Our initial Pt4Ge structure geometries were obtained using our in-house code PGOPT , which uses a bond-length distribution (BLDA) algorithm in order to generate structure that are faster to optimize and less likely to result in errors during optimization. Once ~200 Pt4Ge structures had been generated, we took the thermally accessible structures within a cutoff of 0.4 eV, and generated a number of rough binding modes of C2H6, C2H4, and C2H2 using PGOPT, which we later refined with VASP local optimizations to obtain the final binding modes. The final ensemble of thermally-accessible catalyst states was computed for the initial cluster structures, and re-computed for every intermediate on the reaction profile, by weighting the optimized structures by the Boltzmann probability to be occupied at 700 K, based on DFT electronic energies. The Pt4GeC2 structures were generated from the thermally accessible acetylene binding modes to Pt4Ge by removing the hydrogens then optimizing the resulting structures with DFT.