Mechanistic Insights in Acceptorless Dehydrogenation of N-Heterocycles Using Graphenes as Carbocatalysts
[EN] Catalytic dehydrogenation is a critical transformation in the chemical and energy sectors, particularly for reversible hydrogen storage systems. One of the most promising systems for hydrogen storage is the development of liquid organic hydrogen carriers (LOHCs), which have the potential capaci...
| Autores: | , , , , , |
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| Tipo de recurso: | artículo |
| Fecha de publicación: | 2025 |
| País: | España |
| Institución: | Universitat Politècnica de València (UPV) |
| Repositorio: | RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia |
| Idioma: | inglés |
| OAI Identifier: | oai:riunet.upv.es:10251/233300 |
| Acceso en línea: | https://riunet.upv.es/handle/10251/233300 |
| Access Level: | acceso abierto |
| Palabra clave: | Carbocatalysis Acceptorless Dehydrogenation Graphene N-heterocycles Reaction Mechanism DFT 07.- Asegurar el acceso a energías asequibles, fiables, sostenibles y modernas para todos 08.- Fomentar el crecimiento económico sostenido, inclusivo y sostenible, el empleo pleno y productivo, y el trabajo decente para todos 09.- Desarrollar infraestructuras resilientes, promover la industrialización inclusiva y sostenible, y fomentar la innovación 12.- Garantizar las pautas de consumo y de producción sostenibles |
| Sumario: | [EN] Catalytic dehydrogenation is a critical transformation in the chemical and energy sectors, particularly for reversible hydrogen storage systems. One of the most promising systems for hydrogen storage is the development of liquid organic hydrogen carriers (LOHCs), which have the potential capacity of storing and releasing hydrogen gas on demand. Catalytic direct dehydrogenation represents a greener, promising method to generate hydrogen in situ from these hydrogen-dense carriers. The catalytic activity of graphene materials as metal-free carbocatalysts in the acceptorless dehydrogenation of Nheterocycles has been explored. Herein, a detailed mechanistic investigation has been conducted through both experimental (stoichiometric and masking experiments) and DFT calculations on the reaction mechanism. The proposed mechanism identifies o-quinone groups as the active sites responsible for catalysis, involving the transformation of o-quinone groups into epoxide intermediates, which release molecular hydrogen and regenerate the o-quinone groups, completing the catalytic cycle. This work provides insight into the design of efficient metal-free catalysts for their use in LOHCs storage systems, paving the way for sustainable energy solutions |
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