Authors
Hengming Yan, Bowen Zhang, Xuefan Liu, Lu Wang, Cunlong Hu, Anran Sheng, Congcong Zhang, Linglong Kong, Zhenzhen Wu, Yulin Zhong, Sheng Liu, Shanqing Zhang
Published in
Advanced materials (Deerfield Beach, Fla.). Pages e75158. Sep 28, 2026. Epub Sep 28, 2026.
Abstract
Ion transport in poly(ethylene oxide) (PEO) electrolytes is severely constrained by sluggish Li+ mobility arising from tight chelation of ether oxygens, and by insufficient lithium salt dissociation. Inspired by polycarboxylate ether (PCE) superplasticizers in cement, we demonstrate phosphonate-functionalized PCE (P-PCE) could overcome both limitations. The electron-rich -PO3 2- groups could liberate Li+ from the strong Li+-PEO chelation and promote efficient salt dissociation without trapping Li+. Instead, they facilitate rapid Li+ migration through a unique multi-Li+ coordination mechanism, where the electrostatic repulsion among multiple Li+ ions coordinated to a single -PO3 2- destabilizes solvation and promotes rapid Li+ hopping between adjacent sites. Meanwhile, P-PCE suppresses PEO crystallization and, through multi-Li+ coordination, induces a more extended conformation of PEO, which fosters high-entropy Li+ coordination environments involving TFSI-, ether oxygens, and -PO3 2- in transient combinations, promoting long-range Li+ transport. The simultaneously enhanced Li+ concentration and mobility lead to a high ionic conductivity (1.7 × 10-4 S cm-1, 30°C) without adding liquid plasticizers. Correspondingly, Li||LiFePO4 cells deliver high capacities of 140.6 mAh g-1 at 0.5 C and 119.7 mAh g-1 at 1 C (30°C). This work provides a simple yet effective strategy for developing high-performance solid-state batteries and molecular-level insights for rational polymer electrolyte designs.
PMID:
42802901
Bibliographic data and abstract were imported from PubMed on 28 Sep 2026.
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