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Issue 27, 2015
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Mitigating mechanical failure of crystalline silicon electrodes for lithium batteries by morphological design

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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 LixSi 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.

Graphical abstract: Mitigating mechanical failure of crystalline silicon electrodes for lithium batteries by morphological design

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Publication details

The article was received on 09 Mar 2015, accepted on 08 Jun 2015 and first published on 08 Jun 2015


Article type: Paper
DOI: 10.1039/C5CP01385B
Citation: Phys. Chem. Chem. Phys., 2015,17, 17718-17728
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    Mitigating mechanical failure of crystalline silicon electrodes for lithium batteries by morphological design

    Y. An, B. C. Wood, J. Ye, Y. Chiang, Y. M. Wang, M. Tang and H. Jiang, Phys. Chem. Chem. Phys., 2015, 17, 17718
    DOI: 10.1039/C5CP01385B

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