期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 38, 页码 15635-15643出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c04590
关键词
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资金
- NSFC [21972117, 21925404, 21775127, 21991151, 22122205, 22021001]
- National Key Research and Development Program of China [2019YFA0705400, 2020YFB1505800]
- Fundamental Research Funds for the Central Universities [20720190044]
- 111 Project [B17027]
- Natural Science Foundation of Fujian Province [2019J01030]
- State Key Laboratory of Fine Chemicals [KF2002]
The study investigates the activation and reaction of active oxygen species during CO oxidation at platinum-ceria interfaces using surface-enhanced Raman spectroscopy, revealing the evolution of different oxygen species and reaction pathways. Oxygen efficiently dissociates into chemisorbed O on Pt and lattice Ce-O species simultaneously at interfacial Ce3+ defect sites under CO oxidation, leading to a much higher activity at platinum-ceria interfaces compared to that at Pt alone.
Understanding the fundamental insights of oxygen activation and reaction at metal-oxide interfaces is of significant importance yet remains a major challenge due to the difficulty in in situ characterization of active oxygen species. Herein, the activation and reaction of molecular oxygen during CO oxidation at platinum-ceria interfaces has been in situ explored using surface-enhanced Raman spectroscopy (SERS) via a borrowing strategy, and different active oxygen species and their evolution during CO oxidation at platinum- ceria interfaces have been directly observed. In situ Raman spectroscopic evidence with isotopic exchange experiments demonstrate that oxygen is efficiently dissociated to chemisorbed O on Pt and lattice Ce-O species simultaneously at interfacial Ce3+ defect sites under CO oxidation, leading to a much higher activity at platinum-ceria interfaces compared to that at Pt alone. Further in situ time-resolved SERS studies and density functional theory simulations reveal a more efficient molecular pathway through the reaction between adsorbed CO and chemisorbed Pt-O species transferred from the interfaces. This work deepens the fundamental understandings on oxygen activation and CO oxidation at metal-oxide interfaces and offers a sensitive technique for the in situ characterization of oxygen species under working conditions.
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