4.7 Article

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

Journal

APPLIED SURFACE SCIENCE
Volume 614, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apsusc.2022.156139

Keywords

Mn-Fe oxide; NH3-SCR; Surface acidity; SO2 poisoning; DefectiveTiO2

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A series of Mn-Fe mixed oxide (MnFeOx) supported on high-surface-area TiO2 (Tiov) with engineered Ti3+/oxygen vacancies was used for NH3-SCR of NO. The best catalyst, MnFe/Tiov(0.05)-1, showed excellent NH3-SCR activity (>99% conversion) at 60-260 degrees C and resistance to high H2O content (20 vol%). It also exhibited outstanding durability in the presence of H2O and SO2, while the conventional TiO2-supported catalyst (MnFe/Ti) experienced catalytic deactivation. Various characterization techniques confirmed the strengthened interactions between MnFeOx and Tiov supports.
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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