Interface tuning of Cu+/CuO by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst

作     者：Yujun Zhao Huanhuan Zhang Yuxi Xu Shengnian Wang Yan Xu Shengping Wang Xinbin Ma Yujun Zhao;Huanhuan Zhang;Yuxi Xu;Shengnian Wang;Yan Xu;Shengping Wang;Xinbin Ma

作者机构：Key Laboratory for Green Chemical Technology of Ministry of EducationCollaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Chemical EngineeringInstitute for Micromanufacturing.Louisiana Tech UniversityRustonLA 71272USA 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2020年第29卷第10期

页      面：248-256页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：financial support from the National Natural Science Foundation of China(21878227 U1510203) 

主　　题：Copper Zirconia Hydrogenation Ethylene glycol 

摘      要：An efficient ZrO2-doped Cu/SiO2 catalyst was fabricated through hydrolysis precipitation method(HP)and used to produce ethylene glycol(EG)through dimethyl oxalate(DMO)*** states for zirconia on copper catalyst and roles in DMO hydrogenation were investigated through various characterization tools,including N2 physical adsorption,XRD,H2-TPR,Methyl glycolate-TPD-MS,XPS,XAES as *** with common ammonia evaporation and co-precipitation methods used in catalyst preparation,this HP method is found to effectively suppress the agglomeration and further size growth of copper nanoparticles by enhancing the interactions between copper and zirconia *** importantly,uniform distribution of ZrO2 dopant is achieved due to the pseudo-homogeneous reactions in the mixing step of catalyst preparation.A proper amount of zirconium dopant helps achieve the desirable proportion of Cu+/(Cu++CuO)for surface copper species,especially promotes the production of Cu+species originated from Cu-ZrO2 species at the interface of copper and zirconia *** comparison with Cu+species formed from copper phyllosilicates reduction,the Cu+sites derived from Cu-ZrO2 species show higher adsorption ability of MG,an important intermediate species in ethylene glycol *** adsorbed MG molecules further react with atomic hydrogen shifted from adjacent metallic copper surface,leading to a higher catalytic *** the EG production via DMO hydrogenation,the turnover frequency(TOF)normalized by CuO species on CuZr/SiO2 catalyst is 1.8 times than that of traditional Cu/SiO2 *** to the enhanced synergy effect between Cu+and Cuo active sites,a lower activation energy of ester hydrogenation on this ZrO2-doped Cu/SiO2 catalyst is believed to be responsible for the significant improvement.