Author: ["Lele Duan","Fernando Bozoglian","Sukanta Mandal","Beverly Stewart","Timofei Privalov","Antoni Llobet","Licheng Sun"]
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Abstract
Across chemical disciplines, an interest in developing artificial water splitting to O2 and H2, 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] (H2bda = 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 100–400 s−1 of the oxygen-evolving complex of photosystem II in vivo. Increasing the efficiency and speed of the water-oxidation reaction is crucial to realizing light-driven water splitting. Now, a mononuclear ruthenium complex achieves fast water-oxidation catalysis with a high reaction rate of more than 300 turnovers per second, comparable to the activity of the oxygen-evolving complex in photosystem II. Cite this article
Duan, L., Bozoglian, F., Mandal, S. et al. A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem II. Nature Chem 4, 418–423 (2012). https://doi.org/10.1038/nchem.1301 