Co-CeO2Interaction Induces the Mars-van Krevelen Mechanism in Dehydrogenation of Ethane

Yukiko Hosono, Hikaru Saito, Takuma Higo, Kosuke Watanabe, Kazuharu Ito, Hideaki Tsuneki, Shun Maeda, Kunihide Hashimoto, Yasushi Sekine

Research output: Contribution to journalArticlepeer-review

Abstract

Introducing a catalyst for dehydrogenation of ethane (EDH) for steam cracking represents a promising solution with high feasibility to realize efficient ethylene production. We investigated EDH over transition-metal-doped CeO2 catalysts at 873 K in the presence of steam. Ce0.8Co0.2O2 exhibited high EDH activity and selectivity to ethylene (ca. 95%). In the absence of H2O, the catalytic activity dropped rapidly, indicating the promotive effect of H2O on ethylene formation. Catalytic experiments with water isotopes (D2O and H218O) demonstrated that EDH over Ce0.8Co0.2O2 proceeds through the Mars-van Krevelen (MvK) mechanism in which the reactive lattice oxygen in Ce0.8Co0.2O2 contributes to EDH. The consumed lattice oxygen was subsequently regenerated with H2O. X-ray diffraction and in situ X-ray absorption fine structure spectroscopy revealed that cobalt species were mainly present as CoO under EDH conditions and that redox between Co2+ and Co0 proceeded concomitantly with EDH. In contrast with Ce0.8Co0.2O2, no contribution of the lattice oxygen of CoO to EDH was verified in the case of CoO supported on α-Al2O3, which exhibited lower activity than Ce0.8Co0.2O2. Therefore, Co-CeO2 interactions are expected to play a crucially important role in controlling the characteristics of the reactive lattice oxygen suitable for EDH via the MvK mechanism.

Original languageEnglish
Pages (from-to)11411-11418
Number of pages8
JournalJournal of Physical Chemistry C
Volume125
Issue number21
DOIs
Publication statusPublished - 2021 Jun 3

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Fingerprint

Dive into the research topics of 'Co-CeO<sub>2</sub>Interaction Induces the Mars-van Krevelen Mechanism in Dehydrogenation of Ethane'. Together they form a unique fingerprint.

Cite this