Sulfur Doping Triggering Enhanced Pt–N Coordination in Graphitic Carbon Nitride-Supported Pt Electrocatalysts toward Efficient Oxygen Reduction Reaction

Tailoring the interfacial interaction between metal species and supports in supported electrocatalysts is of great importance for enhanced electrocatalytic performance. Herein, a highly active interface was engineered in S-doped graphitic carbon nitride (SGCN)-supported Pt heterostructured electrocatalysts toward fast oxygen reduction reaction (ORR). The coordination and electronic structure of Pt species is modulated with enhanced Pt–N bonding by S doping, which induces electron deficiency in adjacent C and N atoms and hence reinforces the metal–support interaction. The optimal 20Pt/SGCN-550 electrocatalyst exhibits excellent ORR performance with a half-wave potential of 0.91 V and a mass activity of 0.68 A mgPt–1, substantially surpassing that of 20Pt/GCN and commercial Pt/C. Besides, the 20Pt/SGCN-550 electrocatalyst achieves decent durability due to the superb stability of SGCN and the strong confinement effect at the interface. This work not only advances the development of robust ORR electrocatalysts but also offers a strategy to engineer heterostructured electrocatalysts with tunable interface chemistry toward various catalytic applications.