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
Poly-and perfluoroalkyl substances(PFASs)are important environmental contaminants globally and in the early 2000s they were shown to be ubiquitous contaminants in Arctic wildlife.Previous reviews by Butt et al.and Let...Poly-and perfluoroalkyl substances(PFASs)are important environmental contaminants globally and in the early 2000s they were shown to be ubiquitous contaminants in Arctic wildlife.Previous reviews by Butt et al.and Letcher et al.have covered studies on levels and trends of PFASs in the Arctic that were available to 2009.The purpose of this review is to focus on more recent work,generally published between 2009 and 2018,with emphasis on PFASs of emerging concern such as perfluoroalkyl carboxylates(PFCAs)and short-chain perfluoroalkyl sulfonates(PFSAs)and their precursors.Atmospheric measurements over the period 2006e2014 have shown that fluorotelomer alcohols(FTOHs)as well as perfluorobutanoic acid(PFBA)and perfluoroctanoic acid(PFOA)are the most prominent PFASs in the arctic atmosphere,all with increasing concentrations at Alert although PFOA concentrations declined at the Zeppelin Station(Svalbard).Results from ice cores show generally increasing deposition of PFCAs on the Devon Ice cap in the Canadian arctic while declining fluxes were found in a glacier on Svalbard.An extensive dataset exists for long-term trends of long-chain PFCAs that have been reported in Arctic biota with some datasets including archived samples from the 1970s and 1980s.Trends in PFCAs over time vary among the same species across the North American Arctic,East and West Greenland,and Svalbard.Most long term time series show a decline from higher concentrations in the early 2000s.However there have been recent(post 2010)increasing trends of PFCAs in ringed seals in the Canadian Arctic,East Greenland polar bears and in arctic foxes in Svalbard.Annual biological sampling is helping to determine these relatively short term changes.Rising levels of some PFCAs have been explained by continued emissions of long-chain PFCAs and/or their precursors and inflows to the Arctic Ocean,especially from the North Atlantic.While the effectiveness of biological sampling for temporal trends in long-chain PFCAs and PFSAs has been demonstrated,this does not apply to the C4eC8ePFCAs,perfluorobutane sulfonamide(FBSA),or perfluorobutane sulfonate(PFBS)which are generally present at low concentrations in biota.In addition to air sampling,sampling abiotic media such as glacial cores,and annual sampling of lake waters and seawater would appear to be the best approaches for investigating trends in the less bioaccumulative PFASs.展开更多
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.
基金We thank the Arctic Monitoring and Assessment Programme(AMAP)and the national programs in the circumpolar countries for their funding and support of this work.We are especially grateful to Simon Wilson,Cynthia de Wit,and the reviewers that read the chapter on PFASs in the original AMAP assessment.We are thankful to the northern communities in circumpolar regions for their cooperation and collection of biological samples that yielded the data reviewed here.DCGM was supported by the King Carl XVI Gustaf Professorship in Environmental Science at the Dept of Environmental Science and Analytical Chemistry,Stockholm University during 2018-19.
文摘Poly-and perfluoroalkyl substances(PFASs)are important environmental contaminants globally and in the early 2000s they were shown to be ubiquitous contaminants in Arctic wildlife.Previous reviews by Butt et al.and Letcher et al.have covered studies on levels and trends of PFASs in the Arctic that were available to 2009.The purpose of this review is to focus on more recent work,generally published between 2009 and 2018,with emphasis on PFASs of emerging concern such as perfluoroalkyl carboxylates(PFCAs)and short-chain perfluoroalkyl sulfonates(PFSAs)and their precursors.Atmospheric measurements over the period 2006e2014 have shown that fluorotelomer alcohols(FTOHs)as well as perfluorobutanoic acid(PFBA)and perfluoroctanoic acid(PFOA)are the most prominent PFASs in the arctic atmosphere,all with increasing concentrations at Alert although PFOA concentrations declined at the Zeppelin Station(Svalbard).Results from ice cores show generally increasing deposition of PFCAs on the Devon Ice cap in the Canadian arctic while declining fluxes were found in a glacier on Svalbard.An extensive dataset exists for long-term trends of long-chain PFCAs that have been reported in Arctic biota with some datasets including archived samples from the 1970s and 1980s.Trends in PFCAs over time vary among the same species across the North American Arctic,East and West Greenland,and Svalbard.Most long term time series show a decline from higher concentrations in the early 2000s.However there have been recent(post 2010)increasing trends of PFCAs in ringed seals in the Canadian Arctic,East Greenland polar bears and in arctic foxes in Svalbard.Annual biological sampling is helping to determine these relatively short term changes.Rising levels of some PFCAs have been explained by continued emissions of long-chain PFCAs and/or their precursors and inflows to the Arctic Ocean,especially from the North Atlantic.While the effectiveness of biological sampling for temporal trends in long-chain PFCAs and PFSAs has been demonstrated,this does not apply to the C4eC8ePFCAs,perfluorobutane sulfonamide(FBSA),or perfluorobutane sulfonate(PFBS)which are generally present at low concentrations in biota.In addition to air sampling,sampling abiotic media such as glacial cores,and annual sampling of lake waters and seawater would appear to be the best approaches for investigating trends in the less bioaccumulative PFASs.