Low-temperature stepwise lithiation method toward layered oxide cathodes with low Li+/Ni2+ antisite defects

Although high-temperature solid-phase methods have become the dominant route for manufacturing layered oxide cathode materials in industry, severe Li+/Ni2+ cation mixing problems caused by high-temperature processes still prevent the realization of high-performance lithium-ion batteries. Herein, a wet chemical lithiation method by stepwise lithium intercalation to reduce and shorten the sintering temperature and time of the post-treatment process is proposed. Li0.6HxNi0.52Co0.19Mn0.29O2 stepwise products with lithiation efficiencies exceeding 60% were obtained at reaction temperatures below 200 °C. The as-prepared LiNi0.52Co0.19Mn0.29O2 (HT-52-S) exhibits low Li+/Ni2+ cation mixing and good comprehensive electrochemical performance after subsequent heat treatment to complete all lithiation. Compared with LiNi0.52Co0.19Mn0.29O2 (SS-52) prepared by the conventional high-temperature solid-phase method, the Li+/Ni2+ cation mixing of HT-52-S was relatively reduced by 57.9%, and the capacity retention after 100 cycles at 1 C was relatively improved by 22.1%. We believe that this work can serve as a useful reference to develop manufacturing processes for high-performance layered oxide cathode materials.