Nanomicellar Electrolyte Enables Highly Reversible Zinc Anode Via Strengthening Symmetric Plating/Stripping Chemistry

Abstract Zinc (Zn) metal anodes have garnered significant attentions for their applications in aqueous Zn‐ions batteries (AZIBs), but the electrochemical plating/stripping chemistry and failure mechanism under multifactorial conditions remain ambiguous, and the reversibility is overestimated under the single condition. Herein, a reversibility indicator ( R i ) based on the characteristic crystallization peaks is proposed to evaluate the plating/stripping chemistry and understand the reversibility, particularly in Zn//Cu asymmetric cells. Moreover, a nanomicellar electrolyte composing sodium dodecyl sulfate and curcumin has been designed, which encapsulates Zn 2+ within the nanodomain structure via the strong coordination interaction between β ‐diketone moiety of curcumin molecules and Zn 2+ , leading to the controlled Zn 2+ release and enhancing Zn 2+ transfer kinetics for the dense Zn deposition. Additionally, the initial consecutive hydrogen bonding network is disrupted, thereby suppressing the hopping transport of protons for interfacial side reactions. As a result, the Zn//Zn cell delivers a stable cycling up to 3800 h, a high discharge of depth with 28.5% for over 1200 h, and the Zn//Cu cell with low R i value (0.87) exhibits highly reversible cycling for 1418 h at 5 mA cm −2 . This study provides an innovative insight into promoting the symmetric Zn plating/stripping chemistry for highly reversible AZIBs.