Niobium-based oxides for oxidative and reductive photocatalytic reactions
Autor(a) principal: | |
---|---|
Data de Publicação: | 2020 |
Tipo de documento: | Tese |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UFSCAR |
Texto Completo: | https://repositorio.ufscar.br/handle/ufscar/12652 |
Resumo: | It is growing the number of studies related to alternative technologies allowing both, environmental remediation and clean energy production. In this sense, photocatalysis is a promising process, since it is sustainable and operated under ambient conditions. Niobium pentoxide (Nb2O5) is one of the most promising semiconductors for photocatalytic reactions due to its chemical and physical stability, non-toxicity, versatility, and excellent photoactivity. Considering that (i) photocatalysis is an emerging research field, mainly for energy storage in chemical bonds, and (ii) Brazil has the world`s largest niobium reserves; it is of paramount importance the improvement of niobium properties in order to obtain a valuable product. Thus, the main objective of this thesis is developing strategies to (i) increase the absorption spectrum of Nb2O5 for the visible region, since it is activated only by ultraviolet illumination, and (ii) decrease the recombination rate of the photogenerated charges because it is a factor that directly influences the photocatalytic efficiency. Doping is a suitable option to decrease the band gap of semiconductors because the doping atoms create impurity levels (IL) between the VB and CB, leading to radiations with lower energy to promote an electron from the VB to the IL than from the VB to the CB. Then, the material initially excited only under ultraviolet radiation, can also become active under visible light. In this sense, zinc was chosen as dopant due to its abundance, low-cost, and ionic radius and electronegativity similar to that of Nb5+ that leads to an effective insertion into the Nb2O5 crystalline structure. The synthesized samples showed remarkable activities in the photooxidation of rhodamine B and caffeic acid, under visible radiation, even after consecutive cycles. The results have been correlated to the low concentrations of zinc (0.1 and 0.2 mol%) that were enough to ensure that all particles had at least one doping atom for decreasing the electron excitation energy, but, at same time, the impurities were not in excess to guarantee that the dopants were not acting as recombination centers. Another modification is the formation of a Z-scheme between Nb2O5 and basic bismuth nitrates (BBN). BBN are easily synthesized and have been identified as promising photocatalysts, but their properties in reduction reactions has not been explored yet. The nanocomposites exhibited notable photoresponse for the selective conversion of CO2 to CO and C2H4, mainly due to the band edge positions of the isolated semiconductors that led to a special separation of the photogenerated charges, consequently, molecules were oxidized on the Nb2O5 VB, while CO2 was reduced on the BBN CB. Considering that low-cost materials (Zn and BBN) have been successfully employed to modify Nb2O5 by hydrothermal treatment, a simple method to obtain semiconductors at low temperature, and based on the photocatalytic properties of the as-synthetized photocatalysts, it can be concluded that the Nb2O5-based materials developed in this work have potential to be used for large scale in applications for both, reductive and oxidative reactions. |
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Oliveira, Jéssica Ariane deRuotolo, Luís Augusto Martinshttp://lattes.cnpq.br/6167735734348703Nogueira, Francisco Guilherme Esteveshttp://lattes.cnpq.br/8117497993539795http://lattes.cnpq.br/4765767150921439acad5b6d-48e8-4ee2-8975-09b3af1feadb2020-04-28T12:57:06Z2020-04-28T12:57:06Z2020-02-21OLIVEIRA, Jéssica Ariane de. Niobium-based oxides for oxidative and reductive photocatalytic reactions. 2020. Tese (Doutorado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2020. Disponível em: https://repositorio.ufscar.br/handle/ufscar/12652.https://repositorio.ufscar.br/handle/ufscar/12652It is growing the number of studies related to alternative technologies allowing both, environmental remediation and clean energy production. In this sense, photocatalysis is a promising process, since it is sustainable and operated under ambient conditions. Niobium pentoxide (Nb2O5) is one of the most promising semiconductors for photocatalytic reactions due to its chemical and physical stability, non-toxicity, versatility, and excellent photoactivity. Considering that (i) photocatalysis is an emerging research field, mainly for energy storage in chemical bonds, and (ii) Brazil has the world`s largest niobium reserves; it is of paramount importance the improvement of niobium properties in order to obtain a valuable product. Thus, the main objective of this thesis is developing strategies to (i) increase the absorption spectrum of Nb2O5 for the visible region, since it is activated only by ultraviolet illumination, and (ii) decrease the recombination rate of the photogenerated charges because it is a factor that directly influences the photocatalytic efficiency. Doping is a suitable option to decrease the band gap of semiconductors because the doping atoms create impurity levels (IL) between the VB and CB, leading to radiations with lower energy to promote an electron from the VB to the IL than from the VB to the CB. Then, the material initially excited only under ultraviolet radiation, can also become active under visible light. In this sense, zinc was chosen as dopant due to its abundance, low-cost, and ionic radius and electronegativity similar to that of Nb5+ that leads to an effective insertion into the Nb2O5 crystalline structure. The synthesized samples showed remarkable activities in the photooxidation of rhodamine B and caffeic acid, under visible radiation, even after consecutive cycles. The results have been correlated to the low concentrations of zinc (0.1 and 0.2 mol%) that were enough to ensure that all particles had at least one doping atom for decreasing the electron excitation energy, but, at same time, the impurities were not in excess to guarantee that the dopants were not acting as recombination centers. Another modification is the formation of a Z-scheme between Nb2O5 and basic bismuth nitrates (BBN). BBN are easily synthesized and have been identified as promising photocatalysts, but their properties in reduction reactions has not been explored yet. The nanocomposites exhibited notable photoresponse for the selective conversion of CO2 to CO and C2H4, mainly due to the band edge positions of the isolated semiconductors that led to a special separation of the photogenerated charges, consequently, molecules were oxidized on the Nb2O5 VB, while CO2 was reduced on the BBN CB. Considering that low-cost materials (Zn and BBN) have been successfully employed to modify Nb2O5 by hydrothermal treatment, a simple method to obtain semiconductors at low temperature, and based on the photocatalytic properties of the as-synthetized photocatalysts, it can be concluded that the Nb2O5-based materials developed in this work have potential to be used for large scale in applications for both, reductive and oxidative reactions.Atualmente existe uma busca crescente por tecnologias alternativas que permitam tanto a remediação ambiental quanto a geração de energia. Nesse sentido, a fotocatálise se destaca por ser um processo sustentável que pode ser operado em condições ambientes. O pentóxido de nióbio (Nb2O5) é um dos semicondutores mais promissores para a fotocatálise devido à sua estabilidade química e física, não toxicidade, versatilidade e excelente fotoatividade. Considerando que (i) a fotocatálise é um campo de pesquisa emergente, principalmente para a área de armazenamento de energia na forma de ligações químicas e (ii) o Brasil detém as maiores reservas mundiais de nióbio; faz-se necessário o aprimoramento das propriedades do nióbio para que seja obtido um produto com maior valor agregado. Logo, a presente tese teve como objetivo principal desenvolver estratégias para (i) aumentar o espectro de absorção do Nb2O5 para a região do visível, já que o mesmo é ativado somente sob iluminação ultravioleta e (ii) diminuir a taxa de recombinação do par e-/h+, visto que esse fator influencia diretamente a eficiência fotocatalítica. A dopagem é uma opção adequada para diminuir o band gap de semicondutores pelo fato de os átomos dopantes criarem níveis de impureza (NI) entre a BV e a BC, fazendo com que radiação de menor energia seja necessária para excitar um elétron da BV para o NI do que da BV para a BC. Nessa condição, um material inicialmente excitado somente sob iluminação ultravioleta, também pode se tornar ativo sob radiação visível. Dessa maneira, zinco foi escolhido como dopante por ser um elemento abundante, de baixo custo e que apresenta raio iônico e eletronegatividade próximos ao do Nb5+, podendo ser efetivamente inserido na rede cristalina do Nb2O5. As amostras sintetizadas apresentaram excelentes atividades na fotooxidação de rodamina B e ácido cafeico, sob radiação visível, mesmo após usos consecutivos. Os resultados obtidos foram relacionados às baixas concentrações utilizadas de zinco (0,1 e 0,2 %mol), que foram suficientes para garantir que todas as partículas tivessem pelo menos um átomo dopante para diminuir a energia de excitação do elétron, mas ao mesmo tempo sem tantas impurezas que pudessem começar a atuar como centros de recombinações. Outra modificação realizada no Nb2O5 foi a formação de um esquema Z com nitratos básicos de bismuto (NBB). NBB são materiais de fácil obtenção e têm sido reconhecidos como bons fotocatalisadores, apesar de suas propriedades em reações de redução ainda não terem sido exploradas. Os nanocompósitos apresentaram alta fotoresposta para a conversão seletiva de CO2 a CO e C2H4 devido principalmente a posição das bandas dos semicondutores isolados que permitiram uma separação espacial das cargas fotogeradas, consequentemente, enquanto moléculas foram oxidadas na BV do Nb2O5, CO2 foi reduzido na BC do NBB. Optou-se por utilizar materiais de baixo custo (Zn e NBB) para modificar o Nb2O5 via síntese hidrotermal, um método simples para a obtenção de semicondutores em baixas temperaturas. Portanto, os fotocatalisadores à base de Nb2O5, desenvolvidos nessa tese, têm potencialidade de serem utilizados em larga escala e em outros tipos de aplicações que exijam propriedades fotocatalíticas versáteis para diferentes tipos de reações de oxidação e redução.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Capes: Finance Code 001engUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Engenharia Química - PPGEQUFSCarAttribution-NonCommercial-NoDerivs 3.0 Brazilhttp://creativecommons.org/licenses/by-nc-nd/3.0/br/info:eu-repo/semantics/openAccessFotocatáliseDopagemZincoRodamina BNitrato Básico de BismutoEsquema ZÁcido cafeicoPhotocatalysisDopingZincRhodamine BZ-SchemeBasic Bismuth NitrateCaffeic acidNb2O5CO2COC2H4ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOSENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICAENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICAENGENHARIAS::ENGENHARIA QUIMICACIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::CINETICA QUIMICA E CATALISECIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::QUIMICA DE INTERFACESENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOS::CERAMICOSNiobium-based oxides for oxidative and reductive photocatalytic reactionsÓxidos baseados em nióbio para utilização em reações fotocatalíticas de oxidação e reduçãoinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesis600600cf9213f8-9cfd-427b-96e9-08a34508a5b6reponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALTese.pdfTese.pdfTese apresentada como pré-requisito para obtenção do título de Doutora em Engenharia Químicaapplication/pdf7870513https://repositorio.ufscar.br/bitstream/ufscar/12652/4/Tese.pdfdbd1da6f3eb19dbb78c7004114e9b9d1MD54Carta Comprovante assinada pelo orientador.pdfCarta Comprovante assinada pelo orientador.pdfCarta Comprovante assinada pelo Orientadorapplication/pdf157667https://repositorio.ufscar.br/bitstream/ufscar/12652/2/Carta%20Comprovante%20assinada%20pelo%20orientador.pdf6ad18e24d3925800a166c85a8cd851d7MD52CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8811https://repositorio.ufscar.br/bitstream/ufscar/12652/5/license_rdfe39d27027a6cc9cb039ad269a5db8e34MD55TEXTTese.pdf.txtTese.pdf.txtExtracted texttext/plain183364https://repositorio.ufscar.br/bitstream/ufscar/12652/6/Tese.pdf.txt5328d72de20ddc63e4dbac96e9b8a4cbMD56Carta Comprovante assinada pelo orientador.pdf.txtCarta Comprovante assinada pelo orientador.pdf.txtExtracted texttext/plain1485https://repositorio.ufscar.br/bitstream/ufscar/12652/8/Carta%20Comprovante%20assinada%20pelo%20orientador.pdf.txt78b0cb0bf53d40090da1ec6d48d85a4dMD58THUMBNAILTese.pdf.jpgTese.pdf.jpgIM Thumbnailimage/jpeg5416https://repositorio.ufscar.br/bitstream/ufscar/12652/7/Tese.pdf.jpgbaa0df4d0023e463bcc43f60393d04b0MD57Carta Comprovante assinada pelo orientador.pdf.jpgCarta Comprovante assinada pelo orientador.pdf.jpgIM Thumbnailimage/jpeg10967https://repositorio.ufscar.br/bitstream/ufscar/12652/9/Carta%20Comprovante%20assinada%20pelo%20orientador.pdf.jpg0c1352c6f2a5a4aa102f52d63136c420MD59ufscar/126522023-09-18 18:31:53.876oai:repositorio.ufscar.br:ufscar/12652Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222023-09-18T18:31:53Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false |
dc.title.eng.fl_str_mv |
Niobium-based oxides for oxidative and reductive photocatalytic reactions |
dc.title.alternative.por.fl_str_mv |
Óxidos baseados em nióbio para utilização em reações fotocatalíticas de oxidação e redução |
title |
Niobium-based oxides for oxidative and reductive photocatalytic reactions |
spellingShingle |
Niobium-based oxides for oxidative and reductive photocatalytic reactions Oliveira, Jéssica Ariane de Fotocatálise Dopagem Zinco Rodamina B Nitrato Básico de Bismuto Esquema Z Ácido cafeico Photocatalysis Doping Zinc Rhodamine B Z-Scheme Basic Bismuth Nitrate Caffeic acid Nb2O5 CO2 CO C2H4 ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOS ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA ENGENHARIAS::ENGENHARIA QUIMICA CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::CINETICA QUIMICA E CATALISE CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::QUIMICA DE INTERFACES ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOS::CERAMICOS |
title_short |
Niobium-based oxides for oxidative and reductive photocatalytic reactions |
title_full |
Niobium-based oxides for oxidative and reductive photocatalytic reactions |
title_fullStr |
Niobium-based oxides for oxidative and reductive photocatalytic reactions |
title_full_unstemmed |
Niobium-based oxides for oxidative and reductive photocatalytic reactions |
title_sort |
Niobium-based oxides for oxidative and reductive photocatalytic reactions |
author |
Oliveira, Jéssica Ariane de |
author_facet |
Oliveira, Jéssica Ariane de |
author_role |
author |
dc.contributor.advisor.none.fl_str_mv |
|
dc.contributor.authorlattes.por.fl_str_mv |
http://lattes.cnpq.br/4765767150921439 |
dc.contributor.author.fl_str_mv |
Oliveira, Jéssica Ariane de |
dc.contributor.advisor1.fl_str_mv |
Ruotolo, Luís Augusto Martins |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/6167735734348703 |
dc.contributor.advisor-co1.fl_str_mv |
Nogueira, Francisco Guilherme Esteves |
dc.contributor.advisor-co1Lattes.fl_str_mv |
http://lattes.cnpq.br/8117497993539795 |
dc.contributor.authorID.fl_str_mv |
acad5b6d-48e8-4ee2-8975-09b3af1feadb |
contributor_str_mv |
Ruotolo, Luís Augusto Martins Nogueira, Francisco Guilherme Esteves |
dc.subject.por.fl_str_mv |
Fotocatálise Dopagem Zinco Rodamina B Nitrato Básico de Bismuto Esquema Z Ácido cafeico |
topic |
Fotocatálise Dopagem Zinco Rodamina B Nitrato Básico de Bismuto Esquema Z Ácido cafeico Photocatalysis Doping Zinc Rhodamine B Z-Scheme Basic Bismuth Nitrate Caffeic acid Nb2O5 CO2 CO C2H4 ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOS ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA ENGENHARIAS::ENGENHARIA QUIMICA CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::CINETICA QUIMICA E CATALISE CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::QUIMICA DE INTERFACES ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOS::CERAMICOS |
dc.subject.eng.fl_str_mv |
Photocatalysis Doping Zinc Rhodamine B Z-Scheme Basic Bismuth Nitrate Caffeic acid Nb2O5 CO2 CO C2H4 |
dc.subject.cnpq.fl_str_mv |
ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOS ENGENHARIAS::ENGENHARIA QUIMICA::PROCESSOS INDUSTRIAIS DE ENGENHARIA QUIMICA ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA ENGENHARIAS::ENGENHARIA QUIMICA CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::CINETICA QUIMICA E CATALISE CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA::QUIMICA DE INTERFACES ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA::MATERIAIS NAO METALICOS::CERAMICOS |
description |
It is growing the number of studies related to alternative technologies allowing both, environmental remediation and clean energy production. In this sense, photocatalysis is a promising process, since it is sustainable and operated under ambient conditions. Niobium pentoxide (Nb2O5) is one of the most promising semiconductors for photocatalytic reactions due to its chemical and physical stability, non-toxicity, versatility, and excellent photoactivity. Considering that (i) photocatalysis is an emerging research field, mainly for energy storage in chemical bonds, and (ii) Brazil has the world`s largest niobium reserves; it is of paramount importance the improvement of niobium properties in order to obtain a valuable product. Thus, the main objective of this thesis is developing strategies to (i) increase the absorption spectrum of Nb2O5 for the visible region, since it is activated only by ultraviolet illumination, and (ii) decrease the recombination rate of the photogenerated charges because it is a factor that directly influences the photocatalytic efficiency. Doping is a suitable option to decrease the band gap of semiconductors because the doping atoms create impurity levels (IL) between the VB and CB, leading to radiations with lower energy to promote an electron from the VB to the IL than from the VB to the CB. Then, the material initially excited only under ultraviolet radiation, can also become active under visible light. In this sense, zinc was chosen as dopant due to its abundance, low-cost, and ionic radius and electronegativity similar to that of Nb5+ that leads to an effective insertion into the Nb2O5 crystalline structure. The synthesized samples showed remarkable activities in the photooxidation of rhodamine B and caffeic acid, under visible radiation, even after consecutive cycles. The results have been correlated to the low concentrations of zinc (0.1 and 0.2 mol%) that were enough to ensure that all particles had at least one doping atom for decreasing the electron excitation energy, but, at same time, the impurities were not in excess to guarantee that the dopants were not acting as recombination centers. Another modification is the formation of a Z-scheme between Nb2O5 and basic bismuth nitrates (BBN). BBN are easily synthesized and have been identified as promising photocatalysts, but their properties in reduction reactions has not been explored yet. The nanocomposites exhibited notable photoresponse for the selective conversion of CO2 to CO and C2H4, mainly due to the band edge positions of the isolated semiconductors that led to a special separation of the photogenerated charges, consequently, molecules were oxidized on the Nb2O5 VB, while CO2 was reduced on the BBN CB. Considering that low-cost materials (Zn and BBN) have been successfully employed to modify Nb2O5 by hydrothermal treatment, a simple method to obtain semiconductors at low temperature, and based on the photocatalytic properties of the as-synthetized photocatalysts, it can be concluded that the Nb2O5-based materials developed in this work have potential to be used for large scale in applications for both, reductive and oxidative reactions. |
publishDate |
2020 |
dc.date.accessioned.fl_str_mv |
2020-04-28T12:57:06Z |
dc.date.available.fl_str_mv |
2020-04-28T12:57:06Z |
dc.date.issued.fl_str_mv |
2020-02-21 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/doctoralThesis |
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doctoralThesis |
status_str |
publishedVersion |
dc.identifier.citation.fl_str_mv |
OLIVEIRA, Jéssica Ariane de. Niobium-based oxides for oxidative and reductive photocatalytic reactions. 2020. Tese (Doutorado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2020. Disponível em: https://repositorio.ufscar.br/handle/ufscar/12652. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufscar.br/handle/ufscar/12652 |
identifier_str_mv |
OLIVEIRA, Jéssica Ariane de. Niobium-based oxides for oxidative and reductive photocatalytic reactions. 2020. Tese (Doutorado em Engenharia Química) – Universidade Federal de São Carlos, São Carlos, 2020. Disponível em: https://repositorio.ufscar.br/handle/ufscar/12652. |
url |
https://repositorio.ufscar.br/handle/ufscar/12652 |
dc.language.iso.fl_str_mv |
eng |
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eng |
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600 600 |
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Attribution-NonCommercial-NoDerivs 3.0 Brazil http://creativecommons.org/licenses/by-nc-nd/3.0/br/ info:eu-repo/semantics/openAccess |
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Attribution-NonCommercial-NoDerivs 3.0 Brazil http://creativecommons.org/licenses/by-nc-nd/3.0/br/ |
eu_rights_str_mv |
openAccess |
dc.publisher.none.fl_str_mv |
Universidade Federal de São Carlos Câmpus São Carlos |
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Programa de Pós-Graduação em Engenharia Química - PPGEQ |
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UFSCar |
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Universidade Federal de São Carlos Câmpus São Carlos |
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