Computation-Guided Development of Platinum Alloy Catalyst for Carbon Monoxide Preferential Oxidation

Carbon monoxide preferential oxidation (PROX) in an H 2 -rich stream represents one promising H 2 purification technology but requires the development of active and selective catalysts to make the technology viable. We conducted density functional theory simulations of CO PROX catalysis on model Pt alloy systems to establish correlations between the catalyst parameters and the catalytic properties, which validated E A,COOR and E A,HOR as descriptors for CO oxidation and H 2 oxidation kinetics, Δ E A as a descriptor for CO PROX selectivity, and ε d as a catalyst parameter descriptor for the activation energy barriers. We discovered an interesting compromising relationship between the CO PROX activity and selectivity properties. Pt-Ni and Pt-Mn nanoparticle catalysts were selected for synthesis on the basis of the computational data and tested for their properties, which matched well with the DFT calculations and verified the effectiveness of the computational findings. The use of computation-guided methods and the discovered catalyst parameter–property relationships would establish a rational strategy to aid catalyst development and foster CO PROX research.