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

Lupeng Han; Xiyang Wang; Fuli Wang; Yongjie Shen; Hengxiang Zhang; Weiwei Hu; Min Gao; Yimin A. Wu; Ming Xie; Jianfu Chen; Dengsong Zhang

doi:10.1021/acs.est.4c11440

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

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

Research output: Contribution to journal › Article › peer-review

2 Citations (SciVal)

Abstract

Nowadays, it is challenging to achieve SO₂-tolerant environmental catalysis for NO_x reduction because of the thermodynamically favorable transformation of reactive sites to inactive sulfate species in the presence of SO₂. Herein, we achieve enhanced low-temperature SO₂-tolerant NO_x reduction by manipulating the dynamic coordination environment of active sites. Engineered by coordination chemistry, SiO₂-CeO₂ composite oxides with a short-range ordered Ce-O-Si structure were elaborately constructed on a TiO₂ support. A dynamic coordination environment of active sites is demonstrated from a Ce-O-Si local structure to a low-coordinated Ce-SO₄^2- species in the presence of SO₂. The low-coordinated Ce-SO₄^2- species as new active sites maintain a high NO removal efficiency by preserving the good adsorption and activation capacity of NO and NH₃ reactants. This work proposes a new notion to improve the SO₂ resistance of catalysts by regulating the coordination environment of sulfated active sites, which is of significance for SO₂-tolerant environmental catalysis in practical applications.

Original language	English
Journal	Environmental Science and Technology
Early online date	23 Jan 2025
DOIs	https://doi.org/10.1021/acs.est.4c11440
Publication status	Published - 4 Feb 2025

Funding

The authors from Shanghai University gratefully acknowledge financial support from the National Key R&D Program of China (2021YFB3500600), National Natural Science Foundation of China (22125604, 22436003, and 22106100), and the Science and Technology Commission of Shanghai Municipality (23230713700, 24230711600, and 22QA1403700). These works for Ce L3-edge XAFS were performed at the HXMA beamline of the Canadian Light Source (CLS), a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), and the Government of Saskatchewan.

Keywords

coordination environment
environmental catalysis
NO
selective catalytic reduction
SO-tolerant catalysts

ASJC Scopus subject areas

General Chemistry
Environmental Chemistry

Access to Document

10.1021/acs.est.4c11440

Cite this

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title = "Environmental Catalysis for NOx Reduction by Manipulating the Dynamic Coordination Environment of Active Sites",

abstract = "Nowadays, it is challenging to achieve SO2-tolerant environmental catalysis for NOx reduction because of the thermodynamically favorable transformation of reactive sites to inactive sulfate species in the presence of SO2. Herein, we achieve enhanced low-temperature SO2-tolerant NOx reduction by manipulating the dynamic coordination environment of active sites. Engineered by coordination chemistry, SiO2-CeO2 composite oxides with a short-range ordered Ce-O-Si structure were elaborately constructed on a TiO2 support. A dynamic coordination environment of active sites is demonstrated from a Ce-O-Si local structure to a low-coordinated Ce-SO42- species in the presence of SO2. The low-coordinated Ce-SO42- species as new active sites maintain a high NO removal efficiency by preserving the good adsorption and activation capacity of NO and NH3 reactants. This work proposes a new notion to improve the SO2 resistance of catalysts by regulating the coordination environment of sulfated active sites, which is of significance for SO2-tolerant environmental catalysis in practical applications.",

keywords = "coordination environment, environmental catalysis, NO, selective catalytic reduction, SO-tolerant catalysts",

author = "Lupeng Han and Xiyang Wang and Fuli Wang and Yongjie Shen and Hengxiang Zhang and Weiwei Hu and Min Gao and Wu, {Yimin A.} and Ming Xie and Jianfu Chen and Dengsong Zhang",

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AU - Han, Lupeng

AU - Wang, Xiyang

AU - Wang, Fuli

AU - Shen, Yongjie

AU - Zhang, Hengxiang

AU - Hu, Weiwei

AU - Gao, Min

AU - Wu, Yimin A.

AU - Xie, Ming

AU - Chen, Jianfu

AU - Zhang, Dengsong

PY - 2025/2/4

Y1 - 2025/2/4

N2 - Nowadays, it is challenging to achieve SO2-tolerant environmental catalysis for NOx reduction because of the thermodynamically favorable transformation of reactive sites to inactive sulfate species in the presence of SO2. Herein, we achieve enhanced low-temperature SO2-tolerant NOx reduction by manipulating the dynamic coordination environment of active sites. Engineered by coordination chemistry, SiO2-CeO2 composite oxides with a short-range ordered Ce-O-Si structure were elaborately constructed on a TiO2 support. A dynamic coordination environment of active sites is demonstrated from a Ce-O-Si local structure to a low-coordinated Ce-SO42- species in the presence of SO2. The low-coordinated Ce-SO42- species as new active sites maintain a high NO removal efficiency by preserving the good adsorption and activation capacity of NO and NH3 reactants. This work proposes a new notion to improve the SO2 resistance of catalysts by regulating the coordination environment of sulfated active sites, which is of significance for SO2-tolerant environmental catalysis in practical applications.

AB - Nowadays, it is challenging to achieve SO2-tolerant environmental catalysis for NOx reduction because of the thermodynamically favorable transformation of reactive sites to inactive sulfate species in the presence of SO2. Herein, we achieve enhanced low-temperature SO2-tolerant NOx reduction by manipulating the dynamic coordination environment of active sites. Engineered by coordination chemistry, SiO2-CeO2 composite oxides with a short-range ordered Ce-O-Si structure were elaborately constructed on a TiO2 support. A dynamic coordination environment of active sites is demonstrated from a Ce-O-Si local structure to a low-coordinated Ce-SO42- species in the presence of SO2. The low-coordinated Ce-SO42- species as new active sites maintain a high NO removal efficiency by preserving the good adsorption and activation capacity of NO and NH3 reactants. This work proposes a new notion to improve the SO2 resistance of catalysts by regulating the coordination environment of sulfated active sites, which is of significance for SO2-tolerant environmental catalysis in practical applications.

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KW - selective catalytic reduction

KW - SO-tolerant catalysts

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