Preparation and catalytic performances of ultralarge-pore TiSBA-15 mesoporous molecular sieves with very high Ti content

被引:98
作者
Vinu, A
Srinivasu, P
Miyahara, M
Ariga, K
机构
[1] NIMS, ICYS, Tsukuba, Ibaraki 3050044, Japan
[2] Yokohama Natl Univ, Div Mat Sci & Chem Engn, Yokohama, Kanagawa 2408501, Japan
[3] NIMS, AML, Supermol Grp, Tsukuba, Ibaraki 3050044, Japan
关键词
D O I
10.1021/jp055851d
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
Highly ordered TiSBA-15 mesoporous molecular sieves with different n(Si)/n(Ti) ratios and tunable pore diameters have been prepared through direct synthesis under various hydrochloric acid concentrations and synthetic temperatures. The structure and the textural parameters of the materials were investigated by powder X-ray diffraction and nitrogen adsorption/desorption measurements. Decrease of the acid concentration and nSi/nTi ratio in the synthetic gel enhanced the amount of Ti incorporation in SBA-15 materials without affecting their structural order and textural parameters. Highly ordered mesoporous TiSBA-15 with a very high Ti content up to a n(Si)/n(Ti) ratio of 1.9 was prepared for the first time under the optimized synthesis conditions. Control of synthetic temperature resulted in tuning of pore geometries without structural deterioration and Ti content. Ultralarge-pore TiSBA-15 with a pore size of 12.6 nm and a pore volume of 1.3 cm(3) g(-1) was also synthesized. The nature and the coordination of the Ti atoms in SBA-15 prepared under various synthesis conditions were investigated by UV-vis spectroscopy. It has been found that the Ti atoms are well-dispersed and mostly occupy the tetrahedral coordination under the optimized synthesis conditions. Catalytic performance of the obtained TiSBA-15 materials was also investigated through oxidation of styrene by hydrogen peroxide and tert-butylhydroperoxide as oxidants.
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页码:801 / 806
页数:6
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