Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 203, Issue -, Pages 704-714Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2016.10.039
Keywords
MoFe/Beta; CeO2; Core-shell; SO2 tolerance; Selective catalytic reduction
Funding
- National Natural Science Foundation of China [21673290, 21376261]
- 863 Program of China [2015AA034603]
- Beijing Natural Science Foundation [2142027]
- China University of Petroleum Fund [20130007110007, 2462015QZDX04]
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MoFe/Beta@CeO2 core-shell catalyst was designed with nano-size Beta supporting MoFe bimetallic oxides as the core and CeO2 thin film as the shell. The structure and physico-chemical properties of the coated and uncoated CeO2 catalysts were characterized by TEM, SEM, XRD, N-2 adsorption-desorption, XPS, XANES, ICP-AES, NH3-TPD, H-2-TPR and in-situ DRIFTS. The catalytic activity tests for NH3-SCR of NO indicated that the catalyst coated by CeO2 shell exhibits a remarkable improvement of deNO(x) activity, excellent tolerance to SO2 and H2O, as well as high thermal stability. The both chemisorbed oxygen species (O-2(-), O-) and specific surface area increased for the catalysts after the coating of CeO2 shells. CeO2 shells not only increase the acid amount but also improve its acid strength, which could be beneficial to improving NO oxidation to NO2 during NH3-SCR. Furthermore, there is a strong interaction among the iron oxides, molybdenum oxides and CeO2 shells. CeO2 shells can serve as an effective barrier to inhibit the active metal oxides nanoparticles from aggregating at high temperature. As a result, the coated catalyst with CeO2 thin film shows a better thermal stability than the uncoated one. What's more, CeO2 shells can not only suppress the formation of ammonium nitrate and sulfate species blocking the active iron sites but also restrain the generation of iron sulfate, leading to a higher SO2 and H2O-tolerance. The above results demonstrate that the design of a core-shell structure catalyst is favorable for improving the performance of deNO(x) catalysts. (C) 2016 Elsevier B.V. All rights reserved.
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