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Effects of natural dissolved organic matter on the complexation and biodegradation of 17α-ethinylestradiol in freshwater lakes
2019
Bai, Leilei | Zhang, Qi | Wang, Changhui | Yao, Xiaolong | Zhang, Hui | Jiang, Helong
Natural dissolved organic matter (DOM) produced in algal blooms and overgrowths of macrophyte changes the elimination and ecotoxicity of estrogens in freshwater lakes. The complexation of 17α-ethinylestradiol (EE2) and various DOMs, including the water- and sediment-derived DOMs from the algal-dominant zone in Lake Taihu (TW and TS, respectively) and the macrophyte-dominant zone in Poyang Lake (PW and PS, respectively), and the humic acid (HA), was investigated along with the subsequent effects on EE2 biodegradation. Dialysis equilibrium experiments showed that binding to DOM significantly decreased the freely soluble concentrations of EE2. The binding capacity of the five DOMs followed the order of PW < TW < PS ≈ TS < HA. A negative correlation was found between the organic-carbon-normalized sorption coefficient (logKDOC) and the absorption ratio (E₂/E₃) of DOM, indicating that the large sized, aromatic molecules were involved in the complexation. The reduced freely soluble concentrations of EE2 did not inhibit its biodegradation by an EE2-degrading strain, Rhodobacter blasticus. Conversely, the autochthonous-dominated water-derived DOMs stimulated a more extensive biodegradation of EE2 than the sediment-derived DOMs, and the existence of HA resulted in the smallest increase in EE2 biodegradation. The promoting effect was associated with the increased concentration, activity, and transforming rate of R. blasticus by the bioavailable components in DOM. The present study suggests that the significant impact of natural DOM should be fully considered when assessing the fate and ecological risks of estrogens in eutrophic waters.
Show more [+] Less [-]Characterization of interactions between a metabolic uncoupler O-chlorophenol and extracellular polymeric substances of activated sludge
2019
Fang, Fang | Xu, Run-Ze | Wang, Su-Na | Zhang, Lu-Lu | Huang, Yan-Qiu | Luo, Jing-Yang | Feng, Qian | Cao, Jia-Shun
Metabolic uncouplers are widely used for the in-situ reduction of excess sludge from activated sludge systems. However, the interaction mechanism between the metabolic uncouplers and extracellular polymeric substances (EPS) of activated sludge is unknown yet. In this study, the interactions between a typical metabolic uncoupler, o-chlorophenol (oCP), and the EPS extracted from activated sludge were explored using a suite of spectral methods. The binding constants calculated for the four peaks of three-dimensional excitation-emission matrix fluorescence were in a range of 1.24–1.76 × 10³ L/mol, implying that the tyrosine protein-like substances governed the oCP-EPS interactions. Furthermore, the results of Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and ¹H nuclear magnetic resonance indicated that the carboxyl, carbonyl, amine, and hydroxyl groups of EPS were the main functional groups involved in the formation of the oCP-EPS complex. The results of this study are useful for understanding the interactions between metabolic uncouplers and the EPS of activated sludge as well as their fates in biological wastewater treatment systems.
Show more [+] Less [-]Persistent halogenated organic pollutants in follicular fluid of women undergoing in vitro fertilization from China: Occurrence, congener profiles, and possible sources
2019
Huang, Yumei | Yan, Muting | Nie, Huayue | Wang, Wenjing | Wang, Jun
Analysis of persistent halogenated organic pollutants (HOPs) in human follicular fluid is important given previous reports of their adverse effects on the reproductivity of women. In the present work, HOPs, including polybrominated diphenyl ethers (PBDEs) and polychlorinated biphenyls (PCBs), were analyzed in 127 follicular fluid samples collected from patients who were undergoing in vitro fertilization in Central China. The concentrations of ∑₇BDEs (sum of BDE-28, -47, −99, −100, −153, −154, and −183) in follicular fluid ranged from not detected (n.d.) to 110 ng/g lipid weight (lw), with an average of 50 ± 24 ng/g lw. BDE-100 was suggested to be an indicator of BDE congeners in follicular fluid, with the highest concentrations and showing a significantly high correlation (p < 0.01) with ∑₇BDEs. Penta-BDE products were the principal source of PBDEs in follicular fluid samples. The concentrations of ∑₇CBs (CB-28, -52, −101, −118, −138, −153, and −180) in follicular fluids ranged from n.d. to 250 ng/g lw, with an average of 77 ± 69 ng/g lw. CB-28 and CB-52 were considered to be indicator CB congeners, with tri-CBs and tetra-CBs dominating in follicular fluid. No significant correlation was observed between patient age and PBDE or PCB concentrations in follicular fluid, indicating that age was not the controlling factor influencing the bioaccumulation of most HOPs in this study.
Show more [+] Less [-]Temporal dynamics of urban heat island correlated with the socio-economic development over the past half-century in Seoul, Korea
2019
Hong, Je-Woo | Hong, Jinkyu | Kwon, Eilhann E. | Yoon, D.K.
Urban heat island (UHI), an iconic consequence of anthropogenic activities and climate condition, affects air pollution, energy use, and health. Therefore, better understanding of the temporal dynamics of UHI is required for sustainable urban planning to mitigate air pollution under a changing climate. Here, we present the evolution of UHI intensity (UHIi) and its controlling factors in the Seoul metropolitan area, Korea, over the last 56 years (1962–2017), which has experienced unique compressed economic growth and urban transformation under monsoon climate. The analysis demonstrated an inverted U-shape long-term variation of UHIi with the progress of urban transformation and economic climate which has not been reported in Asian cities before. Meanwhile, short-term variations in UHIi are related to both diurnal temperature range and duration after rainfall event unlike previous studies, and the UHIi was exacerbated by heat waves. Our findings suggest that the UHIi will exhibit different temporal dynamics with future changes in the monsoon climate, and heat waves in the urban area will be reinforced if current rapid urbanization continues without a shift toward sustainable and equitable development. Asian cities that are likely to face the similar urbanization trajectory and the implications are that urban (re)development strategy considers changes in rainfall magnitude and timing due to monsoon system variation under changing climate and plans to mitigate synergy between heat wave and UHI in this area.
Show more [+] Less [-]Negative impact of Novaluron on the nontarget insect Bombyx mori (Lepidoptera: Bombycidae)
2019
Santorum, Marilucia | Brancalhão, Rose Meire Costa | Guimarães, Ana Tereza Bittencourt | Padovani, Carlos Roberto | Tettamanti, Gianluca | dos Santos, Daniela Carvalho
Due to increased use of agrochemicals and growing concerns about ecotoxicology, the development of new insecticides, moving away from those with neurotoxic and broad spectrum effects towards insecticides that are safer for the environment and nontarget beneficial species, has been a research priority. Novaluron stands out among these newer insecticides, is an insect growth regulator that is used for the control of insect pests in crops grown close to mulberry plantations. Mulberry serves as food for the silkworm Bombyx mori, which is a nontarget insect of great economic importance to silk production. We investigated the lethal and sublethal effects of Novaluron on the development of B. mori. Larvae were segregated into experimental groups: the control groups (CGs) and the treatment groups (TGs), which were treated with the Novaluron concentration of 0.15 mL/L. Following exposure, we analyzed: larval mortality, changes in the insect life cicle and cytotoxic effects on the midgut cells. This is the first report about the Novaluron’s effects on B.mori. We detected rupture in the integument, complete cessation of feeding, late development, incomplete ecdysis and production of defective cocoons. After 240 h of exposure, there was 100% mortality in TG larvae exposed in the 3rd instar and 20% mortality from larvae exposed in the 5th instar. Cytotoxic effects was observed, such as dilation of cells, emission of cytoplasmic protrusions, extreme rarefaction of the cytoplasm and nuclei, dilation of the endoplasmic reticulum in addition to changes in mitochondria, the presence of large digestive vacuoles and intercellular spaces and the presence of active caspase. Novaluron exposure impairs the midgut and may affect the physiological functions of this organ. Novaluron additionally compromises several phases of insect development, indicating the importance of toxicology studies that utilize different life stages of nontarget species to evaluate the safe use of insecticides.
Show more [+] Less [-]New insight of ozone pollution impact from flare emissions of chemical plant start-up operations
2019
Ge, Sijie | Zhang, Jian | Wang, Sujing | Xu, Qiang | Ho, Thomas
Flaring is a common and necessary operation for chemical industries, which is designed to manage dangerous process overpressure scenarios or to release and destroy off-spec products during chemical plant upsets or turnarounds. However, excessive flaring can emit large quantities of VOCs and NOx into the atmosphere, which will cause transient and localized ozone pollution events in the presence of sunlight. The objective of this study was to quantify the impact to regional air-quality due to flare emissions from chemical plant start-up operations through the coupling of dynamic process simulations via Aspen Plus and air-quality simulations via CAMx. Simulation results from case studies have indicated that the corresponding ozone increments can vary significantly from 0.2 ppb to 17.8 ppb under different temporal and spatial factors, including the start-up starting hour, starting day, and plant location. Additional ozone sensitivity simulations have also indicated that the corresponding ozone increments are higher when the plant is located in a VOC-limited area than that in a NOx-limited area. The results from this study have delivered a cost-effective air-quality control practice for plant start-ups with a minimum air-quality impact through selecting the optimal starting time within the allowable ranges. The practice has significant potential to benefit all stakeholders, including environmental agencies, chemical industries, and local communities.
Show more [+] Less [-]The lipid metabolism alteration of three spirocyclic tetramic acids on zebrafish (Danio rerio) embryos
2019
Zhang, Jie | Qian, Le | Teng, Miaomiao | Mu, Xiyan | Qi, Suzhen | Chen, Xiangguang | Zhou, Yimeng | Cheng, Yi | Pang, Sen | Li, Xuefeng | Wang, Chengju
Spirocyclic tetramic acids are widely used in controlling phytophagous mite species throughout the world. the data set is incomplete and provides insufficient evidence for drawing the same conclusion for fish. To fill the gap whether these acaricides alter lipid metabolism on vertebrates, zebrafish embryos exposed to a series concentration of pesticides, the developmental effects, enzyme activities and levels of gene expression were assessed, battery of biomarker utilized by the integrated biomarker response (IBRv2) model. The 96 h-LC₅₀ of spirodiclofen, spiromesifen and spirotetramat were 0.14, 0.12 and 5.94 mg/L, respectively. Yolk sac deformity, pericardial edema, spinal curvature and tail malformation were observed. Three spirocyclic acids were unfavouring the lipid accumulation of by inhibited the acetyl-CoA carboxylase (ACC), fatty acid synthesis (FAS), fatty acid binding proteins (FABP2) and lipoprotein lipase (LPL) activity. The total cholesterol (TCHO) level significantly decreased in the 0.072 mg/L spirodiclofen group and 0.015 and 0.030 mg/L in the spiromesifen groups. No expected change in spirotetramat group on the TCHO and triglycerides (TGs) levels for any of the treatments. The mRNA levels of the genes related to lipid metabolism also significantly altered. In both spirodiclofen and spiromesifen, ACC achieved the highest scores among a battery of biomarkers using integrated biomarker response (IBRv2). The results suggest that spiromesifen was the most toxic for embryos development and spirodiclofen was the most toxic for lipid metabolism in embryos. The 0.07 mg/L of spirodiclofen, 0.05 mg/L of spiromesifen and 2.00 mg/L would cause malformation on zebrafish embryos. This study will provide new insight that fatty acid metabolism may be a suitable biomarker for the spirocyclic tetramic acids in fish species.
Show more [+] Less [-]Cyclodextrin functionalized 3D-graphene for the removal of Cr(VI) with the easy and rapid separation strategy
2019
Wang, Zhe | Lin, Fanyu | Huang, Liqin | Chang, Zhili | Yang, Bing | Liu, Shuang | Zheng, Maosheng | Lu, Yuexiang | Chen, Jing
As a useful heavy metal ion, chromium has seen its applications in various fields. While it is also a toxic contaminant in water and may cause serious threats to the environment and human health. To develop a novel material with good adsorption capacity and easy solid-liquid separation strategy was necessary and significant. In this paper, the β-cyclodextrin (β-CD) functionalized three-dimensional structured graphene foam (CDGF) was successfully synthesized with the facile and one-step hydrothermal method. The SEM, BET, XRD, FT-IR and XPS analysis were carried out and the results confirmed the successfully grafting of β-CD onto GF. The batch adsorption of Cr(VI) was also taken out and the CDGF possessed good selectivity compared with other metal ions at pH = 3. The adsorption capacity reduced gradually as the initial pH of the Cr(VI) solution grew higher, which was because the anionic species of Cr(VI) were partial to the positively charged surface of CDGF. The easy separation strategy of the CDGF was also demonstrated and the CDGF could be taken out easily with a tweezer after the adsorption of Cr(VI), which significantly simplified the separation procedure and reduced time. By comparing the FT-IR and XPD analysis results, the adsorption mechanism was explored and the hydroxyl groups on CDGF played the main role in the adsorption process. This work brings a novel material for the adsorption of Cr(VI) from water and provides an innovative direction for the easy and fast solid-liquid separation strategy in the adsorption and other application fields.
Show more [+] Less [-]Perchlorate behavior in the context of black carbon and metal cogeneration following fireworks emission at Oak Lake, Lincoln, Nebraska, USA
2019
Manish Kumar, | Snow, Daniel D. | Li, Yusong | Shea, Patrick J.
The imprints of fireworks displays on the adjacent water body were investigated from the perspective of cogeneration of black carbon, metals and perchlorate (ClO₄⁻). In particular, the mixing and dissipation of ClO₄⁻ were studied at Oak Lake, Lincoln, Nebraska, following fireworks displays in 2015 and 2016. Following the display, ClO₄⁻ concentration in the water increased up to 4.3 μg/L and 4.0 μg/L in 2015 and 2016, respectively. A first-order model generally provided a good fit to the measured perchlorate concentrations from which the rate of dissipation was estimated as 0.07 d⁻¹ in 2015 and 0.43 d⁻¹ in 2016. SEM images show imprints of soot and metal particles in aerosol samples. EDS analysis of the lake sediment confirmed the presence of Si, K, Ca, Zn and Ba, most of which are components of fireworks. The δ¹³C range of −7.55‰ to −9.19‰ in the lake water system closely resembles fire-generated carbon. Cogeneration of black carbon and metal with perchlorate was established, indicating that ClO₄⁻ is an excellent marker of fireworks or a burning event over all other analyzed parameters. Future microcosmic, aggregation and column-based transport studies on black carbon in the presence of perchlorate and metals under different environmental conditions will help in developing transport and fate models for perchlorate and black carbon particles.
Show more [+] Less [-]Examining the relationships between blubber steroid hormones and persistent organic pollutants in common bottlenose dolphins
2019
Galligan, Thomas M. | Balmer, Brian C. | Schwacke, Lori H. | Bolton, Jennie L. | Quigley, Brian M. | Rosel, Patricia E. | Ylitalo, Gina M. | Boggs, Ashley S.P.
Odontocete cetaceans bioaccumulate high concentrations of endocrine disrupting persistent organic pollutants (POPs), including dichlorodiphenyltrichloroethane (DDT), dichlorodiphenyltrichloroethylene (DDE), and dichlorodiphenyldichloroethane (DDD) – collectively DDTs – but few studies have explored DDTs-mediated endocrine disruption in cetaceans. Herein, we use remotely collected blubber biopsies from common bottlenose dolphins (Tursiops truncatus) inhabiting a site with high localized DDTs contamination to study the relationships between DDTs exposure and steroid hormone homeostasis in cetaceans. We quantified blubber steroid hormone concentrations by liquid chromatography-tandem mass spectrometry and blubber POP concentrations by gas chromatography-mass spectrometry. We detected six steroid hormones in blubber, including progesterone (P4), 17-hydroxyprogesterone (17OHP4), androstenedione (AE), testosterone (T), cortisol (F), and cortisone (E). Sampled dolphins (n = 62) exhibited exposure to DDT, DDE, DDD, chlordanes (CHLDs), mirex, dieldrin, hexachlorobenzene, polychlorinated biphenyls (PCBs), and brominated diphenyl ethers (BDEs). Using principal components analysis (PCA), we determined that blubber DDTs primarily loaded to the first principal component (PC1) explaining 81.6% of the total variance in POP exposure, while the remaining POPs primarily loaded to the PC2 (10.4% of variance). PC1 scores were negatively correlated with blubber T in males and blubber F in females, suggesting that exposure to DDTs impacted androgen and corticosteroid homeostasis. These conclusions were further supported by observed negative correlations between T and o,p’-DDE, o,p’-DDD, and p,p’-DDD in males sampled in the fall, and between F and the six individual DDTs and ∑6DDTs in females. Overall, these results suggest that POP-mediated endocrine disruption may have occurred in this stock of dolphins, which could negatively impact their health and fitness. However, this study relied on uncontrolled incidental exposures, making it impossible to establish a causal relationship between DDTs exposure and endocrine effects. Importantly, this study demonstrates that remotely collected blubber biopsies are a useful matrix for studying endocrine disruption in marine mammals.
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