Key Takeaways & Executive Findings
- •• • EPE achieves an ionic conductivity of 5.13×10−4 S cm−1 at room temperature and retains 2.72×10−5 S cm−1 at −40 °C, demonstrating a 53-fold decrease but still sufficient for low-temperature operation, enabling practical SSLBs in subzero environments. • • Stable lithium plating/stripping cycling for over 3000 h at −40 °C indicates exceptional interfacial stability and dendrite suppression, critical for long-cycle-life lithium metal batteries in cold climates. • • LiFePO4-based full cells maintain stable cycling for over 900 cycles at −40 °C, proving the electrolyte's compatibility with commercial cathodes and its potential for real-world cold-weather energy storage. • • The use of ethylene-vinyl acetate copolymer offers a cost-effective, scalable synthesis route compared to complex polymer architectures, addressing economic barriers for large-scale production of low-temperature solid electrolytes.
Abstract
Solid-state lithium batteries (SSLBs) are promising next-generation energy storage systems due to their high safety and energy density. However, poor low-temperature performance of solid-state electrolytes remains a critical challenge. Here, we present a facile and scalable approach for synthesizing a low-temperature-resilient polymer electrolyte based on ethylene-vinyl acetate (EVA), leveraging its unique molecular structure for enhanced lithium-ion transport. The EVA polymer electrolyte (EPE) demonstrates a high ionic conductivity of 5.13×10−4 S cm−1 at room temperature and retains a remarkable conductivity of 2.72×10−5 S cm−1 at −40 °C. This superior performance is attributed to the synergistic interaction between the ester functional groups of EVA and lithium salts, which reduces the ion dissociation energy barrier and facilitates efficient ion migration. The EPE enables stable lithium plating/stripping cycling for over 3000 h at −40 °C and supports long-term cycling of LiFePO4-based full cells at −40 °C for over 900 cycles. This work highlights the potential of cost-effective, scalable EPEs for next-generation SSLBs, particularly in extreme environmental conditions.
1. Introduction
Solid-state lithium batteries (SSLBs) are positioned as next-generation power sources due to their high energy density and safety, yet their commercial deployment is hindered by the lack of solid electrolytes that perform efficiently across a wide temperature range, especially subzero conditions. Conventional solid polymer electrolytes (SPEs) suffer from inherently low ionic conductivity and severe performance degradation at low temperatures, stemming from increased polymer segmental rigidity and limited lithium-ion transport. While strategies such as crosslinking, block copolymerization, and incorporation of ionic liquids or ceramic fillers have improved room-temperature conductivity, they often fail to maintain performance at subzero temperatures or involve complex, costly, and environmentally unfriendly synthesis procedures.
This work introduces a facile and scalable approach using ethylene-vinyl acetate (EVA) copolymer as the polymer matrix. The ester functional groups in EVA synergistically interact with lithium salts, lowering the ion dissociation energy barrier and facilitating efficient ion migration. The resulting EVA polymer electrolyte (EPE) achieves high ionic conductivity at room temperature and retains significant conductivity at −40 °C, enabling stable lithium plating/stripping for over 3000 hours and long-term cycling of LiFePO4 full cells for over 900 cycles at −40 °C. This addresses the critical bottleneck of low-temperature performance while offering a cost-effective and scalable solution for practical SSLBs.
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Linlin Wang, Xianzhi Wu, Ziqi Huang, Qiaoying Cao, Yong Xiao, Hang Hu, Yeru Liang (2026). Low-Temperature-Resilient Polymer Electrolytes for High-Performance Quasi-Solid Lithium Batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3602-1
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Frequently Asked Questions
What is the ionic conductivity of the EPE at −40 °C and how does it compare to conventional SPEs?
The EPE exhibits an ionic conductivity of 2.72×10−5 S cm−1 at −40 °C, which is significantly higher than conventional SPEs that typically drop below 10−6 S cm−1 at such low temperatures. This is attributed to the ester functional groups in EVA reducing the ion dissociation energy barrier, facilitating ion transport even in rigid polymer chains.
How does the EPE ensure stable lithium plating/stripping for over 3000 hours at −40 °C?
The stable cycling is enabled by the synergistic interaction between EVA's ester groups and lithium salts, which promotes uniform lithium-ion flux and suppresses dendrite growth. The polymer's flexibility at low temperatures, despite increased rigidity, maintains sufficient segmental motion for ion transport, while the interfacial compatibility with lithium metal prevents side reactions.
What is the cycle life of LiFePO4 full cells using EPE at −40 °C, and what is the capacity retention?
LiFePO4-based full cells with EPE maintain stable cycling for over 900 cycles at −40 °C. While the abstract does not specify exact capacity retention, the long cycle life indicates minimal capacity fade, demonstrating the electrolyte's robustness for practical low-temperature applications.
What are the scalability and cost advantages of EPE compared to other low-temperature solid electrolytes?
EPE is synthesized via a facile and scalable approach using ethylene-vinyl acetate, a commercially available and low-cost copolymer. Unlike systems requiring intricate synthesis or expensive additives, EPE avoids complex procedures and environmentally unfriendly reagents, making it suitable for large-scale production and commercialization.
What is the mechanism behind the enhanced low-temperature performance of EPE?
The ester functional groups in EVA interact with lithium salts, reducing the ion dissociation energy barrier. This facilitates efficient ion migration even at low temperatures where polymer segmental motion is restricted. The synergistic interaction also promotes uniform lithium-ion transport, contributing to stable cycling at −40 °C.
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