An efficient, highly selective method for polyfluoroalkylation of 2-aminothiazole derivatives was described. Specifically, a di-polyfluoroalkylated derivative was produced when 2-amino-4-chloromethylthiazole was react...An efficient, highly selective method for polyfluoroalkylation of 2-aminothiazole derivatives was described. Specifically, a di-polyfluoroalkylated derivative was produced when 2-amino-4-chloromethylthiazole was reacted with perfluoroalkyl iodides under very mild conditions.展开更多
Reclaimed water for irrigation or hydroponic cultivation provides exposure pathways for per-and polyfluoroalkyl substances(PFAS)to enter the human food chain.This study employed hydroponic methods to investigate the b...Reclaimed water for irrigation or hydroponic cultivation provides exposure pathways for per-and polyfluoroalkyl substances(PFAS)to enter the human food chain.This study employed hydroponic methods to investigate the behavior of legacy PFAS and emerging chlorinated polyfluoroalkyl ether sulfonic acids(Cl-PFESAs)in lettuce grown under environment-related exposure levels and assessed the human exposure risks from consuming contaminated lettuce.Overall,PFAS in lettuce were concentration-dependent,with long-chain PFAS tending to accumulate in roots and short-chain PFAS accumulating more in shoots.The enrichment of PFAS in lettuce was jointly influenced by their chain length and polar functional groups.Specifically,the root concentration factors(RCFs)of PFAS generally increased with increasing chain length,and RCF values of most perfluoroalkanesulfonic acids(PFSAs)were significantly higher than those of perfluoroalkyl carboxylic acids(PFCAs)with the same chain length(p<0.01),while the translocation factors(TFs)exhibited opposite trends.RCF values of perfluorooctane sulfonate(PFOS)and its alternatives,Cl-PFESAs,were ranked as follows:8:2 Cl-PFESA(mean:139)>6:2 Cl-PFESA(28.6)>PFOS(25.7),which was attributed to the increased molecular size and hydrophobicity resulting from the insertion of ether bonds and additional CF2 in 8:2 Cl-PFESA.Notably,TF value of 8:2 Cl-PFESA(mean:0.007)was the smallest among all PFAS,indicating 8:2 Cl-PFESA was difficult to transfer to nutritional compartments.Adults and children would exceed the most conservative health-based reference dose(RfD)by consuming approximately 15.9–148 g and 7.92–74.0 g of contaminated lettuce per day,implying high health risks.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
Objective To investigate the associations between eight serum per-and polyfluoroalkyl substances(PFASs)and regional fat depots,we analyzed the data from the National Health and Nutrition Examination Survey(NHANES)2011...Objective To investigate the associations between eight serum per-and polyfluoroalkyl substances(PFASs)and regional fat depots,we analyzed the data from the National Health and Nutrition Examination Survey(NHANES)2011-2018 cycles.Methods Multiple linear regression models were developed to explore the associations between serum PFAS concentrations and six fat compositions along with a fat distribution score created by summing the concentrations of the six fat compositions.The associations between structurally grouped PFASs and fat distribution were assessed,and a prediction model was developed to estimate the ability of PFAS exposure to predict obesity risk.Results Among females aged 39-59 years,trunk fat mass was positively associated with perfluorooctane sulfonate(PFOS).Higher concentrations of PFOS,perfluorohexane sulfonate(PFHxS),perfluorodecanoate(PFDeA),perfluorononanoate(PFNA),and n-perfluorooctanoate(n-PFOA)were linked to greater visceral adipose tissue in this group.In men,exposure to total perfluoroalkane sulfonates(PFSAs)and long-chain PFSAs was associated with reductions in abdominal fat,while higher abdominal fat in women aged 39-59 years was associated with short-chain PFSAs.The prediction model demonstrated high accuracy,with an area under the curve(AUC)of 0.9925 for predicting obesity risk.Conclusion PFAS exposure is associated with regional fat distribution,with varying effects based on age,sex,and PFAS structure.The findings highlight the potential role of PFAS exposure in influencing fat depots and obesity risk,with significant implications for public health.The prediction model provides a highly accurate tool for assessing obesity risk related to PFAS exposure.展开更多
Per-and polyfluoroalkyl substances(PFASs)can induce a range of adverse health effects,with the precise molecularmechanisms remaining elusive.Extracellular vesicles(EVs)have demonstrated their potential to elucidate un...Per-and polyfluoroalkyl substances(PFASs)can induce a range of adverse health effects,with the precise molecularmechanisms remaining elusive.Extracellular vesicles(EVs)have demonstrated their potential to elucidate unknown molecular mechanisms.Building upon the close alignment of their biological functions with the observed health effects of PFASs,this study innovatively focuses on proteomic insights from EVs into the molecular mechanisms underlying the systemic health effects of PFASs.Through rat exposure experiments and proteomics technology,it not only demonstrated the occurrence of PFASs in EVs but also revealed the alterations in the serum EVs and the expression of their protein cargos following mixed exposure to PFASs,leading to changes in related pathways.These changes encompass various biological processes,including proteasome activity,immune response,cytoskeletal organization,oxidative stress,cell signaling,and nervous system function.Particularly noteworthy is the uncovering of the activation of the proteasome pathway,highlighting significant key contributing proteins.These novel findings provide a new perspective for exploring the molecularmechanism underlying the systemic health effects of PFASs and offer reliable screening for potential biomarkers.Additionally,comparisons with serum confirmed the potential of serum EVs as biological responders and measurable endpoints for evaluating PFASs-induced toxicity.展开更多
Although per-and polyfluoroalkyl substances(PFAS)have been frequently linked to cardiovascular and renal disease separately,evidence remains scarce regarding their systematic effect.Therefore,we recruited 546 newly di...Although per-and polyfluoroalkyl substances(PFAS)have been frequently linked to cardiovascular and renal disease separately,evidence remains scarce regarding their systematic effect.Therefore,we recruited 546 newly diagnosed acute coronary syndrome(ACS)patients and detected seven myocardial enzymes and six kidney function biomarkers.Twelve PFASwere also assessedwith ultra-high-performance liquid chromatography-tandem mass spectrometry.Generalized linear model and restricted cubic spline model were applied to single pollutant analysis.Quantile g-computation was used for mixture analysis.Network model was utilized to identify central and bridge nodes of pollutants and phenotypes.In the present study,perfluorohexane sulfonic acid was positively associated with uric acid(UA)(β=0.04,95%confidence interval(CI):0.01,0.07),and perfluorobutanoic acid was negatively associated with estimated glomerular filtration rate(β=-0.04,95%CI:-0.07,-0.01)but positively associated with UA(β=0.03,95%CI:0.01,0.06).In mixture analysis,each quantile increase in the PFAS mixture was significantly associated with UA(β=0.08,95%CI:0.04,0.11).Network analysis revealed that perfluorooctanoate,UA,and myoglobin were denoted as bridge nodes,and the first principal component of lactate dehydrogenase and creatine kinase-myocardial band was identified as the node with the highest strength and expected influence.This study investigates the systematic impact of PFAS exposure through cardiorenal interaction network,which highlights that PFAS may serve as an upstream approach in UA-modulated cardiorenal network to affect cardiorenal system comprehensively.展开更多
Previous studies have suggested that abnormal hepatobiliary system function may contribute to poor prognosis in patientswith acute coronary syndrome(ACS)and that abnormal hepatobiliary system function may be associate...Previous studies have suggested that abnormal hepatobiliary system function may contribute to poor prognosis in patientswith acute coronary syndrome(ACS)and that abnormal hepatobiliary system function may be associated with per-and polyfluoroalkyl substances(PFAS)exposure.However,there is limited evidence for this association in cardiovascular subpopulations,particularly in the ACS patients.Therefore,we performed this study to evaluate the association between plasma PFAS exposure and hepatobiliary system function biomarkers in patients with ACS.This study included 546 newly diagnosed ACS patients at the Second Hospital of Hebei Medical University,and data on 15 hepatobiliary system function biomarkers were obtained from medical records.Associations between single PFAS and hepatobiliary system function biomarkers were assessed using multiple linear regression models and restricted cubic spline model(RCS),and mixture effects were assessed using the Quantile g-computation model.The results showed that total bile acids(TBA)was negative associated with perfluorohexane sulfonic acid(PFHxS)(-7.69%,95%CI:-12.15%,-3.01%).According to the RCS model,linear associations were found between TBA and PFHxS(P for overall=0.003,P for non-linear=0.234).We also have observed the association between between PFAS congeners and liver enzyme such as aspartate aminotransferase(AST)and α-l-Fucosidase(AFU),but it was not statistically significant after correction.In addition,Our results also revealed an association between prealbumin(PA)and PFAS congeners as well as mixtures.Our findings have provided a piece of epidemiological evidence on associations between PFAS congeners or mixture,and serum hepatobiliary system function biomarkers in ACS patients,which could be a basis for subsequent mechanism studies.展开更多
Associations of per-and polyfluoroalkyl substances(PFAS)on lipid metabolism have been documented but research remains scarce regarding effect of PFAS on lipid variability.To deeply understand their relationship,a step...Associations of per-and polyfluoroalkyl substances(PFAS)on lipid metabolism have been documented but research remains scarce regarding effect of PFAS on lipid variability.To deeply understand their relationship,a step-forward in causal inference is expected.To address these,we conducted a longitudinal study with three repeated measurements involving 201 participants in Beijing,among which 100 eligible participants were included for the present study.Twenty-three PFAS and four lipid indicators were assessed at each visit.We used linear mixed models and quantile g-computation models to investigate associations between PFAS and blood lipid levels.A latent class growth model described PFAS serum exposure patterns,and a generalized linear model demonstrated associations between these patterns and lipid variability.Our study found that PFDA was associated with increased TC(β=0.083,95%CI:0.011,0.155)and HDL-C(β=0.106,95%CI:0.034,0.178).The PFAS mixture also showed a positive relationship with TC(β=0.06,95%CI:0.02,0.10),with PFDA contributing most positively.Compared to the low trajectory group,the middle trajectory group for PFDA was associated with VIM of TC(β=0.756,95%CI:0.153,1.359).Furthermore,PFDA showed biological gradientswith lipid metabolism.This is the first repeated-measures study to identify the impact of PFAS serum exposure pattern on the lipid metabolism and the first to estimate the association between PFAS and blood lipid levels in middle-aged and elderly Chinese and reinforce the evidence of their causal relationship through epidemiological studies.展开更多
[Objectives]To extract and purify perfluoroalkyl and polyfluoroalkyl substances(PFAS)from aquatic products and determine the optimal pretreatment conditions.[Methods]The QuEChERS method was employed for the extraction...[Objectives]To extract and purify perfluoroalkyl and polyfluoroalkyl substances(PFAS)from aquatic products and determine the optimal pretreatment conditions.[Methods]The QuEChERS method was employed for the extraction and purification of PFAS in aquatic products.The detection of PFAS was carried out using liquid chromatography-tandem mass spectrometry(LC-MS/MS)in ESI negative ion mode with multiple reaction monitoring(MRM),and quantification was performed using the external standard method.By optimizing instrument parameters such as ion source temperature,spray voltage,and collision energy,high selectivity and sensitivity of the detection were ensured.[Results]The established calibration curves for 28 PFAS compounds compounds,covering a range of 0.02 to 20 ng/mL,demonstrated excellent linearity.Spike recovery tests yielded limits of detection(LOD)between 0.02 and 0.5μg/kg for the 28 PFAS compounds compounds,with recovery rates ranging from 72.2%to 113.0%.[Conclusions]The method established in this study demonstrates excellent linearity,and is accurate,reliable,efficient,simple,and rapid.It possesses considerable practical applicability and can be used for the quality and risk assessment of 28 PFAS compounds compounds in aquatic products,indicating high practical utility.展开更多
In this work, a method was developed and optimized for the analysis of polyfluoroalkyl and/or perfluoroalkyl substances（PFASs） content in surface water and sediment samples with high instrumental response and good s...In this work, a method was developed and optimized for the analysis of polyfluoroalkyl and/or perfluoroalkyl substances（PFASs） content in surface water and sediment samples with high instrumental response and good separation. Surface water and sediment samples were collected from the Yangtze River Delta（YRD） to analyze the distribution characteristics of perfluoroalkyl carboxylic acids（PFCAs）, perfluoroalkane sulfonic acids（PFSAs）, perfluoroalkyl phosphonic acids（PFPAs）, perfluoroalkyl phosphinic acids（PFPiAs）, and polyfluoroalkyl phosphoric acid diesters（di PAPs）. The results showed that the total concentrations of PFCAs and PFSAs in YRD varied from 31 to 902 ng/L. PFCAs（≥ 11 carbons） and PFSAs（≥ 10 carbons atoms） were not detected in any surface water samples. The mean concentrations of all PFCAs and PFSAs in surface water from the sampling areas decreased in the following order：Yangtze river（191 ng/L） ≈ Taihu lake（189 ng/L） 〉 Huangpu river（122 ng/L） ≈ Qiantang river（120 ng/L） 〉 Jiaxing urban river（100 ng/L）. Strong significant（p 〈 0.05） correlations between the concentrations of many of the compounds were found in the sampling areas, suggesting a common source for these compounds. Only perfluorooctanoic acid（PFOA） was observed in all sediment samples, at concentrations varying from 0.02 to 1.35 ng/g. Finally, detection rates of two di PAPs were only 8% and 10%, respectively and the concentration of di PAPs was two to three times lower compared to PFCAs and PFSAs.展开更多
Studies have shown that per-and polyfluoroalkyl substances(PFASs)may be hepatotoxic in animals or humans.However,data on clinical epidemiology are very limited.In this study,21PFASs were determined in patients with li...Studies have shown that per-and polyfluoroalkyl substances(PFASs)may be hepatotoxic in animals or humans.However,data on clinical epidemiology are very limited.In this study,21PFASs were determined in patients with liver diseases,with the highest median concentrations detected in the serum sample(26.7 ng/mL),followed by blood(10.7 ng/mL)and urine(5.02 ng/mL).Higher total PFAS concentrations were found in hepatocellular carcinoma(HCC)patients compared to non-HCC patients,with significant discrepancies in serum and blood samples.Besides,significant correlations were also found among PFAS concentrations and age,gender,body mass index(BMI),and liver function biomarkers levels.For example,PFAS concentrations are significantly higher in males than in females;Several serum PFASs concentrations increase with age and BMI,while the serum perfluorohexane sulfonic acid(PFHxS)concentrations are negatively correlated with age.In addition,multiple regression models adjusted for age,gender and BMI found that increased serum perfluorobutane sulfonic acid(PFBS),perfluoroheptane sulfonic acid(PFHpS)and perfluorohexylphosphonic acid(PFHxPA)conentrations are correlated with elevated alkaline phosphatase(ALP),aspartate aminotransferase(AST),and alpha-fetoprotein(AFP)(p<0.05).Our results provide epidemiological support for the future study on the potential clinical hepatotoxicity of PFAS.展开更多
Perfluorooctanoic acid(PFOA), its salts, and related compounds were listed as new persistent organic pollutants by the Stockholm Convention in 2019.In this study, the occurrence of residues of PFOA and other per-and p...Perfluorooctanoic acid(PFOA), its salts, and related compounds were listed as new persistent organic pollutants by the Stockholm Convention in 2019.In this study, the occurrence of residues of PFOA and other per-and polyfluoroalkyl substances(PFASs) in raw materials and fluoropolymer products from the Chinese fluoropolymer industries are reported for the first time.The PFOA concentrations in raw materials and fluoropolymer products were in the range of 6.7 to 1.1 × 10^(6) ng/g, and <MDL(method detection limit) to 5.3 × 10^(3) ng/g,respectively.Generally, the levels of PFOA in raw materials were higher than in products,implying that PFOA in the emulsion/dispersion resin could be partly removed during the polymerization or post-processing steps.By tracking a company’s polytetrafluoroethylene(PTFE) production line, it was found that over a 5 year period, the residual levels of PFOA in emulsion samples declined from 1.1 × 10^(6) to 28.4 ng/g, indicating that the contamination of PFOA in fluoropolymer products from production source gradually decreased after its use had been discontinued.High concentrations of HFPO-TrA(2.7 × 10^(5) to 8.2 × 10^(5) ng/g) were detected in some emulsion samples indicating this alternative has been widely applied in fluoropolymer manufacturing in China.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
PFAS(per-and polyfluoroalkyl substances)are omnipresent in the environment and their transportation and transformation have attracted increased attention.Microplastics are another potential risk substances that can se...PFAS(per-and polyfluoroalkyl substances)are omnipresent in the environment and their transportation and transformation have attracted increased attention.Microplastics are another potential risk substances that can serve as a carrier for ubiquitous pollutants,thus affecting the presence of PFAS in the environment.In this study,the adsorption of perfluorooctane sulfonamide(FOSA)and perfluorooctanoic acid(PFOA)on four microplastics(PE,PVC,PS,and PTFE)and their effect on the photodegradation of FOSA were studied.The adsorption capacity of FOSA by PS was the highest,in similar,PS displayed the highest adsorption capacity in the presence of PFOA.Different effects of pH and salinity on the adsorption of FOSA and PFOA were observed among different microplastics indicating inconsistent interaction mechanisms.Furthermore,FOSA could be photodegraded,with PFOA as the main product,while the presence of microplastics had a negligible effect on the degradation of this contaminant.The results indicated that microplastics could act as PFAS concentrators.Moreover,their photochemical inertiasmake the pollutants enriched onmicroplastics more resistant to degradation.展开更多
A novel synthesis of polyfluoroalkyl substituted -butyrolactones from the reaction of polyfluoroalkyl iodides with 4-pentenoic acid initiated with sodium dithionite was realized in good yields.
In order to discover new molecules with good insecticidal activities, a series of anthranilic diamides containing polyfluoroalkyl pyrazole were designed and synthesized, and their structures were characterized by1 H N...In order to discover new molecules with good insecticidal activities, a series of anthranilic diamides containing polyfluoroalkyl pyrazole were designed and synthesized, and their structures were characterized by1 H NMR and HRMS. Bioassays demonstrated that some of the title compound exhibited excellent insecticidal activities. The larvicidal activities of compound 8a, 8c, 8g, 8k and 8l against Mythimna separata Walker were 100% at 0.8 mg/L. The insecticidal activities of compound 8a, 8c,8e, 8g, 8k and 8l against Plutella xylostella Linnaeus were 100% at 0.4 mg/L. Surprisingly compounds 8a and 8c still showed 100% larvicidal activities against Plutella xylostella Linnaeus at 0.08 mg/L comparable to the commercialized Chlorantraniliprole. The LC_（50） of compound 8a and 8c against M. separata is 0.048 and 0.043 mg/L respectively.展开更多
Per-and polyfluoroalkyl substances(PFASs)are emerging persistent organic pollutants(POPs).In this study,47 surface sediment samples were collected from the Yellow River Delta wetland(YRDW)to investigate the occurrence...Per-and polyfluoroalkyl substances(PFASs)are emerging persistent organic pollutants(POPs).In this study,47 surface sediment samples were collected from the Yellow River Delta wetland(YRDW)to investigate the occurrence,spatial distribution,potential sources,and ecological risks of PFASs.Twenty-three out of 26 targeted PFASs were detected in surface sediment samples from the YRDW,with totalΣ23PFASs concentrations ranging from 0.23 to 16.30 ng g^(-1) dw and a median value of 2.27 ng g^(-1) dw.Perfluorooctanoic acid(PFOA),perfluorobutanoic acid(PFBA)and perfluorooctanesulfonic acid(PFOS)were the main contaminants.The detection frequency and concentration of perfluoroalkyl carboxylic acids(PFCAs)were higher than those of perfluoroal-kanesulfonic acids(PFSAs),while those of long-chain PFASs were higher than those of short-chain PFASs.The emerging PFASs substitutes were dominated by 6:2 chlorinated polyfluoroalkyl ether sulfonic acid(6:2 Cl-PFESA).The distribution of PFASs is significantly influenced by the total organic carbon content in the sediments.The concentration of PFASs seems to be related to human activities,with high concentration levels of PFASs near locations such as beaches and villages.By using a positive matrix factorization model,the potential sources of PFASs in the region were identified as metal plating mist inhibitor and fluoropolymer manufacturing sources,metal plating industry and firefighting foam and textile treatment sources,and food packaging material sources.The risk assessment indicated that PFASs in YRDW sediments do not pose a significant ecological risk to benthic organisms in the region overall,but PFOA and PFOS exert a low to moderate risk at individual stations.展开更多
The passive sampling technique, diffusive gradients in thin films(DGT) has attracted increasing interests as an in-situ sampler for organic contaminants including per-and polyfluoroalkyl substances(PFAS). However, its...The passive sampling technique, diffusive gradients in thin films(DGT) has attracted increasing interests as an in-situ sampler for organic contaminants including per-and polyfluoroalkyl substances(PFAS). However, its effectiveness has been questioned because of the small effective sampling area(3.1 cm^(2)). In this study, we developed a DGT probe for rapid sampling of eight PFAS in waters and applied it to a water-sediment system. It has a much larger sampling area(27 cm^(2)) and as a result lower method quantification limits(0.15 –0.21 ng/L for one-day deployment and 0.02 – 0.03 ng/L for one-week deployment) and much higher(by > 10 factors) sampling rate(100 m L/day) compared to the standard DGT(piston configuration). The sampler could linearly accumulate PFAS from wastewater, was sensitive enough even for a 24 hr deployment with performance comparable to grab sampling(500m L). The DGT probe provided homogeneous sampling performance along the large exposure area. The use of the probe to investigate distributions of dissolved PFAS around the sediment-water interface was demonstrated. This work, for the first time, demonstrated that the DGT probe is a promising monitoring tool for trace levels of PFAS and a research tool for studying their distribution, migration, and fate in aquatic environments including the sediment-water interface.展开更多
基金Project supported by special Fund for Agro-scientific Research in the Public Interest （No. 201103007）, the National Key Technologies R＆D Program （No. 2011BAE06B05）, National Basic Research Program of China （No. 2010CB126103）, the Key Program of National Natural Science Foundation of China （No. 21032006） and SIOC startup fund.
文摘An efficient, highly selective method for polyfluoroalkylation of 2-aminothiazole derivatives was described. Specifically, a di-polyfluoroalkylated derivative was produced when 2-amino-4-chloromethylthiazole was reacted with perfluoroalkyl iodides under very mild conditions.
基金supported by the Fundamental Research Funds for Central Non-profit Scientific Institution(No.1610132022015)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0750200)the National Natural Science Foundation of China(No.22176198).
文摘Reclaimed water for irrigation or hydroponic cultivation provides exposure pathways for per-and polyfluoroalkyl substances(PFAS)to enter the human food chain.This study employed hydroponic methods to investigate the behavior of legacy PFAS and emerging chlorinated polyfluoroalkyl ether sulfonic acids(Cl-PFESAs)in lettuce grown under environment-related exposure levels and assessed the human exposure risks from consuming contaminated lettuce.Overall,PFAS in lettuce were concentration-dependent,with long-chain PFAS tending to accumulate in roots and short-chain PFAS accumulating more in shoots.The enrichment of PFAS in lettuce was jointly influenced by their chain length and polar functional groups.Specifically,the root concentration factors(RCFs)of PFAS generally increased with increasing chain length,and RCF values of most perfluoroalkanesulfonic acids(PFSAs)were significantly higher than those of perfluoroalkyl carboxylic acids(PFCAs)with the same chain length(p<0.01),while the translocation factors(TFs)exhibited opposite trends.RCF values of perfluorooctane sulfonate(PFOS)and its alternatives,Cl-PFESAs,were ranked as follows:8:2 Cl-PFESA(mean:139)>6:2 Cl-PFESA(28.6)>PFOS(25.7),which was attributed to the increased molecular size and hydrophobicity resulting from the insertion of ether bonds and additional CF2 in 8:2 Cl-PFESA.Notably,TF value of 8:2 Cl-PFESA(mean:0.007)was the smallest among all PFAS,indicating 8:2 Cl-PFESA was difficult to transfer to nutritional compartments.Adults and children would exceed the most conservative health-based reference dose(RfD)by consuming approximately 15.9–148 g and 7.92–74.0 g of contaminated lettuce per day,implying high health risks.
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supported by the National Key R&D Program of China(No.2021YFC2700605)the National Natural Science Foundation of China(82071700 and 82101679)+4 种基金333 High-level Talent Training Project of the Jiangsu Province((2022)3-16-425)the Natural Science Foundation of Jiangsu Province(BK20220317)Jiangsu Funding Program for Excellent Postdoctoral Talent(2022ZB414)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJB330001)China Postdoctoral Science Foundation(2022M711673).
文摘Objective To investigate the associations between eight serum per-and polyfluoroalkyl substances(PFASs)and regional fat depots,we analyzed the data from the National Health and Nutrition Examination Survey(NHANES)2011-2018 cycles.Methods Multiple linear regression models were developed to explore the associations between serum PFAS concentrations and six fat compositions along with a fat distribution score created by summing the concentrations of the six fat compositions.The associations between structurally grouped PFASs and fat distribution were assessed,and a prediction model was developed to estimate the ability of PFAS exposure to predict obesity risk.Results Among females aged 39-59 years,trunk fat mass was positively associated with perfluorooctane sulfonate(PFOS).Higher concentrations of PFOS,perfluorohexane sulfonate(PFHxS),perfluorodecanoate(PFDeA),perfluorononanoate(PFNA),and n-perfluorooctanoate(n-PFOA)were linked to greater visceral adipose tissue in this group.In men,exposure to total perfluoroalkane sulfonates(PFSAs)and long-chain PFSAs was associated with reductions in abdominal fat,while higher abdominal fat in women aged 39-59 years was associated with short-chain PFSAs.The prediction model demonstrated high accuracy,with an area under the curve(AUC)of 0.9925 for predicting obesity risk.Conclusion PFAS exposure is associated with regional fat distribution,with varying effects based on age,sex,and PFAS structure.The findings highlight the potential role of PFAS exposure in influencing fat depots and obesity risk,with significant implications for public health.The prediction model provides a highly accurate tool for assessing obesity risk related to PFAS exposure.
基金supported by the Key Research and Development Plan of Zhejiang Province(No.2021C03176)Zhejiang Provincial Natural Science Foundation of China(No.LY23B070001)+2 种基金the Key Laboratory of Pollution Exposure and Health Intervention of Zhejiang Province(No.20230009)the National Natural Science Foundation of China(No.22106032)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0750000).
文摘Per-and polyfluoroalkyl substances(PFASs)can induce a range of adverse health effects,with the precise molecularmechanisms remaining elusive.Extracellular vesicles(EVs)have demonstrated their potential to elucidate unknown molecular mechanisms.Building upon the close alignment of their biological functions with the observed health effects of PFASs,this study innovatively focuses on proteomic insights from EVs into the molecular mechanisms underlying the systemic health effects of PFASs.Through rat exposure experiments and proteomics technology,it not only demonstrated the occurrence of PFASs in EVs but also revealed the alterations in the serum EVs and the expression of their protein cargos following mixed exposure to PFASs,leading to changes in related pathways.These changes encompass various biological processes,including proteasome activity,immune response,cytoskeletal organization,oxidative stress,cell signaling,and nervous system function.Particularly noteworthy is the uncovering of the activation of the proteasome pathway,highlighting significant key contributing proteins.These novel findings provide a new perspective for exploring the molecularmechanism underlying the systemic health effects of PFASs and offer reliable screening for potential biomarkers.Additionally,comparisons with serum confirmed the potential of serum EVs as biological responders and measurable endpoints for evaluating PFASs-induced toxicity.
基金supported by the China Postdoctoral Science Foundation(Nos.2023M730317 and 2023T160066)the Fundamental Research Funds for the Central Universities(No.3332023042)+3 种基金the Open Project of Hebei Key Laboratory of Environment and Human Health(No.202301)the Programs of the National Natural Science Foundation of China(No.21976050)the Science and Technology Program of Hebei Province(No.21377779D)the Natural Science Foundation of Hebei Province,China(No.B2020206008).
文摘Although per-and polyfluoroalkyl substances(PFAS)have been frequently linked to cardiovascular and renal disease separately,evidence remains scarce regarding their systematic effect.Therefore,we recruited 546 newly diagnosed acute coronary syndrome(ACS)patients and detected seven myocardial enzymes and six kidney function biomarkers.Twelve PFASwere also assessedwith ultra-high-performance liquid chromatography-tandem mass spectrometry.Generalized linear model and restricted cubic spline model were applied to single pollutant analysis.Quantile g-computation was used for mixture analysis.Network model was utilized to identify central and bridge nodes of pollutants and phenotypes.In the present study,perfluorohexane sulfonic acid was positively associated with uric acid(UA)(β=0.04,95%confidence interval(CI):0.01,0.07),and perfluorobutanoic acid was negatively associated with estimated glomerular filtration rate(β=-0.04,95%CI:-0.07,-0.01)but positively associated with UA(β=0.03,95%CI:0.01,0.06).In mixture analysis,each quantile increase in the PFAS mixture was significantly associated with UA(β=0.08,95%CI:0.04,0.11).Network analysis revealed that perfluorooctanoate,UA,and myoglobin were denoted as bridge nodes,and the first principal component of lactate dehydrogenase and creatine kinase-myocardial band was identified as the node with the highest strength and expected influence.This study investigates the systematic impact of PFAS exposure through cardiorenal interaction network,which highlights that PFAS may serve as an upstream approach in UA-modulated cardiorenal network to affect cardiorenal system comprehensively.
基金supported by the National Natural Science Foundation of China(No.21976050)the Science and Technology Program of Hebei Province(No.21377779D)+3 种基金the Natural Science Foundation of Hebei Province(No.B2020206008)China Postdoctoral Science Foundation(Nos.2023M730317 and 2023T160066)the Fundamental Research Funds for the Central Universities(No.3332023042)the Open Project of Hebei Key Laboratory of Environment and Human Health(No.202301).
文摘Previous studies have suggested that abnormal hepatobiliary system function may contribute to poor prognosis in patientswith acute coronary syndrome(ACS)and that abnormal hepatobiliary system function may be associated with per-and polyfluoroalkyl substances(PFAS)exposure.However,there is limited evidence for this association in cardiovascular subpopulations,particularly in the ACS patients.Therefore,we performed this study to evaluate the association between plasma PFAS exposure and hepatobiliary system function biomarkers in patients with ACS.This study included 546 newly diagnosed ACS patients at the Second Hospital of Hebei Medical University,and data on 15 hepatobiliary system function biomarkers were obtained from medical records.Associations between single PFAS and hepatobiliary system function biomarkers were assessed using multiple linear regression models and restricted cubic spline model(RCS),and mixture effects were assessed using the Quantile g-computation model.The results showed that total bile acids(TBA)was negative associated with perfluorohexane sulfonic acid(PFHxS)(-7.69%,95%CI:-12.15%,-3.01%).According to the RCS model,linear associations were found between TBA and PFHxS(P for overall=0.003,P for non-linear=0.234).We also have observed the association between between PFAS congeners and liver enzyme such as aspartate aminotransferase(AST)and α-l-Fucosidase(AFU),but it was not statistically significant after correction.In addition,Our results also revealed an association between prealbumin(PA)and PFAS congeners as well as mixtures.Our findings have provided a piece of epidemiological evidence on associations between PFAS congeners or mixture,and serum hepatobiliary system function biomarkers in ACS patients,which could be a basis for subsequent mechanism studies.
基金supported by the National Natural Science Foundation of China(No.82404365)the Noncommunicable Chronic Diseases-National Science and Technology Major Project(No.2023ZD0513200)+7 种基金China Medical Board(No.15-230)China Postdoctoral Science Foundation(Nos.2023M730317and 2023T160066)the Fundamental Research Funds for the Central Universities(No.3332023042)the Open Project of Hebei Key Laboratory of Environment and Human Health(No.202301)the National Key Research and Development Program of China(No.2022YFC3703000)the Non-profit Central Research Institute Fund of Chinese Academy of Medical Sciences(No.2022-JKCS-11)the CAMS Innovation Fund for Medical Sciences(No.2022-I2M-JB-003)the Programs of the National Natural Science Foundation of China(No.21976050).
文摘Associations of per-and polyfluoroalkyl substances(PFAS)on lipid metabolism have been documented but research remains scarce regarding effect of PFAS on lipid variability.To deeply understand their relationship,a step-forward in causal inference is expected.To address these,we conducted a longitudinal study with three repeated measurements involving 201 participants in Beijing,among which 100 eligible participants were included for the present study.Twenty-three PFAS and four lipid indicators were assessed at each visit.We used linear mixed models and quantile g-computation models to investigate associations between PFAS and blood lipid levels.A latent class growth model described PFAS serum exposure patterns,and a generalized linear model demonstrated associations between these patterns and lipid variability.Our study found that PFDA was associated with increased TC(β=0.083,95%CI:0.011,0.155)and HDL-C(β=0.106,95%CI:0.034,0.178).The PFAS mixture also showed a positive relationship with TC(β=0.06,95%CI:0.02,0.10),with PFDA contributing most positively.Compared to the low trajectory group,the middle trajectory group for PFDA was associated with VIM of TC(β=0.756,95%CI:0.153,1.359).Furthermore,PFDA showed biological gradientswith lipid metabolism.This is the first repeated-measures study to identify the impact of PFAS serum exposure pattern on the lipid metabolism and the first to estimate the association between PFAS and blood lipid levels in middle-aged and elderly Chinese and reinforce the evidence of their causal relationship through epidemiological studies.
文摘[Objectives]To extract and purify perfluoroalkyl and polyfluoroalkyl substances(PFAS)from aquatic products and determine the optimal pretreatment conditions.[Methods]The QuEChERS method was employed for the extraction and purification of PFAS in aquatic products.The detection of PFAS was carried out using liquid chromatography-tandem mass spectrometry(LC-MS/MS)in ESI negative ion mode with multiple reaction monitoring(MRM),and quantification was performed using the external standard method.By optimizing instrument parameters such as ion source temperature,spray voltage,and collision energy,high selectivity and sensitivity of the detection were ensured.[Results]The established calibration curves for 28 PFAS compounds compounds,covering a range of 0.02 to 20 ng/mL,demonstrated excellent linearity.Spike recovery tests yielded limits of detection(LOD)between 0.02 and 0.5μg/kg for the 28 PFAS compounds compounds,with recovery rates ranging from 72.2%to 113.0%.[Conclusions]The method established in this study demonstrates excellent linearity,and is accurate,reliable,efficient,simple,and rapid.It possesses considerable practical applicability and can be used for the quality and risk assessment of 28 PFAS compounds compounds in aquatic products,indicating high practical utility.
基金supported by the Water Pollution Control and Management Program (2014ZX07405001)Drinking Water Source Environmental Monitoring Project (1441100022)
文摘In this work, a method was developed and optimized for the analysis of polyfluoroalkyl and/or perfluoroalkyl substances（PFASs） content in surface water and sediment samples with high instrumental response and good separation. Surface water and sediment samples were collected from the Yangtze River Delta（YRD） to analyze the distribution characteristics of perfluoroalkyl carboxylic acids（PFCAs）, perfluoroalkane sulfonic acids（PFSAs）, perfluoroalkyl phosphonic acids（PFPAs）, perfluoroalkyl phosphinic acids（PFPiAs）, and polyfluoroalkyl phosphoric acid diesters（di PAPs）. The results showed that the total concentrations of PFCAs and PFSAs in YRD varied from 31 to 902 ng/L. PFCAs（≥ 11 carbons） and PFSAs（≥ 10 carbons atoms） were not detected in any surface water samples. The mean concentrations of all PFCAs and PFSAs in surface water from the sampling areas decreased in the following order：Yangtze river（191 ng/L） ≈ Taihu lake（189 ng/L） 〉 Huangpu river（122 ng/L） ≈ Qiantang river（120 ng/L） 〉 Jiaxing urban river（100 ng/L）. Strong significant（p 〈 0.05） correlations between the concentrations of many of the compounds were found in the sampling areas, suggesting a common source for these compounds. Only perfluorooctanoic acid（PFOA） was observed in all sediment samples, at concentrations varying from 0.02 to 1.35 ng/g. Finally, detection rates of two di PAPs were only 8% and 10%, respectively and the concentration of di PAPs was two to three times lower compared to PFCAs and PFSAs.
基金supported by the National Natural Science Foundation of China(No.42177408)Guangdong(China)Innovative and Entrepreneurial Research Team Program(No.2016ZT06N258)。
文摘Studies have shown that per-and polyfluoroalkyl substances(PFASs)may be hepatotoxic in animals or humans.However,data on clinical epidemiology are very limited.In this study,21PFASs were determined in patients with liver diseases,with the highest median concentrations detected in the serum sample(26.7 ng/mL),followed by blood(10.7 ng/mL)and urine(5.02 ng/mL).Higher total PFAS concentrations were found in hepatocellular carcinoma(HCC)patients compared to non-HCC patients,with significant discrepancies in serum and blood samples.Besides,significant correlations were also found among PFAS concentrations and age,gender,body mass index(BMI),and liver function biomarkers levels.For example,PFAS concentrations are significantly higher in males than in females;Several serum PFASs concentrations increase with age and BMI,while the serum perfluorohexane sulfonic acid(PFHxS)concentrations are negatively correlated with age.In addition,multiple regression models adjusted for age,gender and BMI found that increased serum perfluorobutane sulfonic acid(PFBS),perfluoroheptane sulfonic acid(PFHpS)and perfluorohexylphosphonic acid(PFHxPA)conentrations are correlated with elevated alkaline phosphatase(ALP),aspartate aminotransferase(AST),and alpha-fetoprotein(AFP)(p<0.05).Our results provide epidemiological support for the future study on the potential clinical hepatotoxicity of PFAS.
基金supported by the National Natural Science Foundation of China (No.21625702)。
文摘Perfluorooctanoic acid(PFOA), its salts, and related compounds were listed as new persistent organic pollutants by the Stockholm Convention in 2019.In this study, the occurrence of residues of PFOA and other per-and polyfluoroalkyl substances(PFASs) in raw materials and fluoropolymer products from the Chinese fluoropolymer industries are reported for the first time.The PFOA concentrations in raw materials and fluoropolymer products were in the range of 6.7 to 1.1 × 10^(6) ng/g, and <MDL(method detection limit) to 5.3 × 10^(3) ng/g,respectively.Generally, the levels of PFOA in raw materials were higher than in products,implying that PFOA in the emulsion/dispersion resin could be partly removed during the polymerization or post-processing steps.By tracking a company’s polytetrafluoroethylene(PTFE) production line, it was found that over a 5 year period, the residual levels of PFOA in emulsion samples declined from 1.1 × 10^(6) to 28.4 ng/g, indicating that the contamination of PFOA in fluoropolymer products from production source gradually decreased after its use had been discontinued.High concentrations of HFPO-TrA(2.7 × 10^(5) to 8.2 × 10^(5) ng/g) were detected in some emulsion samples indicating this alternative has been widely applied in fluoropolymer manufacturing in China.
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 National Natural Science Foundation of China(Nos.21625702,22021003).
文摘PFAS(per-and polyfluoroalkyl substances)are omnipresent in the environment and their transportation and transformation have attracted increased attention.Microplastics are another potential risk substances that can serve as a carrier for ubiquitous pollutants,thus affecting the presence of PFAS in the environment.In this study,the adsorption of perfluorooctane sulfonamide(FOSA)and perfluorooctanoic acid(PFOA)on four microplastics(PE,PVC,PS,and PTFE)and their effect on the photodegradation of FOSA were studied.The adsorption capacity of FOSA by PS was the highest,in similar,PS displayed the highest adsorption capacity in the presence of PFOA.Different effects of pH and salinity on the adsorption of FOSA and PFOA were observed among different microplastics indicating inconsistent interaction mechanisms.Furthermore,FOSA could be photodegraded,with PFOA as the main product,while the presence of microplastics had a negligible effect on the degradation of this contaminant.The results indicated that microplastics could act as PFAS concentrators.Moreover,their photochemical inertiasmake the pollutants enriched onmicroplastics more resistant to degradation.
基金This research work is supported by the National Natural Science Foundation of China (Grant No. 29902001) and the Department of Education of China.
文摘A novel synthesis of polyfluoroalkyl substituted -butyrolactones from the reaction of polyfluoroalkyl iodides with 4-pentenoic acid initiated with sodium dithionite was realized in good yields.
基金supported by Key Projects of the National Science and Technology Pillar Program of China(No.2011BAE06B01-20)
文摘In order to discover new molecules with good insecticidal activities, a series of anthranilic diamides containing polyfluoroalkyl pyrazole were designed and synthesized, and their structures were characterized by1 H NMR and HRMS. Bioassays demonstrated that some of the title compound exhibited excellent insecticidal activities. The larvicidal activities of compound 8a, 8c, 8g, 8k and 8l against Mythimna separata Walker were 100% at 0.8 mg/L. The insecticidal activities of compound 8a, 8c,8e, 8g, 8k and 8l against Plutella xylostella Linnaeus were 100% at 0.4 mg/L. Surprisingly compounds 8a and 8c still showed 100% larvicidal activities against Plutella xylostella Linnaeus at 0.08 mg/L comparable to the commercialized Chlorantraniliprole. The LC_（50） of compound 8a and 8c against M. separata is 0.048 and 0.043 mg/L respectively.
基金financially supported by the National Natural Science Foundation of China(NSFC)(No.42377217)the Cooperation Fund between Dongying City and Universities(No.SXHZ-2023-02-6).
文摘Per-and polyfluoroalkyl substances(PFASs)are emerging persistent organic pollutants(POPs).In this study,47 surface sediment samples were collected from the Yellow River Delta wetland(YRDW)to investigate the occurrence,spatial distribution,potential sources,and ecological risks of PFASs.Twenty-three out of 26 targeted PFASs were detected in surface sediment samples from the YRDW,with totalΣ23PFASs concentrations ranging from 0.23 to 16.30 ng g^(-1) dw and a median value of 2.27 ng g^(-1) dw.Perfluorooctanoic acid(PFOA),perfluorobutanoic acid(PFBA)and perfluorooctanesulfonic acid(PFOS)were the main contaminants.The detection frequency and concentration of perfluoroalkyl carboxylic acids(PFCAs)were higher than those of perfluoroal-kanesulfonic acids(PFSAs),while those of long-chain PFASs were higher than those of short-chain PFASs.The emerging PFASs substitutes were dominated by 6:2 chlorinated polyfluoroalkyl ether sulfonic acid(6:2 Cl-PFESA).The distribution of PFASs is significantly influenced by the total organic carbon content in the sediments.The concentration of PFASs seems to be related to human activities,with high concentration levels of PFASs near locations such as beaches and villages.By using a positive matrix factorization model,the potential sources of PFASs in the region were identified as metal plating mist inhibitor and fluoropolymer manufacturing sources,metal plating industry and firefighting foam and textile treatment sources,and food packaging material sources.The risk assessment indicated that PFASs in YRDW sediments do not pose a significant ecological risk to benthic organisms in the region overall,but PFOA and PFOS exert a low to moderate risk at individual stations.
基金supported by the Key Deployment Project of Centre for Ocean Mega-Research of Science, Chinese Academy of Sciences (No. COMS2019J08)the Guangzhou Municipal Science and Technology Project (No. 201904010291)+1 种基金National Natural Science Foundation of China (No. 21806042)Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety (No. 2019B030301008)。
文摘The passive sampling technique, diffusive gradients in thin films(DGT) has attracted increasing interests as an in-situ sampler for organic contaminants including per-and polyfluoroalkyl substances(PFAS). However, its effectiveness has been questioned because of the small effective sampling area(3.1 cm^(2)). In this study, we developed a DGT probe for rapid sampling of eight PFAS in waters and applied it to a water-sediment system. It has a much larger sampling area(27 cm^(2)) and as a result lower method quantification limits(0.15 –0.21 ng/L for one-day deployment and 0.02 – 0.03 ng/L for one-week deployment) and much higher(by > 10 factors) sampling rate(100 m L/day) compared to the standard DGT(piston configuration). The sampler could linearly accumulate PFAS from wastewater, was sensitive enough even for a 24 hr deployment with performance comparable to grab sampling(500m L). The DGT probe provided homogeneous sampling performance along the large exposure area. The use of the probe to investigate distributions of dissolved PFAS around the sediment-water interface was demonstrated. This work, for the first time, demonstrated that the DGT probe is a promising monitoring tool for trace levels of PFAS and a research tool for studying their distribution, migration, and fate in aquatic environments including the sediment-water interface.
