Synthesis and catalytic properties of TS-1 with mesoporous/microporous hierarchical structures obtained in the presence of amphiphilic organosilanes
Synthesis and catalytic properties of TS-1 with mesoporous/microporous hierarchical structures obtained in the presence of amphiphilic organosilanes
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DOI：
10.1016/j.jcat.2009.11.003
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发表时间：
2010-01-01
影响因子：
7.3
通讯作者：
Tuel, Alain
中科院分区：
文献类型：
--
作者：
Cheneviere, Yohan;Chieux, Frederic;Tuel, Alain
在有机硅烷表面活性剂存在下合成了具有介孔/微孔分级结构的钛硅酸盐TS-1。高度多孔的晶体，具有约约的规则孔隙。 2.5-3.5 nm 的直径是在类似于制备常规催化剂所用的水热条件下获得的。有机硅烷对TS-1的织构性能影响较大，但对骨架中Ti物种的数量和配位没有显着影响。介孔 TS-1 已被用作各种含水 H2O2 氧化反应的催化剂，并将其活性与传统 TS-1 和介孔无定形 TiMCM-41 的活性进行了比较。数据表明，介孔TS-1不具备分级催化剂的预期性能，即具有介孔固体优点的常规催化剂的性能。特别是，由于晶内介孔而产生的扩散增益完全被沸石亲水特性的增加所抑制，而沸石亲水特性的增加是由于外表面上非常高的硅烷醇基团数量造成的。 (c) 2009 Elsevier Inc. 保留所有权利。
Titanosilicates TS-1 with mesoporous/microporous hierarchical structures have been synthesized in the presence of an organosilane surfactant. Highly porous crystals, with regular pores of ca. 2.5-3.5 nm diameter, are obtained under hydrothermal conditions similar to those used for the preparation of conventional catalysts. The organosilane has a great influence on the textural properties of TS-1, but does not significantly affect the amount and coordination of Ti species in the framework. Mesoporous TS-1 have been used as catalysts in various oxidation reactions with an aqueous H2O2 and their activity has been compared with those of a conventional TS-1 and a mesoporous amorphous TiMCM-41. Data show that mesoporous TS-1 does not possess the expected properties for hierarchical catalysts, i.e. the properties of the conventional catalysts with advantages of mesoporous solids. In particular, the gain in diffusion due to intracrystalline mesopores is totally inhibited by the increase of the hydrophilic character of the zeolite, resulting from very high silanol group populations on the external surface. (c) 2009 Elsevier Inc. All rights reserved.