SCR of NO with CH4 over Fe/Ga2O3-Al2O3 and the mechanism

被引:23
|
作者
Wen, Nini [1 ]
Lin, Rui [1 ]
Su, Yaxin [1 ]
Deng, Wenyi [1 ]
Zhou, Hao [2 ]
Zhao, Bingtao [3 ]
机构
[1] Donghua Univ, Sch Environm Sci & Engn, Shanghai 201620, Peoples R China
[2] Changzhou Vocat Inst Engn, Changzhou 213164, Peoples R China
[3] Univ Shanghai Sci & Technol, Sch Energy & Power Engn, Shanghai 200093, Peoples R China
来源
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING | 2021年 / 9卷 / 01期
基金
中国国家自然科学基金;
关键词
NO; SCR-CH4; xFe/Ga2O3-Al2O3; Isolated Fe3+; In situ DRIFTS; SELECTIVE CATALYTIC-REDUCTION; WATER-VAPOR; NITROGEN-OXIDES; SOLID-SOLUTIONS; HC-SCR; METHANE; C3H6; GA2O3-AL2O3; PERFORMANCE; ADSORPTION;
D O I
10.1016/j.jece.2020.105014
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The selective catalytic reduction of NO with methane (SCR-CH4) is a very promising alternative method, however, the catalysts reported showed low catalytic activity for SCR-CH4. In order to improve the catalytic activity and resistance to H2O of the catalysts, Fe was introduced to modify the Ga2O3-Al2O3. The xFe/Ga2O3-Al2O3 catalysts were prepared with the co-precipitation method, and the SCR-CH4 performance was investigated. It was found that Fe improved the catalytic activity at medium and high temperatures, the N-2 selectivity, and the resistance to H2O. Among all catalysts, the 5Fe/Ga2O3-Al2O3 catalyst achieved NO conversion of 76% and N-2 selectivity of 100% at 500 degrees C, and still maintained NO conversion of more than 60% in the presence of 5% H2O. Several characterization techniques, XRD, N-2 adsorption-desorption, XPS, UV-Vis, H-2-TPR, Py-IR, etc., were used to explore the relationship between the catalytic activity and structure. The results showed that after the doping of Fe, the pore diameter was increased, resulting in a promotion in the resistance to H2O. In addition, the redox properties and Lewis acid content of the catalysts were promoted by the Fe species, where the isolated Fe3+ species contribute to the catalytic activity at medium and high temperatures. In situ DRIFTS revealed that NO, CH4, and O-2 were adsorbed and reacted on the catalyst surface to form various nitrates, formate, and R-NCO species, where O-2 can promote the formation of bidentate nitrates.
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页数:10
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