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Incorporation of zero valent iron nanoparticles in the matrix of cationic resin beads for the remediation of Cr(VI) contaminated waters Full text
2016
Toli, Aikaterini | Chalastara, Konstantina | Mystrioti, Christiana | Xenidis, Anthimos | Papassiopi, Nymphodora
The objective of present study was to obtain the fixation of nano zero valent iron (nZVI) particles on a permeable matrix and evaluate the performance of this composite material for the removal of Cr(VI) from contaminated waters. The experiments were carried out using the cationic resin Dowex 50WX2 as porous support of the iron nanoparticles. The work was carried out in two phases. The first phase involved the fixation of nZVI on the resin matrix. The resin granules were initially mixed with a FeCl3 solution to obtain the adsorption of Fe(III). Then the Fe(III) loaded resin (RFe) was treated with polyphenol solutions to obtain the reduction of Fe(III) to the elemental state. Two polyphenol solutions were tested as reductants, i.e. green tea extract and gallic acid. Green tea was found to be inefficient, probably due to the relatively big size of the contained polyphenol molecules, but gallic acid molecules were able to reach adsorbed Fe(III) and reduce the cations to the elemental state. The second phase was focused on the investigation of Cr(VI) reduction kinetics using the nanoiron loaded resins (R-nFe). It was found that the reduction follows a kinetic law of first order with respect to Cr(VI) and to the embedded nanoiron. Compared to other similar products, this composite material was found to have comparable performance regarding reaction rates and higher degree of iron utilization. Namely the rate constant for the reduction of Cr(VI), in the presence of 1 mM nZVI, was equivalent to 1.4 h of half-life time at pH 3.2 and increased to 24 h at pH 8.5. The degree of iron utilization was as high as 0.8 mol of reduced Cr(VI) per mole of iron. It was also found that this composite material can be easily regenerated and reused for Cr(VI) reduction without significant loss of efficiency.
Show more [+] Less [-]Correlations and adsorption mechanisms of aromatic compounds on a high heat temperature treated bamboo biochar Full text
2016
Yang, Kun | Yang, Jingjing | Jiang, Yuan | Wu, Wenhao | Lin, Daohui
Adsorption of aromatic compounds, including polycyclic aromatic hydrocarbons, nitrobenzenes, phenols, and anilines, on a bamboo biochar produced at 700 °C (Ba700) was investigated with the mechanism discussion by isotherm fitting using the Polanyi-theory based Dubinin–Ashtakhov (DA) model. Correlations of adsorption capacity (Q0) of organic compounds with their molecular sizes and melting points, as well as correlations of adsorption affinity (E) with their solvatochromic parameters (i.e., π* and αm), on the biochar, were developed and indicating that adsorption is captured by the pore filling mechanism and derived from the hydrophobic effects of organic compounds and the forming of π-π electron donor-acceptor (EDA) interactions and hydrogen bonding interactions of organic molecules with surface sites of the biochar. The effects of organic molecular sizes and melting points on adsorption capacity are ascribed to the molecular sieving effect and the packing efficiency of the organic molecules in the biochar pores, respectively. These correlations can be used to quantitatively estimate the adsorption of organic compounds on biochars from their commonly physicochemical properties including solvatochromic parameters, melting points and molecular cross-sectional area. The prediction using these correlations is important for assessing the unknown adsorption behaviors of new organic compounds and also helpful to guide the surface modification of biochars and make targeted selection in the environmental applications of biochars as adsorbents.
Show more [+] Less [-]Neutral polyfluoroalkyl substances in the atmosphere over the northern South China Sea Full text
2016
Lai, Senchao | Song, Junwei | Song, Tianli | Huang, Zhijiong | Zhang, Yingyi | Zhao, Yan | Liu, Guicheng | Zheng, Junyu | Mi, Wenying | Tang, Jianhui | Zou, Shichun | Ebinghaus, Ralf | Xie, Zhiyong
Neutral Polyfluoroalkyl substances (PFASs) in the atmosphere were measured during a cruise campaign over the northern South China Sea (SCS) from September to October 2013. Four groups of PFASs, i.e., fluorotelomer alcohols (FTOHs), fluorotelomer acrylates (FTAs), fluorooctane sulfonamides (FOSAs) and fluorooctane sulfonamidoethanols (FASEs), were detected in gas samples. FTOHs was the predominant PFAS group, accounting for 95.2–99.3% of total PFASs (ΣPFASs), while the other PFASs accounted for a small fraction of ΣPFASs. The concentrations of ΣPFASs ranged from 18.0 to 109.9 pg m−3 with an average of 54.5 pg m−3. The concentrations are comparable to those reported in other marine atmosphere. Higher concentrations of ΣPFASs were observed in the continental-influenced samples than those in other samples, pointing to the substantial contribution of anthropogenic sources. Long-range transport is suggested to be a major pathway for introducing gaseous PFASs into the atmosphere over the northern SCS. In order to further understand the fate of gaseous PFASs during transport, the atmospheric decay of neutral PFASs under the influence of reaction with OH radicals and atmospheric physical processes were estimated. Concentrations of 8:2 FTOH, 6:2 FTOH and MeFBSE from selected source region to the atmosphere over the SCS after long-range transport were predicted and compared with the observed concentrations. It suggests that the reaction with OH radicals may play an important role in the atmospheric decay of PFAS during long-range transport, especially for shorted-lived species. Moreover, the influence of atmospheric physical processes on the decay of PFAS should be further considered.
Show more [+] Less [-]The fate of phosphorus in sediments after the full operation of the Three Gorges Reservoir, China Full text
2016
Wu, Yanhong | Wang, Xiaoxiao | Zhou, Jun | Bing, Haijian | Sun, Hongyang | Wang, Jipeng
The hydro-dynamic conditions have been changed after the impoundment of Three Gorges Reservoir (TGR), which result in changes of phosphorus (P) distribution in sediments. To investigate the variation and storage of P in the surface sediments of the TGR, continuously and intermittently submerged sediment samples were collected from 14 sites in 2014, and P fractions were analyzed using a modified Hedley sequential extraction method. The results showed that the concentrations of total P (TP) (904 ± 105 mg/kg) in the sediments did not exhibit an apparent spatial trend. A decreasing trend of bioavailable P (Bio-P) concentration in the continuously submerged sediment (177 ± 29 mg/kg) was observed from Fuling to Zigui, while an opposite trend appeared in the intermittently submerged sediment (139 ± 49 mg/kg) from Jiangjin to Zigui. The water depth and sediment grain size had important implications for the variation of the Bio-P in the sediments along the TGR. After the full operation of the TGR, the concentration of TP in the intermittently submerged sediment from Fengjie to Zigui was significantly higher in 2014 compared with that in 2009. The continuously submerged sediment is a major P pool of the TGR with an annual Bio-P deposition flux of 2.14 × 104 t/a, of which 87% was retained in the reaches from Fuling to Zigui. Considering the slow release of P from the sediment (0.16–2.75 t/a), the sediment has been a P “sink” since the full operation of the TGR in 2010.
Show more [+] Less [-]A quantitative assessment of source contributions to fine particulate matter (PM2.5)-bound polycyclic aromatic hydrocarbons (PAHs) and their nitrated and hydroxylated derivatives in Hong Kong Full text
2016
Ma, Yiqiu | Cheng, Yubo | Qiu, Xinghua | Lin, Yan | Cao, Jing | Hu, Di
Atmospheric polycyclic aromatic hydrocarbons (PAHs) and their derivatives are of great concern due to their adverse health effects. However, source identification and apportionment of these compounds, particularly their nitrated and hydroxylated derivatives (i.e., NPAHs and OHPAHs), in fine particulate matter (PM2.5) in Hong Kong are still lacking. In this study, we conducted a 1-year observation at an urban site in Hong Kong. PM2.5-bound PAHs and their derivatives were measured, with median concentrations of 4590, 44.4 and 31.6 pg m−3 for ∑21PAHs, ∑13NPAHs, and ∑12OHPAHs, respectively. Higher levels were observed on regional pollution days than on long regional transport (LRT) or local emission days. Based on positive matrix factorization analysis, four sources were determined: marine vessels, vehicle emissions, biomass burning, and a mixed source of coal combustion and NPAHs secondary formation. Coal combustion and biomass burning were the major sources of PAHs, contributing over 85% of PAHs on regional and LRT days. Biomass burning was the predominant source of OHPAHs throughout the year, while NPAHs mainly originated from secondary formation and fuel combustion. For benzo[a]pyrene (BaP)-based PM2.5 toxicity, the mixed source of coal combustion and NPAHs secondary formation was the major contributor, followed by biomass burning and vehicle emissions.
Show more [+] Less [-]Studies on size distribution and health risk of 37 species of polycyclic aromatic hydrocarbons associated with fine particulate matter collected in the atmosphere of a suburban area of Shanghai city, China Full text
2016
Wang, Qingyue | Kobayashi, Keisuke | Lu, Senlin | Nakajima, Daisuke | Wang, Weiqian | Zhang, Wenchao | Sekiguchi, Kazuhiko | Terasaki, Masanori
Polycyclic aromatic hydrocarbons (PAHs) in suspended particulate matter (SPM) contribute significantly to health risk. Our objectives were to assess the size distribution and sources of 26 PAHs and 11 polycyclic aromatic compounds (PACs) in SPM in the suburban area, Shanghai city, China. Air sampling was carried out on the rooftop of a five-stories building in the campus of Shanghai University. An Andersen high-volume air sampler was employed to collect ambient size-segregated particles from August to September 2015. The toxic particulate PAHs were determined by the gas chromatography mass spectrometry. The concentrations of total PAHs (TPAHs) in SPM and PM1.1 (suspended particulate matter below 1.1 μm) were in the ranges of 4.58–14.5 ng m−3 and 1.82–8.56 ng m−3, respectively. 1,8-naphthalic anhydride showed the highest concentrations among 37 species of PAHs and PACs ranging 7.76–47.9 ng m−3 and 1.50–17.6 ng m−3 in SPM and PM1.1, respectively. The concentrations of high molecular weight 5–6 ring PAHs followed a nearly unimodal size distribution with the highest peak in PM1.1, while other lower molecular weight PAHs were not dependent on particle sizes. The toxicity analysis indicated that the carcinogenic potency of particulate PAHs primarily existed in PM1.1. Regarding meteorological parameters and other pollutants, the positive effect of humidity and NO2 over PAHs was confirmed. Diagnostic ration indicated that the particulate PAHs in Shanghai were mainly derived from motor-vehicle or petroleum combustion. The highest benzo[a]pyrene equivalent (BaPeq) in SPM and PM1.1 were 2.15 ng m−3 and 1.43 ng m−3 calculated by the toxicity equivalency factor, and 69.31 ng m−3 and 47.81 ng m−3 estimated by the potency equivalency factors, respectively. The highest contributors in the total carcinogenicity of the particulate PAHs were dibenzo[a,h]pyrene (46.2% and 45.0%) and benz[j]aceanthrylene (80.2% and 83.1%), respectively while benzo[a]pyrene is lower contributor than other carcinogenic PAHs.
Show more [+] Less [-]Semen phthalate metabolites, semen quality parameters and serum reproductive hormones: A cross-sectional study in China Full text
2016
Wang, Yi-Xin | Zeng, Qiang | Sun, Yang | Yang, Pan | Wang, Peng | Li, Jin | Huang, Zhen | You, Ling | Huang, Yue-Hui | Wang, Cheng | Li, Yu-Feng | Lu, Wen-Qing
Exposure to phthalates has been found to have adverse effects on male reproductive function in animals. However, the findings from human studies are inconsistent. Here we examined the associations of phthalate exposure with semen quality and reproductive hormones in a Chinese population using phthalate metabolite concentrations measured in semen as biomarkers. Semen (n = 687) and blood samples (n = 342) were collected from the male partners of sub-fertile couples who presented to the Reproductive Center of Tongji Hospital in Wuhan, China. Semen quality parameters and serum reproductive hormone levels were determined. Semen concentrations of 8 phthalate metabolites were assessed using high-performance liquid chromatography and tandem mass spectrometry. Associations of the semen phthalate metabolites with semen quality parameters and serum reproductive hormones were assessed using confounder-adjusted linear and logistic regression models. Semen phthalate metabolites were significantly associated with decreases in semen volume [mono-n-butyl phthalate (MBP), mono-(2-ethylhexyl) phthalate (MEHP), mono(2-ethyl-5-hydroxyhexyl) phthalate (MEHHP), mono(2-ethyl-5-oxohexyl) phthalate (MEOHP)], sperm curvilinear velocity [monobenzyl phthalate (MBzP), MEHP, the percentage of di-(2-ethylhexyl)-phthalate metabolites excreted as MEHP (%MEHP)], and straight-line velocity (MBzP, MEHP, %MEHP), and also associated with an increased percentage of abnormal heads and tails (MBzP) (all p for trend <0.05). These associations remained suggestive or significant after adjustment for multiple testing. There were no significant associations between semen phthalate metabolites and serum reproductive hormones. Our findings suggest that environmental exposure to phthalates may impair human semen quality.
Show more [+] Less [-]PM2.5 source attribution for Seoul in May from 2009 to 2013 using GEOS-Chem and its adjoint model Full text
2016
Lee, Hyung-Min | Park, Rokjin J. | Henze, Daven K. | Lee, Seungun | Shim, Changsub | Shin, Hye-Jung | Moon, Kwang-Joo | Woo, Jung-Hun
Enforcement of an air quality standard for PM2.5 in the Seoul metropolitan area (SMA) was enacted in 2015. From May to June of 2016, an international airborne and surface measurement campaign took place to investigate air pollution mechanisms in the SMA. The total and speciated PM2.5 concentrations since 2008 have been measured at an intensive monitoring site for the SMA operated by the National Institute of Environmental Research (NIER). To gain insight on the trends and sources of PM2.5 in the SMA in May, we analyze PM2.5 concentrations from 2009 to 2013 using the measurements and simulations from a 3-dimensional global chemical transport model, GEOS-Chem and its adjoint. The model is updated here with the latest regional emission inventory and diurnally varying NH3 emissions. Monthly average PM2.5 concentration measured by β-ray attenuation ranges from 28 (2010) to 45 (2013) μg/m3, decreased from 2009 to 2010, and then continuously increased until 2013. The model shows good agreement with the measurements for the daily average PM2.5 concentrations (R ≥ 0.5), and reproduces 10 out of 17 measured episodes exceeding the daily air quality standard (50 μg/m3). Using the GEOS-Chem adjoint model, we find that anthropogenic emissions from the Shandong region have the largest modeled influence on PM2.5 in Seoul in May. Average contributions to the high PM2.5 episodes simulated by the model are 39% from the Shandong region, 16% from the Shanghai region, 14% from the Beijing region, and 15% from South Korea. Anthropogenic SO2 emissions from South Korea are negligible with 90% of the total contribution originating from China. Findings from this study may guide interpretation of observations obtained in the KORUS-AQ measurement campaign.
Show more [+] Less [-]Increase in dust storm related PM10 concentrations: A time series analysis of 2001–2015 Full text
2016
Krasnov, Helena | Katra, Itzhak | Friger, Michael
Over the last decades, changes in dust storms characteristics have been observed in different parts of the world. The changing frequency of dust storms in the southeastern Mediterranean has led to growing concern regarding atmospheric PM10 levels. A classic time series additive model was used in order to describe and evaluate the changes in PM10 concentrations during dust storm days in different cities in Israel, which is located at the margins of the global dust belt. The analysis revealed variations in the number of dust events and PM10 concentrations during 2001–2015. A significant increase in PM10 concentrations was identified since 2009 in the arid city of Beer Sheva, southern Israel. Average PM10 concentrations during dust days before 2009 were 406, 312, and 364 μg m−3 (median 337, 269,302) for Beer Sheva, Rehovot (central Israel) and Modi'in (eastern Israel), respectively. After 2009 the average concentrations in these cities during dust storms were 536, 466, and 428 μg m−3 (median 382, 335, 338), respectively. Regression analysis revealed associations between PM10 variations and seasonality, wind speed, as well as relative humidity. The trends and periodicity are stronger in the southern part of Israel, where higher PM10 concentrations are found. Since 2009 dust events became more extreme with much higher daily and hourly levels. The findings demonstrate that in the arid area variations of dust storms can be quantified easier through PM10 levels over a relatively short time scale of several years.
Show more [+] Less [-]Cadmium-induced immune abnormality is a key pathogenic event in human and rat models of preeclampsia Full text
2016
Zhang, Qiong | Huang, Yinping | Zhang, Keke | Huang, Yanjun | Yan, Yan | Wang, Fan | Wu, Jie | Wang, Xiao | Xu, Zhangye | Chen, Yongtao | Cheng, Xue | Li, Yong | Jiao, Jinyu | Ye, Duyun
With increased industrial development, cadmium is an increasingly important environmental pollutant. Studies have identified various adverse effects of cadmium on human beings. However, the relationships between cadmium pollution and the pathogenesis of preeclampsia remain elusive. The objective of this study is to explore the effects of cadmium on immune system among preeclamptic patients and rats. The results showed that the cadmium levels in the peripheral blood of preeclamptic patients were significantly higher than those observed in normal pregnancy. Based on it, a novel rat model of preeclampsia was established by the intraperitoneal administration of cadmium chloride (CdCl2) (0.125 mg of Cd/kg body weight) on gestational days 9–14. Key features of preeclampsia, including hypertension, proteinuria, placental abnormalities and small foetal size, appeared in pregnant rats after the administration of low-dose of CdCl2. Cadmium increased immunoglobulin production, mainly angiotensin II type 1-receptor-agonistic autoantibodies (AT1-AA), by increasing the expression of activation-induced cytosine deaminase (AID) in B cells. AID is critical for the maturation of antibody and autoantibody responses. In addition, angiotensin II type 1-receptor-agonistic autoantibody, which emerged recently as a potential pathogenic contributor to PE, was responsible for the deposition of complement component 5 (C5) in kidneys of pregnant rats via angiotensin II type 1 receptor (AT1R) activation. C5a is a fragment of C5 that is released during C5 activation. Selectively interfering with C5a signalling by a complement C5a receptor-specific antagonist significantly attenuated hypertension and proteinuria in Cd-injected pregnant rats. Our results suggest that cadmium induces immune abnormalities that may be a key pathogenic contributor to preeclampsia and provide new insights into treatment strategies of preeclampsia.
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