Unraveling templated-regulated distribution of isolated SiO_(4) 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 

机构地区：[1]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,Jilin University,Changchun 130012,China [2]School of Textile and Clothing,Yancheng Institute of Technology,Yancheng 224000,China [3]State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics,National Center for Magnetic Resonance in Wuhan,Wuhan Institute of Physics and Mathematics,Innovation Academy for Precision Measurement Science and Technology,Chinese Academy of Sciences,Wuhan 430071,China [4]Australian Synchrotron,Clayton 3168,Australia [5]International Center of Future Science,Jilin University,Changchun 130012,China

出　　处：《National Science Review》2022年第9期14-22,共9页国家科学评论（英文版）

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)。

摘　　要：Silicoaluminophosphate(SAPO)zeolites are well-known catalytic materials because of the mild acidity originating from the isolated SiO_(4) tetrahedra in their frameworks.Regulating the distribution of isolated SiO_(4) tetrahedra in SAPO zeolites is formidably challenging because SiO_(4) tetrahedra tend to agglomerate to form Si islands and the isolated SiO_(4) tetrahedra 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 44697 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 SiO_(4) tetrahedra,which are responsible for the improvement in the chemical properties of zeolites.Our work provides an insight into the template-based regulation of isolated SiO_(4) tetrahedra in SAPO zeolites,which opens a new avenue in the discovery of promising zeolite catalysts with optimal SiO_(4) distribution.

关 键 词：ACIDITY computational chemistry heterogeneous catalysis structure-activity relationships zeolites 

分 类 号：TQ426[化学工程]