Improvement of Cycling Stability of Core–Shell Structured Ni-Rich NMC Cathodes by Using a Tungsten Oxide Stabilization Interlayer

Kurzfassung

The growing demand for higher-energy lithium-ion batteries, encompassing consumer electronics, stationary grid storage, and electric mobility to specialized sectors like aerospace, medical devices, and industrial robotics, requires cathode materials that offer higher capacity while remaining cost-effective. This trend has intensified the development of nickel-rich LiNi1−x−yMnxCoyO2 (NMC) systems. However, high-Ni NMCs such as LiNi0.9Mn0.05Co0.05O2 (NMC90) suffer from limited thermal and cycling stability. Core–shell architectures using LiNi0.6Mn0.2Co0.2O2 (NMC622) as a shell can partially alleviate these drawbacks, but structural degradation caused by interdiffusion between the core and shell persists as a major challenge. This study investigates whether a tungsten oxide interlayer can act as a protective barrier that suppresses interdiffusion, stabilizes the crystal structure, and improves long-term electrochemical performance. In this work, NMC cathode powders were synthesized via a one-pot oxalate co-precipitation route, followed by structural characterization using X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and ion scattering spectroscopy (ISS). Electrochemical performance, including capacity retention, cycling stability, and internal resistance, was evaluated through galvanostatic charge–discharge (GCD) testing and electrochemical impedance spectroscopy (EIS). The core–shell configuration delivered higher specific discharge capacity compared to the individually synthesized core-only and shell-only reference materials, and the incorporation of a tungsten oxide interlayer resulted in a twofold increase in cycle life. These results demonstrate that tungsten oxide effectively enhances cycling stability by inhibiting core–shell interdiffusion, offering a promising pathway toward more durable high-Ni NMC cathodes.