Regulating the redox sites of MMoOx (M = Mn, Fe, Cr) catalysts for highly efficient selective catalytic oxidation of NH3
摘要
Redox sites and acidic sites are the main active sites of bimetallic oxide catalysts used for selective catalytic oxidation of NH3 (NH3-SCO). In this work, three MMoOx (M = Cr, Fe, and Mn) bimetallic oxides catalysts were prepared by simple grinding and calcination to investigate the effect of redox sites (M sites) on the NH3-SCO performance. The NH3-SCO test results showed that the activity of MMoOx is in the order of CrMoOx > MnMoOx > FeMoOx. The characterization results of H2-TPR, O2-TPD, NH3-TPD, and in situ DRIFTS proposed that the NH3-SCO reaction on MMoOx catalysts is proceed via i-SCR mechanism, and the formation of the intermediates of NH3-SCR reaction is the decisive reaction step. Owing to the excellent ability in promoting the formation of nitrate/nitrite species, CrMoOx and MnMoOx samples show much higher NH3-SCO activity than FeMoOx sample. CrMoOx can facilitate the formation of a large amount of –NH2 species, which together with nitrate/nitrite species enhance the NH3-SCO reaction via i-SCR reaction route. Therefore, CrMoOx shows the highest NH3-SCO activity among the MMoOx catalysts. Through this work, the redox sites of bimetallic oxide catalysts are demonstrated as a vital role in inducing the formation of reaction-active intermediates, which highlight the importance of choosing the redox sites in designing NH3-SCO catalyst.