Carbon-13 NMR characterization of actinyl(VI) carbonate complexes in aqueous solution

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The uranyl(VI) carbonate system has been re-examined using {sup 13}C NMR of 99.9% {sup 13}C-enriched U{sup VI}O{sub 2} ({sup 13}CO{sub 3}){sub 3}{sup 4{minus}} in millimolar concentrations. By careful control of carbonate ion concentration, we have confirmed the existence of the trimer, and observed dynamic equilibrium between the monomer and the timer. In addition, the ligand exchange reaction between free and coordinated carbonate on Pu{sup VI}O{sub 2}({sup 13}CO{sub 3}){sub 3}{sup 4{minus}} and Am{sup VI}O{sub 2}({sup 13}CO{sub 3}){sub 3}{sup 4{minus}} systems has been examined by variable temperature {sup 13}C NMR line-broadening techniques {sup 13}C NMR line-broadening techniques. A modified Carr-Purcell-Meiboom-Gill NMR pulse ... continued below

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Clark, D.L.; Hobart, D.E.; Palmer, P.D. (Los Alamos National Lab., NM (United States)); Sullivan, J.C. (Argonne National Lab., IL (United States)) & Stout, B.E. (Cincinnati Univ., OH (United States). Dept. of Chemistry) January 1, 1992.

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The uranyl(VI) carbonate system has been re-examined using {sup 13}C NMR of 99.9% {sup 13}C-enriched U{sup VI}O{sub 2} ({sup 13}CO{sub 3}){sub 3}{sup 4{minus}} in millimolar concentrations. By careful control of carbonate ion concentration, we have confirmed the existence of the trimer, and observed dynamic equilibrium between the monomer and the timer. In addition, the ligand exchange reaction between free and coordinated carbonate on Pu{sup VI}O{sub 2}({sup 13}CO{sub 3}){sub 3}{sup 4{minus}} and Am{sup VI}O{sub 2}({sup 13}CO{sub 3}){sub 3}{sup 4{minus}} systems has been examined by variable temperature {sup 13}C NMR line-broadening techniques {sup 13}C NMR line-broadening techniques. A modified Carr-Purcell-Meiboom-Gill NMR pulse sequence was written to allow for experimental determination of ligand exchange parameters for paramagnetic actinide complexes. Preliminary Eyring analysis has provided activation parameters of {Delta}G{sup {double dagger}}{sub 295} = 56 kJ/M, {Delta}H{sup {double dagger}} = 38 kJ/M, and {Delta}S{sup {double dagger}} = {minus}60 J/M-K for the plutonyl triscarbonate system, suggesting an associative transition state for the plutonyl (VI) carbonate complex self-exchange reaction. Experiments for determination of the activation parameters for the americium (VI) carbonate system are in progress.

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Pages: (15 p)

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OSTI; NTIS; INIS; GPO Dep.

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  • Conference on rare earths, Kyoto (Japan), 1-5 Jun 1992

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  • Other: DE92015150
  • Report No.: LA-UR-92-1648
  • Report No.: CONF-920625--5
  • Grant Number: W-7405-ENG-36
  • Office of Scientific & Technical Information Report Number: 5260638
  • Archival Resource Key: ark:/67531/metadc1072252

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  • January 1, 1992

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  • Feb. 4, 2018, 10:51 a.m.

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  • May 21, 2018, 3:46 p.m.

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Clark, D.L.; Hobart, D.E.; Palmer, P.D. (Los Alamos National Lab., NM (United States)); Sullivan, J.C. (Argonne National Lab., IL (United States)) & Stout, B.E. (Cincinnati Univ., OH (United States). Dept. of Chemistry). Carbon-13 NMR characterization of actinyl(VI) carbonate complexes in aqueous solution, article, January 1, 1992; New Mexico. (digital.library.unt.edu/ark:/67531/metadc1072252/: accessed June 23, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.