Partially Ordered Mesoporous Zeolite Beta Frameworks as Naphtha-Selective Catalysts in Vacuum Gas Oil Hydrocracking

Designing hierarchical zeolites with ordered mesoporosity remains a major synthetic challenge despite their well-established importance in catalysis and separations. In this study, we examine the spatiotemporal dynamics of zeolite dissolution and reorganization to retrace how transient structural changes during zeolite nucleation influence supramolecular self-assembly. For the first time, we demonstrate that subtle differences in the aluminum (Al) spatial proximity and distribution within various zeolite frameworks critically affect their mesostructuring behavior. Notably, beta zeolite comprising distinct polymorphs with marginally different Al environments has shown an anisotropic dissolution pattern, where polymorph B was selectively fragmented, leaving polymorph A unaffected. Through a postsynthetic mesostructuring approach, polymorph B was preferentially reorganized into a gyroidal cubic ordered mesophase, resulting in partially ordered mesoporous beta zeolite. The prepared zeolites exhibit improved catalytic performance in vacuum gas oil hydrocracking, affording high isoparaffin yields and superior naphtha selectivity. These findings provide a direct link between atomic-scale heterogeneity and mesoscale structural evolution in crystals, offering a new strategy for designing advanced catalytic materials.