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Nat Commun. 2015 Jun 25;6:7546. doi: 10.1038/ncomms8546.

Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol.

Author information

1
Department of Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstrasse 4, Garching 85748, Germany.
2
Schuit Institute of Catalysis, Inorganic Materials Chemistry Group, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, PO Box 513, Eindhoven 5600 MB, The Netherlands.
3
Van't Hoff Institute for Molecular Sciences, University of Amsterdam, PO Box 94215, Amsterdam 1090GE, The Netherlands.
4
1] Schuit Institute of Catalysis, Inorganic Materials Chemistry Group, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, PO Box 513, Eindhoven 5600 MB, The Netherlands [2] Institute for Complex Molecular Systems, Eindhoven University of Technology, PO Box 513, Eindhoven 5600 MB, The Netherlands.
5
1] Department of Chemistry and Catalysis Research Center, Technische Universität München, Lichtenbergstrasse 4, Garching 85748, Germany [2] Institute for Integrated Catalysis, Pacific Northwest National Laboratory, PO Box 999, Richland, Washington 99352, USA.

Abstract

Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon-hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite.

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