Partially bonded aluminum site on the external surface of post-treated Au/ZSM-5 enhances methane oxidation to oxygenates

Cao, Jingxian, Qi, Guodong, Yao, Bingqing, He, Qian, Lewis, Richard J., Li, Xu, Deng, Feng, Xu, Jun and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2024. Partially bonded aluminum site on the external surface of post-treated Au/ZSM-5 enhances methane oxidation to oxygenates. ACS Catalysis 14 , pp. 1797-1807. 10.1021/acscatal.3c05030

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Abstract

Au nanoparticles supported on the exterior surface of the ZSM-5 zeolite (Au/ZSM-5) have shown the ability to partially oxidize methane to methanol and acetic acid. However, further improvements to the catalyst activity are required. This study investigates the effect of modifying the acidic properties of the ZSM-5 support through a desilication–recrystallization (DR) process on the activity of Au/ZSM-5 catalysts toward methane oxidation. A DR treatment of 24 h leads to a 50% higher oxygenate yield compared to the analogous catalyst prepared using the untreated support. Characterization using solid-state 27Al NMR and FTIR adsorption of pyridine and 2,4,6-trimethylpyridine reveals that DR induces framework dealumination and redistribution of Brønsted acid sites to the zeolite external surface. Two-dimensional 27Al MQMAS NMR further identifies partially coordinated framework Al sites on the zeolite surface, correlating with a higher oxygenate yield. These external acid sites help stabilize the Au nanoparticles, enhancing catalyst stability for methane partial oxidation.

Item Type:	Article
Date Type:	Published Online
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	American Chemical Society
ISSN:	2155-5435
Funders:	National Key R&D Program of China (2022YFA1504500), the National Natural Science Foundation of China (22272185, 22320102002, 22225205, 22127801 and U1932218), and the Natural Science Foundation of Hubei Province (S22H120101)
Date of First Compliant Deposit:	23 January 2024
Date of Acceptance:	6 December 2023
Last Modified:	24 Jan 2024 16:15
URI:	https://orca.cardiff.ac.uk/id/eprint/165766

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