Activating Inert Surface Pt Single Atoms via Subsurface Doping for Oxygen Reduction Reaction

The performance of single-atom catalysts strongly depends on their particular coordination environments in the near-surface region. Herein, we discover that engineering extra Pt single atoms in the subsurface (Pt-subsurf) can significantly enhance the catalytic efficiency of surface Pt single atoms toward the oxygen reduction reaction (ORR). We experimentally and theoretically investigated the effects of the Pt(subsurf )single atoms implanted in different positions of the subsurface of Co particles. The local environments and catalytic properties of surface Pt-1 are highly tunable via Pt-subsurf doping. Specifically, the obtained Pt-1@Co/NC catalyst displays a remarkable performance for ORR, achieving mass activity of 4.2 mA mu g(Pt)(-1) (28 times higher than that of commercial Pt/C) at 0.9 V versus reversible hydrogen electrode (RHE) in 0.1 M HClO4 solution with high stability over 30000 cycles.

Automated summary

It has been discovered that introducing extra Pt single atoms in the subsurface of single-atom catalysts can significantly enhance their catalytic efficiency towards the oxygen reduction reaction. This doping method allows for tunable local environments and catalytic properties of surface Pt single atoms. The Pt-1@Co/NC catalyst obtained through this method shows remarkable performance for ORR with high stability over 30000 cycles.