Hierarchically Ordered Macro‐/Mesoporous N,P‐Codoped Carbon with Fe‐Co Dual Sites for Efficient Electrocatalytic Oxygen Reduction

The development of high-performance, low-cost non-precious-metal electrocatalysts as alternatives to Pt-based catalysts for the oxygen reduction reaction (ORR) is crucial for promoting the commercial application of fuel cells and metal-air batteries. In this work, we report a novel type of ORR electrocatalyst with Fe and Co sites anchored on N,P-codoped hierarchically ordered macro-/mesoporous carbon (FeCo/NP-HOMMC) through a facile one-pot, controllable synthesis method with the aid of dual-templating technique. The FeCo/NP-HOMMC catalyst shows robust ORR performance under alkaline conditions with a half-wave potential (E_1/2) of 0.90 V vs. reversible hydrogen electrode (RHE), significantly surpassing the commercial 20 wt% Pt/C catalyst, while also exhibiting remarkable long-term stability and great methanol tolerance. Control experiments reveal that the superior performance of the FeCo/NP-HOMMC catalyst for ORR benefits from the synergistic catalysis of highly dispersed Fe and Co dual active sites, and the advantages of the unique hierarchically ordered macro-/mesoporous structure, which can provide improved active site accessibility, excellent conductivity, and maximized mass/charge transport.