Highly Selective Photocatalytic Methane Coupling by Au-Modified Bi 2 WO 6

作者：Muchun Fei, Benjamin P. Williams, Lizhuo Wang, Haoyi Li, Yucheng Yuan, James R. Wilkes, Tianying Liu, Yu Mu, Jier Huang, James Nyakuchena, Jun Huang, Wei Li, Dunwei Wang · 发表于：ACS Catalysis · 年份：2024 · DOI：10.1021/acscatal.3c05534 · 被引用次数：66 · 研究领域：Advanced Photocatalysis Techniques、Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions

Photocatalytic oxidative coupling of methane (OCM) to ethane promises a route to value-added C 2 products from an abundant and low-cost feedstock. However, selective activation of the C–H bond of CH 4 without overoxidation to CO 2 has been a major challenge. In this work, we present the use of Au-modified Bi 2 WO 6 as a prototypical photocatalyst, demonstrating a high performance of OCM through photocatalysis. A C 2 H 6 production rate at 1.69 × 10 3 μmol·g –1 ·h –1 with approximately 85% selectivity was achieved, which ranks among the top-performing photocatalytic OCM systems. Efforts were also made in establishing a correlation between improved OCM performance and the photocatalyst system by examining the nature of the oxide photocatalyst. Our findings indicated that oxygen within the oxide surface, likely from adsorbed and subsequently dissociated oxygen at the vacancy sites, afforded a desired reactivity to selectively activate the C–H bond without significant overoxidation. Surprisingly, it was revealed that the Au cocatalyst plays dual roles of activating the oxide photocatalyst for enhanced CH 4 activation and promoting C–C coupling to yield C 2 H 6 as the main product.