Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors
Ano de defesa: | 2020 |
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Autor(a) principal: | |
Orientador(a): | |
Banca de defesa: | |
Tipo de documento: | Tese |
Tipo de acesso: | Acesso aberto |
Idioma: | eng |
Instituição de defesa: |
Universidade Federal de São Carlos
Câmpus São Carlos |
Programa de Pós-Graduação: |
Programa de Pós-Graduação em Ciência e Engenharia de Materiais - PPGCEM
|
Departamento: |
Não Informado pela instituição
|
País: |
Não Informado pela instituição
|
Palavras-chave em Português: | |
Palavras-chave em Inglês: | |
Área do conhecimento CNPq: | |
Link de acesso: | https://repositorio.ufscar.br/handle/ufscar/15392 |
Resumo: | CH3NH3SnI3 is an environmentally-friendly (lead-free) perovskite whose synthesis depends on SnI2. Some disadvantages of SnI2 include high cost and tin(IV) contamination. Thus, SnSO4 and C16H30O4Sn are presented as cheaper alternatives and different synthesis conditions were studied: 110 oC/10 min, 150 oC/10 min and 150 oC/20 min. Based on X-ray diffraction results, CH3NH3SnI3 was successfully synthesized, being 110 oC/10 min sufficient for phase formation. However, annealing at 150 oC improved crystallinity irrespective of precursor while prolonged annealing time (20 min) was detrimental to the C16H30O4Sn-based perovskite. Film morphology differed by type of precursor. The bandgaps (1.37-1.59 eV) and photoluminescence emissions (831 nm) of the samples characterize them as visible light active semiconductors. Because CH3NH3SnI3 suffers from Sn2+ oxidation to Sn4+, some studies have proposed doping with metal cations. So far, Mn has not been tested. Thus, Mn (2% and 10% mol) doped CH3NH3SnI3 samples were synthesized and characterized. Mn did not disrupt the perovskite structure but slightly increased bandgap. Chlorine from the Mn precursor is not eliminated by annealing, thus could affect material properties. Regarding stability, Mn partially stabilized CH3NH3SnI3, indicating the need for an optimum level of doping. Mn doping does not seem to improve the photovoltaic properties of CH3NH3SnI3, but it should be noted that the solar cells were not optimized. Several questions about CH3NH3SnI3 cells are still open, including alternative TiO2 compatible with the same. Here, oxygen-deficient TiO2 powders were studied. Electron paramagnetic spectroscopy and X-ray photoelectron spectroscopy confirmed oxygen vacancy. Photocatalytic and photocurrent tests showed activity under visible light and an optimum level of oxygen vacancies for lower recombination and high charge separation, important properties for photovoltaic applications. |
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Dawson, MargaretMorelli, Márcio Raymundohttp://lattes.cnpq.br/0172837599844991Oliveira, Cauê Ribeiro dehttp://lattes.cnpq.br/5321313558714462http://lattes.cnpq.br/57100234138749402d693bbd-6008-403f-a8a9-8919bb3cd95c2021-12-21T14:11:27Z2021-12-21T14:11:27Z2020-02-14DAWSON, Margaret. Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors. 2020. Tese (Doutorado em Ciência e Engenharia de Materiais) – Universidade Federal de São Carlos, São Carlos, 2020. Disponível em: https://repositorio.ufscar.br/handle/ufscar/15392.https://repositorio.ufscar.br/handle/ufscar/15392CH3NH3SnI3 is an environmentally-friendly (lead-free) perovskite whose synthesis depends on SnI2. Some disadvantages of SnI2 include high cost and tin(IV) contamination. Thus, SnSO4 and C16H30O4Sn are presented as cheaper alternatives and different synthesis conditions were studied: 110 oC/10 min, 150 oC/10 min and 150 oC/20 min. Based on X-ray diffraction results, CH3NH3SnI3 was successfully synthesized, being 110 oC/10 min sufficient for phase formation. However, annealing at 150 oC improved crystallinity irrespective of precursor while prolonged annealing time (20 min) was detrimental to the C16H30O4Sn-based perovskite. Film morphology differed by type of precursor. The bandgaps (1.37-1.59 eV) and photoluminescence emissions (831 nm) of the samples characterize them as visible light active semiconductors. Because CH3NH3SnI3 suffers from Sn2+ oxidation to Sn4+, some studies have proposed doping with metal cations. So far, Mn has not been tested. Thus, Mn (2% and 10% mol) doped CH3NH3SnI3 samples were synthesized and characterized. Mn did not disrupt the perovskite structure but slightly increased bandgap. Chlorine from the Mn precursor is not eliminated by annealing, thus could affect material properties. Regarding stability, Mn partially stabilized CH3NH3SnI3, indicating the need for an optimum level of doping. Mn doping does not seem to improve the photovoltaic properties of CH3NH3SnI3, but it should be noted that the solar cells were not optimized. Several questions about CH3NH3SnI3 cells are still open, including alternative TiO2 compatible with the same. Here, oxygen-deficient TiO2 powders were studied. Electron paramagnetic spectroscopy and X-ray photoelectron spectroscopy confirmed oxygen vacancy. Photocatalytic and photocurrent tests showed activity under visible light and an optimum level of oxygen vacancies for lower recombination and high charge separation, important properties for photovoltaic applications.CH3NH3SnI3 é uma perovskita ambientalmente amigável (sem chumbo) normalmente sintetizada a partir de Snl2, que apresenta algumas desvantagens como elevado custo e contaminação por Sn(IV). Diante disso, SnSO4 e C16H30O4Sn são apresentados como precursores alternativos para a síntese de CH3NH3SnI3 em diferentes temperaturas e tempos de tratamentos térmicos (110 oC /10 min, 150 oC /10 min e 150 oC /20 min). A eficácia da síntese de CH3NH3SnI3 a partir dos precursores apresentados foi confirmada por raio-X. O tratamento térmico a 110 oC /10 min foi suficiente para a formação de fase, a 150 oC/10min melhorou a cristalinidade, independentemente do precursor, porém a 150 oC/20 min foi prejudicial para a perovskita produzida com C16H30O4Sn. As energias de bandgaps entre 1,37-1,59 eV e valores de emissão de fotoluminescência de 831 nm confirmam que as amostras sintetizadas são semicondutores ativos sob luz visível. Além disso, diferentes morfologias de filmes foram obtidas para cada tipo de precursor utilizado. A CH3NH3SnI3 sintetizada a partir de SnI2 foi dopada com Mn ( 2% e 10% mol de MnCl2) a fim de controlar a sua oxidação. A caracterizacão das amostras dopadas mostrou que o Mn estabiliza parcialmente a CH3NH3SnI3 contra degradação, mas não resulta em nenhuma melhora do desempenho final das células solares. Além disso, o cloro proveniente do MnCl2 não foi eliminado durante o tratamento térmico, o que pode influenciar as propriedades finais do material. Observou-se que o Mn não alterou a estrutura da perovskita, mas aumentou ligeiramente a sua energia de bandgap, mas ainda são necessários estudos para otimizar o nível de dopagem. Várias questões sobre as células de CH3NH3SnI3 ainda estão abertas, incluindo o TiO2 alternativo compatível com as mesmas. Neste trabalho, pós de TiO2 deficientes em oxigênio foram estudados a partir da análise de espectroscopia paramagnética de elétrons e a espectroscopia de fotoelétrons de raios-X. Os resultados confirmaram a vacância de oxigênio. Os testes fotocatalíticos e fotocorrentes mostraram atividade sob luz visível, um nível ótimo de vacâncias de oxigênio para menor recombinação e alta separação de carga, propriedades importantes para aplicações fotovoltaicas.Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)CNPq: 141704/2015-2engUniversidade Federal de São CarlosCâmpus São CarlosPrograma de Pós-Graduação em Ciência e Engenharia de Materiais - PPGCEMUFSCarAttribution-NonCommercial-NoDerivs 3.0 Brazilhttp://creativecommons.org/licenses/by-nc-nd/3.0/br/info:eu-repo/semantics/openAccessPerovskita orgânica-inorgânica de estanhoPerovskita de haleto de estanhoDopagem com MnPrecursor de estanhoTiO2 deficiente de oxigênioMaterial para célula solarOrganic-inorganic tin perovskiteTin halide perovskiteMn dopingTin precursorOxygen deficient TiO2Solar cell materialENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICASynthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductorsSíntese e caracterização de CH3NH3SnI3, CH3NH3SnI3 dopada com Mn e TiO2 deficiente em oxigênio como semicondutores ativos no visívelinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesis600600054faa10-e587-4736-bbba-5c3147983b48reponame:Repositório Institucional da UFSCARinstname:Universidade Federal de São Carlos (UFSCAR)instacron:UFSCARORIGINALMargaret Dawson-Tese.pdfMargaret Dawson-Tese.pdfteseapplication/pdf5799471https://repositorio.ufscar.br/bitstream/ufscar/15392/1/Margaret%20Dawson-Tese.pdf677a5897e852146f6cf96bd3c1131cd1MD51BCO carta comprovante autoarquivamento.pdfBCO carta comprovante autoarquivamento.pdfCarta comprovante orientadorapplication/pdf416928https://repositorio.ufscar.br/bitstream/ufscar/15392/2/BCO%20carta%20comprovante%20autoarquivamento.pdf383b82c60ee351ff6fb614c9ea4cdef4MD52CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8811https://repositorio.ufscar.br/bitstream/ufscar/15392/3/license_rdfe39d27027a6cc9cb039ad269a5db8e34MD53TEXTMargaret Dawson-Tese.pdf.txtMargaret Dawson-Tese.pdf.txtExtracted texttext/plain318050https://repositorio.ufscar.br/bitstream/ufscar/15392/4/Margaret%20Dawson-Tese.pdf.txt84bd78bc996e85dbc38c51cc4b36e08dMD54BCO carta comprovante autoarquivamento.pdf.txtBCO carta comprovante autoarquivamento.pdf.txtExtracted texttext/plain1492https://repositorio.ufscar.br/bitstream/ufscar/15392/6/BCO%20carta%20comprovante%20autoarquivamento.pdf.txt6e903c300c7ba3b4effc4b9fd6936865MD56THUMBNAILMargaret Dawson-Tese.pdf.jpgMargaret Dawson-Tese.pdf.jpgIM Thumbnailimage/jpeg6396https://repositorio.ufscar.br/bitstream/ufscar/15392/5/Margaret%20Dawson-Tese.pdf.jpg7fc882c5816c6a1a1b297edba7a26cd8MD55BCO carta comprovante autoarquivamento.pdf.jpgBCO carta comprovante autoarquivamento.pdf.jpgIM Thumbnailimage/jpeg11070https://repositorio.ufscar.br/bitstream/ufscar/15392/7/BCO%20carta%20comprovante%20autoarquivamento.pdf.jpg1b18cfb47fd8c39260e26b88d865a702MD57ufscar/153922023-09-18 18:32:18.966oai:repositorio.ufscar.br:ufscar/15392Repositório InstitucionalPUBhttps://repositorio.ufscar.br/oai/requestopendoar:43222023-09-18T18:32:18Repositório Institucional da UFSCAR - Universidade Federal de São Carlos (UFSCAR)false |
dc.title.eng.fl_str_mv |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors |
dc.title.alternative.por.fl_str_mv |
Síntese e caracterização de CH3NH3SnI3, CH3NH3SnI3 dopada com Mn e TiO2 deficiente em oxigênio como semicondutores ativos no visível |
title |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors |
spellingShingle |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors Dawson, Margaret Perovskita orgânica-inorgânica de estanho Perovskita de haleto de estanho Dopagem com Mn Precursor de estanho TiO2 deficiente de oxigênio Material para célula solar Organic-inorganic tin perovskite Tin halide perovskite Mn doping Tin precursor Oxygen deficient TiO2 Solar cell material ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA |
title_short |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors |
title_full |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors |
title_fullStr |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors |
title_full_unstemmed |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors |
title_sort |
Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors |
author |
Dawson, Margaret |
author_facet |
Dawson, Margaret |
author_role |
author |
dc.contributor.authorlattes.por.fl_str_mv |
http://lattes.cnpq.br/5710023413874940 |
dc.contributor.author.fl_str_mv |
Dawson, Margaret |
dc.contributor.advisor1.fl_str_mv |
Morelli, Márcio Raymundo |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/0172837599844991 |
dc.contributor.advisor-co1.fl_str_mv |
Oliveira, Cauê Ribeiro de |
dc.contributor.advisor-co1Lattes.fl_str_mv |
http://lattes.cnpq.br/5321313558714462 |
dc.contributor.authorID.fl_str_mv |
2d693bbd-6008-403f-a8a9-8919bb3cd95c |
contributor_str_mv |
Morelli, Márcio Raymundo Oliveira, Cauê Ribeiro de |
dc.subject.por.fl_str_mv |
Perovskita orgânica-inorgânica de estanho Perovskita de haleto de estanho Dopagem com Mn Precursor de estanho TiO2 deficiente de oxigênio Material para célula solar |
topic |
Perovskita orgânica-inorgânica de estanho Perovskita de haleto de estanho Dopagem com Mn Precursor de estanho TiO2 deficiente de oxigênio Material para célula solar Organic-inorganic tin perovskite Tin halide perovskite Mn doping Tin precursor Oxygen deficient TiO2 Solar cell material ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA |
dc.subject.eng.fl_str_mv |
Organic-inorganic tin perovskite Tin halide perovskite Mn doping Tin precursor Oxygen deficient TiO2 Solar cell material |
dc.subject.cnpq.fl_str_mv |
ENGENHARIAS::ENGENHARIA DE MATERIAIS E METALURGICA |
description |
CH3NH3SnI3 is an environmentally-friendly (lead-free) perovskite whose synthesis depends on SnI2. Some disadvantages of SnI2 include high cost and tin(IV) contamination. Thus, SnSO4 and C16H30O4Sn are presented as cheaper alternatives and different synthesis conditions were studied: 110 oC/10 min, 150 oC/10 min and 150 oC/20 min. Based on X-ray diffraction results, CH3NH3SnI3 was successfully synthesized, being 110 oC/10 min sufficient for phase formation. However, annealing at 150 oC improved crystallinity irrespective of precursor while prolonged annealing time (20 min) was detrimental to the C16H30O4Sn-based perovskite. Film morphology differed by type of precursor. The bandgaps (1.37-1.59 eV) and photoluminescence emissions (831 nm) of the samples characterize them as visible light active semiconductors. Because CH3NH3SnI3 suffers from Sn2+ oxidation to Sn4+, some studies have proposed doping with metal cations. So far, Mn has not been tested. Thus, Mn (2% and 10% mol) doped CH3NH3SnI3 samples were synthesized and characterized. Mn did not disrupt the perovskite structure but slightly increased bandgap. Chlorine from the Mn precursor is not eliminated by annealing, thus could affect material properties. Regarding stability, Mn partially stabilized CH3NH3SnI3, indicating the need for an optimum level of doping. Mn doping does not seem to improve the photovoltaic properties of CH3NH3SnI3, but it should be noted that the solar cells were not optimized. Several questions about CH3NH3SnI3 cells are still open, including alternative TiO2 compatible with the same. Here, oxygen-deficient TiO2 powders were studied. Electron paramagnetic spectroscopy and X-ray photoelectron spectroscopy confirmed oxygen vacancy. Photocatalytic and photocurrent tests showed activity under visible light and an optimum level of oxygen vacancies for lower recombination and high charge separation, important properties for photovoltaic applications. |
publishDate |
2020 |
dc.date.issued.fl_str_mv |
2020-02-14 |
dc.date.accessioned.fl_str_mv |
2021-12-21T14:11:27Z |
dc.date.available.fl_str_mv |
2021-12-21T14:11:27Z |
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.citation.fl_str_mv |
DAWSON, Margaret. Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors. 2020. Tese (Doutorado em Ciência e Engenharia de Materiais) – Universidade Federal de São Carlos, São Carlos, 2020. Disponível em: https://repositorio.ufscar.br/handle/ufscar/15392. |
dc.identifier.uri.fl_str_mv |
https://repositorio.ufscar.br/handle/ufscar/15392 |
identifier_str_mv |
DAWSON, Margaret. Synthesis and characterization of CH3NH3SnI3, Mn doped CH3NH3SnI3 and oxygen-deficient TiO2 as visible-light active semiconductors. 2020. Tese (Doutorado em Ciência e Engenharia de Materiais) – Universidade Federal de São Carlos, São Carlos, 2020. Disponível em: https://repositorio.ufscar.br/handle/ufscar/15392. |
url |
https://repositorio.ufscar.br/handle/ufscar/15392 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.confidence.fl_str_mv |
600 600 |
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054faa10-e587-4736-bbba-5c3147983b48 |
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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 |
dc.publisher.program.fl_str_mv |
Programa de Pós-Graduação em Ciência e Engenharia de Materiais - PPGCEM |
dc.publisher.initials.fl_str_mv |
UFSCar |
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Universidade Federal de São Carlos Câmpus São Carlos |
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