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Pressure-sensitive plasticity of lithiated silicon in Li-ion batteries

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Abstract

Lithiation-induced plasticity is a key factor that enables Si electrodes to maintain long cycle life in Li-ion batteries. We study the plasticity of various lithiated silicon phases based on first-principles calculations and identify the linear dependence of the equivalent yield stress on the hydrostatic pressure. Such dependence may cause the compression-tension asymmetry in an amorphous Si thin film electrode from a lithiation to delithiation cycle, and leads to subsequent ratcheting of the electrode after cyclic lithiation. We propose a yield criterion of amorphous lithiated silicon that includes the effects of the hydrostatic stress and the lithiation reaction. We further examine the microscopic mechanism of deformation in lithiated silicon under mechanical load, which is attributed to the flow-defects mediated local bond switching and cavitation. Hydrostatic compression confines the flow defects thus effectively strengthens the amorphous structure, and vice versa.

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Authors and Affiliations

  1. Department of Nuclear Science and Engineering and Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts, 02139, USA

    Ke-Jie Zhao & Yong-Gang Li

  2. Key Laboratory for Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, 230031, Hefei, China

    Yong-Gang Li

  3. Institute of Mechanics, Materials and Civil Engineering, Université catholique de Louvain, Louvain-la-Neuve, 1348, Belgium

    Laurence Brassart

Authors
  1. Ke-Jie Zhao
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  2. Yong-Gang Li
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  3. Laurence Brassart
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Correspondence to Ke-Jie Zhao.

Additional information

The project was supported by the National Natural Science Foundation of China (11005124 and 11275229), the Natural Science Foundation of Anhui Province (1208085QA05), and the National Fund for Scientific Research (FNRS) of Belgium.

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Zhao, KJ., Li, YG. & Brassart, L. Pressure-sensitive plasticity of lithiated silicon in Li-ion batteries. Acta Mech Sin 29, 379–387 (2013). https://doi.org/10.1007/s10409-013-0041-2

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  • DOI: https://doi.org/10.1007/s10409-013-0041-2

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