Novel oxidation reaction at ambient temperature and atmospheric pressure with electric discharge and oxide surface

Yasushi Sekine, Shinjiro Asai, Shigeru Kado, Masahiko Matsukata, Eiichi Kikuchi

Research output: Contribution to journalArticlepeer-review

9 Citations (Scopus)

Abstract

We investigated a novel oxidation reaction with surface-oxygen and lattice-oxygen induced using a non-equilibrium electric discharge at ambient temperature. We employed MgO, ZrO2, and TiO2 for this novel reaction. Methane was oxidized easily and converted into H2, CO, and CO2 by the surface-oxygen and lattice-oxygen of oxide with activation of discharge at ambient temperature without gas-phase oxygen. The oxide itself was stable after the reaction. Among these oxides, the tetragonal phase and amorphous phase of ZrO2 showed remarkably high activity for methane oxidation. Consequently, up to 8% of surface and lattice oxygen of the oxide was consumed by methane oxidation induced by electric discharge. The non-equilibrium electric discharge activated both the surface-oxygen and the lattice-oxygen of the oxides and methane molecules in the gas phase. After these reactions, the oxide surface vacant sites were recovered partially through steam post-treatment. Hydrogen formed simultaneously with steam decomposition. Other reactions were also studied by changing the reaction gas: methane into carbon monoxide, carbon monoxide with oxygen, and carbon monoxide with steam. Furthermore, the correlation of reactivity between the feed gas and surface oxygen was studied. Emission spectra under a CH4 atmosphere with electric discharge showed complex peaks caused by carbon monoxide formation at 280-500 nm at 0-4 min, suggesting that surface oxygen on oxides was probably consumed within 4 min from the start of the reaction.

Original languageEnglish
Pages (from-to)5056-5065
Number of pages10
JournalChemical Engineering Science
Volume63
Issue number20
DOIs
Publication statusPublished - 2008 Oct 1

Keywords

  • Electric discharge
  • Methane oxidation
  • Oxide surface
  • Reaction at ambient temperature

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Industrial and Manufacturing Engineering

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