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Environmental Fate of Emerging Organic Micro-Contaminants

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A special issue of Applied Sciences (ISSN 2076-3417). This special issue belongs to the section "Environmental Sciences".

Deadline for manuscript submissions: closed (30 June 2019) | Viewed by 47261

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Special Issue Editors

Dr. Peter Hooda

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Guest Editor

Faculty of Science, Engineering and Computing - Kingston University, Surrey KT1 1LQ, UK
Interests: fate of contaminants in terrestrial and aquatic environments

Dr. John Wilkinson

E-Mail Website
Guest Editor

Environment Department, The University of York, Heslington, York YO10 5NG, UK
Interests: environmental fate of micro-organic contaminants, their sources, and dynamics (transportation, transformation/biodegradation, sediment storage, and uptake by aquatic plants and other biota) in river systems

Special Issue Information

Dear Colleagues,

The toxicity and fate of pharmaceuticals and other emerging micro-organic contaminants in the natural and built environments have been the focus of much research over the last twenty years. Recently, particular focus has been centred on the fate of antimicrobial chemicals, including antibiotics and antifungals. The occurrence of such chemicals in the environment is thought to contribute to the selection of resistance in exposed microorganisms. Little is known regarding their persistence through sewage treatment facilities, particularly their partition to sewage sludge or fate in sewage sludge-applied soils. Only recently have minimum selective concentrations for resistance in water been determined for a wide degree of antibiotics. However, little research has been conducted to elucidate whether the concentrations found in various environmental matrices influence the selection of resistance in the environment. The common occurrence of non-antibiotic pharmaceuticals and other micro-organic contaminants (e.g. perfluorinated compounds, plasticisers) is equally of great concern in terms of their environmental fate (occurrence, transformation/biodegradation/attenuation, and bioaccumulation). While the focus of this Special Issue is antibiotics and antifungals, we invite you to submit manuscripts on the environmental fate of all other micro-organic contaminants, particularly in the water-sediment, water-biota, and soil–plant systems.

Dr. Peter Hooda
Dr. John Wilkinson
Guest Editors

Manuscript Submission Information

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Keywords

antibiotics
antifungals
microbial resistance
transformations
degradation
attenuation
bioaccumulation
wastewater treatment

Published Papers (11 papers)

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Editorial

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3 pages, 159 KiB

Open AccessEditorial

Special Issue on the Environmental Fate of Emerging Organic Micro-Contaminants

by John Wilkinson and Peter S. Hooda

Appl. Sci. 2019, 9(15), 2997; https://doi.org/10.3390/app9152997 - 26 Jul 2019

Cited by 1 | Viewed by 1872

Abstract

The toxicity and fate of pharmaceuticals and other emerging micro-organic contaminants in the natural and built environments have been the focus of much research over the last 20 years [...] Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

Research

Jump to: Editorial

15 pages, 786 KiB

Open AccessArticle

Distinct Bacterial Consortia Established in ETBE-Degrading Enrichments from a Polluted Aquifer

by Martina Kyselková, Joana Falcão Salles, Alain Dumestre, Yves Benoit and Geneviève L. Grundmann

Appl. Sci. 2019, 9(20), 4247; https://doi.org/10.3390/app9204247 - 11 Oct 2019

Cited by 4 | Viewed by 2025

Abstract

Ethyl tert-butyl ether (ETBE) is a gasoline additive that became an important aquifer pollutant. The information about natural bacterial consortia with a capacity for complete ETBE degradation is limited. Here we assess the taxonomical composition of bacterial communities and diversity of the ethB gene (involved in ETBE biodegradation) in ETBE-enrichment cultures that were established from a gasoline-polluted aquifer, either from anoxic ETBE-polluted plume water (PW), or from an upstream non-polluted water (UW). We used a 16S rRNA microarray, and 16S rRNA and ethB gene sequencing. Despite the dissimilar initial chemical conditions and microbial composition, ETBE-degrading consortia were obtained from both PW and UW. The composition of ETBE-enrichment cultures was distinct from their initial water samples, reflecting the importance of the rare biosphere as a reservoir of potential ETBE degraders. No convergence was observed between the enrichment cultures originating from UW and PW, which were dominated by Mesorhizobium and Hydrogenophaga, respectively, indicating that distinct consortia with the same functional properties may be present at one site. Conserved ethB genes were evidenced in both PW and UW ETBE-enrichment cultures and in PW water. Our results suggest that the presence of ethB genes rather than the taxonomical composition of in situ bacterial communities indicate the potential for the ETBE degradation at a given site. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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9 pages, 1376 KiB

Open AccessArticle

Detection and Treatment Methods for Perfluorinated Compounds in Wastewater Treatment Plants

by Shun-hwa Lee, Yeon-jung Cho, Miran Lee and Byung-Dae Lee

Appl. Sci. 2019, 9(12), 2500; https://doi.org/10.3390/app9122500 - 19 Jun 2019

Cited by 12 | Viewed by 3473

Abstract

We surveyed the variation in perfluorinated compound (PFC) concentrations entering urban wastewater treatment plants and then designed an optimal PFCs treatment method based on a pilot test. The PFCs influent concentration was found to be affected by the types of industries and operating rate. The concentration of PFCs in the wastewater treatment effluent was slightly lower than that of the influent. Thus, PFCs had not been adequately removed by the existing biological treatments. The pilot test results showed that about 10% of PFCs was removed by coagulation and precipitation, and the ozone and chlorine test showed that few, if any, PFCs were removed regardless of the oxidant dose. The activated carbon adsorption test showed that the removal significantly increased with empty bed contact time, with about a 60% removal in five minutes and over 90% removal in over 15 minutes. Therefore, a more stable and higher PFCs removal would result from continuous oxidation processes, such as ozone and adsorption processes involving activated carbon, rather than a single biological treatment. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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11 pages, 217 KiB

Open AccessArticle

Health Risk Assessment of Banned Veterinary Drugs and Quinolone Residues in Shrimp through Liquid Chromatography–Tandem Mass Spectrometry

by Ming-Yang Tsai, Chuen-Fu Lin, Wei-Cheng Yang, Chien-Teng Lin, Kuo-Hsiang Hung and Geng-Ruei Chang

Appl. Sci. 2019, 9(12), 2463; https://doi.org/10.3390/app9122463 - 17 Jun 2019

Cited by 21 | Viewed by 3112

Abstract

The presence of antibiotic residues in seafood and their effect on public health constitute a matter of concern for consumers worldwide. Antibiotic residues can have adverse effects on both humans and animals, especially residues of banned veterinary drugs. In this study, we applied a validated method to analyze veterinary drug residues in shrimp, including the levels of banned chloramphenicol, malachite green, leucomalachite green, and four nitrofuran metabolites as well as thiamphenicol, florfenicol, and five quinolones, which have no recommended maximum residual levels in shrimp tissues in Taiwan. We collected 53 samples of whiteleg, grass, or giant river shrimp from Taiwanese aquafarms and production areas from July 2016 to December 2017. We found 0.31 ng/g of a chloramphenicol in one grass shrimp, 5.62 ng/g of enrofloxacin in one whiteleg shrimp, 1.52 ng/g of flumequine in one whiteleg shrimp, and 1.01 ng/g of flumequine in one giant river shrimp, indicating that 7.55% of the samples contained veterinary drug residues. We evaluated the health risk by deriving the estimated daily intake (EDI). The quinolone residue EDI was below 1.0% of the acceptable daily intake recommended by the United Nations Food and Agriculture Organization and World Health Organization. The risk was thus discovered to be negligible, indicating no immediate health risk associated with shrimp consumption. The present findings can serve as a reference regarding food safety and in monitoring of the veterinary drug residues present in aquatic organisms. Continual monitoring of residues in shrimp is critical for further assessment of possible effects on human health. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

16 pages, 1634 KiB

Open AccessArticle

Extraction Efficiency of a Commercial Espresso Machine Compared to a Stainless-Steel Column Pressurized Hot Water Extraction (PHWE) System for the Determination of 23 Pharmaceuticals, Antibiotics and Hormones in Sewage Sludge

by Ola Svahn and Erland Björklund

Appl. Sci. 2019, 9(7), 1509; https://doi.org/10.3390/app9071509 - 11 Apr 2019

Cited by 12 | Viewed by 4876

Abstract

Two green chemistry extraction systems, an in-house stainless-steel column Pressurized Hot Water Extraction system (PHWE) and a commercially available Espresso machine were applied for analysing 23 active pharmaceutical ingredients (APIs) in sewage sludge. Final analysis was performed on UPLC-MS/MS using two different chromatographic methods: acid and basic. When analysing all 23 APIs in sewage sludge both extraction methods showed good repeatability. The PHWE method allowed for a more complete extraction of APIs that were more tightly bound to the matrix, as exemplified by much higher concentrations of e.g., ketoconazole, citalopram and ciprofloxacin. In total, 19 out of 23 investigated APIs were quantified in sewage sludge, and with a few exceptions the PHWE method was more exhaustive. Mean absolute recoveries of 7 spiked labelled APIs were lower for the PHWE method than the Espresso method. Under acid chromatographic conditions mean recoveries were 16% and 24%, respectively, but increased to 24% and 37% under basic conditions. The difference between the PHWE method and the Espresso method might be interpreted as the Espresso method giving higher extraction efficiency; however, TIC scans of extracts revealed a much higher matrix co-extraction for the PHWE method. Attempts were made to correlate occurrence of compounds in sewage sludge with chemical properties of the 23 APIs and there are strong indications that both the number of aromatic rings and the presence of a positive charge is important for the sorption processes to sewage sludge. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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14 pages, 1881 KiB

Open AccessArticle

Environmental Pollutants Impair Transcriptional Regulation of the Vitellogenin Gene in the Burrowing Mud Crab (Macrophthalmus Japonicus)

by Kiyun Park, Hyunbin Jo, Dong-Kyun Kim and Ihn-Sil Kwak

Appl. Sci. 2019, 9(7), 1401; https://doi.org/10.3390/app9071401 - 03 Apr 2019

Cited by 10 | Viewed by 3269

Abstract

Vitellogenesis is a pivotal reproductive process of the yolk formation in crustaceans. Vitellogenin (VTG) is the precursor of main yolk proteins and synthesized by endogenous estrogens. The intertidal mud crab (Macrophthalmus japonicus) inhabits sediment and is a good indicator for assessing polluted benthic environments. The purpose of this study was to identify potential responses of M. japonicus VTG under environmental stresses caused by chemical pollutants, such as 1, 10, and 30 µg L⁻¹ concentrations in di(2-ethylhexyl) phthalate (DEHP), bisphenol A (BPA) and irgarol. We characterized the M. japonicus VTG gene and analyzed the transcriptional expression of VTG mRNA in M. japonicus exposed to various chemicals and exposure periods. A phylogenetic analysis revealed that the M. japonicus VTG clustered closely with Eriocheir sinensis (Chinese mitten crab) VTG, in contrast with another clade that included the VTG ortholog of other crabs. The basal level of VTG expression was the highest in the hepatopancreas and ovaries, and tissues. VTG expression significantly increased in the ovaries and hepatopancreas after 24 h exposure to DEHP. Increased responses of VTG transcripts were found in M. japonicus exposed to DEHP and BPA for 96 h; however, VTG expression decreased in both tissues after irgarol exposure. After an exposure of 7 d, VTG expression significantly increased in the ovaries and hepatopancreas for all concentrations of all chemicals. These results suggest that the crustacean embryogenesis and endocrine processes are impaired by the environmental chemical pollutants DEHP, BPA, and irgarol. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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14 pages, 2497 KiB

Open AccessFeature PaperArticle

A Novel Method to Characterise Levels of Pharmaceutical Pollution in Large-Scale Aquatic Monitoring Campaigns

by John L. Wilkinson, Alistair B.A. Boxall and Dana W. Kolpin

Appl. Sci. 2019, 9(7), 1368; https://doi.org/10.3390/app9071368 - 01 Apr 2019

Cited by 32 | Viewed by 9400

Abstract

Much of the current understanding of pharmaceutical pollution in the aquatic environment is based on research conducted in Europe, North America and other select high-income nations. One reason for this geographic disparity of data globally is the high cost and analytical intensity of the research, limiting accessibility to necessary equipment. To reduce the impact of such disparities, we present a novel method to support large-scale monitoring campaigns of pharmaceuticals at different geographical scales. The approach employs the use of a miniaturised sampling and shipping approach with a high throughput and fully validated direct-injection High-Performance Liquid Chromatography-Tandem Mass Spectrometry method for the quantification of 61 active pharmaceutical ingredients (APIs) and their metabolites in tap, surface, wastewater treatment plant (WWTP) influent and WWTP effluent water collected globally. A 7-day simulated shipping and sample stability assessment was undertaken demonstrating no significant degradation over the 1–3 days which is typical for global express shipping. Linearity (r²) was consistently ≥0.93 (median = 0.99 ± 0.02), relative standard deviation of intra- and inter-day repeatability and precision was <20% for 75% and 68% of the determinations made at three concentrations, respectively, and recovery from Liquid Chromatography Mass Spectrometry grade water, tap water, surface water and WWTP effluent were within an acceptable range of 60–130% for 87%, 76%, 77% and 63% of determination made at three concentrations respectively. Limits of detection and quantification were determined in all validated matrices and were consistently in the ng/L level needed for environmentally relevant API research. Independent validation of method results was obtained via an interlaboratory comparison of three surface-water samples and one WWTP effluent sample collected in North Liberty, Iowa (USA). Samples used for the interlaboratory validation were analysed at the University of York Centre of Excellence in Mass Spectrometry (York, UK) and the U.S. Geological Survey National Water Quality Laboratory in Denver (Colorado, USA). These results document the robustness of using this method on a global scale. Such application of this method would essentially eliminate the interlaboratory analytical variability typical of such large-scale datasets where multiple methods were used. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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10 pages, 1722 KiB

Open AccessArticle

Biodegradation of Picolinic Acid by Rhodococcus sp. PA18

by Yanting Zhang, Junbin Ji, Siqiong Xu, Hongmei Wang, Biao Shen, Jian He, Jiguo Qiu and Qing Chen

Appl. Sci. 2019, 9(5), 1006; https://doi.org/10.3390/app9051006 - 11 Mar 2019

Cited by 5 | Viewed by 3245

Abstract

Picolinic acid (PA), a C2-carboxylated pyridine derivative, is a significant intermediate used in industrial production. PA is considered hazardous for the environment and human health. In this study, a Gram-positive bacterium, Rhodococcus sp. PA18, which aerobically utilizes PA as a source of carbon and energy, was isolated. The strain completely degraded 100 mg/L PA within 24 h after induction and formed 6-hydroxypicolinic acid (6HPA), a major PA metabolite, which was identified using ultraviolet-visible spectroscopy, high performance liquid chromatography, and liquid chromatography/time of flight-mass spectrometry analyses. The cell-free extracts converted the PA into 6HPA when phenazine methosulfate was used as an electron acceptor. To our knowledge, this is the first report showing that PA can be metabolized by Rhodococcus. In conclusion, Rhodococcus sp. PA18 may be potentially used for the bioremediation of environments polluted with PA. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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12 pages, 1144 KiB

Open AccessArticle

Ultrafiltration/Granulated Active Carbon-Biofilter: Efficient Removal of a Broad Range of Micropollutants

by Christian Baresel, Mila Harding and Johan Fång

Appl. Sci. 2019, 9(4), 710; https://doi.org/10.3390/app9040710 - 18 Feb 2019

Cited by 46 | Viewed by 7738

Abstract

Pharmaceutical residues, and other organic micropollutants that pass naturally through the human body into sewage, are in many cases unaffected by treatment processes at conventional wastewater treatment plants (WWTPs). Accumulated in the environment, however, they can significantly affect aquatic ecosystems. The present study provides an evaluation of a treatment system for the removal of pharmaceutical residues and other micropollutants. The system is based on a Membrane Bioreactor (MBR), including ultrafiltration (UF), followed by a biofilter using granulated active carbon (GAC) as filter material. It was found that all investigated micropollutants, such as pharmaceutical residues, phenolic compounds, bacteria and microplastic particles, present in wastewater, could be removed by the treatment system to below detection limits or very low concentrations. This shows that the combination of filtration, adsorption and biodegradation provides a broad and efficient removal of micropollutants and effects. The tested treatment configuration appears to be one of the most sustainable solutions that meets today’s and future municipal sewage treatment requirements. The treatment system delivers higher resource utilization and security than other advanced treatment systems including solely GAC-filters without biology. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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15 pages, 821 KiB

Open AccessArticle

Quantitative Occurrence of Antibiotic Resistance Genes among Bacterial Populations from Wastewater Treatment Plants Using Activated Sludge

by Adriana Osińska, Ewa Korzeniewska, Monika Harnisz and Sebastian Niestępski

Appl. Sci. 2019, 9(3), 387; https://doi.org/10.3390/app9030387 - 23 Jan 2019

Cited by 41 | Viewed by 4253

Abstract

Wastewater treatment plants (WWTPs) are an important reservoir in the development of drug resistance phenomenon and they provide a potential route of antibiotic resistance gene (ARGs) dissemination in the environment. The aim of this study was to assess the role of WWTPs in the spread of ARGs. Untreated and treated wastewater samples that were collected from thirteen Polish WWTPs (applying four different modifications of activated sludge–based treatment technology) were analyzed. The quantitative occurrence of genes responsible for the resistance to beta-lactams and tetracyclines was determined using the real-time PCR method. Such genes in the DNA of both the total bacterial population and of the E. coli population were analyzed. Among the tested genes that are responsible for the resistance to beta-lactams and tetracyclines, bla_OXA and bla_TEM and tetA were dominant, respectively. This study found an insufficient reduction in the quantity of the genes that are responsible for antibiotic resistance in wastewater treatment processes. The results emphasize the need to monitor the presence of genes determining antibiotic resistance in the wastewater that is discharged from treatment plants, as they can help to identify the hazard that treated wastewater poses to public health. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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14 pages, 15867 KiB

Open AccessArticle

Chitosan Microbeads as Supporter for Pseudomonas putida with Surface Displayed Laccases for Decolorization of Synthetic Dyes

by Zhiqiang Bai, Xiaowen Sun, Xun Yu and Lin Li

Appl. Sci. 2019, 9(1), 138; https://doi.org/10.3390/app9010138 - 03 Jan 2019

Cited by 3 | Viewed by 3204

Abstract

Various untreated wastewaters contaminated with industrial dyes pose significant pollution hazards to the natural environment as well as serious risks to public health. The current study reports a new material with a configurative chitosan matrix and engineered Pseudomonas putida cells with surface-displayed laccases that can decolorize five industrial dyes. Through a self-configuring device, five chitosan microbeads (CTS-MBs) with different particle sizes were prepared. P. putida cells were then immobilized onto the CTS-MBs under optimized immobilization conditions, forming a degrading-biosorbent dual-function decolorization complex. Scanning electron microscope and infrared analysis confirmed the successful immobilization of the cells onto the CTS-MB matrix. The optimized CTS-MB1 with surface-grafted aldehyde groups (aCTS-MB1) complex was capable of decolorizing Acid Green 25 and Acid Red 18 over a pH range of 2.5–8.5 and a relatively broad temperature range of 15–85 °C, with a maximum relative decolorization value of over 94%; the complex was also able to efficiently decolorize Direct Red 243, Reactive Blue 220 and Reactive Blue 198. Moreover, the aCTS-MB1 composite showed favorable activity in continuous and regenerative decolorization reactions. Therefore, the chitosan-immobilized decolorizing material, with both improved mechanical strength and performance, shows potential for further large-scale or continuous processes. Full article

(This article belongs to the Special Issue Environmental Fate of Emerging Organic Micro-Contaminants)

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