Johnson et al. that the surface charge boundary conditions are often misused in L4 models, leading to incorrect conclusions regarding EDL effects. The inconsistencies arise from the adoption of inaccurate permittivity for the adlayer or the artificial imposition of an electric potential at the RP. In our works, we estimate the key parameters, i.e., 𝜀 ad and 𝛿 ad , based on ab initio molecular dynamics (AIMD) simulations. In addition, to the best of our knowledge, our approach is unique in that it considers the surface dipole moment induced by partially charged chemisorbates, 𝜇 chem . It has been shown that 𝜇 chem markedly modifies the surface charging relation and the LRE. Furthermore, it is worth noting that a more detailed EDL structure that accounts for the first water layer can also be integrated into eq 12. The overall model parameters can be categorized into three groups. The first group of parameters describe reaction properties, including adsorption energies, activation barriers, transfer coefficients and lateral interaction coefficients between adsorbates. These parameters are derived primarily from DFT calculations. The second group characterizes the EDL structure, encompassing the permittivity and thickness of adlayer, effective diameters of solvated ions, and dipole moments of adsorbates. These parameters can be obtained with the aid of DFT and AIMD.