Effect of physical mixing of CsCl with Au/Ti-MCM-41 on the gas-phase epoxidation of propene using H2 and O2:: Drastic depression of H2 consumption

被引:106
作者
Uphade, BS [1 ]
Okumura, M [1 ]
Tsubota, S [1 ]
Haruta, M [1 ]
机构
[1] Osaka Natl Res Inst, AIST, Ikeda, Osaka 5638577, Japan
基金
日本科学技术振兴机构;
关键词
epoxidation of propane; gold; Ti-MCM-41; promoter; CsCl;
D O I
10.1016/S0926-860X(99)00285-9
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Vapor-phase epoxidation of propene using H-2 and O-2 over Au/Ti-MCM-41 with or without a promoter has been investigated at various temperatures and at a space velocity of 4000 h(-1) ml/g (cat). As a promoter, CsCl was impregnated and/or physically (simple mixing) or mechanically (crushed in a mortar) mixed at various concentrations. The support, Ti-MCM-41 (Ti/Si = 3/100), was characterized by XRD, UV-Vis, FT-IR, and specific surface area measurement, whereas Au/Ti-MCM-41 with or without a promoter was characterized by TEM, XPS and ICP techniques before and/or after the catalytic tests. Au/Ti-MCM-41 as such gives propene and H-2 conversions of 3.1 and 47%, respectively, with a PO selectivity of 92% at the reaction temperature of 100 degrees C after 60 min of reaction. Physical mixing of CsCl with Au supported on Ti-MCM-41 reduces H-2 consumption by about 90% and improves propene oxide (PO) selectivity up to 97% at a propene conversion of 1.7%. One constraint is that agglomeration of gold particles is caused by Cl- anions: the mean diameter of Au particles, 2.2 nm, in Au/Ti-MCM-41 increases to about 10-20 nm and some clusters are; even larger than 50 nm in size due to direct contact between chloride and Au particles. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:43 / 50
页数:8
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