Importance of Methane Chemical Potential for Its Conversion to Methanol on Cu‐Exchanged Mordenite. Issue 34 (11th May 2020)

• Record Type: Journal Article
• Authors: Zheng, Jian; Lee, Insu; Khramenkova, Elena; Wang, Meng; Peng, Bo; Gutiérrez, Oliver Y.; Fulton, John L.; Camaioni, Donald M.; Khare, Rachit; Jentys, Andreas; Haller, Gary L.; Pidko, Evgeny A.; Sanchez‐Sanchez, Maricruz; Lercher, Johannes A.
• Is Part Of: Chemistry. Volume 26:Issue 34(2020)
• Page Start: 7563
• Page End: 7567
• Publication Date: 2020-05-11
• Subjects: chemical potential -- copper-trimer -- methane oxidation -- methanol production -- zeolite; Chemistry -- Periodicals; 540
• DOI: 10.1002/chem.202000772
• Languages: English
• ISSNs: 0947-6539

Abstract

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. Abstract : On the oxidation of methane : Elevated methane pressure increased the chemical potential of methane to enable the activation of two CH4 molecules by two μ‐O atoms out of the three contained in a [Cu3 (μ‐O)3 ] 2+ tricopper‐oxo cluster.