Xu Le, Choudhary Madhuresh K, Muraoka Koki, Chaikittisilp Watcharop, Wakihara Toru, Rimer Jeffrey D, Okubo Tatsuya
Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan.
Department of Chemical and Biomolecular Engineering, University of Houston, Houston, TX, 77204, USA.
Angew Chem Int Ed Engl. 2019 Oct 7;58(41):14529-14533. doi: 10.1002/anie.201907857. Epub 2019 Sep 5.
There is broad scientific interest in lamellar zeolitic materials for a large variety of technological applications. The traditional synthetic methods towards two-dimensional (2D) zeolitic precursors have made a great impact in the construction of families of related zeolites; however, the connection between structurally distinct 2D zeolitic precursors is much less investigated in comparison, thereby resulting in a synthetic obstacle that theoretically limits the types of zeolites that can be constructed from each layer. Herein, we report a Ge-recycling strategy for the topotactic conversion between different 2D zeolitic precursors through a three-dimensional (3D) germanosilicate. Specifically, the intermediate germanosilicate can be constructed within 150 min by taking advantage of its structural similarity with the parent lamellar precursor. This process enables the conversion of one 2D zeolite structure into another distinct structure, thus overcoming the synthetic obstacle between two families of zeolitic materials.
层状沸石材料因其在众多技术应用中的广泛用途而引发了科学界的浓厚兴趣。传统的二维（2D）沸石前驱体合成方法对相关沸石家族的构建产生了重大影响；然而，相比之下，结构不同的二维沸石前驱体之间的联系研究较少，从而导致了一个合成障碍，从理论上限制了可由每层构建的沸石类型。在此，我们报告了一种通过三维（3D）锗硅酸盐实现不同二维沸石前驱体之间拓扑转化的锗循环策略。具体而言，利用中间锗硅酸盐与母体层状前驱体的结构相似性，可在150分钟内构建出该中间锗硅酸盐。这一过程能够将一种二维沸石结构转化为另一种不同的结构，从而克服了两类沸石材料之间的合成障碍。
