CO2 hydrogenation to methanol over Cu/CeO2 and Cu/ZrO2 catalysts:Tuning methanol selectivity via metal-support interaction  

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 of Sciences,Dalian 116023,Liaoning,China

出　　处：《Journal of Energy Chemistry》2020年第1期22-30,I0002,共10页能源化学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (21577014, 21876019, 21825203, 21688102);Programme of Introducing Talents of Discipline to Universities (B13012);the fund of the State Key Laboratory of Catalysis in DICP (Y401010502)

摘　　要：Copper-based catalysts for CO2 hydrogenation to methanol are supported on ZrO2 and CeO2,respectively.Reaction results at 3.0 MPa and temperatures between 200 and 300°C reveal that Cu catalysts supported on ZrO2 and CeO2 exhibit better activity and selectivity than pure Cu catalyst due to Cu-support(ZrO2 and CeO2)interaction.Combining the structural characterizations with in-situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS),Cu/CeO2 shows the higher methanol selectivity due to the formation of main carbonates intermediates,which are closely related with the oxygen vacancies over Cu/CeO2.In contrast,bicarbonate and carboxyl species are observed on Cu/ZrO2,which originates from the hydroxyl groups presented on catalyst surfaces.Difference in CO2 adsorption intermediates results in the distinct methanol selectivity over the two catalysts.Copper-based catalysts for CO2 hydrogenation to methanol are supported on ZrO2 and CeO2, respectively.Reaction results at 3.0 MPa and temperatures between 200 and 300 °C reveal that Cu catalysts supported on ZrO2 and CeO2 exhibit better activity and selectivity than pure Cu catalyst due to Cu-support（ZrO2 and CeO2） interaction. Combining the structural characterizations with in-situ diffuse reflectance infrared Fourier transform spectroscopy（in-situ DRIFTS）, Cu/CeO2 shows the higher methanol selectivity due to the formation of main carbonates intermediates, which are closely related with the oxygen vacancies over Cu/CeO2. In contrast, bicarbonate and carboxyl species are observed on Cu/ZrO2, which originates from the hydroxyl groups presented on catalyst surfaces. Difference in CO2 adsorption intermediates results in the distinct methanol selectivity over the two catalysts.

关 键 词：CO_2 hydrogenation Methanol selectivity In-situ DRIFTS CeO_2 ZrO_2 

分 类 号：O643.36[理学—物理化学] O623.411[理学—化学]