Journal Article

FZJ-2020-02370

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Impact of dual-layer solid-electrolyte interphase inhomogeneities on early-stage defect formation in Si electrodes

Chen, C. (Corresponding author)FZJ* ; Zhou, T. ; Danilov, D. L.FZJ* ; Gao, L. ; Benning, S.FZJ* ; Schön, N.RWTH* ; Tardif, S. ; Simons, H. ; Hausen, F.FZJ*RWTH* ; Schülli, T. U. ; Eichel, R.-A.FZJ*RWTH* ; Notten, P. H. L. (Corresponding author)FZJ*

2020
Nature Publishing Group UK [London]

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Please use a persistent id in citations: http://hdl.handle.net/2128/25265  doi:10.1038/s41467-020-17104-9

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.

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Contributing Institute(s):

1. Grundlagen der Elektrochemie (IEK-9)

Research Program(s):

1. 131 - Electrochemical Storage (POF3-131) (POF3-131)
2. HITEC - Helmholtz Interdisciplinary Doctoral Training in Energy and Climate Research (HITEC) (HITEC-20170406) (HITEC-20170406)

Appears in the scientific report 2020

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