Tuning the Cobalt–Platinum Alloy Regulating Single‐Atom Platinum for Highly Efficient Hydrogen Evolution Reaction

Abstract Designing atomically dispersed metal catalysts for the electrocatalytic hydrogen evolution reaction (HER) is a promising strategy to efficiently convert electrical energy to chemical fuels. This strategy, however, still faces the challenge of finding a catalyst with high activity and long‐term durability. Here, single‐atom platinum and cobalt–platinum‐alloy nanocrystals in a nitrogen‐doped porous‐carbon framework (CoPt‐Pt SA /NDPCF) is confined. The electrocatalyst exhibits ultralow overpotentials under both alkaline and acidic conditions at a high current density of −300 mA cm −2 and excellent long‐term durability up to 100 h or 10 000 cycles, which are attributed to the synergetic effects of Pt SA and tuning of the CoPt alloy in the NDPCF. First‐principles calculations suggested that Pt SA aided by the CoPt alloy has high d ‐band occupation for promoting the reaction kinetics. This study opens a new avenue for designing heterostructures with the synergic effects of single metal atoms and metal alloys with outstanding performance in the HER.