Measurement and modelling of reactive transport in geological barriers for nuclear waste containment

Xiong, Qingrong; Joseph, Claudia; Schmeide, Katja; Jivkov, Andrey P.

doi:10.1039/c5cp05243b

Title: Measurement and modelling of reactive transport in geological barriers for nuclear waste containment

Journal Article · 26 October 2015 · Physical Chemistry Chemical Physics. PCCP

DOI: https://doi.org/10.1039/c5cp05243b · OSTI ID:1234576

Xiong, Qingrong ^[1]; Joseph, Claudia ^[2]; Schmeide, Katja ^[3]; Jivkov, Andrey P. ^[1]

Univ. of Manchester (United Kingdom). Research Centre for Radwaste & Decommissioning and Modelling & Simulation Centre, Dalton Nuclear Inst.
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Glenn T. Seaborg Inst., Physical & Life Sciences Directorate
Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany). Inst. of Resource Ecology

Compacted clays are considered as excellent candidates for barriers to radionuclide transport in future repositories for nuclear waste due to their very low hydraulic permeability. Diffusion is the dominant transport mechanism, controlled by a nano-scale pore system. Assessment of the clays' long-term containment function requires adequate modelling of such pore systems and their evolution. Existing characterisation techniques do not provide complete pore space information for effective modelling, such as pore and throat size distributions and connectivity. Special network models for reactive transport are proposed here using the complimentary character of the pore space and the solid phase. Here, this balances the insufficient characterisation information and provides the means for future mechanical–physical–chemical coupling. The anisotropy and heterogeneity of clays is represented using different length parameters and percentage of pores in different directions. Resulting networks are described as mathematical graphs with efficient discrete calculus formulation of transport. Opalinus Clay (OPA) is chosen as an example. Experimental data for the tritiated water (HTO) and U(VI) diffusion through OPA are presented. Calculated diffusion coefficients of HTO and uranium species are within the ranges of the experimentally determined data in different clay directions. This verifies the proposed pore network model and validates that uranium complexes are diffusing as neutral species in OPA. In the case of U(VI) diffusion the method is extended to account for sorption and convection. Finally, rather than changing pore radii by coarse grained mathematical formula, physical sorption is simulated in each pore, which is more accurate and realistic.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344; EP/ K016946/1

OSTI ID:: 1234576

Report Number(s):: LLNL-JRNL-676844; PPCPFQ

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 17, Issue 45; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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References (54)

Discrete modelling of contaminant diffusion in porous media with sorption Xiong, Qingrong; Jivkov, Andrey P.; Yates, John R. Microporous and Mesoporous Materials, Vol. 185 https://doi.org/10.1016/j.micromeso.2013.09.038	journal	February 2014
Diffusion of ionic species in bentonite Leroy, P.; Revil, A.; Coelho, D. Journal of Colloid and Interface Science, Vol. 296, Issue 1 https://doi.org/10.1016/j.jcis.2005.08.034	journal	April 2006
Chloride Diffusion in Clay-Water Systems1 van Schaik, J. C.; Kemper, W. D. Soil Science Society of America Journal, Vol. 30, Issue 1 https://doi.org/10.2136/sssaj1966.03615995003000010014x	journal	January 1966
Pore-network extraction from micro-computerized-tomography images Dong, Hu; Blunt, Martin J. Physical Review E, Vol. 80, Issue 3 https://doi.org/10.1103/PhysRevE.80.036307	journal	September 2009
Two methods for pore network of porous media: TWO METHODS FOR PORE NETWORK OF POROUS MEDIA Gao, Shengyan; Meegoda, Jay N.; Hu, Liming International Journal for Numerical and Analytical Methods in Geomechanics, Vol. 36, Issue 18 https://doi.org/10.1002/nag.1134	journal	February 2012
Sorption of uranium(VI) onto Opalinus Clay in the absence and presence of humic acid in Opalinus Clay pore water Joseph, C.; Schmeide, K.; Sachs, S. Chemical Geology, Vol. 284, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2011.03.001	journal	May 2011
Site-bond modelling of porous quasi-brittle media Jivkov, A. P.; Gunther, M.; Travis, K. P. Mineralogical Magazine, Vol. 76, Issue 8 https://doi.org/10.1180/minmag.2012.076.8.12	journal	December 2012
Diffusion of ionic tracers in the Callovo-Oxfordian clay-rock using the Donnan equilibrium model and the formation factor Jougnot, D.; Revil, A.; Leroy, P. Geochimica et Cosmochimica Acta, Vol. 73, Issue 10 https://doi.org/10.1016/j.gca.2009.01.035	journal	May 2009
Extraction of physically realistic pore network properties from three-dimensional synchrotron X-ray microtomography images of unconsolidated porous media systems Al-Raoush, R. I.; Willson, C. S. Journal of Hydrology, Vol. 300, Issue 1-4 https://doi.org/10.1016/j.jhydrol.2004.05.005	journal	January 2005
Pore morphology and distribution in the Shaly facies of Opalinus Clay (Mont Terri, Switzerland): Insights from representative 2D BIB–SEM investigations on mm to nm scale Houben, M. E.; Desbois, G.; Urai, J. L. Applied Clay Science, Vol. 71 https://doi.org/10.1016/j.clay.2012.11.006	journal	January 2013
Invasion percolation: a new form of percolation theory Wilkinson, D.; Willemsen, J. F. Journal of Physics A: Mathematical and General, Vol. 16, Issue 14 https://doi.org/10.1088/0305-4470/16/14/028	journal	October 1983
Monte Carlo simulations of mesoscale fracture modelling of concrete with random aggregates and pores Wang, X. F.; Yang, Z. J.; Yates, J. R. Construction and Building Materials, Vol. 75 https://doi.org/10.1016/j.conbuildmat.2014.09.069	journal	January 2015
3D geometry and topology of pore pathways in Opalinus clay: Implications for mass transport Keller, Lukas M.; Holzer, Lorenz; Wepf, Roger Applied Clay Science, Vol. 52, Issue 1-2 https://doi.org/10.1016/j.clay.2011.02.003	journal	April 2011
Pore space and brittle damage evolution in concrete Jivkov, Andrey P.; Engelberg, Dirk L.; Stein, Robert Engineering Fracture Mechanics, Vol. 110 https://doi.org/10.1016/j.engfracmech.2013.05.007	journal	September 2013
Modeling diffusion and adsorption in compacted bentonite: a critical review Bourg, Ian C.; Bourg, Alain C. M.; Sposito, Garrison Journal of Contaminant Hydrology, Vol. 61, Issue 1-4 https://doi.org/10.1016/S0169-7722(02)00128-6	journal	March 2003
Anisotropic Diffusion in Layered Argillaceous Rocks: A Case Study with Opalinus Clay Van Loon, Luc R.; Soler, Josep M.; Müller, Werner Environmental Science & Technology, Vol. 38, Issue 21 https://doi.org/10.1021/es049937g	journal	November 2004
Stokes-Einstein relation for pure simple fluids Cappelezzo, M.; Capellari, C. A.; Pezzin, S. H. The Journal of Chemical Physics, Vol. 126, Issue 22 https://doi.org/10.1063/1.2738063	journal	June 2007
Cation diffusion in the electrical double layer enhances the mass transfer rates for Sr2+, Co2+ and Zn2+ in compacted illite Glaus, M. A.; Aertsens, M.; Appelo, C. A. J. Geochimica et Cosmochimica Acta, Vol. 165 https://doi.org/10.1016/j.gca.2015.06.014	journal	September 2015
Diffusion of HTO, 36Cl− and 125I− in Opalinus Clay samples from Mont Terri Van Loon, L. R.; Soler, J. M.; Bradbury, M. H. Journal of Contaminant Hydrology, Vol. 61, Issue 1-4 https://doi.org/10.1016/S0169-7722(02)00114-6	journal	March 2003
Multicomponent Diffusion Modeling in Clay Systems with Application to the Diffusion of Tritium, Iodide, and Sodium in Opalinus Clay Appelo, C. Anthony J.; Wersin, Paul Environmental Science & Technology, Vol. 41, Issue 14 https://doi.org/10.1021/es0629256	journal	July 2007
Preferred Orientations and Anisotropy in Shales: Callovo-Oxfordian Shale (France) and Opalinus Clay (Switzerland) Loon, Van L. R. Clays and Clay Minerals, Vol. 56, Issue 3 https://doi.org/10.1346/CCMN.2008.0560301	journal	June 2008
Characterization of multi-scale microstructural features in Opalinus Clay Keller, Lukas M.; Schuetz, Philipp; Erni, Rolf Microporous and Mesoporous Materials, Vol. 170 https://doi.org/10.1016/j.micromeso.2012.11.029	journal	April 2013
A reactive transport modeling approach to simulate biogeochemical processes in pore structures with pore-scale heterogeneities Gharasoo, Mehdi; Centler, Florian; Regnier, Pierre Environmental Modelling & Software, Vol. 30 https://doi.org/10.1016/j.envsoft.2011.10.010	journal	April 2012
A Network Model for Diffusion in Media with Partially Resolvable Pore Space Characteristics Jivkov, Andrey P.; Xiong, Qingrong Transport in Porous Media, Vol. 105, Issue 1 https://doi.org/10.1007/s11242-014-0360-1	journal	July 2014
Assessment of surface area normalisation for interpreting distribution coefficients (Kd) for uranium sorption Payne, Timothy E.; Brendler, Vinzenz; Comarmond, M. Josick Journal of Environmental Radioactivity, Vol. 102, Issue 10 https://doi.org/10.1016/j.jenvrad.2010.04.005	journal	October 2011
Discrete Calculus: Applied Analysis on Graphs for Computational Science Grady, Leo J.; Polimeni, Jonathan R. https://doi.org/10.1007/978-1-84996-290-2	book	January 2010
Diffusion of U(VI) in Opalinus Clay: Influence of temperature and humic acid Joseph, C.; Van Loon, L. R.; Jakob, A. Geochimica et Cosmochimica Acta, Vol. 109 https://doi.org/10.1016/j.gca.2013.01.027	journal	May 2013
A triple-layer model of the surface electrochemical properties of clay minerals Leroy, P.; Revil, A. Journal of Colloid and Interface Science, Vol. 270, Issue 2 https://doi.org/10.1016/j.jcis.2003.08.007	journal	February 2004
Elastic behaviour of a regular lattice for meso-scale modelling of solids Jivkov, Andrey P.; Yates, John R. International Journal of Solids and Structures, Vol. 49, Issue 22 https://doi.org/10.1016/j.ijsolstr.2012.06.010	journal	November 2012
Pore network modelling: determination of the dynamic profiles of the pore diffusivity and its effect on column performance as the loading of the solute in the adsorbed phase varies with time Meyers, J. J.; Crosser, O. K.; Liapis, A. I. Journal of Chromatography A, Vol. 908, Issue 1-2 https://doi.org/10.1016/S0021-9673(00)00795-0	journal	January 2001
Pore-scale imaging and modelling Blunt, Martin J.; Bijeljic, Branko; Dong, Hu Advances in Water Resources, Vol. 51 https://doi.org/10.1016/j.advwatres.2012.03.003	journal	January 2013
Obtaining the porewater composition of a clay rock by modeling the in- and out-diffusion of anions and cations from an in-situ experiment Appelo, C. A. J.; Vinsot, A.; Mettler, S. Journal of Contaminant Hydrology, Vol. 101, Issue 1-4 https://doi.org/10.1016/j.jconhyd.2008.07.009	journal	October 2008
Porewater chemistry in compacted re-saturated MX-80 bentonite Bradbury, Michael H.; Baeyens, Bart Journal of Contaminant Hydrology, Vol. 61, Issue 1-4 https://doi.org/10.1016/S0169-7722(02)00125-0	journal	March 2003
A novel architecture for pore network modelling with applications to permeability of porous media Jivkov, Andrey P.; Hollis, Cathy; Etiese, Friday Journal of Hydrology, Vol. 486 https://doi.org/10.1016/j.jhydrol.2013.01.045	journal	April 2013
Transferability of geoscientific information from various sources (study sites, underground rock laboratories, natural analogues) to support safety cases for radioactive waste repositories in argillaceous formations Mazurek, Martin; Gautschi, Andreas; Marschall, Paul Physics and Chemistry of the Earth, Parts A/B/C, Vol. 33 https://doi.org/10.1016/j.pce.2008.10.046	journal	January 2008
The effect of time on the weathering of silicate minerals: why do weathering rates differ in the laboratory and field? White, Art F.; Brantley, Susan L. Chemical Geology, Vol. 202, Issue 3-4 https://doi.org/10.1016/j.chemgeo.2003.03.001	journal	December 2003
Study of Sorption-Retarded U(VI) Diffusion in Hanford Silt/Clay Material Bai, Jing; Liu, Chongxuan; Ball, William P. Environmental Science & Technology, Vol. 43, Issue 20 https://doi.org/10.1021/es901306c	journal	October 2009
Monte Carlo simulations of mesoscale fracture of concrete with random aggregates and pores: a size effect study Wang, Xiaofeng; Yang, Zhenjun; Jivkov, Andrey P. Construction and Building Materials, Vol. 80 https://doi.org/10.1016/j.conbuildmat.2015.02.002	journal	April 2015
A Consistance Model for Anion Exclusion and Surface Diffusion Lehikoinent, J.; Muurinen, A.; Valkiainen, M. MRS Proceedings, Vol. 556 https://doi.org/10.1557/PROC-556-663	journal	January 1999
Predicting Solute Transport in Structured Soil Using Pore Network Models Köhne, J. Maximilian; Schlüter, Steffen; Vogel, Hans-Jörg Vadose Zone Journal, Vol. 10, Issue 3 https://doi.org/10.2136/vzj2010.0158	journal	January 2011
A high-resolution abrasive method for determining diffusion profiles of sorbing radionuclides in dense argillaceous rocks Van Loon, L. R.; Eikenberg, J. Applied Radiation and Isotopes, Vol. 63, Issue 1 https://doi.org/10.1016/j.apradiso.2005.02.001	journal	July 2005
Flow in porous media — pore-network models and multiphase flow Blunt, Martin J. Current Opinion in Colloid & Interface Science, Vol. 6, Issue 3 https://doi.org/10.1016/S1359-0294(01)00084-X	journal	June 2001
Pore-network modeling of biofilm evolution in porous media Ezeuko, C. C.; Sen, A.; Grigoryan, A. Biotechnology and Bioengineering, Vol. 108, Issue 10 https://doi.org/10.1002/bit.23183	journal	May 2011
Influence of reaction kinetics and mesh refinement on the numerical modelling of concrete/clay interactions Marty, Nicolas C. M.; Tournassat, Christophe; Burnol, André Journal of Hydrology, Vol. 364, Issue 1-2 https://doi.org/10.1016/j.jhydrol.2008.10.013	journal	January 2009
Diffusion and dispersion in porous media Whitaker, Stephen AIChE Journal, Vol. 13, Issue 3 https://doi.org/10.1002/aic.690130308	journal	May 1967
Properties of a three-dimensional Poisson-Voronoi tesselation: A Monte Carlo study Kumar, Susmit; Kurtz, Stewart K.; Banavar, Jayanth R. Journal of Statistical Physics, Vol. 67, Issue 3-4 https://doi.org/10.1007/BF01049719	journal	May 1992
Capillary behavior of a perfectly wetting liquid in irregular triangular tubes Mason, Geoffrey; Morrow, Norman R. Journal of Colloid and Interface Science, Vol. 141, Issue 1 https://doi.org/10.1016/0021-9797(91)90321-X	journal	January 1991
Detailed physics, predictive capabilities and macroscopic consequences for pore-network models of multiphase flow Blunt, Martin J.; Jackson, Matthew D.; Piri, Mohammad Advances in Water Resources, Vol. 25, Issue 8-12 https://doi.org/10.1016/S0309-1708(02)00049-0	journal	August 2002
Microstructure-informed modelling of damage evolution in cement paste Zhang, Mingzhong; Jivkov, Andrey P. Construction and Building Materials, Vol. 66 https://doi.org/10.1016/j.conbuildmat.2014.06.017	journal	September 2014
An integrated sorption–diffusion model for the calculation of consistent distribution and diffusion coefficients in compacted bentonite Ochs, Michael; Lothenbach, Barbara; Wanner, Hans Journal of Contaminant Hydrology, Vol. 47, Issue 2-4 https://doi.org/10.1016/S0169-7722(00)00157-1	journal	February 2001
Multicomponent diffusion of a suite of tracers (HTO, Cl, Br, I, Na, Sr, Cs) in a single sample of Opalinus Clay Appelo, C. A. J.; Van Loon, L. R.; Wersin, P. Geochimica et Cosmochimica Acta, Vol. 74, Issue 4 https://doi.org/10.1016/j.gca.2009.11.013	journal	February 2010
Three-dimensional mixed-wet random pore-scale network modeling of two- and three-phase flow in porous media. II. Results Piri, Mohammad; Blunt, Martin J. Physical Review E, Vol. 71, Issue 2 https://doi.org/10.1103/PhysRevE.71.026302	journal	February 2005
Shape Factor and Hydraulic Conductance in Noncircular Capillaries Patzek, T. W.; Silin, D. B. Journal of Colloid and Interface Science, Vol. 236, Issue 2 https://doi.org/10.1006/jcis.2000.7413	journal	April 2001
Long-term diffusion experiment at Mont Terri: first results from field and laboratory data Wersin, P.; Van Loon, L. R.; Soler, J. M. Applied Clay Science, Vol. 26, Issue 1-4 https://doi.org/10.1016/j.clay.2003.09.007	journal	August 2004

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