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Stabilisation of nanoscale zero-valent iron with biochar for enhanced transport and in-situ remediation of hexavalent chromium in soil
2016
Su, Huijie | Fang, Zhanqiang | Tsang, Pokeung Eric | Fang, Jianzhang | Zhao, Dongye
In this study, a biochar-supported nanoscale zero-valent iron (nZVI@BC) material was used for in situ remediation of hexavalent chromium-contaminated soil. Sedimentation tests and column experiments were used to compare the stability and mobility of nZVI@BC and bare-nZVI. The immobilisation efficiency of chromium, toxic effect of chromium and the content of iron were assessed through leaching tests and pot experiments. Sedimentation tests and transport experiments indicated that nZVI@BC with nZVI to BC mass ratio of 1:1 exhibited better stability and mobility than that of bare-nZVI. The immobilisation efficiency of Cr(VI) and Crtotal was 100% and 92.9%, respectively, when the soil was treated with 8 g/kg of nZVI@BC for 15 days. Moreover, such remediation effectively reduced the leachability of Fe caused by bare-nZVI. In addition, pot experiments showed that such remediation reduced the phytotoxicity of Cr and the leachable Fe and was favourable for plant growth.
显示更多 [+] 显示较少 [-]Position-specific isotope modeling of organic micropollutants transformation through different reaction pathways
2016
Jin, Biao | Rolle, Massimo
The degradation of organic micropollutants occurs via different reaction pathways. Compound specific isotope analysis is a valuable tool to identify such degradation pathways in different environmental systems. We propose a mechanism-based modeling approach that provides a quantitative framework to simultaneously evaluate concentration as well as bulk and position-specific multi-element isotope evolution during the transformation of organic micropollutants. The model explicitly simulates position-specific isotopologues for those atoms that experience isotope effects and, thereby, provides a mechanistic description of isotope fractionation occurring at different molecular positions. To demonstrate specific features of the modeling approach, we simulated the degradation of three selected organic micropollutants: dichlorobenzamide (BAM), isoproturon (IPU) and diclofenac (DCF). The model accurately reproduces the multi-element isotope data observed in previous experimental studies. Furthermore, it precisely captures the dual element isotope trends characteristic of different reaction pathways as well as their range of variation consistent with observed bulk isotope fractionation. It was also possible to directly validate the model capability to predict the evolution of position-specific isotope ratios with available experimental data. Therefore, the approach is useful both for a mechanism-based evaluation of experimental results and as a tool to explore transformation pathways in scenarios for which position-specific isotope data are not yet available.
显示更多 [+] 显示较少 [-]Particulate-bound polycyclic aromatic hydrocarbon sources and determinants in residential homes
2016
Cattaneo, Andrea | Fermo, Paola | Urso, Patrizia | Perrone, Maria Grazia | Piazzalunga, Andrea | Tarlassi, Jessica | Carrer, Paolo | Cavallo, Domenico Maria
Human exposure to polycyclic aromatic hydrocarbons (PAHs) in indoor environments can be particularly relevant because people spend most of their time inside buildings, especially in homes. This study aimed to investigate the most important particle-bound PAH sources and exposure determinants in PM2.5 samples collected in 19 homes located in northern Italy. Complementary information about ion content in PM10 was also collected in 12 of these homes. Three methods were used for the identification of PAH sources and determinants: diagnostic ratios with principal component and hierarchical cluster analyses (PCA and HCA), chemical mass balance (CMB) and linear mixed models (LMMs). This combined and tiered approach allowed the infiltration of outdoor PAHs into indoor environments to be identified as the most important source in winter, with a relevant role played by biomass burning and traffic exhausts to be identified as a general source of PAHs in both seasons. Tobacco smoke exhibited an important impact on PAH levels in smokers' homes, whereas in the whole sample, cooking food and natural gas sources played a minor or negligible role. Nitrate, sulfate and ammonium were the main inorganic constituents of indoor PM10 owing to the secondary formation of ammonium sulfates and nitrates.
显示更多 [+] 显示较少 [-]Transformation of 17β-estradiol in humic acid solution by ε-MnO2 nanorods as probed by high-resolution mass spectrometry combined with 13C labeling
2016
Sun, Kai | Liang, Shangtao | Kang, Fuxing | Gao, Yanzheng | Huang, Qingguo
Steroidal estrogens (SEs), widespread in aquatic systems, have a potential to disrupt the endocrine system of wildlife species and humans. In our experiments, the performance of ε-MnO2 nanorods in transforming 17β-estradiol (E2) was investigated, and the effect of humic acid (HA) on the reaction behaviors was systematically characterized. Reconfiguration of humic molecules was also investigated by high-performance size exclusion chromatography (HPSEC). Results indicated that ε-MnO2 nanomaterials ensured efficient removal of E2 from the aqueous solution. The presence of HA hindered the transformation of E2, while enhanced the cross-coupling between E2 and humic molecules. In particular, we used a mixture of un-labeled E2 and 13C3-labeled E2 at a 1: 1 set ratio (w/w) to probe the reaction products via high-resolution mass spectrometry (HRMS). The combination of HRMS and 13C3-labeling revealed the intermediate products including estrone (E1), and hydroxylated, quinone-like, and ring-opened species, as well as E2 dimer and trimer. More importantly, possible cross-coupling products between E2 and HA were also identified. A reaction mechanism including two-electron oxidation and single-electron oxidation was proposed. The applied analytical approach using HRMS along with 13C3-labeling for reaction-product identification is crucial to understanding the role of HA in the transformation of SEs.
显示更多 [+] 显示较少 [-]UV filters induce transcriptional changes of different hormonal receptors in Chironomus riparius embryos and larvae
2016
Ozáez, Irene | Aquilino, Mónica | Morcillo, Gloria | Martínez-Guitarte, José-Luis
Organic ultraviolet (UV) filters are emerging contaminants that are ubiquitous in fresh and marine aquatic systems due to their extensive use in cosmetics, plastics, paints, textiles, and many other industrial products. The estrogenic effects of organic UV filters have been long demonstrated in vertebrates, and other hormonal activities may be altered, according to more recent reports. The impact of UV filters on the endocrine system of invertebrates is largely unknown. We have previously reported that some UV filters may affect ecdysone-related genes in the aquatic insect Chironomus riparius, an ecotoxicologically important model organism. To further analyze other possible effects on endocrine pathways, we first characterized four pivotal genes related with hormonal pathways in insects; thereafter, these genes were assessed for alterations in transcriptional activity after exposure to 4-methylbenzylidene camphor (4MBC) or benzophenone-3 (BP-3), two extensively used sunscreens. We found that both chemicals disturbed the expression of all four genes analyzed: hormonal receptor 38 (HR38), methoprene-tolerant (Met), membrane-associate progesterone receptor (MAPR) and insulin-like receptor (INSR), measured by changes in mRNA levels by real-time PCR. An upregulatory effect at the genomic level was detected in different developmental stages. Interestingly, embryos appeared to be more sensitive to the action of the UV filters than larvae. Our results suggest that the risk of disruption through different endocrine routes is not negligible, considering the significant effects of UV filters on key hormonal receptor and regulatory genes. Further effort is needed to develop environmental risk assessment studies on these pollutants, particularly for aquatic invertebrate model organisms.
显示更多 [+] 显示较少 [-]Environmental pollution of electronic waste recycling in India: A critical review
2016
Awasthi, Abhishek Kumar | Zeng, Xianlai | Li, Jinhui
The rapid growth of the production of electrical and electronic products has meant an equally rapid growth in the amount of electronic waste (e-waste), much of which is illegally imported to India, for disposal presenting a serious environmental challenge. The environmental impact during e-waste recycling was investigated and metal as well as other pollutants [e.g. polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs)] were found in excessive levels in soil, water and other habitats. The most e-waste is dealt with as general or crudely often by open burning, acid baths, with recovery of only a few materials of value. As resulted of these process; dioxins, furans, and heavy metals are released and harmful to the surrounding environment, engaged workers, and also residents inhabiting near the sites. The informal e-waste sectors are growing rapidly in the developing countries over than in the developed countries because of cheapest labor cost and week legislations systems. It has been confirmed that contaminates are moving through the food chain via root plant translocation system, to the human body thereby threatening human health. We have suggested some possible solution toward in which plants and microbes combine to remediate highly contaminated sites.
显示更多 [+] 显示较少 [-]Pattern of atmospheric mercury speciation during episodes of elevated PM2.5 levels in a coastal city in the Yangtze River Delta, China
2016
Hong, Youwei | Chen, Jinsheng | Deng, Junjun | Tong, Lei | Xu, Lingling | Niu, Zhenchuan | Yin, Liqian | Chen, Yanting | Hong, Zhenyu
Measurement of atmospheric mercury speciation was conducted in a coastal city of the Yangtze River Delta, China from July 2013 to January 2014, in conjunction with air pollutants and meteorological parameters. The mean concentrations of gaseous elemental mercury (GEM), particulate bound mercury (HgP) and reactive gaseous mercury (RGM) were 3.26 ± 1.63 ng m−3, 659 ± 931 pg m−3, and 197 ± 246 pg m−3, respectively. High percentages of HgP during haze days were found, due to the increase in direct emissions and gas-particle partitioning of RGM. The average gas-particle partitioning coefficients (Kp) during moderate or severe haze days (PM2.5 > 150 μg m−3) were obviously decreased. GEM and HgP were positively correlated with PM2.5, SO2, NO2 and CO, suggesting a significant contribution of anthropogenic sources. Elevated HgP concentrations in cold seasons and in the morning were observed while RGM exhibited different seasonal and diurnal pattern. The ratio of HgP/SO2 and Pearson correlation analysis suggested that coal combustion was the main cause of increasing atmospheric Hg concentrations. The monitoring site was affected by local, regional and interregional sources. The back trajectory analysis suggested that air mass from northwest China and Huabei Plain contributed to elevated atmospheric Hg in winter and autumn, while southeast China with clean air masses were the major contributor in summer.
显示更多 [+] 显示较少 [-]Levels and patterns of DDTs in maternal colostrum from an island population and exposure of neonates
2016
Xu, Chenye | Tang, Mengling | Zhang, Honghui | Zhang, Chunlong | Liu, Weiping
Dichlorodiphenyltrichloroethane (DDT) was heavily used in the past in many regions of the world. The occurrence of DDTs in island populations may be elevated if the island is adjacent to major DDT consumption estuaries, such as the Yangtze River Delta. In this study, colostrum samples were collected from maternal-neonate pairs (n = 106) from the Shengsi Island, located directly downstream from the Yangtze River outlet. DDT isomers and enantiomer compositions were analyzed by gas chromatography equipped with mass spectrometer (GC/MS) and GC/MS-MS. The average levels of p,p’-DDE, o,p’-DDD, p,p’-DDD, o,p’-DDT, p,p’-DDT and total DDTs were 1.32, 0.03, 0.09, 0.08, 0.48, and 1.93 μg g⁻¹ lipid weight, respectively. Maternal age and pregnancy body mass index (BMI) were positively associated with levels of DDTs (p < 0.05). High (DDE+DDD)/DDT and p,p′-DDE/p,p′-DDT ratios suggested that current DDT residues originated primarily from historical use of DDT products, but new sources may also contribute partially to some high o,p′-DDT/p,p′-DDT ratios. Enantiomeric enrichment was found for the (−)-enantiomer of o,p’-DDD and the (+)-enantiomer of o,p’-DDT, suggesting stereoselective attenuation. Based on breast milk consumption, the average daily intake of DDTs by neonates was 8.33 ± 7.34 μg kg⁻¹bw per day, which exceeded the WHO's tolerable daily intake guideline of 0.01 mg kg⁻¹ bw per day by 25%, implying some neonates in the Yangtze River region are potentially at high risk from exposure to DDTs.
显示更多 [+] 显示较少 [-]The identification of the metabolites of chlorothalonil in zebrafish (Danio rerio) and their embryo toxicity and endocrine effects at environmentally relevant levels
2016
Zhang, Quan | Ji, Chenyang | Yan, Lu | Lu, Meiya | Lu, Chensheng | Zhao, Meirong
Chlorothalonil is a broad spectrum fungicide with high annual production and environmental contamination. Despite its high consumption, studies regarding the potential ecological risks of chlorothalonil, especially its metabolites, to aquatic organisms are still limited. In this study, we selected the zebrafish (Danio rerio) as the in vivo model and first identified the metabolite (4-hydroxychlorothalonil) of chlorothalonil in zebrafish by tandem quadrupole/orthogonal-acceleration time-of-flight (Q-TOF). Then, the in vivo and in vitro models were applied to comprehensively estimate the embryo toxicity and potential endocrine effect of chlorothalonil and 4-hydroxychlorothalonil. The data from zebrafish embryo toxicity showed that the lowest observed effect concentrations of both chlorothalonil and 4-hydroxychlorothalonil were 50 μg/L after 96 h of exposure. The mortality rate of the 4-hydroxychlorothalonil was 2.6-fold higher than that of the parent compound at the concentration of 50 μg/L. Dual-luciferase reporter gene assays indicated that both chlorothalonil and 4-hydroxychlorothalonil exerted estrogen receptor α (ERα) agonist activity with REC20 values of 2.4 × 10−8 M and 3.6 × 10−8 M, respectively. However, only 4-hydroxychlorothalonil exhibited both thyroid receptor β (TRβ) agonistic and antagonistic activities. Lastly, we employed molecular docking to predict the binding affinity of chlorothalonil and 4-hydroxychlorothalonil with ERα or TRβ. The results revealed that the potential endocrine effect of chlorothalonil and 4-hydroxychlorothaloni might be attributed to the different binding affinities with the receptors. In conclusion, our studies revealed that 4-hydroxychlorothalonil exhibited potent endocrine-disrupting effects compared to its parent compound, chlorothalonil. The results provided here remind us that the assessment of the potential ecological and health risks of the metabolites of fungicides in addition to their parent compounds should arouse great concerns.
显示更多 [+] 显示较少 [-]Reconstructing the Chernobyl Nuclear Power Plant (CNPP) accident 30 years after. A unique database of air concentration and deposition measurements over Europe
2016
Evangeliou, Nikolaos | Hamburger, Thomas | Talerko, Nikolai | Zibtsev, Sergey | Bondar, Yuri | Stohl, Andreas | Balkanski, Yves | Mousseau, Timothy A. | Møller, Anders P.
30 years after the Chernobyl Nuclear Power Plant (CNPP) accident, its radioactive releases still remain of great interest mainly due to the long half-lives of many radionuclides emitted. Observations from the terrestrial environment, which hosts radionuclides for many years after initial deposition, are important for health and environmental assessments. Furthermore, such measurements are the basis for validation of atmospheric transport models and can be used for constraining the still not accurately known source terms. However, although the “Atlas of cesium deposition on Europe after the Chernobyl accident” (hereafter referred to as “Atlas”) has been published since 1998, less than 1% of the direct observations of 137Cs deposition has been made publicly available. The remaining ones are neither accessible nor traceable to specific data providers and a large fraction of these data might have been lost entirely. The present paper is an effort to rescue some of the data collected over the years following the CNPP accident and make them publicly available. The database includes surface air activity concentrations and deposition observations for 131I, 134Cs and 137Cs measured and provided by Former Soviet Union authorities the years that followed the accident. Using the same interpolation tool as the official authorities, we have reconstructed a deposition map of 137Cs based on about 3% of the data used to create the Atlas map. The reconstructed deposition map is very similar to the official one, but it has the advantage that it is based exclusively on documented data sources, which are all made available within this publication. In contrast to the official map, our deposition map is therefore reproducible and all underlying data can be used also for other purposes. The efficacy of the database was proved using simulated activity concentrations and deposition of 137Cs from a Langrangian and a Euleurian transport model.
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