Xie, Jijia; Fu, Cong; Quesne, Matthew G; Guo, Jian; Wang, Chao; Xiong, Lunqiao; Windle, Christopher D; ... Tang, Junwang; + view all Xie, Jijia; Fu, Cong; Quesne, Matthew G; Guo, Jian; Wang, Chao; Xiong, Lunqiao; Windle, Christopher D; Gadipelli, Srinivas; Guo, Zheng Xiao; Huang, Weixin; Catlow, C Richard A; Tang, Junwang; - view fewer (2025) Methane oxidation to ethanol by a molecular junction photocatalyst. Nature 10.1038/s41586-025-08630-x. (In press).

Text Methane oxidation to ethanol by a molecular junction photocatalyst.pdf - Accepted Version Access restricted to UCL open access staff until 21 July 2025. Download (103MB)

Abstract

Methane, the major component of natural and shale gas, is a significant carbon source for chemical synthesis. The direct partial oxidation of methane to liquid oxygenates under mild conditions1-3 is an attractive pathway, but the molecule's inertness makes it challenging to achieve simultaneously high conversion and high selectivity towards a single target product. This difficulty is amplified when aiming for more valuable products that require C-C coupling4,5. While selective partial methane oxidation processes1-3,6-9 have thus typically generated C1 oxygenates6,7, recent reports have documented photocatalytic methane conversion to the C2 oxygenate ethanol with low conversions but good to high selectivities4,5,8-12. Here, we show that the intramolecular junction photocatalyst CTF-1 with alternating benzene and triazine motifs7,13 drives methane coupling and oxidation to ethanol with a high selectivity and much improved conversion. The heterojunction architecture not only enables efficient and long-lived separation of charges after their generation, but also preferential adsorption of H2O and O2 to the triazine and benzene units, respectively. This dual-site feature separates C-C coupling to form ethane intermediates from the sites where •OH radicals are formed and thereby avoids overoxidation. When loaded with Pt to boost performance further, the molecular heterojunction photocatalyst generates ethanol in a packed-bed flow reactor with improved conversion that results in an apparent quantum efficiency of 9.4%. We anticipate that further developing the "intramolecular junction" approach will deliver efficient and selective catalysts for C-C coupling, pertaining, but not limited, to methane conversion to C2+ chemicals.

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