Single atom catalysts (SACs) are emerging as a highly promising catalyst category in oxygen electrocatalysis; however, their real-world implementation in rechargeable zinc-air batteries (ZABs) is restricted by the insufficient bifunctional activity. Here, a secondary single-atom regulation strategy is developed to tailor the coordination environment and thus modify the catalytic behaviors of single atom Ni catalysts. Through introducing atomically dispersed Fe moieties, the coordination environment of single Ni atom is well regulated with a higher Ni-N/O coordination number due to the long-range electronic penetration interaction, which triggers more optimized adsorption strength between active sites and reaction intermediates. As a result, the obtained Fe, Ni dual atom catalyst (FeNi-SAs@NC) requires only 298 mV overpotential to deliver 10 mA cm⁻² in oxygen evolution reaction (OER) catalysis outperforming the benchmarking IrO₂ (313 mV), Fe-SAs@NC (335 mV) and Ni-SAs@NC (356 mV) electrocatalysts. Moreover, FeNi-SAs@NC performs superior oxygen reduction reaction (ORR) activity to the single-atom counterparts and Pt/C benchmark. The practical application of the FeNi-SAs@NC is further validated by a higher ZAB performance (260 mW cm⁻² vs 71 mW cm⁻² for Pt/C-IrO₂), improved long-term durability (100 h at 20 mA cm⁻²) and encouraging performance in all-solid-sate ZABs (70 mW cm⁻²).

在氧电催化中，单原子催化剂（SAC）成为一种很有前途的催化剂。但是，其在现实世界中在可充电锌空气电池（ZAB）中的实施受到双功能活动不足的限制。在此，开发了第二种单原子调节策略来调整配位环境，从而改变单原子Ni催化剂的催化行为。通过引入原子分散的Fe部分，由于长程电子渗透相互作用，单个Ni原子的配位环境受到较高的Ni-N / O配位数的良好调节，从而触发了活性位点和反应中间体之间的最佳吸附强度。结果，所获得的铁，镍双原子催化剂（FeNi-SAs @ NC）仅需298 mV超电势即可输送10 mA cm在放氧反应（OER）催化中的^-2优于基准IrO ₂（313 mV），Fe-SAs @ NC（335 mV）和Ni-SAs @ NC（356 mV）电催化剂。此外，FeNi-SAs @ NC具有比单原子对应物和Pt / C基准更高的氧还原反应（ORR）活性。FeNi-SAs @ NC的实际应用通过更高的ZAB性能（对于Pt / C-IrO ₂为260 mW cm ^-2相对于71 mW cm ^-2）得到了进一步验证，并提高了长期耐久性（在20 mA下100 h） cm ^-2），并在全固态ZAB（70 mW cm ^-2）中具有令人鼓舞的性能。