Xinyi Song, Xinjian He, Cunmin Wang, Jiaqi Li, Xinyu Li, Fangyuan Tian, Ming-Peng Zhuo, Wei Li, Yue Zhao, Shu-Gui Yang, Jiefeng Gao, Weiqing Kong, Huan Xu
The integration of solution electrospinning with biomimetic structures has long been a major challenge in the fabrication of biomimetic membranes. Herein, we unraveled a hydrogen bonding-enabled spider silk-mimicking (HBSS) strategy by multiphase electrospinning. It specifically involved phase-regulating factors to generate a high density of hydrogen bonding within the poly(lactic acid) (PLA) nanofibers of HBSS-PLA. Hydrogen bonding-induced phase separation led to the formation of nanofibrous membranes (NFMs) composed of nanofibers with groove-bead morphology. The NFMs inherited the structural characteristics and low-surface-energy properties of spider silk and demonstrated excellent antifouling performance against surface contaminants including blood and dust. Meanwhile, localized high-density hydrogen bonding promoted fiber refinement (275 nm) and efficient electret stabilization, imparting the bioinspired PLA NFMs with excellent breathability (128 Pa and 190 mm/s at 85 L/min) and high-efficiency particulate matter removal (96.4% for PM 0.3–2.5 at 85 L/min). After five washing cycles, the meta-membranes maintained a high PM capture performance (with only a 0.2% decrease in efficiency), while exhibiting a minimal pressure drop increase of 5.5 Pa. The strategy unites biomimetic structures and multiphase electrospinning techniques, proposing self-polarized stereocomplexed PLA nanofibers that demonstrate an exceptional combination of self-cleaning capability, antifouling performance, high PM filtration efficiency, and enhanced breathability. The bioinspired multifunctional meta-membranes signify a promising high-performance medium for personal protection applications, appealing for next-generation medical and advanced protective systems.