Observing a Zeolite Nucleus (Subcrystal) with a Uniform Framework Structure and Its Oriented Attachment without Single‐Molecule Addition

Multiple and complex crystallization process of zeolite including complementary single‐molecule condensation and particle assembly, and alternately dominant nucleation and growth behavior, plays the critical role in zeolite crystallization but meanwhile makes us hard to study the respective effects. Herein, we strip nuclei from the synthetic solution and find that high‐ordered nucleus (subcrystal) is the premise to ignite high‐speed growth of zeolite crystal. The high‐ordered subcrystals with the size of only 6–10 nm possess regular aperture structure and microporous area similar to zeolite nanocrystal. Interestingly, a unitary oriented aggregation process of the subcrystals towards nanosheets is well observed and characterized where single‐molecule addition process is greatly repressed. If a wider range of zeotype nuclei can be expanded, a new synthetic strategy of zeotype materials with heterogeneous framework and active sites may be expected, which may novelize zeolite catalytic properties. This work clearly observed the MFI zeolite nucleus (subcrystal) with highly uniform microporous structure and detailed its evolution and effects on the crystallization. Notably, a unitary aggregation growth between high‐ordered zeolite nuclei occurred under the mild condition, implying a new possibility to obtain heterogeneous zeotype materials.