Environmental Catalysis for NO<sub><i>x</i></sub> Reduction by Manipulating the Dynamic Coordination Environment of Active Sites

Nowadays, it is challenging to achieve SO<sub>2</sub>-tolerant environmental catalysis for NO<sub><i>x</i></sub> reduction because of the thermodynamically favorable transformation of reactive sites to inactive sulfate species in the presence of SO<sub>2</sub>. Herein, we achieve enhanced low-temperature SO<sub>2</sub>-tolerant NO<sub><i>x</i></sub> reduction by manipulating the dynamic coordination environment of active sites. Engineered by coordination chemistry, SiO<sub>2</sub>-CeO<sub>2</sub> composite oxides with a short-range ordered Ce-O-Si structure were elaborately constructed on a TiO<sub>2</sub> support. A dynamic coordination environment of active sites is demonstrated from a Ce-O-Si local structure to a low-coordinated Ce-SO<sub>4</sub><sup>2-</sup> species in the presence of SO<sub>2</sub>. The low-coordinated Ce-SO<sub>4</sub><sup>2-</sup> species as new active sites maintain a high NO removal efficiency by preserving the good adsorption and activation capacity of NO and NH<sub>3</sub> reactants. This work proposes a new notion to improve the SO<sub>2</sub> resistance of catalysts by regulating the coordination environment of sulfated active sites, which is of significance for SO<sub>2</sub>-tolerant environmental catalysis in practical applications.

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Publication Details

Journal
Environmental Science & Technology
Published
2025-01-23
DOI
https://doi.org/10.1021/acs.est.4c11440
Citations
13
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
6.73

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article

Environmental Catalysis for NOx Reduction by Manipulating the Dynamic Coordination Environment of Active Sites

Yimin A. Wu, Ming Xie, Hengxiang Zhang, Weiwei Hu et al.
13 citations
Environmental Science & Technology
Catalytic Processes in Materials Science
6.73
article

Environmental Catalysis for NOx Reduction by Manipulating the Dynamic Coordination Environment of Active Sites

Yimin A. Wu, Ming Xie, Hengxiang Zhang, Weiwei Hu, Dengsong Zhang, Min Gao, Yongjie Shen, Jianfu Chen, Xiyang Wang, Lupeng Han, Fuli Wang
article en
13 citations

Abstract

Nowadays, it is challenging to achieve SO<sub>2</sub>-tolerant environmental catalysis for NO<sub><i>x</i></sub> reduction because of the thermodynamically favorable transformation of reactive sites to inactive sulfate species in the presence of SO<sub>2</sub>. Herein, we achieve enhanced low-temperature SO<sub>2</sub>-tolerant NO<sub><i>x</i></sub> reduction by manipulating the dynamic coordination environment of active sites. Engineered by coordination chemistry, SiO<sub>2</sub>-CeO<sub>2</sub> composite oxides with a short-range ordered Ce-O-Si structure were elaborately constructed on a TiO<sub>2</sub> support. A dynamic coordination environment of active sites is demonstrated from a Ce-O-Si local structure to a low-coordinated Ce-SO<sub>4</sub><sup>2-</sup> species in the presence of SO<sub>2</sub>. The low-coordinated Ce-SO<sub>4</sub><sup>2-</sup> species as new active sites maintain a high NO removal efficiency by preserving the good adsorption and activation capacity of NO and NH<sub>3</sub> reactants. This work proposes a new notion to improve the SO<sub>2</sub> resistance of catalysts by regulating the coordination environment of sulfated active sites, which is of significance for SO<sub>2</sub>-tolerant environmental catalysis in practical applications.

Environmental Science & TechnologyVol. 59(4)
Shanghai University (CN), East China University of Science and Technology (CN), University of Waterloo (CA), Hokkaido University (JP), Catalytic Materials (United States) (US), Institute of Nanotechnology (GB), University of Bath (GB)
Canadian Light Source, National Natural Science Foundation of China, Science and Technology Commission of Shanghai Municipality, Shanghai Rising-Star Program, Natural Sciences and Engineering Research Council of Canada, National Key Research and Development Program of China
Life in Land
Openalex Percentile: Top 3%
Catalytic Processes in Materials Science
6.73
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