Structure–Activity Relationships in NH3-SCR Over Fe Presence in Cu/SAPO-34 as Revealed by In-Situ EPR and In-Situ FI-IR Spectroscopy
摘要
A series of Cu/SAPO-34, Fe/SAPO-34, and Cu–Fe/SAPO-34 catalysts were prepared using the liquid ion-exchange method based on the synthesized SAPO-34 support. The catalysts were performed for the selective catalytic reduction of NOx with NH3 and were characterized using XRD, FE-SEM, and XPS. In-situ characterization using EPR and FT-IR was also carried out further to understand the behavior of the catalyst during the reaction. The Cu–Fe/SAPO-34 catalyst achieved high NH3-SCR activity, excellent N2 selectivity from 200 °C to 600 °C, and was highly resistant to sulfur dioxide and water vapor. The synergistic impact between copper and iron species can explain the results. The results of XPS indicated that the more active site capacity contributed to the excellent NH3-SCR performance upon adding Fe species into Cu/SAPO-34. Moreover, in-situ EPR and in-situ FT-IR studies have demonstrated that the isolated Cu2+ species are active sites, and the NH3-SCR intermediate species with the Cu–Fe/SAPO-34 catalyst are ammonia nitrites at 200 °C, respectively. Meanwhile, a primary response mechanism to Cu–Fe/SAPO-34 was carried out during the NH3-SCR process, combined with prior study findings.
Graphical Abstract