t i o n I I ) .  y-spectrometer  measurements and  D) .  *  changed  leachant  withdrawn  Counting  Conductivity-and of  to  t o be  multi-channel  detector.  magnitude  were  to polypropylene v i a l s . a  Ge(Li)*  they  Lithium.  Fisher  were  made w i t h  Instruments  (see  the  use  Appendix  47  3.  RESULTS  AND  Visual consistent  interpretation trend  £a A  0  and  D.  slope=0  i n most  leaching  In  this  Although  the  samples.  A.  of  the  inspection  only of  Set  to  of  set  be  can  will  and  long  term  leachant  a  only  one  is  Sets  B,C  approaching  justification  net  by  a  a for  high  AC.  movement  identical  surface  than  in  of  terms  imperfections  leaching  behaviour  rather  to  slope  DIW.  virtually  small  be  explained  cause  bitumen  A's  in comparison  a l l appear  were  show  of:  earlier,  the  behaviour  would  the  be  a  of  would  of  the  function,  sample.  EVALUATION  qualitative  Figures  13  one-independent  variable)  Keuls  6 8  procedure  time). days  A  18  Eqt.IV. 1  differences in  STATISTICAL  Since  profiles  mentioned  area,  initial  to  0 - 5  vs  sets  13  As  a l l samples and  the  t>21  diffusion  However,  ultimately,  at  test  between  volume  explain  cases  behaviour  radionuclides  Figures  (tr,)  16).  case,  in  leached  latter  (Figure  the  mass,  vs  fraction  These  of  i s evident  V F  n  (cumulative greatest  DISCUSSION  was  to  evaluations 18,  an  coupled  employed  as  may  Analysis with a  the  of  be  made  Variance  by (with  Student-Newman-  q u a n t i t a t i v e approach  to  48  determine days  differences  (see  cumulative  Figure  isotopes for  used,  average was  1  3  7  no D.  Cs  Set Co  6 0  Co  a  A1  A3.  Thus,  which  the i n i t i a l  analysis  was  A1  which  supressed.  than  t=93  at  t>14  from  days.  independently  shows  (Figure  i t appears  from  B,C  that sets  the A l l  f o r t h e two  (see Appendix  leaching  E  f o r the e n t i r e  test.  1,2  in turn,  1  3  7  from  Cs  the  Group  A  there  C and D and between  Set  for A  average  is  at  to Set  represent  affects  and was  A  for  behaviour by  Figure  respect  3)  Co  the  of the  21 i n  t o A2  an anomaly was  B  a=0.05.  illustrated  with  and  6 0  average  but e s p e c i a l l y  could  average  However,  low l e a c h i n g  This  ( a t Day  abnormality,  for  homogeneous  low l e a c h i n g A1  the  different  D.  the  samples  Co  analysis  C a n d D's  13).  6 0  and  and  statistical  sample  for  significantly  of the a b n o r m a l l y  abnormally  This  that  statistically  a l l other  shows  E  only  higher  result  of  to  d i f f e r e n c e between  the combined  f o r sample  profiles  t=14  significance level  different  B ' s mean  as  slope~0  were e v a l u a t e d  C a n d D a t a=0.05,  illustrates  significantly  6 0  of Sets  significant Thus,  from  A a n d B were  significantly  was and  of Appendix  Sets  means  means  performed  c=0.05  Since  results).  Inspection of  were  a t an  means.  sample  leached  tests  statistical  means  18),  fraction  statistical  i n sample  and in  unusually statistical  49  B.  CONCLUSION  93  After microbial from  days  attack  bitmen.  Extrapolation  would  these  representative  of  certainly which be  not provide  However,  leachant  of the data  a viable  the cumulative  conductivity  a consideration  under  optimal  the release  case  radionuclides  the conductivity  high.  leaching  d i d not enhance  here,  days).  of  for real  of native  and/or  1  3  7  for  the  and  leaching  is a  C and D ) .  repository groundwaters  6 0  Co  presented of  (t>93  long-term  leached  Appendix  Cs  plots  f o r enhanced  fraction  (see  of  conditions,  function This  is  conditions  in  are expected  to  50  V.  EFFECT  As by  a  OF  result  many  of  of  the  a  naturally  considered  as  that  may  or  various  comprise  ability  may  be  in depth"*  this  used  geologic  radionuclide  barrier will with to  attenuate  augment  high the  radionuclide  adopted  land-burial  media  is  adsorbent.  occur  a  MIGRATION  philosophy  contemplating  occurring  potential  RADIONUCLIDE  adsorption  burial  being  The  naturally  media  in  situ,  capacity  site's  migration  of  natural  through  its  environment.  BACKGROUND  Although to  "defense  materials  to  subsurface  1.  a  A G E N T S ON  organizations  radwastes,  (bentonite)  *  CHELATING  date  on  numerous  the  gravels,  few  materials  under  studies  adsorption experiments  of  2 6  3 0 , 6 9  "  7 5  have  radionuclides  have  non-idealized  "  considered  conditions.  been  to  performed  soils,  adsorption The  sands to  prognosis  and  these for  a  A "defence in depth" philosophy u t i l i z e s m u l t i p l e b a r r i e r s to a r r e s t the r e t u r n of e s c a p e d r a d i o n u c l i d e s t o the biosphere.  51  radionuclide matrix  will  radionuclide  tend  completely  breached  t o reduce the  v i a two i n d e p e n d e n t  dense adsorbent  reduce active  has  but abuts a w e l l packed adsorbent  adsorbent  highly  that  the  groundwater  particle's  "tie-up"  of small flow  linear  movement  of  particle  size  the  This  released  well-packed,  will  drastically  r a t e and t h e r e f o r e d e c r e a s e t h e  velocity;  a n d b) t h e  adsorbent  the escaped n u c l i d e s through v a r i o u s  covalent  van  der  will  physicochemical  Waals  attraction,  bonding, e t c .  Unfortunately, the  attention. compounds  numerous m i t i g a t i n g f a c t o r s e x i s t  ability  radionuclides.  to  of t h e b a c k f i l l  These  For  interactions or  i s q u i t e good.  mechanisms: a) a  mechanisms s u c h a s i o n - e x c h a n g e ,  reduce  i t s solidifying  factors  instance,  have with  strong common  radionuclides.  Of  are  chelating  multidentate  tetraacetic  acid  to bind  released  only  received  cursory  ability  ionic,  fission  n e u t r a l i z e the geologic  material  have  the  of  secondary  products  media's a b i l i t y  p o t e n t i a l concern  (EDTA),  agents  such  as  in  use  essentially  ubiquitous.  A  study  recent  2 6  complex t o impair these Industry  ethylenediamine-  diethylenetriaminepentaacetic  compounds  their  or  t o the Nuclear  many  detergents,  dissolved  to attenuate  acid  these  some  may s e r v e  (DTPA) o r c y c l o h e x a n e d i a m i n e t e t r a a c e t i c of  t h a t may  for  are  used  radioactive  (CDTA).  acid Since  conjunction  with  decontamination  h a s shown a 20,000 f o l d  decrease  is  i n the  52  adsorptive presence result,  capacity of  many  migration the  soil In  6 0  Co  may  bind  above  complexing acids,  complexed  complex  Due  to  was  an  synthetic  granite  in  6 0  acids,  geologic  Co,  were 1  3  7  Cs  was  As  a  high  ability  of  ligands  organics  may  humic  various  act  and  as  fulvic  microbially-  hydroxamate  simplest  amino  other and  8 5  and  deionized,  conditions,  enhanced due  to  and  acid,  may  i f so, that  of  to  compound), demineralized a l l  to  illustrate  to  determine  that  solutions  Turco  would  that  its  show  gabbro (a  SCSSS, water.  if  employed  bentonite,  EDTA,  of  action,  directly  experiments Sr  migration  microbial  designed  and  runs  presence  Groundwater*  The composition of S o l u t i o n ) and G r a n i t e  media  those  decontamination  real  EDTA.  decreased  as  for  effect  radioactive  simulate  and  the  experiments  the  the  abnormally  include  such  observable  of  to  multidentate  organics  potential  populations  adsorption  of  showing the  due  2 6  glycine,  Accompanying  microbial  and  of  Co  radionuclides.  this  set  following  magnitude.  *  waste  the  6 0  naturally occurring  Even  through  the  Co.  These  radionuclides  there  plumes  biochemicals 2 7  for  concentrations  6 0  the  - many  polyhydroxamate. to  to  shale  a t t r i b u t e d to  dicarboxylic  generated  serve  be  agents.  many  low  contaminant  addition  mentioned  Conasauga  extremely  rates to  of  common Granite  In  order  to  contained  SCSSS (Standard Canadian S h i e l d Saline Groundwater i s d i s c u s s e d i n Appendix B.  53  microbial (after  populations  1 week's  combined Turco,  microbes  interrelated.  2.  METHODS  listed  1.0  g  granite)  (  6 0  independent i n Tables  of  was p l a c e d  experiments  of  1 3 7  III-X  Cs,  8  5  Sr-  1  3  7  Cs)  runs  following.  and mixed  "super  Q"*  week's  of s e t A or D described  IV). of to  Standard 6 0  Co  and  1  3  a l l samples  initial tube  total  was t h e n  solutions 7  Cs  or  8  5  Sr  of  6  °Co,  and  not containing activity sealed  with  1  3  7  1 3 7  Cs  Cs,  mesh  were  SCSSS,  parafilm  or  HN0 ) 3  Sr  earlier or  then  and allowed  (1  (see Section  a  combination  added  1.05 X  Granite  material  leachant material  not exceeding  and  gabbro  i n 6N  leachant  8 5  compared  determination,  40-50  water,  or the  of  14.8 m i s o f a d s o r b a t e  EDTA,  contact)  Turco**  be  (10 m i n u t e s  Groundwater,10" M 5  o f EDTA,  performed  F o r each  with  the  effect  could  were  solution From  ( o r enhanced)  i n an a c i d - w a s h e d tube  IV.  the effect  (Fisher-bentonite,  test  consisting  Co-  the leachant  i n Section  experimental  adsorbent  polypropylene  from  and the a n t a g o n i s t i c  and  are  of, these  cations  Eight  taken  contact) mentioned  results  competing  were  (0.2 m i s )  to 10"  1  yield uCi.  to rotate  *  an Each  on  a  " S u p e r Q" w a t e r i s w a t e r t h a t h a s b e e n d i s t i l l e d , deionized, m i l l i p o r e f i l t e r e d and passed through a c t i v a t e d carbon. * T u r c o i s a common decontamination solution containing 6.0 w t . % d i a m m o n i u m h y d r o g e n c i t r a t e , 2.5 w t . % o x a l i c a c i d a n d 1.0 wt.% phenylthiourea. This solution was diluted to a diammonium h y d r o g e n c i t r a t e c o n c e n t r a t i o n o f 10" M. 5  54  Scientific Agitation grain  Industries was  abrasion.  termination via  continued  of each  each  (test  of this  control  were  an  a r e shown  termination  collected,  activity that  phase  evaluate in  6 0  to  Co  were  only)  i n Table  1  3  7  Appropriate were  II)  The  run  with  nutrient had  set-up  Cs.  Upon  separated  the e f f e c t  r u n was and  minimize  20-25°C.  Section  on  consisting results  of  IX.  described  was  Where  0  in polypropylene  y-spectrometer and  in Section  to c o n v e n t i o n ,  evaluated  C  of c e n t r i f u g a t i o n  placed  background  According  of  To  with  from  and adsorbent  experimental  spiked  RPM  rotater.  f o r 60 m i n u t e s .  reported  entire  group  multi-channel  the  ranged  RPM  group.  5  151  ANALYSIS  Upon  K^,  15,000  Model at  radionuclide + liquid  n u t r i e n t media  3.  at  (composition  adsorptivity,  hours  run adsprbate  experimental  media  f o r 48  Temperature  3 0  centrifugation  controls  Incorporated  is  as  count  and M  time  mis of  vials  supernatant  and counted  Section remained  IV.  on a  The  unchanged  y-  (from  IV) f o r a l l a n a l y s e s . the  3 0 1 7 6  distribution  according  to the following  KD  =  (ml/g)  i s t h e mass  coefficient,  formula:  ( C n - Ce ) ( V ) (Ce )(M)  the radionuclide concentration  radionuclide concentration liquid  per  6.0  Eqt.V.1  initially,  at equilibrium, V  of adsorbent  Ce i s  i s t h e volume  material.  55  Evaluation numerical between good  the  of  conditions  initial through  the  minimize Cs  decreased the  net  effected that  K 's D  from  C  contained Since of  a  C  available Section  of  0  net  activity IV)  no  run  each  yields  a  radionuclide  method  allows  adsorbent  or  for other  of  each  contained except  the  from  10"" M E D T A 5  of  of  cobalt  expressed K 's  for  B  6 0  Co  an  these  vessel  was  identical  adsorbent. runs  that  walls  some  occurred.  was  added  to  EDTA  in  control  tubes  walls.  Since  to  by  components for  reaction  presence  radionuclide  the  K )  the  vessel of  6  were  6 0  Co  6 0  Co  is  calculated  and  greatly from  a  C  0  EDTA.  microbial  was  solution.after with  a l l  0  solutions  a  The  (as  of  This  as  evident  to  adsorption  by  that  became  effect,  adsorption  phase.  results  sets  adsorption  the  solid  controls  controls.  every  distribution  concentration  i t  this  for  change.  experimental  radionuclide  7  the  intercomparison  Unfortunately,  3  for and  evaluated  1  equation  liquid  The  To  this  expression  experimental  to  of  the  biomass  containing available of  an  treatment  as  solution that  between  radionuclides  population  and  specific  adsorbed  adsorbent.  were  of  Thus,  remaining  to  free  resolve the  the  (from  i n Methods  will  a l l  evaluated  leachant  earlier  alteration  species,  activity.  activity  described  This  various  cultures  (unadsorbed)  difference  the  adsorb  active  active  evaluated  adsorbent.  may  in but the  microbial  56  4.  RESULTS  AND  Tables than  that  was  much  DISCUSSION  III-V  o f any o t h e r more  adsorbent,  although  reported  by Means  decreased  D  with  1900  and C r e r a r . on  due  1  3  7  Cs  with  metals  2 6  fold  As  6 0  and  Co  was  in  but  EDTA 8  5  Sr  s i n c e EDTA  other  than  transuranics,  K .  had had does  rare  this  EDTA  a granite  i s i n accordance expected,  higher  of  with  decrease  However,  anything  or  cobalt  adsorption  t o EDTA.  complexes  transition  a  of  However, t h e e f f e c t  not as dramatic,  effect K 's  adsorption  nuclide.  i t elicits  negligible  that  pronounced  result,  strong  indicate  effect  0  This  with  that  only  a  slightly not  form  earths, may  be  expected. The greatest to  relative  effect  for  i n which  bentonite  8  5  Sr  was  Sample Bentonite Gabbro Granite Bentonite+EDTA Gabbro+EDTA Granite+EDTA Bentonite+Turco Control  of an  Turco 11  fold  on  decreasing  decrease  K  was  D  in adsorption  observed.  CoUCi/ml) 2.051 X I O " 4.508 X 1 0 " 1.493 X 1 0 ' 3.068 X 1 0 " 1.050 X 1 0 9.813 X 1 0 " 2.908 X l 0 1.016 X 1 0 " 6 0  K 7.41 3.23 1.01 4.82 0.00 5.25 5.22 D  4  3  3  3  1  2  a  1  Table  III -  6 0  Co  ADSORPTION  DATA  X X X X X X  57  Sample Bentonite Gabbro Granite Bentonite+EDTA Gabbro+EDTA Granite+EDTA Bentonite+Turco Control  Cs(„Ci/ml) 1.643 X 1 0 7.325 X 1 0 " 4.615 X 1 0 ' 1.695 X 1 0 " 7.513 X 1 0 ' 3.154 X 1 0 1.899 X 1 0 " 8.41.9 X 1 0 " 1 3 7  3  3  3  3  3  3  IV -  Sample Co,Cs+Bentonite Sr,Cs+Bentonite Co,Cs+Gabbro Sr,Cs+Gabbro Co,Cs+Granite Sr,Cs+Granite  1  3  7  Cs  ADSORPTION  2.23 3.44 1 .88 1 .96 2.02 8.51 1 .90  X X X X X X X  DATA  K  Sr(„Ci/ml) 6.975 X 1 0 " " 3.164 X 1 0 " 4.619 X 1 0 " 7.931 X 1 0 " " 1.028 X 10" 1.036 X 1 0 " 7.625 X 1 0 ' 1.042 X 1 0 " 8 5  0  2  2  1  1  3  1  Table  Sample Co,Cs+Bentonite Sr,Cs+Bentonite Co,Cs+Gabbro Sr,Cs+Gabbro Co,Cs+Granite Sr,Cs+Granite Co,Cs(Control) Sr,Cs(Control)  X X X X X X X  2  Table  Sample Bentonite Gabbro Granite Bentonite+EDTA Gabbro+EDTA Granite+EDTA Bentonite+Turco Control  K 7.54 1 .57 2.59 7.30 1 .53 3.85 6.50 D  3  V  -  e oC o U C i / m l ) 1 .757 X 1 0 " " 1 .7 6 6  X  10"  3  7. 181  X  10-"  1 .224  X  I0"  6 0  Co K 3. 50 X 1 O  8. 46  Table  X X  VI  10  3  2  1O  5  Sr  ADSORPTION  1  CsU 8 .650 8 .906 2 .066 2 .481 1 .824 2 .024 2 .508 3 .658 1  0  3. 35  a  8  2  3 7  Cs 8 .71 8 .45 3 .56 2 .94 4 .05 3 .64  - COMPETING  DATA  Ci/ml) X I0" X 10-" X 10" X 10" X 10~ X 10" X 10" X 10"  X X X X X X  5  Sr UCi/ml)  4 .199 X  10""  1 .403 X  10'  2  2 .141  X  10"  2  1 .743 X  10"  3  3  3  3  3  3  2  K  3 7  8  a  8 0  10 10 J 0 10 10 10  5  Sr  K  0  2  2  1 .83 X  10  3  4 .03 X  10  1  2 .13 X  10  1  2  2  2  2  ION A D S O R P T I O N  DATA  10 10 10 10 10 1 0 10  58  Sample Co,Cs+Bentonite + G r a n i t e G/W Sr,Cs+Bentonite + G r a n i t e G/W Co,Cs+Granite + G r a n i t e G/W Sr,Cs+Granite + G r a n i t e G/W Co,Cs+Bentonite + S C S S S G/W Sr,Cs+Bentonite + S C S S S G/W Co,Cs+Granite + S C S S S G/W Sr,Cs+Granite + Granite G/W  1.774  7.550  8.181  2.236  Sample Co,Cs+Bentonite + G r a n i t e G/W Sr,Cs+Bentonite + Granite Co,Cs+Granite + G r a n i t e G/W Sr,Cs+Granite + Granite Co,Cs+Bentonite + S C S S S G/W Sr,Cs+Bentonite + S C S S S G/W Co,Cs+Granite + S C S S S G/W Sr,Cs+Granite + Granite G/W  Table VII  Co(„Ci/ml)  6 0  6 0  Co  3.47  8.04  7.40  1.26  -  X 10""  X 10-"  X 10"  X 10"  K  4  2  3 7  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 0  X 10  X 10  X 10  X 10  3  2  2  2  ADSORPTION  CsUCi/ml)  3 7  Cs  6. 91  8 5  Ko X  10  Sr(„Ci/ml)  4.911  X 10""  3.870  X 10"  2  5.022  X 10"  2  5.279  X 10"  2  B 5  Sr  K  D  2  7. 27 X  1 o  2. 10 X  10  2  84 X 1 .  10  2  5. 57 X  10  1  5. 52 X  10  1  2. 18 X  10  1  2. 39 X  10  1  2  DATA FOR C O M P E T I N G GROUNDWATERS  1.57  X 10  5.06  X 10°  4.55  X  3  10"  1  0.00  IONS  IN SELECTED  59  Sample CoUCi/ml) S e t A + B e n t o n i t e 3.955 X 1 0 " Set A+Gabbro 1.490 X 1 0 " Set A+Granite 4.411 X 1 0 " " S e t A ( C o n t r o l ) 8.838 X 1 0 "  Cs(„Ci/ml) 7 . 7 6 3 X 10"" 1 .902 X 1.0' 9.788 X 10"" 2.359 X 1 0 ~  6 0  1 3 7  a  3  3  3  Sample Set A+Bentonite Set A+Gabbro Set A+Granite  6  CoK 3.20 X 7.40 X 2.86 X 0  6  J i  6  10 10 10  2  1  2  VIII  Sample °CoJ S e t C + B e n t o n i t e 2.001 Set C+Gabbro 5.815 Set C+Granite 6.030 S e t C ( C o n t r o l ) 5.631  Table  1  o  Table  Sample Set C + B e n t o n i t e Set C+Gabbro Set C+Granite  2  1  3  3  IX - ADSORPTION  Sample °Co(pCi/ml) S e t D + B e n t o n i t e 1.949 X 1 0 ' Set D+Gabbro 7.781 X 1 0 " Set D+Granite 7.819 X 1 0 " S e t D ( C o n t r o l ) 1.135 X 10" °Co K 3.96 X 0.00 0.00  Table  2  2  DATA  7  K X 10 X 10" X 10~  3  2  2  2  0  1  1  1  NUTRIENT MEDIA  Cs(„Ci/ml) 6.519 X 1 0 " 1.795 X 1 0 ~ 1.836 X 1 0 ~ 3.062 X 1 0 " J  3  2  3  2  U  1  D  2  1 3 7  3  ft  6  3  DATA' FOR  6  Sample Set D+Bentonite Set D+Gabbro Set D+Granite  10 10 10  A ADSORPTION  C s 8.93 2.44 5.97  1  1  0  C s (nCi/ml) 1.867 X 1 0 " 1.278 X 1 0 ' 1.249 X 1 0 " 1.299 X 1 0 "  3  D  K X X X  3 7  3  0  10  7  - LEACHANT  CjVml) X 10" X 10' X 10" X 10~  C o K 2.72 X 0.00 0.00  C s 4.41 1.71 3.47 3  Cs K 2.90 X 1 0 9.94 X 1 0 " 6.35 X 1 0 "  3  7  0  10  1  X - LEACHANT  1  1  1  D ADSORPTION  DATA  CONTROL  60  The are  reported  highest 1 3 7  competing  in Table  and  gabbro.  three  adsorbents  from  their  granite  and  of  both  greatest  it  effect  on by  adsorbent  for  adsorptive leachant  tested  granite  on  group  showed  (for  of As  6 0  while  that  due  to  a  VIII  presents  for  the  by  the  bentonite  was  f o r gabbro  and  non-competitive  K .  data  relating  In e v e r y  B  case  granite)  (SCSSS)  This  and  radionuclides  ( b e n t o n i t e and  K„.  the  Co  evidenced  of  Cs  1 3 7  D  conductivity  decreasing  Sr  d i f f e r e n c e in K 's  ions  Table  8 5  bentonite  capacity  (perhaps  the  has  higher  the  figure  is  the  s a t u r a t i o n of a v a i l a b l e  active  sites  by  non-active  i n the  highly  ions present  brine. showed a g r e a t l y r e d u c e d  that  leachant  contacted found  (JJIW) o n l y  with  was  deionized,  demineralized leachants  A  for  C  adsorptivity  in leachant  g r a n i t e and  reduction  of  and  counterpart.  highest  c a p a c i t y of A  Cs  by  each  radionuclides contained  appears  effect  relative  adsorbents the  Bentonite leached  1 3 7  followed  competing  with  concentrated  on  s y n t h e t i c g r o u n d w a t e r s on  explained  the  Co  adsorptive  increased  effect  6 0  In a l l c a s e s  for adsorption).  groundwater  on  the  the  was  for  easily  The  decreased  VI,  by  mechanism the  VI.  non-competitive  in Table  decreased  to  of  adsorptive capacity  Cs)  data  effects  D  slightly  gabbro.  gabbro K 's  or  D  In  on  the  D.  this 6 0  Co  and  the  However,  perturbed the  the  case  of  a < 2  fold  leachant  and  granite,  between  water c o n t a i n i n g and  A and  for  1 3 7  Cs.  adsorption  of  The these  61  radionuclides  to  adsorptivity contained by  of both  evidenced  5.  by  gabbro  significant.  f o r the  d e c r e a s e d more  present  in  values reported  0  is  and granite  C o r D was  agents  the R  or  gabbro  i n leachant  the complexing  XXXIII  granite  the  two  The  radionuclides  than  100  times  solutions  i n Tables VI,IX  (as  and X ) .  and XXXIV.  REMARKS  The  effect  otherwise)  may  radionuclides evidenced 10" M  from  cause  leaching  not  major strong  a  from  the results,  can decrease  5  did  of complexing  a R  decrease  constituent  D  reduced a nuclear strong  (whether  synthetic  attenuation waste  chelating  of  agents  0  a s much  (diammonium agent  as  a s EDTA,  hydrogen EDTA.  or  waste  repository.  As  present at  by up t o 3 o r d e r s o f m a g n i t u d e .  K 's  a complexing  agents  Turco  p r o b a b l y because i t s citrate)  i s  not  as  62  VI.  Throughout for  microbial  under  as  that few  were  idealized expected  in  of  these  maintained  at  environment a  full-scale  experiments, a  of  level a  conditions  only  possible  laboratory.  low-level  The  repository  are  follows:  a)  a  moderately  low  b)  a  low  atmosphere  c)  devoid  Since the  course  growth  the  conditions  the  CONCLUSION  of  any  microbial  i t i s assumed  presence would  oxygen  temperature  of  be  an  that  unusually  bacteriocidal  (approaching  O.Oppm 0 ) ;  and  2  growth.  water  high or  (<20°C);  will  salt  f i l l  content  bacteriostatic  the may for  repository, be  expected  a l l  but  a  halophiles. In  addition  to  constraint  that  repository  conditions  culture  that  may  i s capable  the  conditions  inhibit i s the of  the lack  listed  above,  microbial of  utilizing  an  initial  various  a  fourth  growth  under  contaminating  hydrocarbons  as  a  63  substrate. Also, of  the  oxygen  low  will  environment. these  serve  Even  conditions  source,  the  oxidation In  of  repository culture The  rate  bitumen) to  that  may  i s the  requires  a  molten  bitumen-waste  bitumen  bitumen  steel and  contaminating the  most  alkane  temperature  the  microbes  easily  on  metabolized 3)  microbial  create  then  the  anhydrous  contamination  rate  of  a  with  bitumen  placed  1) 2)  The in  the  a  molten kill  any  volatilize  bitumen  environment;  during  under  175°C.  will:  the  fourth  substrate.  both  of  a  contaminating  as  bitumen;  components  carbon  growth  be  of  container  an  above,  initial  effect  near  under  slow.  approximately will  The  or  sole  radionuclides  mixture  impermeable  an  lack  hostile  therefore  hydrocarbons  of  and  survive  microbial  of  waste  container.  fraction);  prevent  various  of  (and  listed  the  lack  could their  extremely  inhibit  utilize  as  metabolism be  pressure  microbially  organisms  conditions  may  high  a  bitumen  their  the  solidification  stainless  various  would  conditions  (<20°C),  create  utilize of  that  to  if  and  addition  constraint  temperature  storage  (light and  or  4) final  disposal. As the net the  illustrated  anticipated growth  of  overall  a  by  the  results presented  background microbial  genotype  of  in  radioactivity will  population. the  Changes  population  as  Section  III,  not  affect  the  may  occur  to  a  r e s u l t of  an  64  increased  rate  organisms  will  repository  found,  result  of  mutation.  not  change  However, due  microbially a  enhanced  significant  microbial  complexation  action  and/or  but  proliferation  all  enhanced  migration  microbial  action  nuclides  chelated  A in  This  of  prior  to  influence  may  be  turn  to  would  due the  to  any  basis  microbial  action  should  be  factors  such  agents)  would  serve  of  viable  expected  these  on  small. as  to  under  waste be  a  short-term  this  or  effect.  Also,  radionuclide  due  to  migration  of  by  (provided  the  complex  population as  a  present  metabolite.  enhanced  radionuclide  reactions. experiments,  radioactive attack  chelation  agents.  to  or  complexes  chelation  secondary  a  any  "swamped"  decrease  as  limited,  microbial  microbial  diffusion  "swamp"  highly  was  observed  is  be  a  bitumen  was  0  will  long-term  If  K  from  synthetic  organic  previous  of  in  conditioning  of  utilize  leaching  to  probably  secondary  migration On  would  labile).  in  radiation  due  of  thermally  situ  number  i t s importance  chelation  microbial  not  the  decrease  since  is  to  the  conditions.  Although not  of  (to  waste  does  the  disposal  occur,  synthetic  effect  other  chelating  65  BIBLIOGRAPHY  1.  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Fried,S., by R o c k " ,  e t a l . , " R e t e n t i o n of P l u t o n i u m and Americium S c i e n c e , V o l . 1 9 6 , (1977) pp.1087-1089.  71.  de M a r s i l y , G . , e t a l . , " N u c l e a r W a s t e D i s p o s a l : Can Geologist Guarantee I s o l a t i o n ? " , Science, Vol.197, No.4303, (1977) pp.519-527.  72.  S e i t z , M . G . , e t a l . , " S t u d i e s Of N u c l e a r - W a s t e M i g r a t i o n In G e o l o g i c M e d i a , A n n u a l R e p o r t , November 1976-October 1977", A r g o n n e N a t i o n a l L a b o r a t o r y , Rep.ANL-78-8, (1978)  73.  M e a n s , J . L . , e t a l . , " A d s o r p t i o n o f Co a n d selected a c t i n i d e s b y Mn a n d F e o x i d e s i n s o i l s a n d sediments", G e o c h i m i c a and C o s m o c h i m i c a A c t a . , V o l . 4 2 , (1978) pp.1763-1773.  74.  S h e p p a r d , J . C . , e t a l . , " R e t e n t i o n o f R a d i o n u c l i d e s by M o b i l e Humic Compounds a n d S o i l Particles", Environmental S c i e n c e and T e c h n o l o g y , V o l . 1 4 , No.11, (1980) pp.1349-1353.  75.  Walton,F.B., et a l . , "Determination of N u c l i d e G e o l o g i c Media Reaction K i n e t i c s Using Mixing - C e l l Contractors", Submitted to Chemical Geology, June, 1981.  76.  Wilding,M.W., e t a l . , "Removal of Cesium and Strontium from F u e l S t o r a g e B a s i n Water" i n Advances In Chemistry S e r i e s 153 e d . M.H. Campbell (Washington: American Chemical S o c i e t y , 1976), pp.134-151.  the  71  A P P E N D I X A - O N T A R I O M I N I S T R Y OF T H E ENVIRONMENT A N A L Y S I S *  TEST/COLONY  A  B  C  D1  D2  Gram s t a i n Shape Spores Motility 30°C 20°C Catalase Oxidase  -  +  -  -  -  Rod  Rod  Rod  Rod  Rod  +  +  G l u c o s e OF (5 D a y ) Growth TSA  20°C 30°C 35°C 42°C  -  +  + +  -  + +  +  +  +  —  —  —  —  —  —  F  +  + + + +  + +  + +  -  + +  + + +  Weak  -  -  MacConkey Agar 30°C  Gr + LAC-  No G r  No G r  Gr + LAC+  Gr + LAC-  Skim Milk Agar  +  +  +  -  Weak  +  -  —  -  —  -  N i t r a t e (5 D a y ) Reduction  +(Gas)  Gelat inase  -  —  Growth Pigment Caseinase Flouresc.  —  — +  A r g i n i n e (5 Day) Dihydrolase Urease Citrate G r o w t h 6.5% N a C l ONPG  -  +(N0 ) 2  +  +(N0 ) 2  Weak +  -  growth  — -  +  —  -  "+" a n d " - " r e p r e s e n t  *  -  +  -  + +  + +  -  o r no g r o w t h ,  I n d e p e n d e n t a n a l y s i s was p e r f o r m e d d i s t i n c t species found i n C u l t u r e D  respectively.  f o r each  o f t h e two  72  Colony Morphology: TSA 3 0 ° C  A B  - Tan, d r y , w r i n k l e d . - Cream t o w h i t e , irregular, spreading, margin. C - T i n y , c i r u l a r , smooth, p a l e yellow. D1- C i r c u l a r , c r e a m , c o n v e x , s m o o t h , e n t i r e , margin. D2- C i r c u l a r , c r e a m , c o n v e x , s m o o t h .  73  APPENDIX  B - SYNTHETIC  STANDARD 1) T h e f o l l o w i n g a) 11.090 g b) 7.115 g c) 1.512 g d) 1.965 g e) 0.506 g f) 0.291 g  SYNTHETIC  GROUNDWATER  GRANITE  SOLUTIONS  GROUNDWATER"  s t o c k s o l u t i o n s w e r e made u p : MgSO,.7H 0 /25ml MgCl .6H 0 /25ml NaHC0 /25ml KOH /25ml KN0 /25ml KF /25ml 2  2  2  3  3  2) 0.10 m l o f ( a ) , ( b ) , ( c ) , ( d ) , ( e ) a n d ( f ) w e r e p i p e t t e d to a 2 L v o l u m e t r i c f l a s k . 1.00 m l o f ( c ) was a d d e d a n d t h e v o l u m e made u p t o 1700 m i s w i t h d e i o n i z e d w a t e r ( D I W ) . 0.048 g Ca(OH) was a d d e d t o a 200 m l v o l u m e t r i c f l a s k f i l l e d w i t h a b o u t 180 m i s o f DIW. C0 was b u b b l e d t h r o u g h t h i s m i x t u r e while s t i r r i n g u n t i l the solution became c l e a r . I t was t h e n f i l l e d t o t h e m a r k w i t h DIW a n d t h e c o n t e n t s o f t h i s 200 m l f l a s k a d d e d t o the 2 L v o l u m e t r i c f l a s k . T h e f i n a l 100 m l o f DIW was a d d e d t o t h e v o l u m e t r i c f l a s k t o make t h e v o l u m e u p t o 2.00 L a n d t h e solution was s t i r r e d f o r 24 h o u r s i n c o n t a c t w i t h t h e a t m o s p h e r e t o b r i n g t h e pH t o "6.5 + 0 . 5 . 2  2  74  STANDARD CANADIAN To a) b) c) d) e)  100.0 m i s 1.906 g 1.216 g 3.080 g 0.276 g 1.370 g  o f DIW  SHIELD  SALINE  the following KCl SrCl .6H 0 Na Si0 .9H 0 NaHC0 NaN0 2  SOLUTION  (SCSSS)""  dry chemicals  were  added:  2  2  3  2  3  3  10.0 m i s o f t h i s s t o c k s o l u t i o n was a d d e d t o a 2 L v o l u m e t r i c f l a s k a n d made u p t o 2.0 l i t r e s . 1 1 0 . 0 5 0 g C a C l . 2 H 0 , 4.056 g M g S O „ . 7 H 0 a n d 2 5 . 4 2 0 g N a C l w e r e a d d e d a n d t h e e n t i r e m i x t u r e was stirred thoroughly. 2  2  2  75  B A S A L T GROUNDWATER * 4  Stock The a) b) c) d) e) f)  Solution A f o l l o w i n g was 100 m l 8.000 g 5.485 g 0.994 g 1.490 g 0.232 g  T h i s s o l u t i o n was u p t o 200 m i s . T h e f o l l o w i n g was  c o m b i n e d i n a 200 m l v o l u m e t r i c DIW NaHC0 Na SO„.10H 0 MgSO,.7H 0 KC1 KF 3  2  2  2  stirred then  until  dissolved  combined  a)  1800 m l  DIW  b)  0.0109 g  CaS0„.l/2H 0  and  stirred  180 m l  b)  1.871  This To a) b) and  until  in a  2 L volumetric  in a  200 m l v o l u m e t r i c  made  flask:  dissolved.  then  combined  flask:  DIW g  was m i x e d  the s t i r r e d 4.0 m l 4.0 m l made  and t h e volume  2  Stock S o l u t i o n B T h e f o l l o w i n g was a)  flask:  CaCl .2H 0 2  until  2  dissolved  and the volume  made  2 L volumetric flask the following Stock S o l u t i o n A Stock S o l u t i o n B  u p t o 2.0  litres,  then  stirred  overnight.  up t o 2 L. was  added:  76  WN-1  Saline-Solution**  1) T h e f o l l o w i n g s t o c k s o l u t i o n was m a d e - u p i n a 200 m l volumetric f l a s k ( f i l l e d t o t h e m a r k w i t h DIW) a) b) c)  0.537 1.882 0.901  g g g  KCl NaHC0 NaN0  2)  2 0 . 0 m i s o f t h i s s t o c k s o l u t i o n was p i p e t t e d i n t o a 2 L volumetric f l a s k , the f o l l o w i n g d r y c h e m i c a l s added, t h e n made u p t h e m a r k w i t h DIW.  d) e) f) g) h) i)  0.056 0. 150 13.111 1 .232 9.520 1.282  3  3  g g g g g g  FeSO,.7H SrCl .6H CaCl .2H MgSO .7H NaCl Ca(OH) 2  2  a  2  2  2  2  2  0 0 0 0  77  APPENDIX  TEST A l TOTAL TIME DAYS  TOTAL ACTIVITY RELEASED MICROCURIES  C - LEACH  TEST  DATA  1-60 CUMULATIVE FRACTION LEACHED CM  FRACTIONAL RELEASED PERCENT  INCREMENTAL LEACH RATE CM/DAY  MASS LEACH RATE G/CM"»2*DAY  DIFFUSION COEFFICIENT CM"2/SEC  '•  0 686E-01  0 0623  0 284E-03  0 284E-03  O.384E-03  0 734E- 12  2.  0 1G4E*00  0 1495  0 682E-03  0 397E-03  0.537E-03  0 211E- 1 1  3.  0 200E*00  0 1822  0 831E-03  0 149E-03  0.201E-03  0 209E- 11  4.  0 226E*00  0 2056  0 937E-03  0 106E-03  0.144E-03  0 200E- 1 1  5.  0 244E+00  0 2220  0 101E-02  0 751E-04  0.101E-03  0 186E- 11  6  0 257E*00  0 2333  0 106E-02  0 512E-04  0.692E-04  0 171E- 1 1  7.  0 2G6E*00  0 2420  0 110E-02  0 399E-04  0.539E-04  0 158E- 1 1  14 .  0 295E*00  0 2677  0 122E-02  0 167E-04  0. 226E-04  0 967E- 12  21 .  0 355E»00  0 3227  0 147E-02  0 358E-04  0.484E-04  0 937E- 12  2B .  0 423E+00  0 3844  0 175E-02  0 402E-04  0.543E-04  0 997E- 12  . 35 •  0 476E+0O  0 4324  0 197E-02  O 312E-04  0.422E-04  0 101E- 1 1  42 .  0 541E*0O  0 4921  0 224E-02  0 389E-04  0.525E-04  0 109E- 1 1  49.  0 G22E*00  0 5656  0 258E-02  0 479E-04  0.647E-04  0 123E- 1 1  56.  0 717E*00  0 6515  0 297E-02  0 559E-04  0.755E-04  0 143E- 11  63.  0 796E*00  0 7240  0 330E-02  0 472E-04  0.638E-04  0 157E- 11  93.  0 1O8E*01  0 9800  0 447E-02  0 389E-04  0.526E-04  0 195E- 11  " Table  XI -  LEACH TEST  DATA  - T E S T S E T A1 -  6 0  Co  TEST A2 - 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. 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  0.137E-03  0 707E-10  0 . 174E+01  1.6373  0.738E-02  0 101E-03  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  0. 194E-03  0 257E- 10  7.  .  49 .  0.277E+01  2.6091  0.118E-01  0 144E-03  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 A 2 -  60  C  c  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  21 .  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  0 180E-O1  O 142E-03  0 191E-03  0 317E-10  Table  3.9937  XIII  - LEACH  T E S T DATA  - TEST  S E T A3 -  6 0  Co  TEST B l - C0-60 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 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  21 .  0 113E+01  1.2446  0 526E-02  0 114E-03  0 153E-03  0 120E-10  28.  0 125E+01  1 . 3798  0 817E-04  O 1 IOE-03  0 111E-10  35.  0 135E*01  1 .4806  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  -  ,  o o 626E-02 583E-02  LEACH TEST  DATA  -  TEST  S E T B1  -  6 0  Co  79  TEST  TOTAL TIME DAYS  TOTAL A C T I V I T Y RELEASED MICROCURIES  B2 -  CO-60  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  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  0.899E-02  0. G98E-04  0.942E-04  0. 105E-09  18E-02  0. 121E-09  7 .  0. 211E*0I  1.9943  14.  0 . 219E+01  2.0678  0-932E-02  0. 473E-04  0.638E-04  0  2 1 .  0. 226E*01  2.1288  0.959E-02  0., 393E-04  0.53  IE-04  0. 3 9 8 E - 1 0  28 .  0. 233E*01  2.1977  0.99  IE-02  0  444E-04  0. 599E-04  0. 3 1 9 E - 1 0  35.  0 . 239E+01  2.2528  0.102E-01  0  355E-04  0. 479E-04  0. 2 6 8 E - 1 0  42.  0. 244E*0I  2.2993  0.104E-01  0 . 299E-04  0. 404E-04  0. 2 3 2 E - 1 0  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  0.  0. 122E-  Table  TOTAL TIME DAYS  XV - L E A C H T E S T  TOTAL A C T I V I T Y RELEASED MICROCURIES  FRACTIONAL RELEASED PERCENT  DATA  CUMULATIVE FRACTION LEACHED CM  1 .  0 . 145E+01  1.3054  2 .  0 . 165E+01  1.4853  3.  0.  175E+01  1 .5759  0.723E-02  4 .  0.  179E+01  1 .6148  0.74  0.599E-02 . 0.68 IE-02  IE-02  -  984E-05  T E S T SET  INCREMENTAL LEACH RATE CM/DAY  133E-04  B2 -  MASS LEACH RATE G/CM*'2'DAY  564E-I0  6 0  Co  DIFFUSION COEFFICIENT CM«*2/SEC  0 .599E-02  0  810E-02  0. 326E-09  0  825E-03  0  112E-02  0. 2 1 1 E - 0 9  0  415E-03  0. 562E-03  0. 158E-09  0 .179E-03  0. 242E-03  0. 125E-09  0  0  5.  O.  181E+01  ».6292  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 . 7 8 13  0.817E-02  0. 399E-04  0. 540E-04  0. 2B9E-10  28 .  O.203E*01  1.8332  0.841E-02  O. 3 4 0 E - 0 4  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-  49.  0.220E+01  1.98 1 1  0.909E-02  0. 346E-04  0. 468E-04  0. 153E-10  747E-02  660E-04  10.  56.  0.230E+01  2.0692  0.949E-02  0. 577E-04  0 . 78 1E - 0 4  0. 146E-10  63.  0.234E+01  2.1088  0.967E-02  0. 260E-04  0 . 35 I E - 0 4  0. 135E-10  93.  0.246E+01  2.2163  0.102E-01  0. 165E-04  0. 223E-04  0. 101E-10  T a b l e XVI  -  LEACH TEST  DATA  10  - T E S T SET B 3 -  6 0  Co  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 0 802E- 10  5.  0. 153E*01  1.4965  0 664E-02  0 585E-04  0 790E-04  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  T E S T DATA  - TEST  SET  C1  -  6 0  TEST C2 - 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 .  0.47OE+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  0 162E-03  0.219E-03  0.206E-10  4.  0.695E+00  0,68 14  0.301E-02  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  0.8855  0. 392E-02  0 443E-04  0.600E-04  0.664E-11  o 410E-04  0.555E-04  0.573E-11  21 .  0.9O3E+O0  28 .  0.969E+OO  O.9504  0.4 20E-02  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  O.734E-02  0 370E-04  0.501E-04  0.777E-1 1  0.812E-02  0 260E-04  0.352E-04  0.645E- 1 1  63. 93.  1.6600  0.169E+01  1.8366  0.I87E+01  Table  XVIII  -  L E A C H T E S T DATA  -  TEST  SET C2  -  6  Co  81  TEST  -  CO-GO  FRACTIONAL RELEASED PERCENT  TOTAL A C T I V I T Y RELEASED MICROCURIES  TOTAL TIME DAYS  C3  CUMULATIVE FRACTION LEACHED CM  MASS LEACH RATE G/CM-»2*0AY  INCREMENTAL LEACH RATE CM/DAY  DIFFUSION COEFFICIENT CM**2/SEC 185E-09  1.  0 . 108E+01  0.9899  0  451E-02  0  45 I E - 0 2  0.610E-02  0  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  0  536E-02  O 484E-04  0.655E-04  0  523E-10  0  535E-04  0.724E-04  0  444E-10  5.  1.1772  0 . 128E+01  6 .  0 . 130E*01  1.1889  0  542E-02  0  547E-02  0  504E-04  0.682E-04  0  388E-10  7 .  0 . 131E+01  1 .2000  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-  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  0.776E-04  0  766E-11  56.  0  63.  0  93  n  1.5077  164E*01  6B7E-02  0 0  149E-04  0. 202E-04  0  702E-11  0  609E-05  0.824E-05 .  0  500E-11  167E+01  1 .5306  0  171E+01  .1 . 5 7 0 7  0  716E-02  XIX  - LEACH" TEST DATA  TEST  TOTAL TIME DAYS  0  573E-04  697E-02  Table  TOTAL A C T I V I T Y RELEASED MICROCURIES  Dl  -  10  -  TEST SET  C3  -  6 0  Co  CO-GO  FRACTIONAL RELEASED PERCENT  CUMULATIVE FRACTION LEACHED CM  INCREMENTAL LEACH RATE CM/OAY  MASS L E A C H 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  2 .  0.  I26E+01  1.2206  0. 544E-02  0.455E-03  0.613E-03  0.134E-09  3 .  0.  131E  1.27 1 1  0.566E-02  0.225E-03  0.303E-03  O.971E-10 0.751E-10  +01  O.226E-09  4 .  0.133E+01  1 .2905  0. 575E-02  0.864E-04  0. 1 16E-03  5.  0.  135E-»01  1.3109  0. 5 8 4 E - 0 2  0.91  0.  6 .  0.  137E+01  1 .3313  0. 593E-02  0.908E-04 O.792E-04  0.107E-03  0.469E-IO  0.373E-04  0.503E-04  0.255E-10  7 .  0.  139E*0t  1 .349 1  0.60  14 .  0.  1-I5C + 01  1.4078  0.627E-02  IE-02  IE-04  123E-03  0.620E-10  0. 122E-03  0.533E-1O  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.  35.  O . 159E+01  1 . 5427  0.687E-02  0. 162E-04  0.219E-04  0 . I 2 3 E - 10 0.107E-10  148E-10  42 .  0.  1G2E+01  1 .5767  0.702E-02  0.2 16E-04  0.291E-04  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- 11  63 .  0.173E*01  1.6793  O.748E-02  0. 802E-05  0.108E-04  0.807E-11  93 .  0.178E+01  L  0.769E-02  (XG95E-05  0.937E-05  0.578E- 1 1  Table  XX  7 361  - LEACH  TEST  DATA" -  T E S T ~ S E T D1  -  6 0  Co  82  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. 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 0  C  c  TEST D3 - CO-60 TOTAL TIME OAYS  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 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  Table  XXII  -  1  0 175E-04  L E A C H T E S T DATA -• T E S T S E T  D3  q 277E-11  .  60(  83  TEST A1 - 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. 2B9E*01  1.5712  0.716E-02  0 .716E-02  ' 0968E-02  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  0 .466E-09  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  Table  TOTAL TIME DAYS  XXIII  TOTAL ACTIVITY RELEASED MICROCURIES  -  L E A C H T E S T DATA  FRACTIONAL RELEASED PERCENT  CUMULATIVE FRACTION LEACHED CM  -  TEST SET  INCREMENTAL LEACH RATE CM/DAY  A1  0. 198E;10. . _ 1 3  DIFFUSION COEFFICIENT CM**2/SEC  MASS LEACH RATE G/CM"2*DAV  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  0. 276E-03  0.373E-03  0. 152E-09  49.  0 . 1 13E + 02  6 . 3448  0. 286E-01  56.  0.1P2E+02  6 . 8690  0 310E-0I  0. 337E-03  0.456E-03  0. 156E-09  7. 3066  0. 329E-01  0. 282E-03  0. 380E-03  0. 156E-09  UOE+02 0O,. 164E+02  9 . 2055  0. 415E-01  0 285E-03  0. 385E--9?.  0. 168E-09.  63 . 93.  Table  XXIV -  LEACH TEST  DATA -- T E S T S E T  A 2 -.  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 0.438E-09  3.  0 . 47SEKM  2 .6685  0 .120E-01  0 .388E-03  0 . 523E-03  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  0 507E*01  2 .8500  0 .128E-OI  0. 56 IE-04  0. 757E-04  0.107E-09  14. 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 - L E A C H  T E S T DATA  - TEST SET A 3 -  1  3  7  Cs  TEST Bt -CS-137 TOTAL TIME DAYS  TOTAL ACTIVITY RELEASED MICROCURIES  FRACTIONAL RELEASED PERCENT  CUMULATIVE FRACTIPN LEACHED CM  INCREMENTAL LEACH RATE CM/DAY  MASS LEACH RATE G/CM''2'DAY  DIFFUSION COEFFICIENT 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  -  T E S T SET  B1  _  13 7  85  TEST  TOTAL TIME DAYS  TOTAL A C T I V I T Y RELEASED MICROCURIES  B2  -  CS-137  CUMULATIVE FRACTION LEACHEO CM  FRACTIONAL RELEASED PERCENT  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 I E - 0 3  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  0. 201E-03  0. 308E-09  6 .  0 . 563E+01  3 . 1628  0 . 143E-01  0. 149E-03  1826  0. 143E-01  0. 892E-04  0. 120E-03  0. 267E-09  7 .  0 . 5G7E+01  3  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. 9 5 2 E - 0 4  0 .809E-10  •  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  3 . 7 307  0. 168E-01  0. 426E-04  0. 576E-04  0  0. 384E-04  0  519E-04  0 .474E-10  ',  35  49.  0  6G4E+01  5 2 4 E - 10  5G.  0  675E+01  3 . 7903  0. 171E-0I  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  TEST  TOTAL TIME DAYS  TOTAL ACTIVITY RELEASED MICROCURIES  - LEACH  B3  -  T E S T DATA  - TEST  S E T B2  CS-137  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 .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  0  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. 6 8 5 E - 0 4  0 . 6 7 7 E - 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 . 4 3 7 E - 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 . 3 2 5 E - 10  63.  0 . 585E+01  3  1428  0. I44E-01  0. 384E-04  0. 520E-04  0 . 3 0 0 E - 10  93.  0 . 621E+01  3. 3376  0. I53E-01  0. 298E-04  Table  XXVIII  1 3 7  - LEACH  T E S T DATA  925E-04  _  125E-03  . 0 . 403E-04  - TEST  0. 229E-10  SET B 3 -  1  3  7  86  TOTAL TIME DAYS  TOTAL A C T I V I T Y RELEASED MICROCURIES  FRACTIONAL RELEASED PERCENT  CUMULATIVE FRACTION LEACHED CM  INCREMENTAL L E A C H RATE CM/DAY  MASS L E A C H RATE G/CM*«2*DAY  DIFFUSION COEFFICIENT CM"2/SEC  1 .  0.290E>01  1.6936  0.752E-02  O  752E-02  0  I02E-0I  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  269E-03  0  364E-03  0.209E-09  4 .  0.324E+01  1.8951  0  103E-03  0  140E-03  0.161E-09  5.  0.326E*01  1.9091  0.83 IE-02 0.84 IE-02  0  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 1 0 E - 0 9  7 .  0. 329E+-01  1.9248  O.854E-02  0  359E-04  0  485E-04  0.948E-10  14 .  0. 3 3 5 E * 0 1  1.9610  0.870E-02  0  230E-04  0  310E-04  0.492E-10  2.1 .  0. 3 4 6 E + 0 1  2.0226  0.898E-02  0  528E-04  0.349E-10  28.  0.354E*01  2.0700  0.919E-02  0  39 IE-04  0  300E-04  0  406E-04  0 . 2 7 4 E - 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  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. 3 8 7 E + 0 1  2 . 2628  0.100E-01  0  390E-04  0  526E-04  0 . 1 6 4 E - 10  63.  0.397E+01  2.3199  0.103E-01  0  362E-04  0  489E-04  0.153E-10  2.4199  0.107E-01  0  148E-04  0.200E-04  0.113E-10  93.  0.414E+01  Table  XXIX -  LEACH TEST  TEST"C2  TOTAL TIME DAYS  TOTAL A C T I V I T Y RELEASED MICROCURIES  - CS-137""  FRACTIONAL RELEASED PERCENT  29 IE-04  DATA  •  -  TEST  SET C l  0.514E-O9  _  13 7  •  CUMULATIVE FRACTION LEACHED CM  INCREMENTAL LEACH RATE CM/DAY  MASS  DIFFUSION  LEACH RATE G/CM**2*DAY  COEFFICIENT CM-*2/SEC  1 .  0.103E+01  0.6035  0.  267E-02  0.267E-02  0.36  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.  0.349E-10  4 .  0.t36E+01  0.7986  0.353E-02  0.  5.  0.139E*01  0.8204  0.363E-02  0.963E-04  138E-03  IE-02  0.647E-10  375E-03  0.  187E-03  0.283E-1O  0.  130E-03  0.239E-10  128E-03  0.210E-10  6 .  0.143E+0I  0.84  19  0.372E-02  0.948E-04  0.  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.  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  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 . 3 7 13  0.606E-02  0.761E-04  0.103E-O3  0.597E- 1 1  63 .  0. 2 4 0 E + 0 1  1.4110  0.624E-02  0.250E-04  0.339E-04  0.562E- 1 1  93 .  0.  1 .5158  0.670E-02  0.  0.209E-04  Table  2T!8E*01  XXX  11  448E-02  155E-04  - LEACH T E S T DATA -"TEST SET C 2  _  0.439E-1 1  13 7Q  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  0.837E-02  0. 125E-03  0.169E-03  0. 159E-09  1.8500  0.843E-02  0.551E-04  0.746E-04  0. 129E-09  0. 34IE+01  1.8631  0.849E-02  0.597E-04  0.809E -04  0. 109E-09  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  0 .993E-02  0 .279E-04  0.377E-04  0 .1B3E-10  2.2976  0 .105E-01  0 .764E-04  0.103E-03  0 .178E-10  0 .223E-04  O.302E-O4  0 . 163E- 10  O .944E-05  0.128E-04  0 .11GE-10  4. 5. 6. 7.  49. 56.  0. 336E+01 0.339E+01  0. 399E+01 0 420E+01  1 .8379  2.1803  63 .  0 427E+01  2.3319  0 .106E-01  93.  0 .438E+01  2.394 1  0 .109E-01  T a b l e XXXI  - LEACH TEST DATA - TEST SET C3  _  13 7  Cs  TEST 01 - CS-137 TOTAL TIME DAYS  TOTAL ACTIVITY RELEASEO 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.  0.3 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  0.288E-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  Table  0. 1 11E-01  XXXII - LEACH TEST DATA - TEST SET  0. 139E- 10  D1  _  1 3y  Cs  88  T A LR TE OL TE AA LSEDACTIVITYRELEASF R R A CTIOR NATEI ENTR AL TO IT M E E DACTIONALLEC AM CHC EU DMULATIVELC EF A/ CD HA LN EC AR CE HM ATEC O E" F2 F/ IS CE IE NT. O A Y S M I C R O C U R I E S P E R C E N T M Y G / C M « * 2 ' D A Y C M C 1 .03G8E+01 21138 0942E-02 0942E-02 0127E-01 0807E-09 2 .04 1 1E*0123629 0105E-01 0111E-02 .15 0 0E-02 0504E-09 3. 0434E+01 24947 0111E-01 0587E-03 0794E-03 0375E-09 4 .044SE+01 25577 0114E-01 0281E-03 0380E-03 0295E-09 5. 0456E+01 26 ISO 0117E-01 0269E-03 0363E-03 0248E-09 6. 04S0E+01 26447 0118E-01 0119E-03 0161E-03 021 1E-09 7 .0464E+01' 26665 0119E-01 0971E-04 0131E-03 0183E-09 14. 0484E+01 27815 0124E-01 0732E-04 0990E -04 0998E-10 21 .0505E+01- 29004 0129E-01 0757E-04 0102E-O3 0723E-10 26. 0517E+01 29691 0132E-01 0437E-04 059 IE-04 0569E- 10 35. 0530E+01 30436 0136E-01 0474E-04 064 IE-04 0478E-10 42 . 0539E+01 30973 0138E-01 0342E-04 0463E-04 0412E-10 49. 0553E+01 31764 0142E-01 0504E-04 0682E-04 0372E-10 56. 0 32207 0 0282E-04 0382E-04 0335E- IO 63 . 05R5F.*01 32468 0145E-01 0166E-04 0224E-04 0302E-10 9T3.a b l e05nOE 1X I I I 3-3314 I4T8EE-0S1T DATA0126-E-04T E S0 70E 04T D20216-E-10 X* X0 L E A C H0 T1 SE BSOE+OI  144E7OI  1  TELF D 3 SE 1 3 7 FF US IO NENT MM AE S S AE LLEASE AD CTIVITYTESR R A C T IONAL CL C U M U LATIVE FR RE N TALRATD T O T A LTOTR H EI C E A S E D A C H LA EC AT CI HONRATEINC T I M E GL /E CA MC " 2'0AY CO ME *F »F 2I /C SI EC D A Y DAYS MICROCURIES PERCENT CMED CM/ 1 .0111E*01 0.6547 0.290E-02 00 290E-02 0390E-02 0762E-10 2. 0136E*01 0.8022 0.355E-02 0 652E-03 O878E-03 0 572E- 10 3. 014BE*0I 0.8709 0.385E-02 0 304E-03 0409E-03 0 449E-10 4. 0154E+01 0.9087 0.402E-02 0 167E-03 0225E-03 367E-10 5 .0160E*01 0.9405 0.416E-02 0 141E-03 0189E-03 0314E-10 6. 0164E+01 0.9647 0.427E-02 0 107E-03 0145E-03 0276E-10 7 .0I70E*01 1.0014 0.443E-02 0 162E-03 0219E-03 0255E-10 14 .0 195E*01 t.1450 0.506E-02 907E-04 0122E-03 0166E-10 21 .00 214E*01 1.2616 0.558E-02 00 736E-04 0991E-04 0135E-10 28 .0 230E+01 1.3550 0.599E-02 0 590E-04 0795E-04 0117E-10 35. 243E*01 1.4309 0.633E-02 479E-04 0645E-04 0104E-10 42 .00 25GE*01 1.5071 0.666E-02 00 482E-04 0648E-04 0961E-11 49. 0 278E+01 1.6351 0. 723E-02 0 808E-04 0109E-03 00970E-11 56. 0 289E*01 1.6986 0.751E-02 0 40 IE-04 0540E-04 916E-11 63. 0 295E*01 1.7377 0.76BE-02 0 247E-04 0333E-04 0852E-11 13E 0 .84L40 .T81E5ES-0T2 DATA 1-57E-0T4E S T02S11EE-T04D30650E-11 T a b l e3 X+ X1 X I V -1 EACH0 6  _  13 7  89  APPENDIX  D  - LEACHANT  Initial  CONDUCTIVITY  AND  PH  Final 1 Week's c o n t a c t  Set A pH Conductivity  4.10 1.00  X  lO- Mho/cm  5.80 4.90 X  Set B pH Conductivity  6.39 4.80  X  l0" Mho/cm  6.25 6.5 X  l0- Mho/cm  Set C pH Conductivity  6.39 4.80  X  lO" Mho/cm  5.65 5.5 X  10- Mho/cm  Set D ph Conductivity  5.62 1.85 X  lO- Mho/cm  4.99 1.95 X  6  3  3  2  10""Mho/cm  3  3  10" Mho/cm 2  90  APPENDIX  E - A N A L Y S I S OF V A R I A N C E OF Co AT T>14DAYS 6 0  e oC o : Set Mean A 0.0083 B 0.0087 C 0.0064 D 0.0064 F  St E r r o r 0.0010 0.0003 0.0003 0.0003  1 3 7  Cs~SAMPLE  MEANS  95% C o n f i d e n c e 0.0064 0.0080 0.0059 0.0057  I n t e r v a l f o r Mean 0.0103 0.0094 0.0070 0.0071  95% C o n f i d e n c e 0.0156 0.0108 0.0074 0.0093  I n t e r v a l f o r Mean 0.0225 0.0140 0.0092 0.01.1 7  Ratio=4.856  Homogenous Subset  Subset Group Mean  1 3 7  Set A B C D  subsets:  1  Group Mean  F  St Deviation 0, 0 0 5 0 0. 0 0 1 8 0. 0 0 1 3 0, 0 0 1 8  AND  Set D 0.0064  Set C 0.0064  Set A 0.0083  S e t B. 0.0087  2  Cs: Mean 0.0190 0.0124 0.0083 0.0105  St  Deviation 0.0087 0.0040 0.0022 0.0031  St E r r o r 0.0017 0.0008 0.0004 0.0006  Ratio=21.756  Homogenous Subset Group Mean  Subsets:  1 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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