A new monomer of 4, 4-biphenyl-bis[4-phthalazin-1(2H)-one] was synthesized from biphenyl and phthalic anhydride, and a novel copoly(aryl ether ketone) (PPEK) was synthesized from 2, 2-bis(4-hydroxyphenyl)-propane (BPA...A new monomer of 4, 4-biphenyl-bis[4-phthalazin-1(2H)-one] was synthesized from biphenyl and phthalic anhydride, and a novel copoly(aryl ether ketone) (PPEK) was synthesized from 2, 2-bis(4-hydroxyphenyl)-propane (BPA), 4, 4'-biphenyl-bis-[4-phthalazin-1(2H)-one], 4, 4- difluorodiphenylketone (DFK). The monomer and copolymer were characterized by FT-IR and 1H-NMR. DSC and TGA were used to the novel polymer.展开更多
[Objectives]This study was conducted to understand the potential harm of BDE-47 to fish and aquatic ecosystems and obtain relevant toxicological data from the perspective of vitellogenin.[Methods]Adopting the semi-sta...[Objectives]This study was conducted to understand the potential harm of BDE-47 to fish and aquatic ecosystems and obtain relevant toxicological data from the perspective of vitellogenin.[Methods]Adopting the semi-static water exposure method,three exposure concentrations of 5,50,and 500μg/L and five sampling time of 1,3,7,15,and 30 d were set to investigate the effect of BDE-47 on vitellogenin in tilapia liver.[Results]The low concentration of BDE-47(5μg/L)had no effect on the level of vitellogenin in the liver of tilapia.When exposed to high concentrations of BDE-47(50 and 500μg/L),the VTG content of tilapia liver showed a trend of first decreasing,then returning to normal,and then increasing.An abnormal VTG content indicates that the endocrine system of tilapia is disturbed to a certain extent.[Conclusions]This study plays a role in promoting the formulation of relevant water quality standards and the protection of aquatic living resources.展开更多
[Objectives]This study was conducted to investigate the effect of tetrabromodiphenyl ether(BDE-47)on the activity of 11-ketotestosterone(11-KT)in tilapia liver,with a view to understanding the potential hazard of BDE-...[Objectives]This study was conducted to investigate the effect of tetrabromodiphenyl ether(BDE-47)on the activity of 11-ketotestosterone(11-KT)in tilapia liver,with a view to understanding the potential hazard of BDE-47 on fish and aquatic ecosystems from the perspective of sex steroid hormones.[Methods]Adopting the semi-static water exposure method,3 exposure concentrations of 5,50,and 500μg/L and 5 sampling time of 1,3,7,15,and 30 d were set to investigate the effect of BDE-47 on 11-ketotestosterone in tilapia liver.[Results]The low concentration of BDE-47(5μg/L)had no effect on the 11-KT level of tilapia liver;and when exposed to high concentrations of BDE-47(50 and 500μg/L),11-KT in the liver of tilapia was first suppressed and then returned to the normal level.Because the fish reproductive process is completed under the coordinated regulation of sex steroid hormones,significant changes of 11-KT in the liver of tilapia may cause its reproductive dysfunction to a certain extent.[Conclusions]This study provides relevant toxicological data for promoting the formulation(revision)of relevant water quality standards and the formulation of limit standards,and facilitating the protection of aquatic living resources and aquatic ecosystems.展开更多
Polybrominated diphenyl ethers （PBDEs） are ubiquitous global pollutants, which are known to have immune, development, reproduction, and endocrine toxicity in aquatic organisms, including bivalves. 2,2＇,4,4＇-Tetrab...Polybrominated diphenyl ethers （PBDEs） are ubiquitous global pollutants, which are known to have immune, development, reproduction, and endocrine toxicity in aquatic organisms, including bivalves. 2,2＇,4,4＇-Tetrabromodiphenyl ether （BDE-47） is the predominant PBDE congener detected in environmental samples and the tissues of organisms. However, the mechanism of its toxicity remains unclear. In this study, high-throughput sequencing was performed using the clam Mactra veneriformis, a good model for toxicological research, to clarify the transcriptomic response to BDE-47 and the mechanism responsible for the toxicity of BDE-47. The clams were exposed to 5 pg/L BDE-47 for 3 days and the digestive glands were sampled for high-throughput sequencing analysis. We obtained 127 648, 154 225, and 124 985 unigenes by de novo assembly of the control group reads （CG）, BDE-47 group reads （BDEG）, and control and BDE-47 reads （CG ＆ BDEG）, respectively. We annotated 32 176 unigenes from the CG ＆ BDEG reads using the NR database. We categorized 24 401 unigenes into 25 functional COG clusters and 21 749 unigenes were assigned to 259 KEGG pathways. Moreover, 17 625 differentially expressed genes （DEGs） were detected, with 10 028 upregulated DEGs and 7 597 downregulated DEGs. Functional enrichment analysis showed that the DEGs were involved with detoxification, antioxidant defense, immune response, apoptosis, and other functions. The mRNA expression levels of 26 DEGs were verified by quantitative real-time PCR, which demonstrated the high agreement between the two methods. These results provide a good basis for future research using the M. veneriformis model into the mechanism of PBDEs toxicity and molecular biomarkers for BDE-47 pollution. The regulation and interaction of the DEGs would be studied in the future for clarifying the mechanism of PBDEs toxicity.展开更多
[Objectives] This study was conducted to investigate the toxic effects of 2,2',4,4',5,5'-hexabromobiphenyl ether on Chlorella vulgaris and provide basic data for protecting aquatic ecosystems. [Methods] Th...[Objectives] This study was conducted to investigate the toxic effects of 2,2',4,4',5,5'-hexabromobiphenyl ether on Chlorella vulgaris and provide basic data for protecting aquatic ecosystems. [Methods] The acute toxicity effects of 2,2',4,4',5,5'-hexabromodiphenyl ether on C. vulgaris was investigated by the semi-static water contacting acute toxicity method. [Results] The 48,72 and 96 h-EC(50) of 2,2',4,4',5,5'-hexabromodiphenyl ether to C. vulgaris were23. 58,18. 71 and 14. 75 μg/L,respectively,and the safe concentration of 2,2',4,4',5,5'-hexabromodiphenyl ether to C. vulgaris was 1. 475μg/L. For the water solubility of 2,2',4,4',5,5'-hexabromodiphenyl ether is extremely low( 1 μg/L),it could not cause the acute poisoning death of C. vulgaris. According to the grading standards for the assessment of the toxicity on algae,2,2',4,4',5,5'-hexabromodiphenyl ether was extremely highly toxic to C. vulgaris. [Conclusions]The extremely high toxicity of 2,2',4,4',5,5'-hexabromodiphenyl ether to C. vulgaris shows that it has heavy potential harm to aquatic ecosystems and the maximum residue limit standards of 2,2',4,4',5,5'-hexabromodiphenyl ether in water should be formulated to better protect aquatic ecosystems.展开更多
A new technique of zero-valent zinc coupled with ascorbic acid(ZVZ/AA)was developed and applied to debrominate the 2,2,,4,4,-Tetrabromodiphenyl ether(BDE-47),which achieved high conversion and rapid debromination of B...A new technique of zero-valent zinc coupled with ascorbic acid(ZVZ/AA)was developed and applied to debrominate the 2,2,,4,4,-Tetrabromodiphenyl ether(BDE-47),which achieved high conversion and rapid debromination of BDE-47 to less-or non-toxic forms.The reaction conditions were optimized by the addition of 100 mg/L Z V Z particles and 3 mmol/L A A at original solution p H=4.00 using the solvent of methanol/H2O(v:v=4:6),which could convert approximately 94%of 5 mg/L BDE-47 into lower-brominated diphenyl ethers within a 90 min at the ZVZ/AA system.The high debromination of BDE-47 was mainly attributed to the effect of A A that inhibits the formation of Zn(Ⅱ)(hydr)oxide passivation layers and promotes the corrosion of ZVZ,which leads to increase the reactivity of ZVZ.Additionally,ion chromatography and gas chromatography mass spectrometry analyses revealed that bromine ion and lower-debromination diphenyl ethers formed during the reduction of BDE-47.Furthermore,based on the generation of the intermediates products,and its concentration changes over time,it was proposed that the dominant pathway for conversion of BDE-47 was sequential debromination and the final products were diphenyl ethers.These results suggested that the ZVZ/AA system has the potential for highly efficient debromination of BDE-47 from wastewater.展开更多
This paper focuses on the pathway,the kinetic laws and the mechanisms of BDE-47 photo-degradation in the environment.By changing the degradation conditions(such as light sources,solvents,inorganic salts and free radic...This paper focuses on the pathway,the kinetic laws and the mechanisms of BDE-47 photo-degradation in the environment.By changing the degradation conditions(such as light sources,solvents,inorganic salts and free radical scavengers)and analyzing the degradation products using gas chromatography(GC)and gas chromatography/mass spectrometry(GC/MS),a better understanding of the fate of 2,2',4,4'-Tetrabromodiphenyl ether(BDE-47)in the environment is obtained.Results show that(i)the degradation reactions of BDE-47 under four different types of light sources are well described by the first order kinetic equation(r≥0.9995);(ii)hydrogen-donating ability and light absorption property of an organic solvent have a joint influence on the kinetics of degradation of BDE-47,which makes the degradation rate constants of BDE-47 different in different solvents(hexane 0.2735,methanol 0.2720,toluene 0.1280,methanol/water(1:1)0.0673,acetonitrile 0.0471,acetone 0.0030);(iii)the types and quantities of detected degradation products of BDE-47 are different in different solvents,BDE-1 is found only in hexane solvent,BDE-3 is not found in toluene,the relative content of BDE-28 in toluene is the highest(91.3%);(iv)inorganic ions have different effects on the degradation of BDE-47,the half-life of 0.10 mmol Fe^(3+) is reduced by 46.1%compared with that without adding 0.10 mmol Fe^(3+),the half-life of 0.5 mmol NH_(4)^(+) is reduced by 46.7%compared with that without 0.5 mmol NH4 t,50 mg/L TBA can increase the halflife by 5.1%compared with no addition.展开更多
基金This work is sponsored by the National Natural Science Foundation of China (No. 59473901).
文摘A new monomer of 4, 4-biphenyl-bis[4-phthalazin-1(2H)-one] was synthesized from biphenyl and phthalic anhydride, and a novel copoly(aryl ether ketone) (PPEK) was synthesized from 2, 2-bis(4-hydroxyphenyl)-propane (BPA), 4, 4'-biphenyl-bis-[4-phthalazin-1(2H)-one], 4, 4- difluorodiphenylketone (DFK). The monomer and copolymer were characterized by FT-IR and 1H-NMR. DSC and TGA were used to the novel polymer.
基金National Key R&D Program(2020YFD0900502)Special Project of National Characteristic Freshwater Fish Industry Technology System(CARS-46).
文摘[Objectives]This study was conducted to understand the potential harm of BDE-47 to fish and aquatic ecosystems and obtain relevant toxicological data from the perspective of vitellogenin.[Methods]Adopting the semi-static water exposure method,three exposure concentrations of 5,50,and 500μg/L and five sampling time of 1,3,7,15,and 30 d were set to investigate the effect of BDE-47 on vitellogenin in tilapia liver.[Results]The low concentration of BDE-47(5μg/L)had no effect on the level of vitellogenin in the liver of tilapia.When exposed to high concentrations of BDE-47(50 and 500μg/L),the VTG content of tilapia liver showed a trend of first decreasing,then returning to normal,and then increasing.An abnormal VTG content indicates that the endocrine system of tilapia is disturbed to a certain extent.[Conclusions]This study plays a role in promoting the formulation of relevant water quality standards and the protection of aquatic living resources.
基金National Key R&D Program(2020YFD0900502)Special Project of National Characteristic Freshwater Fish Industry Technology System(CARS-46).
文摘[Objectives]This study was conducted to investigate the effect of tetrabromodiphenyl ether(BDE-47)on the activity of 11-ketotestosterone(11-KT)in tilapia liver,with a view to understanding the potential hazard of BDE-47 on fish and aquatic ecosystems from the perspective of sex steroid hormones.[Methods]Adopting the semi-static water exposure method,3 exposure concentrations of 5,50,and 500μg/L and 5 sampling time of 1,3,7,15,and 30 d were set to investigate the effect of BDE-47 on 11-ketotestosterone in tilapia liver.[Results]The low concentration of BDE-47(5μg/L)had no effect on the 11-KT level of tilapia liver;and when exposed to high concentrations of BDE-47(50 and 500μg/L),11-KT in the liver of tilapia was first suppressed and then returned to the normal level.Because the fish reproductive process is completed under the coordinated regulation of sex steroid hormones,significant changes of 11-KT in the liver of tilapia may cause its reproductive dysfunction to a certain extent.[Conclusions]This study provides relevant toxicological data for promoting the formulation(revision)of relevant water quality standards and the formulation of limit standards,and facilitating the protection of aquatic living resources and aquatic ecosystems.
基金Supported by the National Natural Science Foundation of China(No.41206120)the Development Plan of Science and Technology in Yantai(No.2011062)+1 种基金the National Special Research Fund for Non-Profit Marine Sector(No.201205023)the Ludong University Research Funding(No.210-32040301)
文摘Polybrominated diphenyl ethers （PBDEs） are ubiquitous global pollutants, which are known to have immune, development, reproduction, and endocrine toxicity in aquatic organisms, including bivalves. 2,2＇,4,4＇-Tetrabromodiphenyl ether （BDE-47） is the predominant PBDE congener detected in environmental samples and the tissues of organisms. However, the mechanism of its toxicity remains unclear. In this study, high-throughput sequencing was performed using the clam Mactra veneriformis, a good model for toxicological research, to clarify the transcriptomic response to BDE-47 and the mechanism responsible for the toxicity of BDE-47. The clams were exposed to 5 pg/L BDE-47 for 3 days and the digestive glands were sampled for high-throughput sequencing analysis. We obtained 127 648, 154 225, and 124 985 unigenes by de novo assembly of the control group reads （CG）, BDE-47 group reads （BDEG）, and control and BDE-47 reads （CG ＆ BDEG）, respectively. We annotated 32 176 unigenes from the CG ＆ BDEG reads using the NR database. We categorized 24 401 unigenes into 25 functional COG clusters and 21 749 unigenes were assigned to 259 KEGG pathways. Moreover, 17 625 differentially expressed genes （DEGs） were detected, with 10 028 upregulated DEGs and 7 597 downregulated DEGs. Functional enrichment analysis showed that the DEGs were involved with detoxification, antioxidant defense, immune response, apoptosis, and other functions. The mRNA expression levels of 26 DEGs were verified by quantitative real-time PCR, which demonstrated the high agreement between the two methods. These results provide a good basis for future research using the M. veneriformis model into the mechanism of PBDEs toxicity and molecular biomarkers for BDE-47 pollution. The regulation and interaction of the DEGs would be studied in the future for clarifying the mechanism of PBDEs toxicity.
基金Supported by Central Public-interest Scientific Institution Basal Research FundChinese Academy of Fishery Science (2017HY-ZD0208)China Agricultural Research System-Freshwater Fish (CARS-46)。
文摘[Objectives] This study was conducted to investigate the toxic effects of 2,2',4,4',5,5'-hexabromobiphenyl ether on Chlorella vulgaris and provide basic data for protecting aquatic ecosystems. [Methods] The acute toxicity effects of 2,2',4,4',5,5'-hexabromodiphenyl ether on C. vulgaris was investigated by the semi-static water contacting acute toxicity method. [Results] The 48,72 and 96 h-EC(50) of 2,2',4,4',5,5'-hexabromodiphenyl ether to C. vulgaris were23. 58,18. 71 and 14. 75 μg/L,respectively,and the safe concentration of 2,2',4,4',5,5'-hexabromodiphenyl ether to C. vulgaris was 1. 475μg/L. For the water solubility of 2,2',4,4',5,5'-hexabromodiphenyl ether is extremely low( 1 μg/L),it could not cause the acute poisoning death of C. vulgaris. According to the grading standards for the assessment of the toxicity on algae,2,2',4,4',5,5'-hexabromodiphenyl ether was extremely highly toxic to C. vulgaris. [Conclusions]The extremely high toxicity of 2,2',4,4',5,5'-hexabromodiphenyl ether to C. vulgaris shows that it has heavy potential harm to aquatic ecosystems and the maximum residue limit standards of 2,2',4,4',5,5'-hexabromodiphenyl ether in water should be formulated to better protect aquatic ecosystems.
基金The authors thank the Major Science and Technology Program for Water Pollution Control and Treatment,National Water Grant(No.2017ZX07202002)the Key-Area Research and Development Program of Guangdong Provice(No.2019B110205003)the National Natural Science Foundation of China(Grant No.51979141).
文摘A new technique of zero-valent zinc coupled with ascorbic acid(ZVZ/AA)was developed and applied to debrominate the 2,2,,4,4,-Tetrabromodiphenyl ether(BDE-47),which achieved high conversion and rapid debromination of BDE-47 to less-or non-toxic forms.The reaction conditions were optimized by the addition of 100 mg/L Z V Z particles and 3 mmol/L A A at original solution p H=4.00 using the solvent of methanol/H2O(v:v=4:6),which could convert approximately 94%of 5 mg/L BDE-47 into lower-brominated diphenyl ethers within a 90 min at the ZVZ/AA system.The high debromination of BDE-47 was mainly attributed to the effect of A A that inhibits the formation of Zn(Ⅱ)(hydr)oxide passivation layers and promotes the corrosion of ZVZ,which leads to increase the reactivity of ZVZ.Additionally,ion chromatography and gas chromatography mass spectrometry analyses revealed that bromine ion and lower-debromination diphenyl ethers formed during the reduction of BDE-47.Furthermore,based on the generation of the intermediates products,and its concentration changes over time,it was proposed that the dominant pathway for conversion of BDE-47 was sequential debromination and the final products were diphenyl ethers.These results suggested that the ZVZ/AA system has the potential for highly efficient debromination of BDE-47 from wastewater.
基金This work is supported by the National Natural Science Foundation of China(No.21377033),and the Key Program of Hebei Education Department(No.ZD20131046).
文摘This paper focuses on the pathway,the kinetic laws and the mechanisms of BDE-47 photo-degradation in the environment.By changing the degradation conditions(such as light sources,solvents,inorganic salts and free radical scavengers)and analyzing the degradation products using gas chromatography(GC)and gas chromatography/mass spectrometry(GC/MS),a better understanding of the fate of 2,2',4,4'-Tetrabromodiphenyl ether(BDE-47)in the environment is obtained.Results show that(i)the degradation reactions of BDE-47 under four different types of light sources are well described by the first order kinetic equation(r≥0.9995);(ii)hydrogen-donating ability and light absorption property of an organic solvent have a joint influence on the kinetics of degradation of BDE-47,which makes the degradation rate constants of BDE-47 different in different solvents(hexane 0.2735,methanol 0.2720,toluene 0.1280,methanol/water(1:1)0.0673,acetonitrile 0.0471,acetone 0.0030);(iii)the types and quantities of detected degradation products of BDE-47 are different in different solvents,BDE-1 is found only in hexane solvent,BDE-3 is not found in toluene,the relative content of BDE-28 in toluene is the highest(91.3%);(iv)inorganic ions have different effects on the degradation of BDE-47,the half-life of 0.10 mmol Fe^(3+) is reduced by 46.1%compared with that without adding 0.10 mmol Fe^(3+),the half-life of 0.5 mmol NH_(4)^(+) is reduced by 46.7%compared with that without 0.5 mmol NH4 t,50 mg/L TBA can increase the halflife by 5.1%compared with no addition.
