Impact of solid-electrolyte interphase reformation on capacity loss in silicon-based lithium-ion batteries

High-density silicon composite anodes show large volume changes upon charging/discharging triggering the reformation of the solid electrolyte interface (SEI), an interface initially formed at the silicon surface. The question remains how the reformation process and accompanied material evolution, in...

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Bibliographic Details
Published in:	Communications materials Vol. 4; no. 1; pp. 44 - 12
Main Authors:	Vorauer, T., Schöggl, J., Sanadhya, S. G., Poluektov, M., Widanage, W. D., Figiel, L., Schädler, S., Tordoff, B., Fuchsbichler, B., Koller, S., Brunner, R.
Format:	Journal Article
Language:	English
Published:	London Nature Publishing Group UK 06-06-2023 Nature Publishing Group Nature Portfolio
Subjects:	639/301/299/891 639/4077/4079/891 Anodes Chemistry and Materials Science Composite structures Cycles Electrolytes Electrolytic cells Evolution Interface stability Lithium-ion batteries Material properties Materials Science Microscopy Rechargeable batteries Silicon Solid electrolytes Stability analysis Workflow X ray microscopy
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Summary:	High-density silicon composite anodes show large volume changes upon charging/discharging triggering the reformation of the solid electrolyte interface (SEI), an interface initially formed at the silicon surface. The question remains how the reformation process and accompanied material evolution, in particular for industrial up-scalable cells, impacts cell performance. Here, we develop a correlated workflow incorporating X-ray microscopy, field-emission scanning electron microscopy tomography, elemental imaging and deep learning-based microstructure quantification suitable to witness the structural and chemical progression of the silicon and SEI reformation upon cycling. The nanometer-sized SEI layer evolves into a micron-sized silicon electrolyte composite structure at prolonged cycles. Experimental-informed electrochemical modelling endorses an underutilisation of the active material due to the silicon electrolyte composite growth affecting the capacity. A chemo-mechanical model is used to analyse the stability of the SEI/silicon reaction front and to investigate the effects of material properties on the stability that can affect the capacity loss. The solid electrolyte interface reformation process and material evolution in silicon composite anodes is not well understood. Here, the authors develop a correlated workflow to study the structural and chemical progression of silicon and solid electrolyte interface reformation upon cycling.
ISSN:	2662-4443 2662-4443
DOI:	10.1038/s43246-023-00368-1