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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.
"Acta Mechanica Sinica" – Springer Journals
Published: Jun 1, 2013
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