Impact of dual-layer solid-electrolyte interphase inhomogeneities on early-stage defect formation in Si electrodes

Chunguang Chen*, Tao Zhou, Dmitri L. Danilov, Lu Gao, Svenja Benning, Nino Schön, Samuel Tardif, Hugh Simons, Florian Hausen, Tobias U. Schülli, R. A. Eichel, Peter H.L. Notten*

*Corresponding author for this work

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Abstract

While intensive efforts have been devoted to studying the nature of the solid-electrolyte interphase (SEI), little attention has been paid to understanding its role in the mechanical failures of electrodes. Here we unveil the impact of SEI inhomogeneities on early-stage defect formation in Si electrodes. Buried under the SEI, these early-stage defects are inaccessible by most surface-probing techniques. With operando full field diffraction X-ray microscopy, we observe the formation of these defects in real time and connect their origin to a heterogeneous degree of lithiation. This heterogeneous lithiation is further correlated to inhomogeneities in topography and lithium-ion mobility in both the inner- and outer-SEI, thanks to a combination of operando atomic force microscopy, electrochemical strain microscopy and sputter-etched X-ray photoelectron spectroscopy. Our multi-modal study bridges observations across the multi-level interfaces (Si/LixSi/inner-SEI/outer-SEI), thus offering novel insights into the impact of SEI homogeneities on the structural stability of Si-based lithium-ion batteries.
Original languageEnglish
Article number3283
JournalNature Communications
Volume11
Issue number1
Number of pages10
ISSN2041-1723
DOIs
Publication statusPublished - 2020

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