A New Dinuclear Ruthenium Complex as an Efficient Water Oxidation Catalyst

被引:123
作者
Xu, Yunhua [3 ]
Akermark, Torbjorn [3 ]
Gyollai, Viktor [3 ]
Zou, Dapeng [3 ]
Eriksson, Lars [2 ]
Duan, Lele [3 ]
Zhang, Rong [4 ]
Akermark, Bjorn [1 ]
Sun, Licheng [3 ]
机构
[1] Stockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
[2] Stockholm Univ, Dept Struct Chem, Arrhenius Lab, S-10691 Stockholm, Sweden
[3] Royal Inst Technol KTH, Sch Chem Sci & Engn, S-10044 Stockholm, Sweden
[4] Dalian Univ Technol, State Key Lab Fine Chem, KTH Joint Educ & Res Ctr Mol Devices, Dalian 116012, Peoples R China
基金
瑞典研究理事会;
关键词
OXYGEN-EVOLVING COMPLEX; PHOTOSYSTEM-II; DIMANGANESE COMPLEX; MOLECULAR DIOXYGEN; RU COMPLEXES; BLUE DIMER; LIGANDS; MECHANISMS; EVOLUTION; MODEL;
D O I
10.1021/ic802052u
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
A dinuclear ruthenium complex, which acts as a molecular catalyst for water oxidation, has been synthesized and characterized. The electronic and electrochemical properties were studied by UV-vis spectroscopy and cyclic voltammetry. The oxidation potentials of the complex are significantly lowered by introducing a negatively charged carboxylate ligand, in comparison with those of the reported complexes that have neutral ligands. The catalytic activity of the complex toward water oxidation using Ce(NH4)(2)(NO3)(6) as a chemical oxidant was investigated by means of an oxygen electrode and mass spectrometry. The turnover number of this catalyst with Ce-IV as the chemical oxidant was found to be ca. 1700. The mass spectroscopic analysis of the isotopomer distribution in oxygen evolved from O-18-labeled water indicates that O atoms in the evolved oxygen originate from water.
引用
收藏
页码:2717 / 2719
页数:3
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