Key Takeaways & Executive Findings
- •• • The PEG-mediated asymmetric interchain interaction disrupts the ordered ANF hydrogen-bond network, suppressing inert aggregate formation and enhancing Li+ transport efficiency, as evidenced by stable Li||Li cycling for over 1600 h with low polarization voltage. • • The composite electrolyte retains a yield stress of 3.25 MPa, ensuring mechanical robustness against lithium dendrite penetration, a critical requirement for safe all-solid-state batteries. • • In LCO||Li cells at 65 °C, the modified electrolyte delivers 82.7% capacity retention after 300 cycles at 1 C, compared to only 35.5% for the unmodified counterpart, demonstrating a 2.3-fold improvement in cycling stability. • • Destructive tests on pouch cells (puncturing, cutting) show the LED remains illuminated, confirming enhanced safety and mechanical integrity under physical damage, a key step toward practical applications.
Abstract
Poly(ethylene oxide) (PEO)-based all-solid-state polymer electrolytes (SPEs) hold significant promise for high-specific-energy and high-safety Li batteries, yet suffer from poor mechanical robustness and low Li+-conducting efficiency. Aramid nanofibers (ANFs), with exceptional mechanical strength and abundant intramolecular/intermolecular interactions, are effective additives, but their strictly symmetric interchain interactions generate a highly ordered hydrogen-bond network, producing inert aggregates that compromise electrolyte stability. Here, we construct a poly(ethylene glycol) (PEG)-mediated asymmetric interaction between ANF chains. PEG chains introduce weaker H-bonding acceptor sites, higher steric hindrance, and abundant lithiophilic groups, simultaneously disrupting strong symmetric ANF-ANF interactions and creating rapid Li-ion channels. The resulting electrolyte maintains excellent mechanical properties (yield stress of 3.25 MPa) and enables stable cycling of Li||Li symmetric cells for over 1600 h with low polarization voltage. In LCO||Li cells, the electrolyte achieves a capacity retention of 82.7% after 300 cycles at 1 C, markedly higher than the unmodified counterpart (35.5%). This synergistic optimization of interfacial compatibility and mechanical performance demonstrates a practical route toward safe, high-energy-density all-solid-state polymer batteries.
1. Introduction
PEO-based all-solid-state polymer electrolytes are a leading candidate for next-generation lithium batteries due to their processability and flexibility, yet their high crystallinity at ambient temperature results in low ionic conductivity (<10^-5 S cm^-1). Heating above 60 °C activates ion transport but compromises mechanical strength, increasing dendrite penetration risk. Blending with high-strength additives like aramid nanofibers (ANFs) has been explored, but ANFs' symmetric hydrogen-bond network creates inert aggregates that degrade electrolyte stability.
This work introduces a PEG-mediated asymmetric interaction between ANF chains, which disrupts the ordered hydrogen-bond network while providing abundant ether-oxygen coordination sites for Li+ migration. This approach simultaneously enhances mechanical integrity (yield stress 3.25 MPa) and ionic transport, achieving stable cycling over 1600 h and high capacity retention in LCO||Li cells. The strategy addresses the long-standing trade-off between mechanical robustness and ionic conductivity in PEO-based electrolytes.
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Zige Hong, Mingli Zhu, Zhengshuai Bai, Binghong Zhao, Peiming Chen, Meizhen Zhu, Cong Wang, Mingxin Qiu, Yanyan Zhang, You Fan, Yuxin Tang (2026). Asymmetric interchain interaction enables stable all-solid-state PEO-based Li batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3717-6
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Frequently Asked Questions
What is the specific mechanism by which PEG disrupts the symmetric ANF-ANF hydrogen-bond network, and how does this affect Li+ transport?
PEG chains introduce weaker H-bonding acceptor sites and higher steric hindrance, which interfere with the strong, symmetric hydrogen bonds between ANF chains. This disruption prevents the formation of inert aggregates, while the abundant ether-oxygen groups in PEG provide coordination sites for Li+, facilitating rapid, dynamic Li+ migration. The result is improved interfacial compatibility and enhanced ionic conductivity, as evidenced by stable Li||Li cycling for over 1600 h.
How does the mechanical yield stress of 3.25 MPa compare to conventional PEO-based electrolytes, and what implications does this have for dendrite suppression?
Conventional PEO-based electrolytes typically exhibit yield stresses below 1 MPa, especially at elevated temperatures. The 3.25 MPa yield stress achieved here is significantly higher, providing a robust mechanical barrier against lithium dendrite penetration. This mechanical robustness is crucial for preventing short-circuiting and ensuring long-term cycling stability, as demonstrated by the stable Li||Li symmetric cell performance.
What are the specific cycling performance metrics of the LCO||Li cells, and how do they compare to state-of-the-art PEO-based systems?
The LCO||Li cells with the modified electrolyte achieve 82.7% capacity retention after 300 cycles at 1 C and 70.3% after 500 cycles at 1 C (at 65 °C). This is a substantial improvement over the unmodified counterpart, which retains only 35.5% after 300 cycles. These metrics are competitive with recent reports in the literature, highlighting the effectiveness of the asymmetric interaction strategy.
What is the scalability potential of the PEG-mediated ANF modification process for industrial production?
The modification process involves grafting PEG onto ANF surfaces, which can be performed using solution-based methods that are scalable. The use of commercially available PEO and ANF precursors, along with standard polymer processing techniques, suggests that the process can be adapted for roll-to-roll manufacturing. However, further optimization of the grafting efficiency and cost analysis is needed to assess full industrial viability.
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