Rational Electrolyte Structure Engineering for Highly Reversible Zinc Metal Anode in Aqueous Batteries

Aqueous zinc-ion batteries (AZIBs) have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety, cost-effectiveness, and competitive gravimetric energy density. However, their practical commercialization is hindered by critical challenges on the anode side, including dendrite growth and parasitic reactions at the anode/electrolyte interface. Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode. In this review, we systematically summarize state-of-the-art strategies for electrolyte optimization, with a particular focus on the zinc salts regulation, electrolyte additives, and the construction of novel electrolytes, while elucidating the underlying design principles. We further discuss the key structure-property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes. Finally, future perspectives on advanced electrolyte design are proposed. This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.