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Stress-affected two-phase lithiation reactions in spherical elasto-viscoplastic Si particles for Li-ion batteries are studied here to determine the effects of a hyperelastic polymer coating on particle stresses, reaction front velocity, and degree of lithiation. The problem is modelled using finite-strain chemo-mechanical equations that couple stress, with Li-ion diffusion and reaction front velocity, and are solved using the finite-element (FE) approach, taking advantage of spherical symmetry of the problem. FE simulations and the sensitivity analysis reveal: (1) coating thickness is the most influential design parameter that affects the velocity of the reaction front, and (2) increasing values of the coating shear and bulk moduli, and the coating thickness reduce tensile circumferential stresses at the edge of the particle. The latter minimises the risk of particle cracking in the opening mode, but it can also accelerate the arrest of the reaction front, and thus reduce the particle lithiation degree in Li-ion battery anodes.

coatings

Stress-Affected Lithiation Reactions in Elasto-Viscoplastic Si Particles with Hyperelastic Polymer Coatings: A Nonlinear Chemo-Mechanical Finite-Element Study