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Catalytic NO Reduction by NO Pre-Adsorbed RhCeO2 NO- Clusters
Jiao-Jiao Chen1,2, Qing-Yu Liu1,2, Si-Dun Wang1,3,4
1State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
Nitric oxide (NO) adsorption on rhodium-cerium oxide clusters creates a Ce3+ ion, initiating the catalytic reduction of NO by CO. This Ce3+ ion is key for NO reduction, with rhodium acting as an electron buffer.
Area of Science:
- Surface Science
- Catalysis
- Materials Chemistry
Background:
- Understanding dynamic catalyst structural evolution under reaction conditions is crucial for catalyst design.
- Rhodium-cerium oxide (Rh/CeO2) is a key component in three-way catalysts for nitrogen oxide (NOx) removal.
Purpose of the Study:
- To elucidate the mechanism of nitric oxide (NO) reduction by carbon monoxide (CO) over rhodium-cerium bimetallic oxide clusters.
- To identify the role of NO in regulating the catalytic behavior of rhodium under reaction conditions.
Main Methods:
- Utilized mass spectrometry for cluster reactions.
- Employed cryogenic photoelectron imaging spectroscopy.
- Performed quantum-chemical calculations.
Main Results:
- Identified that NO adsorption on RhCeO2- generates a Ce3+ ion in RhCeO2NO-.
- Demonstrated that the Ce3+ ion is the active site for the reduction of subsequent NO molecules to N2O.
- Showed that rhodium acts as a promoter, buffering electrons and cooperating with Ce3+.
Conclusions:
- NO adsorption dynamically alters the rhodium-cerium oxide catalyst structure, creating active Ce3+ sites.
- The Ce3+ ion is essential for triggering and facilitating NO reduction by CO.
- Provides fundamental insights into NO reduction mechanisms over Rh/CeO2 catalysts.
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