Proton-Dominated Reversible Aqueous Zinc Batteries with an Ultraflat Long Discharge Plateau

Aqueous zinc batteries (AZBs) are considered promising candidates for large-scale energy storage systems because of their low cost and high safety. However, currently developed AZB cathodes always suffer from the intense charge repulsion of multivalent-ion and complex multiphase electrochemistry, resulting in an insufficient cycling life and impracticable high-sloping discharge profile. Herein, we found that the synthesized ultrathin Bi₂O₂Se nanosheets can effectively activate stable protons storage in AZBs rather than large zinc ions. This proton-dominated cathode provides an ultraflat discharge plateau (72% capacity proportion) and exhibits long-term cyclability as 90.64% capacity retention after 2300 cycles at 1 A g^-1. Further in situ synchrotron X-ray diffraction, ex situ X-ray photoelectronic spectroscopy, and density functional theory confirm the energy storage mechanism regarding the highly reversible proton insertion/extraction process. Benefiting from the proton-dominated fast dynamics, reliable energy supply (>81.5% discharge plateau capacity proportion) is demonstrated at a high rate of up to 10 A g^-1 and in the frozen electrolyte below -15 °C. This work provides a potential design of high-performance electrode materials for AZBs.