Irreversible catalytic methylcyclohexane dehydrogenation by surface protonics at low temperature

Kent Takise, Ayaka Sato, Kota Murakami, Shuhei Ogo, Jeong Gil Seo, Ken Ichi Imagawa, Shigeru Kado, Yasushi Sekine

Research output: Contribution to journalArticle

Abstract

Liquid organic hydrides are regarded as promising for use as hydrogen carriers via the methylcyclohexane (MCH)-toluene-hydrogen cycle. Because of the endothermic nature of MCH dehydrogenation, the reaction is usually conducted at temperatures higher than 623 K. In this work, low-temperature catalytic MCH dehydrogenation was demonstrated over 3 wt% Pt/CeO 2 catalyst by application of electric field across a fixed-bed flow reactor. Results show that a high conversion of MCH beyond thermodynamic equilibrium was achieved even at 423 K. Kinetic analyses exhibited a positive correlation of hydrogen to the reaction rates and an "inverse" kinetic isotope effect (KIE), suggesting that accelerated proton hopping with the H atoms of MCH promotes the reaction. Operando analyses and DFT calculation proved that the reverse reaction (i.e. toluene hydrogenation) was suppressed by the facilitation of toluene desorption in the electric field. The electric field promoted MCH dehydrogenation by surface proton hopping, even at low temperatures with an irreversible pathway.

Original languageEnglish
Pages (from-to)5918-5924
Number of pages7
JournalRSC Advances
Volume9
Issue number11
DOIs
Publication statusPublished - 2019 Jan 1

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Dehydrogenation
Toluene
Hydrogen
Electric fields
Protons
Temperature
Kinetics
Discrete Fourier transforms
Hydrides
Hydrogenation
Reaction rates
Isotopes
Desorption
Thermodynamics
Atoms
Catalysts
methylcyclohexane
Liquids

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Cite this

Irreversible catalytic methylcyclohexane dehydrogenation by surface protonics at low temperature. / Takise, Kent; Sato, Ayaka; Murakami, Kota; Ogo, Shuhei; Seo, Jeong Gil; Imagawa, Ken Ichi; Kado, Shigeru; Sekine, Yasushi.

In: RSC Advances, Vol. 9, No. 11, 01.01.2019, p. 5918-5924.

Research output: Contribution to journalArticle

Takise, Kent ; Sato, Ayaka ; Murakami, Kota ; Ogo, Shuhei ; Seo, Jeong Gil ; Imagawa, Ken Ichi ; Kado, Shigeru ; Sekine, Yasushi. / Irreversible catalytic methylcyclohexane dehydrogenation by surface protonics at low temperature. In: RSC Advances. 2019 ; Vol. 9, No. 11. pp. 5918-5924.
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