Comparative Study on the Different Interaction Pathways between Amorphous Aluminosilicate Species and Organic Structure-Directing Agents Yielding Different Zeolite Phases

Zeolites possessing novel structures and compositions have been produced using guest organic species, which are called organic structure-directing agents (OSDAs). However, the specific roles of OSDAs have not been clarified yet. In this work, *BEA- and CHA-type zeolites are synthesized from the same starting inorganic materials but with different OSDAs, and the crystallization pathways are observed using various analytical techniques. During the synthesis of *BEA-type zeolite, the gradual evolution of the aluminosilicate structure leads to the transformation from an amorphous structure to a crystalline one. On the other hand, during the synthesis of CHA-type zeolite, a few CHA nuclei are formed in “partially-ordered amorphous species” and grow through the consumption of “buffer amorphous species” on the surfaces of CHA-type zeolite crystals. This clear difference in crystallization behaviors of the two zeolites under the same synthetic conditions is attributed to the differences in the structure-directing ability. This study demonstrates the potential of structure-directing agents to control the crystallization behaviors of zeolites and provides novel insights into zeolite crystallization behavior.