An EXAFS spectroscopy study of speciation of uranium and some fission product elements in chloride melts / May I., Volkovich V.A., Sharrad C.A., Bhatt A.I., Kinoshita H., Koster A., Charnock J.M., Griffiths T.R., Lewin B. // Proceedings - Electrochemical Society. - 2006. - V. PV 2004-24, l. . - P. 814-824.

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Conference Paper

Abstract:

The various chloro complexes of the transition metals U, Y, Zr, Ru, Tc and Re in high-temperature chloride melts (both liquid and quenched) have been investigated using EXAFS spectroscopy. All the oxidation states of uranium (III, IV, V and VI) are stable in molten LiCl. U(III) and U(IV) form UCl 6 x- ions and U(V) and U(VI) form UO2Cl 4 x- ions. U(III) and U(IV) are the most stable oxidation states in LiCl-BeCl2 eutectic melt; even under a Cl2 atmosphere (but in the absence of oxygen) U(VI) species are converted into U(IV){can't make sense of this sentence: do you really mean this, +6 reduced to +4 by chlorine?}. U(III) and U(IV) are present in the melt as hexachloro complexes. Yttrium(III) forms YCl6 3- ions and there is evidence that these units are joined together into chains by sharing two Cl ligands between every two Y atoms. Zr in LiCl melt forms Zr(II) and Zr(IV) ions, both six-coordinated. Ruthenium in LiCl-KCl and NaClKCl between 450 and 750 °C, and in quenched samples forms sixcoordinated complexes with Ru-Cl distances essentially independent of temperature and melt composition. Only quenched melt samples of technetium and rhenium have so far were investigated. Tc can form Tc(IV) and Tc(VIII) ions, TcCl6 2- and TcO 4 -, and rhenium under the same conditions always yielded the Re(IV) species, ReCl6 2-.

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Index keywords:

Eutectics; Extended X ray absorption fine structure spectroscopy; Fission products; Ligands; Oxidation; Quenching; Uranium; High-temperature chloride melts; Melt composition; Molten materials

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Link	https://www.scopus.com/inward/record.uri?eid=2-s2.0-40249096596&partnerID=40&md5=3de7e5c3a69c1d1741346c70c02c459f
Affiliations	Centre for Radiochemistry Research, Department of Chemistry, University of Manchester, Manchester, M13 9PL, United Kingdom; Department of Rare Metals, Ural State Technical University-UPI, Ekaterinburg, 620002, Russian Federation; CLRC Daresbury Laboratory, Warrington, WA4 4AD, United Kingdom; Redston Trevor Consulting Ltd.; School of Chemistry, University of Leeds, Leeds, LS2 9JT, United Kingdom; British Nuclear Fuels Pic, Sellafield R and D, Sellafield, CA20 IPG, United Kingdom
References	Okamoto, Y., Akabori, M., Motohashi, H., Shiwaku, H., Ogawa, T., (2001) J. Synchrotron Rad, 8, p. 1191; Okamoto, Y., Motohashi, H., (2002) Z. Naturforsch, 57 a, p. 277; Okamoto, Y., Akabori, M., Itoh, A., Ogawa, T., (2002) Z Nucl. Sci. Technol, (SUPPL. 3), p. 638; Volkovich, V.A., May, I., Bhatt, A.I., Griffiths, T.R., Charnock, J.M., Lewin, B., (2003) Proc. Int. Symp. Ionic Liquids, p. 253. , H. A. Øye and A. Jagteyen, Editors, p, The Norwegian University of Science and Technology, Trondheim; Volkovich, V.A., May, I., Charnock, J.M., Lewin, B., (2002) Phys. Chem. Chem. Phys, 4, p. 5753; Adams, M.D., Wenz, D.A., Steunenberg, R.K., (1963) Z Phys. Chem, 67, p. 1939; Wenz, D.A., Adams, M.D., Steunenberg, R.K., (1964) Inorg. Chem, 3, p. 989; Fung, K.W., Johnson, K.E., (1971) Inorg. Chem, 10, p. 1347; Dloume, J.P., Faure, R., Thomas-David, G., (1979) Acta Cryst. B, 35, p. 558; Darriet, J., (1981) Rev. Chim. Minerale, 18, p. 27; Day, M.C., Selbin, J., (1976) Theoretical Inorganic Chemistry, p. 444. , Khimiya, Moscow; ibid., 2nd ed., p. 446, Reinhold, New York, (1969)
Correspondence Address	May, I.; Centre for Radiochemistry Research, Department of Chemistry, University of Manchester, Manchester, M13 9PL, United Kingdom
Sponsors	Electrochemical Society Inc, Physical Electrochemistry Division;Electrochemical Society Inc, High Temperature Materials Division;Electrochemical Society Inc, Electrodeposition Division
Conference name	206th ECS Meeting
Conference date	3 October 2004 through 8 October 2004
Conference location	Honolulu, HI
Conference code	71459
ISBN	9781566775144
Language of Original Document	English
Abbreviated Source Title	Proc. Electrochem. Soc.
Source	Scopus