Uneven lithium plating/stripping is an essential issue that inhibits stable cycling of a lithium metal anode and thus hinders its practical applications. The investigation of this process is challenging because it is difficult to observe lithium in an operating device. Here, we demonstrate that the microscopic lithium plating behavior can be observed in situ in a close-to-practical cell setup using X-ray computed tomography. The results reveal the formation of porous structure and its progressive evolution in space over the charging process with a large current. The elaborated analysis indicates that the microstructure of deposited lithium makes a significant impact on the subsequent lithium plating, and the impact of structural inhomogeneity, further exaggerated by the large-current charging, can lead to severely uneven lithium plating and eventually cell failure. Therefore, a codesign strategy involving delicate controls of microstructure and electrochemical conditions could be a necessity for the next-generation battery with lithium metal anode.
Keywords: X-ray computed tomography; dendrite; lithium metal anode; lithium metal battery; lithium plating.