Operando X-ray diffraction analysis of the degradation mechanisms of a spinel LiMn2O4 cathode in dif

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The understanding of reaction mechanisms of electrode materials is of significant importance for the development of advanced batteries.The LiMn2O4 cathode has a voltage plateau around 2.8V (vs.Li+/Li),which can provide an additional capacity for Li storage,but it suffers from a severe capacity degradation.In this study,operando X-ray diffraction is carried out to investigate the structural evolutions and degradation mechanisms of LiMn2O4 in different voltage ranges.In the range of 3.0-4.3V (vs.Li+/Li),the LiMn2O4 cathode exhibits a low capacity but good cycling stability with cycles up to 100 cycles and the charge/discharge processes are associated with the reversible extraction/insertion of Li+ from/into LixMn2O4 (0 ≤x≤ 1).In the range of 1.4-4.4V (vs.Li+/Li),a capacity higher than 200 mAh/g is achieved,but it rapidly decays during the cycling.The voltage plateau around 2.8V (vs.Li+/Li) is related to the transformation of the cubic LiMn2O4 phase to the tetragonal Li2Mn2O4 phase,which leads to the formation of cracks as well as the performance degradation.
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