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多面体和桥联硅倍半氧烷单体组装的杂化介孔材料的合成与催化性能。

Synthesis and catalytic properties of hybrid mesoporous materials assembled from polyhedral and bridged silsesquioxane monomers.

机构信息

Instituto de Tecnología Química (UPV-CSIC), Universidad Politécnica de Valenica, Avenida de los Naranjos s/n, 46022 Valencia, Spain.

出版信息

Chemistry. 2012 Jul 9;18(28):8659-72. doi: 10.1002/chem.201200170. Epub 2012 Jun 8.

Abstract

A family of hybrid mesoporous materials with high temperature stability was obtained by the suitable covalent combination of two types of siloxane precursors. Specifically, cubic T(8) polyhedral oligomeric (POSS) and aryl bridged silsesquioxane monomers (1,4-bis(triethoxysilyl)benzene, BTEB) play the role of nanobuilders. An optimal molar ratio of the two precursors (5-25 mol% of total silicon content from the BTEB disilane) generated a homogenous, highly accessible, and well-defined mesoporous material with hexagonal symmetry and narrow pore-size distribution. Physicochemical, textural, and spectroscopic analysis corroborated the effective integration and preservation of the two different nanoprecursors, thereby confirming the framework of the mesoporous hybrid materials. A post-synthesis amination treatment allowed the effective incorporation of amino groups onto the aryl linkers, thereby obtaining a stable and recyclable basic catalyst for use in C-C bond-formation processes.

摘要

通过两种类型的硅氧烷前体的适当共价结合,获得了具有高温稳定性的混合介孔材料家族。具体来说,立方 T(8) 多面体低聚硅氧烷(POSS)和芳基桥联硅倍半氧烷单体(1,4-双(三乙氧基硅基)苯,BTEB)充当纳米构建块。两种前体的最佳摩尔比(BTEB 二硅烷总硅含量的 5-25 mol%)生成了具有六方对称性和窄孔径分布的均匀、高可及性和明确定义的介孔材料。物理化学、结构和光谱分析证实了两种不同纳米前体的有效整合和保留,从而证实了介孔混合材料的框架。后合成的氨化处理允许氨基有效地结合到芳基连接物上,从而获得了用于 C-C 键形成过程的稳定和可回收的碱性催化剂。

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