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

نویسندگان

  • Lele Duan
  • Fernando Bozoglian
  • Sukanta Mandal
  • Beverly Stewart
  • Timofei Privalov
  • Antoni Llobet
  • Licheng Sun
چکیده

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 100-400 s(-1) of the oxygen-evolving complex of photosystem II in vivo.

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عنوان ژورنال:
  • Nature chemistry

دوره 4 5  شماره 

صفحات  -

تاریخ انتشار 2012