Single-Atom Ru on CeO <sub>2</sub> Nanorods for Efficient N <sub>2</sub> O Decomposition: Mechanistic Insights and Multipollutant Control
Nitrous oxide (N<sub>2</sub>O) has gained increasing attention as a potent greenhouse gas, and its catalytic decomposition offers a promising mitigation strategy. In this study, single-atom Ru embedded in a rod-shaped CeO<sub>2</sub> catalyst was synthesized via a H<sub>2</sub>O<sub>2</sub> chemical etching strategy. The single-atom Ru catalyst demonstrated an exceptional N<sub>2</sub>O decomposition performance with only 0.48 wt % Ru loading, exhibiting a 34-fold increase in the turnover frequency compared to Ru nanoparticle catalysts. Under simulated exhaust conditions (NO, CO, and N<sub>2</sub>O), Ru<sub>1</sub>/CeO<sub>2</sub> enabled complete conversion of all three pollutants at 280 °C. Mechanistic studies revealed that N<sub>2</sub>O decomposition over Ru<sub>1</sub>/CeO<sub>2</sub> and Ru<sub><i>n</i></sub>/CeO<sub>2</sub> followed the Mars-van Krevelen (MvK) and Langmuir-Hinshelwood (L-H) mechanisms, respectively. The exceptional N<sub>2</sub>O decomposition activity of the single-atom catalyst stems from enhanced O<sub>2</sub> desorption through the recombination of oxygen atoms that dissociate from N<sub>2</sub>O with adjacent lattice oxygen. Notably, Ru<sub>1</sub>/CeO<sub>2</sub> exhibits remarkable O<sub>2</sub> tolerance due to the selective adsorption: N<sub>2</sub>O binds to single Ru atoms, whereas O<sub>2</sub> occupies oxygen vacancies. In contrast, the high energy barrier associated with O<sub>2</sub> combination and desorption in Ru<sub><i>n</i></sub>/CeO<sub>2</sub> hindered N<sub>2</sub>O decomposition, and the competitive adsorption of O<sub>2</sub> on its surface led to poor O<sub>2</sub> resistance. This study demonstrates Ru<sub>1</sub>/CeO<sub>2</sub> as an efficient catalyst for abating N<sub>2</sub>O and multipollutant removal.
Authors
- Zhongbiao Wu (ORCID: https://orcid.org/0000-0003-0182-5971)
- Yunshuo Wu (ORCID: https://orcid.org/0000-0002-7751-7097)
- Yuxin Sun
- Haiqiang Wang (ORCID: https://orcid.org/0000-0001-8298-993X)
Institutions
- Environmental and Water Resources Engineering (IL)
- Zhejiang Environmental Monitoring Center (CN)
- Zhejiang University of Technology (CN)
- Zhejiang University (CN)
Publication Details
- Journal
- Environmental Science & Technology
- Published
- 2025-11-12
- DOI
- https://doi.org/10.1021/acs.est.5c11651
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 0.00