Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II)
Ano de defesa: | 2016 |
---|---|
Autor(a) principal: | |
Orientador(a): | |
Banca de defesa: | , |
Tipo de documento: | Dissertação |
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/1/15248 |
Resumo: | The reaction of 1,4-α,α’-xylenediylbis(phenylphosphinic acid) (H2XBPP) with lead(II) generated two different extended structures: [Pb3(XBPP)3(H2O)] 1 and [Pb5(μ3-O)(XBPP)4(H2O)] 5 depending on the pH employed in the reaction. The difference be-tween the structures of 1 and 5 is the presence of a μ3-oxo bridge between three lead atoms. Through post synthetic structure modifications of 1, four new compounds with extended structures were synthesized. Three of these – [Pb4(XBPP)4(H2O)] 2, [Pb(XBPP)] 3 and [Pb2(XBPP)2(H2O)] 4 – are pseudo-polymorphs obtained by a re-versible dehydration/rehydration process. These transformations were observed in the polycrystalline powder as well as in single crystal. The hydrothermal reaction of 1 at pH 2 gave [Pb(HXBPP)2] 7. One pseudo-polymorph, [Pb5(μ3-O)(XBPP)4] 6, was ob-tained from the dehydration of 5. Six structures, 1 – 6, showed a very similar three-dimensional arrangement with the same pcu topology. Compound 7 had a two-dimen-sional extended structure with sql planar topology. The compounds synthesized in this work were characterized by elemental analysis, infrared and Raman spectroscopy, powder and single crystal X ray diffraction, thermogravimetric analysis and 31P solid state nuclear magnetic resonance. A kinetic study of the water loss and water uptake reactions, DFT calculations, and a gas adsorption study with N2, CO2 and water vapor were performed. |
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2019-01-08T15:01:33Z2019-01-08T15:01:33Z2016-09-09http://repositorio.ufsm.br/handle/1/15248The reaction of 1,4-α,α’-xylenediylbis(phenylphosphinic acid) (H2XBPP) with lead(II) generated two different extended structures: [Pb3(XBPP)3(H2O)] 1 and [Pb5(μ3-O)(XBPP)4(H2O)] 5 depending on the pH employed in the reaction. The difference be-tween the structures of 1 and 5 is the presence of a μ3-oxo bridge between three lead atoms. Through post synthetic structure modifications of 1, four new compounds with extended structures were synthesized. Three of these – [Pb4(XBPP)4(H2O)] 2, [Pb(XBPP)] 3 and [Pb2(XBPP)2(H2O)] 4 – are pseudo-polymorphs obtained by a re-versible dehydration/rehydration process. These transformations were observed in the polycrystalline powder as well as in single crystal. The hydrothermal reaction of 1 at pH 2 gave [Pb(HXBPP)2] 7. One pseudo-polymorph, [Pb5(μ3-O)(XBPP)4] 6, was ob-tained from the dehydration of 5. Six structures, 1 – 6, showed a very similar three-dimensional arrangement with the same pcu topology. Compound 7 had a two-dimen-sional extended structure with sql planar topology. The compounds synthesized in this work were characterized by elemental analysis, infrared and Raman spectroscopy, powder and single crystal X ray diffraction, thermogravimetric analysis and 31P solid state nuclear magnetic resonance. A kinetic study of the water loss and water uptake reactions, DFT calculations, and a gas adsorption study with N2, CO2 and water vapor were performed.A reação do 1,4-α,α’-xilenodiilabis(ácido fenilfosfínico) (H2XBPP) com PbII leva a formação de duas estruturas estendidas [Pb3(XBPP)3(H2O)] (1) e [Pb5(μ3-O)(XBPP)4(H2O)] (5) de acordo com o pH empregado na reação. Onde 5 diferencia-se de 1 pela presença de uma ponte μ3 oxo. Através de modificações estruturais pós sintéticas a estrutura 1 origina quatro novas estruturas. Três destas ([Pb4(XBPP)4(H2O)] (2), [Pb(XBPP)] (3) e [Pb2(XBPP)2(H2O)] (4)) são pseudopolimor-fos obtidos através de processos de desidratação/reidratação reversíveis, que são ob-servadas tanto no material policristalino, como em monocristal. A estrutura [Pb(HXBPP)2] (7) é formada a partir da recristalização da estrutura 1 em reação hidro-termal em pH 2. A estrutura 5 apresenta apenas um pseudopolimorfo [Pb5(μ3-O)(XBPP)4] (6) decorrente de desidratação. Com exceção 7 que é uma estrutura es-tendida bidimensional e apresenta uma topologia planar sql, todas as outras seis es-truturas têm um arranjo tridimensional bastante similar e apresentam a mesma topo-logia (pcu). As estruturas sintetizadas neste trabalho foram caracterizadas por análise elementar, espectroscopia de infravermelho, difração de raios-x do pó e em monocris-tal, análise termogravimétrica e ressonância magnética nuclear. Foi realizado também um estudo cinético dos processos de entrada e saída de água, bem como cálculos de DFT e um estudo de adsorção de gases como N2, CO2 e vapor de água.porUniversidade 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/openAccessEstruturas estendidasDesidratação/reidrataçãoCálculos de DFT e adsorção de gasesExtended structuresDehydration/rehydrationDFT calculations and gas adsorptionCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICADinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II)Structural dynamism and single crystal to single crystal transformation of novel chumbo(II) extended structure compoundsinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisBurrow, Robert Alanhttp://lattes.cnpq.br/5452385625669684Tirloni, Bárbarahttp://lattes.cnpq.br/2866324870100182Vicenti, Juliano Rosa de Menezeshttp://lattes.cnpq.br/8692948387211118http://lattes.cnpq.br/4005723344102461Menezes, Bryan Brummelhaus de100600000000600da77a491-2340-4bec-afed-a9ed5dd5092ae98f124a-30b7-4de7-b2e2-47498f39fba3d616ae6f-f10b-4b8d-8598-c3699525193932dd1979-e302-4983-b319-17966b600492reponame:Manancial - Repositório Digital da UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSMORIGINALDIS_PPGQUIMICA_2016_MENEZES_BRYAN.pdfDIS_PPGQUIMICA_2016_MENEZES_BRYAN.pdfDissertação de Mestradoapplication/pdf5647112http://repositorio.ufsm.br/bitstream/1/15248/1/DIS_PPGQUIMICA_2016_MENEZES_BRYAN.pdf8a54e53ac2317b610b2fd618c34905c9MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; 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dc.title.por.fl_str_mv |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) |
dc.title.alternative.eng.fl_str_mv |
Structural dynamism and single crystal to single crystal transformation of novel chumbo(II) extended structure compounds |
title |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) |
spellingShingle |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) Menezes, Bryan Brummelhaus de Estruturas estendidas Desidratação/reidratação Cálculos de DFT e adsorção de gases Extended structures Dehydration/rehydration DFT calculations and gas adsorption CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
title_short |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) |
title_full |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) |
title_fullStr |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) |
title_full_unstemmed |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) |
title_sort |
Dinamismo estrutural e transformação monocristal para monocristal de novas estruturas estendidas de chumbo(II) |
author |
Menezes, Bryan Brummelhaus de |
author_facet |
Menezes, Bryan Brummelhaus de |
author_role |
author |
dc.contributor.advisor1.fl_str_mv |
Burrow, Robert Alan |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/5452385625669684 |
dc.contributor.referee1.fl_str_mv |
Tirloni, Bárbara |
dc.contributor.referee1Lattes.fl_str_mv |
http://lattes.cnpq.br/2866324870100182 |
dc.contributor.referee2.fl_str_mv |
Vicenti, Juliano Rosa de Menezes |
dc.contributor.referee2Lattes.fl_str_mv |
http://lattes.cnpq.br/8692948387211118 |
dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/4005723344102461 |
dc.contributor.author.fl_str_mv |
Menezes, Bryan Brummelhaus de |
contributor_str_mv |
Burrow, Robert Alan Tirloni, Bárbara Vicenti, Juliano Rosa de Menezes |
dc.subject.por.fl_str_mv |
Estruturas estendidas Desidratação/reidratação Cálculos de DFT e adsorção de gases |
topic |
Estruturas estendidas Desidratação/reidratação Cálculos de DFT e adsorção de gases Extended structures Dehydration/rehydration DFT calculations and gas adsorption CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
dc.subject.eng.fl_str_mv |
Extended structures Dehydration/rehydration DFT calculations and gas adsorption |
dc.subject.cnpq.fl_str_mv |
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA |
description |
The reaction of 1,4-α,α’-xylenediylbis(phenylphosphinic acid) (H2XBPP) with lead(II) generated two different extended structures: [Pb3(XBPP)3(H2O)] 1 and [Pb5(μ3-O)(XBPP)4(H2O)] 5 depending on the pH employed in the reaction. The difference be-tween the structures of 1 and 5 is the presence of a μ3-oxo bridge between three lead atoms. Through post synthetic structure modifications of 1, four new compounds with extended structures were synthesized. Three of these – [Pb4(XBPP)4(H2O)] 2, [Pb(XBPP)] 3 and [Pb2(XBPP)2(H2O)] 4 – are pseudo-polymorphs obtained by a re-versible dehydration/rehydration process. These transformations were observed in the polycrystalline powder as well as in single crystal. The hydrothermal reaction of 1 at pH 2 gave [Pb(HXBPP)2] 7. One pseudo-polymorph, [Pb5(μ3-O)(XBPP)4] 6, was ob-tained from the dehydration of 5. Six structures, 1 – 6, showed a very similar three-dimensional arrangement with the same pcu topology. Compound 7 had a two-dimen-sional extended structure with sql planar topology. The compounds synthesized in this work were characterized by elemental analysis, infrared and Raman spectroscopy, powder and single crystal X ray diffraction, thermogravimetric analysis and 31P solid state nuclear magnetic resonance. A kinetic study of the water loss and water uptake reactions, DFT calculations, and a gas adsorption study with N2, CO2 and water vapor were performed. |
publishDate |
2016 |
dc.date.issued.fl_str_mv |
2016-09-09 |
dc.date.accessioned.fl_str_mv |
2019-01-08T15:01:33Z |
dc.date.available.fl_str_mv |
2019-01-08T15:01:33Z |
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/1/15248 |
url |
http://repositorio.ufsm.br/handle/1/15248 |
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 |
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