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

Abstract Silicoaluminophosphate (SAPO) zeolites are well-known catalytic materials because of the mild acidity originating from the isolated SiO4 tetrahedra in their frameworks. Regulating the distribution of isolated SiO4 tetrahedra in SAPO zeolites is formidably challenging because SiO4 tetrahedra tend to agglomerate to form Si islands and the isolated SiO4 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 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 SiO4 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 SiO4 tetrahedra in SAPO zeolites, which opens a new avenue in the discovery of promising zeolite catalysts with optimal SiO4 distribution.