Failure mechanisms of single-crystal silicon electrodes in lithium-ion batteries

Feifei Shi, Zhichao Song, Philip N. Ross, Gabor A. Somorjai, Robert O. Ritchie, Kyriakos Komvopoulos

Research output: Contribution to journalArticlepeer-review

194 Scopus citations


Long-term durability is a major obstacle limiting the widespread use of lithium-ion batteries in heavy-duty applications and others demanding extended lifetime. As one of the root causes of the degradation of battery performance, the electrode failure mechanisms are still unknown. In this paper, we reveal the fundamental fracture mechanisms of single-crystal silicon electrodes over extended lithiation/delithiation cycles, using electrochemical testing, microstructure characterization, fracture mechanics and finite element analysis. Anisotropic lithium invasion causes crack initiation perpendicular to the electrode surface, followed by growth through the electrode thickness. The low fracture energy of the lithiated/unlithiated silicon interface provides a weak microstructural path for crack deflection, accounting for the crack patterns and delamination observed after repeated cycling. On the basis of this physical understanding, we demonstrate how electrolyte additives can heal electrode cracks and provide strategies to enhance the fracture resistance in future lithium-ion batteries from surface chemical, electrochemical and material science perspectives.
Original languageEnglish (US)
Issue number1
StatePublished - Jun 14 2016
Externally publishedYes

Bibliographical note

KAUST Repository Item: Exported on 2022-06-01
Acknowledgements: This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Freedom CAR and Vehicle Technologies, US Department of Energy under contract no. DE-AC02 O5CH1123. K.K. also acknowledges the funding provided for this work by the UCB - KAUST Academic Excellence Alliance Program. The potentiostat instrumentation was purchased with funding from the Director, Office of Science, Office of Basic Energy Sciences, Materials Science and Engineering Division, US Department of Energy, which also provided support to R.O.R. We thank C. Shen for assistance in micropillar sample preparation.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

ASJC Scopus subject areas

  • Biochemistry, Genetics and Molecular Biology(all)
  • Chemistry(all)
  • Physics and Astronomy(all)


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