Key Takeaways & Executive Findings
- •• A novel Zn(TFSI)2-mediated ring-opening polymerization strategy creates a pDOL-based electrolyte that significantly enhances the stability and reversibility of aqueous zinc metal batteries. • The pDOL electrolyte exhibits excellent antioxidant stability, non-flammability, a widened electrochemical window (2.6 V), and a low freezing point (−34.9 °C), enabling superior low-temperature performance. • The electrolyte effectively inhibits Zn dendrite growth and corrosion, leading to an ultra-long lifespan of 8200 h at 1 mAh cm−2 and 2500 h at 60% depth of discharge. • A Zn//VO2 pouch cell with lean electrolyte achieves 92% capacity retention after 600 cycles, demonstrating practical viability for high-energy-density energy storage.
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.
1. Introduction
Zn metal batteries have the advantages of high theoretical specific capacity, low cost, and high safety, making them a promising alternative to lithium-ion batteries for electrochemical energy storage applications [1]. Though the studies of Zn metal batteries in the laboratory have demonstrated enhanced cycle life, energy density, and power density, the performance of Zn metal batteries in practical settings has not met expectations [2, 3]. The main bottlenecks constraining the use of Zn metal batteries in practical applications include (i) Zn dendrite growth which leads to internal short circuits and safety issues [3]; (ii) low utilization of Zn metal anode, giving rise to reduced capacity and energy density [4, 5]; (iii) poor electrolyte stability that results in low Coulomb efficiency (CE), cell bulking, and the formation of passivation products on the Zn surface. These side effects are more severe under practical conditions, such as high depth of discharge (DOD), low negative/positive (N/P) ratios, and intermittent conditions [4, 6]; and (iv) high concentration and high dosage of electrolyte that significantly increases the battery cost and reduces the overall energy density [7].
The rational design of the electrolyte solvation structure is one of the key means to simultaneously address these challenges [8–11]. H2O in the electrolyte is a double-edged sword: It ensures the safety and excellent ion transport kinetics, but its low thermodynamic stability and highly dynamic and disordered solvation structure around Zn2+ can lead to electrolyte decomposition and formation of by-products [12]. These by-products are often loose and difficult to transport ions, ultimately deteriorating battery performance. Therefore, to achieve high capacity and long life of Zn metal batteries, it is necessary to precisely control the amount of free H2O in the electrolyte and regulate the solvation structure of Zn2+. At the same time, it is also essential to accurately regulate the structure and composition of solid electrolyte interphase (SEI) to meet the needs of practical Zn metal batteries.
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Zhenjie Liu, Murong Xi, Rui Sheng, Yudai Huang, Juan Ding, Zhouliang Tan, Jiapei Li, Wenjun Zhang, Yonggang Wang (2025). Zn(TFSI)2-Mediated Ring-Opening Polymerization for Electrolyte Engineering Toward Stable Aqueous Zinc Metal Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01649-9
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Frequently Asked Questions
What is the main innovation of this study?
The study introduces a Zn(TFSI)2-mediated ring-opening polymerization strategy to create a pDOL-based electrolyte, which significantly improves the stability and performance of aqueous zinc metal batteries.
How does the pDOL electrolyte improve battery performance?
The pDOL electrolyte reduces active water molecules, forms a stable SEI, inhibits dendrite growth, widens the electrochemical window, and enhances low-temperature performance, leading to longer cycle life and higher efficiency.
What are the key performance metrics achieved?
The electrolyte enables 4200 cycles with 99.02% Coulombic efficiency, 8200 h lifespan at 1 mAh cm−2, 2500 h at 60% DOD, and a pouch cell with 92% capacity retention after 600 cycles.
What is the significance of the low freezing point?
The freezing point of −34.9 °C allows the battery to operate at low temperatures, expanding its practical application range.
How does this work contribute to practical Zn metal batteries?
By addressing key challenges like dendrite growth and side reactions, this electrolyte engineering approach enables high utilization, long lifespan, and lean electrolyte conditions, making Zn metal batteries more viable for real-world energy storage.
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