The origin of the capacity decrease of lithium-
ion batteries during continuous charge/discharge cycling, as
typified by battery operation in electric vehicles, is elucidated
using LiNi1/3Co1/3Mn1/3O2 (NCM)-based composite electro-
des. Electrochemical cycling tests without any rest process show
the capacity decrease only during discharging. Reaction
distribution analysis by operando energy-scanning confocal X-
ray diffraction indicates that considerable reaction inhomoge-
neity occurs on the lithiation of NCM during discharging,
whereas the delithiation during charging proceeds homoge-
neously. It is shown that the reaction inhomogeneity caused by
limited Li+ transportation in the composite electrode is relaxed
during charging owing to the potential profile of the NCM-
based electrode, whereas no such relaxation occurs during discharging. This result demonstrates that the optimization of the electrode potential profile is important for good cyclability of the batteries in continuous charge/discharge cycling, in addition to improving Li+ transportation within the battery.
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