By combining density functional theory (DFT) calculation, thermodynamics consideration, and finite element simulation, impact of doping and substitution on electrochemo-mechanical properties of Li-based cathodes is studied. It is shown that calculation of magnetic moment using DFT with hybrid exchange-correlation functionals can help us to understand the redox mechanism of active materials. Application of this approach to layered oxide materials is presented. Besides oxidation state of ions, cation migration,
second phase formation, and lattice parameters change with charge/discharge are predicted. In addition, it is shown that how a multiscale-modeling approach can be used to model microstructures and simulate microcracking of layered oxide materials over
cycling.