The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation

Detalhes bibliográficos
Autor(a) principal: Ribeiro, Rui
Data de Publicação: 2017
Outros Autores: Silva, Adrián, Figueiredo, José, Faria, Joaquim, Gomes, Helder
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
Texto Completo: http://hdl.handle.net/10198/15360
Resumo: Three magnetic carbon xerogels were developed by inclusion of iron and/or cobalt precursors during the synthesis procedure. The synthesized materials were tested in the catalytic wet peroxide oxidation (CWPO) of aqueous solutions containing 4-nitrophenol (4-NP) − a refractory organic model pollutant, under a water treatment process intensification approach. For that p urpose, the experimental runs were performed with high pollutant load (5 g L −1 ), low catalyst dosage (2.5 g L −1 , corresponding to a fixed pollutant/catalyst mass ratio of 2), atmospheric pressure, 50 °C, pH = 3 and stoichiometric amount of hydrogen peroxide (H 2 O 2 ). The bimetallic magnetic carbon xerogel catalyst (CX/CoFe) was more active than each of the monometallic catalysts (CX/Fe or CX/Co). The better performance was explained in terms of a synergic association of factors: (i) the enhanced accessibility to the active iron species at the surface of CX/CoFe promoted by the simultaneous incorporation of cobalt, (ii) the ability of metallic Co to catalyse H 2 O 2 decomposition via hydroxyl radicals (HO[rad]) formation, and (iii) the efficient reduction of Fe 3+ to Fe 2+ promoted by metallic Co on the surface of CX/CoFe. A 4-NP conversion of 98.5% was determined after 30 min of CWPO reaction. Leaching of the iron species in the bimetallic CX/CoFe was considerably reduced with relation to the monometallic iron catalyst. However, partial catalyst deactivation occurred due to lower stability of oxidized cobalt species. A detailed reaction mechanism is proposed for the surface catalytic reactions occurring over the CX/CoFe catalyst.
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spelling The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidationBimetallic catalystCatalytic wet peroxide oxidation (CWPO)Heterogeneous Fenton-like processHighly polluted watersMagnetic carbon compositesThree magnetic carbon xerogels were developed by inclusion of iron and/or cobalt precursors during the synthesis procedure. The synthesized materials were tested in the catalytic wet peroxide oxidation (CWPO) of aqueous solutions containing 4-nitrophenol (4-NP) − a refractory organic model pollutant, under a water treatment process intensification approach. For that p urpose, the experimental runs were performed with high pollutant load (5 g L −1 ), low catalyst dosage (2.5 g L −1 , corresponding to a fixed pollutant/catalyst mass ratio of 2), atmospheric pressure, 50 °C, pH = 3 and stoichiometric amount of hydrogen peroxide (H 2 O 2 ). The bimetallic magnetic carbon xerogel catalyst (CX/CoFe) was more active than each of the monometallic catalysts (CX/Fe or CX/Co). The better performance was explained in terms of a synergic association of factors: (i) the enhanced accessibility to the active iron species at the surface of CX/CoFe promoted by the simultaneous incorporation of cobalt, (ii) the ability of metallic Co to catalyse H 2 O 2 decomposition via hydroxyl radicals (HO[rad]) formation, and (iii) the efficient reduction of Fe 3+ to Fe 2+ promoted by metallic Co on the surface of CX/CoFe. A 4-NP conversion of 98.5% was determined after 30 min of CWPO reaction. Leaching of the iron species in the bimetallic CX/CoFe was considerably reduced with relation to the monometallic iron catalyst. However, partial catalyst deactivation occurred due to lower stability of oxidized cobalt species. A detailed reaction mechanism is proposed for the surface catalytic reactions occurring over the CX/CoFe catalyst.This work was financially supported by: Project POCI-01-0145- FEDER-006984 – Associate Laboratory LSRE-LCM funded by FEDER through COMPETE2020 – Programa Operacional Competitividade e Internacionalização (POCI) – and by national funds through FCT - Fundação para a Ciência e a Tecnologia. R.S. Ribeiro acknowledges the individual Ph.D. grant SFRH/BD/94177/2013, with financing from FCT and the European Social Fund (through POPH and QREN). A.M.T. Silva acknowledges the FCT Investigator 2013 Programme (IF/01501/2013), with financing from the European Social Fund and the Human Potential Operational Programme.This work was financially supported by: Project POCI-01-0145- FEDER-006984 – Associate Laboratory LSRE-LCM funded by FEDER through COMPETE2020 – Programa Operacional Competitividade e Internacionalização (POCI) – and by national funds through FCT - Fundação para a Ciência e a Tecnologia. R.S. Ribeiro acknowledges the individual Ph.D. grant SFRH/BD/94177/2013, with financing from FCT and the European Social Fund (through POPH and QREN). A.M.T. Silva acknowledges the FCT Investigator 2013 Programme (IF/01501/2013), with financing from the European Social Fund and the Human Potential Operational Programme.Biblioteca Digital do IPBRibeiro, RuiSilva, AdriánFigueiredo, JoséFaria, JoaquimGomes, Helder2018-01-31T10:00:00Z20172017-01-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10198/15360engRibeiro, Rui; Silva, Adrián M.T.; Figueiredo, José L.; Faria, Joaquim L.; Gomes, Helder (2017). The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation. Catalysis Today. ISSN 0920-5861. 296, p. 66-750920-586110.1016/j.cattod.2017.06.023info: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:RCAAP2023-01-16T12:17:29ZPortal AgregadorONG
dc.title.none.fl_str_mv The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
title The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
spellingShingle The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
Ribeiro, Rui
Bimetallic catalyst
Catalytic wet peroxide oxidation (CWPO)
Heterogeneous Fenton-like process
Highly polluted waters
Magnetic carbon composites
title_short The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
title_full The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
title_fullStr The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
title_full_unstemmed The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
title_sort The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation
author Ribeiro, Rui
author_facet Ribeiro, Rui
Silva, Adrián
Figueiredo, José
Faria, Joaquim
Gomes, Helder
author_role author
author2 Silva, Adrián
Figueiredo, José
Faria, Joaquim
Gomes, Helder
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Biblioteca Digital do IPB
dc.contributor.author.fl_str_mv Ribeiro, Rui
Silva, Adrián
Figueiredo, José
Faria, Joaquim
Gomes, Helder
dc.subject.por.fl_str_mv Bimetallic catalyst
Catalytic wet peroxide oxidation (CWPO)
Heterogeneous Fenton-like process
Highly polluted waters
Magnetic carbon composites
topic Bimetallic catalyst
Catalytic wet peroxide oxidation (CWPO)
Heterogeneous Fenton-like process
Highly polluted waters
Magnetic carbon composites
description Three magnetic carbon xerogels were developed by inclusion of iron and/or cobalt precursors during the synthesis procedure. The synthesized materials were tested in the catalytic wet peroxide oxidation (CWPO) of aqueous solutions containing 4-nitrophenol (4-NP) − a refractory organic model pollutant, under a water treatment process intensification approach. For that p urpose, the experimental runs were performed with high pollutant load (5 g L −1 ), low catalyst dosage (2.5 g L −1 , corresponding to a fixed pollutant/catalyst mass ratio of 2), atmospheric pressure, 50 °C, pH = 3 and stoichiometric amount of hydrogen peroxide (H 2 O 2 ). The bimetallic magnetic carbon xerogel catalyst (CX/CoFe) was more active than each of the monometallic catalysts (CX/Fe or CX/Co). The better performance was explained in terms of a synergic association of factors: (i) the enhanced accessibility to the active iron species at the surface of CX/CoFe promoted by the simultaneous incorporation of cobalt, (ii) the ability of metallic Co to catalyse H 2 O 2 decomposition via hydroxyl radicals (HO[rad]) formation, and (iii) the efficient reduction of Fe 3+ to Fe 2+ promoted by metallic Co on the surface of CX/CoFe. A 4-NP conversion of 98.5% was determined after 30 min of CWPO reaction. Leaching of the iron species in the bimetallic CX/CoFe was considerably reduced with relation to the monometallic iron catalyst. However, partial catalyst deactivation occurred due to lower stability of oxidized cobalt species. A detailed reaction mechanism is proposed for the surface catalytic reactions occurring over the CX/CoFe catalyst.
publishDate 2017
dc.date.none.fl_str_mv 2017
2017-01-01T00:00:00Z
2018-01-31T10:00:00Z
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/10198/15360
url http://hdl.handle.net/10198/15360
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv Ribeiro, Rui; Silva, Adrián M.T.; Figueiredo, José L.; Faria, Joaquim L.; Gomes, Helder (2017). The role of cobalt in bimetallic iron-cobalt magnetic carbon xerogels developed for catalytic wet peroxide oxidation. Catalysis Today. ISSN 0920-5861. 296, p. 66-75
0920-5861
10.1016/j.cattod.2017.06.023
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)
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instname_str Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação
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institution RCAAP
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