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A study of uranyl(VI) carbonato comp...

Conover, Edwin Wheeler,

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A study of uranyl(VI) carbonato complexes in aqueous solution /

Record Type:	Electronic resources : Monograph/item
Title/Author:	A study of uranyl(VI) carbonato complexes in aqueous solution // Edwin Wheeler Conover.
Author:	Conover, Edwin Wheeler,
Description:	1 electronic resource (102 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 58-04, Section: B.
Contained By:	Dissertations Abstracts International58-04B.
Subject:	Chemistry. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=9634245
ISBN:	9798641569260

A study of uranyl(VI) carbonato complexes in aqueous solution /
Conover, Edwin Wheeler,

A study of uranyl(VI) carbonato complexes in aqueous solution /Edwin Wheeler Conover. - 1 electronic resource (102 pages)

Source: Dissertations Abstracts International, Volume: 58-04, Section: B.

Several parameters involved in uranyl(VI) speciation, such as pH, concentration of carbonate anion, concentration of uranyl(VI) cation, and temperature were used to study the behavior of uranyl(VI) carbonato complexes in aqueous solution. In near-neutral solution (pH 7-8), the trinuclear (UO$\\sb2)\\sb3$(CO$\\sb3)\\sb6\\sp{6-}$ was found to be the predominant complex in solution, converting to the mononuclear $\\rm UO\\sb2(CO\\sb3)\\sb3\\sp{4-}$ slightly above pH 8. However, a new complex, proposed to have an empirical formula of $\\rm(UO\\sb2)\\sb{x}(CO\\sb3)\\sb{2x},$ also formed in this pH region. This proposal is based on the observation of two $\\sp{13}$C NMR peaks, one identified as a bridging carbonate peak and one as a terminal carbonate peak. The transition between the trinuclear and mononuclear complexes was also studied via Raman spectroscopy. The uranyl $\u\\sb1$ bands of both complexes coalesced as the pH increased; however, a small inflection appeared between the trinuclear and mononuclear uranyl $\u\\sb1$ bands. Therefore, it is proposed that the new near-neutral complex has the molecular formula $\\rm(UO\\sb2)\\sb2(CO\\sb3)\\sb4\\sp{4-}.$ Also, observations in the strongly-alkaline pH region (pH $>$ 11) suggest that a complex other than the mononuclear complex is the predominant complex in the region. Integrated ratios of free-to-bound carbonate taken from $\\sp{13}$C NMR spectroscopy suggest that a complex with a 2:1 carbonate-to-uranyl ratio is formed. EXAFS spectroscopy was used to investigate the existence of polynuclear uranium interactions in solution. Peaks were observed in all three pH regions near 4 A, consistent with U-U interactions in other polynuclear uranyl(VI)-containing systems.

English

ISBN: 9798641569260Subjects--Topical Terms:

516420
Chemistry.
Subjects--Index Terms:

carbonates

A study of uranyl(VI) carbonato complexes in aqueous solution /
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245 1 2 $a A study of uranyl(VI) carbonato complexes in aqueous solution / $c Edwin Wheeler Conover.
264 1 $a Ann Arbor : $b ProQuest Dissertations & Theses, $c 1996
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500 $a Source: Dissertations Abstracts International, Volume: 58-04, Section: B.
500 $a Publisher info.: Dissertation/Thesis.
500 $a Advisors: Stout, Barbara E.
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520 $a Several parameters involved in uranyl(VI) speciation, such as pH, concentration of carbonate anion, concentration of uranyl(VI) cation, and temperature were used to study the behavior of uranyl(VI) carbonato complexes in aqueous solution. In near-neutral solution (pH 7-8), the trinuclear (UO$\\sb2)\\sb3$(CO$\\sb3)\\sb6\\sp{6-}$ was found to be the predominant complex in solution, converting to the mononuclear $\\rm UO\\sb2(CO\\sb3)\\sb3\\sp{4-}$ slightly above pH 8. However, a new complex, proposed to have an empirical formula of $\\rm(UO\\sb2)\\sb{x}(CO\\sb3)\\sb{2x},$ also formed in this pH region. This proposal is based on the observation of two $\\sp{13}$C NMR peaks, one identified as a bridging carbonate peak and one as a terminal carbonate peak. The transition between the trinuclear and mononuclear complexes was also studied via Raman spectroscopy. The uranyl $\u\\sb1$ bands of both complexes coalesced as the pH increased; however, a small inflection appeared between the trinuclear and mononuclear uranyl $\u\\sb1$ bands. Therefore, it is proposed that the new near-neutral complex has the molecular formula $\\rm(UO\\sb2)\\sb2(CO\\sb3)\\sb4\\sp{4-}.$ Also, observations in the strongly-alkaline pH region (pH $>$ 11) suggest that a complex other than the mononuclear complex is the predominant complex in the region. Integrated ratios of free-to-bound carbonate taken from $\\sp{13}$C NMR spectroscopy suggest that a complex with a 2:1 carbonate-to-uranyl ratio is formed. EXAFS spectroscopy was used to investigate the existence of polynuclear uranium interactions in solution. Peaks were observed in all three pH regions near 4 A, consistent with U-U interactions in other polynuclear uranyl(VI)-containing systems.
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