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Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics

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 elec...

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Autores principales: Takise, Kent, Sato, Ayaka, Ogo, Shuhei, Seo, Jeong Gil, Imagawa, Ken-ichi, Kado, Shigeru, Sekine, Yasushi
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9070780/
https://www.ncbi.nlm.nih.gov/pubmed/35530488
http://dx.doi.org/10.1039/c9ra06042a
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author Takise, Kent
Sato, Ayaka
Ogo, Shuhei
Seo, Jeong Gil
Imagawa, Ken-ichi
Kado, Shigeru
Sekine, Yasushi
author_facet Takise, Kent
Sato, Ayaka
Ogo, Shuhei
Seo, Jeong Gil
Imagawa, Ken-ichi
Kado, Shigeru
Sekine, Yasushi
author_sort Takise, Kent
collection PubMed
description 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/TiO(2) 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/TiO(2) catalyst. Moreover, Pt/TiO(2) catalyst showed no methane by-production and less coke formation during MCH dehydrogenation. DRIFTS and XPS measurements revealed that electron donation from TiO(2) 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/TiO(2) catalyst.
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spelling pubmed-90707802022-05-06 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 RSC Adv Chemistry 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/TiO(2) 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/TiO(2) catalyst. Moreover, Pt/TiO(2) catalyst showed no methane by-production and less coke formation during MCH dehydrogenation. DRIFTS and XPS measurements revealed that electron donation from TiO(2) 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/TiO(2) catalyst. The Royal Society of Chemistry 2019-09-03 /pmc/articles/PMC9070780/ /pubmed/35530488 http://dx.doi.org/10.1039/c9ra06042a Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
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
title Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics
title_full Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics
title_fullStr Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics
title_full_unstemmed Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics
title_short Low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics
title_sort low-temperature selective catalytic dehydrogenation of methylcyclohexane by surface protonics
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9070780/
https://www.ncbi.nlm.nih.gov/pubmed/35530488
http://dx.doi.org/10.1039/c9ra06042a
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