Yang Chao, Zheng Mengting, Qu Rui, Zhang Hanyin, Yin Luming, Hu Wenxi, Han Jin, Lu Jun, You Ya
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, Hubei, 430070, P. R. China.
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, Zhejiang, 310027, P. R. China.
Adv Mater. 2024 Jan;36(1):e2307220. doi: 10.1002/adma.202307220. Epub 2023 Nov 23.
Despite the high energy of LiNi Co Mn O (NCM811) cathode, it still suffers serious decay due to the continuous solvents decomposition and unstable cathode electrolyte interphase (CEI) layers, especially under high temperatures. The intense exothermic reaction between delithiated NCM811 and flammable electrolyte, on the other hand, pushes the batteries to their safety limit. Herein, these two issues are tackled via engineering the electrolytes, that is, utilizing salts with higher HOMO levels and nonflammable solvents with lower HOMO levels, to reduce the massive decomposition of solvents and improve battery safety under elevated temperatures. Consequently, a thin and boron-rich CEI is generated, which effectively inhibited the side reactions, thus improving the cycling stability and safety. Deviated from the highly concentrated electrolytes which heavily relies on the usage of massive salts, the electrolyte recipe can introduce a robust inorganic-rich CEI but use much less salt (i.e., dilute electrolyte), and thus, offer an encouraging alternative toward practical applications. As such, the NCM811 cathode exhibits a high-capacity retention of 81.2% after 950 cycles at 25 °C and 75% after 300 cycles at 55 °C. This work provides a universal electrolyte design strategy for designing stable and safe high-temperature electrolytes for the NCM811 cathode.
尽管LiNiCoMnO(NCM811)正极具有较高的能量,但由于溶剂持续分解和不稳定的正极电解质界面(CEI)层,它仍然会发生严重的衰减,尤其是在高温下。另一方面,脱锂的NCM811与易燃电解质之间强烈的放热反应将电池推向安全极限。在此,通过对电解质进行工程设计来解决这两个问题,即使用具有较高最高占据分子轨道(HOMO)能级的盐和具有较低HOMO能级的不可燃溶剂,以减少溶剂的大量分解并提高高温下的电池安全性。因此,生成了一层薄且富含硼的CEI,有效地抑制了副反应,从而提高了循环稳定性和安全性。与严重依赖大量盐使用的高浓度电解质不同,该电解质配方可以引入坚固的富含无机成分的CEI,但使用的盐要少得多(即稀电解质),因此为实际应用提供了一个令人鼓舞的替代方案。这样,NCM811正极在25℃下950次循环后具有81.2%的高容量保持率,在55℃下300次循环后具有75%的高容量保持率。这项工作为设计用于NCM811正极的稳定且安全的高温电解质提供了一种通用的电解质设计策略。