期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 16, 期 15, 页码 4659-4668出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.200902603
关键词
electrochemistry; homogeneous catalysis; oxidation; ruthenium; water splitting
资金
- Swedish Research Council
- K & A Wallenberg Foundation
- Swedish Energy Agency
- China Scholarship Council (CSC)
- National Natural Science Foundation of China [20633020]
- National Basic Research Program of China [200903220009]
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 turnovers(-1). Under acidic conditions, the equatorial 4-picoline in complex 1 dissociates first. In addition, ligand exchange in 1 occurs when the Rum 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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