The parameterized properties for atop-NN and fcc-NN are provided in SI. Equilibrium simulations were conducted with the coverage-dependent thermodynamic properties. Adsorption isotherms for CO adsorption on Pt(111) at three different temperatures are shown in Figure . Additional transient simulations for the CO oxidation in a batch reactor are provided in the SI. For all the tested temperatures, especially for higher temperatures, the coverage-dependent models resulted in noticeably different isotherms from the ideal-adsorbate model (i.e. no coverage effect model). Among them, we considered the interpolative model isotherm as the most accurate standard-at a minimum they are exact at the nine discrete coverages. The linear model isotherm is furthest away from the interpolative model isotherm. This discrepancy is due to the oversimplification of the coverage dependence as shown by a conspicuous over/under predicting in Figure . The piecewise linear and polynomial model isotherms simulate the interpolative isotherm much more closely. However, jagged features in piecewise linear and interpolative models (Figure ) propagated to their isotherms at 1200 K. The jagged features become apparent at 1200 K because the coverage changes from 0 to 0.5, whereas it remains relatively constant for the lower temperatures. Due to the relatively constant coverage at low temperatures, the coverage-dependence polynomial is in the linear part of the interpolative model resulting to the absence of kinks. Although our piecewise linear isotherm is subtly kinked, the piecewise linear model was reported by Bajpai et al. to render discontinuous predictions. Therefore, the polynomial model is recommended based on its good balance between accuracy and smooth, continuous profile.