Fine-Tuning of Pt Dispersion on Al₂O₃ and Understanding the Nature of Active Pt Sites for Efficient CO and NH₃ Oxidation Reactions

Fine-tuning the dispersion of active metal species on widely used supports is a research hotspot in the catalysis community, which is vital for achieving a balance between the atomic utilization efficiency and the intrinsic activity of active sites. In this work, using bayerite Al(OH)(3) as support directly or after precalcination at 200 or 550 degrees C, Pt/Al2O3 catalysts with distinct Pt dispersions from single atoms to clusters (ca. 2 nm) were prepared and evaluated for CO and NH3 removal. Richer surface hydroxyl groups on AlOx(OH)(y) support were proved to better facilitate the dispersion of Pt. However, Pt/Al2O3 with relatively lower Pt dispersion could exhibit better activity in CO/NH3 oxidation reactions. Further reaction mechanism study revealed that the Pt sites on Pt/Al2O3 with lower Pt dispersion could be activated to Pt-0 species much easier under the CO oxidation condition, on which a higher CO adsorption capacity and more efficient O-2 activation were achieved simultaneously. Compared to Pt single atoms, PtOx clusters could also better activate NH3 into -NH2 and -HNO species. The higher CO adsorption capacity and the more efficient NH3/O-2 activation ability on Pt/Al2O3 with relatively lower Pt dispersion well explained its higher CO/NH3 oxidation activity. This study emphasizes the importance of avoiding a singular pursuit of single-atom catalyst synthesis and instead focusing on achieving the most effective Pt species on Al2O3 support for targeted reactions. This approach avoids unnecessary limitations and enables a more practical and efficient strategy for Pt catalyst fabrication in emission control applications.