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Published on: December 6, 2021
Effects of sulfation on hematite for selective catalytic reduction of nitrogen oxides with ammonia
Yu Zhang1, Shan Yang1, Xiaoyue Zhu1
1College of Chemistry, Chemical Engineering and Materials Science, Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals, Institute of Materials and Clean Energy, Shandong Normal University, Jinan 250014, PR China.
Abstract:
Hematite (α-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 α-Fe2O3 is very low. In this work, α-Fe2O3 obtained excellent N2 selectivity and medium-high temperature activity via a simple surface sulfation method. The α-Fe2O3-350 (sulfated at 350 °C) sample showed an NO conversion rate of ~ 100% in the range of 275-350 °C and exhibited excellent H2O and SO2 resistance ability at 300 °C. Furthermore, pure α-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 α-Fe2O3 changed from surface sulfates to bulk-like sulfates. Although sulfation treatment reduced the redox properties of α-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 α-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.
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