Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2

Detalhes bibliográficos
Ano de defesa: 2014
Autor(a) principal: Mendonça, Vagner Romito de
Orientador(a): Oliveira, Cauê Ribeiro de lattes
Banca de defesa: Não Informado pela instituição
Tipo de documento: Tese
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Universidade Federal de São Carlos
Programa de Pós-Graduação: Programa de Pós-Graduação em Química - PPGQ
Departamento: Não Informado pela instituição
País: BR
Palavras-chave em Português:
Área do conhecimento CNPq:
Link de acesso: https://repositorio.ufscar.br/handle/20.500.14289/6297
Resumo: Heterostructures, systems containing two dissimilar semiconductors in direct contact, has been applied in heterogeneous photocatalysis due to their electronic properties. This work aimed at studying heterostructures containing metallic oxides. Due to their suitable features, both anatase TiO2 and rutile SnO2 were chosen to compose a model-system. In the first part, this work dealt with the synthesis of TiO2/SnO2 heterostructures by using two different routes: the sol gel hydrolytic (Hid) and the polymeric precursor method (Prec). The heterostructures photocatalytic properties were evaluated by the photodegradation of rhodamine B dye (RhB) under UV radiation. The results showed that heterostructures were more active than pristine TiO2, the same used to make heterostructures. That finding was related to charge migration between oxides, a heterostructure feature, as showed by photoluminescence spectroscopy analysis. The homogeneity in the phase formation (i.e., SnO2 dispersion over TiO2) was influenced by the synthesis method, as showed by X ray diffraction, Raman spectroscopy and scanning electron microscopy with X ray microanalysis. The main RhB degradation mechanism was correlated with the process of OH radical generation, which in turn was related to the concentration and nature of the surface hydroxyl groups on the photocatalyst surface, as determined by infrared spectroscopy analysis. Accordingly, the polymeric precursor method was shown to be more adequate for dispersing higher amounts of SnO2 in comparison with the hydrolytic sol gel method. In the second part, due to the difficulty of a controlling morphology in a one-pot crystallization of two components, and to isolate the effect of charge migration between oxides, it was studied the possibility of obtaining heterostructures from pre formed nanoparticles by an aggregation and coalescence process induced by hydrothermal annealing. Morphologically xiv different oxides were separately synthesized and hydrothermally treated in different conditions. A kinetic model based on a diffusion controlled process was applied in the analysis of results. The ability of generating OH radicals under UV radiation was used to verify the charge migration. The results demonstrated the possibility of obtaining heterostructures by an aggregation followed by a coalescence process. It was also showed the charge migration between oxides, despite the interface being a point of charge recombination. The heterostructure formation was confirmed by comparing the heterostructure capability to generate OH radicals with anatase TiO2, the active phase, when treated in the same hydrothermal conditions.
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spelling Mendonça, Vagner Romito deOliveira, Cauê Ribeiro dehttp://lattes.cnpq.br/5321313558714462http://lattes.cnpq.br/427037587394882304228bb1-9471-4093-a4ea-cb4749d662b32016-06-02T20:34:51Z2014-07-072016-06-02T20:34:51Z2014-03-14MENDONÇA, Vagner Romito de. Synthesis and photocatalytic properties of TiO2/SnO2 heterostructures. 2014. 116 f. Tese (Doutorado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2014.https://repositorio.ufscar.br/handle/20.500.14289/6297Heterostructures, systems containing two dissimilar semiconductors in direct contact, has been applied in heterogeneous photocatalysis due to their electronic properties. This work aimed at studying heterostructures containing metallic oxides. Due to their suitable features, both anatase TiO2 and rutile SnO2 were chosen to compose a model-system. In the first part, this work dealt with the synthesis of TiO2/SnO2 heterostructures by using two different routes: the sol gel hydrolytic (Hid) and the polymeric precursor method (Prec). The heterostructures photocatalytic properties were evaluated by the photodegradation of rhodamine B dye (RhB) under UV radiation. The results showed that heterostructures were more active than pristine TiO2, the same used to make heterostructures. That finding was related to charge migration between oxides, a heterostructure feature, as showed by photoluminescence spectroscopy analysis. The homogeneity in the phase formation (i.e., SnO2 dispersion over TiO2) was influenced by the synthesis method, as showed by X ray diffraction, Raman spectroscopy and scanning electron microscopy with X ray microanalysis. The main RhB degradation mechanism was correlated with the process of OH radical generation, which in turn was related to the concentration and nature of the surface hydroxyl groups on the photocatalyst surface, as determined by infrared spectroscopy analysis. Accordingly, the polymeric precursor method was shown to be more adequate for dispersing higher amounts of SnO2 in comparison with the hydrolytic sol gel method. In the second part, due to the difficulty of a controlling morphology in a one-pot crystallization of two components, and to isolate the effect of charge migration between oxides, it was studied the possibility of obtaining heterostructures from pre formed nanoparticles by an aggregation and coalescence process induced by hydrothermal annealing. Morphologically xiv different oxides were separately synthesized and hydrothermally treated in different conditions. A kinetic model based on a diffusion controlled process was applied in the analysis of results. The ability of generating OH radicals under UV radiation was used to verify the charge migration. The results demonstrated the possibility of obtaining heterostructures by an aggregation followed by a coalescence process. It was also showed the charge migration between oxides, despite the interface being a point of charge recombination. The heterostructure formation was confirmed by comparing the heterostructure capability to generate OH radicals with anatase TiO2, the active phase, when treated in the same hydrothermal conditions.Heteroestruturas, sistemas contendo diferentes semicondutores em direto contato físico, têm sido aplicadas em estudos de fotocatálise heterogênea por conta de suas adequadas propriedades eletrônicas. Este trabalho teve por objetivo traçar um paralelo entre o processamento e as propriedades exibidas por heteroestruturas de óxidos metálicos. Por conta de suas características físicas e químicas, os óxidos TiO2 anatásio e SnO2 rutilo são apropriados para compor um sistema modelo. Na primeira parte, este trabalho lidou com a síntese de heteroestruturas de TiO2/SnO2 por duas diferentes rotas: Sol gel hidrolítico (Hid) e Precursores poliméricos (Prec). Suas propriedades fotocatalíticas foram estudadas pela degradação do corante rodamina B (RhB) sob radiação UV. Os resultados mostraram que as heteroestrutura apresentam maior fotoatividade que o TiO2 isolado, resultado este relacionado com a migração de carga entre os óxidos, característica de heteroestruturas, como mostrado por análises de espectroscopia de fotoluminescência. A homogeneidade na formação da fase (i.e., dispersão do SnO2 sobre o TiO2) foi influenciada pelo método de síntese, como mostrado pela difratometria de raios X, espectroscopia Raman e microscopia eletrônica acoplada à espectroscopia por energia dispersiva de raios X. O principal mecanismo de degradação da RhB foi relacionado à formação de radicais OH, que por sua vez foi relacionada à quantidade e natureza de grupos hidroxilas superficiais nos fotocatalisadores, como determinado por análises de espectroscopia no infravermelho médio. Neste sentido, o método Prec foi mais adequado na dispersão de maiores quantidades de SnO2, e na obtenção de estruturas com maior concentração de grupos hidroxilas superficiais. Na segunda parte, por conta da dificuldade de controle morfológico em meios de cristalização simultâneos e para isolar o efeito da migração de cargas entre os óxidos, foi estudada a possibilidade de formação das heteroestruturas por agregação e coalescência das partículas pré-formadas induzidas por tratamento hidrotérmico. Os óxidos em diferentes morfologias foram sintetizados isoladamente e tratados hidrotermicamente em diferentes condições de tempo, temperatura e proporção mássica. Um modelo cinético baseado em reações limitadas por difusão foi aplicado na análise do processo. A capacidade de geração de radicais OH pelas estruturas durante radiação UV foi utilizada para verificação da migração de cargas. Os resultados demonstraram a possibilidade de obtenção de heteroestruturas por este processo de agregação e coalescência e a migração de cargas entre os óxidos, mesmo sendo a interface um ponto de recombinação de cargas. Este ponto foi confirmado comparando-se as capacidades de geração de radicais hidroxila pelas heteroestruturas com a capacidade do TiO2 anatásio, a fase ativa, tratado nas mesmas condições hidrotérmicas.Universidade Federal de Sao Carlosapplication/pdfporUniversidade Federal de São CarlosPrograma de Pós-Graduação em Química - PPGQUFSCarBRFísico-químicaSíntese químicaFotocatáliseÓxidos metálicosCIENCIAS EXATAS E DA TERRA::QUIMICASíntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2Synthesis and photocatalytic properties of TiO2/SnO2 heterostructuresinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesis-1-119447b82-be97-4aec-a6e8-de69229cbfdeinfo:eu-repo/semantics/openAccessreponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINAL5836.pdfapplication/pdf3075052https://repositorio.ufscar.br/bitstreams/22ae5676-217d-437b-b731-f7acd08f147d/downloadcb4aaf76bd24ad274ea467affd19d232MD51trueAnonymousREADTEXT5836.pdf.txt5836.pdf.txtExtracted texttext/plain0https://repositorio.ufscar.br/bitstreams/203cfd9a-1920-49a9-8ff2-08aff866fa45/downloadd41d8cd98f00b204e9800998ecf8427eMD56falseAnonymousREADTHUMBNAIL5836.pdf.jpg5836.pdf.jpgIM Thumbnailimage/jpeg9754https://repositorio.ufscar.br/bitstreams/d3c1cfd7-33f3-4ec9-909b-29c7d2a2d192/downloadf96eb94e7197e287dcbe8c402d3bba9eMD57falseAnonymousREAD20.500.14289/62972025-02-05 15:14:38.014open.accessoai:repositorio.ufscar.br:20.500.14289/6297https://repositorio.ufscar.brRepositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestrepositorio.sibi@ufscar.bropendoar:43222025-02-05T18:14:38Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false
dc.title.por.fl_str_mv Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
dc.title.alternative.eng.fl_str_mv Synthesis and photocatalytic properties of TiO2/SnO2 heterostructures
title Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
spellingShingle Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
Mendonça, Vagner Romito de
Físico-química
Síntese química
Fotocatálise
Óxidos metálicos
CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
title_full Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
title_fullStr Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
title_full_unstemmed Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
title_sort Síntese e propriedades fotocatalíticas de heteroestruturas TiO2/SnO2
author Mendonça, Vagner Romito de
author_facet Mendonça, Vagner Romito de
author_role author
dc.contributor.authorlattes.por.fl_str_mv http://lattes.cnpq.br/4270375873948823
dc.contributor.author.fl_str_mv Mendonça, Vagner Romito de
dc.contributor.advisor1.fl_str_mv Oliveira, Cauê Ribeiro de
dc.contributor.advisor1Lattes.fl_str_mv http://lattes.cnpq.br/5321313558714462
dc.contributor.authorID.fl_str_mv 04228bb1-9471-4093-a4ea-cb4749d662b3
contributor_str_mv Oliveira, Cauê Ribeiro de
dc.subject.por.fl_str_mv Físico-química
Síntese química
Fotocatálise
Óxidos metálicos
topic Físico-química
Síntese química
Fotocatálise
Óxidos metálicos
CIENCIAS EXATAS E DA TERRA::QUIMICA
dc.subject.cnpq.fl_str_mv CIENCIAS EXATAS E DA TERRA::QUIMICA
description Heterostructures, systems containing two dissimilar semiconductors in direct contact, has been applied in heterogeneous photocatalysis due to their electronic properties. This work aimed at studying heterostructures containing metallic oxides. Due to their suitable features, both anatase TiO2 and rutile SnO2 were chosen to compose a model-system. In the first part, this work dealt with the synthesis of TiO2/SnO2 heterostructures by using two different routes: the sol gel hydrolytic (Hid) and the polymeric precursor method (Prec). The heterostructures photocatalytic properties were evaluated by the photodegradation of rhodamine B dye (RhB) under UV radiation. The results showed that heterostructures were more active than pristine TiO2, the same used to make heterostructures. That finding was related to charge migration between oxides, a heterostructure feature, as showed by photoluminescence spectroscopy analysis. The homogeneity in the phase formation (i.e., SnO2 dispersion over TiO2) was influenced by the synthesis method, as showed by X ray diffraction, Raman spectroscopy and scanning electron microscopy with X ray microanalysis. The main RhB degradation mechanism was correlated with the process of OH radical generation, which in turn was related to the concentration and nature of the surface hydroxyl groups on the photocatalyst surface, as determined by infrared spectroscopy analysis. Accordingly, the polymeric precursor method was shown to be more adequate for dispersing higher amounts of SnO2 in comparison with the hydrolytic sol gel method. In the second part, due to the difficulty of a controlling morphology in a one-pot crystallization of two components, and to isolate the effect of charge migration between oxides, it was studied the possibility of obtaining heterostructures from pre formed nanoparticles by an aggregation and coalescence process induced by hydrothermal annealing. Morphologically xiv different oxides were separately synthesized and hydrothermally treated in different conditions. A kinetic model based on a diffusion controlled process was applied in the analysis of results. The ability of generating OH radicals under UV radiation was used to verify the charge migration. The results demonstrated the possibility of obtaining heterostructures by an aggregation followed by a coalescence process. It was also showed the charge migration between oxides, despite the interface being a point of charge recombination. The heterostructure formation was confirmed by comparing the heterostructure capability to generate OH radicals with anatase TiO2, the active phase, when treated in the same hydrothermal conditions.
publishDate 2014
dc.date.available.fl_str_mv 2014-07-07
2016-06-02T20:34:51Z
dc.date.issued.fl_str_mv 2014-03-14
dc.date.accessioned.fl_str_mv 2016-06-02T20:34:51Z
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dc.identifier.citation.fl_str_mv MENDONÇA, Vagner Romito de. Synthesis and photocatalytic properties of TiO2/SnO2 heterostructures. 2014. 116 f. Tese (Doutorado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2014.
dc.identifier.uri.fl_str_mv https://repositorio.ufscar.br/handle/20.500.14289/6297
identifier_str_mv MENDONÇA, Vagner Romito de. Synthesis and photocatalytic properties of TiO2/SnO2 heterostructures. 2014. 116 f. Tese (Doutorado em Ciências Exatas e da Terra) - Universidade Federal de São Carlos, São Carlos, 2014.
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