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Sorption of radionuclides to a cementitious backfill material under near-field conditions

Published online by Cambridge University Press:  05 July 2018

M. Felipe-Sotelo ,
J. Hinchliff ,
N. Evans ,
P. Warwick  and
D. Read
M. Felipe-Sotelo*
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
J. Hinchliff
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
N. Evans
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
P. Warwick
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK Enviras Ltd, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
D. Read
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
*
*E-mail: [email protected]
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Abstract

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The sorption behaviour of I−, Cs+, Ni2+, Eu3+, Th4+ and UO2+ 2on NRVB (Nirex reference vault backfill) a possible vault backfill, at pH 12.8 was studied. Sorption isotherms generated were compared to results obtained in the presence of cellulose degradation products (CDP). Whereas Cs was not affected by the presence of the organic compounds, a notable reduction in the sorption of Th and Eu to cement was observed. The results also indicated limited removal of Ni from solution (with or without an organic ligand) by sorption, the concentration in solution seemingly being determined solely by solubility processes. In the case of uranium, the presence of CDP increased the sorption to cement by almost one order of magnitude. Further studies into the uptake of CDP by cement are being undertaken to identify the mechanism(s) responsible.

Keywords

vault backfilleuropiumgeological disposalradioactive wastesorptionthoriumuraniumuranyl
Type
Research Article
Information
Mineralogical Magazine , Volume 76 , Issue 8 , December 2012 , pp. 3401 - 3410
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., Oliver, P. and McCrohon, R. (2002) Nearfield batch sorption studies - 1992 to 1998. Atomic Energy Authority Technology Report, AEA/ERRA- 0345.Google Scholar
Baston, G.M.N., Berry, J.A., Bond, K.A., Boult, K.A. Brownsword, M. and Linklater, C.M. (1994) Effect of cellulosic degradation products on uranium sorption in the geosphere. Journal of Alloys and Compounds, 213/214, 475–480.CrossRefGoogle Scholar
Baston, G.M.N., Cowper, M. and Marshall, T.A. (2010) Sorption of U(VI) onto leached and hydrothermallyaged NRVB. Serco Assurance Report SA/ENV-0959.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
Biddle, P., Greenfield, B.F., Pilkington, N.J. and Spindler, M.W. (2000) Further studies on the effects of the products from the anaerobic degradation. Atomic Energy Authority Technology Report AEAT/ERRA-0154.Google Scholar
Chambers, A.V., Cowper, M.M., Myatt, B.J. and Williams, S.J. (2004) Further studies of plutonium uptake by non-aqueous phase liquids. Serco Assurance Report SA/ENV-0656.Google Scholar
Cross, J. and Ewart, F. (1990) HATCHES - A Thermodynamic Database and Management System. Nirex Report NSS/R212.Google Scholar
Dario, M., Molera, M. and Allard, B. (2006) Sorption of europium on TiO2 and cement at high pH in presence of organic ligands. Journal of Radioanalytical and Nuclear Chemistry, 270, 495–505.CrossRefGoogle Scholar
Evans, N.D.M. (2008) Binding mechanisms of radionuclides to cements. Cement and Concrete Research, 28, 543–553.CrossRefGoogle Scholar
Greenfield, B.F., Hurdus, M.H., Spindler, M.W. and Thomason, H.P. (1997) The effects of the products of degradation of cellulose on the solubility and sorption of radionuclides in the near field. Nirex Report NSS/R376.Google Scholar
Heath, C.R. (2008) Interactions of radionuclides with cellulose degradation products. Unpublished PhD thesis, Loughborough University, Loughborough, UK.Google Scholar
Holgersson, S., Albinsson, Y., Allard, B., Borén, H., Pavasars, I. and Engkvist, I. (1998) Effects of glucoisosaccharinate on Cs, Ni, Pm and Th sorption onto, and diffusion into cement. Radiochimica Acta, 82, 393–398.CrossRefGoogle Scholar
Holland, T.R. and Tearle, W.M. (2003) A review of NRVB Mineralogy. A Serco report for UK Nirex Limited, SERCO/ERRA-0455.Google Scholar
Komarneni, S. and Roy, D.M. (1981) Mechanisms of immobilisation of nuclear waste elements by cement minerals, cement and mortar. Cement and Concrete Research, 11, 789–794.Google Scholar
Missana, T., Alonso, U., García-Gutiérrez, M. and López, T. (2010) Experimental study of sorption of Cs, I and Pu onto wasteform grouts and NRVB. CIEMAT report LBORO CMNDA4.Google Scholar
Nirex (1997) Development of the Nirex Reference Vault Backfill; Report on Current Status in 1994. Nirex Science Report S/97/014.Google Scholar
Nuclear Decommissioning Authority (2010) Geological Disposal: Steps Towards Implementation. Nuclear Decommissioning Authority Report NDA/RWMD/ 013.Google Scholar
Ochs, M., Pointeau, I. and Giffaut, E. (2006) Caesium sorption by hydrated cement as a function of degradation state: Experiments and modelling. Waste Management, 26, 725–732.Google ScholarPubMed
Pourchez, J., Govin, A., Grosseau, P., Guyonnet, R., Guilhot, B. and Ruot, B. (2006) Alkaline stability of cellulose ethers and impact of their degradation products on cement hydration. Cement and Concrete Research, 36, 1252–1257.CrossRefGoogle Scholar
Small, J. and Dutton, M. (2009) Review of the research on cellulose degradation and input data for the Simplified Model of Gas Generation (SMOGG). National Nuclear Laboratory Report NNL(09) 8870.Google Scholar
Sutton, M., Warwick, P. and Hall, A. (2003) Uranium(VI) interaction with OPC/PFA front. Journal of Environmental. Monitoring, 5, 922–928.CrossRefGoogle Scholar
Tits, J., Stumpf, T., Rabung, T., Wieland, E. and Fanghänel, T. (2003) Uptake of Cm(III) and Eu(III) by calcium silicate hydrates: a solution chemistry and time-resolved laser fluorescence spectroscopy study. Environmental Science and Technology, 37, 3568–3573.CrossRefGoogle ScholarPubMed
Van der Lee, J. (1998) Thermodynamic and Mathematical Concepts of CHESS. Technical Report LHM/RD/98/39, CIG, Ecole de Mines de Paris, Fontainebleu, France.Google Scholar
Van Loon, L.R. and Glaus, M.A. (1998) Experimental and theoretical studies on alkaline degradation of cellulose and its impact on the sorption of radionuclides. PSI Bericht Nr 98–07. Paul Scherrer Institute, Würenlingen, Switzerland.Google Scholar
Van Loon, L.R., Glaus, M.A., Stallone, S. and Laube, A. (1997) Sorption of isosaccharinic acid, a cellulose degradation product, on cement. Environmental Science and Technology, 31, 1243–1245.Google Scholar
Warwick, P. and Felipe-Sotelo, M. (2009) Effect of ‘as disposed’ complexants and polymer encapsulant leachates on the solubility of nickel, thorium and uranium(VI) and uranium(IV). Loughborough University Report for the NDA, LBORO CMNDA4.Google Scholar
Wieland, E., Tits, J., Dobler, J.P. and Spieler P. (2002) The effect of a-isosaccharinic acid on the stability of Th(IV) uptake by hardened cement paste. Radiochimica Acta, 90, 683–688.CrossRefGoogle Scholar
Wieland, E., Tits, J., Ulrich, A. and Bradbury, M.H. (2006) Experimental evidence for solubility limitation of the aqueous Ni(II) concentration and isotopic exchange in cementitious systems. Radiochimica Acta, 94, 29–36.CrossRefGoogle Scholar