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Single-atom catalysts (SACs) have recently attracted broad attention in the catalysis field due to their maximized atom efficiency and unique catalytic properties. An atomic-level understanding of the interaction between the metal atoms and support is vital for developing stable and high-performance SACs. In this work, Pt1 single atoms with loadings up to 4 wt.% were fabricated on ceria nanorods using the atomic layer deposition technique. To understand the Pt–O–Ce bond interfacial interactions, the stability of Pt1 single atoms in the hydrogen reducing environment was extensively investigated by using in situ diffuse reflectance infrared Fourier transform spectroscopy CO chemisorption measurements. It was found that ceria defect sites, metal loadings and high-temperature calcination are effective ways to tune the stability of Pt1 single atoms in the hydrogen environment. X-ray photoemission spectroscopy further showed that Pt1 single atoms on ceria are dominantly at a +2 valence state at the defect and step edge sites, while those on terrace sites are at a +4 state. The above tailored stability and electronic properties of Pt1 single atoms are found to be strongly correlated with the catalytic activity in the dry and water-mediated CO oxidation reactions.
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