Facet Engineering in Constructing Lewis Acid-Base Pairs for CO_(2) Cycloaddition to High Value-Added Carbonates  

作　　者：Shu Shang Wei Shao Xiao Luo Ming Zuo Hui Wang Xiaodong Zhang Yi Xie 

机构地区：[1]Hefei National Research Center for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei 230026,China [2]Institute of Energy,Hefei Comprehensive National Science Center,Hefei 230031,China

出　　处：《Research》2023年第1期331-339,共9页研究（英文）

基　　金：supported by the National Key R&D Program of China(2021YFA1501502,2019YFA0210004);Anhui Provincial Key Research and Development Program(2022a05020054);the National Natural Science Foundation of China(21922509,92163105,21905262,T2122004,21890754,U2032212,U2032160);the Strategic Priority Research Program of Chinese Academy of Sciences(XDB36000000);Anhui Provincial Natural Science Foundation(2008085QB88);the Youth Innovation Promotion Association of CAS(Y2021123);the Fundamental Research Funds for the Central Universities(WK2060000039);the University Synergy Innovation Program of Anhui Province(GXXT-2020-005).

摘　　要：Cycloaddition of epoxides with CO_(2) to synthesis cyclic carbonates is an atom-economic pathway for CO_(2) utilization with promising industry application value,while its efficiency was greatly inhibited for the lack of highly active catalytic sites.Herein,by taking BiOx(X=Cl,Br)with layered structure for example,we proposed a facet engineering strategy to construct Lewis acid-base pairs for CO_(2) cycloaddition,where the typical BiOBr with(O10)facets expose surface Lewis acid Bi sites and Lewis base Br sites simultaneously.By the combination of in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and theoretical calculations,the oxygen atom of the epoxide is interacted with the Lewis acid Bi site to activate the ternary ring,then facilitates the attack of the carbon atom by the Lewis base Br site for the ring-opening of the epoxide,which is the rate-determining step in the cycloaddition reaction.As a result,the BiOBr-(010)with rich surface Lewis acid-base pairs showed a high conversion of 85%with 100% atomic economy in the synthesis of cyclic-carbonates without any cocatalyst.This study provides a model structure for CO,cycloaddition to high value-added long chain chemicals.

关 键 词：REACTION base synthesis 

分 类 号：O64[理学—物理化学]