@article{26824,
  author = {Eunseok Lee and Kristin A Persson},
  title = {Solid-Solution Li Intercalation as a Function of Cation Order/Disorder in the High-Voltage Li<sub>x</sub>Ni<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> Spinel},
  abstract = {<p>Many Li-ion cathode materials transform via two-phase reactions, which can lead to long-term structural damage and limited cyclability. To elucidate the coupling between favorable solid-solution Li intercalation and the underlying cation ordering, we take the high-voltage spinel, LixNi0.5Mn1.5O4 (0 ≤ x ≤ 1), as a case example. Through grand canonical Monte Carlo (MC) simulations based on the ab initio cluster expansion model, we show a striking dependence between the solid-solution phase domain and the Ni−Mn cation ordering. The perfectly ordered LixNi0.5- Mn1.5O4 spinel resists solid solution until very high temperatures, but introducing various degrees of Ni−Mn cation disorder results in a dramatic increase in stability for a single-phase reaction, particularly at high Li contents. This opens up the possibility of designing single-phase reaction materials via targeted cation ordering, and to this end, we show that a uniformly distributed cation high-voltage spinel has access to solid solution throughout the entire Li composition range at room temperature.</p>},
  year = {2013},
  journal = {Chemistry of Materials},
  volume = {25},
  pages = {2885-2889},
  month = {07/2013},
  doi = {10.1021/cm4014738},
  language = {eng},
}