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通过改进的溶胶-凝胶法制备的三维介孔钛硅酸盐:用于增强丙烯环氧化的理想金催化剂载体。

Three-dimensional mesoporous titanosilicates prepared by modified sol-gel method: Ideal gold catalyst supports for enhanced propene epoxidation.

作者信息

Sinha A K, Seelan S, Okumura M, Akita T, Tsubota S, Haruta M

机构信息

Special Division of Green Life Technology, AIST Kansai, Midorigaoka 1-8-31, Ikeda 563-8577, Japan.

出版信息

J Phys Chem B. 2005 Mar 10;109(9):3956-65. doi: 10.1021/jp0465229.

Abstract

Mesoporous titanosilicates with 1-12 mol % Ti content and with three-dimensional wormhole-like mesoporosity are prepared by a modified sol-gel technique. Sorption analysis shows that there is little change in the surface properties with increasing Ti concentration in the samples, implying that Ti atoms either are well-dispersed on the walls of the silica matrix or are present inside the framework with no pore blocking effect. Spectroscopic analysis shows that the Ti atoms are atomically dispersed in the silica matrix even at very high Ti concentration and there is no observable Ti aggregate (anatase) present in the samples. These titanosilicate samples after Au deposition followed by trimethylsilylation (for enhanced hydrophobicity) are highly efficient catalysts for vapor-phase propene epoxidation using O2 and H2. It was possible to achieve commercially desirable performance with about 7% propene conversion, >90% propene oxide selectivity, and about 40% hydrogen efficiency.

摘要

采用改进的溶胶-凝胶技术制备了钛含量为1-12摩尔%且具有三维蠕虫状介孔结构的介孔钛硅酸盐。吸附分析表明,随着样品中钛浓度的增加,表面性质变化不大,这意味着钛原子要么很好地分散在二氧化硅基质壁上,要么存在于骨架内部且无孔堵塞效应。光谱分析表明,即使在非常高的钛浓度下,钛原子也以原子形式分散在二氧化硅基质中,样品中没有可观察到的钛聚集体(锐钛矿)。这些钛硅酸盐样品在沉积金后进行三甲基硅烷化(以增强疏水性),是使用O2和H2进行气相丙烯环氧化的高效催化剂。使用约7%的丙烯转化率、>90%的环氧丙烷选择性和约40%的氢效率,可以实现商业上期望的性能。

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