Unique solvent effect of microporous crystalline titanosilicates in the oxidation of 1-hexene and cyclohexene

被引:155
作者
Fan, Weibin [1 ,2 ]
Wu, Peng [3 ]
Tatsumi, Takashi [1 ]
机构
[1] Tokyo Inst Technol, Chem Resources Lab, Catalyt Chem Div, Midori Ku, Yokohama, Kanagawa 2268503, Japan
[2] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
[3] E China Normal Univ, Dept Chem, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
基金
日本学术振兴会; 日本科学技术振兴机构;
关键词
cyclohexene; 1-hexene; oxidation; solvent effect; Ti-beta; Ti-MWW; TS-1; titanosilicate;
D O I
10.1016/j.jcat.2008.03.001
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
We investigated the influence of solvent on the activity, epoxide selectivity, and H2O2 efficiency of three types of zeolites-TS-1, Ti-Beta, and Ti-MWW-in the liquid-phase epoxidation of 1-hexene and cyclohexene. We found that the effect of solvent not only was related to the hydrophilicity/hydrophobicity of titanosilicates, but also was highly dependent on substrates. Acetonitrile should be the solvent of choice for the oxidation of 1-hexene over Ti-Beta and Ti-MWW, whereas methanol is preferred by TS-1. In contrast, for cyclohexene oxidation, methanol is favorable for Ti-Beta, whereas acetonitrile is the best for TS-1 and Ti-MWW. The effect of hydrophilicity/hydrophobicity is demonstrated by a series of catalytic results, but this cannot explain the solvent effect on the oxidation of cyclohexene over Ti-Beta. The H2O2 efficiency depends strongly on the aprotic/protic nature and polarity of solvents, as well as on the properties of titanosilicates. (C) 2008 Elsevier Inc. All rights reserved.
引用
收藏
页码:62 / 73
页数:12
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