Issue 4, 2015

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

Abstract

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 (∼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.

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

Supplementary files

Article information

Article type
Edge Article
Submitted
06 jan 2015
Accepted
04 feb 2015
First published
04 feb 2015
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2015,6, 2405-2410

Author version available

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

A. G. Walden and A. J. M. Miller, Chem. Sci., 2015, 6, 2405 DOI: 10.1039/C5SC00032G

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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