Integrated Modification Strategy Enables Remarkable Cyclability and Thermal Stability of Ni-Rich Cathode Materials for Lithium-Ion Batteries.

Structural degradation and surface chemical instability are dominant issues of Ni-rich layered cathodes, which trigger capacity fading and safety concerns, hindering the extensive application of Ni-rich cathodes toward high-energy, long-life lithium-ion batteries. Here, by combining trace Ta doping and an ultrathin Zr-Y mixed oxide coating, an integrated modification strategy significantly improves the cycling and thermal stability of Ni-rich LiNiCoAlO (NCA) cathodes. The integrated modified Ni-rich cathode provides an unprecedented comprehensive performance with a high discharge capacity of 212.2 mA h g at 0.1 , an 88.6% cycling retention after 500 cycles at 1 , and a high exothermic peak temperature of 261 °C compared with the pristine NCA cathode (67.4% capacity retention for 500 cycles and 221 °C for the exothermic peak). Further mechanism studies illustrate that a dual-structural surface constructed of a rock salt surface induced by Ta doping and ultrathin Zr-Y mixed oxide coating jointly suppresses surface side reactions between cathodes and electrolytes. Moreover, trace Ta doping in the bulk stabilizes the bulk structure and prevents mechanical cracks. This study highlights the importance of comprehensive modification of the bulk and surface for improving the electrochemical performance and provides a potential optimizing strategy for the commercialization of high-capacity Ni-rich cathode materials.