Unveiling the Genesis and Effectiveness of Negative Fading in Nanostructured Iron Oxide Anode Materials for Lithium-Ion Batteries.

Iron oxide anode materials for rechargeable lithium-ion batteries have garnered extensive attention because of their inexpensiveness, safety, and high theoretical capacity. Nanostructured iron oxide anodes often undergo negative fading, that is, unconventional capacity increase, which results in a capacity increasing upon cycling. However, the detailed mechanism of negative fading still remains unclear, and there is no consensus on the provenance. Herein, we comprehensively investigate the negative fading of iron oxide anodes with a highly ordered mesoporous structure by utilizing advanced synchrotron-based analysis. Electrochemical and structural analyses identified that the negative fading originates from an optimization of the electrolyte-derived surface layer, and the thus formed layer significantly contributes to the structural stability of the nanostructured electrode materials, as well as their cycle stability. This work provides an insight into understanding the origin of negative fading and its influence on nanostructured anode materials.