Dynamic Evolution of a Cathode Interphase Layer at the Surface of LiNi_0.5Co_0.2Mn_0.3O₂ in Quasi-Solid-State Lithium Batteries

Intensive understanding of the surface mechanism of cathode materials, such as structural evolution and chemical and mechanical stability upon charging/discharging, is crucial to design advanced solid-state lithium batteries (SSLBs) of tomorrow. Here, via <i>in situ</i> atomic force microscopy monitoring, we explore the dynamic evolution process at the surface of LiNi_0.5Co_0.2Mn_0.3O₂ cathode particles inside a working SSLB. The dynamic formation process of the cathode interphase layer, with an inorganic–organic hybrid structure, was real-time imaged, as well as the evolution of its mechanical property by <i>in situ</i> scanning of the Derjaguin–Muller–Toporov modulus. Moreover, different components of the cathode interphase layer, such as LiF, Li₂CO₃, and specific organic species, were identified in detailat different stages of cycling, which can be directly correlated with the impedance buildup of the battery. In addition, the transition metal migration and the formation of new phases can further exacerbate the degradation of the SSLB. A relatively stable cathode interphase is key to improving the performance of SSLBs. Our findings provide deep insights into the dynamic evolution of surface morphology, chemical components and mechanical properties of the cathode interphase layer, which are pivotal for the performance optimization of SSLBs.