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
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
Liquid-solid phase transfer promotes the interaction of perfluoroalkyl acids(PFAAs)with the microbial system of river sediments,which may affect the environmental behavior of antibiotic resistance genes(ARGs)contained...Liquid-solid phase transfer promotes the interaction of perfluoroalkyl acids(PFAAs)with the microbial system of river sediments,which may affect the environmental behavior of antibiotic resistance genes(ARGs)contained in benthic environments.Sediments collected from the receiving water of the largest fluoropolymer production facility in China were analyzed to investigate the impact of PFAAs on microbial communities and ARG profiles.The main contributors to the PFAAs were perfluorooctanoic acid and perfluorobutanoic acid,whose proportions(86.9%-93.4%)in the downstream surface sediments affected by industrial effluents were significantly higher than in the corresponding upstream samples(53.3%).A reduction in microbial diversity and richness was observed in the presence of high concentrations of PFAAs at the downstream sites.144 ARG subtypes,including three high-risk subtypes(bacA,aac(6′)-I and aadA),were identified in sediment samples.The discharge of fluorochemical effluents also results in a reduction of ARG diversity at subtype level.PFAAs exert a pronounced influence on the profile of ARGs in sediment.PFAAs and water quality parameters(e.g.pH and total phosphorus)were key drivers of the microbial community composition in the sediment.The regulation of microbial communities by PFAAs may represent an important pathway by which these compounds affect ARG profiles.展开更多
The Yellow River is the main source of water for urban and rural area and agricultural irrigation in northern China.Herein,the distribution and risk assessment of perfluoroalkyl acids(PFAAs)were investigated from the ...The Yellow River is the main source of water for urban and rural area and agricultural irrigation in northern China.Herein,the distribution and risk assessment of perfluoroalkyl acids(PFAAs)were investigated from the Yellow River in Shandong Province,China.The total concentration of PFAAs(P PFAAs)in surface water and sediments were 37.5-2128 ng/L(mean:167 ng/L)and not detected6.95 ng/g dry weight(dw)(mean:1.02 ng/g dw),respectively.Short-chain PFAAs-perfluorobutanoic acid(PFBA),perfluorohexanoic acid(PFHxA),and perfluorobutane sulfonic acid(PFBS)were the most prevalent PFAAs in surface water.Source analysis showed that firefighting foam(proportion:31.3%)and textile treatments and food packaging(proportion:30.3%)were the main sources of PFAAs in water.Based on the concentration of PFAAs in water,ecological and potential human health risks were assessed.Perfluorooctanoic acid(PFOA),perfluorononanoate(PFNA),perfluorodecanoate(PFDA)and perfluoroundecanoic acid(PFUnDA)posed nonnegligible ecological risk for some aquatic organisms.Levels of PFAAs(e.g.,PFOA,PFNA,and PFDA etc.)in some water samples were higher than the advisory guidelines of PFAAs concentrations in water worldwide,indicating a potential human health risk.Therefore,PFOA,PFNA,PFDA,and PFUnDA are the key focus of pollutants in the water of the Yellow River in Shandong Province,and the standards and limits of these PFAAs in environments including surface water and sediment should be promoted.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
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 organic pollutants that have attracted significant attention in the fields of environmental chemistry and toxicology.Although PFAAs are pervasive in soils and sediments,there is...Perfluoroalkyl acids(PFAAs)are emerging organic pollutants that have attracted significant attention in the fields of environmental chemistry and toxicology.Although PFAAs are pervasive in soils and sediments,there is a paucity of research regarding their environmental forms and driving mechanisms.This review provides an overview of the classification and biotoxicity of per-and polyfluoroalkyl substances(PFAS),organic pollutant forms,PFAS extraction and analytical methods,the prediction of PFAS distribution in soils,and current PFAS remediation strategies.Four predominant PFAA forms have been proposed in soils:(i)aqueous-extracted PFAAs,(ii)organic-solvent extracted PFAAs,(ii)embedded or sequestered PFAAs,and(iv)covalently bound PFAAs.Furthermore,it suggests suitable extraction methods and predictive models for different PFAA forms,which are instrumental in the research on PFAA speciation and prediction in soils.Simultaneously,it was proposed that elemental cycling and microbial activity may affect the speciation of PFAs.Additionally,the categorization of PFAA forms facilitated the analysis of pollution remediation.Understanding the interplay between PFAA speciation,element cycling,and bacterial activity during soil remediation is essential for understanding remediation mechanisms and assessing the long-term stability of remediation methods.Future studies should expand the investigation of varying PFAA forms in different media,consider the potential binding forms of PFAAs to minerals,organic matter,and microbes,and evaluate the possible mechanisms of PFAA speciation variation.展开更多
Perfluoroalkyl acid analogs(PFAAs)are a class of chemically stable environmentally persistent organic pollutants(POPs)that are difficult to degrade and have a strong capacity to accumulate in the human body.PFAAs have...Perfluoroalkyl acid analogs(PFAAs)are a class of chemically stable environmentally persistent organic pollutants(POPs)that are difficult to degrade and have a strong capacity to accumulate in the human body.PFAAs have been found to be biotoxic to humans and have been detected in various environmental media,especially in the cryosphere at trace concentrations.The cryosphere,sensitively responds to climate change,plays a crucial role in the global water,carbon and energy cycles.However,researches on cryosphere PFAAs especially in Tibetan Plateau(TP)is limited.Therefore,we summarize the physicochemical properties,physiological toxicity,spatiotemporal distribution,sources,diffusion and migration pathways,as well as analysis and removal methods of PFAAs in the cryosphere regions.The results show that PFAAs pollutants are mainly produced and distributed in the more economically developed countries in Europe and the United States,as well as in East Asia,and PFAAs can be transported by atmospheric circulation and water cycle to remote regions including cryosphere regions.The current detection methods for PFAAs in cryosphere need to be further refined for increased accuracy and convenience.There is also a need to develop more effective removal methods that will reduce the environmental and human threats posed by these PFAAs.Finally,we propose key scientific questions for future research in cryosphere including PFAAs redistribution influenced by cryosphere changes,human activities,and the interaction of other spheres.展开更多
Many per-and polyfluoralkyl substances(PFASs)may disrupt maternal thyroid hormone homeostasis in pregnancy.Concerns should be raised regarding the PFASs exposure in pregnant women because thyroid hormones are involved...Many per-and polyfluoralkyl substances(PFASs)may disrupt maternal thyroid hormone homeostasis in pregnancy.Concerns should be raised regarding the PFASs exposure in pregnant women because thyroid hormones are involved in the early development of the fetus.In this study,we measured the concentrations of 13 PFASs,including five novel shortchain PFASs,in serum from 123 pregnant women in Beijing,China.Linear regression models were used to investigate the association between thyroid-stimulating hormone(TSH)or free thyroxine(FT4)levels and PFASs concentrations under consideration of the impacts of pregnancy-induced physiological factors.We found that perfluorobutanoic acid(PFBA)(β=0.189,95%CI=-0.039,0.417,p=0.10)and perfluorodecanoic acid(PFDA)(β=-0.554,95%CI=-1.16,0.049,p=0.071)were suggestive of significant association with TSH in thyroid peroxidase antibody(TPOAb)negative women.No association was observed between all PFASs and FT4 levels after controlling for these confounding factors,such as BMI,gestational weight gain and maternal age.These findings suggest that it should pay more attention to the association between thyroid hormone levels and short-chain PFASs concentrations.Future studies could consider a greater sample and the inclusion of other clinical indicators of thyroid function,such as free T3 and total T3.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
The detection of per-and polyfluoroalkyl substances(PFAS)in water presents a significant challenge for developing countries,requiring urgent attention.This review focuses on understanding the emergence of PFAS in drin...The detection of per-and polyfluoroalkyl substances(PFAS)in water presents a significant challenge for developing countries,requiring urgent attention.This review focuses on understanding the emergence of PFAS in drinking water,health concerns,and removal strategies for PFAS in water systems in developing countries.This review indicates the need for more studies to be conducted in many developing nations due to limited information on the environmental status and fate of PFAS.The health consequences of PFAS in water are enormous and cannot be overemphasized.Efforts are ongoing to legislate a national standard for PFAS in drinking water.Currently,there are few known mitigation efforts from African countries,in contrast to several developing nations in Asia.Therefore,there is an urgent need to develop economically viable techniques that could be integrated into largescale operations to remove PFAS from water systems in the region.However,despite the success achieved with removing long-chain PFAS from water,more studies are required on strategies for eliminating short-chain moieties in water.展开更多
Veined rapa whelks(Rapana venosa)are predatory marine snails that are widely distributed in the coastal water worldwide.In our previous studies,perfluoro-2-methoxy acetic acid(PFMOAA)has been found at extremely high l...Veined rapa whelks(Rapana venosa)are predatory marine snails that are widely distributed in the coastal water worldwide.In our previous studies,perfluoro-2-methoxy acetic acid(PFMOAA)has been found at extremely high levels in this species than in other benthos and fishes in estuaries and coastal waters.However,there is a knowledge gap regarding geographical bioaccumulative characteristics and tissue distribution patterns of PFMOAA in veined rapa whelk.This is the first study to investigate the tissue distributions of 17 legacy per-and polyfluoroalkyl substance(PFAS),6 emerging polyfluoroether sulfonic acids(PFESAs),and 14 emerging perfluoroalkyl ether carboxylic acids(PFECAs)including PFMOAA in the kidney,liver,gill,foot,adductor muscle,Lebrin's gland,gonad,digestive tract,and mixed tissues of the veined rapa whelk(R.venosa)from five regions around the Bohai Sea.Overall,PFMOAA was consistently the predominant PFAS(20.7-93.7%)in all tissues.The kidney presented the highest PFAS concentration,followed by the gill,Lebrin's gland,digestive tract,and liver.Whelks from the Xiaoqing River Estuary showed the highest kidney∑PFAS level(mean 629.2 ng/g dw)compared to those from other regions(119.9 ng/g dw).For PFMOAA,the contributions of the foot and mixed tissues to the whole-body levels were relatively high despite their low concentrations in these tissues.PFOA and PFOS showed the highest concentrations and the largest contributions in terms of whole-body concentrations in Lebrin's glands and the livers,respectively.Further research on the toxicity of PFMOAA and its associated risks to the ecosystem and human beings are urgently needed.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 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supported by the National Key Research and Develop-ment Program of China(No.2021YFC3200805)the National Natu-ral Science Foundation of China(Nos.52325001 and 52170009).
文摘Liquid-solid phase transfer promotes the interaction of perfluoroalkyl acids(PFAAs)with the microbial system of river sediments,which may affect the environmental behavior of antibiotic resistance genes(ARGs)contained in benthic environments.Sediments collected from the receiving water of the largest fluoropolymer production facility in China were analyzed to investigate the impact of PFAAs on microbial communities and ARG profiles.The main contributors to the PFAAs were perfluorooctanoic acid and perfluorobutanoic acid,whose proportions(86.9%-93.4%)in the downstream surface sediments affected by industrial effluents were significantly higher than in the corresponding upstream samples(53.3%).A reduction in microbial diversity and richness was observed in the presence of high concentrations of PFAAs at the downstream sites.144 ARG subtypes,including three high-risk subtypes(bacA,aac(6′)-I and aadA),were identified in sediment samples.The discharge of fluorochemical effluents also results in a reduction of ARG diversity at subtype level.PFAAs exert a pronounced influence on the profile of ARGs in sediment.PFAAs and water quality parameters(e.g.pH and total phosphorus)were key drivers of the microbial community composition in the sediment.The regulation of microbial communities by PFAAs may represent an important pathway by which these compounds affect ARG profiles.
基金supported by the fellowship of China Post-doctoral Science Foundation(2021M693323).
文摘The Yellow River is the main source of water for urban and rural area and agricultural irrigation in northern China.Herein,the distribution and risk assessment of perfluoroalkyl acids(PFAAs)were investigated from the Yellow River in Shandong Province,China.The total concentration of PFAAs(P PFAAs)in surface water and sediments were 37.5-2128 ng/L(mean:167 ng/L)and not detected6.95 ng/g dry weight(dw)(mean:1.02 ng/g dw),respectively.Short-chain PFAAs-perfluorobutanoic acid(PFBA),perfluorohexanoic acid(PFHxA),and perfluorobutane sulfonic acid(PFBS)were the most prevalent PFAAs in surface water.Source analysis showed that firefighting foam(proportion:31.3%)and textile treatments and food packaging(proportion:30.3%)were the main sources of PFAAs in water.Based on the concentration of PFAAs in water,ecological and potential human health risks were assessed.Perfluorooctanoic acid(PFOA),perfluorononanoate(PFNA),perfluorodecanoate(PFDA)and perfluoroundecanoic acid(PFUnDA)posed nonnegligible ecological risk for some aquatic organisms.Levels of PFAAs(e.g.,PFOA,PFNA,and PFDA etc.)in some water samples were higher than the advisory guidelines of PFAAs concentrations in water worldwide,indicating a potential human health risk.Therefore,PFOA,PFNA,PFDA,and PFUnDA are the key focus of pollutants in the water of the Yellow River in Shandong Province,and the standards and limits of these PFAAs in environments including surface water and sediment should be promoted.
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supported by the Guangdong Major Project of Basic and Applied Basic Research (No.2023B0303000006)National Natural Science Foundation of China (Nos.42125704,42261160644,42277479,and 42077307)+2 种基金the Guangzhou Basic and Applied Basic Research Foundation (No.2023A04J0931)the GDAS'Project of Science and Technology Developmen (Nos.2023GDASZH-2023010103,2022GDASZH-2022010201-04,2022GDASZH-2022010105 and 2019GDASYL-0102002-2)Guangdong Foundation for Program of Science and Technology Research (No.2023B1212060044)。
文摘Perfluoroalkyl acids(PFAAs)are emerging organic pollutants that have attracted significant attention in the fields of environmental chemistry and toxicology.Although PFAAs are pervasive in soils and sediments,there is a paucity of research regarding their environmental forms and driving mechanisms.This review provides an overview of the classification and biotoxicity of per-and polyfluoroalkyl substances(PFAS),organic pollutant forms,PFAS extraction and analytical methods,the prediction of PFAS distribution in soils,and current PFAS remediation strategies.Four predominant PFAA forms have been proposed in soils:(i)aqueous-extracted PFAAs,(ii)organic-solvent extracted PFAAs,(ii)embedded or sequestered PFAAs,and(iv)covalently bound PFAAs.Furthermore,it suggests suitable extraction methods and predictive models for different PFAA forms,which are instrumental in the research on PFAA speciation and prediction in soils.Simultaneously,it was proposed that elemental cycling and microbial activity may affect the speciation of PFAs.Additionally,the categorization of PFAA forms facilitated the analysis of pollution remediation.Understanding the interplay between PFAA speciation,element cycling,and bacterial activity during soil remediation is essential for understanding remediation mechanisms and assessing the long-term stability of remediation methods.Future studies should expand the investigation of varying PFAA forms in different media,consider the potential binding forms of PFAAs to minerals,organic matter,and microbes,and evaluate the possible mechanisms of PFAA speciation variation.
基金supported by the Gansu Provincial Science and Technology Program(22ZD6FA005)West Light Foundation of The Chinese Academy of Sciences(xbzg-zdsys-202306)+2 种基金Science Fund for Creative Research Groups of Gansu Province(Grant No.23JRRA567)Taishan Scholars Program of Shandong Province(No.tsqn202312158)Key Research and Development Program of Gansu Province(22YF7FA041)。
文摘Perfluoroalkyl acid analogs(PFAAs)are a class of chemically stable environmentally persistent organic pollutants(POPs)that are difficult to degrade and have a strong capacity to accumulate in the human body.PFAAs have been found to be biotoxic to humans and have been detected in various environmental media,especially in the cryosphere at trace concentrations.The cryosphere,sensitively responds to climate change,plays a crucial role in the global water,carbon and energy cycles.However,researches on cryosphere PFAAs especially in Tibetan Plateau(TP)is limited.Therefore,we summarize the physicochemical properties,physiological toxicity,spatiotemporal distribution,sources,diffusion and migration pathways,as well as analysis and removal methods of PFAAs in the cryosphere regions.The results show that PFAAs pollutants are mainly produced and distributed in the more economically developed countries in Europe and the United States,as well as in East Asia,and PFAAs can be transported by atmospheric circulation and water cycle to remote regions including cryosphere regions.The current detection methods for PFAAs in cryosphere need to be further refined for increased accuracy and convenience.There is also a need to develop more effective removal methods that will reduce the environmental and human threats posed by these PFAAs.Finally,we propose key scientific questions for future research in cryosphere including PFAAs redistribution influenced by cryosphere changes,human activities,and the interaction of other spheres.
基金supported by the National Key R&D Program of China (No. 2018YFA0901200)the National Natural Science Foundation of China (Nos. 21876194 and 21677170)
文摘Many per-and polyfluoralkyl substances(PFASs)may disrupt maternal thyroid hormone homeostasis in pregnancy.Concerns should be raised regarding the PFASs exposure in pregnant women because thyroid hormones are involved in the early development of the fetus.In this study,we measured the concentrations of 13 PFASs,including five novel shortchain PFASs,in serum from 123 pregnant women in Beijing,China.Linear regression models were used to investigate the association between thyroid-stimulating hormone(TSH)or free thyroxine(FT4)levels and PFASs concentrations under consideration of the impacts of pregnancy-induced physiological factors.We found that perfluorobutanoic acid(PFBA)(β=0.189,95%CI=-0.039,0.417,p=0.10)and perfluorodecanoic acid(PFDA)(β=-0.554,95%CI=-1.16,0.049,p=0.071)were suggestive of significant association with TSH in thyroid peroxidase antibody(TPOAb)negative women.No association was observed between all PFASs and FT4 levels after controlling for these confounding factors,such as BMI,gestational weight gain and maternal age.These findings suggest that it should pay more attention to the association between thyroid hormone levels and short-chain PFASs concentrations.Future studies could consider a greater sample and the inclusion of other clinical indicators of thyroid function,such as free T3 and total T3.
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.
基金support received from the Fulbright African Research Scholar Program grant(PS00349260).
文摘The detection of per-and polyfluoroalkyl substances(PFAS)in water presents a significant challenge for developing countries,requiring urgent attention.This review focuses on understanding the emergence of PFAS in drinking water,health concerns,and removal strategies for PFAS in water systems in developing countries.This review indicates the need for more studies to be conducted in many developing nations due to limited information on the environmental status and fate of PFAS.The health consequences of PFAS in water are enormous and cannot be overemphasized.Efforts are ongoing to legislate a national standard for PFAS in drinking water.Currently,there are few known mitigation efforts from African countries,in contrast to several developing nations in Asia.Therefore,there is an urgent need to develop economically viable techniques that could be integrated into largescale operations to remove PFAS from water systems in the region.However,despite the success achieved with removing long-chain PFAS from water,more studies are required on strategies for eliminating short-chain moieties in water.
基金supported by the National Natural Science Foundation of China(U22A20607 and 42149301)Key R&D Program of Shandong Province,China(2022CXPT019)+1 种基金the National Key Research and Development Program of China(2022YFC3105700)Marine Science Program for Guangxi First-Class Discipline,Beibu Gulf University.
文摘Veined rapa whelks(Rapana venosa)are predatory marine snails that are widely distributed in the coastal water worldwide.In our previous studies,perfluoro-2-methoxy acetic acid(PFMOAA)has been found at extremely high levels in this species than in other benthos and fishes in estuaries and coastal waters.However,there is a knowledge gap regarding geographical bioaccumulative characteristics and tissue distribution patterns of PFMOAA in veined rapa whelk.This is the first study to investigate the tissue distributions of 17 legacy per-and polyfluoroalkyl substance(PFAS),6 emerging polyfluoroether sulfonic acids(PFESAs),and 14 emerging perfluoroalkyl ether carboxylic acids(PFECAs)including PFMOAA in the kidney,liver,gill,foot,adductor muscle,Lebrin's gland,gonad,digestive tract,and mixed tissues of the veined rapa whelk(R.venosa)from five regions around the Bohai Sea.Overall,PFMOAA was consistently the predominant PFAS(20.7-93.7%)in all tissues.The kidney presented the highest PFAS concentration,followed by the gill,Lebrin's gland,digestive tract,and liver.Whelks from the Xiaoqing River Estuary showed the highest kidney∑PFAS level(mean 629.2 ng/g dw)compared to those from other regions(119.9 ng/g dw).For PFMOAA,the contributions of the foot and mixed tissues to the whole-body levels were relatively high despite their low concentrations in these tissues.PFOA and PFOS showed the highest concentrations and the largest contributions in terms of whole-body concentrations in Lebrin's glands and the livers,respectively.Further research on the toxicity of PFMOAA and its associated risks to the ecosystem and human beings are urgently needed.
