Abstract

Silk fibroin and silk microfibers, both derived from silk cocoon, have been widely used for prospective biomedical, energy, and environmental applications. However, various complex and catalyst-based approaches have been adopted for chemical modification and integration of different functionalities in silk fibroin-based materials. Here, both tailored water wettability and mechanical property have been associated with silk microfiber reinforced silk fibroin sponges (SMFRSFSs) through the strategic introduction of β-sheets and a facile and catalyst-free chemical reaction at ambient conditions. While the controlled tailoring of β-sheets in the silk fibroin skeletal framework of the sponges allowed us to modulate the compressive modulus, the 1,4-conjugate addition reaction between amine residues of silk (fiber and fibroin) and acrylate groups of a multifunctional cross-linker provided residual chemical reactivity. Further, the chemically "reactive" sponge was postmodified with the selected alkylamines to introduce a wide range of water wettability (from 36 to 161°) without affecting the mechanical property. Thereafter, the silk cocoon-derived and extremely water-repellent sponge was used for environment-friendly cleaning of oil spillages through selective absorption-based and filtration-based oil/water separation at different and severe aqueous conditions. This silk cocoon-derived mechanically tailorable and chemically reactive sponge could also be useful for various biomedical and energy-related applications.

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