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Vol. 17 (2025)

Zn(TFSI)2-Mediated Ring-Opening Polymerization for Electrolyte Engineering Toward Stable Aqueous Zinc Metal Batteries

https://doi.org/10.1007/s40820-025-01649-9
Zhenjie Liu
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, People’s Republic of China
Murong Xi
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, People’s Republic of China
Rui Sheng
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, People’s Republic of China
Yudai Huang
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, People’s Republic of China
Juan Ding
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, People’s Republic of China
Zhouliang Tan
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, People’s Republic of China
Jiapei Li
Department of Materials Science and Engineering & Center of Super‑Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong SAR, People’s Republic of China
Wenjun Zhang
Department of Materials Science and Engineering & Center of Super‑Diamond and Advanced Films, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong SAR, People’s Republic of China
Yonggang Wang
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Fudan University, Shanghai 200433, People’s Republic of China

Corresponding Author: Yonggang Wang

ygwang@fudan.edu.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 120

Abstract

Practical Zn metal batteries have been hindered by several challenges, including Zn dendrite growth, undesirable side reactions, and unstable electrode/electrolyte interface. These issues are particularly more serious in low-concentration electrolytes. Herein, we design a Zn salt-mediated electrolyte with in situ ring-opening polymerization of the small molecule organic solvent. The Zn(TFSI)2 salt catalyzes the ring-opening polymerization of (1,3-dioxolane (DOL)), generating oxidation-resistant and non-combustible long-chain polymer (poly(1,3-dioxolane) (pDOL)). The pDOL reduces the active H2O molecules in electrolyte and assists in forming stable organic–inorganic gradient solid electrolyte interphase with rich organic constituents, ZnO and ZnF2. The introduction of pDOL endows the electrolyte with several advantages: excellent Zn dendrite inhibition, improved corrosion resistance, widened electrochemical window (2.6 V), and enhanced low-temperature performance (freezing point =  − 34.9 °C). Zn plating/stripping in pDOL-enhanced electrolyte lasts for 4200 cycles at 99.02% Coulomb efficiency and maintains a lifetime of 8200 h. Moreover, Zn metal anodes deliver stable cycling for 2500 h with a high Zn utilization of 60%. A Zn//VO2 pouch cell assembled with lean electrolyte (electrolyte/capacity (E/C = 41 mL (Ah)−1) also demonstrates a capacity retention ratio of 92% after 600 cycles. These results highlight the promising application prospects of practical Zn metal batteries enabled by the Zn(TFSI)2-mediated electrolyte engineering.


Highlights:
1 A novel electrolyte enabled by Zn(TFSI)2-mediated ring-opening polymerization strategy for highly reversible aqueous zinc metal batteries was proposed.
2 The novel electrolyte has good antioxidant stability and non-inflammability.
3 The novel electrolyte widens the electrochemical window, improves the low-temperature performance, and inhibits Zn dendrite. The Zn metal anode shows an 8200 h lifespan at 1 mAh cm−2 and a 2500 h lifespan at 60% depth of discharge.

Keywords

Electrolyte engineering Ring-opening polymerization Lewis acid catalyst Zn metal battery
Liu, Zhenjie, Murong Xi, Rui Sheng, Yudai Huang, Juan Ding, Zhouliang Tan, Jiapei Li, Wenjun Zhang, and Yonggang Wang. 2025. “Zn(TFSI)2-Mediated Ring-Opening Polymerization for Electrolyte Engineering Toward Stable Aqueous Zinc Metal Batteries”. Nano-Micro Letters 17 (January):120. https://doi.org/10.1007/s40820-025-01649-9.
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