Asymmetric Monolayer Mesoporous Nanosheets of Regularly Arranged Semi-Opened Pores via a Dual-Emulsion-Directed Micelle Assembly

Constructing asymmetric two-dimensional (2D) mesoporous nanomaterials with new pore structure, tunable monolayer architectures, and especially anisotropic surfaces remains a great challenge in materials science. Here, we report a dual-emulsion directed micelle assembly approach to fabricate a novel type of asymmetric monolayer mesoporous organosilica nanosheet for the first time. In this asymmetric 2D structure, numerous quasi-spherical semiopened mesopores (∼20 nm in diameter, 24 nm in opening size) were regularly arranged on a plane, endowing the porous nanosheets (several micrometers in size) with a typical surface anisotropy on two sides. Meanwhile, lots of triangular intervoids (4.0-5.0 nm in size) can also be found among each three semiopened mesopores, enabling the nanosheet to be interconnected. Vitally, such interconnected, anisotropic porous nanosheets exhibit ultrahigh accessible surface area (∼714 m2 g-1) and good lipophilicity properties owing to the abundant semiopened mesopores. Additionally, besides the nanosheet, the configuration of the asymmetric porous structure can also be transformed into a microcapsule when controlling the emulsification size via a facile ultrasonic treatment. As a demonstration, we show that the asymmetric microcapsule shows a high demulsification efficiency (>98%) and cyclic stability (>6 recycle times). Our protocol opens up a new avenue for developing next-generation asymmetric mesoporous materials for various applications.