Lanthanum modified Fe-ZSM-5 zeolites for selective methane oxidation with H2O2

Sun, Songmei, Barnes, Alexandra J., Gong, Xiaoxiao, Lewis, Richard J., Dummer, Nicholas F. ORCID: https://orcid.org/0000-0002-0946-6304, Bere, Takudzwa, Shaw, Greg, Richards, Nia, Morgan, David J. ORCID: https://orcid.org/0000-0002-6571-5731 and Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560 2021. Lanthanum modified Fe-ZSM-5 zeolites for selective methane oxidation with H2O2. Catalysis Science & Technology 11 (24) , pp. 8052-8064. 10.1039/D1CY01643A

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Abstract

Selective partial oxidation of methane to methanol under ambient conditions is a great challenge in chemistry. Iron modified ZSM-5 catalysts are shown to be effective for this reaction using H2O2 as the oxidant. However, the high consumption of H2O2 over this catalyst presents a major disadvantage. Here we report a lanthanum modified Fe-ZSM-5 (LaFe-ZSM-5) catalyst for enhanced selective methane oxidation with suppressed H2O2 consumption. Using 0.5 wt% LaFe-ZSM-5 pretreated with H2 the productivity of primary oxygenated products (CH3OH, CH3OOH, HCOOH) is 3200 mol kgLaFe−1 h−1 in 0.1 M H2O2, with a selectivity of 98.9% to primary oxygenated products. The productivity is increased to 11 460 mol kgLaFe−1 h−1 in 0.5 M H2O2. Compared with Fe-ZSM-5, LaFe-ZSM-5 uses 31% less H2O2 for obtaining per mol of product under the same conditions. In situ DRIFT spectroscopy and solid state MAS NMR revealed the high H2O2 consumption in ZSM-5 based catalyst maybe closely related to the acidity of strong Brønsted acid sites (Si(OH)Al). The La modified ZSM-5 catalyst can decrease the acidity of the strong Brønsted acid sites and this suppresses the decomposition of H2O2.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Additional Information:	This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.
Publisher:	Royal Society of Chemistry
ISSN:	2044-4753
Funders:	National Natural Science Foundation of China and European Union's Horizon 2020 research and innovation program under the Marie Sk�odowska-Curie Actions
Date of First Compliant Deposit:	16 November 2021
Date of Acceptance:	10 November 2021
Last Modified:	11 Oct 2023 20:11
URI:	https://orca.cardiff.ac.uk/id/eprint/145542

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