Coupling Single-Atom Sites and Ordered Intermetallic PtM Nanoparticles for Efficient Catalysis in Fuel Cells

Abstract

The design of an efficient catalytic system with low Pt loading and excellent stability for the acidic oxygen reduction reaction is still a challenge for the extensive application of proton-exchange membrane fuel cells. Here, a gas-phase ordered alloying strategy is proposed to construct an effective synergistic catalytic system that blends PtM intermetallic compounds (PtM IMC, M = Fe, Cu, and Ni) and dense isolated transition metal sites (M-N₄ ) on nitrogen-doped carbon (NC). This strategy enables Pt nanoparticles and defects on the NC support to timely trap flowing metal salt without partial aggregation, which is attributed to the good diffusivity of gaseous transition metal salts with low boiling points. In particular, the resulting Pt₁ Fe₁ IMC cooperating with Fe-N₄ sites achieves cooperative oxygen reduction with a half-wave potential up to 0.94 V and leads to a high mass activity of 0.51 A mg_Pt ^-1 and only 23.5% decay after 30 k cycles, both of which exceed DOE 2025 targets. This strategy provides a method for reducing Pt loading in fuel cells by integrating Pt-based intermetallics and single transition metal sites to produce an efficient synergistic catalytic system.

Keywords: gas-phase ordered alloying strategy; intermetallic compounds; proton-exchange membrane fuel cells; single atom catalysts; synergistic catalytic systems.