Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato

Detalhes bibliográficos
Autor(a) principal: Diel, Júlia Cristina
Data de Publicação: 2021
Tipo de documento: Dissertação
Idioma: por
Título da fonte: Manancial - Repositório Digital da UFSM
dARK ID: ark:/26339/0013000010wjs
Texto Completo: http://repositorio.ufsm.br/handle/1/23322
Resumo: In the present work, commercial multiwalled carbon nanotubes (MWCNTs) were modified via green synthesis for impregnation of metallic nanoparticles (MPNs), evaluating the influence of plant extracts (pomegranate leaves, eucalyptus leaves and nutshells) as reducing agents, of metal species (copper and iron), the metallic specifications and the type of functionalization (OH and COOH) in the characteristics of the materials. After synthesis, the modified materials were characterized by different techniques, identifying that MWCNTs were resistant to the synthesis process, preserving their structure and morphological characteristics. After characterization, the potential of the materials was evaluated in the removal of the herbicide glyphosate (GLY) by adsorption in an aqueous matrix. MWCNTs impregnated with iron MPNs using nutshells as a reducing agent proved to be more effective in adsorbing GLY, being the material selected to study the effect of pH, kinetic and equilibrium modeling, thermodynamic behavior, of the simulated effluent, material regeneration statistics and physical modeling. The pH test indicates that the best adsorption results were obtained under pH 4, identified as the natural pH of the GLY solution, favoring the process by dispensing with the use of acids or bases for adjustment. Kinetic studies showed a removal percentage of up to 86.23%, for an initial GLY concentration of 35 mg L-1, with the process equilibrium being reached in about 120 min of contact. The kinetic and equilibrium models that best fit the experimental data were Pseudo-first order and Sips, respectively. It was observed that the adsorptive capacity increased with decreasing temperature, indicating that the process was favored at lower temperatures, with the maximum adsorptive capacity found at 43.66 mg g-1 at 298 K. Regarding the application of the material under circumstances In real terms, removals of 68.38% were achieved for effluent A (containing GLY) and 40.33% for effluent B (containing GLY, atrazine and 2,4- D). Furthermore, the adsorbent was applied for six adsorption/regeneration cycles, maintaining similar values of adsorptive capacity in all cycles. To obtain new insights into this process, the experimental equation curves were simulated from statistical physical models and the Hill model with 1 energy and ideal fluid approach presented the best data prediction, indicating that GLY adsorption occurs by formation of a monolayer and that the interactions of adsorbate with the adsorbent are characterized by only one energy. A combination of the system's steric and energetic parameters in relation to its evolution with temperature indicated that it is an exothermic process, inferring the occurrence of a physisorption mechanism, complementing the results obtained by thermodynamic calculations. Finally, the new insights showed that the adsorbent favored the adsorption of the herbicide by the interaction of GLY molecules with the iron MPNs present on the surface of the adsorbent.
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spelling Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosatoModification of carbon nanotubes by impregnation of metallic nanoparticles via green synthesis for glyphosate adsorptionNanotubos de carbonoSíntese verdeGlifosatoAdsorçãoFísica estatísticaCarbon nanotubesGreen synthesisGlyphosateAdsorptionStatistical physicsCNPQ::ENGENHARIAS::ENGENHARIA QUIMICAIn the present work, commercial multiwalled carbon nanotubes (MWCNTs) were modified via green synthesis for impregnation of metallic nanoparticles (MPNs), evaluating the influence of plant extracts (pomegranate leaves, eucalyptus leaves and nutshells) as reducing agents, of metal species (copper and iron), the metallic specifications and the type of functionalization (OH and COOH) in the characteristics of the materials. After synthesis, the modified materials were characterized by different techniques, identifying that MWCNTs were resistant to the synthesis process, preserving their structure and morphological characteristics. After characterization, the potential of the materials was evaluated in the removal of the herbicide glyphosate (GLY) by adsorption in an aqueous matrix. MWCNTs impregnated with iron MPNs using nutshells as a reducing agent proved to be more effective in adsorbing GLY, being the material selected to study the effect of pH, kinetic and equilibrium modeling, thermodynamic behavior, of the simulated effluent, material regeneration statistics and physical modeling. The pH test indicates that the best adsorption results were obtained under pH 4, identified as the natural pH of the GLY solution, favoring the process by dispensing with the use of acids or bases for adjustment. Kinetic studies showed a removal percentage of up to 86.23%, for an initial GLY concentration of 35 mg L-1, with the process equilibrium being reached in about 120 min of contact. The kinetic and equilibrium models that best fit the experimental data were Pseudo-first order and Sips, respectively. It was observed that the adsorptive capacity increased with decreasing temperature, indicating that the process was favored at lower temperatures, with the maximum adsorptive capacity found at 43.66 mg g-1 at 298 K. Regarding the application of the material under circumstances In real terms, removals of 68.38% were achieved for effluent A (containing GLY) and 40.33% for effluent B (containing GLY, atrazine and 2,4- D). Furthermore, the adsorbent was applied for six adsorption/regeneration cycles, maintaining similar values of adsorptive capacity in all cycles. To obtain new insights into this process, the experimental equation curves were simulated from statistical physical models and the Hill model with 1 energy and ideal fluid approach presented the best data prediction, indicating that GLY adsorption occurs by formation of a monolayer and that the interactions of adsorbate with the adsorbent are characterized by only one energy. A combination of the system's steric and energetic parameters in relation to its evolution with temperature indicated that it is an exothermic process, inferring the occurrence of a physisorption mechanism, complementing the results obtained by thermodynamic calculations. Finally, the new insights showed that the adsorbent favored the adsorption of the herbicide by the interaction of GLY molecules with the iron MPNs present on the surface of the adsorbent.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESNo presente trabalho, nanotubos de carbono comerciais de paredes múltiplas (MWCNTs) foram modificados via síntese verde para impregnação de nanopartículas metálicas (MPNs), avaliando a influência dos extratos vegetais (folhas de romã, folhas de eucalipto e cascas de noz-pecã) como agentes redutores, das espécies de metal (cobre e ferro), das concentrações metálicas e do tipo de funcionalização (OH e COOH) nas características dos materiais. Após a síntese, os materiais modificados foram caracterizados por diferentes técnicas, identificandose que os MWCNTs foram resistentes ao processo de síntese, preservando sua estrutura e características morfológicas. Em sequência a caracterização, a potencialidade dos materiais foi avaliada na remoção do herbicida glifosato (GLY) por adsorção em matriz aquosa. Os MWCNTs impregnados com MPNs de ferro usando cascas de noz-pecã como agente redutor demonstraram ser mais efetivos na adsorção de GLY, sendo o material selecionado para estudo do efeito do pH, da modelagem cinética e de equilíbrio, do comportamento termodinâmico, do efluente simulado, de regeneração do material e da modelagem física estatística. O teste de pH indicou que os melhores resultados de adsorção foram obtidos sob pH 4, identificado como o pH natural da solução de GLY, favorecendo o processo ao dispensar a utilização de ácidos ou bases para ajuste. Os estudos cinéticos apontaram uma porcentagem de remoção de até 86,23%, para uma concentração inicial de GLY de 35 mg L-1, sendo o equilíbrio do processo atingido em cerca de 120 min de contato. Os modelos cinéticos e de equilíbrio que melhor se ajustaram aos dados experimentais foram Pseudo-primeira ordem e Sips, respectivamente. Observou-se que a capacidade adsortiva aumentou com a diminuição da temperatura, indicando que o processo foi favorecido em temperaturas mais baixas, sendo a máxima capacidade adsortiva encontrada de 43,66 mg g-1 a 298 K. Quanto à aplicação do material em circunstâncias reais, alcançaram-se remoções de 68,38% para o efluente A (contendo GLY) e de 40,33% para o efluente B (contendo GLY, atrazina e 2,4-D). Além disso, o adsorvente foi aplicado por seis ciclos de adsorção/regeneração mantendo valores semelhantes de capacidade adsortiva em todos os ciclos. Para a obtenção de novos insights sobre esse processo, as curvas experimentais de equíbrio foram simuladas a partir de modelos físico estatítiscos e o modelo de Hill com 1 energia e abordagem para fluido ideal apresentou a melhor previsão dos dados, indicando que a adsorção de GLY ocorre pela formação de uma monocamada e que as interações do adsorbato com o adsorvente são caracterizadas por apenas uma energia. A combinação dos paramêtros estéricos e energéticos do sistema em relação a sua evolução com a temperatura apontou tratar-se de um processo de natureza exotérmica inferindo-se a ocorrência de um mecanismo de fisissorção, complementando os resultados obtidos pelos cálculos termodinâmicos. Por fim, os novos insights apontaram que o adsorvente favoreceu a adsorção do herbicida pela interação das moléculas de GLY com as MPNs de ferro presentes na superfície do adsorvente.Universidade Federal de Santa MariaBrasilEngenharia QuímicaUFSMPrograma de Pós-Graduação em Engenharia QuímicaCentro de TecnologiaDotto, Guilherme Luizhttp://lattes.cnpq.br/5412544199323879Silveira, Christian Luiz daGeorgin, JordanaZazycki, Maria AméliaDiel, Júlia Cristina2021-12-15T14:32:06Z2021-12-15T14:32:06Z2021-09-27info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisapplication/pdfhttp://repositorio.ufsm.br/handle/1/23322ark:/26339/0013000010wjsporAttribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessreponame:Manancial - Repositório Digital da UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSM2022-07-04T17:34:31Zoai:repositorio.ufsm.br:1/23322Biblioteca Digital de Teses e Dissertaçõeshttps://repositorio.ufsm.br/ONGhttps://repositorio.ufsm.br/oai/requestatendimento.sib@ufsm.br||tedebc@gmail.comopendoar:2022-07-04T17:34:31Manancial - Repositório Digital da UFSM - Universidade Federal de Santa Maria (UFSM)false
dc.title.none.fl_str_mv Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
Modification of carbon nanotubes by impregnation of metallic nanoparticles via green synthesis for glyphosate adsorption
title Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
spellingShingle Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
Diel, Júlia Cristina
Nanotubos de carbono
Síntese verde
Glifosato
Adsorção
Física estatística
Carbon nanotubes
Green synthesis
Glyphosate
Adsorption
Statistical physics
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
title_short Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
title_full Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
title_fullStr Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
title_full_unstemmed Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
title_sort Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
author Diel, Júlia Cristina
author_facet Diel, Júlia Cristina
author_role author
dc.contributor.none.fl_str_mv Dotto, Guilherme Luiz
http://lattes.cnpq.br/5412544199323879
Silveira, Christian Luiz da
Georgin, Jordana
Zazycki, Maria Amélia
dc.contributor.author.fl_str_mv Diel, Júlia Cristina
dc.subject.por.fl_str_mv Nanotubos de carbono
Síntese verde
Glifosato
Adsorção
Física estatística
Carbon nanotubes
Green synthesis
Glyphosate
Adsorption
Statistical physics
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
topic Nanotubos de carbono
Síntese verde
Glifosato
Adsorção
Física estatística
Carbon nanotubes
Green synthesis
Glyphosate
Adsorption
Statistical physics
CNPQ::ENGENHARIAS::ENGENHARIA QUIMICA
description In the present work, commercial multiwalled carbon nanotubes (MWCNTs) were modified via green synthesis for impregnation of metallic nanoparticles (MPNs), evaluating the influence of plant extracts (pomegranate leaves, eucalyptus leaves and nutshells) as reducing agents, of metal species (copper and iron), the metallic specifications and the type of functionalization (OH and COOH) in the characteristics of the materials. After synthesis, the modified materials were characterized by different techniques, identifying that MWCNTs were resistant to the synthesis process, preserving their structure and morphological characteristics. After characterization, the potential of the materials was evaluated in the removal of the herbicide glyphosate (GLY) by adsorption in an aqueous matrix. MWCNTs impregnated with iron MPNs using nutshells as a reducing agent proved to be more effective in adsorbing GLY, being the material selected to study the effect of pH, kinetic and equilibrium modeling, thermodynamic behavior, of the simulated effluent, material regeneration statistics and physical modeling. The pH test indicates that the best adsorption results were obtained under pH 4, identified as the natural pH of the GLY solution, favoring the process by dispensing with the use of acids or bases for adjustment. Kinetic studies showed a removal percentage of up to 86.23%, for an initial GLY concentration of 35 mg L-1, with the process equilibrium being reached in about 120 min of contact. The kinetic and equilibrium models that best fit the experimental data were Pseudo-first order and Sips, respectively. It was observed that the adsorptive capacity increased with decreasing temperature, indicating that the process was favored at lower temperatures, with the maximum adsorptive capacity found at 43.66 mg g-1 at 298 K. Regarding the application of the material under circumstances In real terms, removals of 68.38% were achieved for effluent A (containing GLY) and 40.33% for effluent B (containing GLY, atrazine and 2,4- D). Furthermore, the adsorbent was applied for six adsorption/regeneration cycles, maintaining similar values of adsorptive capacity in all cycles. To obtain new insights into this process, the experimental equation curves were simulated from statistical physical models and the Hill model with 1 energy and ideal fluid approach presented the best data prediction, indicating that GLY adsorption occurs by formation of a monolayer and that the interactions of adsorbate with the adsorbent are characterized by only one energy. A combination of the system's steric and energetic parameters in relation to its evolution with temperature indicated that it is an exothermic process, inferring the occurrence of a physisorption mechanism, complementing the results obtained by thermodynamic calculations. Finally, the new insights showed that the adsorbent favored the adsorption of the herbicide by the interaction of GLY molecules with the iron MPNs present on the surface of the adsorbent.
publishDate 2021
dc.date.none.fl_str_mv 2021-12-15T14:32:06Z
2021-12-15T14:32:06Z
2021-09-27
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/masterThesis
format masterThesis
status_str publishedVersion
dc.identifier.uri.fl_str_mv http://repositorio.ufsm.br/handle/1/23322
dc.identifier.dark.fl_str_mv ark:/26339/0013000010wjs
url http://repositorio.ufsm.br/handle/1/23322
identifier_str_mv ark:/26339/0013000010wjs
dc.language.iso.fl_str_mv por
language por
dc.rights.driver.fl_str_mv Attribution-NonCommercial-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Attribution-NonCommercial-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Universidade Federal de Santa Maria
Brasil
Engenharia Química
UFSM
Programa de Pós-Graduação em Engenharia Química
Centro de Tecnologia
publisher.none.fl_str_mv Universidade Federal de Santa Maria
Brasil
Engenharia Química
UFSM
Programa de Pós-Graduação em Engenharia Química
Centro de Tecnologia
dc.source.none.fl_str_mv reponame:Manancial - Repositório Digital da UFSM
instname:Universidade Federal de Santa Maria (UFSM)
instacron:UFSM
instname_str Universidade Federal de Santa Maria (UFSM)
instacron_str UFSM
institution UFSM
reponame_str Manancial - Repositório Digital da UFSM
collection Manancial - Repositório Digital da UFSM
repository.name.fl_str_mv Manancial - Repositório Digital da UFSM - Universidade Federal de Santa Maria (UFSM)
repository.mail.fl_str_mv atendimento.sib@ufsm.br||tedebc@gmail.com
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