The design of temperature-adaptive Zn-air batteries (ZABs) with long life spans and high energy efficiencies is challenging owing to sluggish oxygen reduction reaction (ORR) kinetics and an unstable Zn/electrolyte interface. Herein, a quasi-solid-state ZAB is designed by combining atomically dispersed Fe-N-C catalysts containing pyridinic N vacancies (FeNC-V) with a polarized organo-hydrogel electrolyte. First-principles calculation predicts that adjacent V sites effectively enhance the covalency of Fe-N moieties and moderately weaken *OH binding energies, significantly boosting the ORR kinetics and stability.
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