Authors
Xiaoping Yi, Guoqing Qi, Wending Pan, Kaishan Xiao, Yixin Yang, Yang Yang, Bitong Wang, Xiaolong Zhao, Xunliang Liu, Hong Li
Published in
Nature communications. Jun 24, 2026. Epub Jun 24, 2026.
Abstract
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.
PMID:
42343066
Bibliographic data and abstract were imported from PubMed on 25 Jun 2026.
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