H2-reduced phosphomolybdate promotes room-temperature aerobic oxidation of methane to methanol

Wang, Sikai, Fung, Victor, Hülsey, Max J., Liang, Xiaocong, Yu, Zhiyang, Chang, Jinquan, Folli, Andrea ORCID: https://orcid.org/0000-0001-8913-6606, Lewis, Richard J., Hutchings, Graham J. ORCID: https://orcid.org/0000-0001-8885-1560, He, Qian and Yan, Ning 2023. H2-reduced phosphomolybdate promotes room-temperature aerobic oxidation of methane to methanol. Nature Catalysis 6 , pp. 895-905. 10.1038/s41929-023-01011-5

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Abstract

The selective partial oxidation of methane to methanol using molecular oxygen (O2) represents a long-standing challenge, inspiring extensive study for many decades. However, considerable challenges still prevent low-temperature methane activation via the aerobic route. Here we report a precipitated Pd-containing phosphomolybdate, which, after activation by molecular hydrogen (H2), converts methane and O2 almost exclusively to methanol at room temperature. The highest activity reaches 67.4 μmol gcat−1 h−1. Pd enables rapid H2 activation and H spillover to phosphomolybdate for Mo reduction, while facile O2 activation and subsequent methane activation occur on the reduced phosphomolybdate sites. Continuous production of methanol from methane was also achieved by concurrently introducing H2, O2 and methane into the system, where H2 assists in maintaining a moderately reduced state of phosphomolybdate. This work reveals the underexplored potential of such a Mo-based catalyst for aerobic methane oxidation and highlights the importance of regulating the chemical valence state to construct methane active sites.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Nature Research
ISSN:	2520-1158
Funders:	Cardiff University and the Max Planck Centre for Fundamental Heterogeneous Catalysis (FUNCAT)
Date of First Compliant Deposit:	7 September 2023
Date of Acceptance:	24 July 2023
Last Modified:	11 Nov 2024 13:45
URI:	https://orca.cardiff.ac.uk/id/eprint/162312

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