Li(1+x)[Ni-M](1-x)O2基化合物d0过渡金属的无序固溶结构设计与电化学性能优化

锂离子电池由于能量密度高、循环寿命长等特点受到广泛关注，然而资源丰富、成本低廉的LiNiO2锂电池正极材料具有热稳定性不佳、循环性能差等问题，限制了其大规模应用。通过富锂相d0过渡金属氧化物Li-d0-O与LiNiO2固溶形成阳离子无序的富锂镍氧化物是提升LiNiO2材料电化学性能的有效途径。本项目通过第一性原理计算与电极材料结构表征以及电化学测试结合，研究不同富锂相d0过渡金属氧化物在不同固溶浓度下对阳离子无序结构、电化学性能的影响规律，并筛选出具有热力学稳定、高锂离子扩散率、高氧空位稳定性的阳离子无序材料，从而提升LiNiO2材料的电化学性能。项目的顺利实施将推动锂离子电池正极材料的应用，并为其它正极材料的设计和优化提供新思路。

Li-ion battery has been of great interest owing to its high energy density and long cycling life. Unfortunately, when used as cathode material, LiNiO2 is energy unstable upon cycling and displays severe capacity fading, which limits the large-scale applications. It is an effective method to improve the electrochemical performance of LiNiO2 by utilizing cation-disorder lithium-excess nickel oxide, which is a solid solution formed by Li-rich d0-transition metal oxide Li-d0-O and lithium nickelate LiNiO2. Based on first principles calculations, structural characteristics and electrochemical measurement, we systemically investigate the influence of various solid-solution concentrations of different d0 transition metal on cation-disorder structure and its electrochemical performance. The cation-disorder structures with thermodynamical stability, high lithium diffusivity, and high oxygen-vacancy stability should be selected as material with the best performance. The successful implementation of this project will promote the application of cathode materials of Li-ion batteries, and provide new ideas for the design and performance optimization of other cathode materials.