Vapor phase propylene epoxidation over Au/Ti-MCM-41 catalysts prepared by different Ti incorporation modes

被引:123
作者
Sinha, AK
Seelan, S
Akita, T
Tsubota, S
Haruta, M
机构
[1] AIST, Res Inst Green Technol, Tsukuba, Ibaraki 3058569, Japan
[2] Natl Res Inst Adv Ind Sci & Technol, Special Div Green Life Technol, Ikeda, Osaka 5638577, Japan
基金
日本科学技术振兴机构;
关键词
epoxidation; propene; propene oxide; gold; Ti-MCM-41; Ti grafting;
D O I
10.1016/S0926-860X(02)00451-9
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
Ti-containing MCM-41 supports were prepared by: (a) hydrothermal crystallization; (b) post-synthesis grafting; and (c) two-step Ti incorporation-hydrothermal incorporation followed by post-synthesis grafting. XRD revealed little change in crystallinity and long range order of MCM-41 phase after Ti incorporation by different methods. UV-Vis spectra show the presence of tetrahedral Ti sites at lower Ti contents (upto 4.5 mol%), but aggregated titania formation could be observed at higher Ti loadings (>4.5 mol%). The samples exhibit surface areas and pore volumes in the mesoporous range. Vapor phase epoxidation of propene using H-2 and O-2 was carried out over these supports after Au deposition by deposition-precipitation (DP) method. The Ti-MCM-41 supports prepared by two-step Ti incorporation (with up to 4.5 mol% input Ti), which probably have more number of isolated Ti sites, showed higher catalytic activity than Ti-MCM-41 prepared by one-step Ti incorporation method, at comparable propylene oxide selectivities and hydrogen efficiencies. The former catalyst also deactivates more slowly than the latter ones, probably due to a decrease in the number of silanol sites (those responsible for deactivation) due to grafted Ti. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:243 / 252
页数:10
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