Rapid water oxidation electrocatalysis by a ruthenium complex of the tripodal ligand tris(2-pyridyl)phosphine oxide

被引：48

作者：

Walden, Andrew G. ^{[1
]}

Miller, Alexander J. M. ^{[1
]}

机构：

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

来源：

CHEMICAL SCIENCE | 2015年 / 6卷 / 04期

关键词：

PHOTOSYSTEM-II; CATALYTIC-OXIDATION; CYCLIC VOLTAMMETRY; ELECTRON-TRANSFER; OXYGEN EVOLUTION; MONONUCLEAR; SITE; PHOTOSYNTHESIS; 2-PYRIDYL; SYSTEMS;

D O I：

10.1039/c5sc00032g

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The tris(2-pyridyl)phosphine oxide (Py3PO) complex [Ru(Py3PO)(bpy)(OH2)](2+) (bpy is 2,2'-bipyridine) is a pH-dependent water oxidation electrocatalyst that accelerates dramatically with increasing pH-up to 780 s(-1) at pH 10 (similar to 1 V overpotential). Despite retaining the pentakis(pyridine) ligand arrangement common to previously reported catalysts, the tripodal Py3PO ligand framework supports much faster electrocatalysis. The early stages of the catalytic cycle are proposed to follow the typical pattern of single-site ruthenium catalysts, with two sequential 1H(+)/1e(-) proton-coupled electron transfer (PCET) oxidations, but the pH-dependent onset of catalysis and rapid rates are distinguishing features of the present system.

引用

页码：2405 / 2410

页数：6

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