Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise

Detalhes bibliográficos
Ano de defesa: 2016
Autor(a) principal: Vargas, Josimar lattes
Orientador(a): Rodrigues, Oscar Endrigo Dorneles lattes
Banca de defesa: Emmerich, Daniel Jacintho lattes, Alves, Elenilson Freitas lattes, Giacomelli, Cristiano lattes, Ilha, Vinicius lattes
Tipo de documento: Tese
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Universidade Federal de Santa Maria
Centro de Ciências Naturais e Exatas
Programa de Pós-Graduação: Programa de Pós-Graduação em Química
Departamento: Química
País: Brasil
Palavras-chave em Português:
Palavras-chave em Inglês:
Área do conhecimento CNPq:
Link de acesso: http://repositorio.ufsm.br/handle/1/11952
Resumo: The present work describes the synthesis of a new catalyst of palladium nanoparticles supported on multi-walled carbon nanotubes containing nitrogen (Pd@CNxNCPM) 1 and its use in carbon-carbon coupling reactions (Suzuki and Heck) as well as reactions catalytic hydrogenation (reduction of double C-C bonds and nitro compounds reduction). The synthetic strategy employed afforded the simple way to obtain the catalyst with reaction in a short time and efficiently. To this was employed as the palladium precursor, the salt potassium hexacloropalladate IV and hydrazine monohydrate as the reducing agent, without the need for stabilizing agents for the control of nucleation and size of nanoparticle. The catalyst system was characterized as its morphology: dispersion, size and shape of nanoparticles by scanning electron microscopy. Also the catalyst was performed Raman spectroscopy and determination of amount of palladium. After characterization the catalyst, it was tested for coupling reactions of carbon-carbon: Suzuki and Heck leading to the formation of their products with 70-> 95% for Suzuki coupling and 75-> 95% for Heck. For the synthesis in question were used 0.5 mol% of catalyst (based amount of palladium) for Suzuki and 10 mol% for Heck. It should be noted that the catalyst shown stable in the reaction conditions tested, and observed the possibility of reuse of this system for additional reaction cycles without loss of efficiency for the Suzuki coupling. Also, the catalyst was efficient and chemoselectiv for catalytic hydrogenations of unsaturated carbon-carbon bonds and nitro compounds leading to their products in good yields. Thus, the synthesized catalyst proved versatile and can be used in reactions of carbon-carbon coupling well as in catalytic reduction may also be recovered and reused, which provides an environmentally friendly at the same characteristic.
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spelling 2017-11-01T13:26:07Z2017-11-01T13:26:07Z2016-02-05http://repositorio.ufsm.br/handle/1/11952The present work describes the synthesis of a new catalyst of palladium nanoparticles supported on multi-walled carbon nanotubes containing nitrogen (Pd@CNxNCPM) 1 and its use in carbon-carbon coupling reactions (Suzuki and Heck) as well as reactions catalytic hydrogenation (reduction of double C-C bonds and nitro compounds reduction). The synthetic strategy employed afforded the simple way to obtain the catalyst with reaction in a short time and efficiently. To this was employed as the palladium precursor, the salt potassium hexacloropalladate IV and hydrazine monohydrate as the reducing agent, without the need for stabilizing agents for the control of nucleation and size of nanoparticle. The catalyst system was characterized as its morphology: dispersion, size and shape of nanoparticles by scanning electron microscopy. Also the catalyst was performed Raman spectroscopy and determination of amount of palladium. After characterization the catalyst, it was tested for coupling reactions of carbon-carbon: Suzuki and Heck leading to the formation of their products with 70-> 95% for Suzuki coupling and 75-> 95% for Heck. For the synthesis in question were used 0.5 mol% of catalyst (based amount of palladium) for Suzuki and 10 mol% for Heck. It should be noted that the catalyst shown stable in the reaction conditions tested, and observed the possibility of reuse of this system for additional reaction cycles without loss of efficiency for the Suzuki coupling. Also, the catalyst was efficient and chemoselectiv for catalytic hydrogenations of unsaturated carbon-carbon bonds and nitro compounds leading to their products in good yields. Thus, the synthesized catalyst proved versatile and can be used in reactions of carbon-carbon coupling well as in catalytic reduction may also be recovered and reused, which provides an environmentally friendly at the same characteristic.O presente trabalho apresenta a síntese de um novo catalisador de nanopartículas de paládio suportadas em nanotubos de carbono de paredes múltiplas contendo nitrogênio (Pd@CNxNCPM) 1 e sua utilização em reações de acoplamento carbono-carbono (Suzuki e Heck) bem como em reações de Hidrogenações catalíticas (reduções de duplas ligações C-C e redução de nitrocompostos). A estratégia sintética utilizada permitiu a obtenção do catalisador de maneira simples, em curto tempo reacional e de maneira eficiente e sem a presença de agentes estabilizantes externos. Para isso foi empregado como precursor de paládio o sal hexacloropaladato IV de potássio e como agente redutor, hidrazina monohidratada sem a necessidade de agentes estabilizantes para o controle da nucleação e tamanho de nanopartículas. O sistema catalítico foi caracterizado quanto sua morfologia: dispersão, tamanho e forma de nanopartículas através de microscopia eletrônica de varredura. Também foi realizada espectroscopia Raman do catalisador bem como determinação do teor de paládio. Após devidamente analisado o catalisador, o mesmo foi testado para reações de acoplamento carbono-carbono de Suzuki e Heck levando a formação dos respectivos produtos com rendimentos de 70-> 95% para os acoplamentos de Suzuki e 75-> 95% para Heck. Para as sínteses em questão foram usados 0,5 mol% de catalisador (baseados na massa de paládio) para Suzuki e 10 mol% para Heck. Cabe salientar que o catalisador se mostra estável nas condições reacionais testadas, sendo observada a possibilidade de reuso deste sistema por ciclos reacionais adicionais, sem perdas de eficiência para o acoplamento de Suzuki. Ainda, o catalisador se mostrou eficiente para hidrogenações catalíticas quimiosseletivas de ligações de carbono-carbono insaturadas e nitrocompostos levando aos respectivos produtos em bons rendimentos. Dessa forma o catalisador sintetizado se mostrou versátil, sendo possível ser utilizado em reações de acoplamento carbono-carbono bem como em reduções catalíticas, também pode ser recuperado e reutilizado, o que confere ao mesmo uma característica ambientalmente correta.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESporUniversidade Federal de Santa MariaCentro de Ciências Naturais e ExatasPrograma de Pós-Graduação em QuímicaUFSMBrasilQuímicaAttribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessNanotubos de carbono dopados com nitrogênioNanopartículas de paládioCatáliseMulti walled carbon nanotubes doped with nitrogenPaladium nanoparticlesCatalysisCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICANanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catáliseMulti walled carbon nanotubes doped with nitrogen and decorated with paladium nanoparticles and their apllications in catalysis reactionsinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisRodrigues, Oscar Endrigo Dorneleshttp://lattes.cnpq.br/6536519955416085Emmerich, Daniel Jacinthohttp://lattes.cnpq.br/8251907460764870Alves, Elenilson Freitashttp://lattes.cnpq.br/5541226399395863Giacomelli, Cristianohttp://lattes.cnpq.br/1429116139250396Ilha, Viniciushttp://lattes.cnpq.br/3882671719676564http://lattes.cnpq.br/6558536357135507Vargas, Josimar10060000000060009fef019-ac43-4d8b-83d3-3565e4686d7b2fe4fd27-125e-435a-a95b-56a041287414a62807af-3e21-47f7-ac84-903d01d9d3f8187c6d50-eb76-4941-9300-bfb6050501d47dc7675e-3956-47d1-a76a-e3797351c4a7a297d48a-1e32-4b0b-884b-f34573af5115reponame:Manancial - Repositório Digital da UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSMORIGINALTES_PPGQUÍMICA_2016_VARGAS_JOSIMAR.pdfTES_PPGQUÍMICA_2016_VARGAS_JOSIMAR.pdfTese de Doutoradoapplication/pdf8204719http://repositorio.ufsm.br/bitstream/1/11952/1/TES_PPGQU%c3%8dMICA_2016_VARGAS_JOSIMAR.pdf7eba519c0ed2ae98cde3b803d758c625MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; 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dc.title.por.fl_str_mv Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
dc.title.alternative.eng.fl_str_mv Multi walled carbon nanotubes doped with nitrogen and decorated with paladium nanoparticles and their apllications in catalysis reactions
title Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
spellingShingle Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
Vargas, Josimar
Nanotubos de carbono dopados com nitrogênio
Nanopartículas de paládio
Catálise
Multi walled carbon nanotubes doped with nitrogen
Paladium nanoparticles
Catalysis
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
title_full Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
title_fullStr Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
title_full_unstemmed Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
title_sort Nanotubos de carbono de paredes múltiplas dopados com nitrogênio e decorados com nanopartículas de paládio e suas aplicações em reações de catálise
author Vargas, Josimar
author_facet Vargas, Josimar
author_role author
dc.contributor.advisor1.fl_str_mv Rodrigues, Oscar Endrigo Dorneles
dc.contributor.advisor1Lattes.fl_str_mv http://lattes.cnpq.br/6536519955416085
dc.contributor.referee1.fl_str_mv Emmerich, Daniel Jacintho
dc.contributor.referee1Lattes.fl_str_mv http://lattes.cnpq.br/8251907460764870
dc.contributor.referee2.fl_str_mv Alves, Elenilson Freitas
dc.contributor.referee2Lattes.fl_str_mv http://lattes.cnpq.br/5541226399395863
dc.contributor.referee3.fl_str_mv Giacomelli, Cristiano
dc.contributor.referee3Lattes.fl_str_mv http://lattes.cnpq.br/1429116139250396
dc.contributor.referee4.fl_str_mv Ilha, Vinicius
dc.contributor.referee4Lattes.fl_str_mv http://lattes.cnpq.br/3882671719676564
dc.contributor.authorLattes.fl_str_mv http://lattes.cnpq.br/6558536357135507
dc.contributor.author.fl_str_mv Vargas, Josimar
contributor_str_mv Rodrigues, Oscar Endrigo Dorneles
Emmerich, Daniel Jacintho
Alves, Elenilson Freitas
Giacomelli, Cristiano
Ilha, Vinicius
dc.subject.por.fl_str_mv Nanotubos de carbono dopados com nitrogênio
Nanopartículas de paládio
Catálise
topic Nanotubos de carbono dopados com nitrogênio
Nanopartículas de paládio
Catálise
Multi walled carbon nanotubes doped with nitrogen
Paladium nanoparticles
Catalysis
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
dc.subject.eng.fl_str_mv Multi walled carbon nanotubes doped with nitrogen
Paladium nanoparticles
Catalysis
dc.subject.cnpq.fl_str_mv CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
description The present work describes the synthesis of a new catalyst of palladium nanoparticles supported on multi-walled carbon nanotubes containing nitrogen (Pd@CNxNCPM) 1 and its use in carbon-carbon coupling reactions (Suzuki and Heck) as well as reactions catalytic hydrogenation (reduction of double C-C bonds and nitro compounds reduction). The synthetic strategy employed afforded the simple way to obtain the catalyst with reaction in a short time and efficiently. To this was employed as the palladium precursor, the salt potassium hexacloropalladate IV and hydrazine monohydrate as the reducing agent, without the need for stabilizing agents for the control of nucleation and size of nanoparticle. The catalyst system was characterized as its morphology: dispersion, size and shape of nanoparticles by scanning electron microscopy. Also the catalyst was performed Raman spectroscopy and determination of amount of palladium. After characterization the catalyst, it was tested for coupling reactions of carbon-carbon: Suzuki and Heck leading to the formation of their products with 70-> 95% for Suzuki coupling and 75-> 95% for Heck. For the synthesis in question were used 0.5 mol% of catalyst (based amount of palladium) for Suzuki and 10 mol% for Heck. It should be noted that the catalyst shown stable in the reaction conditions tested, and observed the possibility of reuse of this system for additional reaction cycles without loss of efficiency for the Suzuki coupling. Also, the catalyst was efficient and chemoselectiv for catalytic hydrogenations of unsaturated carbon-carbon bonds and nitro compounds leading to their products in good yields. Thus, the synthesized catalyst proved versatile and can be used in reactions of carbon-carbon coupling well as in catalytic reduction may also be recovered and reused, which provides an environmentally friendly at the same characteristic.
publishDate 2016
dc.date.issued.fl_str_mv 2016-02-05
dc.date.accessioned.fl_str_mv 2017-11-01T13:26:07Z
dc.date.available.fl_str_mv 2017-11-01T13:26:07Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
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rights_invalid_str_mv Attribution-NonCommercial-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
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dc.publisher.none.fl_str_mv Universidade Federal de Santa Maria
Centro de Ciências Naturais e Exatas
dc.publisher.program.fl_str_mv Programa de Pós-Graduação em Química
dc.publisher.initials.fl_str_mv UFSM
dc.publisher.country.fl_str_mv Brasil
dc.publisher.department.fl_str_mv Química
publisher.none.fl_str_mv Universidade Federal de Santa Maria
Centro de Ciências Naturais e Exatas
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