二次元ナノ構造をもつゼオライトの合成と触媒応用

首先，本文重点研究了不同晶体对称性元素对沸石层堆积的控制。在受控条件下，1-乙基-3-甲基咪唑的“二聚体”和“单体”有机物分别选择性地与具有新拓扑结构的ECNU-16和具有UOS拓扑结构的现有IM-16直接作用于不同但相关的锗硅酸盐。基于分子力学模拟的综合计算研究表明，沸石相选择性取决于“二聚体”和“单体”有机物独特的空间填充行为，这与它们的旋转自由度以及主体沸石通道的包裹体体积密切相关；另一方面，本研究发现了一种通过三维(3D)锗硅酸盐UTL实现不同片状沸石前驱体(FER-型和PCR型)之间拓扑转化的Ge回收策略。这种Ge回收过程的发现使片状沸石前驱体从一种结构切换到另一种结构，这两种结构都可以进一步从不同的沸石衍生出来。这项研究不仅在结构上不同的片状沸石之间建立了新的联系，而且在两类沸石材料之间建立了新的联系。

First, the control of the zeolitic layer stacking with different crystal symmetry elements was focused in this research. Under controlled conditions, the “dimer” and “monomer” organics of 1-ethyl-3-methylimidazolium selectively direct different, but related, germanosilicates, the ECNU-16 with a new topology and the existing IM-16 with the UOS topology, respectively. The comprehensive computational study based on the molecular mechanic simulations revealed that the zeolite phase selectivity was determined by the unique space-filling behavior of the “dimer” and “monomer” organics, which was closely correlated with their rotation freedom, as well as the included volume of host zeolite channels.On the other hand, a Ge-recycling strategy that realized the topotatic transformation between different lamellar zeolitic precursors (fer-type and pcr-type) through three-dimensional (3D) germanosilicate UTL was discovered in this research. The discovery of this Ge-recycling process enabled to switch the lamellar zeolitic precursor from one structure to the other, both of which could be further derived of diverse zeolites. This study established new relationships not only between structurally distinct lamellar zeolites but also two families of zeolitic materials.