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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

Agote-Arán, M; Lezcano-González, I; Greenaway, AG; Hayama, S; Díaz-Moreno, S; Kroner, AB; Beale, AM; (2019) 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. Applied Catalysis A: General , 570 pp. 283-291. 10.1016/j.apcata.2018.11.026. (In press). Green open access

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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.

Type: Article
Title: 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
Open access status: An open access version is available from UCL Discovery
DOI: 10.1016/j.apcata.2018.11.026
Publisher version: https://doi.org/10.1016/j.apcata.2018.11.026
Language: English
Additional information: Copyright © 2018 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/BY/4.0/).
Keywords: NH3-SCR, NO, Fe-containing zeolites, HERFD-XANES, XES
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10065130
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