High-entropy solvation chemistry towards affordable and practical Ah-level zinc metal battery

Linhui Chang, Hongwei Cheng (), Jiamin Li, Lei Zhang, Bomian Zhang, Liheng Zheng, Qiangchao Sun, Jiantao Li, Xionggang Lu () and Kangning Zhao ()
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Linhui Chang: Shanghai University
Hongwei Cheng: Shanghai University
Jiamin Li: Shanghai University
Lei Zhang: Wuhan University of Technology
Bomian Zhang: Wuhan University of Technology
Liheng Zheng: Wuhan University of Technology
Qiangchao Sun: Shanghai University
Jiantao Li: Northwestern University
Xionggang Lu: Shanghai University
Kangning Zhao: Great Bay University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Aqueous zinc-ion batteries offer sustainable large-scale storage potential with inherent safety and low cost, yet suffer from limited energy density and cycle life due to aqueous electrolyte constraints. Here, we introduce affordable, stable electrolyte (0.33 $·kg−1) incorporating minimal multi-halogen anions (Cl−, Br−, and I−) to create a high-entropy solvation structure enabling high-performance zinc batteries. Despite the small amount, the diversified mono-halogenated contact ion pair and multi-halogenated aggregate solvation structures create the unique high-entropy solvation structure, to form the lean-water halogenated interfacial environment, suppressing the hydrogen evolution reaction, while facilitating cascade desolvation. Multi-halogen additives generate diverse contact ion pairs (Zn-X, X = Cl/Br/I) with compact solvation shells accelerating ion transport. In this way, the high-entropy solvation structure breaks the trade-off between plating overpotential (energy efficiency) and plating/stripping reversibility (Coulombic efficiency). As a result, the high-entropy solvation-based electrolyte enables practical zinc metal battery with 152.2 Wh kg−1electrode for 120 cycles at lean electrolyte of 2.4 μL mg−1 and an Ah-level pouch cell is validated with high Coulombic efficiency of over 99.90% for over 250 cycles. Our findings emphasize the importance of electrolyte design for the precise control of anion-cation interactions for stable Zn/electrolyte interface and enable practical zinc metal battery with high energy and low cost.

Date: 2025
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DOI: 10.1038/s41467-025-61456-z

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