Coordination‐etching fabrication of ZIF‐67‐derived nickel–cobalt layered double hydroxides for aqueous Ni‐Zn batteries

Abstract Aqueous zinc‐based batteries (ZBBs) are promising for grid‐scale energy storage owing to their safety and cost‐effectiveness; however, their practical application is hindered by rapid capacity fading and unstable cathodes caused by sluggish Zn 2+ kinetics and structural degradation in alkaline electrolytes. Herein, to address these challenges, we utilize amphiphilic polymer (PVP) to realize the composite of nickel‐based complexes and ZIF‐67. The hierarchical nickel–cobalt layered double hydroxide (NiCo‐LDH) was prepared by metal ion exchange strategy. PVP‐mediated‐mediated suppression of agglomeration, combined with Ni 2+ ‐induced framework reconstruction, synergistically modulated the morphology, resulting in mesoporous nanosheets with hydroxyl‐rich surfaces. This design generated high‐valence Co 3+ species through charge‐compensation‐driven oxidation, thereby significantly accelerating Zn 2+ ion diffusion and reducing the interfacial resistance. The optimized NiCo‐LDH‐100 cathode (Ni:Co = 3:1) achieves cycling stability and exceptional energy/power densities (0.49 mWh cm –2 /49.1 mW cm –2 ). This study provides a solution for the cathode instability of Ni‐Zn batteries through a coordination‐derivatization strategy, which is promising for advancing sustainable energy storage technologies.