Hierarchically Porous Materials via Co-Assembly of Exfoliated Layered Silicate with Mesoporous Silica Nanoparticles

Anisotropic nanoscale building blocks offer significant potential for the construction of porous architectures with tailored structural and functional properties. In this study, we report the successful exfoliation of magadiite─a crystalline layered silicate─into two-dimensional silica nanosheets and their co-assembly with mesoporous silica nanoparticles (MSNs) to fabricate a new class of hierarchically porous silica-based materials. Structural analysis confirmed that MSNs are uniformly distributed between the silica nanosheets, retaining the in-plane crystallinity of magadiite. The resulting composite exhibited a remarkable nitrogen adsorption capacity, a high specific surface area (909 m² g^-1), and a large pore volume (1.89 cm³ g^-1). A distinct feature is the emergence of new mesopores (∼11.5 nm), which are attributed to interparticle gaps formed through nanosheet-particle co-assembly. These findings demonstrate the utility of exfoliated layered silicates as versatile building blocks for the design of porous silica materials.