Microenvironment regulation of anode-electrolyte interface enables highly stable Zn anodes

Lin Peng, Xincheng Liang, Zelong Sun, Xingfa Chen, Dexin Meng, Renshu Huang, Qian Liu, Huan Wen, Shibin Yin*

Chin. J. Struct. Chem., 2025, 44(4), 100542. DOI: 10.1016/j.cjsc.2025.100542

April 1, 2025

Aqueous zinc ion batteries; Zn anodes; Electrolyte additives; Anode-electrolyte interface; Capture effect; pH buffer

ABSTRACT

H2O-induced side reactions and dendrite growth occurring at the Zn anode-electrolyte interface (AEI) limit the electrochemical performances of aqueous zinc ion batteries. Herein, methionine (Met) is introduced as an electrolyte additive to solve the above issues by three aspects: Firstly, Met is anchored on Zn anode by amino/methylthio groups to form an H2O-poor AEI, thus increasing the overpotential of hydrogen evolution reaction (HER); secondly, Met serves as a pH buffer to neutralize the HER generated OH, thereby preventing the formation of by-products (e.g. Zn4SO4(OH)6xH2O); thirdly, Zn2+ could be captured by carboxyl group of the anchored Met through electrostatic interaction, which promotes the dense and flat Zn deposition. Consequently, the Zn||Zn symmetric cell obtains a long cycle life of 3200 h at 1.0 mA cm−2, 1.0 mAh cm−2, and 1400 h at 5.0 mA cm−2, 5.0 mAh cm−2. Moreover, Zn||VO2 full cell exhibits a capacity retention of 91.0% after operating for 7000 cycles at 5.0 A g−1. This study offers a novel strategy for modulating the interface microenvironment of AEI via integrating the molecular adsorption, pH buffer, and Zn2+ capture strategies to design advanced industrial-oriented batteries.

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