The development of oxygen reduction reaction (ORR) electrocatalysts based on earth‐abundant nonprecious materials is critically important for sustainable large‐scale applications of fuel cells and metal–air batteries. Herein, a hetero‐single‐atom (h‐SA) ORR electrocatalyst is presented, which has atomically dispersed Fe and Ni coanchored to a microsized nitrogen‐doped graphitic carbon support with unique trimodal‐porous structure configured by highly ordered macropores interconnected through mesopores. Extended X‐ray absorption fine structure spectra confirm that Fe‐ and Ni‐SAs are affixed to the carbon support via FeN₄ and NiN₄ coordination bonds. The resultant Fe/Ni h‐SA electrocatalyst exhibits an outstanding ORR activity, outperforming SA electrocatalysts with only Fe‐ or Ni‐SAs, and the benchmark Pt/C. The obtained experimental results indicate that the achieved outstanding ORR performance results from the synergetic enhancement induced by the coexisting FeN₄ and NiN₄ sites, and the superior mass‐transfer capability promoted by the trimodal‐porous‐structured carbon support.

中文翻译：

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作为高效ORR电催化剂，在有序排列的多孔碳上同时存在单原子的Fe和Ni原子。

基于富含地球的非贵重材料的氧还原反应（ORR）电催化剂的开发对于燃料电池和金属空气电池的可持续大规模应用至关重要。本文介绍了一种杂-单原子（h-SA）ORR电催化剂，它已将Fe和Ni原子分散在锚定的微米级氮掺杂石墨碳载体上，该载体具有独特的三峰-多孔结构，该结构由通过中孔相互连接的高度有序的大孔构成。扩展X射线吸收精细结构谱证实，铁-和Ni-SAS经由铁固定到碳载体 Ñ ₄和Ni  Ñ ₄协调纽带。所得的Fe / Ni h-SA电催化剂表现出出色的ORR活性，优于仅含Fe-或Ni-SAs和基准Pt / C的SA电催化剂。将所得到的实验结果表明，从由铁共存引起的协同增强取得优异ORR性能结果 Ñ ₄和Ni  Ñ ₄位点，并且通过所述三峰-多孔构造的碳载体促进了优越的传质能力。