Chemical and Photochemical Water Oxidation Catalyzed by Mononuclear Ruthenium Complexes with a Negatively Charged Tridentate Ligand

被引：143

作者：

Duan, Lele ^{[1
]}

Xu, Yunhua ^{[1
]}

Gorlov, Mikhail ^{[1
]}

Tong, Lianpeng ^{[1
]}

Andersson, Samir ^{[1
]}

Sun, Licheng ^{[1
,2
]}

机构：

[1] Royal Inst Technol KTH, Dept Chem, S-10044 Stockholm, Sweden

[2] Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116012, Peoples R China

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2010年 / 16卷 / 15期

基金：

中国国家自然科学基金; 瑞典研究理事会;

关键词：

electrochemistry; homogeneous catalysis; oxidation; ruthenium; water splitting; O-O BOND; VISIBLE-LIGHT; FUNCTIONAL-MODEL; ARTIFICIAL PHOTOSYNTHESIS; CRYSTAL-STRUCTURE; RU(II) COMPLEXES; PHOTOSYSTEM-II; O-2; EVOLUTION; OXYGEN; EFFICIENT;

D O I：

10.1002/chem.200902603

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：4659 / 4668

页数：10

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