Issue

Vol. 17 (2025)

Electrode/Electrolyte Optimization-Induced Double-Layered Architecture for High-Performance Aqueous Zinc-(Dual) Halogen Batteries

https://doi.org/10.1007/s40820-024-01551-w
Chengwang Zhou
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
Zhezheng Ding
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
Shengzhe Ying
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
Hao Jiang
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
Yan Wang
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
Timing Fang
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
You Zhang
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
Bing Sun
Centre for Clean Energy Technology, School of Mathematical and Physical Sciences, Faculty of Science, University of Technology Sydney, Ultimo, NSW 2007, Australia
Xiao Tang
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China
Xiaomin Liu
School of Textiles and Clothing, School of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Shandong, People’s Republic of China

Corresponding Author: Xiaomin Liu

liuxiaomin@qdu.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 58

Abstract

Aqueous zinc-halogen batteries are promising candidates for large-scale energy storage due to their abundant resources, intrinsic safety, and high theoretical capacity. Nevertheless, the uncontrollable zinc dendrite growth and spontaneous shuttle effect of active species have prohibited their practical implementation. Herein, a double-layered protective film based on zinc-ethylenediamine tetramethylene phosphonic acid (ZEA) artificial film and ZnF2-rich solid electrolyte interphase (SEI) layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization. The ZEA-based artificial film shows strong affinity for the ZnF2-rich SEI layer, therefore effectively suppressing the SEI breakage and facilitating the construction of double-layered protective film on the zinc metal anode. Such double-layered architecture not only modulates Zn2+ flux and suppresses the zinc dendrite growth, but also blocks the direct contact between the metal anode and electrolyte, thus mitigating the corrosion from the active species. When employing optimized metal anodes and electrolytes, the as-developed zinc-(dual) halogen batteries present high areal capacity and satisfactory cycling stability. This work provides a new avenue for developing aqueous zinc-(dual) halogen batteries.


Highlights:
1 A double-layered protective film based on zinc-based coordination compound and ZnF2-rich solid electrolyte interphase layer has been successfully fabricated on the zinc metal anode via electrode/electrolyte synergistic optimization.
2 The double-layered architecture can effectively modulate Zn2+ flux and suppress the zinc dendrite growth, thus facilitating the uniform zinc deposition.
3 The as-developed zinc-(dual) halogen batteries based on double-layered protective film can present high areal capacity and satisfactory cycling stability.

Keywords

Zn metal anodes Double-layered protective film Electrode/electrolyte optimization Aqueous zinc-(dual) halogen batteries
Zhou, Chengwang, Zhezheng Ding, Shengzhe Ying, Hao Jiang, Yan Wang, Timing Fang, You Zhang, Bing Sun, Xiao Tang, and Xiaomin Liu. 2024. “Electrode/Electrolyte Optimization-Induced Double-Layered Architecture for High-Performance Aqueous Zinc-(Dual) Halogen Batteries”. Nano-Micro Letters 17 (November):58. https://doi.org/10.1007/s40820-024-01551-w.
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