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Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions

dc.contributor.authorRibeiro, Rui
dc.contributor.authorSilva, Adrián
dc.contributor.authorPastrana-Martínez, Luisa
dc.contributor.authorFigueiredo, José
dc.contributor.authorFaria, Joaquim
dc.contributor.authorGomes, Helder
dc.date.accessioned2015-06-19T09:40:47Z
dc.date.available2015-06-19T09:40:47Z
dc.date.issued2015
dc.description.abstractReduced graphene oxide (rGO) samples were prepared from graphene oxide (GO) using different reducing agents (i.e., glucose, hydrazine and vitamin C, resulting in rGOG, rGOH and rGOV, respectively). These samples were tested in the catalytic wet peroxide oxidation (CWPO) of highly concentrated 4-nitrophenol(4-NP) solutions (5 g L−1) at mild operating conditions (i.e., atmospheric pressure, T = 323 K, pH = 3,[catalyst] = 2.5 g L−1and [H2O2]0= 17.8 g L−1). The highest catalytic activity was found for the rGOV sample, reaching a 4-NP removal of 1294 mg g−1and a TOC removal of 241 mg g−1after 24 h runs (corresponding to 4-NP and TOC removals of 65% and 23%, respectively). The TOC removal per unit of H2O2decomposed decreases with the increase of the surface oxygen content of the samples, as well as with the increase of their amounts of structural defects. This was ascribed, respectively, to the electron withdrawal capacity of oxygen-containing functionalities and to reduced adsorption of 4-NP in the samples with higher amounts of defects, which diminish the efficiency of the reaction between hydroxyl radicals resulting from the decomposition of H2O2and the organic compounds.In a series of three consecutive CWPO runs, rGOH was the most stable material (4-NP removal slightly decreasing from 980 mg g−1, in the first and second runs, to 841 mg g−1in the third run, corresponding to4-NP removals of 49% and 42%, respectively). The development of oxygen functionalities at the surface of the rGO samples during the CWPO runs was found to be the major cause of catalyst deactivation.4-Nitrocatechol was the main aromatic intermediate detected in the CWPO of 4-NP. Hydroquinone, benzoquinone, catechol and several low molecular weight carboxylic acids (e.g., malonic, malic, maleic and acetic acids) were also identified as reaction intermediates.To the best of our knowledge, graphene-based materials are reported for the first time as active and stable catalysts in the CWPO process, even when applied to highly polluted waters at mild conditions.por
dc.identifier.citationRibeiro R.S.; Silva A.M.T.; Pastrana-Martínez L.M.; Figueiredo J.L.; Faria J.L.; Gomes Helder (2015). Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions. Catalysis Today. ISSN 0920-5861. 249, p. 204-212por
dc.identifier.doi10.1016/j.cattod.2014.10.004
dc.identifier.issn0920-5861
dc.identifier.urihttp://hdl.handle.net/10198/11878
dc.language.isoengpor
dc.peerreviewedyespor
dc.publisherElsevierpor
dc.subjectGraphene-based materialspor
dc.subjectReduced graphene oxidepor
dc.subjectCatalytic wet peroxide oxidation (CWPO)por
dc.subjectHighly polluted waterspor
dc.subject4-Nitrophenolpor
dc.titleGraphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutionspor
dc.typejournal article
dspace.entity.typePublication
oaire.citation.endPage212por
oaire.citation.startPage204por
oaire.citation.titleCatalysis Todaypor
oaire.citation.volume249por
person.familyNameGomes
person.givenNameHelder
person.identifier.ciencia-id6218-1E19-13EE
person.identifier.orcid0000-0001-6898-2408
rcaap.rightsrestrictedAccesspor
rcaap.typearticlepor
relation.isAuthorOfPublication0eb96337-224a-4339-9918-334436fbbb99
relation.isAuthorOfPublication.latestForDiscovery0eb96337-224a-4339-9918-334436fbbb99

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