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Multiple Hydrogen Bonds Enable Ultra-Rapid Self-Healing Polymer Electrolyte for Long-Lasting Lithium-Metal Batteries

A collaboration co-led by Oregon State University chemistry researcher David Ji is hoping to spark a green battery revolution by showing that iron instead of cobalt and nickel can be used as a cathode material in lithium-ion batteries. CREDIT: Xiulei "David" Ji, Oregon State University

Solid-state lithium-metal batteries are considered a leading candidate for next-generation energy storage due to their high energy density and improved safety. However, their practical application has been hindered by low ionic conductivity, poor interface stability with lithium metal, and uncontrolled dendrite growth. Self-healing polymer electrolytes have emerged as a potential solution to these challenges, but achieving rapid self-healing without compromising electrochemical performance has remained a critical barrier.

A team led by Lingling Zhang from Northeast Agricultural University and Chuankai Fu from Harbin Institute of Technology has designed a new self-healing polymer electrolyte (SHPE) that addresses these issues through a synergistic mechanism. The SHPE integrates quadruple hydrogen bonds from UPyMA, flexible ethoxy chains from ETPTA, and a plasticizing agent PEGMA to form a three-dimensional crosslinked network.

The team published their manuscript in Nano Research on May 21, 2026.

“Our design allows the electrolyte to rapidly self-heal surface damage within 30 minutes at 60 °C” said Zhang, noting this is “significantly faster than most reported systems.” The researcher emphasized that “the self-healed electrolyte recovers over 98% of its original ionic conductivity.”

The electrolyte achieves an ionic conductivity of 9.07×10⁻⁴ S·cm⁻¹ at 60 °C, a wide electrochemical stability window up to 5.14 V, and a high lithium-ion transference number of 0.66. Li||Li symmetric cells using this electrolyte stably cycle for more than 4000 hours at 0.05 mA·cm⁻² with only a 10 Ω increase in impedance. Post-cycling analysis reveals a dense and dendrite-free lithium metal surface, with the formation of a stable solid-electrolyte interphase rich in LiF and Li3N.

“The synergy between flexible segmental movement and reversible hydrogen bonding achieves fast self-healing” explained Fu, while also accelerating ion transport and stabilizing interfacial chemistry.

The team further demonstrated that Li||LiFePO4 cells incorporating the electrolyte exhibit excellent rate capability and long-term cycling stability. A pouch cell fabricated with the electrolyte remained functional even after folding and cutting, successfully powering an LED light.

Looking ahead, the researchers believe this design strategy opens new avenues for developing durable and safe solid-state batteries. Zhang stated the team’s “ultimate goal is to translate this self-healing electrolyte technology into practical battery systems with extended service life and enhanced safety,” noting they are currently exploring high-voltage cathode compatibility and scaling material synthesis.

This work was supported by National Natural Science Foundation of China (Grant Nos. 22209022 and 52302234), Natural Science Foundation of Heilongjiang Province (Grant No. LH2023B009), and Fundamental Research Funds for the Central Universities (HIT.NSFJG202214).


Journal: Nano Research
DOI: 10.26599/NR.2026.94908586
Article Title: Multiple hydrogen bonds enable ultra-rapid self-healing polymer electrolyte for long-lasting lithium-metal batteries
Article Publication Date: 21-May-2026
Publisher: Tsinghua University Press

Featured image credit: Xiulei “David” Ji, Oregon State University

Source: EurekAlert

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