Decoding Electrochemical Processes of Lithium-Ion Batteries by Classical Molecular Dynamics Simulations

Lithium-ion batteries (LIBs) have played an essential role in the energy storage industry and dominated the power sources for consumer electronics and electric vehicles. Understanding the electrochemistry of LIBs at the molecular scale is significant for improving their performance, stability, lifetime, and safety. Classical molecular dynamics (MD) simulations could directly capture the atomic and molecular motions and thus provide dynamic insights into the electrochemical processes and ion transport in LIBs during charging and discharging that are usually challenging to observe experimentally, which is momentous in developing LIBs with superb performance. This review discusses developments in MD approaches using non-reactive force fields, reactive force fields, and machine learning potential for modeling chemical reactions and transport of reactants in the electrodes, electrolytes, and electrode-electrolyte interfaces. It also comprehensively discusses how molecular interactions, structures, transport, and reaction processes affect electrode stability, energy capacity, and interfacial properties. Finally, the remaining challenges and envisioned future routes are commented on for high-fidelity, effective simulation methods to decode the invisible interactions and chemical reactions in LIBs. This review summarizes the latest advancements in molecular simulations for modeling electrochemical processes in lithium-ion batteries, highlights the current challenges, and offers insights into future directions. These insights are crucial for promoting the computational techniques essential to developing next-generation lithium-ion batteries with superb energy density, charging speed, stability, cycling life, and safety. image