An investigation of Zr/Ce ratio influencing the catalytic performance of CuO/Ce1-xZrxO2 catalyst for CO2 hydrogenation to CH3OH  

作　　者：Weiwei Wang Zhenping Qu Lixin Song Qiang Fu 

机构地区：[1]Key Laboratory of Industrial Ecology and Environmental Engineering,School of Environmental Science and Technology,Dalian University of Technology,Dalian 116024,Liaoning,China [2]State Key Lab of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy Sciences,Dalian 116023,Liaoning,China

出　　处：《Journal of Energy Chemistry》2020年第8期18-28,I0002,共12页能源化学（英文版）

基　　金：financially supported by the National Nature Science Foundation of China (21876019, 21577014);Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020000);the fund of the State Key Laboratory of Catalysis in DICP (N18-08)。

摘　　要：A series of CuO/Ce1-xZrxO2 catalysts(x=0.2,0.4,0.6 and 0.8)are applied to elaborate the effect of the Zr/Ce ratio on the catalytic performance of CO2 hydrogenation to CH3OH.The best catalytic performance is achieved with CuO/Ce0.4Zr0.6O2,exhibiting XCO2=13.2%and YCH3OH=9.47%(T=280℃,P=3 MPa).The formation of dispersed surface CuO species and larger number of oxygen vacancies are detected over CuO/Ce0.4Zr0.6O2 due to stronger interaction between CuO and Ce0.4Zr0.6O2,resulting in the superior activation ability for H2 and CO2 respectively.Additionally,the evidence is provided by in situ DRIFTS under the activity test pressure(3 MPa)that bi/m-HCOO* species are preferable for accumulating over ceria-rich(CuO/Ce0.6Zr0.4O2 and CuO/Ce0.8Zr0.2O2)catalysts while zirconia-rich(CuO/Ce0.4Zr0.6O2 and CuO/Ce0.2Zr0.8O2)catalysts are benefit to encourage the transformation of bi/m-HCOO* species to CH3OH.The abundant population and high activity of intermediate species over CuO/Ce0.4Zr0.6O2 give a strong positive effect on the catalytic performance.

关 键 词：CO2 hydrogenation Ce1-xZrxO2 m-HCOO^* bi-HCOO^* in-situ DRIFTS 

分 类 号：O621.251[理学—有机化学] O623.411[理学—化学]