LAUSR

Abstract A numerical modeling of electrolyte oxidation based on the Bulter-Volmer equation is built to evaluate the relative importance of the irreversible reactions involved in the charging processes of high voltage lithium-ion battery. The modeling offers the possibility to judge oxidative sustainability of electrolyte under different charging conditions. Applying this model to series of charging procedures for a carbon coating LiCoPO4 (LCP/C), the measured quantities of the charge related to irreversible reactions show a linear correlation with the calculated specific quantities of charge associated with electrolyte oxidation. The capacity fading of high voltage cathode materials, in conjunction with an imperfect electrolyte dominated by the irreversible reactions related to electrolyte oxidation, can be regulated with the charging procedures. Therefore, the best charging strategy is to charge the cell at high C-rate with a suitable upper voltage. With the optimized procedure, the undoped LCP/C can achieve a final capacity of 63.1 mAh g−1 after 500 cycles at 1 C.