Developing Single-Site Pt Catalysts For The Preferential Oxidation Of Co: A Surface Science And First Principles-Guided Approach

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 H-2 over single-site Pt-1/CuxO catalysts. Surface science studies show that while PU/CuxO model surfaces enable low-temperature CO oxidation via a Mars-van Krevelen mechanism, there was no evidence for H-2 activation or oxidation. DFT-based calculations explain these results and demonstrate that the H-2 oxidation barrier is high as compared to H-2 desorption from PU/CuxO. Inspired by these model catalyst studies, nanoporous Pt-1/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 Pt-1/CuxO catalyst for the preferential oxidation of CO.