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Uranium uptake onto Magnox sludge minerals studied using EXAFS

Published online by Cambridge University Press:  05 July 2018

A. van Veelen ,
R. Copping ,
G. T. W. Law ,
A. J. Smith ,
J. R. Bargar ,
J. Rogers ,
D. K. Shuh  and
R. A. Wogelius
A. van Veelen
Affiliation:
University of Manchester, School of Earth, Atmospheric and Environmental Sciences, Oxford Road, Manchester, M13 9PL, UK
R. Copping
Affiliation:
Chemical Sciences Division, Lawrence Berkeley National Laboratory, MS70A1150, One Cyclotron Road, Berkeley, California 94720, USA
G. T. W. Law
Affiliation:
University of Manchester, Centre for Radiochemistry Research, School of Chemistry, Oxford Road, Manchester, M13 9PL, UK
A. J. Smith
Affiliation:
University of Manchester, School of Earth, Atmospheric and Environmental Sciences, Oxford Road, Manchester, M13 9PL, UK
J. R. Bargar
Affiliation:
Stanford Synchrotron Radiation Lightsource, PO Box 4349, Stanford, California 94309, USA
J. Rogers
Affiliation:
Stanford Synchrotron Radiation Lightsource, PO Box 4349, Stanford, California 94309, USA
D. K. Shuh
Affiliation:
Chemical Sciences Division, Lawrence Berkeley National Laboratory, MS70A1150, One Cyclotron Road, Berkeley, California 94720, USA
R. A. Wogelius*
Affiliation:
University of Manchester, School of Earth, Atmospheric and Environmental Sciences, Oxford Road, Manchester, M13 9PL, UK
*
*E-mail: [email protected]
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Abstract

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Around the world large quantities of sludge wastes derived from nuclear energy production are currently kept in storage facilities. In the UK, the British government has marked sludge removal as a top priority as these facilities are nearing the end of their operational lifetimes. Therefore chemical understanding of uranium uptake in Mg-rich sludge is critical for successful remediation strategies. Previous studies have explored uranium uptake by the calcium carbonate minerals, calcite and aragonite, under conditions applicable to both natural and anthropogenically perturbed systems. However, studies of the uptake by Mg-rich minerals such as brucite [Mg(OH)2], nesquehonite [MgCO3·3H2O] and hydromagnesite [Mg5(CO3)4 (OH)2·4H2O], have not been previously conducted. Such experiments will improve our understanding of the mobility of uranium and other actinides in natural lithologies as well as provide key information applicable to nuclear waste repository strategies involving Mg-rich phases. Experiments with mineral powders were used to determine the partition coefficients (Kd) and coordination of UO22+ during adsorption and co-precipitation with brucite, nesquehonite and hydromagnesite. The Kd values for the selected Mg-rich minerals were comparable or greater than those published for calcium carbonates. Extended X-ray absorption fine structure analysis results showed that the structure of the uranyl-triscarbonato [UO2(CO3)3] species was maintained after surface attachment and that uptake of uranyl ions took place mainly via mineral surface reactions.

Keywords

hydromagnesitenesquehonitemagnesium carbonatesmagnox sludge waste remediation
Type
Research Article
Information
Mineralogical Magazine , Volume 76 , Issue 8 , December 2012 , pp. 3095 - 3104
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

Allen, P.G., Bucher, J.J., Clark, D.L., Edelstein, N.M., Ekberg, S.A., Gohdes, J.W., Hudson, E.A., Kaltsoyannis, N., Lukens, W.W., Neu, M.P., Palmer, P.D., Reich, T., Shuh, D.K., Tait, C.D. and Zwick, B.D. (1995) Multinuclear NMR, Raman, EXAFS, and X-ray diffraction studies of uranyl carbonate complexes in near-neutral aqueous solution. X-ray structure of [C(NH2)3]6[(UO2)3 (CO3)6]•6.5H2O. Inorganic Chemistry, 34, 4797–4807.CrossRefGoogle Scholar
Bargar, J.R., Reitmeyer, R. and Davis, J.A. (1999) Spectroscopic confirmation of uranium(VI)– carbonato adsorption complexes on hematite. Environmental Science & Technology, 33, 2481–2484.CrossRefGoogle Scholar
Christ, C.L., Clark, J.R. and Evans, H.T. (1955) Crystal structure of rutherfordine, UO2CO3. Science, 121, 472–473.CrossRefGoogle ScholarPubMed
Clark, D.L., Hobart, D.E. and Neu, M.P. (1995) Actinide carbonate complexes and their importance in actinide environmental chemistry. Chemical Reviews, 95, 25–48.CrossRefGoogle Scholar
Daniel, A.S. and Acton, R.A. (2006) Spent fuel management in the United Kingdom Pp. 57 in: Scientific and technical issues in the management of spent fuel of decommissioned nuclear submarines (A. Sarkisov, and A. Tournyol du Clos, editors). Springer, Dordrecht, The Netherlands.Google Scholar
Denecke, M.A. (2006) Actinide speciation using X-ray absorption fine structure spectroscopy. Coordination Chemistry Reviews, 250, 730–754.CrossRefGoogle Scholar
Denecke, M.A., Rothe, J., Dardenne, K. and Lindqvist- Reis, P. (2003) Grazing incidence (GI) XAFS measurements of Hf(IV) and U(VI) sorption onto mineral surfaces. Physical Chemistry Chemical Physics, 5, 939–946.CrossRefGoogle Scholar
Denecke, M.A., Bosbach, D., Dardenne, K., Lindqvist- Reis, P., Rothe, J. and Yin, R. (2005) Polarization dependent grazing incidence (GI) XAFS measurements of uranyl cation sorption onto mineral surfaces. Physica Scripta, T115, 877–881.CrossRefGoogle Scholar
Elzinga, E.J., Tait, C.D., Reeder, R.J., Rector, K.D., Donohoe, R. J . and Morris, D.E. (2004) Spectroscopic investigation of U(VI) sorption at the cal c i te-wat e r int erfa c e. Geochimica et Cosmochimica Acta, 68, 2437–2448.CrossRefGoogle Scholar
Finch, A.A. and Allison, N. (2007) Coordination of Sr and Mg in calcite and aragonite. Mineralogical Magazine, 71, 539–552.CrossRefGoogle Scholar
Geipel, G., Reich, T., Brendler, V., Bernhard, G. and Nitsche, H. (1997) Laser and X-ray spectroscopic studies of uranium-calcite interface phenomena. Journal of Nuclear Materials, 248, 408–411.CrossRefGoogle Scholar
Greathouse, J.A. and Cygan, R.T. (2005) Molecular dynamics simulation of uranyl(VI) adsorption equilibria onto an external montmorillonite surface. Physical Chemistry Chemical Physics, 7, 3580–3586.CrossRefGoogle ScholarPubMed
Greathouse, J.A., Stellalevinsohn, H.R., Denecke, M.A., Bauer, A. and Pabalan, R.T. (2005) Uranyl surface complexes in a mixed-charge montmorillonite: Monte Carlo computer simulation and polarized XAFS results. Clays and Clay Minerals, 53, 278–286.CrossRefGoogle Scholar
Hänchen, M., Prigiobbe, V., Baciocchi, R. and Mazzotti, M. (2008) Precipitation in the Mg-carbonate system - effects of temperature and CO2 pressure. Chemical Engineering Science, 63, 1012–1028.CrossRefGoogle Scholar
Hastings, J.J., Rhodes, D., Fellerman, A.S., McKendrick, D. and Dixon, C. (2007) New approaches for sludge management in the nuclear industry. Powder Technology, 174, 18–24.CrossRefGoogle Scholar
Horsley, D.M.C. and Hallington, P.J. (2005) Nuclear power and the management of the radioactive waste legacy. Chemical Engineering Research and Design, 83, 773–776.CrossRefGoogle Scholar
Hudson, E.A., Allen, P.G., Terminello, L.J., Denecke, M.A. and Reich, T. (1996) Polarized X-rayabsorption spectroscopy of the uranyl ion: comparison of experiment and theory. Physical Review B, 54, 156–165.CrossRefGoogle Scholar
Hudson, E.A., Terminello, L.J., Viani, B.E., Denecke, M., Reich, T., Allen, P.G., Bucher, J.J., Shuh, D.K. and Edelstein, N.M. (1999) The structure of U6+ sorption complexes on vermiculite and hydrobiotite. Clays and Clay Minerals, 47, 439–457.CrossRefGoogle Scholar
Kelly, S.D., Newville, M.G., Cheng, L., Kemner, K.M., Sutton, S.R., Fenter, P., Sturchio, N.C. and Spötl, C. (2003) Uranyl incorporation in natural calcite. Environmental Science & Technology, 37, 1284–1287.CrossRefGoogle Scholar
Kelly, S.D., Rasbury, E.T., Chattopadhyay, S., Kropf, A.J. and Kemner, K.M. (2006) Evidence of a stable uranyl site in ancient organic-rich calcite. Environmental Science & Technology, 40, 2262–2268.CrossRefGoogle ScholarPubMed
Reeder, R.J., Nugent, M., Lamble, G.M., Tait, C.D. and Morris, D.E. (2000) Uranyl incorporation into calcite and aragonite: XAFS and luminescence studies. Environmental Science & Technology, 34, 638–644.CrossRefGoogle Scholar
Reeder, R.J., Nugent, M., Tait, C.D., Morris, D.E., Heald, S.M., Beck, K.M., Hess, W.P. and Lanzirotti, A. (2001) Coprecipitation of uranium(VI) with calcite: XAFS, micro-XAS, and luminescence characterization. Geochimica et Cosmochimica Acta, 65, 3491–3503.CrossRefGoogle Scholar
Russell, A.D., Emerson, S., Nelson, B.K., Erez, J. and Lea, D.W. (1994) Uranium in foraminiferal calcite as a recorder of seawater uranium concentrations. Geochimica et Cosmochimica Acta, 58, 671–681.CrossRefGoogle Scholar
Schindler, M. and Putnis, A. (2004) Crystal growth of schoepite on the (104) surface of calcite. The Canadian Mineralogist, 42, 1667–1681.CrossRefGoogle Scholar
Sturchio, N., Antonio, M., Soderholm, L., Sutton, S. and Brannon, J. (1998) Tetravalent uranium in calcite. Science, 281, 971–973.CrossRefGoogle ScholarPubMed
Topping, S. and Bruce, S. (2006) A ponderous hazard. Nuclear Engineering International, 51, 28–32.Google Scholar
Vaughan, D.J. and Wogelius, R.A. (2000) Environmental Mineralogy. Eötvös University Press, Budapest.Google Scholar