Jinlong Zhang, Qing Wu, Xiude Liu, Song Yang, Fusheng Luo, Zeyu Yan, Jun Huang, Yiwang Chen
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.