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Cycling-induced structural damage/degradation of electrode materials-microscopic viewpoint

机译：Cycling-induced structural damage/degradation of electrode materials-microscopic viewpoint

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Most analyses of the mechanical deformation of electrode materials of lithium-ion battery in the framework of continuum mechanics suggest the occurring of structural damage/degradation during the de-lithiation phase and cannot explain the lithiation-induced damage/degradation in electrode materials, as observed experimentally. In this work, we present first-principle analysis of the interaction between two adjacent silicon atoms from the Stillinger-Weber two-body potential and obtain the critical separation between the two silicon atoms for the rupture of Si-Si bonds. Simple calculation of the engineering-tensile strain for the formation of Li-Si intermetallic compounds from the lithiation of silicon reveals that cracking and cavitation in lithiated silicon can occur due to the formation of Li-Si intermetallic compounds. Assuming the proportionality between the net mass flux across the tip surface of a slit crack and the migration rate of the crack tip, we develop analytical formulas for the growth and healing of the slit crack controlled by lithiation and de-lithiation, respectively. It is the combinational effects of the state of charge, the radius of curvature of the crack tip and local electromotive force that determine the cycling-induced growth and healing of surface cracks in lithiated silicon.

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