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

Journal article (2018)

Authors

D. Osadchii King Abdullah University of Science and Technology,
Gopinathan Sankar University College London
E.A. Pidko Eindhoven University of Technology, ITMO University, ChemE/Algemeen ,
J. Gascon Sabate , King Abdullah University of Science and Technology
A. Szécsényi Eindhoven University of Technology, King Abdullah University of Science and Technology,
G. Li Eindhoven University of Technology,
A.I. Dugulan RID/TS/Technici Pool
P. Serra Crespo , RST/Applied Radiation & Isotopes - AS
Emiel J.M. Hensen Eindhoven University of Technology
Sergey L. Veber Novosibirsk State University, International Tomography Center SB RAS
Matvey V. Fedin Novosibirsk State University
Copyright: © 2018 D. Osadchii, A.I. Olivos Suarez, A. Szécsényi, G. Li, M. Nasalevich, A.I. Dugulan, P. Serra Crespo, Emiel J.M. Hensen, Sergey L. Veber, Matvey V. Fedin, Gopinathan Sankar, E.A. Pidko, Jorge Gascon
DOI
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https://doi.org/10.1021/acscatal.8b00505
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Published Date

01-06-2018

Language

English

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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.