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Durability of potential plutonium wasteforms under repository conditions

Published online by Cambridge University Press:  05 July 2018

G. Deissmann ,
S. Neumeier ,
G. Modolo  and
D. Bosbach
G. Deissmann*
Affiliation:
Brenk Systemplanung, Heider-Hof-Weg 23, 52080 Aachen, Germany
S. Neumeier
Affiliation:
Institute of Energy and Climate Research IEK-6, Forschungszentrum Jülich, 52425 Jülich, Germany
G. Modolo
Affiliation:
Institute of Energy and Climate Research IEK-6, Forschungszentrum Jülich, 52425 Jülich, Germany
D. Bosbach
Affiliation:
Institute of Energy and Climate Research IEK-6, Forschungszentrum Jülich, 52425 Jülich, Germany
*
*E-mail: [email protected]
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Abstract

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Separated stocks of UK civil plutonium are currently held as a zero value asset in storage, as there is no final decision about whether they should be treated as a resource for future use as nuclear fuel or as waste. Irrespective of future UK government strategies regarding plutonium, at least a portion of the UK civil plutonium inventory will be designated for geological disposal. In this context, we performed a high-level review of the performance of potential wasteforms for the disposal of separated civil plutonium. The key issues considered were the durability and chemical reactivity of the wasteforms in aqueous environments and the long-term radionuclide release under conditions relevant to geological disposal. The major findings of the review, relevant not only to the situation in the UK but to plutonium disposal in general, are summarized in this paper. The review showed that, in the event of a decision being taken to declare plutonium as a waste for disposal, more systematic studies would be required to constrain the wasteform performance under repository conditions in order to derive realistic source terms for a safety case.

Keywords

plutoniumwasteformsrepository
Type
Research Article
Information
Mineralogical Magazine , Volume 76 , Issue 8 , December 2012 , pp. 2911 - 2918
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

Baston, G.M.N., Berry, J.A., Brownsword, M., Heath, T.G., Tweed, C.J. and Williams, S.J. (1995) Sorption of plutonium and americium on repository, backfill and geological materials relevant to the JNFL lowlevel radioactive waste repository at Rokkasho- Mura. Materials Research Society Symposium Proceedings, 353, 957–964.CrossRefGoogle Scholar
Berner, U.R. (1988) Modelling the incongruent dissolution of hydrated cement minerals. Radiochimica Acta, 44/45, 387–393.Google Scholar
Berner, U. (2002) Project Opalinus Clay: Radionuclide Concentration Limits in the Cementitious Near-Field of an ILW Repository. NAGRA Technical Report 02–22. Nagra, Wettingen, Switzerland, 48 pp.Google Scholar
Bingham, P.A., Hand, R.J., Stennett, M.C., Hyatt, N.C. and Harrison, M.T. (2008) The use of surrogates in waste immobilization studies: a case study of plutonium. Materials Research Society Symposium Proceedings, 1107, 421–428.CrossRefGoogle Scholar
British Pugwash Group (2009) The management of separated plutonium in the UK. British Pugwash Group, London, 60 pp.Google Scholar
Burakov, B.E., Ojovan, M.I. and Lee, W.E. (2011) Crystalline Materials for Actinide Immobilisation. Imperial College Press, London, 197 pp.CrossRefGoogle Scholar
CoRWM (2005) Position Paper on Plutonium. Committee on Radioactive Waste Management, Document No. 1281, 62 pp.Google Scholar
Curti, E., Grolimund, D. and Borca, C.N. (2012) A micro-XAS/XRF and thermodynamic study of CeIII/IV speciation after long-term aqueous alteration of simulated nuclear waste glass: relevance for predicting Pu behavior? Applied Geochemistry, 27, 56–63.Google Scholar
DECC (2011) Management of the UK’s Plutonium Stocks - A consultation response on the long-term management of UK owned separated civil plutonium. Department of Energy & Climate Change, London.Google Scholar
Deissmann, G., Neumeier, S., Modolo, G. and Bosbach, D. (2011) Review of the durability of potential plutonium wasteforms under conditions relevant to geological disposal. FZ Julich / Brenk Systemplanung Report to NDA RWMD, 85 pp.Google Scholar
Deschanels, X., Peuget, S., Cachia, J.N. and Charpentier, T. (2007) Plutonium solubility and self-irradiation effects in borosilicate glass. Progress in Nuclear Energy, 49, 623–634.CrossRefGoogle Scholar
Donald, I.W. (2007) Immobilisation of radioactive and non-radioactive wastes in glass-based systems: an overview. Glass Technology: European Journal of Glass Science and Technology A, 48, 155–163.Google Scholar
Donald, I.W., Metcalfe, B.L. and Taylor, R.N.J. (1997) Review: the immobilization of high level radioactive wastes using glasses and ceramics. Journal of Materials Sciences, 32, 5851–5857.CrossRefGoogle Scholar
Ewing, R.C. (1999) Nuclear wasteforms for actinides. Proceedings of the National Academy of Sciences of the United States of America, 96, 3432–3439.CrossRefGoogle Scholar
Ewing, R.C. (2007) Ceramic matrices for plutonium disposition. Progress in Nuclear Energy, 49, 635–643.CrossRefGoogle Scholar
Ewing, R.C. (2011) Actinides and radiation effects: impact on the back-end of the nuclear fuel cycle. Mineralogical Magazine, 75, 2359–2377.CrossRefGoogle Scholar
Fortner, J.A., Mertz, C.J., Bakel, A.J., Finch, R.J. and Chamberlain, D.B. (2000) Plutonium silicate alteration phases produced by aqueous corrosion of borosilicate glass. Materials Research Society Symposium Proceedings, 608, 739–744.CrossRefGoogle Scholar
International Atomic Energy Agency (1998) Safe handling and storage of plutonium. Safety Reports Series No. 9. International Atomic Energy Agency (IAEA), Vienna, 136 pp.Google Scholar
Harris, A.W., Manning, M.C., Tearle, W.M. and Tweed, C.J. (2002) Testing of models of the dissolution of cements - leaching of synthetic CSH gels. Cement and Concrete Research, 32, 731–746.CrossRefGoogle Scholar
Harrison, M.T. and Scales, C.R. (2008a) Development of borosilicate glass compositions for the immobilisation of the UK’s separated plutonium stocks. Materials Research Society Symposium Proceedings, 1107, 405–412.CrossRefGoogle Scholar
Harrison, M.T. and Scales, C.R. (2008b) Durability of borosilicate glass compositions for the immobilisation of the UK’s separated plutonium stocks. Materials Research Society Symposium Proceedings, 1107, 429–436.CrossRefGoogle Scholar
Harrison, M.T., Scales, C.R., Bingham, P.A. and Hand, R.J. (2007) Survey of potential glass compositions for the immobilisation of the UK’s separated plutonium stocks. Materials Research Society Symposium Proceedings, 985, http://dx.doi.org/ 10.1557/PROC-985-0985.NN04-03.Google Scholar
Harrison, M.T., Scales, C.R. and Maddrell, E.R. (2008) Progress in the assessment of wasteforms for the immobilisation of UK civil plutonium. Proceedings Waste Management ’08 Conference, February 24–28. 2008, Phoenix, AZ, USA, 6 pp.Google Scholar
Health and Safety Executive (2011) Annual figures for holdings of civil unirradiated plutonium. Office of Nuclear Regulation, www.hse.gov.uk/nuclear/safeguards/ civilplut10.htm [as at 08/11/2011].Google Scholar
Kang, J., von Hippel, F.N., Macfarlane, A. and Nelson, R. (2002) Storage MOX: a third way for plutonium disposal? Science & Global Security, 10, 85–101.Google Scholar
Lumpkin, G.R. (2006) Ceramic waste forms for actinides. Elements, 2, 365–372.CrossRefGoogle Scholar
Macfarlane, A.M. (2007) Another option for separated plutonium management: storage MOX. Progress in Nuclear Energy, 49, 644–650.CrossRefGoogle Scholar
Nuclear Decommissioning Authority (2009) NDA Plutonium Topic Strategy: Credible Options Technical Analysis. Report No. SAF/081208/006.2. Nuclear Decommissioning Authority, UK, 142 pp.Google Scholar
Pierce, E.M., McGrail, B.P., Martin, P.F., Marra, J., Arey, B.W. and Geiszler, K.N. (2007) Accelerated weathering of high-level and plutonium-bearing lanthanide borosilicate waste glasses under hydraul i c ally unsaturated conditions. Applied Geochemistry, 22, 1841–1859.CrossRefGoogle Scholar
Ronchi, C. and Hiernaut, J.P. (2004) Helium diffusion in uranium and plutonium oxides. Journal of Nuclear Materials, 325, 1–12.CrossRefGoogle Scholar
Stefanovsky, S.V., Yudintsev, S.V., Gieré, R. and Lumpkin, G.R. (2004) Nuclear waste forms. Pp. 37–63.in: Energy, Waste, and the Environment: A Geochemical Perspective (R. Gieré and P. Stille, editors). Geological Society Special Publications, 236. Geological Society, London.Google Scholar
Strachan, D.M. (2001) Glass dissolution: testing and modeling for long-term behavior. Journal of Nuclear Materials, 298, 69–77.CrossRefGoogle Scholar
The Royal Society (1998) Management of Separated Plutonium. The Royal Society, London, 14 pp.Google Scholar
Weber, W.J., Ewing, R.C., Angell, C.A., Arnold, G.W., Cormack, A.N., Delaye, J.M., Griscom, D.L., Hobbs, L.W., Navrotsky, A., Price, D.L., Stoneham, A.M. and Weinberg, M.C. (1997) Radiation effects in glasses used for immobilization of high-level waste and plutonium disposition. Journal of Materials Research, 12, 1946–1978.CrossRefGoogle Scholar
Weber, W.J., Navrotsky, A., Stefanovsky, S., Vance, E.R. and Vernaz, E. (2009) Materials science of high-level nuclear waste immobilization. Materials Research Society Bulletin, 34, 46–53.CrossRefGoogle Scholar
Wellman, D.M., Icenhower, J.P. and Weber, W.J. (2005) Elemental dissolution study of Pu-bearing borosilicate glasses. Journal of Nuclear Materials, 340, 149–162.CrossRefGoogle Scholar