A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine
Autor(a) principal: | |
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Data de Publicação: | 2021 |
Outros Autores: | , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1007/s11356-021-14714-8 http://hdl.handle.net/11449/208766 |
Resumo: | Two compositions of graphene oxide-magnetite nanocomposites were studied as catalysts in the heterogeneous Fenton process. Transmission electron microscopy and X-ray diffraction revealed that the graphene oxide sheets were covered with nanoparticles of magnetite, with an average crystallite size of 7 nm. Infrared spectroscopy analysis indicated that the phases interacted through covalent Fe-O-C bonds. The composites presented significantly improved catalytic activity, compared to pure magnetite, with a synergistic effect of up to a factor of 17.1 for the Fenton degradation of caffeine, achieving total removal after 90 min. This synergistic effect was a consequence of the interaction between the phases, resulting in improved mass transfer of caffeine to the catalyst surface, adsorption and efficient degradation, with enhanced HO• generation. The surface reaction constant increased by up to three orders of magnitude, demonstrating the important role of graphene oxide in the degradation kinetics of the heterogeneous Fenton process. The surface-bonded hydroxyl radicals were responsible for caffeine degradation, achieving 9.4 μmol L-1. After five degradation cycles, a loss of Fe-O-C bonds and increase in oxygenated groups were associated with a small decrease of caffeine removal efficiency, from 98 to 82%, without significant iron leaching, in the dark, and with low consumption of hydrogen peroxide. |
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A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeineEnhanced kineticGraphene oxideMagnetitePharmaceuticalRadical reactionSurface reactionTwo compositions of graphene oxide-magnetite nanocomposites were studied as catalysts in the heterogeneous Fenton process. Transmission electron microscopy and X-ray diffraction revealed that the graphene oxide sheets were covered with nanoparticles of magnetite, with an average crystallite size of 7 nm. Infrared spectroscopy analysis indicated that the phases interacted through covalent Fe-O-C bonds. The composites presented significantly improved catalytic activity, compared to pure magnetite, with a synergistic effect of up to a factor of 17.1 for the Fenton degradation of caffeine, achieving total removal after 90 min. This synergistic effect was a consequence of the interaction between the phases, resulting in improved mass transfer of caffeine to the catalyst surface, adsorption and efficient degradation, with enhanced HO• generation. The surface reaction constant increased by up to three orders of magnitude, demonstrating the important role of graphene oxide in the degradation kinetics of the heterogeneous Fenton process. The surface-bonded hydroxyl radicals were responsible for caffeine degradation, achieving 9.4 μmol L-1. After five degradation cycles, a loss of Fe-O-C bonds and increase in oxygenated groups were associated with a small decrease of caffeine removal efficiency, from 98 to 82%, without significant iron leaching, in the dark, and with low consumption of hydrogen peroxide.Institute of Chemistry São Paulo State University (UNESP)UNESP National Institute for Alternative Technologies of Detection Toxicological Evaluation and Removal of Micropollutants and Radioactives (INCT-DATREM) Institute of ChemistryInstitute of Chemistry São Paulo State University (UNESP)UNESP National Institute for Alternative Technologies of Detection Toxicological Evaluation and Removal of Micropollutants and Radioactives (INCT-DATREM) Institute of ChemistryUniversidade Estadual Paulista (Unesp)Ramirez-Ubillus, Manuel Alejandro [UNESP]de Melo Costa-Serge, Nayara [UNESP]Hammer, Peter [UNESP]Nogueira, Raquel Fernandes Pupo [UNESP]2021-06-25T11:18:42Z2021-06-25T11:18:42Z2021-01-01info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articlehttp://dx.doi.org/10.1007/s11356-021-14714-8Environmental Science and Pollution Research.1614-74990944-1344http://hdl.handle.net/11449/20876610.1007/s11356-021-14714-82-s2.0-85107756449Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengEnvironmental Science and Pollution Researchinfo:eu-repo/semantics/openAccess2021-10-23T19:02:29Zoai:repositorio.unesp.br:11449/208766Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462021-10-23T19:02:29Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine |
title |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine |
spellingShingle |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine Ramirez-Ubillus, Manuel Alejandro [UNESP] Enhanced kinetic Graphene oxide Magnetite Pharmaceutical Radical reaction Surface reaction |
title_short |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine |
title_full |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine |
title_fullStr |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine |
title_full_unstemmed |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine |
title_sort |
A new approach on synergistic effect and chemical stability of graphene oxide-magnetic nanocomposite in the heterogeneous Fenton degradation of caffeine |
author |
Ramirez-Ubillus, Manuel Alejandro [UNESP] |
author_facet |
Ramirez-Ubillus, Manuel Alejandro [UNESP] de Melo Costa-Serge, Nayara [UNESP] Hammer, Peter [UNESP] Nogueira, Raquel Fernandes Pupo [UNESP] |
author_role |
author |
author2 |
de Melo Costa-Serge, Nayara [UNESP] Hammer, Peter [UNESP] Nogueira, Raquel Fernandes Pupo [UNESP] |
author2_role |
author author author |
dc.contributor.none.fl_str_mv |
Universidade Estadual Paulista (Unesp) |
dc.contributor.author.fl_str_mv |
Ramirez-Ubillus, Manuel Alejandro [UNESP] de Melo Costa-Serge, Nayara [UNESP] Hammer, Peter [UNESP] Nogueira, Raquel Fernandes Pupo [UNESP] |
dc.subject.por.fl_str_mv |
Enhanced kinetic Graphene oxide Magnetite Pharmaceutical Radical reaction Surface reaction |
topic |
Enhanced kinetic Graphene oxide Magnetite Pharmaceutical Radical reaction Surface reaction |
description |
Two compositions of graphene oxide-magnetite nanocomposites were studied as catalysts in the heterogeneous Fenton process. Transmission electron microscopy and X-ray diffraction revealed that the graphene oxide sheets were covered with nanoparticles of magnetite, with an average crystallite size of 7 nm. Infrared spectroscopy analysis indicated that the phases interacted through covalent Fe-O-C bonds. The composites presented significantly improved catalytic activity, compared to pure magnetite, with a synergistic effect of up to a factor of 17.1 for the Fenton degradation of caffeine, achieving total removal after 90 min. This synergistic effect was a consequence of the interaction between the phases, resulting in improved mass transfer of caffeine to the catalyst surface, adsorption and efficient degradation, with enhanced HO• generation. The surface reaction constant increased by up to three orders of magnitude, demonstrating the important role of graphene oxide in the degradation kinetics of the heterogeneous Fenton process. The surface-bonded hydroxyl radicals were responsible for caffeine degradation, achieving 9.4 μmol L-1. After five degradation cycles, a loss of Fe-O-C bonds and increase in oxygenated groups were associated with a small decrease of caffeine removal efficiency, from 98 to 82%, without significant iron leaching, in the dark, and with low consumption of hydrogen peroxide. |
publishDate |
2021 |
dc.date.none.fl_str_mv |
2021-06-25T11:18:42Z 2021-06-25T11:18:42Z 2021-01-01 |
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://dx.doi.org/10.1007/s11356-021-14714-8 Environmental Science and Pollution Research. 1614-7499 0944-1344 http://hdl.handle.net/11449/208766 10.1007/s11356-021-14714-8 2-s2.0-85107756449 |
url |
http://dx.doi.org/10.1007/s11356-021-14714-8 http://hdl.handle.net/11449/208766 |
identifier_str_mv |
Environmental Science and Pollution Research. 1614-7499 0944-1344 10.1007/s11356-021-14714-8 2-s2.0-85107756449 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Environmental Science and Pollution Research |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.source.none.fl_str_mv |
Scopus reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
_version_ |
1803046269642342400 |