Complete restriction of 36Cl-diffusion by celestite precipitation in densely compacted illite

Aurélie Chagneau 1, 2 Christophe Tournassat 1, 3 Carl I. Steefel 3 Ian C. Bourg 4, 3 Stéphane Gaboreau 1 Imène Esteve 5 Tomas Kupcik 2 Francis Claret 1 Thorsten Schäfer 2
1 BRGM - Bureau de Recherches Géologiques et Minières (BRGM)
2 KIT - Karlsruhe Institute of Technology
3 LBNL - Lawrence Berkeley National Laboratory [Berkeley]
4 Princeton University
5 IMPMC - Institut de minéralogie, de physique des matériaux et de cosmochimie
Abstract : Industrial companies and public waste management agencies envision clay-rich materials as efficient barriers for large-scale confinement of nuclear waste and subsurface CO2. In clays, small pores hinder water flow and make diffusion the dominant solute-transport mechanism. Most clay mineral structures exhibit a negative charge that is balanced by an electrical double layer at the mineral water interface. This clay mineral property delays cation migration through adsorption processes, decreases the accessible porosity and diffusion fluxes for anions compared to those of water and cations, and gives rise to semipermeable membrane properties. Here we present experimental data that demonstrate for the first time that anions can be completely excluded from the smallest pores within a compacted illitic clay material, an observation that has important implications for the ability to accurately predict the containment capacity of clay-based barriers. In a series of multitracer diffusion experiments, celestite (SrSO4) precipitation reduced the porosity of compacted illite to the point where the water tracer diffusion flux decreased by half, while the chloride diffusion flux decreased to zero. This result demonstrates that anions can be completely excluded from the smallest pores within a compacted clay material.
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Contributeur : Christophe Tournassat <>
Soumis le : vendredi 5 février 2016 - 14:17:52
Dernière modification le : mardi 2 avril 2019 - 03:05:59

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BRGM | IMPMC | ALLINSP | UPMC | SORBONNE-UNIVERSITE | SU-SCIENCES | MNHN

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Aurélie Chagneau, Christophe Tournassat, Carl I. Steefel, Ian C. Bourg, Stéphane Gaboreau, et al.. Complete restriction of 36Cl-diffusion by celestite precipitation in densely compacted illite. Environmental Science & Technology Letters, 2015, 2 (5), pp.139-143. 〈10.1021/acs.estlett.5b00080〉. 〈hal-01269920〉

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