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*

*この研究の対応する著者

研究成果: Article査読

抄録

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.

本文言語English
ページ(範囲)11411-11418
ページ数8
ジャーナルJournal of Physical Chemistry C
125
21
DOI
出版ステータスPublished - 2021 6 3

ASJC Scopus subject areas

  • 電子材料、光学材料、および磁性材料
  • エネルギー(全般)
  • 物理化学および理論化学
  • 表面、皮膜および薄膜

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