Achieving high-rate and durable aqueous rechargeable Zn-Ion batteries by enhancing the successive electrochemical conversion reactions.

The mild electrolyte working environment of rechargeable aqueous Zn-ion batteries (AZIBs) features its promising characteristic and potential application for large-scale energy storage system. However, the poor cycling stability significantly hinders the broad application of AZIBs due to the complex electrochemical conversion reactions during charge-discharge process. Herein, we propose a strategy to improve the electrochemical performance of AZIB by enhancing the successive electrochemical conversion reactions. With a rational design of electrode, an even homogeneous electric field can be achieved in the cathode side, resulting to significantly enhanced efficiency of successive electrochemical conversion reactions. Charge storage mechanism studies reveal that the reversibility behaviors of byproducts alkaline zinc sulfate (ZHS) can dramatically determine the H/Zn de/intercalation process, and a high reversibility characteristic ensures the facilitated electrochemical kinetics. As expected, the resultant AZIB possesses outstanding electrochemical performance with a high specific capacity of 425.08 mAh⋅g at 0.1 A⋅g, an excellent rate capacity of about 60% (246.6 mAh⋅g at 1 A⋅g) and superior cycling stability of 93.7% after 3000 cycles (at 3 A⋅g). This effective strategy and thinking proposed here may open a new avenue for the development of high-performing AZIBs.