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Spectroscopic Investigation of Actinide Speciation inConcentrated 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 aboutone order of magnitude higher than in similar inert electrolyte (NaClO4) solutions. This increased solubility is due tointeractions between actinide and chloride ions. Contradictory results existregarding the interaction mechanism between actinide and chloride ions.Specifically, both inner-sphere complex formation and ion pair associationhave been implicated in the interpretation of spectrophotometric andextraction data. To address this controversy, we investigated theinteraction between actinide ions in the (III), (IV), (V) and (VI) oxidationstates and chloride ions using a multi-method approach. Spectroscopietechniques (TRLFS, Raman, UV-Vis absorption, EXAFS) were used to distinguishbetween changes in the inner coordination sphere of the actinide ion andeffects of ion pairing. X-ray absorption spectroscopy and single crystalX-ray diffraction were used to determine structural details of the actinidechloro complexes formed in solution and solid states.

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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

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