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

Chen, Yue and Wu, Wenkai and Gonzalez Munoz, Sergio and Forcieri, Leonardo and Wells, Charlie and Jarvis, Samuel and Wu, Fangling and Young, Robert and Dey, Avishek and Isaaks, Mark and Nagarathinam, Mangayarkarasi and Palgrave, Robert and Tapia-Ruiz, Nuria and Kolosov, Oleg (2023) Nanoarchitecture factors of solid – electrolyte interphase formation via 3D nano-rheology microscopy and surface force-distance spectroscopy. Nature Communications, 14. ISSN 2041-1723

Abstract

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.