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Operando HERFD-XANES/XES studies reveal differences in the activity of Fe-species in MFI and CHA structures for the standard selective catalytic reduction of NO with NH3

2018/11/27 by Miren Agote-Arán, Miren Agote‐Arán, Inés Lezcano-González +9
Chemical Engineering · Chemistry · Materials Science · #Catalysis and Oxidation Reactions #Catalytic Processes in Materials Science #Nanomaterials for catalytic reactions

paper · pdf · doi:10.1016/j.apcata.2018.11.026

openalex publication_date 2018/11/27 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/31

Abstract

Fe-containing zeolites were studied as catalysts for the standard NH3-SCR reaction with the primary aim of gaining insight into the structure-function relationship of these materials. Catalysts with different Fe nuclearity (i.e. isolated species, clusters, large particles) were synthesised by incipient wetness impregnation, using H-ZSM-5, H-SSZ-13 and Silicalite-1 as supports, and characterised by in situ and operando X-ray emission spectroscopy (XES) and high energy resolution fluorescence detected X-ray absorption near-edge spectroscopy (HERFD-XANES) under NH3-SCR conditions. The combination of these techniques allowed us to obtain a detailed understanding of the changes in Fe coordination, oxidation state and geometry occurring during reaction. The results obtained suggested that isolated octahedral Fe3+ species on H-ZSM-5 are highly active under the conditions studied, undergoing reduction when exposed to NH3 or under SCR conditions. In contrast, isolated tetrahedral Fe3+ sites present in Silicalite-1 exhibited lower redox properties, leading to a reduced NO conversion. Clusters and FexOy particles on H-SSZ-13 exhibited low SCR activity.

Citations