Hostname: page-component-cd9895bd7-mkpzs Total loading time: 0 Render date: 2024-12-23T12:20:40.762Z Has data issue: false hasContentIssue false
  • English
  • Français

Retention of chlorine-36 by a cementitious backfill

Published online by Cambridge University Press:  02 January 2018

E. van Es ,
J. Hinchliff ,
M. Felipe-Sotelo ,
A.E. Milodowski ,
L.P. Field ,
N.D.M. Evans  and
D. Read
E. van Es
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
J. Hinchliff
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
M. Felipe-Sotelo*
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
A.E. Milodowski
Affiliation:
British Geological Survey, Keyworth, Nottingham NG12 5GG, UK
L.P. Field
Affiliation:
British Geological Survey, Keyworth, Nottingham NG12 5GG, UK
N.D.M. Evans
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
D. Read
Affiliation:
Chemistry Department, Loughborough University, Loughborough, Leicestershire LE11 3TU, UK
*
*E-mail: [email protected]
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.

Radial diffusion experiments have been carried out to assess the migration of 36Cl, as chloride, through a cementitious backfill material. Further experiments in the presence of cellulose degradation products were performed to assess the effect of organic ligands on the extent and rate of chloride diffusion. Results show that breakthrough of 36Cl is dependent on chloride concentration: as the carrier concentration increases, both breakthrough time and the quantity retained by the cement matrix decreases. Experiments in the presence of cellulose degradation products also show a decrease in time to initial breakthrough. However, uptake at various carrier concentrations in the presence of organic ligands converges at 45% of the initial concentration as equilibrium is reached. The results are consistent with organic ligands blocking sites on the cement that would otherwise be available for chloride binding, though further work is required to confirm that this is the case. Post-experimental digital autoradiographs of the cement cylinders, and elemental mapping showed evidence of increased 36Cl activity associated with black ash-like particles in the matrix, believed to correspond to partially hydrated glassy calcium-silicate-sulfate-rich clinker.

Keywords

36Cldiffusionradioactive wastecellulose degradation productsNirex Reference Vault Backfill
Type
Research Article
Information
Mineralogical Magazine , Volume 79 , Issue 6 , November 2015 , pp. 1297 - 1305
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

Footnotes

†

Present address: National Physical Laboratory, Hampton Road, Teddington, Middlesex TW11 0LW, UK

References

Abdel Rahman, R., Zaki, A. and El-Kamash, A. (2007) Modelling the long-term leaching behaviour of (137)Cs, (60)Co, and (152,154)Eu radionuclides from cement-clay matrices. Journal of Hazardous Materials, 145, 372–380.Google Scholar
Beaudoin, J., Ramachandran, V and Feldman, R. (1990) Interaction of chloride and C-S-H. Cement and Concrete Research, 20, 875–883.CrossRefGoogle Scholar
Birnin-Yauri, U. and Glasser, F. (1998) Friedel's Salt, Ca2Al(OH)6(Cl,OH).2H2O: Its solid solutions and their role in chloride binding. Cement and Concrete Research, 28, 1713–1723.CrossRefGoogle 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
DECC (Department of Energy & Climate Change) and NDA (Nuclear Decommissioning Authority) (2011) The 2010 UK radioactive waste inventory: Main report. Pöyry Energy Limited. DECC (RRN 10D/985) and NDA (NDA/ST/STY(11)0004).Google Scholar
Defra (Department for Environment, Food and Rural Affairs) and NDA (Nuclear Decommissioning Authority) (2008) The 2007 UK Radioactive Waste Inventory: Main Report. Pöyry Energy Limited. Defra (Defra/RAS/08.002) and NDA (NDA/RWMN/004).Google Scholar
Felipe-Sotelo, M. Hinchliff, J. Drury, D. Evans, N. Williams, S. and Read, D. (2014) Radial diffusion of radiocaesium and radioiodide through cementitious backfill. Physics and Chemistry of the Earth, 70-71, 60-70.Google Scholar
Francis, A., Cather, R. and Crossland, I. (1997) Development of the Nirex Reference Vault Backfill; report on current status in 1994. Nirex Science Report S/97/014, UK Nirex Ltd., Harwell, UK.Google Scholar
Glaus, M., van Loon, L., Achatz, S., Chodura, A. and Fischer, K (1999) Degradation of cellulosic materials under the alkaline conditions of a cementitious repository for low and intermediate level radioactive waste. Analytica Chimica Acta, 398, 111–122.CrossRefGoogle Scholar
Hicks, T., Baldwin, T., Hooker, P., Richardson, P., Chapman, N., McKinley, I. and Neall, F. (2008) Concepts for the Geological Disposal of Intermediate-level Radioactive Waste, Contractor Report for the NDA April 2008. Galson Sciences, Oakham, UK.Google Scholar
IAEA (2013) Isotope Methods for Dating Old Groundwater. IAEA (International Atomic Energy Agency), STI/PUB/1587, Vienna, 357 pp.Google Scholar
Markovaara-Koivisto, M., Read, D., Lindberg, A., Siitari-Kauppi, M. and Marcos, N. (2008) Uranium mineralogy at the Askola ore deposit, Southern Finland. Materials Research Society Symposium Series. Scientific Basis for Nuclear Waste Management, 32, 1124.Google Scholar
Nielsen, E.P., Herfort, D. and Geiker, M.R. (2005) Binding of chloride and alkalis in Portland cement systems. Cement and Concrete Research, 35, 117–123.CrossRefGoogle Scholar
Nuclear Decommissioning Authority (2010) Geological disposal: Radionuclide behaviour status report. Pp. 1-151 in: NDA Report No. RWMD/034 2010.Google Scholar
Ogard, A., Thompson, J., Rundberg, R., Wolfsberg, K., Kubik, P., Elmore, D. and Bentley, H. (1988) Migration of chlorine-36 and tritium from an underground nuclear test. Radiochimica Acta, 44-45, 213–218.Google Scholar
Parrington, J., Knox, H., Breneman, S., Baum, E. and Feiner, F. (1996) Nuclides and Isotopes. 15th edition. General Electric Nuclear Energy Co.Google Scholar
Pointeau, I., Coreau, N. and Reiller, P.E. (2008) Uptake of anionic radionuclides onto degraded cement pastes and competing effect of organic ligands. Radiochimica Acta, 96, 367–374.CrossRefGoogle Scholar
Rizoulis, A., Steele, H.M., Morris, K. and Lloyd, J.R. (2012) The potental impact of anaerobic microbial metabolism during the geological disposal of inter-mediate-level waste. Mineralogical Magazine, 76, 3261–3270.CrossRefGoogle Scholar
Shand, P., Edmunds, W.M., Lawrence, A.R., Smedley, P. L and Burke, S. (2007) The Natural (Baseline) Quality of Groundwater in England and Wales. British Geological Survey and Environmental Agency, Research Report RR/07/06 and Technical Report NC/99/74/24.Google Scholar
Song, Z., Jiang, L., Chu, H., Xiong, C., Liu, R., and You, L. (2014) Modelling of chloride diffusion in concrete immersed in CaCl2 and NaCl solutions with account of multi-phase reactions and ionic interactions. Construction and Building Materials, 66, 1–9.CrossRefGoogle Scholar
Suryavanshi, A., Scantlebury, J. and Lyon, S. (1996) Mechanism of Friedel's Salt formation in cements rich in tri-calcium aluminate. Cement and Concrete Research, 26, 717–727.CrossRefGoogle Scholar
Tang, L. (1999a) Concentration dependence of diffusion and migration of chloride ions Part 1. Theoretical considerations. Cement and Concrete Research, 29, 1463–1468.CrossRefGoogle Scholar
Tang, L. (1999b). Concentration dependence of diffusion and migration of chloride ions Part 2. Experimental evaluations. Cement and Concrete Research, 29, 1469–1474.Google Scholar
Yu, P. and Kirkpatrick, R. (2001) 35Cl NMR relaxation study of cement hydrate suspensions. Cement and Concrete Research, 31, 1479–1485.CrossRefGoogle Scholar