Micron‐Sized Zeolite Beta Single Crystals Featuring Intracrystal Interconnected Ordered Macro‐Meso‐Microporosity Displaying Superior Catalytic Performance

Abstract Zeolite Beta single crystals with intracrystalline hierarchical porosity at macro‐, meso‐, and micro‐length scales can effectively overcome the diffusion limitations in the conversion of bulky molecules. However, the construction of large zeolite Beta single crystals with such porosity is a challenge. We report herein the synthesis of hierarchically ordered macro‐mesoporous single‐crystalline zeolite Beta (OMMS‐Beta) with a rare micron‐scale crystal size by an in situ bottom‐up confined zeolite crystallization strategy. The fully interconnected intracrystalline macro‐meso‐microporous hierarchy and the micron‐sized single‐crystalline nature of OMMS‐Beta lead to improved accessibility to active sites and outstanding (hydro)thermal stability. Higher catalytic performances in gas‐phase and liquid‐phase acid‐catalyzed reactions involving bulky molecules are obtained compared to commercial Beta and nanosized Beta zeolites. The strategy has been extended to the synthesis of other zeolitic materials, including ZSM‐5, TS‐1, and SAPO‐34.