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

Nano Lett. 2024 Feb 7;24(5):1801-1807. doi: 10.1021/acs.nanolett.3c04978. Epub 2024 Jan 26.

Abstract

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.

Keywords: electrooxidation of propylene; in-plane C−O coupling; propylene glycol; single-atom catalysts.