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Unravelling the mechanism of NO and NO₂ storage in ceria: The role of defects and Ce-O surface sites

Filtschew, Anastasia ; Hess, Christian (2018)
Unravelling the mechanism of NO and NO₂ storage in ceria: The role of defects and Ce-O surface sites.
In: Applied Catalysis B: Environment and Energy, 237
doi: 10.1016/j.apcatb.2018.06.058
Artikel, Bibliographie

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Kurzbeschreibung (Abstract)

Ceria is an important NOₓ storage material often used in combination with barium or zirconia. To elucidate the NO and NO₂ storage mechanism in ceria we employed in situ Raman spectroscopy coupled with simultaneous FT-IR gas-phase analysis. The Raman spectra reveal new information about the dynamics of the surface and bulk structure of ceria upon NOₓ exposure at 30 °C besides the identification of nitrite and nitrate adsorbates. In particular, Raman spectra provide direct evidence of the involvement of Ce-O surface sites so far not accessible by spectroscopic methods. These Ce-O sites play a key role for NOₓ storage, as their amount strongly influences the NOₓ storage capacity. A reduction of ceria prior to NOₓ exposure resulted in a lower NOₓ storage capacity, as long as no strong oxidizing agent (e.g. NO₂) was present to form new Ce-O sites. In the case of NO storage at 30 °C, new reaction pathways are postulated that describe the activation of gas-phase oxygen for ionic nitrite transformation and formation of new NOₓ adsorption sites. However, it is shown that the activated oxygen species is not a peroxide, as no correlation was found between the peroxides and formed nitrate and nitrite species. Based on our results, a mechanism for NO and NO₂ storage in ceria was formulated.

Typ des Eintrags: Artikel
Erschienen: 2018
Autor(en): Filtschew, Anastasia ; Hess, Christian
Art des Eintrags: Bibliographie
Titel: Unravelling the mechanism of NO and NO₂ storage in ceria: The role of defects and Ce-O surface sites
Sprache: Englisch
Publikationsjahr: 23 Juni 2018
Ort: Amsterdam
Verlag: Elsevier
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Applied Catalysis B: Environment and Energy
Jahrgang/Volume einer Zeitschrift: 237
DOI: 10.1016/j.apcatb.2018.06.058
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Kurzbeschreibung (Abstract):

Ceria is an important NOₓ storage material often used in combination with barium or zirconia. To elucidate the NO and NO₂ storage mechanism in ceria we employed in situ Raman spectroscopy coupled with simultaneous FT-IR gas-phase analysis. The Raman spectra reveal new information about the dynamics of the surface and bulk structure of ceria upon NOₓ exposure at 30 °C besides the identification of nitrite and nitrate adsorbates. In particular, Raman spectra provide direct evidence of the involvement of Ce-O surface sites so far not accessible by spectroscopic methods. These Ce-O sites play a key role for NOₓ storage, as their amount strongly influences the NOₓ storage capacity. A reduction of ceria prior to NOₓ exposure resulted in a lower NOₓ storage capacity, as long as no strong oxidizing agent (e.g. NO₂) was present to form new Ce-O sites. In the case of NO storage at 30 °C, new reaction pathways are postulated that describe the activation of gas-phase oxygen for ionic nitrite transformation and formation of new NOₓ adsorption sites. However, it is shown that the activated oxygen species is not a peroxide, as no correlation was found between the peroxides and formed nitrate and nitrite species. Based on our results, a mechanism for NO and NO₂ storage in ceria was formulated.

Freie Schlagworte: Ceria, NOx storage mechanism, In situ Raman, Defects, NOx adsorber
Sachgruppe der Dewey Dezimalklassifikatin (DDC): 500 Naturwissenschaften und Mathematik > 540 Chemie
Fachbereich(e)/-gebiet(e): 07 Fachbereich Chemie
07 Fachbereich Chemie > Eduard Zintl-Institut
07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie
Hinterlegungsdatum: 12 Dez 2024 11:50
Letzte Änderung: 12 Dez 2024 11:56
PPN: 524554374
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