Efficient water oxidation catalysts based on readily available iron coordination complexes

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dc.contributor.author Lloret Fillol, Julio
dc.contributor.author Codolà Duch, Zoel
dc.contributor.author Garcia Bosch, Isaac
dc.contributor.author Gómez Martín, Laura
dc.contributor.author Pla, Juan José
dc.contributor.author Costas Salgueiro, Miquel
dc.date.issued 2011
dc.identifier.issn 1755-4330 (versió paper)
dc.identifier.issn 1755-4349 (versió electrònica)
dc.identifier.uri http://hdl.handle.net/10256/7146
dc.description.abstract 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
dc.description.sponsorship 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.)
dc.format.mimetype application/pdf
dc.language.iso eng
dc.publisher Macmillan Publishers
dc.relation MICINN/PN 2010-2012/CTQ2009-08464
dc.relation.isformatof Reproducció digital del document publicat a: http://dx.doi.org/10.1038/nchem.1140
dc.relation.ispartof © Nature Chemistry, 2011, núm. 3, p. 807–813
dc.relation.ispartofseries Articles publicats (D-Q)
dc.rights Tots els drets reservats
dc.subject Ferro -- Compostos
dc.subject Iron compounds
dc.subject Catàlisi homogènia
dc.subject Homogeneous catalysis
dc.subject Oxidació
dc.subject Oxidation
dc.title Efficient water oxidation catalysts based on readily available iron coordination complexes
dc.type info:eu-repo/semantics/article
dc.rights.accessRights info:eu-repo/semantics/closedAccess
dc.relation.projectID info:eu-repo/grantAgreement/EC/FP7/268445
dc.relation.projectID info:eu-repo/grantAgreement/EC/FP7/239910
dc.type.version info:eu-repo/semantics/publishedVersion
dc.identifier.doi http://dx.doi.org/10.1038/nchem.1140
dc.contributor.funder Ministerio de Ciencia e Innovación (Espanya)


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