Hostname: page-component-cd9895bd7-fscjk Total loading time: 0 Render date: 2024-12-27T14:25:52.819Z Has data issue: false hasContentIssue false

Evaluation of the long-term behavior of potential plutonium waste forms in a geological repository

Published online by Cambridge University Press:  30 June 2014

Guido Deissmann
Affiliation:
Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research IEK-6: Nuclear Waste Management and Reactor Safety, 52425 Jülich, Germany Brenk Systemplanung GmbH, Heider-Hof-Weg 23, 52080 Aachen, Germany
Stefan Neumeier
Affiliation:
Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research IEK-6: Nuclear Waste Management and Reactor Safety, 52425 Jülich, Germany
Felix Brandt
Affiliation:
Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research IEK-6: Nuclear Waste Management and Reactor Safety, 52425 Jülich, Germany
Giuseppe Modolo
Affiliation:
Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research IEK-6: Nuclear Waste Management and Reactor Safety, 52425 Jülich, Germany
Dirk Bosbach
Affiliation:
Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research IEK-6: Nuclear Waste Management and Reactor Safety, 52425 Jülich, Germany
Get access

Abstract

Various candidate waste matrices such as nuclear waste glasses, ceramic waste forms and low-specification “storage” MOX have been considered within the current UK geological disposal program for the immobilization of separated civilian plutonium, in the case this material is declared as waste. A review and evaluation of the long-term performance of potential plutonium waste forms in a deep geological repository showed that (i) the current knowledge base on the behavior and durability of plutonium waste forms under post-closure conditions is relatively limited compared to HLW-glasses from reprocessing and spent nuclear fuels, and (ii) the relevant processes and factors that govern plutonium waste form corrosion, radionuclide release and total systems behavior in the repository environment are not yet fully understood in detail on a molecular level. Bounding values for the corrosion rates of potential plutonium waste forms under repository conditions were derived from available experimental data and analogue evidence, taking into account that the current UK disposal program is in a generic stage, i.e. no preferred host rock type or disposal concept has yet been selected. The derived expected corrosion rates for potential plutonium waste forms under conditions relevant for a UK geological disposal facility are in the range of 10-4 to 10-2 g m-2 d-1 and 10-5 to 10-4 g m-2 d-1 for borosilicate glasses, and generic ceramic waste forms, respectively, and ∼5·10-6 g m-2 d-1 for storage MOX. More realistic assessments of the long-term behavior of the waste forms under post-closure conditions would require additional systematic studies regarding the corrosion and leaching behavior under more realistic post-closure conditions, to explore the safety margins of the various potential waste forms and to build confidence in long-term safety assessments for geological disposal.

Type
Articles
Copyright
Copyright © Materials Research Society 2014 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

International Panel on Fissile Materials, Global fissile material report 2011, (Princeton, NJ, 2012) 42 p.Google Scholar
Health & Safety Executive, Annual figures for holdings of civil unirradiated plutonium, www.hse.gov.uk/nuclear/safeguards/civilplut12.htm (2013).Google Scholar
Department of Energy & Climate Change, Management of the UK’s Plutonium Stocks, (London, 2011) 33p.Google Scholar
Clements, T., Lyman, E. and von Hippel, F., Arms Control Today 43, July/August (2013).Google Scholar
Lutze, W. and Ewing, R.C., in Radioactive waste forms for the future, edited by Lutze, W. and Ewing, R.C. (Elsevier, Berlin, 1988) p. 699.Google Scholar
Donald, I.W., Metcalfe, B.L. and Taylor, R.N.J., J. Mater. Sci. 32, 5851 (1997).CrossRefGoogle Scholar
Macfarlane, A., Science & Global Security 7, 271 (1998).CrossRefGoogle Scholar
Ewing, R.C., Proc. Nat. Acad. Sci. 96, 3432, (1999).10.1073/pnas.96.7.3432CrossRefGoogle Scholar
Stefanovsky, S., Yudintsev, S.V., Gieré, R. and Lumpkin, G.R., Geological Society of London Special Publications 236, 37 (2004).10.1144/GSL.SP.2004.236.01.04CrossRefGoogle Scholar
Donald, I.W., Waste immobilization in glass and ceramic based hosts: Radioactive, toxic and hazardous wastes (Wiley, Chichester, 2010), 507 p.CrossRefGoogle Scholar
Deissmann, G., Neumeier, S., Modolo, G. and Bosbach, D., Review of the durability of potential plutonium wasteforms under conditions relevant to geological disposal, (Aachen, 2011) 85 p.Google Scholar
Deissmann, G., Neumeier, S., Brandt, F., Modolo, G. and Bosbach, D., Elicitation of dissolution rate data for potential wasteform types for plutonium (Aachen, 2011) 98 p.Google Scholar
Wellman, D.M., Icenhower, J.P. and Weber, W.J., J. Nucl. Mater. 340, 149 (2005).10.1016/j.jnucmat.2004.10.166CrossRefGoogle Scholar
Harrison, M.T. and Scales, C.R., Mater. Res. Soc. Symp. Proc. 1107, 405 (2008).10.1557/PROC-1107-405CrossRefGoogle Scholar
Harrison, M.T., Scales, C.R., Bingham, P.A. and Hand, R.J., Mater. Res. Soc. Symp. Proc. 985, 0985-NN04-03 (2007).Google Scholar
Ewing, R.C., Prog. Nucl. Energy 49, 635 (2007).10.1016/j.pnucene.2007.02.003CrossRefGoogle Scholar
Ewing, R.C., Min. Mag. 75, 2359 (2011).10.1180/minmag.2011.075.4.2359CrossRefGoogle Scholar
Lumpkin, G.R., Elements 2, 365 (2006).CrossRefGoogle Scholar
Weber, W.J., Navrotsky, A., Stefanovsky, S., Vance, E.R. and Vernaz, E., Mater. Res. Soc. Bull. 34, 46 (2009).10.1557/mrs2009.12CrossRefGoogle Scholar
Burakov, B.E., Ojovan, M.I. and Lee, W.E., Crystalline materials for actinide immobilisation (Imperial College Press, London, 2011) 197 p.10.1142/p652CrossRefGoogle Scholar
Kang, J., von Hippel, F.N., Macfarlane, A. and Nelson, R., Science & Global Security 10, 85 (2002).10.1080/08929880213803CrossRefGoogle Scholar
Macfarlane, A.M., Prog. Nucl. Energy 49, 644 (2007).CrossRefGoogle Scholar
Nuclear Decommissioning Authority, NDA Plutonium topic strategy: Credible options technical analysis (Doc No: SAF/081208/006.2, 2009) 142 p.Google Scholar
Pierce, E.M., McGrail, B.P., Martin, P.F., Marra, J., Arey, B.W. and Geiszler, K.N., Appl. Geochem. 22, 1841 (2007).CrossRefGoogle Scholar
Deissmann, G., Neumeier, S., Modolo, G. and Bosbach, D., Min. Mag. 76, 2911 (2012).10.1180/minmag.2012.076.8.06CrossRefGoogle 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., J. Mat. Res. 12, p. 1946 (1997).CrossRefGoogle Scholar
Weber, W.J. and Ewing, R.C., in Uranium – Cradle to grave, edited by Burns, P.C. and Sigmon, G.E. (Mineralogical Association of Canada, Short Course Series 43, 2013), p. 317.Google Scholar
Nuclear Decommissioning Authority, Geological disposal: Generic disposal facility designs (Report NDA/RWMD/048, 2010) 129 p.Google Scholar