Core/shell-structured TS-1@mesoporous silica-supported Au nanoparticles for selective epoxidation of propylene with H2 and O2

Core/shell-structured TS-1@mesoporous silica-supported Au nanoparticles for selective epoxidation of propylene with H2 and O2
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核/壳结构TS-1@介孔二氧化硅负载Au纳米粒子用于丙烯与H2和O2的选择性环氧化

DOI:
10.1039/c1jm10483g
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发表时间:
2011-07
影响因子:
--
通讯作者:
Wu, Peng
Wu, Peng
中科院分区:
--
文献类型:
--
作者:
Wang, Zhendong;Xu, Jiajia;Peng, Honggen;Xu, Le;Liu, Yueming;Ren, Yingjie;Zhang, Yingtian;Wu, Haihong;Wu, Peng

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采用逐层法合成了具有核/壳结构的层次化有序材料。新型微孔/介孔杂化材料由以TS-1沸石为核、以介孔二氧化硅为壳组成。用聚二烯丙基二甲基氯化铵修饰TS-1晶体,使其外表面带正电荷,从而诱导正硅酸乙酯(TEOS)与十六烷基三甲基溴化铵在TS-1颗粒表面定向自组装,形成一层中间相二氧化硅壳层。通过改变合成中正硅酸乙酯的加入量,控制介孔二氧化硅壳层厚度在30~55 nm之间。壳层中的介孔通道垂直于沸石核,这使得核内的微孔可以从外部通过介孔进入。利用介孔的限制作用,金纳米粒子被引入到壳层中,形成了比传统的Au/TS-1催化剂更具选择性的双功能催化剂,用于丙烯与H2和O2的直接环氧化制环氧丙烷。
Hierarchically ordered materials with core/shell structures were synthesized through a layer-by-layer approach. The novel microporous/mesoporous hybrid materials were composed of a TS-1 zeolite particle for the core and mesoporous silica for the shell. The as-synthesized TS-1 crystals were modified with polydiallyldimethylammonium chloride to make their external surface positively charged, which induced an oriented self-assembly of tetraethoxysilane (TEOS) with cetyltrimethyl ammonium bromide on the TS-1 particle surface to form a shell of mesophase silica. The thickness of the mesoporous silica shell was controlled to be in the range 30–55 nm by changing the amount of TEOS added in the synthesis. The mesoporous channels in the shell were perpendicular to the zeolite core, which made the micropores inside the core accessible from the outside through the mesopores. Taking advantage of the confining effect of the mesopores, Au nanoparticles were incorporated into the shell, resulting in bifunctional catalysts which were more selective than conventional Au/TS-1 catalysts in the direct epoxidation of propylene to propylene oxide with H2 and O2.
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