A complex synthesis system consisting of multiple framework T atoms ([Si,Ge,Al] or [Si,Ge,B]) and a simple OSDA was designed to synthesize zeolites. The different framework T atoms were expected to trigger the formation of a diverse variety of building units and result in various framework structures, and the OSDA mainly plays a pore-filling role. In each case, the product was obtained as a complex polycrystalline powder, whose phase composition was then studied by SerialRED. SerialRED automatically screens hundreds of crystals on a TEM grid and collects a 3D ED dataset on each crystal. The unit cell parameters obtained from the 3D ED datasets of a large number of crystals were clustered and assigned to each zeolite phase (*CTH , *UOE, and so on) via HCA, where the Euclidean distances between the unit cell parameters were used as a metric. The diffraction intensities of the 3D ED datasets of each zeolite phase were then further clustered based on the correlations of their diffraction intensities. The datasets within the same cluster were merged and used for structure determination. The detailed phase and structural information allowed us to understand the correlations between the framework T atoms, building units and framework structures, which enables the rational development of zeolite materials.
