Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente
Ano de defesa: | 2018 |
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Autor(a) principal: | |
Orientador(a): | |
Banca de defesa: | |
Tipo de documento: | Tese |
Tipo de acesso: | Acesso aberto |
Idioma: | por |
Instituição de defesa: |
Não Informado pela instituição
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Programa de Pós-Graduação: |
Pós-Graduação em Química
|
Departamento: |
Não Informado pela instituição
|
País: |
Não Informado pela instituição
|
Palavras-chave em Português: | |
Palavras-chave em Inglês: | |
Área do conhecimento CNPq: | |
Link de acesso: | http://ri.ufs.br/jspui/handle/riufs/8144 |
Resumo: | Hybrid coordination networks such as metal-organic networks, also known as MOF (Metal Organic Framework), have attracted great attention from the scientific community due to their wide diversity and wide range of applications, however, the investigation of applications of these structures still forms a large area of research, with great exploration potential, either through experimental or theoretical chemistry. The present work aims at the use of computational chemistry methods with focus on semiempirical methods for the study of MOFs, so we will initially address results regarding the evaluation of the prediction capacity of solid phase structures of MOFs containing lanthanide as a metallic center. Performed using the semi-empirical methods Sparkle/AM1, Sparkle/PM3, Sparkle/PM6, Sparkle/PM7, Sparkle/RM1 and RM1. The results obtained from the calculation of optimization of the structures suggest that the Sparkle/PM3 and Sparkle/RM1 methods provide more accurate results, with less variability and great agreement with the experimental data, both structural and luminescent. The health application study initially evaluated the structure of the drug doxorubicin and MOF ZnDBC ([Zn(BDC)(H2O)2]n), and then evaluated the drug’s anchoring potential, in order to obtain results that justify the MOF to be chosen as a candidate for application as a drug carrier. This analysis resulted in obtaining a viable anchorage between the MOF lamellae. A simulation of the effects of temperature variation on the structure of the MOF EuBTC ([Eu2(MELL)(H2O)6]) and its effect on the luminescent properties was performed to obtain data that could validate your application with gunshot residues marker, aiming at its use in public safety. This analysis explored the potential of structural description of Sparkle/PM3 as well as the obtaining of luminescent properties, which led to the conclusion that the increase in temperature resulted in an increase in the emission quantum yield caused by the loss of water molecules contained in the first sphere of the coordinating polyhedron. For the application of MOFs in energy, an investigation was carried out regarding the degree of adsorption of the hydrogen gas and methane in the IRMOF-8 and in this one after the doping of its aromatic rings with aluminum atoms, in order to elucidate the effect that the realization of this Doping brings the storage capacity of these gases, for use in gas storage cylinders used in motor vehicles. And it was verified a slight reduction in the storage capacity of the methane gas, since for the hydrogen gas no significant changes were verified. Finally, a study was carried out to evaluate the capture capacity of carbon dioxide and hydrogen sulfide gases in IRMOF-8 and in this doped with aluminum, so the same structure of the previous study was used. It was found that doping gave a considerable increase in the degree of adsorption, being more effective for the carbon dioxide, whose interactions had energy of magnitude of a chemical adsorption. |
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Rodrigues, Nailton MartinsFreire, Ricardo OliveiraDutra, José Diogo de Lisboa2018-05-16T19:20:50Z2018-05-16T19:20:50Z2018-03-23RODRIGUES, Nailton Martins. Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente. 2018. 233 f. Tese (Doutorado em Química) - Universidade Federal de Sergipe, São Cristóvão, SE, 2018.http://ri.ufs.br/jspui/handle/riufs/8144Hybrid coordination networks such as metal-organic networks, also known as MOF (Metal Organic Framework), have attracted great attention from the scientific community due to their wide diversity and wide range of applications, however, the investigation of applications of these structures still forms a large area of research, with great exploration potential, either through experimental or theoretical chemistry. The present work aims at the use of computational chemistry methods with focus on semiempirical methods for the study of MOFs, so we will initially address results regarding the evaluation of the prediction capacity of solid phase structures of MOFs containing lanthanide as a metallic center. Performed using the semi-empirical methods Sparkle/AM1, Sparkle/PM3, Sparkle/PM6, Sparkle/PM7, Sparkle/RM1 and RM1. The results obtained from the calculation of optimization of the structures suggest that the Sparkle/PM3 and Sparkle/RM1 methods provide more accurate results, with less variability and great agreement with the experimental data, both structural and luminescent. The health application study initially evaluated the structure of the drug doxorubicin and MOF ZnDBC ([Zn(BDC)(H2O)2]n), and then evaluated the drug’s anchoring potential, in order to obtain results that justify the MOF to be chosen as a candidate for application as a drug carrier. This analysis resulted in obtaining a viable anchorage between the MOF lamellae. A simulation of the effects of temperature variation on the structure of the MOF EuBTC ([Eu2(MELL)(H2O)6]) and its effect on the luminescent properties was performed to obtain data that could validate your application with gunshot residues marker, aiming at its use in public safety. This analysis explored the potential of structural description of Sparkle/PM3 as well as the obtaining of luminescent properties, which led to the conclusion that the increase in temperature resulted in an increase in the emission quantum yield caused by the loss of water molecules contained in the first sphere of the coordinating polyhedron. For the application of MOFs in energy, an investigation was carried out regarding the degree of adsorption of the hydrogen gas and methane in the IRMOF-8 and in this one after the doping of its aromatic rings with aluminum atoms, in order to elucidate the effect that the realization of this Doping brings the storage capacity of these gases, for use in gas storage cylinders used in motor vehicles. And it was verified a slight reduction in the storage capacity of the methane gas, since for the hydrogen gas no significant changes were verified. Finally, a study was carried out to evaluate the capture capacity of carbon dioxide and hydrogen sulfide gases in IRMOF-8 and in this doped with aluminum, so the same structure of the previous study was used. It was found that doping gave a considerable increase in the degree of adsorption, being more effective for the carbon dioxide, whose interactions had energy of magnitude of a chemical adsorption.As redes metalorgânicas também conhecidas como MOF (do inglês Metal Organic Framework) têm atraído grande atenção da comunidade científica devido a sua ampla diversidade e vasta gama de aplicações. Entretanto, a investigação de aplicações destas estruturas ainda configura uma grande área de pesquisa, com potencial de exploração, seja por meio de um viés experimental ou teórico. O presente trabalho tem como objetivo o uso de métodos de química computacional com foco em métodos semiempíricos para o estudo das MOFs. Assim, inicialmente abordaremos resultados referentes à avaliação da capacidade de predição das estruturas em fase sólida de MOFs contendo íons lantanídeos como centro metálico. Este estudo foi realizado através do uso dos métodos semiempíricos Sparkle/AM1, Sparkle/PM3, Sparkle/PM6, Sparkle/PM7, Sparkle/RM1 e o RM1. Os resultados obtidos a partir do cálculo de otimização das estruturas sugerem que o método Sparkle/PM3 e o Sparkle/RM1 proporcionam resultados mais exatos, com menor variabilidade e grande concordância com os dados experimentais, tanto estruturais como luminescentes. Foi avaliado o potencial de ancoragem da doxorrubicina na MOF ZnDBC ([Zn(BDC)(H2O)2]n). Esta análise mostrou viabilidade de ancoragem entre as lamelas da MOF. Além disso, foi realizada uma simulação dos efeitos da variação da temperatura sobre as propriedades luminescentes da MOF EuBTC ([Eu2(MELL)(H2O)6). Com isso, buscou-se validar a aplicação desta MOF como marcador de resíduos de disparo de arma de fogo. Esta análise explorou o potencial de descrição estrutural do Sparkle/PM3, bem como obtenção de propriedades luminescentes. A elevação da temperatura resultou no aumento do rendimento quântico de emissão, causado pela perda de moléculas de água contidas na primeira esfera do poliedro de coordenação. Para aplicação de MOFs na área de energia, foi realizada uma investigação referente ao grau de adsorção de gás hidrogênio e metano na IRMOF-8. Foi realizada a inclusão de átomos de alumínio nos anéis aromáticos, visando elucidar qual o efeito provocado sobre a capacidade de armazenamento desses gases. A dopagem levou a uma leve redução na capacidade de armazenamento do gás metano. Já para o gás hidrogênio não foram verificadas alterações significativas. Por fim, foi feito um estudo de avaliação da capacidade de captura dos gases dióxido de carbono e sulfeto de hidrogênio na IRMOF-8, tanto pura quanto dopada com alumínio. Notou-se que a dopagem proporcionou um considerável aumento no grau de adsorção, sendo mais efetivo para o dióxido de carbono, cujas interações tiveram energia de magnitude de uma adsorção química.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESSão Cristóvão, SEporQuímicaPolímerosEurópioMétodos semiempíricosPropriedades luminescentesAdsorçãoRedes Metalorgânicas (MOFs)Európio (III)Metal Organic Framework (MOFs)Europium (III)Semiempirical methodsLuminescent propertiesAdsorptionCIENCIAS EXATAS E DA TERRA::QUIMICAEstudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambienteTheoretical study of structural and spectroscopic properties of metal organic frameworks with applications in health, public safety, energy, and environmentinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisPós-Graduação em QuímicaUniversidade Federal de Sergipereponame:Repositório Institucional da UFSinstname:Universidade Federal de Sergipe (UFS)instacron:UFSinfo:eu-repo/semantics/openAccessLICENSElicense.txtlicense.txttext/plain; charset=utf-81475https://ri.ufs.br/jspui/bitstream/riufs/8144/1/license.txt098cbbf65c2c15e1fb2e49c5d306a44cMD51ORIGINALNAILTON_MARTINS_RODRIGUES.pdfNAILTON_MARTINS_RODRIGUES.pdfapplication/pdf13427656https://ri.ufs.br/jspui/bitstream/riufs/8144/2/NAILTON_MARTINS_RODRIGUES.pdf71c052a0bca7b8aba57b6b284d692fd3MD52TEXTNAILTON_MARTINS_RODRIGUES.pdf.txtNAILTON_MARTINS_RODRIGUES.pdf.txtExtracted texttext/plain455530https://ri.ufs.br/jspui/bitstream/riufs/8144/3/NAILTON_MARTINS_RODRIGUES.pdf.txt86d365c09993da1cbb994eefa9ad6b32MD53THUMBNAILNAILTON_MARTINS_RODRIGUES.pdf.jpgNAILTON_MARTINS_RODRIGUES.pdf.jpgGenerated Thumbnailimage/jpeg1499https://ri.ufs.br/jspui/bitstream/riufs/8144/4/NAILTON_MARTINS_RODRIGUES.pdf.jpgb65f8ec259f6141ae67bc5a326e435afMD54riufs/81442018-05-16 16:20:50.84oai:ufs.br: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Repositório InstitucionalPUBhttps://ri.ufs.br/oai/requestrepositorio@academico.ufs.bropendoar:2018-05-16T19:20:50Repositório Institucional da UFS - Universidade Federal de Sergipe (UFS)false |
dc.title.pt_BR.fl_str_mv |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente |
dc.title.alternative.eng.fl_str_mv |
Theoretical study of structural and spectroscopic properties of metal organic frameworks with applications in health, public safety, energy, and environment |
title |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente |
spellingShingle |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente Rodrigues, Nailton Martins Química Polímeros Európio Métodos semiempíricos Propriedades luminescentes Adsorção Redes Metalorgânicas (MOFs) Európio (III) Metal Organic Framework (MOFs) Europium (III) Semiempirical methods Luminescent properties Adsorption CIENCIAS EXATAS E DA TERRA::QUIMICA |
title_short |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente |
title_full |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente |
title_fullStr |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente |
title_full_unstemmed |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente |
title_sort |
Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente |
author |
Rodrigues, Nailton Martins |
author_facet |
Rodrigues, Nailton Martins |
author_role |
author |
dc.contributor.author.fl_str_mv |
Rodrigues, Nailton Martins |
dc.contributor.advisor1.fl_str_mv |
Freire, Ricardo Oliveira |
dc.contributor.advisor-co1.fl_str_mv |
Dutra, José Diogo de Lisboa |
contributor_str_mv |
Freire, Ricardo Oliveira Dutra, José Diogo de Lisboa |
dc.subject.por.fl_str_mv |
Química Polímeros Európio Métodos semiempíricos Propriedades luminescentes Adsorção Redes Metalorgânicas (MOFs) Európio (III) Metal Organic Framework (MOFs) |
topic |
Química Polímeros Európio Métodos semiempíricos Propriedades luminescentes Adsorção Redes Metalorgânicas (MOFs) Európio (III) Metal Organic Framework (MOFs) Europium (III) Semiempirical methods Luminescent properties Adsorption CIENCIAS EXATAS E DA TERRA::QUIMICA |
dc.subject.eng.fl_str_mv |
Europium (III) Semiempirical methods Luminescent properties Adsorption |
dc.subject.cnpq.fl_str_mv |
CIENCIAS EXATAS E DA TERRA::QUIMICA |
description |
Hybrid coordination networks such as metal-organic networks, also known as MOF (Metal Organic Framework), have attracted great attention from the scientific community due to their wide diversity and wide range of applications, however, the investigation of applications of these structures still forms a large area of research, with great exploration potential, either through experimental or theoretical chemistry. The present work aims at the use of computational chemistry methods with focus on semiempirical methods for the study of MOFs, so we will initially address results regarding the evaluation of the prediction capacity of solid phase structures of MOFs containing lanthanide as a metallic center. Performed using the semi-empirical methods Sparkle/AM1, Sparkle/PM3, Sparkle/PM6, Sparkle/PM7, Sparkle/RM1 and RM1. The results obtained from the calculation of optimization of the structures suggest that the Sparkle/PM3 and Sparkle/RM1 methods provide more accurate results, with less variability and great agreement with the experimental data, both structural and luminescent. The health application study initially evaluated the structure of the drug doxorubicin and MOF ZnDBC ([Zn(BDC)(H2O)2]n), and then evaluated the drug’s anchoring potential, in order to obtain results that justify the MOF to be chosen as a candidate for application as a drug carrier. This analysis resulted in obtaining a viable anchorage between the MOF lamellae. A simulation of the effects of temperature variation on the structure of the MOF EuBTC ([Eu2(MELL)(H2O)6]) and its effect on the luminescent properties was performed to obtain data that could validate your application with gunshot residues marker, aiming at its use in public safety. This analysis explored the potential of structural description of Sparkle/PM3 as well as the obtaining of luminescent properties, which led to the conclusion that the increase in temperature resulted in an increase in the emission quantum yield caused by the loss of water molecules contained in the first sphere of the coordinating polyhedron. For the application of MOFs in energy, an investigation was carried out regarding the degree of adsorption of the hydrogen gas and methane in the IRMOF-8 and in this one after the doping of its aromatic rings with aluminum atoms, in order to elucidate the effect that the realization of this Doping brings the storage capacity of these gases, for use in gas storage cylinders used in motor vehicles. And it was verified a slight reduction in the storage capacity of the methane gas, since for the hydrogen gas no significant changes were verified. Finally, a study was carried out to evaluate the capture capacity of carbon dioxide and hydrogen sulfide gases in IRMOF-8 and in this doped with aluminum, so the same structure of the previous study was used. It was found that doping gave a considerable increase in the degree of adsorption, being more effective for the carbon dioxide, whose interactions had energy of magnitude of a chemical adsorption. |
publishDate |
2018 |
dc.date.accessioned.fl_str_mv |
2018-05-16T19:20:50Z |
dc.date.available.fl_str_mv |
2018-05-16T19:20:50Z |
dc.date.issued.fl_str_mv |
2018-03-23 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
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info:eu-repo/semantics/doctoralThesis |
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dc.identifier.citation.fl_str_mv |
RODRIGUES, Nailton Martins. Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente. 2018. 233 f. Tese (Doutorado em Química) - Universidade Federal de Sergipe, São Cristóvão, SE, 2018. |
dc.identifier.uri.fl_str_mv |
http://ri.ufs.br/jspui/handle/riufs/8144 |
identifier_str_mv |
RODRIGUES, Nailton Martins. Estudo teórico das propriedades estruturais e espectroscópicas de redes metalorgânicas com aplicações em saúde, segurança pública, energia e meio ambiente. 2018. 233 f. Tese (Doutorado em Química) - Universidade Federal de Sergipe, São Cristóvão, SE, 2018. |
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