Framework Effects on Activation and Functionalisation of Methane in Zinc‐Exchanged Zeolites

Shah, Meera A; Raynes, Sam; Apperley, David C; Taylor, Russell A.

doi:10.1002/cphc.201900973

Framework Effects on Activation and Functionalisation of Methane in Zinc‐Exchanged Zeolites

Shah, Meera A; Raynes, Sam; Apperley, David C; Taylor, Russell A.

Authors

Meera A Shah

Sam Raynes

David C Apperley

Dr Russell Taylor russell.taylor@durham.ac.uk
Associate Professor

Abstract

The first selective oxidation of methane to methanol is reported herein for zinc‐exchanged MOR (Zn/MOR). Under identical conditions, Zn/FER and Zn/ZSM‐5 both form zinc formate and methanol. Selective methane activation to form [Zn‐CH 3 ] + species was confirmed by 13 C MAS NMR spectroscopy for all three frameworks. The percentage of active zinc sites, measured through quantitative NMR spectroscopy studies, varied with the zeolite framework and was found to be ZSM‐5 (5.7%), MOR (1.2%) and FER (0.8%). For Zn/MOR, two signals were observed in the 13 C MAS NMR spectrum, resulting from two distinct [Zn‐CH 3 ] + species present in the 12 MR and 8 MR side pockets, as supported by additional NMR experiments. The observed products of oxidation of the [Zn‐CH 3 ] + species is shown to depend on the zeolite framework type and the oxidative conditions used. These results lay the foundation for developing structure‐function correlations for methane conversion over zinc‐exchanged zeolites

Citation

Shah, M. A., Raynes, S., Apperley, D. C., & Taylor, R. A. (2020). Framework Effects on Activation and Functionalisation of Methane in Zinc‐Exchanged Zeolites. ChemPhysChem, 21(7), 673-679. https://doi.org/10.1002/cphc.201900973

Journal Article Type	Article
Acceptance Date	Nov 26, 2019
Online Publication Date	Jan 17, 2020
Publication Date	Apr 2, 2020
Deposit Date	Dec 3, 2019
Publicly Available Date	Jan 17, 2021
Journal	ChemPhysChem
Print ISSN	1439-4235
Electronic ISSN	1439-7641
Publisher	Wiley
Peer Reviewed	Peer Reviewed
Volume	21
Issue	7
Pages	673-679
DOI	https://doi.org/10.1002/cphc.201900973

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Copyright Statement
This is the accepted version of the following article: Shah, Meera A, Raynes, Sam, Apperley, David C & Taylor, Russell A. (2020). Framework Effects on Activation and Functionalisation of Methane in Zinc‐Exchanged Zeolites. ChemPhysChem 21(7): 673-679 which has been published in final form at https://doi.org/10.1002/cphc.201900973. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for self-archiving.