Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics

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

Research output: Contribution to journalArticle

Abstract

The methylcyclohexane (MCH)-toluene cycle is a promising liquid organic hydride system as a hydrogen carrier. Generally, MCH dehydrogenation has been conducted over Pt-supported catalysts, for which it requires temperatures higher than 623 K because of its endothermic nature. For this study, an electric field was applied to Pt/TiO2 catalyst to promote MCH dehydrogenation at low temperatures. Selective dehydrogenation was achieved with the electric field application exceeding thermodynamic equilibrium, even at 423 K. With the electric field, "inverse" kinetic isotope effect (KIE) was observed by accelerated proton collision with MCH on the Pt/TiO2 catalyst. Moreover, Pt/TiO2 catalyst showed no methane by-production and less coke formation during MCH dehydrogenation. DRIFTS and XPS measurements revealed that electron donation from TiO2 to Pt weakened the interaction between catalyst surface and π-coordination of toluene. Results show that the electric field facilitated MCH dehydrogenation without methane and coke by-production over Pt/TiO2 catalyst.

Original languageEnglish
Pages (from-to)27743-27748
Number of pages6
JournalRSC Advances
Volume9
Issue number48
DOIs
Publication statusPublished - 2019 Jan 1

Fingerprint

Dehydrogenation
Catalysts
Electric fields
Coke
Methane
Toluene
Temperature
Catalyst supports
Hydrides
Isotopes
Protons
X ray photoelectron spectroscopy
methylcyclohexane
Thermodynamics
Hydrogen
Kinetics
Electrons
Liquids

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Cite this

Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics. / Takise, Kent; Sato, Ayaka; Ogo, Shuhei; Seo, Jeong Gil; Imagawa, Ken Ichi; Kado, Shigeru; Sekine, Yasushi.

In: RSC Advances, Vol. 9, No. 48, 01.01.2019, p. 27743-27748.

Research output: Contribution to journalArticle

Takise, Kent ; Sato, Ayaka ; Ogo, Shuhei ; Seo, Jeong Gil ; Imagawa, Ken Ichi ; Kado, Shigeru ; Sekine, Yasushi. / Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics. In: RSC Advances. 2019 ; Vol. 9, No. 48. pp. 27743-27748.
@article{2ff00cec1f2048deb912c1589b890998,
title = "Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics",
abstract = "The methylcyclohexane (MCH)-toluene cycle is a promising liquid organic hydride system as a hydrogen carrier. Generally, MCH dehydrogenation has been conducted over Pt-supported catalysts, for which it requires temperatures higher than 623 K because of its endothermic nature. For this study, an electric field was applied to Pt/TiO2 catalyst to promote MCH dehydrogenation at low temperatures. Selective dehydrogenation was achieved with the electric field application exceeding thermodynamic equilibrium, even at 423 K. With the electric field, {"}inverse{"} kinetic isotope effect (KIE) was observed by accelerated proton collision with MCH on the Pt/TiO2 catalyst. Moreover, Pt/TiO2 catalyst showed no methane by-production and less coke formation during MCH dehydrogenation. DRIFTS and XPS measurements revealed that electron donation from TiO2 to Pt weakened the interaction between catalyst surface and π-coordination of toluene. Results show that the electric field facilitated MCH dehydrogenation without methane and coke by-production over Pt/TiO2 catalyst.",
author = "Kent Takise and Ayaka Sato and Shuhei Ogo and Seo, {Jeong Gil} and Imagawa, {Ken Ichi} and Shigeru Kado and Yasushi Sekine",
year = "2019",
month = "1",
day = "1",
doi = "10.1039/c9ra06042a",
language = "English",
volume = "9",
pages = "27743--27748",
journal = "RSC Advances",
issn = "2046-2069",
publisher = "Royal Society of Chemistry",
number = "48",

}

TY - JOUR

T1 - Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics

AU - Takise, Kent

AU - Sato, Ayaka

AU - Ogo, Shuhei

AU - Seo, Jeong Gil

AU - Imagawa, Ken Ichi

AU - Kado, Shigeru

AU - Sekine, Yasushi

PY - 2019/1/1

Y1 - 2019/1/1

N2 - The methylcyclohexane (MCH)-toluene cycle is a promising liquid organic hydride system as a hydrogen carrier. Generally, MCH dehydrogenation has been conducted over Pt-supported catalysts, for which it requires temperatures higher than 623 K because of its endothermic nature. For this study, an electric field was applied to Pt/TiO2 catalyst to promote MCH dehydrogenation at low temperatures. Selective dehydrogenation was achieved with the electric field application exceeding thermodynamic equilibrium, even at 423 K. With the electric field, "inverse" kinetic isotope effect (KIE) was observed by accelerated proton collision with MCH on the Pt/TiO2 catalyst. Moreover, Pt/TiO2 catalyst showed no methane by-production and less coke formation during MCH dehydrogenation. DRIFTS and XPS measurements revealed that electron donation from TiO2 to Pt weakened the interaction between catalyst surface and π-coordination of toluene. Results show that the electric field facilitated MCH dehydrogenation without methane and coke by-production over Pt/TiO2 catalyst.

AB - The methylcyclohexane (MCH)-toluene cycle is a promising liquid organic hydride system as a hydrogen carrier. Generally, MCH dehydrogenation has been conducted over Pt-supported catalysts, for which it requires temperatures higher than 623 K because of its endothermic nature. For this study, an electric field was applied to Pt/TiO2 catalyst to promote MCH dehydrogenation at low temperatures. Selective dehydrogenation was achieved with the electric field application exceeding thermodynamic equilibrium, even at 423 K. With the electric field, "inverse" kinetic isotope effect (KIE) was observed by accelerated proton collision with MCH on the Pt/TiO2 catalyst. Moreover, Pt/TiO2 catalyst showed no methane by-production and less coke formation during MCH dehydrogenation. DRIFTS and XPS measurements revealed that electron donation from TiO2 to Pt weakened the interaction between catalyst surface and π-coordination of toluene. Results show that the electric field facilitated MCH dehydrogenation without methane and coke by-production over Pt/TiO2 catalyst.

UR - http://www.scopus.com/inward/record.url?scp=85072321970&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85072321970&partnerID=8YFLogxK

U2 - 10.1039/c9ra06042a

DO - 10.1039/c9ra06042a

M3 - Article

VL - 9

SP - 27743

EP - 27748

JO - RSC Advances

JF - RSC Advances

SN - 2046-2069

IS - 48

ER -