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 · 25 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

OSTI ID:: 1234576

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

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

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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