期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 131, 期 44, 页码 16051-+出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja905067u
关键词
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资金
- CNR, MIUR (FIRB) [CAMERE-RBNE03JCR5]
- PRIN [2006034372]
- University of Padova (Progetto Strategico 2008, HELIOS) [STPD08RCX]
- Generalitat de Catalunya [2009FIC00026]
- University and Research Commission of Innovation
- University and Enterprise Department of Catalan Government and European Social
- MICINN of the Spanish Government [CTQ2007-67918/BQU, CTQ2008-06549-C02-02/BQU]
- Consolider Ingenio 2010 [CSD2006-0003]
- Catalan Government [2009SGR69, 2009SGR259]
- ICIQ Foundation
Converging UV-vis, EPR, rRaman, and DFT calculations highlight the evolution of [Ru-4(H2O)(4)(mu-O)(4)(mu-OH)(2)(gamma-SiW10O36)(2)](10-), 1, to high-valent intermediates. In analogy with the natural enzyme, five different oxidation states, generated from 1, have been found to power the catalytic cycle for water oxidation. A high electrophilic tetra ruthenium (V)-hydroxo species is envisaged as the competent intermediate, undergoing nucleophilic attack by an external water molecule as a key step in the formation of a new O-O bond under catalytic conditions.
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