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<p>All-solid-state batteries are considered as attractive options for next-generation energy storage
owing to the favourable properties (unit transference number and thermal stabilities) of solid
electrolytes. However, there are also serious concerns about mechanical deformation of solid
electrolytes leading to the degradation of the battery performance. Therefore, understanding
the mechanism underlying the electro-mechanical properties in SSBs are essentially important.
Here, we show three-dimensional and time-resolved measurements of an all-solid-state cell
using synchrotron radiation x-ray tomographic microscopy. We could clearly observe the
gradient of the electrochemical reaction and the morphological evolution in the composite
layer. Volume expansion/compression of the active material (Sn) was strongly oriented along
the thickness of the electrode. While this results in significant deformation (cracking) in the
solid electrolyte region, we also find organized cracking patterns depending on the particle
size and their arrangements. This study based on operando visualization therefore opens the
door towards rational design of particles and electrode morphology for all-solid-state batteries. </p>
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