Revealing the Distribution of Lithium Compounds in Lithium Dendrites by Four-Dimensional Electron Microscopy Analysis

Characterizing the microstructure of radiation- and chemical-sensitive lithium dendrites and its solid electrolyte interphase (SEI) is an important task when investigating the performance and reliability of lithium-ion batteries. Widely used methods, such as cryogenic high-resolution transmission electron microscopy as well as related spectroscopy, are able to reveal the local structure at nanometer and atomic scale; however, these methods are unable to show the distribution of various crystal phases along the dendrite in a large field of view. In this work, two types of four-dimensional electron microscopy diffractive imaging methods, i.e., scanning electron nanodiffraction (SEND) and scanning convergent beam electron diffraction (SCBED), are employed to show a new pathway on characterizing the sensitive lithium dendrite samples at room temperature and in a large field of view. Combining with the non-negative matrix factorization (NMF) algorithm, orientations of different lithium metal grains along the lithium dendrite as well as different lithium compounds in the SEI layer are clearly identified.