It is extremely important to analyze the contaminative behaviors of Perfluoroalkyl acids(PFAAs) due to their serious threats to urban environments which are closely related to humans. Current study aimed to explore th...It is extremely important to analyze the contaminative behaviors of Perfluoroalkyl acids(PFAAs) due to their serious threats to urban environments which are closely related to humans. Current study aimed to explore the distribution, source apportionment and ecological risk assessment of PFAAs in surface water from Shijiazhuang, China. The concentrations of ΣPFAAs ranged from 19.5 to 125.9 ng/L in the investigation area. Perfluorobutanesulfonic acid(PFBS) and perfluoropentanoic acid(PFPeA) were the predominant contaminants(mean value: 14.3 ng/L and 16.6 ng/L, respectively). The distribution of PFAAs according to geospatial analysis and hierarchical clustering analysis(HCA) showed that higher levels of ΣPFAAs were detected in the southern surface water of Shijiazhuang and there was a stepwise decrease from the wet season to the dry season. Furthermore, based on source apportionment,the dominant potential sources were found to be wastewater treatment plant(WWTP) effluents and industrial discharge. The risk quotients(RQs) revealed low ecological risks of all PFAAs for aquatic organisms in Shijiazhuang surface water. Collectively, this study provided basic data for regulatory strategies for controlling PFAA pollutions in urban surface water.展开更多
As crucial homologous members of per-and polyfluoroalkyl substances(PFASs),perfluoroalkyl acids(PFAAs)have aroused wide public concern because of their unique properties(persistence,bioaccumulation,long-distance migra...As crucial homologous members of per-and polyfluoroalkyl substances(PFASs),perfluoroalkyl acids(PFAAs)have aroused wide public concern because of their unique properties(persistence,bioaccumulation,long-distance migration and toxicity).Studies have shown their potential hazard to wildlife and humans,with food consumption as one of the primary routes of PFAA exposure for general population,especially seafood intake.In this study,17 PFAAs were quantified in 9 shellfish species from Yuhuan City,a typical coastal area of the East China.The total mean concentrations of PFAAs were in the range of 5.03–381 ng/g dry weight(dw),with the highest concentration found in Neverita didyma and the lowest in Babylonia lutosa.Concentrations and composition profiles of PFAAs varied significantly among different species,indicating differences in the bioaccumulation potential of PFAAs among species.Perfluorooctanoic acid(PFOA)was presented as the most abundant PFAA in this study,followed by perfluorobutanoic acid(PFBA).Significant positive correlations were observed among some individual PFAAs(p<0.05),indicating that they may share similar pollution sources or undergo similar compound behaviors.Health risk assessment indicated a relatively high threat for local residents exposed to PFAAs through shellfish consumption.展开更多
Perfluoroalkyl acids(PFAAs)are considered forever chemicals,gaining increasing attention for their hazardous impacts.However,the ecological effects of PFAAs remain unclear.Environmental DNA(eDNA),as the environmental ...Perfluoroalkyl acids(PFAAs)are considered forever chemicals,gaining increasing attention for their hazardous impacts.However,the ecological effects of PFAAs remain unclear.Environmental DNA(eDNA),as the environmental gene pool,is often collected for evaluating the ecotoxicological effects of pollutants.In this study,we found that all PFAAs investigated,including perfluorohexanoic acid,perfluorooctanoic acid,perfluorononanoic acid,and perfluorooctane sulfonate,even at low concentrations(0.02 and 0.05 mg/L),expedited the enzymatic degradation of DNA in a nonlinear dose–effect relationship,with DNA degradation fragment sizes being lower than 1,000 bp and 200 bp after 15 and 30 min of degradation,respectively.This phenomenon was attributed to the binding interaction between PFAAs and AT bases in DNA via groove binding.van der Waals force(especially dispersion force)and hydrogen bonding are the main binding forces.DNA binding with PFAAs led to decreased base stacking and right-handed helicity,resulting in loose DNA structure exposing more digestion sites for degrading enzymes,and accelerating the enzymatic degradation of DNA.The global ecological risk evaluation results indicated that PFAA contamination could cause medium and high molecular ecological risk in 497 samples from 11 contamination-hot countries(such as the USA,Canada,and China).The findings of this study show new insights into the influence of PFAAs on the environmental fates of biomacromolecules and reveal the hidden molecular ecological effects of PFAAs in the environment.展开更多
Perfluoroalkyl acids(PFAAs)are emerging persistent organic pollutants that are globally distributed in the environment.In the present review,the occurrence of PFAAs and their behavior in aquatic ecosystem were summari...Perfluoroalkyl acids(PFAAs)are emerging persistent organic pollutants that are globally distributed in the environment.In the present review,the occurrence of PFAAs and their behavior in aquatic ecosystem were summarized,and the health and ecological risk assessment and the multimedia fate simulation were investigated.PFAAs are most likely to exist in the aqueous phase,and PFAAs in atmosphere are also able to enter water bodies through diffusion and wet and dry deposition and eventually become widely distributed in various environmental media.The air-solid partition is considered to be one of the major factors in the long-distance transportation of the pollutants.The pKa values and organic carbon fraction of the sediment could influence the partition of PFAAs between water and sediment.Otherwise,PFAAs have teratogenic,mutagenic and other toxic effects and they could be accumulated by biota,and magnified through trophic level.The ecological and health risks of PFOA and PFOS were assessment.In order to explore the partition mechanism and reduce the uncertainty of the simulation of the transport,transformation and fate,the experimental methods on physicochemical properties of PFAAs should be developed.Moreover,further studies on toxicities of PFAAs are necessary for health and ecological risk assessment.展开更多
This study examined concentrations of 15 perfluoroalkyl acids（PFAAs） in tissues from male Mozambique tilapia（Oreochromis mossambicus） collected at Loskop Dam, Mpumalanga,South Africa in 2014 and 2016. Nine of the ...This study examined concentrations of 15 perfluoroalkyl acids（PFAAs） in tissues from male Mozambique tilapia（Oreochromis mossambicus） collected at Loskop Dam, Mpumalanga,South Africa in 2014 and 2016. Nine of the 15 PFAAs were detected frequently and were included in statistical analysis and included two of the most commonly known PFAAs,perfluorooctanesulfonic acid（PFOS）（median, 41.6 ng/g） and perfluorooctanoic acid（PFOA）（median, 0.0825 ng/g）. Of the tissues measured, plasma（2016 and 2014 median, 22.2 ng/g）contained the highest PFAA burden followed by（in descending order）： liver（median,11.6 ng/g）, kidney（median, 9.04 ng/g）, spleen（median, 5.92 ng/g）, adipose（median, 2.54 ng/g）, and muscle（median, 1.11 ng/g）. Loskop Dam tilapia have been affected by an inflammatory disease of the adipose tissue known as pansteatitis, so this study also aimed to investigate relationships between PFAA tissue concentrations and incidence of pansteatitis or fish health status. Results revealed that healthy tilapia exhibited an overall higher（p-value 〈 0.05） PFAA burden than pansteatitis-affected tilapia across all tissues.Further analysis showed that organs previously noted in the literature to contain the highest PFAA concentrations, such as kidney, liver, and plasma, were the organs driving the difference in PFAA burden between the two tilapia groups. Care must be taken in the interpretations we draw from not only the results of our study, but also other PFAA measurements made on populations（human and wildlife alike） under differing health status.展开更多
Perfluorinated compounds(PFCs)are ubiquitously distributed in the environment mainly as perfluorocarboxylic acids(PFCAs)and perfluoroalkyl sulfonates(PFASs).In this paper,six PFCAs and two PFASs were quantified in sur...Perfluorinated compounds(PFCs)are ubiquitously distributed in the environment mainly as perfluorocarboxylic acids(PFCAs)and perfluoroalkyl sulfonates(PFASs).In this paper,six PFCAs and two PFASs were quantified in surface and tap water samples from 12 sites around Lake Taihu near Shanghai City in East China.Predominant PFCs were perfluorooctanoic acid(PFOA)and perfluorooctane sulfonate(PFOS),of which the concentration ranges were 6.8–206 and 1.2–45 ng·L^(–1),the geometric means were 35.3 and 9.4 ng·L^(–1),and the median(quartile range)values were 31.4(34.4)and 10.4(10.7)ng·L^(–1),respectively.Other PFCs were also detected but in much lower concentrations than PFOA.The sources of the PFCs were expected to be direct industrial discharges in the Lake Taihu area,and this area was also a possible source of PFCs contaminations in Shanghai district in the downstream.PFCs distributions were found different in the upstream,downstream and north part of Lake Taihu.Occurrences of PFCs in the tap water in Lake Taihu area indicated their exposure to the local people.A brief estimation of the environmental risks by PFCs implied no acute or immediate risks from PFCs to local human health,but chronic risks from PFOA in the tap water should be considered in the downstream regions.展开更多
The deoxyfluorination of carboxylic,sulfonic,phosphinic acids and phosphine oxides is a fundamentally important approach to access acyl fluorides,sulfonyl fluorides and phosphoric fluorides,thus the development of ine...The deoxyfluorination of carboxylic,sulfonic,phosphinic acids and phosphine oxides is a fundamentally important approach to access acyl fluorides,sulfonyl fluorides and phosphoric fluorides,thus the development of inexpensive,stable,easy-to-handle,versatile,and efficient deoxyfluorination reagents is highly desired.Herein,we report the use of potassium salts of perfluoroalkyl ether carboxylic acids(PFECA)featuring CF_(2)0 units as deoxyfluorination reagents,which are generated mainly as by-products in the manufacture of hexafluoropropene oxide(HFPO).The synthesis of acyl fluorides,sulfonyl fluorides and phosphoric fluorides can be realized via carbonic difluoride(COF_(2))generated in situ from thermal degradation of the PFECA salt.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 41907321, 21777182)the Natural Science Foundation of Hebei Province (No. B2019208273)State Key Laboratory of Environmental Chemistry and Ecotoxicology, RCEES, Chinese Academy of Sciences (No. KF2018-17)。
文摘It is extremely important to analyze the contaminative behaviors of Perfluoroalkyl acids(PFAAs) due to their serious threats to urban environments which are closely related to humans. Current study aimed to explore the distribution, source apportionment and ecological risk assessment of PFAAs in surface water from Shijiazhuang, China. The concentrations of ΣPFAAs ranged from 19.5 to 125.9 ng/L in the investigation area. Perfluorobutanesulfonic acid(PFBS) and perfluoropentanoic acid(PFPeA) were the predominant contaminants(mean value: 14.3 ng/L and 16.6 ng/L, respectively). The distribution of PFAAs according to geospatial analysis and hierarchical clustering analysis(HCA) showed that higher levels of ΣPFAAs were detected in the southern surface water of Shijiazhuang and there was a stepwise decrease from the wet season to the dry season. Furthermore, based on source apportionment,the dominant potential sources were found to be wastewater treatment plant(WWTP) effluents and industrial discharge. The risk quotients(RQs) revealed low ecological risks of all PFAAs for aquatic organisms in Shijiazhuang surface water. Collectively, this study provided basic data for regulatory strategies for controlling PFAA pollutions in urban surface water.
基金supported by the National Natural Science Foundation of China(No.22193052)the Special Project of Eco-Environmental Technology for Peak Carbon Dioxide Emissions and Carbon Neutrality,Chinese Academy of Sciences(No.RCEES-TDZ-2021-23)the Taizhou(China)Flexible Talent Introduction Program.
文摘As crucial homologous members of per-and polyfluoroalkyl substances(PFASs),perfluoroalkyl acids(PFAAs)have aroused wide public concern because of their unique properties(persistence,bioaccumulation,long-distance migration and toxicity).Studies have shown their potential hazard to wildlife and humans,with food consumption as one of the primary routes of PFAA exposure for general population,especially seafood intake.In this study,17 PFAAs were quantified in 9 shellfish species from Yuhuan City,a typical coastal area of the East China.The total mean concentrations of PFAAs were in the range of 5.03–381 ng/g dry weight(dw),with the highest concentration found in Neverita didyma and the lowest in Babylonia lutosa.Concentrations and composition profiles of PFAAs varied significantly among different species,indicating differences in the bioaccumulation potential of PFAAs among species.Perfluorooctanoic acid(PFOA)was presented as the most abundant PFAA in this study,followed by perfluorobutanoic acid(PFBA).Significant positive correlations were observed among some individual PFAAs(p<0.05),indicating that they may share similar pollution sources or undergo similar compound behaviors.Health risk assessment indicated a relatively high threat for local residents exposed to PFAAs through shellfish consumption.
基金This work was funded by the National Natural Science Foundation of China(42030713,42107221,42177187)Fundamental Research Funds for the Cornell University(21622109)the Natural Science Foundation of Guangdong Province(2020A1515110535,2018A030310629).
文摘Perfluoroalkyl acids(PFAAs)are considered forever chemicals,gaining increasing attention for their hazardous impacts.However,the ecological effects of PFAAs remain unclear.Environmental DNA(eDNA),as the environmental gene pool,is often collected for evaluating the ecotoxicological effects of pollutants.In this study,we found that all PFAAs investigated,including perfluorohexanoic acid,perfluorooctanoic acid,perfluorononanoic acid,and perfluorooctane sulfonate,even at low concentrations(0.02 and 0.05 mg/L),expedited the enzymatic degradation of DNA in a nonlinear dose–effect relationship,with DNA degradation fragment sizes being lower than 1,000 bp and 200 bp after 15 and 30 min of degradation,respectively.This phenomenon was attributed to the binding interaction between PFAAs and AT bases in DNA via groove binding.van der Waals force(especially dispersion force)and hydrogen bonding are the main binding forces.DNA binding with PFAAs led to decreased base stacking and right-handed helicity,resulting in loose DNA structure exposing more digestion sites for degrading enzymes,and accelerating the enzymatic degradation of DNA.The global ecological risk evaluation results indicated that PFAA contamination could cause medium and high molecular ecological risk in 497 samples from 11 contamination-hot countries(such as the USA,Canada,and China).The findings of this study show new insights into the influence of PFAAs on the environmental fates of biomacromolecules and reveal the hidden molecular ecological effects of PFAAs in the environment.
基金Funding for this study was provided by the National Natural Science Foundation of China(NSFC)(41271462)the Undergraduate Student Research Training Program of the Ministry of Education.
文摘Perfluoroalkyl acids(PFAAs)are emerging persistent organic pollutants that are globally distributed in the environment.In the present review,the occurrence of PFAAs and their behavior in aquatic ecosystem were summarized,and the health and ecological risk assessment and the multimedia fate simulation were investigated.PFAAs are most likely to exist in the aqueous phase,and PFAAs in atmosphere are also able to enter water bodies through diffusion and wet and dry deposition and eventually become widely distributed in various environmental media.The air-solid partition is considered to be one of the major factors in the long-distance transportation of the pollutants.The pKa values and organic carbon fraction of the sediment could influence the partition of PFAAs between water and sediment.Otherwise,PFAAs have teratogenic,mutagenic and other toxic effects and they could be accumulated by biota,and magnified through trophic level.The ecological and health risks of PFOA and PFOS were assessment.In order to explore the partition mechanism and reduce the uncertainty of the simulation of the transport,transformation and fate,the experimental methods on physicochemical properties of PFAAs should be developed.Moreover,further studies on toxicities of PFAAs are necessary for health and ecological risk assessment.
基金supported by the Medical University of South Carolina Center for Global Healthsupported by the South African Research Chairs Initiative of the Department of Science and Technology and National Research Foundation (NRF) of South Africa (Grant No 101054)
文摘This study examined concentrations of 15 perfluoroalkyl acids（PFAAs） in tissues from male Mozambique tilapia（Oreochromis mossambicus） collected at Loskop Dam, Mpumalanga,South Africa in 2014 and 2016. Nine of the 15 PFAAs were detected frequently and were included in statistical analysis and included two of the most commonly known PFAAs,perfluorooctanesulfonic acid（PFOS）（median, 41.6 ng/g） and perfluorooctanoic acid（PFOA）（median, 0.0825 ng/g）. Of the tissues measured, plasma（2016 and 2014 median, 22.2 ng/g）contained the highest PFAA burden followed by（in descending order）： liver（median,11.6 ng/g）, kidney（median, 9.04 ng/g）, spleen（median, 5.92 ng/g）, adipose（median, 2.54 ng/g）, and muscle（median, 1.11 ng/g）. Loskop Dam tilapia have been affected by an inflammatory disease of the adipose tissue known as pansteatitis, so this study also aimed to investigate relationships between PFAA tissue concentrations and incidence of pansteatitis or fish health status. Results revealed that healthy tilapia exhibited an overall higher（p-value 〈 0.05） PFAA burden than pansteatitis-affected tilapia across all tissues.Further analysis showed that organs previously noted in the literature to contain the highest PFAA concentrations, such as kidney, liver, and plasma, were the organs driving the difference in PFAA burden between the two tilapia groups. Care must be taken in the interpretations we draw from not only the results of our study, but also other PFAA measurements made on populations（human and wildlife alike） under differing health status.
基金the National Science and Technology Pillar Program of China(Grant No.2006BAC19B06)the Major Projects on Control and Rectification of Water Body Pollution(2009ZX07313-003).
文摘Perfluorinated compounds(PFCs)are ubiquitously distributed in the environment mainly as perfluorocarboxylic acids(PFCAs)and perfluoroalkyl sulfonates(PFASs).In this paper,six PFCAs and two PFASs were quantified in surface and tap water samples from 12 sites around Lake Taihu near Shanghai City in East China.Predominant PFCs were perfluorooctanoic acid(PFOA)and perfluorooctane sulfonate(PFOS),of which the concentration ranges were 6.8–206 and 1.2–45 ng·L^(–1),the geometric means were 35.3 and 9.4 ng·L^(–1),and the median(quartile range)values were 31.4(34.4)and 10.4(10.7)ng·L^(–1),respectively.Other PFCs were also detected but in much lower concentrations than PFOA.The sources of the PFCs were expected to be direct industrial discharges in the Lake Taihu area,and this area was also a possible source of PFCs contaminations in Shanghai district in the downstream.PFCs distributions were found different in the upstream,downstream and north part of Lake Taihu.Occurrences of PFCs in the tap water in Lake Taihu area indicated their exposure to the local people.A brief estimation of the environmental risks by PFCs implied no acute or immediate risks from PFCs to local human health,but chronic risks from PFOA in the tap water should be considered in the downstream regions.
基金the National Natural Science Foundation of China(Nos.21737004,21672239,and 21421002)Chinese Academy of Science(KF-STS-QYZX-068)is gratefully acknowledged.
文摘The deoxyfluorination of carboxylic,sulfonic,phosphinic acids and phosphine oxides is a fundamentally important approach to access acyl fluorides,sulfonyl fluorides and phosphoric fluorides,thus the development of inexpensive,stable,easy-to-handle,versatile,and efficient deoxyfluorination reagents is highly desired.Herein,we report the use of potassium salts of perfluoroalkyl ether carboxylic acids(PFECA)featuring CF_(2)0 units as deoxyfluorination reagents,which are generated mainly as by-products in the manufacture of hexafluoropropene oxide(HFPO).The synthesis of acyl fluorides,sulfonyl fluorides and phosphoric fluorides can be realized via carbonic difluoride(COF_(2))generated in situ from thermal degradation of the PFECA salt.
