Immobilization of complex ruthenium in mesoporous silica
Autor(a) principal: | |
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Data de Publicação: | 2013 |
Tipo de documento: | Dissertação |
Idioma: | por |
Título da fonte: | Biblioteca Digital de Teses e Dissertações da UFC |
Texto Completo: | http://www.teses.ufc.br/tde_busca/arquivo.php?codArquivo=11972 |
Resumo: | In recent years, mesoporous silica has attracted considerable scientifical and industrial interest. This material possess physical and chemical properties, which makes it to be used in a variety of applications. These properties include thermal stability, mechanical strength and low solubility, which makes it an ideal matrix support for catalysts. The heterogeneous catalysis has the advantage of separating catalyst from the reaction medium, which justifies the interest in heterogeneous catalysts. Coordination compounds are widely used in homogeneous catalytic processes, based on this there is a growing interest in producing catalytic systems onto heterogeneous silica matrices making very interesting materials. In this work, ruthenium complexes, [RuIICl2(dppb)(PPh3)] and [RuIIICl3(dppb)(OH2)] were synthesized and immobilized onto mesoporous silica matrices modified with aminopropyl and bipyridine groups forming the systems known as Si-apts-bipy-RuIICl2dppb and Si-apts-[bipy-RuIIICl2dppb]Cl-. These systems were characterized by spectroscopic techniques (FTIR, NMR and electronic absorption), electrochemical (cyclic and square wave voltammetry), thermogravimetry (TG), isotherms of adsorption / desorption of N2 and elemental analysis (CHN). The N2 adsorption isotherms using BJH (Barret, Joyner and Halenda) method for matrices shows the synthesized material has characteristics of micro and mesoporous with predominantly mesopore size. Si-apts-bipy-RuIICl2dppb system was the only one that showed catalytic activity in the reaction of hydrogenation of acetophenone with a yield of 53%. The development of catalysts in solid matrices is an area of great interest, which has justified this work. |
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info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisImmobilization of complex ruthenium in mesoporous silicaImobilizaÃÃo de complexos de rutÃnio em matriz de sÃlica mesoporosa2013-07-31Jackson Rodrigues de Sousa41560922320http://lattes.cnpq.br/016849900668393602439203343http://lattes.cnpq.br/2247810507943396Ricardo Douglas de Sousa BernardoUniversidade Federal do CearÃPrograma de PÃs-GraduaÃÃo em QuÃmica UFCBRSÃlica Modificada CatÃlise heterogÃneaSilica Modified Phosphines Heterogeneous catalysisQUIMICA INORGANICAIn recent years, mesoporous silica has attracted considerable scientifical and industrial interest. This material possess physical and chemical properties, which makes it to be used in a variety of applications. These properties include thermal stability, mechanical strength and low solubility, which makes it an ideal matrix support for catalysts. The heterogeneous catalysis has the advantage of separating catalyst from the reaction medium, which justifies the interest in heterogeneous catalysts. Coordination compounds are widely used in homogeneous catalytic processes, based on this there is a growing interest in producing catalytic systems onto heterogeneous silica matrices making very interesting materials. In this work, ruthenium complexes, [RuIICl2(dppb)(PPh3)] and [RuIIICl3(dppb)(OH2)] were synthesized and immobilized onto mesoporous silica matrices modified with aminopropyl and bipyridine groups forming the systems known as Si-apts-bipy-RuIICl2dppb and Si-apts-[bipy-RuIIICl2dppb]Cl-. These systems were characterized by spectroscopic techniques (FTIR, NMR and electronic absorption), electrochemical (cyclic and square wave voltammetry), thermogravimetry (TG), isotherms of adsorption / desorption of N2 and elemental analysis (CHN). The N2 adsorption isotherms using BJH (Barret, Joyner and Halenda) method for matrices shows the synthesized material has characteristics of micro and mesoporous with predominantly mesopore size. Si-apts-bipy-RuIICl2dppb system was the only one that showed catalytic activity in the reaction of hydrogenation of acetophenone with a yield of 53%. The development of catalysts in solid matrices is an area of great interest, which has justified this work.A sÃlica mesoporosa à um material bastante versÃtil, com porosidade fÃcil de ser moldada tanto em forma quanto em tamanho, alÃm de possuir propriedades fÃsicas e quÃmicas que lhe possibilitam diversas aplicaÃÃes. Dessas propriedades destacamos a sua estabilidade tÃrmica, sua resistÃncia mecÃnica e sua pouca solubilidade as quais a tornam um suporte ideal para catalisadores. Nesse sentido, o uso de compostos de coordenaÃÃo ancorados em matrizes sÃlidas torna-se um interessante sistema a ser estudado, tendo em vista as propriedades, jà bem conhecidas, de alguns complexos metÃlicos de atuarem em catÃlise homogÃnea. De acordo com dados na literatura hà um contÃnuo interesse na sÃntese e caracterizaÃÃo de materiais mesoestruturados aplicados a heterogeinizaÃÃo de catalisadores, como por exemplo, o uso de compostos de coordenaÃÃo. Neste trabalho os complexos de rutÃnio, [RuIICl2(dppb)(PPh3)] e [RuIIICl3(dppb)(OH2)] foram sintetizados e imobilizados em matrizes de sÃlica mesoporosa modificada com grupos aminopropil e bipiridinÃcos, formando os sistemas denominados como Si-apts-bipy-RuIICl2dppb e Si-apts-[bipy-RuIIICl2dppb]Cl. Estes sistemas foram caracterizados por tÃcnicas espectroscÃpicas (FTIR, UV-Vis e RMN de 13C, 29Si e 31P), eletroquÃmicas (voltametria CÃclica e Voltametria de onda quadrada), termogravimÃtricas (TG), isotermas de adsorÃÃo/desorÃÃo de N2 e anÃlise elementar (CHN). As isotermas de N2 para adsorÃÃo pelo mÃtodo BJH (Barret, Joyner e Halenda) para as matrizes indicam que o material sintetizado neste trabalho apresenta caraterÃsticas micro e mesoporosas com predominÃncia de mesoporos. Dos materiais sintetizados apenas o sistema Si-apts-bipy-RuIICl2dppb apresentou atividade catalÃtica na reaÃÃo de hidrogenaÃÃo da acetofenona com um rendimento de 53%. O desenvolvimento de catalisadores em matrizes sÃlidas à uma Ãrea ampla e de grande interesse o que justifica o desenvolvimento deste trabalho.CoordenaÃÃo de AperfeiÃoamento de Pessoal de NÃvel Superiorhttp://www.teses.ufc.br/tde_busca/arquivo.php?codArquivo=11972application/pdfinfo:eu-repo/semantics/openAccessporreponame:Biblioteca Digital de Teses e Dissertações da UFCinstname:Universidade Federal do Cearáinstacron:UFC2019-01-21T11:25:45Zmail@mail.com - |
dc.title.en.fl_str_mv |
Immobilization of complex ruthenium in mesoporous silica |
dc.title.alternative.pt.fl_str_mv |
ImobilizaÃÃo de complexos de rutÃnio em matriz de sÃlica mesoporosa |
title |
Immobilization of complex ruthenium in mesoporous silica |
spellingShingle |
Immobilization of complex ruthenium in mesoporous silica Ricardo Douglas de Sousa Bernardo SÃlica Modificada CatÃlise heterogÃnea Silica Modified Phosphines Heterogeneous catalysis QUIMICA INORGANICA |
title_short |
Immobilization of complex ruthenium in mesoporous silica |
title_full |
Immobilization of complex ruthenium in mesoporous silica |
title_fullStr |
Immobilization of complex ruthenium in mesoporous silica |
title_full_unstemmed |
Immobilization of complex ruthenium in mesoporous silica |
title_sort |
Immobilization of complex ruthenium in mesoporous silica |
author |
Ricardo Douglas de Sousa Bernardo |
author_facet |
Ricardo Douglas de Sousa Bernardo |
author_role |
author |
dc.contributor.advisor1.fl_str_mv |
Jackson Rodrigues de Sousa |
dc.contributor.advisor1ID.fl_str_mv |
41560922320 |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/0168499006683936 |
dc.contributor.authorID.fl_str_mv |
02439203343 |
dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/2247810507943396 |
dc.contributor.author.fl_str_mv |
Ricardo Douglas de Sousa Bernardo |
contributor_str_mv |
Jackson Rodrigues de Sousa |
dc.subject.por.fl_str_mv |
SÃlica Modificada CatÃlise heterogÃnea |
topic |
SÃlica Modificada CatÃlise heterogÃnea Silica Modified Phosphines Heterogeneous catalysis QUIMICA INORGANICA |
dc.subject.eng.fl_str_mv |
Silica Modified Phosphines Heterogeneous catalysis |
dc.subject.cnpq.fl_str_mv |
QUIMICA INORGANICA |
dc.description.sponsorship.fl_txt_mv |
CoordenaÃÃo de AperfeiÃoamento de Pessoal de NÃvel Superior |
dc.description.abstract.por.fl_txt_mv |
In recent years, mesoporous silica has attracted considerable scientifical and industrial interest. This material possess physical and chemical properties, which makes it to be used in a variety of applications. These properties include thermal stability, mechanical strength and low solubility, which makes it an ideal matrix support for catalysts. The heterogeneous catalysis has the advantage of separating catalyst from the reaction medium, which justifies the interest in heterogeneous catalysts. Coordination compounds are widely used in homogeneous catalytic processes, based on this there is a growing interest in producing catalytic systems onto heterogeneous silica matrices making very interesting materials. In this work, ruthenium complexes, [RuIICl2(dppb)(PPh3)] and [RuIIICl3(dppb)(OH2)] were synthesized and immobilized onto mesoporous silica matrices modified with aminopropyl and bipyridine groups forming the systems known as Si-apts-bipy-RuIICl2dppb and Si-apts-[bipy-RuIIICl2dppb]Cl-. These systems were characterized by spectroscopic techniques (FTIR, NMR and electronic absorption), electrochemical (cyclic and square wave voltammetry), thermogravimetry (TG), isotherms of adsorption / desorption of N2 and elemental analysis (CHN). The N2 adsorption isotherms using BJH (Barret, Joyner and Halenda) method for matrices shows the synthesized material has characteristics of micro and mesoporous with predominantly mesopore size. Si-apts-bipy-RuIICl2dppb system was the only one that showed catalytic activity in the reaction of hydrogenation of acetophenone with a yield of 53%. The development of catalysts in solid matrices is an area of great interest, which has justified this work. A sÃlica mesoporosa à um material bastante versÃtil, com porosidade fÃcil de ser moldada tanto em forma quanto em tamanho, alÃm de possuir propriedades fÃsicas e quÃmicas que lhe possibilitam diversas aplicaÃÃes. Dessas propriedades destacamos a sua estabilidade tÃrmica, sua resistÃncia mecÃnica e sua pouca solubilidade as quais a tornam um suporte ideal para catalisadores. Nesse sentido, o uso de compostos de coordenaÃÃo ancorados em matrizes sÃlidas torna-se um interessante sistema a ser estudado, tendo em vista as propriedades, jà bem conhecidas, de alguns complexos metÃlicos de atuarem em catÃlise homogÃnea. De acordo com dados na literatura hà um contÃnuo interesse na sÃntese e caracterizaÃÃo de materiais mesoestruturados aplicados a heterogeinizaÃÃo de catalisadores, como por exemplo, o uso de compostos de coordenaÃÃo. Neste trabalho os complexos de rutÃnio, [RuIICl2(dppb)(PPh3)] e [RuIIICl3(dppb)(OH2)] foram sintetizados e imobilizados em matrizes de sÃlica mesoporosa modificada com grupos aminopropil e bipiridinÃcos, formando os sistemas denominados como Si-apts-bipy-RuIICl2dppb e Si-apts-[bipy-RuIIICl2dppb]Cl. Estes sistemas foram caracterizados por tÃcnicas espectroscÃpicas (FTIR, UV-Vis e RMN de 13C, 29Si e 31P), eletroquÃmicas (voltametria CÃclica e Voltametria de onda quadrada), termogravimÃtricas (TG), isotermas de adsorÃÃo/desorÃÃo de N2 e anÃlise elementar (CHN). As isotermas de N2 para adsorÃÃo pelo mÃtodo BJH (Barret, Joyner e Halenda) para as matrizes indicam que o material sintetizado neste trabalho apresenta caraterÃsticas micro e mesoporosas com predominÃncia de mesoporos. Dos materiais sintetizados apenas o sistema Si-apts-bipy-RuIICl2dppb apresentou atividade catalÃtica na reaÃÃo de hidrogenaÃÃo da acetofenona com um rendimento de 53%. O desenvolvimento de catalisadores em matrizes sÃlidas à uma Ãrea ampla e de grande interesse o que justifica o desenvolvimento deste trabalho. |
description |
In recent years, mesoporous silica has attracted considerable scientifical and industrial interest. This material possess physical and chemical properties, which makes it to be used in a variety of applications. These properties include thermal stability, mechanical strength and low solubility, which makes it an ideal matrix support for catalysts. The heterogeneous catalysis has the advantage of separating catalyst from the reaction medium, which justifies the interest in heterogeneous catalysts. Coordination compounds are widely used in homogeneous catalytic processes, based on this there is a growing interest in producing catalytic systems onto heterogeneous silica matrices making very interesting materials. In this work, ruthenium complexes, [RuIICl2(dppb)(PPh3)] and [RuIIICl3(dppb)(OH2)] were synthesized and immobilized onto mesoporous silica matrices modified with aminopropyl and bipyridine groups forming the systems known as Si-apts-bipy-RuIICl2dppb and Si-apts-[bipy-RuIIICl2dppb]Cl-. These systems were characterized by spectroscopic techniques (FTIR, NMR and electronic absorption), electrochemical (cyclic and square wave voltammetry), thermogravimetry (TG), isotherms of adsorption / desorption of N2 and elemental analysis (CHN). The N2 adsorption isotherms using BJH (Barret, Joyner and Halenda) method for matrices shows the synthesized material has characteristics of micro and mesoporous with predominantly mesopore size. Si-apts-bipy-RuIICl2dppb system was the only one that showed catalytic activity in the reaction of hydrogenation of acetophenone with a yield of 53%. The development of catalysts in solid matrices is an area of great interest, which has justified this work. |
publishDate |
2013 |
dc.date.issued.fl_str_mv |
2013-07-31 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/masterThesis |
status_str |
publishedVersion |
format |
masterThesis |
dc.identifier.uri.fl_str_mv |
http://www.teses.ufc.br/tde_busca/arquivo.php?codArquivo=11972 |
url |
http://www.teses.ufc.br/tde_busca/arquivo.php?codArquivo=11972 |
dc.language.iso.fl_str_mv |
por |
language |
por |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.publisher.none.fl_str_mv |
Universidade Federal do Cearà |
dc.publisher.program.fl_str_mv |
Programa de PÃs-GraduaÃÃo em QuÃmica |
dc.publisher.initials.fl_str_mv |
UFC |
dc.publisher.country.fl_str_mv |
BR |
publisher.none.fl_str_mv |
Universidade Federal do Cearà |
dc.source.none.fl_str_mv |
reponame:Biblioteca Digital de Teses e Dissertações da UFC instname:Universidade Federal do Ceará instacron:UFC |
reponame_str |
Biblioteca Digital de Teses e Dissertações da UFC |
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Biblioteca Digital de Teses e Dissertações da UFC |
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Universidade Federal do Ceará |
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UFC |
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UFC |
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mail@mail.com |
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1643295193017876480 |