Enabling stable 4.6 V LiCoO_(2) cathode through oxygen charge regulation strategy

LiCoO_(2) is the preferred cathode material for consumer electronic products due to its high volumetric energy density. However, the unfavorable phase transition and surface oxygen release limits the practical application of LiCoO_(2)at a high-voltage of 4.6 V to achieve a higher energy density demanded by the market. Herein, both bulk and surface structures of LiCoO_(2)are stabilized at 4.6 V through oxygen charge regulation by Gd-gradient doping. The enrichment of highly electropositive Gd on LiCoO_(2) surface will increase the effective charge on oxygen and improve the oxygen framework stability against oxygen loss.On the other hand, Gd ions occupy the Co-sites and suppress the unfavorable phase transition and microcrack. The modified LiCoO_(2) exhibits superior cycling stability with capacity retention of 90.1% over 200 cycles at 4.6 V, and also obtains a high capacity of 145.7 m Ah/g at 5 C. This work shows great promise for developing high-voltage LiCoO_(2) at 4.6 V and the strategy could also contribute to optimizing other cathode materials with high voltage and large capacity, such as cobalt-free high-nickel and lithiumrich manganese-based cathode materials.