A Bottom‐Up Strategy for the Synthesis of Highly Siliceous Faujasite‐Type Zeolite

Abstract High‐silica zeolite Y is a desired catalytic material for oil refining and the petrochemical industry. However, its direct synthesis remains a symbolic challenge in the field of zeolite synthesis, with a limited improvement of the framework SiO₂/Al₂O₃ ratio (SAR) from ≈5 to 9 over the past 60 years. Here, the synthesis of highly siliceous zeolite Y with tunable SAR up to 15.6 through a cooperative strategy is reported, which involves the use of FAU nuclei, a bulky organic structure‐directing agent (OSDA), and a gel system with low alkalinity (named NOA‐co strategy). A series of quaternary alkylammonium ions is discovered as effective OSDAs based on the NOA‐co strategy, and the relevant crystallization mechanism is elucidated. Moreover, the high‐silica products are demonstrated to have greatly improved (hydro)thermal stability, high concentration of strong acid sites, and uniform acid distribution, which lead to superior catalytic performance in the cracking of bulky hydrocarbons. It is anticipated that this synthetic strategy will benefit the synthesis and development of zeolitic catalysts in a wide range of reaction processes.