Bipyridine-Confined Silver Single-Atom Catalysts Facilitate In-Plane C–O Coupling for Propylene Electrooxidation

• Published in: Nano letters 2024-02, Vol.24 (5), p.1801-1807
• Main Authors: Chi, Mingfang, Zhao, Jiankang, Ke, Jingwen, Liu, Yan, Wang, Ruyang, Wang, Chuanhao, Hung, Sung-Fu, Lee, Tsung-Ju, Geng, Zhigang, Zeng, Jie
• Format: Article
• Language: English
• ISSN: 1530-6984; 1530-6992
• DOI: 10.1021/acs.nanolett.3c04978

The electrooxidation of propylene presents a promising route for the production of 1,2-propylene glycol (PG) under ambient conditions. However, the C–O coupling process remains a challenge owing to the high energy barrier. In this work, we developed a highly efficient electrocatalyst of bipyridine-confined Ag single atoms on UiO-bpy substrates (Ag SAs/UiO-bpy), which exposed two in-plane coordination vacancies during reaction for the co-adsorption of key intermediates. Detailed structure and electronic property analyses demonstrate that CH3CHCH2OH* and *OH could stably co-adsorb in a square planar configuration, which then accelerates the charge transfer between them. The combination of stable co-adsorption and efficient charge transfer facilitates the C–O coupling process, thus significantly lowering its energy barrier. At 2.4 V versus a reversible hydrogen electrode, Ag SAs/UiO-bpy achieved a record-high activity of 61.9 gPG m–2 h–1. Our work not only presents a robust electrocatalyst but also advances a new perspective on catalyst design for propylene electrooxidation.