Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais

Detalhes bibliográficos
Autor(a) principal: Souza, Juliana Kelly Dionízio de
Data de Publicação: 2018
Tipo de documento: Tese
Idioma: por
Título da fonte: Biblioteca Digital de Teses e Dissertações da UFPB
Texto Completo: https://repositorio.ufpb.br/jspui/handle/123456789/14841
Resumo: The use of semiconductors as photocatalysts is a promising strategy in the treatment of organic pollutants. In this sense, the photocatalytic performance of lamellar potassium niobates and their protonated forms were tested for the degradation of the model dye Remazol Yelow Gold (RNL). The niobates (KNb3O8 and K4Nb6O17) were prepared by the polymeric precursor (PP) and solid state (SS) methods. The protonated forms HNb3O8.H2O and K4-xHxNb6O17, obtained by the PP method, were prepared via a ion exchange reaction using a HNO3 solution. The materials were characterized by X-ray di?raction (XDR), infrared (IR), Raman, ultraviolet visible (UV-vis), scanning electron microscopy (SEM), surface area (BET) and photoluminescence (PL). Theoretical Computational calculation were performed (DFT) to de?ne the structural and vibrational aspects of niobates in the potassium form. Their structures were characterized at long, medium and short range are in accordance with those in the literature. The theoretical studies of octahedron distortions showed that KNb3O8 has two types of distortion, where as K4Nb6O17 has four types. The octahedron with the largest distortion degree for K4Nb6O17 has a short Nb - O bond (high covalent character) and another much elongated one (with a transient character between the covalent and the ionic). It is observed that niobates in the potassium form have better photocatalytic performances when compared to either their protaned forms or P25. Studies to elucidate the mechanism of discoloration for the potassium niobates used suppressors of •OH, O•- 2 radicals, e- and h+. The results show that the mechanism of photocatalysis is indirect, that is, by the formation of •OH radicals . For KNb3O8 the formation of •OH radicals a high contribution of photogenerated e- in the conduction band is observed, whereas, both e- and h+ are responsible for the formation of these radicals for K4Nb6O17. For the RNL discoloration reaction using KNb3O8 reactional parameters were studied, such as pH, initial concentration of dye (C0), photocatalyst quantity and calcination temperature. Three reuse cycles were analyzed for potassium niobates, which indicated little loss of catalytic activity.
id UFPB_d3c7068c15919e045200fef3b3e3c779
oai_identifier_str oai:repositorio.ufpb.br:123456789/14841
network_acronym_str UFPB
network_name_str Biblioteca Digital de Teses e Dissertações da UFPB
repository_id_str
spelling Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentaisKNb3O8K4Nb6O17Distorção dos octaedrosFotocatáliseReúsoOctahedron distortionPhotocatalysisReuseCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICAThe use of semiconductors as photocatalysts is a promising strategy in the treatment of organic pollutants. In this sense, the photocatalytic performance of lamellar potassium niobates and their protonated forms were tested for the degradation of the model dye Remazol Yelow Gold (RNL). The niobates (KNb3O8 and K4Nb6O17) were prepared by the polymeric precursor (PP) and solid state (SS) methods. The protonated forms HNb3O8.H2O and K4-xHxNb6O17, obtained by the PP method, were prepared via a ion exchange reaction using a HNO3 solution. The materials were characterized by X-ray di?raction (XDR), infrared (IR), Raman, ultraviolet visible (UV-vis), scanning electron microscopy (SEM), surface area (BET) and photoluminescence (PL). Theoretical Computational calculation were performed (DFT) to de?ne the structural and vibrational aspects of niobates in the potassium form. Their structures were characterized at long, medium and short range are in accordance with those in the literature. The theoretical studies of octahedron distortions showed that KNb3O8 has two types of distortion, where as K4Nb6O17 has four types. The octahedron with the largest distortion degree for K4Nb6O17 has a short Nb - O bond (high covalent character) and another much elongated one (with a transient character between the covalent and the ionic). It is observed that niobates in the potassium form have better photocatalytic performances when compared to either their protaned forms or P25. Studies to elucidate the mechanism of discoloration for the potassium niobates used suppressors of •OH, O•- 2 radicals, e- and h+. The results show that the mechanism of photocatalysis is indirect, that is, by the formation of •OH radicals . For KNb3O8 the formation of •OH radicals a high contribution of photogenerated e- in the conduction band is observed, whereas, both e- and h+ are responsible for the formation of these radicals for K4Nb6O17. For the RNL discoloration reaction using KNb3O8 reactional parameters were studied, such as pH, initial concentration of dye (C0), photocatalyst quantity and calcination temperature. Three reuse cycles were analyzed for potassium niobates, which indicated little loss of catalytic activity.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESO uso de semicondutores como fotocatalisadores apresenta-se como estratégia promissora no tratamento de poluentes orgânicos. Nesse sentido, o desempenho fotocatalítico dos Niobatos de Potássio Lamelares e suas formas protonadas foi testado na reação de degradação do corante modelo Remazol Amarelo Ouro (RNL). Os niobatos (KNb3O8 e K4Nb6O17) foram preparados pelo método dos precursores poliméricos (PP) e estado sólido (ES). As formas protonadas, HNb3O8.H2O e K4−xHxNb6O17.nH2O, obtidas pelo método PP, foram preparadas por reação de troca iônica, utilizando uma solução de HNO3. Os niobatos foram caracterizados por difração de raios X (DRX), espectroscopia de absorção na região do infravermelho (IV), do ultravioleta - visível (UV-vis), Raman, fotoluminescência (PL) e microscopia eletrônica de varredura (MEV) em seguida área superficial (BET).Também foram realizados cálculos teóricos a nível DFT para elucidação de aspectos estruturais e vibracionais dos niobatos na forma potássica. Suas estruturas, caracterizadas a longo, médio e curto alcance, estão de acordo com as propostas pela literatura. Estudo teórico das distorções dos octaedros mostrou que o KNb3O8 possui dois tipos de distorções; já o K4Nb6O17 apresenta quatro tipos. O octaedro com maior grau de distorção do K4Nb6O17 possui uma ligação curta Nb-O (maior caráter covalente) e outra bem alongada (com caráter transiente entre o covalente e o iônico). Observa-se que os niobatos na forma potássica possuem os melhores desempenhos fotocatalíticos quando comparados às suas formas protonadas e ao P25. Foram feitos estudos para elucidar o mecanismo de descoloração para os Niobatos de Potássio, utilizando supressores de radicais •OH, O•− 2 e de e− e h+. Os resultados obtidos mostram que o mecanismo de fotocatálise é por via indireta, ou seja, pela formação dos radicais •OH. Para o KNb3O8 a formação dos radicais •OH tem contribuição majoritária dos e− fotogerados na BC; por outro lado, tanto os e− como os h+ são responsáveis pela formação desses radicais para o K4Nb6O17. Para a reação de descoloração utilizando o KNb3O8 parâmetros reacionais foram estudados, como pH, concentração inicial (C0) do corante, quantidade e variação da temperatura de calcinação do foto catalisador. Analisaram três ciclos de reúso para os Niobatos de Potássio, os quais indicam pouca perda de atividade catalítica.Universidade Federal da ParaíbaBrasilQuímicaPrograma de Pós-Graduação em QuímicaUFPBMaia, Ary da Silvahttp://lattes.cnpq.br/0234548596508203Souza, Juliana Kelly Dionízio de2019-06-26T17:57:32Z2019-06-262019-06-26T17:57:32Z2018-08-30info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesishttps://repositorio.ufpb.br/jspui/handle/123456789/14841porAttribution-NoDerivs 3.0 Brazilhttp://creativecommons.org/licenses/by-nd/3.0/br/info:eu-repo/semantics/openAccessreponame:Biblioteca Digital de Teses e Dissertações da UFPBinstname:Universidade Federal da Paraíba (UFPB)instacron:UFPB2019-06-26T17:57:32Zoai:repositorio.ufpb.br:123456789/14841Biblioteca Digital de Teses e Dissertaçõeshttps://repositorio.ufpb.br/PUBhttp://tede.biblioteca.ufpb.br:8080/oai/requestdiretoria@ufpb.br|| diretoria@ufpb.bropendoar:2019-06-26T17:57:32Biblioteca Digital de Teses e Dissertações da UFPB - Universidade Federal da Paraíba (UFPB)false
dc.title.none.fl_str_mv Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
title Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
spellingShingle Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
Souza, Juliana Kelly Dionízio de
KNb3O8
K4Nb6O17
Distorção dos octaedros
Fotocatálise
Reúso
Octahedron distortion
Photocatalysis
Reuse
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
title_full Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
title_fullStr Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
title_full_unstemmed Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
title_sort Avaliação fotocatalítica de niobatos lamelares: influência dos métodos de síntese, aspectos teóricos e experimentais
author Souza, Juliana Kelly Dionízio de
author_facet Souza, Juliana Kelly Dionízio de
author_role author
dc.contributor.none.fl_str_mv Maia, Ary da Silva
http://lattes.cnpq.br/0234548596508203
dc.contributor.author.fl_str_mv Souza, Juliana Kelly Dionízio de
dc.subject.por.fl_str_mv KNb3O8
K4Nb6O17
Distorção dos octaedros
Fotocatálise
Reúso
Octahedron distortion
Photocatalysis
Reuse
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
topic KNb3O8
K4Nb6O17
Distorção dos octaedros
Fotocatálise
Reúso
Octahedron distortion
Photocatalysis
Reuse
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
description The use of semiconductors as photocatalysts is a promising strategy in the treatment of organic pollutants. In this sense, the photocatalytic performance of lamellar potassium niobates and their protonated forms were tested for the degradation of the model dye Remazol Yelow Gold (RNL). The niobates (KNb3O8 and K4Nb6O17) were prepared by the polymeric precursor (PP) and solid state (SS) methods. The protonated forms HNb3O8.H2O and K4-xHxNb6O17, obtained by the PP method, were prepared via a ion exchange reaction using a HNO3 solution. The materials were characterized by X-ray di?raction (XDR), infrared (IR), Raman, ultraviolet visible (UV-vis), scanning electron microscopy (SEM), surface area (BET) and photoluminescence (PL). Theoretical Computational calculation were performed (DFT) to de?ne the structural and vibrational aspects of niobates in the potassium form. Their structures were characterized at long, medium and short range are in accordance with those in the literature. The theoretical studies of octahedron distortions showed that KNb3O8 has two types of distortion, where as K4Nb6O17 has four types. The octahedron with the largest distortion degree for K4Nb6O17 has a short Nb - O bond (high covalent character) and another much elongated one (with a transient character between the covalent and the ionic). It is observed that niobates in the potassium form have better photocatalytic performances when compared to either their protaned forms or P25. Studies to elucidate the mechanism of discoloration for the potassium niobates used suppressors of •OH, O•- 2 radicals, e- and h+. The results show that the mechanism of photocatalysis is indirect, that is, by the formation of •OH radicals . For KNb3O8 the formation of •OH radicals a high contribution of photogenerated e- in the conduction band is observed, whereas, both e- and h+ are responsible for the formation of these radicals for K4Nb6O17. For the RNL discoloration reaction using KNb3O8 reactional parameters were studied, such as pH, initial concentration of dye (C0), photocatalyst quantity and calcination temperature. Three reuse cycles were analyzed for potassium niobates, which indicated little loss of catalytic activity.
publishDate 2018
dc.date.none.fl_str_mv 2018-08-30
2019-06-26T17:57:32Z
2019-06-26
2019-06-26T17:57:32Z
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 https://repositorio.ufpb.br/jspui/handle/123456789/14841
url https://repositorio.ufpb.br/jspui/handle/123456789/14841
dc.language.iso.fl_str_mv por
language por
dc.rights.driver.fl_str_mv Attribution-NoDerivs 3.0 Brazil
http://creativecommons.org/licenses/by-nd/3.0/br/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv Attribution-NoDerivs 3.0 Brazil
http://creativecommons.org/licenses/by-nd/3.0/br/
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Universidade Federal da Paraíba
Brasil
Química
Programa de Pós-Graduação em Química
UFPB
publisher.none.fl_str_mv Universidade Federal da Paraíba
Brasil
Química
Programa de Pós-Graduação em Química
UFPB
dc.source.none.fl_str_mv reponame:Biblioteca Digital de Teses e Dissertações da UFPB
instname:Universidade Federal da Paraíba (UFPB)
instacron:UFPB
instname_str Universidade Federal da Paraíba (UFPB)
instacron_str UFPB
institution UFPB
reponame_str Biblioteca Digital de Teses e Dissertações da UFPB
collection Biblioteca Digital de Teses e Dissertações da UFPB
repository.name.fl_str_mv Biblioteca Digital de Teses e Dissertações da UFPB - Universidade Federal da Paraíba (UFPB)
repository.mail.fl_str_mv diretoria@ufpb.br|| diretoria@ufpb.br
_version_ 1801842949653266432