Insight into structure defects and catalytic mechanism for NO oxidation over Ce0.6Mn0.4Ox solid solutions catalysts: Effect of Manganese precursors

被引:25
作者
Hao, Boyuan [1 ,2 ]
Sun, Yonggang [3 ]
Shen, Qun [4 ]
Zhang, Xin [5 ]
Zhang, Zhongshen [5 ]
机构
[1] China Univ Min & Technol, Sch Chem & Environm Engn, Beijing 100083, Peoples R China
[2] Imperial Coll London, Dept Chem, London SW7 2AZ, England
[3] Ningxia Univ, Coll Chem & Chem Engn, State Key Lab High Efficiency Coal Utilizat & Gre, Yinchuan 750021, Peoples R China
[4] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
[5] Univ Chinese Acad Sci, Res Ctr Environm Mat & Pollut Control Technol, Natl Engn Lab VOCs Pollut Control Mat & Technol, Beijing 101408, Peoples R China
基金
中国国家自然科学基金;
关键词
Mn precursors; NO oxidation; Oxygen species; Ce0.6Mn0.4Ox; MNOX-CEO2 MIXED OXIDES; LOW-TEMPERATURE; SUPERIOR CATALYST; OXYGEN VACANCIES; REDUCTION; SURFACE; NH3; MN; ADSORPTION; PEROVSKITE;
D O I
10.1016/j.chemosphere.2019.125406
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The effects of Mn precursors on structure defects and NO catalytic mechanism over Ce0.6Mn0.4Ox catalysts were fully investigated. The Ce0.6Mn0.4Ox-Ac catalyst, synthesized by using MnAc2 as a Mn precursor, showed the best catalytic activity for NO conversion (86.9%) at 250 degrees C under high space velocity (40,000 mL g(-1) h(-1)). Detailed structure-activity relationship reveals that the abundant oxygen vacancies and the highly migratory oxygen species formed on Ce0.6Mn0.4Ox are the crucial factors that leading to the better NO oxidation activity than that of the other Ce0.6Mn0.4Ox-Y (Y=NO3,SO4, Cl) catalysts. In situ DRIFTS technique confirms that the differences in formation mode and desorption ability of N-based (nitrates, nitrites, and dimer nitroso) intermediate species are the vital factors for NO high-efficiency catalytic oxidation. The highly reactive surface intermediate species, like monodentate nitrates, were observed particularly on Ce0.6Mn0.4Ox-Ac catalyst, so that the NO oxidation performance on Ce0.6Mn0.4Ox-Ac catalyst was more active comparing with other Ce0.6Mn0.4Ox-Y catalysts. This study can broaden the horizons for understanding NO catalytic oxidation mechanism on serial Ce0.6Mn0.4Ox catalysts and serve as a reference guide in design of structure defects for functional materials by modulating precursor species. (C) 2019 Elsevier Ltd. All rights reserved.
引用
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页数:9
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