Hostname: page-component-8448b6f56d-cfpbc Total loading time: 0 Render date: 2024-04-24T22:28:30.756Z Has data issue: false hasContentIssue false

Sorption properties of aged cements

Published online by Cambridge University Press:  05 July 2018

G. M. N. Baston*
Affiliation:
AMEC, B150 Building, Harwell, Didcot, Oxfordshire OX11 0QB, UK
M. M. Cowper
Affiliation:
AMEC, B150 Building, Harwell, Didcot, Oxfordshire OX11 0QB, UK
T. A. Marshall
Affiliation:
Research Centre for Radwaste Disposal, School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester M13 9PL, 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.

Samples of artificially aged Nirex reference vault backfill (NRVB) were prepared by progressive leaching with deionized water, after which some of the samples underwent hydrothermal treatment. Compared to unaltered NRVB, X-ray diffraction (XRD) and differential scanning calorimetry (DSC) provided evidence for the ageing resulting in alteration of the mineralogy, in particular the absence of portlandite was observed. The specific surface area of NRVB initially increased due to leaching, but then decreased after further leaching.

Sorption distribution ratios (RD values) of uranium(VI), neptunium(IV), tin and zirconium onto aged NRVB samples were measured using the batch sorption technique. For all four elements, there was little difference between RD values for aged NRVB and those for untreated material. The most probable explanation for these findings is that even though the ageing treatments altered the NRVB mineralogy, calcium silicate hydrate (C-S-H) phases are responsible for most of the radionuclide uptake and their transformation to more crystalline forms has little effect on the bulk sorption capacity of the aged material.

Type
Research Article
Creative Commons
Creative Common License - CCCreative Common License - BY
© [2012] The Mineralogical Society of Great Britain and Ireland. This is an open access article distributed under the terms of the Creative Commons Attribution (CC BY) licence (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 2012

References

Baker, S., McCrohon, R., Oliver, P. and Pilkington, N.J. (1994) Sorption of niobium, tin, iodine and chlorine onto Nirex reference vault backfill. Scientific Basis for Nuclear Waste Management XVII. Materials Research Society Symposia Proceedings, 333, 719724.CrossRefGoogle Scholar
Baker, S., Oliver, P. and McCrohon, R. (2002) Nearfield batch sorption studies - 1992 to 1998. AEA Technology Report AEAT/ERRA-0345.Google Scholar
Baston, G.M.N., Brownsword, M., Smith, A.J. and Smith-Briggs, J.L. (1996) Further Near-field Solubility Studies. Nirex Report NSS/R357.Google Scholar
Bayliss, S., McCrohon, R., Oliver, P., Pilkington, N.J. and Thomason, H.P. (1996) Near-field Sorption Studies: January 1989 to June 1991. Nirex Report NSS/R277.Google Scholar
Bayliss, S., Howse, R.M., McCrohon, R., Oliver, P., Smith Briggs, J.L. and Thomason, H.P. (2000) Nearfield Sorption Studies. AEA Technology Report AEAT/ERRA-0073.Google Scholar
Berner, U.R. (1992) Evolution of pore water chemistry during degradation of cement in a radioactive waste repository environment. Waste Management, 12, 201219.CrossRefGoogle Scholar
Bonhoure, I., Wieland, E., Scheidegger, A.M., Ochs, M. and Kunz, D. (2003) EXAFS study of Sn(IV) immobilization by hardened cement paste and calcium silicate hydrates. Environmental Science & Technology, 37, 21842191.CrossRefGoogle ScholarPubMed
Brownsword, M., Buchan, A.B., Ewart, F.T., McCrohon, R., Ormerod, G.J., Smith-Briggs, J.L. and Thomason, H.P. (1990) The solubility and sorption of uranium(VI) in a cementitious repository. Scientific Basis for Nuclear Waste Management XIII Materials Research Society Symposium Proceedings, 176, 577582.Google Scholar
Brownsword, M., Manning, M.C., Pilkington, N.J. and Williams, S.J. (2002) The Effects of Cellulose Degradation Products on the Solubility and Sorption of Zirconium and the Sorption of Lead under Cementitious Repository Conditions. AEA Technology Report AEAT/ENV/0549.Google Scholar
Chen, J.J., Thomas, J.J., Taylor, H.F.W. and Jennings, H.M. (2004) Solubility and structure of calcium silicate hydrate. Cement and Concrete Research, 34, 14991519.CrossRefGoogle Scholar
Francis, A.J., Cather, R. and Crossland, I.G. (1997) Nirex Safety Assessment Research Programme: Development of the Nirex Reference Vault Backfill: Report on Current Status in 1994. NDA/Nirex Report S/97/014.Google Scholar
Gaona, X., Kulik, D.A., Macé, N. and Wieland, E. (2012) Aqueous-solid solution thermodynamic model of U(VI) uptake in C-S-H phases. Applied Geochemistry, 27, 8195.CrossRefGoogle Scholar
Garbev, K., Bornefeld, M., Beuchle, G. and Stemmermann, P. (2008) Cell dimensions and composition of nanocrystalline calcium silicate hydrate solid solutions. Part 2: X-ray and thermogravimetry study. Journal of the American Ceramic Society, 91, 30153023.CrossRefGoogle Scholar
Glasser, F.P., Marchand, J. and Samson, E. (2008) Durability of concrete - degradation phenomena involving detrimental chemical reactions. Cement and Concrete Research, 38, 226246.CrossRefGoogle Scholar
Guillaumont, R., Fanghänel, J., Neck, V., Fuger, J., Palmer, D.A., Grenthe, I. and Rand, M. H (2003) Chemical Thermodynamics, Vol. 5, Update on the Chemical Thermodynamics of Uranium, Neptunium, Plutonium, Americium and Technetium. Elsevier, Amsterdam.Google Scholar
Heath, T.G., Hunter, F.M.I. and Smith, V. (2012) Update of Thermodynamic Data for Thorium in the HATCHES Database. Serco Report TCS/00473/005 Issue 2.Google Scholar
Hidalgo, A., Petit, S., Domingo, C., Alonso, C. and Andrade, C. (2007) Microstructural characterization of leaching effects in cement pastes due to neutralisation of their alkaline nature. Part I: Portland cement pastes. Cement and Concrete Research, 37, 6370.CrossRefGoogle Scholar
Nuclear Decommissioning Authority (2010) Geological disposal: Near-field Evolution Status Report. NDA ReportNDA/RWMD/033 . Nuclear Decommissioning Authority, Harwell, Didcot, Oxfordshire, UK.Google Scholar
Parkhurst, D.L. and Appelo, C.A.J. (1999) User’s guide to PHREEQC (version 2) - A Computer Program for Speciation, Reaction-path, 1D-transport, and Inverse Geochemical Calculations. US Geological Survey Water Resources Investigation Report 99- 4259.Google Scholar
Pointeau, I., Landesman, C., Giffaut, E. and Reiller, P. (2004) Reproducibility of the uptake of U(VI) onto degraded cement pastes and calcium silicate hydrate phases. Radiochimica Acta, 92, 645650.CrossRefGoogle Scholar
Sha, W., O’Neill, E.A. and Guo, Z (1999) Differential scanning calorimetry study of ordinary Portland cement. Cement and Concrete Research, 29, 14871489.CrossRefGoogle Scholar
Sylwester, E.R., Allen, P.G., Zhao, P. and Viani, B.E. (2000) Interactions of uranium and neptunium with cementitious materials studies by XAFS. Scientific Basis for Nuclear Waste Management XXIII. Materials Research Society Symposia Proceedings, 608, 307312.CrossRefGoogle Scholar
Thomas, J.J., Chen, J.J., Allen, A.J. and Jennings, H.M. (2004) Effects of decalcification on the microstructure and surface area of cement and tricalcium silicate pastes. Cement and Concrete Research, 34, 22972307.Google Scholar
Thomason, H.P. and Williams, S.J. (1992) Near-field Solubility Studies. Nirex Report NSS/R128.Google Scholar
Tits, J., Fujita, T., Tsukamoto, M. and Wieland, E. (2008) Uranium(VI) Uptake by Synthetic Calcium Silicate Hydrates. Scientific Basis for Nuclear Waste Management XXXI Materials Research Society Symposium Proceedings, 1107, 467474 Google Scholar
Tits, J., Gaona, X., Laube, A. and Wieland, E. (2012) Influence of the redox state on the neptunium sorption by cementitious materials. In: 3rd Annual Workshop Proceedings of the Collaborative Project ‘‘Redox Phenomena Controlling Systems’’ (7th EC FP CP RECOSY) (M. Altmaier L. Duro M. Grivé and V. Montoya, editors). KIT Scientific Publishing, Karlsruhe, Germany.Google Scholar
Wieland, E. and Van Loon, L.R. (2002) Cementitious Near-Field Sorption Data Base for Performance Assessment of an ILW Repository in Opalinus Clay. PSI technical report PSI Bericht Nr. 03–06. and Nagra Technical Report NTB 0220.Google Scholar
Zhao, P., Allen, P.G., Sylwester, E.R. and Viani, B.E.(2000) The partitioning of uranium and neptunium onto hydrothermally altered concrete. Radiochimica Acta, 88, 729736.Google Scholar