Radionuclide behaviour in the natural environment docx

© Woodhead Publishing Limited, 2012
Radionuclide behaviour in the natural environment
© Woodhead Publishing Limited, 2012
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© Woodhead Publishing Limited, 2012
Woodhead Publishing Series in Energy: Number 42
Radionuclide
behaviour in
the natural
environment
Science, implications and lessons for
the nuclear industry
Edited by
Christophe Poinssot and Horst Geckeis
Oxford Cambridge Philadelphia New Delhi
© Woodhead Publishing Limited, 2012

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Contributor contact details xiii
Woodhead Publishing Series in Energy xix
Foreword xxv
1 Overview of radionuclide behaviour in the natural
environment 1
C. Po i n s s o t , French Nuclear and Alternative Energies Commission
(CEA), France and H. Ge c k e i s , Karlsruhe Institute of Technology
(KIT), Germany
1.1 Introduction 1
1.2 Radionuclides of interest 2
1.3 Environmental compartments to be considered 5
1.4 References 10
Part I Radionuclide chemistry in the natural
environment 11
2 Fundamentals of aquatic chemistry relevant to
radionuclide behaviour in the environment 13

T. ne u m a n n , Karlsruhe Institute of Technology (KIT), Germany
2.1 Introduction 13
2.2 Composition of natural waters 14
2.3 Dissolution and precipitation 16
2.4 Aqueous complexes 24
2.5 Surface sorption 27
2.6 Colloids 34
2.7 Redox reactions 35
2.8 References 41
Contents
© Woodhead Publishing Limited, 2012
vi Contents
3 Aquatic chemistry of the actinides: aspects relevant
to their environmental behavior 44
M. al t m a i e r , Karlsruhe Institute of Technology (KIT), Germany
and T. Ve r c o u t e r , French Alternative Energies and Atomic Energy
Commission (CEA), France
3.1 Introduction 44
3.2 Oxidation states of actinides in aqueous solution 46
3.3 Actinide solid phases and solubility phenomena 52
3.4 Actinide complexation reactions 56
3.5 Chemical modeling tools and thermodynamic databases 64
3.6 Recommended literature 65
3.7 References 66
4 Aquatic chemistry of long-lived mobile fission and
activation products in the context of deep
geological disposal 70
A. ab d e l o u a s and B. Gr a m b o w , École des Mines de Nantes –
SUBATECH, France
4.1 Introduction 70

4.2 The effects of the near eld in high-level radioactive
waste disposal 73
4.3 Solution and interfacial chemistry of selected
radionuclides 77
4.4 Summary 92
4.5 References 93
5 Impacts of humic substances on the geochemical
behaviour of radionuclides 103
P. E. re i l l e r , French Nuclear and Alternative Energies
Commission (CEA), France and G. bu c k a u , Institute for
Transuranium Elements, Germany
5.1 Introduction to humic substances 103
5.2 The ‘humic acid molecule’ 106
5.3 Discrete models of metal ion–humic interactions 110
5.4 Multiligand and macromolecular models of metal
ion–humic interactions 122
5.5 Kinetic models of metal ion–humic interactions 128
5.6 Impacts of humic substances on radionuclide transport in
different sites worldwide 135
5.7 Conclusions and future trends 141
5.8 References 141
© Woodhead Publishing Limited, 2012
viiContents
6 Impacts of microorganisms on radionuclides in
contaminated environments and waste materials 161
A. J. Fr a n c i s , Pohang University of Science and Technology,
South Korea and Brookhaven National Laboratory, USA
6.1 Introduction 161
6.2 Biotransformation of uranium 165
6.3 Biotransformation of plutonium 179

6.4 Biosorption and bioaccumulation of uranium and
plutonium 187
6.5 Biotransformation of other actinides and related
elements 193
6.6 Biotransformation of ssion and activation products 196
6.7 Microbiological studies of low- and intermediate-level
wastes, and high-level waste repository sites 206
6.8 Conclusion 213
6.9 Acknowledgments 214
6.10 Suggested reading 214
6.11 References 215
Part II Radionuclide migration 227
7 Hydrogeological features relevant to radionuclide
migration in the natural environment 229
E. le d o u x , P. Go b l e t and d. br u e l , Mines-ParisTech, France
7.1 Introduction 229
7.2 The water content of the subsoil 230
7.3 Groundwater movement in the soil and subsoil 233
7.4 Aquifer systems 242
7.5 Groundwater ow equations for aquifer systems 246
7.6 Solving the ow equations for aquifer systems 249
7.7 References 259
8 Radionuclide retention at mineral–water interfaces in
the natural environment 261
M. ma r q u e s Fe r n a n d e s and B. ba e y e n s , Paul Scherrer Institut,
Switzerland and C. be a u c a i r e , French Alternative Energies and
Atomic Energy Commission (CEA), France
8.1 Introduction 261
8.2 Macroscopic studies of radionuclide sorption 263
8.3 Sorption models 271

8.4 Spectroscopic techniques 282
8.5 Future developments 286
© Woodhead Publishing Limited, 2012
viii Contents
8.6 Acknowledgements 288
8.7 References 288
9 Radionuclide migration: coupling transport and
chemistry 302
J. ca r r e r a , C. ay o r a , Institute of Environmental Assessment and
Water Research (IDAEA-CSIC), Spain, M. W. sa a l t i n k , Technical
University of Catalonia (UPC), Spain and M. de n t z , Institute of
Environmental Assessment and Water Research (IDAEA-CSIC),
Spain
9.1 Introduction 302
9.2 The transport phenomenon 303
9.3 Coupling chemistry to transport 316
9.4 Application examples 348
9.5 References 379
10 Impact of colloidal transport on radionuclide migration
in the natural environment 384
A. B. ke r s t i n G , Lawrence Livermore National Laboratory, USA
10.1 Introduction 384
10.2 Geochemistry and sorption behavior of radionuclides 387
10.3 Nature and origin of colloids 388
10.4 Colloid characteristics 393
10.5 Laboratory experiments of colloid-facilitated radionuclide
transport 395
10.6 Field studies of radionuclide migration 397
10.7 Conclusion and future trends 403
10.8 Acknowledgments 404

10.9 References 404
11 Natural analogues of nuclear waste repositories:
studies and their implications for the development of
radionuclide migration models 411
L. du r o and J. br u n o , Amphos 21 Consulting S.L., Spain
11.1 Introduction 411
11.2 Nature and limitations of natural analogues 413
11.3 Selected natural analogue sites 415
11.4 Lessons on radionuclide (RN) geochemistry and migration
from main natural analogues studies 429
11.5 Conclusion 440
11.6 Acknowledgement 441
11.7 References 441
© Woodhead Publishing Limited, 2012
ixContents
12 Studying radionuclide migration on different scales:
the complementary roles of laboratory and in situ
experiments 446
l. Va n lo o n and m. Gl a u s , Paul Scherrer Institut, Switzerland
and C. Fe r r y and C. la t r i l l e , French Alternative Energies and
Atomic Energy Commission (CEA), France
12.1 Introduction 446
12.2 Designing laboratory studies at different scales on
radionuclide diffusion in underground environments 448
12.3 Studies at different scales on diffusion in Swiss Opalinus
Clay 453
12.4 Studies at different scales on diffusion in French
Callovo-Oxfordian claystone 458
12.5 Laboratory experiments at the decimetre-scale on the
transport of radionuclides in non-consolidated porous

media 466
12.6 Conclusions and future trends 472
12.7 References 474
12.8 Appendix: denitions and abbreviations 482
13 Radionuclide transfer processes in the biosphere 484
e. an s o b o r l o , French Nuclear and Alternative Energies
Commission (CEA), France and C. ad a m -Gu i l l e r m i n , French
Institute for Radiological Protection and Nuclear Safety (IRSN),
France
13.1 Introduction 484
13.2 Radionuclide speciation and interactions with biological
ligands 486
13.3 Transfer to plants and biodistribution 490
13.4 Transfer to animal species and biodistribution 493
13.5 Transfer to man 496
13.6 Effect on metabolic pathways 498
13.7 Transfers through epithelial barriers: the digestive barrier 500
13.8 Membrane transport 502
13.9 Intracellular mechanisms: homeostasis and stress 505
13.10 Future trends 506
13.11 Acknowledgements 507
13.12 References 507
© Woodhead Publishing Limited, 2012
x Contents
Part III Environmental impact and remediation 515
14 Modelling radionuclide transport in the environment
and calculating radiation doses 517
M. th o r n e , Mike Thorne and Associates Limited, UK
14.1 Introduction 517
14.2 Modelling radionuclide transport in the environment 519

14.3 Assessing radiation doses to humans 540
14.4 Assessing radiation doses to non-human biota 551
14.5 Achieving a comprehensive assessment 559
14.6 Conclusion and future trends 560
14.7 References 563
15 Quantitative assessment of radionuclide migration
from near-surface radioactive waste burial sites: the
waste dumps in the Chernobyl exclusion zone as an
example 570
a. ma r t i n -Ga r i n , n. Va n me i r and c. si m o n u c c i , French Institute for
Radiological Protection and Nuclear Safety (IRSN), France,
V. ka s h P a r o V , Ukrainian Institute of Agricultural Radiology
(UIAR/NUBiP), Ukraine and D. bu G a i , Institute of Geological
Sciences (IGS), Ukraine
15.1 Introduction 570
15.2 The Chernobyl Pilot Site in the Red Forest 573
15.3 Modelling radionuclide migration in the aquifer considering
stationary hydrodynamic and geochemical conditions 582
15.4 Prediction of
90
Sr migration, assuming non-stationary
hydro-biogeochemical conditions 585
15.5 Conclusions and future trends 592
15.6 Acknowledgements 596
15.7 References 596
16 Remediation of sites contaminated by radionuclides 601
B. J. me r k e l and M. ho y e r , TU Bergakademie Freiberg, Germany
16.1 Introduction 601
16.2 Potential sources of radionuclide release 602
16.3 Methods of cleaning contaminated sites 622

16.4 Environmental monitoring tools 633
16.5 Modelling tools for planning clean-up 634
16.6 Risk assessment studies of hazardous sites and clean-up
measures 636
16.7 Examples of remediation of contaminated sites 637
16.8 Sources of further information 640
16.9 References 640
© Woodhead Publishing Limited, 2012
xiContents
17 Safety assessment of nuclear waste repositories: a
radionuclide migration perspective 646
J. br u n o , and A. de l o s , University of Catalonia, Spain
17.1 Introduction 646
17.2 Repository concepts 648
17.3 Safety assessment (SA) methodology 661
17.4 Integration of the main radionuclide migration processes and
parameters in the safety assessment (SA) models 686
17.5 Gaps in understanding and the qualication and
quantication of the safety assessment (SA) models 689
17.6 Conclusions 690
17.7 Acknowledgements 691
17.8 References 691
Index 693

© Woodhead Publishing Limited, 2012
Editors and Chapter 1
Professor C. Poinssot
French Nuclear and Alternative
Energies Commission (CEA)
Nuclear Energy Division

Department of Radio Chemistry
and Processes
CEA Marcoule
F-30207 Bagnols Sur Ceze Cedex
France
E-mail:
Professor H. Geckeis
Karlsruhe Institute of Technology
(KIT)
Institute for Nuclear Waste
Disposal
P.O. Box 3640
D-76021 Karlsruhe
Germany
E-mail:
Contributor contact details
Chapter 2
T. Neumann
Institute of Mineralogy and
Geochemistry
Karlsruhe Institute of Technology
(KIT)
Adenauerring 20 b
76131 Karlsruhe
Germany
E-mail:
Chapter 3
M. Altmaier*
Karlsruhe Institute of Technology
(KIT)

Institute for Nuclear Waste
Disposal
P.O. Box 3640
D-76021 Karlsruhe
Germany
E-mail:
(* = main contact)
© Woodhead Publishing Limited, 2012
xiv Contributor contact details
T. Vercouter
French Alternative Energies and
Atomic Energy Commission
(CEA)
Nuclear Energy Division
DEN, DANS, DPC, SEARS,
LANIE
Bat 391, PC 33
F-91191 Gif-sur-Yvette Cedex
France
E-mail:
Chapter 4
A. Abdelouas* and B. Grambow
École des Mines de Nantes –
SUBATECH
4, rue Alfred Kastler – La
chantrerie
BP 20722
44307 Nantes Cedex 3
France
E-mail: abdesselam.abdelouas@

subatech.in2p3.fr
Chapter 5
P. E. Reiller*
French Alternative Energies and
Atomic Energy Commission
(CEA)
Nuclear Energy Division
Centre d’Étude de Saclay
Bâtiment 391, PC 33
91191 Gif-sur-Yvette Cedex
France
E-mail:
G. Buckau
Institute for Transuranium
Elements
Joint Research Centre
Hermann-von-Helmholtz-Platz 1
76344 Eggenstein-Leopoldshafen
Germany
E-mail:
On leave from
Institut für Nukleare Entsorgung
Karlsruhe Institute of Technology
(KIT)
P.O. Box 3640
76021 Karlsruhe
Germany
Chapter 6
A. J. Francis
Division of Advanced Nuclear

Engineering
Pohang University of Science and
Technology
Pohang
South Korea
and
Environmental Sciences
Department
Brookhaven National Laboratory
Upton
NY 11973-5000
USA
E-mail:
© Woodhead Publishing Limited, 2012
xvContributor contact details
Chapter 7
E. Ledoux*, P. Goblet and D. Bruel
Department of Geosciences
Mines-ParisTech
35, rue Saint Honoré
77305 Fontainebleau
France
E-mail: emmanuel.ledoux@mines-
paristech.fr
Chapter 8
M. Marques Fernandes* and B.
Baeyens
Laboratory for Waste Management
Paul Scherrer Institut
5232 Villigen

Switzerland
E-mail: ; bart.

C. Beaucaire
French Alternative Energies and
Atomic Energy Commission
(CEA)
Centre d’Étude de Saclay
Department of Physics and
Chemistry
91191 Gif-sur-Yvette Cedex
France
E-mail:
Chapter 9
J. Carrera*, C. Ayora and M. Dentz
Department of Geosciences
Institute of Environmental
Assessment and Water Research
(IDAEA-CSIC)
Calle Jordi Girona 18–26
08034 Barcelona
Spain
E-mail: ; jesus.

M. W. Saaltink
Department of Geotechnical
Engineering and Geosciences
Technical University of Catalonia
Spain
Chapter 10

A. B. Kersting
Glenn T. Seaborg Institute
Physical and Life Sciences
Lawrence Livermore National
Laboratory
L-231
P.O. Box 808
Livermore
CA 94550
USA
E-mail:
Chapter 11
L. Duro* and J. Bruno
Amphos 21 Consulting S.L.
P. Garcia I Faria 49–51, 1-1
08019 Barcelona
Spain
E-mail:
© Woodhead Publishing Limited, 2012
xvi Contributor contact details
Chapter 12
L. Van Loon* and M. Glaus
Laboratory for Waste Management
Paul Scherrer Institut
5232 Villigen
Switzerland
E-mail:
C. Ferry and C. Latrille
French Alternative Energies and
Atomic Energy Commission

(CEA)
Nuclear Energy Division
Bâtiment 450
91191 Gif-sur-Yvette Cedex
France
E-mail:
Chapter 13
E. Ansoborlo*
French Alternative Energies and
Atomic Energy Commission
(CEA)
Nuclear Energy Division
Department of Radio Chemistry
and Processes
CEA Marcoule, BP-17171
30207 Bagnols-sur-Cèze
France
E-mail:
C. Adam-Guillermin
French Institute for Radiological
Protection and Nuclear Safety
(IRSN)
PRP-ENV/SERIS/LECO
Division for Research and
Expertise in Environmental
Risks
Bâtiment 186
Cadarache, BP 3
13115 Saint-Paul-lez-Durance
Cedex

France
E-mail: Christelle.adam-guillermin@
irsn.fr
Chapter 14
M. Thorne
Mike Thorne and Associates
Limited
Quarry Cottage
Hamsterley
Bishop Auckland DL13 3NJ
UK
E-mail:
Chapter 15
A. Martin-Garin*
French Institute for Radiological
Protection and Nuclear Safety
(IRSN)
Bâtiment 186
Cadarache BP3 13115 Saint-Paul-
lez-Durance Cedex
France
E-mail:
© Woodhead Publishing Limited, 2012
xviiContributor contact details
N. Van Meir and C. Simonucci
French Institute for Radiological
Protection and Nuclear Safety
(IRSN)
Fontenay-aux-Roses, Bâtiment 76/2
92262 Fontenay-aux-Roses Cedex

France
E-mail: ;

V. Kashparov
Ukrainian Institute of Agricultural
Radiology
UIAR/NUBiP of Ukraine
Mashinobudivnykiv str. 7
Chabany, Kyiv-Svjatoshin Distr.
08162 Kiev Region
Ukraine
E-mail:
D. Bugai
Institute of Geological Sciences
(IGS)
Gonchara str. 55-b
01054 Kiev
Ukraine
E-mail:
Chapter 16
B. J. Merkel* and M. Hoyer
TU Bergakademie Freiberg
Gustav-Zeuner-Str. 12
09596 Freiberg/Sa.
Germany
E-mail:
Chapter 17
J. Bruno and A. Delos*
University of Catalonia
Parc Tecnològic del Vallés

Cerdanyola
08290 Barcelona
Spain
E-mail: ;


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Edited by Angelo Basile and Suzana Pereira Nunes

26 Irradiationembrittlementofreactorpressurevessels(RPVs)in
nuclearpowerplants
Edited by Naoki Soneda
27 Hightemperaturesuperconductors(HTS)forenergyapplications
Edited by Ziad Melhem
28 Infrastructureandmethodologiesforthejusticationofnuclear
powerprogrammes
Edited by Agustín Alonso
29 Wastetoenergy(WtE)conversiontechnology
Edited by Marco Castaldi
30 Polymerelectrolytemembraneanddirectmethanolfuelcell
technologyVolume1:Fundamentalsandperformanceoflow
temperaturefuelcells
Edited by Christoph Hartnig and Christina Roth
31 Polymerelectrolytemembraneanddirectmethanolfuelcell
technologyVolume2:In situcharacterisationtechniquesforlow
temperaturefuelcells
Edited by Christoph Hartnig and Christina Roth
32 Combinedcyclesystemsfornear-zeroemissionpowergeneration
Edited by Ashok D. Rao
33 Modernearthbuildings:Materials,engineering,constructionand
applications
Edited by Matthew R. Hall, Rick Lindsay and Meror Krayenhoff
34 Handbookofmetropolitansustainability:Understandingand
improvingtheurbanenvironment
Edited by Frank Zeman
35 Functionalmaterialsforenergyapplications
Edited by John Kilner, Stephen Skinner, Stuart Irvine and Peter
Edwards
© Woodhead Publishing Limited, 2012

xxii Woodhead Publishing Series in Energy
36 Nucleardecommissioning:Planning,executionandinternational
experience
Edited by Michele Laraia
37 Nuclearfuelcyclescienceandengineering
Edited by Ian Crossland
38 Electricitytransmission,distributionandstoragesystems
Edited by Ziad Melhem
39 Advancesinbiodieselproduction:Processesandtechnologies
Edited by Rafael Luque and Juan Antonio Melero
40 Biomasscombustionscience,technologyandengineering
Edited by Lasse Rosendahl
41 Ultra-supercriticalcoalpowerplant:Materials,technologiesand
optimisation
Edited by Dongke Zhang
42 Radionuclidebehaviourinthenaturalenvironment:Science,
implicationsandlessonsforthenuclearindustry
Edited by Christophe Poinssot and Horst Geckeis
43 Calciumandchemicalloopingtechnologyforpowergenerationand
carbondioxide(CO
2
)capture:Solidoxygen-andCO
2
-carriers
P. Fennell and E. J. Anthony
44 Materialsageinganddegradationinlightwaterreactors:
Mechanisms,modellingandmitigation
Edited by K. L. Murty
45 Structuralalloysforpowerplants:Operationalchallengesand
high-temperaturematerials

Edited by Amir Shirzadi, Rob Wallach and Susan Jackson
46 Biolubricants:Scienceandtechnology
Jan C. J. Bart, Emanuele Gucciardi and Stefano Cavallaro
47 Windturbinebladedesignandmaterials:Improvingreliability,
costandperformance
Edited by Povl Brøndsted and Rogier Nijssen
48 Radioactivewastemanagementandcontaminatedsiteclean-up:
Processes,technologiesandinternationalexperience
Edited by William E. Lee, Michael I. Ojovan, Carol M. Jantzen
© Woodhead Publishing Limited, 2012
xxiiiWoodhead Publishing Series in Energy
49 Probabilisticsafetyassessmentforoptimumnuclearpowerplant
lifemanagement(PLiM):Theoryandapplicationsofreliability
analysismethodsformajorpowerplantcomponents
Gennadij V. Arkadov, Alexander F. Getman and Andrei N. Rodionov
50 Coalutilizationinindustry
Edited by D. G. Osborne
51 Coalpowerplantmaterialsandlifeassessment:Developmentsand
applications
Edited by Ahmed Shibli
52 Thebiogashandbook:Science,productionandapplications
Edited by Arthur Wellinger and David Baxter
53 Advancesinbioreneries:Biomassandwastesupplychain
exploitation
Edited by K. W. Waldron
54 Geoscienceofcarbondioxide(CO
2
)storage
Edited by Jon Gluyas and Simon Mathias
55 HandbookofmembranereactorsVolumeI:Fundamentalmaterials

science,designandoptimisation
Edited by Angelo Basile
56 HandbookofmembranereactorsVolumeII:Industrialapplications
andeconomics
Edited by Angelo Basile
57 Alternativefuelsandadvancedvehicletechnologies:Towardszero
carbontransportation
Edited by Richard Folkson
58 Handbookofmicroalgalbioprocessengineering
Christopher Lan and Bei Wang
59 Fluidized-bedtechnologiesfornear-zeroemissioncombustionand
gasication
Edited by Fabrizio Scala
60 Managingnuclearprojects:Acomprehensivemanagementresource
Edited by Jas Devgun
61 Handbookofprocessintegration:Energy,water,wasteand
emissionsmanagementinprocessingandpowerindustries
Edited by Jiří Klemeš
62 Membranesforcleanandrenewablepowerapplications
Edited by Annarosa Gugliuzza and Angelo Basile