Heterostructure Engineering of NiCo‐LDHs for Enhanced Energy Storage Performance in Aqueous Zinc‐Ion Batteries

Abstract Aqueous zinc‐ion batteries (AZIBs) are considered a promising device for next‐generation energy storage due to their high safety and low cost. However, developing high−performance cathodes that can be matched with zinc metal anodes remains a challenge in unlocking the full potential of AZIBs. In this study, a typical transition metal layered double hydroxides (NiCo−LDHs) can be in situ reconstructed to NiCo−LDHs/Ni(Co)OOH heterostructure using an electrochemical cycling activation (ECA) method, serving as a novel cathode material for AZIBs. The optimized ECA−NiCo−LDHs cathode demonstrates a high capacity of 181.5 mAh g −1 at 1 A g −1 and retains 75% of initial capacity after 700 cycles at 5 A g −1 . The abundant heterointerfaces of the NiCo−LDHs/Ni(Co)OOH material can activate additional active sites for zinc‐ion storage and accelerate ion diffusion. Theoretical calculations also suggest the heterostructure can boost charge transfer and regulate ion−adsorption capability, thereby improving the electrochemical performance. Additionally, the flexible AZIBs device exhibits good service performance. This study on interface engineering introduces a new possibility for utilizing LDHs in AZIBs and offers a novel strategy for designing electrode materials.