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, the lack of
multi-functionality for sequential reactions and pore adaptability
towards specific adsorbates, due to the small micropore size and simple
aluminosilicate framework. Introducing mesopores into the zeolitic
framework towards hierarchical zeolites is prevailing, but usually
suffers from compromised crystallinity as well as insufficient
interconnectivity and openness of mesopores. Herein, a novel of
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 the solid acid and Fe-oxy redox
sites in a hierarchical MEL zeolite with well characterized
microporosity and mesoporosity. It exhibits superior activity and
stability towards the alkylation between mesitylene with benzyl alcohol,
arising from greatly facilitated intracrystalline molecular diffusion,
mitigated metal leaching and optimized adsorbate-pore wall interactions.