Electrolyte Tuned Robust Interface toward Fast‐Charging Zn–Air Battery with Atomic Mo Site Catalyst

Abstract Stable operation of sustainable Zn–air batteries (ZABs) has attracted considerable attention, but it remains a huge challenge to achieve temperature‐adaptive and fast‐charging ZABs. The poor Zn | electrolyte interface and the sluggish charging kinetic are the major obstacles. Here, high‐performance ZABs are constructed by designing polarized zincophilic solid‐state electrolyte (SSE) with the unique solvation interaction of Zn 2+ with ethylene glycol (EG), and atomic Mo site cathode catalyst. On the one hand, the modulation of the solvation structure of Zn 2+ ions by partial substitution of H 2 O with EG inhibits Zn dendrite growth and parasitic reactions, leading to the improvement of the Zn | electrolyte interface. Moreover, the polarized terminal groups in SSE are strongly coordinated with Zn/H 2 O, which exerts a profound influence on Zn | electrolyte interface stability and low‐temperature properties. On the other hand, atomic Mo incorporated α‐Co(OH) 2 mesoporous nanosheets decrease the overpotential of oxygen evolution reaction via strong electronic interaction. Consequently, the assembled aqueous ZABs exhibit ten‐time fast‐charging ability and remarkable cycling stability. Moreover, the assembled solid‐state ZABs show unprecedented stability (1400 cycles at 5 mA cm −2 ) and high energy efficiency at −40 °C.