Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants
Autor(a) principal: | |
---|---|
Data de Publicação: | 2021 |
Tipo de documento: | Dissertação |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UFMG |
Texto Completo: | http://hdl.handle.net/1843/38408 https://orcid.org/0000-0002-8264-1818 |
Resumo: | The contamination of ecosystems with toxic materials is a recurring problem in human history. Pollutants such as heavy metals, organic materials, industrial dyes, radioactive waste, and solvents are commonly found in various environments, causing harmful effects to humans and other species. The pharmaceuticals and personal care products (PPCPs) pose a specific concern due to its extensive use and incorrect disposal around the world, specifically the non-steroidal anti-inflammatory drugs (NSAIDs), with ibuprofen (IBP) and diclofenac (DIC) being on the top list. The use of materials with controlled pore structures is an effective strategy for both capturing and degrading these pollutants. Through adsorption and photocatalysis, these compounds can remove several toxic species present in soil, water, and atmosphere. This work evaluates the adsorption and degradation capacity of methylene blue (MB), IBP, and DIC using the metal-organic frameworks (MOFs) HKUST-1 and MIL-100(Al). The MOFs were synthesized through a hydrothermal treatment and later impregnated with titania, which is a well-established semiconductor worldwide due to its low cost and low toxicity coupled with a high photoactivity and chemical stability. TiO2 was produced by a sol-gel route without the presence of an acid, using the MOFs as a site for heterogeneous nucleation. In order to evaluate the influence of TiO2 nanoparticles in the MOFs over their photocatalytic activity, UV-vis kinetic studies were conducted, and the apparent first-order constant (Kapp) were calculated using the Langmuir-Hinshelwood (L-H) kinetic model. It was observed that aluminum trimesate withstood the modification step, and anatase nanoparticles were successfully anchored onto its surface and within its pore framework. This composite showed an improved capacity of degrading MB, IBP, and DIC under UVA illumination. Copper trimesate, on the other hand, showed a structural collapse during the modification step, probably due its fragility in water-rich media. However, the novel composite material experienced an increase in its photocatalytic activity compared to HKUST-1, due to the presence of crystallized TiO2 in the form of rutile on its surface. This work contributes to the knowledge about the incorporation of semiconductor nanoparticles into MOFs for photocatalytic applications |
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Eduardo Henrique Martins Nuneshttp://lattes.cnpq.br/6595175997456989Manuel HoumardCristophe VolkringerAlain Moissettehttp://lattes.cnpq.br/9189339050614301Pedro Henrique Morais Andrade2021-10-18T13:04:47Z2021-10-18T13:04:47Z2021-07-07http://hdl.handle.net/1843/38408https://orcid.org/0000-0002-8264-1818The contamination of ecosystems with toxic materials is a recurring problem in human history. Pollutants such as heavy metals, organic materials, industrial dyes, radioactive waste, and solvents are commonly found in various environments, causing harmful effects to humans and other species. The pharmaceuticals and personal care products (PPCPs) pose a specific concern due to its extensive use and incorrect disposal around the world, specifically the non-steroidal anti-inflammatory drugs (NSAIDs), with ibuprofen (IBP) and diclofenac (DIC) being on the top list. The use of materials with controlled pore structures is an effective strategy for both capturing and degrading these pollutants. Through adsorption and photocatalysis, these compounds can remove several toxic species present in soil, water, and atmosphere. This work evaluates the adsorption and degradation capacity of methylene blue (MB), IBP, and DIC using the metal-organic frameworks (MOFs) HKUST-1 and MIL-100(Al). The MOFs were synthesized through a hydrothermal treatment and later impregnated with titania, which is a well-established semiconductor worldwide due to its low cost and low toxicity coupled with a high photoactivity and chemical stability. TiO2 was produced by a sol-gel route without the presence of an acid, using the MOFs as a site for heterogeneous nucleation. In order to evaluate the influence of TiO2 nanoparticles in the MOFs over their photocatalytic activity, UV-vis kinetic studies were conducted, and the apparent first-order constant (Kapp) were calculated using the Langmuir-Hinshelwood (L-H) kinetic model. It was observed that aluminum trimesate withstood the modification step, and anatase nanoparticles were successfully anchored onto its surface and within its pore framework. This composite showed an improved capacity of degrading MB, IBP, and DIC under UVA illumination. Copper trimesate, on the other hand, showed a structural collapse during the modification step, probably due its fragility in water-rich media. However, the novel composite material experienced an increase in its photocatalytic activity compared to HKUST-1, due to the presence of crystallized TiO2 in the form of rutile on its surface. This work contributes to the knowledge about the incorporation of semiconductor nanoparticles into MOFs for photocatalytic applicationsA contaminação de ecossistemas com materiais tóxicos é um problema recorrente na história. Poluentes como metais pesados, materiais orgânicos, corantes industriais, lixo radioativo e solventes são comumente encontrados em vários ambientes, causando efeitos nocivos aos humanos e outras espécies. Os produtos farmacêuticos e de higiene pessoal (PPCPs) levantam preocupações relacionadas ao seu uso extensivo e ao descarte incorreto em todo o planeta, especificamente os anti-inflamatórios e drogas não esteroidais (NSAIDs), valendo citar o ibuprofeno (IBP) e o diclofenaco (DIC) como um dos principais. O uso de materiais com estrutura de poros controlada é uma alternativa eficiente para capturar e degradar esses poluentes. Através da adsorção e fotocatálise, esses compostos conseguem remover diversas espécies tóxicas presentes no solo, na água e na atmosfera. Esse trabalho avalia a capacidade de adsorção e degradação do azul de metileno (MB), IBP e DIC, usando as redes organometálicas (MOFs) HKUST-1 e MIL-100 (Al). As MOFs foram sintetizadas por meio de um tratamento hidrotérmico e posteriormente impregnadas com titânia, que é um semicondutor bem estabelecido mundialmente, devido ao seu baixo custo e à sua baixa toxicidade aliado a uma alta fotoatividade e estabilidade química. O TiO2 foi produzido pela rota sol-gel sem a presença de ácido, utilizando as MOFs como matrizes de nucleação heterogênea. A fim de avaliar a influência das nanopartículas de TiO2 nos MOFs sobre sua atividade fotocatalítica, estudos cinéticos UV-vis foram conduzidos e as constantes aparentes de primeira ordem (Kapp) foram calculadas usando o modelo cinético de Langmuir-Hinshelwood (L-H). Foi observado que o trimesato de alumínio resistiu à etapa de modificação e as nanopartículas de anatasio foram ancoradas com sucesso em sua superfície e dentro de sua estrutura de poros. Esse composto mostrou uma capacidade melhorada de degradar MB, IBP e DIC sob iluminação UVA. O trimesato de cobre, por outro lado, apresentou um colapso estrutural durante a etapa de modificação, provavelmente devido à sua fragilidade em meio rico em água. No entanto, o novo compósito experimentou um aumento em sua atividade fotocatalítica em relação ao HKUST-1, devido à presença de TiO2 cristalizado na forma de rutilo em sua superfície. Esse trabalho contribui para o conhecimento sobre a incorporação de nanopartículas semicondutoras em MOFs para aplicações fotocatalíticas.CNPq - Conselho Nacional de Desenvolvimento Científico e TecnológicoFAPEMIG - Fundação de Amparo à Pesquisa do Estado de Minas GeraisCAPES - Coordenação de Aperfeiçoamento de Pessoal de Nível SuperiorengUniversidade Federal de Minas GeraisPrograma de Pós-Graduação em Engenharia Metalúrgica, Materiais e de MinasUFMGBrasilENG - DEPARTAMENTO DE ENGENHARIA METALÚRGICAhttp://creativecommons.org/licenses/by/3.0/pt/info:eu-repo/semantics/openAccessMateriaisCiência dos materiaisDiclofenacoDióxido de titânioFotocatáliseMOFHKUST-1MIL-100(Al)TiO2PhotocatalysisNSAIDsIbuprofenDiclofenacSynthesis of TiO2@MOF composites for the photodegradation of organic pollutantsSíntese de compósitos do tipo TiO2@MOF com aplicação na fotodegradação de poluentes orgânicosinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisreponame:Repositório Institucional da UFMGinstname:Universidade Federal de Minas Gerais (UFMG)instacron:UFMGORIGINALMasters dissertation - Pedro H. M. Andrade.pdfMasters dissertation - Pedro H. M. Andrade.pdfDissertação de mestradoapplication/pdf3322448https://repositorio.ufmg.br/bitstream/1843/38408/1/Masters%20dissertation%20-%20Pedro%20H.%20M.%20Andrade.pdff644824fa9e7655995b1dc276d98052bMD51CC-LICENSElicense_rdflicense_rdfapplication/rdf+xml; charset=utf-8914https://repositorio.ufmg.br/bitstream/1843/38408/2/license_rdff9944a358a0c32770bd9bed185bb5395MD52LICENSElicense.txtlicense.txttext/plain; charset=utf-82118https://repositorio.ufmg.br/bitstream/1843/38408/3/license.txtcda590c95a0b51b4d15f60c9642ca272MD531843/384082021-10-18 10:04:47.47oai:repositorio.ufmg.br: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ório de PublicaçõesPUBhttps://repositorio.ufmg.br/oaiopendoar:2021-10-18T13:04:47Repositório Institucional da UFMG - Universidade Federal de Minas Gerais (UFMG)false |
dc.title.pt_BR.fl_str_mv |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants |
dc.title.alternative.pt_BR.fl_str_mv |
Síntese de compósitos do tipo TiO2@MOF com aplicação na fotodegradação de poluentes orgânicos |
title |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants |
spellingShingle |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants Pedro Henrique Morais Andrade MOF HKUST-1 MIL-100(Al) TiO2 Photocatalysis NSAIDs Ibuprofen Diclofenac Materiais Ciência dos materiais Diclofenaco Dióxido de titânio Fotocatálise |
title_short |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants |
title_full |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants |
title_fullStr |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants |
title_full_unstemmed |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants |
title_sort |
Synthesis of TiO2@MOF composites for the photodegradation of organic pollutants |
author |
Pedro Henrique Morais Andrade |
author_facet |
Pedro Henrique Morais Andrade |
author_role |
author |
dc.contributor.advisor1.fl_str_mv |
Eduardo Henrique Martins Nunes |
dc.contributor.advisor1Lattes.fl_str_mv |
http://lattes.cnpq.br/6595175997456989 |
dc.contributor.advisor-co1.fl_str_mv |
Manuel Houmard |
dc.contributor.referee1.fl_str_mv |
Cristophe Volkringer |
dc.contributor.referee2.fl_str_mv |
Alain Moissette |
dc.contributor.authorLattes.fl_str_mv |
http://lattes.cnpq.br/9189339050614301 |
dc.contributor.author.fl_str_mv |
Pedro Henrique Morais Andrade |
contributor_str_mv |
Eduardo Henrique Martins Nunes Manuel Houmard Cristophe Volkringer Alain Moissette |
dc.subject.por.fl_str_mv |
MOF HKUST-1 MIL-100(Al) TiO2 Photocatalysis NSAIDs Ibuprofen Diclofenac |
topic |
MOF HKUST-1 MIL-100(Al) TiO2 Photocatalysis NSAIDs Ibuprofen Diclofenac Materiais Ciência dos materiais Diclofenaco Dióxido de titânio Fotocatálise |
dc.subject.other.pt_BR.fl_str_mv |
Materiais Ciência dos materiais Diclofenaco Dióxido de titânio Fotocatálise |
description |
The contamination of ecosystems with toxic materials is a recurring problem in human history. Pollutants such as heavy metals, organic materials, industrial dyes, radioactive waste, and solvents are commonly found in various environments, causing harmful effects to humans and other species. The pharmaceuticals and personal care products (PPCPs) pose a specific concern due to its extensive use and incorrect disposal around the world, specifically the non-steroidal anti-inflammatory drugs (NSAIDs), with ibuprofen (IBP) and diclofenac (DIC) being on the top list. The use of materials with controlled pore structures is an effective strategy for both capturing and degrading these pollutants. Through adsorption and photocatalysis, these compounds can remove several toxic species present in soil, water, and atmosphere. This work evaluates the adsorption and degradation capacity of methylene blue (MB), IBP, and DIC using the metal-organic frameworks (MOFs) HKUST-1 and MIL-100(Al). The MOFs were synthesized through a hydrothermal treatment and later impregnated with titania, which is a well-established semiconductor worldwide due to its low cost and low toxicity coupled with a high photoactivity and chemical stability. TiO2 was produced by a sol-gel route without the presence of an acid, using the MOFs as a site for heterogeneous nucleation. In order to evaluate the influence of TiO2 nanoparticles in the MOFs over their photocatalytic activity, UV-vis kinetic studies were conducted, and the apparent first-order constant (Kapp) were calculated using the Langmuir-Hinshelwood (L-H) kinetic model. It was observed that aluminum trimesate withstood the modification step, and anatase nanoparticles were successfully anchored onto its surface and within its pore framework. This composite showed an improved capacity of degrading MB, IBP, and DIC under UVA illumination. Copper trimesate, on the other hand, showed a structural collapse during the modification step, probably due its fragility in water-rich media. However, the novel composite material experienced an increase in its photocatalytic activity compared to HKUST-1, due to the presence of crystallized TiO2 in the form of rutile on its surface. This work contributes to the knowledge about the incorporation of semiconductor nanoparticles into MOFs for photocatalytic applications |
publishDate |
2021 |
dc.date.accessioned.fl_str_mv |
2021-10-18T13:04:47Z |
dc.date.available.fl_str_mv |
2021-10-18T13:04:47Z |
dc.date.issued.fl_str_mv |
2021-07-07 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/masterThesis |
format |
masterThesis |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/1843/38408 |
dc.identifier.orcid.pt_BR.fl_str_mv |
https://orcid.org/0000-0002-8264-1818 |
url |
http://hdl.handle.net/1843/38408 https://orcid.org/0000-0002-8264-1818 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.rights.driver.fl_str_mv |
http://creativecommons.org/licenses/by/3.0/pt/ info:eu-repo/semantics/openAccess |
rights_invalid_str_mv |
http://creativecommons.org/licenses/by/3.0/pt/ |
eu_rights_str_mv |
openAccess |
dc.publisher.none.fl_str_mv |
Universidade Federal de Minas Gerais |
dc.publisher.program.fl_str_mv |
Programa de Pós-Graduação em Engenharia Metalúrgica, Materiais e de Minas |
dc.publisher.initials.fl_str_mv |
UFMG |
dc.publisher.country.fl_str_mv |
Brasil |
dc.publisher.department.fl_str_mv |
ENG - DEPARTAMENTO DE ENGENHARIA METALÚRGICA |
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Universidade Federal de Minas Gerais |
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