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Drugs in the Environment—Risks and Solutions

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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Green Chemistry".

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 24921

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Dr. Urszula Guzik

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Institute of Biology, Biotechnology and Environmental Protection, Faculty of Natural Science, University of Silesia in Katowice, Jagiellońska 28, 40 032 Katowice, Poland
Interests: microbiological decomposition of compounds with aromatic structure; biochemistry of microorganisms; toxicity testing of xenobiotics to microorganisms; immobilization of enzymes and bacteria
Special Issues, Collections and Topics in MDPI journals

Dr. Danuta Wojcieszyńska

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Institute of Biology, Faculty of Natural Science, Biotechnology and Environmental Protection, University of Silesia in Katowice, Jagiellońska 28, 40 032 Katowice, Poland
Interests: biodegradation of aromatics; including nonsteroidal anti-inflammatory drugs; enzymes involved in the breakdown of aromatics; immobilization of microorganisms and enzymatic proteins; microbial metabolism
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

In recent years, the increased usage of pharmaceuticals such as antibiotics, contraceptive hormones, non-steroidal anti-inflammatory drugs, lipid regulators, anti-cancer drugs, anti-epileptic drugs, and regulating blood pressure drugs has resulted in their presence in the environment. They reach the environment through usage in human and veterinary medicine, and disposal of unused or out-of-date drugs. This is an emerging problem due to their potential influence on human health and ecological community.

We invite investigators to contribute original research articles, as well as review articles, that will stimulate continuing efforts to develop strategies that can limit environmental contamination by drugs and help remove them from contaminated sites.

Topics of interest for Special Issue include, but are not limited to the following:

Environmental risks connected with the presence of pharmaceuticals in the ecosystems;
Human and veterinary medicine, animal production, and disposal of unused or out-of-date drugs as sources of drugs in the environment;
the metagenomics analysis of the ecosystems involved in the pharmaceuticals disposal sites;
Advanced oxidation processes (AOPs) and their value for pharmaceutical utilization;
Sewage treatment plant (STP) processes for removing pharmaceutical products;
Development of new methods allowing to the intensification of pharmaceuticals degradation;
Biotransformation and biodegradation of drugs;
Analysis of bioproducts from physicochemical and biological conversions of drugs.

Dr. Urszula Guzik
Dr. Danuta Wojcieszyńska
Guest Editors

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Keywords

Pharmaceuticals
Biodegradation
Environmental risk
Advanced oxidation processes

Published Papers (10 papers)

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Research

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28 pages, 16027 KiB

Open AccessArticle

Enhanced Efficiency of the Removal of Cytostatic Anthracycline Drugs Using Immobilized Mycelium of Bjerkandera adusta CCBAS 930

by Kamila Rybczyńska-Tkaczyk

Molecules 2021, 26(22), 6842; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26226842 - 12 Nov 2021

Cited by 1 | Viewed by 1384

Abstract

The aim of this study was to evaluate the bioremoval of anthracycline antibiotics (daunomycin-DNR, doxorubicin–DOX, and mitoxantrone-MTX) by immobilized mycelium of B. adusta CCBAS 930. The activity of oxidoreductases: versatile peroxidases (VP), superoxide dismutase (SOD), catalase (CAT), and glucose oxidase (GOX), and the levels of phenolic compounds (PhC) and free radicals (SOR) were determined during the biotransformation of anthracyclines by B. adusta strain CCBAS 930. Moreover, the phytotoxicity (Lepidium sativum L.), biotoxicity (MARA assay), and genotoxicity of anthracyclines were evaluated after biological treatment. After 120 h, more than 90% of anthracyclines were removed by the immobilized mycelium of B. adusta CCBAS 930. The effective biotransformation of anthracyclines was correlated with detoxification and reduced genotoxicity. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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19 pages, 6067 KiB

Open AccessArticle

Pigeon Pea Husk for Removal of Emerging Contaminants Trimethoprim and Atenolol from Water

by Severin Eder, Manuel Torko, Alessia Montalbetti, Paride Azzari and Laura Nyström

Molecules 2021, 26(11), 3158; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26113158 - 25 May 2021

Cited by 6 | Viewed by 2034

Abstract

The pace of industrialization and rapid population growth in countries such as India entail an increased input of industrial and sanitary organic micropollutants, the so-called emerging contaminants (EC), into the environment. The emission of EC, such as pharmaceuticals, reaching Indian water bodies causes a detrimental effect on aquatic life and ultimately on human health. However, the financial burden of expanding sophisticated water treatment capacities renders complementary, cost-efficient alternatives, such as adsorption, attractive. Here we show the merits of washed and milled pigeon pea husk (PPH) as low-cost adsorbent for the removal of the EC trimethoprim (TMP) and atenolol (ATN) that are among the most detected pharmaceuticals in Indian waters. We found a linear increase in adsorption capacity of PPH for TMP and ATN at concentrations ranging from 10 to 200 μg/L and from 50 to 400 μg/L, respectively, reflecting the concentrations occurring in Indian water bodies. Investigation of adsorption kinetics using the external mass transfer model (EMTM) revealed that film diffusion resistance governed the adsorption process of TMP or ATN onto PPH. Moreover, analysis of the adsorption performance of PPH across an extensive range of pH and temperature illustrated that the highest adsorption loadings achieved concurred with actual conditions of Indian waters. We anticipate our work as starting point towards the development of a feasible adsorbent system aiming at low-cost water treatment. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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15 pages, 3665 KiB

Open AccessArticle

Effect of Pseudomonas moorei KB4 Cells’ Immobilisation on Their Degradation Potential and Tolerance towards Paracetamol

by Robert Surma, Danuta Wojcieszyńska, Jagna Karcz and Urszula Guzik

Molecules 2021, 26(4), 820; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26040820 - 04 Feb 2021

Cited by 9 | Viewed by 2297

Abstract

Pseudomonas moorei KB4 is capable of degrading paracetamol, but high concentrations of this drug may cause an accumulation of toxic metabolites. It is known that immobilisation can have a protective effect on bacterial cells; therefore, the toxicity and degradation rate of paracetamol by the immobilised strain KB4 were assessed. Strain KB4 was immobilised on a plant sponge. A toxicity assessment was performed by measuring the concentration of ATP using the colony-forming unit (CFU) method. The kinetic parameters of paracetamol degradation were estimated using the Hill equation. Toxicity analysis showed a protective effect of the carrier at low concentrations of paracetamol. Moreover, a pronounced phenomenon of hormesis was observed in the immobilised systems. The obtained kinetic parameters and the course of the kinetic curves clearly indicate a decrease in the degradation activity of cells after their immobilisation. There was a delay in degradation in the systems with free cells without glucose and immobilised cells with glucose. However, it was demonstrated that the immobilised systems can degrade at least ten succeeding cycles of 20 mg/L paracetamol degradation. The obtained results indicate that the immobilised strain may become a useful tool in the process of paracetamol degradation. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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20 pages, 2793 KiB

Open AccessArticle

Possibility to Biotransform Anthracyclines by Peroxidases Produced by Bjerkandera adusta CCBAS 930 with Reduction of Geno- and Cytotoxicity and Pro-Oxidative Activity

by Kamila Rybczyńska-Tkaczyk, Teresa Korniłłowicz-Kowalska and Konrad A. Szychowski

Molecules 2021, 26(2), 462; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules26020462 - 17 Jan 2021

Cited by 5 | Viewed by 2054

Abstract

The aim of this study was to evaluate the bioremoval mechanism of anthracycline antibiotics by the white-rot fungus B. adusta CCBAS 930. The activity of oxidoreductases and levels of phenolic compounds and free radicals were determined during the biotransformation of anthraquinone antibiotics: daunomycin (DNR) and doxorubicin (DOX) by B. adusta strain CCBAS 930. Moreover, phytotoxicity (Lepidium sativum L.), ecotoxicity (Vibrio fischeri), genotoxicity and cytotoxicity of anthraquinone dyes were evaluated before and after biological treatment. More than 80% and 90% of DNR and DOX were removed by biodegradation (decolorization). Initial solutions of DNR and DOX were characterized by eco-, phyto-, geno- and cytotoxicity. Despite efficient decolorization, secondary metabolites, toxic to bacteria, formed during biotransformation of anthracycline antibiotics in B. adusta CCBAS 930 cultures. DNR and DOX metabolites did not increase reactive oxygen species (ROS) production in human fibroblasts and resazurin reduction. DNR metabolites did not change caspase-3 activity. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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20 pages, 1581 KiB

Open AccessFeature PaperArticle

Supramolecular Solvent-Based Microextraction of Selected Anticonvulsant and Nonsteroidal Anti-Inflammatory Drugs from Sediment Samples

by Sylwia Bajkacz, Paulina Adamczewska, Klaudia Kokoszka, Elżbieta Kycia-Słocka, Adam Sochacki and Ewa Felis

Molecules 2020, 25(23), 5671; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25235671 - 01 Dec 2020

Cited by 4 | Viewed by 1893

Abstract

The increase in the production and consumption of pharmaceuticals increases their presence in the global environment, which may result in direct threats to living organisms. For this reason, there is a need for new methods to analyze drugs in environmental samples. Here, a new procedure for separating and determining selected drugs (diclofenac, ibuprofen, and carbamazepine) from bottom sediment and water samples was developed. Drugs were determined by ultra-high performance liquid chromatography coupled with an ultraviolet detector (UHPLC-UV). In this work, a universal and single-step sample treatment, based on supramolecular solvents (SUPRAS), was proposed to isolate selected anticonvulsants and nonsteroidal anti-inflammatory drugs (NSAIDs) from sediment samples. The following parameters were experimentally selected: composition of the supramolecular solvent (composition THF:H₂O (v/v), amount of decanoic acid), volume of extractant, sample mass, extraction time, centrifugation time, and centrifugation speed. Finally, the developed procedure was validated. A Speedisk procedure was also developed to extract selected drugs from water samples. The recovery of analytes using the SUPRAS procedure was in the range of 88.8–115%, while the recoveries of the Speedisk solid-phase extraction procedure ranged from 81.0–106%. The effectiveness of the sorption of the tested drugs by sediment was also examined. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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15 pages, 1498 KiB

Open AccessArticle

Rapid, Precise and Affordable Estimation of Venlafaxine and Its Metabolites in Highly Polluted Effluent Waters: Proof-of-Concept for Methodology

by Snawar Hussain, Chandramouli Ramnarayanan, Teeka S. Roopashree, Md. Khalid Anwer, Nagaraja Sreeharsha and Anroop B. Nair

Molecules 2020, 25(20), 4793; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25204793 - 19 Oct 2020

Cited by 3 | Viewed by 2660

Abstract

Widespread presence of pharmaceuticals and their metabolites in the environment of industrialized countries is an emerging global concern. Potential contamination of the soil and water by such pharmacologically active substances poses serious ecotoxicological implications. Several studies assessing the long-term ecological risks of pharmaceutical contaminants mainly focus on the risk assessment of the parent drug, while the potential contributions of their metabolites is often neglected. Presence of selective serotonin and norepinephrine reuptake inhibitor venlafaxine, an antidepressant drug, and its metabolites is a matter of serious concern for aquatic systems, since they are difficult to remove by traditional wastewater treatment processes. The concentration of VEN present in water is reportedly one of the highest among pharmaceuticals; however, the long-term effects of its metabolites have not yet been systematically studied. Given the consideration to complex and time-consuming effluent treatment, and realizing the importance of levels of venlafaxine and its metabolites, a simple and accurate analytical method for quick determination is needed. We designed a selective colorimetric method by using oxidative coupling of drug molecules with 3-methyl-2-benzothiazolinone hydrazone hydrochloride (MBTH) reagent, to quantify the presence of venlafaxine and its metabolites in aquatic samples, with special emphasis on effluent. The method was validated for selectivity, specificity and robustness as per the ICH Q2 guidelines to assess its suitability in pharmaceutical samples, as well. Highly sensitive and green economical analytical method was successfully established for estimation of venlafaxine and its metabolites in aquatic samples. The method was quick, as it involved minimum processing steps. The method was accurate and linear in the range of 0.5 to 80 ppm and could successfully detect lowest concentration of 1.3 ppm, thus qualifying its applicability for the desired purpose to check the presence of trace levels of VEN or its metabolites in aquatic samples or in pharmaceutical formulations. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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15 pages, 5099 KiB

Open AccessArticle

Photoluminescence as a Valuable Tool in the Optical Characterization of Acetaminophen and the Monitoring of Its Photodegradation Reactions

by Monica Daescu, Adelina Matea, Catalin Negrila, Constantin Serbschi, Alina C. Ion and Mihaela Baibarac

Molecules 2020, 25(19), 4571; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25194571 - 07 Oct 2020

Cited by 7 | Viewed by 2694

Abstract

In this work, new evidence for the photodegradation reactions of acetaminophen (AC) is reported by photoluminescence (PL), Raman scattering and FTIR spectroscopy. Under excitation wavelength of 320 nm, AC shows a PL band in the spectral range of 340–550 nm, whose intensity decreases by exposure to UV light. The chemical interaction of AC with the NaOH solutions, having the concentration ranging between 0.001 and 0.3 M, induces a gradual enhancement of the photoluminescence excitation (PLE) and PL spectra, when the exposure time of samples at the UV light increases until 140 min, as a result of the formation of p-aminophenol and sodium acetate. This behavior is not influenced by the excipients or other active compounds in pharmaceutical products as demonstrated by PLE and PL studies. Experimental arguments for the obtaining of p-aminophenol and sodium acetate, when AC has interacted with NaOH, are shown by Raman scattering and FTIR spectroscopy. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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10 pages, 1802 KiB

Open AccessArticle

The Uptake of Ivermectin and Its Effects in Roots, Leaves and Seeds of Soybean (Glycine max)

by Martina Navrátilová, Lucie Raisová Stuchlíková, Kateřina Moťková, Barbora Szotáková, Lenka Skálová, Lenka Langhansová and Radka Podlipná

Molecules 2020, 25(16), 3655; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25163655 - 11 Aug 2020

Cited by 8 | Viewed by 2832

Abstract

In recent years interest has grown in the occurrence and the effects of pharmaceuticals in the environment. The aim of this work is to evaluate the risk of fertilizing crops with manure from livestock treated with anthelmintics. The present study was designed to follow the fate of the commonly used anthelmintic drug, ivermectin (IVM) and its metabolites in soybeans (Glycine max (L.) Merr.), a plant that is grown and consumed world-wide for its high content of nutritional and health-beneficial substances. In vitro plantlets and soybean plants, cultivated in a greenhouse, were used for this purpose. Our results showed the uptake of IVM and its translocation to the leaves, but not in the pods and the beans. Four IVM metabolites were detected in the roots, and one in the leaves. IVM exposure decreased slightly the number and weight of the beans and induced changes in the activities of antioxidant enzymes. In addition, the presence of IVM affected the proportion of individual isoflavones and reduced the content of isoflavones aglycones, which might decrease the therapeutic value of soybeans. Fertilization of soybean fields with manure from IVM-treated animals appears to be safe for humans, due to the absence of IVM in beans, the food part of plants. On the other hand, it could negatively affect soybean plants and herbivorous invertebrates. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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11 pages, 440 KiB

Open AccessCommunication

In Vitro Metabolic Transformation of Pharmaceuticals by Hepatic S9 Fractions from Common Carp (Cyprinus carpio)

by Viktoriia Burkina, Sidika Sakalli, Pham Thai Giang, Kateřina Grabicová, Andrea Vojs Staňová, Galia Zamaratskaia and Vladimir Zlabek

Molecules 2020, 25(11), 2690; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25112690 - 10 Jun 2020

Cited by 2 | Viewed by 3415

Abstract

Water from wastewater treatment plants contains concentrations of pharmaceutically active compounds as high as micrograms per liter, which can adversely affect fish health and behavior, and contaminate the food chain. Here, we tested the ability of the common carp hepatic S9 fraction to produce the main metabolites from citalopram, metoprolol, sertraline, and venlafaxine. Metabolism in fish S9 fractions was compared to that in sheep. The metabolism of citalopram was further studied in fish. Our results suggest a large difference in the rate of metabolites formation between fish and sheep. Fish hepatic S9 fractions do not show an ability to form metabolites from venlafaxine, which was also the case for sheep. Citalopram, metoprolol, and sertraline were metabolized by both fish and sheep S9. Citalopram showed concentration-dependent N-desmethylcitalopram formation with V_max = 1781 pmol/min/mg and K_m = 29.7 μM. The presence of ellipticine, a specific CYP1A inhibitor, in the incubations reduced the formation of N-desmethylcitalopram by 30–100% depending on the applied concentration. These findings suggest that CYP1A is the major enzyme contributing to the formation of N-desmethylcitalopram. In summary, the results from the present in vitro study suggest that common carp can form the major metabolites of citalopram, metoprolol, and sertraline. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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Review

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25 pages, 5040 KiB

Open AccessReview

Suitability of Immobilized Systems for Microbiological Degradation of Endocrine Disrupting Compounds

by Danuta Wojcieszyńska, Ariel Marchlewicz and Urszula Guzik

Molecules 2020, 25(19), 4473; https://0-doi-org.brum.beds.ac.uk/10.3390/molecules25194473 - 29 Sep 2020

Cited by 12 | Viewed by 2885

Abstract

The rising pollution of the environment with endocrine disrupting compounds has increased interest in searching for new, effective bioremediation methods. Particular attention is paid to the search for microorganisms with high degradation potential and the possibility of their use in the degradation of endocrine disrupting compounds. Increasingly, immobilized microorganisms or enzymes are used in biodegradation systems. This review presents the main sources of endocrine disrupting compounds and identifies the risks associated with their presence in the environment. The main pathways of degradation of these compounds by microorganisms are also presented. The last part is devoted to an overview of the immobilization methods used for the purposes of enabling the use of biocatalysts in environmental bioremediation. Full article

(This article belongs to the Special Issue Drugs in the Environment—Risks and Solutions)

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