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

Abstract

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.

Optical sensors for operando stress monitoring in lithium-based batteries containing solid-state or liquid electrolytes

“…6g ). This finding is consistent with the recent operando synchrotron radiation X-ray tomographic microscopy report, which indicates the higher stress contribution is coming from the axial axis of the cell that is equivalent to the fiber transversal axis 54 . Moreover, we noted that the measured stress was nearly independent of the applied stack pressure in agreement with previous work 16 while it enables to reduce the cell polarization, hence favoring the charge transfer (Fig.…”

Understanding Transformations in Battery Materials Using in Situ and Operando Experiments: Progress and Outlook

“…In situ and operando methods for imaging structure and morphology of SSBs at longer length scales will be necessary to understand the origins of a variety of phenomena, including metal filament growth through solid-state electrolytes, 89,90 chemo-mechanical degradation of solid-state composite electrodes, 91 and the evolution of metal anode morphology. X-ray imaging promises to be an important technique to further our understanding of these phenomena, as it can provide spatial information from submicrometer to millimeter length scales.…”

“…A few in situ X-ray imaging studies of SSBs have recently been published, focusing on mechanical degradation due to reaction of active materials and interfaces (Figure 3a). 82,91 In situ optical imaging or SEM of SSB cells 90 could also lead to improved knowledge of electrode evolution and metal filament growth.…”

Challenges, interface engineering, and processing strategies toward practical sulfide‐based all‐solid‐state lithium batteries

“…Many efforts have been dedicated to the direct observation of stress-induced crack evolution. 85,[102][103][104][105][106][107][108][109] In general, the chemomechanics failures would occur inside CAM particles and in the contact region between CAMs and SEs. As illustrated in Figure 3A, the obvious cracks can be observed at the surface and extend to the inside of the NCM811 particle after the cell cycling.…”

“…Many efforts have been dedicated to the direct observation of stress‐induced crack evolution 85,102–109 . In general, the chemomechanics failures would occur inside CAM particles and in the contact region between CAMs and SEs.…”