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Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel

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Resumo:The treatment of dinitrophenol (DNP) and trinitrophenol (TNP), typically found in the effluents from the process of mononitrobenzene (MNB) synthesis, was investigated by wet air oxidation in both non-catalytic (WAO) and catalytic (CWAO) conditions, operating as two phase and three phase reactors, respectively. In the first case, the effect of treating DNP and TNP separately (single-component system) or using mixtures of these compounds (multi-component systems) was assessed by analysing the decrease of the individual pollutant concentration, the total organic carbon (TOC) evolution and the reaction by-products. Of the various systems screened, it was possible to conclude that the presence of DNP enhances the overall oxidation in multi-component systems. TNP is not oxidized individually but totally degraded in the presence of DNP. The observed reactivities were correlated with the number and type of functional groups attached to the aromatic ring and the HO induced denitration may be considered as the main reaction mechanism. Concerning the CWAO experiments, two catalysts were synthesized in this study, a carbon xerogel (CX) and a nanosized cerium oxide (CeO2), using sol–gel and solvothermal methodologies, respectively, and tested for the degradation of the multi-component system. The CX catalyst operating in slurry conditions was found to be highly active and led to practically complete removal of DNP and TNP, total bleaching of color and 83% mineralization after 120 min of reaction. The best catalyst was thoroughly characterized. An increase in the concentration of carboxylic acid groups at the catalyst surface was observed by TPD analysis of the catalyst after the reaction, followed by a decrease in the concentration of phenolic and quinone functional groups. The catalyst surface modification was a consequence of the large amounts of nitrates produced from the model compounds. Nitrites were not detected and, therefore, CWAO seems to be a potential treatment which can be coupled with a biological process to remove the nitrates formed during the reaction.
Autores principais:Apolinário, Ângela
Outros Autores:Silva, Adrián; Machado, Bruno; Gomes, Helder; Araújo, Paulo P.; Figueiredo, José; Faria, Joaquim
Assunto:Wet air oxidation (WAO); Dinitrophenol Trinitrophenol Carbon xerogel Cerium oxide
Ano:2008
País:Portugal
Tipo de documento:artigo
Tipo de acesso:acesso restrito
Instituição associada:Instituto Politécnico de Bragança
Idioma:inglês
Origem:Biblioteca Digital do IPB
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author Apolinário, Ângela
author2 Silva, Adrián
Machado, Bruno
Gomes, Helder
Araújo, Paulo P.
Figueiredo, José
Faria, Joaquim
author2_role author
author
author
author
author
author
author_facet Apolinário, Ângela
Silva, Adrián
Machado, Bruno
Gomes, Helder
Araújo, Paulo P.
Figueiredo, José
Faria, Joaquim
author_role author
contributor_name_str_mv Biblioteca Digital do IPB
country_str PT
creators_json_str [{\"Person.name\":\"Apolinário, Ângela\"},{\"Person.name\":\"Silva, Adrián\"},{\"Person.name\":\"Machado, Bruno\"},{\"Person.name\":\"Gomes, Helder\",\"Person.identifier.orcid\":\"0000-0001-6898-2408\"},{\"Person.name\":\"Araújo, Paulo P.\"},{\"Person.name\":\"Figueiredo, José\"},{\"Person.name\":\"Faria, Joaquim\"}]
datacite.contributors.contributor.contributorName.fl_str_mv Biblioteca Digital do IPB
datacite.creators.creator.creatorName.fl_str_mv Apolinário, Ângela
Silva, Adrián
Machado, Bruno
Gomes, Helder
Araújo, Paulo P.
Figueiredo, José
Faria, Joaquim
datacite.date.Accepted.fl_str_mv 2008-01-01T00:00:00Z
datacite.date.available.fl_str_mv 2009-03-30T14:50:32Z
datacite.date.embargoed.fl_str_mv 2009-03-30T14:50:32Z
datacite.rights.fl_str_mv http://purl.org/coar/access_right/c_16ec
datacite.subjects.subject.fl_str_mv Wet air oxidation (WAO);
Dinitrophenol
Trinitrophenol
Carbon xerogel
Cerium oxide
datacite.titles.title.fl_str_mv Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
dc.contributor.none.fl_str_mv Biblioteca Digital do IPB
dc.creator.none.fl_str_mv Apolinário, Ângela
Silva, Adrián
Machado, Bruno
Gomes, Helder
Araújo, Paulo P.
Figueiredo, José
Faria, Joaquim
dc.date.Accepted.fl_str_mv 2008-01-01T00:00:00Z
dc.date.available.fl_str_mv 2009-03-30T14:50:32Z
dc.date.embargoed.fl_str_mv 2009-03-30T14:50:32Z
dc.format.none.fl_str_mv application/pdf
dc.identifier.none.fl_str_mv http://hdl.handle.net/10198/1141
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 Wet air oxidation (WAO);
Dinitrophenol
Trinitrophenol
Carbon xerogel
Cerium oxide
dc.title.fl_str_mv Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
dc.type.none.fl_str_mv http://purl.org/coar/resource_type/c_6501
description The treatment of dinitrophenol (DNP) and trinitrophenol (TNP), typically found in the effluents from the process of mononitrobenzene (MNB) synthesis, was investigated by wet air oxidation in both non-catalytic (WAO) and catalytic (CWAO) conditions, operating as two phase and three phase reactors, respectively. In the first case, the effect of treating DNP and TNP separately (single-component system) or using mixtures of these compounds (multi-component systems) was assessed by analysing the decrease of the individual pollutant concentration, the total organic carbon (TOC) evolution and the reaction by-products. Of the various systems screened, it was possible to conclude that the presence of DNP enhances the overall oxidation in multi-component systems. TNP is not oxidized individually but totally degraded in the presence of DNP. The observed reactivities were correlated with the number and type of functional groups attached to the aromatic ring and the HO induced denitration may be considered as the main reaction mechanism. Concerning the CWAO experiments, two catalysts were synthesized in this study, a carbon xerogel (CX) and a nanosized cerium oxide (CeO2), using sol–gel and solvothermal methodologies, respectively, and tested for the degradation of the multi-component system. The CX catalyst operating in slurry conditions was found to be highly active and led to practically complete removal of DNP and TNP, total bleaching of color and 83% mineralization after 120 min of reaction. The best catalyst was thoroughly characterized. An increase in the concentration of carboxylic acid groups at the catalyst surface was observed by TPD analysis of the catalyst after the reaction, followed by a decrease in the concentration of phenolic and quinone functional groups. The catalyst surface modification was a consequence of the large amounts of nitrates produced from the model compounds. Nitrites were not detected and, therefore, CWAO seems to be a potential treatment which can be coupled with a biological process to remove the nitrates formed during the reaction.
dirty 0
eu_rights_str_mv restrictedAccess
format article
fulltext.url.fl_str_mv https://bibliotecadigital.ipb.pt/bitstreams/bf3138e0-c59b-4bc2-8cc6-ac890823afb0/download
id ipb_dee2137efa6746854e7d8cc61ea403af
identifier.url.fl_str_mv http://hdl.handle.net/10198/1141
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:10198/1141
organization_str_mv urn:organizationAcronym:ipb
person_str_mv Apolinário, Ângela
Silva, Adrián
Machado, Bruno
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
Araújo, Paulo P.
Figueiredo, José
Faria, Joaquim
publishDate 2008
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 engElsevierenThe treatment of dinitrophenol (DNP) and trinitrophenol (TNP), typically found in the effluents from the process of mononitrobenzene (MNB) synthesis, was investigated by wet air oxidation in both non-catalytic (WAO) and catalytic (CWAO) conditions, operating as two phase and three phase reactors, respectively. In the first case, the effect of treating DNP and TNP separately (single-component system) or using mixtures of these compounds (multi-component systems) was assessed by analysing the decrease of the individual pollutant concentration, the total organic carbon (TOC) evolution and the reaction by-products. Of the various systems screened, it was possible to conclude that the presence of DNP enhances the overall oxidation in multi-component systems. TNP is not oxidized individually but totally degraded in the presence of DNP. The observed reactivities were correlated with the number and type of functional groups attached to the aromatic ring and the HO induced denitration may be considered as the main reaction mechanism. Concerning the CWAO experiments, two catalysts were synthesized in this study, a carbon xerogel (CX) and a nanosized cerium oxide (CeO2), using sol–gel and solvothermal methodologies, respectively, and tested for the degradation of the multi-component system. The CX catalyst operating in slurry conditions was found to be highly active and led to practically complete removal of DNP and TNP, total bleaching of color and 83% mineralization after 120 min of reaction. The best catalyst was thoroughly characterized. An increase in the concentration of carboxylic acid groups at the catalyst surface was observed by TPD analysis of the catalyst after the reaction, followed by a decrease in the concentration of phenolic and quinone functional groups. The catalyst surface modification was a consequence of the large amounts of nitrates produced from the model compounds. Nitrites were not detected and, therefore, CWAO seems to be a potential treatment which can be coupled with a biological process to remove the nitrates formed during the reaction.application/pdfenWet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogelApolinário, ÂngelaSilva, AdriánMachado, BrunoPersonalGomes, 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.org0000-0001-6898-2408Araújo, Paulo P.Figueiredo, JoséFaria, JoaquimHostingInstitutionOrganizationalBiblioteca Digital do IPBe-mailmailto:dspace@ipb.ptdspace@ipb.ptISSNIsPartOf0926-3373DOIIsPartOf10.1016/j.apcatb.2007.12.0182009-03-30T14:50:32Z20082008-01-01T00:00:00ZHandlehttp://hdl.handle.net/10198/1141http://purl.org/coar/access_right/c_16ecrestricted accessWet air oxidation (WAO);DinitrophenolTrinitrophenolCarbon xerogelCerium oxide1397504 bytesliteraturehttp://purl.org/coar/resource_type/c_6501journal articlehttp://purl.org/coar/access_right/c_16ecapplication/pdffulltexthttps://bibliotecadigital.ipb.pt/bitstreams/bf3138e0-c59b-4bc2-8cc6-ac890823afb0/download
spellingShingle Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
Apolinário, Ângela
Wet air oxidation (WAO);
Dinitrophenol
Trinitrophenol
Carbon xerogel
Cerium oxide
subject.fl_str_mv Wet air oxidation (WAO);
Dinitrophenol
Trinitrophenol
Carbon xerogel
Cerium oxide
title Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
title_full Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
title_fullStr Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
title_full_unstemmed Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
title_short Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
title_sort Wet air oxidation of nitro-aromatic compounds: reactivity on single- and multi-component systems and surface chemistry studies with a carbon xerogel
topic Wet air oxidation (WAO);
Dinitrophenol
Trinitrophenol
Carbon xerogel
Cerium oxide
topic_facet Wet air oxidation (WAO);
Dinitrophenol
Trinitrophenol
Carbon xerogel
Cerium oxide
url http://hdl.handle.net/10198/1141
visible 1