Synthesis and Catalytic Water Oxidation Activities of Ruthenium Complexes Containing Neutral Ligands

被引：29

作者：

Xu, Yunhua ^{[1
]}

Duan, Lele ^{[1
]}

Akermark, Torbjorn ^{[2
]}

Tong, Lianpeng ^{[1
]}

Lee, Bao-Lin ^{[3
]}

Zhang, Rong ^{[4
]}

Akermark, Bjorn ^{[3
]}

Sun, Licheng ^{[1
,4
]}

机构：

[1] Royal Inst Technol KTH, Dept Chem, Sch Chem Sci & Engn, S-10044 Stockholm, Sweden

[2] Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden

[3] Stockholm Univ, Dept Organ Chem, Arrhenius Lab, S-10691 Stockholm, Sweden

[4] Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 11602, Peoples R China

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2011年 / 17卷 / 34期

基金：

瑞典研究理事会;

关键词：

homogeneous catalysis; isotopic labeling; neutral ligands; ruthenium; water oxidation; OXYGEN-EVOLVING CATALYST; MOLECULAR CATALYSTS; PHOTOSYSTEM-II; EFFICIENT; EVOLUTION; DIOXYGEN; FAMILY; STATE; DIMER;

D O I：

10.1002/chem.201100274

中图分类号：

O6 [化学];

学科分类号：

0703 ;

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.

引用

页码：9520 / 9528

页数：9

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