PNNL

Abstract

Li-rich and Mn-rich (LMR) layered structured materials are very promising cathodes for high-energy lithium-ion batteries. However, their fundamental structure and voltage fading mechanisms are far from being well understood. Here we report the first evidence on the reduced voltage and energy fade of LMR cathode by improving the atomic level spatial distribution of the chemical species. LMR cathode (Li[Li0.2Ni0.2M0.6]O2) prepared by co-precipitation and sol-gel methods are dominated by R-3m phase and show significant Ni-segregation at the surface of the particles. They exhibit large voltage-fade and fast capacity degradation. In contrast, LMR cathode prepared by hydrothermal assisted method is dominated by C2/m phase and minimal Ni-segregation. It also demonstrates much smaller voltage-fade and excellent capacity retention. The fundamental correlation between the atomic level spatial distribution of the chemical species and the functional stability of the materials found in this work also guide the design of other functional materials with enhanced stabilities.