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

Zheng, Jian; Lee, Insu; Khramenkova, E.; Wang, Meng; Peng, B.; Gutiérrez, Oliver Y.; Fulton, John L.; Camaioni, Donald M.; Pidko, E.A.

doi:10.1002/chem.202000772

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

Title

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

Author

Zheng, Jian (Pacific Northwest National Laboratory)
Lee, Insu (Technische Universität München)
Khramenkova, E. (TU Delft ChemE/Inorganic Systems Engineering)
Wang, Meng (Pacific Northwest National Laboratory)
Peng, B. (Pacific Northwest National Laboratory)
Gutiérrez, Oliver Y. (Pacific Northwest National Laboratory)
Fulton, John L. (Pacific Northwest National Laboratory)
Camaioni, Donald M. (Pacific Northwest National Laboratory)
Pidko, E.A. (TU Delft ChemE/Algemeen; TU Delft ChemE/Inorganic Systems Engineering)

Date

2020

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.

Subject

chemical potential
copper-trimer
methane oxidation
methanol production
zeolite

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http://resolver.tudelft.nl/uuid:3341616f-1d54-4a2d-87d8-c01800e20d0b

DOI

https://doi.org/10.1002/chem.202000772

ISSN

0947-6539

Source

Chemistry: A European Journal, 26 (34), 7563-7567

Part of collection

Institutional Repository