A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II

Abstract

Across chemical disciplines, an interest in developing artificial water splitting to O 2 and H 2, driven by sunlight, has been motivated by the need for practical and environmentally friendly power generation without the consumption of fossil fuels. The central issue in light-driven water splitting is the efficiency of the water oxidation, which in the best-known catalysts falls short of the desired level by approximately two orders of magnitude. Here, we show that it is possible to close that 'two orders of magnitude' gap with a rationally designed molecular catalyst [Ru(bda)(isoq) 2] (H 2 bda = 2,2'-bipyridine-6,6'- dicarboxylic acid; isoq = isoquinoline). This speeds up the water oxidation to an unprecedentedly high reaction rate with a turnover frequency of >300 s -1. This value is, for the first time, moderately comparable with the reaction rate of 100-400s -1 of the oxygen-evolving complex of photosystem II in vivo. © 2012 Macmillan Publishers Limited. All rights reserved.