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
Perfluoroalkyl and polyfluoroalkyl substances(PFASs)pollution with their toxicity,carcinogenicity,and persistence has been concerned worldwide.Research into novel materials for detecting and removing PFASs has increas...Perfluoroalkyl and polyfluoroalkyl substances(PFASs)pollution with their toxicity,carcinogenicity,and persistence has been concerned worldwide.Research into novel materials for detecting and removing PFASs has increased rapidly,particularly in regard to the emergence of well-characterized single-atom materials(SAMs).Owing to the high selectivity,high atom utilization,and abundant active sites of SAMs,these materials exhibit remarkable efficacy in the detection and removal of PFASs.In this work,recent advances in the synthesis of SAMs for the detection and removal PFASs are reviewed.In-depth discussions of the structure-activity relationship and reaction mechanisms have demonstrated the high efficiency,activity,and selectivity of SAMs for the detection,adsorption,and degradation of PFASs.To optimize the application of SAMs in PFASs remediation,this review comprehensively surveys SAMs applications for PFASs and analyzes potential design strategies based on synthesis methods and corresponding properties.Synthesis strategies such as wet-chemistry,which offer ease of operation and high potential for large-scale production,are recommended for the further exploration of specific SAMs for the detection and removal of PFASs.Finally,this review identifies the challenges and opportunities for development of SAMs for the detection and remediation of PFASs,providing an outlook on strategic goals for a green economy and sustainable development.展开更多
The purpose of this study was to determine perfluoroalkyl substances（PFASs） in human serum, urine, hair and nail from general populations, and to investigate the possibility for human urine, hair and nail used as th...The purpose of this study was to determine perfluoroalkyl substances（PFASs） in human serum, urine, hair and nail from general populations, and to investigate the possibility for human urine, hair and nail used as the biomonitoring sample for PFASs exposure. We detected the concentrations of PFHx A, PFOA, PFNA, PFDA, PFUn DA, PFDo A, PFHx S and PFOS in 39 matched human serum, urine, hair and nail samples from Shenzhen in China. The detection frequency and the median level of PFOS were all higher than that of the other PFASs in four matrices. The median concentration of PFOS in serum, urine, hair, and nail were 9.24 ng/mL, 13.96 ng/L, 0.58 ng/g and 0.63 ng/g, respectively. The results of spearman correlation test indicated that nail was an ideal matrix for biomonitoring PFOS rather than human urine and hair in general populations for the non-invasive sampling.展开更多
The levels of six perfluoroalkyl substances（PFASs） in surface sediment and their vertical variations in dated sediment cores from the Haihe River were investigated; studied substances included perfluorooctanoic acid...The levels of six perfluoroalkyl substances（PFASs） in surface sediment and their vertical variations in dated sediment cores from the Haihe River were investigated; studied substances included perfluorooctanoic acid（PFOA）,perfluorononanoic acid（PFNA）,perfluorooctane sulfonate（PFOS）,perfluorodecanoic acid（PFDA）,perfluoroundecanoic acid（PFUnA）,and perfluorododecanoic acid（PFDoA）. Results showed that the total PFAS concentration in surface sediment ranged between 0.52 and 16.33 ng/g dry weight（dw） with an average of3.47 ng/g dw,with PFOS and PFOA as the dominant PFASs. In general,the PFAS concentrations in the mainstream increased from the upper to the lower reaches,except that a drop occurred downstream of the Erdao dam. Although the PFASs in the sediment cores did not show a clear decreasing or increasing trend with depth,the three cores had a similar vertical variation.The PFAS levels were relatively low in the surface sediment,and reached the first high point at8–20 cm as a result of the wide use of PFASs from 1990 to 2000. After that the PFAS levels decreased,and then increased to a second high point at about 40–48 cm,which might be caused by the leaching of PFASs in sediment. Because PFASs have hydrophilic groups and relatively high solubility,the PFASs will transfer from the upper to lower layers of sediment when water infiltration occurs,leading to the fluctuation of PFAS levels in sediment cores. This study suggests that both the temporal variation of sources and transfer processes of PFASs in sediments are important factors influencing the vertical variation of PFASs in sediment cores.展开更多
This study was conducted to examine the association of perfluoroalkyl substance（PFAS）exposure with gestational diabetes mellitus（GDM） risk and postpartum fasting blood glucose.We used a 1：2 matched case–control ...This study was conducted to examine the association of perfluoroalkyl substance（PFAS）exposure with gestational diabetes mellitus（GDM） risk and postpartum fasting blood glucose.We used a 1：2 matched case–control study with 84 GDM subjects and 168 healthy pregnant women from Beijing, China. The maternal blood was collected at 1–2 days before delivery, and eight linear isomers and fourteen branched isomers were determined in maternal serum.Logistic regression analyses were performed to evaluate the associations after adjusting for potential confounders. The median of the sum of levels of total PFASs was 4.24 ng/m L with a interquartile range（IQR） of 2.82–6.54 ng/m L. Although maternal PFAS exposure was not associated with risk of GDM, significant positive associations were observed between evaluated exposure to specific PFAS congeners and increasing blood glucose. The odds ratio（ORs） of the highest category of postpartum fasting blood glucose for perfluoro-1-metylheptylsulfonat（1 m-PFOS）, perfluoro-3/4-metylheptylsulfonat（3 m＋4 m-PFOS）, perfluoro-5-metylheptylsulfonat（5 m-PFOS）, and perfluorohexane sulfonate（PFHx S） were 2.03（95% CI： 1.09–3.77）, 1.93（95% CI：1.04–3.58）, 2.48（95% CI： 1.33–4.65）, and 2.26（95% CI： 1.21–4.21）, respectively, suggesting negative effects of maternal exposure to specific PFAS compounds on glucose metabolism.展开更多
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
Imagine if a group of toxic substances that increase oxidative stress and disrupt glucose and lipid metabolism have been broadly used worldwide for applications such as repellent,food packaging,and non-stick frying pa...Imagine if a group of toxic substances that increase oxidative stress and disrupt glucose and lipid metabolism have been broadly used worldwide for applications such as repellent,food packaging,and non-stick frying pan coatings.Now imagine if some of these substances have half-lives as long as 3-8 years.展开更多
Receptor models have been proved as useful tools to identify source categories and quantitatively calculate the contributions of extracted sources.In this study,sixty surface sediment samples were collected from fourt...Receptor models have been proved as useful tools to identify source categories and quantitatively calculate the contributions of extracted sources.In this study,sixty surface sediment samples were collected from fourteen lakes in Jiangsu Province,China.The total concentrations of C_4–C_（14）-perfluoroalkyl carboxylic acids and perfluorooctane sulfonic acid（∑_（12）PFASs） in sediments ranged from 0.264 to 4.44 ng/g dw（dry weight）,with an average of 1.76 ng/g dw.Three commonly-applied receptor models,namely principal component analysis-multiple linear regression（PCA-MLR）,positive matrix factorization（PMF） and Unmix models,were employed to apportion PFAS sources in sediments.Overall,these three models all could well track the ∑_（12） PFASs concentrations as well as the concentrations explained in sediments.These three models identified consistently four PFAS sources：the textile treatment sources,the fluoropolymer processing aid/fluororesin coating sources,the textile treatment/metal plating sources and the precious metal sources,contributing 28.1%,37.0%,29.7% and 5.3% by PCA-MLR model,30.60%,39.3%,22.4% and 7.7% by PMF model,and 20.6%,52.4%,20.2% and 6.8% by Unmix model to the ∑_（12） PFASs,respectively.Comparative statistics of multiple analytical methods could minimize individual-method weaknesses and provide convergent results to enhance the persuasiveness of the conclusions.The findings could give us a better knowledge of PFAS sources in aquatic environments.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
An on-line solid phase extraction-high performance liquid chromatography-tandem mass spectrometry method for the analysis of perfluoroalkyl substances（PFASs） in water samples was developed.The optimal analytical con...An on-line solid phase extraction-high performance liquid chromatography-tandem mass spectrometry method for the analysis of perfluoroalkyl substances（PFASs） in water samples was developed.The optimal analytical conditions were obtained through the optimization of the extraction efficiency of online solid phase extraction column,sample loading rate and loading volume,and the concentration of ammonium acetate in mobile phase.Under the optimal condition,the analytical method displayed good linearity（r^2〉0.99） for 12 PFASs（C5-C14 perfluoroalkyl carboxylic acids and C6/C8 perfluoroalkyl sulfonic acids） over a concentration range of 0.5-100 ng/L.The limits of quantitation for samples were between 0.025 ng/L and 0.5 ng/L and the relative standard deviations（RSD） of five consecutive analyses were less than 10%for 1 ng/L standard solution.Satisfactory results were obtained using this analytical method for the analysis of perfluoroalkyl substances in Antarctic ice core samples.The recoveries of all perfluoroalkyl substances were in a range of 73%-117%when the samples were spiked with standards at the concentrations of 2.5 ng/L and 25 ng/L.展开更多
Perfluoroalkyl substances （PFASs） are a class of fluorine substituted carboxylic acid, sulfonic acid and alcohol, structurally similar to their corresponding parent compounds. Previous study demonstrated the potenti...Perfluoroalkyl substances （PFASs） are a class of fluorine substituted carboxylic acid, sulfonic acid and alcohol, structurally similar to their corresponding parent compounds. Previous study demonstrated the potential endocrine disruption and reproductive toxicity of perfluorooctane sulfonic acid and perfluorooctanoic acid, two dominant PFASs in animals and humans. We explored the relationship between eleven perfluoroalkyl acids （PFAAs） with different carbon chain length and their ability to inhibit progesterone production in mouse Leydig tumor cells （mLTC-1）. We found an obvious dose-response relationship between progesterone inhibition rate and PFAA exposure concentration in mLTC-1. The relative inhibition rate of progesterone by PFAAs was linearly related to the carbon chain length and molar refractivity of PFAAs. Mitochondrial membrane potential （MMP） decreased after PFAA exposure at the half-maximal inhibitory effect concentration （IC50） of progesterone production in mLTC-1, while the reactive oxygen species （ROS） content increased significantly. These results imply that the inhibition effect of PFAAs on progesterone production might be due, in part, to ROS damage and the decrease in MMP in mLTC-1.展开更多
The perfluoroalkylsulfonylation(CF_(3)SO_(2),C_(2)F_(5)SO_(2)and CHF_(2)SO_(2))in the enaminone C-H bonds has been developed simply via the promotion of molecular iodine by using stable and cheap sodium perfluoroalkyl...The perfluoroalkylsulfonylation(CF_(3)SO_(2),C_(2)F_(5)SO_(2)and CHF_(2)SO_(2))in the enaminone C-H bonds has been developed simply via the promotion of molecular iodine by using stable and cheap sodium perfluoroalkyl sulfinates as coupling partners.The stereoselective synthesis of E-configuratedα-perfluoroalkylsulfonyl enaminones has been realized via unprecedented C-H bond elaboration and C=C double bond configuration inversion by free radical process.展开更多
Certain poly-and perfluoroalkyl substances(PFASs)exhibit significant bioaccumulation/biomagnification behaviors in ecosystems.PFASs,such as perfluorooctane sulfonate(PFOS),perfluorooctanoic acid(PFOA),perfluorohexanes...Certain poly-and perfluoroalkyl substances(PFASs)exhibit significant bioaccumulation/biomagnification behaviors in ecosystems.PFASs,such as perfluorooctane sulfonate(PFOS),perfluorooctanoic acid(PFOA),perfluorohexanesulfonic acid(PFHxS)and related precursors,have elicited attention from both public and national regulatory agencies,which has resulted in worldwide restrictions on their production and use.Apex predators occupy the top trophic positions in ecosystems and are most affected by the biomagnification behavior of PFASs.Meanwhile,the long lifespans of apex predators also lead to the high body burden of PFASs.The high body burden of PFASs might be linked to adverse health effects and even pose a potential threat to their reproduction.As seen in previous reviews of PFASs,knowledge is lacking between the current stage of the PFAS body burden and related effects in apex predators.This review summarized PFAS occurrence in global apex predators,including information on the geographic distribution,levels,profiles,and tissue distribution,and discussed the trophic transfer and ecotoxicity of PFASs.In the case where legacy PFASs were restricted under international convention,the occurrence of novel PFASs,such as 6:2 chlorinated polyfluorinated ether sulfonate(6:2 Cl-PFESA)and perfluoroethylcyclohexane sulfonate(PFECHS),in apex predators arose as an emerging issue.Future studies should develop an effective analytical method and focus on the toxicity and trophic transfer behavior of novel PFASs.展开更多
Intraocular lenses can be manufactured from a wide variety of polymers, but due to the lost cost associated with the use of Poly (methyl methacrylate) (PMMA), it is still the preferred material used in the developing ...Intraocular lenses can be manufactured from a wide variety of polymers, but due to the lost cost associated with the use of Poly (methyl methacrylate) (PMMA), it is still the preferred material used in the developing countries. However, a major drawback to its use is the build-up of calcium containing deposits that are formed on the intraocular lens over a period of time. In an attempt to hinder this deposition, surface modification of medical grade PMMA has been carried out using perfluoroalkyl chain (1,2,4-trifluoro-3-(C10F21CH2O)-7-(N,N)-dimethylaminoacridine) segregation. The segregation was explored using a 1% 1,2,4-trifluoro-3-(C10F21CH2O)-7-(N,N)-dimethyla-minoacridine in two methods: film casting and spin-coating, a thin film onto preformed PMMA discs. Both methods were compared against control PMMA to determine which method provided the best hindrance against calcium containing deposits when immersed in a simulated aqueous humour solution. Characterisation of the surface using scanning electron microscopy coupled with energy;dispersive x-ray analysis indicated that the surface segregation of perfluoroalkyl chains had hindered calcification in both methods. This pleminary research shows promising results of employing perfluoroalkyl chains in the surface segregation of biomaterials that can be employed in intraocular lenses.展开更多
Electron transfer reactions between O-benzoyl t-butylhydroxyl- amine,t-BuNHOCOPh(1)and perfluorodiacyl peroxides(RfCO_2)_2(2)may serve as a novel method for generating useful t-hutyl perfluoroalkyl nitroxldes at room ...Electron transfer reactions between O-benzoyl t-butylhydroxyl- amine,t-BuNHOCOPh(1)and perfluorodiacyl peroxides(RfCO_2)_2(2)may serve as a novel method for generating useful t-hutyl perfluoroalkyl nitroxldes at room temperature in CFCl2-CF2Cl.展开更多
The reaction between 2,5-Dimethylpyrrole (1) and R_FI (2)(R_F: a, Cl(CF_2)_4; b, Cl(CF_2)_6; c, Cl(CF_2)_8; d, n-C_6F_(13); e, n-C_8F_(17)) in the presence of Na_2S_2O_4-NaHCO_3 in acetonitrile resulted in the formati...The reaction between 2,5-Dimethylpyrrole (1) and R_FI (2)(R_F: a, Cl(CF_2)_4; b, Cl(CF_2)_6; c, Cl(CF_2)_8; d, n-C_6F_(13); e, n-C_8F_(17)) in the presence of Na_2S_2O_4-NaHCO_3 in acetonitrile resulted in the formation of 2-perfluoroalkyl-2,5-dimethyl-2H-pyrrole (3) as a major product in good yield.展开更多
The epidemiological associations between the prenatal perfluoroalkyl substances(PFASs)exposure and the reproductive outcomes remain controversial.A continuous evaluation is needed to combine the inconsistent results.I...The epidemiological associations between the prenatal perfluoroalkyl substances(PFASs)exposure and the reproductive outcomes remain controversial.A continuous evaluation is needed to combine the inconsistent results.In this study,we explored the associations between PFASs exposure and the low birth weight(LBW),preterm birth and small for gestational age(SGA).The quality of selected literature,quantitative estimates,publication bias and subgroup analysis were performed on the basis of 17 retrieved articles published before December 2020.The results showed a significant positive association between the perfluorooctane sulfonate(PFOS)exposure and the risk of LBW[Odds ratio(OR)=1.17;95%confidence interval(CI):1.01,1.36;heterogeneity:P=0.30,I2=17%].The positive association was also observed between the PFOS and the risk of preterm birth(OR=1.19;95%CI:1.01,1.39,P=0.007;I2=62%).There was a paucity of evidence regarding the negative effects of perfluorooctanoic acid(PFOA),perfluorohexanesulfonic acid(PFHxS)and perfluorononanoic acid(PFNA)on the pregnancy outcomes.The findings from the subgroup analysis(the sampling period,the birth gender and biologic specimens)did not substantially altered the results of the overall pooled estimate ORs.The increased prevalence of negative birth outcomes with gestational PFASs exposure warrants further explorations from biological process perspective.展开更多
In this work, an efficient and facile method for the preparation of 5-perfluoroalkylation uracils and uracil nucleosides through visible-light-mediated reaction has been developed. The reaction processes in high effic...In this work, an efficient and facile method for the preparation of 5-perfluoroalkylation uracils and uracil nucleosides through visible-light-mediated reaction has been developed. The reaction processes in high efficiency under mild reaction conditions and show broad substrate scope by employing commercial available perfluoroalkyl sources, thus demonstrates high potent application in life and medicinal science.展开更多
The stereoselective syntheses of (Z)-methyl 3-perfluoroalkyl-4-(3-carboethoxy-2-furanyl)-3-butenoates 5a-c were investigated. The reaction of (3-carboethoxy-2-fu-ranyl)-methyltriphenylphosphonium bromide 1 with methyl...The stereoselective syntheses of (Z)-methyl 3-perfluoroalkyl-4-(3-carboethoxy-2-furanyl)-3-butenoates 5a-c were investigated. The reaction of (3-carboethoxy-2-fu-ranyl)-methyltriphenylphosphonium bromide 1 with methyl 2-perfluoroalkynoates 2a-c in the presence of K2CO3 at room temperature gives two adducts, (E)-methyl 3-per-fluoroalkyl-4-( 3-carboethoxy-2-furanyl )-2-triphenylphosphoranylidene-3-butenoates 3a-c and (E)-methyl 3-perfluoroalkyl-4-(3-carboethoxy-2-furanyl)-4-triphenylphos-phoranylidene-2-butenoates 4a-c. (Z)-Methyl 3-perfluoroalkyl-4-(3-carboethoxy-2-furanyl)-3-butenoates 5a-c can be synthesized stereoselectively with high yields when an aqueous DMF solution of 3c, 4c or a mixture of 3a-b and 4a-b was heated at 140℃ for 8 h.展开更多
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 Shenzhen Science and Technology Program(NO.JCYJ20210324094000001).
文摘Perfluoroalkyl and polyfluoroalkyl substances(PFASs)pollution with their toxicity,carcinogenicity,and persistence has been concerned worldwide.Research into novel materials for detecting and removing PFASs has increased rapidly,particularly in regard to the emergence of well-characterized single-atom materials(SAMs).Owing to the high selectivity,high atom utilization,and abundant active sites of SAMs,these materials exhibit remarkable efficacy in the detection and removal of PFASs.In this work,recent advances in the synthesis of SAMs for the detection and removal PFASs are reviewed.In-depth discussions of the structure-activity relationship and reaction mechanisms have demonstrated the high efficiency,activity,and selectivity of SAMs for the detection,adsorption,and degradation of PFASs.To optimize the application of SAMs in PFASs remediation,this review comprehensively surveys SAMs applications for PFASs and analyzes potential design strategies based on synthesis methods and corresponding properties.Synthesis strategies such as wet-chemistry,which offer ease of operation and high potential for large-scale production,are recommended for the further exploration of specific SAMs for the detection and removal of PFASs.Finally,this review identifies the challenges and opportunities for development of SAMs for the detection and remediation of PFASs,providing an outlook on strategic goals for a green economy and sustainable development.
基金funded by the National Natural Science of Foundation of China(Nos.21537001 and 21407033)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB14010100)
文摘The purpose of this study was to determine perfluoroalkyl substances（PFASs） in human serum, urine, hair and nail from general populations, and to investigate the possibility for human urine, hair and nail used as the biomonitoring sample for PFASs exposure. We detected the concentrations of PFHx A, PFOA, PFNA, PFDA, PFUn DA, PFDo A, PFHx S and PFOS in 39 matched human serum, urine, hair and nail samples from Shenzhen in China. The detection frequency and the median level of PFOS were all higher than that of the other PFASs in four matrices. The median concentration of PFOS in serum, urine, hair, and nail were 9.24 ng/mL, 13.96 ng/L, 0.58 ng/g and 0.63 ng/g, respectively. The results of spearman correlation test indicated that nail was an ideal matrix for biomonitoring PFOS rather than human urine and hair in general populations for the non-invasive sampling.
基金supported by the Major State Basic Research Development Program (No.2010CB951104)the National Science Foundation for Distinguished Young Scholars (No.51325902)+1 种基金the Specialized Research Fund for the Doctoral Program of Higher Education (No.20110003110030)the National Natural Science Foundation of China (No.51279010)
文摘The levels of six perfluoroalkyl substances（PFASs） in surface sediment and their vertical variations in dated sediment cores from the Haihe River were investigated; studied substances included perfluorooctanoic acid（PFOA）,perfluorononanoic acid（PFNA）,perfluorooctane sulfonate（PFOS）,perfluorodecanoic acid（PFDA）,perfluoroundecanoic acid（PFUnA）,and perfluorododecanoic acid（PFDoA）. Results showed that the total PFAS concentration in surface sediment ranged between 0.52 and 16.33 ng/g dry weight（dw） with an average of3.47 ng/g dw,with PFOS and PFOA as the dominant PFASs. In general,the PFAS concentrations in the mainstream increased from the upper to the lower reaches,except that a drop occurred downstream of the Erdao dam. Although the PFASs in the sediment cores did not show a clear decreasing or increasing trend with depth,the three cores had a similar vertical variation.The PFAS levels were relatively low in the surface sediment,and reached the first high point at8–20 cm as a result of the wide use of PFASs from 1990 to 2000. After that the PFAS levels decreased,and then increased to a second high point at about 40–48 cm,which might be caused by the leaching of PFASs in sediment. Because PFASs have hydrophilic groups and relatively high solubility,the PFASs will transfer from the upper to lower layers of sediment when water infiltration occurs,leading to the fluctuation of PFAS levels in sediment cores. This study suggests that both the temporal variation of sources and transfer processes of PFASs in sediments are important factors influencing the vertical variation of PFASs in sediment cores.
基金supported by the National Natural Science Foundation of China(Nos.21537001and 21477030)the National Key Research and Development Program of China(No.2017YFC1600502)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB14010100)
文摘This study was conducted to examine the association of perfluoroalkyl substance（PFAS）exposure with gestational diabetes mellitus（GDM） risk and postpartum fasting blood glucose.We used a 1：2 matched case–control study with 84 GDM subjects and 168 healthy pregnant women from Beijing, China. The maternal blood was collected at 1–2 days before delivery, and eight linear isomers and fourteen branched isomers were determined in maternal serum.Logistic regression analyses were performed to evaluate the associations after adjusting for potential confounders. The median of the sum of levels of total PFASs was 4.24 ng/m L with a interquartile range（IQR） of 2.82–6.54 ng/m L. Although maternal PFAS exposure was not associated with risk of GDM, significant positive associations were observed between evaluated exposure to specific PFAS congeners and increasing blood glucose. The odds ratio（ORs） of the highest category of postpartum fasting blood glucose for perfluoro-1-metylheptylsulfonat（1 m-PFOS）, perfluoro-3/4-metylheptylsulfonat（3 m＋4 m-PFOS）, perfluoro-5-metylheptylsulfonat（5 m-PFOS）, and perfluorohexane sulfonate（PFHx S） were 2.03（95% CI： 1.09–3.77）, 1.93（95% CI：1.04–3.58）, 2.48（95% CI： 1.33–4.65）, and 2.26（95% CI： 1.21–4.21）, respectively, suggesting negative effects of maternal exposure to specific PFAS compounds on glucose metabolism.
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.
文摘Imagine if a group of toxic substances that increase oxidative stress and disrupt glucose and lipid metabolism have been broadly used worldwide for applications such as repellent,food packaging,and non-stick frying pan coatings.Now imagine if some of these substances have half-lives as long as 3-8 years.
基金supported by the Mega-projects of Science Research for Water Environmental Improvement(No.2012ZX07101-002)the National Natural Science Foundation of China(No.41521003)
文摘Receptor models have been proved as useful tools to identify source categories and quantitatively calculate the contributions of extracted sources.In this study,sixty surface sediment samples were collected from fourteen lakes in Jiangsu Province,China.The total concentrations of C_4–C_（14）-perfluoroalkyl carboxylic acids and perfluorooctane sulfonic acid（∑_（12）PFASs） in sediments ranged from 0.264 to 4.44 ng/g dw（dry weight）,with an average of 1.76 ng/g dw.Three commonly-applied receptor models,namely principal component analysis-multiple linear regression（PCA-MLR）,positive matrix factorization（PMF） and Unmix models,were employed to apportion PFAS sources in sediments.Overall,these three models all could well track the ∑_（12） PFASs concentrations as well as the concentrations explained in sediments.These three models identified consistently four PFAS sources：the textile treatment sources,the fluoropolymer processing aid/fluororesin coating sources,the textile treatment/metal plating sources and the precious metal sources,contributing 28.1%,37.0%,29.7% and 5.3% by PCA-MLR model,30.60%,39.3%,22.4% and 7.7% by PMF model,and 20.6%,52.4%,20.2% and 6.8% by Unmix model to the ∑_（12） PFASs,respectively.Comparative statistics of multiple analytical methods could minimize individual-method weaknesses and provide convergent results to enhance the persuasiveness of the conclusions.The findings could give us a better knowledge of PFAS sources in aquatic environments.
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 Natural Science Foundation of China(Nos.21377145,21321004)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB01020300)
文摘An on-line solid phase extraction-high performance liquid chromatography-tandem mass spectrometry method for the analysis of perfluoroalkyl substances（PFASs） in water samples was developed.The optimal analytical conditions were obtained through the optimization of the extraction efficiency of online solid phase extraction column,sample loading rate and loading volume,and the concentration of ammonium acetate in mobile phase.Under the optimal condition,the analytical method displayed good linearity（r^2〉0.99） for 12 PFASs（C5-C14 perfluoroalkyl carboxylic acids and C6/C8 perfluoroalkyl sulfonic acids） over a concentration range of 0.5-100 ng/L.The limits of quantitation for samples were between 0.025 ng/L and 0.5 ng/L and the relative standard deviations（RSD） of five consecutive analyses were less than 10%for 1 ng/L standard solution.Satisfactory results were obtained using this analytical method for the analysis of perfluoroalkyl substances in Antarctic ice core samples.The recoveries of all perfluoroalkyl substances were in a range of 73%-117%when the samples were spiked with standards at the concentrations of 2.5 ng/L and 25 ng/L.
基金supported by the National Basic Research Program(973)of China(No.2013CB945004)
文摘Perfluoroalkyl substances （PFASs） are a class of fluorine substituted carboxylic acid, sulfonic acid and alcohol, structurally similar to their corresponding parent compounds. Previous study demonstrated the potential endocrine disruption and reproductive toxicity of perfluorooctane sulfonic acid and perfluorooctanoic acid, two dominant PFASs in animals and humans. We explored the relationship between eleven perfluoroalkyl acids （PFAAs） with different carbon chain length and their ability to inhibit progesterone production in mouse Leydig tumor cells （mLTC-1）. We found an obvious dose-response relationship between progesterone inhibition rate and PFAA exposure concentration in mLTC-1. The relative inhibition rate of progesterone by PFAAs was linearly related to the carbon chain length and molar refractivity of PFAAs. Mitochondrial membrane potential （MMP） decreased after PFAA exposure at the half-maximal inhibitory effect concentration （IC50） of progesterone production in mLTC-1, while the reactive oxygen species （ROS） content increased significantly. These results imply that the inhibition effect of PFAAs on progesterone production might be due, in part, to ROS damage and the decrease in MMP in mLTC-1.
基金financially supported by National Natural Science Foundation of China(No.21861019)Natural Science Foundation of Jiangxi Province(No.20202ACBL203006).
文摘The perfluoroalkylsulfonylation(CF_(3)SO_(2),C_(2)F_(5)SO_(2)and CHF_(2)SO_(2))in the enaminone C-H bonds has been developed simply via the promotion of molecular iodine by using stable and cheap sodium perfluoroalkyl sulfinates as coupling partners.The stereoselective synthesis of E-configuratedα-perfluoroalkylsulfonyl enaminones has been realized via unprecedented C-H bond elaboration and C=C double bond configuration inversion by free radical process.
基金supported by the National Natural Science Foundation of China(Nos.22022611,21906096)the National Key Research and Development Program of China(No.2020YFA0907500)the Youth Innovation Promotion Association of CAS(No.2018052).
文摘Certain poly-and perfluoroalkyl substances(PFASs)exhibit significant bioaccumulation/biomagnification behaviors in ecosystems.PFASs,such as perfluorooctane sulfonate(PFOS),perfluorooctanoic acid(PFOA),perfluorohexanesulfonic acid(PFHxS)and related precursors,have elicited attention from both public and national regulatory agencies,which has resulted in worldwide restrictions on their production and use.Apex predators occupy the top trophic positions in ecosystems and are most affected by the biomagnification behavior of PFASs.Meanwhile,the long lifespans of apex predators also lead to the high body burden of PFASs.The high body burden of PFASs might be linked to adverse health effects and even pose a potential threat to their reproduction.As seen in previous reviews of PFASs,knowledge is lacking between the current stage of the PFAS body burden and related effects in apex predators.This review summarized PFAS occurrence in global apex predators,including information on the geographic distribution,levels,profiles,and tissue distribution,and discussed the trophic transfer and ecotoxicity of PFASs.In the case where legacy PFASs were restricted under international convention,the occurrence of novel PFASs,such as 6:2 chlorinated polyfluorinated ether sulfonate(6:2 Cl-PFESA)and perfluoroethylcyclohexane sulfonate(PFECHS),in apex predators arose as an emerging issue.Future studies should develop an effective analytical method and focus on the toxicity and trophic transfer behavior of novel PFASs.
文摘Intraocular lenses can be manufactured from a wide variety of polymers, but due to the lost cost associated with the use of Poly (methyl methacrylate) (PMMA), it is still the preferred material used in the developing countries. However, a major drawback to its use is the build-up of calcium containing deposits that are formed on the intraocular lens over a period of time. In an attempt to hinder this deposition, surface modification of medical grade PMMA has been carried out using perfluoroalkyl chain (1,2,4-trifluoro-3-(C10F21CH2O)-7-(N,N)-dimethylaminoacridine) segregation. The segregation was explored using a 1% 1,2,4-trifluoro-3-(C10F21CH2O)-7-(N,N)-dimethyla-minoacridine in two methods: film casting and spin-coating, a thin film onto preformed PMMA discs. Both methods were compared against control PMMA to determine which method provided the best hindrance against calcium containing deposits when immersed in a simulated aqueous humour solution. Characterisation of the surface using scanning electron microscopy coupled with energy;dispersive x-ray analysis indicated that the surface segregation of perfluoroalkyl chains had hindered calcification in both methods. This pleminary research shows promising results of employing perfluoroalkyl chains in the surface segregation of biomaterials that can be employed in intraocular lenses.
文摘Electron transfer reactions between O-benzoyl t-butylhydroxyl- amine,t-BuNHOCOPh(1)and perfluorodiacyl peroxides(RfCO_2)_2(2)may serve as a novel method for generating useful t-hutyl perfluoroalkyl nitroxldes at room temperature in CFCl2-CF2Cl.
文摘The reaction between 2,5-Dimethylpyrrole (1) and R_FI (2)(R_F: a, Cl(CF_2)_4; b, Cl(CF_2)_6; c, Cl(CF_2)_8; d, n-C_6F_(13); e, n-C_8F_(17)) in the presence of Na_2S_2O_4-NaHCO_3 in acetonitrile resulted in the formation of 2-perfluoroalkyl-2,5-dimethyl-2H-pyrrole (3) as a major product in good yield.
基金National Natural Science Foundation of China(No.22006010)Shanghai Sailing Program,China(No.19YF1400500)。
文摘The epidemiological associations between the prenatal perfluoroalkyl substances(PFASs)exposure and the reproductive outcomes remain controversial.A continuous evaluation is needed to combine the inconsistent results.In this study,we explored the associations between PFASs exposure and the low birth weight(LBW),preterm birth and small for gestational age(SGA).The quality of selected literature,quantitative estimates,publication bias and subgroup analysis were performed on the basis of 17 retrieved articles published before December 2020.The results showed a significant positive association between the perfluorooctane sulfonate(PFOS)exposure and the risk of LBW[Odds ratio(OR)=1.17;95%confidence interval(CI):1.01,1.36;heterogeneity:P=0.30,I2=17%].The positive association was also observed between the PFOS and the risk of preterm birth(OR=1.19;95%CI:1.01,1.39,P=0.007;I2=62%).There was a paucity of evidence regarding the negative effects of perfluorooctanoic acid(PFOA),perfluorohexanesulfonic acid(PFHxS)and perfluorononanoic acid(PFNA)on the pregnancy outcomes.The findings from the subgroup analysis(the sampling period,the birth gender and biologic specimens)did not substantially altered the results of the overall pooled estimate ORs.The increased prevalence of negative birth outcomes with gestational PFASs exposure warrants further explorations from biological process perspective.
基金financially supported by the Young Talents Cultivation Program of the China Association for Science and Technology(No.2015-41)The Training Programme Foundation for the Talents of the Zun Yi Science and Technology Bureau(No.201540)+1 种基金Key Programs of Guizhou Province(125 Program,No.2015039)The Natural Science Foundation of Jiangsu Province(No.BK20141265)
文摘In this work, an efficient and facile method for the preparation of 5-perfluoroalkylation uracils and uracil nucleosides through visible-light-mediated reaction has been developed. The reaction processes in high efficiency under mild reaction conditions and show broad substrate scope by employing commercial available perfluoroalkyl sources, thus demonstrates high potent application in life and medicinal science.
基金Supported by the National Natural Science Foundation of ChinaFor part XVII of the series, see Chinese J. of Chem. (to be published)
文摘The stereoselective syntheses of (Z)-methyl 3-perfluoroalkyl-4-(3-carboethoxy-2-furanyl)-3-butenoates 5a-c were investigated. The reaction of (3-carboethoxy-2-fu-ranyl)-methyltriphenylphosphonium bromide 1 with methyl 2-perfluoroalkynoates 2a-c in the presence of K2CO3 at room temperature gives two adducts, (E)-methyl 3-per-fluoroalkyl-4-( 3-carboethoxy-2-furanyl )-2-triphenylphosphoranylidene-3-butenoates 3a-c and (E)-methyl 3-perfluoroalkyl-4-(3-carboethoxy-2-furanyl)-4-triphenylphos-phoranylidene-2-butenoates 4a-c. (Z)-Methyl 3-perfluoroalkyl-4-(3-carboethoxy-2-furanyl)-3-butenoates 5a-c can be synthesized stereoselectively with high yields when an aqueous DMF solution of 3c, 4c or a mixture of 3a-b and 4a-b was heated at 140℃ for 8 h.
