Fe-HFER and Cu-HFER as catalysts for the NOx SCR using acetylene as a reducing agent: Reaction mechanism revealed by FT-IR operando study coupled with (NO)-N-15 isotopic labelling

摘要

Among NOx emission sources, the automotive industry and specifically Diesel engines are the main pollutants. Selective catalytic reduction by Hydrocarbons (HC-SCR) may lead to efficiencies as high as 70% in reducing NOx into N-2 specially by using economical catalysts (zeolites). We report here an HC-SCR study using acetylene (C2H2) as a reducing agent that presents intersting activity at low temperatures. A ferrierite zeolite catalyst was used and modified by the introduction of either copper or iron and the NOx reduction activity was analysed by InfraRed (IR) operando techniques subsequent to a preliminary IR in-situ characterization. The later technique allowed the identification of the species formed on the surface after NO or C2H2 adsorption at room temperature. The thermal stability of adsorbed acetylene was also investigated. The obtained information on vibrational bands typical for adsorbed species served as an input for the IR operando study. Cu-HFER catalyst presents a strong redox character upon room temperature interaction with NO as well as a strong affinity for C2H2 adsorption. However, Fe-HFER shows a higher NOx reduction efficiency when submitted to SCR conditions. Indeed, iron ions enhance the NO oxidation into NO2 that seems to be more reactive with C2H2. The reaction mechanism was revealed by an FT-IR operando study coupled with (NO)-N-15 isotopic labelling that proved the formation of hydrocyanic acid and isocyanate species as key intermediate species. (C) 2017 Elsevier B.V. All rights reserved.