Developing single-site Pt catalysts for the preferential oxidation of CO: A surface science and first principles-guided approach

Abstract We report a comprehensive study combining surface science, Density Functional Theory (DFT) calculations, and catalyst synthesis, characterization, and testing to investigate the preferential oxidation of CO in the presence of H2 over single-site Pt1/CuxO catalysts. Surface science studies show that while Pt1/CuxO model surfaces enable low-temperature CO oxidation via a Mars-van Krevelen mechanism, there was no evidence for H2 activation or oxidation. DFT-based calculations explain these results and demonstrate that the H2 oxidation barrier is high as compared to H2 desorption from Pt1/CuxO. Inspired by these model catalyst studies, nanoporous Pt1/CuxO catalysts were synthesized and demonstrated to be active and highly selective for the preferential oxidation of CO. This work highlights the potential of combined surface science, theory, and catalyst studies for identifying new catalytic materials, which in this case led to the development of a promising single-site Pt1/CuxO catalyst for the preferential oxidation of CO.