Silk fibroin (SF) has attracted wide attention due to its excellent biocompatibility and versatile adjustability. The regeneration and reutilization of silk fibroin can efficiently utilize waste cocoons and silk. However, the regenerated SF hydrogels suffer from inadequate mechanical properties and lack inherent antibacterial capabilities, limiting their application in seawater desalination. This study achieved a novel hydrogel (STS@Fe) with photothermal antimicrobial activity, good mechanical property, and excellent durability using a green dual-directional crosslink and meso-reconstruction strategy. The metal-phenolic networks (MPN) were synthesized utilizing the natural plant polyphenol tannic acid (TA) and Fe3O4 nanoparticles. This research incorporated MPN into dissolved and regenerated silk fibroin and sodium alginate solution, enhanced mechanical properties through cryogenic salt precipitation, and prepared STS@Fe hydrogel. The inherent photothermal properties of Fe3O4 nanoparticles and TA complex, coupled with their synergistic effect under near-infrared radiation, can confer excellent photothermal-enhanced antibacterial activity to the fibroin hydrogel. The tensile strength of STS@Fe hydrogel is enhanced 31 times than that of traditional fibroin hydrogel, and its evaporation rate is 4.77 times higher than that of pure water evaporation. The hydrogel has an efficient seawater desalination rate and outstanding antibacterial properties in real seawater conditions. Moreover, The STS@Fe shows effective treatment capabilities for dyeing wastewater and oily saline water.
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