Evidence for an ​oxygen evolving iron–oxo–cerium intermediate in iron-catalysed ​water oxidation

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​ ​ scopusId Codolà Duch, Zoel​ ​
Codolà Duch, Zoel
orcId Gómez Martín, Laura​ ​ scopusId Gómez Martín, Laura​ ​
Gómez Martín, Laura
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Kleespies, Scott T.
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Que, Lawrence
orcId Costas Salgueiro, Miquel​ researcherId Costas Salgueiro, Miquel​ scopusId Costas Salgueiro, Miquel​ ​
Costas Salgueiro, Miquel
orcId Lloret Fillol, Julio​ researcherId Lloret Fillol, Julio​ scopusId Lloret Fillol, Julio​ ​
Lloret Fillol, Julio
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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 ​
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