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Developing a self-supported structure with an enriched active site is crucial for enhancing the water splitting performance of transition metal selenide electrocatalysts. Herein, we present a cobalt selenide/waste silk-derived carbon (CoSe/SC) hybrid catalyst synthesized through a synergistic alcohol-mediated solvothermal and controlled pyrolysis strategy. Notably, the incorporation of ethanol transforms silk from a random coil to a highly crystalline β-sheet conformation, which effectively preserves the hierarchical architecture during carbonization. The resulting self-supporting SC matrix demonstrates exceptional electrical conductivity, enabling optimal dispersion and electronic coupling of the CoSe nanoparticles. Electrochemical evaluations reveal the optimized CoSe/SC-2 catalyst achieves overpotentials of 254.4 mV and 278.7 mV to drive 10 mA cm–2 for the HER and the OER, respectively. Importantly, the formation of Se–C bonds endows a strong coupling between cobalt selenide and waste silk-derived carbon, leading to enhanced stability (130 h) of CoSe/SC-2 in overall water splitting. This work offers valuable insights for designing transition metal selenides supported on regenerated biomass to achieve efficient electrocatalytic water splitting.
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