While our AIMD simulations reproduce experimental ∆φ and U PZC with a reasonable accuracy, we note that, for many surfaces other than the ones considered here, the available experimental data for U PZC is sparse or non-existent. Because of the importance of U PZC in understanding the structure and properties of electrified metal-water interfaces that are central to several technologically important energy conversion schemes, we implore researchers to continue to pursue experimental methods for the accurate estimation of U PZC . In the meantime, the simple scheme presented in this work based on detailed atomistic simulations of metal-water interfaces can help us understand and predict U PZC , ∆φ, and its individual contributions.