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).
Preview |
Text
1-s2.0-S0926860X18305817-main.pdf - Published Version Download (3MB) | Preview |
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 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 |
Archive Staff Only
 |
View Item |
