Electrochemistry is fundamental to the development of new technologies in various research areas, such as energy conversion and storage, 1 corrosion, 2,3 sensors. Central to these technologies is the knowledge from electrocatalysis, where reactions at the electrode-electrolyte interface are controlled by applied voltages. This interface, called the electrochemical double layer (EDL), forms when the metal electrode and electrolyte solution carry charges of equal magnitude but opposite sign. Understanding the atomic-level processes within the EDL is critical to optimize device efficiency and durability. Thus, computational electrochemistry addresses two challenges: (a) understanding the interfacial processes at the atomistic level, and (b) investigating how atoms move and react when a certain potential is applied. Those questions are hard to answer, because atoms at interfaces behave differently than in bulk and models that take into account electric field effects are not well developed. Moreover, bridging results of experiments and simulations is not straightforward. Experiments often use different thermodynamic variables than the ones accessible in simulations. Directly calculating activation energies is difficult due to the complexity of the systems and reactions in the experimental condition. System sizes and timescales generally differ significantly between experiments and simulations. In first-principles molecular dynamics, simulations are typically conducted at scales of a few angstroms and over picoseconds. It is not possible to incorporate those complexities into the model systems studied in simulations.