Espinosa-López, JC.; Alvaro Rodríguez, MM.; Dhakshinamoorthy, A.; Navalón Oltra, S.; García Gómez, H. (2019). Engineering Active Sites in Reduced Graphene Oxide: Tuning the Catalytic Activity for Aerobic Oxidation. ACS Sustainable Chemistry & Engineering. 7(19):15948-15956. https://doi.org/10.1021/acssuschemeng.9b02237
Por favor, use este identificador para citar o enlazar este ítem: http://hdl.handle.net/10251/152255
Título:
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Engineering Active Sites in Reduced Graphene Oxide: Tuning the Catalytic Activity for Aerobic Oxidation
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Autor:
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Espinosa-López, Juan Carlos
Alvaro Rodríguez, Maria Mercedes
Dhakshinamoorthy, Amarajothi
Navalón Oltra, Sergio
García Gómez, Hermenegildo
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Entidad UPV:
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Universitat Politècnica de València. Departamento de Química - Departament de Química
Universitat Politècnica de València. Instituto de Tecnología Eléctrica - Institut de Tecnologia Elèctrica
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Fecha difusión:
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Resumen:
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[EN] The influence of the graphene oxide (GO) reduction method on the activity of the resulting reduced graphene oxide (rGO) for the aerobic oxidation of benzylamine is reported. Starting from GO obtained by the Hummers ...[+]
[EN] The influence of the graphene oxide (GO) reduction method on the activity of the resulting reduced graphene oxide (rGO) for the aerobic oxidation of benzylamine is reported. Starting from GO obtained by the Hummers method, a series of rGO samples were obtained either by chemical (hydroquinone (HQ), hydrazine (HZ) or ascorbic acid (ASC)) or by thermal reduction were prepared. Analytical and spectroscopic techniques provide evidence showing that chemical reducing agents reduce GO with different functional groups that influence the catalytic activity of the resulting rGO for the activation of molecular oxygen in benzylamine oxidation. The highest activity in the aerobic oxidation of benzylamine at 80 degrees C was found for the rGO-HQ1 sample prepared using HQ as a reducing agent. It is proposed that HQ introduces hydroquinone/p-benzoquinone-like moieties on the graphene sheet that act as active sites in the oxidation reaction. This proposal is supported by the activity of HQand/or p-benzoquinone as organocatalysts and by selective masking of oxygen-functional groups present in the most active rGO sample. The most active rGO sample exhibited good reusability and stability in five consecutive uses. Selective quenching experiments revealed that hydroperoxyl radicals are the primary reactive oxygen species generated in the system.
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Palabras clave:
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Carbocatalysis
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Reduced graphene oxide
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Graphene active sites
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Aerobic oxidation
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Benzylamine
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Derechos de uso:
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Reserva de todos los derechos
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Fuente:
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ACS Sustainable Chemistry & Engineering. (issn:
2168-0485
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DOI:
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10.1021/acssuschemeng.9b02237
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Editorial:
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American Chemical Society
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Versión del editor:
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https://doi.org/10.1021/acssuschemeng.9b02237
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Código del Proyecto:
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info:eu-repo/grantAgreement/DST//EMR%2F2016%2F006500/
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-098237-B-C21/ES/HETEROUNIONES DE GRAFENO CON CONFIGURACION CONTROLADA. SINTESIS Y APLICACIONES COMO SOPORTE EN CATALISIS Y EN ELECTRODOS/
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-099482-A-I00/ES/DESCOMPOSICION FOTOCATALITICA DEL AGUA ASISTIDA POR LUZ VISIBLE EMPLEANDO MATERIALES NOVEDOSOS Y MULTIFUNCIONALES UIO-66%2F67/
info:eu-repo/grantAgreement/GVA//PROMETEO%2F2017%2F083/
info:eu-repo/grantAgreement/GVA//AICO%2F2019%2F214/
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Descripción:
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"This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Sustainable Chemistry & Engineering, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acssuschemeng.9b02237."
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Agradecimientos:
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Financial support by the Spanish Ministry of Science and Innovation (Severo Ochoa and RTI2018-098237-CO21) and Generalitat Valenciana (Prometeo 2017/083) is gratefully acknowledged. S.N. thanks financial support by the ...[+]
Financial support by the Spanish Ministry of Science and Innovation (Severo Ochoa and RTI2018-098237-CO21) and Generalitat Valenciana (Prometeo 2017/083) is gratefully acknowledged. S.N. thanks financial support by the Fundacion RamOn Areces (XVIII Concurso Nacional para la Adjudication de Ayudas a la Investigation en Ciencias de la Vida y de la Materia, 2016) and Ministerio de Ciencia, Innovation y Universidades RTI2018-099482-A-I00 project and Generalitat Valenciana (grupos de investigation consolidables 2019, AICO/2019/214). A.D. thanks the University Grants Commission, New Delhi, for the award of an Assistant Professorship under its Faculty Recharge Programme. A.D. also thanks the Department of Science and Technology, India, for the financial support through Extramural Research Funding (EMR/2016/006500).
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Tipo:
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Artículo
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