Ma Ye, Hu Junyi, Fan Kai, Chen Wei, Han Shichao, Wu Qinming, Ma Yanhang, Zheng Anmin, Kunkes Eduard, De Baerdemaeker Trees, Parvulescu Andrei-Nicolae, Bottke Nils, Yokoi Toshiyuki, De Vos Dirk E, Meng Xiangju, Xiao Feng-Shou
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
School of Physical Science and Technology & Shanghai Key Laboratory of High-resolution Electron Microscopy, ShanghaiTech University, Shanghai 201210, China.
J Am Chem Soc. 2023 Aug 9;145(31):17284-17291. doi: 10.1021/jacs.3c04652. Epub 2023 Jul 25.
Germanosilicate zeolites with various structures have been extensively synthesized, but the syntheses of corresponding zeolite structures in the absence of germanium species remain a challenge. One such example is an ITR zeolite structure, which is a twin of the ITH zeolite structure. Through the modification of a classic organic template for synthesizing ITH zeolites and thus designing a new organic template with high compatibility to ITR zeolite assisted by theoretical simulation, we, for the first time, show the Ge-free synthesis of an ITR structure including pure silica, aluminosilicate, and borosilicate ITR zeolites. These materials have high crystallinity, corresponding to an ITR content of more than 95%. In the methanol-to-propylene (MTP) reaction, the obtained aluminosilicate ITR zeolite exhibits excellent propylene selectivity and a long lifetime compared with conventional aluminosilicate ZSM-5 zeolite. The strategy for the design of organic templates might offer a new opportunity for rational syntheses of novel zeolites and, thus, the development of highly efficient zeolite catalysts in the future.
具有各种结构的锗硅酸盐沸石已被广泛合成，但在没有锗物种的情况下合成相应的沸石结构仍然是一个挑战。一个这样的例子是ITR沸石结构，它是ITH沸石结构的孪晶。通过对用于合成ITH沸石的经典有机模板进行改性，并在理论模拟的辅助下设计出与ITR沸石具有高兼容性的新型有机模板，我们首次展示了不含锗的ITR结构的合成，包括纯硅、铝硅和硼硅ITR沸石。这些材料具有高结晶度，对应的ITR含量超过95%。在甲醇制丙烯（MTP）反应中，与传统的铝硅ZSM-5沸石相比，所得的铝硅ITR沸石表现出优异的丙烯选择性和长寿命。有机模板的设计策略可能为合理合成新型沸石提供新的机会，从而在未来开发高效的沸石催化剂。
