Despite the development of several synthetic strategies employing various templates as (pore) structure directing agents, the preparation of high-quality aluminum-rich hierarchical zeolites (designated as ZH) with Si/Al < 5 from its molecular precursors is still a challenge to the scientific community. For the first time, we report here, a successful synthesis methodology for the preparation of hierarchical zeolites, having FAU and LTA topologies with uniform micropores and mesopores by a rationally designed method. Here, a stable supramolecular self-assembly was achieved under the challenging synthesis conditions by tailoring the zeolitization process, viz., by a homogeneous nucleation and a multi-step crystallization. This has resulted in regular mesoporosity in FAU-type zeolites and a unique mesoporosity in LTA-type zeolites, hitherto not reported so far.
