Endosulfan and hexachlorobenzene(HCB)were previously widely used organochlorine pesticides.Much attention has been paid to trends in human exposure to endosulfan and HCB and to the transport and distribution of endosu...Endosulfan and hexachlorobenzene(HCB)were previously widely used organochlorine pesticides.Much attention has been paid to trends in human exposure to endosulfan and HCB and to the transport and distribution of endosulfan and HCB within the body.We determined endosulfan I,endosulfan II,and HCB concentrations in serum samples collected from the general population of Wuxi in Jiangsu Province(China)between 2012 and 2016.The endosulfan concentrations varied little throughout the study period,but the HCB concentrations increased.The HCB concentrations were significantly higher in serum from overweight people and smokers than in serum from normal weight people(p?0.028)and non-smokers(p?0.011),respectively.HCB binds to human serum albumin(HSA)and can form halogen bonds to CYS-461 and ARG-484 at site II(subdomain IIIA).Fatty acids and nicotine increase the affinity between HCB and HSA,explaining the higher HCB concentrations in serum from overweight people and smokers than normal weight people and non-smokers,respectively.展开更多
Organochlorine pesticides are chlorinated hydrocarbon compounds.The production and use of organochlorine pesticides have been restricted around the world because they are persistent and toxic and able to undergo long-...Organochlorine pesticides are chlorinated hydrocarbon compounds.The production and use of organochlorine pesticides have been restricted around the world because they are persistent and toxic and able to undergo long-range transport and bioaccumulate.It is necessary to develop efficient techniques for eliminating organochlorine pesticides from environmental media,and we also need to better understand how these techniques operate.Understanding how organochlorine herbicides behave in various environmental settings is very crucial.We looked on the photodegradation of endosulfan(endosulfan Ⅰ and Ⅱ)and hexachlorobenzene(HCB),two common organochlorine insecticides.Tests were conducted with pesticides at different concentrations,dissolved in various organic solvents,and exposed to light at different wavelengths.Density Functional Theory(DFT)was employed to study solvent effects.Degradation kinetics followed first-order models.The pesticides dissolved in various organic solvents showed a decrease in their degradation rates in the following order:toluene>acetone>n-hexane.It was discovered that there was a good chance the Cl atoms on the benzene ring in HCB would be eliminated through nucleophilic processes.It was discovered that endosulfan breaks preferentially at the S=O double bond.The findings will aid in the development of strategies for successfully eliminating organochlorine pesticides from environmental media by aiding in the prediction and assessment of the photochemical behaviors of the pesticides under various environmental circumstances.展开更多
Direct membrane filtration(DMF)is a popular option for raw sewage pre-concentration for the subsequent organic resource recovery.It undergoes rapid and severe fouling.To achieve a fundamental understanding of the cont...Direct membrane filtration(DMF)is a popular option for raw sewage pre-concentration for the subsequent organic resource recovery.It undergoes rapid and severe fouling.To achieve a fundamental understanding of the contributions of key foulants to DMF,principal component analysis(PCA)using Fourier transform infrared spectroscopy(FTIR)was applied to identify three stages of DMF.Variance partitioning analysis(VPA)and partial least squares(PLS)were used to quantitatively determine the contributions of key foulants.Humic acid(HA)achieved the highest intersection contribution(40.5%)to the total variance of the increase in resistance.Meanwhile,HA and protein(PN)explained 20.1%in the middle stage of DMF.The overall marginal effect of HA accounted for 42.5%of the variance,in conjunction with an overall individual effect of 11.0%(which was the highest in the initial stage:15.1%).The variable importance in projection(VIP)of impact on the resistance increase of DMF were 1.16(PN),0.99(HA),and 0.82(polysaccharides,PS).HA&PN with a VIP value approaching or larger than one significantly influenced the resistance increase in DMF.Meanwhile,the VIP of impact on blocking model alteration were 1.03(PS),1.01(PN),and 0.96(HA).HA,PS,and PN were regarded as vital factors in the fouling mode alteration.PS drives the fouling mode in the initial stage,whereas HA&PN and PN play dominant roles in the middle and final stages.Measures targeting HA and PN removal can be adapted for the efficient and cost-effective fouling control of raw sewage DMF.展开更多
Polychlorinated naphthalenes(PCNs)comprise 75 congeners,with varying concentrations and major congeners across different populations.Recent studies have found a relationship between PCNs and thyroid hormone levels,sug...Polychlorinated naphthalenes(PCNs)comprise 75 congeners,with varying concentrations and major congeners across different populations.Recent studies have found a relationship between PCNs and thyroid hormone levels,suggesting they may interfere with thyroid function.Investigating the con-centrations of PCNs in individuals with thyroid dysfunction helps identify the predominant congeners and enables targeted analysis of their interference with thyroid function.In this study,serum con-centrations of PCNs from 55 adults with thyroid dysfunction were measured.PCN-13,-15,17/25/26,20,23,and 24/14 detected at over 70%,and PCN-23 and-24/14 being the major congeners.No significant difference in PCN concentrations was found between males and females,but the concen-trations of PCN-23 and-24/14 increased with age.Logistic regression and QGC models revealed a sig-nificant association between PCN-23 and thyroid dysfunction,while mediation analysis indicated PCN-23 affects physiological processes involving the BRAF 600E gene,which influences normal thyroid function.Molecular docking results showed that all six PCNs impacted thyroid hormone metabolism and receptor binding,with PCN-23 binding more effectively to TBG and disrupting thyroid hormone transport compared to PCN-24/14.Future studies should focus on the concentrations of trichlorinated PCNs,particularly PCN-23,in the human body and their relationship with thyroid function.展开更多
Polychlorinated biphenyls(PCBs)are persistent organic pollutants renowned for their bioaccumation and toxicity.Although PCBs production and use were banned worldwide decades ago,PCBs still pose a health risk due to th...Polychlorinated biphenyls(PCBs)are persistent organic pollutants renowned for their bioaccumation and toxicity.Although PCBs production and use were banned worldwide decades ago,PCBs still pose a health risk due to their environmental persistence and unintentional production.In this report,PCB concentrations and temporal trends in serum from residents of urban areas in eastern China is investigated.The endocrine-disrupting potentials of PCBs are also investigated,particularly effects on thyroid hormone receptors.Through analysis of five years of data,results indicated that dioxin-like PCBs and congener PCB209 concentrations maintained low and had no marked temporal trends,but that the indicator PCBs and particularly PCB52,PCB153,and PCB180 concentrations increased.Furthermore,to evaluate binding of PCBs to the thyroid hormone receptor TRβ1,molecular docking simulations are performed.It is found that the PCBs of PCB28,PCB52,and PCB153 can interfere with triiodothyronine binding to TRβ1,which are comparable to the effects of the polybrominated biphenyl BB-153,a known thyroid function disruptor.What's more,the PCB180 binds to TRβ1 more strongly than that of BB-153.Our results indicated that a continuously monitoring of human exposures to PCB28,PCB52,PCB153,PCB180,and a detailed assessment of thyroid function interference is necessary.展开更多
The widespread use of brominated flame retardants(BFRs),including polybrominated diphenyl ethers(PBDEs)and novel brominated flame retardants(NBFRs),poses significant environmental and health risks,yet data on their co...The widespread use of brominated flame retardants(BFRs),including polybrominated diphenyl ethers(PBDEs)and novel brominated flame retardants(NBFRs),poses significant environmental and health risks,yet data on their contamination in remote agro-pastoral regions remain scarce.This study systematically investigated the pollution characteristics,sources,and human exposure risks of PBDEs and NBFRs in indoor dust and human hair from 11 households in Inner Mongolian grasslands.Results revealed that PBDEs were ubiquitous in all dust samples(median Σ_(10)PBDEs:15.8 ng/g dw,with a 95% confidence interval of 2.8848.1 ng/g dw),dominated by BDE-209(73.6100%),reflecting legacy Deca-BDE usage despite regulatory restrictions.NBFRs(medianΣNBFRs:0.77 ng/g dw,95%CI:0.421.14 ng/g dw)in dust were predominated by hexabromobenzene(HBB,41.7%)and pentabromobenzylacrylate(PBBA,18.8%).In human hair,PBDEs(medianΣ10PBDEs:6.77 ng/g dw,95%CI:2.3152 ng/g dw)showed comparable levels to urban populations,with BDE-209 contributing 71.799.7%,while NBFRs(medianΣNBFRs:0.64 ng/g dw,95%CI:0.231.97)mirrored dust profiles(HBB:43.4%),suggesting dust as a likely exposure route(r=0.5750.699,p<0.05).Source analysis identified Penta-/Octa-BDE degradation and industrial applications(plastics/textiles for tetrabromo-p-xylene(pTBx)-pentabromobenzene(PBBz)-pentabromotoluene(PBT);electronics for PBBA-HBB)as key contributors.Human age-dependent accumulation patterns was observed,with higher PBDEs in the elderly and increasing PBBz/PBT levels with age(r=0.5280.564,p<0.05).Despite lower dust contamination than urban areas,hair-based exposure highlighted non-dust pathways(e.g.,air inhalation)for low-brominated congeners.These findings underscore the persistent risks of legacy PBDEs and emerging NBFRs in remote regions,advocating for stricter lifecycle management of BFR-containing products and long-term health monitoring.展开更多
The global obesity epidemic is increasingly linked to environmental chemical exposure,yet the role of novel brominated flame retardants(NBFRs)remains poorly understood.In this cross-ethnic study of elderly agro-pastor...The global obesity epidemic is increasingly linked to environmental chemical exposure,yet the role of novel brominated flame retardants(NBFRs)remains poorly understood.In this cross-ethnic study of elderly agro-pastoralists in Inner Mongolia,we compared serum NBFRs levels and metabolic biomarkers between Mongolian(n=30)and Han(n=47)populations.The Mongolian group,with relatively higher meat/dairy-rich diets,showed significantly higher NBFR concentrations,body mass index(BMI),and low-density lipoprotein cholesterol(LDL-C).Alarmingly,72.7%of participants were classified as overweight/obese,far exceeding China's national average.Serum pentabromotoluene(PBT),pentabromoethylbenzene(PBEB),and pentabromobenzyl acrylate(PBBA)showed significant positive correlations with BMI(p<0.05).The quantile G-computation(QGC)model further revealed that PBBA exerted particularly prominent effects on BMl.Strikingly,piecewise regression revealed accelerated NBFRs accumulation in individuals with BMI≥28(p<0.05),indicating a bidirectional"NBFRs-BMI feedback loop".Molecular docking studies demonstrated that PBBA and PBT exhibit a higher binding affinity to PPARγthan the conventional agonist Rosiglitazone,with specific interactions at key amino acid residues(ARG-288 and ILE-326)on helix H3.These findings suggest that PBBA and PBT may act as novel PPARγagonists,potentially promoting adipogenesis and consequently leading to weight gain.展开更多
Halogenated polycyclic aromatic hydrocarbons(HPAHs)and polycyclic aromatic hydrocarbons(PAHs)were determined in human serum samples pooled by donor age(<20,20–29,30–39,40–49 and≥50 y).The pooled samples were co...Halogenated polycyclic aromatic hydrocarbons(HPAHs)and polycyclic aromatic hydrocarbons(PAHs)were determined in human serum samples pooled by donor age(<20,20–29,30–39,40–49 and≥50 y).The pooled samples were collected from four Chinese cities,Yantai(Shandong Province),Ganzi(Sichuan Province),Huaihua(Hunan Province),and Lingshui(Hainan Province).The concentrations of HPAHs and PAHs were in the range of 4.26–633 ng/g lipid and 249–1642 ng/g lipid from the different cities.Although the levels of HPAHs in blood samples varied among the populations of the four cities,1,5-dichloroanthracene(1,5-Cl_(2)Ant)was the predominant contributor to HPAHs in the serum samples,accounting for over 85.7%of its total concentration.Furthermore,1,5-Cl_(2)Ant serum concentrations increased significantly with age.Notably,molecular docking results show that 1,5-Cl_(2)Ant not only ac-quires the ability to bind d-AhR PAS-B domain,but also binds at the similar sites as 2,3,7,8-tetrachlorodibenzo-p-dioxin(TCDD)and benzo[a]pyrene(BaP),suggesting that 1,5-Cl_(2)Ant,like TCDD and BaP,may cause a wide variety of toxicity via AhR-mediated signaling pathways.The bio-accumulation potential of 1,5-Cl_(2)Ant in the human body and its associated toxicity observed in this study need special attention.展开更多
文摘Endosulfan and hexachlorobenzene(HCB)were previously widely used organochlorine pesticides.Much attention has been paid to trends in human exposure to endosulfan and HCB and to the transport and distribution of endosulfan and HCB within the body.We determined endosulfan I,endosulfan II,and HCB concentrations in serum samples collected from the general population of Wuxi in Jiangsu Province(China)between 2012 and 2016.The endosulfan concentrations varied little throughout the study period,but the HCB concentrations increased.The HCB concentrations were significantly higher in serum from overweight people and smokers than in serum from normal weight people(p?0.028)and non-smokers(p?0.011),respectively.HCB binds to human serum albumin(HSA)and can form halogen bonds to CYS-461 and ARG-484 at site II(subdomain IIIA).Fatty acids and nicotine increase the affinity between HCB and HSA,explaining the higher HCB concentrations in serum from overweight people and smokers than normal weight people and non-smokers,respectively.
文摘Organochlorine pesticides are chlorinated hydrocarbon compounds.The production and use of organochlorine pesticides have been restricted around the world because they are persistent and toxic and able to undergo long-range transport and bioaccumulate.It is necessary to develop efficient techniques for eliminating organochlorine pesticides from environmental media,and we also need to better understand how these techniques operate.Understanding how organochlorine herbicides behave in various environmental settings is very crucial.We looked on the photodegradation of endosulfan(endosulfan Ⅰ and Ⅱ)and hexachlorobenzene(HCB),two common organochlorine insecticides.Tests were conducted with pesticides at different concentrations,dissolved in various organic solvents,and exposed to light at different wavelengths.Density Functional Theory(DFT)was employed to study solvent effects.Degradation kinetics followed first-order models.The pesticides dissolved in various organic solvents showed a decrease in their degradation rates in the following order:toluene>acetone>n-hexane.It was discovered that there was a good chance the Cl atoms on the benzene ring in HCB would be eliminated through nucleophilic processes.It was discovered that endosulfan breaks preferentially at the S=O double bond.The findings will aid in the development of strategies for successfully eliminating organochlorine pesticides from environmental media by aiding in the prediction and assessment of the photochemical behaviors of the pesticides under various environmental circumstances.
基金supported by the National Natural Science Foundation of China(No.51608298)the Open Research Fund Program of Cultivation Project of Double First-Class Disciplines of Environmental Science and Engineering,Beijing Technology&Business University(BTBU,ESE2022YB07)the Graduate Research and Practice Projects of Minzu University of China.We would like to thank Editage for English language editing。
文摘Direct membrane filtration(DMF)is a popular option for raw sewage pre-concentration for the subsequent organic resource recovery.It undergoes rapid and severe fouling.To achieve a fundamental understanding of the contributions of key foulants to DMF,principal component analysis(PCA)using Fourier transform infrared spectroscopy(FTIR)was applied to identify three stages of DMF.Variance partitioning analysis(VPA)and partial least squares(PLS)were used to quantitatively determine the contributions of key foulants.Humic acid(HA)achieved the highest intersection contribution(40.5%)to the total variance of the increase in resistance.Meanwhile,HA and protein(PN)explained 20.1%in the middle stage of DMF.The overall marginal effect of HA accounted for 42.5%of the variance,in conjunction with an overall individual effect of 11.0%(which was the highest in the initial stage:15.1%).The variable importance in projection(VIP)of impact on the resistance increase of DMF were 1.16(PN),0.99(HA),and 0.82(polysaccharides,PS).HA&PN with a VIP value approaching or larger than one significantly influenced the resistance increase in DMF.Meanwhile,the VIP of impact on blocking model alteration were 1.03(PS),1.01(PN),and 0.96(HA).HA,PS,and PN were regarded as vital factors in the fouling mode alteration.PS drives the fouling mode in the initial stage,whereas HA&PN and PN play dominant roles in the middle and final stages.Measures targeting HA and PN removal can be adapted for the efficient and cost-effective fouling control of raw sewage DMF.
文摘Polychlorinated naphthalenes(PCNs)comprise 75 congeners,with varying concentrations and major congeners across different populations.Recent studies have found a relationship between PCNs and thyroid hormone levels,suggesting they may interfere with thyroid function.Investigating the con-centrations of PCNs in individuals with thyroid dysfunction helps identify the predominant congeners and enables targeted analysis of their interference with thyroid function.In this study,serum con-centrations of PCNs from 55 adults with thyroid dysfunction were measured.PCN-13,-15,17/25/26,20,23,and 24/14 detected at over 70%,and PCN-23 and-24/14 being the major congeners.No significant difference in PCN concentrations was found between males and females,but the concen-trations of PCN-23 and-24/14 increased with age.Logistic regression and QGC models revealed a sig-nificant association between PCN-23 and thyroid dysfunction,while mediation analysis indicated PCN-23 affects physiological processes involving the BRAF 600E gene,which influences normal thyroid function.Molecular docking results showed that all six PCNs impacted thyroid hormone metabolism and receptor binding,with PCN-23 binding more effectively to TBG and disrupting thyroid hormone transport compared to PCN-24/14.Future studies should focus on the concentrations of trichlorinated PCNs,particularly PCN-23,in the human body and their relationship with thyroid function.
基金supported by the Fundamental Research Funds for the Central Universities(grant no.2021JCXK01)the National Natural Science Foundation of China(grant no.81803199).
文摘Polychlorinated biphenyls(PCBs)are persistent organic pollutants renowned for their bioaccumation and toxicity.Although PCBs production and use were banned worldwide decades ago,PCBs still pose a health risk due to their environmental persistence and unintentional production.In this report,PCB concentrations and temporal trends in serum from residents of urban areas in eastern China is investigated.The endocrine-disrupting potentials of PCBs are also investigated,particularly effects on thyroid hormone receptors.Through analysis of five years of data,results indicated that dioxin-like PCBs and congener PCB209 concentrations maintained low and had no marked temporal trends,but that the indicator PCBs and particularly PCB52,PCB153,and PCB180 concentrations increased.Furthermore,to evaluate binding of PCBs to the thyroid hormone receptor TRβ1,molecular docking simulations are performed.It is found that the PCBs of PCB28,PCB52,and PCB153 can interfere with triiodothyronine binding to TRβ1,which are comparable to the effects of the polybrominated biphenyl BB-153,a known thyroid function disruptor.What's more,the PCB180 binds to TRβ1 more strongly than that of BB-153.Our results indicated that a continuously monitoring of human exposures to PCB28,PCB52,PCB153,PCB180,and a detailed assessment of thyroid function interference is necessary.
基金supported by the Fundamental Research Funds for the Central Universities(grant no.2021JCXK01)the Graduate Research and Practice Projects of Minzu University of China(grant no.BZKY2021036)Strategic Pioneering Science and Technology Project of Inner Mongolia University of Technology-Environmental Governance under the Background of Energy Transition(grant no.DC2400003368).
文摘The widespread use of brominated flame retardants(BFRs),including polybrominated diphenyl ethers(PBDEs)and novel brominated flame retardants(NBFRs),poses significant environmental and health risks,yet data on their contamination in remote agro-pastoral regions remain scarce.This study systematically investigated the pollution characteristics,sources,and human exposure risks of PBDEs and NBFRs in indoor dust and human hair from 11 households in Inner Mongolian grasslands.Results revealed that PBDEs were ubiquitous in all dust samples(median Σ_(10)PBDEs:15.8 ng/g dw,with a 95% confidence interval of 2.8848.1 ng/g dw),dominated by BDE-209(73.6100%),reflecting legacy Deca-BDE usage despite regulatory restrictions.NBFRs(medianΣNBFRs:0.77 ng/g dw,95%CI:0.421.14 ng/g dw)in dust were predominated by hexabromobenzene(HBB,41.7%)and pentabromobenzylacrylate(PBBA,18.8%).In human hair,PBDEs(medianΣ10PBDEs:6.77 ng/g dw,95%CI:2.3152 ng/g dw)showed comparable levels to urban populations,with BDE-209 contributing 71.799.7%,while NBFRs(medianΣNBFRs:0.64 ng/g dw,95%CI:0.231.97)mirrored dust profiles(HBB:43.4%),suggesting dust as a likely exposure route(r=0.5750.699,p<0.05).Source analysis identified Penta-/Octa-BDE degradation and industrial applications(plastics/textiles for tetrabromo-p-xylene(pTBx)-pentabromobenzene(PBBz)-pentabromotoluene(PBT);electronics for PBBA-HBB)as key contributors.Human age-dependent accumulation patterns was observed,with higher PBDEs in the elderly and increasing PBBz/PBT levels with age(r=0.5280.564,p<0.05).Despite lower dust contamination than urban areas,hair-based exposure highlighted non-dust pathways(e.g.,air inhalation)for low-brominated congeners.These findings underscore the persistent risks of legacy PBDEs and emerging NBFRs in remote regions,advocating for stricter lifecycle management of BFR-containing products and long-term health monitoring.
基金supported by the Strategic Pioneering Science and Technology Project of Inner Mongolia University of Technology-Environmental Governance under the Background of Energy Transition(Grant No.DC2400003368).
文摘The global obesity epidemic is increasingly linked to environmental chemical exposure,yet the role of novel brominated flame retardants(NBFRs)remains poorly understood.In this cross-ethnic study of elderly agro-pastoralists in Inner Mongolia,we compared serum NBFRs levels and metabolic biomarkers between Mongolian(n=30)and Han(n=47)populations.The Mongolian group,with relatively higher meat/dairy-rich diets,showed significantly higher NBFR concentrations,body mass index(BMI),and low-density lipoprotein cholesterol(LDL-C).Alarmingly,72.7%of participants were classified as overweight/obese,far exceeding China's national average.Serum pentabromotoluene(PBT),pentabromoethylbenzene(PBEB),and pentabromobenzyl acrylate(PBBA)showed significant positive correlations with BMI(p<0.05).The quantile G-computation(QGC)model further revealed that PBBA exerted particularly prominent effects on BMl.Strikingly,piecewise regression revealed accelerated NBFRs accumulation in individuals with BMI≥28(p<0.05),indicating a bidirectional"NBFRs-BMI feedback loop".Molecular docking studies demonstrated that PBBA and PBT exhibit a higher binding affinity to PPARγthan the conventional agonist Rosiglitazone,with specific interactions at key amino acid residues(ARG-288 and ILE-326)on helix H3.These findings suggest that PBBA and PBT may act as novel PPARγagonists,potentially promoting adipogenesis and consequently leading to weight gain.
基金supported by Beijing Natural Science Foundation grant 8232043Fundamental Research Funds for the Central Universities grant 2022QNPY57.
文摘Halogenated polycyclic aromatic hydrocarbons(HPAHs)and polycyclic aromatic hydrocarbons(PAHs)were determined in human serum samples pooled by donor age(<20,20–29,30–39,40–49 and≥50 y).The pooled samples were collected from four Chinese cities,Yantai(Shandong Province),Ganzi(Sichuan Province),Huaihua(Hunan Province),and Lingshui(Hainan Province).The concentrations of HPAHs and PAHs were in the range of 4.26–633 ng/g lipid and 249–1642 ng/g lipid from the different cities.Although the levels of HPAHs in blood samples varied among the populations of the four cities,1,5-dichloroanthracene(1,5-Cl_(2)Ant)was the predominant contributor to HPAHs in the serum samples,accounting for over 85.7%of its total concentration.Furthermore,1,5-Cl_(2)Ant serum concentrations increased significantly with age.Notably,molecular docking results show that 1,5-Cl_(2)Ant not only ac-quires the ability to bind d-AhR PAS-B domain,but also binds at the similar sites as 2,3,7,8-tetrachlorodibenzo-p-dioxin(TCDD)and benzo[a]pyrene(BaP),suggesting that 1,5-Cl_(2)Ant,like TCDD and BaP,may cause a wide variety of toxicity via AhR-mediated signaling pathways.The bio-accumulation potential of 1,5-Cl_(2)Ant in the human body and its associated toxicity observed in this study need special attention.
