期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 47, 期 13, 页码 8261-8274出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2021.12.170
关键词
Ce-La-Fe/gamma-Al2O3; NH3-SCR; Surface adsorption oxygen; DRIFTS; Reaction mechanism
资金
- Inner Mongolia Graduate Education Innovation Program Graduate Research Innovation Project Grant (2020) - Inner Mongolia Natural Science Autonomous Region [2021LHMS02003, 2019MS02005, 2019MS05050]
- National Key Laboratory for Rare Earth Resources [RERU2021010]
- National Natural Science Foundation of China [51964039, 22068029]
- Baotou Science and Technology Bureau [2019Z3004-3]
- Collaborative Innovation Center of Integrated Exploitation of Bayan Obo Multi-Metal Resources, Inner Mongolia University of Science and Technology, Baotou, China
Ce-La-Fe/gamma-Al2O3 catalysts were prepared to investigate the synergistic relationship between Ce, La, and Fe in natural bastnasite and their effects on NH3-SCR. The results showed that increasing Fe species improved the denitration performance of the catalysts and enhanced surface properties and adsorption capabilities.
A number of Ce-La-Fe/gamma-Al2O3 catalysts were prepared by impregnation and microwave hydrothermal heating based on the ratio of Ce, La, and Fe in natural bastnasite to examine the synergistic relationship between Ce, La, and Fe in natural bastnasite and its effects on ammonia selective catalytic reduction (NH3-SCR). The results demonstrated that an increase in Fe species is beneficial to the denitration performance of catalysts with a Ce:La:Fe mole ratio of 1:0.6:0.12, thus providing high NO conversion (>95%) at 350 degrees C. X-ray diffraction, transmission electron microscopy, and Raman spectroscopy results confirmed the formation of a solid solution between Ce, La, and Fe in the catalysts. The BET isotherms and NH3-TPD demonstrated that the addition of Fe increased the surface area and strengthened the surface acidity of Lewis acid sites. XPS and in situ DRIFTS indicated that electron transfer occurred between Fe3+/Fe2+ and Ce4+/Ce3+ redox cycles in the catalyst, thereby improving the adsorption and activation ability of NO and NH3. NO species were adsorbed on the catalysts in the form of monodentate nitrate, and then monodentate nitrate was oxidized to bidentate nitrate. The SCR reaction route was the coexistence of Eley-Rideal and Langmuir-Hinshelwood mechanisms. (C) 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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