Atomically dispersed catalysts with high electrocatalytic performance are emerging as promising electrocatalysts for energy conversion and storage devices. Nevertheless, achieving superior bifunctional catalytic activity with single-atom catalysts toward reactions involving multi-intermediates is still facing great challenges. Herein, dual-atomic Fe-Ni pairs dispersed in hierarchical porous nitrogen-doped carbon (FeNi-HPNC) catalysts were successfully synthesized using a facile mechanochemical strategy. By virtue of the engineered electronic structure of Fe coordinated with Ni, the as-synthesized FeNi-HPNC with atomically dispersed dual-metal active sites and pore-rich structure exhibits remarkable bifunctional activities. A high half-wave potential of 0.868 V for oxygen reduction reaction and a low potential of 1.59 V at 10 mA/cm² for oxygen evolution reaction have been obtained for FeNi-HPNC, which are superior to the single-atom catalysts of Fe-HPNC and Ni-HPNC, respectively, and are even greater than the precious metal catalysts. Combined experimental and theoretical results have revealed that the enhanced bifunctional catalytic activity of FeNi-HPNC is ascribed to the electronic interaction of Fe-Ni sites, which decreases the adsorption energy of oxygen intermediates during oxygen reduction reaction/oxygen evolution reaction. Furthermore, the practical application of FeNi-HPNC catalysts in Zn-air batteries has been demonstrated; a high peak power density and long-term durability are delivered.

具有高电催化性能的原子分散催化剂正在成为用于能量转换和存储设备的有前途的电催化剂。然而，在涉及多中间体的反应中，用单原子催化剂实现优异的双功能催化活性仍然面临着巨大的挑战。在此，使用简便的机械化学策略成功地合成了分散在分级多孔氮掺杂碳 (FeNi-HPNC) 催化剂中的双原子 Fe-Ni 对。凭借 Fe 与 Ni 配位的工程化电子结构，所合成的具有原子分散的双金属活性位点和富孔结构的 FeNi-HPNC 表现出显着的双功能活性。氧还原反应的高半波电位为 0.868 V，在 10 mA/cm 时的低电位为 1.59 VFeNi-HPNC的析氧反应得到了2，分别优于Fe-HPNC和Ni-HPNC的单原子催化剂，甚至优于贵金属催化剂^。结合实验和理论结果表明，FeNi-HPNC的双功能催化活性增强归因于Fe-Ni位点的电子相互作用，降低了氧还原反应/析氧反应过程中氧中间体的吸附能。此外，已经证明了 FeNi-HPNC 催化剂在锌空气电池中的实际应用；提供高峰值功率密度和长期耐用性。