Yttrium Surface Gradient Doping for Enhancing Structure and Thermal Stability of High-Ni Layered Oxide as Cathode for Li-Ion Batteries.

The high-nickel layered oxides are potential candidate cathode materials of next-generation high energy lithium-ion batteries, in which higher nickel/lower cobalt strategy is effective for increasing specific capacity and reducing cost of cathode. Unfortunately, the fast decay of capacity/potential, and serious thermal concern are critical obstacles for the commercialization of high-nickel oxides due to structural instability. Herein, in order to improve the structure and thermal stability of high-nickel layered oxides, we demonstrate a feasible and simple strategy of the surface gradient doping with yttrium, without forming the hard interface between coating layer and bulk. As expected, after introducing yttrium, the surface gradient doping layer is formed tightly based on the oxidation induced segregation, leading to improved structure and thermal stability. Correspondingly, the good capacity retention and potential stability are obtained for the yttrium-doped sample, together with the superior thermal behavior. The excellent electrochemical performance of the yttrium-doped sample is primarily attributed to the strong yttrium-oxygen bonding and stable oxygen framework on the surface layer. Therefore, the surface manipulating strategy with the surface gradient doping is feasible and effective for improving the structure and thermal stability, as well as the capacity/potential stability during cycling for the high-Ni layered oxides.