Integrating pore interconnectivity and adaptability in a single crystal hierarchical zeolite for liquid alkylation

Abstract Zeolite belongs to one of the most important families of solid acid catalysts in chemical industries. It is, however, severely constrained by the diffusion limitation for bulky molecules, a lack of multifunctionality for sequential reactions and pore adaptability toward specific adsorbates due to its small micropore size and simple aluminosilicate framework. Introducing mesopores into a zeolite toward realizing hierarchical zeolites is a prevailing strategy but one that usually suffers from compromised crystallinity as well as insufficient interconnectivity and openness of the mesopores. Herein, a novel acid‐redox co‐functionalized single‐crystalline zeolite with highly open and interconnected mesopores is designed and fabricated. As a proof‐of‐concept study, we integrate solid acid and Fe‐oxy redox sites into a hierarchical MEL zeolite with well‐characterized microporosity and mesoporosity. This zeolite exhibits superior activity and stability toward alkylation between mesitylene with benzyl alcohol, arising from greatly facilitated intra‐crystal molecular diffusion, mitigated metal leaching and optimized adsorbate‐pore wall interactions.