Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters
Autor(a) principal: | |
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Data de Publicação: | 2021 |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10773/31493 |
Resumo: | Over the last few decades, the occurrence of emerging contaminants (EC) has raised concerns due to their ubiquitous presence in the environment and potential to cause undesirable ecological effects. Their main source are the discharges of wastewater treatment plants (WWTPs), which are not effective barriers to these pollutants. In order to assess the fate of EC, as well as to evaluate possible strategies to attenuate their presence, the study of natural processes is of the greatest importance. Adsorption, biodegradation and photodegradation appear as significant mechanisms of removal of EC in aquatic environments. Among the EC, two antibiotics, sulfadiazine (SDZ) and oxolinic acid (OXA), and two estrogens, estrone (E1) and 17α-ethinylestradiol (EE2), have received considerable attention because of their high consumption and persistence in the environment. Since SDZ and OXA resist to biodegradation and tend to remain in aqueous phase, while E1 and EE2 have high affinity to solid phase, in the present work, the photodegradation of antibiotics and the adsorption and biodegradation of estrogens were investigated. In what concerns SDZ and OXA photodegradation, the effect of environmentally relevant factors such as the pH, the presence of fractions of estuarine humic substances and salinity were evaluated. The results obtained indicated that at higher pH, and in the presence of photosensitizers, the SDZ photodegradation was much faster than in ultrapure water. Different results were obtained for OXA, with a significant decrease in its photodegradation in presence of photosensitizers. These observations may explain the results obtained in environmental matrices, namely the final effluent of a WWTP, fresh water and brackish water, in which the photodegradation of SDZ (t½ between 2.32 h and 3.48 h) was found to be much faster than in ultrapure water (t½ = 6.76 h). In contrast, OXA photodegradation was much slower in the final effluent of a WWTP, fresh water and brackish water (t½ between 1.65 h and 4.03 h) than in ultrapure water (t½ = 0.99 h). In WWTPs estrogens are mainly adsorbed onto sludge. Thus, a simple, reliable and inexpensive method for the quantification of E1 and EE2 in fresh sludge samples was developed. Recovery values of 103 % and 97 % were obtained for E1 and EE2, respectively. Regarding the estrogens’ removal under anaerobic conditions, the influence of different factors was investigated. A higher E1 removal from solid phase of sludge was obtained for higher temperatures (25 C and 34 C) and lower sludge content (2 g L-1). In the case of EE2, higher removal was obtained for lower sludge content (2 g L-1 and 3 g L-1). However, temperature had no effect on the removal of EE2. The presence of nitrate does not appear to influence the removal of both E1 and EE2 from sludge. Finally, the performance of continuous (CO) and intermittent operation (IO) of Upflow Anaerobic Sludge Blanket (UASB) reactors on the removal of E1 and EE2 was assessed. Higher biodegradation values (69.4 % vs. 43.3 % for E1 and 21.8 % vs. 8.0 % for EE2) and adsorption values (26.5 % vs. 5.7 % for E1 and 72.7 % vs. 31.0% for EE2) were found with the IO, compared to CO. Thus, the IO of UASB reactors can be a promising, sustainable, and robust alternative for E1 and EE2 removal from wastewaters. |
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Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewatersSulfadiazineOxolinic acidEstrone17α-ethinylestradiolBiodegradationAdsorptionPhotodegradationPhotosensitizersIntermittent UASB reactorOver the last few decades, the occurrence of emerging contaminants (EC) has raised concerns due to their ubiquitous presence in the environment and potential to cause undesirable ecological effects. Their main source are the discharges of wastewater treatment plants (WWTPs), which are not effective barriers to these pollutants. In order to assess the fate of EC, as well as to evaluate possible strategies to attenuate their presence, the study of natural processes is of the greatest importance. Adsorption, biodegradation and photodegradation appear as significant mechanisms of removal of EC in aquatic environments. Among the EC, two antibiotics, sulfadiazine (SDZ) and oxolinic acid (OXA), and two estrogens, estrone (E1) and 17α-ethinylestradiol (EE2), have received considerable attention because of their high consumption and persistence in the environment. Since SDZ and OXA resist to biodegradation and tend to remain in aqueous phase, while E1 and EE2 have high affinity to solid phase, in the present work, the photodegradation of antibiotics and the adsorption and biodegradation of estrogens were investigated. In what concerns SDZ and OXA photodegradation, the effect of environmentally relevant factors such as the pH, the presence of fractions of estuarine humic substances and salinity were evaluated. The results obtained indicated that at higher pH, and in the presence of photosensitizers, the SDZ photodegradation was much faster than in ultrapure water. Different results were obtained for OXA, with a significant decrease in its photodegradation in presence of photosensitizers. These observations may explain the results obtained in environmental matrices, namely the final effluent of a WWTP, fresh water and brackish water, in which the photodegradation of SDZ (t½ between 2.32 h and 3.48 h) was found to be much faster than in ultrapure water (t½ = 6.76 h). In contrast, OXA photodegradation was much slower in the final effluent of a WWTP, fresh water and brackish water (t½ between 1.65 h and 4.03 h) than in ultrapure water (t½ = 0.99 h). In WWTPs estrogens are mainly adsorbed onto sludge. Thus, a simple, reliable and inexpensive method for the quantification of E1 and EE2 in fresh sludge samples was developed. Recovery values of 103 % and 97 % were obtained for E1 and EE2, respectively. Regarding the estrogens’ removal under anaerobic conditions, the influence of different factors was investigated. A higher E1 removal from solid phase of sludge was obtained for higher temperatures (25 C and 34 C) and lower sludge content (2 g L-1). In the case of EE2, higher removal was obtained for lower sludge content (2 g L-1 and 3 g L-1). However, temperature had no effect on the removal of EE2. The presence of nitrate does not appear to influence the removal of both E1 and EE2 from sludge. Finally, the performance of continuous (CO) and intermittent operation (IO) of Upflow Anaerobic Sludge Blanket (UASB) reactors on the removal of E1 and EE2 was assessed. Higher biodegradation values (69.4 % vs. 43.3 % for E1 and 21.8 % vs. 8.0 % for EE2) and adsorption values (26.5 % vs. 5.7 % for E1 and 72.7 % vs. 31.0% for EE2) were found with the IO, compared to CO. Thus, the IO of UASB reactors can be a promising, sustainable, and robust alternative for E1 and EE2 removal from wastewaters.Nas últimas décadas, a ocorrência de contaminantes emergentes (CE) suscitou preocupações devido à sua presença no ambiente e ao seu potencial para causar efeitos ecológicos indesejáveis. A sua principal fonte são as descargas de estações de tratamento de águas residuais (ETARs), que não são eficazes na remoção destes poluentes. A fim de avaliar o destino de CE, bem como de avaliar possíveis estratégias para atenuar a sua presença, o estudo dos processos naturais é de maior importância. Adsorção, biodegradação e fotodegradação aparecem como mecanismos significativos de remoção de CE em ambientes aquáticos. Entre os CE, dois antibióticos, sulfadiazina (SDZ) e ácido oxolínico (OXA), e dois estrogénios, estrona (E1) e 17α-etinilestradiol (EE2), têm recebido especial atenção devido ao seu elevado consumo e persistência no ambiente. Uma vez que os antibióticos SDZ e OXA resistem à biodegradação e tendem a permanecer na fase aquosa, e os estrogénios E1 e EE2 têm grande afinidade com a fase sólida, no presente trabalho foram investigadas a fotodegradação dos antibióticos e a adsorção e biodegradação dos estrogénios. No que diz respeito à fotodegradação de SDZ e OXA, foi avaliado o efeito de fatores ambientalmente relevantes como o pH, a presença de frações de substâncias húmicas estuarinas e a salinidade. Os resultados obtidos indicaram que a pH mais elevado, e na presença de fotossensibilizadores, a fotodegradação da SDZ foi muito mais rápida do que em água ultrapura. Para o OXA foram obtidos resultados diferentes, tendo-se observado uma diminuição significativa da sua fotodegradação na presença de fotossensibilizadores. Estas observações podem explicar os resultados obtidos em matrizes ambientais, nomeadamente, o efluente final de uma ETAR, água doce e água salobra, nas quais a fotodegradação da SDZ (t½ entre 2,32 h e 3,48 h) foi muito mais rápida do que em água ultrapura (t½ = 6,76 h), enquanto que para o OXA foi muito mais lenta (t½ entre 1,65 h e 4,03 h) do que em água ultrapura (t½ = 0,99 h). Nas ETARs os estrogénios são principalmente adsorvidos às lamas. Assim, foi desenvolvido um método simples, fiável e barato para a quantificação de E1 e EE2 em amostras de lamas frescas. Foram obtidos valores de recuperação de 103 % e 97 % para E1 e EE2, respetivamente. Relativamente à remoção de estrogénios em condições anaeróbias, foi investigada a influência de diferentes fatores. Obtiveram-se remoções mais elevadas de E1 da fase sólida das lamas a temperaturas mais elevadas (25 C e 34 C) e menor teor de lamas (2 g L-1). No caso do EE2, foram observadas remoções mais elevadas com menor teor de lamas (2 g L-1 e 3 g L-1). No entanto, não foi observado qualquer efeito da temperatura na remoção do EE2. A presença de nitrato não parece influenciar a remoção, tanto do E1 como do EE2 das lamas. Finalmente, foi avaliado o desempenho do modo de operação contínuo (OC) e intermitente (OI) dos reatores de leito de lamas e fluxo ascendente (UASB) na remoção de E1 e EE2. Valores mais elevados de biodegradação (69,4 % vs. 43,3 % para E1 e 21,8 % vs. 8,0 % para EE2) e de adsorção (26,5 % vs. 5,7 % para E1 e 72,7 % vs. 31,0 % para EE2) foram obtidos com a OI em comparação com a OC. Assim, a OI dos reatores UASB pode ser uma alternativa promissora, sustentável e robusta para a remoção de E1 e EE2 das águas residuais.2023-05-26T00:00:00Z2021-05-20T00:00:00Z2021-05-20doctoral thesisinfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10773/31493TID:101586590engLouros, Vitória Loureiro dosinfo:eu-repo/semantics/embargoedAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2024-05-06T04:32:11Zoai:ria.ua.pt:10773/31493Portal AgregadorONGhttps://www.rcaap.pt/oai/openairemluisa.alvim@gmail.comopendoar:71602024-05-06T04:32:11Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters |
title |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters |
spellingShingle |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters Louros, Vitória Loureiro dos Sulfadiazine Oxolinic acid Estrone 17α-ethinylestradiol Biodegradation Adsorption Photodegradation Photosensitizers Intermittent UASB reactor |
title_short |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters |
title_full |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters |
title_fullStr |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters |
title_full_unstemmed |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters |
title_sort |
Bio- and photodegradation as strategies for the removal of estrogens and antibiotics from wastewaters |
author |
Louros, Vitória Loureiro dos |
author_facet |
Louros, Vitória Loureiro dos |
author_role |
author |
dc.contributor.author.fl_str_mv |
Louros, Vitória Loureiro dos |
dc.subject.por.fl_str_mv |
Sulfadiazine Oxolinic acid Estrone 17α-ethinylestradiol Biodegradation Adsorption Photodegradation Photosensitizers Intermittent UASB reactor |
topic |
Sulfadiazine Oxolinic acid Estrone 17α-ethinylestradiol Biodegradation Adsorption Photodegradation Photosensitizers Intermittent UASB reactor |
description |
Over the last few decades, the occurrence of emerging contaminants (EC) has raised concerns due to their ubiquitous presence in the environment and potential to cause undesirable ecological effects. Their main source are the discharges of wastewater treatment plants (WWTPs), which are not effective barriers to these pollutants. In order to assess the fate of EC, as well as to evaluate possible strategies to attenuate their presence, the study of natural processes is of the greatest importance. Adsorption, biodegradation and photodegradation appear as significant mechanisms of removal of EC in aquatic environments. Among the EC, two antibiotics, sulfadiazine (SDZ) and oxolinic acid (OXA), and two estrogens, estrone (E1) and 17α-ethinylestradiol (EE2), have received considerable attention because of their high consumption and persistence in the environment. Since SDZ and OXA resist to biodegradation and tend to remain in aqueous phase, while E1 and EE2 have high affinity to solid phase, in the present work, the photodegradation of antibiotics and the adsorption and biodegradation of estrogens were investigated. In what concerns SDZ and OXA photodegradation, the effect of environmentally relevant factors such as the pH, the presence of fractions of estuarine humic substances and salinity were evaluated. The results obtained indicated that at higher pH, and in the presence of photosensitizers, the SDZ photodegradation was much faster than in ultrapure water. Different results were obtained for OXA, with a significant decrease in its photodegradation in presence of photosensitizers. These observations may explain the results obtained in environmental matrices, namely the final effluent of a WWTP, fresh water and brackish water, in which the photodegradation of SDZ (t½ between 2.32 h and 3.48 h) was found to be much faster than in ultrapure water (t½ = 6.76 h). In contrast, OXA photodegradation was much slower in the final effluent of a WWTP, fresh water and brackish water (t½ between 1.65 h and 4.03 h) than in ultrapure water (t½ = 0.99 h). In WWTPs estrogens are mainly adsorbed onto sludge. Thus, a simple, reliable and inexpensive method for the quantification of E1 and EE2 in fresh sludge samples was developed. Recovery values of 103 % and 97 % were obtained for E1 and EE2, respectively. Regarding the estrogens’ removal under anaerobic conditions, the influence of different factors was investigated. A higher E1 removal from solid phase of sludge was obtained for higher temperatures (25 C and 34 C) and lower sludge content (2 g L-1). In the case of EE2, higher removal was obtained for lower sludge content (2 g L-1 and 3 g L-1). However, temperature had no effect on the removal of EE2. The presence of nitrate does not appear to influence the removal of both E1 and EE2 from sludge. Finally, the performance of continuous (CO) and intermittent operation (IO) of Upflow Anaerobic Sludge Blanket (UASB) reactors on the removal of E1 and EE2 was assessed. Higher biodegradation values (69.4 % vs. 43.3 % for E1 and 21.8 % vs. 8.0 % for EE2) and adsorption values (26.5 % vs. 5.7 % for E1 and 72.7 % vs. 31.0% for EE2) were found with the IO, compared to CO. Thus, the IO of UASB reactors can be a promising, sustainable, and robust alternative for E1 and EE2 removal from wastewaters. |
publishDate |
2021 |
dc.date.none.fl_str_mv |
2021-05-20T00:00:00Z 2021-05-20 2023-05-26T00:00:00Z |
dc.type.driver.fl_str_mv |
doctoral thesis |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10773/31493 TID:101586590 |
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http://hdl.handle.net/10773/31493 |
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TID:101586590 |
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eng |
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eng |
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Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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RCAAP |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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