American Chemical Society
jp2c03480_si_001.pdf (1.69 MB)

Monomeric Fe Species in Square Planar Geometry Active for Low Temperature NH3‑SCR of NO

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journal contribution
posted on 2022-10-05, 21:29 authored by Dominik Wierzbicki, Adam H. Clark, Oliver Kröcher, Davide Ferri, Maarten Nachtegaal
Monomeric Fe species in zeolites are considered to be the active sites for the low temperature activity toward ammonia-assisted selective catalytic reduction of nitrogen oxides (NH3-SCR) in exhaust gases. Herein, we report on a preparation method to synthesize single-site Fe/ZSM-5 by combination of dealumination with the use of a bulky iron complex to introduce Fe. Transient in situ XAS experiments at the Fe K-edge under dynamic NH3-SCR reaction conditions demonstrated the involvement of all iron atoms in the redox cycle and, with that, suggest that Fe species in the studied Fe/ZSM-5 catalyst are monomers. Simulation of experimental X-ray absorption data revealed that the Fe species in the sample obtained by this approach adopt a square planar geometry, which changes into fivefold coordination at low temperature by strongly binding either NO or NH3 as the ligand. The presence of monomeric Fe species in this Fe/ZSM-5 conveys molecular level insights into the temperature-dependent NH3-SCR activity and might prove useful in the study of other reactions over monomeric Fe species, such as methane partial oxidation or dehydroaromatization reactions.