Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures

Detalhes bibliográficos
Autor(a) principal: Silva, Valentina Guimarães da
Data de Publicação: 2021
Tipo de documento: Dissertação
Idioma: eng
Título da fonte: Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
Texto Completo: http://hdl.handle.net/10773/32842
Resumo: To satisfy the world consumption of fish and seafood, the exploitation of aquaculture has been increasing in the last decades. As in other zootechnics, aquaculture uses antibiotics, such as oxolinic acid (OXA) and sulfadiazine (SDZ), for prevention and treatment of diseases. Unfortunately, part of these antibiotics remains in the aquaculture recirculating water systems, as well as in effluents. Thus, the development of sustainable green treatments for antibiotic removal is essential to avoid antibiotics discharge in the aquatic environment and the consequent increase of antimicrobial resistance (AMR). Among these treatments, photodegradation under natural irradiation is a promising alternative. Aiming an efficiency enhancement, the use of semiconductor photocatalysts as titanium dioxide (TiO2) and the versatile carbon quantum dots (CQDs) has risen great interest in the scientific community since they are solar driven photocatalysts, inexpensive to produce and easy to use. In this work, two types of CQDs were synthesized: (i) using citric acid and urea (CQDs-CAU); or (ii) using only citric acid (CQDs-CA). Through a hydrothermal calcination method, different composites were produced by incorporating 4%, 5%, 6% or 8% (w/w) of CQDs in commercial TiO2 (P25). For comparison purposes, calcination was also applied to the single TiO2 and CQDs. The structural characterization of the synthesized photocatalysts was confirmed by X-ray diffraction, Fourier-transform infrared spectroscopy and diffraction reflectance spectrometry, while optical properties were investigated using ultraviolet-visible absorbance and fluorescence spectroscopy. Then, all the materials were tested for OXA and SDZ photocatalysis, namely solutions of each antibiotic (10 mg L -1 ) either in 0.001 mol L -1 phosphate buffer (PB) or in 30 g L -1 synthetic sea salts (SSS), both with pH adjusted to 8.6. In PB, TiO2/CQDs CA 4% (w/w) (500 mg L-1 ) was the most efficient for OXA photodegradation (93.8% removal in 15 min) and SDZ (79.6% removal in 18 min). In SSS, TiO2/CQDs-CA 4% (w/w) (1000 mg L-1) was the most efficient for the degradation of OXA (75.4% removal in 1 h) while CQDs-CAUC (500 mg L-1) was the most efficient for SDZ (69.4% removal in 18 min). The study of photodegradation kinetics using the most efficient photocatalysts and concentrations showed the accentuated decrease of OXA and SDZ half-life time (t1/2). The application of optimal photocatalysis conditions for each antibiotic was tested in brackish aquaculture effluent, where the t1/2 of OXA and SDZ decreased from 3.71 h and 3.98 h to 41.7 min and 4.64 min, respectively. Under these conditions, it was also proved that the bacterial activity of E. coli and V. parahaemolyticus increased with the total photodegradation of OXA and SDZ. Therefore, it was concluded that the produced photocatalysts are efficient in the solar driven removal of OXA and SDZ and in the fight against AMR so they may be used for such a purpose in the sustainable treatment of aquaculture waters.
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spelling Solar driven photocatalysis as a way to eliminate antibiotics from aquaculturesPhotocatalysisAquacultureOxolinic acidSulfadiazineCarbon quantum dotsTitanium dioxideTo satisfy the world consumption of fish and seafood, the exploitation of aquaculture has been increasing in the last decades. As in other zootechnics, aquaculture uses antibiotics, such as oxolinic acid (OXA) and sulfadiazine (SDZ), for prevention and treatment of diseases. Unfortunately, part of these antibiotics remains in the aquaculture recirculating water systems, as well as in effluents. Thus, the development of sustainable green treatments for antibiotic removal is essential to avoid antibiotics discharge in the aquatic environment and the consequent increase of antimicrobial resistance (AMR). Among these treatments, photodegradation under natural irradiation is a promising alternative. Aiming an efficiency enhancement, the use of semiconductor photocatalysts as titanium dioxide (TiO2) and the versatile carbon quantum dots (CQDs) has risen great interest in the scientific community since they are solar driven photocatalysts, inexpensive to produce and easy to use. In this work, two types of CQDs were synthesized: (i) using citric acid and urea (CQDs-CAU); or (ii) using only citric acid (CQDs-CA). Through a hydrothermal calcination method, different composites were produced by incorporating 4%, 5%, 6% or 8% (w/w) of CQDs in commercial TiO2 (P25). For comparison purposes, calcination was also applied to the single TiO2 and CQDs. The structural characterization of the synthesized photocatalysts was confirmed by X-ray diffraction, Fourier-transform infrared spectroscopy and diffraction reflectance spectrometry, while optical properties were investigated using ultraviolet-visible absorbance and fluorescence spectroscopy. Then, all the materials were tested for OXA and SDZ photocatalysis, namely solutions of each antibiotic (10 mg L -1 ) either in 0.001 mol L -1 phosphate buffer (PB) or in 30 g L -1 synthetic sea salts (SSS), both with pH adjusted to 8.6. In PB, TiO2/CQDs CA 4% (w/w) (500 mg L-1 ) was the most efficient for OXA photodegradation (93.8% removal in 15 min) and SDZ (79.6% removal in 18 min). In SSS, TiO2/CQDs-CA 4% (w/w) (1000 mg L-1) was the most efficient for the degradation of OXA (75.4% removal in 1 h) while CQDs-CAUC (500 mg L-1) was the most efficient for SDZ (69.4% removal in 18 min). The study of photodegradation kinetics using the most efficient photocatalysts and concentrations showed the accentuated decrease of OXA and SDZ half-life time (t1/2). The application of optimal photocatalysis conditions for each antibiotic was tested in brackish aquaculture effluent, where the t1/2 of OXA and SDZ decreased from 3.71 h and 3.98 h to 41.7 min and 4.64 min, respectively. Under these conditions, it was also proved that the bacterial activity of E. coli and V. parahaemolyticus increased with the total photodegradation of OXA and SDZ. Therefore, it was concluded that the produced photocatalysts are efficient in the solar driven removal of OXA and SDZ and in the fight against AMR so they may be used for such a purpose in the sustainable treatment of aquaculture waters.Para satisfazer o consumo mundial de peixe e marisco, a exploração da aquacultura tem crescido nas últimas décadas. Tal como outras zootecnias, a aquacultura utiliza antibióticos, como ácido oxolínico (OXA) e sulfadiazina (SDZ), para a prevenção e tratamento de doenças. Infelizmente, parte destes antibióticos permanece nos sistemas de recirculação de água e nos efluentes da aquacultura. O desenvolvimento de tratamentos sustentáveis para a remoção de antibióticos é essencial para evitar a sua descarga no ambiente aquático e o consequente aumento da resistência antimicrobiana (AMR). Entre estes tratamentos, a fotodegradação sob irradiação natural é uma alternativa promissora. Para aumentar a eficiência, o uso de semicondutores, como o dióxido de titânio (TiO2) e os carbon quantum dots (CQDs), tem gerado grande interesse na comunidade científica, uma vez que são fotocatalisadores que utilizam energia solar, são baratos e fáceis de utilizar. Neste trabalho, dois tipos de CQDs foram sintetizados: (i) utilizando ácido cítrico e ureia (CQDs-CAU); e (ii) utilizando apenas ácido cítrico (CQDs-CA). Através de um método de calcinação hidrotérmica, diferentes compósitos foram produzidos incorporando 4%, 5%, 6% ou 8% (m/m) de CQDs em TiO2 comercial (P25). Para fins de comparação, a calcinação foi também aplicada ao TiO2 e aos CQDs. A caraterização estrutural dos fotocatalisadores foi confirmada por difração de raio X, espectroscopia no infravermelho por transformada de Fourier e espetrometria de refletância difusa, enquanto as propriedades óticas foram investigadas usando espetroscopia de absorção de ultravioleta-visível e de fluorescência. Todos os materiais foram testados para a fotocatálise de OXA e SDZ, nomeadamente, soluções de cada antibiótico (10 mg L-1 ), quer em tampão fosfato 0,001 mol L-1 (PB), quer em 30 g L-1 de sais marinhos sintéticos (SSS), ambos com pH ajustado a 8,6. Em PB, TiO2/CQDs CA 4% (m/m) (500 mg L-1 ) foi o fotocatalisador mais eficiente para a degradação do OXA (93,8% de remoção em 15 min) e da SDZ (79,6% de remoção em 18 min). Em SSS, TiO2/CQDs-CA 4% (m/m) (1000 mg L-1) foi o mais eficiente para o OXA (75,4% de remoção em 1 h), enquanto CQDs-CAUC (500 mg L-1) o foi para a SDZ (69,4% de remoção em 18 min). O estudo da cinética de fotodegradação com os fotocatalisadores e concentrações mais eficientes mostrou a diminuição acentuada do tempo de meia-vida (t1/2) de OXA e SDZ. A aplicação das condições ótimas de fotocatálise para cada antibiótico foi testada em efluente de aquacultura salobra onde proveram uma diminuição do t1/2 de OXA e SDZ de 3,71 h e 3,98 h para 41,7 min e 4,64 min, respetivamente. Nestas condições, comprovou-se também que a atividade bacteriana de E. coli e V. parahaemolyticus aumentou com a fotodegradação total de OXA e SDZ. Assim, concluiu-se que os fotocatalisadores produzidos são eficientes na remoção de OXA e SDZ e no combate à AMR e, com este fim, podem ser usados para o tratamento sustentável das águas de aquacultura.2022-01-10T14:31:26Z2021-12-03T00:00:00Z2021-12-03info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/masterThesisapplication/pdfhttp://hdl.handle.net/10773/32842engSilva, Valentina Guimarães dainfo:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2024-02-22T12:03:17Zoai:ria.ua.pt:10773/32842Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-20T03:04:24.606323Repositório 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 Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
title Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
spellingShingle Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
Silva, Valentina Guimarães da
Photocatalysis
Aquaculture
Oxolinic acid
Sulfadiazine
Carbon quantum dots
Titanium dioxide
title_short Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
title_full Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
title_fullStr Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
title_full_unstemmed Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
title_sort Solar driven photocatalysis as a way to eliminate antibiotics from aquacultures
author Silva, Valentina Guimarães da
author_facet Silva, Valentina Guimarães da
author_role author
dc.contributor.author.fl_str_mv Silva, Valentina Guimarães da
dc.subject.por.fl_str_mv Photocatalysis
Aquaculture
Oxolinic acid
Sulfadiazine
Carbon quantum dots
Titanium dioxide
topic Photocatalysis
Aquaculture
Oxolinic acid
Sulfadiazine
Carbon quantum dots
Titanium dioxide
description To satisfy the world consumption of fish and seafood, the exploitation of aquaculture has been increasing in the last decades. As in other zootechnics, aquaculture uses antibiotics, such as oxolinic acid (OXA) and sulfadiazine (SDZ), for prevention and treatment of diseases. Unfortunately, part of these antibiotics remains in the aquaculture recirculating water systems, as well as in effluents. Thus, the development of sustainable green treatments for antibiotic removal is essential to avoid antibiotics discharge in the aquatic environment and the consequent increase of antimicrobial resistance (AMR). Among these treatments, photodegradation under natural irradiation is a promising alternative. Aiming an efficiency enhancement, the use of semiconductor photocatalysts as titanium dioxide (TiO2) and the versatile carbon quantum dots (CQDs) has risen great interest in the scientific community since they are solar driven photocatalysts, inexpensive to produce and easy to use. In this work, two types of CQDs were synthesized: (i) using citric acid and urea (CQDs-CAU); or (ii) using only citric acid (CQDs-CA). Through a hydrothermal calcination method, different composites were produced by incorporating 4%, 5%, 6% or 8% (w/w) of CQDs in commercial TiO2 (P25). For comparison purposes, calcination was also applied to the single TiO2 and CQDs. The structural characterization of the synthesized photocatalysts was confirmed by X-ray diffraction, Fourier-transform infrared spectroscopy and diffraction reflectance spectrometry, while optical properties were investigated using ultraviolet-visible absorbance and fluorescence spectroscopy. Then, all the materials were tested for OXA and SDZ photocatalysis, namely solutions of each antibiotic (10 mg L -1 ) either in 0.001 mol L -1 phosphate buffer (PB) or in 30 g L -1 synthetic sea salts (SSS), both with pH adjusted to 8.6. In PB, TiO2/CQDs CA 4% (w/w) (500 mg L-1 ) was the most efficient for OXA photodegradation (93.8% removal in 15 min) and SDZ (79.6% removal in 18 min). In SSS, TiO2/CQDs-CA 4% (w/w) (1000 mg L-1) was the most efficient for the degradation of OXA (75.4% removal in 1 h) while CQDs-CAUC (500 mg L-1) was the most efficient for SDZ (69.4% removal in 18 min). The study of photodegradation kinetics using the most efficient photocatalysts and concentrations showed the accentuated decrease of OXA and SDZ half-life time (t1/2). The application of optimal photocatalysis conditions for each antibiotic was tested in brackish aquaculture effluent, where the t1/2 of OXA and SDZ decreased from 3.71 h and 3.98 h to 41.7 min and 4.64 min, respectively. Under these conditions, it was also proved that the bacterial activity of E. coli and V. parahaemolyticus increased with the total photodegradation of OXA and SDZ. Therefore, it was concluded that the produced photocatalysts are efficient in the solar driven removal of OXA and SDZ and in the fight against AMR so they may be used for such a purpose in the sustainable treatment of aquaculture waters.
publishDate 2021
dc.date.none.fl_str_mv 2021-12-03T00:00:00Z
2021-12-03
2022-01-10T14:31:26Z
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