Direct gas-phase epoxidation of propylene to propylene oxide using air as oxidant on supported gold catalyst

作     者：Zhanghuai Suo Mingshan Jin Jiqing Lu Zhaobin Wei Can Li 

作者机构：Institute of Applied Catalysis Yantai University Yantai 264005 Shandong China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 Liaoning China 

出 版 物：《Journal of Natural Gas Chemistry》 (天然气化学杂志（英文版）)

年 卷 期：2008年第17卷第2期

页      面：184-190页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基　　金：The Natural Science Foundation of China (No.20273057 20473070) 

主　　题：gold catalyst support modified impregnation method epoxidation of propylene molecular oxygen 

摘      要：Gold catalysts supported on SiO2, TiO2, TiO2-SiO2, and ZrO2-SiO2 supports were prepared by impregnating each support with a basic solution of tetrachloroauric acid. X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and X-ray photoelectron spectroscopy （XPS） techniques were used to characterize their structure and surface composition. The results indicated that the size of gold particles could be controlled to below 10 nm by this method of preparation. Washing gold catalysts with water could markedly enhance the dispersion of metallic gold particles on the surface, but it could not completely remove the chloride ions left on the surface. The catalytic performance of direct vapor-phase epoxidation of propylene using air as an oxidant over these catalysts was evaluated at atmospheric pressure. The selectivity to propylene oxide （PO） was found to vary with reaction time on the stream. At the reaction conditions of atmosphere pressure, temperature 325 ℃, feed gas ratio V（C3H6）/V（O2）= 1/2, and GHSV =6000h^-1, 17.9% PO selectivity with 0.9% propylene conversion were obtained at initial 10 min for Au/SiO2 catalyst. After reacting 60 min only 8.9% PO selectivity were detected, but the propylene conversion rises to 1.4% and the main product is transferred to acrolein （72% selectivity）. Washing Au/TiO2-SiO2 and Aa/ZrO2-SiO2 samples with magnesium citrate solution could markedly enhance the activity and PO selectivity because smaller gold particles were obtained.