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论文类型：期刊论文

发表时间：2011-08-16

发表刊物：CHEMISTRY-A EUROPEAN JOURNAL

收录刊物：SCIE、EI

卷号：17

期号：34

页面范围：9520-9528

ISSN号：0947-6539

关键字：homogeneous catalysis; isotopic labeling; neutral ligands; ruthenium; water oxidation

摘要：Two dinuclear and one mononuclear ruthenium complexes containing neutral polypyridyl ligands have been synthesised as pre-water oxidation catalysts and characterised by (1)H and (13)C NMR spectroscopy and ESI-MS. Their catalytic water oxidation properties in the presence of [Ce(NH(4))(2)(NO(3))(6)] (Ce(IV)) as oxidant at pH 1.0 have been investigated. At low concentrations of Ce(IV) (5 mm), high turnover numbers of up to 4500 have been achieved. An (18)O-labelling experiment established that both O atoms in the evolved O(2) originate from water. Combined electrochemical study and electrospray ionisation mass spectrometric analysis suggest that ligand exchange between coordinated 4-picoline and free water produces Ru aquo species as the real water oxidation catalysts.