Crystallization of a Novel Germanosilicate ECNU-16 Provides Insights into the Space-Filling Effect on Zeolite Crystal Symmetry
Crystallization of a Novel Germanosilicate ECNU-16 Provides Insights into the Space-Filling Effect on Zeolite Crystal Symmetry
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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
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发表时间：
2018
期刊：
影响因子：
--
通讯作者：
Wu Peng
中科院分区：
文献类型：
--
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
涉及有机分子的新沸石的合成在很大程度上依赖于试错法，因为很难解释有机物对沸石晶体对称性的决定性影响。在这里，有机物的空间填充，包括通道的体积和沸石晶体对称性之间的内在关系，通过实验和计算手段系统地证明。在受控条件下，1-乙基-3-甲基咪唑鎓的“二聚体”和“单体”有机物分别选择性地引导不同但相关的锗硅酸盐、具有新拓扑结构的ECNU-16和具有UOS拓扑结构的现有IM-16。全面的计算研究表明，沸石相选择性是由“二聚体”和“单体”有机物的独特空间填充行为决定的，这与它们的旋转自由度以及主体沸石通道的包含体积密切相关。从基本观点阐明这种关键的空间填充效应将为今后合理设计和合成新型沸石分子筛提供新的指导。
Synthesis of new zeolites involving organic molecules relies heavily on the trial‐and‐error approach, because it is difficult to interpret the determining effects of organics on zeolite crystal symmetry. Here, the intrinsic relationships among the space‐filling of organics, included volume of channels, and zeolite crystal symmetry, are systematically demonstrated by experimental and computational means. 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 reveals that the zeolite phase selectivity is determined by the unique space‐filling behavior of the “dimer” and “monomer” organics, which is closely correlated to their rotation freedom, as well as the included volume of host zeolite channels. The elucidation of this crucial space‐filling effect from the fundamental viewpoint will provide new guidelines for the rational design and synthesis of new zeolites in future.