Exploring efficient, easy-to-manufacture, and inexpensive bifunctional electrocatalysts with abundant accessible active sites is crucial for rechargeable zinc-air batteries (ZABs). Herein, we report the strategy consisting of the space confinement and pore-making engineering to fabricate single-atom catalyst enriched with Fe-N₄ sites anchored on N-doped hierarchically porous carbon (Fe-NC-C₃N₄). The optimized Fe-NC-C₃N₄ exhibits excellent oxygen reduction/evolution reaction (ORR/OER) activities with a half-wave potential (E_1/2) of 0.90 V vs. RHE and a promising low overpotential of 0.305 V vs. RHE at 10 mA·cm⁻² in alkaline electrolyte. These superior catalytic activities are attributed to the combined effect between the atomic active sites and the well-balanced micro-meso-macropore structures. The homemade liquid Zn-air battery (ZAB) assembled with Fe-NC-C₃N₄ catalyst displays a power density of 133.59 mW·cm⁻² and a significant energy density of 882.58 mAh·g⁻¹, exceeding those of the equipment with commercial Pt/C-RuO₂ (56.82 mW·cm⁻² and 643.87 mAh·g⁻¹, respectively). Particularly, the corresponding flexible wearable ZAB manifests outstanding foldability and cyclical stability. This work opens a new perspective for the structural design of single-atom catalysts in the energy storage and conversion area.

探索高效、易于制造且廉价且具有丰富的活性位点的双功能电催化剂对于可充电锌空气电池（ZAB）至关重要。在此，我们报告了由空间限制和造孔工程组成的策略，以制造锚定在N掺杂分级多孔碳（Fe-NC-C ₃ N ₄）上的富含Fe-N ₄位点的单原子催化剂。优化的 Fe-NC-C ₃ N ₄表现出优异的氧还原/析出反应 (ORR/OER) 活性，半波电位 ( E _1/2 ) 为 0.90 V （与RHE 相比），并且具有 0.305 V（与 RHE 相比）的低过电位，有前景。。碱性电解液中，RHE 为 10 mA·cm ^{-2 。}这些优异的催化活性归因于原子活性位点和平衡良好的微-介观-大孔结构之间的综合作用。自制的Fe-NC-C ₃ N ₄催化剂组装的液态锌空气电池（ZAB）的功率密度为133.59 mW·cm ^-2，能量密度高达882.58 mAh·g ^-1，超过了设备的能量密度与商用Pt/C-RuO ₂（分别为56.82 mW·cm ^-2和643.87 mAh·g ^-1）。特别是，相应的柔性可穿戴ZAB表现出出色的可折叠性和循环稳定性。这项工作为能量存储和转换领域的单原子催化剂的结构设计开辟了新的视角。