Constructing highly efficient and durable non-noble metal modified carbon catalysts for oxygen reduction reaction (ORR) in the whole pH range is essential for energy conversion devices but still remains a challenge. Herein, the Fe/Fe₃C nanoparticles and Fe-N_X species anchored on the interconnected mesoporous carbon materials are fabricated through an economical and facile template-assisted polymerization-pyrolysis strategy. The catalyst exhibits unique features with the electronic interaction between Fe/Fe₃C and Fe−N_X, large specific surface area and high mesoporous structure as well as nitrogen doping in porous carbon skeletons, which can effectively catalyze ORR over the full pH range. In an alkaline electrolyte, the optimized catalyst displays favorable ORR performance with positive onset potential (E_onset = 0.91 V), half-wave potential (E_1/2 = 0.83 V), long-term cycles stability and methanol tolerance, exceeding those for the commercial Pt/C. Furthermore, the prepared catalyst could be directly assembled into the alkaline Zn−air battery that exhibits the open-circuit voltage of 1.44 V, high power density of 96.0 mW cm⁻² and long-term durability. Therefore, the template-assisted polymerization-pyrolysis strategy provides a promising route for designing high-performance non-noble metal decorated ORR electrocatalysts.

构建高效、耐用的非贵金属改性碳催化剂在整个 pH 范围内用于氧还原反应 (ORR) 对于能量转换装置至关重要，但仍然是一个挑战。在此，Fe/Fe ₃ C 纳米粒子和锚定在相互连接的介孔碳材料上的Fe-N _X物种是通过经济简便的模板辅助聚合热解策略制造的。该催化剂表现出独特的特性，即 Fe/Fe ₃ C 和 Fe-N _X之间的电子相互作用，大比表面积和高介孔结构以及多孔碳骨架中的氮掺杂，可以在整个pH范围内有效催化ORR。在碱性电解质中，优化后的催化剂显示出良好的 ORR 性能，具有正起始电位 ( E _onset  = 0.91 V)、半波电位 ( E _1/2  = 0.83 V)、长期循环稳定性和甲醇耐受性，超过了商业 Pt/C。此外，制备的催化剂可以直接组装成碱性锌空气电池，开路电压为1.44 V，功率密度为96.0 mW cm ^-2和长期的耐用性。因此，模板辅助聚合热解策略为设计高性能非贵金属装饰的 ORR 电催化剂提供了一条有前途的途径。