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Gear-Meshing Design Reduces Heterointerfacial Mass-Transfer Barriers for Accelerated Li+ Conduction in Composite Polymer Electrolytes.

Created on 01 Nov 2026

Authors

Mingjie Li, Jiquan Lu, Hanfeng Huang, Yiming Gao, Jiajie Pan, Zexin Su, Guocong Liu, Yonggang Min, Quanbing Liu, Yuying Zheng

Published in

Small (Weinheim an der Bergstrasse, Germany). Oct 31, 2026. Epub Oct 31, 2026.

Abstract

Composite polymer electrolytes (CPEs) are promising for all-solid-state lithium metal batteries (LMBs), yet their practical implementation is still hindered by sluggish Li+ transport kinetics. This limitation is associated with heterointerfacial mass-transfer barriers between inorganic fillers and polymer matrices. Herein, a gear-meshing composite polymer electrolyte (GMCPE) is developed to reduce these barriers and enhance Li+ transport kinetics in CPEs. In this design, the hydroxyl- and amino-rich polydopamine (PDA) coating functions as a molecular gear-like interfacial coupler, which meshes polymer chains to improve filler/polymer compatibility and anchors anions to promote Li-salt dissociation, thereby liberating more mobile Li+. Meanwhile, the Al2O3 with a low Li+ diffusion barrier and the three-dimensional (3D) polyacrylonitrile (PAN) framework synergistically construct continuous Li+ transport pathways while reinforcing mechanical robustness. Consequently, GMCPE achieves an enhanced Li+ transference number of 0.52 and an ionic conductivity of 0.5 mS cm-1 at 60 °C. Moreover, Li|GMCPE|Li symmetric cells exhibit stable dendrite-free Li plating/stripping for over 4200 h. All-solid-state Li|GMCPE|LiFePO4 cells maintain 84.7% capacity retention after 500 cycles at 1 C. This work provides a novel gear-meshing interfacial design paradigm for advancing accelerated Li+ transport in CPEs toward high-performance all-solid-state LMBs.

PMID:
42966825
Bibliographic data and abstract were imported from PubMed on 01 Nov 2026.

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