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 sili-con phases based on first-principles calculat...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 sili-con phases based on first-principles calculations and iden-tify 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 lithi-ated silicon that includes the effects of the hydrostatic stress and the lithiation reaction. We further examine the micro-scopic 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 strength-ens the amorphous structure, and vice versa.展开更多
基金supported by the National Natural Science Foundation of China (11005124 and 11275229)the Natural Science Foundation of Anhui Province (1208085QA05)+1 种基金the National Fund for Scientific Research (FNRS) of Belgium, support by the SEAS Academic Computing teamthe Extreme Science and Engineering Discovery Environment (XSEDE),supported by NSF of US (TG-DMR130025 andTG-DMR130038)
文摘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 sili-con phases based on first-principles calculations and iden-tify 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 lithi-ated silicon that includes the effects of the hydrostatic stress and the lithiation reaction. We further examine the micro-scopic 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 strength-ens the amorphous structure, and vice versa.
