The spatially resolved and quantitative observation and
analysis
of an all-solid-state lithium-ion battery (ASSLiB) under operating
conditions play an important role in understanding the reaction or
degradation mechanisms of the battery system. In this study, the chemical
state distribution of a LiCoO2 cathode and Fe2(MoO4)3 anode layers in a thin-film-type ASSLiB
under operating conditions is visualized in the single field of view
from a cross-sectional direction using full-field transmission microscopy
with X-ray absorption fine structure spectroscopy. Operando measurements during stepped charge/discharging processes revealed
the different tendencies of the redox percolation of Co and Fe in
the cathode and anode layers, respectively, during the charging/discharging
process according to the difference in their lithiation/delithiation
mechanisms. We also determine that structural and chemical degradation
occurs in both layers after repeating charge–discharge cycling.
In the cathode layer, the electrode is exfoliated and the Co in the
entire layer becomes more oxidized after degradation, while in the
anode layer, Fe2(MoO4)3 decomposes
into γ-Fe2O3 and causes the layer to crack.