A novel cathode interphase formation methodology by preferential adsorption of a borate-based electrolyte additive

Natl Sci Rev. 2024 Jun 25;11(8):nwae219. doi: 10.1093/nsr/nwae219. eCollection 2024 Aug.

Abstract

The coupling of high-capacity cathodes and lithium metal anodes promises to be the next generation of high-energy-density batteries. However, the fast-structural degradations of the cathode and anode challenge their practical application. Herein, we synthesize an electrolyte additive, tris(2,2,3,3,3-pentafluoropropyl) borane (TPFPB), for ultra-stable lithium (Li) metal||Ni-rich layered oxide batteries. It can be preferentially adsorbed on the cathode surface to form a stable (B and F)-rich cathode electrolyte interface film, which greatly suppresses the electrolyte-cathode side reactions and improves the stability of the cathode. In addition, the electrophilicity of B atoms in TPFPB enhances the solubility of LiNO3 by 30 times in ester electrolyte to significantly improve the stability of the Li metal anode. Thus, the Li||Ni-rich layered oxide full batteries using TPFPB show high stability and an ultralong cycle life (up to 1500 cycles), which also present excellent performance even under high voltage (4.8 V), high areal mass loading (30 mg cm-2) and wide temperature range (-30∼60°C). The Li||LiNi0.9Co0.05Mn0.05O2 (NCM90) pouch cell using TPFPB with a capacity of 3.1 Ah reaches a high energy density of 420 Wh kg-1 at 0.1 C and presents outstanding cycling performance.

Keywords: Ni-rich layered oxides cathode; electrolyte additives; high-energy-density pouch cells; interfacial stability; preferential adsorption.