Tailored approach for hierarchization of all-silica zeolites

• RS FT-IR spectroscopy offers comprehensive insights into the hierarchical porous architecture. • Mesoporous zeolite fabrication depends on their pore size, shape, and structural defects. • Enhanced functionality by introducing mesoporosity into all-silica zeolites. Adding secondary mesoporosity to all-silica zeolites can improve mass transfer, potentially leading to new applications in catalysis and separation. The tailored post-synthesis methods involving detemplation, desilication, and application of pore-directing agents were applied to examine the influence of zeolite type structure, crystal properties, and synthesis conditions on the hierarchization feasibility of all-silica ITQ-29 (LTA), silicalite-1 (MFI), silicalite-2 (MEL), and beta (*BEA) zeolites. Advanced characterization tools such as rapid scan RS FT-IR spectroscopy, field emission scanning electron microscopy, and focused ion beam provided insight into the properties of hierarchical all-silica zeolites. The formation of hierarchical all-silica zeolites was found to be pore size and shape-dependent and defects-oriented; however, the ultimate influence of these factors on hierarchization is interdependent.