In the following, after a brief description of the computational model, we will first describe and discuss our approach for determining the surface energies and formation enthalpies. We will then present results for the different Pt(111)-and Pd(111)-based bimetallic systems, discuss trends and specific differences between Pt(111)-and Pd(111)-based systems, and discuss possible reasons for specific discrepancies. Finally, we will briefly comment on the general validity and applicability of the approach presented here and on possible limitations.