000165753 001__ 165753
000165753 005__ 20260113234335.0
000165753 0247_ $$2doi$$a10.1021/acsami.5c11895
000165753 0248_ $$2sideral$$a147368
000165753 037__ $$aART-2025-147368
000165753 041__ $$aeng
000165753 100__ $$aMollar-Cuni, Andrés
000165753 245__ $$aMechanistic Insights in Acceptorless Dehydrogenation of N-Heterocycles Using Graphenes as Carbocatalysts
000165753 260__ $$c2025
000165753 5060_ $$aAccess copy available to the general public$$fUnrestricted
000165753 5203_ $$aCatalytic 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 N-heterocycles 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.
000165753 536__ $$9info:eu-repo/grantAgreement/ES/AEI/PID2021-126071OB-C21$$9info:eu-repo/grantAgreement/ES/AEI/PID2021-126071OB-C22$$9info:eu-repo/grantAgreement/ES/AEI/PID2022-141433OB-I00$$9info:eu-repo/grantAgreement/ES/DGA/E31-23R
000165753 540__ $$9info:eu-repo/semantics/openAccess$$aby$$uhttps://creativecommons.org/licenses/by/4.0/deed.es
000165753 655_4 $$ainfo:eu-repo/semantics/article$$vinfo:eu-repo/semantics/publishedVersion
000165753 700__ $$aGarcía-Aznar, Pablo
000165753 700__ $$0(orcid)0000-0001-9193-3874$$aMartín, Santiago$$uUniversidad de Zaragoza
000165753 700__ $$aSastre, German
000165753 700__ $$aGarcía, Hermenegildo
000165753 700__ $$aMata, Jose A.
000165753 7102_ $$12012$$2755$$aUniversidad de Zaragoza$$bDpto. Química Física$$cÁrea Química Física
000165753 773__ $$g17, 51 (2025), 69234-69244$$pACS appl. mater. interfaces$$tACS applied materials & interfaces$$x1944-8244
000165753 8564_ $$s5123269$$uhttps://zaguan.unizar.es/record/165753/files/texto_completo.pdf$$yVersión publicada
000165753 8564_ $$s3295394$$uhttps://zaguan.unizar.es/record/165753/files/texto_completo.jpg?subformat=icon$$xicon$$yVersión publicada
000165753 909CO $$ooai:zaguan.unizar.es:165753$$particulos$$pdriver
000165753 951__ $$a2026-01-13-22:07:37
000165753 980__ $$aARTICLE