Issue 31, 2022

Transition between growth of dense and porous films: theory of dual-layer SEI

Abstract

The formation of passivating films is a common aging phenomenon, for example in weathering of rocks, silicon, and metals. In many cases, a dual-layer structure with a dense inner and a porous outer layer emerges. However, the origin of this dual-layer growth is so far not fully understood. In this work, a continuum model is developed, which describes the morphology evolution of the solid-electrolyte interphase (SEI) in lithium-ion batteries. Transport through the SEI and a growth reaction governed by the SEI surface energies are modelled. In agreement with experiments, this theory predicts that SEI grows initially as a dense film and subsequently as a porous layer. This dynamic phase transition is driven by the slowing down of electron transport as the film thickens. Thereby, the model offers a universal explanation for the emergence of dual-layer structures in passivating films.

Graphical abstract: Transition between growth of dense and porous films: theory of dual-layer SEI

Supplementary files

Article information

Article type
Communication
Submitted
12 Jan 2022
Accepted
23 May 2022
First published
17 Jun 2022
This article is Open Access
Creative Commons BY license

Phys. Chem. Chem. Phys., 2022,24, 18469-18476

Transition between growth of dense and porous films: theory of dual-layer SEI

L. von Kolzenberg, M. Werres, J. Tetzloff and B. Horstmann, Phys. Chem. Chem. Phys., 2022, 24, 18469 DOI: 10.1039/D2CP00188H

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