The gap between first-principles and classical simulation is slowly closing due to the development of hybrid approaches, such as QM/MM, 86,88,89 and generalized Langevin equation approaches. In addition, machine learning interatomic potentials (MLIPs) are improving the accuracy and efficiency of molecular simulations. 91-95 However, MLIPs for interfacial systems are still in development and traditional ab initio and classical force field simulations remain a valuable tool in investigating the EDL.