This paper explores the use of multimodal X-ray and neutron operando tomography to study all-solid-state lithium-ion batteries (ASSBs). The use of operando neutron tomography as a method for quantifying the local lithium distribution in battery cells under charging is explored in conjunction with the use of simultaneous operando X-ray tomography to obtain complementary information about the internal battery structure. It is demonstrated how the components of an ASSB can be segmented in the dual modality images to reveal the topology of the electrodes. Next, 4D mapping of the lithium isotope content in the separator revealed spatial inhomogeneities in the distribution of Li-6 and Li-7. Furthermore, the delithiation process in the cathode of an ASSB has been followed in 4D, revealing lithium concentration gradients in the cathode, even with the slow delithiation rate used in the experiment.
Vestin et al. (Thu,) studied this question.