Lu Gongxun, Qiao Qiangqiang, Zhang Mengtian, Zhang Jinsen, Li Shuai, Jin Chengbin, Yuan Huadong, Ju Zhijin, Huang Rong, Liu Yujing, Luo Jianmin, Wang Yao, Zhou Guangmin, Tao Xinyong, Nai Jianwei
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
Tsinghua-Berkeley Shenzhen Institute and Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China.
Sci Adv. 2024 Aug 9;10(32):eado7348. doi: 10.1126/sciadv.ado7348. Epub 2024 Aug 7.
Hybrid materials with a rational organic-inorganic configuration can offer multifunctionality and superior properties. This principle is crucial but challenging to be applied in designing the solid electrolyte interphase (SEI) on lithium metal anodes (LMAs), as it substantially affects Li transport from the electrolyte to the anode. Here, an artificial SEI with an ultrahigh fluorine content (as high as 70.12 wt %) can be successfully constructed on the LMA using a high-voltage electrosynthesis strategy. This SEI consists of ultrafine lithium fluoride nanocrystals embedded in a fluorinated organic matrix, exhibiting excellent passivation and mechanical strength. Notably, the organic-inorganic interface demonstrates a high dielectric constant that enables fast Li transport throughout the SEI. Consequently, LMA coated with this SEI substantially enhances the cyclability of both half-cells and full cells, even under rigorous conditions. This work demonstrates the potential of rationally designed hybrid materials via a unique electrosynthetic approach for advanced electrochemical systems.
具有合理有机-无机结构的混合材料可提供多功能性和优异性能。这一原理在设计锂金属阳极（LMA）上的固体电解质界面（SEI）时至关重要但具有挑战性，因为它会极大地影响锂从电解质到阳极的传输。在此，使用高压电合成策略可在LMA上成功构建具有超高氟含量（高达70.12 wt%）的人工SEI。该SEI由嵌入氟化有机基质中的超细氟化锂纳米晶体组成，具有出色的钝化性能和机械强度。值得注意的是，有机-无机界面表现出高介电常数，能够使锂在整个SEI中快速传输。因此，涂覆有这种SEI的LMA即使在严苛条件下也能显著提高半电池和全电池的循环稳定性。这项工作通过独特的电合成方法展示了合理设计的混合材料在先进电化学系统中的潜力。
