Publicação
Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions
| Resumo: | Reduced 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. |
|---|---|
| Autores principais: | Ribeiro, Rui |
| Outros Autores: | Silva, Adrián; Pastrana-Martínez, Luisa; Figueiredo, José; Faria, Joaquim; Gomes, Helder |
| Assunto: | Graphene-based materials Reduced graphene oxide Catalytic wet peroxide oxidation (CWPO) Highly polluted waters 4-Nitrophenol |
| Ano: | 2015 |
| País: | Portugal |
| Tipo de documento: | artigo |
| Tipo de acesso: | acesso restrito |
| Instituição associada: | Instituto Politécnico de Bragança |
| Idioma: | inglês |
| Origem: | Biblioteca Digital do IPB |
| _version_ | 1863850704145219584 |
|---|---|
| author | Ribeiro, Rui |
| author2 | Silva, Adrián Pastrana-Martínez, Luisa Figueiredo, José Faria, Joaquim Gomes, Helder |
| author2_role | author author author author author |
| author_facet | Ribeiro, Rui Silva, Adrián Pastrana-Martínez, Luisa Figueiredo, José Faria, Joaquim Gomes, Helder |
| author_role | author |
| contributor_name_str_mv | Biblioteca Digital do IPB |
| country_str | PT |
| creators_json_str | [{\"Person.name\":\"Ribeiro, Rui\"},{\"Person.name\":\"Silva, Adrián\"},{\"Person.name\":\"Pastrana-Martínez, Luisa\"},{\"Person.name\":\"Figueiredo, José\"},{\"Person.name\":\"Faria, Joaquim\"},{\"Person.name\":\"Gomes, Helder\",\"Person.identifier.orcid\":\"0000-0001-6898-2408\"}] |
| datacite.contributors.contributor.contributorName.fl_str_mv | Biblioteca Digital do IPB |
| datacite.creators.creator.creatorName.fl_str_mv | Ribeiro, Rui Silva, Adrián Pastrana-Martínez, Luisa Figueiredo, José Faria, Joaquim Gomes, Helder |
| datacite.date.Accepted.fl_str_mv | 2015-01-01T00:00:00Z |
| datacite.date.available.fl_str_mv | 2015-06-19T09:40:47Z |
| datacite.date.embargoed.fl_str_mv | 2015-06-19T09:40:47Z |
| datacite.rights.fl_str_mv | http://purl.org/coar/access_right/c_16ec |
| datacite.subjects.subject.fl_str_mv | Graphene-based materials Reduced graphene oxide Catalytic wet peroxide oxidation (CWPO) Highly polluted waters 4-Nitrophenol |
| datacite.titles.title.fl_str_mv | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| dc.contributor.none.fl_str_mv | Biblioteca Digital do IPB |
| dc.creator.none.fl_str_mv | Ribeiro, Rui Silva, Adrián Pastrana-Martínez, Luisa Figueiredo, José Faria, Joaquim Gomes, Helder |
| dc.date.Accepted.fl_str_mv | 2015-01-01T00:00:00Z |
| dc.date.available.fl_str_mv | 2015-06-19T09:40:47Z |
| dc.date.embargoed.fl_str_mv | 2015-06-19T09:40:47Z |
| dc.format.none.fl_str_mv | application/pdf |
| dc.identifier.none.fl_str_mv | http://hdl.handle.net/10198/11878 |
| dc.language.none.fl_str_mv | eng |
| dc.publisher.none.fl_str_mv | Elsevier |
| dc.rights.none.fl_str_mv | http://purl.org/coar/access_right/c_16ec |
| dc.subject.none.fl_str_mv | Graphene-based materials Reduced graphene oxide Catalytic wet peroxide oxidation (CWPO) Highly polluted waters 4-Nitrophenol |
| dc.title.fl_str_mv | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| dc.type.none.fl_str_mv | http://purl.org/coar/resource_type/c_6501 |
| description | Reduced 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. |
| dirty | 0 |
| eu_rights_str_mv | restrictedAccess |
| format | article |
| fulltext.url.fl_str_mv | https://bibliotecadigital.ipb.pt/bitstreams/fed10d72-3f39-462c-81c3-d55bb8018785/download |
| id | ipb_6e3d3bc16d04decb570d752bcb2aa208 |
| identifier.url.fl_str_mv | http://hdl.handle.net/10198/11878 |
| instacron_str | ipb |
| institution | Instituto Politécnico de Bragança |
| instname_str | Instituto Politécnico de Bragança |
| language | eng |
| network_acronym_str | ipb |
| network_name_str | Biblioteca Digital do IPB |
| oai_identifier_str | oai:bibliotecadigital.ipb.pt:10198/11878 |
| organization_str_mv | urn:organizationAcronym:ipb |
| person_str_mv | Ribeiro, Rui Silva, Adrián Pastrana-Martínez, Luisa Figueiredo, José Faria, Joaquim Gomes, Helder Gomes, Helder https://www.ciencia-id.pt/6218-1E19-13EE 6218-1E19-13EE http://orcid.org/0000-0001-6898-2408 0000-0001-6898-2408 |
| publishDate | 2015 |
| publisher.none.fl_str_mv | Elsevier |
| reponame_str | Biblioteca Digital do IPB |
| repository_id_str | urn:repositoryAcronym:ipb |
| service_str_mv | urn:repositoryAcronym:ipb |
| spelling | engElsevierporReduced 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.application/pdfporGraphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutionsRibeiro, RuiSilva, AdriánPastrana-Martínez, LuisaFigueiredo, JoséFaria, JoaquimPersonalGomes, HelderDSpacehttp://dspace.org/items/0eb96337-224a-4339-9918-334436fbbb99DSpacehttp://dspace.org/items/0eb96337-224a-4339-9918-334436fbbb99GomesHelder T.Ciência IDhttps://www.ciencia-id.pt6218-1E19-13EEORCIDhttp://orcid.org0000-0001-6898-2408HostingInstitutionOrganizationalBiblioteca Digital do IPBe-mailmailto:dspace@ipb.ptdspace@ipb.ptISSNIsPartOf0920-5861DOIIsPartOf10.1016/j.cattod.2014.10.0042015-06-19T09:40:47Z20152015-01-01T00:00:00ZHandlehttp://hdl.handle.net/10198/11878http://purl.org/coar/access_right/c_16ecrestricted accessGraphene-based materialsReduced graphene oxideCatalytic wet peroxide oxidation (CWPO)Highly polluted waters4-Nitrophenol868710 bytesliteraturehttp://purl.org/coar/resource_type/c_6501journal articlehttp://purl.org/coar/access_right/c_16ecapplication/pdffulltexthttps://bibliotecadigital.ipb.pt/bitstreams/fed10d72-3f39-462c-81c3-d55bb8018785/downloadCatalysis Today249204212 |
| spellingShingle | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions Ribeiro, Rui Graphene-based materials Reduced graphene oxide Catalytic wet peroxide oxidation (CWPO) Highly polluted waters 4-Nitrophenol |
| subject.fl_str_mv | Graphene-based materials Reduced graphene oxide Catalytic wet peroxide oxidation (CWPO) Highly polluted waters 4-Nitrophenol |
| title | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| title_full | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| title_fullStr | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| title_full_unstemmed | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| title_short | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| title_sort | Graphene-based materials for the catalytic wet peroxide oxidation of highly concentrated 4-nitrophenol solutions |
| topic | Graphene-based materials Reduced graphene oxide Catalytic wet peroxide oxidation (CWPO) Highly polluted waters 4-Nitrophenol |
| topic_facet | Graphene-based materials Reduced graphene oxide Catalytic wet peroxide oxidation (CWPO) Highly polluted waters 4-Nitrophenol |
| url | http://hdl.handle.net/10198/11878 |
| visible | 1 |