Hostname: page-component-586b7cd67f-rdxmf Total loading time: 0 Render date: 2024-11-28T03:20:35.289Z Has data issue: false hasContentIssue false

The Tournemire industrial analogue: reactive-transport modelling of a cement–clay interface

Published online by Cambridge University Press:  09 July 2018

C. Watson*
Affiliation:
Quintessa Ltd., The Hub, 14 Station Road, Henley-on-Thames, Oxfordshire RG9 1AY, UK
D. Savage
Affiliation:
Savage Earth Associates Limited, 32 St Albans Avenue, Bournemouth, BH8 9EE, UK
J. Wilson
Affiliation:
Quintessa Ltd., The Hub, 14 Station Road, Henley-on-Thames, Oxfordshire RG9 1AY, UK
S. Benbow
Affiliation:
Quintessa Ltd., The Hub, 14 Station Road, Henley-on-Thames, Oxfordshire RG9 1AY, UK
C. Walker
Affiliation:
JAEA, 4-33 Muramatsu, Tokai, Naka-gun, Ibaraki, 319-1194, Japan
S. Norris
Affiliation:
Nuclear Decommissioning Authority, Building 587, Curie Avenue, Harwell, Oxfordshire OX11 0RH, UK
*
Rights & Permissions [Opens in a new window]

Abstract

Core share and HTML view are not available for this content. However, as you have access to this content, a full PDF is available via the ‘Save PDF’ action button.

In the post-closure period of a geological disposal facility for radioactive waste, leaching of cement components is likely to give rise to an alkaline plume which will be in chemical disequilibrium with the host rock (which is clay in some concepts) and other engineered barrier system materials used in the facility, such as bentonite. An industrial analogue for cement-clay interaction can be found at Tournemire, southern France, where boreholes filled with concrete and cement remained in contact with the natural mudstone for 15–20 years. The boreholes have been overcored, extracted and mineralogical characterization has been performed. In this study, a reactive-transport model of the Tournemire system has been set up using the general-purpose modelling tool QPAC. Previous modelling work has been built upon by using the most up-to-date data and modelling techniques, and by adding both ion exchange and surface complexation processes in the mudstone. The main features observed at Tournemire were replicated by the model, including porosity variations and precipitation of carbonates, K-feldspar, ettringite and calcite. It was found that ion exchange needed to be included in order for C-S-H minerals to precipitate in the mudstone, providing a better match with the mineralogical characterization. The additional inclusion of surface complexation, however, led to limited calcite growth at the concrete-mudstone interface unlike samples taken from the Tournemire site that have a visible line of crusty carbonates along the interface.

Type
Research Article
Creative Commons
Creative Common License - CCCreative Common License - BY
Copyright © The Mineralogical Society of Great Britain and Ireland 2013 This is an Open Access article, distributed under the terms of the Creative Commons Attribution license. (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted re-use, distribution, and reproduction in any medium, provided the original work is properly cited.
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2013

References

ANDRA (2005) Dossier 2005 Argile Synthesis: Evaluation of the Feasibility of a Geological Repository in an Argillaceous Formation. Available online. Agencie Nationale pour la Gestion des Déchets Radioactifs, Paris, France.Google Scholar
Appelo, C.A.J. & Postma, D. (2007) Geochemistry, Groundwater and Pollution, 2nd Edition. Balkema Publishers, Leiden, The Netherlands.Google Scholar
Baur, I., Keller, P., Mavrocordatos, D., Wehrli, B. & Johnson, C.A. (2004) Dissolution-precipitation behaviour of ettringite, monosulfate, and calcium silicate hydrate. Cement and Concrete Research, 34, 341–348.10.1016/j.cemconres.2003.08.016Google Scholar
Beaucaire, C., Michelot, J.-L., Savoye, S. & Cabrera, J. (2008) Groundwater characterisation and modelling of water-rock interaction in an argillaceous formation (Tournemire, France). Applied Geochemistry, 23, 2182–2197.10.1016/j.apgeochem.2008.03.003Google Scholar
Bethke, C. (2008) Geochemical and Biogeochemical Reaction Modeling. Cambridge University Press, Cambridge, UK.Google Scholar
Bradbury, M.H. & Baeyens, B. (1997) A mechanistic description of Ni and Zn sorption on Na-montmorillonite 2: Modeling. Journal of Contaminant Hydrology, 27, 223–248.10.1016/S0169-7722(97)00007-7Google Scholar
Bradbury, M.H. & Baeyens, B. (2003) Porewater chemistry in compacted re-saturated MX-80 bentonite. Journal of Contaminant Hydrology, 61, 329–338.10.1016/S0169-7722(02)00125-0Google Scholar
Busenberg, E. & Plummer, L.N. (1982) The kinetics of dissolution of dolomite in CO2-H2O systems at 1.5 to 65°C an d 0 to 1 atm PCO2 . American Journal of Science 282:4578.Google Scholar
Davies, C.W. (1962) Ion Association. Butterworths, London, UK.Google Scholar
Davis, J.A., Coston, J.A., Kent, D.B. & Fuller, C.C. (1998) Application of the surface complexation concept to complex mineral assemblages. Environmental Science & Technology, 32, 2820–2828.10.1021/es980312qGoogle Scholar
De Windt, L., Marsal, F., Tinseau, E. & Pellegrini, D. (2008) Reactive transport modeling of geochemical interactions at a concrete/argillite interface, Tournemire site (France). Physics and Chemistry of the Earth, 33, S295–S305.Google Scholar
Gaines, G.L. & Thomas, H.C. (1953) Adsorption studies on clay minerals. II. A formulation of the thermodynamics of exchange adsorption. Journal of Chemical Physics, 21, 714–718.10.1063/1.1698996Google Scholar
Gaucher, E. & Blanc, P. (2006) Cement/clay interactions – a review: Experiments, natural analogues, and modeling. Waste Management, 26, 776–788.10.1016/j.wasman.2006.01.027Google Scholar
Kline, W.E. & Fogler, H.S. (1981) Dissolution kinetics: the nature of the particle attack of layered silicates in HF. Chemical Engineering Science, 36, 871–884.10.1016/0009-2509(81)85041-5CrossRefGoogle Scholar
Kulik, D.A. & Kersten, M. (2001) Aqueous solubility diagrams for cementitious waste stabilization systems: II. End-member stoichiometries of ideal calcium silicate hydrate solid solutions. Journal of the American Ceramic Society, 84, 3017–3026.10.1111/j.1151-2916.2001.tb01130.xGoogle Scholar
Lasaga, A.C. (1998) Kinetic Theory in the Earth Sciences. Princeton University Press, Princeton, New Jersey, USA.10.1515/9781400864874Google Scholar
Lothenbach, B., Matschei, T., Moschner, G. & Glasser, F.P. (2008) Thermodynamic modelling of the effect of temperature on the hydration and porosity of Portland cement. Cement and Concrete Research, 38, 1–18.10.1016/j.cemconres.2007.08.017Google Scholar
Marty, N.C.M., Tournassat, C., Burnol, A., Giffaut, E. & Gaucher, E.C. (2009) Influence of reaction kinetics and mesh refinement on the numerical modelling of concrete/clay interactions. Journal of Hydrology, 364, 58–72.10.1016/j.jhydrol.2008.10.013Google Scholar
Matschei, T., Lothenbach, B. & Glasser, F.P. (2007) Thermodynamic properties of Portland cement hydrates in the system CaO-Al2O3-SiO2-CaSO4- CaCO3-H2O. Cement and Concrete Research, 37, 1379–1410.10.1016/j.cemconres.2007.06.002Google Scholar
Micheau, N. (2005) ECOCLAY II: Effects of cement on clay barrier performance. ANDRA Report C.RP.ASCM.04.0009. Agencie Nationale pour la Gestion des Déchets Radioactifs, Paris, France.Google Scholar
NDA (2010) Geological Disposal: Generic Post-Closure Safety Assessment. NDA Report NDA/ RWMD/030. Available online. Nuclear Decommissioning Authority, Harwell, UK.Google Scholar
NDA (2011) Geological Disposal: R&D Programme Overview. Research and Development Needs in the Preparatory Studies Phase. NDA Report NDA/ RWMD/073. Available online. Nuclear Decommissioning Authority, Harwell, UK.Google Scholar
Palandri, J.L. & Kharaka, Y.K. (2004) A Compilation of Rate Parameters of Water-Mineral Interaction Kinetics for Application to Geochemical Modelling. USGS Open File Report 2004-1068, United States Geological Survey, Menlo Park, California, USA.Google Scholar
Plettinck, S., Chou, L. & Wollast, R. (1994) Kinetics and mechanisms of dissolution of silica at room temperature and pressure. Mineralogical Magazine, 58, 728–729.Google Scholar
Quintessa, (2012) QPAC: Quintessa's General-Purpose Modelling Software. Quintessa Report QRS-QPAC- 11. Available online. Quintessa Ltd., Henley-on-Thames, UK.Google Scholar
Sato, T., Kuroda, M., Yokoyama, S., Tsutsui, M., Fukushi, K., Tanaka, T. & Nakayama, S. (2004) Dissolution mechanism and kinetics of smectite under alkaline conditions. In: International Workshop on Bentonite-Cement Interaction in Repository Environments, (R. Metcalfe & C. Walker, editors). NUMO/Posiva, Tokyo, Japan.Google Scholar
Savage, D. (2010) A Review of PA-Relevant Data from Analogues of Alkaline Alteration, Nagra Report NAB 10-10. Available online. Nagra, Wettingen, Switzerland.Google Scholar
Savage, D., Watson, C.E., Benbow, S.J., Wilson, J.C. (2010) Modelling iron-bentonite interactions. Applied Clay Science, 47, 91–98.10.1016/j.clay.2008.03.011Google Scholar
SKB (2011) Long-Term Safety for the Final Repository for Spent Nuclear Fuel at Forsmark: Main Report of the SR-Site Project. SKB Technical Report TR-11-01. Available online. Swedish Nuclear Fuel and Waste Management Co., Stockholm, Sweden.Google Scholar
Techer, I., Bartier, D., Boulvais, Ph., Tinseau, E., Suchorski, K., Cabrera, J. & Dauzères, A. (2012) Tracing interactions between natural argillites and hyper-alkaline fluids from engineered cement paste and concrete: Chemical and isotopic monitoring of a 15-years old deep disposal analogue. Applied Geochemistry, 27, 1384–1402.10.1016/j.apgeochem.2011.08.013Google Scholar
Tinseau, E., Bartier, D., Hassouta, L., Devol-Brown, I. & Stammose, D. (2006) Mineralogical characterization of the Tournemire argillite after in situ interaction with concretes. Waste Management, 26, 789–800.10.1016/j.wasman.2006.01.024Google Scholar
Watson, C., Savage, D., Wilson, J. & Walker, C. (2011) Reactive Transport Modelling of the Tournemire Analogue: LCS Phase II. Quintessa Report QRS-1523A-1 v2.0 for NDA RWMD. Available online. Nuclear Decommissioning Authority, Harwell, UK.Google Scholar
Watson, C., Savage, D., Wilson, J., Walker, C. & Benbow, S. (2012) The Long-Term Cement Studies Project: The UK contribution to model development and testing. Mineralogical Magazine, 76, 3445–3455.10.1180/minmag.2012.076.8.58Google Scholar
Wilson, J., Savage, D., Bond, A., Watson, S., Pusch, R. & Bennett, D. (2011) Bentonite: A Review of Key Properties, Processes and Issues for Consideration in the UK Context. Quintessa Report QRS-1378ZG v1.1 for NDA RWMD. Available online. Nuclear Decommissioning Authority, Harwell, UK.Google Scholar