Issue 7, 2024

An alternative catalytic cycle for selective methane oxidation to methanol with Cu clusters in zeolites

Abstract

The partial oxidation of methane to methanol catalyzed by Cu-exchanged zeolites involves at present a three-step procedure that requires changing reaction conditions along the catalytic cycle. In this work we present an alternative catalytic cycle for selective methane conversion to methanol using as active species small Cu5 clusters supported on CHA zeolite. Periodic DFT calculations show that molecular O2 is easily activated on Cu5 clusters producing bi-coordinated O atoms able to dissociate homolytically a CH bond from CH4 and to react with the radical-like non-adsorbed methyl intermediate formed producing methanol, while competitive overoxidation to CO2 is energetically disfavored. The present mechanistic study opens a new avenue to design catalytic materials based on their ability to stabilize radical species.

Graphical abstract: An alternative catalytic cycle for selective methane oxidation to methanol with Cu clusters in zeolites

Supplementary files

Article information

Article type
Paper
Submitted
28 Du 2023
Accepted
24 Gen. 2024
First published
31 Gen. 2024

Phys. Chem. Chem. Phys., 2024,26, 5914-5921

An alternative catalytic cycle for selective methane oxidation to methanol with Cu clusters in zeolites

M. Gallego, A. Corma and M. Boronat, Phys. Chem. Chem. Phys., 2024, 26, 5914 DOI: 10.1039/D3CP05802F

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