Electric vehicles (EVs) are poised to dominate the next generation of transportation, but meeting the power requirements of EVs with lithium ion batteries is challenging because electrolytes containing LiPF6 and carbonates do not perform well at high temperatures and voltages. However, lithium benzimidazole salt is a promising electrolyte additive that can stabilize LiPF6 through a Lewis acid–base reaction. The imidazole ring is not eligible for high-voltage applications owing to its resonance structure, but in this research, electron-withdrawing (−CF3) and electron-donating (−CH3) substitutions on imidazole rings were investigated. According to the calculation results, the CF3 substitution facilitates a high electron cloud density on imidazole ring structures to resist the electron releases from bezimidazole in oxidation reactions. In addition, through CF3 substitution, electrons are accepted from the lattice oxygen (O2–) in lithium-rich layer material and O– is converted by an electron released. The O– is then adsorbed with the ethylene carbonate and catalyzed to alkyl carbonate by Ni2+. The −CF3 substituted benzimidazole triggers a further reaction with alkyl carbonate and forms a new polyionic liquid solid electrolyte interphase on the cathode’s surface. Furthermore, the cycle performance tested at 60 °C and 4.8 V showed that the CF3 substitution maintains the battery retention effectively and exhibits almost no fading compared with both the blank electrolyte and the CH3 substitution.

Ni-rich high-energy-density lithium ion batteries pose great risks to safety due to internal short circuits and overcharging; they also have poor performance because of cation mixing and disordering problems. For Ni-rich layered cathodes, these factors cause gas evolution, the formation of side products, and life cycle decay. In this study, a new cathode electrolyte interphase (CEI) for Ni2+ self-oxidation is developed. By using a branched oligomer electrode additive, the new CEI is formed and prevents the reduction of Ni3+ to Ni2+ on the surface of Ni-rich layered cathode; this maintains the layered structure and the cation mixing during cycling. In addition, this new CEI ensures the stability of Ni4+ that is formed at 100% state of charge in the crystal lattice at high temperature (660 K); this prevents the rock-salt formation and the over-reduction of Ni4+ to Ni2+. These findings are obtained using in situ X-ray absorption spectroscopy, operando X-ray diffraction, operando gas chromatography–mass spectroscopy, and X-ray photoelectron spectroscopy. Transmission electron microscopy reveals that the new CEI has an elliptical shape on the material surface, which is approximately 100 nm in length and 50 nm in width, and covers selected particle surfaces. After the new CEI was formed on the surface, the Ni2+ self-oxidation gradually affects from the surface to the bulk of the material. It found that the bond energy and bond length of the Ni–O are stabilized, which dramatically inhibit gas evolution. The new CEI is successfully applied in a Ni-rich layered compound, and the 18650- and the punch-type full cells are fabricated. The energy density of the designed cells is up to 300 Wh/kg. Internal short circuit and overcharging safety tests are passed when using the standard regulations of commercial evaluation. This new CEI technology is ready and planned for future applications in electric vehicle and energy storage.

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