Abstract

Although crystalline silicon (c-Si) anodes promise very high energy densities in Li-ion batteries, their practical use is complicated by amorphization, large volume expansion and severe plastic deformation upon lithium insertion. Recent experiments have revealed the existence of a sharp interface between crystalline Si (c-Si) and the amorphous Li<inf>x</inf>Si alloy during lithiation, which propagates with a velocity that is orientation dependent; the resulting anisotropic swelling generates substantial strain concentrations that initiate cracks even in nanostructured Si. Here we describe a novel strategy to mitigate lithiation-induced fracture by using pristine c-Si structures with engineered anisometric morphologies that are deliberately designed to counteract the anisotropy in the crystalline/amorphous interface velocity. This produces a much more uniform volume expansion, significantly reducing strain concentration. Based on a new, validated methodology that improves previous models of anisotropic swelling of c-Si, we propose optimal morphological designs for c-Si pillars and particles. The advantages of the new morphologies are clearly demonstrated by mesoscale simulations and verified by experiments on engineered c-Si micropillars. The results of this study illustrate that morphological design is effective in improving the fracture resistance of micron-sized Si electrodes, which will facilitate their practical application in next-generation Li-ion batteries. The model and design approach present in this paper also have general implications for the study and mitigation of mechanical failure of electrode materials that undergo large anisotropic volume change upon ion insertion and extraction.

Original languageEnglish (US)
Pages (from-to)17718-17728
Number of pages11
JournalPhysical Chemistry Chemical Physics
Volume17
Issue number27
DOIs
StatePublished - Jul 21 2015

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Lithium batteries
lithium batteries
Silicon
Crystalline materials
Electrodes
electrodes
silicon
swelling
electric batteries
insertion
Swelling
ions
expansion
electrode materials
fracture strength
plastic deformation
Amorphization
anodes
cracks
flux density

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Physics and Astronomy(all)

Cite this

Mitigating mechanical failure of crystalline silicon electrodes for lithium batteries by morphological design. / An, Yonghao; Wood, Brandon C.; Ye, Jianchao; Chiang, Yet Ming; Wang, Y. Morris; Tang, Ming; Jiang, Hanqing.

In: Physical Chemistry Chemical Physics, Vol. 17, No. 27, 21.07.2015, p. 17718-17728.

Research output: Contribution to journalArticle

An, Yonghao ; Wood, Brandon C. ; Ye, Jianchao ; Chiang, Yet Ming ; Wang, Y. Morris ; Tang, Ming ; Jiang, Hanqing. / Mitigating mechanical failure of crystalline silicon electrodes for lithium batteries by morphological design. In: Physical Chemistry Chemical Physics. 2015 ; Vol. 17, No. 27. pp. 17718-17728.
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