Microscale diffusion-mechanics model for a polymer-based solid-state battery cathode

[Display omitted] •Diffusion-mechanics model captures in-situ behaviour of a polymer-based cathode.•Cathode microstructure resolved with an axisymmetric unit cell.•Numerical solution with a non-linear finite element approach.•Plastic deformation of the polymer affects the interfacial opening displacement.•Slower charging rates lead to a smaller interfacial opening. A non-linear microscale diffusion-mechanics model combining mass transport and linear momentum balance equations, with elasto-viscoplastic polymer constitutive law and interfacial traction-separation law is proposed to provide a new insight into the effects of viscoplasticity and interfacial damage on the in situ diffusive-mechanical behaviour of a polymer-based cathode for a solid-state battery (SSB). Diffusion and mechanics are coupled through two mechanisms: (1) active particle (AP) volumetric change dependence on Li concentration, and (2) interfacial flux dependence on mechanical opening. The model is resolved for a simple cathode microstructure using an axisymmetric unit cell concept, and integrated with the non-linear finite-element solver ABAQUS with the help of its user subroutines (UMAT and UINTER). Finite-element simulations reveal that plastic deformations of the polymer due to volumetric changes of the AP reduce the value of the interfacial opening displacement, which is desirable for maintaining interfacial flux. The results also demonstrate that slower battery charging rates may lead to a softer polymer response, and thus a smaller interfacial gap. Moreover, a comparison between the linear elastic and current elasto-viscoplastic models for the polymer electrolyte shows that even 5% volumetric shrinkage of the AP leads to an overprediction of the interfacial opening with the linear elastic material law, which limits its validity in modelling polymer-based SSBs.