DUGiDocsEvidence for an oxygen evolving iron–oxo–cerium intermediate in iron-catalysed water oxidation
dc.contributor.author
dc.date.accessioned
2016-03-15T11:12:54Z
dc.date.available
2016-03-15T11:12:54Z
dc.date.issued
2015
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2041-1723
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dc.description
L' afiliació dels autors Laura Gómez, Scott T. Kleespies i Lawrence Que Jr són incorrectes en aquest article. L'errata està publicada a 'Nature Communications', vol. 6, Article number: 6405 doi: http://dx.doi.org/10.1038/ncomms7405
dc.description.abstract
The non-haem iron complex α-[FeII(CF3SO3)2(mcp)] (mcp=(N,N′-dimethyl-N,N′-bis(2-pyridylmethyl)-1,2-cis-diaminocyclohexane) reacts with CeIV to oxidize water to O2, representing an iron-based functional model for the oxygen evolving complex of photosystem II. Here we trap an intermediate, characterized by cryospray ionization high resolution mass spectrometry and resonance Raman spectroscopy, and formulated as [(mcp)FeIV(O)(μ-O)CeIV(NO3)3]+, the first example of a well-characterized inner-sphere complex to be formed in cerium(IV)-mediated water oxidation. The identification of this reactive FeIV–O–CeIV adduct may open new pathways to validate mechanistic notions of an analogous MnV–O–CaII unit in the oxygen evolving complex that is responsible for carrying out the key O–O bond forming step
dc.description.sponsorship
We thank Dr. Xavi Ribas and Dr. Anna Company for reading this work and for helpful comments. We also thank the European Research Foundation for project FP7-PEOPLE- 2010-ERG-268445 (J.L.-F), MICINN for project CTQ2009-08464 (M.C.) and for a Ramon y Cajal contract (J.L.-F.), Generalitat de Catalunya for an ICREA Academia Award and the European Research Foundation for Project ERC-2009-StG-239910 (M.C.). The work carried out at the University of Minnesota was supported by US National Institutes of Health grant GM38767 to L.Q. We appreciate financial support from INNPLANTA project INP-2011-0059-PCT-420000-ACT1 to Dr. X. Ribas
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application/pdf
dc.language.iso
eng
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Macmillan
dc.relation
MICINN/PN 2011/INP-2011-0059-PCT-420000
MICINN/PN 2010-2012/ CTQ2009-08464
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Reproducció digital del document publicat a: http://dx.doi.org/10.1038/ncomms6865
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© Nature Communications, 2015, vol. 6, núm. art. 5865
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Articles publicats (D-Q)
dc.rights
Tots els drets reservats
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dc.title
Evidence for an oxygen evolving iron–oxo–cerium intermediate in iron-catalysed water oxidation
dc.type
info:eu-repo/semantics/article
dc.rights.accessRights
info:eu-repo/semantics/embargoedAccess
dc.embargo.terms
Cap
dc.date.embargoEndDate
info:eu-repo/date/embargoEnd/2026-01-01
dc.relation.projectID
info:eu-repo/grantAgreement/EC/FP7/239910/EU/Bio-inspired Design of Catalysts for Selective Oxidations of C-H and C=C Bonds/BIDECASEOX
info:eu-repo/grantAgreement/EC/FP7/268445/EU/Modular Ligands for Water Splitting/WATERSPLIT
dc.type.version
info:eu-repo/semantics/publishedVersion
dc.identifier.doi
dc.identifier.idgrec
022169
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