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  4. Aging of industrial Fe-zeolite based catalysts for nitrous oxide abatement in nitric acid production plants
 
research article

Aging of industrial Fe-zeolite based catalysts for nitrous oxide abatement in nitric acid production plants

Buttignol, Filippo
•
Rentsch, Daniel
•
Alxneit, Ivo
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October 31, 2022
Catalysis Science & Technology

The influence of hydrothermal aging on the structural and catalytic properties of two commercial Fe-exchanged zeolite catalysts (Fe-FER and Fe-ZSM-5) in the extruded form employed for the removal of N2O from the exhaust of nitric acid production plants has been investigated. Catalytic experiments showed that N2O conversion was retained on Fe-FER while it was totally lost on Fe-ZSM-5, which promoted N2O formation under reaction conditions of selective catalytic reduction of NOx with NH3 (SCR). Combining data from several characterization techniques, we were able to identify a unique difference in the aging behaviour of the two catalysts. Irrespective of the catalyst, Al-27 and Si-29-MAS NMR spectroscopy demonstrated significant loss of framework Al. NH3-TPD experiments corroborated the NMR results indicating a remarkable loss of NH3 storage capacity, especially at the expense of the Bronsted acidity. In contrast, UV-vis and X-ray absorption spectroscopy showed that the two catalysts experienced opposite behaviour with respect to the evolution of Fe species upon aging. Fe-ZSM-5 suffered from Fe agglomeration, while Fe species experienced re-dispersion in Fe-FER. These results indicate that the aging treatment of the Fe-exchanged zeolite catalysts does not inevitably lead to the agglomeration of isolated Fe sites. Hence, Fe-ZSM-5 develops into a less selective catalyst, promoting N2O formation through the undesired nonselective NH3 oxidation. Differently, this Fe-FER retains its catalytic activity and becomes less active towards NH3 oxidation. The results of our characterization and catalytic activity study could be of relevance for the selection of Fe-zeolite-based catalysts for this type of application. Furthermore, our investigation provides evidence that the fate of extra-framework Fe species under hydrothermal aging cannot be thoroughly described just by an agglomeration phenomenon.

  • Details
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Type
research article
DOI
10.1039/d2cy01486f
Web of Science ID

WOS:000883082700001

Author(s)
Buttignol, Filippo
Rentsch, Daniel
Alxneit, Ivo
Garbujo, Alberto
Biasi, Pierdomenico
Kroecher, Oliver  
Ferri, Davide
Date Issued

2022-10-31

Publisher

ROYAL SOC CHEMISTRY

Published in
Catalysis Science & Technology
Volume

12

Issue

24

Start page

7308

End page

7321

Subjects

Chemistry, Physical

•

Chemistry

•

active-site structure

•

wet ion-exchange

•

n2o decomposition

•

hydrothermal stability

•

surface-chemistry

•

hzsm-5 zeolite

•

zsm-5 zeolites

•

iron sites

•

fe-zsm-5

•

nmr

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
GR-KRO  
Available on Infoscience
December 5, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/192998
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