Entropy regulation induced hollow prismatic structural NiCoFeInZnV-based layered double hydroxide with prominent electrochemical kinetics and stability for aqueous zinc-ion batteries

Layered double hydroxides (LDHs) hold great promise as cathode materials for aqueous zinc-ion batteries (AZIBs). Nevertheless, they also face challenges of sluggish kinetics and rapid capacity loss. Herein, a conformational entropy regulation strategy has been applied to surmount the shortcomings. A medium-entropy iron-based metal organic framework (MIL-88) derived NiCoFeInZnV-based layered double hydroxide with carbon loaded (ME-NiCoFeInZnV-LDH/C) has been first proposed and prepared with a designed method. The increased entropy optimizes electron conductivity and alleviates structure alteration and diffusion barrier during interactions with charge carriers, due to electron-induced effect and “cocktail” effect. Moreover, the nanosheet assembled hollow prismatic structures could homogenize flux distribution and electric field distribution. Therefore, the electrochemical kinetics, crystal structure stability, and activity could be dramatically improved. Leveraging the advantages of structure and composition regulation, Zn||ME-NiCoFeInZnV-LDH/C zinc battery delivers high specific capacities, rate performance, and cycling stability. This work proposes a novel and feasible medium-entropy strategy to prepare a high-performance cathode for advanced AZIBs, which is of prominent significance for the development of charge storage devices.