TY - JOUR PY - 2023// TI - Stable operation of lithium metal batteries with aggressive cathode chemistries at 4.9 V JO - Angewandte Chemie (International ed. in English) A1 - Piao, Zhihong A1 - Ren, Hong-Rui A1 - Lu, Gongxun A1 - Jia, Kai A1 - Tan, Junyang A1 - Wu, Xinru A1 - Zhuang, Zhaofeng A1 - Han, Zhiyuan A1 - Li, Chuang A1 - Gao, Runhua A1 - Tao, Xinyong A1 - Zhou, Guangmin A1 - Cheng, Hui-Ming SP - ePub EP - ePub VL - ePub IS - ePub N2 - High-voltage lithium metal batteries (LMBs) pose severe challenges for the matching of electrolytes with aggressive electrodes, especially at low temperatures. Here, we report a rational modification of the Li+ solvation structure to extend the voltage and temperature operating ranges of conventional electrolytes. Ion-ion and ion-dipole interactions as well as the electrochemical window of solvents were tailored to improve oxidation stability and de-solvation kinetics of the electrolyte. Meanwhile, robust and elastic B and F-rich interphases are formed on both electrodes. Such optimization enables Li||LiNi0.5Mn1.5O4 cells (90.2% retention after 400 cycles) and Li||LiNi0.6Co0.2Mn0.2O2 (NCM622) cells (74.0% retention after 200 cycles) to cycle stably at an ultra-high voltage of 4.9 V. Moreover, NCM622 cells deliver a considerable capacity of 143.5 mAh/g at -20 ℃, showing great potential for practical uses. The proposed strategy sheds light on further optimization for high-voltage LMBs.

Language: en

LA - en SN - 1433-7851 UR - http://dx.doi.org/10.1002/anie.202300966 ID - ref1 ER -