Understanding oxygen transfer on ceria with Pt single atoms for surface reaction.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41513644.
- Also identified by DOI 10.1038/s41467-025-66242-5 and PMC identifier 12789587.
- Licence recorded as CC BY-NC-ND.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
Reducible metal oxides are widely used in surface reactions, primarily due to their ability to activate and transfer oxygen. Ceria, known for its rapid Ce<sup>3+</sup>/Ce<sup>4+</sup> redox property, is well-known to follow Mars van Krevelen mechanism. In this study, we prepare Pt/CeO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub> catalysts with different ceria domain sizes of 3.7, 5.6, and 7.3 nm to understand oxygen transfer, mainly O<sub>2</sub> activation and lattice oxygen transfer. The ceria domains are isolated on the alumina, preventing oxygen transfer between the ceria. Pt single atomic structures are meticulously prepared to exclude O<sub>2</sub> activation on Pt nanoparticles and provide uniform active sites. Interestingly, the activity trend for CO oxidation is reversed in O<sub>2</sub>-rich and O<sub>2</sub>-deficient conditions. O<sub>2</sub> activation occurs efficiently in small ceria domains of 3.7 nm. In contrast, larger ceria domains exhibit less O<sub>2</sub> activation but significant lattice oxygen transfer. This behavior is also modeled using large-scale molecular dynamics simulations with a neural network potential trained on first-principles data. Based on these understanding, the catalyst for methane oxidation is proposed by accelerating O<sub>2</sub> activation in O<sub>2</sub>-rich condition. This work provides an impactful platform for understanding metal oxide catalysts.