The quest for a general and facile way to regulate polymer self-assembled nanostructures with low-to high-order ergodicity is an eternal theme in soft nanoparticle fabrication. Here we present an unprecedented gas-bri...The quest for a general and facile way to regulate polymer self-assembled nanostructures with low-to high-order ergodicity is an eternal theme in soft nanoparticle fabrication. Here we present an unprecedented gas-bridging strategy that allows to use gas to direct polymer self-assembly in continuous and tunable manners. Such system comprises a partner of frustrated Lewis polymers with bulky Lewis acid and base groups. They can together “breathe in” external gases to form gas-bridged structures between the two complementary moieties, which drive their mutual complexation and assemble into polymer nanoparticles of diverse geometries and dimensionalities. This strategy is applicable to a broad family of gas substances including but not limited to carbon oxides, nitrogen oxides, sulfur oxides, and even olefins;moreover, tailoring gas types and levels can dictate distinct assembling evolutionary pathways and deformable behaviors among spherical, fibrous, polymersomal, tubesomal and cubosomal morphologies. We also discover that the gas-based bonding chemistry is the mechanistic basis underlying the phase transitional control and phase window regulation. This will open a new direction of making bespoke polymer nanostructures with gas.展开更多
基金supported by the National Natural Science Foundation of China (21674022, 51703034)the National Defense Science and Technology Innovation Zone (163 Program)the Shanghai Rising-Star Program (19QA1400700)。
文摘The quest for a general and facile way to regulate polymer self-assembled nanostructures with low-to high-order ergodicity is an eternal theme in soft nanoparticle fabrication. Here we present an unprecedented gas-bridging strategy that allows to use gas to direct polymer self-assembly in continuous and tunable manners. Such system comprises a partner of frustrated Lewis polymers with bulky Lewis acid and base groups. They can together “breathe in” external gases to form gas-bridged structures between the two complementary moieties, which drive their mutual complexation and assemble into polymer nanoparticles of diverse geometries and dimensionalities. This strategy is applicable to a broad family of gas substances including but not limited to carbon oxides, nitrogen oxides, sulfur oxides, and even olefins;moreover, tailoring gas types and levels can dictate distinct assembling evolutionary pathways and deformable behaviors among spherical, fibrous, polymersomal, tubesomal and cubosomal morphologies. We also discover that the gas-based bonding chemistry is the mechanistic basis underlying the phase transitional control and phase window regulation. This will open a new direction of making bespoke polymer nanostructures with gas.
