Isolated Fe sites in Metal Organic Framework catalyze the direct conversion of methane to methanol

by D. Osadchii, A.I. Olivos Suarez, A. Szécsényi, G. Li, M. Nasalevich, A. Dugulan, P. Serra-Crespo, E. Hensen, S. Veber, M. Fedin, G. Sankar, E. Pidko, J. Gascon
Year: 2018

Bibliography

D. Osadchii, A.I. Olivos Suarez, A. Szécsényi, G. Li, M. Nasalevich, A. Dugulan, P. Serra-Crespo, E. Hensen, S. Veber, M. Fedin, G. Sankar, E. Pidko and J. Gascon. ACS Catal 8 (2018) 5542–5548, Isolated Fe sites in Metal Organic Framework catalyze the direct conversion of methane to methanol

Abstract

​Hybrid materials bearing organic and inorganic motives 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 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 characterisation 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 behaviour of the enzyme to produce methanol, and shows that the key to this reactivity is the formation of isolated oxo-bridged Fe units.​

Keywords

MOFs methane oxidation isolated metal sites Enzyme-mimicking catalysts