期刊
NATURE CHEMISTRY
卷 3, 期 10, 页码 807-813出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1140
关键词
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资金
- European Research Foundation [FP7-PEOPLE-2010-ERG-268445]
- El Ministerio de Ciencia e Innovacion [CTQ2009-08464]
- Ramon y Cajal contract
- Generalitat de Catalunya for an ICREA Academia
- European Research Council [ERC-2009-StG-239910]
Water oxidation catalysis constitutes the bottleneck for the development of energy-conversion schemes based on sunlight. To date, state-of-the-art homogeneous water oxidation catalysis is performed efficiently with expensive, toxic and earth-scarce transition metals, but 3d metal-based catalysts are much less established. Here we show that readily available, environmentally benign iron coordination complexes catalyse homogeneous water oxidation to give O-2, with high efficiency during a period of hours. Turnover numbers >350 and >1,000 were obtained using cerium ammonium nitrate at pH 1 and sodium periodate at pH 2, respectively. Spectroscopic monitoring of the catalytic reactions, in combination with kinetic studies, show that high valent oxo-iron species are responsible for the O-O forming event. A systematic study of iron complexes that contain a broad family of neutral tetradentate organic ligands identifies first-principle structural features to sustain water oxidation catalysis. Iron-based catalysts described herein open a novel strategy that could eventually enable sustainable artificial photosynthetic schemes.
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