Pd-modified CuO-ZnO-Al_(2)O_(3)catalysts via mixed-phases-containing precursor for methanol synthesis from CO_(2)hydrogenation under mild conditions  

作　　者：Xiao Fan Kaiying Wang Xiaoqing He Shiguang Li Miao Yu Xinhua Liang 

机构地区：[1]Linda and Bipin Doshi Department of Chemical and Biochemical Engineering,Missouri University of Science and Technology,Rolla,MO 65409,United States [2]Department of Energy,Environmental and Chemical Engineering,Washington University in St.Louis,St.Louis,MO 63130,United States [3]Electron Microscopy Core Facility,University of Missouri,Columbia,MO 65211,United States [4]Department of Mechanical and Aerospace Engineering,University of Missouri,Columbia,MO 65211,United States [5]Gas Technology Institute,1700 South Mount Prospect Road,Des Plaines,IL 60018,United States [6]Department of Chemical and Biological Engineering,University at Buffalo,Buffalo,NY 14260,United States

出　　处：《Carbon Resources Conversion》2024年第1期10-20,共11页碳资源转化（英文）

基　　金：supported in part by the U.S.Department of Energy through contracts DE-FE0031909 and DE-FE0031909.

摘　　要：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.

关 键 词：CO_(2)hydrogenation Low-temperature methanol synthesis Pd-modification CuO-ZnO-Al_(2)O_(3) Hydrogen spillover 

分 类 号：O643[理学—物理化学]