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Integration of biochar into Ag3PO4/α-Fe2O3 heterojunction for enhanced reactive oxygen species generation towards organic pollutants removal
2022
Qian, Yifan | Shi, Jun | Yang, Xianni | Yuan, Yangfan | Liu, Li | Zhou, Ganghua | Yi, Jianjian | Wang, Xiaozhi | Wang, Shengsen
A biochar (BC) harbored Ag₃PO₄/α-Fe₂O₃ type-Ⅰ heterojunction (Ag-Fe-BC) was prepared by a hydrothermal-impregnation method to transfer active center of heterojunctions. The electrochemical and spectroscopic tests demonstrated that BC enhanced the catalytic performance of the heterojunction by enhancing photocurrent, reducing fluorescence intensity, and facilitating separation of electron-hole pairs. The photocatalytic activity showed the Ag-Fe-BC (5:1:3) could degrade Rhodamine B (20 mg/L) by up to 92.7%, which was 3.35 times higher than Ag₃PO₄/α-Fe₂O₃. Tetracycline and ciprofloxacin (20 mg/L) were degraded efficiently by 58.3% and 79.4% within 2 h, respectively. Electron paramagnetic resonance and scavenging experiments confirmed the major reactive oxygen species (ROS) consisted of singlet oxygen (¹O₂) and superoxide (·O₂⁻). Excellent RhB adsorption and electrons capturing capacity of BC facilitated electron-hole pairs separation and ROS transferring to target organics followed by elevated degradation. Thus, a facile method was proposed to synthesize a highly efficient visible-light responsive photocatalyst for degradation of various organics in water.
Show more [+] Less [-]Effect of fulvic acid concentration levels on the cleavage of piperazinyl and defluorination of ciprofloxacin photodegradation in ice
2022
Li, Zhuojuan | Dong, Deming | Zhang, Liwen | Li, Yanchun | Guo, Zhiyong
Ice is an important physical and chemical sink for various pollutants in cold regions. The photodegradation of emerging fluoroquinolone (FQ) antibiotic contaminants with dissolved organic matter (DOM) in ice remains poorly understood. Here, the photodegradation of ciprofloxacin (CIP) and fulvic acid (FA) in different proportions as representative FQ and DOM in ice were investigated. Results suggested that the photodegradation rate constant of CIP in ice was 1.9 times higher than that in water. When CFA/CCIP ≤ 60, promotion was caused by FA sensitization. FA increased the formation rate of cleavage in the piperazine ring and defluorination products. When 60 < CFA/CCIP < 650, the effect of FA on CIP changed from promoting to inhibiting. When 650 ≤ CFA/CCIP ≤ 2600, inhibition was caused by both quenching effects of 143.9%–51.3% and light screening effects of 0%–48.7%. FA inhibited cleavage in the piperazine ring for CIP by the scavenging reaction intermediate of aniline radical cation in ice. When CFA/CCIP > 2600, the light screening effect was greater than the quenching effect. This work provides new insights into how DOM affects the FQ photodegradation with different concentration proportions, which is beneficial for understanding the environmental behaviors of fluorinated pharmaceuticals in cold regions.
Show more [+] Less [-]Quinolone distribution, trophodynamics, and human exposure risk in a transit-station lake for water diversion in east China
2022
Liu, Yuanyuan | Hua, Zulin | Lü, Ying | Gu, Li | Luan, Chengmei | Li, Xiaoqing | Wu, Jianyi | Chu, Kejian
Quinolone antibiotics (QNs) pollution in lake environments is increasingly raising public concern due to their potential combined toxicity and associated risks. However, the spatiotemporal distribution and trophodynamics of QNs in transit-station lakes for water diversion are not well documented or understood. In this study, a comprehensive investigation of QNs in water, sediment, and aquatic fauna, including norfloxacin (NOR), ciprofloxacin (CIP), enrofloxacin (ENR), and ofloxacin (OFL), was conducted in Luoma Lake, a major transit station for the eastern route of the South-to-North Water Diversion Project in China. The target QNs were widely distributed in the water (∑QNs: 70.12 ± 62.79 ng/L) and sediment samples (∑QNs: 13.35 ± 10.78 ng/g dw) in both the non-diversion period (NDP) and the diversion period (DP), where NOR and ENR were predominant. All the QNs were detected in all biotic samples in DP (∑QNs: 80.04 ± 20.59 ng/g dw). The concentration of ∑QNs in the water in NDP was significantly higher than those in DP, whereas the concentration in the sediments in NDP was comparable to those in DP. ∑QNs in the water-sediment system exhibited decreasing trends from northwest (NW) to southeast (SE) in both periods; however, the Kₒc (organic carbon normalized partition coefficients) of individual QNs in DP sharply rose compared with those in NDP, which indicated that water diversion would alter the environmental fate of QNs in Luoma Lake. In DP, all QNs, excluding NOR, were all biodiluted across the food web; whereas their bioaccumulation potentials in the SE subregion were higher than those in the NW subregion, which was in contrast to the spatial distribution of their exposure concentrations. The estimated daily QN intakes via drinking water and aquatic products suggested that residents in the SE side were exposed to greater health risks, despite less aquatic pollution in the region.
Show more [+] Less [-]Distribution of antibiotics in water, sediments and biofilm in an urban river (Córdoba, Argentina, LA)
2021
Valdés, M Eugenia | Santos, Lúcia H.M.L.M. | Rodríguez Castro, M Carolina | Giorgi, Adonis | Barceló, Damià | Rodríguez-Mozaz, Sara | Amé, M Valeria
In this study, we evaluated the distribution of up to forty-three antibiotics and 4 metabolites residues in different environmental compartments of an urban river receiving both diffuse and point sources of pollution. This is the first study to assess the fate of different antibiotic families in water, biofilms and sediments simultaneously under a real urban river scenario. Solid phase extraction, bead-beating disruption and pressurized liquid extraction were applied for sample preparation of water, biofilm and sediment respectively, followed by the quantification of target antibiotics by UPLC-ESI-MS/MS. Twelve antibiotics belonging to eight chemical families were detected in Suquía River samples (67% positive samples). Sites downstream the WWTP discharge were the most polluted ones. Concentrations of positive samples ranged 0.003-0.29 µg L⁻¹ in water (max. cephalexin), 2-652 µg kg⁻¹d.w. in biofilm (max. ciprofloxacin) and 2-34 µg kg⁻¹d.w. in sediment (max. ofloxacin). Fluoroquinolones, macrolides and trimethoprim were the most frequently detected antibiotics in the three compartments. However cephalexin was the prevalent antibiotic in water. Antibiotics exhibited preference for their accumulation from water into biofilms rather than in sediments (bioaccumulation factors > 1,000 L kg⁻¹d.w. in biofilms, while pseudo-partition coefficients in sediments < 1,000 L kg⁻¹d.w.). Downstream the WWTP there was an association of antibiotics levels in biofilms with ash-free dry weight, opposite to chlorophyll-a (indicative of heterotrophic communities). Cephalexin and clarithromycin in river water were found to pose high risk for the aquatic ecosystem, while ciprofloxacin presented high risk for development of antimicrobial resistance. This study contributes to the understanding of the fate and distribution of antibiotic pollution in urban rivers, reveals biofilm accumulation as an important environmental fate, and calls for attention to government authorities to manage identified highly risk antibiotics.
Show more [+] Less [-]Pentachlorophenol and ciprofloxacin present dissimilar joint toxicities with carbon nanotubes to Bacillus subtilis
2021
Deng, Rui | Yang, Kun | Lin, Daohui
Discharged carbon nanotubes (CNTs) likely interact with co-existing organic contaminants (OCs) and pose joint toxicity to environmental microbes. Herein, hydrophobic pentachlorophenol (PCP) and hydrophilic ciprofloxacin (CIP) were used as representative OCs and their joint toxicities with CNTs to Bacillus subtilis were systematically investigated at cellular, biochemical, and omics levels. The 3-h bacterial growth half inhibitory concentrations of CNTs, PCP, and CIP were 12.5 ± 2.6, 3.5 ± 0.5, and 0.46 ± 0.03 mg/L, respectively, and they all could damage cell membrane, increase intracellular oxidative stress, and alter bacterial metabolomics and transcriptomics; while CNTs-PCP and CNTs-CIP binary exposures exhibited distinct additive and synergistic toxicities, respectively. CNTs increased bacterial bioaccumulation of PCP and CIP via destabilizing and damaging cell membrane. PCP reduced the bioaccumulation of CNTs, while CIP had no significant effect; this difference could be owing to the different effects of the two OCs on cell-surface hydrophobicity and CNTs electronegativity. The additive toxicity outcome upon CNTs-PCP co-exposure could be a result of the balance between the increased toxicity from increased PCP bioaccumulation and the decreased toxicity from decreased CNTs bioaccumulation. The increased bioaccumulation of CIP contributed to the synergistic toxicity upon CNTs-CIP co-exposure, as confirmed by the increased inhibition of topoisomerase Ⅳ activity and interference in gene expressions regulating ABC transporters and lysine biosynthesis. The findings provide novel insights into environmental risks of CNTs.
Show more [+] Less [-]Antibiotic-accelerated cyanobacterial growth and aquatic community succession towards the formation of cyanobacterial bloom in eutrophic lake water
2021
Xu, Sijia | Jiang, Yunhan | Liu, Ying | Zhang, Jian
Antibiotics can stimulate the growth of model cyanobacterial species under pure culture conditions, but their influence on cyanobacterial blooms in natural aquatic ecosystems remains unclear. In this study, three commonly detected antibiotics (sulfamethoxazole, tetracycline, and ciprofloxacin) and their ternary mixture were proved to selectively stimulate (p < 0.05) the growth and photosynthetic activity of cyanobacteria in an aquatic microcosm at an environmentally relevant exposure dose of 300 ng/L under both oligotrophic and eutrophic conditions. Under the eutrophic condition, cyanobacteria reached a bloom density of 1.61 × 10⁶ cells/mL in 15 days without antibiotics, while the cyanobacteria exposed to tetracycline, sulfamethoxazole, ciprofloxacin, and their ternary mixture exceeded this bloom density within only 10, 8, 7, and 6 days, respectively. Principal coordinate analysis indicated that the antibiotic contaminants accelerated the prokaryotic community succession towards the formation of a cyanobacterial bloom by promoting the dominance of Microcystis, Synechococcus, and Oscillatoria under the eutrophic condition. After 15 days of culture, the antibiotic exposure increased the density of cyanobacteria by 1.38–2.31-fold and 2.28–3.94-fold under eutrophic and oligotrophic conditions, respectively. Antibiotic exposure generated higher stimulatory effects on cyanobacterial growth under the oligotrophic condition, but the antibiotic(s)-treated cyanobacteria did not form a bloom due to nutrient limitation. Redundancy analysis indicated that the three target antibiotics and their ternary mixture affected the prokaryotic community structure in a similar manner, while tetracycline showed some differences compared to sulfamethoxazole, ciprofloxacin, and the ternary antibiotic mixture with regard to the regulation of the eukaryotic community structure. This study demonstrates that antibiotic contaminants accelerate the formation of cyanobacterial blooms in eutrophic lake water and provides insights into the ecological effects of antibiotics on aquatic microbial communities.
Show more [+] Less [-]Combining an effect-based methodology with chemical analysis for antibiotics determination in wastewater and receiving freshwater and marine environment
2021
Serra-Compte, Albert | Pikkemaat, Mariël G. | Elferink, Alexander | Almeida, David | Diogène, Jorge | Campillo, Juan Antonio | Llorca, Marta | Álvarez-Muñoz, Diana | Barceló, Damià | Rodríguez-Mozaz, Sara
Two different methodologies were combined to evaluate the risks that antibiotics can pose in the environment; i) an effect-based methodology based on microbial growth inhibition and ii) an analytical method based on liquid-chromatography coupled to mass spectrometry (LC-MS). The first approach was adapted and validated for the screening of four antibiotic families, specifically macrolides/β-lactams, quinolones, sulfonamides and tetracyclines. The LC-MS method was applied for the identification and quantification of target antibiotics; then, the obtained results were combined with ecotoxicological data from literature to determine the environmental risk. The two methodologies were used for the analysis of antibiotics in water samples (wastewater, river water and seawater) and biofluids (fish plasma and mollusk hemolymph) in two monitoring campaigns undertaken in the Ebro Delta and Mar Menor Lagoon (both in the Mediterranean coast of Spain). Both approaches highlighted macrolides (azithromycin) and quinolones (ciprofloxacin and ofloxacin) as the main antibiotics in wastewater treatment plant (WWTP) effluents with potential risk for the environment. However, no risk for the aquatic life was identified in the river, lagoon and seawater as antibiotic levels were much lower than those in WWTP effluents. Fish from Ebro River were the organisms presenting the highest antibiotic concentration when compared with bivalves (mussels) from the Mediterranean Sea and gastropods (marine snails) from the Mar Menor Lagoon. The effect-based methodology successfully determined antibiotic risk in wastewater, but its applicability was less clear in environmental waters such as seawater, due to its high detection limits. Improving sample preconcentration could increase the method sensibility. Overall, combination of both methodologies provides comprehensive insights in antibiotic occurrence and risk associated in areas under study.
Show more [+] Less [-]Benzalkonium chloride alters phenotypic and genotypic antibiotic resistance profiles in a source water used for drinking water treatment
2020
Harrison, Katherine R. | Kappell, Anthony D. | McNamara, Patrick J.
Antibiotic resistance is a major public health concern. Triclosan is an antimicrobial compound with direct links to antibiotic resistance that was widely used in soaps in the U.S. until its ban by the U.S. Food and Drug Administration. Benzalkonium chloride (BAC), a quaternary ammonium compound, has widely replaced triclosan in soaps marketed as an antibacterial. BAC has been detected in surface waters and its presence will likely increase following increased use in soap products. The objective of this study was to determine the effect of BAC on relative abundance of antibiotic resistance in a bacterial community from a surface water used as a source for drinking water treatment. Bench-scale microcosm experiments were conducted with microbial communities amended with BAC at concentrations ranging from 0.1 μg L⁻¹ to 500 μg L⁻¹. Phenotypic antibiotic resistance was quantified by culturing bacteria in the presence of different antibiotics, and genotypic resistance was determined using qPCR to quantify antibiotic resistance genes (ARGs). BAC at concentrations ranging from 0.1 μg L⁻¹ to 500 μg L⁻¹ was found to positively select for bacteria resistant to ciprofloxacin and sulfamethoxazole, and negatively select against bacteria with resistance to six other antibiotics. Exposure to BAC for 14 days increased the relative abundance of sul1 and blaTEM. This study re-highlights the importance of employing both culture and non-culture-based techniques to identify selection for antibiotic resistance. The widespread use of BAC will likely impact antibiotic resistance profiles of bacteria in the environment, including in source waters used for drinking water, wastewater treatment plants, and natural waterways.
Show more [+] Less [-]Antimicrobial resistance in freshwater Plesiomonas shigelloides isolates: Implications for environmental pollution and risk assessment
2020
Ekundayo, Temitope Cyrus | Okoh, Anthony I.
Antibiotic resistance is known to impact treatment efficiency of Plesiomonas infections negatively with fatal outcomes. This study investigated antibiogram fingerprint of P. shigelloides (n = 182) isolated from three South Africa rivers using the disc diffusion technique. Environmental pollution and analogous health risk (given infections) that could associate with the freshwaters and empirical treatment of Plesiomonas were assessed using Antibiotic Resistance Index (ARI) and Multiple Antibiotic Resistance Indices (MARI), respectively. Thirteen EUCAST recommended (ERAs) and eleven non-recommended antibiotics (NAs) used as first line agents in the treatment of gastroenteritis and extraintestinal infections were tested. Resistance against ERAs decreased from cefoxitin (37.91%), cefuroxime (35.17%), cefepime (31.87%), ceftriaxone (29.67%), ciprofloxacin (18.13%), trimethoprim-sulfamethoxazole (10.44%), piperacillin/tazobactam (8.79%), ertapenem (4.95%), norfloxacin (4.40%), levofloxacin (2.75%), meropenem (1.10%) to imipenem (0.55%). The isolates had higher resistance (≥36.07%) against NAs but were susceptible to amikacin (67.58%), gentamycin (73.08%), and tetracycline (80.77%). MARI of the isolates were significantly different between ERAs and NAs (P-value < 0.05) and had an average of 0.17 ± 0.18 and 0.45 ± 0.13, respectively. About 33.87% and 95.63% of the isolates had MARI value from 0.23 to 0.62 and 0.27–0.82 to ERAs and NAs, respectively. Also, ERAs-based and NAs-based ARI across sampling units showed significantly different (P-value < 0.05) means of 0.18 ± 0.09 and 0.46 ± 0.05, respectively. MARI attributed low risk of empirical treatment to recommended antibiotics but higher risk to non-recommended antibiotics. Model estimated successful and unsuccessful empirical treatment of infections risks due to resistance in the isolates using recommended antibiotics as 65.93% and 34.07%, respectively; 1.65% and 98.35% in the case of non-recommended antibiotics, respectively. ARI based on recommended antibiotics identified potential environmental pollutions in a number of sites. Resistance in freshwater P. shigelloides especially against cephalosporin, quinolones and fluoroquinolones is distressing and might suggests high pollution of the freshwaters in the Eastern Cape Province.
Show more [+] Less [-]Occurrence, distribution, and risk assessment of pharmerciuticals in wastewater and open surface drains of peri-urban areas: Case study of Juja town, Kenya
2020
Muriuki, Cecilia W. | Home, Patrick G. | Raude, James M. | Ngumba, Elijah K. | Munala, Gerryshom K. | Kairigo, Pius K. | Gachanja, Anthony N. | Tuhkanen, Tuula A.
The occurrence of Active Pharmaceutical Ingredients (APIs) in the environment is becoming a major area of concern due to their undesirable effects on non-target organisms. This study investigated the occurrence and risk of contamination by five antibiotics and three antiretrovirals drugs in a fast-growing peri-urban area in Kenya, with inadequate sewer system coverage. Due to poor sewage connectivity and poorly designed decentralized systems, wastewater is directly released in open drains. Water and sediment samples were collected from open surface water drains, while wastewater samples were collected from centralized wastewater treatment plants (WWTP). Solid-phase extraction and ultrasonic-assisted extraction for the aqueous and sediment samples respectively were carried out and extracts analyzed by liquid chromatography-electrospray ionization tandem mass spectrometry (LC-ESI-MS/MS) using isotopically labeled internal standards. APIs were observed with the detection frequency ranging from 36% to 100%. High mean concentrations of 48.7 μg L⁻¹, 108 μg L⁻¹, and 532 μg L⁻¹ were observed in surface drains for Lamivudine (3 TC), Sulfamethoxazole (SMX), Ciprofloxacin (CIP) respectively. Drain sediments also showed high concentrations of APIs ranging from 2.1 to 13,100 μg kg⁻¹. APIs in this study exceeded those observed in existing literature studies. JKUAT WWTP removal efficiencies varied from −90.68% to 72.67%. Total APIs emission load of the study area was 3550 mg d⁻¹ with WWTP effluent contributing higher loads (2620 mg d⁻¹) than surface water drains (640 mg d⁻¹). Zidovudine (ZDV), nevirapine (NVP), and trimethoprim (TMP) loads in drains, however, exceeded WWTP effluent. Low to high ecotoxicity risk of the individual APIs were observed to the aquatic environment, with high risks for the development of antibiotic resistance in microbiome as determined by the risk quotient (RQ) approach. Risk management through efficient wastewater collection, conveyance, and treatment is necessary to suppress the measured concentrations.
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