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.

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Journal
Environmental Science & Technology
Published
2025-11-12
DOI
https://doi.org/10.1021/acs.est.5c11651
Primary Topic
Catalytic Processes in Materials Science
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article
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article

Single-Atom Ru on CeO 2 Nanorods for Efficient N 2 O Decomposition: Mechanistic Insights and Multipollutant Control

Zhongbiao Wu, Yunshuo Wu, Yuxin Sun, Haiqiang Wang
Environmental Science & Technology
Catalytic Processes in Materials Science
article

Single-Atom Ru on CeO 2 Nanorods for Efficient N 2 O Decomposition: Mechanistic Insights and Multipollutant Control

Zhongbiao Wu, Yunshuo Wu, Yuxin Sun, Haiqiang Wang
article en

Abstract

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.

Environmental Science & TechnologyVol. 59(46)
Environmental and Water Resources Engineering (IL), Zhejiang Environmental Monitoring Center (CN), Zhejiang University of Technology (CN), Zhejiang University (CN)
Openalex Percentile: Top 73%
Catalytic Processes in Materials Science
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