二次元ナノ構造をもつゼオライトの合成と触媒応用

二维纳米结构沸石的合成及催化应用

• 批准号: 17F17083
• 负责人: 大久保 達也
• 金额: $ 1.47万
• 依托单位: The University of Tokyo
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for JSPS Fellows
• 财政年份: 2017
• 资助国家: 日本
• 起止时间: 2017-04-26 至 2019-03-31
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-17F17083/
• 关键词: layered zeolite; Layered zeolite; zeolite structure; structure transformation

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.

首先，重点研究了不同晶体对称元对沸石层堆积的控制。在控制条件下，1-乙基-3-甲基咪唑的“二聚体”和“单体”有机物选择性地引导不同但相关的锗硅酸盐，ECNU-16具有新的拓扑结构，IM-16具有UOS拓扑结构。基于分子力学模拟的综合计算研究表明，沸石的相选择性是由“二聚体”和“单体”有机物独特的空间填充行为决定的，这种行为与它们的旋转自由度以及宿主沸石通道的包含体积密切相关。另一方面，本研究发现了一种通过三维（3D）锗硅酸盐UTL实现不同层状沸石前驱体（fe型和pcr型）之间拓扑转换的ge回收策略。这种锗循环过程的发现使层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衍生出不同的沸石。该研究不仅在结构上不同的层状沸石之间建立了新的关系，而且在沸石材料的两个家族之间建立了新的关系。

项目成果

Crystallization of a Novel Germanosilicate ECNU-16 Provides Insights into the Space-Filling Effect on Zeolite Crystal Symmetry

新型德国硅酸盐 ECNU-16 的结晶提供了对沸石晶体对称性的空间填充效应的见解

• DOI: 10.1002/chem.201802087
• 发表时间: 2018
• 期刊: Chemistry - A European Journal
• 作者: Xu Le;Zhang Lin;Li Jian;Muraoka Koki;Peng Fei;Xu Hao;Lin Cong;Gao Zihao;Jiang Jin Gang;Chaikittisilp Watcharop;Sun Junliang;Okubo Tatsuya;Wu Peng
• 通讯作者: Wu Peng

255th American Chemical Society Meeting and exposition

第 255 届美国化学会会议暨博览会

• 发表时间: 2018