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Uranium fate during crystallization of magnetite from ferrihydrite in conditions relevant to the disposal of radioactive waste

Published online by Cambridge University Press:  02 January 2018

Timothy A. Marshall ,
Katherine Morris ,
Gareth T.W. Law ,
J. Frederick W. Mosselmans ,
Pieter Bots ,
Hannah Roberts  and
Samuel Shaw
Timothy A. Marshall
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre for Molecular Environmental Science, School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester M13 9PL, United Kingdom
Katherine Morris
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre for Molecular Environmental Science, School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester M13 9PL, United Kingdom
Gareth T.W. Law
Affiliation:
Centre for Radiochemistry Research, School of Chemistry and Research Centre for Radwaste Disposal, School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester M13 9PL, United Kingdom
J. Frederick W. Mosselmans
Affiliation:
Diamond Light Source Ltd, Diamond House, Harwell Science and Innovation Campus, Didcot, Oxfordshire OX11 0DE, United Kingdom
Pieter Bots
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre for Molecular Environmental Science, School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester M13 9PL, United Kingdom
Hannah Roberts
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre for Molecular Environmental Science, School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester M13 9PL, United Kingdom
Samuel Shaw*
Affiliation:
Research Centre for Radwaste Disposal and Williamson Research Centre for Molecular Environmental Science, School of Earth, Atmospheric and Environmental Science, The University of Manchester, Manchester M13 9PL, United Kingdom
*
*E-mail: sam.shaw@manchester.ac.uk
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Abstract

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Uranium incorporation into magnetite and its behaviour during subsequent oxidation has been investigated at high pH to determine the uranium retention mechanism(s) on formation and oxidative perturbation of magnetite in systems relevant to radioactive waste disposal. Ferrihydrite was exposed to U(VI)aq containing cement leachates (pH 10.5–13.1) and crystallization of magnetite was induced via addition of Fe(II)aq. A combination of XRD, chemical extraction and XAS techniques provided direct evidence that U(VI) was reduced and incorporated into the magnetite structure, possibly as U(V), with a significant fraction recalcitrant to oxidative remobilization. Immobilization of U(VI) by reduction and incorporation into magnetite at high pH, and with significant stability upon reoxidation, has clear and important implications for limiting uranium migration in geological disposal of radioactive wastes.

Keywords

uraniummagnetiteincorporationEXAFSradioactive wastegeodisposal
Type
Research Article
Information
Mineralogical Magazine , Volume 79 , Issue 6 , November 2015 , pp. 1265 - 1274
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

References

Berner, U.R. (1992) Evolution of pore water chemistry during degradation of cement in a radioactive waste repository environment. Waste Management, 12, 201–219.CrossRefGoogle Scholar
Boland, D.D., Collins, R.N., Payne, T.E. andWaite, T.D. (2011) Effect of amorphous Fe(III) oxide transformation on the Fe(II)-mediated reduction of U(VI). Environmental Science & Technology, 45, 1327–1333.CrossRefGoogle Scholar
Boland, D., Collins, R.N., Glover, C., Payne, T. and Waite, T.D. (2014) Reduction of U(VI) by Fe(II) during the Fe(II)-accelerated transformation of ferrihydrite. Environmental Science & Technology, 48, 9086–9093.CrossRefGoogle ScholarPubMed
Bots, P., Morris, K., Hibberd, R., Law, G.T.W., Mosselmans, LEW, Brown, A.P., Doutch, J., Smith, A.J. and Shaw, S. (2014) Formation of stable uranium(VI) colloidal nanoparticles in conditions relevant to radioactive waste disposal. Langmuir, 30, 14396–14405.CrossRefGoogle ScholarPubMed
Burns, P.C., Ewing, R.C. and Hawthorne, F.C. (1997) The crystal chemistry of hexavalent uranium: polyhedron geometries, bond-valence parameters, and polymerization of polyhedra. The Canadian Mineralogist, 35, 1551–1570.Google Scholar
Campbell, K.M., Veeramani, H., Urich, K.-U., Blue, L.Y., Giammar, D.E., Bernier-Latmani, R., Stubbs, J.E., Suvorova, E., Yabusaki, S., Lezama-Pacheco, J.S., Mehta, A., Long, P.E. and Bargar, J.R. (2011) Oxidative dissolution of biogenic uraninite in ground-water at Old Rifle, CO. Environmental Science & Technology, 45, 8748–8754.CrossRefGoogle ScholarPubMed
Catalano, J.G., Heald, S.M., Zachara, J.M. and Brown, G. E (2004) Spectroscopic and diffraction study of uranium speciation in contaminated vadose zone sediments from the Hanford site, Washington State. Environmental Science & Technology, 38, 2822–2828.CrossRefGoogle ScholarPubMed
Clark, D.L., Hobart, D.E. andNeu, M.P (1995) Actinide carbonate complexes and their importance in actinide environmental chemistry. Chemical Reviews, 95, 25–48.CrossRefGoogle Scholar
Cornell, R.M. and Schwertmann, U. (2003) The Iron Oxides: Structure, Properties, Reactions, Occurences and Uses, 2nd edition. Wiley-VCH: Weinham.Google Scholar
Dardenne, K., Schäfer, T., Lindqvist-Reis, P., Denecke, M. A, Plaschke, M., Rothe, J. and Kim, J.I. (2002) Low temperature XAFS investigation on the lutetium binding changes during the 2-line ferrihydrite alteration process. Environmental Science & Technology, 36, 5092–5099.CrossRefGoogle ScholarPubMed
Dent, A.J., Cibin, G., Ramos, S., Smith, A.D., Scott, S.M., Varandas, L., Pearson, M.R., Krumpa, N.A., Jones, C.P. andRobbins, P.E. (2009) B18: A coreXAS spectroscopy beamline for diamond. Journal of Physics: Conference Series, 190, 012039. Iop Publishing Ltd, Bristol.Google Scholar
Docrat, T.I., Mosselmans, J.F.W., Charnock, J.M., Whiteley, M.W., Collison, D., Livens, F.R., Jones, C. and Edmiston, M.J. (1999) X-ray absorption spectroscopy of tricarbonatodioxouranate(V), [UO2(CO3)3]5-, in aqueous solution. Inorganic Chemistry, 38, 1879–1882.CrossRefGoogle Scholar
Dodge, C.J., Francis, A.J., Gillow, J.B., Halada, G.P., Eng, C. and Clayton, C.R. (2002) Association of uranium with iron oxides typically formed on corroding steel surfaces. Environmental Science & Technology, 36, 3504–3511.CrossRefGoogle ScholarPubMed
Fleet, M.E. (1981) The structure of magnetite. Acta Crystallographica Section B —Structural Science, 2549, 917–920.CrossRefGoogle Scholar
Gorski, C.A., Nurmi, J.T., Tratnyek, P.G., Hofstetter, T.B. and Scherer, M.M. (2010) Redox behavior of magnetite: implications for contaminant reduction. Environmental Science & Technology, 44, 55–60.CrossRefGoogle ScholarPubMed
Hansel, C.M., Benner, S.G., Neiss, J., Dohnalkova, A., Kukkadapu, R.K. and Fendorf, S. (2003) Secondary mineralization pathways induced by dissimilatory iron reduction of ferrihydrite under advective flow. Geochimica et Cosmochimica Acta, 67, 2977–2992.CrossRefGoogle Scholar
Huber, F., Schild, D., Vitova, T., Rothe, J., Kirsch, R. and Schäfer, T (2012) U(VI) Removal kinetics in presence of synthetic magnetite nanoparticles. Geochimica et Cosmochimica Acta, 96, 154–173.CrossRefGoogle Scholar
Ilton, E.S., Boily, IF, Buck, E.C., Skomurski, F.N., Rosso, K.M., Cahill, C.L., Bargar, J.R. and Felmy, A. R (2010) Influence of dynamical conditions on the reduction of U(VI) at the magnetite-solution interface. Environmental Science & Technology, 44, 170–176.CrossRefGoogle ScholarPubMed
Ilton, E.S., Pacheco, J.S.L., Bargar, J.R., Shi, Z., Liu, J., Kovarik, L., Engelhard, M.H. and Felmy, A.R. (2012) Reduction of U(VI) incorporated in the structure of hematite. Environmental Science & Technology, 46, 9428–9436.CrossRefGoogle ScholarPubMed
Kahlweit, M. (1975) Ostwald ripening of precipitates. Advances in Colloid and Interface Science, 5, 1–35.CrossRefGoogle Scholar
Kerisit, S., Felmy, A.R. and Ilton, E.S. (2011) Atomistic simulations of uranium incorporation into iron (hydr) oxides. Environmental Science & Technology, 45, 2770–2776.CrossRefGoogle ScholarPubMed
Latta, D.E., Mishra, B., Cook, R.E., Kemner, K.M. and Boyanov, M.I. (2014) Stable U(IV) complexes form at high-affinity mineral surface sites. Environmental Science & Technology, 48, 1683–1691.CrossRefGoogle ScholarPubMed
Lloyd, J.R. and Renshaw, J.C. (2005) Bioremediation of radioactive waste: radionuclide-microbe interactions in laboratory and field-scale studies. Current Opinion in Biotechnology, 16, 254–260.CrossRefGoogle ScholarPubMed
Marshall, T.A., Morris, K.M., Law, G.T.W., Mosselmans, J.F.W., Bots, P., Parry, S.A. and Shaw, S. (2014a) Incorporation and retention of 99-Tc(IV) in magnetite under high pH conditions. Environmental Science & Technology, 48, 11853–11862.CrossRefGoogle ScholarPubMed
Marshall, T.A., Morris, K., Law, G.T.W., Livens, F.R., Mosselmans, J.F.W., Bots, P. and Shaw, S. (2014b) Incorporation of uranium into hematite during crystallization from ferrihydrite. Environmental Science & Technology, 48, 3724–3731.CrossRefGoogle ScholarPubMed
Missana, T., Maffiotte, U. and García-Gutiérrez, M. (2003) Surface reactions kinetics between nanocrystal-line magnetite and uranyl. Journal of Colloid and Interface Science, 261, 154–160.CrossRefGoogle ScholarPubMed
Moyce, E.B.A., Rochelle, C., Morris, K., Milodowski, A. E, Chen, X., Thornton, S., Small, J.S. and Shaw, S. (2014) Rock alteration in alkaline cement waters over 15 years and its relevance to the geological disposal of nuclear waste. Applied Geochemistry, 50, 91–105.CrossRefGoogle Scholar
Murphy, W.M. and Shock, E.L. (1999) Environmental aqueous geochemistry of actinides. Pp. 221–253. in: Uranium: Mineralogy, Geochemistry, and the Environment (P.C. Burns and R. Finch, editors). Reviews in Mineralogy, 38. Mineralogical Society of America, Washington DC.Google Scholar
Music, S., Gotic, M. and Popovic, S. (1993) X-ray diffraction and Fourier-transform infrared-analysis of the rust formed by corrosion of steel in aqueous-solutions. Journal of Materials Science, 28, 5744–5752.CrossRefGoogle Scholar
Nico, P.S., Stewart, B.D. and Fendorf, S. (2009) Incorporation of oxidized uranium into Fe (hydr) oxides during Fe(II) catalyzed remineralization. Environmental Science & Technology, 43, 7391–7396.CrossRefGoogle ScholarPubMed
Payne, T.E., Davis, J.A. and Waite, T.D. (1994) Uranium retention by weathered schists-the role of iron minerals. Radiochimica Acta, 66/67, 297-303.Google Scholar
Ravel, B. and Newville, M. (2005) Athena, Artemis, Hephaestus: data analysis for X-ray absorption spectroscopy using IFEFFIT. Journal of Synchrotron Radiation, 12, 537–541.CrossRefGoogle ScholarPubMed
Scott, T.., Allen, G.C., Heard, P.J. and Randell, M.G. (2005) Reduction of U(VI) to U(IV) on the surface of magnetite. Geochimica et Cosmochimica Acta, 69, 5639–5646.CrossRefGoogle Scholar
Senko, J.M., Istok, J.D., Suflita, J.M. and Krumholz, L.R. (2002) In situ evidence for uranium immobilization and remobilization. Environmental Science & Technology, 36, 1491–1496.CrossRefGoogle ScholarPubMed
Senko, J.M., Kelly, S.D., Dohnalkova, A.C., McDonough, IT, Kemner, K.M. and Burgos, W.D. (2007) The effect of U(VI) bioreduction kinetics on subsequent reoxida-tion of biogenic U(IV). Geochimica et Cosmochimica Acta, 71, 4644–4654.CrossRefGoogle Scholar
Shannon, R.D. (1976) Revised effective ionic-radii and systematic studies of interatomic distances in halides and chalcogenides. Acta Crystallographica Section A, 32, 751–767.CrossRefGoogle Scholar
Shuibo, X., Chun, Z., Xinghuo, Z., Jing, Y., Xiaojian, Z. and Jingsong, W. (2009) Removal of uranium(VI) from aqueous solution by adsorption of hematite. Journal of Environmental Radioactivity, 100, 162–166.CrossRefGoogle ScholarPubMed
Shuller-Nickles, L., Bender, W., Walker, S. and Becker, U. (2014) Quantum-mechanical methods for quantifying incorporation of contaminants in proximal minerals. Minerals, 4, 690–715.CrossRefGoogle Scholar
Sidhu, P.S., Gilkes, R.J. and Posner, A.M. (1977) Mechanism of the low temperature oxidation of synthetic magnetites. Journal of Inorganic and Nuclear Chemistry, 39, 1953–1958.CrossRefGoogle Scholar
Sidhu, P.S., Gilkes, R.J. and Posner, A.M. (1978) The synthesis and some properties of Co, Ni, Zn, Cu, Mn and Cd substituted magnetites. Journal of Inorganic and Nuclear Chemistry, 40, 429–435.CrossRefGoogle Scholar
Singer, D.M., Chatman, S.M., Ilton, E.S., Rosso, K.M., Banfield, J.F. and Waychunas, G.A. (2012a) Identification of simultaneous U(VI) sorption complexes and U(IV) nanoprecipitates on the magnetite (111) surface. Environmental Science & Technology, 46, 3811–3820.CrossRefGoogle ScholarPubMed
Singer, D.M., Chatman, S.M., Ilton, E.S., Rosso, K.M., Banfield, J.F. and Waychunas, G.A. (2012b) U(VI) sorption and reduction kinetics on the magnetite (111) surface. Environmental Science & Technology, 46, 3821–3830.CrossRefGoogle ScholarPubMed
Skomurski, F.N., Ilton, E.S., Engelhard, M.H., Arey, B.W. and Rosso, K.M. (2011) Heterogeneous reduction of U6+ by structural Fe2+ from theory and experiment. Geochimica et Cosmochimica Acta, 75, 7277–7290.CrossRefGoogle Scholar
Smith, K.F., Bryan, N.D., Swinburne, A.N., Bots, P., Shaw, S., Natrajan, L.S., Mosselmans, J.F.W., Livens, F.R. and Morris, K. (2014) U(VI) behaviour in hyperalkaline calcite systems. Geochimica et Cosmochimica Acta, 148, 343–359.CrossRefGoogle Scholar
Soldatov, A.V., Lamoen, D., Konstantinovic, M.J., Van den Berghe, S., Scheinost, A.C. and Verwerft, M. (2007) Local structure and oxidation state of uranium in some ternary oxides: X-ray absorption analysis. Journal of Solid State Chemistry, 180, 54–61.CrossRefGoogle Scholar
Stewart, B.D., Nico, P.S. and Fendorf, S. (2009) Stability of uranium incorporated into Fe (hydr)oxides under fluctuating redox conditions. Environmental Science & Technology, 43, 4922–4927.CrossRefGoogle ScholarPubMed
Tang, J., Myers, M., Bosnick, K.A. and Brus, L.E. (2003) Magnetite Fe3O4 nanocrystals: spectroscopic observation of aqueous oxidation kinetics. Journal of Physical Chemistry B, 107, 7501–7506.CrossRefGoogle Scholar
Van den Berghe, S., Verwerft, M., Laval, J.-P., Gaudreau, B., Allen, P.G. and Van Wyngarden, A. (2002) The local uranium environment in cesium uranates: a combined XPS, XAS, XRD, and neutron diffraction analysis. Journal of Solid State Chemistry, 166, 320–329.CrossRefGoogle Scholar
Viollier, E., Inglett, P.W., Hunter, K., Roychoudhury, A.N. and Van Cappellen, P. (2000) The ferrozine method revisited: Fe(II)/Fe(III) determination in natural waters. Applied Geochemistry, 15, 785–790.CrossRefGoogle Scholar
Waite, T.D., Davis, J.A., Payne, T.E., Waychunas, G.A. and Xu, N. (1994) Uranium(VI) adsorption to ferrihydrite—application of a surface complexation model. Geochimica et Cosmochimica Acta, 58, 5465–5478.CrossRefGoogle Scholar
Wallace, S.H., Shaw, S., Morris, K., Small, J.S., Fuller, A. J and Burke, I.T (2012) Effect of groundwater pH and ionic strength on strontium sorption in aquifer sediments: implications for 90Sr mobility at contaminated nuclear sites. Applied Geochemistry, 27, 1482–1491.CrossRefGoogle Scholar
Wallace, S.H., Shaw, S., Morris, K., Small, J.S. and Burke, I.T. (2013) Alteration of sediments by hyperalkaline K-rich cement leachate: implications for strontium adsorption and incorporation. Environmental Science & Technology, 47, 3694–3700.CrossRefGoogle ScholarPubMed
Walter, M., Somers, J., Bouëxiere, D., Gaczynski, P. and Brendebach, B. (2009) Oxidation behaviour of uranium and neptunium in stabilised zirconia. Journal of Solid State Chemistry, 182, 3305–3311.CrossRefGoogle Scholar
Wellman, D.M., Mattigod, S.V., Arey, B.W., Wood, M.I. and Forrester, S.W (2007) Experimental limitations regarding the formation and characterization of uranium-mineral phases in concrete waste forms. Cement and Concrete Research, 37, 151–160.CrossRefGoogle Scholar
Yanina, S.V and Rosso, K.M. (2008) Linked reactivity at mineral-water interfaces through bulk crystal conduction. Science (New York), 320, 218–222.CrossRefGoogle ScholarPubMed