Nanoarchitecture factors of solid electrolyte interphase formation via 3D nano-rheology microscopy and surface force-distance spectroscopy

• Published in: Nature communications Vol. 14; no. 1; p. 1321
• Main Authors: Chen, Yue, Wu, Wenkai, Gonzalez-Munoz, Sergio, Forcieri, Leonardo, Wells, Charlie, Jarvis, Samuel P., Wu, Fangling, Young, Robert, Dey, Avishek, Isaacs, Mark, Nagarathinam, Mangayarkarasi, Palgrave, Robert G., Tapia-Ruiz, Nuria, Kolosov, Oleg V.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 10.03.2023; Nature Publishing Group; Nature Portfolio
• Subjects: 140/133; 140/146; 147/136; 147/3; 639/301/299/891; 639/4077/4079/891; 639/638/675; 639/925/357/995; Atomic force microscopy; Electric double layer; Electrochemistry; Electrodes; Electrolytes; Energy storage; Graphite; Humanities and Social Sciences; Interfaces; Interphase; Liquid-solid interfaces; Lithium-ion batteries; Microscopy; Molten salt electrolytes; multidisciplinary; Rechargeable batteries; Rheological properties; Rheology; Science; Science (multidisciplinary); Solid electrolytes; Spectroscopy; Spectrum analysis
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-37033-7

The solid electrolyte interphase in rechargeable Li-ion batteries, its dynamics and, significantly, its nanoscale structure and composition, hold clues to high-performing and safe energy storage. Unfortunately, knowledge of solid electrolyte interphase formation is limited due to the lack of in situ nano-characterization tools for probing solid-liquid interfaces. Here, we link electrochemical atomic force microscopy, three-dimensional nano-rheology microscopy and surface force-distance spectroscopy, to study, in situ and operando, the dynamic formation of the solid electrolyte interphase starting from a few 0.1 nm thick electrical double layer to the full three-dimensional nanostructured solid electrolyte interphase on the typical graphite basal and edge planes in a Li-ion battery negative electrode. By probing the arrangement of solvent molecules and ions within the electric double layer and quantifying the three-dimensional mechanical property distribution of organic and inorganic components in the as-formed solid electrolyte interphase layer, we reveal the nanoarchitecture factors and atomistic picture of initial solid electrolyte interphase formation on graphite-based negative electrodes in strongly and weakly solvating electrolytes. Characterization of the solid electrolyte interphase formed on Li-ion battery electrodes presents significant experimental challenges. Here the authors use atomic force microscopy-based force-spectroscopy techniques to depict the initial interphase formation in two different electrolyte classes.