In this article, a sustainable defect-engineering strategy for dealumination of Y zeolite is described. This strategy includes the green synthesis of a well-crystallized Y zeolite with point defects arising from the incorporation of Fe atoms by using a Fe-containing perlite and the subsequent preparation of ultra-stable Y (USY) zeolite by effective dealumination. The systematic characterizations verify that Fe atoms originally existing in the perlite are incorporated into the as-synthesized Y zeolite and function as point defects, leading to the distortion of framework Al. The step-by-step investigation of the dealumination process shows that vacancies are formed by the extraction of framework Fe in the ammonium exchange, and the framework dealumination is promoted under the combined effect of the distorted framework Al and the formed vacancies during the steaming treatment. The resulting USY zeolite owns excellent features in (hydro)thermal stability, pore structure and acid property, and thus exhibits outstanding catalytic cracking performance.

Aluminum-rich hierarchical MFI-type zeolites with high acidic-site density exhibit excellent activity and selectivity in bulky molecule-involved reactions. However, it is challenging to develop a facile and environmentally benign method for fabricating them. Herein, we employ a polymer that does not contain nitrogen and halogen elements to successfully synthesize aluminum-rich hierarchical ZSM-5 zeolite with a Si/Al ratio of 8 and a significant number of mesopores comprised of oriented-assembled nanocrystals. It is demonstrated that the nitrogen- and halogen-free polymer is instrumental in the formation of the ZSM-5 zeolite by serving as a template for constructing the hierarchical micro/mesoporous structure. Moreover, this polymer also acts as a crystal growth modifier to form a single-crystalline zeolite. Notably, the resultant zeolite shows a better catalytic performance in converting waste plastic into hydrocarbons than a commercial one. Our work enables the synthesis of high-quality hierarchical zeolites without requiring quaternary ammonium templates.

A sustainable defect‐engineering strategy for the dealumination of Y zeolite is described. This strategy includes the green synthesis of a well‐crystallized Y zeolite with point defects arising from the incorporation of Fe atoms by using Fe‐containing perlite and the subsequent preparation of ultra‐stable Y (USY) zeolite by efficient steaming dealumination. The systematic characterizations verify that Fe atoms originally existing in the perlite are incorporated into the as‐synthesized Y zeolite and function as point defects, leading to the distortion of framework Al. The step‐by‐step investigation of dealumination process shows that vacancies are formed by the extraction of framework Fe in ammonium exchange, and the framework dealumination is promoted under the combined effect of the distorted framework Al and the formed vacancies during steaming treatment. The resulting USY zeolite owns excellent features in (hydro)thermal stability, pore structure and acid property, and exhibits outstanding catalytic performance in the cracking of n‐octane and 1,3,5‐triisopropylbenzene.