A series of palladium-modified(Pd-modified)CuO-ZnO-Al_(2)O_(3)(CZA)catalysts with various Pd loadings(0.3 wt%to 2.4 wt%)were prepared using the wetness impregnation method,on two CZA supports with different structures...A series of palladium-modified(Pd-modified)CuO-ZnO-Al_(2)O_(3)(CZA)catalysts with various Pd loadings(0.3 wt%to 2.4 wt%)were prepared using the wetness impregnation method,on two CZA supports with different structures that are CZA-aged precursor composed of a mixture of zincian-malachite and hydrotalcite-like phases(CZA-zH),and CuO-ZnO-Al_(2)O_(3)metal oxide nanoparticles(CZA-MO).Enhancement on catalytic activity can be observed on both Pd-modified CZA catalysts in a temperature range of 180-240℃for methanol synthesis via CO_(2)hydrogenation.Pd/CZA-zH catalysts exhibited a more efficient and stable production of methanol at a relatively low reaction temperature of 180℃for 100 hrs of reaction.The improvement of activity is mainly ascribed to a higher surface area and abundant oxygen-containing functional groups(e.g.,-OH)of CZA-zH support,which is beneficial for better adsorption and distribution of Pd promoter.Hydrogen temperature programmed reduction and X-ray photoelectron spectroscopy results demonstrated a better interaction between Pd and Cu on Pd/CZA-zH catalysts via enhanced reducibility of CuO,and peak shift of Cu to a lower binding energy.The difference in the efficient utilization of hydrogen spillover effect of Pd promoter over two CZA supports resulted in the different performances for methanol synthesis under mild reaction co℃nditions.展开更多
基金supported in part by the U.S.Department of Energy through contracts DE-FE0031909 and DE-FE0031909.
文摘A series of palladium-modified(Pd-modified)CuO-ZnO-Al_(2)O_(3)(CZA)catalysts with various Pd loadings(0.3 wt%to 2.4 wt%)were prepared using the wetness impregnation method,on two CZA supports with different structures that are CZA-aged precursor composed of a mixture of zincian-malachite and hydrotalcite-like phases(CZA-zH),and CuO-ZnO-Al_(2)O_(3)metal oxide nanoparticles(CZA-MO).Enhancement on catalytic activity can be observed on both Pd-modified CZA catalysts in a temperature range of 180-240℃for methanol synthesis via CO_(2)hydrogenation.Pd/CZA-zH catalysts exhibited a more efficient and stable production of methanol at a relatively low reaction temperature of 180℃for 100 hrs of reaction.The improvement of activity is mainly ascribed to a higher surface area and abundant oxygen-containing functional groups(e.g.,-OH)of CZA-zH support,which is beneficial for better adsorption and distribution of Pd promoter.Hydrogen temperature programmed reduction and X-ray photoelectron spectroscopy results demonstrated a better interaction between Pd and Cu on Pd/CZA-zH catalysts via enhanced reducibility of CuO,and peak shift of Cu to a lower binding energy.The difference in the efficient utilization of hydrogen spillover effect of Pd promoter over two CZA supports resulted in the different performances for methanol synthesis under mild reaction co℃nditions.
基金supported by the National Natural Science Foundation of China (U21A20496,61922060,62205235,62204157,61805172,12104334,62174117,and 61905173)the Graduate Innovation Project of Shanxi Province (2020BY117)+9 种基金the Key Research and Development (International Cooperation)Program of Shanxi Province (201803D421044)the Natural Science Foundation of Shanxi Province (20210302123154 and 20210302123169)Research Project Supported by Shanxi Scholarship Council of China (2021-033)Research Project Supported by Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering (2021SX-FR008 and 2022SX-TD020)Introduction of Talents Special Project of Lvliang City (Rc2020206,Rc2020207)Transformation Cultivation Project of University Scientific and Technological Achievements of Shanxi Province (2020CG013)the Key Research and Development Program of Shanxi Province (202102150101007)the support from the Research Grants Council,University Grants Committee,Hong Kong,General Research Fund (12303920)SZ-HK-Macao Science and Technology Plan Project (SGDX2020110309540000)Guangdong Basic and Applied Basic Research Fund (2022A1515010020)。
