Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol

Detalhes bibliográficos
Ano de defesa: 2019
Autor(a) principal: Magalhães, Monah Marques lattes
Orientador(a): Colmati Júnior, Flávio lattes
Banca de defesa: Colmati Júnior, Flávio, Ribeiro, Josimar, Souza, Elki Cristina de, Sgobbi, Lívia Flório, Cabral, Murilo Feitosa
Tipo de documento: Tese
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Universidade Federal de Goiás
Programa de Pós-Graduação: Programa de Pós-graduação em Química (IQ)
Departamento: Instituto de Química - IQ (RMG)
País: Brasil
Palavras-chave em Português:
EIE
Palavras-chave em Inglês:
EIS
Área do conhecimento CNPq:
Link de acesso: http://repositorio.bc.ufg.br/tede/handle/tede/13034
Resumo: Renewable energies are increasingly desirable. One of the proposed alternatives is proton-exchange membrane fuel cells (PEMFC). The use of ethanol as fuel in these cells is advantageous because it has a low contribution to the greenhouse effect when the CO2 cycle is completed. However, complete oxidation of the ethanol requires the breaking of the CC bond, to oxidize the intermediates that are formed during the reaction, which are stable and if not oxidized promote a decrease in the efficiency, due to the poisoning of Pt. The study is presented with catalysts of PtxSnyCuz supported on high surface area colloidal carbon. The electrocatalysts were produced with the alcohol reduction method. The synthesis used with modification to obtain the materials allowed the formation of nanoparticles with high catalytic activity, in the range of 2 to 3 nm. The physical characterization techniques used, such as XRD, MET and XPS, allowed to verify that the particles are crystalline, with majority crystal of the CFC structure of Pt, and that Sn and Cu atoms were inserted in this crystal, causing modifications in the peaks to the crystalline planes of the Pt network. Microscopies showed the morphology of the nanoparticles and helped to understand the relation of the high catalytic activity with the good dispersion of particles and their high surface area coming from their size. The analysis by XPS allowed to prove the elements present in the samples, besides determining the composition of atoms in the surface in which the catalysis occurs. The electrochemical characterization by VC showed the high activity of the ternaries with low potential values for the beginning of the ethanol oxidation compared to the Pt/C, PtSn/C and PtCu/C catalysts. The chromaamperometric technique evaluated the stability of the catalysts and verified that in the studied time the materials have constant and stable behavior. Through the EIS it was possible to understand the electrical resistance of the catalytic surface and to verify that such property for the ROE decreases as the potential increases, the studied compositions showed that the composition of the material influences in the reduction of the electrical resistance when oxidizing the molecule of ethanol and that can two or more reaction mechanisms occur during catalysis.
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spelling Colmati Júnior, Fláviohttp://lattes.cnpq.br/0231242349462585Colmati Júnior, FlávioRibeiro, JosimarSouza, Elki Cristina deSgobbi, Lívia FlórioCabral, Murilo Feitosahttp://lattes.cnpq.br/4284701321279523Magalhães, Monah Marques2023-09-08T11:20:53Z2023-09-08T11:20:53Z2019-11-28MAGALHÃES, M. M. Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol. 2023. 119 f. Tese (Doutorado em Química) - Universidade Federal de Goiás, Goiânia, 2019.http://repositorio.bc.ufg.br/tede/handle/tede/13034Renewable energies are increasingly desirable. One of the proposed alternatives is proton-exchange membrane fuel cells (PEMFC). The use of ethanol as fuel in these cells is advantageous because it has a low contribution to the greenhouse effect when the CO2 cycle is completed. However, complete oxidation of the ethanol requires the breaking of the CC bond, to oxidize the intermediates that are formed during the reaction, which are stable and if not oxidized promote a decrease in the efficiency, due to the poisoning of Pt. The study is presented with catalysts of PtxSnyCuz supported on high surface area colloidal carbon. The electrocatalysts were produced with the alcohol reduction method. The synthesis used with modification to obtain the materials allowed the formation of nanoparticles with high catalytic activity, in the range of 2 to 3 nm. The physical characterization techniques used, such as XRD, MET and XPS, allowed to verify that the particles are crystalline, with majority crystal of the CFC structure of Pt, and that Sn and Cu atoms were inserted in this crystal, causing modifications in the peaks to the crystalline planes of the Pt network. Microscopies showed the morphology of the nanoparticles and helped to understand the relation of the high catalytic activity with the good dispersion of particles and their high surface area coming from their size. The analysis by XPS allowed to prove the elements present in the samples, besides determining the composition of atoms in the surface in which the catalysis occurs. The electrochemical characterization by VC showed the high activity of the ternaries with low potential values for the beginning of the ethanol oxidation compared to the Pt/C, PtSn/C and PtCu/C catalysts. The chromaamperometric technique evaluated the stability of the catalysts and verified that in the studied time the materials have constant and stable behavior. Through the EIS it was possible to understand the electrical resistance of the catalytic surface and to verify that such property for the ROE decreases as the potential increases, the studied compositions showed that the composition of the material influences in the reduction of the electrical resistance when oxidizing the molecule of ethanol and that can two or more reaction mechanisms occur during catalysis.As energias renováveis são cada vez mais desejáveis. Uma das alternativas proposta são as células a combustíveis de membrana trocadora de prótons (do inglês PEMFC). A utilização de etanol como combustível nessas células é vantajosa por apresentar contribuição baixa para o efeito estufa quando completado o ciclo do CO2. Porém, a oxidação completa do etanol requer a quebra da ligação C-C, para oxidar os intermediários que são formados durante a reação, que são estáveis e se não forem oxidados promovem diminuição na eficiência, decorrente do envenenamento da Pt. É apresentado o estudo com catalisadores de PtxSnyCuz suportados em carbono coloidal de alta área superficial. Os eletrocatalisadores foram produzidos com o método de redução por álcool. A síntese empregada com modificação para obtenção dos materiais possibilitou a formação de nanopartículas com elevada atividade catalítica, na faixa de 2 a 3 nm. As técnicas de caraterização física utilizadas, tais como DRX, MET e XPS, permitiram verificar que as partículas são cristalinas, com cristal majoritário da estrutura CFC da Pt, e que os átomos de Sn e Cu se inseriram nesse cristal, provocando modificações nos picos referentes aos planos cristalinos da rede de Pt. As microscopias mostraram a morfologia das nanopartículas e auxiliaram a compreender a relação da alta atividade catalítica com a boa dispersão de partículas e sua alta área superficial proveniente do tamanho destas. A análise por XPS permitiu comprovar os elementos presentes nas amostras, além de determinar a composição de átomos na superfície em que ocorre a catálise. A caracterização eletroquímica por VC mostrou a elevada atividade dos ternários com baixos valores de potencial para o início da oxidação de etanol comparados aos catalisadores de Pt/C, PtSn/C e PtCu/C. A técnica cronoamperométrica avaliou a estabilidade dos catalisadores e verificou que no tempo estudado os materiais possuem comportamento constante e estável. Através da EIE foi possível compreender a resistência elétrica da superfície catalítica e verificar que tal propriedade para a ROE diminui conforme aumenta o potencial, as composições estudadas mostraram que a composição do material influencia na diminuição da resistência elétrica ao oxidar a molécula de etanol e que podem ocorrer dois ou mais mecanismos reacionais durante a catálise.Submitted by Marlene Santos (marlene.bc.ufg@gmail.com) on 2023-09-06T18:47:58Z No. of bitstreams: 2 Tese - Monah Marques Magalhães - 2023.pdf: 8574577 bytes, checksum: 843a3ee66f1ee01c21005bed766755d1 (MD5) license_rdf: 805 bytes, checksum: 4460e5956bc1d1639be9ae6146a50347 (MD5)Approved for entry into archive by Luciana Ferreira (lucgeral@gmail.com) on 2023-09-08T11:20:53Z (GMT) No. of bitstreams: 2 Tese - Monah Marques Magalhães - 2023.pdf: 8574577 bytes, checksum: 843a3ee66f1ee01c21005bed766755d1 (MD5) license_rdf: 805 bytes, checksum: 4460e5956bc1d1639be9ae6146a50347 (MD5)Made available in DSpace on 2023-09-08T11:20:53Z (GMT). No. of bitstreams: 2 Tese - Monah Marques Magalhães - 2023.pdf: 8574577 bytes, checksum: 843a3ee66f1ee01c21005bed766755d1 (MD5) license_rdf: 805 bytes, checksum: 4460e5956bc1d1639be9ae6146a50347 (MD5) Previous issue date: 2019-11-28Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESFundação de Amparo à Pesquisa do Estado de GoiásporUniversidade Federal de GoiásPrograma de Pós-graduação em Química (IQ)UFGBrasilInstituto de Química - IQ (RMG)Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessEtanolCatalisadoresCélula combustívelPEMFCEIEPtSnCu/CPtCu/CEthanolCatalystsFuel cellEISCIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICASíntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanolSynthesis and characterization of nanostructured catalysts containing PtSnCu for the electrochemical presentation of ethanolinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesis8450050050050050029109213reponame:Biblioteca Digital de Teses e Dissertações da UFGinstname:Universidade Federal de Goiás (UFG)instacron:UFGORIGINALTese - Monah Marques Magalhães - 2023.pdfTese - Monah Marques Magalhães - 2023.pdfapplication/pdf8574577http://repositorio.bc.ufg.br/tede/bitstreams/ee6d511c-b836-425e-aacd-9081cd4a97bf/download843a3ee66f1ee01c21005bed766755d1MD53LICENSElicense.txtlicense.txttext/plain; charset=utf-81748http://repositorio.bc.ufg.br/tede/bitstreams/56873c5d-a0f4-4686-875a-e2f2f2795ca6/download8a4605be74aa9ea9d79846c1fba20a33MD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8805http://repositorio.bc.ufg.br/tede/bitstreams/f560e36c-d17a-456d-99be-bda5dd141137/download4460e5956bc1d1639be9ae6146a50347MD52tede/130342023-09-08 08:20:53.623http://creativecommons.org/licenses/by-nc-nd/4.0/Attribution-NonCommercial-NoDerivatives 4.0 Internationalopen.accessoai:repositorio.bc.ufg.br:tede/13034http://repositorio.bc.ufg.br/tedeBiblioteca Digital de Teses e Dissertaçõeshttp://repositorio.bc.ufg.br/PUBhttps://repositorio.bc.ufg.br/tede_oai/requesttesesdissertacoes.bc@ufg.br ||tesesdissertacoes.bc@ufg.bropendoar:32082023-09-08T11:20:53Biblioteca Digital de Teses e Dissertações da UFG - Universidade Federal de Goiás (UFG)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
dc.title.pt_BR.fl_str_mv Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
dc.title.alternative.eng.fl_str_mv Synthesis and characterization of nanostructured catalysts containing PtSnCu for the electrochemical presentation of ethanol
title Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
spellingShingle Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
Magalhães, Monah Marques
Etanol
Catalisadores
Célula combustível
PEMFC
EIE
PtSnCu/C
PtCu/C
Ethanol
Catalysts
Fuel cell
EIS
CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA
title_short Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
title_full Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
title_fullStr Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
title_full_unstemmed Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
title_sort Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol
author Magalhães, Monah Marques
author_facet Magalhães, Monah Marques
author_role author
dc.contributor.advisor1.fl_str_mv Colmati Júnior, Flávio
dc.contributor.advisor1Lattes.fl_str_mv http://lattes.cnpq.br/0231242349462585
dc.contributor.referee1.fl_str_mv Colmati Júnior, Flávio
dc.contributor.referee2.fl_str_mv Ribeiro, Josimar
dc.contributor.referee3.fl_str_mv Souza, Elki Cristina de
dc.contributor.referee4.fl_str_mv Sgobbi, Lívia Flório
dc.contributor.referee5.fl_str_mv Cabral, Murilo Feitosa
dc.contributor.authorLattes.fl_str_mv http://lattes.cnpq.br/4284701321279523
dc.contributor.author.fl_str_mv Magalhães, Monah Marques
contributor_str_mv Colmati Júnior, Flávio
Colmati Júnior, Flávio
Ribeiro, Josimar
Souza, Elki Cristina de
Sgobbi, Lívia Flório
Cabral, Murilo Feitosa
dc.subject.por.fl_str_mv Etanol
Catalisadores
Célula combustível
PEMFC
EIE
PtSnCu/C
PtCu/C
topic Etanol
Catalisadores
Célula combustível
PEMFC
EIE
PtSnCu/C
PtCu/C
Ethanol
Catalysts
Fuel cell
EIS
CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA
dc.subject.eng.fl_str_mv Ethanol
Catalysts
Fuel cell
EIS
dc.subject.cnpq.fl_str_mv CIENCIAS EXATAS E DA TERRA::QUIMICA::FISICO-QUIMICA
description Renewable energies are increasingly desirable. One of the proposed alternatives is proton-exchange membrane fuel cells (PEMFC). The use of ethanol as fuel in these cells is advantageous because it has a low contribution to the greenhouse effect when the CO2 cycle is completed. However, complete oxidation of the ethanol requires the breaking of the CC bond, to oxidize the intermediates that are formed during the reaction, which are stable and if not oxidized promote a decrease in the efficiency, due to the poisoning of Pt. The study is presented with catalysts of PtxSnyCuz supported on high surface area colloidal carbon. The electrocatalysts were produced with the alcohol reduction method. The synthesis used with modification to obtain the materials allowed the formation of nanoparticles with high catalytic activity, in the range of 2 to 3 nm. The physical characterization techniques used, such as XRD, MET and XPS, allowed to verify that the particles are crystalline, with majority crystal of the CFC structure of Pt, and that Sn and Cu atoms were inserted in this crystal, causing modifications in the peaks to the crystalline planes of the Pt network. Microscopies showed the morphology of the nanoparticles and helped to understand the relation of the high catalytic activity with the good dispersion of particles and their high surface area coming from their size. The analysis by XPS allowed to prove the elements present in the samples, besides determining the composition of atoms in the surface in which the catalysis occurs. The electrochemical characterization by VC showed the high activity of the ternaries with low potential values for the beginning of the ethanol oxidation compared to the Pt/C, PtSn/C and PtCu/C catalysts. The chromaamperometric technique evaluated the stability of the catalysts and verified that in the studied time the materials have constant and stable behavior. Through the EIS it was possible to understand the electrical resistance of the catalytic surface and to verify that such property for the ROE decreases as the potential increases, the studied compositions showed that the composition of the material influences in the reduction of the electrical resistance when oxidizing the molecule of ethanol and that can two or more reaction mechanisms occur during catalysis.
publishDate 2019
dc.date.issued.fl_str_mv 2019-11-28
dc.date.accessioned.fl_str_mv 2023-09-08T11:20:53Z
dc.date.available.fl_str_mv 2023-09-08T11:20:53Z
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dc.identifier.citation.fl_str_mv MAGALHÃES, M. M. Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol. 2023. 119 f. Tese (Doutorado em Química) - Universidade Federal de Goiás, Goiânia, 2019.
dc.identifier.uri.fl_str_mv http://repositorio.bc.ufg.br/tede/handle/tede/13034
identifier_str_mv MAGALHÃES, M. M. Síntese e caracterização de catalisadores nanoestruturados contendo PtSnCu para a oxidação eletroquímica de etanol. 2023. 119 f. Tese (Doutorado em Química) - Universidade Federal de Goiás, Goiânia, 2019.
url http://repositorio.bc.ufg.br/tede/handle/tede/13034
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dc.relation.cnpq.fl_str_mv 1092
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dc.publisher.none.fl_str_mv Universidade Federal de Goiás
dc.publisher.program.fl_str_mv Programa de Pós-graduação em Química (IQ)
dc.publisher.initials.fl_str_mv UFG
dc.publisher.country.fl_str_mv Brasil
dc.publisher.department.fl_str_mv Instituto de Química - IQ (RMG)
publisher.none.fl_str_mv Universidade Federal de Goiás
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