Hybrid Fe‐N‐C Catalyst Integrating Single‐Atom Fe and Nanoscale CeO ₂ towards Efficient Oxygen Reduction Reaction for Zinc‐Air Batteries ^†

Comprehensive Summary Developing high‐performance, durable, and cost‐effective oxygen reduction reaction (ORR) catalysts is essential for advancing next‐generation energy devices like zinc‐air batteries (ZABs). Herein, we engineer a hybrid Fe‐N‐C catalyst (FeSA‐Fe NP /CeO 2 @NC) integrating atomically dispersed Fe‐N x sites, Fe nanoparticles, and oxygen vacancy‐rich CeO 2 nanoparticles within a nitrogen‐doped carbon matrix. Interfacial charge transfer and oxygen vacancy‐mediated electron redistribution, synergistically enhanced by strong metal‐support interactions (SMSI), optimize the electronic configuration of Fe‐N x sites and reduce their electron density. The resulting catalyst exhibits exceptional ORR activity and stability, featuring a half‐wave potential of 0.925 V (vs. RHE) in alkaline media and minimal degradation (1% and 2.8% negative shifts after 10,000/20,000 cycles). In ZABs, it achieves a peak power density of 310.29 mW·cm –2 while sustaining stable operation for over 600 h. This work demonstrates dual role of CeO 2 in enhancing activity and stability, establishing a design principle for high‐performance electrocatalysts in energy conversion systems.