Modificação de nanotubos de carbono por impregnação de nanopartículas metálicas via síntese verde para adsorção de glifosato
Autor(a) principal: | |
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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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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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1815172426788503552 |