Aqueous Zn-ion batteries (AZIBs), being safe, inexpensive,
and
pollution-free, are a promising candidate for future large-scale sustainable
energy storage. However, in a conventional AZIBs setup, the Zn metal
anode suffers oxidative corrosion, side reactions with electrolytes,
disordered dendrite growth during operation, and consequently low
efficiency and short lifespan. In this work, we discover that purging
CO2 gas into the electrolyte could address these issues
by eliminating dissolved O2, inhibiting side reactions
by buffering the local pH change, and preventing dendrite growth by
inducing the in situ formation of a ZnCO3 solid electrolyte
interphase layer. Moreover, the CO2-purged electrolyte
could enable a highly reversible plating/stripping behavior with a
high Coulombic efficiency of 99.97% and an ultralong lifespan of 32,000
cycles (1600 h) even under an ultrahigh current density of 40 mA cm–2. Consequently, the CO2-purged symmetrical
cells deliver long cycling stability at a high depth of discharge
of 57%, while the CO2-purged Zn/V2O5 full cells exhibit outstanding capacity retention of 66% after 1000
cycles at a high current density of 5 A g–1. Our
strategy, the simple introduction of CO2 gas into the electrolyte,
could effectively mediate the zinc anode’s critical issues
and provide a scalable and cost-effective pathway for the commercialization
of AZIBs.