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Uranyl oxo activation and functionalization by metal cation coordination

Journal Article:

Abstract

The oxo groups in the uranyl ion [UO{sub 2}]{sup 2+} - one of many oxo cations formed by metals from across the periodic table - are particularly inert, which explains the dominance of this ion in the laboratory and its persistence as an environmental contaminant. In contrast, transition metal oxo (M=O) compounds can be highly reactive and carry out difficult reactions such as the oxygenation of hydrocarbons. Here we show how the sequential addition of a lithium metal base to the uranyl ion constrained in a 'Pacman' environment results in lithium coordination to the U=O bonds and single-electron reduction. This reaction depends on the nature and stoichiometry of the lithium reagent and suggests that competing reduction and C-H bond activation reactions are occurring. (authors)
Authors:
Arnold Polly, L; Pecharman, A F; Hollis, E; Parsons, S; Love, J B; [1]  Yahia, A; Maron, L; [2]  Yahia, A; Maron, L [3] 
  1. Univ Edinburgh, EaStCHEM Sch Chem, Edinburgh EH9 3JJ, Midlothian (United Kingdom)
  2. Univ Toulouse 3, LPCNO, UMR 5215, INSA, CNRS, F-31077 Toulouse 4 (France)
  3. Univ Montpellier 2, ENSCM, CNRS, ICSM, UMR 5257, CEA, Ctr Marcoule, F-30207 Bagnols Sur Ceze (France)
Publication Date:
Jul 01, 2010
Product Type:
Journal Article
Resource Relation:
Journal Name: Nature Chemistry; Journal Volume: 2; Journal Issue: no.12; Other Information: 25 refs.
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; DENSITY FUNCTIONAL METHOD; LITHIUM COMPOUNDS; LITHIUM IONS; REDUCTION; STOICHIOMETRY; URANYL COMPLEXES; ACTINIDE COMPLEXES; ALKALI METAL COMPOUNDS; CALCULATION METHODS; CHARGED PARTICLES; CHEMICAL REACTIONS; COMPLEXES; IONS; URANIUM COMPLEXES; VARIATIONAL METHODS
OSTI ID:
21517750
Country of Origin:
France
Language:
English
Other Identifying Numbers:
Journal ID: ISSN 1755-4330; TRN: FR1102278108371
Availability:
Available from doi: http://dx.doi.org/10.1038/NCHEM.904
Submitting Site:
FRN
Size:
page(s) 1056-1061
Announcement Date:
Dec 29, 2011

Journal Article:

Citation Formats

Arnold Polly, L, Pecharman, A F, Hollis, E, Parsons, S, Love, J B, Yahia, A, Maron, L, Yahia, A, and Maron, L. Uranyl oxo activation and functionalization by metal cation coordination. France: N. p., 2010. Web. doi:10.1038/NCHEM.904.
Arnold Polly, L, Pecharman, A F, Hollis, E, Parsons, S, Love, J B, Yahia, A, Maron, L, Yahia, A, & Maron, L. Uranyl oxo activation and functionalization by metal cation coordination. France. doi:10.1038/NCHEM.904.
Arnold Polly, L, Pecharman, A F, Hollis, E, Parsons, S, Love, J B, Yahia, A, Maron, L, Yahia, A, and Maron, L. 2010. "Uranyl oxo activation and functionalization by metal cation coordination." France. doi:10.1038/NCHEM.904. https://www.osti.gov/servlets/purl/10.1038/NCHEM.904.
@misc{etde_21517750,
title = {Uranyl oxo activation and functionalization by metal cation coordination}
author = {Arnold Polly, L, Pecharman, A F, Hollis, E, Parsons, S, Love, J B, Yahia, A, Maron, L, Yahia, A, and Maron, L}
abstractNote = {The oxo groups in the uranyl ion [UO{sub 2}]{sup 2+} - one of many oxo cations formed by metals from across the periodic table - are particularly inert, which explains the dominance of this ion in the laboratory and its persistence as an environmental contaminant. In contrast, transition metal oxo (M=O) compounds can be highly reactive and carry out difficult reactions such as the oxygenation of hydrocarbons. Here we show how the sequential addition of a lithium metal base to the uranyl ion constrained in a 'Pacman' environment results in lithium coordination to the U=O bonds and single-electron reduction. This reaction depends on the nature and stoichiometry of the lithium reagent and suggests that competing reduction and C-H bond activation reactions are occurring. (authors)}
doi = {10.1038/NCHEM.904}
journal = {Nature Chemistry}
issue = {no.12}
volume = {2}
place = {France}
year = {2010}
month = {Jul}
}