Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries

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

doi:10.1002/sstr.202300301

Small Structures (Jan 2024)

Regulating Lewis Acid–Base Interaction in Poly (ethylene oxide)‐Based Electrolyte to Enhance the Cycling Stability of Solid‐State Lithium Metal Batteries

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

Affiliations

Chengkun Zhang: State 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 China
Shiyu Zhang: State 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 China
Yinggan Zhang: State 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 China
Xiaoyu Wu: State 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 China
Liang Lin: State 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 China
Xinchao Hu: State 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 China
Laisen Wang: State 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 China
Jie Lin: State 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 China
Baisheng Sa: Multiscale Computational Materials Facility College of Materials Science and Engineering Fuzhou University Fuzhou 350100 China
Guoying Wei: College of Materials & Chemistry China Jiliang University Hangzhou 310018 China
Dong-Liang Peng: State 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 China
Qingshui Xie: State 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 China

DOI: https://doi.org/10.1002/sstr.202300301
Journal volume & issue: Vol. 5, no. 1
pp. n/a – n/a

Abstract

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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.

Published in Small Structures

ISSN: 2688-4062 (Online)
Publisher: Wiley-VCH
Country of publisher: Germany
LCC subjects: Science: Physics; Science: Chemistry
Website: https://onlinelibrary.wiley.com/journal/26884062

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