Evolution Process of the Interfacial Chemical Reaction in Ni-Rich Layered Cathodes for All-Solid-State Batteries

All-solid-state batteries (ASSBs) have attracted much attention in the fields of energy storage, electric vehicles, and portable electronic devices due to their safety and high energy density. Ni-rich layered ternary materials (LiNi_1-CoMnO₂, 1 - y - z ≥ 0.7) are considered to be among the most promising candidates for cathode materials in ASSBs due to their unique advantages. Nevertheless, the interfacial chemical reaction between the ternary cathode (NCM) and solid-state electrolytes (SSEs) has become the main issue to limit the long-cycle stability of the cathode. Relative studies have shown that when NCM materials are in direct contact with sulfide-based SSEs, byproducts generated by the interfacial chemical reaction accumulate at the interface, resulting in increasing interfacial impedance. However, up to now, the formation mechanism of the NCM/SSE interfacial chemical reaction, as well as its properties and evolution process, still lacks detailed characterization. In this paper, batteries at different stages during the long-cycling process are characterized to reveal the dynamic evolution process of the chemical reaction from the cathode-electrolyte interface to the interior of the particle and to determine the chemical reaction effect on the irreversible degradation of the battery capacity. On this basis, a surface coating of LiNbO₃ is adopted to establish a passivation protection layer at the cathode-electrolyte interface. The coated battery has been subjected to 2000 charge/discharge cycles at a rate of 1 C and achieved a capacity retention rate of up to 82%.