Effects of Nb-modified CeVO4 to form surface Ce-O-Nb bonds on improving low-temperature NH3-SCR deNOx activity and resistance to SO2 & H2O

Abstract

A series of novel ternary CeVO4 modified with different Nb contents (CeNbVO) catalysts were synthesized via alkali-assisted hydrothermal method, and applied for selective catalytic reduction (SCR) of NOx with NH3. The as-prepared CeNbVO catalysts show enhanced NH3-SCR performance compared with the CeVO catalyst. Especially, the optimal CeNbVO-2 with appropriate Nb amount displays the superior NH3-SCR activity with above 90 % NO conversion in the range of 210–420 °C with 5 %vol·H2O and excellent resistance to H2O/SO2. Effects of Nb-modified CeVO4 to form surface Ce-O-Nb bonds on improving low-temperature NH3-SCR activity and resistance to SO2 & H2O were investigated by using various characterization methods, including XRD, Raman spectroscopy, N2 physical adsorption, TEM, H2-TPR, NH3-TPD, O2-TPD, NO-TPD, XPS, kinetic tests and in-situ DRIFTS. Different phases can be obtained with the different Nb amount doping, leading to different SCR activity. The pure CeVO4 phase with the short-range ordered Nbn+–O2–-Cen+ bond is formed by adding a small amount of Nb in CeNbVO-2. The superior catalytic performance of CeNbVO-2 can be ascribed to its improved acidity and suitable oxidation ability, which may counteract the negative effects of nonselective NH3 oxidation to N2O. It is found that the formation of Nbn+–O2–-Cen+ bonds can significantly increase the surface active oxygen species and oxygen vacancy of the catalyst. Additionally, the NH3-SCR reaction mechanism is revealed using in-situ DRIFTS and kinetic studies.