Abstract
The rapid development of ultrahigh-capacity alloying or conversion-type anodes in rechargeable lithium (Li)-ion batteries calls for matching cathodes for next-generation energy storage devices. The high volumetric and gravimetric capacities, low cost, and abundance of iron (Fe) make conversion-type iron fluoride (FeF2 and FeF3 )-based cathodes extremely promising candidates for high specific energy cells. Here, the substantial boost in the capacity of FeF2 achieved with the addition of NiF2 is reported. A systematic study of a series of FeF2 -NiF2 solid solution cathodes with precisely controlled morphology and composition reveals that the presence of Ni may undesirably accelerate capacity fading. Using a powerful combination of state-of-the-art analytical techniques in combination with the density functional theory calculations, fundamental mechanisms responsible for such a behavior are uncovered. The unique insights reported in this study highlight the importance of careful selection of metals and electrolytes for optimizing electrochemical properties of metal fluoride cathodes.
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