Perfluorooctanoic acid(PFOA)is a widespread synthetic persistent organic pollutant that may enrich along the food chain and affect the growth,development,reproduction,and lipid metabolism of aquatic organisms,particul...Perfluorooctanoic acid(PFOA)is a widespread synthetic persistent organic pollutant that may enrich along the food chain and affect the growth,development,reproduction,and lipid metabolism of aquatic organisms,particularly the benthic organisms.How-ever,the toxic effects of PFOA on the half-smooth tongue sole Cynoglossus semilaevis,a commercial benthic fish in China,have rarely been reported.Because juvenile fish are sensitive to environmental pollutants,in the present study,histological assessment and tran-scriptome sequencing were performed to determine the short-term impact of PFOA on juvenile half-smooth tongue soles.Histologi-cal analysis showed that PFOA exposure caused hepatocyte rupture,intestinal villi breakage,increased goblet cell count,and brain ab-normal.Transcriptome results showed that some interesting signaling pathways,such as glycolysis/gluconeogenesis,PPAR signaling pathway and GABAergic synapse signaling pathway,were enriched after PFOA exposure.In addition,some metabolic,immune and neural genes were differentially expressed,which including ependymin,hbb1-like and gad 1,and they were up-regulated after 14 days of exposure.Transcriptome results also indicated that half-smooth tongue sole might improve energy metabolism in response to PFOA toxicity after 7 days of exposure.These findings provide a basis for studying the ecological effects of PFOA on marine benthic fishes.展开更多
The photodegradation of persistent and bioaccumulative perftuorooctanoic acid (PFOA) in water by 185 nm vacuum ultraviolet (VUV) light was examined to develop an effective technology to deal with PFOA pollution. P...The photodegradation of persistent and bioaccumulative perftuorooctanoic acid (PFOA) in water by 185 nm vacuum ultraviolet (VUV) light was examined to develop an effective technology to deal with PFOA pollution. PFOA degraded very slowly under irradiation of 254 nm UV light. However, 61.7% of initial PFOA was degraded by 185 nm VUV light within 2 h, and defluorination ratio reached 17.1%. Pseudo first-order-kinetics well simulated its degradation and defluorination. Besides, fluoride ion formed in water, 4 shorter-chain perfluorinated carboxylic acids (PFCAs), that is, perfluoroheptanoic acid, perfluorohexanoic acid, perfluoropentanoic acid, and perfluorobutanoic acid. These were identified as intermediates by LC-MS measurement. These PFCAs consecutively formed and further degraded with irradiation time. According to the mass balance calculation, no other byproducts were formed. It was proposed that PFCAs initially are decarboxylated by 185 nm light, and the radical thus formed reacts with water to form shorter-chain PFCA with one less CF2 unit.展开更多
Environmentally persistent and bioaccumulative perfluorooctanic acid (PFOA) was difficult to be decomposed under the irradiation of 254 nm UV light. However, in the presence of 80μmol/L Fe(Ⅲ), 80% of PFOA with i...Environmentally persistent and bioaccumulative perfluorooctanic acid (PFOA) was difficult to be decomposed under the irradiation of 254 nm UV light. However, in the presence of 80μmol/L Fe(Ⅲ), 80% of PFOA with initial concentration of 48μmol/L (20 mg/L) was effectively degraded and 47.8% of fluorine atoms in PFOA molecule were transformed into inorganic fluoride ion after 4 h reaction. Shorter chain perfluorocarboxylic acids bearing C3-C7 and fluoride ion were detected and identified by LC/MS and IC as the degradation products in the aqueous solution. It was proposed that complexes of PFOA with Fe(Ⅲ) initiated degradation of PFOA irradiated with 254 nm UV light.展开更多
Aqueous perfluorooctanoic acid(PFOA)elimination has raised significant concerns due to its persistence and bioaccumulation.Althoughβ-PbO_(2)plate anodes have shown efficient mineralization of PFOA,it remains unclear ...Aqueous perfluorooctanoic acid(PFOA)elimination has raised significant concerns due to its persistence and bioaccumulation.Althoughβ-PbO_(2)plate anodes have shown efficient mineralization of PFOA,it remains unclear whether PFOA can be effectively degraded usingβ-PbO_(2)reactive electrochemical membrane(REM).Herein,we assessed the performance of Ti/SnO_(2)-Sb/La-PbO_(2)REM for PFOA removal and proposed a possible degradation mechanism.At a current density of 10 mA/cm2and a membrane flux of 8500(liters per square meter per hour,LMH),the degradation efficiency of 10 mg/L PFOA was merely8.8%,whereas the degradation efficiency of 0.1 mg/L PFOA increased to 96.6%.Although the porous structure of theβ-PbO_(2)REM provided numerous electroactive sites for PFOA,the generated oxygen bubbles in the pores could block the pore channels and adsorb PFOA molecules.These hindered the protonation process and significantly impeded the degradation of high-concentration PFOA.Quenching experiments indicated that·OH played dominant role in PFOA degradation.The electrical energy per order to remove 0.1 mg/L PFOA was merely 0.74 Wh/L,which was almost an order of magnitude lower than that of other anode materials.This study presents fresh opportunities for the electrochemical degradation of low-concentration PFOA usingβ-PbO_(2)REM.展开更多
Perfluorooctanoyl modified poly(vinyl alcohol)s (FPVA) were prepared by means of substituting a small amount of hydroxyl groups on the backbone of poly(vinyl alcohol), for which the initial degree of polymerization is...Perfluorooctanoyl modified poly(vinyl alcohol)s (FPVA) were prepared by means of substituting a small amount of hydroxyl groups on the backbone of poly(vinyl alcohol), for which the initial degree of polymerization is equal to 1750. The substitution extent, defined by the number of substituting units in a chain, for the four FPVA samples was in the range of 0.5-5 perfluorooctanoyl groups per chain. The FPVA samples with the highest substitution extent still had good solubility in water. It was shown by experimental measurement at 30.0 +/- 0.1 degreesC that the surface tension of the aqueous solution of the highest substituted FPVA decreased to 16.6 mN/m at a higher concentration, e.g. about 0.1 g/mL. Obviously, macromolecules of FPVA exhibit a very strong tendency to adsorb at the air-water interface, because the hydrophobic perfluorooctanoyl groups in FPVA have a very high surface activity as they are in small molecular fluorinated surfactants. The chain conformation of such a model polymer adsorbed on the air-water interface was also discussed.展开更多
Perfluorooctanoic acid(PFOA)is a novel type of persistent synthetic organic pollutant,and its exposure on pregnant women can cause some adverse effects,such as pregnancy-induced hypertension,gestational diabetes melli...Perfluorooctanoic acid(PFOA)is a novel type of persistent synthetic organic pollutant,and its exposure on pregnant women can cause some adverse effects,such as pregnancy-induced hypertension,gestational diabetes mellitus,and preeclampsia.Therefore,understanding the metabolic changes caused by PFOA exposure is of great significance to protect pregnant women from its adverse effects.In this study,the metabolomes from the urine samples of pregnant women exposure to PFOA at different degrees were analyzed by GC-MS and LC-MS.The samples in different groups were distinguished and the differential metabolites were screened based on the VIP value,FC,and P-value of each comparison group through multivariate statistical analysis.The pathways related to differential metabolites were searched to reveal the effects of PFOA exposure on metabolic changes in pregnant women at different degrees.Finally,the ROC of differential metabolites was performed,and the differential metabolites with large area under the curve(AUC)values were selected and compared to identify the mutually differential metabolites.Meanwhile,these metabolites were fitted with a multivariable to explore if they could be used to distinguish different groups.The quantitative comparison of mutually differential metabolites revealed that the levels of L-cysteine,glycine,and 5-aminovaleric acid were positively correlated with the degree of PFOA exposure,indicating that different degrees of PFOA exposure could affect the synthesis or degradation of GSH and change the metabolism of oral or intestinal microbiota.Additionally,they may cause oxidative stress and abnormal fat metabolism in pregnant women.展开更多
Heterogeneous photocatalysis has gained substantial research interest in treating per-and polyfluoroalkyl substances(PFAS)-contaminated water.However,sluggish degradation kinetics and low defluorination efficiency com...Heterogeneous photocatalysis has gained substantial research interest in treating per-and polyfluoroalkyl substances(PFAS)-contaminated water.However,sluggish degradation kinetics and low defluorination efficiency compromise their practical applications.Here,we report a superior photocatalyst,defected Bi_(3)O(OH)(PO_(4))_(2),which could effectively degrade typical PFAS,perfluorooctanoic acid(PFOA),with high defluorination efficiency.The UV light irradiation could in situ generate oxygen vacancies on Bi_(3)O(OH)(PO_(4))_(2) through oxidation of the lattice hydroxyls,which further promotes the formation of Lewis acidic coordinately unsaturated bismuth sites.Then,the Lewis acidic sites couple with the proximal surface hydroxyls to constitute the surface frustrated Lewis pairs(SFLPs).With the in-depth spectroscopic analysis,we revealed that the photo-induced SFLPs act as collection centers to effectively adsorb PFOA and endow accessible pathways to transfer photogenerated holes to PFOA rapidly.Consequently,activation of the terminal carboxyl,a ratelimiting step for PFOA decomposition,could be easily achieved over the defected Bi_(3)O(OH)(PO_(4))_(2) photocatalyst.These results suggest that SFLPs exhibit great potential in developing highly efficient photocatalysts to degrade persistent organic pollutants.展开更多
Microwave-hydrothermal treatment of persis- tent and bioaccumulative perfluorooctanoic acid (PFOA) in water with persulfate (S2O2-) has been found effective. However, applications of this process to effectively re...Microwave-hydrothermal treatment of persis- tent and bioaccumulative perfluorooctanoic acid (PFOA) in water with persulfate (S2O2-) has been found effective. However, applications of this process to effectively remediate PFOA pollution require a better understanding on free-radical scavenging reactions that also take place. The objectives of this study were to investigate the effects ofpH (pH= 2.5, 6.6, 8.8, and 10.5), chloride concentra- tions (0.01-0.15 mol.L-1), and temperature (60℃, 90℃, and 130℃) on persulfate oxidation of PFOA under microwave irradiation. Maximum PFOA degradation occurred at pH 2.5, while little or no degradation at pH 10.5. Lowering system pH resulted in an increase in PFOA degradation rate. Both high pH and chloride concentrations would result in more scavenging of sulfate free radicals and slow down PFOA degradation. When chloride concentrations were less than 0.04 mol.L^-1 at 90℃ and 0.06mol.L^-1 at 60℃, presence of chloride ions had insignificant impacts on PFOA degradation. However, beyond these concentration levels, PFOA degradation rates reduced significantly with an increase in chloride concentrations, especially under the higher temperature.展开更多
Perfluorooctanoic acid (PFOA) is a new-found hazardous persistent organic pollutant, and it is resistant to decomposition by hydroxyl radical (HO.) due to its stable chemical structure and the high electronegativi...Perfluorooctanoic acid (PFOA) is a new-found hazardous persistent organic pollutant, and it is resistant to decomposition by hydroxyl radical (HO.) due to its stable chemical structure and the high electronegativity of fluorine. Photocatalytic reduction of PFOA with β-Ga2O3 in anoxic aqueous solution was investigated for the first time, and the results showed that the photoinduced electron (ecb) coming from the β-Ga2O3 conduction band was the major degradation substance for PFOA, and shorter-chain perfluorinated carboxylic acids (PFCAs, CnF2n+1COOH, 1 ≤ n ≤ 6) were the dominant products. Furthermore, the concentration of F- was measured by the IC technique and defluorination efficiency was calculated. After 3 hr, the photocatalytic degradation efficiency was 98.8% and defluorination efficiency was 31.6% in the presence of thiosulfate and bubbling N2. The degradation reaction followed first-order kinetics (k = 0.0239 min-1, t1/2 = 0.48 hr). PFCAs (CnF2n+xCOOH, 1 ≤ n≤ 7) were detected and measured by LC-MS and LC-MS/MS methods. It was deduced that the probable photocatalytic degradation mechanism involves ec-b attacking the carboxyl of CnF2n+1COOH, resulting in decarboxylation and the generation of CnFzn+1. The produced CnF2n+1 reacted with H2O, forming CnF2n+1OH, then CnF2n+1OH underwent HF loss and hydrolysis to form CnF2,+1COOH.展开更多
Bismuth-based material has been broadly studied due to their potential applications in various areas,especially used as promising photocatalysts for the removal of persistent organic pollutants(POPs) and several appro...Bismuth-based material has been broadly studied due to their potential applications in various areas,especially used as promising photocatalysts for the removal of persistent organic pollutants(POPs) and several approaches have been adopted to tailor their features.Herein,the bismuth-based photocatalysts(BiOCl,BiPO4,BiOPO4/BiOCl) were synthesized by hydrothermal method and advanced characterization techniques(XRD,SEM,EDS elemental mapping,Raman and UV-vis DRS) were employed to analyze their morphology,crystal structure,and purity of the prepared photocatalysts.These synthesized photocatalysts offered a praiseworthy activity as compared to commercial TiO2(P25) for the degradation of model pollutant perfluorooctanoic acid(PFOA) under 254 nm UV light.It was interesting to observe that all synthesized photocatalysts show significant degradation of PFOA and their photocatalytic activity follows the order:bismuth-based catalysts> TiO2(P25)> without catalyst.Bismuth-based catalysts degraded the PFOA by almost 99.99% within 45 min while this degradation efficiency was 66.05% with TiO2 under the same reaction condition.Our work shows that the bismuth-based photocatalysts are promising in PFOA treatment.展开更多
Nanophotocatalysts have shown great potential for degrading poly-and perfluorinated substances(PFAS).In light of the fact that most of these catalysts were studied in pure water,this study was designed to elucidate ef...Nanophotocatalysts have shown great potential for degrading poly-and perfluorinated substances(PFAS).In light of the fact that most of these catalysts were studied in pure water,this study was designed to elucidate effects from common environmental factors on decomposing and defluorinating perfluorooctanoic acid(PFOA)by In2O3 nanoparticles.Results from this work demonstrated that among the seven parameters,pH,sulfate,chloride,H2O2,In2O3 dose,NOM and O2,the first four had statistically significant negative effects on PFOA degradation.Since PFOA is a strong acid,the best condition leading to the highest PFOA removal was identified for two pH ranges.When pH was between 4 and 8,the optimal condition was:pH=4.2;sulfate=5.00 mg/L;chloride=20.43 mg/L;H2O2=0 mmol/L.Under this condition,PFOA decomposition and defluorination were 55.22 and 23.56%,respectively.When pH was between 2 and 6,the optimal condition was:pH=2;sulfate=5.00 mg/L;chloride=27.31 mg/L;H2O2=0 mmol/L.With this condition,the modeled PFOA decomposition was 97.59%with a defluorination of approximately 100%.These predicted results were all confirmed by experimental data.Thus,In2O3 nanoparticles can be used for degrading PFOA in aqueous solutions.This approach works best when the target contaminated water contains low concentrations of NOM,sulfate and chloride and at a low pH.展开更多
Perfluorooctanoic acid(PFOA)is recalcitrant to degrade and mineralize.Here,the effect of temperature on the photolytic decomposition of PFOA was investigated.The decomposition of PFOA was enhanced from 34% to 99% in...Perfluorooctanoic acid(PFOA)is recalcitrant to degrade and mineralize.Here,the effect of temperature on the photolytic decomposition of PFOA was investigated.The decomposition of PFOA was enhanced from 34% to 99% in 60 min of exposure when the temperature was increased from 25 to 85℃ under UV light(201–600 nm).The limited degree of decomposition at 25℃ was due to low quantum yield,which was increased by a factor of 12 at 85℃.Under the imposed conditions,the defluorination ratio increased from 8% at 25℃ to 50% at85℃ in 60 min.Production of perfluorinated carboxylic acids(PFCAs,C7–C5),PFCAs(C4–C3)and TFA(trifluoroacetic acid,C2)accelerated and attained a maximum within 30 to 90 min at 85℃.However,these reactions did not occur at 25℃ despite extended irradiation to180 min.PFOA was decomposed in a step-wise process by surrendering one CF2unit.In each cyclical process,increased temperature enhanced the quantum yields of irradiation and reactions between water molecules and intermediates radicals.The energy consumption for removing eachμmol of PFOA was reduced from 82.5 k J at 25℃ to 10.9 k J at 85℃ using photolysis.Photolysis coupled with heat achieved high rates of PFOA degradation and defluorination.展开更多
In order to optimize the solid phase extraction(SPE)conditions of perfluorooctanoic acid(PFOA)in the raw leachate and treated leachate,the effects of activator properties,SPE cartridge,p H value,ionic strength,and elu...In order to optimize the solid phase extraction(SPE)conditions of perfluorooctanoic acid(PFOA)in the raw leachate and treated leachate,the effects of activator properties,SPE cartridge,p H value,ionic strength,and eluent properties were studied through single factor experiments.The optimal results of each single factor were obtained.Considering that the concentration of PFOA in the treated leachate is lower than that of the raw leachate,the SPE conditions of the treated leachate have been further optimized.Based on the above single-factor experiment,the main influencing factors were screened out as the volume of activator,ionic strength,and volume of eluent,and the three-factor threelevel response surface methodology(RSM)was optimized.The optimum SPE conditions of PFOA from treated landfill leachate were as follows:Activation of weak anion exchange(WAX)cartridge with 10 mL methanol,dosage of 600 mg KCl,6 m L 1%ammonia methanol eluted PFOA,the theory recovery rate is over95.67%.It has been verified that the error between the predicted value and the actual extraction recovery is small and has good repeatability.展开更多
The aggregation of multi-walled carbon nanotubes (MWCNTs) in the aqueous phase not only inhibits their extensive utilization in various aspects but also dominates their environmental fate and transport.The role of s...The aggregation of multi-walled carbon nanotubes (MWCNTs) in the aqueous phase not only inhibits their extensive utilization in various aspects but also dominates their environmental fate and transport.The role of surfactants at low concentration in the aggregation of MWCNTs has been studied,however the effect of perfluorinated surfactants at low concentration is uncertain.To understand this interfacial phenomenon,the influences of perfluorooctanoic acid (PFOA),and sodium dodecyl sulfate (SDS) as a control,on MWCNT aggregation in the aqueous phase were examined by the UV absorbency method.Influences of pH and cationic species on the critical coagulation concentration (CCC) value were evaluated.The CCC values were dependent on the concentration of PFOA,however a pronounced effect of SDS concentration on the CCC values was not observed.The CCC values of the MWCNTs were 51.6 mmol/L in NaCl and 0.28 mmol/L in CaCl 2 solutions,which suggested pronounced differences in the effects of Na+ and Ca2+ ions on the aggregation of the MWCNTs.The presence of both PFOA and SDS significantly decreased the CCC values of the MWCNTs in NaCl solution.The aggregation of the MWCNTs took place under acidic conditions and was not notably altered under neutral and alkaline conditions due to the electrostatic repulsion of deprotonated functional groups on the surface of the MWCNTs.展开更多
Liquid-liquid extraction(LLE)using ionic liquids(ILs)-based methods to remove perfluoroalkyl chemicals(PFACs),such as perfluorooctanoic acid(PFOA)and perfluorooctane sulfonic acid(PFOS),from wastewater,is an important...Liquid-liquid extraction(LLE)using ionic liquids(ILs)-based methods to remove perfluoroalkyl chemicals(PFACs),such as perfluorooctanoic acid(PFOA)and perfluorooctane sulfonic acid(PFOS),from wastewater,is an important strategy.However,the lack of physicochemical and LLE data limits the selection of the most suitable ILs for the extraction of PFACs.In this work,1763 ILs for PFACs extraction from water were systematically screened using COSMOtherm to estimate the infinite dilution activity coefficient(lnγ^(∞))of PFOA and PFOS in water and ILs.To evaluate the accuracy of COSMOtherm,8 ILs with various lnγ^(∞)values were selected,and their extraction efficiency(E)and distribution coefficient(D_(exp))were measured experimentally.The results showed that the predicted lnγ^(∞)decreased as the increase of experimental extraction efficiency of PFOA or PFOS,while the tendency of predicted distribution coefficient(D_(pre))was consistent with the experimental(D_(exp))results.This work provides an efficient basis for selecting ILs for the extraction of PFACs from wastewater.展开更多
When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PF...When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PFOA) from groundwater. With favorable tailoring, QAE-AC removed PFOA from groundwater for 118,000 bed volumes before halfbreakthrough in rapid small scale column tests, while the influent PFOA concentration was 200 ng/L. The tailoring involved pre-dosing QAE at an array of proportions onto this carbon, and then monitoring bed life for PFOA removal. When pre-dosing with 1 mL QAE, this PFOA bed life reached an interim peak, whereas bed life was less following 3 mL QAE pre-dosing, then PFOA bed life exhibited a steady rise for yet subsequently higher QAE pre-dosing levels. Large-scale atomistic modelling was used herein to provide new insight into the mechanism of PFOA removal by QAE-AC. Based on experimental results and modelling, the authors perceived that the QAE's epoxide functionalities cross-linked with phenolics that were present along the activated carbon's graphene edge sites, in a manner that created mesopores within macroporous regions or created micropores within mesopores regions. Also, the QAE could react with hydroxyls outside of these pore, including the hydroxyls of both graphene edge sites and other QAE molecules. This latter reaction formed new pore-like structures that were external to the activated carbon grains. Adsorption of PFOA could occur via either charge balance between negatively charged PFOA with positively charged QAE, or by van der Waals forces between PFOA's fluoro-carbon tail and the graphene or QAE carbon surfaces.展开更多
The distribution of polyfluoroalkyl compounds(PFCs)in the dissolved and particulate phase and their discharge from the river Elbe into the North Sea were studied.The PFCs quantified included C_(4)-C_(8) perfluorinated...The distribution of polyfluoroalkyl compounds(PFCs)in the dissolved and particulate phase and their discharge from the river Elbe into the North Sea were studied.The PFCs quantified included C_(4)-C_(8) perfluorinated sulfonates(PFSAs),6∶2 fluorotelomer sulfonate(6∶2 FTS),C_(6) and C_(8) perfluorinated sulfinates(PFSiAs),C_(4)-C_(12) perfluorinated carboxylic acids(PFCAs),perfluoro-3,7-dimethyl-octanoic acid(3,7m_(2)-PFOA),perfluorooctane sulfonamide(FOSA),and n-ethyl perfluroctane sulfonamidoethanol(EtFOSE).PFCs were mostly distributed in the dissolved phase,where perfluorooctanoic acid(PFOA)dominated with 2.9–12.5 ng/L.In the suspended particulate matter FOSA and perfluorooctane sulfonate(PFOS)showed the highest concentrations(4.0 ng/L and 2.3 ng/L,respectively).The total flux ofΣPFCs from the river Elbe was estimated to be 802 kg/year for the dissolved phase and 152 kg/year for the particulate phase.This indicates that the river Elbe acts as a source of PFCs into the North Sea.However,the concentrations of perfluorobutane sulfonate(PFBS)and perfluorobutanoic acid(PFBA)in the North Sea were higher than that in the river Elbe,thus an alternative source must exist for these compounds.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
Poly-and perfluoroalkyl substances(PFASs)are important environmental contaminants globally and in the early 2000s they were shown to be ubiquitous contaminants in Arctic wildlife.Previous reviews by Butt et al.and Let...Poly-and perfluoroalkyl substances(PFASs)are important environmental contaminants globally and in the early 2000s they were shown to be ubiquitous contaminants in Arctic wildlife.Previous reviews by Butt et al.and Letcher et al.have covered studies on levels and trends of PFASs in the Arctic that were available to 2009.The purpose of this review is to focus on more recent work,generally published between 2009 and 2018,with emphasis on PFASs of emerging concern such as perfluoroalkyl carboxylates(PFCAs)and short-chain perfluoroalkyl sulfonates(PFSAs)and their precursors.Atmospheric measurements over the period 2006e2014 have shown that fluorotelomer alcohols(FTOHs)as well as perfluorobutanoic acid(PFBA)and perfluoroctanoic acid(PFOA)are the most prominent PFASs in the arctic atmosphere,all with increasing concentrations at Alert although PFOA concentrations declined at the Zeppelin Station(Svalbard).Results from ice cores show generally increasing deposition of PFCAs on the Devon Ice cap in the Canadian arctic while declining fluxes were found in a glacier on Svalbard.An extensive dataset exists for long-term trends of long-chain PFCAs that have been reported in Arctic biota with some datasets including archived samples from the 1970s and 1980s.Trends in PFCAs over time vary among the same species across the North American Arctic,East and West Greenland,and Svalbard.Most long term time series show a decline from higher concentrations in the early 2000s.However there have been recent(post 2010)increasing trends of PFCAs in ringed seals in the Canadian Arctic,East Greenland polar bears and in arctic foxes in Svalbard.Annual biological sampling is helping to determine these relatively short term changes.Rising levels of some PFCAs have been explained by continued emissions of long-chain PFCAs and/or their precursors and inflows to the Arctic Ocean,especially from the North Atlantic.While the effectiveness of biological sampling for temporal trends in long-chain PFCAs and PFSAs has been demonstrated,this does not apply to the C4eC8ePFCAs,perfluorobutane sulfonamide(FBSA),or perfluorobutane sulfonate(PFBS)which are generally present at low concentrations in biota.In addition to air sampling,sampling abiotic media such as glacial cores,and annual sampling of lake waters and seawater would appear to be the best approaches for investigating trends in the less bioaccumulative PFASs.展开更多
Nanofiltration(NF)process has become one of the most promising technologies to remove micro-organic combined water pollution.Developing a NF membrane material with efficient separation for perfluorooctanoic acid(PFOA)...Nanofiltration(NF)process has become one of the most promising technologies to remove micro-organic combined water pollution.Developing a NF membrane material with efficient separation for perfluorooctanoic acid(PFOA)combined pollution is highly desired,this manuscript targets this unmet need specifically.In this work,hydrophilic SiO_(2)nanoparticles with various contents blended with carboxylic multiwalled carbon nanotube were used to modify poly(m-phenylene isophthal amide)(SiO_(2)/CMWCNT/PMIA)hollow fiber NF membrane.The modified membrane with 0.1 wt%SiO_(2)doping exhibits way better fouling resistance with irreversible fouling ratio decreased dramatically from 18.7%to 2.3%,and the recovery rate of water flux increases significantly from 81.2%to 97.7%.The separation experiment results had confirmed that the modified membrane could improve the rejection from 97.2%to 98.6%for perfluorooctanoic acid(PFOA)and its combined pollution with bovine serum albumin(BSA).It is clear that this reported SiO_(2)/CMWCNT/PMIA hollow fiber NF membrane potentially could be applied in water treatment.This research also provides a theoretical basis for efficiently removal of PFOA and its combined pollution by NF membrane.展开更多
基金supported by the National Key R&D Program(No.2018YFD0900301-03)the MNR Key Laboratory of Marine Eco-Environmental Science and Technology,China(No.MEEST-2021-04).
文摘Perfluorooctanoic acid(PFOA)is a widespread synthetic persistent organic pollutant that may enrich along the food chain and affect the growth,development,reproduction,and lipid metabolism of aquatic organisms,particularly the benthic organisms.How-ever,the toxic effects of PFOA on the half-smooth tongue sole Cynoglossus semilaevis,a commercial benthic fish in China,have rarely been reported.Because juvenile fish are sensitive to environmental pollutants,in the present study,histological assessment and tran-scriptome sequencing were performed to determine the short-term impact of PFOA on juvenile half-smooth tongue soles.Histologi-cal analysis showed that PFOA exposure caused hepatocyte rupture,intestinal villi breakage,increased goblet cell count,and brain ab-normal.Transcriptome results showed that some interesting signaling pathways,such as glycolysis/gluconeogenesis,PPAR signaling pathway and GABAergic synapse signaling pathway,were enriched after PFOA exposure.In addition,some metabolic,immune and neural genes were differentially expressed,which including ependymin,hbb1-like and gad 1,and they were up-regulated after 14 days of exposure.Transcriptome results also indicated that half-smooth tongue sole might improve energy metabolism in response to PFOA toxicity after 7 days of exposure.These findings provide a basis for studying the ecological effects of PFOA on marine benthic fishes.
基金Project supported by the National Natural Science Foundation of China (No. 20577026) the New Century Excellent Talents in University (No. NCET-04-0090).
文摘The photodegradation of persistent and bioaccumulative perftuorooctanoic acid (PFOA) in water by 185 nm vacuum ultraviolet (VUV) light was examined to develop an effective technology to deal with PFOA pollution. PFOA degraded very slowly under irradiation of 254 nm UV light. However, 61.7% of initial PFOA was degraded by 185 nm VUV light within 2 h, and defluorination ratio reached 17.1%. Pseudo first-order-kinetics well simulated its degradation and defluorination. Besides, fluoride ion formed in water, 4 shorter-chain perfluorinated carboxylic acids (PFCAs), that is, perfluoroheptanoic acid, perfluorohexanoic acid, perfluoropentanoic acid, and perfluorobutanoic acid. These were identified as intermediates by LC-MS measurement. These PFCAs consecutively formed and further degraded with irradiation time. According to the mass balance calculation, no other byproducts were formed. It was proposed that PFCAs initially are decarboxylated by 185 nm light, and the radical thus formed reacts with water to form shorter-chain PFCA with one less CF2 unit.
文摘Environmentally persistent and bioaccumulative perfluorooctanic acid (PFOA) was difficult to be decomposed under the irradiation of 254 nm UV light. However, in the presence of 80μmol/L Fe(Ⅲ), 80% of PFOA with initial concentration of 48μmol/L (20 mg/L) was effectively degraded and 47.8% of fluorine atoms in PFOA molecule were transformed into inorganic fluoride ion after 4 h reaction. Shorter chain perfluorocarboxylic acids bearing C3-C7 and fluoride ion were detected and identified by LC/MS and IC as the degradation products in the aqueous solution. It was proposed that complexes of PFOA with Fe(Ⅲ) initiated degradation of PFOA irradiated with 254 nm UV light.
基金financially supported by the National Key Research and Development Program(No.2022YFE0135700)the National Natural Science Foundation of China(Nos.52000028,52370076 and 51978658)+1 种基金the Fundamental Research Funds for the Central Universities(No.2023MS063)Australian Research Council(No.G180200015)。
文摘Aqueous perfluorooctanoic acid(PFOA)elimination has raised significant concerns due to its persistence and bioaccumulation.Althoughβ-PbO_(2)plate anodes have shown efficient mineralization of PFOA,it remains unclear whether PFOA can be effectively degraded usingβ-PbO_(2)reactive electrochemical membrane(REM).Herein,we assessed the performance of Ti/SnO_(2)-Sb/La-PbO_(2)REM for PFOA removal and proposed a possible degradation mechanism.At a current density of 10 mA/cm2and a membrane flux of 8500(liters per square meter per hour,LMH),the degradation efficiency of 10 mg/L PFOA was merely8.8%,whereas the degradation efficiency of 0.1 mg/L PFOA increased to 96.6%.Although the porous structure of theβ-PbO_(2)REM provided numerous electroactive sites for PFOA,the generated oxygen bubbles in the pores could block the pore channels and adsorb PFOA molecules.These hindered the protonation process and significantly impeded the degradation of high-concentration PFOA.Quenching experiments indicated that·OH played dominant role in PFOA degradation.The electrical energy per order to remove 0.1 mg/L PFOA was merely 0.74 Wh/L,which was almost an order of magnitude lower than that of other anode materials.This study presents fresh opportunities for the electrochemical degradation of low-concentration PFOA usingβ-PbO_(2)REM.
基金The project was supported by the National Natural Science Foundation of China (No.29774016).
文摘Perfluorooctanoyl modified poly(vinyl alcohol)s (FPVA) were prepared by means of substituting a small amount of hydroxyl groups on the backbone of poly(vinyl alcohol), for which the initial degree of polymerization is equal to 1750. The substitution extent, defined by the number of substituting units in a chain, for the four FPVA samples was in the range of 0.5-5 perfluorooctanoyl groups per chain. The FPVA samples with the highest substitution extent still had good solubility in water. It was shown by experimental measurement at 30.0 +/- 0.1 degreesC that the surface tension of the aqueous solution of the highest substituted FPVA decreased to 16.6 mN/m at a higher concentration, e.g. about 0.1 g/mL. Obviously, macromolecules of FPVA exhibit a very strong tendency to adsorb at the air-water interface, because the hydrophobic perfluorooctanoyl groups in FPVA have a very high surface activity as they are in small molecular fluorinated surfactants. The chain conformation of such a model polymer adsorbed on the air-water interface was also discussed.
基金the National Natural Science Foundation of China(Nos.81874307 and 21874088)the Shanghai Science and Technology Commission Scientific Research Project(Nos.19142203100,20142200400,18490731500,and 19DZ2202200)the National Facility for Translational Medicine,Shanghai(No.TMSK-2020-131).
文摘Perfluorooctanoic acid(PFOA)is a novel type of persistent synthetic organic pollutant,and its exposure on pregnant women can cause some adverse effects,such as pregnancy-induced hypertension,gestational diabetes mellitus,and preeclampsia.Therefore,understanding the metabolic changes caused by PFOA exposure is of great significance to protect pregnant women from its adverse effects.In this study,the metabolomes from the urine samples of pregnant women exposure to PFOA at different degrees were analyzed by GC-MS and LC-MS.The samples in different groups were distinguished and the differential metabolites were screened based on the VIP value,FC,and P-value of each comparison group through multivariate statistical analysis.The pathways related to differential metabolites were searched to reveal the effects of PFOA exposure on metabolic changes in pregnant women at different degrees.Finally,the ROC of differential metabolites was performed,and the differential metabolites with large area under the curve(AUC)values were selected and compared to identify the mutually differential metabolites.Meanwhile,these metabolites were fitted with a multivariable to explore if they could be used to distinguish different groups.The quantitative comparison of mutually differential metabolites revealed that the levels of L-cysteine,glycine,and 5-aminovaleric acid were positively correlated with the degree of PFOA exposure,indicating that different degrees of PFOA exposure could affect the synthesis or degradation of GSH and change the metabolism of oral or intestinal microbiota.Additionally,they may cause oxidative stress and abnormal fat metabolism in pregnant women.
基金financially supported by the National Natural Science Foundation of China(Nos.22006088 and 42077293)the Natural Science Foundation of Guangdong Province(China)(No.2019QN01L797)+1 种基金the Shenzhen Municipal Science and Technology Innovation Committee(China)(Nos.WDZC20200817103015002 and RCYX20210609104448111)the Tsinghua Shenzhen International Graduate School(China)(Nos.HW2020002 and QD2021010N).
文摘Heterogeneous photocatalysis has gained substantial research interest in treating per-and polyfluoroalkyl substances(PFAS)-contaminated water.However,sluggish degradation kinetics and low defluorination efficiency compromise their practical applications.Here,we report a superior photocatalyst,defected Bi_(3)O(OH)(PO_(4))_(2),which could effectively degrade typical PFAS,perfluorooctanoic acid(PFOA),with high defluorination efficiency.The UV light irradiation could in situ generate oxygen vacancies on Bi_(3)O(OH)(PO_(4))_(2) through oxidation of the lattice hydroxyls,which further promotes the formation of Lewis acidic coordinately unsaturated bismuth sites.Then,the Lewis acidic sites couple with the proximal surface hydroxyls to constitute the surface frustrated Lewis pairs(SFLPs).With the in-depth spectroscopic analysis,we revealed that the photo-induced SFLPs act as collection centers to effectively adsorb PFOA and endow accessible pathways to transfer photogenerated holes to PFOA rapidly.Consequently,activation of the terminal carboxyl,a ratelimiting step for PFOA decomposition,could be easily achieved over the defected Bi_(3)O(OH)(PO_(4))_(2) photocatalyst.These results suggest that SFLPs exhibit great potential in developing highly efficient photocatalysts to degrade persistent organic pollutants.
文摘Microwave-hydrothermal treatment of persis- tent and bioaccumulative perfluorooctanoic acid (PFOA) in water with persulfate (S2O2-) has been found effective. However, applications of this process to effectively remediate PFOA pollution require a better understanding on free-radical scavenging reactions that also take place. The objectives of this study were to investigate the effects ofpH (pH= 2.5, 6.6, 8.8, and 10.5), chloride concentra- tions (0.01-0.15 mol.L-1), and temperature (60℃, 90℃, and 130℃) on persulfate oxidation of PFOA under microwave irradiation. Maximum PFOA degradation occurred at pH 2.5, while little or no degradation at pH 10.5. Lowering system pH resulted in an increase in PFOA degradation rate. Both high pH and chloride concentrations would result in more scavenging of sulfate free radicals and slow down PFOA degradation. When chloride concentrations were less than 0.04 mol.L^-1 at 90℃ and 0.06mol.L^-1 at 60℃, presence of chloride ions had insignificant impacts on PFOA degradation. However, beyond these concentration levels, PFOA degradation rates reduced significantly with an increase in chloride concentrations, especially under the higher temperature.
基金supported by the National Natural Science Foundation of China (No. 20907026)the High Level Talent Research Foundation of Qindao Technological University (No:C-10-210)
文摘Perfluorooctanoic acid (PFOA) is a new-found hazardous persistent organic pollutant, and it is resistant to decomposition by hydroxyl radical (HO.) due to its stable chemical structure and the high electronegativity of fluorine. Photocatalytic reduction of PFOA with β-Ga2O3 in anoxic aqueous solution was investigated for the first time, and the results showed that the photoinduced electron (ecb) coming from the β-Ga2O3 conduction band was the major degradation substance for PFOA, and shorter-chain perfluorinated carboxylic acids (PFCAs, CnF2n+1COOH, 1 ≤ n ≤ 6) were the dominant products. Furthermore, the concentration of F- was measured by the IC technique and defluorination efficiency was calculated. After 3 hr, the photocatalytic degradation efficiency was 98.8% and defluorination efficiency was 31.6% in the presence of thiosulfate and bubbling N2. The degradation reaction followed first-order kinetics (k = 0.0239 min-1, t1/2 = 0.48 hr). PFCAs (CnF2n+xCOOH, 1 ≤ n≤ 7) were detected and measured by LC-MS and LC-MS/MS methods. It was deduced that the probable photocatalytic degradation mechanism involves ec-b attacking the carboxyl of CnF2n+1COOH, resulting in decarboxylation and the generation of CnFzn+1. The produced CnF2n+1 reacted with H2O, forming CnF2n+1OH, then CnF2n+1OH underwent HF loss and hydrolysis to form CnF2,+1COOH.
基金financial support from Ministry of Science and Technology of the People’s Republic of China (Nos.2016YFE0112200 and 2016YFC0202700)National Natural Science Foundation of China (Nos.21507011,21677037 and 21607027)Natural Science Foundation of Shanghai (Nos. 19ZR1471200,17ZR1440200)
文摘Bismuth-based material has been broadly studied due to their potential applications in various areas,especially used as promising photocatalysts for the removal of persistent organic pollutants(POPs) and several approaches have been adopted to tailor their features.Herein,the bismuth-based photocatalysts(BiOCl,BiPO4,BiOPO4/BiOCl) were synthesized by hydrothermal method and advanced characterization techniques(XRD,SEM,EDS elemental mapping,Raman and UV-vis DRS) were employed to analyze their morphology,crystal structure,and purity of the prepared photocatalysts.These synthesized photocatalysts offered a praiseworthy activity as compared to commercial TiO2(P25) for the degradation of model pollutant perfluorooctanoic acid(PFOA) under 254 nm UV light.It was interesting to observe that all synthesized photocatalysts show significant degradation of PFOA and their photocatalytic activity follows the order:bismuth-based catalysts> TiO2(P25)> without catalyst.Bismuth-based catalysts degraded the PFOA by almost 99.99% within 45 min while this degradation efficiency was 66.05% with TiO2 under the same reaction condition.Our work shows that the bismuth-based photocatalysts are promising in PFOA treatment.
基金funding provided by University at Albany,State University of New York。
文摘Nanophotocatalysts have shown great potential for degrading poly-and perfluorinated substances(PFAS).In light of the fact that most of these catalysts were studied in pure water,this study was designed to elucidate effects from common environmental factors on decomposing and defluorinating perfluorooctanoic acid(PFOA)by In2O3 nanoparticles.Results from this work demonstrated that among the seven parameters,pH,sulfate,chloride,H2O2,In2O3 dose,NOM and O2,the first four had statistically significant negative effects on PFOA degradation.Since PFOA is a strong acid,the best condition leading to the highest PFOA removal was identified for two pH ranges.When pH was between 4 and 8,the optimal condition was:pH=4.2;sulfate=5.00 mg/L;chloride=20.43 mg/L;H2O2=0 mmol/L.Under this condition,PFOA decomposition and defluorination were 55.22 and 23.56%,respectively.When pH was between 2 and 6,the optimal condition was:pH=2;sulfate=5.00 mg/L;chloride=27.31 mg/L;H2O2=0 mmol/L.With this condition,the modeled PFOA decomposition was 97.59%with a defluorination of approximately 100%.These predicted results were all confirmed by experimental data.Thus,In2O3 nanoparticles can be used for degrading PFOA in aqueous solutions.This approach works best when the target contaminated water contains low concentrations of NOM,sulfate and chloride and at a low pH.
基金supported by the National Basic Research Program(973)of China(No.2010CB933600)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA09030203)+4 种基金the National Natural Science Foundation of China(Nos.2127716141103076)the special fund from the State Key Laboratory of Environmental Aquatic Chemistry(No.10Y10ESPCR)the Youth Innovation Promotion AssociationChinese Academy of Sciences(29QNCX2012005)
文摘Perfluorooctanoic acid(PFOA)is recalcitrant to degrade and mineralize.Here,the effect of temperature on the photolytic decomposition of PFOA was investigated.The decomposition of PFOA was enhanced from 34% to 99% in 60 min of exposure when the temperature was increased from 25 to 85℃ under UV light(201–600 nm).The limited degree of decomposition at 25℃ was due to low quantum yield,which was increased by a factor of 12 at 85℃.Under the imposed conditions,the defluorination ratio increased from 8% at 25℃ to 50% at85℃ in 60 min.Production of perfluorinated carboxylic acids(PFCAs,C7–C5),PFCAs(C4–C3)and TFA(trifluoroacetic acid,C2)accelerated and attained a maximum within 30 to 90 min at 85℃.However,these reactions did not occur at 25℃ despite extended irradiation to180 min.PFOA was decomposed in a step-wise process by surrendering one CF2unit.In each cyclical process,increased temperature enhanced the quantum yields of irradiation and reactions between water molecules and intermediates radicals.The energy consumption for removing eachμmol of PFOA was reduced from 82.5 k J at 25℃ to 10.9 k J at 85℃ using photolysis.Photolysis coupled with heat achieved high rates of PFOA degradation and defluorination.
基金Supported by the Grant from the Science and Technique Key Programs of Power China Ltd.(P45220)the Open-ended Fund of Chongqing University’s Large-Scale Equipment(202203150184)
文摘In order to optimize the solid phase extraction(SPE)conditions of perfluorooctanoic acid(PFOA)in the raw leachate and treated leachate,the effects of activator properties,SPE cartridge,p H value,ionic strength,and eluent properties were studied through single factor experiments.The optimal results of each single factor were obtained.Considering that the concentration of PFOA in the treated leachate is lower than that of the raw leachate,the SPE conditions of the treated leachate have been further optimized.Based on the above single-factor experiment,the main influencing factors were screened out as the volume of activator,ionic strength,and volume of eluent,and the three-factor threelevel response surface methodology(RSM)was optimized.The optimum SPE conditions of PFOA from treated landfill leachate were as follows:Activation of weak anion exchange(WAX)cartridge with 10 mL methanol,dosage of 600 mg KCl,6 m L 1%ammonia methanol eluted PFOA,the theory recovery rate is over95.67%.It has been verified that the error between the predicted value and the actual extraction recovery is small and has good repeatability.
基金supported by the National Natural Science Foundation of China(No.20977043,20777033)the Opening Funding of State Key Laboratory of Pollution Control and Resource Reuse(No.PCRRF12012)
文摘The aggregation of multi-walled carbon nanotubes (MWCNTs) in the aqueous phase not only inhibits their extensive utilization in various aspects but also dominates their environmental fate and transport.The role of surfactants at low concentration in the aggregation of MWCNTs has been studied,however the effect of perfluorinated surfactants at low concentration is uncertain.To understand this interfacial phenomenon,the influences of perfluorooctanoic acid (PFOA),and sodium dodecyl sulfate (SDS) as a control,on MWCNT aggregation in the aqueous phase were examined by the UV absorbency method.Influences of pH and cationic species on the critical coagulation concentration (CCC) value were evaluated.The CCC values were dependent on the concentration of PFOA,however a pronounced effect of SDS concentration on the CCC values was not observed.The CCC values of the MWCNTs were 51.6 mmol/L in NaCl and 0.28 mmol/L in CaCl 2 solutions,which suggested pronounced differences in the effects of Na+ and Ca2+ ions on the aggregation of the MWCNTs.The presence of both PFOA and SDS significantly decreased the CCC values of the MWCNTs in NaCl solution.The aggregation of the MWCNTs took place under acidic conditions and was not notably altered under neutral and alkaline conditions due to the electrostatic repulsion of deprotonated functional groups on the surface of the MWCNTs.
基金support from the Brook Byers Institute for Sustainable Systems,Hightower Chair,and Georgia Research Alliance at the Georgia Institute of Technology.
文摘Liquid-liquid extraction(LLE)using ionic liquids(ILs)-based methods to remove perfluoroalkyl chemicals(PFACs),such as perfluorooctanoic acid(PFOA)and perfluorooctane sulfonic acid(PFOS),from wastewater,is an important strategy.However,the lack of physicochemical and LLE data limits the selection of the most suitable ILs for the extraction of PFACs.In this work,1763 ILs for PFACs extraction from water were systematically screened using COSMOtherm to estimate the infinite dilution activity coefficient(lnγ^(∞))of PFOA and PFOS in water and ILs.To evaluate the accuracy of COSMOtherm,8 ILs with various lnγ^(∞)values were selected,and their extraction efficiency(E)and distribution coefficient(D_(exp))were measured experimentally.The results showed that the predicted lnγ^(∞)decreased as the increase of experimental extraction efficiency of PFOA or PFOS,while the tendency of predicted distribution coefficient(D_(pre))was consistent with the experimental(D_(exp))results.This work provides an efficient basis for selecting ILs for the extraction of PFACs from wastewater.
基金funding from Evoqua Companythe National Natural Science Foundation of China (Nos. 51878090 and 51808066)the Chinese Scholarship Council for financial support。
文摘When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PFOA) from groundwater. With favorable tailoring, QAE-AC removed PFOA from groundwater for 118,000 bed volumes before halfbreakthrough in rapid small scale column tests, while the influent PFOA concentration was 200 ng/L. The tailoring involved pre-dosing QAE at an array of proportions onto this carbon, and then monitoring bed life for PFOA removal. When pre-dosing with 1 mL QAE, this PFOA bed life reached an interim peak, whereas bed life was less following 3 mL QAE pre-dosing, then PFOA bed life exhibited a steady rise for yet subsequently higher QAE pre-dosing levels. Large-scale atomistic modelling was used herein to provide new insight into the mechanism of PFOA removal by QAE-AC. Based on experimental results and modelling, the authors perceived that the QAE's epoxide functionalities cross-linked with phenolics that were present along the activated carbon's graphene edge sites, in a manner that created mesopores within macroporous regions or created micropores within mesopores regions. Also, the QAE could react with hydroxyls outside of these pore, including the hydroxyls of both graphene edge sites and other QAE molecules. This latter reaction formed new pore-like structures that were external to the activated carbon grains. Adsorption of PFOA could occur via either charge balance between negatively charged PFOA with positively charged QAE, or by van der Waals forces between PFOA's fluoro-carbon tail and the graphene or QAE carbon surfaces.
基金the German Federal Environmental Foundation for sponsoring the project.
文摘The distribution of polyfluoroalkyl compounds(PFCs)in the dissolved and particulate phase and their discharge from the river Elbe into the North Sea were studied.The PFCs quantified included C_(4)-C_(8) perfluorinated sulfonates(PFSAs),6∶2 fluorotelomer sulfonate(6∶2 FTS),C_(6) and C_(8) perfluorinated sulfinates(PFSiAs),C_(4)-C_(12) perfluorinated carboxylic acids(PFCAs),perfluoro-3,7-dimethyl-octanoic acid(3,7m_(2)-PFOA),perfluorooctane sulfonamide(FOSA),and n-ethyl perfluroctane sulfonamidoethanol(EtFOSE).PFCs were mostly distributed in the dissolved phase,where perfluorooctanoic acid(PFOA)dominated with 2.9–12.5 ng/L.In the suspended particulate matter FOSA and perfluorooctane sulfonate(PFOS)showed the highest concentrations(4.0 ng/L and 2.3 ng/L,respectively).The total flux ofΣPFCs from the river Elbe was estimated to be 802 kg/year for the dissolved phase and 152 kg/year for the particulate phase.This indicates that the river Elbe acts as a source of PFCs into the North Sea.However,the concentrations of perfluorobutane sulfonate(PFBS)and perfluorobutanoic acid(PFBA)in the North Sea were higher than that in the river Elbe,thus an alternative source must exist for these compounds.
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.
基金We thank the Arctic Monitoring and Assessment Programme(AMAP)and the national programs in the circumpolar countries for their funding and support of this work.We are especially grateful to Simon Wilson,Cynthia de Wit,and the reviewers that read the chapter on PFASs in the original AMAP assessment.We are thankful to the northern communities in circumpolar regions for their cooperation and collection of biological samples that yielded the data reviewed here.DCGM was supported by the King Carl XVI Gustaf Professorship in Environmental Science at the Dept of Environmental Science and Analytical Chemistry,Stockholm University during 2018-19.
文摘Poly-and perfluoroalkyl substances(PFASs)are important environmental contaminants globally and in the early 2000s they were shown to be ubiquitous contaminants in Arctic wildlife.Previous reviews by Butt et al.and Letcher et al.have covered studies on levels and trends of PFASs in the Arctic that were available to 2009.The purpose of this review is to focus on more recent work,generally published between 2009 and 2018,with emphasis on PFASs of emerging concern such as perfluoroalkyl carboxylates(PFCAs)and short-chain perfluoroalkyl sulfonates(PFSAs)and their precursors.Atmospheric measurements over the period 2006e2014 have shown that fluorotelomer alcohols(FTOHs)as well as perfluorobutanoic acid(PFBA)and perfluoroctanoic acid(PFOA)are the most prominent PFASs in the arctic atmosphere,all with increasing concentrations at Alert although PFOA concentrations declined at the Zeppelin Station(Svalbard).Results from ice cores show generally increasing deposition of PFCAs on the Devon Ice cap in the Canadian arctic while declining fluxes were found in a glacier on Svalbard.An extensive dataset exists for long-term trends of long-chain PFCAs that have been reported in Arctic biota with some datasets including archived samples from the 1970s and 1980s.Trends in PFCAs over time vary among the same species across the North American Arctic,East and West Greenland,and Svalbard.Most long term time series show a decline from higher concentrations in the early 2000s.However there have been recent(post 2010)increasing trends of PFCAs in ringed seals in the Canadian Arctic,East Greenland polar bears and in arctic foxes in Svalbard.Annual biological sampling is helping to determine these relatively short term changes.Rising levels of some PFCAs have been explained by continued emissions of long-chain PFCAs and/or their precursors and inflows to the Arctic Ocean,especially from the North Atlantic.While the effectiveness of biological sampling for temporal trends in long-chain PFCAs and PFSAs has been demonstrated,this does not apply to the C4eC8ePFCAs,perfluorobutane sulfonamide(FBSA),or perfluorobutane sulfonate(PFBS)which are generally present at low concentrations in biota.In addition to air sampling,sampling abiotic media such as glacial cores,and annual sampling of lake waters and seawater would appear to be the best approaches for investigating trends in the less bioaccumulative PFASs.
基金supported by the National Natural Science Foundation of China(Nos.21878323,21736001)National Key R&D Program of China(No.2020YFC1807901)Talent program(No.2021RC022)。
文摘Nanofiltration(NF)process has become one of the most promising technologies to remove micro-organic combined water pollution.Developing a NF membrane material with efficient separation for perfluorooctanoic acid(PFOA)combined pollution is highly desired,this manuscript targets this unmet need specifically.In this work,hydrophilic SiO_(2)nanoparticles with various contents blended with carboxylic multiwalled carbon nanotube were used to modify poly(m-phenylene isophthal amide)(SiO_(2)/CMWCNT/PMIA)hollow fiber NF membrane.The modified membrane with 0.1 wt%SiO_(2)doping exhibits way better fouling resistance with irreversible fouling ratio decreased dramatically from 18.7%to 2.3%,and the recovery rate of water flux increases significantly from 81.2%to 97.7%.The separation experiment results had confirmed that the modified membrane could improve the rejection from 97.2%to 98.6%for perfluorooctanoic acid(PFOA)and its combined pollution with bovine serum albumin(BSA).It is clear that this reported SiO_(2)/CMWCNT/PMIA hollow fiber NF membrane potentially could be applied in water treatment.This research also provides a theoretical basis for efficiently removal of PFOA and its combined pollution by NF membrane.