Mn/beta与Mn/ZSM-5催化剂对氨选择性催化还原NO的低温催化活性比较:锰前驱体的影响

Abstract Two series of Mn/beta and Mn/ZSM-5 catalysts were prepared to study the influence of how different Mn precursors, introduced to the respective parent zeolites by wet impregnation, affected the selective catalytic reduction (SCR) of NO by NH 3 across a low reaction temperature window of 50–350 °C. In this study, the catalysts were characterized using N 2 adsorption/desorption, X-ray diffraction, X-ray fluorescence, H 2 temperature-programmed reduction, NH 3 temperature-programmed desorption and X-ray photoelectron spectroscopy. As the manganese chloride precursor only partially decomposed this primarily resulted in the formation of MnCl 2 in addition to the presence of low levels of crystalline Mn 3 O 4 , which resulted in poor catalytic performance. However, the manganese nitrate precursor formed crystalline MnO 2 as the major phase in addition to a minor presence of unconverted Mn-nitrate. Furthermore, manganese acetate resulted principally in a mixture of amorphous Mn 2 O 3 and MnO 2 , and crystalline Mn 3 O 4 . From all the catalysts screened, the test performance data showed Mn/beta-Ac to exhibit the highest NO conversion (97.5%) at 240 °C, which remained >90% across a temperature window of 220–350 °C. The excellent catalytic performance was ascribed to the enrichment of highly dispersed MnO x (Mn 2 O 3 and MnO 2 ) species that act as the active phase in the NH 3 -SCR process. Furthermore, together with a suitable amount of weakly acidic centers, higher concentration of surface manganese and a greater presence of surface labile oxygen groups, SCR performance was collectively enhanced at low temperature.