Ping Liang, Honglu Hu, Yang Dong, Zhaodong Wang, Kuiming Liu, Guoyu Ding, Fangyi Cheng

Competitive Coordination of Ternary Anions Enabling Fast Li‐Ion Desolvation for Low‐Temperature Lithium Metal Batteries

  • Electrochemistry
  • Condensed Matter Physics
  • Biomaterials
  • Electronic, Optical and Magnetic Materials

AbstractLithium metal batteries (LMBs) working at subzero temperatures are plagued by severe restrictions from the increased energy barrier of Li‐ion migration and desolvation. Herein, a competitive coordination strategy based on the ternary‐anion (TA) coupling of PF6, TFSI, and NO3 toward Li+ to achieve an anti‐freezing electrolyte with rapid kinetics is proposed. Computational and spectroscopic analyses reveal that the repulsive interaction among three anions and the preponderant coordination of the Li+‐NO3 further weaken the involvement degree of other anions in the Li+ solvation structure. As a result, the formulated TA electrolyte exhibits low binding energy of Li+‐anions (−4.62 eV), Li+ desolvation energy (17.04 kJ mol−1), and high ionic conductivity (3.39 mS cm−1 at −60 °C), simultaneously promoting anion‐derived solid electrolyte interphase on Li anode. Assembled Li||LiNi0.8Co0.1Mn0.1O2 cells employing the TA electrolyte exhibit robust capacity retention of 86.74% over 200 cycles at 25 °C and deliver a specific cathode capacity of 103.85 mAh g−1 at −60 °C. This study will enlighten the rational design of multi‐anion electrolytes to tailor the Li+ solvation/desolvation for advanced low‐temperature LMBs.

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