the ability to draw a direct connection to measurable experimental variables. The remaining model parameters are then either taken from the literature or approximated to fit experiment (SI, Sec. S1.4). Values for the activation free energies in particular, as well the potentialdependent ∆G ‡ rdx (U ) functional form, are unfortunately mostly unavailable and are thus fitted to reproduce measured selectivity curves. It is important to stress, however, that the effect of ρ in these situations is always simulated by consistently re-using the same set of parameters within each reaction model studied. This allows for an unbiased comparison of the results when specifically focusing on the response to varying catalyst morphology.