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Promoting effect and mechanism of neodymium on low-temperature selective catalytic reduction with NH3 over Mn/TiO2 catalysts
Affiliation:1. Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, China;2. State Power Environmental Protection Research Institute, Nanjing 210031, China;1. College of Resources and Environment, Zunyi Normal University, Zunyi 563006, China;2. State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China;3. University of Chinese Academy of Sciences, Beijing 100049, China;4. Air Quality Research Division, Science and Technology Branch, Environment and Climate Change Canada, Toronto, M3H 5T4, Canada;5. College of Chemical Engineering, Huaqiao University, Xiamen 361021, China;1. College of Physics and Energy, Fujian Normal University, Fuzhou 350117, China;2. Department of Physics and Electronic Information Engineering, Minjiang University, Fuzhou 350121, China;3. Fujian Provincial Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Xiamen 361005, China;1. School of Resources and Environmental Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China;2. Cooperative Innovation Center of Efficient Development and Application for Ionic Rare Earth Resources, Jiangxi University of Science and Technology, Ganzhou 341000, China;3. School of Architectural and Surveying and Mapping Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China;1. Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, Jiangsu, China;2. State Power Environmental Protection Research Institute, Nanjing 210031, Jiangsu, China;1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;2. Division of Nuclear Technology and Applications, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
Abstract:Series of Mn/TiO2 catalysts modified with various contents of Nd for low-temperature SCR were synthesized. It can be found that the appropriate amount of Nd can markedly reduce the take-off temperature of Mn/TiO2 catalyst to 80 °C and NOx conversion is stabilized over 90% in the wide temperature range of 100–260 °C. 0.1Nd–Mn/Ti shows higher N2 selectivity and better SO2 resistance than Mn/Ti catalyst. The results reveal that Nd-doped Mn/TiO2 catalyst exhibits larger BET surface area and better dispersion of active component Mn2O3. XPS results indicate that the optimal 0.1Nd–Mn/Ti sample possesses higher concentration of Mn4+ and larger amount of adsorbed oxygen at the surface compared with the unmodified counterpart. In situ DRIFTS show that the surface acidity is evidently increased after adding Nd, especially, the Lewis acid sites, and the intermediate (-NH2) is more stable. The reaction mechanism over Mn/Ti and 0.1Nd–Mn/Ti catalysts obey the Eley-Rideal (E-R) mechanisms under low temperature reaction conditions. H2-TPR results show that Nd–Mn/TiO2 catalyst exhibits better low-temperature redox properties.
Keywords:Nd modification  Low-temperature  Selective catalyst reduction  Mechanism  Rare earths
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