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Spectroscopic Investigation of Actinide Speciation in Concentrated Chloride Solution

Published online by Cambridge University Press:  03 September 2012

W. Runde ,
M. P. Neu ,
S. D. Conradson ,
D. L. Clark ,
P. D. Palmer ,
S. D. Reilly ,
B. L. Scott  and
C. D. Tait
W. Runde
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
M. P. Neu
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
S. D. Conradson
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
D. L. Clark
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
P. D. Palmer
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
S. D. Reilly
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
B. L. Scott
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
C. D. Tait
Affiliation:
Environmental and Structural Actinide Chemistry, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
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Abstract

Actinide solubilities in highly concentrated chloride solutions are about one order of magnitude higher than in similar inert electrolyte (NaClO4) solutions. This increased solubility is due to interactions between actinide and chloride ions. Contradictory results exist regarding the interaction mechanism between actinide and chloride ions. Specifically, both inner-sphere complex formation and ion pair association have been implicated in the interpretation of spectrophotometric and extraction data. To address this controversy, we investigated the interaction between actinide ions in the (III), (IV), (V) and (VI) oxidation states and chloride ions using a multi-method approach. Spectroscopie techniques (TRLFS, Raman, UV-Vis absorption, EXAFS) were used to distinguish between changes in the inner coordination sphere of the actinide ion and effects of ion pairing. X-ray absorption spectroscopy and single crystal X-ray diffraction were used to determine structural details of the actinide chloro complexes formed in solution and solid states.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 465: Symposium II – Scienfific Basis for Nuclear Waste Management XX , 1996 , 693
Copyright
Copyright © Materials Research Society 1997

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References

LITERATURE

[1] Fuger, J., Khodakovsky, I.L., Sergeyeva, E.I., Medvedev, V.A., Navratil, J.D., The Chemical Thermodynamics of Actinide Elements and Compounds. Part 12. The Actinide Aqueous Inorganic Compexes. IAEA, Vienna, 1992.Google Scholar
[2] Grenthe, I., Fuger, J., Donigs, R.J.M., Lemire, R.J., Muller, A.B., Nguyen-Trung, C., Wanner, H., Chemical Thermodynamics of Uranium. Vol. 1. Elsevier Science Publishing Company Inc., North-Holland, 1992.Google Scholar
[3] Silva, R.J., Bidoglio, G., Rand, M.H., Robouch, P.B., Wanner, H., Puigdomenech, I., Chemical Thermodynamics of Americium. Vol. 2. Elsevier Science Publishing Company Inc., North-Holland, 1995.Google Scholar
[4] Marcus, Y., Shiloh, M., Israel J. Chem. 7, 31 (1969).Google Scholar
[5] Grenthe, I., Acat Chem. Scand. 16, 2300 (1962).Google Scholar
[6] Bansal, M., Sommer, L., Z. Phys. Chem. 226, 309 (1964).Google Scholar
[7] Runde, W., Neu, M.P., Cark, D.L., Geochim. Cosmochim. Acta 60 (12), 2065–2073, (1996).Google Scholar
[8] Clark, D.L., Conradson, S.D., Ekberg, S.A., Hess, N.J., Neu, M.P., Palmer, P.D., Runde, W., Tait, C.D., J. Am. Chem. Soc. 118, 2089–2090, (1996).Google Scholar
[9] Rogers, R.D., Bond, A.H., Hippie, W.G., Rollins, A.N., Henry, R.F., Inorg. Chem. 30, 2671, (1991).Google Scholar
[10] Clark, D.L., Conradson, S.D., Ekberg, S.A., Hess, N.J., Janecky, D.R., Neu, M.P., Palmer, P.D., Tait, C.D., New J. Chem. 20, 211–220, (1996).Google Scholar
[11] Maya, L., Begun, G.M., J. Inorg. Nucl. Chem. 43, 2827, (1981).Google Scholar
[12] Nakamoto, K., Infrared and Raman Spectra of Inorganic and Coordination Compounds. 4th edition, Wiley-Interscience, New York, 1986, pp. 141–145.Google Scholar