An Aza-Fused π-Conjugated Microporous Framework Catalyzes the Production of Hydrogen Peroxide

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Show simple item record Briega-Martos, V. Ferre-Vilaplana, A. De La Penìa, A. Segura, J. L. Zamora, F. Feliu, J. M. Herrero, E.
dc.contributor.other UAM. Departamento de Química Inorgánica es_ES
dc.contributor.other UAM. Departamento de Química Orgánica es_ES 2019-10-21T10:36:57Z 2019-10-21T10:36:57Z 2017-02-03
dc.identifier.citation ACS Catalysis 7.2 (2017): 1015-1024 en_US
dc.identifier.issn 2155-5435 es_ES
dc.description This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see en_US
dc.description.abstract In order to produce hydrogen peroxide in small-scale electrochemical plants, selective catalysts for the oxygen reduction reaction (ORR) toward the desired species are required. Here, we report about the synthesis, characterization, ORR electrochemical behavior, and reaction mechanism of an aza-fused π-conjugated microporous polymer, which presents high selectivity toward hydrogen peroxide. It was synthesized by polycondensation of 1,2,4,5-benzenetetramine tetrahydrochloride and triquinoyl octahydrate. A cobalt-modified version of the material was also prepared by a simple postsynthesis treatment with a Co(II) salt. The characterization of the material is consistent with the formation of a conductive robust porous covalent laminar polyaza structure. The ORR properties of these catalysts were investigated using rotating disk and rotating disk-ring arrangements. The results indicate that hydrogen peroxide is almost exclusively produced at very low overpotentials on these materials. Density functional theory calculations provide key elements to understand the reaction mechanism. It is found that, at the relevant potential for the reaction, half of the nitrogen atoms of the material would be hydrogenated. This hydrogenation process would destabilize some carbon atoms in the lattice and would provide segregated charge. On the destabilized carbon atoms, molecular oxygen would be chemisorbed with the aid of charge transferred from the hydrogenated nitrogen atoms and solvation effects. Due to the low destabilization of the carbon sites, the resulting molecular oxygen chemisorbed state, which would have the characteristics of a superoxide species, would be only slightly stable, promoting the formation of hydrogen peroxide en_US
dc.description.sponsorship This work has been financially supported by the MCINNFEDER (projects CTQ 2016-76221-P, MAT2013-46753-C2-1-P, and MAT2014-52305-P) and Generalitat Valenciana (project PROMETEO/2014/013) en_US
dc.format.extent 11 pag. en_US
dc.format.mimetype application/pdf en
dc.language.iso eng en
dc.publisher American Chemical Society en_US
dc.relation.ispartof ACS Catalysis es_ES
dc.rights © 2016 American Chemical Society en_US
dc.subject.other Conjugated covalent porous polymer en_US
dc.subject.other Electrocatalyst en_US
dc.subject.other Hydrogen peroxide production en_US
dc.subject.other Microporous framework en_US
dc.subject.other Oxygen reduction en_US
dc.title An Aza-Fused π-Conjugated Microporous Framework Catalyzes the Production of Hydrogen Peroxide en_US
dc.type article en
dc.subject.eciencia Química es_ES 2018-02-03
dc.relation.publisherversion es_ES
dc.identifier.doi 10.1021/acscatal.6b03043 es_ES
dc.identifier.publicationfirstpage 1015 es_ES
dc.identifier.publicationissue 2 es_ES
dc.identifier.publicationlastpage 1024 es_ES
dc.identifier.publicationvolume 7 es_ES
dc.relation.projectID Gobierno de España. CTQ 2016-76221-P es_ES
dc.relation.projectID Gobierno de España. MAT2013-46753-C2-1-P es_ES
dc.relation.projectID Gobierno de España. MAT2014-52305-P es_ES
dc.type.version info:eu-repo/semantics/acceptedVersion en
dc.rights.accessRights openAccess en
dc.authorUAM Zamora Abanades, Félix Juan (258846)

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