As taken from experimental observations (e.g. XPS, In Fig. , the realization of the potential-dependent surface coverages in our simulations are displayed. The depicted composition of oxygenated adsorbates is thermodynamically stable and mirrors the corresponding electrochemical environment at the respective electrode potential, without including the potential as an explicit parameter of the simulation. The total coverage of OH * , H 2 O * and O * is around 0.6 ML over the whole potential range. This resembles the coverage as known from traditional water bilayer models, demanding an intensive structural elucidation of the hydrogen bonding present and adsorbate configurations (see results section). For a description of the location of charges and the total amount of K + and F -ions, see the SI.