Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais
Ano de defesa: | 2017 |
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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: |
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/1/13614 |
Resumo: | This work shows the synthesis of unpublished Zn(II), Cd(II) and Pd(II) complexes with bis-cated triazene molecules, including macrocycles. Together these compounds, a series of symmetrical ortho-halogenated single-catenad Au(I) triazenide complexes, previously synthesized by Zambiazi (2013), were used with the main purpose of evaluating the pendulum effect that the halogen substituents provoke on the linear coordination geometry of the N1– AuPPh3 fragment, as a consequence of the intramolecular interactions, besides the studies of the intermolecular interactions such as Halogen···Halogen and Halogen···π approaching the supramolecular cluster as delimitation of the crystalline arrangement. The macrocyclic complexes were evaluated by the triad of parameters (geometric, energetic and topological) with the objective of proposing crystallization mechanisms through retrocrystallization, besides the evaluation of the effect of the crystallization solvent present in compounds 6·Py, 7·Py and 8·Py to understand the consequences and importance that these solvates cause to the crystalline packaging. The acyclic bis-triazenide complexes of Pd(II) with different spacers between the triazoalilic chains (1,4-butyl fragment in compound 9 and 2,6-pyridyl fragment in compound 10) were compared on their different modes of coordination to the metal center. Compound 9 showed the expected lantern effect while compound 10 showed an unusual coordination of the central nitrogen atom of the triazenide chain. Both compounds were also analyzed through the topological approach in order to understand the stability of their molecular models and proposition of the crystallization mechanism of each compound. |
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2018-06-28T21:42:38Z2018-06-28T21:42:38Z2017-09-15http://repositorio.ufsm.br/handle/1/13614This work shows the synthesis of unpublished Zn(II), Cd(II) and Pd(II) complexes with bis-cated triazene molecules, including macrocycles. Together these compounds, a series of symmetrical ortho-halogenated single-catenad Au(I) triazenide complexes, previously synthesized by Zambiazi (2013), were used with the main purpose of evaluating the pendulum effect that the halogen substituents provoke on the linear coordination geometry of the N1– AuPPh3 fragment, as a consequence of the intramolecular interactions, besides the studies of the intermolecular interactions such as Halogen···Halogen and Halogen···π approaching the supramolecular cluster as delimitation of the crystalline arrangement. The macrocyclic complexes were evaluated by the triad of parameters (geometric, energetic and topological) with the objective of proposing crystallization mechanisms through retrocrystallization, besides the evaluation of the effect of the crystallization solvent present in compounds 6·Py, 7·Py and 8·Py to understand the consequences and importance that these solvates cause to the crystalline packaging. The acyclic bis-triazenide complexes of Pd(II) with different spacers between the triazoalilic chains (1,4-butyl fragment in compound 9 and 2,6-pyridyl fragment in compound 10) were compared on their different modes of coordination to the metal center. Compound 9 showed the expected lantern effect while compound 10 showed an unusual coordination of the central nitrogen atom of the triazenide chain. Both compounds were also analyzed through the topological approach in order to understand the stability of their molecular models and proposition of the crystallization mechanism of each compound.Este trabalho apresenta a síntese de complexos inéditos de Zn(II), Cd(II) e Pd(II) com moléculas de triazeno biscatenados, incluindo macrocíclos. Juntamente a estes compostos foram utilizados uma série de complexos triazenidos de Au(I) monocatenados orto-halogenados simétricos, previamente sintetizados em Zambiazi (2013), com a finalidade principal de avaliação do efeito pêndulo que os substituintes halogenados provocam sobre a geometria de coordenação linear do fragmento N1–AuPPh3, em consequência das interações intramoleculares, além dos estudos das interações intermoleculares tais como Halogênio···Halogênio e Halogênio···! abordando o cluster supramolecular como delimitação do arranjo cristalino. Os complexos macrocíclicos foram avaliados pela tríade de parâmetros (geométricos, energéticos e topológicos) com o objetivo de propor mecanismos de cristalização através da retrocristalização, além de avaliar o efeito do solvente de cristalização presente nos compostos 6·Py, 7·Py e 8·Py e entender quais as consequências e a importância que esses solvatos acarretam ao empacotamento cristalino. Os complexos bis-triazenidos acíclicos de Pd(II), com diferentes espaçadores entre as cadeias triazoalílicas (um fragmento butano 9 e o outro um apresentando como espaçador um fragmento piridina, 10), foram comparados quanto aos seus diferentes modos de coordenação ao centro metálico. O composto 9 apresentou o esperado efeito lanterna enquanto o composto 10 apresentou um incomum modo de coordenado do átomo de nitrogênio central da cadeia triazenida. Ambos compostos foram igualmente analisados através da abordagem topológica com a finalidade de compreender a estabilidade dos modelos moleculares e propor mecanismos de cristalização.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/openAccessComplexos triazenidosEstruturas cristalinasQuímica supramolecularEngenharia de cristaisTriazenide compoundsCrystals structuresSupramolecular chemistryCrystal engineeringCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICAEstudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristaisMolecular and supramolecular studies of triazenides complexes with transition metals: an approach to crystal engineering.info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisHörner, Manfredohttp://lattes.cnpq.br/8922528250830998Nunes, Fabio Souzahttp://lattes.cnpq.br/7117607785614286Araki, Koitihttp://lattes.cnpq.br/9785076666437938Bresolin, Leandrohttp://lattes.cnpq.br/3961672079507969Martins, Marcos Antonio Pintohttp://lattes.cnpq.br/6457412713967642http://lattes.cnpq.br/5833091143764435Zambiazi, Priscilla Jussiane1006000000006007e7796b1-053d-4bbe-8e62-e769f0da5cea362da7d8-5946-4f2b-8ecd-f9f5df3600af3694402e-84bf-43d1-a3a8-562172c5265550b8dd02-6c73-4d05-b476-2e7ce82190b567ed52a8-91fa-4e1a-b8bb-f266fe5782ce60d6f462-2deb-40c5-aa32-3dbcf79699bbreponame:Biblioteca Digital de Teses e Dissertações do UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSMORIGINALTES_PPGQUIMICA_2017_ZAMBIAZI_PRISCILLA.pdfTES_PPGQUIMICA_2017_ZAMBIAZI_PRISCILLA.pdfTese de Doutoradoapplication/pdf58832772http://repositorio.ufsm.br/bitstream/1/13614/1/TES_PPGQUIMICA_2017_ZAMBIAZI_PRISCILLA.pdf06de8e0254de0f7fc206b1a3765e32b0MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; 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dc.title.por.fl_str_mv |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais |
dc.title.alternative.eng.fl_str_mv |
Molecular and supramolecular studies of triazenides complexes with transition metals: an approach to crystal engineering. |
title |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais |
spellingShingle |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais Zambiazi, Priscilla Jussiane Complexos triazenidos Estruturas cristalinas Química supramolecular Engenharia de cristais Triazenide compounds Crystals structures Supramolecular chemistry Crystal engineering CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
title_short |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais |
title_full |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais |
title_fullStr |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais |
title_full_unstemmed |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais |
title_sort |
Estudo molecular e supramolecular de complexos triazenidos com metais de transição: uma abordagem voltada à engenharia de cristais |
author |
Zambiazi, Priscilla Jussiane |
author_facet |
Zambiazi, Priscilla Jussiane |
author_role |
author |
dc.contributor.advisor1.fl_str_mv |
Hörner, Manfredo |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/8922528250830998 |
dc.contributor.referee1.fl_str_mv |
Nunes, Fabio Souza |
dc.contributor.referee1Lattes.fl_str_mv |
http://lattes.cnpq.br/7117607785614286 |
dc.contributor.referee2.fl_str_mv |
Araki, Koiti |
dc.contributor.referee2Lattes.fl_str_mv |
http://lattes.cnpq.br/9785076666437938 |
dc.contributor.referee3.fl_str_mv |
Bresolin, Leandro |
dc.contributor.referee3Lattes.fl_str_mv |
http://lattes.cnpq.br/3961672079507969 |
dc.contributor.referee4.fl_str_mv |
Martins, Marcos Antonio Pinto |
dc.contributor.referee4Lattes.fl_str_mv |
http://lattes.cnpq.br/6457412713967642 |
dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/5833091143764435 |
dc.contributor.author.fl_str_mv |
Zambiazi, Priscilla Jussiane |
contributor_str_mv |
Hörner, Manfredo Nunes, Fabio Souza Araki, Koiti Bresolin, Leandro Martins, Marcos Antonio Pinto |
dc.subject.por.fl_str_mv |
Complexos triazenidos Estruturas cristalinas Química supramolecular Engenharia de cristais |
topic |
Complexos triazenidos Estruturas cristalinas Química supramolecular Engenharia de cristais Triazenide compounds Crystals structures Supramolecular chemistry Crystal engineering CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
dc.subject.eng.fl_str_mv |
Triazenide compounds Crystals structures Supramolecular chemistry Crystal engineering |
dc.subject.cnpq.fl_str_mv |
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
description |
This work shows the synthesis of unpublished Zn(II), Cd(II) and Pd(II) complexes with bis-cated triazene molecules, including macrocycles. Together these compounds, a series of symmetrical ortho-halogenated single-catenad Au(I) triazenide complexes, previously synthesized by Zambiazi (2013), were used with the main purpose of evaluating the pendulum effect that the halogen substituents provoke on the linear coordination geometry of the N1– AuPPh3 fragment, as a consequence of the intramolecular interactions, besides the studies of the intermolecular interactions such as Halogen···Halogen and Halogen···π approaching the supramolecular cluster as delimitation of the crystalline arrangement. The macrocyclic complexes were evaluated by the triad of parameters (geometric, energetic and topological) with the objective of proposing crystallization mechanisms through retrocrystallization, besides the evaluation of the effect of the crystallization solvent present in compounds 6·Py, 7·Py and 8·Py to understand the consequences and importance that these solvates cause to the crystalline packaging. The acyclic bis-triazenide complexes of Pd(II) with different spacers between the triazoalilic chains (1,4-butyl fragment in compound 9 and 2,6-pyridyl fragment in compound 10) were compared on their different modes of coordination to the metal center. Compound 9 showed the expected lantern effect while compound 10 showed an unusual coordination of the central nitrogen atom of the triazenide chain. Both compounds were also analyzed through the topological approach in order to understand the stability of their molecular models and proposition of the crystallization mechanism of each compound. |
publishDate |
2017 |
dc.date.issued.fl_str_mv |
2017-09-15 |
dc.date.accessioned.fl_str_mv |
2018-06-28T21:42:38Z |
dc.date.available.fl_str_mv |
2018-06-28T21:42:38Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/doctoralThesis |
format |
doctoralThesis |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://repositorio.ufsm.br/handle/1/13614 |
url |
http://repositorio.ufsm.br/handle/1/13614 |
dc.language.iso.fl_str_mv |
por |
language |
por |
dc.relation.cnpq.fl_str_mv |
100600000000 |
dc.relation.confidence.fl_str_mv |
600 |
dc.relation.authority.fl_str_mv |
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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.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 |
dc.source.none.fl_str_mv |
reponame:Biblioteca Digital de Teses e Dissertações do UFSM instname:Universidade Federal de Santa Maria (UFSM) instacron:UFSM |
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UFSM |
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Biblioteca Digital de Teses e Dissertações do UFSM |
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