Journal
APPLIED CATALYSIS A-GENERAL
Volume 570, Issue -, Pages 283-291Publisher
ELSEVIER
DOI: 10.1016/j.apcata.2018.11.026
Keywords
NH3-SCR; NO; Fe-containing zeolites; HERFD-XANES; XES
Categories
Funding
- EPSRC (EPK, a UCL Impact PhD award)
- EPSRC (Diamond Light Source)
- EPSRC (Johnson Matthey)
- EPSRC [EP/K014706/1, EP/K014668/1, EP/K014854/1, EP/K014714/1, EP/I019693/1, EP/K007467/1]
- [SP9925-2]
- EPSRC [EP/I019693/1, EP/K014714/1, EP/K007467/1] Funding Source: UKRI
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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 (HERFDXANES) 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.
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