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American Chemical Society, Journal of the American Chemical Society, 44(131), p. 16051-16053, 2009

DOI: 10.1021/ja905067u

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Water Oxidation at a Tetraruthenate Core Stabilized by Polyoxometalate Ligands: Experimental and Computational Evidence To Trace the Competent Intermediates

Journal article published in 2009 by Andrea Sartorel, Pere Miró, Enrico Salvadori, Sophie Romain, Mauro Carraro ORCID, Gianfranco Scorrano, Marilena Di Valentin, M. Di Valentin ORCID, Antoni Llobet, Carles Bo ORCID, Marcella Bonchio
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Abstract

Converging UV-vis, EPR, rRaman, and DFT calculations highlight the evolution of [Ru(4)(H(2)O)(4)(mu-O)(4)(mu-OH)(2)(gamma-SiW(10)O(36))(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.