Dynamically Reversible Interconversion of Molecular Catalysts for Efficient Electrooxidation of Propylene into Propylene Glycol

• DOI: 10.1021/jacs.3c00660
• Publication Date: 2023-03-21T19:59:58Z
• Authors: Jingwen Ke; Mingfang Chi; Jiankang Zhao; Yan Liu; Ruyang Wang; Kaiyuan Fan; Yuxuan Zhou; Zhikai Xi; Xiangdong Kong; Hongliang Li; Jie Zeng; Zhigang Geng
• Keywords: Polyvinyl Alcohol; Propylene oxide

For the electrooxidation of propylene into 1,2-propylene glycol (PG), process involves two key steps generation *OH and transfer to C═C bond in propylene. The strong binding energy (EB(*OH)) favors dissociation H2O *OH, whereas will be impeded. scaling relationship EB(*OH) plays a role affecting catalytic performance toward electrooxidation. Herein, we adopt an immobilized Ag pyrazole molecular catalyst (denoted as AgPz) electrocatalyst. pyrrolic N–H AgPz could undergo deprotonation form N AgPz-Hvac), which can protonated reversibly. During electrooxidation, on *OH. Subsequently, transforms AgPz-Hvac that possesses weak EB(*OH), benefiting further combination dynamically reversible interconversion between accompanied by changeable breaks relationship, thus greatly lowering reaction barrier. At 2.0 V versus Ag/AgCl electrode, achieves remarkable yield rate 288.9 mmolPG gcat–1 h–1, is more than one order magnitude higher highest value ever reported.