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Updated: Jun 26, 2026

Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications
Published on: August 12, 2013
Multihydrogen-bond-bridged composite solid electrolytes enabling continuous Li+ pathways for stable solid-state
Xin Jia1, Xinyu Da1, Yanyang Qin2
1School of Chemistry, Engineering Research Center of Energy Storage Materials and Devices of Ministry of Education, National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology, Xi'an Jiaotong University, Xi'an 710049, China.
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 Li6.4La3Zr1.7Ta0.3O12 (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.
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