Title |
A Non‐Heme Iron Photocatalyst for Light‐Driven Aerobic Oxidation of Methanol
|
---|---|
Published in |
Angewandte Chemie. International Edition, February 2018
|
DOI | 10.1002/anie.201712678 |
Pubmed ID | |
Authors |
Juan Chen, Stepan Stepanovic, Apparao Draksharapu, Maja Gruden, Wesley R. Browne |
Abstract |
The non-heme (L)FeIII and (L)FeIII-O-FeIII(L) complexes (L = 1,1-di(pyridin-2-yl)-N,N-bis(pyridin-2-ylmethyl)ethan-1-amine) undergoes reduction under irradiation to the FeII state with concomitant oxidation of methanol to methanal, without the need for a secondary photosensitizer. Spectroscopic and Density Functional Theory (DFT) studies support a mechanism in which irradiation results in charge transfer excitation of a FeIII--O-FeIII complex to generate [(L)FeIV=O]2+ (observed transiently during irradiation in acetonitrile), and an equivalent of LFeII. Under aerobic conditions, irradiation accelerates reoxidation from the FeII to FeIII state with O2 closing the cycle of methanol oxidation to methanal. |
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