Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar

Detalhes bibliográficos
Autor(a) principal: Minetto, Luciane
Data de Publicação: 2013
Tipo de documento: Tese
Idioma: por
Título da fonte: Manancial - Repositório Digital da UFSM
dARK ID: ark:/26339/001300000q952
Texto Completo: http://repositorio.ufsm.br/handle/1/4262
Resumo: Macrolide antibiotics are an important group of prescription drugs; as a consequence of the large and continuous use, they are commonly found in the environment. In the present study, it was developed and optimized a chromatographic method to assess the occurrence of macrolide antibiotics Azithromycin, Clarithromycin, Erythromycin and Roxithromycin in the effluent of the University Hospital of Santa Maria, in two sampling points, by applying high performance liquid chromatography coupled to mass detection with quadrupole ion trap (HPLC-MS/MS_QTrap) and clean-up/pre-concentration by solid phase extraction with the aid of Surface Methodology Response. The concentrations measured during a week in the hospital effluent were 1.32±0.13 and 0.22±0.06 μg L-1 for Azithromycin and Clarithromycin; in the receptor water sream was 1.12±0.20, 0.20±0.05 and 0.01±0.004 μg L-1 for Azithromycin, Clarithromycin and Erythromycin. Roxithromycin was not detected in all effluent samples. After this, it was done the evaluation of the risk quotient of the macrolide antibiotics. The value of the risk quotient for the hospital effluent for Azithromycin and Clarithromycin was 11 (high risk), and for the receptor water stream the risk quotient was 9.3 and 10.0 for Azithromycin and Clarithromycin; for Erythromycin, a quocient risk value of 0.5 (medium risk). For degradation of the antibiotics in aqueous solution, it was used UV-photolysis, by which the influence of pH (3-11) was evaluated. Azithromycin showed low degradation by acid pH; for other pH, as well, for all the other antibiotics, the degradation was above 70% after 60 min of treatment. It was conducted a kinetic study of the degradation process of macrolide antibiotics in different pHs, by which Azithromycin revealed a recalcitrant profile, and Roxithromycin, as the more easily degradable one. For identification of the products formed during the photolysis experiments it was used independent information acquisition and as precursor ions of fragments m/z 116 and 158, characteristic of the macrolide compounds, at three collision energies (30, 45, and 60 V). It was proposed fragmentation routes of the degradation products: 8 products for Azithromycin, 7 for Clarithromycin, 6 of Erythromycin and 8 Roxithromycin. Through the same experiments with independent information acquisition, it was investigated the presence of eventual metabolites in hospital effluent, and three metabolites were found. By applying photolysis to the hospital effluent fortified, at pH 7, it was observed that the degradation occurs above 80% for all compounds after 60 min of irradiation. It was observed the formation of degradation products previously determined by experiments in aqueous solution. It was also found three degradation products for Azithromycin, 2 for Clarithromycin, 1 for Erythromycin and 3 for Roxithromycin.
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spelling Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalarMacrolides antibiotics: determination and identification of metabolites and degradation subproducts in hospital effluentAntibióticos macrolídeosEfluente hospitalarFotodegradaçãoProdutos de degradaçãoMetabólitosMacrolide antibioticsEffluent hospitalPhotodegradationDegradation productsMetabolitesCNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICAMacrolide antibiotics are an important group of prescription drugs; as a consequence of the large and continuous use, they are commonly found in the environment. In the present study, it was developed and optimized a chromatographic method to assess the occurrence of macrolide antibiotics Azithromycin, Clarithromycin, Erythromycin and Roxithromycin in the effluent of the University Hospital of Santa Maria, in two sampling points, by applying high performance liquid chromatography coupled to mass detection with quadrupole ion trap (HPLC-MS/MS_QTrap) and clean-up/pre-concentration by solid phase extraction with the aid of Surface Methodology Response. The concentrations measured during a week in the hospital effluent were 1.32±0.13 and 0.22±0.06 μg L-1 for Azithromycin and Clarithromycin; in the receptor water sream was 1.12±0.20, 0.20±0.05 and 0.01±0.004 μg L-1 for Azithromycin, Clarithromycin and Erythromycin. Roxithromycin was not detected in all effluent samples. After this, it was done the evaluation of the risk quotient of the macrolide antibiotics. The value of the risk quotient for the hospital effluent for Azithromycin and Clarithromycin was 11 (high risk), and for the receptor water stream the risk quotient was 9.3 and 10.0 for Azithromycin and Clarithromycin; for Erythromycin, a quocient risk value of 0.5 (medium risk). For degradation of the antibiotics in aqueous solution, it was used UV-photolysis, by which the influence of pH (3-11) was evaluated. Azithromycin showed low degradation by acid pH; for other pH, as well, for all the other antibiotics, the degradation was above 70% after 60 min of treatment. It was conducted a kinetic study of the degradation process of macrolide antibiotics in different pHs, by which Azithromycin revealed a recalcitrant profile, and Roxithromycin, as the more easily degradable one. For identification of the products formed during the photolysis experiments it was used independent information acquisition and as precursor ions of fragments m/z 116 and 158, characteristic of the macrolide compounds, at three collision energies (30, 45, and 60 V). It was proposed fragmentation routes of the degradation products: 8 products for Azithromycin, 7 for Clarithromycin, 6 of Erythromycin and 8 Roxithromycin. Through the same experiments with independent information acquisition, it was investigated the presence of eventual metabolites in hospital effluent, and three metabolites were found. By applying photolysis to the hospital effluent fortified, at pH 7, it was observed that the degradation occurs above 80% for all compounds after 60 min of irradiation. It was observed the formation of degradation products previously determined by experiments in aqueous solution. It was also found three degradation products for Azithromycin, 2 for Clarithromycin, 1 for Erythromycin and 3 for Roxithromycin.Conselho Nacional de Desenvolvimento Científico e TecnológicoOs antibióticos macrolídeos são uma importante classe de fármacos preescritos no tratamento das mais variadas infecções, e como consequência se seu grande e continuo uso são comumente encontradas no ambiente. No presente estudo foi desenvolvido e otimizado método de cromatografia líquida de alta eficiência acoplada à detector de massas quadrupolo íon trap (HPLC-MS/MS_QTrap) e de clean-up/pré-concentração por extração em fase sólida com auxílio de Metodologia de Superfície de Resposta para avaliar a ocorrência dos antibióticos macrolídeos Azitromicina, Claritromicina, Eritromicina e Roxitromicina no efluente hospitalar do Hospital Universitário de Santa Maria em dois ponto de amostragem. As concentrações médias durante o ciclo de uma semana de amostragem no efluente do pronto atendimento foram de 1,32±0,13 e 0,22±0,06 g L-1 para Azitromicina e Claritromicina; no corpo recpetor foram de 1,12±0,20; 0,20±0,05 e 0,01±0,004 g L-1 para Azitromicina, Claritromicina e Eritromicina, respectivamente. Roxitromicina não foi detectada. Após foi feita a avaliação do quociente de risco dos antibióticos macrolídeos. O quociente de risco no efluente do pronto atendimento para Azitromicina e Claritromicina foi de 11, risco alto, o qual também foi evidenciado no corpo receptor com quociente de risco de 9,3 e 10 para Azitromicina e Claritromicna, e risco médio para Eritromicina de 0,5. Para degradação dos antibióticos foi utilizado fotólise artificial em solução aquosa, sendo avaliado a influência do pH de 3-11 na degradação destes compostos. Azitromicina apresentou baixa degradação em pH ácido, para os outros pH e demais compostos a degradação foi acima de 70% após 60 min de tratamento. Foi feito um estudo cinético do processo de degradação dos antibióticos macrolídeos em diferentes pH, observando-se que a Azitromicina apresentou um perfil recalcitrante para o processo, e Roxitromicina foi degradada com maior facilidade. Para a identificação dos produtos formados durante os experimentos de fotodegradação foram montados experimentos de informação independente de aquisição utilizando como íons precursores os íons de m/z 116 e 158 característicos dos compostos macrolídeos em três energias de colisão (30, 45 e 60 V). Foram identificadas e propostas rotas de fragmentação para 8 produtos de degradação de Azitromicina, 7 para Claritromicina, 6 para Eritromicina e 8 produtos de degradação de Roxiromicina. Através dos mesmos experimentos de informação independente de aquisição, foi investigada a presença de possíveis metabólitos no efluente hospitalar sendo encontrados 3 metabólitos. Com a aplicação de fotólise ao efluente hospitalar fortificado, em pH 7, observou-se que ocorre degradação acima de 80% para todos os compostos após 60 min de tratamneto. Foi observada a formação de produtos de degradação, que tinham sido previamente determinados em solução aquosa. Foram encontrados 3 produtos de degradação de Azitromicina, 2 para Claritromicina, 1 para Eritromicina e 3 produtos para Roxitromicina.Universidade Federal de Santa MariaBRQuímicaUFSMPrograma de Pós-Graduação em QuímicaMartins, Ayrton Figueiredohttp://lattes.cnpq.br/2113532494494821Arsand, Daniel Ricardohttp://lattes.cnpq.br/2243464346389170Primel, Ednei Gilbertohttp://lattes.cnpq.br/3259602390948297Vasconcelos, Tibiriçá Gonçalveshttp://lattes.cnpq.br/6407925163803842Martins, Manoel Leonardohttp://lattes.cnpq.br/4404290090180984Minetto, Luciane2017-05-182017-05-182013-08-09info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/doctoralThesisapplication/pdfapplication/pdfMINETTO, Luciane. Macrolides antibiotics: determination and identification of metabolites and degradation subproducts in hospital effluent. 2013. 146 f. Tese (Doutorado em Química) - Universidade Federal de Santa Maria, Santa Maria, 2013.http://repositorio.ufsm.br/handle/1/4262ark:/26339/001300000q952porinfo:eu-repo/semantics/openAccessreponame:Manancial - Repositório Digital da UFSMinstname:Universidade Federal de Santa Maria (UFSM)instacron:UFSM2022-06-03T12:54:28Zoai:repositorio.ufsm.br:1/4262Biblioteca Digital de Teses e Dissertaçõeshttps://repositorio.ufsm.br/ONGhttps://repositorio.ufsm.br/oai/requestatendimento.sib@ufsm.br||tedebc@gmail.comopendoar:2022-06-03T12:54:28Manancial - Repositório Digital da UFSM - Universidade Federal de Santa Maria (UFSM)false
dc.title.none.fl_str_mv Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
Macrolides antibiotics: determination and identification of metabolites and degradation subproducts in hospital effluent
title Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
spellingShingle Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
Minetto, Luciane
Antibióticos macrolídeos
Efluente hospitalar
Fotodegradação
Produtos de degradação
Metabólitos
Macrolide antibiotics
Effluent hospital
Photodegradation
Degradation products
Metabolites
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
title_short Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
title_full Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
title_fullStr Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
title_full_unstemmed Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
title_sort Antibióticos macrolídeos: determinação e identificação de metabólitos e subprodutos de degradação em efluente hospitalar
author Minetto, Luciane
author_facet Minetto, Luciane
author_role author
dc.contributor.none.fl_str_mv Martins, Ayrton Figueiredo
http://lattes.cnpq.br/2113532494494821
Arsand, Daniel Ricardo
http://lattes.cnpq.br/2243464346389170
Primel, Ednei Gilberto
http://lattes.cnpq.br/3259602390948297
Vasconcelos, Tibiriçá Gonçalves
http://lattes.cnpq.br/6407925163803842
Martins, Manoel Leonardo
http://lattes.cnpq.br/4404290090180984
dc.contributor.author.fl_str_mv Minetto, Luciane
dc.subject.por.fl_str_mv Antibióticos macrolídeos
Efluente hospitalar
Fotodegradação
Produtos de degradação
Metabólitos
Macrolide antibiotics
Effluent hospital
Photodegradation
Degradation products
Metabolites
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
topic Antibióticos macrolídeos
Efluente hospitalar
Fotodegradação
Produtos de degradação
Metabólitos
Macrolide antibiotics
Effluent hospital
Photodegradation
Degradation products
Metabolites
CNPQ::CIENCIAS EXATAS E DA TERRA::QUIMICA
description Macrolide antibiotics are an important group of prescription drugs; as a consequence of the large and continuous use, they are commonly found in the environment. In the present study, it was developed and optimized a chromatographic method to assess the occurrence of macrolide antibiotics Azithromycin, Clarithromycin, Erythromycin and Roxithromycin in the effluent of the University Hospital of Santa Maria, in two sampling points, by applying high performance liquid chromatography coupled to mass detection with quadrupole ion trap (HPLC-MS/MS_QTrap) and clean-up/pre-concentration by solid phase extraction with the aid of Surface Methodology Response. The concentrations measured during a week in the hospital effluent were 1.32±0.13 and 0.22±0.06 μg L-1 for Azithromycin and Clarithromycin; in the receptor water sream was 1.12±0.20, 0.20±0.05 and 0.01±0.004 μg L-1 for Azithromycin, Clarithromycin and Erythromycin. Roxithromycin was not detected in all effluent samples. After this, it was done the evaluation of the risk quotient of the macrolide antibiotics. The value of the risk quotient for the hospital effluent for Azithromycin and Clarithromycin was 11 (high risk), and for the receptor water stream the risk quotient was 9.3 and 10.0 for Azithromycin and Clarithromycin; for Erythromycin, a quocient risk value of 0.5 (medium risk). For degradation of the antibiotics in aqueous solution, it was used UV-photolysis, by which the influence of pH (3-11) was evaluated. Azithromycin showed low degradation by acid pH; for other pH, as well, for all the other antibiotics, the degradation was above 70% after 60 min of treatment. It was conducted a kinetic study of the degradation process of macrolide antibiotics in different pHs, by which Azithromycin revealed a recalcitrant profile, and Roxithromycin, as the more easily degradable one. For identification of the products formed during the photolysis experiments it was used independent information acquisition and as precursor ions of fragments m/z 116 and 158, characteristic of the macrolide compounds, at three collision energies (30, 45, and 60 V). It was proposed fragmentation routes of the degradation products: 8 products for Azithromycin, 7 for Clarithromycin, 6 of Erythromycin and 8 Roxithromycin. Through the same experiments with independent information acquisition, it was investigated the presence of eventual metabolites in hospital effluent, and three metabolites were found. By applying photolysis to the hospital effluent fortified, at pH 7, it was observed that the degradation occurs above 80% for all compounds after 60 min of irradiation. It was observed the formation of degradation products previously determined by experiments in aqueous solution. It was also found three degradation products for Azithromycin, 2 for Clarithromycin, 1 for Erythromycin and 3 for Roxithromycin.
publishDate 2013
dc.date.none.fl_str_mv 2013-08-09
2017-05-18
2017-05-18
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.uri.fl_str_mv MINETTO, Luciane. Macrolides antibiotics: determination and identification of metabolites and degradation subproducts in hospital effluent. 2013. 146 f. Tese (Doutorado em Química) - Universidade Federal de Santa Maria, Santa Maria, 2013.
http://repositorio.ufsm.br/handle/1/4262
dc.identifier.dark.fl_str_mv ark:/26339/001300000q952
identifier_str_mv MINETTO, Luciane. Macrolides antibiotics: determination and identification of metabolites and degradation subproducts in hospital effluent. 2013. 146 f. Tese (Doutorado em Química) - Universidade Federal de Santa Maria, Santa Maria, 2013.
ark:/26339/001300000q952
url http://repositorio.ufsm.br/handle/1/4262
dc.language.iso.fl_str_mv por
language por
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Universidade Federal de Santa Maria
BR
Química
UFSM
Programa de Pós-Graduação em Química
publisher.none.fl_str_mv Universidade Federal de Santa Maria
BR
Química
UFSM
Programa de Pós-Graduação em Química
dc.source.none.fl_str_mv reponame:Manancial - Repositório Digital da UFSM
instname:Universidade Federal de Santa Maria (UFSM)
instacron:UFSM
instname_str Universidade Federal de Santa Maria (UFSM)
instacron_str UFSM
institution UFSM
reponame_str Manancial - Repositório Digital da UFSM
collection Manancial - Repositório Digital da UFSM
repository.name.fl_str_mv Manancial - Repositório Digital da UFSM - Universidade Federal de Santa Maria (UFSM)
repository.mail.fl_str_mv atendimento.sib@ufsm.br||tedebc@gmail.com
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