Radionuclide behaviour in the natural environment docx

Radionuclide behaviour in the natural environment © Woodhead Publishing Limited, 2012 Related titles: Geological repository systems for safe disposal of spent nuclear fuels and radioactive waste (ISBN 978-1-84569-542-2) The long-term safety of spent nuclear fuel and radioactive waste materials must be assured without active human oversight, based on the requirement that we not pass the burden of nuclear waste onto future generations Geological disposal systems and technology, utilising both natural geological barriers and engineered barrier systems, have been developed to isolate nuclear wastes from the human environment This book critically reviews state-of-the-art technologies, scientific methods and engineering practices directly related to the design, operation and safety of geological repositories Infrastructure and methodologies for the justification of nuclear power programmes (ISBN 978-1-84569-973-4) The potential development of any nuclear power programme requires a rigorous justification process built upon an objective infrastructure, reviewing the substantial regulatory, economic and technical information required to appropriately decide upon implementation of such a long-term commitment Both new entrants and those countries wishing to renovate their nuclear fleets after a moratorium will need to develop and apply appropriate infrastructures to review the justification of the potential use of nuclear power This book provides a comprehensive review of the infrastructure and methodologies required to justify the implementation of nuclear power programmes in any country choosing to review this path Handbook of advanced radioactive waste conditioning technologies (ISBN 978-1-84569-626-9) Radioactive wastes are generated from a wide range of sources presenting a variety of challenges in dealing with a diverse set of radionuclides of varying concentrations Conditioning technologies are essential for the encapsulation and immobilisation of these radioactive wastes, forming the initial engineered barrier required for their transportation, storage and disposal The need to ensure the long-term performance of radioactive waste forms is a key driver in the development of advanced conditioning technologies This book provides a comprehensive and systematic reference on the various options available as well as those under development for the treatment and immobilisation of radioactive wastes Details of these and other Woodhead Publishing books can be obtained by: ∑ visiting our web site at www.woodheadpublishing.com ∑ contacting Customer Services (e-mail: sales@woodheadpublishing.com; fax: +44 (0) 1223 832819; tel.: +44 (0) 1223 499140 ext 130; address: Woodhead Publishing Limited, 80 High Street, Sawston, Cambridge CB22 3HJ, UK) ∑ contacting our US office (e-mail: usmarketing@woodheadpublishing.com; tel (215) 928 9112; address: Woodhead Publishing, 1518 Walnut Street, Suite 1100, Philadelphia, PA 19102-3406, USA) If you would like e-versions of our content, please visit our online platform: www.woodheadpublishingonline.com Please recommend it to your librarian so that everyone in your institution can benefit from the wealth of content on the site © 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 Published by Woodhead Publishing Limited, 80 High Street, Sawston, Cambridge CB22 3HJ, UK www.woodheadpublishing.com www.woodheadpublishingonline.com Woodhead Publishing, 1518 Walnut Street, Suite 1100, Philadelphia, PA 19102-3406, USA Woodhead Publishing India Private Limited, G-2, Vardaan House, 7/28 Ansari Road, Daryaganj, New Delhi – 110002, India www.woodheadpublishingindia.com First published 2012, Woodhead Publishing Limited © Woodhead Publishing Limited, 2012 The publisher has made every effort to ensure that permission for copyright material has been obtained by authors wishing to use such material The authors and the publisher will be glad to hear from any copyright holder it has not been possible to contact The authors have asserted their moral rights This book contains information obtained from authentic and highly regarded sources Reprinted material is quoted with permission, and sources are indicated Reasonable efforts have been made to publish reliable data and information, but the authors and the publishers cannot assume responsibility for the validity of all materials Neither the authors nor the publishers, nor anyone else associated with this publication, shall be liable for any loss, damage or liability directly or indirectly caused or alleged to be caused by this book Neither this book nor any part may be reproduced or transmitted in any form or by any means, electronic or mechanical, including photocopying, microfilming and recording, or by any information storage or retrieval system, without permission in writing from Woodhead Publishing Limited The consent of Woodhead Publishing Limited does not extend to copying for general distribution, for promotion, for creating new works, or for resale Specific permission must be obtained in writing from Woodhead Publishing Limited for such copying Trademark notice: Product or corporate names may be trademarks or registered trademarks, and are used only for identification and explanation, without intent to infringe British Library Cataloguing in Publication Data A catalogue record for this book is available from the British Library Library of Congress Control Number: 2012943209 ISBN 978-0-85709-132-1 (print) ISBN 978-0-85709-719-4 (online) ISSN 2044-9364 Woodhead Publishing Series in Energy (print) ISSN 2044-9372 Woodhead Publishing Series in Energy (online) The publisher’s policy is to use permanent paper from mills that operate a sustainable forestry policy, and which has been manufactured from pulp which is processed using acid-free and elemental chlorine-free practices Furthermore, the publisher ensures that the text paper and cover board used have met acceptable environmental accreditation standards Typeset by Replika Press Pvt Ltd, India Printed by TJ International Limited, Padstow, Cornwall, UK © Woodhead Publishing Limited, 2012 Contents Contributor contact details Woodhead Publishing Series in Energy Foreword Overview of radionuclide behaviour in the natural environment C Poinssot, French Nuclear and Alternative Energies Commission (CEA), France and H Geckeis, Karlsruhe Institute of Technology (KIT), Germany 1.1 1.2 1.3 1.4 Introduction Radionuclides of interest Environmental compartments to be considered References Part I Radionuclide chemistry in the natural environment Fundamentals of aquatic chemistry relevant to radionuclide behaviour in the environment Introduction Composition of natural waters Dissolution and precipitation Aqueous complexes Surface sorption Colloids Redox reactions References 1 10 11 T Neumann, Karlsruhe Institute of Technology (KIT), Germany 2.1 2.2 2.3 2.4 2.5 2.6 2.7 2.8 xiii xix xxv © Woodhead Publishing Limited, 2012 13 13 14 16 24 27 34 35 41 vi Contents Aquatic chemistry of the actinides: aspects relevant to their environmental behavior M Altmaier, Karlsruhe Institute of Technology (KIT), Germany and T Vercouter, French Alternative Energies and Atomic Energy Commission (CEA), France 3.1 3.2 3.3 3.4 3.5 3.6 3.7 Introduction Oxidation states of actinides in aqueous solution Actinide solid phases and solubility phenomena Actinide complexation reactions Chemical modeling tools and thermodynamic databases Recommended literature References 44 46 52 56 64 65 66 Aquatic chemistry of long-lived mobile fission and activation products in the context of deep geological disposal 70 A Abdelouas and B Grambow, École des Mines de Nantes – SUBATECH, France 4.1 4.2 Introduction The effects of the near field in high-level radioactive waste disposal Solution and interfacial chemistry of selected radionuclides Summary References 4.3 4.4 4.5 Impacts of humic substances on the geochemical behaviour of radionuclides Introduction to humic substances The ‘humic acid molecule’ Discrete models of metal ion–humic interactions Multiligand and macromolecular models of metal ion–humic interactions Kinetic models of metal ion–humic interactions Impacts of humic substances on radionuclide transport in different sites worldwide Conclusions and future trends References 70 73 77 92 93 P E Reiller, French Nuclear and Alternative Energies Commission (CEA), France and G Buckau, Institute for Transuranium Elements, Germany 5.1 5.2 5.3 5.4 44 5.5 5.6 5.7 5.8 © Woodhead Publishing Limited, 2012 103 103 106 110 122 128 135 141 141 Contents Impacts of microorganisms on radionuclides in contaminated environments and waste materials A J Francis, Pohang University of Science and Technology, South Korea and Brookhaven National Laboratory, USA 6.1 6.2 6.3 6.4 Introduction Biotransformation of uranium Biotransformation of plutonium Biosorption and bioaccumulation of uranium and plutonium Biotransformation of other actinides and related elements Biotransformation of fission and activation products Microbiological studies of low- and intermediate-level wastes, and high-level waste repository sites Conclusion Acknowledgments Suggested reading References vii 6.5 6.6 6.7 6.8 6.9 6.10 6.11 Part II Radionuclide migration 161 161 165 179 187 193 196 206 213 214 214 215 227 Hydrogeological features relevant to radionuclide migration in the natural environment E Ledoux, P Goblet and D Bruel, Mines-ParisTech, France 7.1 7.2 7.3 7.4 7.5 7.6 7.7 Introduction The water content of the subsoil Groundwater movement in the soil and subsoil Aquifer systems Groundwater flow equations for aquifer systems Solving the flow equations for aquifer systems References 229 230 233 242 246 249 259 Radionuclide retention at mineral–water interfaces in the natural environment 261 M Marques Fernandes and B Baeyens, Paul Scherrer Institut, Switzerland and C Beaucaire, French Alternative Energies and Atomic Energy Commission (CEA), France 8.1 8.2 8.3 8.4 8.5 Introduction Macroscopic studies of radionuclide sorption Sorption models Spectroscopic techniques Future developments © Woodhead Publishing Limited, 2012 229 261 263 271 282 286 viii Contents 8.6 8.7 Acknowledgements References 288 288 Radionuclide migration: coupling transport and chemistry 302 J Carrera, C Ayora, Institute of Environmental Assessment and Water Research (IDAEA-CSIC), Spain, M W Saaltink, Technical University of Catalonia (UPC), Spain and M Dentz, Institute of Environmental Assessment and Water Research (IDAEA-CSIC), Spain 9.1 9.2 9.3 9.4 9.5 Introduction The transport phenomenon Coupling chemistry to transport Application examples References 302 303 316 348 379 10 Impact of colloidal transport on radionuclide migration in the natural environment 384 A B Kersting, Lawrence Livermore National Laboratory, USA 10.1 10.2 10.3 10.4 10.5 Introduction Geochemistry and sorption behavior of radionuclides Nature and origin of colloids Colloid characteristics Laboratory experiments of colloid-facilitated radionuclide transport Field studies of radionuclide migration Conclusion and future trends Acknowledgments References 10.6 10.7 10.8 10.9 11 Natural analogues of nuclear waste repositories: studies and their implications for the development of radionuclide migration models Introduction Nature and limitations of natural analogues Selected natural analogue sites Lessons on radionuclide (RN) geochemistry and migration from main natural analogues studies Conclusion Acknowledgement References 395 397 403 404 404 L Duro and J Bruno, Amphos 21 Consulting S.L., Spain 11.1 11.2 11.3 11.4 384 387 388 393 11.5 11.6 11.7 © Woodhead Publishing Limited, 2012 411 411 413 415 429 440 441 441 Contents ix 12 Studying radionuclide migration on different scales: the complementary roles of laboratory and in situ experiments L Van Loon and M Glaus, Paul Scherrer Institut, Switzerland and C Ferry and C Latrille, French Alternative Energies and Atomic Energy Commission (CEA), France 12.1 12.2 Introduction Designing laboratory studies at different scales on radionuclide diffusion in underground environments Studies at different scales on diffusion in Swiss Opalinus Clay Studies at different scales on diffusion in French Callovo-Oxfordian claystone Laboratory experiments at the decimetre-scale on the transport of radionuclides in non-consolidated porous media Conclusions and future trends References Appendix: definitions and abbreviations 446 13 Radionuclide transfer processes in the biosphere 484 E Ansoborlo, French Nuclear and Alternative Energies Commission (CEA), France and C Adam-Guillermin, French Institute for Radiological Protection and Nuclear Safety (IRSN), France 12.3 12.4 12.5 12.6 12.7 12.8 13.1 13.2 Introduction Radionuclide speciation and interactions with biological ligands 13.3 Transfer to plants and biodistribution 13.4 Transfer to animal species and biodistribution 13.5 Transfer to man 13.6 Effect on metabolic pathways 13.7 Transfers through epithelial barriers: the digestive barrier 13.8 Membrane transport 13.9 Intracellular mechanisms: homeostasis and stress 13.10 Future trends 13.11 Acknowledgements 13.12 References © Woodhead Publishing Limited, 2012 446 448 453 458 466 472 474 482 484 486 490 493 496 498 500 502 505 506 507 507 696 Index affinity in the four main oxidation states, 58 solubility curves corresponding to selected actinide solid phases, 60 speciation diagram in air-equilibrated solution, 62 component additivity see bottom-up approach concrete, 74 conditional constants, 112 confined aquifers cross section, 245 equations, 247 radial flow, 251–2 constant activity species, 338, 345–8 constant-capacitance (CC), 34 containers, 73–4 contaminated sites methods of cleaning, 622–33 soil, sediments, and construction materials, 624–9 type of contaminated sites, 623 water treatment, 629–33 coprecipitation, 75–6 secondary phases in radionuclide analogues, 76 coupled equations, 342–8 constant activity species, 345–8 crystalline rock aquifers, 244 curium, 194–5 Damkhoeler number, 320–2 concentration vs x – vt/s, 323 Darcy’s law, 234–8 basic expression, 234–5 experiment, 235 experiment in 3D, 236 intrinsic permeability, 235–6 permeability tensor, 236–7 permeability values, 237–8 hard rocks, 237 unconsolidated dentritic rocks, 237 Debye-Hückel limited equation, 18, 56 decomposition time dynamics, 587–8 Density Functional Theory (DFT), 64 DEPA-TOPO, 608 deposition velocity, 525 deterministic effect, 540 diffuse-layer (DL), 34 diffusion designing laboratory studies in underground environments, 448–54 diffusion at the microscopic level, 451–2 overview of different techniques, 452 through- and in-diffusion experiments at centimetre scale, 449–51 studies at different scales in French Callovo-Oxfordian claystone, 458–66 studies at different scales in Swiss Opalinus Clay, 453–8 diffusivity equation numerical methods, 255–9 finite-difference square grid on a bounded domain, 257 modelling tools, 259 dioxocations, 47 dissociation modes, 128–9 dissolution, 16–24 distribution coefficient, 318 DLVO theory, 395 dry deposition, 524–6 dust control, 603 ecosphere, effective dose, 543 eigencolloids, 392 El Berrocal (Spain), 425–6 cross-section of natural analogue site, 426 electrostatic interactions, 32, 57 elemental composition, 106–7 typical composition guided by data for Gohy-573(HA), 107 environmental behaviour aquatic chemistry of actinides, 44–65 chemical modelling tools and thermodynamic databases, 64–5 complexation reactions, 56–64 oxidation states in aqueous solution, 46–52 solid phase and solubility phenomena, 52–6 environmental compartments, 5–10 characteristic time scales for radionuclide mobility, different radionuclide release sources, main process occurring in porous rock and governing radionuclide mobility, environmental monitoring tools, 633–7 modelling tools for planning clean-up, 634–6 risk assessment studies, 636–7 © Woodhead Publishing Limited, 2012 Index Environmental Risk from Ionising Contaminants: Assessment and Management (ERICA), 552 EQ3/6, 65 equilibrium constant, 334, 347 equilibrium controlled transport, 140–1 equivalent dose, 542 ERICA Tool, 559 experimental underground laboratory, 209–10 external exposure, 544–6 finite differences, 257–8 piezometric map, 258 finite elements, 258–9 flow pattern calculation, 259 first-order kinetic reactions, 321 fission products aquatic chemistry in context to deep geological disposal, 70–93 biotransformation, 196–206 near field effects in high-level radioactive waste disposal, 73–7 overview, 70–3 radionuclide mobility controlling interfacial ractions, 71 stable species of actinides, 72 solution and interfacial chemistry of radionuclides, 77–92 fission reactors, fixed point method see Picard method fluoride complexes, 57 fly ash deposition, 618–19 food products, 549–51 Fourier boundary conditions, 250–1 aquifer and a river, 251 fractured media reactive transport, 363–6 conceptualisation and upscaled version model, 364 conservative component concentrations and cumulative precipitate, 366 flow and conservative transport boundary conditions, 365 outflow concentration of a conservative component, 367 fractured rocks, 233 Framework for Assessment of Environmental Impact (FASSET), 552 Franceville Basin, 421 FREDERICA database, 556 French Callovo-Oxfordian claystone, 458–66 697 diffusion measurements in Underground Research Laboratory in Bure, 463–4 influence of diffusion coefficient values on radionuclide concentration, 467 monitoring of radionuclide concentration, 465 rock core extracted from borehole, 466 large-scale laboratory experiment, 462–3 experimental set-up, 463 limitations of diffusion experiments, 464–6 characteristics, merits and limitations of laboratory and field experiments, 468 small-scale laboratory experiment, 460–2 diffusion coefficient as a function of cation radii, 462 effect of clay minerals content on diffusion of anionic species, 461 French safety assessment gaps in understanding and qualification and quantification of models, 690 radionuclide migration processes and parameters integration, 687 C waste compartment thermal evolution, 680 cement degradation around B-type waste package, 682 chemical evolution of the system, 679, 681 EDZ evolution around a B-type waste package, 683 evolution of dose at most penalising outlet, 688 four-steps long-term safety analysis, 683–4, 686 hydraulic evolution of the system, 679 iterative procedure of feasibility study, 678 main safety functions over time, 685 mechanical evolution of the system, 683 migration process in PARS analysis, 676, 678 safety analysis steps sequence, 684 structure of the Dossier Argile 2005, 677 thermal evolution of the system, 678–9 fresh-salt water mixing zone calcite dissolution, 348–53 © Woodhead Publishing Limited, 2012 698 Index function of the saline water fraction for a non-reactive medium, 352 linear mixing of fresh and saline groundwaters, 350 sensitivity of mixing to the Pco2 of freshwater end-member, 353 Gauss–Jordan elimination, 337, 345, 346 general composite see top-down approach Geochemist’s Workbench (GWB), 65 geological disposal long-lived mobile fission and activation products, 70–93 near field effects in high-level radioactive waste disposal, 73–7 overview, 70–3 radionuclide mobility controlling interfacial ractions, 71 solution and interfacial chemistry of radionuclides, 77–92 geosphere, geosphere system, 652–5, 661 fracture fillings, 652–3 groundwater composition, 653 hydrogeology, 653 measured hydraulic transmissivities, 654–5 porewater composition of CallovoOxfordian formation, 662 rock composition, 652 Gibbs phase rule, 336 global models, 539–40 groundwater chemical composition, 585–6 block scheme of biogeochemical process in trench no 22, 586 composition, 653 chlorine concentration, 656 organic matter decomposition and consequence on chemistry, 586–8 impact of radioactivity, 588 organic substrate and physical environment, 587 time dynamics of decomposition, 587–8 groundwater movement, 233–42 Darcy’s law, 234–8 hydraulic head and piezometric level principle of a piezometer, 234 modelling in porous medium, 238–42 capillary pressure vs moisture content, 242 continuity equation, 238 diffusivity equation, 240 equation of state, 239–40 permeability vs moisture content, 241 unsaturated zone, 240–2 Hanford sediments, 396 Hanford Site, 402–3 heterotrophic bacteria, 167, 183 heterotrophic fungi, 167, 183 heterotrophs, 163 high-level radioactive waste clay environment, 655–61 C-waste steel overpack concept and layout, 659 disposal concept for B-type waste, 658 engineered barrier materials, 657, 660 general repository organisation, 657 geosphere, 661 proposed spent fuel package, 659 waste, 657 waste package activity in actinides, 660 waste package activity in fission and activation products, 660 near field effects in disposal, 73–7 near field system technical components, 73–4 waste matrix, 74–7 high-level waste repository site, 206–13 human respiratory tract model (HRTM), 547 humic acid molecule, 106–10 elemental composition, 106–7 hydrodynamic size, 107 mass distribution, 107–8 proton-exchanging functional groups, 109–10 redox properties, 108–9 humic substances future trends, 141 humic acid molecule, 106–10 impact geochemical radionuclide behaviour, 103–41 impact on radionuclide transport, 135–41 metal ion-humic interactions discrete model, 110–22 metal ion-humic interactions kinetic models, 128–35 metal ion-humic interactions multiligand and macromolecular models, 122–8 overview, 103–6 © Woodhead Publishing Limited, 2012 Index composition and properties, 104–6 origin and isolation, 104 Hydrochemical Equilibrium Constant Database (HYDRA), 65 hydrodynamic size, 107 hydrogeology aquifer system, 242–6 groundwater flow equations for aquifer systems, 246–9 radionuclide migration in natural environment, 229–59 soil and subsoil groundwater movement, 233–42 solving flow equations for aquifer systems, 249–59 subsoil water content, 230–3 hydroxide complexes, 58–9 hydroxosulfato complexes, 63 IAEA (2004), 522 illite, 418 immobilisation in site, 627 in-diffusion technique, 451 in situ leaching (ISL), 603–4, 637 ingestion, 547–51 drinking water, 548–9 food products, 549–51 soils and sediment, 549 ingestion factor, 496 inhalation, 546–7 inner-sphere complexes, 25–6 intermediate-level waste repository site, 206–13 intrinsic colloids, 392 iodine, 86–8, 201–3, 498, 504 aquatic ecosystems, 86–7 Eh–pH diagram in water, 87 biotransformation, 202 geological disposal of radioactive waste, 88 terrestrial ecosystems, 87–8 ion exchange, 277–82 characterisation of major sites in pure mineral phase, 279–80 Na+ sorption onto Wyoming montmorillonite, 280 effects of ligands on trace element sorption, 281–2 minor site identification, 280–1 Zn sorption isotherm on Wyoming montmorillonite, 281 ionic strength, 17–20, 115, 126 699 evolution of complexation constants, 116 seawater composition, 17 iron-clay effect, 681 iron metabolism, 500 iron–uranium–citrate complex, 174–5 molecular structure for 2:2:4 Fe:U:citric acid complex, 175 Jacob solution, 252–3 jacobian of f, 340 KBS3 concept, 648 scheme for spent fuel disposal in crystalline rock, 649 Kd model, 318–20 kinematic porosity, 230–1 kinetic reaction rates, 342–3 kinetically controlled transport, 140–1 Königstein mine, 637–8 Lake Karachai, 401–2 landfills, 615, 617 Langmuir adsorption isotherm, 29, 30 leaching, 164 ligands, 26–7 Linear Energy Transfer (LET), 541 linear non-threshold hypothesis, 540–1 liquid thermal diffusion, 605 long-lived radionuclides, 3, aquatic chemistry of mobile fission and activation products, 70–93 near field effects in high-level radioactive waste disposal, 73–7 overview, 70–3 solution and interfacial chemistry of radionuclides, 77–92 low-level waste repository site, 206–13 magnesium transporters, 503 mammalian species, 495–6 in vivo distribution of Cs(I), Co(II), Am(III), Pu(IV), Np(V) citrate forms and U(VI) chloride or carbonate, 495 Maqarin (Jordan), 419–20 map of natural analogue site, 420 mass action law, 318, 333, 341 mass distribution, 107–8 mathematical modelling techniques, 522–4 compartmental modelling, 522–3 equilibrium models, 523–4 © Woodhead Publishing Limited, 2012 700 Index groundwater transport and advectiondispersion equation, 523 MATLAB, 635 matrix diffusion, 428 matrix-vector notation, 333 Mayak, 401–2 meta-schoepite, 59 metal-citrate complexes, 174 metal ion-humic interactions discrete model, 110–22 kinetic models, 128–35 humic acid actinide complex dissociation kinetics, 130 multiligand and macromolecular models, 122–8 metal ions, 26–7 classifications, 26 microbial activity, 163–5 autotrophic, 166 heterotrophic, 166–8 dissolution of uranium by Halomonas sp under anaerobic conditions, 169 impact on yucca mountain, 212–13 mobilisation of plutonium from contaminated soil, 187 release of radioactive gases, 205–6 microbial gas generation implication for disposal, 207 WIPP repository, 207–9 microbial transformation, 165 microorganisms biosorption and bioaccumulation of uranium and plutonium, 187–92 biotransformation of actinides and related elements, 193–6 biotransformation of fission and activation products, 196–206 biotransformation of plutonium, 179–87 biotransformation of uranium, 165–79 impact on radionuclides in contaminated environments and waste materials, 161–214 low-, intermediate, and high-level waste repository site, 206–13 experimental underground laboratory studies, 209–10 microbial activity yucca mountain, 212–13 microbial gas generation at WIPP repository, 207–9 microbial gas generation implication for disposal, 207 microbial population and related sites, 206–7 Yucca Mountain site, 210–12 overview, 161–5 microbial activity and its impact on radionuclide chemistry, 163–5 microbial transformation of actinides, 165 MIKE-SHE model, 529 minerals sorption, 131–3 mixed-ligand complexes log HAb with pH, 115–20 humic complexation data of actinides(IV), 119 ternary Cm3+-hydroxo–humic acid formation and interaction constants, 118 mixed oxidation model, 378–9 mixing, 322–30 cumulative dimensionless precipitation, 331 dimensionless concentrations and reaction rate in response to pulse injection, 329 ideal for two end members, 326 precipitation rate, 330 Moab mill, 638 Model V, 123–5 model validation, 520 Model VI, 123–5 abundance of different sites defined for Am(III) complexation, 125 distribution of the pKi values, 124 Model VII, 123–5 modelling sorption, 637 Modflow-MT3D, 583, 591, 636 moisture content, 231–2 moisture steady-state profile in soil, 232 molecular modelling, 286–7 Morro Ferro, 416–17 multi-rate-masstransfer (MRMT) reactive transport, 316 multi rate mass transfer system, 317 multi-scale approach, 287–8 multi-site complexation (MUSIC), 34 multicomponent reactive transport Ratones uranium mine, 366–79 chemical composition of initial and boundary water solution, 373 © Woodhead Publishing Limited, 2012 Index chemistry of representative groundwater analyses using model calibration, 371 concentration measured and computed comparison, 377 geological and hydrogeological setting, 368–71 initial volume fraction of minerals and reactive surface area, 374 location, structural features and conceptual flow model, 369 numerical modelling, 371–3 pe and pH measured and computed comparison, 376 results, 374–7 spatial distribution of pe and pH, mineral dissolution and mine precipitation, 375–6 stoichiometry of minerals, 373 three models description, 371 multilayered aquifers, 245–6 Paris Basin showing the major aquifers and aquitards, 246 National Diet and Nutrition Surveys, 549–50 natural analogues, 411–12 development of sorption models in NNAA studies, 436–40 distribution coefficient of Cs on different types of granite, 438 reproduction of sorption edge of uranium, 440 nature and limitations, 413–15 retention and migration processes of metals in underground environments, 414 nuclear waste repository 411-41 radionuclide geochemistry and migration 429-40 speciation/solubility models, 430–6 selected natural analogue sites, 415–29 Alligator Rivers (Australia), 428–9 Cigar Lake (Canada), 418–19 El Berrocal (Spain), 425–6 map sites of relevance for radionuclide migration, 415 Maqarin (Jordan), 419–20 Oklo (Gabon), 421–5 Palmottu (Finland), 426–8 Pocos de Caldas (Brazil), 415–18 Ruprechtov (Czech Republic), 420–1 701 summary of NNAA studies, 429 natural colloidal load, 394 natural colloids, 389 natural environment aquatic chemistry and radionuclide behaviour, 13–41 aqueous complexes, 24–7 colloids, 34–5 dissolution and precipitation, 16–24 natural water composition, 14–16 redox reactions, 35–41 surface sorption, 27–34 hydrogeology features relevant to radionuclide migration, 229–59 aquifer system, 242–6 groundwater flow equations for aquifer systems, 246–9 soil and subsoil groundwater movement, 233–42 solving flow equations for aquifer systems, 249–59 subsoil water content, 230–3 impact of colloidal transport on radionuclide migration, 384–404 colloid-facilitated radionuclide transport, 395–7 colloids characteristics, 393–5 colloids nature and origin, 388–93 field studies, 397–403 future trends, 403–4 overview, 384–7 radionuclides geochemistry and sorption, 387–8 radionuclide behaviour, 1–10 environmental compartments, 5–10 radionuclides, 2–5 radionuclide retention at solid/liquid interfaces, 261–88 future trends, 286–88 radionuclide sorption macroscopic studies, 263–71 sorption model, 271–82 spectroscopic techniques, 282–6 natural organic matter (NOM), 103, 106 sorption of metals, 133–5 addition order on M4+ sorption onto minerals, 134 uranium migration, 137 natural radioactivity, natural water, 14–16 components, 15–16 isotopic composition, 16 © Woodhead Publishing Limited, 2012 702 Index physical and chemical properties, 14–15 redox state, 39–41 classification scheme of redox environments, 41 stability of water and the ranges of Eh and pH conditions, 40 Naturally-Occurring Radioactive Materials, 610–11 near field system, 73–4 neptunium, 51, 193–4 Nevada Test Site, 137–8, 397–400, 610 locations of underground nuclear tests, 398 Newton–Raphson method, 339–41 nicotianamins, 489–90 Non-Ideal Competitive Adsorption–Donnan model, 125–8 distribution of proton sites of generic humic acid, 127 influence of ionic strength on humic acid, 127 Novaya Zemlya island, 610 nuclear power plants after severe accidents, 613–15 quantities of emitted radionuclides, 614 radioactive fallout in Europe after the Chernobyl accident, 616 during operation and after dismantling, 612–13 nuclear waste glasses, 74–5 nuclear waste repository natural analogues and development of radionuclide migration models, 411–41 nature and limitations, 413–15 radionuclide geochemistry and migration, 429–40 selected natural analogue sites, 415–29 safety assessment, 646–91 gaps in understanding and qualification and quantification of models, 689–90 integration of main radionuclide migration processes and parameters, 686–9 repository concepts, 648–61 safety assessment methodology, 661–86 nuclear weapon test sites, 609–10 Oak Ridge Reservation, 605 Office of Legacy Management, 640 Oklo (Gabon), 421–5 cross-section of the Okelobondo deep reactor, 423 cross-section of zone and location of reactors, 422 isotopic ratio of 90Zr/91Zr of bulk rock samples, 425 shallow reactor of Bangombe, 423 on-site burial, 624–5 organic colloids, 389 organic compounds, 185 organic ligand, 171–2 citric acid, 172 organic matter, 586–8 Osamu Utsumi, 416–17 outer-sphere complexes, 25–6 overpack, 73–4 oxidation state actinide in aqueous solution, 46–52 light actinides, 47 Pourbaix diagrams, 50 oxidation–reduction reactions, 162 oxides, 266–71 Palmottu (Finland), 426–8 cross-section of site showing lithology, hydraulic barrier and groundwater location, 427 uranium concentrations in calcite fractions, 428 parallel flow, 251 particulate facilitated transport, 417 perched aquifers, 243–4 illustration, 244 local water table above a low permeability layer, 244 PHAST, 636 phenolic groups, 110 phosphate complexes, 63 phosphate fertiliser agricultural land after fertiliser application, 621 mining and production sites, 606–9 minimal and maximal concentrations of radionuclides, 608 plants for uranium recovery, 609 uranium recovery from phosphate rocks, 609 photolithotrophs see phototrophs photosynthesis, 498–9 phototrophs, 163 © Woodhead Publishing Limited, 2012 Index PhreePlot, 65 phytochelatins, 489–90 phytoextraction, 627 phytoremediation, 627–9 phytovolatilisation, 628 Picard method, 339 pitchblende, 418 plutonium, 51–2, 492, 497 biosorption and bioaccumulation, 187–92 interaction with bacteria and kaolinite clay, 192 biotransformation, 179–87 biodegradation of Pu(IV)-citrate complexes, 185–7 dissolution of PuO2, 182–3 dissolution of PuO2 by heterotrophic bacteria and fungi, 183 microbial and abiotic reduction of Pu(VI) to Pu(III), 182 mobilisation from contaminated soil due to microbial activity, 187 organic compounds, 185 oxidation and reduction, 182 oxidative dissolution of PuO2 to Pu(VI), 183 reductive dissolution of Pu(IV) to Pu(III) by anaerobic bacteria, 184–5 reductive precipitation, 184 migration after fallout in Nagasaki, Japan, 135–6 migration in the soils of Chernobyl, Ukraine, 136 plutonium dioxide (PuO2) dissolution, 182–3 dissolution by heterotrophic bacteria and fungi, 183 oxidative dissolution to Pu(VI), 183 plutonium (III) Pu(III), 184–5 plutonium (IV) Pu(IV), 184–5 plutonium (VI) Pu(VI), 183 Pocos de Caldas (Brazil), 415–18 cross-section of Morro Ferro area, 417 cross-section of Osamu Utsumi mine, 416 polyelectrolytic model, 112–13 porous medium, 230–33 distribution of solutes, 232–3 Pourbaix diagrams, 49 precipitation, 16–24, 75–6 prescribed flux boundaries, 250 prescribed head boundaries, 249–50 outcrop of a confined aquifer, 250 703 primordial nuclides, Protection of the Environment from Ionising Radiation in a Regulatory Context (PROTECT), 552, 556–7 proton-exchanging functional groups, 109–10 pseudocolloid, 386, 392 Pu(IV)-citrate complexes, 185–7 ESI–MS of 242Pu-citrate, 186 proposed structures at pH 6, 186 pulse injection solution, 308–11 ADE solution to a step input, 311 one-dimensional ADE, 309 radial flow, 251–2 pumping well, 252 radiation doses assessing in humans, 540–51 concepts and quantities, 540–4 exposure by ingestion, 547–51 exposure by inhalation, 546–7 external exposure, 544–6 other pathways, 551 radiation weighting factors, 542 tissue weighting factors, 542 assessing in non-human biota, 551–9 development of approaches and tools, 557–9 effects of radiation, 553–5 generic interaction matrix, 562–3 protection approaches and tools development, 557–9 radiological protection in environmental context, 552–3 species sensitivity distribution based on EDR10 values, 556 threshold dose rates for radiation effect, 555–7 radioactive materials, 611–12 radioactive waste disposal carbon, 92 iodine, 88 selenium, 81–4 technetium, 80 radioactive waste repositories, 617–18 radioactive waste site quantitative assessment of radionuclide migration, 570–96 Chernobyl Pilot site in the Red Forest, 573–82 future trends, 592–6 prediction of 90Sr migration, 585–92 © Woodhead Publishing Limited, 2012 704 Index stationary hydrodynamic and geochemical conditions in modelling, 582–4 radioactivity, 588 radiochemistry, 1, radioelements, radioisotopes, radiological protection environmental context, 552–3 radionuclide behaviour aquatic chemistry in the environment, 13–41 aqueous complexes, 24–7 colloids, 34–5 dissolution and precipitation, 16–24 natural water composition, 14–16 redox reactions, 35–41 surface sorption, 27–34 environmental compartments, 5–10 impact of humic substances, 103–41 future trends, 141 humic acid molecule, 106–10 impact on radionuclide transport, 135–41 metal ion-humic interactions discrete model, 110–22 metal ion–humic interactions kinetic models, 128–35 metal ion–humic interactions multiligand and macromolecular models, 122–8 overview, 103–6 natural environment, 1–10 radionuclides, 2–5 radionuclide bioavailability, radionuclide chemistry, 163–5 radionuclide deposition, 262 radionuclide migration, 10, 302–379 applications, 348–79 calcite dissolution in fresh-salt water mixing zone, 348–53 137 Cs contaminated soil remediation, 353–62 fractured media reactive transport, 363–6 multicomponent reactive transport at Ratones uranium mine, 366–79 coupling chemistry to transport, 316–48 binary system in equilibrium, 322–30 coupled equations, 342–8 Damkhoeler number, 320–2 formulation of reactions, 330–41 sorption effect, 318–20 hydrogeology features in natural environment, 229–59 aquifer system, 242–6 groundwater flow equations for aquifer systems, 246–9 soil and subsoil groundwater movement, 233–42 solving flow equations for aquifer systems, 249–59 subsoil water content, 230–3 impact of colloidal transport in natural environment, 384–404 colloid-facilitated radionuclide transport, 395–7 colloids characteristics, 393–5 colloids nature and origin, 388–93 field studies, 397–403 future trends, 403–4 overview, 384–7 radionuclides geochemistry and sorption, 387–8 laboratory and in situ experiments, 446–83 decimetre-scale on radionuclide transport in non-consolidated media, 466–72 French Callovo-Oxfordian claystone, 458–66 future trends, 472–4 information on different scales, 447 studies at different scales on radionuclide diffusion, 448–54 Swiss Opalinus Clay, 453–8 quantitative assessment of waste dumps in Chernobyl exclusion zone, 570–96 Chernobyl Pilot site in the Red Forest, 573–82 future trends, 592–6 prediction of 90Sr migration, 585–92 stationary hydrodynamic and geochemical conditions in modelling, 582–4 repository concepts, 648–61 bentonite buffer material, 650, 652 geosphere system, 652–5 high-level radioactive waste in clay environment, 655–61 KBS3 concept, 648 spent nuclear fuel, 648, 650 safety assessment of nuclear waste repository, 646–91 © Woodhead Publishing Limited, 2012 Index gaps in understanding and qualification and quantification of models, 689–90 integration of main radionuclide migration processes and parameters, 686–9 safety assessment methodology, 661–86 transport phenomenon, 303–16 radionuclide migration models natural analogues of nuclear waste repository, 411–41 nature and limitations, 413–15 radionuclide geochemistry and migration, 429–40 selected natural analogue sites, 415–29 radionuclide mobility, radionuclide retention future trends, 286–88 radionuclide sorption macroscopic studies, 263–71 solid/liquid interfaces in natural environment, 261–88 sorption model, 271–82 spectroscopic techniques, 282–6 radionuclide sorption macroscopic studies, 263–71 clay minerals, 264–6 distribution coefficients Kds* and Kdd*, 270–1 oxides and calcite, 266–71 sorption isotherm of Eu onto Camontmorillonte, 267 model, 271–82 cation exchange on clay minerals, 272–3 general, 271–2 ion exchange, 277–82 surface complexation on oxides and clay minerals, 274–7 radionuclide transfer processes biosphere, 484–507 digestive barrier, 500–2 effect on metabolic pathways, 498–500 animals, 499 iron metabolism, 500 plants, 498–9 vitamin D and cholesterol metabolisms, 499–500 future trends, 506–7 homeostasis and stress, 505–6 main antioxidant molecules, 505–6 705 major pro-oxidant molecules, 505 uranium, 506 membrane transport, 502–5 main classes of transport in the cell, 502 speciation and interactions with biological ligands, 486–90 generic information on RN speciation, 486–7 hard interactions with oxygen-rich peptide sequences, 489 phytochelatins and nicotianamins, 489–90 soft interactions with cysteine-rich peptide sequences, 489 specific interactions with other elements, 487 transferrin, 489 transfer to animal species and biodistribution, 493–6 animal living in aquatic medium, 494–5 mammalian species, 495–6 nominal values of transfer factors, 494 values of bioconcentration factors, 494 transfer to man, 496–8 ingestion factors, 497 transfer to plants and biodistribution, 490–3 foliar pathway, 491 root pathway, 490–1 root transfer factor of uranium, 492 soil-plant transfer factors, 490 uptake of different RNs, 491–3 radionuclide transport, 395–7 modelling and radiation dose calculation, 517–63 comprehensive assessment, 559–60 future trends, 560–3 modelling in the environment, 519–40 radiation doses to humans, 540–51 radiation doses to non-human biota, 551–9 radionuclides, 2–5 colloid-facilitated migration, lowsolubility, 403 concentration in coal, fly ash and bottom ash, 619 geochemistry and sorption, 387–8 impact of humic substances on transport, 135–41 © Woodhead Publishing Limited, 2012 706 Index migration in organic-rich deep underground media, 138–40 transport of HTO, Th, U and Am through a column, 139 microorganisms impact in contaminated environments and waste materials, 161–214 biosorption and bioaccumulation of uranium and plutonium, 187–92 biotransformation of actinides and related elements, 193–6 biotransformation of fission and activation products, 196–206 biotransformation of plutonium, 179–87 biotransformation of uranium, 165–79 low-, intermediate, and high-level waste repository site, 206–13 overview, 161–5 summary of key microbial processes and transformations, 213 physical and chemical properties of some long-lived radionuclides, 6–7 remediation of contaminated sites, 601–40 environmental monitoring tools, 633–7 examples of remediation, 637–40 methods of cleaning contaminated sites, 622–33 potential sources of radionuclide release, 602–22 retention in bentonite and clay rock, 76–7 solution and interfacial chemistry, 77–92 sources, 517–18 spent nuclear UO2 fuel, radium, 195–6 reactive transport, 342, 344 Red Forest, 571 Chernobyl Pilot site, 573–82 redox equilibrium, 82 redox fronts, 417, 424 redox properties, 108–9 redox reactions, 35–41 Eh/pH stability field of water, 38–9 diagram for the Fe–S–H2O system, 39 redox state of natural waters, 39–41 classification scheme of redox environments, 41 stability of water and the ranges of Eh and pH conditions, 40 redox theory, 36–7 redox theory, 36–7 standard potential E0 of major redox couples, 37 reductive dissolution Pu(IV) to Pu(III) by anaerobic bacteria, 184–5 dissolution and reduction by Clostridium sp., 185 reductive precipitation, 168, 170–1 plutonium, 184 uranium(VI) reduction to U(IV) by Clostridium sp., 170 Relative Biological Effectiveness (RBE), 541 remediation 137 Cs contaminated soil, 353–62 base cases results, 359–60 cation exchange reactions and selectivity coefficients, 357 composition (mol/kg water) of initial and infiltrating water, 358 Cs extraction with K in batch experiments, 357 hydraulic parameters of the mobile and immobile zones, 357 numerical and conceptual model, 355–7 results, 357–62 sensitivity, 361–2 site description, 354 soil aggregates representation model, 356 potential sources of radionuclide release, 602–22 agricultural land after long-term phosphate fertiliser application, 621 coal power plants and fly ash deposition, 618–19 landfills and waste deposits, 615, 617 nuclear facilities after severe accidents, 613–15 nuclear power facilities during operation and after dismantling, 612–13 oil/gas production and treatment sites, 610–11 other sources, 622 phosphor-fertiliser mining and production sites, 606–9 production and use for medical, research or industrial purposes, 611–12 radioactive waste repositories, 617–18 © Woodhead Publishing Limited, 2012 Index sites contaminated with depleted uranium, 620 surface and subsurface nuclear weapon test sites, 609–10 uranium enrichment and reprocessing plants, 604–6 uranium mining and milling sites, 602–4 radionuclide contaminated sites, 601–40 environmental monitoring tools, 633–7 examples of remediation, 637–40 methods of cleaning contaminated sites, 622–33 residual, 341 RESRAD-BIOTA, 558 resuspension aquatic environment, 539 terrestrial environment, 533–5 resuspension factor, 534 RETRASO code, 349 rhizofiltration, 627–8 RICH-PHREQC, 636 risk assessment, 636–7 river solution, 254–5 contact with a confined aquifer, 255 rock oxidation model, 378 Rocky Flats, 400–1 Rocky Flats Nuclear Weapons Plant, 401 Rocky Flats Nuclear Weapons Plant, 400 Rocky Flats Plant, 638–9 Ruprechtov (Czech Republic), 420–1 simplified geological cross-section of the Tertiary basin, 421 safety assessment integration of main radionuclide migration processes and parameters, 686–9 consequences for migration, 689 French SA models, 687, 689 processes and parameters is SKB safety assessment, 686–7 methodology, 661–86 French methodology, 676, 678–9, 681, 683–4, 686 SKB methodology, 662–76 nuclear waste repository, 646–91 gaps in understanding and qualification and quantification of models, 689–90 integration of main radionuclide migration processes and parameters, 686–9 707 repository concepts, 648–61 safety assessment methodology, 661–86 saturation index, 20 scale effect, 312 sediments, 549 selectivity coefficients, 273 selenium, 80–6, 199–200, 487, 492–3, 498, 504–5 aquatic ecosystems and geological disposal of radioactive waste, 81–4 solubility-controlled aqueous concentrations, 83 Eh–pH diagram in water, 81 terrestrial ecosystems, 84–6 semi-analytical models, 536 Semipalatinsk, 610 sensitivity analysis, 521 sequential iteration see Picard method SHETRAN model, 529 SKB safety assessment gaps in understanding and qualification and quantification of models, 689–90 safety assessment methodology, 662–76 additional analyses, 673 analysis of selected scenarios, 668, 673 central canister corrosion case, 674 climatic evolutions in SR-Site, 665 consequence analyses and conclusions, 673, 675–6 equilibrium data, 668–71 features, events and processes, 663–4 geosphere fluxes, 675 indicators and margins from SR-Site, 666 key data, 667 near-field doses assuming radionuclide solubility limits, 674 process description, 664–5 reference evolution, 667–8 safety functions, 665–6 sorption partition coefficients, 672–3 11-step safety assessment, 663 slug-test solution, 254 cylindrical symmetry, 255 soil-plant transfer factor, 529 uranium, 530–1 soil rehabilitation, 625–7 dig and dump, 626 dig and treat, 626–7 © Woodhead Publishing Limited, 2012 708 Index exclusion, 626 soils, 549 solid actinide phases, 45 solid/liquid interfaces future trends, 286–88 radionuclide retention in natural environment, 261–88 radionuclide sorption macroscopic studies, 263–71 sorption model, 271–82 spectroscopic techniques, 282–6 solid phase, 52–6 solid-solutions, 22–4 lipmann diagram for a hypothetical system, 24 solid surface characteristics, 27–8 cation exchange capacities, 27 pH of the point of zero charge of minerals, 28 solubility limits, 75–6 solubility phenomena, 52–6 solubility product, 20 selected for common minerals, 21 solute mass, 305 solutus curve, 23 sorption distribution coefficients, 428 sorption isotherms, 29–31 adsorption of arsenate by calcite surfaces, 29 Langmuir and Freundlich isotherms, 31 sorptive fractionation, 132 speciation calculations, 339–41 radionuclide, 486–7 stability constants log, 488 speciation/solubility models, 430–6 analytical and mineralogical characterisation data, 432–4 dissolved uranium concentration in Bangombe reactor and concentration in equilibrium, 434 theoretical molar fraction of REE, 433 improvement of thermodynamic databases, 431 limitations/differences of geochemical codes used, 432 validity assessment and alternative conceptual approaches 434-6 sample calculations of uranium concentration, 435 Sr:Ca correlation in groundwater samples, 436 Specific Interaction Theory, 18 Specific Ion Interaction Theory (SIT), 56 spent fuels, 75 spent nuclear fuel, 648, 650 inventory of various fuel types, 651 90 Sr geochemical conditions on strontium-90 migration, 590–2 distribution patterns of strontium-90 in LAB multilevel well profile, 591 other factors in strontium-90 leaching, 588–90 hydrologic leaching losses, 588 laboratory multilevel well profile, 589 pine root uptake of nutrient elements, 589–90 prediction of migration, 585–92 chemical composition of groundwater upstream, 585–6 other factors in strontium-90 leaching, 588–90 steady-state flux phase, 449 STERM-1D, 583 stochastic effect, 540 stoichiometric matrix, 331–5 straight-line boundary solution, 253–4 real well and image well, 254 strontium, 200 subsoil soil groundwater movement, 233–42 water content, 230–3 fractured rocks, 233 porous medium, 230–33 sulfate-reducing bacteria, 195–6 surface complexation anions and cations, 275–7 sorption of selenite on Na-illite, 276 surface complexation modelling, 278 oxides and clay minerals, 274–7 surface complexation modelling (SCM), 33–4, 634–5 surface precipitation, 32 surface sorption, 27–34 influence of NOM on metal, 133–5 addition order on M4+ sorption onto minerals, 134 mechanisms, 31–4 mineral–water interfaces processes, 31 metal ion retention implications, 131 sorption isotherms, 29–31 © Woodhead Publishing Limited, 2012 Index surface characteristics of solids, 27–8 Swiss Opalinus Clay, 453–8 diffusion measurements in field laboratory at Mont Terri, 457–8 field diffusion experiment layout, 459 field experiments performed in Mont Terri URL, 457 large-scale laboratory experiment, 456–7 schematic overview of experiment, 457 small-scale laboratory experiment, 453–6 technetium, 77–80, 197–9 aquatic and terrestrial ecosystems, 77–80 Eh–pH diagram in water, 78 soil sulfate-reducing bacterium, 79 geological disposal of radioactive waste, 80 microbial speciation, 198–9 reduction of pertechnetate by Clostridium sphenoides, 198 Tc(IV) solubility in the presence of organic ligands, 198 technetium (IV) Tc(IV) solubility in the presence of organic ligands, 198 terrestrial ecosystems carbon, 91–2 chlorine, 89–90 iodine, 87–8 selenium, 84–6 technetium, 77–80 terrestrial environment, 524–35 dry deposition, 524–6 integrated model for soil transport and plant uptake, 529, 532–3 resuspension, 533–5 transfer to animals, 533 translocation, 527–8 uptake of radionuclides from the soil, 528–9 weathering, 527 wet deposition, 526–7 Theis solution, 252–3 Theis-type curve, 253 thermodynamic sorption models, 437 thorium, 2, 50–1, 52–3, 196, 602–3 Three Mile Island accident, 614 through-diffusion technique, 449, 451 experimental setup, 450 time resolved laser fluorescence spectroscopy, 284–5 709 Tomsk-7, 605 top-down approach, 439 total activity product, 22, 23 total inorganic carbon (TIC), 337 total porosity, 230 common values of rock porosity, 231 transferrin, 489 translocation, 527–8 translocation factor, 528 transport equations, 343 transport phenomenon, 303–16 advection–dispersion equation (ADE), 303–6 advection–dispersion equation (ADE) behaviour, 306–11 advection–dispersion equation (ADE) limitation, 311–16 reactive transport in multi-rate-mass transfer (MRMT) formulations, 316 Trench 22, 576, 579–80 tricarbonato-uranyl complexes, 62 triple-layer (TL), 34 tritium, 204–6, 493, 498, 501 microbial generation of carbon-14 and tritiated gases, 205 release of radioactive gases by microbial activity, 205–6 uncertainty analysis, 521 unconfined aquifers, 242–4 equations, 247–8 United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR), 539 unsaturated medium, 231–2 uraninite, 418 uranium, 2, 51, 52–3, 487, 496–7, 501, 506 biosorption and bioaccumulation, 187–92 biofilms, 190–1 extra- and intracellular accumulation by Halomonas sp., 189 predominant structures associated with bacteria, 188 biotransformation, 165–79 autotrophic microbial activity, 166 dissolution from ores, 165 heterotrophic microbial activity, 166–8 metal-citrate complexes under denitrifying conditions, 174 organic ligand association, 171–2 reductive precipitation, 168, 170–1 © Woodhead Publishing Limited, 2012 710 Index ternary iron–uranium–citrate complex, 174–5 uranyl citrate under aerobic conditions, 173–4 uranyl citrate under anaerobic conditions, 175–9 contaminated sites, 620 enrichment and reprocessing plants, 604–6 contaminated area after Tomsk accident with gamma dose rates, 607 migration and association to NOM, 137 mining and milling sites, 602–4 specific activity of 238U decay series nuclides, 604 uptake by Phaseolus vulgaris, 491–2 uranium hexafluoride, 605 uranyl citrate biotransformation under aerobic conditions, 173–4 biodegradation of metal–citrate complexes, 173 biotransformation under anaerobic conditions, 175–9 bioreduction of U(VI)–citrate complex by Clostridia, 176 complexes before and after bacterial reduction, 177 re-oxidation of uranium(IV) complexed with organic ligands, 180–1 reduction of biligand U(VI)–citrate to monoligand U(IV)–citrate complex, 178 reduction of U-phthalate by Clostridium sp., 179 uranium citrate before and after reduction by Clostridium sp., 177 UV-vis spectra show reduction of U(VI) to U(IV), 176 uranyl ion, 489 validation, 532–3 valley aquifers, 243 vector-matrix notation, 336 verification, 532 vitamin D, 499–500 volatilisation, 84, 85–6 volcanic rock aquifers, 244 waste deposits, 615, 617 waste matrix, 74–7 water content subsoil, 230–3 fractured rocks, 233 porous medium, 230–33 water treatment, 629–33 schematic of passive water treatment systems, 632 treatment technologies for certain radioactive contaminants, 630 weathering, 527 wet deposition, 526–7 X-ray absorption fine structure spectroscopy, 282–3 X-ray standing waves, 284 Yucca Mountain site, 210–12 microbial activity impact, 212–13 zeta potential, 268 ZIP transporters, 503 © Woodhead Publishing Limited, 2012 ... principles of aquatic chemistry and water–rock interaction that determine the composition of natural waters and therefore influence the behaviour of aquatic species including radionuclides in the. .. is in- situ experiments (Chapter 12) and in- situ investigations of radionuclides in natural analogue sites (Chapter 11) The latter studies help in understanding radionuclide behaviour under the. .. 2012 10 Radionuclide behaviour in the natural environment play a significant role for the overall radionuclide migration and their relative contribution differs from one environment to the other