Dual-Salt Localized High-Concentration Electrolyte for Long Cycle Life Silicon-Based Lithium-Ion Batteries

Gaopan Liu; Meng Xia; Jian Gao; Yong Cheng; Mingsheng Wang; Wenjing Hong; Yong Yang; Jianming Zheng

doi:10.1021/acsami.2c17512

Dual-Salt Localized High-Concentration Electrolyte for Long Cycle Life Silicon-Based Lithium-Ion Batteries

ACS Appl Mater Interfaces. 2023 Jan 18;15(2):3586-3598. doi: 10.1021/acsami.2c17512. Epub 2023 Jan 4.

Authors

Gaopan Liu¹, Meng Xia¹, Jian Gao¹, Yong Cheng^{1

2}, Mingsheng Wang², Wenjing Hong¹, Yong Yang¹, Jianming Zheng¹

Affiliations

¹ State Key Laboratory for Physical Chemistry of Solid Surface, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
² State Key Laboratory for Physical Chemistry of Solid Surface, College of Materials, Xiamen University, Xiamen 361005, China.

PMID: 36598884
DOI: 10.1021/acsami.2c17512

Abstract

Silicon-based materials are considered the most promising anodes for next-generation lithium-ion batteries (LIBs) owing to their high specific capacity. However, poor interfacial stability due to enormous volume changes severely restricts their mass application in LIBs. Here, we design a fluoroethylene carbonate (FEC)-containing dual-salt (LiFSI-LiPF₆) ether-based localized high-concentration electrolyte (D-LHCE-F) for enhancing the interfacial stability of silicon-based electrodes. It is revealed that the dominating LiFSI salt of superior chemical and thermal stability prevents the formation of corrosive HF, while the addition of FEC improves the interface stability by promoting the formation of protective LiF-rich SEI and increasing the flexibility of the interface. This robust and flexible SEI layer can adapt to substantial variations in the volume of silicon electrodes while preserving the integrity of the interface. The SiO_x/C electrode using the unique D-LHCE-F retains up to 78.5% of its initial capacity after 500 cycles at 0.5C, well surpassing that of the control electrolyte (3.4% capacity retention). More notably, the cycle life of the SiO_x/C||NCM90 (LiNi_0.9Co_0.05Mn_0.05O₂) full batteries is effectively enhanced thanks to the stabilized electrode/electrolyte interfaces. The key findings of this work offer crucial knowledge for rationally designing electrolyte chemistry to enable the practical application of high-energy-density LIBs adopting silicon-based anodes.

Keywords: electrolyte; high energy density; interfacial stability; lithium-ion batteries; silicon-based electrode; solvation structure.