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

Lai, Wei-Hong; Zhang, Lifu; Yan, Zichao; Hua, Weibo; Indris, Sylvio; Lei, Yaojie; Liu, Hanwen; Wang, Yun-Xiao et al. · Nano Lett · 2021

basic_science · Level V

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Abstract

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<sub>subsurf</sub>) 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<sub>subsurf</sub> single atoms implanted in different positions of the subsurface of Co particles. The local environments and catalytic properties of surface Pt<sub>1</sub> are highly tunable via Pt<sub>subsurf</sub> doping. Specifically, the obtained Pt<sub>1</sub>@Co/NC catalyst displays a remarkable performance for ORR, achieving mass activity of 4.2 mA μg<sub>Pt</sub><sup>-1</sup> (28 times higher than that of commercial Pt/C) at 0.9 V versus reversible hydrogen electrode (RHE) in 0.1 M HClO<sub>4</sub> solution with high stability over 30000 cycles.