Postsynthesis of mesoporous MOR-type titanosilicate and its unique catalytic properties in liquid-phase oxidations

被引:76
|
作者
Xu, Hao [1 ]
Zhang, Yingtian [1 ]
Wu, Haihong [1 ]
Liu, Yueming [1 ]
Li, Xiaohong [1 ]
Jiang, Jingang [1 ]
He, Mingyuan [1 ]
Wu, Peng [1 ]
机构
[1] E China Normal Univ, Dept Chem, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
关键词
Titanosilicate; Mesopore; Mordenite; Postsynthesis; Liquid-phase oxidation; TS-1; MOLECULAR-SIEVE TS-1; HYDROGEN-PEROXIDE; TITANIUM SILICALITE; MWW STRUCTURE; DEALUMINATED MORDENITES; SELECTIVE OXIDATION; MFI ZEOLITE; ACID; TI; DESILICATION;
D O I
10.1016/j.jcat.2011.05.009
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
Mesoporous titanosilicate with the MOR topology, denoted as Ti-Meso-MOR, was postsynthesized from commercially available mordenite by sequential acid, alkaline, acid, and TiCl(4) vapor treatments, and its catalytic oxidation properties were investigated in detail in liquid-phase oxidation reactions with hydrogen peroxide as an oxidant. A controllable acid leaching was first carried out on H-mordenite (Si/Al = 7.8) to induce a partial dealumination to Si/Al = 80, which was suitable for constructing secondary mesopores by subsequent alkaline treatment. Alkaline treatment-induced desilication introduced a large number of intracrystal mesopores. Tetracoordinated Ti species were then inserted into the resultant mesoporous mordenite with a high dealumination degree (Si/Al = 145) through the gas-solid reaction with TiCl(4) vapor at elevated temperatures. In comparison with conventional Ti-MOR and TS-1, Ti-Meso-MOR thus prepared exhibited an improved catalytic activity in the hydroxylation of toluene and the ammoximation of cyclohexanone as well. Moreover, Ti-Meso-MOR proved to be a robust catalyst for continuous ammoximation since the mesopores minimized diffusion limitation and suppressed coke formation efficiently. (C) 2011 Elsevier Inc. All rights reserved.
引用
收藏
页码:263 / 272
页数:10
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