Division of Materials and Manufacturing Science, Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan.
Phys Chem Chem Phys. 2013 Aug 28;15(32):13323-8. doi: 10.1039/c3cp51022k.
Aluminum-containing mesoporous silica with hierarchical macroporous architecture (Al-MMS) was successfully prepared using a solvent evaporation method through the combination of precursor solution for synthesis of Al-containing mesoporous silica (Al-MS) and poly(methyl methacrylate) (PMMA) colloidal crystals as a hard template. The porous structure and the state of aluminum were investigated using various characterization techniques. The construction of combined structure of Al-MMS, i.e., hierarchical macroporous architecture consisting of thin mesoporous silica frameworks, led to the formation of many mesopore entrances and the shortening of the mesoporous channels. In the tetrahydropyranylation of linear alcohols with dihydropyran (DHP), Al-MMS exhibited higher catalytic activities for the formation of corresponding tetrahydropyranyl ethers as compared to Al-MS. The advantageous structure of Al-MMS enables the efficient transport of reactants to the catalytically active sites, which realizes the significant enhancement of catalytic performances in the reaction of DHP with alcohols having longer alkyl chains.
采用溶剂挥发法，通过将含铝介孔硅前体溶液与聚甲基丙烯酸甲酯（PMMA）胶体晶体相结合，成功制备出具有分级大孔结构的含铝介孔硅（Al-MMS）。采用多种表征技术对多孔结构和铝的状态进行了研究。Al-MMS 的组合结构（由薄介孔硅骨架组成的分级大孔结构）的构建导致了许多介孔入口的形成和介孔通道的缩短。在以线性醇和二氢吡喃（DHP）为原料合成相应的四氢吡喃醚的反应中，Al-MMS 表现出比 Al-MS 更高的催化活性。Al-MMS 的有利结构能够将反应物有效地输送到催化活性位点，从而实现了在具有较长烷基链的醇与 DHP 的反应中催化性能的显著提高。
