Isotopic studies on the degradation of acetaldehyde on anatase surfaces

Research output: Contribution to journal › Article › Research › peer review

Authors

  • S. Melchers
  • J. Schneider
  • D.W. Bahnemann

Research Organisations

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Details

Original languageEnglish
Pages (from-to)318-322
Number of pages5
JournalCatalysis today
Volume340
Early online date21 Oct 2018
Publication statusPublished - 15 Jan 2020

Abstract

Herein, we studied the role of bridging oxygen (O br 2−) in the photocatalytic degradation reaction of gaseous acetaldehyde under anaerobic conditions. Ti 16O 2 and the isotopologues Ti 18O 2 were treated with acetaldehyde in the dark and upon UV illumination and at the reactor outlet the evolved C 16O 2 and C 18O 16O were monitored by mass spectrometry (MS). Ti 16O 2 exhibited a constant C 18O 16O/C 16O 2 ratio in the dark and upon UV illumination. In the dark the C 18O 16O/C 16O 2 ratio obtained with Ti 18O 2 was similar to the ratio monitored with Ti 16O 2, while upon UV illumination the ratio increased evincing an incorporation of O br 2− into the formation of CO 2. Accordingly, a following reaction mechanism could be derived: upon UV illumination the generated holes are trapped by the bridging oxygens forming O br [rad]− , which then react with adsorbed acetaldehyde forming acetate that is decomposed into CO 2 and CH 4. The remaining oxygen vacancy is replenished by an oxygen atom supplied by adsorbed water. This is, to the best of our knowledge, the first time that the crucial role of O br 2− within the photocatalytic process has been described for a gas phase reaction.

Keywords

    Acetaldehyde, Degradation mechanism, Lattice oxygen, Photocatalysis, TiO

ASJC Scopus subject areas

Cite this

Isotopic studies on the degradation of acetaldehyde on anatase surfaces. / Melchers, S.; Schneider, J.; Bahnemann, D.W.
In: Catalysis today, Vol. 340, 15.01.2020, p. 318-322.

Research output: Contribution to journal › Article › Research › peer review

Melchers S, Schneider J, Bahnemann DW. Isotopic studies on the degradation of acetaldehyde on anatase surfaces. Catalysis today. 2020 Jan 15;340:318-322. Epub 2018 Oct 21. doi: 10.1016/j.cattod.2018.10.016
Melchers, S. ; Schneider, J. ; Bahnemann, D.W. / Isotopic studies on the degradation of acetaldehyde on anatase surfaces. In: Catalysis today. 2020 ; Vol. 340. pp. 318-322.
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abstract = "Herein, we studied the role of bridging oxygen (O br 2−) in the photocatalytic degradation reaction of gaseous acetaldehyde under anaerobic conditions. Ti 16O 2 and the isotopologues Ti 18O 2 were treated with acetaldehyde in the dark and upon UV illumination and at the reactor outlet the evolved C 16O 2 and C 18O 16O were monitored by mass spectrometry (MS). Ti 16O 2 exhibited a constant C 18O 16O/C 16O 2 ratio in the dark and upon UV illumination. In the dark the C 18O 16O/C 16O 2 ratio obtained with Ti 18O 2 was similar to the ratio monitored with Ti 16O 2, while upon UV illumination the ratio increased evincing an incorporation of O br 2− into the formation of CO 2. Accordingly, a following reaction mechanism could be derived: upon UV illumination the generated holes are trapped by the bridging oxygens forming O br [rad]− , which then react with adsorbed acetaldehyde forming acetate that is decomposed into CO 2 and CH 4. The remaining oxygen vacancy is replenished by an oxygen atom supplied by adsorbed water. This is, to the best of our knowledge, the first time that the crucial role of O br 2− within the photocatalytic process has been described for a gas phase reaction. ",
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AU - Schneider, J.

AU - Bahnemann, D.W.

N1 - Funding information: This work was funded by the German Federal Ministry of Education and Research (contract no. 13N13350, PureBau – Untersuchung von Werkstoffsystemen für photokatalytisch hocheffiziente Baustoffe- Teilvorhaben: Oberflächenchemie der Photokatalysatoren und der Werkstoffe). The authors wish to thank Juan F. Montoya for the synthesis of Ti 18 O 2 and Luis Granone for the Raman and XRD analysis.

PY - 2020/1/15

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N2 - Herein, we studied the role of bridging oxygen (O br 2−) in the photocatalytic degradation reaction of gaseous acetaldehyde under anaerobic conditions. Ti 16O 2 and the isotopologues Ti 18O 2 were treated with acetaldehyde in the dark and upon UV illumination and at the reactor outlet the evolved C 16O 2 and C 18O 16O were monitored by mass spectrometry (MS). Ti 16O 2 exhibited a constant C 18O 16O/C 16O 2 ratio in the dark and upon UV illumination. In the dark the C 18O 16O/C 16O 2 ratio obtained with Ti 18O 2 was similar to the ratio monitored with Ti 16O 2, while upon UV illumination the ratio increased evincing an incorporation of O br 2− into the formation of CO 2. Accordingly, a following reaction mechanism could be derived: upon UV illumination the generated holes are trapped by the bridging oxygens forming O br [rad]− , which then react with adsorbed acetaldehyde forming acetate that is decomposed into CO 2 and CH 4. The remaining oxygen vacancy is replenished by an oxygen atom supplied by adsorbed water. This is, to the best of our knowledge, the first time that the crucial role of O br 2− within the photocatalytic process has been described for a gas phase reaction.

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