High‐Entropy Aqueous Electrolyte Induced Formation of Water‐Poor Zn 2+ Solvation Structures and Gradient Solid‐Electrolyte Interphase for Long‐Life Zn‐Metal Anodes

Abstract Electrolyte engineering has emerged as an effective strategy for stabilizing Zn‐metal anodes. However, a single solute or solvent additive is far from sufficient to meet the requirements for electrolyte cycling stability. Here, we report a new‐type high‐entropy electrolyte composed of equal molar amounts of Zn(OTf) 2 and LiOTf, along with equal volumes of H 2 O, triethyl phosphate, and dimethyl sulfoxide, which enhances electrolyte stability by increasing solvation entropy. Specifically, this well‐designed high‐entropy electrolyte reduces the content of solvated and free water molecules while forming a robust gradient solid‐electrolyte interphase on the Zn anode surface, protecting the Zn anode from…

• NN
  National Natural Science Foundation of China

  Award: T2422028 and 52473270
• FR
  Fundamental Research Funds for the Central Universities

  Award: No. 2024300440