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<p>Overcoming interfacial mechano-electrochemical failure remains a fundamental challenge in solid-state lithium metal batteries, where polymers offer conformal interfacial contact but suffer from low ionic conductivity, while oxides/sulfides provide high ionic conductivity but face severe interfacial issues. Here we show a mechano-integrated gradient electrolyte based on a hydrogen-bonded polyurethane matrix with dual chain extenders. The polyurethane matrix exhibits high viscoelasticity (&gt;5000% fracture strain) and self-healing, allowing high filler loading and continuous triphasic lithium-ion percolation networks. A spatially graded Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> architecture (10–100 wt%) decouples interfacial requirements: conformal contact with lithium metal negative electrode, high ionic conductivity (~10<sup>−4</sup> S cm<sup>−1</sup>), and an electrochemical stability window up to 4.9 V. The homologous polymer framework eliminates chemo-mechanical degradation while providing mechanical strength (&gt;80 MPa) and solution processability. This integrated design suppresses interfacial delamination and dendrite growth (&gt;7500 h of stable lithium plating/stripping), and mitigates positive electrode degradation (74% capacity retention after 1000 cycles in Li | |LiFePO<sub>4</sub> cells at 0.5 C and stable operation in stack-pressure-free NCM811 pouch cells). This work provides a scalable platform for high-energy-density, long-lifespan solid-state lithium metal batteries.</p>

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A mechano-integrated gradient electrolyte for long-cycling solid-state lithium metal batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月24日

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  • Xiaoping Yi,
  • Guoqing Qi,
  • Wending Pan,
  • Kaishan Xiao,
  • Yixin Yang,
  • Yang Yang,
  • Bitong Wang,
  • Xiaolong Zhao,
  • Xunliang Liu,
  • Hong Li

摘要

Overcoming interfacial mechano-electrochemical failure remains a fundamental challenge in solid-state lithium metal batteries, where polymers offer conformal interfacial contact but suffer from low ionic conductivity, while oxides/sulfides provide high ionic conductivity but face severe interfacial issues. Here we show a mechano-integrated gradient electrolyte based on a hydrogen-bonded polyurethane matrix with dual chain extenders. The polyurethane matrix exhibits high viscoelasticity (>5000% fracture strain) and self-healing, allowing high filler loading and continuous triphasic lithium-ion percolation networks. A spatially graded Li1.3Al0.3Ti1.7(PO4)3 architecture (10–100 wt%) decouples interfacial requirements: conformal contact with lithium metal negative electrode, high ionic conductivity (~10−4 S cm−1), and an electrochemical stability window up to 4.9 V. The homologous polymer framework eliminates chemo-mechanical degradation while providing mechanical strength (>80 MPa) and solution processability. This integrated design suppresses interfacial delamination and dendrite growth (>7500 h of stable lithium plating/stripping), and mitigates positive electrode degradation (74% capacity retention after 1000 cycles in Li | |LiFePO4 cells at 0.5 C and stable operation in stack-pressure-free NCM811 pouch cells). This work provides a scalable platform for high-energy-density, long-lifespan solid-state lithium metal batteries.