Unraveling templated-regulated distribution of isolated SiO4 tetrahedra in silicoaluminophosphate zeolites with high-throughput computations

作     者：Yan Li Chao Shi Lin Li Guoju Yang Junyan Li Jun Xu Qinfen Gu Xingxing Wang Ji Han Tianjun Zhang Yi Li Jihong Yu 

作者机构：State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University School of Textile and Clothing Yancheng Institute of Technology State Key Laboratory of Magnetic Resonance and Atomic and Molecular PhysicsNational Center for Magnetic Resonance in Wuhan Wuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of Sciences Australian Synchrotron International Center of Future ScienceJilin University 

出 版 物：《National Science Review》 (国家科学评论(英文版))

年 卷 期：2022年第9卷第9期

页      面：19-27页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the National Key Research and Development Program of China (2021YFA1501202) the National Natural Science Foundation of China (21920102005, 21835002,22175073 and 21621001) the Overseas Expertise Introduction Project for Discipline Innovation (111 Project, B17020) 

主　　题：acidity computational chemistry heterogeneous catalysis structure–activity relationships zeolites 

摘      要：Silicoaluminophosphate(SAPO) zeolites are well-known catalytic materials because of the mild acidity originating from the isolated SiO4tetrahedra in their frameworks. Regulating the distribution of isolated SiO4tetrahedra in SAPO zeolites is formidably challenging because SiO4tetrahedra tend to agglomerate to form Si islands and the isolated SiO4tetrahedra are difficult to determine using conventional characterization techniques. Here we synthesized Si-island-free SAPO-35 zeolites by using N-methylpiperidine as a new template, which exhibited excellent thermal stability compared to conventional SAPO-35 zeolites and a substantially improved methanol-to-olefins catalytic lifetime even comparable to that of commercial SAPO-34 zeolites. More strikingly, with the aid of high-throughput computations on 44 697 structure models combined with various state-of-the-art characterization techniques, for the first time, we reveal that the host–guest interactions between template molecules and SAPO frameworks determine the specific distributions of isolated SiO4tetrahedra, which are responsible for the improvement in the chemical properties of zeolites. Our work provides an insight into the template-based regulation of isolated SiO4tetrahedra in SAPO zeolites, which opens a new avenue in the discovery of promising zeolite catalysts with optimal Si O4distribution.