Hierarchical and two-dimensional (2D) zeolites have drawn much attention in catalysis and separation process due to their fast mass transfer. However, the facile manipulation in controllable mesopore volumes and morphologies for hierarchical nanozeolites is full of challenges. Herein, a facile strategy is presented for the synthesis of single-crystalline 2D hierarchical MFI zeolite nanosheets (HNSs) with tunable mesopore volumes through the amino acid-assisted crystallization of nucleated amorphous silicon precursors (NASPs). The tailored synthesis of HNSs with controllable aspect ratios ((Lc + La)/Lb), b-axis thicknesses (a few tens of nanometers) and mesopore volumes is achieved by adjusting the preparation of the NASPs and the amount of amino acid in the synthesis mixture. The HNSs exhibit large BET surface area (>400 m2/g), high micropore volume (0.16–0.18 cm3 g−1) as well as rich mesopore volume (>0.10 cm3 g−1), indicating the high crystallinity of the hierarchical zeolite nanosheets. Specially, the higher adsorption capability and faster adsorption rate for the dye (Rhodamine B) adsorption demonstrate the excellent performance of the hierarchical zeolite nanosheets, which exhibit the maximum adsorption capacity of 115.7 mg g−1. The controllable manipulation of mesoporous volumes and morphologies in MFI zeolites represents a significant contribution to the field of zeolite microstructure engineering.
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