Synergistic Effects of Surface Coating and Bulk Doping in Ni‐Rich Lithium Nickel Cobalt Manganese Oxide Cathode Materials for High‐Energy Lithium Ion Batteries

Ni‐rich layered oxide cathodes are promising candidates to satisfy the increasing energy demand of lithium‐ion batteries for automotive applications. Thermal and cycling stability issues originating from increasing Ni contents are addressed by mitigation strategies such as elemental bulk substitution (“doping”) and surface coating. Although both approaches separately benefit the cycling stability, there are only few reports investigating the combination of two of such approaches. Herein, the combination of Zr as common dopant in commercial materials with effective Li2WO4 and WO3 coatings was investigated with special focus on the impact of different material processing conditions on structural parameters and electrochemical performance in nickel‐cobalt‐manganese (NCM) || graphite cells. Results indicated that the Zr4+ dopant diffusing to the surface during annealing improved the electrochemical performance compared to samples without additional coatings. This work emphasizes the importance to not only investigate the effect of individual dopants or coatings but also the influences between both. (I can't get no) satisfaction: Ni‐rich nickel‐cobalt‐manganese (NCM)‐type layered oxide materials are promising candidates to satisfy the increasing energy demand of lithium‐ion batteries for automotive applications but have major drawbacks in terms of mechanical stability and cycling stability. Herein, the challenges of combining two mitigation strategies (i. e., Zr4+ doping and W6+ coating), their synergistic effects, and the importance of investigating heat‐treated references are reported.