Generating Beta Zeolite Nanosheets of Intergrown Polymorph B and C Using Polycationic Structure‐Directing Agent

H} heteronuclear correlation NMR spectra reveal that the framework Al atoms are mainly situated close to the ammonium moieties of the OSDA inside straight channels, owing to a strong OSDA-framework attraction. The selectivities of ethylene, propylene and catalyst lifetime have been promoted in n-heptane cracking, due to stronger acidity and enhanced diffusion property. Moreover, the architecture is robust toward deep dealumination and Ti- modification, allowing it to be a superior catalyst in cyclohexene epoxidation. The polycation OSDA design concept and the recipe for Beta nanosheets may find broader applications in catalysis.