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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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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author Xinglong Gao
Zhong Zheng
Yifan Pan
Shuyi Song
Zhen Xu
author_facet Xinglong Gao
Zhong Zheng
Yifan Pan
Shuyi Song
Zhen Xu
author_sort Xinglong Gao
collection DOAJ
description 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.
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spelling doaj-art-eb69d082bbb54a189c8f40b051a65c082025-01-13T15:29:43ZengWileyAdvanced Science2198-38442025-01-01122n/an/a10.1002/advs.202411437Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate PerformanceXinglong Gao0Zhong Zheng1Yifan Pan2Shuyi Song3Zhen Xu4Hubei Key Laboratory of Modern Manufacturing Quantity Engineering School of Mechanical Engineering Hubei University of Technology Wuhan Hubei 430068 ChinaHubei Key Laboratory of Modern Manufacturing Quantity Engineering School of Mechanical Engineering Hubei University of Technology Wuhan Hubei 430068 ChinaHubei Key Laboratory of Modern Manufacturing Quantity Engineering School of Mechanical Engineering Hubei University of Technology Wuhan Hubei 430068 ChinaHubei Key Laboratory of Modern Manufacturing Quantity Engineering School of Mechanical Engineering Hubei University of Technology Wuhan Hubei 430068 ChinaXinjiang Key Laboratory of High Value Green Utilization of Low‐Rank Coal School of Physics and Materials Science Changji University Changji Xinjiang 831100 ChinaAbstract 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.https://doi.org/10.1002/advs.202411437hollow silicon nanorodsionic liquidlithium‐ion conductivityorientation alignmentsolid‐state lithium battery
spellingShingle Xinglong Gao
Zhong Zheng
Yifan Pan
Shuyi Song
Zhen Xu
Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate Performance
Advanced Science
hollow silicon nanorods
ionic liquid
lithium‐ion conductivity
orientation alignment
solid‐state lithium battery
title Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate Performance
title_full Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate Performance
title_fullStr Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate Performance
title_full_unstemmed Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate Performance
title_short Aligned Hollow Silicon Nanorods Containing Ionic Liquid Enhanced Solid Polymer Electrolytes with Superior Cycling and Rate Performance
title_sort aligned hollow silicon nanorods containing ionic liquid enhanced solid polymer electrolytes with superior cycling and rate performance
topic hollow silicon nanorods
ionic liquid
lithium‐ion conductivity
orientation alignment
solid‐state lithium battery
url https://doi.org/10.1002/advs.202411437
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AT zhongzheng alignedhollowsiliconnanorodscontainingionicliquidenhancedsolidpolymerelectrolyteswithsuperiorcyclingandrateperformance
AT yifanpan alignedhollowsiliconnanorodscontainingionicliquidenhancedsolidpolymerelectrolyteswithsuperiorcyclingandrateperformance
AT shuyisong alignedhollowsiliconnanorodscontainingionicliquidenhancedsolidpolymerelectrolyteswithsuperiorcyclingandrateperformance
AT zhenxu alignedhollowsiliconnanorodscontainingionicliquidenhancedsolidpolymerelectrolyteswithsuperiorcyclingandrateperformance