Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol

Dmitrii Y. Osadchii, Alma I. Olivos-Suarez, Ágnes Szécsényi, Guanna Li, Maxim A. Nasalevich, Iulian A. Dugulan, Pablo Serra Crespo, Emiel J.M. Hensen, Sergey L. Veber, Matvey V. Fedin, Gopinathan Sankar, Evgeny A. Pidko, Jorge Gascon

Research output: Contribution to journalArticleScientificpeer-review

69 Citations (Scopus)
27 Downloads (Pure)

Abstract

Hybrid materials bearing organic and inorganic motifs have been extensively discussed as playgrounds for the implementation of atomically resolved inorganic sites within a confined environment, with an exciting similarity to enzymes. Here, we present the successful design of a site-isolated mixed-metal metal organic framework (MOF) that mimics the reactivity of soluble methane monooxygenase enzyme and demonstrates the potential of this strategy to overcome current challenges in selective methane oxidation. We describe the synthesis and characterization of an Fe-containing MOF that comprises the desired antiferromagnetically coupled high-spin species in a coordination environment closely resembling that of the enzyme. An electrochemical synthesis method is used to build the microporous MOF matrix while integrating the atomically dispersed Fe active sites in the crystalline scaffold. The model mimics the catalytic C-H activation behavior of the enzyme to produce methanol and shows that the key to this reactivity is the formation of isolated oxo-bridged Fe units.

Original languageEnglish
Pages (from-to)5542-5548
Number of pages7
JournalACS Catalysis
Volume8
Issue number6
DOIs
Publication statusPublished - 1 Jun 2018

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