Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water

Detalhes bibliográficos
Ano de defesa: 2021
Autor(a) principal: Pinheiro, Bruna Bandeira
Orientador(a): Gonçalves, Luciana Rocha Barros
Banca de defesa: Não Informado pela instituição
Tipo de documento: Tese
Tipo de acesso: Acesso aberto
Idioma: por
Instituição de defesa: Não Informado pela instituição
Programa de Pós-Graduação: Não Informado pela instituição
Departamento: Não Informado pela instituição
País: Não Informado pela instituição
Palavras-chave em Português:
Link de acesso: http://www.repositorio.ufc.br/handle/riufc/59936
Resumo: Over the last years, design a green and environmentally biocatalyst to improve water quality emerges as one of the most relevant studies nowadays. Among the micropollutants present in water are acetaminophen and mefenamic acid, two drugs widely used to treat pain and fever around the world. They are related to asthma and increased toxicity of the central nervous system. Laccase-based biocatalysts have gained attention to degrade micro-pollutants. Laccase catalyzes the oxidation of phenolic substrates and has many applications which make this enzyme suitable and attractive for industrial applications. However, soluble laccases have diminished availability due to loss of stability, high cost of production, and non-reusability. In this way, laccase immobilization emerges as a way to make these potential applications a reality. In the first approach of this work, chemical amination of laccase following by ionic adsorption on cationic and anionic supports was performed in order to improve the laccase properties. The amination process introduces amino groups on the enzyme surface and may be controlled by the 1-ethyl-3-(3-dimethylamino propyl) carbodiimide (EDAC) concentration. Three quantities of EDAC were tested (0.024 g, 0.048 g e 0.168 g), evidencing that the stability of the laccase improves as more amino groups are introduced. In the second approach of this work, a study of laccase layer-by-layer immobilization onto chitosan activated with genipin or glutaraldehyde was performed. In this way, laccase multilayers were prepared following different combinations of genipin and glutaraldehyde to prepare the first and second laccase layers. This technique was chosen to enhance the loading capacity of the support; however, the addition of a second layer did not always produce a more active biocatalyst. Finally, the biocatalysts produced were used in the degradation of acetaminophen and mefenamic acid. The genipin-coated double-layer biocatalysts promoted greater removal of contaminants with 100% degradation of mefenamic acid and 66% of acetaminophen, under the conditions tested.
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spelling Pinheiro, Bruna BandeiraGonçalves, Luciana Rocha Barros2021-08-12T16:29:56Z2021-08-12T16:29:56Z2021PINHEIRO, Bruna Bandeira. Immobilized laccase biocatalysts as a way to improve degradation of micropollutants from water. 2021. 129 f. Tese (Doutorado em Engenharia Química) – Universidade Federal do Ceará, Centro de Tecnologia, Programa de Pós-Graduação em Engenharia Química, Fortaleza, 2021.http://www.repositorio.ufc.br/handle/riufc/59936Over the last years, design a green and environmentally biocatalyst to improve water quality emerges as one of the most relevant studies nowadays. Among the micropollutants present in water are acetaminophen and mefenamic acid, two drugs widely used to treat pain and fever around the world. They are related to asthma and increased toxicity of the central nervous system. Laccase-based biocatalysts have gained attention to degrade micro-pollutants. Laccase catalyzes the oxidation of phenolic substrates and has many applications which make this enzyme suitable and attractive for industrial applications. However, soluble laccases have diminished availability due to loss of stability, high cost of production, and non-reusability. In this way, laccase immobilization emerges as a way to make these potential applications a reality. In the first approach of this work, chemical amination of laccase following by ionic adsorption on cationic and anionic supports was performed in order to improve the laccase properties. The amination process introduces amino groups on the enzyme surface and may be controlled by the 1-ethyl-3-(3-dimethylamino propyl) carbodiimide (EDAC) concentration. Three quantities of EDAC were tested (0.024 g, 0.048 g e 0.168 g), evidencing that the stability of the laccase improves as more amino groups are introduced. In the second approach of this work, a study of laccase layer-by-layer immobilization onto chitosan activated with genipin or glutaraldehyde was performed. In this way, laccase multilayers were prepared following different combinations of genipin and glutaraldehyde to prepare the first and second laccase layers. This technique was chosen to enhance the loading capacity of the support; however, the addition of a second layer did not always produce a more active biocatalyst. Finally, the biocatalysts produced were used in the degradation of acetaminophen and mefenamic acid. The genipin-coated double-layer biocatalysts promoted greater removal of contaminants with 100% degradation of mefenamic acid and 66% of acetaminophen, under the conditions tested.Nos últimos anos, desenvolver um biocatalisador ecológico para melhorar a qualidade da água surge como um dos estudos mais relevantes. Dentre os micropoluentes presentes na água estão o acetaminofeno e ácido mefenâmico, duas drogas muito utilizadas para tratar dores e febre pelo mundo que estão relacionadas com asma e aumento da toxicidade do sistema nervoso central. Biocatalisadores produzidos com lacase têm ganhado atenção para degradar esses poluentes. A lacase catalisa a oxidação de substratos fenólicos e possuem muitas aplicações, o que torna esta enzima adequada e atrativa para aplicações industriais. No entanto, as lacases solúveis têm sua disponibilidade diminuída devido à perda de estabilidade, alto custo de produção e não reutilização. Desta forma, a imobilização surge como uma forma de tornar essas potenciais aplicações uma realidade. Na primeira abordagem deste trabalho, a aminação química da lacase seguida de adsorção iônica em suportes catiônicos e aniônicos foi realizada a fim de melhorar as propriedades da enzima. O processo de aminação introduz grupos amino na superfície da proteína e podem ser controlados através do uso de diferentes concentrações de 1-etil-3-(3-dimetilaminopropil) carbodiimida (EDAC). Três quantidades de EDAC foram testadas(0.024 g, 0.048 g e 0.168 g), evidenciando que a estabilidade da lacase melhora à medida que mais grupos amino são introduzidos. Na segunda abordagem deste trabalho, foi realizado um estudo da imobilização layer-by-layer da lacase em quitosana ativada com genipina ou glutaraldeído. Desta forma, as multicamadas de lacase foram preparadas seguindo diferentes combinações de genipina e glutaraldeído para preparar a primeira e a segunda camadas de lacase. Essa técnica foi escolhida para aumentar a capacidade de carregamento do suporte, porém a adição de uma segunda camada nem sempre produziu biocatalisadores mais ativos. Finalmente, os biocatalisadores produzidos foram usados na degradação do acetaminofeno e do ácido mefenâmico. Os biocatalisadores de dupla camada revestido com genipina promoveram maior remoção dos contaminantes com 100% de degradação do ácido mefenâmico e de 66% do acetaminofeno, nas condições testadas.ImmobilizaçãoLacaseAminaçãoLayer-by-layerAdsorçãoImmobilized Laccase biocatalysts as a way to improve degradation of micropollutants from waterinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisporreponame:Repositório Institucional da Universidade Federal do Ceará (UFC)instname:Universidade Federal do Ceará (UFC)instacron:UFCinfo:eu-repo/semantics/openAccessLICENSElicense.txtlicense.txttext/plain; charset=utf-81748http://repositorio.ufc.br/bitstream/riufc/59936/2/license.txt8a4605be74aa9ea9d79846c1fba20a33MD52ORIGINAL2021_tese_bbpinheiro.pdf2021_tese_bbpinheiro.pdfapplication/pdf5492580http://repositorio.ufc.br/bitstream/riufc/59936/1/2021_tese_bbpinheiro.pdf716294a2f3de4d0b2b60fbe61f338e56MD51riufc/599362021-08-12 13:29:56.812oai:repositorio.ufc.br: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Repositório InstitucionalPUBhttp://www.repositorio.ufc.br/ri-oai/requestbu@ufc.br || repositorio@ufc.bropendoar:2021-08-12T16:29:56Repositório Institucional da Universidade Federal do Ceará (UFC) - Universidade Federal do Ceará (UFC)false
dc.title.pt_BR.fl_str_mv Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
title Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
spellingShingle Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
Pinheiro, Bruna Bandeira
Immobilização
Lacase
Aminação
Layer-by-layer
Adsorção
title_short Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
title_full Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
title_fullStr Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
title_full_unstemmed Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
title_sort Immobilized Laccase biocatalysts as a way to improve degradation of micropollutants from water
author Pinheiro, Bruna Bandeira
author_facet Pinheiro, Bruna Bandeira
author_role author
dc.contributor.author.fl_str_mv Pinheiro, Bruna Bandeira
dc.contributor.advisor1.fl_str_mv Gonçalves, Luciana Rocha Barros
contributor_str_mv Gonçalves, Luciana Rocha Barros
dc.subject.por.fl_str_mv Immobilização
Lacase
Aminação
Layer-by-layer
Adsorção
topic Immobilização
Lacase
Aminação
Layer-by-layer
Adsorção
description Over the last years, design a green and environmentally biocatalyst to improve water quality emerges as one of the most relevant studies nowadays. Among the micropollutants present in water are acetaminophen and mefenamic acid, two drugs widely used to treat pain and fever around the world. They are related to asthma and increased toxicity of the central nervous system. Laccase-based biocatalysts have gained attention to degrade micro-pollutants. Laccase catalyzes the oxidation of phenolic substrates and has many applications which make this enzyme suitable and attractive for industrial applications. However, soluble laccases have diminished availability due to loss of stability, high cost of production, and non-reusability. In this way, laccase immobilization emerges as a way to make these potential applications a reality. In the first approach of this work, chemical amination of laccase following by ionic adsorption on cationic and anionic supports was performed in order to improve the laccase properties. The amination process introduces amino groups on the enzyme surface and may be controlled by the 1-ethyl-3-(3-dimethylamino propyl) carbodiimide (EDAC) concentration. Three quantities of EDAC were tested (0.024 g, 0.048 g e 0.168 g), evidencing that the stability of the laccase improves as more amino groups are introduced. In the second approach of this work, a study of laccase layer-by-layer immobilization onto chitosan activated with genipin or glutaraldehyde was performed. In this way, laccase multilayers were prepared following different combinations of genipin and glutaraldehyde to prepare the first and second laccase layers. This technique was chosen to enhance the loading capacity of the support; however, the addition of a second layer did not always produce a more active biocatalyst. Finally, the biocatalysts produced were used in the degradation of acetaminophen and mefenamic acid. The genipin-coated double-layer biocatalysts promoted greater removal of contaminants with 100% degradation of mefenamic acid and 66% of acetaminophen, under the conditions tested.
publishDate 2021
dc.date.accessioned.fl_str_mv 2021-08-12T16:29:56Z
dc.date.available.fl_str_mv 2021-08-12T16:29:56Z
dc.date.issued.fl_str_mv 2021
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/doctoralThesis
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status_str publishedVersion
dc.identifier.citation.fl_str_mv PINHEIRO, Bruna Bandeira. Immobilized laccase biocatalysts as a way to improve degradation of micropollutants from water. 2021. 129 f. Tese (Doutorado em Engenharia Química) – Universidade Federal do Ceará, Centro de Tecnologia, Programa de Pós-Graduação em Engenharia Química, Fortaleza, 2021.
dc.identifier.uri.fl_str_mv http://www.repositorio.ufc.br/handle/riufc/59936
identifier_str_mv PINHEIRO, Bruna Bandeira. Immobilized laccase biocatalysts as a way to improve degradation of micropollutants from water. 2021. 129 f. Tese (Doutorado em Engenharia Química) – Universidade Federal do Ceará, Centro de Tecnologia, Programa de Pós-Graduação em Engenharia Química, Fortaleza, 2021.
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