Multihydrogen-bond-bridged composite solid electrolytes enabling continuous Li⁺ pathways for stable solid-state lithium batteries.

Authors

Xin Jia, Xinyu Da, Yanyang Qin, Yuxin Ouyang, Yuanjun Zhao, Na Li, Jing Chen, Shujiang Ding

Published in

Science advances. Volume 12. Issue 26. Pages eaed5972. Jun 26, 2026. Epub Jun 24, 2026.

Abstract

Composite solid electrolytes (CSEs) hold great promise for advancing safer and higher-energy-density solid-state batteries. However, the poor interface compatibility caused by the lithium carbonate (Li₂CO₃) passivation layer on the garnet-type Li_6.4La₃Zr_1.7Ta_0.3O₁₂ (LLZTO) surface leads to an inhomogeneous distribution of ceramic particles and discontinuous lithium ion (Li⁺) transport, especially for high-content ceramics. Herein, we chemically convert the Li₂CO₃ layer into brushlike poly(ethylene glycol) methyl ether acrylate-co-2-(3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl)ureido)ethyl methacrylate (PEGMA-co-UPyMA) polymers. These modified ceramics (LLZTO-g-PEGMA-co-UPyMA) are integrated with a dynamic supramolecular ionic conducting polymer (DSICP) through hydrogen bond coupling, yielding a homogeneous LLZTO-g-PEGMA-co-UPyMA@DSICP CSE with continuous Li⁺ transport pathways, even at 90 weight % ceramic loading. This CSE enables exceptional cycling stability, with Li|LiFePO₄ cells retaining 88.8% capacity after 2000 cycles and 4.4-volt Li|NMC811 cells maintaining 83.7% after 300 cycles. Impressively, the 1.26-ampere hour pouch cell retains 85.6% capacity after 100 cycles, demonstrating unprecedented feasibility for practical solid-state lithium batteries.

PMID:
42341112
Bibliographic data and abstract were imported from PubMed on 25 Jun 2026.

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