Remarkable enhancement in the N2 selectivity of NH3-SCR over the CeNb3Fe0.3/TiO2 catalyst in the presence of chlorobenzene

Abstract

The simultaneous removal of NO_x and dioxins is the frontier of environmental catalysis, which is still in the initial stage and poses several challenges. In this study, a series of CeNb₃Fe_x/TiO₂ (x = 0, 0.3, 0.6, and 1.0) catalysts were prepared by the sol-gel method and examined for the synergistic removal of NO_x and CB. The CeNb₃Fe_0.3/TiO₂ catalyst exhibits an optimum catalytic performance, with an NO_x conversion greater than 95% at 260-380 °C. It also exhibits an optimal CB oxidation activity, in which CB promoted both the NO_x conversion and N₂ selectivity below 250 °C. Moreover, the more favorable ratios of Ce⁴⁺ to Ce³⁺ and plentiful surface-adsorbed oxygen species are the reasons why CeNb₃Fe_0.3/TiO₂ catalyst has better catalytic activity than other catalysts at the lower temperature. Simultaneously, owing to the modulation of Fe to the redox properties of Ce and Nb, the large number of oxygen vacancies and acid sites was generated, and the CeNb₃Fe_0.3/TiO₂ catalyst is beneficial to NO_x reduction and CB oxidation. Furthermore, the results of in situ DRIFTS study reveal the NH₃-SCR reactions over CeNb₃Fe_0.3/TiO₂ catalysts are mainly conformed to by the L-H mechanism (< 350 °C) and E-R mechanism (> 350 °C), respectively, and the multi-pollutant conversion mechanism in the synergistic reaction was systematically studied.

Keywords: Ce-based catalysts; Chlorobenzene; NH3-SCR; Redox; Synergy; VOC removal.