材料科学
金属锂
锂(药物)
共价键
离子键合
固态
金属
复合材料
纳米技术
化学工程
电极
离子
工程物理
冶金
物理化学
有机化学
阳极
内分泌学
化学
工程类
医学
作者
Jun Huang,Cheng Liu,Zhenyang Zhang,Chen Li,Ki‐Taek Bang,Andrew Liem,Hang Luo,Chuan Hu,Young Moo Lee,Yingying Lü,Yanming Wang,Yoonseob Kim
标识
DOI:10.1002/aenm.202400762
摘要
Abstract Ionic covalent organic frameworks (iCOFs) are crystalline materials with stable porous structures. They hold great potential for ion transport, particularly as solid‐state electrolytes (SSEs) for all‐solid‐state lithium metal batteries (ASSLMBs). However, achieving an ionic conductivity of over 10 −3 S cm −1 at room temperature using pure‐iCOF‐based SSEs, even adding additives such as lithium salts, is challenging as the voids work as strong resistances. Thus, highly conductive iCOFs typically require quasi‐solid‐state configurations with organic solvents or plasticizers. In this study, composites comprising iCOFs and poly(ionic liquid) (PIL) are prepared to make all‐solid‐state iCOFs electrolytes with an exceptional ionic conductivity up to 1.50 × 10 −3 S cm −1 and a high Li + transference number of > 0.80 at room temperature. Combined experimental and computational studies show that the co‐coordination and competitive coordination mechanism established between the PIL, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and iCOFs enabled rapid Li + transport while restricting TFSI − movement. ASSLMB cells, made of composite SSEs and LiFePO 4 composite cathode, demonstrate an initial discharge capacity of 141.5 mAh g −1 at 1C and r.t., with an impressive capacity retention of 87% up to 800 cycles. Overall, this work presents a breakthrough approach for developing advanced SSEs for next‐generation high‐energy‐density ASSLMBs.
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