Decoding electrochemical processes of lithium-ion batteries by classical molecular dynamics simulations

we provide an extensive review, focusing on the application of MD simulations to decode the electrochemical processes in LIBs. To our knowledge, this is the first article to provide an exhaustive review of the electrochemical processes within electrodes, electrolytes, and electrode-electrolyte interfaces LIBs, exclusively from the perspective of pure MD simulations. Advancing further, this article elucidates the state-of-the-art advancements in MD simulation applications for a diverse range of electrochemical processes across different LIB components. Building on this foundation, our review then delves into the following three critical dimensions:

1) Reviewing the recent developments in non-reactive force fields, reactive force fields, and machine learning potential for modeling electrochemistry in LIBs, we comprehensively summarized the advantages and limitations of these different approaches.

2) Discussing the molecular and atomic scale insights into electrochemical processes in different LIB components, including fundamental physical or chemical properties, lithium insertion and removal dynamics of electrodes, solvation structures and transport physics of electrolytes, as well as the electrochemistry at the electrochemical interfaces including the electric double layer, solid-electrolyte interphases, and lithium dendrite.

3) Commenting on the remaining challenges and providing an outlook for future routes, including improving the accessibility of reactive force fields and machine learning potentials, developing methods of describing long-range interatomic coupling, and realistic modeling charging/discharging electrochemistry of LIBs under constant potential or currents.

In summary, this article distinguishes from previous reviews on theoretical methodologies by performing customized and concentrated discussions in computational approaches focusing on LIBs and providing atomic-scale insights into the electrochemistry of different components of LIBs. We believe this review article would not only serve as an important tutorial to prepare researchers interested in studying LIBs using MD but also provide an in-depth outlook of future directions for pushing forward the computational techniques that are important for developing next-generation LIBs with superb energy density, charging speed, stability, cycling life and safety.

Download paper here.