Dictating the interfacial stability of nickel-rich LiNi0.90Co0.05Mn0.05O2 via a diazacyclo electrolyte additive – 2-Fluoropyrazine

Nickel-rich (Ni-rich) cathode materials, LiNixCoyMnzO2 (NCM, x ≥ 0.9, x + y + z = 1) hold great promise for developing high energy density lithium ion batteries especially for vehicle electrification. However, the practical application of Ni-rich cathode materials is still suffered from fast structural and interfacial degradation, and the resulted capacity decay. In this study, a diazacyclo type electrolyte additive, 2-fluoropyrazine (2-FP), was explored for the first time to boost the interfacial stabilization of single crystal LiNi0.90Co0.05Mn0.05O2 (NCM90) cathode. The capacity retention of the NCM90 is evidently promoted from 72.3% to 82.1% after 200 cycles at 1C (180 mA g-1) when adding 0.2% 2-FP into the electrolyte. The improvement of the electrochemical performance is ascribed to the generation of a compact and homogeneous cathode electrolyte interphase (CEI) film through ring-opening electrochemical polymerization of 2-FP upon the NCM90 electrode particles. This enhanced CEI layer benefits the suppression of the decomposition of LiPF6 electrolyte and the dissolution of the transition metals (Co and Mn), thus preventing the detrimental side reactions between the NCM90 electrode and the electrolyte.