A Non-Heme Iron Photocatalyst for Light-Driven Aerobic Oxidation of Methanol

Juan Chen, Stepan Stepanovic, Apparao Draksharapu, Maja Gruden, Wesley R Browne

Research output: Contribution to journalArticleAcademicpeer-review

13 Citations (Scopus)
245 Downloads (Pure)

Abstract

Non-heme (L)FeIIIand (L)FeIII-O-FeIII(L) complexes (L=1,1-di(pyridin-2-yl)-N,N-bis(pyridin-2-ylmethyl)ethan-1-amine) underwent reduction under irradiation to the FeIIstate with concomitant oxidation of methanol to methanal, without the need for a secondary photosensitizer. Spectroscopic and DFT studies support a mechanism in which irradiation results in charge-transfer excitation of a FeIII-μ-O-FeIIIcomplex to generate [(L)FeIV=O]2+(observed transiently during irradiation in acetonitrile), and an equivalent of (L)FeII. Under aerobic conditions, irradiation accelerates reoxidation from the FeIIto the FeIIIstate with O2, thus closing the cycle of methanol oxidation to methanal.

Original languageEnglish
Pages (from-to)3207-3211
Number of pages5
JournalAngewandte Chemie - International Edition
Volume57
Issue number12
DOIs
Publication statusPublished - 12-Mar-2018

Keywords

  • Journal Article

Cite this