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Nanoparticles of WC-Co, WC, Co and Cu of relevance for traffic wear particles – Particle stability and reactivity in synthetic surface water and influence of humic matter Полный текст
2017
Hedberg, Yolanda S. | Hedberg, Jonas F. | Isaksson, Sara | Mei, Nanxuan | Blomberg, Eva | Wold, Susanna | Odnevall Wallinder, Inger
Studded tyres made of tungsten carbide cobalt (WC-Co) are in the Northern countries commonly used during the winter time. Tungsten (W)-containing nano- and micron-sized particles have been detected close to busy roads in several European countries. Other typical traffic wear particles consist of copper (Cu). The aims of this study were to investigate particle stability and transformation/dissolution properties of nanoparticles (NPs) of WC-Co compared with NPs of tungsten carbide (WC), cobalt (Co), and Cu. Their physicochemical characteristics (primarily surface oxide and charge) are compared with their extent of sedimentation and metal release in synthetic surface water (SW) with and without two different model organic molecules, 2,3- and 3,4-dihydroxybenzoic acid (DHBA) mimicking certain sorption sites of humic substances, for time periods up to 22 days. The WC-Co NPs possessed a higher electrochemical and chemical reactivity in SW with and without DHBA molecules as compared with NPs of WC, Co, and Cu. Co was completely released from the WC-Co NPs within a few hours of exposure, although it remained adsorbed/bonded to the particle surface and enabled the adsorption of negatively charged DHBA molecules, in contrast with the WC NPs (no adsorption of DHBA). The DHBA molecules were found to rapidly adsorb on the Co and Cu NPs. The sedimentation of the WC and WC-Co NPs was not influenced by the presence of the 2,3- or 3,4-DHBA molecules. A slight influence (slower sedimentation) was observed for the Co NPs, and a strong influence (slower sedimentation) was observed for the Cu NPs in SW with 2,3-DHBA compared with SW alone. The extent of metal release increased in the order: WC < Cu < Co < WC-Co NPs. All NPs released more than 1 wt-% of their metal total mass. The release from the Cu NPs was most influenced by the presence of DHBA molecules.
Показать больше [+] Меньше [-]Hierarchy of factors which influence polycyclic aromatic hydrocarbons (PAHs) distribution in river sediments Полный текст
2017
Liu, An | Duodu, Godfred O. | Mummullage, Sandya | Ayoko, G. A. (Godwin A.) | Goonetilleke, Ashantha
The sediment environment provides habitat for fauna and flora. As pollutants can interchange between water and sediments, pollution will exert a significant influence on the water environment. Previous studies on polycyclic aromatic hydrocarbon (PAHs) pollution of sediments have primarily focused on the comparison of concentrations between seasons, land uses and species. Studies on the identification of the hierarchy of factors which influence PAHs distribution and its variability in river sediments are limited. This paper discusses a comprehensive investigation into the inherent variability of PAHs in sediments and the primary factors which influence this variability. The study outcomes confirmed that key factors exerting influence on PAH distribution in sediments can be ranked in the order: land use > population > seasons. Accordingly, intensive urban land use was identified as the most important factor influencing PAHs distribution. Additionally, it was found that with increasing urban development, PAHs concentrations and their variability in sediments increase in terms of the molecular weight of different species. The study outcomes are expected to enhance management strategies to mitigate PAHs pollution of urban water environments including the prioritisation of factors requiring management and the selection of appropriate approaches in the context of cost-effectiveness.
Показать больше [+] Меньше [-]Revealing the ability of a novel polysaccharide bioflocculant in bioremediation of heavy metals sensed in a Vibrio bioluminescence reporter assay Полный текст
2017
Sajayan, Arya | Seghal Kiran, G. | Priyadharshini, S. | Poulose, Navya | Selvin, Joseph
A bioflocculant-producing bacterial strain, designated MSI021, was isolated from the marine sponge Dendrilla nigra and demonstrated 94% flocculation activity in a kaolin clay suspension. MSI021 was identified as Bacillus cereus based on phylogenetic affiliation and biochemical characteristics. The purified extra-cellular bioflocculant was chemically elucidated as a polysaccharide molecule. The polysaccharide bioflocculant was stable under both acidic and alkaline conditions (pH 2.0–10.0) and temperatures up to 100 °C. The purified bioflocculant efficiently nucleated the formation of silver nanoparticles which showed broad spectrum antibacterial activity. The ability of the bioflocculant to remediate heavy metal toxicity was evaluated by measuring the inhibition of bioluminescence expression in Vibrio harveyi. Enrichment of heavy metals such as zinc, mercury and copper at concentrations of 1, 2 and 3 mM in culture media showed significant reduction of bioluminescence in Vibrio, whereas media enriched with heavy metals and bioflocculant showed dose dependent improvement in the expression of bioluminescence. The assay results demonstrated that the polysaccharide bioflocculant effectively mitigates heavy metal toxicity, thereby improving the expression of bioluminescence in Vibrio. This bioluminescence reporter assay can be developed into a high-throughput format to monitor and evaluate of heavy metal toxicity. The findings of this study revealed that a novel polysaccharide bioflocculant produced by a marine B. cereus demonstrated strong flocculating performance and was effective in nucleating the formation antibacterial silver nanoparticles and removing heavy metals. These results suggest that the MSI021 polysaccharide bioflocculant can be used to develop greener waste water treatment systems.
Показать больше [+] Меньше [-]Relative roles of H-atom transfer and electron transfer in the debromination of polybrominated diphenyl ethers by palladized nanoscale zerovalent iron Полный текст
2017
Wang, Rui | Lu, Guining | Lin, Haozhong | Huang, Kaibo | Tang, Ting | Xue, Xiuling | Yang, Xingjian | Yin, Hua | Dang, Zhi
The relative significance of H-atom transfer versus electron transfer in the dehalogenation of halogenated organic compounds (HOCs) in bimetallic systems has long been debated. In this study, we have investigated this question through the case study of the debromination of 2, 2′, 4, 4’-tetrabromodiphenyl ether (BDE-47). The debromination rates of isomer products of BDE-47 by palladized nano zero-valent iron (n-ZVI/Pd) in the same reactor were compared. The results confirmed a shift in the debromination pathway of BDE-47 when treated with unpalladized nano zero-valent iron (n-ZVI) vs. treatment with n-ZVI/Pd. Study showed that BDEs could be rapidly debrominated in a palladium-H2 system, and the debromination pathway in this system is the same as that in the n-ZVI/Pd system. These results suggest that the H-atom species adsorbed on the surface of palladium are responsible for the enhanced reaction rates and the shift of the debromination pathway in the n-ZVI/Pd system. The Mulliken charges, calculated with density functional theory, on bromine atoms of PBDEs were directly correlated with the susceptibility to the e-transfer pathway in the n-ZVI system and inversely correlated with the susceptibility to the H-transfer pathway in n-ZVI/Pd system. These experimentally verified correlations in BDE-47 permit the prediction of the dominant debromination pathway in other BDEs.
Показать больше [+] Меньше [-]Fate of nano- and microplastic in freshwater systems: A modeling study Полный текст
2017
Besseling, Ellen | Quik, Joris T.K. | Sun, Muzhi | Koelmans, Albert A.
Riverine transport to the marine environment is an important pathway for microplastic. However, information on fate and transport of nano- and microplastic in freshwater systems is lacking. Here we present scenario studies on the fate and transport of nano-to millimetre sized spherical particles like microbeads (100 nm–10 mm) with a state of the art spatiotemporally resolved hydrological model. The model accounts for advective transport, homo- and heteroaggregation, sedimentation-resuspension, polymer degradation, presence of biofilm and burial. Literature data were used to parameterize the model and additionally the attachment efficiency for heteroaggregation was determined experimentally. The attachment efficiency ranged from 0.004 to 0.2 for 70 nm and 1050 nm polystyrene particles aggregating with kaolin or bentonite clays in natural freshwater. Modeled effects of polymer density (1–1.5 kg/L) and biofilm formation were not large, due to the fact that variations in polymer density are largely overwhelmed by excess mass of suspended solids that form heteroaggregates with microplastic. Particle size had a dramatic effect on the modeled fate and retention of microplastic and on the positioning of the accumulation hot spots in the sediment along the river. Remarkably, retention was lowest (18–25%) for intermediate sized particles of about 5 μm, which implies that the smaller submicron particles as well as larger micro- and millimetre sized plastic are preferentially retained. Our results suggest that river hydrodynamics affect microplastic size distributions with profound implications for emissions to marine systems.
Показать больше [+] Меньше [-]Carboxylesterase-involved metabolism of di-n-butyl phthalate in pumpkin (Cucurbita moschata) seedlings Полный текст
2017
Lin, Qingqi | Chen, Siyuan | Chao, Yuanqing | Huang, Xiongfei | Wang, Shizhong | Qiu, Rongliang
Uptake and accumulation by plants is a significant pathway in the migration and transformation of phthalate esters (PAEs) in the environment. However, limited information is available on the mechanisms of PAE metabolism in plants. Here, we investigated the metabolism of di-n-butyl phthalate (DnBP), one of the most frequently detected PAEs, in pumpkin (Cucurbita moschata) seedlings via a series of hydroponic experiments with an initial concentration of 10 mg L⁻¹. DnBP hydrolysis occurred primarily in the root, and two of its metabolites, mono-n-butyl phthalate (MnBP) and phthalic acid (PA), were detected in all plant tissues. The MnBP concentration was an order of magnitude higher than that of PA in shoots, which indicated MnBP was more readily transported to the shoot than was PA because of the former's dual hydrophilic and lipophilic characteristics. More than 80% of MnBP and PA were located in the cell water-soluble component except that 96% of MnBP was distributed into the two solid cellular fractions (i.e., cell wall and organelles) at 96 h. A 13–20% and 29–54% increase of carboxylesterase (CXE) activity shown in time-dependent and concentration-dependent experiments, respectively, indicated the involvement of CXEs in plant metabolism of DnBP. The level of CXE activity in root subcellular fractions was in the order: the cell water-soluble component (88–94%) >> cell wall (3–7%) > cell organelles (3–4%), suggesting that the cell water-soluble component is the dominant locus of CXE activity and also the domain of CXE-catalyzed hydrolysis of DnBP. The addition of triphenyl phosphate, a CXE inhibitor, led to 43–56% inhibition of CXE activity and 16–25% increase of DnBP content, which demonstrated the involvement of CXEs in plant metabolism of DnBP. This study contributes to our understanding of enzymitic mechanisms of PAE transformation in plants.
Показать больше [+] Меньше [-]Using new hetero-spectral two-dimensional correlation analyses and synchrotron-radiation-based spectromicroscopy to characterize binding of Cu to soil dissolved organic matter Полный текст
2017
Sun, Fusheng | Li, Yaqing | Wang, Xiang | Chi, Zhilai | Yu, Guanghui
Understanding the binding characteristics of copper (Cu) to different functional groups in soil dissolved organic matter (DOM) is important to explore Cu toxicity, bioavailability and ultimate fate in the environment. However, the methods used to explore such binding characteristics are still limited. Here, two-dimensional correlation spectroscopy (2DCOS) integrated with Fourier transform infrared (FTIR), 29Si nuclear magnetic resonance (NMR), 27Al NMR, and synchrotron-radiation-based FTIR spectromicroscopy were used to explore the binding characteristics of Cu to soil DOM as part of a long-term (23 years) fertilization experiment. Compared with no fertilization and inorganic fertilization (NPK), long-term pig manure fertilization (M) treatment significantly increased the concentration of total and bioavailable Cu in soils. Furthermore, hetero-spectral 2DCOS analyses demonstrated that the binding characteristics of Cu onto functional groups in soil DOM were modified by fertilization regimes. In the NPK treatment, Cu was bound to aliphatic C, whereas in the manure treatment SiO groups had higher affinity toward Cu than aliphatic C. Also, the sequence of binding of functional groups to Cu was modified by the fertilization treatments. Moreover, synchrotron-radiation-based FTIR spectromicroscopy showed that Cu, clay minerals and sesquioxides, and C functional groups were heterogeneously distributed at the micro-scale. Specifically, clay-OH as well as mineral elements had a distribution pattern similar to Cu, but certain (but not all) C forms showed a distribution pattern inconsistent with that of Cu. The combination of synchrotron radiation spectromicroscopy and 2DCOS is a useful tool in exploring the interactions among heavy metals, minerals and organic components in soils.
Показать больше [+] Меньше [-]Antibiotics degradation in soil: A case of clindamycin, trimethoprim, sulfamethoxazole and their transformation products Полный текст
2017
Koba, Olga | Golovko, Oksana | Kodešová, Radka | Fér, Miroslav | Grabic, Roman
Twelve different soil types that represent the soil compartments of the Czech Republic were fortified with three antibiotics (clindamycin (CLI), sulfamethoxazole (SUL), and trimethoprim (TRI)) to investigate their fate. Five metabolites (clindamycin sulfoxide (CSO), hydroxy clindamycin sulfoxide (HCSO), S-(SDC) and N-demethyl clindamycin (NDC), N4-acetyl sulfamethoxazole (N4AS), and hydroxy trimethoprim (HTR)) were detected and identified using HPLC/HRMS and HRPS in the soil matrix in this study. The identities of CSO and N4AS were confirmed using commercially available reference standards.The parent compounds degraded in all soils. Almost all of the metabolites have been shown to be persistent in soils, with the exception of N4AS, which was formed and degraded completely within 23 days of exposure. The rate of degradation mainly depended on the soil properties.The PCA results showed a high dependence between the soil type and behaviour of the pharmaceutical metabolites.The mentioned metabolites can be formed in soils, and the most persistent ones may be transported to the ground water and environmental water bodies. Because no information on the effects of those metabolites on living organism are available, more studies should be performed in the future to predict the risk to the environment.
Показать больше [+] Меньше [-]Polybrominated diphenyl ethers (PBDES) and hexa-brominated biphenyls (Hexa-BBs) in fresh foods ingested in Taiwan Полный текст
2017
Chang, Jung-Wei | Hung, Chung-Feng | Hsu, Ya-Chen | Kao, Yi-Ting | Lee, Ching-Chang
Polybrominated diphenyl ethers (PBDEs) and hexa-brominated biphenyls (Hexa-BBs) are bioaccumulative and aggregate in the food chain. Therefore, background monitoring and risk assessment for dietary intake are necessary. In present study, a systematic sampling method was first used to collect the high fat content foodstuff such as poultry, livestock, eggs, fish, other seafood, dairy products, and the infant foods and then foodstuff with high consumption in seven categories of 600 food samples. After integrating four years of background surveys of PBDE levels (2010–2013) and one year of that of Hexa-BBs (2013), the highest estimated daily intake (EDI) of PBDEs for Taiwanese food consumption was found in 0- to 3-year-olds (mean = 9.38 ng kg−1 bw d−1, the 95% upper limit of Monte Carlo Simulation (MCS P95) was 21.52 ng kg−1 bw d−1), and the lowest in 16- to 18-year-old girls (mean = 3.35 ng kg−1 bw d−1, MCS P95 was 6.53 ng kg−1 bw d−1). Moreover, the highest of EDI of Hexa-BBs was found in 0–3 years old (mean = 0.007 ng kg−1 bw d−1, MCS P95 = 0.019 ng kg−1 bw d−1), and lowest in 17–18 years old female (mean = 0.002 ng/kg/day, MCS P95 = 0.005 ng kg−1 bw d−1). This study suggests that the large MOEs (>2.5) for the four important congeners BDE-47, -99, −153, and −209, indicate that the dietary exposures are not probably a significant health concern for Taiwanese.
Показать больше [+] Меньше [-]Ambient sulfur dioxide levels associated with reduced risk of initial outpatient visits for tuberculosis: A population based time series analysis Полный текст
2017
Ge, Erjia | Fan, Min | Qiu, Hong | Hu, Howard | Tian, Linwei | Wang, Xiaomeng | Xu, Guozhang | Wei, Xiaolin
Recent biochemical studies suggest that exogenous sulfur dioxide (SO2) at low concentrations may have been beneficial in inhibiting mycobacteria tuberculosis (TB) growth. However, there is a dearth of population-based studies.To examine the association of ambient SO2 levels and initial TB outpatient visits.In Ningbo, China, we collected all daily initial outpatient visits for TB and routinely air pollution monitoring data between January 2009 and December 2013. A time-series study was conducted by using generalized additive regression (GAM) with log-linear Poisson models to estimate the associations between daily initial TB outpatient visits and daily average concentration of SO2. Other traffic-related co-pollutants were adjusted. Sensitivity analyses were conducted to examine the relationship when 1% extreme SO2 concentrations excluded or if related to the early onsets of TB symptoms.SO2 concentrations in Ningbo were low with a daily average of 25 μg/m3 (i.e. 0.0089 ppm). Negative associations were identified between ambient SO2 concentrations and daily initial TB outpatient visits. A 10 μg/m3 increase in SO2 at lag3 and lag0-3 days were associated with −2.0% (95%CI, −3.2, −0.8) and −4.6% (95%CI, −6.8, −2.4) changes, respectively, in initial TB outpatient visits according to single-pollutant models. The negative association became stronger when nitrogen dioxide (NO2) or particulate matter with aerodynamic diameter less than 10 μm (PM10) was adjusted in two-pollutant models. This association was higher in males vs. females and in middle-aged adults vs. the elderly. We found a stronger negative association between SO2 concentration and the initial symptom occurrence.Short-term exposure to ambient SO2 was associated with reduced risk of initial TB outpatient visits, suggesting acute protective effects of low-level ambient SO2 exposure on bacteria-induced pulmonary infections.
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