Hodnocení výskytu vybraných léčivých látek v půdním ekosystému
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Fučík, Jan
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Mark
P
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Vysoké učení technické v Brně. Fakulta chemická
Abstract
Pharmaceuticals, including antibiotics, are essential for treating infectious diseases in humans, livestock, and aquaculture. However, up to 90% of the administered dose may be excreted unmetabolised as the parent compound in faeces or urine. Consequently, these pharmaceuticals, along with their degradation products and metabolites, can enter the terrestrial environment through various pathways, such as irrigation with contaminated wastewater, incorporation of biosolids, or application of animal manure. Pharmaceutical residues in soil pose ecotoxicological risks and can be taken up by plants and soil organisms, potentially disrupting soil ecosystems and amplifying their environmental impact. Additionally, there are growing concerns about the risks to human health associated with the long-term intake of these micropollutants through food, including their potential contribution to the development of antimicrobial resistance. Recognizing these threats, the EU and international organizations such as WHO, UNEP, and OECD have highlighted pharmaceutical residues in the environment as a major concern, though current scientific knowledge remains inadequate to constructing relevant policy and management recommendations. This doctoral thesis presents multiresidue methods for quantifying up to 42 pharmaceutical residues in soil using SPE, and in lettuce and earthworms using QuEChERS, followed by LC-MS analysis. A novel analytical workflow for pharmaceutical metabolite identification, utilising in silico spectral libraries coupled with UHPLC-HRMS, was introduced for lettuce and earthworms, leading to the identification of 26 compounds. Furthermore, uptake experiments with Eisenia fetida in soil and Lactuca sativa under both soil and hydroponic conditions, exposed to varying pharmaceutical concentrations, were conducted to assess the fate of pharmaceuticals (including bioconcentration and translocation factors, as well as pharmaceutical degradation kinetics) and ecotoxicological endpoints (e.g., mortality rates and biomass weight). The data from these experiments were statistically analysed to enable meaningful and objective evaluation of the conclusions, trends, and effects of pharmaceutical residues on these organisms. In addition, risk assessments were performed to evaluate the potential for antimicrobial resistance emergence in the environment and to estimate potential health risks associated with lettuce consumption due to pharmaceutical residues. Finally, various advanced oxidation processes for wastewater treatment, fermentation of animal manure and the effect of biochar in soil were assessed as potential solutions for mitigating pharmaceutical residues in the environment. In particular, the impact of biochar on the bioavailability of these compounds to organisms, including lettuce and earthworms, was evaluated. Overall, this doctoral thesis aimed to contribute to filling the following research gaps: 1) Development and optimisation of multiresidue analytical methods for pharmaceutical extraction from various matrices, 2) Identification of pharmaceutical metabolites in L. sativa and E. fetida using LC-HRMS, 3) Fate of pharmaceutical residues in the environmental: uptake by L. sativa in aquatic and soil systems and E. fetida in soil environment, 4) Assessment of the ecotoxicological effect of pharmaceutical residues in the environment, and 5) Proposing solutions for addressing pharmaceutical residues in various environmental compartments.
Pharmaceuticals, including antibiotics, are essential for treating infectious diseases in humans, livestock, and aquaculture. However, up to 90% of the administered dose may be excreted unmetabolised as the parent compound in faeces or urine. Consequently, these pharmaceuticals, along with their degradation products and metabolites, can enter the terrestrial environment through various pathways, such as irrigation with contaminated wastewater, incorporation of biosolids, or application of animal manure. Pharmaceutical residues in soil pose ecotoxicological risks and can be taken up by plants and soil organisms, potentially disrupting soil ecosystems and amplifying their environmental impact. Additionally, there are growing concerns about the risks to human health associated with the long-term intake of these micropollutants through food, including their potential contribution to the development of antimicrobial resistance. Recognizing these threats, the EU and international organizations such as WHO, UNEP, and OECD have highlighted pharmaceutical residues in the environment as a major concern, though current scientific knowledge remains inadequate to constructing relevant policy and management recommendations. This doctoral thesis presents multiresidue methods for quantifying up to 42 pharmaceutical residues in soil using SPE, and in lettuce and earthworms using QuEChERS, followed by LC-MS analysis. A novel analytical workflow for pharmaceutical metabolite identification, utilising in silico spectral libraries coupled with UHPLC-HRMS, was introduced for lettuce and earthworms, leading to the identification of 26 compounds. Furthermore, uptake experiments with Eisenia fetida in soil and Lactuca sativa under both soil and hydroponic conditions, exposed to varying pharmaceutical concentrations, were conducted to assess the fate of pharmaceuticals (including bioconcentration and translocation factors, as well as pharmaceutical degradation kinetics) and ecotoxicological endpoints (e.g., mortality rates and biomass weight). The data from these experiments were statistically analysed to enable meaningful and objective evaluation of the conclusions, trends, and effects of pharmaceutical residues on these organisms. In addition, risk assessments were performed to evaluate the potential for antimicrobial resistance emergence in the environment and to estimate potential health risks associated with lettuce consumption due to pharmaceutical residues. Finally, various advanced oxidation processes for wastewater treatment, fermentation of animal manure and the effect of biochar in soil were assessed as potential solutions for mitigating pharmaceutical residues in the environment. In particular, the impact of biochar on the bioavailability of these compounds to organisms, including lettuce and earthworms, was evaluated. Overall, this doctoral thesis aimed to contribute to filling the following research gaps: 1) Development and optimisation of multiresidue analytical methods for pharmaceutical extraction from various matrices, 2) Identification of pharmaceutical metabolites in L. sativa and E. fetida using LC-HRMS, 3) Fate of pharmaceutical residues in the environmental: uptake by L. sativa in aquatic and soil systems and E. fetida in soil environment, 4) Assessment of the ecotoxicological effect of pharmaceutical residues in the environment, and 5) Proposing solutions for addressing pharmaceutical residues in various environmental compartments.
Pharmaceuticals, including antibiotics, are essential for treating infectious diseases in humans, livestock, and aquaculture. However, up to 90% of the administered dose may be excreted unmetabolised as the parent compound in faeces or urine. Consequently, these pharmaceuticals, along with their degradation products and metabolites, can enter the terrestrial environment through various pathways, such as irrigation with contaminated wastewater, incorporation of biosolids, or application of animal manure. Pharmaceutical residues in soil pose ecotoxicological risks and can be taken up by plants and soil organisms, potentially disrupting soil ecosystems and amplifying their environmental impact. Additionally, there are growing concerns about the risks to human health associated with the long-term intake of these micropollutants through food, including their potential contribution to the development of antimicrobial resistance. Recognizing these threats, the EU and international organizations such as WHO, UNEP, and OECD have highlighted pharmaceutical residues in the environment as a major concern, though current scientific knowledge remains inadequate to constructing relevant policy and management recommendations. This doctoral thesis presents multiresidue methods for quantifying up to 42 pharmaceutical residues in soil using SPE, and in lettuce and earthworms using QuEChERS, followed by LC-MS analysis. A novel analytical workflow for pharmaceutical metabolite identification, utilising in silico spectral libraries coupled with UHPLC-HRMS, was introduced for lettuce and earthworms, leading to the identification of 26 compounds. Furthermore, uptake experiments with Eisenia fetida in soil and Lactuca sativa under both soil and hydroponic conditions, exposed to varying pharmaceutical concentrations, were conducted to assess the fate of pharmaceuticals (including bioconcentration and translocation factors, as well as pharmaceutical degradation kinetics) and ecotoxicological endpoints (e.g., mortality rates and biomass weight). The data from these experiments were statistically analysed to enable meaningful and objective evaluation of the conclusions, trends, and effects of pharmaceutical residues on these organisms. In addition, risk assessments were performed to evaluate the potential for antimicrobial resistance emergence in the environment and to estimate potential health risks associated with lettuce consumption due to pharmaceutical residues. Finally, various advanced oxidation processes for wastewater treatment, fermentation of animal manure and the effect of biochar in soil were assessed as potential solutions for mitigating pharmaceutical residues in the environment. In particular, the impact of biochar on the bioavailability of these compounds to organisms, including lettuce and earthworms, was evaluated. Overall, this doctoral thesis aimed to contribute to filling the following research gaps: 1) Development and optimisation of multiresidue analytical methods for pharmaceutical extraction from various matrices, 2) Identification of pharmaceutical metabolites in L. sativa and E. fetida using LC-HRMS, 3) Fate of pharmaceutical residues in the environmental: uptake by L. sativa in aquatic and soil systems and E. fetida in soil environment, 4) Assessment of the ecotoxicological effect of pharmaceutical residues in the environment, and 5) Proposing solutions for addressing pharmaceutical residues in various environmental compartments.
Description
Keywords
pharmaceutical residues, solid-phase extraction, QuEChERS, liquid chromatography, mass spectrometry, pharmaceutical uptake, ecotoxicology, risk assessment, pharmaceutical residues, solid-phase extraction, QuEChERS, liquid chromatography, mass spectrometry, pharmaceutical uptake, ecotoxicology, risk assessment
Citation
FUČÍK, J. Hodnocení výskytu vybraných léčivých látek v půdním ekosystému [online]. Brno: Vysoké učení technické v Brně. Fakulta chemická. 2025.
Document type
Document version
Date of access to the full text
Language of document
en
Study field
bez specializace
Comittee
prof. Ing. Jozef Krajčovič, Ph.D. (předseda)
doc. Mgr. Michaela Vašinová Galiová, Ph.D. (člen)
doc. Mgr. Renata Komendová, Ph.D. (člen)
doc. RNDr. Václav Slovák, Ph.D. (člen)
prof. Ing. Josef Čáslavský, CSc. (člen)
Prof. Stuart Gibb (člen)
Date of acceptance
2025-05-05
Defence
Předseda komise představil doktoranda a předal mu slovo. Ing. Fučík má již řadu pracovních zkušeností z České republiky i ze zahraničí. Je spoluautorem řady konferenčních příspěvků. Spolupodílel se také na několika projektových zprávách. Obhajoba proběhla v angličtině.
Result of defence
práce byla úspěšně obhájena
Document licence
Standardní licenční smlouva - přístup k plnému textu bez omezení