A Biomimetic Copper Water Oxidation Catalyst with Low Overpotential

被引：317

作者：

Zhang, Teng ^{[1
]}

Wang, Cheng ^{[1
,2
]}

Liu, Shubin ^{[3
]}

Wang, Jin-Liang ^{[2
]}

Lin, Wenbin ^{[1
]}

机构：

[1] Univ Chicago, Dept Chem, Chicago, IL 60637 USA

[2] Univ N Carolina, Dept Chem, Caudill & Kenan Labs, Chapel Hill, NC 27599 USA

[3] Univ N Carolina, Ctr Res Comp, Chapel Hill, NC 27599 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2014年 / 136卷 / 01期

基金：

美国国家科学基金会;

关键词：

PHOTOSYSTEM-II; VISIBLE-LIGHT; RUTHENIUM CATALYST; BIPYRIDINE LIGANDS; CRYSTAL-STRUCTURE; COMPLEXES; OXYGEN; REDOX; EFFICIENT; RESOLUTION;

D O I：

10.1021/ja409267p

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Simply mixing a Cu(II) salt and 6,6'-dihydroxy-2,2'-bipyridine (H2L) in a basic aqueous solution afforded a highly active water oxidation catalyst (WOC). Cyclic voltammetry of the solution at pH = 12-14 shows irreversible catalytic current with an onset potential of similar to 0.8 V versus NHE. Catalytic oxygen evolution takes place in controlled potential electrolysis at a relatively low overpotential of 640 mV. Experimental and computational studies suggest that the L ligand participates in electron transfer processes to facilitate the oxidation of the Cu center to lead to an active WOC with low overpotential, akin to the use of the tyrosine radical by Photosystem II to oxidize the CaMn4 center for water oxidation.

引用

收藏

页码：273 / 281

页数：9

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