Constructing Asymmetric Dual Active Sites Through Bimetallic Synergy for Achieving Selective Photocatalytic Nonoxidative Coupling of Methane toward Ethylene

作者：Huimin Li, Qianqian Shen, Zhe Sun, Wenjie Wang, Jinbo Xue, Jiaguo Yu · 发表于：ACS Catalysis · 年份：2025 · DOI：10.1021/acscatal.5c01732 · 被引用次数：37 · 研究领域：CO2 Reduction Techniques and Catalysts、Carbon dioxide utilization in catalysis、Catalysis and Oxidation Reactions

Photocatalytic nonoxidation coupling of methane reactions can directly convert methane into high-value C 2 products under mild conditions. However, the efficient conversion of CH 4 to C 2 H 4 is severely limited by the high C–H bond energy of CH 4 and the slow kinetic process of C–C coupling. Herein, Mo-WO 3– x catalysts with dual active sites were constructed by the isomorphic substitution of Mo 6+ for W in WO 3 . Among them, Mo doping not only induces the preferential formation of oxygen vacancies between Mo and W atoms, but also enhances the catalytic activity of frustrated Lewis pairs composed of unsaturated W and lattice oxygen. The results show that the asymmetric dual active sites of unsaturated Mo and FLPs accelerate the cleavage of CH 4 molecules, reduce the coupling energy barrier of CH 2 intermediates, and synergistically promote the desorption of C 2 H 4 . The catalyst presents a C 2 H 4 yield of up to 152.19 μmol g –1 h –1 with a selectivity of 95%. This work provides insights into the preparation of highly efficient NOCM photocatalysts with a bimetallic synergistic effect.