Insight into the enhanced catalytic activity and H2O/SO2 resistance of MnFeOx/Defect-Engineered TiO2 for low-temperature selective catalytic reduction of NO with NH3

被引:12
|
作者
Lin, Liang-Yi [1 ]
Hsieh, Tsung-Ta [1 ]
Hsu, Ju-Chen [1 ]
Wang, Yu-Chen [1 ]
机构
[1] Natl Yang Ming Chiao Tung Univ, Inst Environm Engn, Hsinchu 300, Taiwan
关键词
Mn-Fe oxide; NH3-SCR; Surface acidity; SO2; poisoning; DefectiveTiO2; SO2; TOLERANCE; TITANIUM-DIOXIDE; OXIDE CATALYST; NH3-SCR; SCR; PERFORMANCE; MECHANISM; PROMOTION; DISPERSION; V2O5/TIO2;
D O I
10.1016/j.apsusc.2022.156139
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A series of Mn-Fe mixed oxide (MnFeOx) supported on high-surface-area TiO2 (Tiov) containing engineered Ti3+/ oxygen vacancies was demonstrated for NH3-SCR of NO. The best catalyst MnFe/Tiov(0.05)-1 exhibited excellent NH3-SCR activity (>99 % conversion) over 60-260 degrees C and superior resistance to high H2O content (20 vol%), with NO conversion exceeding 90 % at temperatures lower than 150 degrees C. Furthermore, MnFe/Tiov(0.05)-1 exhibited outstanding durability over 70 h of sustained operation in the co-presence of H2O and SO2, whereas catalytic deactivation was observed for the conventional TiO2-supported catalyst (MnFe/Ti). The combined re-sults of various characterization techniques confirmed that the interactions between the MnFeOx and Tiov sup-ports were strengthened. The defect-rich surface of the Tiov support promoted the dispersion of MnFeOx and facilitated the redox cycle Mn4+ + Ti3+ <-> Mn3+ + Ti4+, thus facilitating the adsorption and activation of NH3 and NO molecules. Moreover, the in situ diffuse reflectance infrared Fourier transform results indicated that H2O strongly suppressed the adsorption/activation of NH3 and NOx and the reactions between NH3 and NOx through the Langmuir-Hinshelwood pathway on MnFe/Ti, while such adverse effects were significantly reduced when using MnFe/Tiov(0.05)-1, in which the Eley-Rideal mechanism was dominant.
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页数:15
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