Abstract
The sluggish oxygen reduction/evolution reaction (ORR/OER) at the oxygen electrode has significantly hindered the development of Zn-air batteries. Modulating single-atom active sites with neighboring atoms is an effective strategy to enhance ORR/OER activity. Herein, an ordered assembly strategy is employed to anchor FeN4 sites onto hollow carbon nanospheres and then Mn atoms are introduced to modulate the FeN4 sites to construct a electrocatalyst (Fe,Mn-HCNS). Theoretical simulations reveal that neighboring Mn atoms induces a negative shift in the d-band center of Fe, thereby optimizing the adsorption–desorption of key oxygenated intermediates and accelerating ORR/OER kinetics. In addition, the introduction of Mn atoms optimizes the energy barrier for Fe dissolution, which inhibits the demetalation of the FeN4 site. The assembled aqueous Zn-air battery demonstrates ultrahigh open-circuit voltage (1.55 V) and outstanding durability (2000 h at 10 mA cm−2). This work provides an insightful prospect for neighboring Mn atoms in enhancing oxygen electrocatalytic activity at FeN4 sites, thereby advancing the development of superior electrocatalysts.
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