Publication date: 10th April 2024
Mn-based cation-disordered rock-salts (DRXs) cathodes such as Li1.2Mn0.6Nb0.2O2, offer an attractive higher energy density (~860 Wh/kg) without using costly Ni/Co. However, existing Mn-DRXs experience rapid voltage and capacity fading due to O-redox-driven side reactions, including Mn dissolution and O-loss, after just several tens of cycles. Our study shows that tailored formation cycle conditions can significantly mitigate these side reactions in Mn-rich DRXs. By increasing the charging cut-off voltage and decreasing the charging rate during the formation cycle, a metal-densified partial spinel-like phase forms on the surface of Mn-rich DRXs, leading to enhanced voltage and capacity retention. Moreover, we found that increasing the cycling temperature could trigger similar surface transformations with a lower charging cut-off voltage. Conversely, the less Mn-rich DRX displays a surface densified DRX phase under controlled formation cycle conditions, showing comparable cycling stability. This research underscores the pivotal role of formation cycle conditions and Mn content in controlling the surface structure of Mn-based DRX cathodes, suggesting a promising avenue to improve their electrochemical stability.
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