Rechargeable aqueous zinc–air
cells (ZACs) promise an extremely
safe and high energy technology. However, they are still significantly
limited by sluggish electrochemical kinetics and irreversibility originating
from the parasitic reactions of the bifunctional catalysts and electrolytes.
Here, we report the preferential in situ building
of interfacial structures featuring the edge sites constituted by
FeCo single/dual atoms with the integration of Co sites in the nitrogenized
graphitic carbon frameworks (FeCo SAs@Co/N-GC) by electronic structure
modulation approach. Compared to commercial Pt/C and RuO2, FeCo SAs@Co/N-GC reveals exceptional electrochemical performance,
reversible redox kinetics, and durability toward oxygen reduction
and evolution reactions under universal pH environments, i.e., alkaline,
neutral, and acidic, due to synergistic effect at interfaces and preferred
charge/mass transfer. The aqueous (alkaline, nonalkaline, and acidic
electrolytes) ZACs constructed with a FeCo SAs@Co/N-GC cathode tolerate
stable operations, have significant reversibility, and have the highest
energy densities, outperforming those of noble metal counterparts
and state-of-the-art ZACs in the ambient atmosphere. Additionally,
flexible solid-state ZACs demonstrate excellent mechanical and electrochemical
performances with a highest power density of 186 mW cm–2, specific capacity of 817 mAh gZn
–1, energy density of 1017 Wh kgZn
–1,
and cycle life >680 cycles with extremely harsh operating conditions,
which illustrates the great potential of triphasic catalyst for green
energy storage technologies.