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Herbert's Quarry, South Wales – an analogue for host-rock alteration at a cementitious radioactive waste repository?

Published online by Cambridge University Press:  02 January 2018

Elizabeth B. A. Moyce ,
Antoni E. Milodowski ,
Katherine Morris  and
Samuel Shaw
Elizabeth B. A. Moyce*
Affiliation:
Earth Surface Science Institute, School of Earth and Environment, University of Leeds, Leeds LS2 9JT, UK
Antoni E. Milodowski
Affiliation:
British Geological Survey, Nicker Hill, Keyworth, Nottingham NG12 5GG, UK
Katherine Morris
Affiliation:
Research Centre for Radwaste and Decommissioining, School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
Samuel Shaw
Affiliation:
Research Centre for Radwaste and Decommissioining, School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Manchester M13 9PL, UK
*
*E-mail: [email protected]
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Abstract

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Cement in radioactive waste repositories will produce leachates of pH > 10 which may alter the host rock, affecting its ability to act as a barrier to radionuclide migration. To complement the many laboratory and modelling studies of rock alteration in cement leachates, analogue sites have been investigated to understand reactions at time scales relevant to geodisposal. However, analogue site histories may be poorly constrained and these systems may be influenced by site specific factors. Therefore increasing the number of sites studied is important to minimize uncertainty in the applicability of results. Herbert's Quarry has been characterized and assessed as a potential anthropogenic analogue. Streamwater sampling at the site identified Ca-rich fluids, ≤ pH 12, analogous to cement leachates. However, rock and sediment samples exhibited extensive CaCO3 precipitation in these fluids and no reaction of silicate rock. The streamwaters were also found to be oxidizing, unlike the reducing conditions expected at a repository, and temperatures were 15–25°C below those predicted for repositories. Therefore, Herbert's Quarry is believed to have limited applicability as an analogue in this context.

Keywords

hyperalkalineanaloguegeodisposalC–S–Hcarbonatestreamwater
Type
Research Article
Information
Mineralogical Magazine , Volume 79 , Issue 6 , November 2015 , pp. 1407 - 1418
Creative Commons
Creative Common License - CCCreative Common License - BY
Copyright © The Mineralogical Society of Great Britain and Ireland 2015. This is an open access article, distributed under the terms of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2015

References

ANDRA (2012) Low and Intermediate Level Short-lived Waste [online]. Available at: <http://www.andra.fr/international/pages/en/menu21/waste-management/waste-classification/short-lived-low—and-intermediate-level-waste-1609.html= [accessed 19/01/2014].Google Scholar
Andrews, J.E., Gare, S.G. and Dennis, P.F. (1997) Unusual isotopic phenomena in Welsh quarry water and carbonate crusts. Terra Nova, 9, 67–70.CrossRefGoogle Scholar
Atkinson, A. (1985) The Time Dependence ofpHwithin a Repository for Radioactive Waste Disposal. UKAEA, AERE-R 11777.Google Scholar
Bassil, N.M., Bryan, N. and Lloyd, J.R. (2014). Microbial degradation of isosaccharinic acid at high pH. The ISME Journal. 1751-7362/14. 1-11.Google Scholar
Berner, U.R. (1992) Evolution of pore water chemistry during degradation of cement in a radioactive waste repository environment. Waste Management, 12, 201–219.CrossRefGoogle Scholar
Braney, M.C., Haworth, A., Jefferies, N.L. and Smith, A.C. (1993) A study of the effects of an alkaline plume from a cementitious repository on geological materials. Journal of Contaminant Hydrology, 13, 379–02.CrossRefGoogle Scholar
British Geological Survey (2014) BGS Lexicon — Named Rock Unit: Dowlais Limestone Formation [online]. Available at http://data.bgs.ac.uk/doc/Lexicon/NamedRockUnit/DWL.html [accessed 07/6/2014]Google Scholar
Calch (2014) Discover the Lime Industry of the Black Mountains [online]. Available at: http://www.calch.org.uk/ [accessed 20/04/2014]Google Scholar
Chermak, I A. (1992) Low temperature experimental investigation of the effect of high pH NaOH solutions on the Opalinus shale, Switzerland. Clays and Clay Minerals, 40, 650–658.CrossRefGoogle Scholar
Chermak, I A. (1993) Low temperature experimental investigation of the effect of high pH KOH solutions on the Opalinus shale, Switzerland. Clays and Clay Minerals, 41, 365–372.CrossRefGoogle Scholar
DEFRA (2008) Managing Radioactive Waste Safely: A Framework for Implementing Geological Disposal. Department of the Environment, Food and Rural Affairs, UK.Google Scholar
Fernandez, R., Rodríguez, M., Vigil de la Villa, R. and Cuevas, I (2010) Geochemical constraints on the stability of zeolites and C-S-H in the high pH reaction of bentonite. Geochimica et Cosmochimica Acta, 74, 890–906.CrossRefGoogle Scholar
Gaucher, E. and Blanc, P. (2006) Cement/clay interactions — A review: experiments, natural analogues, and modeling. Waste Management, 26, 776–788.CrossRefGoogle ScholarPubMed
Hodgkinson, E.S. and Hughes, C.R. (1999) The miner-alogy and geochemistry of cement/rock reactions: high-resolution studies of experimental and analogue materials. Geological Society of London, Special Publications, 157, 195–211.CrossRefGoogle Scholar
IAEA (1989) Natural Analogues in Performance Assessments for the Disposal of Long Lived Radioactive Wastes. Technical Report Series, 304.Google Scholar
Lagerblad, B. and Tragardh, I (1994) Conceptual Model for Concrete Long Time Degradation in a Deep Nuclear Waste Repository. SKB Technical Report 95-21.Google Scholar
Mäder, U., Fierz, T., Frieg, B., Eikenberg, J., Ruthi, M., Albinsson, Y., Mori, A., Ekberg, S. and Stille, P. (2006) Interaction of hyperalkaline fluid with fractured rock: Field and laboratory experiments of the HPF project (Grimsel Test Site, Switzerland). Journal of Geochemical Exploration, 90, 68–94.CrossRefGoogle Scholar
McKinley, I.G. and Alexander, W.R. (1992) A review of the use of natural analogues to test performance assessment models of a cementitious near field. Waste Management, 12, 253–259.CrossRefGoogle Scholar
May, H.M., Helmke, P.A. and Jackson, M.L. (1979) Gibbsite solubility and thermodynamic properties of hydroxy-aluminium ions in aqueous solution at 25°C. Geochimica et Cosmochimica Acta, 43, 861–868.CrossRefGoogle Scholar
Miller, W., Alexander, R., Chapman, N., McKinley, I. and Smellie, I (2000) Geological Disposal of Radioactive Wastes & Natural Analogues. Elsevier Science Ltd., Oxford, UK.Google Scholar
Milodowski, A.E., Hysslop, E.K., Pearce, J.M., Wetton, P. D, Kemp, S.J., Longworth, G., Hodgkinson, E.S. and Hughes, C.R. (1998) Mineralogy, petrology and geochemistry. In: Maqarin Natural Analogue Study: Phase III (J. A.T. Smellie, editor). TR 98-04. Swedish Nuclear Fuel and Waste Management Company, Stockholm.Google Scholar
Moyce, E.B.A., Rochelle, C., Morris, K., Milodowski, A.E., Chen, X., Thornton, S., Small, J.S. and Shaw, S. (2014) Rock alteration in alkaline cement waters over 15 years and its relevance to the geological disposal of nuclear waste. Applied Geochemistry, 50, 91–105.CrossRefGoogle Scholar
NAGRA (2014) Geological Repository for Low- and Intermediate-level Waste [online]. Available at: <http://www.nagra.ch/en/tlsmae.htm= [accessed 19/01/2014].Google Scholar
NDA (2010a) Geological Disposal: Generic Disposal System Technical Specification. NDA/RWMD/044.Google Scholar
NDA (2010b) Geological Disposal: Geosphere Status Report. NDA/RWMD/035.Google Scholar
Nuclear Waste Management Organisation (2010) DGR Key Features [online]. Available at: <http://www.nwmo.ca/dgr_keyfeatures= [accessed 19/01/2014].Google Scholar
OECD-NEA (2008) Moving Forward with Geological Disposal of Radioactive Waste: a Collective Statement by the NEA Radioactive Waste Management Committee (RWMC). NEA no. 6433.Google Scholar
Pokrovsky, O.S. and Schott, I (2004) Experimental study of brucite and precipitation in aqueous solutions: surface speciation and chemical affinity control. Geochimica et Cosmochimica Acta, 68, 31–45.CrossRefGoogle Scholar
Ramirez, S. (2005) Alteration of the Callovo-Oxfordian clay from Meuse-Haute Marne underground laboratory (France) by alkaline solution. I. A XRD and CEC study. Applied Geochemistry, 20, 89–99.CrossRefGoogle Scholar
Rizoulis, A., Steele, H., Morris, K. and Lloyd, I (2012) The potential impact of anaerobic microbial metabolism during the geological disposal of intermediate-level waste. MineralogicalMagazine. 76, 3261–3270.Google Scholar
Savage, D. (2010) A Review of PA-relevant Data from Analogues of Alkaline Alteration. Wettingen: NAGRA.Google Scholar
Savage, D. (2011). A review of analogues of alkaline alteration with regard to long-term barrier perform-ance. Mineralogical Magazine, 75, 2401–2418.Google Scholar
Savage, D. and Rochelle, C. (1993) Modelling reactions between cement pore fluids and rock: Implications for porosity change. Journal of Contaminant Hydrology, 13, 365–378.CrossRefGoogle Scholar
Savage, D., Bateman, K., Hill, P., Hughes, C., Milowdowski, A., Pearce, J., Rae, M. and Rochelle, C. (1992) Rate and mechanism of the reaction of silicates with cement pore fluids. Applied Clay Science, 7, 33–15.CrossRefGoogle Scholar
Surdam, R.C. (1977) Zeolites in closed hydrologic systems. Pp. 65-92 in: Mineralogy and Geology of Natural Zeolites (F.A. Mumpton, editor). Mineralogical Society of America, Short Course Notes, 5.CrossRefGoogle Scholar
Taylor, M.W. and Surdam, R.C. (1981) Zeolite reactions in the tuffaceous sediments at Teels Marsh, Nevada. Clays and Clay Minerals, 90, 341–352.CrossRefGoogle Scholar
Techer, I., Bartier, D., Boulvais, Ph., Tinseau, E., Suchorski, K., Cabrera, 1 and Dauzeres, A. (2012) Tracing interaction 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.CrossRefGoogle Scholar
Tinseau, E., Bartier, D., Hassouta, L., Devol-Brown, I. and Stammose, D. (2006) Mineralogical characterization of the Tournemire Argillite after in situ interaction with concretes. Waste Management, 26, 789–800.CrossRefGoogle ScholarPubMed
Williamson, A.J., Morris, K., Shaw, S., Byrne, J.M., Boothman, C. and Lloyd, J.R. (2013) Microbial reduction of Fe(III) under alkaline conditions relevant to geological disposal. Applied and Environmental Microbiology, 79, 3320–3326.CrossRefGoogle ScholarPubMed