Ni-Rich LiNi_0.8Co_0.1Mn_0.1O₂ Oxide Coated by Dual-Conductive Layers as High Performance Cathode Material for Lithium-Ion Batteries

Ni-rich materials are appealing to replace LiCoO₂ as cathodes in Li-ion batteries due to their low cost and high capacity. However, there are also some disadvantages for Ni-rich cathode materials such as poor cycling and rate performance, especially under high voltage. Here, we demonstrate the effect of dual-conductive layers composed of Li₃PO₄ and PPy for layered Ni-rich cathode material. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy show that the coating layers are composed of Li₃PO₄ and PPy. (NH₄)₂HPO₄ transformed to Li₃PO₄ after reacting with surface lithium residuals and formed an inhomogeneous coating layer which would remarkably improve the ionic conductivity of the cathode materials and reduce the generation of HF. The PPy layer could form a uniform film which can make up for the Li₃PO₄ coating defects and enhance the electronic conductivity. The stretchy PPy capsule shell can reduce the generation of internal cracks by resisting the internal pressure as well. Thus, ionic and electronic conductivity, as well as surface structure stability have been enhanced after the modification. The electrochemistry tests show that the modified cathodes exhibited much improved cycling stability and rate capability. The capacity retention of the modified cathode material is 95.1% at 0.1 C after 50 cycles, whereas the bare sample is only 86%, and performs 159.7 mAh/g at 10 C compared with 125.7 mAh/g for the bare. This effective design strategy can be utilized to enhance the cycle stability and rate performance of other layered cathode materials.