Before starting the QM/MD simulation, graphene structure was optimized at the PBE-DFT level using the Quantum Espresso software suite and Optimized Norm Conserving Vanderbilt pseudopotentials . The optimization resulted in a carbon-carbon bond length of 0.143 nm. The QM/MD simulation was performed using the iterative process developed by Elliott et al. with more details in Figure in the SI, which combines quantum mechanical self-consistent charge (SCC) Density Functional Tight-Binding (DFTB) calculations of the electrode's electronic structure with classical molecular dynamics trajectories of the electrolyte.