4.8 Article

A molecular catalyst for water oxidation that binds to metal oxide surfaces

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NATURE COMMUNICATIONS
卷 6, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms7469

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资金

  1. National Science Foundation [NSF MRSEC DMR 1119826]
  2. NSF Graduate Research Fellowship
  3. U.S. Department of Energy [DE-FG02-07ER15909]
  4. Center for Catalytic Hydrocarbon Functionalization (CCHF)
  5. Argonne-Northwestern Solar Energy Research (ANSER) Center, Energy Frontier Research Centers - U.S. Department of Energy [DE-SC0001298, DE-SC0001059]
  6. Alexander von Humboldt Foundation
  7. Centre for Sustainable Chemical Technologies at the University of Bath (EPSRC) [EP/G03768X/1]

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Molecular catalysts are known for their high activity and tunability, but their solubility and limited stability often restrict their use in practical applications. Here we describe how a molecular iridium catalyst for water oxidation directly and robustly binds to oxide surfaces without the need for any external stimulus or additional linking groups. On conductive electrode surfaces, this heterogenized molecular catalyst oxidizes water with low overpotential, high turnover frequency and minimal degradation. Spectroscopic and electrochemical studies show that it does not decompose into iridium oxide, thus preserving its molecular identity, and that it is capable of sustaining high activity towards water oxidation with stability comparable to state-of-the-art bulk metal oxide catalysts.

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