Observation of Radiolytic Field Alteration of the Uranyl Cation in Bicarbonate Solution
- Pacific Northwest National Laboratory, Mail Stop, P.O. Box 999, Richland, WA 99352 (United States)
Auto radiolysis of uranium (VI) carbonate solutions between pH 5.9 and 7.2 is shown to alter the uranium speciation over relatively short periods of time and was followed by {sup 13}C NMR and visible spectrophotometry, using dissolved [({sup 233}UO{sub 2}){sub 3}(CO{sub 3}){sub 6}]{sup 6-} both as the radiolysis source (D 14.9 Gy/hr) and as a trap for the newly formed hydrogen peroxide. The speciation is different than the uranyl mixed peroxy carbonate species that have been reported for higher pH carbonate solutions. Direct addition of hydrogen peroxide to solutions of the uranyl-carbonate trimer is shown to reproduce the {sup 13}C, {sup 17}O NMR signatures of the complex(es) formed by radiolysis, but additionally a variety of new complexes are revealed. Ratios of H{sub 2}O{sub 2}/trimer <1.5 produced uranyl peroxo carbonate adducts that are shown to be common to the radiolytically produced species. Ratios of H{sub 2}O{sub 2}/trimer >1.5 resulted in formation of stable higher order peroxo carbonate complexes. The {sup 13}C, {sup 17}O NMR signatures and visible spectra of these complexes are described here. Rigorous characterization of the species is an ongoing effort. (authors)
- Research Organization:
- Materials Research Society, 506 Keystone Drive, Warrendale, PA, 15086-7573 (United States)
- OSTI ID:
- 21083712
- Resource Relation:
- Conference: Symposium Actinides 2006 - Basic Science, Applications and Technology, Boston, MA (United States), 26-30 Nov 2006; Other Information: Country of input: France; Related Information: In: Proceedings of the symposium Actinides 2006 - Basic Science, Applications and Technology, by Blobaum, Kerri J.M. [ed. CMS, Lawrence Livermore National Laboratory, Livermore, California (United States)]; Chandler, Elaine A. [ed. Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (United States)]; Havela, Ladislav [ed. Faculty of Mathematics and Physics, Charles University, Prague (Czech Republic)]; Maple, M. Brian [ed. University of California, San Diego, La Jolla, California (United States)]; Neu, Mary P. [ed. Los Alamos National Laboratory, Los Alamos NM (United States)], v. 986, 209 pages.
- Country of Publication:
- United States
- Language:
- English
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