Electrochemical oxidation of water by an adsorbed μ-oxo-bridged Ru complex

被引：69

作者：

Liu, Feng

Cardolaccia, Thomas

Hornstein, Brooks J.

Schoonover, Jon R.

Meyer, Thomas J.

机构：

[1] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA

[2] Los Alamos Natl Lab, Los Alamos, NM 87545 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2007年 / 129卷 / 09期

关键词：

D O I：

10.1021/ja068630+

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The (mu)-oxo-bridged complex, [((OH)(2)OP-tpy)(H2O)(2)RuORu(OH2)(2)(tpy-PO(OH)(2))](4+) (tpy-PO(OH)(2) is 4'-phosphonato-2,2':6',2 ''-terpyridine), was prepared and attached to ITO (Sn(IV)-doped In2O3) and nanocrystalline 10-20 nm diameter TiO2, ZrO2, and SnO2 thin film (similar to 10 m thickness) electrodes. The complex retains its proton-coupled electron transfer (PCET) and water oxidation properties on oxide surfaces. The electrochemically generated Ru-VI-O-Ru-V and Ru-V-O-Ru-V forms of the complex oxidize water with turnover numbers of 3.0 and 2.6 for Ru-VI-O-Ru-V and 1.8 and 1.0 for Ru-V-O-Ru-V at pH = 1 (triflic acid) and pH = 6 (terephthalic acid buffer), respectively. Cyclic voltammetric and spectroelectrochemical measurements have given significant insight into the water oxidation mechanism and origins of catalyst deactivation.

引用

页码：2446 / +

页数：3

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