Multiscale Digital-Twin Modeling of Energy-Storage Materials by Integrating First-Principles Calculations and Machine-Learning Interatomic Potentials

Conventional modeling of energy-storage materials is constrained by the computational cost of first-principles calculations, limited electrochemical-state awareness in machine-learning interatomic potentials, and weak coupling between materials-scale models and online battery decision-making. This study proposes a first-principles-constrained electrochemically conditioned machine-learning interatomic potential (FP-EMLP) integrated with a multiscale digital-twin framework (FP-EMLP-DT). A multistate configuration space spanning ion concentration, temperature, defects, strain, and phase boundaries is combined with active learning based on committee uncertainty, structural novelty, and physics-based risk. The equivariant graph model incorporates electrochemical-state gating, charge-conserving projection, and differentiable long-range electrostatics, and is trained using energies, forces, stresses, equilibrium voltages, and migration barriers. Predicted diffusion coefficients, free energies, elastic tensors, and chemical expansion coefficients are transferred to an electrochemical-mechanical-thermal-damage model. The resulting model is further integrated with a physics-based reduced-order network, uncertainty-gated residual learning, online data assimilation, and degradation-aware control. FP-EMLP achieves mean absolute errors of 6.5 meV atom−1, 33 meV Å−1, 0.051 V, and 0.038 eV for energy, force, voltage, and migration barrier, respectively, with a 4.8% aggregate relative error across multiscale fields. Active learning reduces required first-principles labels by 33.3% while covering 91.2% of high-risk configurations. FP-EMLP-DT achieves mean absolute errors of 0.93% for state of charge and 1.21% for state of health. Degradation-aware control reduces maximum material stress and damage increment by 16.5% and 36.8%, respectively, demonstrating an effective multiscale pathway from electronic structure to online battery management.