Optimizing the hydrogen adsorption Gibbs free energy (ΔG ) of active sites is essential to improve the overpotential of the electrocatalytic hydrogen evolution reaction (HER). We doped graphene-like Co Se with sulfur and found that the active sites are reversed (from cationic Co sites to anionic S sites), which contributed to an enhancement in electrocatalytic HER performance. The optimal S-doped Co Se composite has an overpotential of 108 mV (at 10 mA cm ) and a Tafel slope of 59 mV dec , which exceeds other reported Co Se-based electrocatalysts. The doped S sites have much higher activity than the Co sites, with a hydrogen adsorption Gibbs free energy (ΔG ) close to zero (0.067 eV), which reduces the reaction barrier for hydrogen production. This work provides inspiration for optimizing the intrinsic HER activity of other related transition metal chalcogenides.
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