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Noncovalent interactions between fluoroquinolone antibiotics with dissolved organic matter: A 1H NMR binding site study and multi-spectroscopic methods
2019
Zhao, Xiating | Hu, Zhongzheng | Yang, Xing | Cai, Xuewei | Wang, Zhaowei | Xie, Xiaoyun
Fluoroquinolone antibiotics (FQs) are considered to be emerging environmental contaminants that have been detected extensively in aquatic environment. It is of quite importance to explore FQs interacting with dissolved organic matter (DOM). The interactions of FQs with DOM were examined by nuclear magnetic resonance (NMR) spectroscopy, fluorescence quenching, UV–vis, Fourier transform infrared (FT-IR) spectroscopic techniques. The bindings of FQs to DOM had one single binding site and their quenching mechanisms were static, which were evaluated by the Stern-Volmer and Site-binding equations. Addition of DOM could result in micro-environmental changes of fluorophores groups in FQs. The location adjacent oxygen right of Ofloxacin (OFL) and the aromatic ring (the adjacency replaced by two nitrogen-containing groups) of Ciprofloxacin (CIP), Enrofloxacin (ENR), Norfloxacin (NOR) might be highly affected by DOM molecule. The negative enthalpy change (ΔH⁰), negative entropy change (ΔS⁰) and the positive Gibbs' energy change (ΔG⁰) figured out that the binding processes were exothermic but not thermodynamic favorable, the formation of HA-FQs complexes would be powered chiefly by the ΔS⁰. H-bonding, electrostatic effect, van der Waals force were the acting force in the binding reactions and the π-π stacking effect was the major binding force under alkaline conditions. Moreover, the protonated, deprotonated, or partially protonated state of FQs were found to have different binding capacity to DOM, and the binding reactions for FQs-HA system were suppressed as the ionic strength increased. Meanwhile, alterations of FQs conformation in the presence of DOM were evaluated by FT-IR and UV–vis spectra.
Show more [+] Less [-]The final discharge: Quantifying contaminants in embalming process effluents discharged to sewers in ontario, Canada
2019
Kleywegt, Sonya | Payne, Mark | Raby, Melanie | Filippi, Daniel | Ng, Chi-Fai | Fletcher, Tim
The process of embalming human remains as part of the funeral home industry, entails replacing blood with embalming fluid. Typically the unused/excess fluids are disposed of directly to the sewershed or septic system. The presence of select contaminants in sewer discharges from 8 funeral homes (facilities) in York Region, Ontario during active embalming processes was studied. A wide range of contaminants including embalming fluids (formaldehyde and triclosan); metals, conventional parameters, persistent organic pollutants (polycyclic aromatic hydrocarbons, pesticides, and polychlorinated byphenyls), nonyl phenols and active pharmaceutical ingredients (APIs) were measured in the final embalming effluent and compared to regulatory sewer limits where available. Two main constituents of embalming fluids—formaldehyde and triclosan—were detected at maximum concentrations of 561,000 μg/L and 505 μg/L respectively. Other persistent organic pollutants detected in embalming effluent included banned pesticides lindane (83 ng/L) and metabolites of DDT (DDE; 2,300 ng/L). Elevated APIs found in over-the-counter drugs and products were also frequently detected at elevated concentrations (oxybenzone, hydrocortisone, lidocaine, naproxen, ibuprofen, ciprofloxacin and DEET). Most contaminants did not exceed regulatory sewer limits where available, however others including biochemical oxygen demand (cBOD5) and conventional parameters were consistently above regulatory limits. Large amounts of formaldehyde and triclosan may pose a risk to receiving sewersheds and receiving sewage treatment plants due to their antimicrobial activities.
Show more [+] Less [-]Enrofloxacin and Roundup® interactive effects on the aquatic macrophyte Elodea canadensis physiology
2019
Gomes, Marcelo Pedrosa | Tavares, Davi Santos | Richardi, Vinícius Sobrinho | Marques, Raizza Zorman | Wistuba, Natalia | Moreira de Brito, Júlio César | Soffiatti, Patrícia | Sant’Anna-Santos, Bruno Francisco | Navarro da Silva, Mário Antônio | Juneau, Philippe
The co-occurrence of aquatic contaminants, such as antibiotics and herbicides, has motivated investigations into their interactive effects on aquatic organisms. We examined the combined effects of environmental concentrations of the antibiotic Enrofloxacin (Enro; 0–2.25 μg l−1) and Roundup OriginalDI (Roundup®; 0–0.75 μg active ingredient l−1), a glyphosate based-herbicide, on Elodea canadensis. Enro alone was not toxic, but the plants were highly sensitive to Roundup® whose toxicity is related to the induction of oxidative stress. The metabolism of Enro by plants into Ciprofloxacin (Cipro) was observed, and although former is not phytotoxic, oxidative events associated with Cipro generation were observed. The activity of cytochrome P450 was shown to be involved in Enro degradation in E. canadensis. As a cytochrome P450 inhibitor, Roundup® decreases Enro metabolism in plants. Enro, in turn, increases glyphosate uptake and toxicity, so that Enro and Roundup® have synergistic effects, disrupting the physiological processes of E. canadensis. Our results suggest E. canadensis as a potential candidate for the reclamation of Enro in contaminated waters, but not for Roundup® due to its high sensitivity to that herbicide.
Show more [+] Less [-]The cardiovascular toxicity induced by high doses of gatifloxacin and ciprofloxacin in zebrafish
2019
Shen, Rong | Yu, Yichang | Lan, Rong | Yu, Ran | Yuan, Ze | Xia, Zhining
As a new type of pollutant, fluoroquinolones (FQs) antibiotics are ubiquitous in environment and have some threat to human health and ecological environment. Their ecological toxicity to the environment urgently need to be assessed. Therefore, we firstly explored the toxic effects and possible mechanism of cardiovascular toxicity induced by gatifloxacin (GTFX) and ciprofloxacin (CPFX) using zebrafish model. After 24 h exposure, the zebrafish treated with GTFX showed pericardial edema which was further investigated by histopathological examination, while CPFX exposure did not induce morphological abnormalities. However, both of them induced cardiac dysfunction, such as decreased heart rate and cardiac output which was showed a positive correlation with the concentration. To better understand the possible molecular mechanisms underlying cardiovascular toxicity in zebrafish, we investigated the transcriptional level of genes related to calcium signaling pathway and cardiac muscle contraction. The results indicated that the expression of ATPase (atp2a1l) and cardiac troponin C (tnnc1a) genes were significantly inhibited, the expression of calcium channel (cacna1ab) gene showed slight promoted trend after CPFX exposure. For zebrafish treated with GTFX, the expression of atp2a1l genes was also significantly inhibited, while the expression of tnnc1a genes was slightly inhibited and cacna1ab genes expression had no obvious effect. The present study firstly revealed that GTFX exposure can induce morphological and functional abnormalities on the cardiovascular system of zebrafish. Though CPFX exposure did not induce morphological abnormalities, the function of cardiovascular system was still damaged. Mechanistically, this toxicity might result from the pressure of down-regulation of genes associated with calcium signaling pathway and cardiac muscle contraction. The results of this study can provide a valuable theoretical basis for the establishment of FQs environmental quality standards in water environment, environmental drug regulation and risk management.
Show more [+] Less [-]Persistence and migration of tetracycline, sulfonamide, fluoroquinolone, and macrolide antibiotics in streams using a simulated hydrodynamic system
2019
Liu, Xiaowei | Lv, Kai | Deng, Chengxun | Yu, Zhimin | Shi, Jianghong | Johnson, Andrew C.
The potential persistence and migration of 14 antibiotics comprising sulfonamides, fluoroquinolones, macrolides and tetracyclines were conducted using a 50-d recirculating flume study supported by batch attenuation experiments with spiked concentrations. The study demonstrated that photodegradation was the dominant attenuation process for these antibiotics in the water environment. The half-lives of 2–26 d were in order of sulfadiazine > sulfadimethoxine > sulfamerazine > sulfamethoxazole > sulfamethazine > sulfathiazole > ofloxacin > enrofloxacin > norfloxacin > ciprofloxacin > erythromycin > tetracycline > roxithromycin > oxytetracycline. These modest half-lives meant that the antibiotics were predicted to travel 30–400 km down a typical river before half the concentration would be lost. All antibiotics were detected on the surface sediment in the flume study. Under hyporheic exchange, some of them continually migrated into the deeper sediment and also the sediment pore water. All fluoroquinolones were detected in the sediments. The sulfonamides were detected in the pore water with relatively high concentrations and frequencies. Sulfadiazine, sulfamethazine and sulfathiazole in the upper layer pore water were found to be approaching equilibrium with the surface water. The high presence of sulfonamides in the pore water indicated that their high mobility and persistence potentially pose a risk to hyporheic zone.
Show more [+] Less [-]Occurrence and risk assessment of antibiotics in the Xi'an section of the Weihe River, northwestern China
2019
Wang, Jiawei | Wei, Hong | Zhou, Xiaode | Li, Kebin | Wu, Wei | Guo, Mengjing
Fifteen antibiotics, including seven sulfonamides (SAs); three macrolides (MLs); three quinolones (QNs); one lincosamide, lincomycin (LIN); and one tetracycline (TC), were detected in the surface water of the Xi'an section of the Weihe River by using high-performance liquid chromatography-mass spectrometry (HPLC-MS/MS). The detection rates were 12.50–100%, and the detected concentrations were in the range of nd-270.60 ng/L. The average detected concentrations of the SAs, MLs, QNs, LIN and TC were 113.68, 111.79, 20.55, 23.81 and 25.66 ng/L, respectively. Among these, SAs and MLs were the dominant antibiotics detected in the Weihe River. Compared with those in other water bodies in China and abroad, the antibiotic residues in the Weihe River were at a moderate contamination level. The SAs concentration distribution followed upstream > midstream > downstream, while the MLs concentration distribution was midstream < downstream < upstream. The correlation analysis and principal component analysis (PCA) indicated that domestic sewage, livestock discharge, and aquaculture and pharmaceutical wastewater are the main sources of antibiotic residues in the Weihe River. In addition, the detected ciprofloxacin (CFX), ofloxacin (OFX) and sulfamethoxazole (SMX) pose high ecological risk in the short and long term.
Show more [+] Less [-]Kinetic, equilibrium, and thermodynamic studies on the adsorption of ciprofloxacin by activated carbon produced from Jerivá (Syagrus romanzoffiana)
2019
de Oliveira Carvalho, Caroline | Costa Rodrigues, Daniel Lucas | Lima, Éder Cláudio | Santanna Umpierres, Cibele | Caicedo Chaguezac, Diana Fernanda | Machado Machado, Fernando
High specific surface area activated carbon prepared from endocarp of Jerivá (Syagrus romanzoffiana) (ACJ) was used for ciprofloxacin (CIP) antibiotic removal from aqueous effluents. The activated carbon (AC) was characterized via scanning electron microscope, Fourier transform infrared spectroscopy, N₂ adsorption/desorption, and pH value at the zero-charge point. Avrami kinetic model was the one that best fit the experimental results in comparison to the pseudo-first-order and pseudo-second-order kinetic models. The equilibrium data obeyed the Liu isotherm equation, showing a maximum adsorption capacity of 335.8 mg g⁻¹ at 40 °C. The calculated thermodynamic parameters indicate that the adsorption of CIP was spontaneous and endothermic at all studied temperatures. Also, the free enthalpy changes (∆H° = 3.34 kJ mol⁻¹) suggested physical adsorption between CIP and ACJ. Simulated effluents were utilized to check the potential of the ACJ for wastewater purification. The highly efficient features enable the activated carbon prepared from endocarp of Jerivá, an attractive carbon adsorbent, to remove ciprofloxacin from wastewaters.
Show more [+] Less [-]Electrochemical degradation of ciprofloxacin on BDD anode using a differential column batch reactor: mechanisms, kinetics and pathways
2019
Li, Guangchao | Zhou, Shiqing | Shi, Zhou | Meng, Xiaoyang | Li, Ling | Liu, Bin
A growing number of electrochemical oxidation system was employed for the degradation of refractory contaminants. In this study, a boron-doped diamond (BDD) anode/Ti cathode equipped in the differential column batch reactor (DCBR) was utilized for electrochemical oxidation of ciprofloxacin (CIP). The feed solution within the DCBR system was confirmed as a uniform flow state through a computational fluid dynamics (CFD) simulation analysis. The results showed that the BDD anode/Ti cathode electrochemical system was with a high efficiency oxidation performance when treating the CIP contaminant. The CIP was completely degraded within 20 min, and over 50% DOC removed after 120 min. Therefore, two-stage electrochemical oxidation mechanism was proposed. Four major factors, the initial concentration, current density, pH, and electrolyte concentration, on the CIP degradation efficiency were systematically investigated. The CIP degradation curve followed pseudo first-order degradation kinetics. The electric efficiency per order (EE/O) of the electrochemical oxidation system was calculated to determine an optimal operation condition. Moreover, the oxidation intermediates were identified with a mass spectrometry (LC/MS/MS) and the degradation pathways were proposed in this study. The destruction of quinolone moiety and piperazine ring and fluorine substitution were the three possible degradation pathways during BDD anode oxidation process.
Show more [+] Less [-]A Comparative Adsorption Study with Various Adsorbents for the Removal of Ciprofloxacin Hydrochloride from Water
2019
Avcı, Ayça | İnci, İsmail | Baylan, Nilay
In this study, the removal of ciprofloxacin hydrochloride (a fluoroquinolone antibiotic) by using various effective adsorbents such as activated carbon, montmorillonite, modified montmorillonite (commercial name Cloisite 20A), and alumina was investigated. Adsorption experiments were performed to determine and compare the adsorption capacities of these adsorbents. The adsorption capacities of adsorbents were examined at different initial concentrations of ciprofloxacin hydrochloride. Activated carbon was found to be having the best adsorption capacity for the removal of ciprofloxacin hydrochloride. For the solution having an initial ciprofloxacin hydrochloride concentration of 4 ppm, the adsorption capacities of adsorbents were obtained as 1.86 mg g⁻¹ for activated carbon, 1.67 mg g⁻¹ for modified montmorillonite, 1.15 mg g⁻¹ for alumina, and 0.60 mg g⁻¹ for montmorillonite. And also, about 92% of the ciprofloxacin hydrochloride was removed from the water using the activated carbon. In addition, Langmuir, Freundlich, and Temkin isotherm models were employed to express the adsorption process. For all adsorbents, Freundlich isotherm model provided best fitting to the experimental data because of very high values of R² (> 0.99). Kinetic models of pseudo-first order, pseudo-second order, Elovich, and Weber-Morris intraparticle diffusion model were utilized to evaluate the experimental adsorption data. Adsorption kinetics data were well represented by pseudo-second order kinetic model with values of R² (> 0.999).
Show more [+] Less [-]Ecotoxicological effects and accumulation of ciprofloxacin in Eichhornia crassipes under hydroponic conditions
2019
Yan, Yan | Xu, Xiaoguang | Shi, Chenfei | Yan, Wang | Zhang, Limin | Wang, Guoxiang
Antibiotic residues pose a threat to the health of aquatic organisms. The effects and accumulation of antibiotic ciprofloxacin (CIP) in a floating macrophyte (Eichhornia crassipes) under hydroponic conditions were investigated. It was found that E. crassipes exposure to CIP (< 1000 μg L⁻¹) could maintain a stable photosynthesis efficiency. In response to CIP stress, catalase and peroxidase activities of leaves were 7.24–37.51 nmol min⁻¹ g⁻¹ and 98.46–173.16 U g⁻¹, respectively. The presence of CIP did not inhibit the growth of the plant. After 14 days of exposure, tender leaves became white and withered, ascribed to the decline of chlorophyll content and chlorophyll fluorescence parameters. The CIP concentrations, absorbed by E. crassipes, were highest in the roots, followed by white aerial parts and green aerial parts at CIP concentrations of 100 and 1000 μg L⁻¹. These findings demonstrated that E. crassipes could absorb and tolerate CIP in a limited time-scale and imply an alternative solution for phytoremediation in water bodies contaminated with antibiotics.
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