Dual‐Pt‐Sites/Mo 2 C Nano‐Islands Confined in N‐Doped Porous Carbon Hemispheres Boosting Hydrogen Evolution

Abstract The pursuit of low‐cost yet high‐performance catalysts to substitute Pt/C represents a critical challenge in hydrogen production. Despite the excellent water dissociation ability of Mo 2 C, the strong adsorption of hydrogen largely hinders the Heyrovsky process. Here, N‐doped porous carbon hemispheres supporting Mo 2 C islands co‐decorated with Pt nanoparticles and single atoms (Pt 1.15wt% ‐Mo 2 C/NCH) are constructed via a solid‐phase pyrolysis strategy, with a low Pt loading of 1.15 wt%. Benefiting from the continuous 3D porous structure and the strong interaction between dual‐Pt‐sites and Mo 2 C, Pt 1.15wt% ‐Mo 2 C/NCH exhibits superior catalytic activity and stability across a broad pH range. Under 10 mA cm −2 , it delivers low overpotentials of 32, 40, and 83 mV in acidic, alkaline, and neutral media, respectively. The density functional theory (DFT) calculations reveal that the Pt cluster preferentially anchors on Mo 2 C due to the strong interaction. During the hydrogen evolution reaction (HER), H 2 O is initially adsorbed on Pt clusters, followed by cooperative cleavage of the O─H bond at the interfacial Pt single atoms and Mo 2 C. This synergistic cooperation endows the catalyst with balanced H 2 O adsorption energy, reduced dissociation energy barrier, and favorable hydrogen adsorption, establishing it as a promising candidate for efficient HER.