Facile preparation of hierarchically meso-mesoporous silicas with ultra-large pores and pore volumes via partitioned cooperative self-assembly process

• Improved ternary templating system for hierarchically meso-mesoporous (HMM) silica.
• Newly found combined effect of hydrothermal treatments and PCSA process on HMM structures.
• Ultra-large pores/volumes can be achieved.

This work demonstrates that based on a simple improved ternary nonionic surfactant templating system, hierarchically meso-mesoporous (HMM) silicas with ultra-large pores and pore volumes can be facilely prepared by combining hydrothermal treatments (HTT) with the partitioned cooperative self-assembly (PCSA) process. The obtained clew-like HMM silica particles contain bimodal pore size distributions. The disordered 1st mode mesostructures (pore sizes of 7–20 nm) form the ‘yarns’, while the 3D-interconnected 2nd mode intra-particulate pores (33–118 nm in sizes) exist between the ‘yarns’. The ultra-large pore volume reaching 3.22 cm3 g−1 can be achieved. The formation of such HMM silicas arises from the HTT induced fragmentation of the 1st mode mesostructures.

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