Photo-induced reactions in the CO2-methane system on titanate nanotubes modified with Au and Rh nanoparticles

L. Bugyi, Kornélia Baán, Erika Varga, A. Oszkó, A. Erdóhelyi, Z. Kónya, J. Kiss

Research output: Contribution to journalArticle

36 Citations (Scopus)

Abstract

The photocatalytic transformation of the methane-carbon dioxide system was investigated by in-situ methods in the present study. Titanate nanotube (TNT) supported gold and rhodium catalysts were used in the catalytic tests. Our main goal was the analysis of the role of the catalysts in the different parts of the reaction mechanism. The catalysts were characterized by X-ray photoelectron spectroscopy (XPS), high resolution transmission electron microscopy (HRTEM) and diffuse reflectance UV–vis spectroscopy (DR-UV–vis). Photocatalytic tests were performed in a continuous flow quartz reactor equipped with mass spectrometer detector and mercury-arc UV source. Diffuse reflectance infrared spectroscopy (DRIFTS) was used to analyze the surface of the catalyst during photoreaction. Post-catalytic tests were also carried out on the catalysts including XPS, temperature programmed reduction (TPR) and Raman spectroscopy methods in order to follow the changes of the materials. Titanate nanotube can stabilize even the smallest, molecular-like Au clusters which showed the highest activity in the reactions. Approximately 3% methane conversion was reached in the best cases while the carbon dioxide conversion was not traceable. It was revealed that water has a very important role in the oxidation reaction. The main discovered reaction routes are methane dehydrogenation and oxidation, the methyl coupling and the forming of structured carbon deposits on the catalyst surface. The source of the surplus CO can be mostly the reduction of carbon dioxide. During the reduction process photoelectrons and hydrogen ions brings about the CO2 reduction via CO2 radical anion.

Original languageEnglish
Pages (from-to)473-484
Number of pages12
JournalApplied Catalysis B: Environmental
Volume199
DOIs
Publication statusPublished - Dec 15 2016

    Fingerprint

Keywords

  • Carbon dioxide photocatalysis
  • Gold nanoclusters
  • Methane photocatalysis
  • Rhodium nanoparticles
  • Titanate nanotubes

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology
  • Environmental Science(all)

Cite this