Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane

作者：Pu Zhang, Junwei Li, Haowei Huang, Xiaoyu Sui, Haihua Zeng, Haijiao Lu, Ying Wang, Yanyan Jia, Julian A. Steele, Yanhui Ao, Maarten B. J. Roeffaers, Sheng Dai, Zizhong Zhang, Lianzhou Wang, Xianzhi Fu, Jinlin Long · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.4c08901 · 被引用次数：62 · 研究领域：Advanced Photocatalysis Techniques、Catalytic Processes in Materials Science、CO2 Reduction Techniques and Catalysts

This work introduces a new strategy of a single-atom nest catalyst, whereby several single atoms are positioned closely, aiming to achieve the dual benefits of high atom-utilization efficiency while avoiding the steric hindrance in the coupling reaction. As a proof of concept, Pt single-atom nests, where the adjacent Pt single atoms are approximately 4 Å apart, are precisely engineered on the TiO 2 photocatalyst for photocatalytic non-oxidative coupling of methane. The Pt single-atom nest photocatalyst demonstrates remarkable activity, achieving a C 2 H 6 yield and turnover frequency of 251.6 μmol g cat –1 h –1 and 20 h –1, respectively, representing a 3.2-fold improvement compared to the Pt single-atom photocatalyst. Density functional theory calculations reveal that the Pt single-atom nest can significantly decrease the energy barrier for the activation of both CH 4 molecules in the coupling process.