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  • Title: Chemical and photochemical water oxidation catalyzed by mononuclear ruthenium complexes with a negatively charged tridentate ligand.
    Author: Duan L, Xu Y, Gorlov M, Tong L, Andersson S, Sun L.
    Journal: Chemistry; 2010 Apr 19; 16(15):4659-68. PubMed ID: 20229528.
    Abstract:
    Two mononuclear ruthenium complexes [RuL(pic)3] (1) and [RuL(bpy)(pic)] (2) (H2L = 2,6-pyridinedicarboxylic acid, pic = 4-picoline, bpy =2,2'-bipyridine) have been synthesized and fully characterized. Both complexes could promote water oxidation chemically and photochemically. Compared with other known ruthenium-based water oxidation catalysts using [Ce(NH4)2(NO3)6] (Ce(IV)) as the oxidant in solution at pH 1.0, complex 1 is one of the most active catalysts yet reported with an initial rate of 0.23 turnover s(-1). Under acidic conditions, the equatorial 4-picoline in complex 1 dissociates first. In addition, ligand exchange in 1 occurs when the Ru(III) state is reached. Based on the above observations and MS measurements of the intermediates during water oxidation by 1 using Ce(IV) as oxidant, [RuL(pic)2(H2O)](+) is proposed as the real water oxidation catalyst.
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