Stretch-Induced Robust Intrinsic Antibacterial Thermoplastic Gelatin Organohydrogel for a Thermoenhanced...

Sustainable organohydrogel electronics have shown promise in resolving the electronic waste (e-waste) evoked by traditional chemical cross-linking hydrogels. Herein, thermoplastic-recycled gelatin/oxidized starch (OST)/glycerol/ZnCl₂ organohydrogels (GOGZs) were fabricated by introducing the anionic polyelectrolyte OST and solvent exchange strategy to construct noncovalently cross-linking networks. Benefiting from the electrostatic interaction and hydrogen and coordination bonds, GOGZ possessed triple-supramolecular interactions and a continuous ion transport pathway, which resulted in excellent thermoplasticity and high ionic conductivities and mechanical and antibacterial properties. Because of the thermally induced phase transition of gelatin, GOGZ exhibited isotropic-ionic conductivity with a positive temperature coefficient and realized intrinsic affinity with the activated carbon electrode for fabricating a double-layer structure supercapacitor. These novel features significantly decreased the impedance (3.71 Ω) and facilitated the flexible supercapacitors to achieve thermoenhanced performance with 4.89 Wh kg^-1 energy density and 49.2 F g^-1 specific mass capacitance at 65 °C. Fantastically, the GOGZ-based stress sensor exhibited a monolinear gauge factor (R² = 0.999) at its full-range strain (0 to 350%), and its sensitivity increased with the thermoplastic-recycled times. Consequently, this sustainable and temperature-sensitive sensor (-40 to 60 °C) could serve as health monitoring wearable devices with excellent reliability (R² = 0.999) at tiny strain. Moreover, GOGZ could achieve efficient self-enhancement by stretch-induced alignment. The sustained weighted load, tensile strength, and elongation at break of the stretch-induced GOGZ were 6 kg/g, 2.37 MPa, and 300%, respectively. This self-enhanced feature indicated that GOGZ can be utilized as an artificial muscle. Eventually, GOGZ obtained high intrinsic antibiosis (D_{inhibition circle} > 25 mm) by a binding species (-COO^-NH₃⁺-) from COOH in OST and NH₂ in gelatin, freezing resistance, and water retention. In summary, this study provided an effective strategy to fabricate thermoplastic-recycled organohydrogels for multifunctional sustainable electronics with novel performance.