Print Email Facebook Twitter Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol Title Isolated fe sites in metal organic frameworks catalyze the direct conversion of methane to methanol Author Osadchii, D. (TU Delft ChemE/Catalysis Engineering; King Abdullah University of Science and Technology) Olivos Suarez, A.I. (TU Delft ChemE/Catalysis Engineering) Szécsényi, A. (TU Delft ChemE/Catalysis Engineering; King Abdullah University of Science and Technology; Eindhoven University of Technology) Li, G. (TU Delft ChemE/Catalysis Engineering; Eindhoven University of Technology) Nasalevich, M. (TU Delft ChemE/Catalysis Engineering) Dugulan, A.I. (TU Delft RID/TS/Technici Pool) Serra Crespo, P. (TU Delft ChemE/Catalysis Engineering; TU Delft RST/Applied Radiation & Isotopes) Hensen, Emiel J.M. (Eindhoven University of Technology) Veber, Sergey L. (International Tomography Center SB RAS; Novosibirsk State University) Fedin, Matvey V. (Novosibirsk State University) Sankar, Gopinathan (University College London (UCL)) Pidko, E.A. (TU Delft ChemE/Catalysis Engineering; TU Delft ChemE/Algemeen; Eindhoven University of Technology; ITMO University) Gascon, Jorge (TU Delft ChemE/Catalysis Engineering; King Abdullah University of Science and Technology) Date 2018-06-01 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. To reference this document use: http://resolver.tudelft.nl/uuid:545133cc-398a-4e6b-8bad-45cfed120933 DOI https://doi.org/10.1021/acscatal.8b00505 Embargo date 2019-06-01 ISSN 2155-5435 Source ACS Catalysis, 8 (6), 5542-5548 Bibliographical note Accepted Author Manuscript Part of collection Institutional Repository Document type journal article Rights © 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 Files PDF Osadchii2018_post_print.pdf 1.41 MB Close viewer /islandora/object/uuid:545133cc-398a-4e6b-8bad-45cfed120933/datastream/OBJ/view