Integrated energy storage and CO₂ conversion using an aqueous battery with tamed asymmetric reactions

Developing a CO₂-utilization and energy-storage integrated system possesses great advantages for carbon- and energy-intensive industries. Efforts have been made to developing the Zn-CO₂ batteries, but access to long cycling life and low charging voltage remains a grand challenge. Here we unambiguously show such inefficiencies originate from the high-barrier oxygen evolution reaction on charge, and by recharging the battery via oxidation of reducing molecules, Faradaic efficiency-enhanced CO₂ reduction and low-overpotential battery regeneration can be simultaneously achieved. Showcased by using hydrazine oxidation, our battery demonstrates a long life over 1000 hours with a charging voltage as low as 1.2 V. The low charging voltage and formation of gaseous product upon hydrazine oxidation are the key to stabilize the catalyst over cycling. Our findings suggest that by fundamentally taming the asymmetric reactions, aqueous batteries are viable tools to achieve integrated energy storage and CO₂ conversion that is economical, highly energy efficient, and scalable.