NO reduction by CO over CuO supported on CeO2-doped TiO2: the effect of the amount of a few CeO2

作者:Deng, Changshun; Li, Bin*; Dong, Lihui; Zhang, Feiyue; Fan, Minguang; Jin, Guangzhou; Gao, Junbin; Gao, Liwen; Zhang, Fei; Zhou, Xinpeng
来源:Physical Chemistry Chemical Physics, 2015, 17(24): 16092-16109.
DOI:10.1039/c5cp00745c

摘要

This work is mainly focused on the investigation of the influence of the amount of a few CeO2 on the physicochemical and catalytic properties of CeO2-doped TiO2 catalysts for NO reduction by a CO model reaction. The obtained samples were characterized by means of XRD, N-2-physisorption (BET), LRS, UV-vis DRS, XPS, (O-2, CO, and NO)-TPD, H-2-TPR, in situ FT-IR, and a NO + CO model reaction. These results indicate that a small quantity of CeO2 doping into the TiO2 support will cause an obvious change in the properties of the catalyst and the TC-60 : 1 (the TiO2/CeO2 molar ratio is 60 : 1) support exhibits the most extent of lattice expansion, which indicates that the band lengths of Ce-O-Ti are longer than other TC (the solid solution of TiO2 and CeO2) samples, probably contributing to larger structural distortion and disorder, more defects and oxygen vacancies. Copper oxide species supported on TC supports are much easier to be reduced than those supported on the pure TiO2 and CeO2 surface-modified TiO2 supports. Furthermore, the Cu/TC-60 : 1 catalyst shows the highest activity and selectivity due to more oxygen vacancies, higher mobility of surface and lattice oxygen at lower temperature (which contributes to the regeneration of oxygen vacancies, and the best reducing ability), the most content of Cu+, and the strongest synergistic effect between Ti3+, Ce3+ and Cu+. On the other hand, the CeO2 doping into TiO2 promotes the formation of a Cu+/Cu-0 redox cycle at high temperatures, which has a crucial effect on N2O reduction. Finally, in order to further understand the nature of the catalytic performances of these samples, taking the Cu/TC-60 : 1 catalyst as an example, a possible reaction mechanism is tentatively proposed.