期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 606, 期 -, 页码 1445-1456出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.08.088
关键词
Sulfated alpha-Fe2O3; NH3-SCR; H2O+SO2 tolerance; Surface acidity; DFT calculations
资金
- National Natural Science Foun-dation of China [21976111]
- Shandong Provincial Natural Science Foundation [ZR2019MB052]
- Large Instrument Open Founda-tion of Shandong Normal University [KFJJ2019004, KFJJ2021006]
In this study, the activity and selectivity of hematite were improved via surface sulfation, with moderate sulfate species enhancing activity while excessive sulfates decreasing it, ultimately inhibiting the Langmuir-Hinshelwood mechanism in NH3-SCR reactions.
Hematite (alpha-Fe2O3) is a promising candidate for NH3 selective catalytic reduction (NH3-SCR) of NOx due to its good sulfur resistance. However, the activity of pure alpha-Fe2O3 is very low. In this work, alpha-Fe2O3 obtained excellent N-2 selectivity and medium-high temperature activity via a simple surface sulfation method. The alpha-Fe2O3-350 (sulfated at 350 degrees C) sample showed an NO conversion rate of similar to 100% in the range of 275-350 degrees C and exhibited excellent H2O and SO2 resistance ability at 300 degrees C. Furthermore, pure alpha-Fe2O3 was used as a model catalyst to fully uncover the effect of sulfation on FeOx-based catalysts in NH3-SCR reactions. Structural characterization indicated that the degree of surface sulfation of the catalyst would be deepened with increasing temperature, and the states of sulfate species on alpha-Fe2O3 changed from surface sulfates to bulk-like sulfates. Although sulfation treatment reduced the redox properties of alpha-Fe2O3, it significantly increased its surface acidity and thus the activity. Excessive bulk-like sulfates induced a decrease in activity. Sulfation inhibited the adsorption of NOx on the alpha-Fe2O3 catalyst surface and reduced the thermal stability of nitrates at medium-high temperature. Thus, the Langmuir-Hinshelwood (L-H) mechanism was inhibited, and the reaction mainly followed the Eley-Rideal (E-R) mechanism. (C) 2021 Elsevier Inc. All rights reserved.
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