Superelastic and multifunctional fibroin aerogels from multiscale silk micro-nanofibrils exfoliated via deep eutectic solvent

Superelastic silk fibroin (SF)-based aerogels can be used as multifunctional substrates, exhibiting a promising prospect in air filtration, thermal insulation, and biomedical materials. However, fabrication of the superelastic pure SF aerogels without adding synthetic polymers remains challenging. Here, the SF micro-nano fibrils (SMNFs) that preserved mesostructures are extracted from SF fibers as building blocks of aerogels by a controllable deep eutectic solvent liquid exfoliation technique. SMNFs can assemble into multiscale fibril networks during the freeze-inducing process, resulting in all-natural SMNF aerogels (SMNFAs) with hierarchical cellular architectures after lyophilization. Benefiting from these structural features, the SMNFAs demonstrate desirable properties including ultra-low density (as low as 4.71 mg/cm 3 ) and superelasticity (over 85 % stress retention after 100 compression cycles at 60 % strain). Furthermore, the potential applications of superelastic SMNFAs in air purification and thermal insulation are investigated to exhibit their functionality, mechanical elasticity, and structural stability. This work provides a reliable approach for the fabrication of highly elastic SF aerogels and endows application prospects in air purification and thermal insulation opportunities.