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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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Detalles Bibliográficos
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
Descripción
Sumario: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.