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Find video protocols related to scientific articles indexed in Pubmed.
IFN-stimulated gene LY6E in monocytes regulates the CD14/TLR4 pathway but inadequately restrains the hyperactivation of monocytes during chronic HIV-1 infection.
J. Immunol.
PUBLISHED: 09-15-2014
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Owing to ongoing recognition of pathogen-associated molecular patterns, immune activation and upregulation of IFN-stimulated genes (ISGs) are sustained in the chronically infected host. Albeit most ISGs are important effectors for containing viral replication, some might exert compensatory immune suppression to limit pathological dysfunctions, although the mechanisms are not fully understood. In this study, we report that the ISG lymphocyte Ag 6 complex, locus E (LY6E) is a negative immune regulator of monocytes. LY6E in monocytes negatively modulated CD14 expression and subsequently dampened the responsiveness to LPS stimulation in vitro. In the setting of chronic HIV infection, the upregulation of LY6E was correlated with reduced CD14 level on monocytes; however, the immunosuppressive effect of LY6E was not adequate to remedy the hyperresponsiveness of activated monocytes. Taken together, the regulatory LY6E pathway in monocytes represents one of negative feedback mechanisms that counterbalance monocyte activation, which might be caused by LPS translocation through the compromised gastrointestinal tract during persistent HIV-1 infection and may serve as a potential target for immune intervention.
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Pressure dependence of the forward and backward rates of 9-tert-butylanthracene Dewar isomerization.
J Phys Chem A
PUBLISHED: 06-30-2014
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9-tert-Butylanthracene undergoes a photochemical reaction to form its strained Dewar isomer, which thermally back-reacts to reform the original molecule. When 9-tert-butylanthracene is dissolved in a polymer host, we find that both the forward and reverse isomerization rates are pressure-dependent. The forward photoreaction rate, which reflects the sum of contributions from photoperoxidation and Dewar isomerization, decreases by a factor of 1000 at high pressure (1.5 GPa). The back-reaction rate, on the other hand, increases by a factor of ?3 at high pressure. Despite being highly strained and higher volume, the back-reaction reaction rate of the Dewar isomer is at least 100× less sensitive to pressure than that of the bi(anthracene-9,10-dimethylene) photodimer studied previously by our group. These results suggest that the high pressure sensitivity of the bi(anthracene-9,10-dimethylene) photodimer reaction is not just due to the presence of strained four-membered rings but instead relies on the unique molecular geometry of this molecule.
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Comparison of the sorption behaviors and mechanisms of perfluorosulfonates and perfluorocarboxylic acids on three kinds of clay minerals.
Chemosphere
PUBLISHED: 05-08-2014
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The sorption of four perfluoroalkyl acids (PFAAs) [perfluorooctane sulfonate (PFOS), perfluorohexane sulfonate (PFHxS), perfluorooctanoic acid (PFOA) and perfluorohexanoic acid (PFHxA)] on three typical minerals [montmorillonite (MM), kaolinite (KL) and hematite (HM)] was studied. The sorption of PFOS and PFHxS was much stronger than PFOA and PFHxA. The sorption of each PFAA on the minerals followed an order of HM>KL>MM, even though MM was positively while KL and HM were negatively charged, implying that the sorption is driven by some other interactions besides electrostatic attraction. The sorption decreased with an increase in pH and a decrease in ionic strength of the solution, and their impacts on PFOS were much stronger than other three PFAAs. Surface complexing and hydrogen-bonding could make great contributions to the sorption of PFOS on the minerals. The results are important for understanding the transport and fate of PFAAs in sediment and ground water.
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Biochars derived from various crop straws: characterization and Cd(II) removal potential.
Ecotoxicol. Environ. Saf.
PUBLISHED: 04-29-2014
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Five types of biochars prepared from four crop straws and one wood shaving at 600 °C were characterized, and their sorption to Cd(II) were determined to investigate the differences in capacity to function as sorbents to heavy metals. Surface areas and pore volumes of the biochars were inversely correlated to the lignin content of raw biomass. The biochars derived from crop straws displayed more developed pore structure than wood char due to the higher lignin content of wood. Sorption capacity of the biochars to Cd(II) followed the order of corn straw>cotton straw>wheat straw>rice straw>poplar shaving, which was not strictly consistent with the surface area of the chars. The surface characteristics of chars before and after Cd(II) sorption were investigated with scanning electron microscopy equipped with an energy dispersive X-ray spectroscopy and Fourier transform infrared spectroscopy, which suggested that the higher sorption of Cd(II) on corn straw chars was mainly attributed to cation exchange, surface precipitation of carbonate, and surface complexation with oxygen-containing groups. This study indicated that crop straw biochars exhibit distinct sorption capacities to heavy metals due to various surface characteristics, and thus the sorption efficiency should be carefully evaluated specific to target contaminant.
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Distribution of perfluoroalkyl substances (PFASs) with isomer analysis among the tissues of aquatic organisms in Taihu Lake, China.
Environ. Pollut.
PUBLISHED: 04-15-2014
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The distribution of perfluoroalkyl substances (PFASs) and the isomers of perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) was investigated among various tissues (including muscle, gill, kidney, liver) and eggs, in aquatic organisms in Taihu Lake, China. Highest concentration of ?PFASs was mostly found in liver (278-685 ng/g ww) and eggs (66.0-467 ng/g ww) while the lowest was in muscle (40.6-165 ng/g ww). n-PFOS was the predominant PFOS isomer in most of the tissues with a proportion of 46.3-96.5%. Ratios of PFAS concentrations in eggs to those in liver (E/L) increased positively with the protein-water partition coefficient. The E/L of PFOS isomers descended in the order: linear > monomethyl > diperfluoromethyl isomers. The liver/muscle and kidney/muscle ratios of n-PFOS were higher than branched isomers, suggesting that n-PFOS has higher binding affinity with hepatic proteins or branched isomers are preferentially excreted though liver and kidney.
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Novel mesoporous graphite carbon nitride/BiOI heterojunction for enhancing photocatalytic performance under visible-light irradiation.
ACS Appl Mater Interfaces
PUBLISHED: 03-25-2014
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A novel organic-inorganic three-dimensional (3D) mesoporous graphite carbon nitride/BiOI (MCN/BiOI) heterojunction photocatalyst with excellent visible-light-driven photocatalytic performance was synthesized by a facile solvothermal method and used for degradation of bisphenol A (BPA) in water. After hybridization with MCN, a heterojunction was formed and the photogenerated carriers could be effectively separated by the internal electric field built at the heterojunction interface. The photocatalytic and photoelectrochemical performance of BiOI were improved and much higher than pure BiOI and MCN. The best photocatalytic performance was achieved with MCN proportion of 10%, and the kobs was approximately 1.6 times of pure BiOI and 3.4 times of MCN under simulated solar light irradiation, respectively. The photocurrent intensity generated by 10%-MCN/BiOI electrode was about 1.5 and 2.0 times of those induced by BiOI and MCN under visible-light irradiation, respectively. The superoxide radical species were predominant in the reaction system.
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Perfluoroalkyl acids and the isomers of perfluorooctanesulfonate and perfluorooctanoate in the sera of 50 new couples in Tianjin, China.
Environ Int
PUBLISHED: 03-21-2014
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A total of 100 serum samples from 50 new couples (none of the females in this study has ever been pregnant) in Tianjin, North China, were analyzed for eleven perfluoroalkyl acids (PFAAs) with isomer-specific method. Among all samples, total perfluorooctanesulfonate (?PFOS, mean 11.3 ng/mL) was predominant followed by total perfluorooctanoate (?PFOA, 2.95 ng/mL), perfluorodecanoate (PFDA, 1.17 ng/mL), perfluorononanoate (PFNA, 0.93 ng/mL) and perfluorohexanesulfonate (PFHxS, 0.67 ng/mL). The mean concentrations of ?PFOS and PFHxS in males (14.2 and 0.89 ng/mL) were significantly higher (p=0.001) than in females (8.36 and 0.45 ng/mL). No statistical difference between genders was observed for the other PFAAs. This suggests that menstruation is one important elimination pathway for ?PFOS and PFHxS in females. Linear PFOA was the dominant isomer with mean proportion of 99.7%, suggesting that telomeric PFOA (and its precursors), which contains almost pure linear isomer, might be the dominant exposure source of PFOA in Tianjin. On average, the proportion of linear PFOS (n-PFOS) was 59.2% of ?PFOS, which was lower than that in technical PFOS products (ca. 70% linear). Except perfluoroisopropyl PFOS, all the other monomethyl branched PFOS isomers were enriched in human serum compared to the commercial products, suggesting the monomethyl branched PFOS precursors were preferentially biotransformed in humans.
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Boosting functional avidity of CD8+ T cells by vaccinia virus vaccination depends on intrinsic T-cell MyD88 expression but not the inflammatory milieu.
J. Virol.
PUBLISHED: 02-19-2014
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T-cell functional avidity is a crucial determinant for efficient pathogen clearance. Although recombinant DNA priming coupled with a vaccinia-vectored vaccine (VACV) boost has been widely used to mount robust CD8+ T-cell responses, how VACV boost shapes the properties of memory CD8+ T cells remains poorly defined. Here, we characterize the memory CD8+ T cells boosted by VACV and demonstrate that the intrinsic expression of MyD88 is critical for their high functional avidity. Independent of selection of clones with high-affinity T-cell receptor (TCR) or of enhanced proximal TCR signaling, the VACV boost significantly increased T-cell functional avidity through a decrease in the activation threshold. VACV-induced inflammatory milieu is not sufficient for this improvement, as simultaneous administration of the DNA vaccine and mock VACV had no effects on the functional avidity of memory CD8+ T cells. Furthermore, reciprocal adoptive transfer models revealed that the intrinsic MyD88 pathway is required for instructing the functional avidity of CD8+ T cells boosted by VACV. Taking these results together, the intrinsic MyD88 pathway is required for the high functional avidity of VACV-boosted CD8+ T cells independent of TCR selection or the VACV infection-induced MyD88-mediated inflammatory milieu.
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Trophic magnification and isomer fractionation of perfluoroalkyl substances in the food web of Taihu Lake, China.
Environ. Sci. Technol.
PUBLISHED: 02-06-2014
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Biomagnification of perfluoroalkyl substances (PFASs) are well studied in marine food webs, but related information in fresh water ecosystem and knowledge on fractionation of their isomers along the food web are limited. The distribution, bioaccumulation, magnification, and isomer fractionation of PFASs were investigated in a food web of Taihu Lake, China. Perfluorooctanesulfonate (PFOS) and perfluorocarboxylates (PFCAs) with longer carbon chain lengths, such as perfluorodecanoate (PFDA) and perfluoroundecanoate (PFUnA), were predominant in organisms, while perfluorohexanoate (PFHxA) and perfluorooctanoate (?PFOA) contributed more in the water phase. The consistent profile signature of PFOA isomers in water phase with 3M electrochemical fluorination (ECF) products suggests that ECF production of PFOA still exists in China. Linear proportions of PFOA, PFOS and perfluorooctane sulfonamide (PFOSA) in the biota were in the range of 91.9-100%, 78.6-95.5%, and 72.2-95.5%, respectively, indicating preferential bioaccumulation of linear isomers in biota. Trophic magnification factors (TMFs) were estimated for PFDA (2.43), perfluorododecanoate (PFDoA) (2.68) and PFOS (3.46) when all biota were included, suggesting that PFOS and long-chained PFCAs are biomagnified in the fresh water food web. The TMF of PFOS isomers descended in the order: n-PFOS (3.86) > 3+5m-PFOS (3.35) > 4m-PFOS (3.32) > 1m-PFOS (2.92) > m2-PFOS (2.67) > iso-PFOS (2.59), which is roughly identical to their elution order on a FluoroSep-RP Octyl column, suggesting that hydrophobicity may be an important contributor for isomer discrimination in biota.
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Organic photomechanical materials.
Chemphyschem
PUBLISHED: 01-27-2014
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Organic molecules can transform photons into Angstrom-scale motions by undergoing photochemical reactions. Ordered media, for example, liquid crystals or molecular crystals, can align these molecular-scale motions to produce motion on much larger (micron to millimeter) length scales. In this Review, we describe the basic principles that underlie organic photomechanical materials, starting with a brief survey of molecular photochromic systems that have been used as elements of photomechanical materials. We then describe various options for incorporating these active elements into a solid-state material, including dispersal in a polymer matrix, covalent attachment to a polymer chain, or self-assembly into molecular crystals. Particular emphasis is placed on ordered media, such as liquid-crystal elastomers and molecular crystals, that have been shown to produce motion on large (micron to millimeter) length scales. We also discuss other mechanisms for generating photomechanical motion that do not involve photochemical reactions, such as photothermal expansion and photoinduced charge transfer. Finally, we identify areas for future research, ranging from the study of basic phenomena in solid-state photochemistry, to molecular and host matrix design, and the optimization of photoexcitation conditions. The ultimate realization of photon-fueled micromachines will likely involve advances spanning the disciplines of chemistry, physics and engineering.
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Concentration profiles and spatial distribution of perfluoroalkyl substances in an industrial center with condensed fluorochemical facilities.
Sci. Total Environ.
PUBLISHED: 01-24-2014
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Jiangsu Hi-tech Fluorochemical Industry Park, China, is one of the largest fluorochemical industry centers in Asia and could be a point source of polyfluoroalkyl substances (PFASs) to the surrounding environment. Besides water, sediment and soil samples, tree leaves and bark were also collected to monitor airborne PFASs around the facilities. Perfluorooctanoic acid and short-chain perfluorocarboxylates including perfluorohexanoic acid and perfluoropentanoic acid were found predominantly in all the samples. The target ?PFASs were distributed in the dissolved phase with a proportion of 96.5±2.9%. High concentrations of ?PFASs (up to 12,700 ng/L in surface water) were found at sites near and within the wastewater treatment plant and the facilities. The ?PFASs in the sediment/sludge were in the range of 3.33-324 ng/g dw. For the first time, tree samples were used for bio-monitoring airborne PFASs in the environment. The ?PFASs in the tree leaf and bark samples were in the range of 10.0-276 and 6.76-120 ng/g dw, respectively. The spatial distribution of ?PFASs in the tree leaves suggested that airborne PFASs could be transported from the center to the surrounding environment by prevailing wind.
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Willingness to Participate in HIV Therapeutic Vaccine Trials among HIV-Infected Patients on ART in China.
PLoS ONE
PUBLISHED: 01-01-2014
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More and more HIV therapeutic vaccines will enter clinical trials; however, little is known about the willingness to participate (WTP) in HIV therapeutic vaccine trials among HIV-positive individuals.
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Polydiacetylene-based high-throughput screen for surfactin producing strains of Bacillus subtilis.
PLoS ONE
PUBLISHED: 01-01-2014
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Although traditional mutation is still an attractive approach for strain improvement, it is tedious, time-consuming, and inefficient to screen for surfactin producing strains. To overcome this, we developed a high-throughput screening method for surfactin producing mutants by applying polydiacetylene (PDA) vesicles as sensors with visible chromatic change from blue to red, detected as colorimetric response (CR%) signal, which can even semi-quantify the yields of surfactin. Bacillus subtilis 723 was used as parent strain and multiply mutated with atmospheric and room temperature plasma (ARTP). Mutants were cultured in MicroFlask by Duetz (24 square deepwell plates, Applikon Biotechnology) and surfactin titers were tested in 96-well plates with PDA vesicles. Mutants with surfactin titers above150 mg/L (CR% value above 26%) were selected as high-yield strains and further quantified by HPLC. By integrating MicroFlask cultivation and the PDA vesicles detection, we screened 27,000 mutants and found 37 high-yield strains. From these, one mutant produced 473.6 mg/L surfactin (including 353.1 mg/L C15 surfactin), which was 5.4-fold than that of the parent strain. This method is efficient, cost-effective and provides wider application in screening for various surfactants.
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MCPIP1 restricts HIV infection and is rapidly degraded in activated CD4+ T cells.
Proc. Natl. Acad. Sci. U.S.A.
PUBLISHED: 11-04-2013
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HIV-1 primarily infects activated CD4+ T cells and macrophages. Quiescent CD4+ T cells, however, possess cellular factors that limit HIV-1 infection at different postentry steps of the viral life cycle. Here, we show that the previously reported immune regulator monocyte chemotactic protein-induced protein 1 (MCPIP1) restricts HIV-1 production in CD4+ T cells. While the ectopic expression of MCPIP1 in cell lines abolished the production of HIV-1, silencing of MCPIP1 enhanced HIV-1 production. Subsequent analysis indicated that MCPIP1 imposes its restriction by decreasing the steady levels of viral mRNA species through its RNase domain. Remarkably, common T-cell stimuli induced the rapid degradation of MCPIP1 in both T-cell lines and quiescent human CD4+ T cells. Lastly, blocking the proteosomal degradation of MCPIP1 by MG132 abrogated HIV-1 production in phorbol 12-myristate 13-acetate/ionomycin-stimulated human CD4+ T cells isolated from healthy donors. Overall, MCPIP1 poses a potent barrier against HIV-1 infection at a posttranscriptional stage. Although the observed HIV restriction conferred by MCPIP1 does not seem to be overcome by any viral protein, it is removed during cellular stimulation. These findings provide insights into the mechanisms of cellular activation-mediated HIV-1 production in CD4+ T cells.
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Fc-independent phagocytosis: implications for IVIG and other therapies in immune-mediated thrombocytopenia.
Cardiovasc Hematol Disord Drug Targets
PUBLISHED: 09-12-2013
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Phagocytes were first described by Dr. Metchnikoff in 1873. The roles of phagocytes in innate and adaptive immunity have been well established to date, although the molecular mechanisms involved in initiating phagocytosis (through Fc or other receptors) remain to be further explored. Phagocytes in the reticuloendothelial system, particularly macrophages, have been implicated in the clearance of senescent blood cells. The destruction of these cells may be primarily mediated via an Fc-independent pathway. Fc-independent phagocytosis may also play an important role in platelet clearance, including in autoimmune thrombocytopenia (ITP), and in clearance of platelet-rich emboli detached from sites of vascular injury. In ITP, the two major platelet auto-antigens have been located on glycoprotein (GP)IIbIIIa and the GPIb complex. It has been demonstrated that anti-GPIb antibodies, in contrast to anti-GPIIbIIIa, can induce thrombocytopenia in an Fc-independent manner. We further demonstrated in an animal model that intravenous IgG (IVIG) is unable to ameliorate thrombocytopenia caused by most anti-GPIb antibodies, despite its efficacy in anti- GPIIbIIIa-mediated thrombocytopenia. Our data was supported by subsequent retrospective studies with ITP patients by several independent groups. Most recently, we found that anti-GPIb-mediated ITP was also resistant to steroid therapy and that platelet activation and apoptosis induced by anti-GPIb antibodies may be involved in the Fc-independent platelet clearance. Therefore, identification of antibody specificity in patients, e.g. anti-GPIIbIIIa (Fc-dependent) versus anti-GPIb (Fc-independent), may be important for therapies against ITP, as well as other immune-mediated thrombocytopenias.
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Biomonitoring of perfluoroalkyl acids in human urine and estimates of biological half-life.
Environ. Sci. Technol.
PUBLISHED: 08-27-2013
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Perfluoroalkyl acids (PFAAs) are persistent and bioaccumulative compounds that have been associated with adverse health outcomes. In human blood, PFAAs exist as both linear and branched isomers, yet for most linear homologues, and for all branched isomers, elimination rates are unknown. Paired blood and urine samples (n = 86) were collected from adults in China. They were analyzed by a sensitive isomer-specific method that permitted the detection of many PFAAs in human urine for the first time. For all PFAAs except perfluoroundecanoate (PFUnA), levels in urine correlated positively with levels in blood. Perfluoroalkyl carboxylates (PFCAs) were excreted more efficiently than perfluoroalkane sulfonates (PFSAs) of the same carbon chain-length. In general, shorter PFCAs were excreted more efficiently than longer ones, but for PFSAs, perfluorooctanesulfonate (PFOS, a C8 compound) was excreted more efficiently than perfluorohexanesulfonate (PFHxS, a C6 compound). Among PFOS and perfluorooctanoate (PFOA) isomers, major branched isomers were more efficiently excreted than the corresponding linear isomer. A one-compartment model was used to estimate the biological elimination half-lives of PFAAs. Among all PFAAs, the estimated arithmetic mean elimination half-lives ranged from 0.5 ± 0.1 years (for one branched PFOA isomer, 5m-PFOA) to 90 ± 11 years (for one branched PFOS isomer, 1m-PFOS). Urinary excretion was the major elimination route for short PFCAs (C ? 8), but for longer PFCAs, PFOS and PFHxS, other routes of excretion likely contribute to overall elimination. Urinary concentrations are good biomarkers of the internal dose, and this less invasive strategy can therefore be used in future epidemiological and biomonitoring studies. The very long half-lives of long-chain PFCAs, PFHxS, and PFOS isomers in humans stress the importance of global and domestic exposure mitigation strategies.
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Mutual impacts of wheat (Triticum aestivum L.) and earthworms (Eisenia fetida) on the bioavailability of perfluoroalkyl substances (PFASs) in soil.
Environ. Pollut.
PUBLISHED: 07-28-2013
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Wheat and earthworms were exposed individually and together to soils contaminated with 11 perfluoroalkyl substances (PFASs). Wheat accumulated PFASs from soil with root concentration factors and bioconcentration factors that decreased as the number of perfluorinated carbons in the molecule increased. Earthworms accumulated PFASs from soil with biota-to-soil accumulation factors that increased with the number of carbons. Translocation factors (TF) of perfluorinated carboxylates (PFCAs) in wheat peaked at perfluorohexanoic acid and decreased significantly as the number of carbons increased or decreased. Perfluorohexane sulfonate produced the greatest TF of the three perfluorinated sulfonates (PFSAs) examined. Wheat increased the bioaccumulation of all 11 PFASs in earthworms and earthworms increased the bioaccumulation in wheat of PFCAs containing seven or less perfluorinated carbons, decreased bioaccumulation of PFCAs with more than seven carbons, and decreased bioaccumulation of PFSAs. In general, the co-presence of wheat and earthworms enhanced the bioavailability of PFASs in soil.
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Serum levels of perfluoroalkyl acids (PFAAs) with isomer analysis and their associations with medical parameters in Chinese pregnant women.
Environ Int
PUBLISHED: 07-09-2013
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Perfluoroalkyl acids (PFAAs) are a group of chemicals used for many applications and widely present in the environment and humans. In this study, serum levels of PFAAs and isomers of perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) were analyzed in 141 Chinese pregnant women. Among all the samples, total PFOS (?PFOS, mean concentration 7.32ng/mL) was predominant, followed by ?PFOA (mean 4.78ng/mL) and perfluorodecanoate (PFDA, mean 1.45ng/mL). On average, the proportion of linear PFOS (n-PFOS) was 66.7% of ?PFOS, which was higher than the general population, implying that maternal women could excrete branched PFOS isomers to the fetus by transplacental transfer. Moreover, the proportion of n-PFOS decreased significantly with the increasing concentration of ?PFOS in the serum samples (r=-0.342, p<0.001). The mean proportion of n-PFOA in the serum samples was 99.0%, which was much higher than the technical ECF (electrochemical fluorination) products (ca. 70%). The small proportion of branched isomers of PFOA suggests that there is still a source of ECF PFOA in China. Significant correlations (p<0.005) were observed between the concentrations of some PFAAs with certain medical parameters in the pregnant women. For example, the levels of most perfluorinated carboxylic acids (PFCAs) were found to correlate with albumin significantly, which might be a sign of immunotoxicity of these chemicals. The adverse effects of PFAA exposure to pregnant women may increase the health risk of the fetus. Interestingly, not only the PFAA concentrations but also the percentages of PFOS and PFOA isomers were correlated with certain medical parameters. This implies that the compositions of PFOS or PFOA should be considered in human health risk assessment in the future.
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Study on parameter optimization for support vector regression in solving the inverse ECG problem.
Comput Math Methods Med
PUBLISHED: 05-09-2013
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The typical inverse ECG problem is to noninvasively reconstruct the transmembrane potentials (TMPs) from body surface potentials (BSPs). In the study, the inverse ECG problem can be treated as a regression problem with multi-inputs (body surface potentials) and multi-outputs (transmembrane potentials), which can be solved by the support vector regression (SVR) method. In order to obtain an effective SVR model with optimal regression accuracy and generalization performance, the hyperparameters of SVR must be set carefully. Three different optimization methods, that is, genetic algorithm (GA), differential evolution (DE) algorithm, and particle swarm optimization (PSO), are proposed to determine optimal hyperparameters of the SVR model. In this paper, we attempt to investigate which one is the most effective way in reconstructing the cardiac TMPs from BSPs, and a full comparison of their performances is also provided. The experimental results show that these three optimization methods are well performed in finding the proper parameters of SVR and can yield good generalization performance in solving the inverse ECG problem. Moreover, compared with DE and GA, PSO algorithm is more efficient in parameters optimization and performs better in solving the inverse ECG problem, leading to a more accurate reconstruction of the TMPs.
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Cell morphology variations of Klebsiella pneumoniae induced by acetate stress using biomimetic vesicle assay.
Appl. Biochem. Biotechnol.
PUBLISHED: 04-15-2013
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Supplementation with acetate under low levels was used as a novel approach to control the morphological development of Klebsiella pneumoniae aimed to improve 1,3-propanediol (1,3-PD) production. A full range of morphological types formed from rod shape to oval shape even round shape in response to different concentrations of acetate. The cell growth and 1,3-PD productions in the shake flasks with 0.5 g/L acetate addition were improved by 9.4 and 28.37%, respectively, as compared to the control, while the cell became shorter and began to lose its original shape. The cell membrane penetration by acetate was investigated by the biomimetic vesicles, while higher concentration of acetate led to more moderate colorimetric transitions. Moreover, the percentage composition of unsaturated fatty acid (UFA) was increased as well as the increased concentrations of acetate, whereas higher UFA percentage, higher fluidity of bacterial cell membrane.
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Enhanced cytotoxicity of pentachlorophenol by perfluorooctane sulfonate or perfluorooctanoic acid in HepG2 cells.
Chemosphere
PUBLISHED: 03-18-2013
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Chlorinated phenols and perfluoroalkyl acids (PFAAs) are two kinds of pollutants which are widely present in the environment. Considering liver is the primary toxic target organ for these two groups of chemicals, it is interesting to evaluate the possible joint effects of them on liver. In this work, the combined toxicity of pentachlorophenol (PCP) and perfluorooctane sulfonate (PFOS) or perfluorooctanoic acid (PFOA) were investigated using HepG2 cells. The results indicated that PFOS and PFOA could strengthen PCPs hepatotoxicity. Further studies showed that rather than intensify the oxidative stress or promote the biotransformation of PCP, PFOS (or PFOA) might lead to strengthening of the oxidative phosphorylation uncoupling of PCP. By measuring the intracellular PCP concentration and the cell membrane properties, it was suggested that PFOS and PFOA could disrupt the plasma membrane and increase the membrane permeability. Thus, more cellular accessibility of PCP was induced when they were co-exposed to PCP and PFOS (or PFOA), leading to increased cytotoxicity. Further research is warranted to better understand the combined toxicity of PFAAs and other environmental pollutants.
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Mechanistic understanding of tetracycline sorption on waste tire powder and its chars as affected by Cu(2+) and pH.
Environ. Pollut.
PUBLISHED: 02-19-2013
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The sorption characteristics of tetracycline (TC) by waste tire powder and its chars were investigated to explore the potential of using waste tires as effective sorbents for removal of TC from aqueous solution. Naphthalene (NAPH), a typical hydrophobic organic compound, was selected as asorbate for comparison. TC displayed much lower sorption affinity to tire powder than NAPH. However, it exhibited similar adsorption affinity as NAPH on the pyrolyzed tire chars, which was mainly attributed to ?-? electron-donor-acceptor interactions of TC with the graphite surface of chars. TC and Cu(2+) could mutually facilitate the sorption of each other on both tire powder and pyrolyzed chars in a wide pH range. This could be explained by the metallic complexation and/or surface-bridging mechanisms (i.e., Cu- or TC-bridging). However, Cu(2+) and NAPH depressed the sorption of each other on tire powder and displayed negligible impact to each other on the highly pyrolyzed chars.
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Sediment quality guidelines: challenges and opportunities for improving sediment management.
Environ Sci Pollut Res Int
PUBLISHED: 01-30-2013
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During the International Conference on Deriving Environmental Quality Standards for the Protection of Aquatic Ecosystems held in Hong Kong in December 2011, an expert group, comprising scientists, government officials, and consultants from four continents, was formed to discuss the important scientific and regulatory challenges with developing sediment quality guidelines (SQGs). We identified the problems associated with SQG development and made a series of recommendations to ensure that the methods being applied were scientifically defensible and internationally applicable. This document summarizes the key findings from the expert group. To enable evaluation of current SQG derivation and application systems, a feedback mechanism is required to communicate confounding factors and effects in differing environments, while field validation is necessary to gauge the effectiveness of SQG values in sediment quality assessments. International collaboration is instrumental to knowledge exchange and method advancement, as well as promotion of best practices. Since the paucity of sediment toxicity data poses the largest obstacle to improving current SQGs and deriving new SQGs, a standardized international database should be established as an information resource for sediment toxicity testing and monitoring data. We also identify several areas of scientific research that are needed to improve sediment quality assessment, including determining the importance of dietary exposure in sediment toxicity, mixture toxicity studies, toxicity screening of emerging chemicals, how climate change influence sediments and its biota, and possible use of new toxicity study approaches such as high throughput omic-based toxicity screenings.
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Bioaccumulation of perfluoroalkyl carboxylates (PFCAs) and perfluoroalkane sulfonates (PFSAs) by earthworms (Eisenia fetida) in soil.
Environ. Pollut.
PUBLISHED: 01-18-2013
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Earthworms were exposed to artificially contaminated soils with ten perfluoroalkyl substances (PFASs). PFASs with longer perfluorinated carbon chain displayed higher uptake rate coefficients (k(u)), longer half-life (t(½)) and time to steady-state (t(ss)) but lower elimination rate coefficients (k(e)) than the shorter ones. Similarly, perfluorosulfonates acids (PFSAs) displayed higher ku, longer t(½) and tss but lower ke than perflurocarboxylic acids (PFCAs) with the same perfluorinated chain length. All the studied PFASs, including those with seven or less perfluorinated carbons, were bioaccumulated in the earthworms and the biota-to-soil accumulation factors (BSAFs) increased with perfluorinated carbon chain length and were greater for PFSAs than for PFCAs of equal perfluoroalkyl chain length. The BSAFs were found to be dependent on the concentrations of PFASs in soil and decreased as the level of PFASs in soil increased.
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Enhanced photocatalytic performance of boron doped Bi?WO? nanosheets under simulated solar light irradiation.
J. Hazard. Mater.
PUBLISHED: 01-14-2013
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Bi?WO6 doped with different amounts of boron atoms (0.1, 0.5, 1.0, 5.0 and 10% B) were synthesized using hydrothermal method and their photocatalytic activities to degrade rhodamine B (RhB) under simulated solar light was investigated. The successful incorporation of B atoms in Bi?WO? was proved by FT-IR, Raman spectra and XPS. Doping with B could affect the pore structure and volume. 0.5% B/Bi?WO? displayed more mesopores with higher total pore volume than pure Bi?W?; while the pores of 10% B/Bi?WO? mainly distributed in microporous range with much less total pore volume. As a result, 0.5% B/Bi?WO? displayed stronger adsorption capacity to RhB, favoring the photodegradation. In addition, the doped B atoms could act as electron traps and facilitate the separation of photogenerated electron-hole pairs due to its electron deficient and oxytropic characteristics. 0.5% B/Bi?WO? displayed the highest photocatalytic activity under simulated solar light with rate constant (kobs) 8.8 times of that using pure Bi?WO?. Its photoactivity was affected by solution pH and the optimum was achieved at pH 7. At this condition, around 100% of RhB (10(-5)mol/L) was degraded in 180 min. The photogenerated holes were the main active species responsible for the photodegradation of RhB by B/Bi?WO?.
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Isomers of perfluorooctanesulfonate and perfluorooctanoate and total perfluoroalkyl acids in human serum from two cities in North China.
Environ Int
PUBLISHED: 01-08-2013
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The sources and pathways of human exposure to perfluoroalkyl acids (PFAAs) are not well characterized, particularly in China where many perfluorinated substances are now manufactured. Here, isomer-specific PFAA analysis was used for the first time to evaluate exposure sources for Chinese people, by applying the method to 129 serum samples collected in two typical cities (Shijiazhuang and Handan) in North China. Among all samples, total perfluorooctanesulfonate (?PFOS, mean 33.3 ng/ml) was the predominant PFAA followed by perfluorohexanesulfonate (2.95 ng/ml), total perfluorooctanoate (?PFOA, 2.38 ng/ml), and perfluorononanoate (0.51 ng/ml). The level of ?PFOS was higher than in people from North America in recent years. The mean concentrations of ?PFAAs in the participants living in urban Shijiazhuang (59.0 ng/ml) and urban Handan (35.6 ng/ml) were significantly higher (p<0.001 and p=0.041, respectively) than those living in the rural district of Shijiazhuang (24.3 ng/ml). The young female sub-population had the lowest ?PFAA concentrations compared with older females and all males. On average, the proportion of linear PFOS (n-PFOS) was only 48.1% of ?PFOS, which is much lower than what was present in technical PFOS from the major historical manufacturer (ca. 70% linear), and which is also lower than data reported from any other countries. Moreover, the proportion of n-PFOS decreased significantly with increasing ?PFOS concentration in the serum samples (r=-0.694, p<0.001). Taken together, the data lend weight to previous suggestions that i) high branched PFOS content in serum is a biomarker of exposure to PFOS-precursors, and ii) that people with the highest ?PFOS concentrations are exposed disproportionately to high concentrations of PFOS-precursors. On average, linear PFOA (n-PFOA) contributed 96.1% of ?PFOA, significantly higher than in technical PFOA (ca. 75-80% linear), but lower than in Americans, suggesting higher exposure to electrochemically fluorinated PFOA than in other countries, including the United States.
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Relative efficacy of steroid therapy in immune thrombocytopenia mediated by anti-platelet GPIIbIIIa versus GPIb? antibodies.
Am. J. Hematol.
PUBLISHED: 09-06-2011
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Immune thrombocytopenia (ITP) is characterized by platelet clearance mediated primarily by autoantibodies against the platelet GPIIbIIIa and/or GPIb?. Steroid therapy is a first-line treatment for ITP. However, some patients are refractory to this therapy and currently no method can predict which patients will respond. To evaluate whether steroids are equally efficacious in treating patients with ITP caused by anti-GPIIbIIIa versus anti-GPIb? antibodies, we performed a retrospective study on 176 newly diagnosed patients with acute ITP who had severe bleeding symptoms and were admitted as resident patients to the hospital. The patients were treated first with intravenous administration of high-dose dexamethasone (DXM), followed by oral administration of prednisone. Response to therapy was observed in a majority of patients with antibodies specific for GPIIbIIIa (31/43) or without detectable antibodies against either GPIIbIIIa or GPIb? (36/45). In contrast, the steroid response was significantly lower in patients with anti-GPIb? antibodies (9/34) or with antibodies against both GPIb? and GPIIbIIIa (16/54). The preliminary findings of this study suggest that in future prospective clinical trials including corticosteroids, the anti-GPIb?, and -GPIIbIIIa status should be assessed in order to test its potential relevance in deciding future treatments.
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Photodegradation of perfluorooctanoic acid by synthesized TiO2-MWCNT composites under 365nm UV irradiation.
Chemosphere
PUBLISHED: 08-16-2011
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Degradation of perfluorooctanoic acid (PFOA) is of great importance due to its global distribution, persistence and toxicity to bioorganisms. In present study, a composite TiO(2) with multiple wall carbon nanotubes (MWCNTs) was synthesized using sol-gel method and it was used as photocatalyst to degrade PFOA in water. The prepared composite catalyst displayed significant absorption in UV to visible light region. The loading content of TiO(2) on MWCNTs could be adjusted by changing the ratio of precursor to MWCNTs. Due to the combined effect of the adsorption ability and e(-) transport capacity of MWCNT, the composites displayed much higher photocatalytic ability to PFOA as compared to pure TiO(2) under UV irradiation. The photocatalyst prepared with 10:1 of tetrabutyl titanate/MWCNT was the most effective. With the optimal dosage at 1.6 g L(-1), almost 100% of PFOA was degraded in acid medium after irradiation for 8h. It was proposed that PFOA were mainly degraded by stepwise losing a moiety of CF(2).
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Photolytic reaction mechanism and impacts of coexisting substances on photodegradation of bisphenol A by Bi2WO6 in water.
Water Res.
PUBLISHED: 07-27-2011
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Bi(2)WO(6) displayed great photolytic degradation efficiency to bisphenol A (BPA) under simulated solar light irradiation but its reaction mechanism and the impacts of coexisting substances on the degradation remain unclear. In present study, the reaction mechanism was investigated using DMPO spin-trapping ESR spectra and experiments with scavengers of hydroxyl radicals (*OH) and holes. The results supported that hole oxidation mainly governed the photodegradation process. As a common humic substance in natural water, humic acid accelerated the degradation of BPA when its concentration was 1mg/L, while the photodegradation was impeded with the increase of humic acid concentration in the range of 5-20mg/L. Almost all anions, including NO(3)(-), HCO(3)(-), Cl(-), SO(4)(2-) inhibited the degradation of BPA by Bi(2)WO(6) and their inhibition effects followed the order of SO(4)(2-)>Cl(-)>HCO(3)(-)>NO(3)(-). Cations of Na(+), K(+), Ca(2+) and Mg(2+) displayed slight suppressing effect on BPA degradation mainly due to the impact of Cl(-) coexisting in the solution. However, Cu(2+) hindered the BPA photodegradation heavily. Fe(3+) and H(2)O(2) affected the photodegradation in a complicated way: they suppressed or promoted the photodegradation depending on their concentrations. This could be the result of competition between photolyitc hole generated by Bi(2)WO(6) and OH produced by Fe(3+) or H(2)O(2.).
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Reversible photoinduced twisting of molecular crystal microribbons.
J. Am. Chem. Soc.
PUBLISHED: 07-27-2011
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9-Anthracenecarboxylic acid, a molecule that undergoes a reversible [4 + 4] photodimerization, is prepared in the form of oriented crystalline microribbons. When exposed to spatially uniform light irradiation, these photoreactive ribbons rapidly twist. After the light is turned off, they relax back to their original shape over the course of minutes. This photoinduced motion can be repeated for multiple cycles. The final twist period and cross-sectional dimensions of individual microribbons are measured using a combination of atomic force and optical microscopies. Analysis of this data suggests that the reversible twisting involves the generation of interfacial strain within the ribbons between unreacted monomer and photoreacted dimer regions, with an interaction energy on the order of 3.4 kJ/mol. The demonstration of reversible twisting without the need for specialized irradiation conditions represents a new type of photoinduced motion in molecular crystals and may provide new modes of operation for photomechanical actuators.
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Removal of Cd2+ from contaminated water by nano-sized aragonite mollusk shell and the competition of coexisting metal ions.
J Colloid Interface Sci
PUBLISHED: 06-30-2011
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The potential of using nano-sized aragonite mollusk shell (nano-Bio-ARA) to remove Cd(2+) from contaminated water was investigated by comparing the sorption kinetics and isotherms with the nano-sized calcite-type mollusk shell (nano-Bio-CAL) and nano-sized geological calcite (nano-Geo-CAL). Nano-Bio-ARA displayed extremely high sorption capacity to Cd(2+) (8.91mmol/g), much higher than nano-Bio/Geo-CAL, and many other natural or engineered materials. The results of thermodynamic experiments indicated that the sorption of Cd(2+) on the nano-ARA was a spontaneous and endothermic process. The coexisting metals in the solution displayed competition effect to the sorption of Cd(2+) on nano-Bio-ARA in the following order: Cu(2+)>Cr(3+)>Pb(2+)>Zn(2+)>Ca(2+). EDTA impeded the sorption of Cd(2+) on nano-Bio-ARA due to its strong chelating capacity to Cd(2+) in the solution. The results demonstrate that nano-Bio-ARA is a potential high-effective material to treat Cd(2+) contaminated water.
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Simultaneous adsorption and degradation of ?-HCH by nZVI/Cu bimetallic nanoparticles with activated carbon support.
Environ. Pollut.
PUBLISHED: 06-06-2011
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Cu amended zero valent iron bimetallic nanoparticles were synthesized by doping Cu on the surface of iron. They were incorporated with granular activated carbon (AC) to prepare supported particles (AC-Fe(0)-Cu), which were used to remove ?-HCH. Cu on the surface of iron enhanced the dechlorination activity of Fe(0). The dechlorination rate constant (k(obs)) increased with the Cu loading on the surface of iron and the maximum was achieved with 6.073% Cu. AC as a support was effective for increasing the dispersion of the nanoparticles and avoiding the agglomeration of the metallic nanoparticles. The simultaneous adsorption of ?-HCH on AC accelerated the degradation rate of ?-HCH by the bimetals. After reaction for 165 min, around 99% of ?-HCH was removed by the solids of AC-Fe(0)-Cu. In addition, AC could adsorb the degradation products. The degradation of ?-HCH was mainly through dehydrochlorination and dichloroelmination based on the intermediate products detected by GC/MS.
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Biosorption of divalent Pb, Cd and Zn on aragonite and calcite mollusk shells.
Environ. Pollut.
PUBLISHED: 03-26-2011
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The potential of using mollusk shell powder in aragonite (razor clam shells, RCS) and calcite phase (oyster shells, OS) to remove Pb(2+), Cd(2+) and Zn(2+) from contaminated water was investigated. Both biogenic sorbents displayed very high sorption capacities for the three metals except for Cd on OS. XRD, SEM and XPS results demonstrated that surface precipitation leading to crystal growth took place during sorption. Calcite OS displayed a remarkably higher sorption capacity to Pb than aragonite RCS, while the opposite was observed for Cd. However, both sorbents displayed similar sorption capacities to Zn. These could be due to the different extent of matching in crystal lattice between the metal bearing precipitate and the substrates. The initial pH of the solution, sorbents dosage and grain size affected the removal efficiency of the heavy meals significantly, while the organic matter in mollusk shells affected the removal efficiency to a lesser extent.
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Predicting the bioavailability of sediment-associated polybrominated diphenyl ethers using a 45-d sequential Tenax extraction.
Chemosphere
PUBLISHED: 03-03-2011
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A 45-d Tenax extraction was used to evaluate the bioavailability of polybrominated diphenyl ethers (PBDEs) in three spiked sediments. The effect of aging on desorption kinetics of PBDEs was investigated by incubating one of the sediments for 7, 14, 30 and 60 d at room temperature. Desorption kinetics were well described by a three-compartment model. The fraction of very slow desorption (Fvs) contributed the most of the desorbed PBDEs from sediments. The total desorption amount of PBDEs decreased with the increase of total organic carbon in the sediments, suggesting that organic matter is an important factor controlling the partition of PBDEs in sediments. The total desorption amount of PBDEs decreased while log [(Fslow+Fvs)/Frap] increased with logKow of PBDE congeners, indicating that the bioavailability of PBDEs in sediment decreases with logKow of the congeners. As the residential time of PBDEs in the sediment increased from 7 to 60 d, Frap of individual PBDE congeners decreased gradually with simultaneous increase of Fvs. There was a good positive correlation between Frap and F6/F24, indicating that either 6 h or 24 h Tenax extraction could be a proxy for Frap and bioavailability. In general, the results in present study suggest that the bioavailability of nona- and deca-BDEs in sediment is very low due to their strong hydrophobicity and large molecular size.
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Application of kernel principal component analysis and support vector regression for reconstruction of cardiac transmembrane potentials.
Phys Med Biol
PUBLISHED: 02-23-2011
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Non-invasively reconstructing the transmembrane potentials (TMPs) from body surface potentials (BSPs) constitutes one form of the inverse ECG problem that can be treated as a regression problem with multi-inputs and multi-outputs, and which can be solved using the support vector regression (SVR) method. In developing an effective SVR model, feature extraction is an important task for pre-processing the original input data. This paper proposes the application of principal component analysis (PCA) and kernel principal component analysis (KPCA) to the SVR method for feature extraction. Also, the genetic algorithm and simplex optimization method is invoked to determine the hyper-parameters of the SVR. Based on the realistic heart-torso model, the equivalent double-layer source method is applied to generate the data set for training and testing the SVR model. The experimental results show that the SVR method with feature extraction (PCA-SVR and KPCA-SVR) can perform better than that without the extract feature extraction (single SVR) in terms of the reconstruction of the TMPs on epi- and endocardial surfaces. Moreover, compared with the PCA-SVR, the KPCA-SVR features good approximation and generalization ability when reconstructing the TMPs.
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Comparative study on composition, structure, and adsorption behavior of activated carbons derived from different synthetic waste polymers.
J Colloid Interface Sci
PUBLISHED: 02-06-2011
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The composition, structure, and adsorption behavior of activated carbons (ACs) derived from three different types of waste polymers, i.e., tire rubber (TR), polyvinyl chloride (PVC), and polyethyleneterephtalate (PET), by KOH activation were compared. The AC derived from PET exhibited the largest surface area (2831 m(2)/g) and pore volume (1.68 cm(3)/g) due to the homogenous aromatic composition of PET. The AC derived from PVC exhibited relatively lower surface area (2666 m(2)/g) but more narrowed pore size distribution (2-3 nm). The complex composition and high ash content of tire particles resulted in AC product with significantly lower surface area (398.5 m(2)/g) and heterogeneous pore width. Adsorption data of methylene blue (MB) were fitted well by Langmuir equation, indicating monolayer coverage on the ACs. The high oxygen content of PET-derived AC heavily affected its adsorption to MB and iodine. Due to the remarkable surface area and highly mesoporous structures, ACs based on both PET and PVC exhibited much higher adsorption capacities than that of TR and commercial coal-based AC (F400). This study demonstrates that the properties of ACs are highly dependent on their starting polymers and the potential of converting synthetic polymer waste into effective adsorbents for environmental remediation and cleanup.
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Bioaccumulation kinetics of sediment-associated DE-83 in benthic invertebrates (Nereis succinea, polychaete).
Chemosphere
PUBLISHED: 01-26-2011
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Polychaetes (Nereis succinea) were exposed to DE-83 contaminated sediments to investigate the bioaccumulation and bioavailability of nona- and deca-BDEs in sediment. All the major congeners in DE-83 were bioavailable to the lugworms. The uptake coefficients (K(s)) of nona- and deca-BDE congeners in lugworms were in the range of 0.18-0.65 (d(-1)), with the values of BDE-207 and -208 slightly higher than those of BDE-206 and -209. Elimination of nona- and deca-BDE congeners from lugworms was very fast. The estimated half-lives of nona- and deca-BDE congeners in the lugworms were at 0.7d. The bioavailability of nona- and deca-BDE congeners was very low, with BSAF of 0.017 for BDE-206 and -209 and 0.054 for BDE-207 and -208. These may be due to the large molecular size and high affinity of PBDEs to sediment particles. The contribution of BDE-206 in the profile of nona-BDEs in lugworm tissue decreased with exposure time while those of BDE-207 and -208 increased, which could be the result of the biotransformation of BDE-209 to BDE-207 and -208.
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Occurrence and partition of perfluorinated compounds in water and sediment from Liao River and Taihu Lake, China.
Chemosphere
PUBLISHED: 01-18-2011
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The concentrations of four perfluorinated sulfonate acids (PFSAs) and 10 perfluorinated carboxylate acids (PFCAs) were measured in water and sediment samples from Liao River and Taihu Lake, China. In the water samples from Taihu Lake, PFOA and PFOS were the most detected perfluorinated compounds (PFCs); in Liao River, PFHxS was the predominant PFC followed by PFOA, while PFOS was only detected in two of the samples. This suggests that different PFC products are used in the two regions. PFOS and PFOA in both watersheds are at similar level as in the rivers of Japan, but significantly lower than in Great Lakes. The contributions of PFOS and long chain PFCAs in sediments were much higher than in water samples of both watersheds, indicating preferential partition of these PFCs in sediment. The concentrations of PFOS and PFOA were three orders of magnitude of lower than that of polycyclic aromatic hydrocarbons in the same sediments. The average sediment-water partition coefficients (log K(oc)) of PFHxS, PFOS and PFOA were determined to be 2.16, 2.88 and 2.28 respectively.
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Sorption of apolar and polar organic contaminants by waste tire rubber and its chars in single- and bi-solute systems.
Environ. Pollut.
PUBLISHED: 01-04-2011
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Single- and bi-solute sorption of organic compounds [1,3-dichlorbenzene (DCB), 1,3-dinitrobenzene (DNB) and 2,4-dichlorophenol (DCP)] on ground tire rubber and its chars was studied. The chars were prepared by pyrolyzing tire rubber at different temperatures (200-800 °C). Their surface area, aromaticity and hydrophobicity increase greatly with pyrolytic temperature, and the polymeric phase is partly converted into a condensed phase. The sorption of DNB and DCP increases with pyrolytic temperature and is characterized by a transition from a partition dominant to an adsorption dominant process. However, the sorption of DCB linearly decreases with the pyrolytic temperature. The enhanced adsorption of DNB and DCP on carbonized phase is primarily attributed to nonhydrophobic interactions such as ?-? electron-donor-acceptor interactions and/or H bonding. The higher partition of DCB to polymeric phase is attributed to its high hydrophobicity. Competitive sorption between DCB and DCP on the tire chars is highly dependent on dissociation of the latter.
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Bioaccumulation and distribution of polybrominated diphenyl ethers in marine species from Bohai Bay, China.
Environ. Toxicol. Chem.
PUBLISHED: 09-28-2010
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Polybrominated diphenyl ethers (PBDEs) were analyzed in invertebrate and fish species collected from Bohai Bay, China in 2007 to 2008. The concentrations of the 16 detected PBDE congeners were in the range of 1.4 to 425 and 2.9 to 767 ng/g lipid for invertebrates and fish, respectively. The summed concentrations of the six major PBDE congeners (BDE-28, 47, 99, 100, 153, 154) (?(6)PBDEs) in fish were significantly higher than in invertebrates, while demersal fish concentrations were higher than pelagic fish. The congeners BDE-47, 99, and 100 contributed more in viscera or liver than in muscle, indicating that the metabolic capability of the viscera or liver is greater than that of muscle. The ratio of BDE-47/99 was relatively higher in fish than in invertebrate samples, suggesting a more developed metabolism capacity in fish. Polybrominated diphenyl ether congeners tend to accumulate in viscera or liver rather than in muscle. The fully brominated congener BDE-209 was detected in some species, suggesting that it can be accumulated by organisms. Uptake from sediment may be the major uptake pathway for most brominated PBDEs in benthic species.
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Degradation and mineralization of bisphenol A by mesoporous Bi2WO6 under simulated solar light irradiation.
Environ. Sci. Technol.
PUBLISHED: 08-14-2010
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Bismuth tungstate (Bi2WO6) catalysts of different morphology were synthesized with a hydrothermal method by controlling the pH of the reaction solution. The properties of the synthesized catalysts were characterized and all catalysts presented high photoabsorption capacity in the range of UV light to visible light around 450 nm. The surface area of the catalysts decreased but the crystallinity increased with the pH of the hydrothermal reaction solution in the range of 4-11. It was found that the crystallinity of the catalysts played an important role on their degradation capacity to Bisphenol A (BPA). Bi2WO6 catalyst prepared at pH 11 displayed a mesoporous structure and it showed the highest photocatalytic activity to degrade BPA under simulated solar light irradiation. Nearly 100% of BPA with original concentration at 20 ppm was removed after 30 min irradiation in a solution with pH 10 and Bi2WO6 amount of 1.0 g L(-1). Furthermore, 86.6 and 99.1% of the total organic carbon was eliminated after 60 and 120 min irradiation, respectively. Only one intermediate at m/z 133 was observed by LC/MS and a simple pathway of BPA degradation by Bi2WO6 was proposed.
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Determination of rutin on the poly(p-aminobenzene sulfonic acid) modified glassy carbon electrode.
Chem. Pharm. Bull.
PUBLISHED: 04-23-2010
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The electrochemical behaviors of rutin at a poly(p-aminobenzene sulfonic acid) modified glassy carbon electrode (PABSA/GC) have been investigated. Rutin can generate a pair of well-defined redox peaks at the PABSA/GC located at 0.440 V (E(pa)) and 0.396 V (E(pc)) (vs. saturated calomel electrode (SCE)), respectively. The results indicate that the reaction involves two electrons transfer, accompanied by two protons and the electrochemical process is controlled by adsorption. The electrochemical parameters of rutin on the modified electrode were calculated with the results of the charge transfer coefficient (alpha), the number of electron transfer (n) and the electrode reaction rate constant (k(s)) as 0.61, 2.08 and 2.18 s(-1), respectively. Under the selected conditions, the oxidation peak current was linear to the rutin concentration over the range of 2.5x10(-7)-1.0x10(-5) M with a detection limit of 1.0x10(-7) M. The proposed method has been successfully applied to the determination of compound rutin tablets with no interference from the coexisting ascorbic acid.
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Bioaccumulation and bioavailability of polybrominated diphenyl ethers [corrected] (PBDEs) in soil.
Environ. Pollut.
PUBLISHED: 04-13-2010
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Earthworms were exposed to artificially contaminated soils of DE-71 and DE-79 to investigate the bioaccumulation and bioavailability of PBDEs in soil. All major congeners were bioavailable to earthworms. The uptake and elimination rate coefficients of PBDEs decreased with their logK(ow)s. The biota soil accumulation factors of PBDEs also declined with logK(ow). These may be due to the large molecular size and the high affinity of PBDEs to soil particles. The concentrations extracted by Tenax for 6 h correlated very well with those found in earthworms, suggesting that the bioavailability of PBDEs in soil is related to the fraction of rapid desorption from soil. This also indicates that 6 h Tenax extraction is a good proxy for the bioavailability of PBDEs to earthworms in soil. The BSAFs of PBDEs in aged soil decreased 22-84% compared to freshly spiked soil, indicating that aging may diminish the bioavailability of PBDEs in soil significantly.
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Electronic energy migration on different time scales: concentration dependence of the time-resolved anisotropy and fluorescence quenching of Lumogen Red in poly(methyl methacrylate).
J Phys Chem A
PUBLISHED: 02-23-2010
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Electronic energy transfer plays an important role in many types of organic electronic devices. Forster-type theories of exciton diffusion provide a way to calculate diffusion constants and lengths, but their applicability to amorphous polymer systems must be evaluated. In this paper, the perylenediimide dye Lumogen Red in a poly(methyl methacrylate) host matrix is used to test theories of exciton motion over Lumogen Red concentrations (C(LR)s) ranging from 1 x 10(-4) to 5 x 10(-2) M. Two experimental quantities are measured. First, time-resolved anisotropy decays in films containing only Lumogen Red provide an estimate of the initial energy transfer rate from the photoexcited molecule. Second, the Lumogen Red lifetime decays in mixed systems where the dyes Malachite Green and Rhodamine 700 act as energy acceptors are measured to estimate the diffusive quenching of the exciton. From the anisotropy measurements, it is found that theory accurately predicts both the C(LR)(-2) concentration dependence of the polarization decay time tau(pol), as well as its magnitude to within 30%. The theory also predicts that the diffusive quenching rate is proportional to C(LR)(alpha), where alpha ranges between 1.00 and 1.33. Experimentally, it is found that alpha = 1.1 +/- 0.2 when Malachite Green is used as an acceptor, and alpha = 1.2 +/- 0.2 when Rhodamine 700 is the acceptor. On the basis of the theory that correctly describes the anisotropy data, the exciton diffusion constant is projected to be 4-9 nm(2)/ns. By use of several different analysis methods for the quenching data, the experimental diffusion constant is found to be in the range of 0.32-1.20 nm(2)/ns. Thus the theory successfully describes the early time anisotropy data but fails to quantitatively describe the quenching experiments which are sensitive to motion on longer time scales. The data are consistent with the idea that orientational and energetic disorder leads to a time-dependent exciton migration rate, suggesting that simple diffusion models cannot accurately describe exciton motion within this system.
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Brominated flame retardants in serum from the general population in northern China.
Environ. Sci. Technol.
PUBLISHED: 10-08-2009
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In 2006, 128 serum samples were collected from three populations in Tianjin, China: office cleaners, university students, and policemen. These samples were all analyzed for polybrominated diphenyl ethers (PBDEs) and for other brominated flame retardants (BFRs). The median concentration of total PBDEs (sum of 41 congeners) was 7.1 ng/g lipid, ranging from 0.48 to 1980 ng/g lipid. Among these PBDE congeners, the median sum of the tri- to hepta-PBDE (SigmaPBDE3-7) congener concentrations was 2.9 ng/g lipid, ranging from 0.48 to 20 ng/g lipid. The most common tri- to heptabrominated congeners were BDE-47 (30% of total), BDE-99 (24%), BDE-183 (15%), BDE-153 (12%), BDE-28 (9.5%), and BDE-100 (6.2%). These levels of SigmaPBDE3-7 were similar to those observed in Europe and Asia but were much lower than those observed in North America. Highly brominated BDE congeners were detected in some serum samples. In particular, BDE-209 was detected in 28 samples; the median BDE-209 concentration in these samples was 42 ng/g lipid, ranging from ND to 1770 ng/g lipid. The total PBDE levels in office cleaners were significantly higher than in university students and policemen. In addition, we also measured several other BFRs. Hexabromobenzene (HBB) was identified in 26 samples with a median concentration of 0.27 ng/g lipid, ranging from 0.11 to 1.50 ng/g lipid. Pentabromoethylbenzene (PBEB), hexabromocyclododecane (HBCD), 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE), and decabromodiphenylethane (DBDPE) were not detected in any of these samples.
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[Research progress of pharmaceutical and personal care products on ecological and human health].
Wei Sheng Yan Jiu
PUBLISHED: 05-05-2009
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EU (European Union) and Center of Water Pollution and Control in the United States have continued to measure persistent bioaccumulate and toxic (PB&T) chemicals and persistent organic pollutants (POPs) since the 1970s. In resent years, Pharmaceutical and personal care products (PPCPs) have raised more concern among chemists and toxicologists. The present paper introduced the main properties of PPCPs and their present situation of research. Additionally, the potential toxicites of PPCPs to ecological and human health were detailedly reviewed in this article.
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Immobilization of lead and cadmium from aqueous solution and contaminated sediment using nano-hydroxyapatite.
Environ. Pollut.
PUBLISHED: 04-17-2009
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The effectiveness and mechanism of nano-hydroxyapatite particles (nHAp) in immobilizing Pb and Cd from aqueous solutions and contaminated sediment were investigated. The maximum sorption amount (Q(max)) of Pb and Cd in aqueous solution was 1.17 and 0.57 mmol/g. The X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) surface and depth analysis indicated that dissolution-precipitation is the primary immobilization mechanism for Pb, while surface complexation and intraparticle diffusion account for Cd sequestration. Different amounts of nHAp (0-10% nHAp/dry weight) were added to the contaminated sediment. Sequential extraction showed that nHAp could effectively reduce the exchangeable fraction of Pb and Cd in the sediment and significantly reduce the concentration in porewater. The results in this study showed that nHAp can immobilize Pb and Cd in sediment effectively.
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Activated toxicity of diesel particulate extract by ultraviolet a radiation in mammalian cells: role of singlet oxygen.
Environ. Health Perspect.
PUBLISHED: 04-02-2009
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Diesel exhaust [diesel exhaust particles (DEPs) and their extracts (DPE)] and ultraviolet A radiation (UVA) are two ubiquitous environmental factors that have been identified as essential risk factors for various benign or malignant human diseases, either alone or in combination with other agents.
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Enhanced radiation damage in irradiated and non-irradiated bystander regions by co-exposure to myosmine.
Mutat. Res.
PUBLISHED: 04-01-2009
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It is important to evaluate the health effects of radiation concurrent exposure to chemicals in our daily life. Myosmine, an alkaloid in tobacco plants and various edibles and staple foods, has been considered as a co-genotoxic agent in vitro. In the present study, the damage induced by radiation concurrent exposure to myosmine was assessed in human primary cell line AG1522. Myosmine at 5 or 10 mM for 3 h treatment induced a significantly dose-dependent increase in micronucleus (MN) frequencies, but not for 1 mM. However, 1 mM myosmine distinctly enhanced MN frequencies in both irradiated and non-irradiated bystander regions after different doses (0.2, 1 and 10 cGy) of alpha-particle irradiation. Treatment with c-PTIO, a nitric oxide (NO) scavenger, the induced fractions of MN frequencies were dramatically inhibited both in 1 cGy alpha-particle irradiated and non-irradiated bystander regions with or without myosmine treatment. Moreover, 1mM myosmine treatment distinctly enhanced gamma-H2AX foci formation in both 1 cGy alpha-particle irradiated and non-irradiated bystander regions. These data indicated that myosmine effectively enhanced the low dose alpha-particle-induced DNA damage in both irradiated and non-irradiated bystander regions and nitric oxide played a very important role in such process.
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Distribution of polybrominated diphenyl ethers in breast milk from North China: implication of exposure pathways.
Chemosphere
PUBLISHED: 01-31-2009
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The breast milk concentrations of polybrominated diphenyl ethers (PBDEs; sum of eight congeners: BDE-28, 47, 99, 100, 153, 154, 183 and 209) were determined (by high resolution gas chromatographic high resolution mass spectrometry) in samples from primiparous women collected in 2006 in Tianjin, China. Dietary and lifestyle habits of the participants were obtained by questionnaires. The median total PBDE concentration (including BDE-28, 47, 99, 100, 153, 154, 183) was 2500 pg g(-1) lipid weight, ranging from 1700 to 4500 pg g(-1) lipid weight. These levels were in the same range as those from Europe and Japan but much lower than those from North America. The congener profile in China was also different from other countries. The contribution of BDE-28 was around 15%, much higher than any other country, implying that a different Penta-BDE formulation might be used in the Chinese market. The lower ratio of the sum of BDE-47, 99, and 100 to the sum of BDE-153 and 154 suggested that Octa-products were in more demand in China. A significant correlation was found between a womans PBDE concentration and the time she used electronic appliances (h/d). This implies that electronics are a potential source of PBDEs to people. Inhalation or ingestion of particulate matter (such as dust) may also be an important exposure pathway. There was no significant correlation between the PBDE concentration and the consumption of meat, fish, and milk. Further research is needed to determine the specific contribution of each exposure route and their health effects.
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Effects of chemical oxidation on sorption and desorption of PAHs in typical Chinese soils.
Environ. Pollut.
PUBLISHED: 01-08-2009
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In situ chemical oxidation is a commonly applied soil and groundwater remediation technology, but can have significant effects on soil properties, which in turn might affect fate and transport of organic contaminants. In this study, it was found that oxidation treatment resulted mainly in breakdown of soil organic matter (SOM) components. Sorption of naphthalene and phenanthrene to the original soils and the KMnO(4)-treated soils was linear, indicating that hydrophobic partitioning to SOM was the predominant mechanism for sorption. Desorption from the original and treated soils was highly resistant, and was well modeled with a biphasic desorption model. Desorption of residual naphthalene after treating naphthalene-contaminated soils with different doses of KMnO(4) also followed the biphasic desorption model very well. It appears that neither changes of soil properties caused by chemical oxidation nor direct chemical oxidation of contaminated soils had a noticeable effect on the nature of PAH-SOM interactions.
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Sorption and resistant desorption of atrazine in typical Chinese soils.
J. Environ. Qual.
PUBLISHED: 01-01-2009
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Atrazine is one of the most commonly used herbicides and is produced and used in large quantity worldwide. In the present study, the sorption and desorption of atrazine in five typical Chinese soils were examined. The sorption of atrazine followed the conventional linear isotherm reasonably well, indicating that sorption was driven largely by hydrophobic partitioning into soil organic matter. However, strong resistant desorption (desorption hysteresis) was observed for all five soils. The desorption data could be well modeled with several biphasic sorption/desorption isotherms that include a quasi-Langmuir or a Freundlich term to account for the nonlinear sorptive property associated with the desorption-resistant fraction. Experimental observations in the present study are consistent with studies reported in the literature and with our previous work with other hydrophobic organic compounds and different sorbents. These observations suggest that physical entrapment within porous soil matrix was likely the predominant mechanism controlling the observed desorption resistance. The unique characteristics associated with the resistant-desorption fraction have important implications for risk assessment of atrazine-contaminated soil/sediment and should be taken into account in the regulation, management, and remediation of atrazine-contaminated sites.
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Bioaccumulation and distribution of perfloroalkyl acids in seafood products from Bohai Bay, China.
Environ. Toxicol. Chem.
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Ten perfluoroalkyl acids (PFAAs) were measured in seafood collected from Bohai Bay, China in 2010. The summed concentrations of the PFAAs were in the ranges of not detected to 194 ng/g dry weight and 4.0 to 304 ng/g dry weight for invertebrates and fish, respectively. The levels of perflurooctanesulfonate (PFOS) and perfluorooctanoic acid (PFOA) in the seafood were lower than those from North America, the Mediterranean Sea, and South Korea. Living habitat, trophic level, and feeding habits had important impacts on the bioaccumulation and distribution of PFAAs in the seafood. The species at higher trophic levels had the potential to accumulate more PFAAs than benthic invertebrates. Tidal-flat organisms tended to accumulate more PFOA than PFOS, whereas the opposite was seen for shallow-water species. For all the species, PFOS and PFOA were partitioned preferentially in the liver or viscera. Risk assessment indicated that the current level of PFAAs in the seafood of Bohai Bay does not represent an immediate source of harm to public health.
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Distribution and desorption of perfluorinated compounds in fractionated sediments.
Chemosphere
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This study provides particle-scale understanding of perfluorinated compounds (PFCs) distribution in sediments collected from two locations in Tianjin, China. The sediments were fractionated according to particle size and density. Even though lower density carbonaceous fractions contributed only 17.8-22.3% of the total sediment mass, they displayed stronger affinity to PFCs with much higher PFC concentrations than in the heavy fractions. Hydrophobic interaction predominated the partition of longer chain PFCs while electrostatic interaction could affect the sorption of short chain PFCs in sediment fractions. The individual PFC concentrations increased with increasing perfluorocarbon chain length, and the concentrations of perfluoroalkanesulfonates (PFSAs) in the same sediment fraction were higher than perfluorocarboxylates (PFCAs) with the same chain length. Log K(oc) was in the range of 1.70-3.80 for C5-C12 PFCAs and 1.75-2.97 for C4-C8 PFSAs. Desorption experiments indicated desorption became difficult as the chain length increased, and PFSAs were harder to be desorbed than the corresponding PFCAs.
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Pressure catalyzed bond dissociation in an anthracene cyclophane photodimer.
J. Am. Chem. Soc.
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The anthracene cyclophane bis-anthracene (BA) can undergo a [4 + 4] photocycloaddition reaction that results in a photodimer with two cyclobutane rings. We find that the subsequent dissociation of the dimer, which involves the rupture of two carbon-carbon bonds, is strongly accelerated by the application of mild pressures. The reaction kinetics of the dimer dissociation in a Zeonex (polycycloolefin) polymer matrix were measured at various pressures and temperatures. Biexponential reaction kinetics were observed for all pressures, consistent with the presence of two different isomers of bis(anthracene). One of the rates showed a strong dependence on pressure, yielding a negative activation volume for the dissociation reaction of ?V(++) = -16 Å(3). The 93 kJ/mol activation energy for the dissociation reaction at ambient pressure is lowered by more than an order of magnitude from 93 to 7 kJ/mol with the application of modest pressure (0.9 GPa). Both observations are consistent with a transition state that is stabilized at higher pressures, and a mechanism for this is proposed in terms of a two-step process where a flattening of the anthracene rings precedes rupture of the cyclobutane rings. The ability to catalyze covalent bond breakage in isolated small molecules using compressive forces may present opportunities for the development of materials that can be activated by acoustic shock or stress.
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Bioaccumulation and metabolism of polybrominated diphenyl ethers in carp (Cyprinus carpio) in a water/sediment microcosm: important role of particulate matter exposure.
Environ. Sci. Technol.
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Microcosms were built up to simulate a pond system with polybrominated diphenyl ether (PBDE) contaminated sediment and bioorganisms. The microcosms were divided into groups A and B. In group A, both benthic invertebrates (tubificid worms) and carp (Cyprinu carpio) were added, while in group B, only fish were added. After exposure for 20 d, the fish were sampled (exposure I). A net was fixed in the microcosms, and new fish were added (exposure II). These fish were prohibited from contacting the sediment by the net, and the accumulation and depuration of PBDEs in the fish were investigated. Among 11 monitored PBDE congeners (BDE-28, BDE-47, BDE-99, BDE-100, BDE-153, BDE-154, BDE-183, BDE-206, BDE-207, BDE-208, and BDE-209), only 5 congeners (BDE-28, BDE-47, BDE-100, BDE-153, and BDE-154) were detected in the carp fillets and liver. BDE-99 and BDE-183 were not detected in the fish because of the efficient metabolic debromination in carp tissues. The uptake of PBDEs in exposure I was significantly higher/faster than that in exposure II, since the fish in exposure I had an opportunity to take in more of the highly contaminated particles. The uptake kinetics (k(s)) and elimination (k(e)) rate coefficients showed a general trend of decreasing with increasing log K(ow). No significant difference was observed in uptake/depuration kinetics between groups A and B, indicating that the tubificids reworking does not affect the bioaccumulation of sediment-associated PBDEs in fish significantly. All the PBDE congeners, including nona- and deca-BDEs, were bioaccumulated in the tubificid worms. The PBDE concentrations in the worms were significantly higher than those in the fish, and the congener profile of the sevem major congeners (BDE-28, BDE-47, BDE-99, BDE-100, BDE-153, BDE-154, and BDE-183) was distinctly different from that of fish tissues. The biota-sediment accumulation factors in the worms ranged from 0.01 to 5.89 and declined with increasing bromination and log K(ow.).
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Photocatalytic degradation efficiency and mechanism of microcystin-RR by mesoporous Bi?WO? under near ultraviolet light.
Environ. Sci. Technol.
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Microcystin-RR (MC-RR) is one of the most common cyanotoxin microcystins in fresh water and is of great concern due to its potential hepatotoxicity. In the present study, Bi(2)WO(6) was synthesized with a hydrothermal method by varying the pH of the reaction solution in the range of 1-11. The surface area of the catalysts decreased, but the crystallinity and crystal size increased with the pH. The adsorption and degradation capacities of the catalysts decreased with increasing the preparation solution pH. The Bi(2)WO(6) prepared at pH 1 (Bi(2)WO(6)-pH1) displayed the highest adsorption and degradation capacity to MC-RR even though it consisted of randomly aggregated particles. Nearly 100% of MC-RR at 10 mg L(-1) was removed after 30 min of irradiation of near-ultraviolet light (300-400 nm) in a solution with Bi(2)WO(6) concentration of 0.2 g L(-1). The photodegradation efficiency of Bi(2)WO(6)-pH1 was greater in acid medium than in basic solutions. Several intermediate products were observed and identified by liquid chromatography/mass spectrometry/mass spectrometry, and a unique photodegradation pathway was proposed. It was assumed that a photo-Kolbe process happened at the site carboxyl acid group of the d-Glu residue by the photogenerated holes, producing a hydroperoxyl product at m/z 513.8. This intermediate could be further decomposed to an alcohol product at m/z 505.8 and a ketone product at m/z 504.8. The aromatic ring and diene bond of the Adda chain could also be attacked by the holes and form phenol and diol products.
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