As an ideal anode material, silicon has the highest lithium-ion capacity in theory, but the broader application is limited by the huge volumetric strain caused by lithium insertion and extraction. To better understand the physical process and to resolve the related reliability issue, enormous efforts have been made. Recent experiments observed sharp reaction fronts in both crystalline and amorphous silicon during the first lithiation half-cycle. Such a concentration profile indicates that the process is likely to be reaction limited. Based on this postulation, a phase-field model is developed and implemented into a finite-element code to simulate the coupled large inelastic deformation and motion of the reaction front in a silicon electrode. In contrast to most existing models, the model treats both volumetric and deviatoric inelastic deformation in silicon as a direct consequence of the lithiation at the reaction front. The amount of deviatoric deformation is determined by using the recently developed kinetic model of stress-induced anisotropic reaction. By considering the role of stress in the lithiation process, this model successfully recovers the self-limiting phenomenon of silicon electrodes, and relates it to the local geometry of electrodes. The model is also used to evaluate the energy-release rate of the surface crack on a spherical electrode, and the result suggests a critical size of silicon nanoparticles to avert fracture. As examples, the morphology evolution of a silicon disk and a Si nanowire during lithiation are also investigated.
Journal of the Mechanics and Physics of Solids – Elsevier
Published: Sep 1, 2016
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