期刊
CHEMISTRY OF MATERIALS
卷 25, 期 14, 页码 2885-2889出版社
AMER CHEMICAL SOC
DOI: 10.1021/cm4014738
关键词
Ni-Mn spinel; rate capability; phase diagram; solid-solution; first-principles calculation
资金
- Office of Vehicle Technologies of the U.S. Department of Energy [DE-AC02-05CH11231]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
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 LixNi0.5Mn1.5O4 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.
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