Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries
Solid polymer electrolytes (SPE) offer an outstanding choice because of their lightweight, flexibility, and excellent thin‐film forming ability. However, the low ionic conductivity and poor lithium ion transfer number (tLi+) restrict its application in all‐solid‐state lithium batteries (ASSLBs). Her...
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Wiley-VCH
2024-01-01
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Online Access: | https://doi.org/10.1002/sstr.202300301 |
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author | Chengkun Zhang Shiyu Zhang Yinggan Zhang Xiaoyu Wu Liang Lin Xinchao Hu Laisen Wang Jie Lin Baisheng Sa Guoying Wei Dong-Liang Peng Qingshui Xie |
author_facet | Chengkun Zhang Shiyu Zhang Yinggan Zhang Xiaoyu Wu Liang Lin Xinchao Hu Laisen Wang Jie Lin Baisheng Sa Guoying Wei Dong-Liang Peng Qingshui Xie |
author_sort | Chengkun Zhang |
collection | DOAJ |
description | Solid polymer electrolytes (SPE) offer an outstanding choice because of their lightweight, flexibility, and excellent thin‐film forming ability. However, the low ionic conductivity and poor lithium ion transfer number (tLi+) restrict its application in all‐solid‐state lithium batteries (ASSLBs). Herein, UIO66‐X metal‐organic frameworks with controllable Lewis basicity, acidity, or neutrality functional groups are synthesized successfully and then incorporated into the poly (ethylene oxide) (PEO) matrix to fabricate SPE. The influence of different organic ligands on the interface interaction between PEO and LiTFSI is investigated by solid‐state nuclear magnetic resonance, Fourier transform infrared spectoscopy and Raman tests, as well as density functional theory calculations. The Lewis acidity group plays a key role in enhancing the ionic conductivity and tLi+. As a result, the constructed Li–Li symmetrical cells retain stable cycling for 2300 h and the LiFePO4‐based ASSLBs deliver outstanding electrochemical properties with 147 mAh g−1 of reversible capacity after 500 cycles at 1C and 60 °C, 131 mAh g−1 after 150 cycles at 0.1C and 30 °C. The fabricated SPEs are self‐standing and flexible with good mechanical stability, demonstrating the great potential for practical application. The results can guide choosing the inorganic filler to prepare high‐performance SPE. |
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language | English |
last_indexed | 2024-03-08T15:51:11Z |
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series | Small Structures |
spelling | doaj.art-d6bdaac55add4c96b51d7f5746f1fd412024-01-09T05:33:21ZengWiley-VCHSmall Structures2688-40622024-01-0151n/an/a10.1002/sstr.202300301Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal BatteriesChengkun Zhang0Shiyu Zhang1Yinggan Zhang2Xiaoyu Wu3Liang Lin4Xinchao Hu5Laisen Wang6Jie Lin7Baisheng Sa8Guoying Wei9Dong-Liang Peng10Qingshui Xie11State Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaMultiscale Computational Materials Facility College of Materials Science and Engineering Fuzhou University Fuzhou 350100 ChinaCollege of Materials & Chemistry China Jiliang University Hangzhou 310018 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaState Key Laboratory for Physical Chemistry of Solid Surfaces Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials College of Materials Xiamen University Xiamen 361005 ChinaSolid polymer electrolytes (SPE) offer an outstanding choice because of their lightweight, flexibility, and excellent thin‐film forming ability. However, the low ionic conductivity and poor lithium ion transfer number (tLi+) restrict its application in all‐solid‐state lithium batteries (ASSLBs). Herein, UIO66‐X metal‐organic frameworks with controllable Lewis basicity, acidity, or neutrality functional groups are synthesized successfully and then incorporated into the poly (ethylene oxide) (PEO) matrix to fabricate SPE. The influence of different organic ligands on the interface interaction between PEO and LiTFSI is investigated by solid‐state nuclear magnetic resonance, Fourier transform infrared spectoscopy and Raman tests, as well as density functional theory calculations. The Lewis acidity group plays a key role in enhancing the ionic conductivity and tLi+. As a result, the constructed Li–Li symmetrical cells retain stable cycling for 2300 h and the LiFePO4‐based ASSLBs deliver outstanding electrochemical properties with 147 mAh g−1 of reversible capacity after 500 cycles at 1C and 60 °C, 131 mAh g−1 after 150 cycles at 0.1C and 30 °C. The fabricated SPEs are self‐standing and flexible with good mechanical stability, demonstrating the great potential for practical application. The results can guide choosing the inorganic filler to prepare high‐performance SPE.https://doi.org/10.1002/sstr.202300301ionic conductivityLewis acid–base interactionsolid lithium batteriessolid polymer electrolytesUIO66 |
spellingShingle | Chengkun Zhang Shiyu Zhang Yinggan Zhang Xiaoyu Wu Liang Lin Xinchao Hu Laisen Wang Jie Lin Baisheng Sa Guoying Wei Dong-Liang Peng Qingshui Xie Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries Small Structures ionic conductivity Lewis acid–base interaction solid lithium batteries solid polymer electrolytes UIO66 |
title | Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries |
title_full | Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries |
title_fullStr | Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries |
title_full_unstemmed | Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries |
title_short | Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries |
title_sort | regulating lewis acid base interaction in poly ethylene oxide based electrolyte to enhance the cycling stability of solid state lithium metal batteries |
topic | ionic conductivity Lewis acid–base interaction solid lithium batteries solid polymer electrolytes UIO66 |
url | https://doi.org/10.1002/sstr.202300301 |
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