<p>Enhancing high-capacity silicon-graphite negative electrodes and high-voltage positive electrodes is crucial for improving specific energy of lithium-ion batteries. However, challenges like large volume change in silicon-graphite electrode and electrolyte decomposition at high voltage compromise electrochemical stability. Furthermore, sluggish Li<sup>+</sup> exchange between electrolytes and electrodes severely hinders electrochemical kinetics. Herein, we design an anion-rich electrolyte with high oxidation resistance and rapid desolvation behavior, which enabling the formation of effective interphases for improving electrochemical performance. The optimized electrolyte allows silicon-graphite electrode to achieve 1838.9 mAh g<sup>−1</sup> capacity at 0.1 C with a long-term electrochemical stability, while a lithium-rich layered oxide positive electrode maintains 72.3% retention after 600 cycles at 1 C. The designed electrolyte with nonflammability also enhances safety in pouch cells after nail penetration. This design significantly improves cycling stability in high-specific-energy batteries, reaching specific energy of 278 Wh kg<sup>−1</sup> for graphite | |lithium-rich layered oxide and 355 Wh kg<sup>−1</sup> for silicon-graphite | |Ni-rich layer oxide pouch cells, calculated based on all cell components (positive electrode, negative electrode, separator and electrolyte). The design of the high-voltage electrolyte introduces a feasible approach to formulate a suitable solvation structure for high-specific-energy batteries.</p>

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High-voltage and high-safety lithium-ion batteries enabled by nonflammable electrolyte with enhanced Li+ desolvation behavior

  • Jiahe Chen,
  • Fangkun Li,
  • Lei Xi,
  • Shiman He,
  • Linwei Zhao,
  • Jun Zeng,
  • Jinpeng Lin,
  • Zhaoyu Sun,
  • Conghui Zhang,
  • Yihong Tong,
  • Chenchen Li,
  • Zhijun Wu,
  • Hongge Pan,
  • Jingwei Zhao,
  • Min Zhu,
  • Jun Liu

摘要

Enhancing high-capacity silicon-graphite negative electrodes and high-voltage positive electrodes is crucial for improving specific energy of lithium-ion batteries. However, challenges like large volume change in silicon-graphite electrode and electrolyte decomposition at high voltage compromise electrochemical stability. Furthermore, sluggish Li+ exchange between electrolytes and electrodes severely hinders electrochemical kinetics. Herein, we design an anion-rich electrolyte with high oxidation resistance and rapid desolvation behavior, which enabling the formation of effective interphases for improving electrochemical performance. The optimized electrolyte allows silicon-graphite electrode to achieve 1838.9 mAh g−1 capacity at 0.1 C with a long-term electrochemical stability, while a lithium-rich layered oxide positive electrode maintains 72.3% retention after 600 cycles at 1 C. The designed electrolyte with nonflammability also enhances safety in pouch cells after nail penetration. This design significantly improves cycling stability in high-specific-energy batteries, reaching specific energy of 278 Wh kg−1 for graphite | |lithium-rich layered oxide and 355 Wh kg−1 for silicon-graphite | |Ni-rich layer oxide pouch cells, calculated based on all cell components (positive electrode, negative electrode, separator and electrolyte). The design of the high-voltage electrolyte introduces a feasible approach to formulate a suitable solvation structure for high-specific-energy batteries.