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MIL-101(Cr)-NO2 as efficient catalyst for the aerobic oxidation of thiophenols and the oxidative desulfurization of dibenzothiophenes

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MIL-101(Cr)-NO2 as efficient catalyst for the aerobic oxidation of thiophenols and the oxidative desulfurization of dibenzothiophenes

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dc.contributor.author Vallés-García, Cristina es_ES
dc.contributor.author Santiago-Portillo, Andrea es_ES
dc.contributor.author Alvaro Rodríguez, Maria Mercedes es_ES
dc.contributor.author Navalón Oltra, Sergio es_ES
dc.contributor.author García Gómez, Hermenegildo es_ES
dc.date.accessioned 2021-03-25T04:31:47Z
dc.date.available 2021-03-25T04:31:47Z
dc.date.issued 2020-01-25 es_ES
dc.identifier.issn 0926-860X es_ES
dc.identifier.uri http://hdl.handle.net/10251/164221
dc.description.abstract [EN] A series of MIL-101(Cr)-X functionalized with electron withdrawing (NO2, SO3H or Cl) or electron donor (NH2 or CH3) groups has been tested for the solvent-free oxidative coupling of thiophenol to disulfides. No byproducts were observed. A relationship between the catalytic activity of these MOFs with the substituent meta Hammet constant on the terephthalate ligand and with their redox potential was found, MIL-101(Cr)-NO2 being the most active catalyst. NO2-substituted MIL-101 is also more efficient than the parent MIL-101(Cr) to promote the aerobic desulfurization of dibenzothiophenes in n-dodecane or commercial Diesel as solvent. No byproduct formation was observed. Mechanistic studies reveal that MIL-101(Cr)-NO2 is acting as heterogeneous catalyst in thiophenol oxidation and as radical initiator for the aerobic desulfurization. For both reactions, the catalyst can be reused without deactivation, maintaining its crystallinity and with negligible metal leaching. es_ES
dc.description.sponsorship 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 Adjudicacion de Ayudas a la Investigacion en Ciencias de la Vida y de la Materia, 2016), Ministerio de Ciencia, Innovacion y Universidades CTQ-2018 RTI2018-099482-A-I00 project and Generalitat Valenciana grupos de investigacion consolidables 2019 (AICO2019/214 project). es_ES
dc.language Inglés es_ES
dc.publisher Elsevier es_ES
dc.relation.ispartof Applied Catalysis A General es_ES
dc.rights Reconocimiento - No comercial - Sin obra derivada (by-nc-nd) es_ES
dc.subject Heterogeneous catalysis es_ES
dc.subject MIL-101(Cr)-NO(2)as catalyst es_ES
dc.subject Aerobic oxidations es_ES
dc.subject Thiophenol coupling es_ES
dc.subject Fuel es_ES
dc.subject Desulfurization es_ES
dc.subject.classification QUIMICA ORGANICA es_ES
dc.subject.classification QUIMICA ANALITICA es_ES
dc.title MIL-101(Cr)-NO2 as efficient catalyst for the aerobic oxidation of thiophenols and the oxidative desulfurization of dibenzothiophenes es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1016/j.apcata.2019.117340 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/GVA//PROMETEO%2F2017%2F083/ es_ES
dc.relation.projectID 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/ es_ES
dc.relation.projectID 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/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/GVA//AICO%2F2019%2F214/ es_ES
dc.rights.accessRights Abierto es_ES
dc.contributor.affiliation Universitat Politècnica de València. Departamento de Química - Departament de Química es_ES
dc.description.bibliographicCitation Vallés-García, C.; Santiago-Portillo, A.; Alvaro Rodríguez, MM.; Navalón Oltra, S.; García Gómez, H. (2020). MIL-101(Cr)-NO2 as efficient catalyst for the aerobic oxidation of thiophenols and the oxidative desulfurization of dibenzothiophenes. Applied Catalysis A General. 590:1-8. https://doi.org/10.1016/j.apcata.2019.117340 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1016/j.apcata.2019.117340 es_ES
dc.description.upvformatpinicio 1 es_ES
dc.description.upvformatpfin 8 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 590 es_ES
dc.relation.pasarela S\405837 es_ES
dc.contributor.funder Generalitat Valenciana es_ES
dc.contributor.funder Fundación Ramón Areces es_ES
dc.contributor.funder Agencia Estatal de Investigación es_ES
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