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JOURNAL ARTICLE
RESEARCH SUPPORT, NON-U.S. GOV'T
RESEARCH SUPPORT, U.S. GOV'T, NON-P.H.S.
Chloride Oxidation by Ruthenium Excited-States in Solution.
Journal of the American Chemical Society 2017 September 21
Photodriven HCl splitting to produce solar fuels is an important goal that requires strong photo-oxidants capable of chloride oxidation. In a molecular approach toward this goal, three ruthenium compounds with 2,2'-bipyrazine backbones were found to oxidize chloride ions in acetone solution. Nanosecond transient absorption measurements provide compelling evidence for excited-state electron transfer from chloride to the Ru metal center with rate constants in excess of 1010 M-1 s-1 . The Cl atom product was trapped with an olefin. This reactivity was promoted through pre-organization of ground-state precursors in ion pairs. Chloride oxidation with a tetra-cationic ruthenium complex was most favorable, as the dicationic complexes were susceptible to photochemical ligand loss. Marcus analysis afforded an estimate of the chlorine formal reduction potential E°(Cl•/- ) = 1.87 V vs NHE that is at least 300 meV more favorable than the accepted values in water.
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