Selective catalytic oxidation of DMF over Cu-Ce/H-MOR by modulating the surface active sites.

Autor: Xu HH; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Xian YW; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Zhao X; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Xu LY; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Wen CH; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Zhao H; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Tang C; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Jia WZ; Huzhou Key Laboratory of Environmental Functional Materials and Pollution Control, Department of Materials Engineering, Huzhou University, Huzhou 313000, China. Electronic address: jiawenzhi@126.com., Luo MF; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China., Chen J; Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, China. Electronic address: jianchen@zjnu.cn.
Jazyk: angličtina
Zdroj: Journal of hazardous materials [J Hazard Mater] 2024 Aug 05; Vol. 474, pp. 134829. Date of Electronic Publication: 2024 Jun 09.
DOI: 10.1016/j.jhazmat.2024.134829
Abstrakt: Selective catalytic oxidation of the hazardous DMF exhaust gas presents a significant challenge in balancing oxidation activity and products selectivity (CO, NO x , N 2 , etc.). It is found that Cu/H-MOR demonstrates superior performance for DMF oxidation compared to CuO on other supports (γ-Al 2 O 3 , HY, ZSM-5) in terms of product selectivity and stability. The geometric and electronic structures of CuO active sites in Cu/H-MOR have been regulated by CeO 2 promoter, leading to an increase in the ratio of active CuO (highly dispersed CuO and Cu + specie). As a result, the oxidation activity and stability of the Cu/H-MOR catalyst were enhanced for DMF selective catalytic oxidation. However, excessive CuO or CeO 2 content led to decreased N 2 selectivity due to over-high oxidation activity. It is also revealed that Ce 3+ species, active CuO species, and surface acid sites play a critical role in internal selective catalytic reduction reaction during DMF oxidation. The 10Cu-Ce/H-MOR (1/4) catalyst exhibited both high oxidation activity and internal selective catalytic reduction activity due to its abundance of active CuO specie as well as Ce 3+ species and surface acid sites. Consequently, the 10Cu-Ce/H-MOR (1/4) catalyst demonstrated the widest temperature window for DMF oxidation with high N 2 selectivity. These findings emphasize the importance of surface active sites modification for DMF selective catalytic oxidation.
Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
(Copyright © 2024 Elsevier B.V. All rights reserved.)
Databáze: MEDLINE
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