Using the molecular electronegativity distance vector descriptors derived directly from the molecular topological structures, the relative retention time （RRT） of polybrominated diphenyl ethers （PBDEs） were predic...Using the molecular electronegativity distance vector descriptors derived directly from the molecular topological structures, the relative retention time （RRT） of polybrominated diphenyl ethers （PBDEs） were predicted. A four-variable regression model （M30） with the correlation coefficient of 0.9816 and the root mean square errors of 0.061 was developed using a training set including 30 PBDEs. The correlation coefficient of 0.9841 and the root mean square errors of 0.054 between the values of RRT predicted by M30 and the RRT observed for 16 external PBDEs show a good predictive potential of M30. The descriptors included in the M30 represent four interactions between four pairs of atom types, i.e., atom -C= and -C=, -C= and 〉C=, 〉C= and 〉C=, -C= and -Br.展开更多
Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway...Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway of anaerobic degradation.On the basis of experimental study,Octa-BDE 197,Hepta-BDE 183,Hexa-BDE 153,Penta-BDE 99 and Tetra-BDE 47 were selected as the initial degradation objects,and their debromination degradation were studied using density functional theory.The structures were optimized by Gaussian 09 program.Furthermore,the molecular orbitals and charge distribution were analyzed.All C-Br bond dissociation energies at different positions including ortho,meta and para bromine atoms were calculated and the sequence of debromination was obtained.There is a close relationship between molecular structure,charge,molecular orbital and C-Br bond.All PBDEs exhibited similar debromination pathways with preferential removal of meta and para bromines.展开更多
To understand potential ecotoxicological effects of electrical and electronic equipment waste （e-waste） recycling and polybrominated diphenyl ethers （PBDEs） bioaccumulation in loaches, a semi-field experiment usin...To understand potential ecotoxicological effects of electrical and electronic equipment waste （e-waste） recycling and polybrominated diphenyl ethers （PBDEs） bioaccumulation in loaches, a semi-field experiment using Chinese loach （Misgurnus anguiUicaudatus） as experimental fish was performed. Larval loaches were kept in net-cage for three months in an e-wastes recycling site and a reference site in Southeastern China. There was significant difference of the survival rate between the loaches from the e-wastes recycling site （27%, 19/70） and from reference site （70%, 49/70）. Histopathological responses were also found in all the livers examined in loaches from the e-wastes recycling site. These results showed that mixed pollutants resulted from e-wastes recycling led to ecotoxicological effects on loaches. The bioaccumulation of polybrominated diphenyl ethers （PBDEs）, the main pollutants in e-waste, in loaches was also studied, the mean concentration of total PBDEs in sediment was 6726.17 ng/g wet weight and in water samples was 4.08 ng/L （dissolved phase）. BDE 209 was the dominant congener in sediment and with relatively high concentration in water. Relatively low concentration of BDE 209 （less than 0.01% of total PBDEs） and high concentration of BDE47 （up to 39.34% of total PBDEs） were detected in loaches.展开更多
We measured 39 polybrominated diphenyl ethers （PBDEs） in the muscle tissue of three species of fish （Sciaenops ocellatus,Sparus macrocephalus,and Lateolabrax japonicus） and four species of shellfish （Tegillarca g...We measured 39 polybrominated diphenyl ethers （PBDEs） in the muscle tissue of three species of fish （Sciaenops ocellatus,Sparus macrocephalus,and Lateolabrax japonicus） and four species of shellfish （Tegillarca granosa,Cyclina sinensis,Sinonovacula constricta,and Ostrea cucullata） that were collected downstream of electronic-waste recycling plants in Taizhou,China.A total of 24 PBDE congeners （PBDE 24） in the samples were detected.The PBDE 24 （total PBDE） ranged from 545.4 to 1688.7 ng/kg ww （wet weight）.The mean PBDE 24 concentration was 1382.6 ng/kg ww in fish and 858.1 ng/kg ww in shellfish.The lower brominated congeners were detected at relatively high concentrations in all species.The penta-products,produced from e-waste,were found at relatively low levels.A principal component analysis suggested a significant correlation among di-,tri-,tetra-,and hepta-BDEs for the three species of fish.Similarly,we found a significant correlation between mono-and tri-BDEs in the shellfish.Our results suggested that the processes of PBDE metabolism and elimination were similar in both fish and shellfish.In addition,the primary source of PBDEs appeared to be from the debromination of high brominated PBDEs.展开更多
Sixty sediment samples were collected from the main Songhua River in three years. Twelve polybrominated diphenyl ether( PBDE) congeners( BDE17,28,47,66,99,100,153,154,138,183,and BDE-209) were detected to state the po...Sixty sediment samples were collected from the main Songhua River in three years. Twelve polybrominated diphenyl ether( PBDE) congeners( BDE17,28,47,66,99,100,153,154,138,183,and BDE-209) were detected to state the pollution situation. The results showed that the total concentration of total PBDEs ranges from 0. 424 to 23. 0 ng / g dry weight,with the mean of 3. 02 ng / g,and the total PBDEs concentration is at relative low level compared with those worldwide. The congener profile showed that BDE-209 is the dominant congener that accounts for more than 80. 1% of total PBDEs in sediments,followed by BDE-47 and BDE-99. These profiles are consistent with a high consumption of Deca-BDEs for the brominated flame retardant market in China. The results of spatial and seasonal observations indicated that local sources,temperature variation, and hydrologic conditions are significant factors on PBDEs concentrations. Hazard quotients suggested that PBDEs pose no potential risk to benthic organisms in detected area at present.展开更多
Objective To explore the effects of prenatal exposure to polybrominated diphenyl ethers(PBDEs)on placental size and birth outcomes.Methods Based on the perspective Wenzhou Birth Cohort,this nested case-control study i...Objective To explore the effects of prenatal exposure to polybrominated diphenyl ethers(PBDEs)on placental size and birth outcomes.Methods Based on the perspective Wenzhou Birth Cohort,this nested case-control study included 101 fetal growth restriction(FGR)and 101 healthy newborns.Maternal serum samples were collected during the third trimester and measured for PBDEs by gas chromatography tandem mass spectrometry.The basic information of mother-newborn pairs was collected from questionnaires,whereas the placental size and birth outcomes of newborns were obtained from hospital records.Results A total of 19 brominated diphenyle ether(BDE)congeners were detected in maternal serum samples.Higher concentrations of BDE-207,-208,-209,and∑19PBDEs were detected in FGR cases than in controls.Increased BDE-207,-208,-209,and∑19PBDEs levels in maternal serum were related to decreased placental length,breadth,surface area,birth weight,birth length,gestational age,and Quetelet index of newborns.After adjusting for confounders,BDE-207 and∑19PBDE concentrations in maternal serum were significantly associated with an increased risk of FGR.Conclusion A negative association was found between PBDE levels in maternal serum and placental size and birth outcomes.Prenatal PBDE exposure may be associated with elevated risk of the incidence of FGR birth.展开更多
PBDEs are widely used brominated flame retardant, which are increasingly reported in the environment. Concentrations of thirteen PBDEs in a large number of channel catfish and fish feeds collected from Hubei province ...PBDEs are widely used brominated flame retardant, which are increasingly reported in the environment. Concentrations of thirteen PBDEs in a large number of channel catfish and fish feeds collected from Hubei province of China were investigated in this study. A fast isotopic dilution GC-MS method was firstly developed to simultaneously determine thirteen PBDEs in channel catfish and fish feeds in this study, and especially for the first time PBDEs in fish feeds. Pressurized liquid extraction and multi-layer silica gel column chromatography cleanup were used, some important steps and crucial parameters were modified and intensified compared with other literatures, and GC and MS conditions were optimized. The limits of quantitation values of 0.25 - 5 μg·kg-1 wet weight in channel catfish were calculated for PBDEs;so did 1 - 20 μg·kg-1 wet weight in fish feeds. In addition, good repeatability and accuracy of the whole method were achieved. The established methods were therefore suitable for the simultaneous determinations of thirteen PBDEs in these samples at trace contamination levels. Using the established methods, PBDEs emerged in 10 of 180 channel catfish and 13 of 115 fish feeds, and the dominant PBDEs homologues were PBDE-28, PBDE-47, PBDE-100, PBDE-99, PBDE-154, PBDE-153 and PBDE-183. The detection rates of seven PBDEs congeners were in turn respectively 1.74%, 7.83%, 4.35%, 5.22%, 3.48%, 2.61% and 2.61% in fish feeds, and detection rates of seven PBDEs congeners were in turn respectively 1.11%, 3.89%, 2.22%, 1.67%, 1.11%, 1.11% and 1.11% in channel catfish. There was significant correlation in PBDEs between matching channel catfish and fish feeds (R2 = 0.742, P < 0.001, n = 30), suggesting that fish feeds contaminated with PBDEs possibly resulted in PBDEs residual in channel catfish through biological transfer.展开更多
Objective：To investigate the metabolites of polybrominated diphenyl ether 99（BDE-99）and its related cytochrome P450s in an in vitro system.Methods：Rat primary hepatocytes were isolated and treated with BDE-99 for ...Objective：To investigate the metabolites of polybrominated diphenyl ether 99（BDE-99）and its related cytochrome P450s in an in vitro system.Methods：Rat primary hepatocytes were isolated and treated with BDE-99 for 24-72 h.Metabolites were then extracted from the hepatocytes and media,and detected by GC/MS.Several mRNAs of metabolic enzymes were also extracted from the same cells and the gene expression levels were determined using quantitative real-time PCR.In addition,selected recombinant cytochrome P450s（CYPs） were expressed in a bacurovirus/sf9 system,and these were further used to explore the metabolism of BDE-99 in vitro.The parent depletion approach was used for screening the ability of CYPs to eliminate BDE-99.Results： A reductively debrominated metabolite,BDE-47,and three oxidative metabolites,2,4,5-tribromophenol,5-OH-BDE-47,and 5＇-OH-BDE-99,were identified from the BDE-99-treated rat hepatocytes,whereas no MeO metabolite was detected in the system.RT-PCR analysis showed that CYP 3A23/3A1,1A2,and 2B1/2 were induced by BDE-99.Furthermore,using the heterological expressed CYP proteins in in vitro BDE-99 metabolism experiments we found that CYP1A2 and CYP3A4 showed the highest metabolic efficiency for BDE-99,with the metabolic clearance rates of CYP1A2 and CYP3A4 being 30.3%and 27.7%,respectively.CYP1A1 and CYP2A6 displayed relatively low clearance rates,while CYP2E1 seemed not to be associated with the BDE-99 metabolism.Conclusions：In our in vitro rat primary hepatocyte metabolism system,four metabolites of BDE-99 were identified,and CYP3A4 and CYP1A2 were demonstrated to be involved in the BDE-99 metabolism.展开更多
Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surf...Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surface soil to the vadose zone and groundwater are unclear. Here, colloid-enhanced leaching of PBDEs from undisturbed soil cores collected at an e-waste recycling site in Tianjin, China, is reported. Spatially heterogeneous release of colloids and PBDEs was observed in all the tested soil cores under chemical and hydrodynamic perturbations, indicating the presence of preferential flow paths. Colloid concentration in the effluent significantly increased as ionic strength decreased (from 10 to 0.01 mmol/L), probably due to the stronger electrostatic repulsion between colloidal particles and the soil matrix at lower ionic strength. In contrast, colloid mobilization was not significantly affected by the changes in pH of the influent (from 4.0 to 10.0) and flow rate (from a Darcy velocity of 1.5 to 6.0 cm/h). The concentrations of 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209), the predominant PBDE congener at the site, detected in the leachate (ranging from 1.09 to 3.43 ng/L) were much lower than previously reported results from packed column leaching tests, and were positively correlated with colloid concentrations. This indicates that remobilization of colloids at e-waste recycling sites can promote the leaching and downward migration of PBDEs from surface soil. The findings highlight the potential risk of surface soil PBDE contamination to groundwater quality and call for further understanding of colloid-facilitated transport for predicting the fate of PBDEs at e-waste recycling sites.展开更多
The spatial,temporal,and vertical distributions of polybrominated diphenyl ethers(PBDEs) in water columns from the Zhujiang River Estuary were examined,and the partition behavior of PBDEs between particle and dissolve...The spatial,temporal,and vertical distributions of polybrominated diphenyl ethers(PBDEs) in water columns from the Zhujiang River Estuary were examined,and the partition behavior of PBDEs between particle and dissolved phases was investigated in the present study.The results show that the distributions of PBDEs concentrations in the water varied with the sampling seasons.The PBDEs concentrations in water samples were lower in May 2005,when the brackish water was dominant in the estuary,than in October 2005,when fresh water from river runoff dominated the estuary.The spatial distribution of PBDEs in October 2005 indicated that the river runoff was the major mode to input PBDEs to the estuary,and the concentration of PBDEs in water might be dissolved organic carbon(DOC) dependence.The spatial and vertical distributions of PBDEs in May 2005 were relatively homogeneous,and SPM was the major factor on controlling the levels of PBDEs in this sampling time.Both DOC and POC could play certain roles in determining the distribution and partition of PBDEs between particle and dissolved phases,but their effects varied with the water properties.展开更多
This review focuses on the occurrence and interactions of engineered nanoparticles(ENPs)and brominated flame retardants(BFRs)such as polybrominated diphenyl ethers(PBDEs)in water systems and the generation of highly c...This review focuses on the occurrence and interactions of engineered nanoparticles(ENPs)and brominated flame retardants(BFRs)such as polybrominated diphenyl ethers(PBDEs)in water systems and the generation of highly complex compounds in the environment.The release of ENPs and BFRs(e.g.PBDEs)to aquatic environments during their usage and disposal are summarised together with their key interaction mechanisms.The major interaction mechanisms including electrostatic,van derWaals,hydrophobic,molecular bridging and steric,hydrogen andπ-bonding,cation bridging and ligand exchange were identified.The presence of ENPs could influence the fate and behaviour of PBDEs through the interactions as well as induced reactions under certain conditions which increases the formation of complex compounds.The interaction leads to alteration of behaviour for PBDEs and their toxic effects to ecological receptors.The intermingled compound(ENPs-BFRs)would show different behaviour from the parental ENPs or BFRs,which are currently lack of investigation.This review provided insights on the interactions of ENPs and BFRs in artificial,environmental water systems and wastewater treatment plants(WWTPs),which are important for a comprehensive risk assessment.展开更多
Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing e...Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing effluent and recycling of surfactant solutions.In this study,a molecular imprinting technique was applied to selectively sorb polybrominated diphenyl ethers(PBDEs)in soil washing effluent.The novel molecular imprinted polymers(MIPs)using different template molecules were synthesized by precipitation polymerization.Adsorption behaviors andmechanisms ofMIPs were studied through experiments and theoretical calculations.The results show that 4-bromo-4'-hydroxybiphenyl and toluene can be effective imprinting molecule for MIPs synthesis.The maximal adsorption capacity of selected dummy molecular imprinted polymer(D1-MIP)was 1032.36μmol/g,and that of part molecular imprinted polymer(P-MIP)was 981.13μmol/g.Their imprinting factors in 5 PBDEs adsorption ranged from 2.13 to 5.88,the recovery percentage of Triton X-100 can reach 99.09%,confirming the feasibility of reusing surfactant.Various PBDEs could be removed by MIPs,and Quantitative Structure Property Relationship analysis revealed that PBDEs’molecular volume,planarity,polarity,and hydrophobicity have major influences on their adsorption performance.DFT calculation revealed that Van derWaals force and hydrogen bonding played important roles during selective adsorption.These results can provide effective theoretical guidance for surfactant enhanced soil elution in practical engineering applications.展开更多
基金the National Basic Research Program of China(2003CB415002)the National Natural Science Foundation of China(No.20377022) the Guangxi Natural Science Fund(No.0236063)for their financial supports.
文摘Using the molecular electronegativity distance vector descriptors derived directly from the molecular topological structures, the relative retention time （RRT） of polybrominated diphenyl ethers （PBDEs） were predicted. A four-variable regression model （M30） with the correlation coefficient of 0.9816 and the root mean square errors of 0.061 was developed using a training set including 30 PBDEs. The correlation coefficient of 0.9841 and the root mean square errors of 0.054 between the values of RRT predicted by M30 and the RRT observed for 16 external PBDEs show a good predictive potential of M30. The descriptors included in the M30 represent four interactions between four pairs of atom types, i.e., atom -C= and -C=, -C= and 〉C=, 〉C= and 〉C=, -C= and -Br.
基金the National Natural Science Foundation of China(Nos.41406090,42176045)the Science Foundation of Qingdao Agricultural University(No.631302)+1 种基金the Fujian Key Laboratory of Functional Marine Sensing Materials,Minjiang University(No.MJUKF-FMSM202102)the Natural Science Foundation of Shandong Province(Nos.ZR2019 MB020,ZR2020MB119)。
文摘Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway of anaerobic degradation.On the basis of experimental study,Octa-BDE 197,Hepta-BDE 183,Hexa-BDE 153,Penta-BDE 99 and Tetra-BDE 47 were selected as the initial degradation objects,and their debromination degradation were studied using density functional theory.The structures were optimized by Gaussian 09 program.Furthermore,the molecular orbitals and charge distribution were analyzed.All C-Br bond dissociation energies at different positions including ortho,meta and para bromine atoms were calculated and the sequence of debromination was obtained.There is a close relationship between molecular structure,charge,molecular orbital and C-Br bond.All PBDEs exhibited similar debromination pathways with preferential removal of meta and para bromines.
基金supported by the Knowledge Innovation Program of the Chinese Academy of Sciences(No. KZCX2-YW-420-3)the National Basic Research Program (973) of China (No. 2003CB415005)the National Natural Science Foundation of China (No.20437020, 20677074)
文摘To understand potential ecotoxicological effects of electrical and electronic equipment waste （e-waste） recycling and polybrominated diphenyl ethers （PBDEs） bioaccumulation in loaches, a semi-field experiment using Chinese loach （Misgurnus anguiUicaudatus） as experimental fish was performed. Larval loaches were kept in net-cage for three months in an e-wastes recycling site and a reference site in Southeastern China. There was significant difference of the survival rate between the loaches from the e-wastes recycling site （27%, 19/70） and from reference site （70%, 49/70）. Histopathological responses were also found in all the livers examined in loaches from the e-wastes recycling site. These results showed that mixed pollutants resulted from e-wastes recycling led to ecotoxicological effects on loaches. The bioaccumulation of polybrominated diphenyl ethers （PBDEs）, the main pollutants in e-waste, in loaches was also studied, the mean concentration of total PBDEs in sediment was 6726.17 ng/g wet weight and in water samples was 4.08 ng/L （dissolved phase）. BDE 209 was the dominant congener in sediment and with relatively high concentration in water. Relatively low concentration of BDE 209 （less than 0.01% of total PBDEs） and high concentration of BDE47 （up to 39.34% of total PBDEs） were detected in loaches.
基金supported by the Wenling Science and Technology Bureau of Zhejiang Province (No. 2007-35)
文摘We measured 39 polybrominated diphenyl ethers （PBDEs） in the muscle tissue of three species of fish （Sciaenops ocellatus,Sparus macrocephalus,and Lateolabrax japonicus） and four species of shellfish （Tegillarca granosa,Cyclina sinensis,Sinonovacula constricta,and Ostrea cucullata） that were collected downstream of electronic-waste recycling plants in Taizhou,China.A total of 24 PBDE congeners （PBDE 24） in the samples were detected.The PBDE 24 （total PBDE） ranged from 545.4 to 1688.7 ng/kg ww （wet weight）.The mean PBDE 24 concentration was 1382.6 ng/kg ww in fish and 858.1 ng/kg ww in shellfish.The lower brominated congeners were detected at relatively high concentrations in all species.The penta-products,produced from e-waste,were found at relatively low levels.A principal component analysis suggested a significant correlation among di-,tri-,tetra-,and hepta-BDEs for the three species of fish.Similarly,we found a significant correlation between mono-and tri-BDEs in the shellfish.Our results suggested that the processes of PBDE metabolism and elimination were similar in both fish and shellfish.In addition,the primary source of PBDEs appeared to be from the debromination of high brominated PBDEs.
基金Sponsored by the National Natural Science Foundation of China(Grant No.21277038)
文摘Sixty sediment samples were collected from the main Songhua River in three years. Twelve polybrominated diphenyl ether( PBDE) congeners( BDE17,28,47,66,99,100,153,154,138,183,and BDE-209) were detected to state the pollution situation. The results showed that the total concentration of total PBDEs ranges from 0. 424 to 23. 0 ng / g dry weight,with the mean of 3. 02 ng / g,and the total PBDEs concentration is at relative low level compared with those worldwide. The congener profile showed that BDE-209 is the dominant congener that accounts for more than 80. 1% of total PBDEs in sediments,followed by BDE-47 and BDE-99. These profiles are consistent with a high consumption of Deca-BDEs for the brominated flame retardant market in China. The results of spatial and seasonal observations indicated that local sources,temperature variation, and hydrologic conditions are significant factors on PBDEs concentrations. Hazard quotients suggested that PBDEs pose no potential risk to benthic organisms in detected area at present.
基金the National Natural Science Foundation of China[No.21577026]。
文摘Objective To explore the effects of prenatal exposure to polybrominated diphenyl ethers(PBDEs)on placental size and birth outcomes.Methods Based on the perspective Wenzhou Birth Cohort,this nested case-control study included 101 fetal growth restriction(FGR)and 101 healthy newborns.Maternal serum samples were collected during the third trimester and measured for PBDEs by gas chromatography tandem mass spectrometry.The basic information of mother-newborn pairs was collected from questionnaires,whereas the placental size and birth outcomes of newborns were obtained from hospital records.Results A total of 19 brominated diphenyle ether(BDE)congeners were detected in maternal serum samples.Higher concentrations of BDE-207,-208,-209,and∑19PBDEs were detected in FGR cases than in controls.Increased BDE-207,-208,-209,and∑19PBDEs levels in maternal serum were related to decreased placental length,breadth,surface area,birth weight,birth length,gestational age,and Quetelet index of newborns.After adjusting for confounders,BDE-207 and∑19PBDE concentrations in maternal serum were significantly associated with an increased risk of FGR.Conclusion A negative association was found between PBDE levels in maternal serum and placental size and birth outcomes.Prenatal PBDE exposure may be associated with elevated risk of the incidence of FGR birth.
文摘PBDEs are widely used brominated flame retardant, which are increasingly reported in the environment. Concentrations of thirteen PBDEs in a large number of channel catfish and fish feeds collected from Hubei province of China were investigated in this study. A fast isotopic dilution GC-MS method was firstly developed to simultaneously determine thirteen PBDEs in channel catfish and fish feeds in this study, and especially for the first time PBDEs in fish feeds. Pressurized liquid extraction and multi-layer silica gel column chromatography cleanup were used, some important steps and crucial parameters were modified and intensified compared with other literatures, and GC and MS conditions were optimized. The limits of quantitation values of 0.25 - 5 μg·kg-1 wet weight in channel catfish were calculated for PBDEs;so did 1 - 20 μg·kg-1 wet weight in fish feeds. In addition, good repeatability and accuracy of the whole method were achieved. The established methods were therefore suitable for the simultaneous determinations of thirteen PBDEs in these samples at trace contamination levels. Using the established methods, PBDEs emerged in 10 of 180 channel catfish and 13 of 115 fish feeds, and the dominant PBDEs homologues were PBDE-28, PBDE-47, PBDE-100, PBDE-99, PBDE-154, PBDE-153 and PBDE-183. The detection rates of seven PBDEs congeners were in turn respectively 1.74%, 7.83%, 4.35%, 5.22%, 3.48%, 2.61% and 2.61% in fish feeds, and detection rates of seven PBDEs congeners were in turn respectively 1.11%, 3.89%, 2.22%, 1.67%, 1.11%, 1.11% and 1.11% in channel catfish. There was significant correlation in PBDEs between matching channel catfish and fish feeds (R2 = 0.742, P < 0.001, n = 30), suggesting that fish feeds contaminated with PBDEs possibly resulted in PBDEs residual in channel catfish through biological transfer.
基金supported by 973 program(No.2009CB941701)NSFC grant(No.30972508)MOE Foundation for PhD Program(No 20093234110002)
文摘Objective：To investigate the metabolites of polybrominated diphenyl ether 99（BDE-99）and its related cytochrome P450s in an in vitro system.Methods：Rat primary hepatocytes were isolated and treated with BDE-99 for 24-72 h.Metabolites were then extracted from the hepatocytes and media,and detected by GC/MS.Several mRNAs of metabolic enzymes were also extracted from the same cells and the gene expression levels were determined using quantitative real-time PCR.In addition,selected recombinant cytochrome P450s（CYPs） were expressed in a bacurovirus/sf9 system,and these were further used to explore the metabolism of BDE-99 in vitro.The parent depletion approach was used for screening the ability of CYPs to eliminate BDE-99.Results： A reductively debrominated metabolite,BDE-47,and three oxidative metabolites,2,4,5-tribromophenol,5-OH-BDE-47,and 5＇-OH-BDE-99,were identified from the BDE-99-treated rat hepatocytes,whereas no MeO metabolite was detected in the system.RT-PCR analysis showed that CYP 3A23/3A1,1A2,and 2B1/2 were induced by BDE-99.Furthermore,using the heterological expressed CYP proteins in in vitro BDE-99 metabolism experiments we found that CYP1A2 and CYP3A4 showed the highest metabolic efficiency for BDE-99,with the metabolic clearance rates of CYP1A2 and CYP3A4 being 30.3%and 27.7%,respectively.CYP1A1 and CYP2A6 displayed relatively low clearance rates,while CYP2E1 seemed not to be associated with the BDE-99 metabolism.Conclusions：In our in vitro rat primary hepatocyte metabolism system,four metabolites of BDE-99 were identified,and CYP3A4 and CYP1A2 were demonstrated to be involved in the BDE-99 metabolism.
基金supported by the National Key Research and Development Program of China(No.2019YFC1804202)the National Natural Science Foundation of China(No.22020102004)+2 种基金the Tianjin Municipal Science and Technology Bureau(China)(No.21JCZDJC00280)the Fundamental Research Funds for the Central Universities(China)(No.63233056)the Ministry of Education of China(No.T2017002).
文摘Polybrominated diphenyl ethers (PBDEs), a class of persistent organic pollutants, have been frequently detected in soil at e-waste recycling sites. However, the key factors controlling the transport of PBDEs from surface soil to the vadose zone and groundwater are unclear. Here, colloid-enhanced leaching of PBDEs from undisturbed soil cores collected at an e-waste recycling site in Tianjin, China, is reported. Spatially heterogeneous release of colloids and PBDEs was observed in all the tested soil cores under chemical and hydrodynamic perturbations, indicating the presence of preferential flow paths. Colloid concentration in the effluent significantly increased as ionic strength decreased (from 10 to 0.01 mmol/L), probably due to the stronger electrostatic repulsion between colloidal particles and the soil matrix at lower ionic strength. In contrast, colloid mobilization was not significantly affected by the changes in pH of the influent (from 4.0 to 10.0) and flow rate (from a Darcy velocity of 1.5 to 6.0 cm/h). The concentrations of 2,2′,3,3′,4,4′,5,5′,6,6′-decabromodiphenyl ether (BDE-209), the predominant PBDE congener at the site, detected in the leachate (ranging from 1.09 to 3.43 ng/L) were much lower than previously reported results from packed column leaching tests, and were positively correlated with colloid concentrations. This indicates that remobilization of colloids at e-waste recycling sites can promote the leaching and downward migration of PBDEs from surface soil. The findings highlight the potential risk of surface soil PBDE contamination to groundwater quality and call for further understanding of colloid-facilitated transport for predicting the fate of PBDEs at e-waste recycling sites.
基金Supported by the State Key Basic Research Project (973 Project) of China (Grant No. 2003CB415002)the National Natural Science Foundation of China (Grant Nos. 40525012,20507018 and 40632012)
文摘The spatial,temporal,and vertical distributions of polybrominated diphenyl ethers(PBDEs) in water columns from the Zhujiang River Estuary were examined,and the partition behavior of PBDEs between particle and dissolved phases was investigated in the present study.The results show that the distributions of PBDEs concentrations in the water varied with the sampling seasons.The PBDEs concentrations in water samples were lower in May 2005,when the brackish water was dominant in the estuary,than in October 2005,when fresh water from river runoff dominated the estuary.The spatial distribution of PBDEs in October 2005 indicated that the river runoff was the major mode to input PBDEs to the estuary,and the concentration of PBDEs in water might be dissolved organic carbon(DOC) dependence.The spatial and vertical distributions of PBDEs in May 2005 were relatively homogeneous,and SPM was the major factor on controlling the levels of PBDEs in this sampling time.Both DOC and POC could play certain roles in determining the distribution and partition of PBDEs between particle and dissolved phases,but their effects varied with the water properties.
文摘This review focuses on the occurrence and interactions of engineered nanoparticles(ENPs)and brominated flame retardants(BFRs)such as polybrominated diphenyl ethers(PBDEs)in water systems and the generation of highly complex compounds in the environment.The release of ENPs and BFRs(e.g.PBDEs)to aquatic environments during their usage and disposal are summarised together with their key interaction mechanisms.The major interaction mechanisms including electrostatic,van derWaals,hydrophobic,molecular bridging and steric,hydrogen andπ-bonding,cation bridging and ligand exchange were identified.The presence of ENPs could influence the fate and behaviour of PBDEs through the interactions as well as induced reactions under certain conditions which increases the formation of complex compounds.The interaction leads to alteration of behaviour for PBDEs and their toxic effects to ecological receptors.The intermingled compound(ENPs-BFRs)would show different behaviour from the parental ENPs or BFRs,which are currently lack of investigation.This review provided insights on the interactions of ENPs and BFRs in artificial,environmental water systems and wastewater treatment plants(WWTPs),which are important for a comprehensive risk assessment.
基金This work was supported by the National Natural Science Foundation of China(Nos.42077114 and 41771346)the Local Innovation and Entrepreneurship Team Project of Guangdong Special Support Program(No.2019BT02L218)Zhaoqing University Innovation Research Team Funding Project.
文摘Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing effluent and recycling of surfactant solutions.In this study,a molecular imprinting technique was applied to selectively sorb polybrominated diphenyl ethers(PBDEs)in soil washing effluent.The novel molecular imprinted polymers(MIPs)using different template molecules were synthesized by precipitation polymerization.Adsorption behaviors andmechanisms ofMIPs were studied through experiments and theoretical calculations.The results show that 4-bromo-4'-hydroxybiphenyl and toluene can be effective imprinting molecule for MIPs synthesis.The maximal adsorption capacity of selected dummy molecular imprinted polymer(D1-MIP)was 1032.36μmol/g,and that of part molecular imprinted polymer(P-MIP)was 981.13μmol/g.Their imprinting factors in 5 PBDEs adsorption ranged from 2.13 to 5.88,the recovery percentage of Triton X-100 can reach 99.09%,confirming the feasibility of reusing surfactant.Various PBDEs could be removed by MIPs,and Quantitative Structure Property Relationship analysis revealed that PBDEs’molecular volume,planarity,polarity,and hydrophobicity have major influences on their adsorption performance.DFT calculation revealed that Van derWaals force and hydrogen bonding played important roles during selective adsorption.These results can provide effective theoretical guidance for surfactant enhanced soil elution in practical engineering applications.
