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

Journal Article (2020)
Author(s)

Jian Zheng (Pacific Northwest National Laboratory)

Insu Lee (Technische Universität München)

Elena Khramenkova (TU Delft - ChemE/Inorganic Systems Engineering)

Meng Wang (Pacific Northwest National Laboratory)

Bo 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)

Evgeny A. Pidko (TU Delft - ChemE/Algemeen, TU Delft - ChemE/Inorganic Systems Engineering)

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Research Group
ChemE/Inorganic Systems Engineering
DOI related publication
https://doi.org/10.1002/chem.202000772
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Publication Year
2020
Language
English
Research Group
ChemE/Inorganic Systems Engineering
Issue number
34
Volume number
26
Pages (from-to)
7563-7567
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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.