Covalent Organic Framework Enhanced Solid Polymer Electrolyte for Lithium Metal Batteries

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Abstract
High ionic conductivity, outstanding mechanical stability, and a wide electrochemical window are the keys to the application of solid-state lithium metal batteries (LMBs). Due to their regular channels for ion transport and tailored functional groups, covalent organic frameworks (COFs) have been applied to solid electrolytes to improve their performance. Herein, we report a flexible polyethylene oxide-COF-LZU1 (abbreviated as PEO-COF) electrolyte membrane with a high lithium ion transference number and satisfactory mechanical strength, allowing for dendrite-free and long-time cycling for LMBs. Benefiting from the interaction between bis(triflfluoromethanesulonyl)imide anions (TFSI−) and aldehyde groups in COF-LZU1, the Li+ transference number of the PEO-5% COF-LZU1 electrolyte reached up to 0.43, much higher than that of neat PEO electrolyte (0.18). Orderly channels are conducive to the homogenous Li-+ deposition, thereby inhibiting the lithium dendrites. The assembled LiFePO4|PEO-5% COF-LZU1/Li cells delivered a discharge specific capacity of 146 mAh g−1 and displayed a capacity retention of 80% after 200 cycles at 0.1 C (60 °C). The Li/Li symmetrical cells of the PEO-5% COF-LZU1 electrolyte presented a longer working stability at different current densities compared to that of the PEO electrolyte. Therefore, the enhanced comprehensive performance of the solid electrolyte shows potential application prospects for use in LMBs.
Funding Information
  • National Key Research and Development Program of China (2019YFA0705701, 22179149, 22075329, 22008267, 51573215, 21978332, 2021A0505030022, 2019A1515010803, 2020A1515011445, 232018002)
  • National Natural Science Foundation of China (2019YFA0705701, 22179149, 22075329, 22008267, 51573215, 21978332, 2021A0505030022, 2019A1515010803, 2020A1515011445, 232018002)
  • Guangdong Basic and Applied Basic Research Foundation (2019YFA0705701, 22179149, 22075329, 22008267, 51573215, 21978332, 2021A0505030022, 2019A1515010803, 2020A1515011445, 232018002)
  • Research and Development Project of Henan Academy of Sciences China (2019YFA0705701, 22179149, 22075329, 22008267, 51573215, 21978332, 2021A0505030022, 2019A1515010803, 2020A1515011445, 232018002)

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