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 and Peter H. L. Notten ()
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Chunguang Chen: IEK-9, Forschungszentrum Jülich
Tao Zhou: ID01 ESRF, CS 40220
Dmitri L. Danilov: IEK-9, Forschungszentrum Jülich
Lu Gao: Eindhoven University of Technology
Svenja Benning: IEK-9, Forschungszentrum Jülich
Nino Schön: IEK-9, Forschungszentrum Jülich
Samuel Tardif: Univ. Grenoble Alpes, CEA, IRIG-MEM
Hugh Simons: Technical University of Denmark
Florian Hausen: IEK-9, Forschungszentrum Jülich
Tobias U. Schülli: ID01 ESRF, CS 40220
R.-A. Eichel: IEK-9, Forschungszentrum Jülich
Peter H. L. Notten: IEK-9, Forschungszentrum Jülich

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-17104-9

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