Integrating photochemical and photothermal effects for selective oxidative coupling of methane into C2+ hydrocarbons with multiple active sites

Hui Song (), Kai Sun, Hengming Huang (), Shangbo Ning, Shengyao Wang, Zhuan Wang, Yuxiang Weng, Yi Cui, Yifan Li, Xu-sheng Wang, Defa Wang, Lequan Liu, Zhou-jun Wang () and Jinhua Ye ()
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Hui Song: Tianjin University
Kai Sun: Tianjin University
Hengming Huang: Nanjing Tech University
Shangbo Ning: Hebei University
Shengyao Wang: Huazhong Agricultural University
Zhuan Wang: Chinese Academy of Sciences
Yuxiang Weng: Chinese Academy of Sciences
Yi Cui: Chinese Academy of Sciences
Yifan Li: Chinese Academy of Sciences
Xu-sheng Wang: Zhejiang Sci-Tech University
Defa Wang: Tianjin University
Lequan Liu: Tianjin University
Zhou-jun Wang: Ningxia University
Jinhua Ye: Tianjin University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract The direct photocatalytic oxidation of methane to value-added chemicals has garnered considerable interest in recent years. However, achieving high productivity while maintaining high selectivity at an appreciable methane conversion rate remains a formidable challenge. Here, we present photochemically-triggered and photothermally-enhanced oxidative coupling of methane to multi-carbon C2+ alkanes over an Au and CeO2 nanoparticle-decorated ZnO photocatalyst, which exhibits a record-breaking C2+ production rate of 17,260 μmol g−1 h−1 with ~90% C2+ selectivity under wide-spectrum light irradiation without a secondary source of heating. Comprehensive characterizations and computational studies reveal that CH4 activation is a photochemical reaction initiated by ultraviolet light-excited ZnO, and the introduction of CeO2 substantially enhances the activation of CH4 and O2 due to the cooperative interaction between Au and CeO2. Concurrently, Au nanoparticles capture visible and near-infrared light to generate localized heating, which greatly promotes the subsequent desorption of produced methyl radical for C–C coupling prior to undergoing further undesired overoxidation.

Date: 2025
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DOI: 10.1038/s41467-025-58101-0

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