Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane

作者：Yihong Chen, Yuan Zhao, Dong Liu, Gang Wang, Wenbin Jiang, Shengkun Liu, Wenqing Zhang, Yaping Li, Zili Ma, Tianyi Shao, Hengjie Liu, Xiyu Li, Zhiyong Tang, Chao Gao, Yujie Xiong · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.3c10069 · 被引用次数：84 · 研究领域：Catalytic Processes in Materials Science、Advanced Photocatalysis Techniques、Catalysis and Oxidation Reactions

Photocatalytic oxidative coupling of methane (OCM) into value-added industrial chemicals offers an appealing green technique for achieving sustainable development, whereas it encounters double bottlenecks in relatively low methane conversion rate and severe overoxidation. Herein, we engineer a continuous gas flow system to achieve efficient photocatalytic OCM while suppressing overoxidation by synergizing the moderate active oxygen species, surface plasmon-mediated polarization, and multipoint gas intake flow reactor. Particularly, a remarkable CH 4 conversion rate of 218.2 μmol h –1 with an excellent selectivity of ∼90% toward C 2+ hydrocarbons and a remarkable stability over 240 h is achieved over a designed Au/TiO 2 photocatalyst in our continuous gas flow system with a homemade three-dimensional (3D) printed flow reactor. This work provides an informative concept to engineer a high-performance flow system for photocatalytic OCM by synergizing the design of the reactor and photocatalyst to synchronously regulate the mass transfer, activation of reactants, and inhibition of overoxidation.