Mechanism and catalytic performance for direct dimethyl ether synthesis by CO2 hydrogenation over CuZnZr/ferrierite hybrid catalyst  

作　　者：Qingtao Sheng Run-Ping Ye Weibo Gong Xiufeng Shi Bang Xu Morris Argyle Hertanto Adidharma Maohong Fan 

机构地区：[1]College of Chemistry and Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,China [2]Department of Engineering and Applied Science,University of Wyoming,Laramie,WY 82071,USA [3]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fujian 350002,China [4]University of Chinese Academy of Sciences,Beijing 100049,China [5]Institute of Engineering Thermophysics,Chinese Academy of Sciences,Beijing 100190,China [6]Department of Chemical Engineering,Brigham Young University,UT 84602,USA [7]Department of Petroleum Engineering,University of Wyoming,Laramie,WY 82071,USA [8]School of Energy Resources,University of Wyoming,Laramie,WY 82071,USA [9]School of Civil and Environmental Engineering,Georgia Institute of Technology,Atlanta,GA 30332,USA

出　　处：《Journal of Environmental Sciences》2020年第6期106-117,共12页环境科学学报（英文版）

基　　金：supported by the China Scholarship Council(No.201608140182);the University of Wyoming;and State of Wyoming。

摘　　要：Direct synthesis of dimethyl ether(DME)by CO2 hydrogenation has been investigated over three hybrid catalysts prepared by different methods:co-precipitation,sol-gel,and solid grinding to produce mixed Cu,ZnO,ZrO2 catalysts that were physically mixed with a commercial ferrierite(FER)zeolite.The catalysts were characterized by N2 physisorption,X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),temperature programmed desorption of CO2(CO2-TPD),temperature programmed desorption of NH3(NH3-TPD),and temperature programmed H2 reduction(H2-TPR).The results demonstrate that smaller CuO and Cu crystallite sizes resulting in better dispersion of the active phases,higher surface area,and lower reduction temperature are all favorable for catalytic activity.The reaction mechanism has been studied using in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).Methanol appears to be formed via the bidentate-formate(b-HCOO)species undergoing stepwise hydrogenation,while DME formation occurs from methanol dehydration and reaction of two surface methoxy groups.

关 键 词：CO2 hydrogenation ETHER Dimethyl ether(DME)synthesis MECHANISM 

分 类 号：X701[环境科学与工程—环境工程] TQ223.24[化学工程—有机化工]