Improving Zn anode electrochemical reversibility via crystallographic plane regulation by polyethylene glycol electrolyte additive

• Published in: Journal of solid state electrochemistry Vol. 28; no. 9; pp. 3209 - 3219
• Main Authors: Li, Xiaogang, Zhou, Yanhui, Tu, Huan, Wang, Zongnan, Wu, Rui, Lu, Yaokang, Zong, Yujie, Liu, Qian, He, Jie, Qian, Li, Song, Siyu, Zhang, Yixian, Meng, Chunfeng, Yuan, Aihua
• Format: Journal Article
• Language: English
• Published: Berlin/Heidelberg Springer Berlin Heidelberg 01.09.2024; Springer Nature B.V
• Subjects: Analytical Chemistry; Aqueous electrolytes; Characterization and Evaluation of Materials; Chemistry; Chemistry and Materials Science; Condensed Matter Physics; Copper; Corrosion mechanisms; Crystallography; Deposition; Electrochemistry; Electrolytes; Electrolytic cells; Energy Storage; Hydrogen evolution reactions; Molecular structure; Nucleation; Original Paper; Physical Chemistry; Plating; Polyethylene glycol; Solvation; Texturing; Zinc; Dendrite suppression; Electrolyte additive; Aqueous zinc-ion batteries; Polyethylene glycol; Reversibility enhancement
• ISSN: 1432-8488; 1433-0768
• DOI: 10.1007/s10008-024-05901-x

Aqueous zinc-ion batteries (AZIBs) are considered promising candidates for scalable and sustainable energy storage devices due to their low cost and high safety advantages. However, the practical application of AZIBs is subject to the limits of the reversibility of the Zn 2+ stripping/plating, such as the growth of Zn dendrites, corrosion of Zn anode, and hydrogen evolution reaction (HER). Herein, we propose a solution to the issues of AZIBs by creating a versatile electrolyte via the addition of polyethylene glycol (PEG). PEG additive changes the coordination environment of Zn 2+ and disturbs the solvation structure of H 2 O, which is beneficial to alleviate the side reactions triggered by water molecules in the Zn 2+ solvation structure. In addition, the Zn 2+ nucleation behavior is optimized by texturing the hexagonal deposition plane and inducing the compact-grained deposition manner to resist corrosion reactions and dendrite aggravation. The solvation structure of Zn 2+ is optimized to improve the reversibility of the Zn anode. As a result, improved reversibility of Zn plating/stripping on the Cu-working electrode is achieved by 20% PEG electrolyte with high Coulombic efficiency (CE) of 99.43% at 1 mA cm −2 , stably cycled for 750 cycles. Furthermore, the Zn||Zn symmetrical half-cell with 20% PEG electrolyte shows stable plating/stripping overpotentials for more than 1400 h. Finally, the Zn||V 2 O 5 full-cells exhibit excellent long cycling stability for over 180 cycles even at 1000 mA g −1 with a high reversible capacity of 168 mAh g −1 . This work provides valuable insights into designing electrolytes for aqueous zinc metal batteries.