Nanoscale modelling of polymer electrolytes for rechargeable batteries

Rechargeable solid-state batteries (SSBs) are of prime importance for developing the necessary safe and efficient energy infrastructures of the future. With several inherent advantages such as cost-effectiveness, superior flexibility, and good processability, polymer electrolytes (PEs) have emerged as one of the most promising solid-state electrolytes for building high-performance rechargeable SSBs. In this quest, the combined drastic growth of materials chemistry and computational science in recent years has made computer simulation of PE components (e.g., salt, polymers, and plasticizers) and their mixtures an essential approach to understand and quickly screen suitable electrolyte materials for SSBs. In this review, the theoretical background of prominent simulation methods at the nanoscale level is briefly discussed in terms of their general capabilities, accuracies, and computational cost. By considering a literature selection of key studies on the nanoscale modelling of PEs over the last years, special focus is paid to review the advances that have yielded comprehensive fundamental understanding of individual electrolyte components at the molecular level. Furthermore, the limitations and cautions as well as future directions on the nanoscale modelling of PEs are summarized.