Vanadia-based SCR Catalysts Supported on Tungstated and Sulfated Zirconia: Influence of Doping with Potassium

Johannes Due-Hansen, Soghomon Boghosian, Arkadii Kustov, Peter Fristrup, George Tsilomelekis, Kenny Ståhl, Claus H. Christensen, Rasmus Fehrmann

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

A series of vanadium-based SCR catalysts supported on sulfated or tungstated ZrO2 were synthesized and characterized by means of N2-BET, XRD, NH3-TPD and in situ Raman spectroscopy. The effect of potassium doping on the properties of vanadia species is studied in detail. A number of catalyst preparation parameters were examined, including the choice of precipitant, variation of carrier surface area, potassium poisoning, crystallinity, and ZrO2-phase composition. The results show that the catalysts structure and SCR activity is affected from the synthesis route by means of support crystallinity and morphology, the surface composition and the molecular configuration of the dispersed vanadates. It was observed that poisoning with potassium had a negligible effect on the surface vanadate species (especially the V=O stretching frequency observed by in situ Raman spectroscopy) if supported on the sulfated zirconia. Conversely, a more pronounced influence on the structure of surface vanadate was observed for the corresponding unsulfated samples, where a significant red shift in V=O stretching frequency was observed upon potassium doping. Computational studies suggests that potassium is responsible for both the observed decrease in V=O stretching frequency and the higher proportion of dimers and higher polymers through coordination between K+ and two neighbouring V=O. The results suggest an increased resistance towards potassium doping for the vanadia-based catalysts supported on sulfated zirconia.
Original languageEnglish
JournalJournal of Catalysis
Volume251
Issue number2
Pages (from-to)459-473
ISSN0021-9517
DOIs
Publication statusPublished - 2007

Keywords

  • NO SCR with ammonia
  • Tungstated zirconia
  • Sulfated zirconia
  • In situ Raman
  • Vanadium oxide
  • Potassium poisoning
  • Deactivation
  • Biomass

Cite this

Due-Hansen, Johannes ; Boghosian, Soghomon ; Kustov, Arkadii ; Fristrup, Peter ; Tsilomelekis, George ; Ståhl, Kenny ; Christensen, Claus H. ; Fehrmann, Rasmus. / Vanadia-based SCR Catalysts Supported on Tungstated and Sulfated Zirconia: Influence of Doping with Potassium. In: Journal of Catalysis. 2007 ; Vol. 251, No. 2. pp. 459-473.
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title = "Vanadia-based SCR Catalysts Supported on Tungstated and Sulfated Zirconia: Influence of Doping with Potassium",
abstract = "A series of vanadium-based SCR catalysts supported on sulfated or tungstated ZrO2 were synthesized and characterized by means of N2-BET, XRD, NH3-TPD and in situ Raman spectroscopy. The effect of potassium doping on the properties of vanadia species is studied in detail. A number of catalyst preparation parameters were examined, including the choice of precipitant, variation of carrier surface area, potassium poisoning, crystallinity, and ZrO2-phase composition. The results show that the catalysts structure and SCR activity is affected from the synthesis route by means of support crystallinity and morphology, the surface composition and the molecular configuration of the dispersed vanadates. It was observed that poisoning with potassium had a negligible effect on the surface vanadate species (especially the V=O stretching frequency observed by in situ Raman spectroscopy) if supported on the sulfated zirconia. Conversely, a more pronounced influence on the structure of surface vanadate was observed for the corresponding unsulfated samples, where a significant red shift in V=O stretching frequency was observed upon potassium doping. Computational studies suggests that potassium is responsible for both the observed decrease in V=O stretching frequency and the higher proportion of dimers and higher polymers through coordination between K+ and two neighbouring V=O. The results suggest an increased resistance towards potassium doping for the vanadia-based catalysts supported on sulfated zirconia.",
keywords = "NO SCR with ammonia, Tungstated zirconia, Sulfated zirconia, In situ Raman, Vanadium oxide, Potassium poisoning, Deactivation, Biomass",
author = "Johannes Due-Hansen and Soghomon Boghosian and Arkadii Kustov and Peter Fristrup and George Tsilomelekis and Kenny St{\aa}hl and Christensen, {Claus H.} and Rasmus Fehrmann",
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language = "English",
volume = "251",
pages = "459--473",
journal = "Journal of Catalysis",
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Vanadia-based SCR Catalysts Supported on Tungstated and Sulfated Zirconia: Influence of Doping with Potassium. / Due-Hansen, Johannes; Boghosian, Soghomon; Kustov, Arkadii; Fristrup, Peter; Tsilomelekis, George; Ståhl, Kenny; Christensen, Claus H.; Fehrmann, Rasmus.

In: Journal of Catalysis, Vol. 251, No. 2, 2007, p. 459-473.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Vanadia-based SCR Catalysts Supported on Tungstated and Sulfated Zirconia: Influence of Doping with Potassium

AU - Due-Hansen, Johannes

AU - Boghosian, Soghomon

AU - Kustov, Arkadii

AU - Fristrup, Peter

AU - Tsilomelekis, George

AU - Ståhl, Kenny

AU - Christensen, Claus H.

AU - Fehrmann, Rasmus

PY - 2007

Y1 - 2007

N2 - A series of vanadium-based SCR catalysts supported on sulfated or tungstated ZrO2 were synthesized and characterized by means of N2-BET, XRD, NH3-TPD and in situ Raman spectroscopy. The effect of potassium doping on the properties of vanadia species is studied in detail. A number of catalyst preparation parameters were examined, including the choice of precipitant, variation of carrier surface area, potassium poisoning, crystallinity, and ZrO2-phase composition. The results show that the catalysts structure and SCR activity is affected from the synthesis route by means of support crystallinity and morphology, the surface composition and the molecular configuration of the dispersed vanadates. It was observed that poisoning with potassium had a negligible effect on the surface vanadate species (especially the V=O stretching frequency observed by in situ Raman spectroscopy) if supported on the sulfated zirconia. Conversely, a more pronounced influence on the structure of surface vanadate was observed for the corresponding unsulfated samples, where a significant red shift in V=O stretching frequency was observed upon potassium doping. Computational studies suggests that potassium is responsible for both the observed decrease in V=O stretching frequency and the higher proportion of dimers and higher polymers through coordination between K+ and two neighbouring V=O. The results suggest an increased resistance towards potassium doping for the vanadia-based catalysts supported on sulfated zirconia.

AB - A series of vanadium-based SCR catalysts supported on sulfated or tungstated ZrO2 were synthesized and characterized by means of N2-BET, XRD, NH3-TPD and in situ Raman spectroscopy. The effect of potassium doping on the properties of vanadia species is studied in detail. A number of catalyst preparation parameters were examined, including the choice of precipitant, variation of carrier surface area, potassium poisoning, crystallinity, and ZrO2-phase composition. The results show that the catalysts structure and SCR activity is affected from the synthesis route by means of support crystallinity and morphology, the surface composition and the molecular configuration of the dispersed vanadates. It was observed that poisoning with potassium had a negligible effect on the surface vanadate species (especially the V=O stretching frequency observed by in situ Raman spectroscopy) if supported on the sulfated zirconia. Conversely, a more pronounced influence on the structure of surface vanadate was observed for the corresponding unsulfated samples, where a significant red shift in V=O stretching frequency was observed upon potassium doping. Computational studies suggests that potassium is responsible for both the observed decrease in V=O stretching frequency and the higher proportion of dimers and higher polymers through coordination between K+ and two neighbouring V=O. The results suggest an increased resistance towards potassium doping for the vanadia-based catalysts supported on sulfated zirconia.

KW - NO SCR with ammonia

KW - Tungstated zirconia

KW - Sulfated zirconia

KW - In situ Raman

KW - Vanadium oxide

KW - Potassium poisoning

KW - Deactivation

KW - Biomass

U2 - 10.1016/j.jcat.2007.07.016

DO - 10.1016/j.jcat.2007.07.016

M3 - Journal article

VL - 251

SP - 459

EP - 473

JO - Journal of Catalysis

JF - Journal of Catalysis

SN - 0021-9517

IS - 2

ER -