| Summary: | Abstract Single‐atomic transition metal–nitrogen–carbon (M–N–C) structures are promising alternatives toward noble‐metal‐based catalysts for oxygen reduction reaction (ORR) catalysis involved in sustainable energy devices. The symmetrical electronic density distribution of the M─N4 moieties, however, leads to unfavorable intermediate adsorption and sluggish kinetics. Herein, a Fe–N–C catalyst with electronic asymmetry induced by one nearest carbon vacancy adjacent to Fe─N4 is conceptually produced, which induces an optimized d‐band center, lowered free energy barrier, and thus superior ORR activity with a half‐wave potential (E1/2) of 0.934 V in a challenging acidic solution and 0.901 V in an alkaline solution. When assembled as the cathode of a Zinc–air battery (ZAB), a peak power density of 218 mW cm−2 and long‐term durability up to 200 h are recorded, 1.5 times higher than the noble metal‐based Pt/C+RuO2 catalyst. This work provides a new strategy on developing efficient M–N–C catalysts and offers an opportunity for the real‐world application of fuel cells and metal–air batteries.
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