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Entropymetry for non-destructive structural analysis of LiCoO2 cathodes
Energy & Environmental Science ( IF 33.250 ) Pub Date : 2019/12/04 , DOI: 10.1039/c9ee02964h
Hye Jin Kim; Youngkyu Park; Yoonjin Kwon; Jaeho Shin; Young-Han Kim; Hyun-Seok Ahn; Rachid Yazami; Jang Wook Choi

Upon the emergence of electric vehicles, accurate and non-destructive monitoring of battery electrode materials during operation is highly desirable. Structural degradation of widely adopted intercalation-based materials constitutes the origin of their capacity fading and safety deterioration. Here, we introduce entropymetry to monitor the structural changes of LiCoO2 (LCO) and its nickel (Ni)-doped derivatives at different states of charge (SOC). While simple lithium (Li) extraction on charging gives a monotonic decline of entropy change (ΔS) based on progressive vacancy occupation over Li sites, the presence of a monoclinic intermediate phase inverses the slope of the ΔS profile to reflect its limited atomic configurations with high ordering. Furthermore, Ni-doping lessens the ordering of the monoclinic phase, decreasing the height amplitude of ΔS profile in the monoclinic regime. The increased disorder by Ni-doping enhances the stability of the lattice framework, extending the cycle life with high voltage cut-off (4.6 V vs. Li/Li+). The present study highlights entropymetry as a unique, non-destructive tool in monitoring the structural ordering and relevant degradation of electrode materials in lithium-ion batteries.
更新日期:2020-02-13

 

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