Multifunctional Aerogel‐Structured Metafabrics Assembled by Hierarchically Porous Microsphere/Nanofibril

ABSTRACT The micro/nanoporous materials that have both hierarchical pore structures and robust mechanical properties would have broad implications for areas ranging from damping and filter separation to adsorbent materials; however, creating such micro/nanoporous materials has proven extremely challenging. Herein, the multifunctional aerogel‐structured metafabrics composed of wholly porous microspheres and nanofibril scaffolds are fabricated by innovatively integrating millisecond microphase separation molding technology with multi‐parameter coupling control strategy. The aerogel‐like porous microspheres with abundant vortex sheets can be realized by customizing the Taylor cone ejection morphology and regulating the bidirectional mass‐transfer between the external environment and solvents. The hierarchical pore structure consisting of micro/nanofibrous networks and porous aerogel microspheres is developed, which endows metafabrics with high porosity (>90%). Attributed to the flexible and stable structure of micro/nanofibrils, the resulting aerogel‐structured metafabrics exhibit mechanical robustness and shape‐memory property even under −196°C. Moreover, such aerogel structures endow the metafabrics with surprising potential for energy dissipation and filtration separation, particularly ultrathin noise reduction (NRC of 0.5 at 10 mm), high‐efficiency air filtration (99.96% efficiency, 23.3 Pa air resistance), and high‐utilisation CO 2 capture (0.68 mmol g −1 ) at extremely low amine loading, obviously superior to cutting‐edge materials. This work provides a new pathway for the design of multifunctional aerogel‐structured metafabrics.