Efficient hydrogenation of ethylene carbonate derived from CO_(2) to synthesize methanol and ethylene glycol over core-shell Cu@GO catalyst

作     者：Chanjuan Zhang Liguo Wang Zhuo Han Peng He Yan Cao Jiachen Li Huiquan Li Chanjuan Zhang;Liguo Wang;Zhuo Han;Peng He;Yan Cao;Jiachen Li;Huiquan Li

作者机构：CAS Key Laboratory of Green Process and EngineeringNational Engineering Research Center of Green Recycling for Strategic Metal ResourcesInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China Sino-Danish CollegeUniversity of Chinese Academy of SciencesBeijing100049China Sino-Danish Center for Education and ResearchUniversity of Chinese Academy of SciencesBeijing100049China School of Chemical EngineeringUniversity of Chinese Academy of SciencesBeijing100049China Dalian National Laboratory for Clean EnergyDalian116023China 

出 版 物：《Green Chemical Engineering》 (绿色化学工程（英文）)

年 卷 期：2022年第3卷第3期

页      面：228-239页

核心收录：

学科分类：083002[工学-环境工程] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 081702[工学-化学工艺] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 

基　　金：We are grateful to the National Natural Science Foundation of China(21576272) “Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA 21030600) Science and Technology Service Network Initiative,Chinese Academy of Sciences(KFJ-STS-QYZD-138) the National Key Research and Development Program of China(2019YFC1906701)for the financial supports. 

主　　题：Ethylene carbonate Selective hydrogenation Methanol Ethylene glycol Cu-based catalyst 

摘      要：The synthesis of sustainable methanol and ethylene glycol(EG)via hydrogenation of ethylene carbonate(EC)has caught researchers’growing interests on account of the indirect chemical utilization of CO_(2).Core-shell Cu@GO catalysts with random nanoporous network of graphite oxide(GO)were synthesized via a simple method of ul-trasonic precipitation.Cu@GO catalysts were analyzed systematically by N_(2) physisorption,TGA measurement,XRD,FT-IR,Raman,TEM,SEM,and XPS(XAES).In particular,the mentioned method was confirmed to be effective to fabricate the high dispersity core-shell Cu@GO catalysts through promoting the specific surface area.The as-prepared Cu@GO catalyst was then successfully applied in the hydrogenation of CO_(2)-derived EC to pro-duce methanol and EG.A high TOF of 1526 mg EC g cat^(-1) h^(-1) could be attained in EC hydrogenation at the reaction temperature of 493K.Accordingly,the correlation of catalytic structure and performance disclosed that the synergistic effect between Cu^(+) and Cu^(0) was responsible for achieving high activity of the catalyst.In addition,the reusability of Cu@GO catalyst suggested that graphite oxide shell structure could decrease the aggregation of Cu particles,thus enhance the stability of Cu-based catalysts.DFT calculation results suggested that the involvement of carbon film on Cu was favorable for the stabilization of the active sites.This study is helpful for developing new and stable catalytic system for indirect chemical utilization of CO_(2) to synthesize commodity methanol and EG.