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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

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