Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2
| Ano de defesa: | 2016 |
|---|---|
| Autor(a) principal: | |
| Orientador(a): | |
| Banca de defesa: | , |
| Tipo de documento: | Dissertação |
| Tipo de acesso: | Acesso aberto |
| Idioma: | por |
| Instituição de defesa: |
Universidade Federal de Alfenas
|
| Programa de Pós-Graduação: |
Programa de Pós-Graduação em Ciência e Engenharia de Materiais
|
| Departamento: |
Instituto de Ciência e Tecnologia
|
| País: |
Brasil
|
| Palavras-chave em Português: | |
| Área do conhecimento CNPq: | |
| Link de acesso: | https://repositorio.unifal-mg.edu.br/handle/123456789/1068 |
Resumo: | The environmental problems have been intensified by accumulation of carbon dioxide (CO2) in the atmosphere. Photocatalytic processes can be used to convert CO2 into other value-added compounds. For this purpose, semiconductors are used as photocatalysts and one of the most utilized is ZnO. The photocatalytic activity is usually improved by doping, thus, in this work, methods of synthesis of ZnO doped with N (ZnO:N) using urea as N source are analyzed. Four doping methods were evaluated by adding urea in the particles of: (1) amorphous ZnO and (2) crystalline ZnO; and in the solution of Zn (3) after polymerizing agent (PA) and (4) before PA. The materials were heat-treated (HT) in nine different conditions (400 °C, 450 °C and 500 °C for 2 h, 12 h and 24 h) and characterized by TGA/DTG, XRD, Raman, FTIR, XPS, DRS, BET and SEM-FEG. By TGA/DTG it was noticed that the temperature of 400 oC was not appropriate for synthesis of the particles. By XRD, it was observed that the samples are in the wurtzite phase of ZnO, the crystallites are in nanometer scale and they increase their size with the increment in the temperature and time of HT. By Raman and FTIR, it was verified that higher times of HT and/or the methodology 4 (M4) provide samples with higher symmetry and less contaminants adsorbed in the surface. By XPS, it was identified the doping of N in the crystalline structure of some previously select samples. By DRS, it was found that pure ZnO has lower band gap than the reported in the literature, fact that is related to the synthesis method. Then, it was identified that particles synthesized in higher times of HT and/or by the M4 have greater definition of crystallinity and lower quantity of residues of synthesis. Other characterizations were done for pure ZnO (ZP) and the samples of ZnO:N synthesized by M4. By BET and SEM-FEG, it was observed a tendency in the decrease of surface area with the increase in the temperature of HT due to the formation of clusters in higher temperatures of HT. Therefore, it was used ZP and the samples synthesized by M4 as photocatalysts in the reaction of photoreduction of CO2. The progress in the reaction was monitored by CH4 production. It was noticed that lower times of HT provide materials with better photocatalytic activity since the higher quantities of CH4 were identified for the samples synthesized by M4 e submitted to heat treatment at 450 ºC for 2 h and 500 ºC for 2 h. |
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Oliveira, Jéssica Ariane Dehttp://lattes.cnpq.br/0847092755379350Poirier, Gael Yveshttp://lattes.cnpq.br/2457188837334937Mendonça, Vagner Romito DeHirano, Laos AlexandreGiraldi, Tania Reginahttp://lattes.cnpq.br/47657671509214392018-01-05T20:04:31Z2016-02-29OLIVEIRA, Jéssica Ariane de. Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2. 2016. 93 f. Dissertação (Mestrado em Ciência e Engenharia de Materiais) - Universidade Federal de Alfenas, Poços de Caldas, MG, 2016.https://repositorio.unifal-mg.edu.br/handle/123456789/1068The environmental problems have been intensified by accumulation of carbon dioxide (CO2) in the atmosphere. Photocatalytic processes can be used to convert CO2 into other value-added compounds. For this purpose, semiconductors are used as photocatalysts and one of the most utilized is ZnO. The photocatalytic activity is usually improved by doping, thus, in this work, methods of synthesis of ZnO doped with N (ZnO:N) using urea as N source are analyzed. Four doping methods were evaluated by adding urea in the particles of: (1) amorphous ZnO and (2) crystalline ZnO; and in the solution of Zn (3) after polymerizing agent (PA) and (4) before PA. The materials were heat-treated (HT) in nine different conditions (400 °C, 450 °C and 500 °C for 2 h, 12 h and 24 h) and characterized by TGA/DTG, XRD, Raman, FTIR, XPS, DRS, BET and SEM-FEG. By TGA/DTG it was noticed that the temperature of 400 oC was not appropriate for synthesis of the particles. By XRD, it was observed that the samples are in the wurtzite phase of ZnO, the crystallites are in nanometer scale and they increase their size with the increment in the temperature and time of HT. By Raman and FTIR, it was verified that higher times of HT and/or the methodology 4 (M4) provide samples with higher symmetry and less contaminants adsorbed in the surface. By XPS, it was identified the doping of N in the crystalline structure of some previously select samples. By DRS, it was found that pure ZnO has lower band gap than the reported in the literature, fact that is related to the synthesis method. Then, it was identified that particles synthesized in higher times of HT and/or by the M4 have greater definition of crystallinity and lower quantity of residues of synthesis. Other characterizations were done for pure ZnO (ZP) and the samples of ZnO:N synthesized by M4. By BET and SEM-FEG, it was observed a tendency in the decrease of surface area with the increase in the temperature of HT due to the formation of clusters in higher temperatures of HT. Therefore, it was used ZP and the samples synthesized by M4 as photocatalysts in the reaction of photoreduction of CO2. The progress in the reaction was monitored by CH4 production. It was noticed that lower times of HT provide materials with better photocatalytic activity since the higher quantities of CH4 were identified for the samples synthesized by M4 e submitted to heat treatment at 450 ºC for 2 h and 500 ºC for 2 h.O acúmulo de gás carbônico (CO2) na atmosfera tem intensificado os problemas ambientais. Processos fotocatalíticos podem ser empregados para converter o CO2 em outros compostos com valores agregados. Para tanto, utilizam-se semicondutores como fotocatalisadores e um dos mais empregados é o óxido de zinco (ZnO). Geralmente a dopagem melhora a atividade fotocatalítica do semicondutor, logo, o presente estudo analisa metodologias de síntese de ZnO dopado com N (ZnO:N), utilizando a ureia como fonte de N. Foram analisadas quatro metodologias de dopagem pela adição de ureia em partículas de: (1) ZnO amorfo e (2) ZnO cristalino; e na solução de Zn (3) posteriormente ao agente polimerizante (AP) e (4) anteriormente ao AP. Os materiais obtidos foram submetidos a tratamento térmico (TT) em nove condições distintas (400 ºC, 450 ºC e 500 ºC por 2 h, 12 h e 24 h) e caracterizados por TGA/DTG, DRX, Raman, FTIR, XPS, DRS, BET e MEV-FEG. Por TGA/DTG, constatou-se que a temperatura de 400 ºC não foi adequada para a obtenção das partículas. Por DRX, observou-se que as amostras possuem a fase wurtzita do ZnO, os cristalitos se encontram em escala nanométrica e aumentam de tamanho conforme se aumenta a temperatura e o tempo do TT. Por Raman e por FTIR, verificou-se que maiores tempos de TT e/ou a metodologia 4 (M4) fornecem amostras com maior simetria e menos contaminantes adsorvidos na superfície. Por XPS, averiguou-se a dopagem de N na rede cristalina de algumas amostras previamente selecionadas. Por DRS, observou-se que o ZnO puro possui band gap inferior ao relatado na literatura, sendo esse fato relacionado ao método de síntese utilizado. Percebeu-se, pois, que as partículas sintetizadas em maiores tempos de TT e/ou pela M4 possuem maior definição de cristalinidade e menor quantidade de resíduos de síntese. Outras caracterizações foram feitas para ZnO puro (ZP) e para as amostras de ZnO:N obtidas pela M4, observando-se por BET e MEV-FEG uma tendência na diminuição de área superficial com o aumento da temperatura de TT, fato esse decorrente da formação de aglomerados em maiores temperaturas de TT. Por fim, empregaram-se ZP e as amostras sintetizadas pela M4 como fotocatalisadores na reação de fotorredução do CO2. Monitorou-se o avanço da reação pela produção de CH4, identificando-se que menores tempos de TT fornecem materiais com melhores atividades fotocatalíticas, já que maiores quantidades de CH4 foram identificadas para as amostras obtidas pela M4 e submetidas a tratamento térmico de 450 ºC por 2 h e 500 ºC por 2 h.Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPESapplication/pdfporUniversidade Federal de AlfenasPrograma de Pós-Graduação em Ciência e Engenharia de MateriaisUNIFAL-MGBrasilInstituto de Ciência e Tecnologiainfo:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc-nd/4.0/Óxido de zinco.Nanopartículas.Fotocatálise.MATERIAIS NAO METALICOS::CERAMICOSObtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2Synthesis of nitrogen doped ZnO nanoparticles for application in the photocatalytic reaction of CO2 reductioninfo:eu-repo/semantics/masterThesisinfo:eu-repo/semantics/publishedVersion-429741725949863893160060060048338425044343672042075167498588264571reponame:Repositório Institucional da Universidade Federal de Alfenas - RiUnifalinstname:Universidade Federal de Alfenas (UNIFAL)instacron:UNIFALOliveira, Jéssica Ariane DeLICENSElicense.txtlicense.txttext/plain; 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| dc.title.pt-BR.fl_str_mv |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 |
| dc.title.alternative.eng.fl_str_mv |
Synthesis of nitrogen doped ZnO nanoparticles for application in the photocatalytic reaction of CO2 reduction |
| title |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 |
| spellingShingle |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 Oliveira, Jéssica Ariane De Óxido de zinco. Nanopartículas. Fotocatálise. MATERIAIS NAO METALICOS::CERAMICOS |
| title_short |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 |
| title_full |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 |
| title_fullStr |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 |
| title_full_unstemmed |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 |
| title_sort |
Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2 |
| author |
Oliveira, Jéssica Ariane De |
| author_facet |
Oliveira, Jéssica Ariane De |
| author_role |
author |
| dc.contributor.author.fl_str_mv |
Oliveira, Jéssica Ariane De |
| dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/0847092755379350 |
| dc.contributor.advisor-co1.fl_str_mv |
Poirier, Gael Yves |
| dc.contributor.advisor-co1Lattes.fl_str_mv |
http://lattes.cnpq.br/2457188837334937 |
| dc.contributor.referee1.fl_str_mv |
Mendonça, Vagner Romito De |
| dc.contributor.referee2.fl_str_mv |
Hirano, Laos Alexandre |
| dc.contributor.advisor1.fl_str_mv |
Giraldi, Tania Regina |
| dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/4765767150921439 |
| contributor_str_mv |
Poirier, Gael Yves Mendonça, Vagner Romito De Hirano, Laos Alexandre Giraldi, Tania Regina |
| dc.subject.por.fl_str_mv |
Óxido de zinco. Nanopartículas. Fotocatálise. |
| topic |
Óxido de zinco. Nanopartículas. Fotocatálise. MATERIAIS NAO METALICOS::CERAMICOS |
| dc.subject.cnpq.fl_str_mv |
MATERIAIS NAO METALICOS::CERAMICOS |
| description |
The environmental problems have been intensified by accumulation of carbon dioxide (CO2) in the atmosphere. Photocatalytic processes can be used to convert CO2 into other value-added compounds. For this purpose, semiconductors are used as photocatalysts and one of the most utilized is ZnO. The photocatalytic activity is usually improved by doping, thus, in this work, methods of synthesis of ZnO doped with N (ZnO:N) using urea as N source are analyzed. Four doping methods were evaluated by adding urea in the particles of: (1) amorphous ZnO and (2) crystalline ZnO; and in the solution of Zn (3) after polymerizing agent (PA) and (4) before PA. The materials were heat-treated (HT) in nine different conditions (400 °C, 450 °C and 500 °C for 2 h, 12 h and 24 h) and characterized by TGA/DTG, XRD, Raman, FTIR, XPS, DRS, BET and SEM-FEG. By TGA/DTG it was noticed that the temperature of 400 oC was not appropriate for synthesis of the particles. By XRD, it was observed that the samples are in the wurtzite phase of ZnO, the crystallites are in nanometer scale and they increase their size with the increment in the temperature and time of HT. By Raman and FTIR, it was verified that higher times of HT and/or the methodology 4 (M4) provide samples with higher symmetry and less contaminants adsorbed in the surface. By XPS, it was identified the doping of N in the crystalline structure of some previously select samples. By DRS, it was found that pure ZnO has lower band gap than the reported in the literature, fact that is related to the synthesis method. Then, it was identified that particles synthesized in higher times of HT and/or by the M4 have greater definition of crystallinity and lower quantity of residues of synthesis. Other characterizations were done for pure ZnO (ZP) and the samples of ZnO:N synthesized by M4. By BET and SEM-FEG, it was observed a tendency in the decrease of surface area with the increase in the temperature of HT due to the formation of clusters in higher temperatures of HT. Therefore, it was used ZP and the samples synthesized by M4 as photocatalysts in the reaction of photoreduction of CO2. The progress in the reaction was monitored by CH4 production. It was noticed that lower times of HT provide materials with better photocatalytic activity since the higher quantities of CH4 were identified for the samples synthesized by M4 e submitted to heat treatment at 450 ºC for 2 h and 500 ºC for 2 h. |
| publishDate |
2016 |
| dc.date.issued.fl_str_mv |
2016-02-29 |
| dc.date.accessioned.fl_str_mv |
2018-01-05T20:04:31Z |
| dc.type.driver.fl_str_mv |
info:eu-repo/semantics/masterThesis |
| dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
| format |
masterThesis |
| status_str |
publishedVersion |
| dc.identifier.citation.fl_str_mv |
OLIVEIRA, Jéssica Ariane de. Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2. 2016. 93 f. Dissertação (Mestrado em Ciência e Engenharia de Materiais) - Universidade Federal de Alfenas, Poços de Caldas, MG, 2016. |
| dc.identifier.uri.fl_str_mv |
https://repositorio.unifal-mg.edu.br/handle/123456789/1068 |
| identifier_str_mv |
OLIVEIRA, Jéssica Ariane de. Obtenção de nanopartículas de ZnO dopado com nitrogênio para a reação fotocatalítica de redução do CO2. 2016. 93 f. Dissertação (Mestrado em Ciência e Engenharia de Materiais) - Universidade Federal de Alfenas, Poços de Caldas, MG, 2016. |
| url |
https://repositorio.unifal-mg.edu.br/handle/123456789/1068 |
| dc.language.iso.fl_str_mv |
por |
| language |
por |
| dc.relation.department.fl_str_mv |
-4297417259498638931 |
| dc.relation.confidence.fl_str_mv |
600 600 600 |
| dc.relation.cnpq.fl_str_mv |
4833842504434367204 |
| dc.relation.sponsorship.fl_str_mv |
2075167498588264571 |
| dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by-nc-nd/4.0/ |
| eu_rights_str_mv |
openAccess |
| rights_invalid_str_mv |
http://creativecommons.org/licenses/by-nc-nd/4.0/ |
| dc.format.none.fl_str_mv |
application/pdf |
| dc.publisher.none.fl_str_mv |
Universidade Federal de Alfenas |
| dc.publisher.program.fl_str_mv |
Programa de Pós-Graduação em Ciência e Engenharia de Materiais |
| dc.publisher.initials.fl_str_mv |
UNIFAL-MG |
| dc.publisher.country.fl_str_mv |
Brasil |
| dc.publisher.department.fl_str_mv |
Instituto de Ciência e Tecnologia |
| publisher.none.fl_str_mv |
Universidade Federal de Alfenas |
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