Sulfur doping activated metal–support interaction drives Pt nanoparticles to achieve acid–base hydrogen evolution reaction

Abstract

Adjusting the interfacial interaction between metal and support in loaded electrocatalysts is critical for enhancing the performance of electrocatalytic hydrogen evolution in both acidic and basic media, yet it continues to pose a significant challenge. This study proposes a sulfur doping strategy aimed at enhancing the strong metal–support interaction (SMSI) of ultra-small platinum (Pt) nanoparticles (NPs) uniformly encapsulated within nitrogen–sulfur co-doped carbon materials (NSC). This approach modulates the coordination environment and electronic structure of the Pt material, leading to substantial charge redistribution at the closely interfaced Pt–carbon layer heterojunction, thereby facilitating a rapid hydrogen evolution reaction (HER). The Pt/NSC exhibits excellent intrinsic activity at 1.0 M KOH (η₁₀ = 17.8 mV, 30.59 mV dec⁻¹) and 0.5 M H₂SO₄ (η₁₀ = 10.2 mV, 18.85 mV dec⁻¹), demonstrating a lower overpotential and a reduced Tafel slope, significantly outperforming the commercial Pt/C catalyst. Furthermore, owing to the exceptional stability of NSC and the pronounced confinement effect at the interface, Pt/NSC exhibits robust resistance to both acid and alkaline corrosion. Experimental and theoretical investigations reveal that the strong interfacial coupling effect can facilitate spontaneous electron transfer from the support to the Pt NPs. The electron-rich Pt NPs significantly enhance the efficiency of charge transfer and optimize the chemisorption behavior of intermediates, thereby improving the kinetics of hydrogen production.