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Efficient water oxidation catalysts based on readily available iron coordination complexes

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 O2, 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

We thank R. Hage, X. Ribas and P. Lahuerta for reading this work and for comments. We thank the European Research Foundation for project FP7-PEOPLE-2010-ERG-268445 (J.Ll.), El Ministerio de Ciencia e Innovacion for project CTQ2009-08464 (M. C.), for a Ramon y Cajal contract (J.Ll.) and for a PhD grant (I. G-B.), Generalitat de Catalunya for an ICREA Academia Award and the European Research Council for Project ERC-2009-StG-239910 (M. C.)

© Nature Chemistry, 2011, núm. 3, p. 807–813

Macmillan Publishers

Autor: Lloret Fillol, Julio
Codolà Duch, Zoel
Garcia Bosch, Isaac
Gómez Martín, Laura
Pla, Juan José
Costas Salgueiro, Miquel
Data: 2011
Resum: 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 O2, 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
We thank R. Hage, X. Ribas and P. Lahuerta for reading this work and for comments. We thank the European Research Foundation for project FP7-PEOPLE-2010-ERG-268445 (J.Ll.), El Ministerio de Ciencia e Innovacion for project CTQ2009-08464 (M. C.), for a Ramon y Cajal contract (J.Ll.) and for a PhD grant (I. G-B.), Generalitat de Catalunya for an ICREA Academia Award and the European Research Council for Project ERC-2009-StG-239910 (M. C.)
Format: application/pdf
ISSN: 1755-4330 (versió paper)
1755-4349 (versió electrònica)
Accés al document: http://hdl.handle.net/10256/7146
Llenguatge: eng
Editor: Macmillan Publishers
Col·lecció: MICINN/PN 2010-2012/CTQ2009-08464
Reproducció digital del document publicat a: http://dx.doi.org/10.1038/nchem.1140
Articles publicats (D-Q)
info:eu-repo/grantAgreement/EC/FP7/268445
info:eu-repo/grantAgreement/EC/FP7/239910
És part de: © Nature Chemistry, 2011, núm. 3, p. 807–813
Drets: Tots els drets reservats
Matèria: Ferro -- Compostos
Iron compounds
Catàlisi homogènia
Homogeneous catalysis
Oxidació
Oxidation
Títol: Efficient water oxidation catalysts based on readily available iron coordination complexes
Tipus: info:eu-repo/semantics/article
Repositori: DUGiDocs

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