Enhancing the Stability and Performance of Ni-rich Cathode Materials through Ta Doping: A Combined Theoretical and Experimental Study

As the demand for high-energy batteries to power electric vehicles continues to grow, Ni-rich cathode materials have emerged as promising candidates due to their high capacity. However, these materials are prone to rapid degradation under increased voltages, posing significant challenges for their long-term stability and safety. In this study, we investigate the effects of tantalum (Ta) doping on the performance and stability of LiNi0.80Mn0.1Co0.1O2 (NMC811) cathode materials. Using a combined theoretical and experimental approach, we employ Density Functional Theory (DFT) and Cluster Expansion models to analyze the electronic structure and oxygen vacancy formation enthalpy in Ta-doped NMC811. Experimental validation is conducted using cycling and gas measurements via On-line Electrochemical Mass Spectrometry (OEMS) on in-house synthesized cathode active materials.