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Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise

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Main Author: Silva, Adervando Sebastião da
Publication Date: 2024
Format: Doctoral thesis
Language: por
Source: Biblioteca Digital de Teses e Dissertações da UFPB
Download full: https://repositorio.ufpb.br/jspui/handle/123456789/34281
Summary: SrSnO3 perovskite (SSO) is a material with an orthorhombic structure (Pbnm) and has been the focus of numerous studies due to its potential technological applications, such as capacitors, gas sensors, humidity sensors, among others. In recent years, the number of studies in which this material has been successfully used in other important areas, such as catalysis and photocatalysis, has been increasing. In this work, photocatalysts based on pure SrSnO3 and doped with Cu2+ were synthesized by the modified Pechini method at a calcination temperature of 900 °C for 4 h. Photodeposition of Ag on the surface of the material was also performed using UV-C radiation, Ag@SSO. The obtained powders were characterized by X-ray diffraction (XRD), infrared (IR) spectroscopy, ultraviolet-visible region, Raman spectroscopy, field emission scanning electron microscopy (FE-SEM), scanning transmission electron microscopy (STEM), electron paramagnetic resonance (EPR) spectroscopy and zeta potential. The solids were subsequently tested in the photocatalysis reaction for generation of hydroxyl radicals (•OH) through the photohydroxylation of terephthalic acid, followed by analysis by fluorescence spectroscopy. The obtained materials had the dominant phase of SrSnO3 with low or almost no presence of the secondary phase of SrCO3. The characterization of SrSnO3 by EPR revealed the presence of the novel paramagnetic species of Sn3+ in addition to three other types of defects. The results of the photocatalytic evaluation for SrSnO3 demonstrated satisfactory performance in the generation of hydroxyl radicals, unlike the Cu2+ doped system, which demonstrated considerably lower performance, which can be initially attributed to a greater recombination of charge carriers (e-/h+) after the entry of copper into the SrSnO3 Crystal lattice. The best photocatalytic performance observed was for the Agx@SSO system, possibly associated with the interaction of silver on the perovskite surface sequestering electrons and preventing the recombination of charge carriers, thus ensuring oxidationreduction reactions in the respective valence and conduction bands, favoring the generation of efficient oxidative species for photocatalytic reactions. Finally, most of the solids showed promising photocatalytic activity in tetracycline degradation, reaching approximately 77% and 74% for the Ag@SSO_0,625 and AgAF@SSO_0,625 samples, respectively. For the photohydroxylation of terephthalic acid, the solids Ag@SSO_5,0 and AgAF@SSO_2,5 demonstrated excellent photocatalytic activity in the generation of 2-hydroxy-terephthalic acid.
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spelling Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálisePerovskitaSrSn03FotocatáliseEstanatos alcalinos terrososDeposição de prataDopagem com cobrePhotocatalysisAlkaline earth stannatesSilver depositionCopper dopingCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICASrSnO3 perovskite (SSO) is a material with an orthorhombic structure (Pbnm) and has been the focus of numerous studies due to its potential technological applications, such as capacitors, gas sensors, humidity sensors, among others. In recent years, the number of studies in which this material has been successfully used in other important areas, such as catalysis and photocatalysis, has been increasing. In this work, photocatalysts based on pure SrSnO3 and doped with Cu2+ were synthesized by the modified Pechini method at a calcination temperature of 900 °C for 4 h. Photodeposition of Ag on the surface of the material was also performed using UV-C radiation, Ag@SSO. The obtained powders were characterized by X-ray diffraction (XRD), infrared (IR) spectroscopy, ultraviolet-visible region, Raman spectroscopy, field emission scanning electron microscopy (FE-SEM), scanning transmission electron microscopy (STEM), electron paramagnetic resonance (EPR) spectroscopy and zeta potential. The solids were subsequently tested in the photocatalysis reaction for generation of hydroxyl radicals (•OH) through the photohydroxylation of terephthalic acid, followed by analysis by fluorescence spectroscopy. The obtained materials had the dominant phase of SrSnO3 with low or almost no presence of the secondary phase of SrCO3. The characterization of SrSnO3 by EPR revealed the presence of the novel paramagnetic species of Sn3+ in addition to three other types of defects. The results of the photocatalytic evaluation for SrSnO3 demonstrated satisfactory performance in the generation of hydroxyl radicals, unlike the Cu2+ doped system, which demonstrated considerably lower performance, which can be initially attributed to a greater recombination of charge carriers (e-/h+) after the entry of copper into the SrSnO3 Crystal lattice. The best photocatalytic performance observed was for the Agx@SSO system, possibly associated with the interaction of silver on the perovskite surface sequestering electrons and preventing the recombination of charge carriers, thus ensuring oxidationreduction reactions in the respective valence and conduction bands, favoring the generation of efficient oxidative species for photocatalytic reactions. Finally, most of the solids showed promising photocatalytic activity in tetracycline degradation, reaching approximately 77% and 74% for the Ag@SSO_0,625 and AgAF@SSO_0,625 samples, respectively. For the photohydroxylation of terephthalic acid, the solids Ag@SSO_5,0 and AgAF@SSO_2,5 demonstrated excellent photocatalytic activity in the generation of 2-hydroxy-terephthalic acid.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESA perovskita de SrSnO3 (SSO) é um material com estrutura ortorrômbica (Pbnm) e tem sido foco de inúmeras pesquisas em função de potenciais aplicações tecnológicas como: capacitores, sensores de gases, sensores de umidade entre outras. Nos últimos anos vem crescendo o número de trabalhos em que esse material vem sendo empregado com sucesso em outras áreas importantes como a catálise e fotocatálise. Nesse trabalho, fotocatalisadores à base de SrSnO3 puro e dopado com Cu2+ foram sintetizados pelo método de Pechini modificado em uma temperatura de calcinação de 900 °C por 4 h. Também foi realizada a fotodeposição de Ag na superfície do material utilizando radiação UV-C, Ag@SSO. Os pós obtidos foram caracterizados por difração de raios-X (DRX), espectroscopia na região do infravermelho (IR), na região do Ultravioletavisível, espectroscopia Raman, microscopia eletrônica de varredura por emissão de campo (FE-SEM), microscopia eletrônica de transmissão de varredura (STEM), espectroscopia de ressonância paramagnética eletrônica (EPR) e potencial Zeta. Os sólidos posteriormente foram testados na reação de fotocatálise para geração de radicais hidroxila (•OH) por meio da fotohidroxilação do ácido tereftálico, seguido de análise por espectroscopia de fluorescência. Os materiais obtidos tiveram a fase dominante do SrSnO3 com baixa ou quase nenhuma presença da fase secundária de SrCO3. A caracterização do SrSnO3 por EPR revelou a presença da espécie paramagnética inédita de Sn3+ além de outros três tipos de defeitos. Os resultados da avaliação fotocatalítica para o SrSnO3 demonstraram desempenho satisfatório na geração dos radicais hidroxila, diferentemente do sistema dopado com Cu2+ que demonstrou desempenho consideravelmente inferior, podendo ser atribuído inicialmente a uma maior recombinação dos portadores de carga (e-/h+) após a entrada do cobre na rede cristalina do SrSnO3. O melhor desempenho fotocatalítico observado foi para o sistema Agx@SSO, possivelmente associado à interação da prata na superfície da perovskita sequestrando elétrons e impedindo a recombinação dos portadores de carga garantindo assim as reações de oxirredução nas respectivas bandas de valência e condução favorecendo a geração de espécies oxidativas eficientes para reações fotocatalíticas. Por fim a maioria dos sólidos se mostraram promissores quanto à sua atividade fotocatalítica em degradação de Tetraciclina atingindo cerca de 77% e 74% para as amostras Ag@SSO_0,625 e AgAF@SSO_0,625 respectivamente. Já para a fotohidroxilação de ácido tereftálico os sólidos Ag@SSO_5,0 e AgAF@SSO_2,5 demonstraram excelente atividade fotocatalítica na geração do ácido 2-hidroxitereftálico.Universidade Federal da ParaíbaBrasilQuímicaPrograma de Pós-Graduação em QuímicaUFPBSantos, Ieda Maria Garcia doshttp://lattes.cnpq.br/7060067415685353Oliveira, André Luiz Menezes dehttp://lattes.cnpq.br/9080934823929646Maia, Ary da Silvahttp://lattes.cnpq.br/0234548596508203Silva, Adervando Sebastião da2025-04-18T23:33:36Z2024-08-262025-04-18T23:33:36Z2024-06-26info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesishttps://repositorio.ufpb.br/jspui/handle/123456789/34281porAttribution-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:UFPB2025-04-19T06:06:58Zoai:repositorio.ufpb.br:123456789/34281Biblioteca Digital de Teses e Dissertaçõeshttps://repositorio.ufpb.br/PUBhttp://tede.biblioteca.ufpb.br:8080/oai/requestdiretoria@ufpb.br|| bdtd@biblioteca.ufpb.bropendoar:2025-04-19T06:06:58Biblioteca Digital de Teses e Dissertações da UFPB - Universidade Federal da Paraíba (UFPB)false
dc.title.none.fl_str_mv Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
title Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
spellingShingle Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
Silva, Adervando Sebastião da
Perovskita
SrSn03
Fotocatálise
Estanatos alcalinos terrosos
Deposição de prata
Dopagem com cobre
Photocatalysis
Alkaline earth stannates
Silver deposition
Copper doping
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
title_full Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
title_fullStr Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
title_full_unstemmed Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
title_sort Perovskita à base de SrSnO3, caracterizada por EPR, e modificada com prata ou cobre, aplicada em fotocatálise
author Silva, Adervando Sebastião da
author_facet Silva, Adervando Sebastião da
author_role author
dc.contributor.none.fl_str_mv Santos, Ieda Maria Garcia dos
http://lattes.cnpq.br/7060067415685353
Oliveira, André Luiz Menezes de
http://lattes.cnpq.br/9080934823929646
Maia, Ary da Silva
http://lattes.cnpq.br/0234548596508203
dc.contributor.author.fl_str_mv Silva, Adervando Sebastião da
dc.subject.por.fl_str_mv Perovskita
SrSn03
Fotocatálise
Estanatos alcalinos terrosos
Deposição de prata
Dopagem com cobre
Photocatalysis
Alkaline earth stannates
Silver deposition
Copper doping
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
topic Perovskita
SrSn03
Fotocatálise
Estanatos alcalinos terrosos
Deposição de prata
Dopagem com cobre
Photocatalysis
Alkaline earth stannates
Silver deposition
Copper doping
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
description SrSnO3 perovskite (SSO) is a material with an orthorhombic structure (Pbnm) and has been the focus of numerous studies due to its potential technological applications, such as capacitors, gas sensors, humidity sensors, among others. In recent years, the number of studies in which this material has been successfully used in other important areas, such as catalysis and photocatalysis, has been increasing. In this work, photocatalysts based on pure SrSnO3 and doped with Cu2+ were synthesized by the modified Pechini method at a calcination temperature of 900 °C for 4 h. Photodeposition of Ag on the surface of the material was also performed using UV-C radiation, Ag@SSO. The obtained powders were characterized by X-ray diffraction (XRD), infrared (IR) spectroscopy, ultraviolet-visible region, Raman spectroscopy, field emission scanning electron microscopy (FE-SEM), scanning transmission electron microscopy (STEM), electron paramagnetic resonance (EPR) spectroscopy and zeta potential. The solids were subsequently tested in the photocatalysis reaction for generation of hydroxyl radicals (•OH) through the photohydroxylation of terephthalic acid, followed by analysis by fluorescence spectroscopy. The obtained materials had the dominant phase of SrSnO3 with low or almost no presence of the secondary phase of SrCO3. The characterization of SrSnO3 by EPR revealed the presence of the novel paramagnetic species of Sn3+ in addition to three other types of defects. The results of the photocatalytic evaluation for SrSnO3 demonstrated satisfactory performance in the generation of hydroxyl radicals, unlike the Cu2+ doped system, which demonstrated considerably lower performance, which can be initially attributed to a greater recombination of charge carriers (e-/h+) after the entry of copper into the SrSnO3 Crystal lattice. The best photocatalytic performance observed was for the Agx@SSO system, possibly associated with the interaction of silver on the perovskite surface sequestering electrons and preventing the recombination of charge carriers, thus ensuring oxidationreduction reactions in the respective valence and conduction bands, favoring the generation of efficient oxidative species for photocatalytic reactions. Finally, most of the solids showed promising photocatalytic activity in tetracycline degradation, reaching approximately 77% and 74% for the Ag@SSO_0,625 and AgAF@SSO_0,625 samples, respectively. For the photohydroxylation of terephthalic acid, the solids Ag@SSO_5,0 and AgAF@SSO_2,5 demonstrated excellent photocatalytic activity in the generation of 2-hydroxy-terephthalic acid.
publishDate 2024
dc.date.none.fl_str_mv 2024-08-26
2024-06-26
2025-04-18T23:33:36Z
2025-04-18T23:33:36Z
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/123456789/34281
url https://repositorio.ufpb.br/jspui/handle/123456789/34281
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|| bdtd@biblioteca.ufpb.br
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