Design of multifunctional titania-based photocatalysts by controlled redox reactions

Detalhes bibliográficos
Autor(a) principal: Lopes, Diogo João Breda
Data de Publicação: 2019
Tipo de documento: Dissertação
Idioma: eng
Título da fonte: Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
Texto Completo: http://hdl.handle.net/10773/26433
Resumo: This work was focused on designing the phase composition and microstructure of composite rutile – silicon carbide mixture by controlled redox reactions, aiming the preparation of multifunctional titania-based photocatalysts with inherent capabilities for thermal co-activation and stabilization of the anatase polymorph. The materials were processed using a conventional solid state route, involving a partial reduction of the rutile by SiC in inert Ar atmosphere, followed by the post-oxidation in air. The impacts of processing conditions on the phase composition of the oxidized samples and their photocatalytic activity were evaluated using Taguchi experimental planning. The XRD studies confirmed the presence of rutile/anatase mixtures in the oxidized samples. The results emphasized that the pre-reduction and post-oxidation temperatures are the most critical parameters in defining the phase composition, while the post-oxidation time appears to be relevant for the photocatalytic performance. Microstructural studies revealed the formation of core-shell particles in the pre-reduced and post-oxidized samples, which can suppress the photocatalytic activity. The highest apparent reaction rate (0.089 min-1) of the photodegradation of methylene blue was observed for the sample pre-reduced in Ar at 1300ºC for 5 h and then oxidized in air at 400ºC for 25 h, which is only 1.6-times lower than that for nanostructured industrial P25 photocatalyst, tested under the same conditions. The observed trends demonstrate good prospects for designing multifunctional titania-based photocatalysts based on the flexibility of the phase composition control
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spelling Design of multifunctional titania-based photocatalysts by controlled redox reactionsPhotocatalysisTiO2AnataseRutileTaguchi planningRedox reactionsTitanium oxycarbideCore-shell microstructureThis work was focused on designing the phase composition and microstructure of composite rutile – silicon carbide mixture by controlled redox reactions, aiming the preparation of multifunctional titania-based photocatalysts with inherent capabilities for thermal co-activation and stabilization of the anatase polymorph. The materials were processed using a conventional solid state route, involving a partial reduction of the rutile by SiC in inert Ar atmosphere, followed by the post-oxidation in air. The impacts of processing conditions on the phase composition of the oxidized samples and their photocatalytic activity were evaluated using Taguchi experimental planning. The XRD studies confirmed the presence of rutile/anatase mixtures in the oxidized samples. The results emphasized that the pre-reduction and post-oxidation temperatures are the most critical parameters in defining the phase composition, while the post-oxidation time appears to be relevant for the photocatalytic performance. Microstructural studies revealed the formation of core-shell particles in the pre-reduced and post-oxidized samples, which can suppress the photocatalytic activity. The highest apparent reaction rate (0.089 min-1) of the photodegradation of methylene blue was observed for the sample pre-reduced in Ar at 1300ºC for 5 h and then oxidized in air at 400ºC for 25 h, which is only 1.6-times lower than that for nanostructured industrial P25 photocatalyst, tested under the same conditions. The observed trends demonstrate good prospects for designing multifunctional titania-based photocatalysts based on the flexibility of the phase composition controlO presente trabalho teve como objetivo o design da composição de fases e microestrutura de compósitos à base de rutilo – carboneto de silício, através de reações redox controladas, visando a preparação de fotocatalizadores multifuncionais à base de titânia, com capacidades inerentes de coativação térmica e estabilização do polimorfo anatase. Os materiais foram processados utilizando um método convencional de processamento no estado sólido, envolvendo uma redução parcial do rutilo através do SiC numa atmosfera inerte de árgon, seguido por uma pós-oxidação em ar. O impacto das condições de processamento na composição de fases das amostras oxidadas e a sua atividade fotocatalítica foram avaliadas utilizando o método experimental de Taguchi. As análises de DRX confirmaram a presença de misturas rutilo/anatase nas amostras oxidadas. Os resultados enfatizam que as temperaturas de pré-redução e pós-oxidação são os parâmetros mais críticos na definição da composição de fases, enquanto que o tempo de pós-oxidação parece ser relevante para o desempenho fotocatalítico. Estudos microestruturais revelaram a formação de partículas core-shell nas amostras pré-reduzidas e pós-oxidadas, que podem suprimir a atividade fotocatalítica. A maior velocidade de reação aparente (0.089 min-1) da foto-degradação do azul de metileno foi observada na amostra pré-reduzida em árgon a 1300 ⁰C durante 5 horas e depois oxidada em ar a 400 ⁰C durante 25 horas, sendo apenas 1.6 vezes menor que a velocidade observada utilizando o pó industrial, nanoestruturado P25 como fotocatalisador, testado nas mesmas condições. As tendências observadas demonstram boas perspetivas para o design de fotocatalizadores multifuncionais à base de titânia baseado na flexibilidade do controlo da composição de fases2019-08-26T10:47:08Z2019-05-09T00:00:00Z2019-05-09info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisapplication/pdfhttp://hdl.handle.net/10773/26433engLopes, Diogo João Bredainfo:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2024-02-22T11:51:13Zoai:ria.ua.pt:10773/26433Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-20T02:59:26.038367Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse
dc.title.none.fl_str_mv Design of multifunctional titania-based photocatalysts by controlled redox reactions
title Design of multifunctional titania-based photocatalysts by controlled redox reactions
spellingShingle Design of multifunctional titania-based photocatalysts by controlled redox reactions
Lopes, Diogo João Breda
Photocatalysis
TiO2
Anatase
Rutile
Taguchi planning
Redox reactions
Titanium oxycarbide
Core-shell microstructure
title_short Design of multifunctional titania-based photocatalysts by controlled redox reactions
title_full Design of multifunctional titania-based photocatalysts by controlled redox reactions
title_fullStr Design of multifunctional titania-based photocatalysts by controlled redox reactions
title_full_unstemmed Design of multifunctional titania-based photocatalysts by controlled redox reactions
title_sort Design of multifunctional titania-based photocatalysts by controlled redox reactions
author Lopes, Diogo João Breda
author_facet Lopes, Diogo João Breda
author_role author
dc.contributor.author.fl_str_mv Lopes, Diogo João Breda
dc.subject.por.fl_str_mv Photocatalysis
TiO2
Anatase
Rutile
Taguchi planning
Redox reactions
Titanium oxycarbide
Core-shell microstructure
topic Photocatalysis
TiO2
Anatase
Rutile
Taguchi planning
Redox reactions
Titanium oxycarbide
Core-shell microstructure
description This work was focused on designing the phase composition and microstructure of composite rutile – silicon carbide mixture by controlled redox reactions, aiming the preparation of multifunctional titania-based photocatalysts with inherent capabilities for thermal co-activation and stabilization of the anatase polymorph. The materials were processed using a conventional solid state route, involving a partial reduction of the rutile by SiC in inert Ar atmosphere, followed by the post-oxidation in air. The impacts of processing conditions on the phase composition of the oxidized samples and their photocatalytic activity were evaluated using Taguchi experimental planning. The XRD studies confirmed the presence of rutile/anatase mixtures in the oxidized samples. The results emphasized that the pre-reduction and post-oxidation temperatures are the most critical parameters in defining the phase composition, while the post-oxidation time appears to be relevant for the photocatalytic performance. Microstructural studies revealed the formation of core-shell particles in the pre-reduced and post-oxidized samples, which can suppress the photocatalytic activity. The highest apparent reaction rate (0.089 min-1) of the photodegradation of methylene blue was observed for the sample pre-reduced in Ar at 1300ºC for 5 h and then oxidized in air at 400ºC for 25 h, which is only 1.6-times lower than that for nanostructured industrial P25 photocatalyst, tested under the same conditions. The observed trends demonstrate good prospects for designing multifunctional titania-based photocatalysts based on the flexibility of the phase composition control
publishDate 2019
dc.date.none.fl_str_mv 2019-08-26T10:47:08Z
2019-05-09T00:00:00Z
2019-05-09
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://hdl.handle.net/10773/26433
url http://hdl.handle.net/10773/26433
dc.language.iso.fl_str_mv eng
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instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação
instacron:RCAAP
instname_str Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação
instacron_str RCAAP
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reponame_str Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
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