The Unique CO Activation Effects for Boosting NH3 Selective Catalytic Oxidation over CuOx-CeO2

ABSTRACT: Slip NH3 is a priority pollutant of concern to be removed in various flue gases with NOx and CO after denitrification using NH3-SCR or NH3-SNCR, and the simultaneous catalytic removal of NH3 and CO has become one of the new topics in the deep treatment of such flue gases. Synergistic catalytic oxidation of CO and NH3 appears to be a promising method but still has many challenges. Due to the competition for active oxidizing species, CO was supposed to hinder the NH3 selective catalytic oxidation (NH3-SCO). However, it is first found that CO could significantly promote NH3-SCO over the CuOx- CeO2 catalyst. The NH3 conversion rates increased linearly with CO concentrations in the range of 180-300 degrees C. Specifically, it accelerated by 2.8 times with 10,000 ppm CO inflow at 220 degrees C. Mechanism studies found that the Cu-O-Ce solid solution was more active for CO oxidation, while the CuOx species facilitated the NH3 dehydrogenation and mitigated the competition of NH3 and CO, further stabilizing the promotion effects. Gaseous CO boosted the generation of active isolated oxygen atoms (Oi) by actuating the Cu+/Cu2+ redox cycle. The enriched Oi facilitated oxidation of NH3 to NO and was conducive to the NH3-SCO via the i-SCR approach. This study tapped the potential of CO for promoting simultaneous catalytic oxidation of coexisting pollutants in the flue gas.

Automated summary

Slip NH3 is a priority pollutant to be removed after denitrification using NH3-SCR or NH3-SNCR. The simultaneous catalytic removal of NH3 and CO has become a new topic in the treatment of flue gases. In this study, it was found that CO can significantly promote NH3-SCO over the CuOx-CeO2 catalyst by facilitating the generation of active oxygen atoms (Oi) and enhancing the NH3 conversion rates.