Promotion effect of epoxy group neighboring single-atom Cu site on acetylene hydrochlorination  

作　　者：Junchen Peng Xue Yin Dandan Dong Zhongyuan Guo Qinqin Wang Minmin Liu Fei He Bin Dai Chaofeng Huang 

机构地区：[1]School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering,Shihezi University,Shihezi 832000,China [2]College of Chemistry&Chemical Engineering,Yantai University,Yantai 264010,China [3]School of Material Science and Engineering,University of Jinan,Ji’nan 250022,China

出　　处：《Chinese Chemical Letters》2024年第6期258-262,共5页中国化学快报（英文版）

基　　金：supported by the National Natural Science Foundation of China(No.22062021);the Science and Technology Project of Xinjiang supported by Central Government(No.2022BC001);Tianshan Talents Training Program of Xinjiang(Science and Technology Innovation Team,No.CZ002701);the Opening Project of Key Laboratory for Green Processing of Chemical Engineering of Xinjiang(No.KF2019010);the Start-Up Foundation for high-level professionals of Shihezi University(No.RCZK201932);research project of Shihezi University(No.CXFZ202205)。

摘　　要：Carbon materials have been used as the support for catalysts in the field of acetylene hydrochlorination,the influence of inevitable oxygen-containing moieties on the reaction is often ignored and the mechanism of the oxygen-doping structure remains ambiguous.Herein,we explored the effect of the oxygen-containing group(C-O-C)in the support on the activity of single-atom dispersed Cu catalysts.By immersing the Cu single-atom catalyst in an alkaline solution,the epoxy species on the carbon support was cleaved to obtain a pure ether species while the Cu site was modified to a more electron-deficient state.The turnover frequency value of Cu/O-FLP catalyst with epoxy groups was 1.6-fold higher than that of alkaline treated catalyst.Our result indicated that the epoxy groups could assist adjacent single-atom Cu sites to synergistically promote the adsorption and cleavage of the reactant hydrogen chloride toward form C-OH and Cu-Cl bonds,and reduce the reaction energy barrier.The presence of electron deficient Cu sites and ether species could induce competitive adsorption of the acetylene and hydrogen chloride,thereby reducing the activity of the catalyst.This study highlights the influence of surface oxygen species and the tunability of the support,providing the foundation for the fabrication of higher-activity Cu catalysts for acetylene hydrochlorination.

关 键 词：Epoxy group Acetylene hydrochlorination Single-atom Cu catalyst Synergistic dissociation 

分 类 号：O643.36[理学—物理化学]