Designing low-cost oxygen reduction reaction (ORR) electrocatalysts to replace platinum group metal holds great promise for boosting the wide use of metal-air batteries. Herein, atomically dispersed iron supported on nitrogen-doped carbon (A-Fe-NC) was fabricated via an effective ligand-stabilized pyrolysis strategy. Owing to the high density of the active sites and the two-dimensional (2-D) nanosheet structure, the as-prepared A-Fe-NC electrocatalyst delivers excellent ORR performance with a positive half-wave potential of 0.865 V in alkaline solution, which is superior to that of Pt/C (0.82 V vs RHE). Moreover, the primary Zn-air battery assembled with the A-Fe-NC delivered an ultrahigh specific power of 132.2 mW cm⁻² and stable long-term operation. It also displayed robust charging-discharging cycling performance with voltage gap of 0.83 V after 240 h, lower than that of the Pt/C + RuO₂ electrode (0.95 V). To reveal the catalytic mechanism of A-Fe-NC, density functional theory calculation was conducted and the results revealed that the interaction between Fe and nitrogen regulated the electronic structure of active sites, thus improving charge transfer and further promoting the electrocatalytic reactivity for ORR. This work provided a facile and effective strategy for constructing Fe/N codoped 2-D carbon nanocomposite as high performance electrocatalysts for energy conversion.

设计低成本的氧还原反应 (ORR) 电催化剂来替代铂族金属对于促进金属-空气电池的广泛应用具有广阔的前景。在此，通过有效的配体稳定热解策略制造了负载在氮掺杂碳上的原子分散铁（A-Fe-NC）。由于活性位点的高密度和二维（2-D）纳米片结构，所制备的 A-Fe-NC 电催化剂具有优异的 ORR 性能，在碱性溶液中的正半波电位为 0.865 V，这优于 Pt/C (0.82 V vs RHE)。此外，与 A-Fe-NC 组装的初级锌空气电池提供了 132.2 mW cm ^-2的超高比功率并长期稳定运行。它还显示出强劲的充放电循环性能，240 小时后的电压间隙为 0.83 V，低于 Pt/C + RuO ₂电极的电压间隙(0.95 V)。为了揭示A-Fe-NC的催化机理，进行了密度泛函理论计算，结果表明Fe和氮之间的相互作用调节了活性位点的电子结构，从而改善了电荷转移并进一步促进了ORR的电催化反应。这项工作为构建 Fe/N 共掺杂二维碳纳米复合材料作为能量转换的高性能电催化剂提供了一种简便有效的策略。