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Synergetic catalytic removal of chlorobenzene and NOx from waste incineration exhaust over MnNb0.4Ce0.2Ox catalysts: Performance and mechanism study
Affiliation:1. Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences, Beijing 10083, China;2. State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 10084, China
Abstract:Nb doped MnCe0.2Ox complex oxides catalysts prepared via a homogeneous precipitation method were investigated for synergistic catalytic removal of NOx and chlorobenzene (CB) at low temperatures. The MnNb0.4Ce0.2Ox catalyst with a molar ratio of Nb/Mn = 0.4 exhibits excellent activity and the NOx and CB removal efficiency reaches 94.5% and 96% at 220 °C, respectively. Furthermore, the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox still remains above 80% after injecting 300 ppm SO2 and 7 vol% H2O for 36 h. In addition, the presence of CB and NOx + NH3 can improve the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox, respectively. The analysis results from N2-BET, Py-IR, H2-TPR and NH3-TPD reveal that the introduction of Nb increases the average pore size, pore volume and surface area, promoted the growth of Lewis acid amount obviously, and enhances redox ability of MnCe0.2Ox at 100–250 °C. Moreover, the molecular migration process of NOx, NH3, CB and SO2 in NH3-SCR and CB oxidation reaction over MnNb0.4Ce0.2Ox catalysts were systematically studied. In situ DRIFTS, FT-IR and XPS also confirm that the adsorption of sulfate species and SO2 on the surface of MnNb0.4Ce0.2Ox is inhibited effectively by the introduction of Nb in the presence of SO2 and H2O. Moreover, Nb additives also enhance the structural stability of MnNb0.4Ce0.2Ox, due to the interactions among Mn, Nb and Ce. The NH3-TPD, H2-TPR and in situ DRIFTS results also confirm that the MnNb0.4Ce0.2Ox still retains abundant acid sites and high redox ability in the presence of SO2 and H2O. In summary, MnNb0.4Ce0.2Ox catalysts represent a promising and effective candidate for controlling NOx and CB at low temperatures.
Keywords:Synergistic catalytic removal  Chlorobenzene (CB)  Hydrothermal stability  Removal mechanism  Rare earths
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