Gas‐Constructed Vesicles with Gas‐Moldable Membrane Architectures

Abstract Integrating gas as a main building block into nanomaterial construction is a challenging mission that remains elusive. Herein, we report a gas‐constructed vesicular system formed by CO 2 gas and frustrated Lewis pairs (FLPs). Two molecular triads bearing three bulky borane and phosphine groups are designed as trivalent disc‐like FLP monomers. CO 2 , as a gas cross‐linker, can drive the two‐dimensional polymerization of these two FLP monomers, leading to the generation of planar FLP networks that further transform into a thermodynamically favored membranous vesicle structure. Gas‐guided vesicle formation is also applicable to other inert but FLP‐activatable gases. Different gas linkages can form vesicles with distinct architectures, sizes, and morphologies. We envisage that this study would suggest a new concept that exploits gases to fabricate tunable nanomaterials.