A strong Lewis acid imparts high ionic conductivity and interfacial stability to polymer composite electrolytes towards all-solid-state Li-metal batteries

Science China Materials - Tập 65 - Trang 2179-2188 - 2022
Litong Wang1, Yunlei Zhong1, Zhaorui Wen1, Chaowei Li1, Jingxin Zhao1, Mingzheng Ge1,2, Pengfei Zhou1, Yanyan Zhang3, Yuxin Tang3, Guo Hong1,4
1Institute of Applied Physics and Materials Engineering, University of Macau, Taipa, Macau SAR, China
2School of Textile and Clothing, Nantong University, Nantong, China
3College of Chemical Engineering, Fuzhou University, Fuzhou, China
4Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Avenida da Universidade, Taipa, Macau SAR, China

Tóm tắt

The development of high-performance solid polymer electrolytes is crucial for producing all-solid-state lithium metal batteries with high safety and high energy density. However, the low ionic conductivity of solid polymer electrolytes and their unstable electrolyte/electrode interfaces have hindered their widespread utilization. To address these critical challenges, a strong Lewis acid (aluminum fluoride (AlF3)) with dual functionality is introduced into polyethylene oxide) (PEO)-based polymer electrolyte. The AlF3 facilitates the dissociation of lithium salt, increasing the iontransfer efficiency due to the Lewis acid-base interaction; further the in-situ formation of lithium fluoride-rich interfacial layer is promoted, which suppresses the uneven lithium deposition and continuous undesired reactions between the Li metal and PEO matrix. Benefiting from our rational design, the symmetric Li/Li battery with the modified electrolyte exhibits much longer cycling stability (over 3600 h) than that of the pure PEO/lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) electrolyte (550 h). Furthermore, the all-solid-state LiFePO4 full cell with the composite electrolyte displays a much higher Coulombic efficiency (98.4% after 150 cycles) than that of the electrolyte without the AlF3 additive (63.3% after 150 cycles) at a large voltage window of 2.4–4.2 V, demonstrating the improved interface and cycling stability of solid polymer lithium metal batteries.

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