Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process
Autor(a) principal: | |
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Data de Publicação: | 2018 |
Outros Autores: | , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10198/19953 |
Resumo: | The deposition of condensation by-products onto the catalyst surface upon wet peroxide and wet air oxidation processes has usually been associated with catalyst deactivation. However, in Part I of this paper, it was demonstrated that these carbonaceous deposits actually act as catalytic promoters in the oxygen-assisted wet peroxide oxidation (WPO-O2) of phenol. Herein, the intrinsic activity, nature and stability of these species have been investigated. To achieve this goal, an up-flow fixed bed reactor packed with porous Al2O3 spheres was used to facilitate the deposition of the condensation by-products formed in the liquid phase. It was demonstrated that the condensation by-products catalyzed the decomposition of H2O2 and a higher amount of these species leads to a higher degree of oxidation degree The reaction rates, conversion values and intermediates’ distribution were analyzed. The characterization of the carbonaceous deposits on the Al2O3 spheres showed a significant amount of condensation by-products (~6 wt.%) after 650 h of time on stream. They are of aromatic nature and present oxygen functional groups consisting of quinones, phenols, aldehydes, carboxylics and ketones. The initial phenol concentration and H2O2 dose were found to be crucial variables for the generation and consumption of such species, respectively |
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Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic processAutocatalytic kineticsCondensation by-productsFoulingWet air oxidationWet peroxide oxidationThe deposition of condensation by-products onto the catalyst surface upon wet peroxide and wet air oxidation processes has usually been associated with catalyst deactivation. However, in Part I of this paper, it was demonstrated that these carbonaceous deposits actually act as catalytic promoters in the oxygen-assisted wet peroxide oxidation (WPO-O2) of phenol. Herein, the intrinsic activity, nature and stability of these species have been investigated. To achieve this goal, an up-flow fixed bed reactor packed with porous Al2O3 spheres was used to facilitate the deposition of the condensation by-products formed in the liquid phase. It was demonstrated that the condensation by-products catalyzed the decomposition of H2O2 and a higher amount of these species leads to a higher degree of oxidation degree The reaction rates, conversion values and intermediates’ distribution were analyzed. The characterization of the carbonaceous deposits on the Al2O3 spheres showed a significant amount of condensation by-products (~6 wt.%) after 650 h of time on stream. They are of aromatic nature and present oxygen functional groups consisting of quinones, phenols, aldehydes, carboxylics and ketones. The initial phenol concentration and H2O2 dose were found to be crucial variables for the generation and consumption of such species, respectivelyThis research was supported by the Spanish MINECO through the project CTM-2016-76454-R and by the CM through the project P2018/EMT-4341. M. Munoz thanks the Spanish MINECO for the Ramón y Cajal postdoctoral contract (RYC-2016-20648).Biblioteca Digital do IPBQuintanilla, AsunciónDíaz de Tuesta, Jose LuisFigueruelo, CristinaMunoz, MacarenaCasas, Jose A.2018-01-19T10:00:00Z20192019-01-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10198/19953engQuintanilla, Asunción; Diaz de Tuesta, Jose L.; Figueruelo, Cristina; Munoz, Macarena; Casas, Jose A. (2019). Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process. Catalysts. ISSN 2073-4344. 9:6, p. 1-1610.3390/catal9060516info:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2023-11-21T10:45:40Zoai:bibliotecadigital.ipb.pt:10198/19953Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-19T23:10:43.144720Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process |
title |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process |
spellingShingle |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process Quintanilla, Asunción Autocatalytic kinetics Condensation by-products Fouling Wet air oxidation Wet peroxide oxidation |
title_short |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process |
title_full |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process |
title_fullStr |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process |
title_full_unstemmed |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process |
title_sort |
Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process |
author |
Quintanilla, Asunción |
author_facet |
Quintanilla, Asunción Díaz de Tuesta, Jose Luis Figueruelo, Cristina Munoz, Macarena Casas, Jose A. |
author_role |
author |
author2 |
Díaz de Tuesta, Jose Luis Figueruelo, Cristina Munoz, Macarena Casas, Jose A. |
author2_role |
author author author author |
dc.contributor.none.fl_str_mv |
Biblioteca Digital do IPB |
dc.contributor.author.fl_str_mv |
Quintanilla, Asunción Díaz de Tuesta, Jose Luis Figueruelo, Cristina Munoz, Macarena Casas, Jose A. |
dc.subject.por.fl_str_mv |
Autocatalytic kinetics Condensation by-products Fouling Wet air oxidation Wet peroxide oxidation |
topic |
Autocatalytic kinetics Condensation by-products Fouling Wet air oxidation Wet peroxide oxidation |
description |
The deposition of condensation by-products onto the catalyst surface upon wet peroxide and wet air oxidation processes has usually been associated with catalyst deactivation. However, in Part I of this paper, it was demonstrated that these carbonaceous deposits actually act as catalytic promoters in the oxygen-assisted wet peroxide oxidation (WPO-O2) of phenol. Herein, the intrinsic activity, nature and stability of these species have been investigated. To achieve this goal, an up-flow fixed bed reactor packed with porous Al2O3 spheres was used to facilitate the deposition of the condensation by-products formed in the liquid phase. It was demonstrated that the condensation by-products catalyzed the decomposition of H2O2 and a higher amount of these species leads to a higher degree of oxidation degree The reaction rates, conversion values and intermediates’ distribution were analyzed. The characterization of the carbonaceous deposits on the Al2O3 spheres showed a significant amount of condensation by-products (~6 wt.%) after 650 h of time on stream. They are of aromatic nature and present oxygen functional groups consisting of quinones, phenols, aldehydes, carboxylics and ketones. The initial phenol concentration and H2O2 dose were found to be crucial variables for the generation and consumption of such species, respectively |
publishDate |
2018 |
dc.date.none.fl_str_mv |
2018-01-19T10:00:00Z 2019 2019-01-01T00:00:00Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10198/19953 |
url |
http://hdl.handle.net/10198/19953 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Quintanilla, Asunción; Diaz de Tuesta, Jose L.; Figueruelo, Cristina; Munoz, Macarena; Casas, Jose A. (2019). Condensation by-products in wet peroxide oxidation: Fouling or catalytic promotion? Part I: Evidences of an autocatalytic process. Catalysts. ISSN 2073-4344. 9:6, p. 1-16 10.3390/catal9060516 |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.source.none.fl_str_mv |
reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação instacron:RCAAP |
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Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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RCAAP |
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RCAAP |
reponame_str |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
collection |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
repository.name.fl_str_mv |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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