Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal

Detalhes bibliográficos
Autor(a) principal: FRAGA, Tiago José Marques
Data de Publicação: 2020
Tipo de documento: Tese
Idioma: eng
Título da fonte: Repositório Institucional da UFPE
dARK ID: ark:/64986/0013000003kv1
Texto Completo: https://repositorio.ufpe.br/handle/123456789/40718
Resumo: GHISLANDI, Marcos Gomes, também é conhecido(a) em citações bibliográficas por: GHISLANDI, M. & MOTTA SOBRINHO, Mauricio Alves da, também é conhecido(a) em citações bibliográficas por: Motta, Mauricio da.
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spelling FRAGA, Tiago José Marqueshttp://lattes.cnpq.br/2429790209914530http://lattes.cnpq.br/3644581240048018http://lattes.cnpq.br/3409757365313853http://lattes.cnpq.br/7280351763016108MOTTA SOBRINHO, Mauricio Alves daGHISLANDI, Marcos GomesCARVALHO, Marilda Nascimento2021-07-30T16:06:37Z2021-07-30T16:06:37Z2020-02-16FRAGA, Tiago José Marques. Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal. 2020. Tese (Doutorado em Engenharia Química) – Universidade Federal de Pernambuco, Recife, 2020.https://repositorio.ufpe.br/handle/123456789/40718ark:/64986/0013000003kv1GHISLANDI, Marcos Gomes, também é conhecido(a) em citações bibliográficas por: GHISLANDI, M. & MOTTA SOBRINHO, Mauricio Alves da, também é conhecido(a) em citações bibliográficas por: Motta, Mauricio da.In this work, n-Layer Graphene Oxide (nGO) was synthetized from graphite oxidation via modified Hummers method. Afterwards, the nGO was functionalized with diethylenetriamine (DETA) and FeCl3 at 180 oC to obtain the novel n-layer amino-iron oxide-functionalized graphene oxide (nGO-NH2-Fe3O4). Infrared (FTIR) and Raman spectroscopies, X-Ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM) and Thermogravimetric Analysis (TGA) were performed to characterize both nGO and nGO-NH2- Fe3O4. These materials were then evaluated as adsorbents of the cationic dye Methylene Blue (MB) and the anionic Remazol Black B (RB) and Drimaren Red (DR) through a comparative approach. Adsorption experiments were performed in batch, and studies of kinetics, equilibrium, thermodynamic and sorbent regeneration were carried out to investigate the affinity of nGO, nGO-NH2-Fe3O4 and the amino-functionalized nGO supported in wood waste charcoal (nGO(NH)R/C) towards the MB, RB and DR. Analysis of the point of zero net charge (pHPZC) and pH effect showed that the nGO-NH2-Fe3O4 pHPZC was 8.2, hence the MB adsorption was higher at pH 12.0; however, the adsorption of RB and DR was not influenced by pH changes. Kinetics studies indicated that the system reached the equilibrium state after 5 min, 90 min and 120 min for MB, RB and DR, respectively. Adsorption capacity at equilibrium (qe) were 971.43±3.13 and 177.86±10.32 mg/g; and kinetic constant (kS) of 0.053±0.025 and 0.0024±0.0007 g/mg/min, for MB and RB, respectively. The pseudo-second-order model was better fitted to the experimental data. Equilibrium studies showed maximum monolayer adsorption capacity (qm) of 2319.20±269.37, 264.17±15.04 and 219.75±78.55 mg/g for MB, RB and DR, respectively; furthermore, Langmuir-Freundlich isotherm best fitted the adsorption for almost all system evaluated. Thermodynamic experiments revealed that all systems were spontaneous [Delta(Go) < 0] and evidenced the physical nature of the adsorption of MB [Delta(Ho) –150 kJ/mol] by nGO-NH2-Fe3O4, whilst the removal of RB and DR was characterized as chemisorption, with Delta(Ho) 92.83 kJ/mol and 66.43 kJ/mol respectively. Recycling experiments showed that the nGO-NH2-Fe3O4 maintained the MB removal rate above 95% after ten cycles. Amino-nGO was then anchored on vegetal charcoal with the objective to ease sorbent separation from aqueous medium. Despite the relatively lower adsorptive capacity towards MB dye (qm 52.98 mg/g) in comparison to nGO-NH2-Fe3O4, nGO(NH)R/C showed a quick decantation in comparison to nGO. Phytotoxicology studies on lettuce seeds evidenced an elevated germination and elongation when exposed to nGO-NH2-Fe3O4 suspension differently from pristine material, nGO. All the results showed sorbent high adsorption capacity and outstanding regeneration capability and evidenced the employment of novel nGO-NH2-Fe3O4 as a highly efficient adsorbent of textile dyes. Aiming to ease the separation of the adsorbent from the effluent after the adsorption, nGO(NH)R was supported in wood waste charcoal. Sedimentation tests showed that nGO(NH)R/C fully decanted within one day, differently from nGO, that decanted after four days. Furthermore, adsorption experiments with MB were carried out for nGO(NH)R/C and showed an equilibrium time of 20 min, maximum adsorption capacity in the monolayer of 54 mg/g and a spontaneous and exothermic behavior.FACEPENeste trabalho, o óxido de grafeno em n-camadas (nOG) foi sintetizado a partir da oxidação de grafite pelo método de Hummers modificado. Posteriormente, o nOG foi funcionalizado com dietilenotriamina (DETA) e FeCl3 a 180 oC para obtenção do novo óxido de grafeno amino-Fe3O4-funcionalizado (nOG-NH2-Fe3O4). Análises de espectroscopia no Infravermelho (FTIR) e de Raman, Difração de Raios-X (XRD), Microscopia Eletrônica de Varredura (MEV), Microscopia de Força Atômica (AFM) e Termogravimetria (ATG) foram realizadas para caracterizar o nOG e nOG-NH2-Fe3O4. O nOG-NH2-Fe3O4 e o nGO foram então avaliados como adsorventes do corante catiônico Azul de Metileno (AM) e dos corantes aniônicos Remazol Preto B (RB) e Drimaren Vermelho (DV) através de uma abordagem comparativa. Estudos em batelada de cinética, equilíbrio, termodinâmica e regeneração do adsorvente foram realizados para investigar a afinidade do nOG, nOG-NH2-Fe3O4 e o nOG amino-funcionalizado suportado em carvão vegetal de resíduos de madeira (nOG(NH)R/C) para o AM, RB e DV. A análise do ponto de carga zero (pHPZC) e o efeito da variação do pH mostraram que o pHPZC do nOG-NH2-Fe3O4 foi de 8,2, e a adsorção de AM foi maior em pH 12,0. A adsorção do RB não foi influenciada pela variação do pH. Estudos de cinética indicaram que o sistema atingiu o estado de equilíbrio após 5 min, 90 min e 120 min para o AM, RB e DV. A capacidade de adsorção no equilíbrio (qe) foi de 971,43±3,13 e 177,86±10,32 mg/g; e a constante cinética (kS) de 0,0529±0,0248 e 0,0024±0,0007 g/mg/min, para o AM e o RB, respectivamente. Além disso, o modelo de pseudo-segunda ordem foi o que melhor se ajustou aos dados experimentais. Estudos de equilíbrio mostraram capacidade máxima de adsorção na monocamada de 2319,20±269,37 e 264,17±15,04 e 219,75±78,55 mg/g para o AM, RB e DV, respectivamente; além disso, a isoterma de Langmuir-Freundlich se ajustou melhor à adsorção em praticamente todos os sistemas avaliados. Experimentos de termodinâmica revelaram que todos os sistemas foram espontâneos [Delta(Go) < 0] e evidenciaram a natureza física da adsorção do AM pelo nOG-NH2-Fe3O4 [Delta(Ho) –150 kJ/mol], enquanto a remoção de RB e DV foi caracterizado como quimissorção, com Delta(Ho) 92,83 kJ/mol e 66,43 kJ/mol respectivamente. Experimentos de reciclagem mostraram que o nOG-NH2-Fe3O4 manteve a taxa de remoção de AM acima de 95% após dez ciclos. Estudos de fitotoxicologia em sementes de alface evidenciaram uma elevada germinação e alongamento quando expostas à suspensão de nOG- NH2-Fe3O4, diferentemente do material precursor, nOG. Todos os resultados mostraram elevada capacidade de adsorção e de regeneração do adsorvente, evidenciando o nOG-NH2-Fe3O4 como um adsorvente de alta eficiência de corantes têxteis. Com o objetivo de facilitar a separação do adsorvente do efluente após a adsorção, o nOG(NH)R foi suportado em carvão vegetal de resíduo de madeira. Testes de sedimentação mostraram que o nOG(NH)R/C decantou em dois dias, diferentemente do nOG, que decantou após quatro dias. Além disso, experimentos de adsorção com AM foram realizados para nOG(NH)R/C e mostraram um tempo de equilíbrio de 20 min, capacidade máxima de adsorção de 54 mg/g e comportamento espontâneo e exotérmico.engUniversidade Federal de PernambucoPrograma de Pos Graduacao em Engenharia QuimicaUFPEBrasilAttribution-NonCommercial-NoDerivs 3.0 Brazilhttp://creativecommons.org/licenses/by-nc-nd/3.0/br/info:eu-repo/semantics/openAccessEngenharia QuímicaGrafenoNanomateriais 2DFuncionalizaçãoAdsorçãoEfluentes têxteisInterações intermolecularesDevelopment of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removalinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisdoutoradoreponame:Repositório Institucional da UFPEinstname:Universidade Federal de Pernambuco (UFPE)instacron:UFPEORIGINALTESE Tiago José Marques Fraga.pdfTESE Tiago José Marques Fraga.pdfapplication/pdf6755518https://repositorio.ufpe.br/bitstream/123456789/40718/1/TESE%20Tiago%20Jos%c3%a9%20Marques%20Fraga.pdfce7de840b9165aacabac5be4014b1b11MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; 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dc.title.pt_BR.fl_str_mv Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
title Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
spellingShingle Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
FRAGA, Tiago José Marques
Engenharia Química
Grafeno
Nanomateriais 2D
Funcionalização
Adsorção
Efluentes têxteis
Interações intermoleculares
title_short Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
title_full Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
title_fullStr Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
title_full_unstemmed Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
title_sort Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal
author FRAGA, Tiago José Marques
author_facet FRAGA, Tiago José Marques
author_role author
dc.contributor.authorLattes.pt_BR.fl_str_mv http://lattes.cnpq.br/2429790209914530
dc.contributor.advisorLattes.pt_BR.fl_str_mv http://lattes.cnpq.br/3644581240048018
dc.contributor.advisor-coLattes.pt_BR.fl_str_mv http://lattes.cnpq.br/3409757365313853
http://lattes.cnpq.br/7280351763016108
dc.contributor.author.fl_str_mv FRAGA, Tiago José Marques
dc.contributor.advisor1.fl_str_mv MOTTA SOBRINHO, Mauricio Alves da
dc.contributor.advisor-co1.fl_str_mv GHISLANDI, Marcos Gomes
CARVALHO, Marilda Nascimento
contributor_str_mv MOTTA SOBRINHO, Mauricio Alves da
GHISLANDI, Marcos Gomes
CARVALHO, Marilda Nascimento
dc.subject.por.fl_str_mv Engenharia Química
Grafeno
Nanomateriais 2D
Funcionalização
Adsorção
Efluentes têxteis
Interações intermoleculares
topic Engenharia Química
Grafeno
Nanomateriais 2D
Funcionalização
Adsorção
Efluentes têxteis
Interações intermoleculares
description GHISLANDI, Marcos Gomes, também é conhecido(a) em citações bibliográficas por: GHISLANDI, M. & MOTTA SOBRINHO, Mauricio Alves da, também é conhecido(a) em citações bibliográficas por: Motta, Mauricio da.
publishDate 2020
dc.date.issued.fl_str_mv 2020-02-16
dc.date.accessioned.fl_str_mv 2021-07-30T16:06:37Z
dc.date.available.fl_str_mv 2021-07-30T16:06:37Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/doctoralThesis
format doctoralThesis
status_str publishedVersion
dc.identifier.citation.fl_str_mv FRAGA, Tiago José Marques. Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal. 2020. Tese (Doutorado em Engenharia Química) – Universidade Federal de Pernambuco, Recife, 2020.
dc.identifier.uri.fl_str_mv https://repositorio.ufpe.br/handle/123456789/40718
dc.identifier.dark.fl_str_mv ark:/64986/0013000003kv1
identifier_str_mv FRAGA, Tiago José Marques. Development of nanosorbents derived from functionalized n-layered graphene nanosheets for dye removal. 2020. Tese (Doutorado em Engenharia Química) – Universidade Federal de Pernambuco, Recife, 2020.
ark:/64986/0013000003kv1
url https://repositorio.ufpe.br/handle/123456789/40718
dc.language.iso.fl_str_mv eng
language eng
dc.rights.driver.fl_str_mv Attribution-NonCommercial-NoDerivs 3.0 Brazil
http://creativecommons.org/licenses/by-nc-nd/3.0/br/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Attribution-NonCommercial-NoDerivs 3.0 Brazil
http://creativecommons.org/licenses/by-nc-nd/3.0/br/
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Universidade Federal de Pernambuco
dc.publisher.program.fl_str_mv Programa de Pos Graduacao em Engenharia Quimica
dc.publisher.initials.fl_str_mv UFPE
dc.publisher.country.fl_str_mv Brasil
publisher.none.fl_str_mv Universidade Federal de Pernambuco
dc.source.none.fl_str_mv reponame:Repositório Institucional da UFPE
instname:Universidade Federal de Pernambuco (UFPE)
instacron:UFPE
instname_str Universidade Federal de Pernambuco (UFPE)
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institution UFPE
reponame_str Repositório Institucional da UFPE
collection Repositório Institucional da UFPE
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