Surface oxygenation of multicomponent nanoparticles toward active and stable oxidation catalysts

• Published in: Nature communications Vol. 11; no. 1; p. 4201
• Main Authors: Shan, Shiyao, Li, Jing, Maswadeh, Yazan, O’Brien, Casey, Kareem, Haval, Tran, Dat T., Lee, Ivan C., Wu, Zhi-Peng, Wang, Shan, Yan, Shan, Cronk, Hannah, Mott, Derrick, Yang, Lefu, Luo, Jin, Petkov, Valeri, Zhong, Chuan-Jian
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 21.08.2020; Nature Publishing Group; Nature Portfolio
• Subjects: 140/58; 639/638/77; 639/925/357; Aging; Alloy plating; Alloying; Catalysis; Catalysts; Cobalt; Fourier transforms; Humanities and Social Sciences; Hydrocarbons; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Intermediates; Kinetics; multidisciplinary; Nanoalloys; Nanoparticles; Nanoscale materials; Nickel; Oxidation; Oxygen; Oxygenation; Platinum; Pollutants; Reaction kinetics; Science; Science (multidisciplinary); Surface layers; Sustainability; Synchrotron radiation; Ternary alloys; X-ray diffraction
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-020-18017-3

The need for active and stable oxidation catalysts is driven by the demands in production of valuable chemicals, remediation of hydrocarbon pollutants and energy sustainability. Traditional approaches focus on oxygen-activating oxides as support which provides the oxygen activation at the catalyst-support peripheral interface. Here we report a new approach to oxidation catalysts for total oxidation of hydrocarbons (e.g., propane) by surface oxygenation of platinum (Pt)-alloyed multicomponent nanoparticles (e.g., platinum-nickel cobalt (Pt–NiCo)). The in-situ/operando time-resolved studies, including high-energy synchrotron X-ray diffraction and diffuse reflectance infrared Fourier transform spectroscopy, demonstrate the formation of oxygenated Pt–NiOCoO surface layer and disordered ternary alloy core. The results reveal largely-irregular oscillatory kinetics associated with the dynamic lattice expansion/shrinking, ordering/disordering, and formation of surface-oxygenated sites and intermediates. The catalytic synergy is responsible for reduction of the oxidation temperature by ~100 °C and the high stability under 800 °C hydrothermal aging in comparison with Pt, and may represent a paradigm shift in the design of self-supported catalysts. Traditional approach to oxidation catalysts relies on metal/oxide supported peripheral interfacial oxygen activity. Here the authors show surface oxygenation of platinum-alloyed multicomponent nanoparticles, and reveals irregular oscillatory kinetics associated with the surface oxygenated sites.