2. Computational studies of the charging mechanisms. While porous carbons have complex amorphous structures which are challenging to model, the crystalline structure of MOFs enables molecular simulations that can much more accurately represent the experimental systems. MD simulations are an effective tool to study a variety of properties of MOF supercapacitors, including ion transport and electrochemical performance. It is crucial to describe the electrode-electrolyte interface from firstprinciples, e.g. with DFT, to describe any electron transfer processes, a key factor in pseudo-capacitance, as well as to describe the heterogeneous electron density on the electrode from EDLC contributions. However, it is currently intractable to describe all components of a supercapacitor from first-principles for MD simulation. Our recently developed QM/MM method is thus ideal for investigating MOF-based systems, and machine learning force fields may also contribute to investigating the interface in the future based on their recent rapid development. Those methods may not only help to understand the in-pore electric double layer structure but can also describe chemical reactions at the interface. However, it is still challenging to find a proper method that can capture both the kinetic and thermodynamic phenomena at the same time, due to the high computational cost. Therefore, employing classical MD simulation is still important to understand the kinetics of MOF supercapacitors, and advanced charge equilibration methods are needed.