Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu-Exchanged Mordenite

Journal article (2020)

Authors

Jian Zheng Pacific Northwest National Laboratory
Insu Lee Technische Universität München
E. Khramenkova ChemE/Inorganic Systems Engineering - AS
Meng Wang Pacific Northwest National Laboratory
B. Peng Pacific Northwest National Laboratory
Oliver Y. Gutiérrez Pacific Northwest National Laboratory
John L. Fulton Pacific Northwest National Laboratory
Donald M. Camaioni Pacific Northwest National Laboratory
E.A. Pidko ChemE/Inorganic Systems Engineering - AS , ChemE/Algemeen
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Research Group
ChemE/Inorganic Systems Engineering (AS) (TU Delft)
Copyright: © 2020 Jian Zheng, Insu Lee, E. Khramenkova, Meng Wang, B. Peng, Oliver Y. Gutiérrez, John L. Fulton, Donald M. Camaioni, E.A. Pidko, More Authors
DOI
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https://doi.org/10.1002/chem.202000772
Zeolite Chemical potential Methane oxidation Copper-trimer Methanol production
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Published Date

2020

Language

English

Faculty

Applied Sciences

Department

ChemE/Chemical Engineering

Research Group

ChemE/Inorganic Systems Engineering

Abstract

Copper-oxo clusters exchanged in zeolite mordenite are active in the stoichiometric conversion of methane to methanol at low temperatures. Here, we show an unprecedented methanol yield per Cu of 0.6, with a 90–95 % selectivity, on a MOR solely containing [Cu3(μ-O)3]2+ active sites. DFT calculations, spectroscopic characterization and kinetic analysis show that increasing the chemical potential of methane enables the utilization of two μ-oxo bridge oxygen out of the three available in the tricopper-oxo cluster structure. Methanol and methoxy groups are stabilized in parallel, leading to methanol desorption in the presence of water.