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

• Published in: Journal of the American Chemical Society 2024-08, Vol.146 (34), p.24150-24157
• Main Authors: Zhang, Pu, Li, Junwei, Huang, Haowei, Sui, Xiaoyu, Zeng, Haihua, Lu, Haijiao, Wang, Ying, Jia, Yanyan, Steele, Julian A., Ao, Yanhui, Roeffaers, Maarten B. J., Dai, Sheng, Zhang, Zizhong, Wang, Lianzhou, Fu, Xianzhi, Long, Jinlin
• Format: Article
• Language: English
• ISSN: 0002-7863; 1520-5126; 1520-5126
• DOI: 10.1021/jacs.4c08901

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 TiO2 photocatalyst for photocatalytic non-oxidative coupling of methane. The Pt single-atom nest photocatalyst demonstrates remarkable activity, achieving a C2H6 yield and turnover frequency of 251.6 μmol gcat –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 CH4 molecules in the coupling process.