Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate Performance

Abstract The low lithium‐ion conductivity of polyethylene oxide (PEO)‐based polymer electrolytes limits their application in solid‐state lithium batteries and related fields. Here, ionic liquids (ILs) are injected into hollow silicon nanorods (HSNRs) to prepare a composite solid polymer electrolyte...

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Bibliographic Details
Main Authors: Xinglong Gao, Zhong Zheng, Yifan Pan, Shuyi Song, Zhen Xu
Format: Article
Language:English
Published: Wiley 2025-01-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202411437
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Summary:Abstract The low lithium‐ion conductivity of polyethylene oxide (PEO)‐based polymer electrolytes limits their application in solid‐state lithium batteries and related fields. Here, ionic liquids (ILs) are injected into hollow silicon nanorods (HSNRs) to prepare a composite solid polymer electrolyte (CSPE) with aligned HSNRs containing ILs (F‐ILs@HSNRs). Applying a magnetic field promoted uniform dispersion and orientation of F‐ILs@HSNRs in CSPE. The addition of F‐ILs@HSNRs reduced PEO crystallinity and formed Li+ transport pathways at the F‐ILs@HSNRs/PEO interface. Calculations and multi‐physics simulations reveal that ILs within F‐ILs@HSNRs contribute most to lithium‐ion conduction, followed by the F‐ILs@HSNRs/PEO interface. When F‐ILs@HSNRs are arranged perpendicular to the electrodes, the CSPE exhibits the shortest Li+ migration pathways, resulting in stable and efficient lithium‐ion conduction. The conductivity (2.14 × 10−4 S cm−1) and lithium‐ion migration number tLi+ (0.307) are the highest, being 125 times and 184% higher, respectively, than those of PEO‐LiTFSI, when compared to CSPEs with randomly arranged or parallel‐aligned F‐ILs@HSNRs. Furthermore, Li|CSPE|Li batteries and LiFePO4|CSPE|Li batteries display stable cycling for over 2000 h, with coulombic efficiency approaching 100%. Excellent electrochemical reversibility is also confirmed in the rate performance test.
ISSN:2198-3844