Operando Visualization of Morphological Dynamics in All-Solid-State Batteries


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.