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Article Abstract
Nitriles have been successfully used as electrolyte additives for performance improvement of commercialized lithium-ion batteries based on the LiCoO cathode, but the underlying mechanism is unclear. In this work, we present an insight into the contribution of nitriles via experimental and theoretical investigations, taking for example succinonitrile. It is found that succinonitrile can be oxidized together with PF preferentially on LiCoO compared to the solvents in the electrolyte, making it possible to avoid the formation of hydrogen fluoride from the electrolyte oxidation decomposition, which is detrimental to the LiCoO cathode. Additionally, inorganic LiF and -NH group-containing polymers are formed from the preferential oxidation of succinonitrile, constructing a protective interphase on LiCoO, which suppresses electrolyte oxidation decomposition and prevents LiCoO from structural deterioration. Consequently, the LiCoO cathode presents excellent stability under cycling and storing at high voltages.
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