Investigation of Fluorine and Nitrogen as Anionic Dopants in Nickel-Rich Cathode Materials for Lithium-Ion Batteries
2018
Binder, Jan O. | Culver, Sean P. | Pinedo, Ricardo | Weber, Dominik A. | Friedrich, Markus S. | Gries, Katharina I. | Volz, Kerstin | Zeier, Wolfgang G. | Janek, Jürgen
Advanced lithium-ion batteries are of great interest for consumer electronics and electric vehicle applications; however, they still suffer from drawbacks stemming from cathode active material limitations (e.g., insufficient capacities and capacity fading). One approach for alleviating such limitations and stabilizing the active material structure may be anion doping. In this work, fluorine and nitrogen are investigated as potential dopants in Li₁.₀₂(Ni₀.₈Co₀.₁Mn₀.₁)₀.₉₈O₂ (NCM) as a prototypical nickel-rich cathode active material. Nitrogen doping is achieved by ammonia treatment of NCM in the presence of oxygen, which serves as an unconventional and new approach. The crystal structure was investigated by means of Rietveld and pair distribution function analysis of X-ray diffraction data, which provide very precise information regarding both the average and local structure, respectively. Meanwhile, time-of-flight secondary-ion mass spectroscopy was used to assess the efficacy of dopant incorporation within the NCM structure. Moreover, scanning electron microscopy and scanning transmission electron microscopy were conducted to thoroughly investigate the dopant influences on the NCM morphology. Finally, the electrochemical performance was tested via galvanostatic cycling of half- and full-cells between 0.1 and 2 C. Ultimately, a dopant-dependent modulation of the NCM structure was found to enable the enhancement of the electrochemical performance, thereby opening a route to cathode active material optimization.
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