A method of quantification of perfluorinated compounds(PFCs)from atmospheric particulate matter(APM)is described.A single step pretreatment method,selective pressurized liquid extraction(SPLE),was developed to reduce ...A method of quantification of perfluorinated compounds(PFCs)from atmospheric particulate matter(APM)is described.A single step pretreatment method,selective pressurized liquid extraction(SPLE),was developed to reduce the high matrix background and avoid contamination from commonly used multiple sample pretreatment steps.An effective sorbent was selected to purify the PFCs during SPLE,followed by liquid chromatography-tandem mass spectrometry(LC–MS/MS),for quantification of PFCs.Conditions affecting the SPLE efficiency,including temperature,static extraction time,and number of extraction cycles used,were studied.The optimum conditions were found to be 120℃,10 min,and 3 cycles,respectively.LC-MS/MS method was developed to obtain the optimal sensitivity specific to PFCs.The method detection limits(MDLs)were 0.006 to 0.48 ng/g for the PFCs studied and the linear response range was from 0.1 to 100 ng/g.To ensure accurate values were obtained,each step of the experiment was evaluated and controlled to prevent contamination.The optimized method was tested by performing spiking experiments in natural particulate matter matrices and good rates of recovery and reproducibility were obtained for all target compounds.Finally,the method was successfully used to measure 16 PFCs in the APM samples collected in Beijing over five years from 2015 to 2019.It is observed that some PFCs follow the trend of total PFC changes,and can be attributed to the environment influencing events and policy enforcement,while others don't seem to change as much with time of the year or from year to year.展开更多
Perfuorinated compounds(PFCs)are toxic and widely present in the environment,and therefore effective adsorbents are required to remove PFCs from environmental water.In the present study,a new type of fuorinated biomas...Perfuorinated compounds(PFCs)are toxic and widely present in the environment,and therefore effective adsorbents are required to remove PFCs from environmental water.In the present study,a new type of fuorinated biomass materials was synthesized via an ingenious fuorosilanization reaction.These adsorbents were applied for the adsorption of 13typical PFCs,including perfuorocarboxylic acids(PFCAs)and perfuorosulfonic acids(PFSAs).By comparing their adsorption performance,Fluorinated cedar slag(FCS)was discovered to have the best absorption efficiency and enabled highly efficient enrichment of PFCs.The adsorption recovery of FCS with the investigated PFCs is greater than 90%under the optimal adsorption condition.Ascribed to the high affinity of F-F sorbent-sorbate interaction,FCS had good adsorption capacities of PFCs from aqueous solution,with the maximum adsorption capacity of 15.80 mg/g for PFOS and 10.71 mg/g for PFOA,respectively.Moreover,the adsorption time could be achieved in a short time(8 min).Using the FCS absorbent,an innovative FCS-solid phase extraction assisted with high performance liquid chromatography-electrospray-tandem mass spectrometry(FCS-SPE-HPLC-ESI-MS/MS)method was first developed to sensitively detect PFCs in the environmental water samples.The intra-day and inter-day recovery rates of the 13 compounds ranged from 90.7%-104.3%,with the RSD of 2.1%-4.7%(intra-day)and 2.5%-8.5%(inter-day),respectively.This research demonstrates the potential of the newly fuoro-functionalized plant biomass to adsorb PFCs from environmental water,with the advantages of high adsorption efficiencies,high antiinterference,easy operation and low economic cost.展开更多
Per- and polyfluoroalkyl substances (PFAS) pose serious human health and environmental risks due to their persistence and toxicity. Among the available PFAS remediation options, the electrochemical approach is promisi...Per- and polyfluoroalkyl substances (PFAS) pose serious human health and environmental risks due to their persistence and toxicity. Among the available PFAS remediation options, the electrochemical approach is promising with better control. In this review, recent advances in the decontamination of PFAS from water using several state-of-the-art electrochemical strategies, including electro-oxidation, electro-adsorption, and electro-coagulation, were systematically reviewed. We aimed to elucidate their design principles, underlying working mechanisms, and the effects of operation factors (e.g., solution pH, applied voltage, and reactor configuration). The recent developments of innovative electrochemical systems and novel electrode materials were highlighted. In addition, the development of coupled processes that could overcome the shortcomings of low efficiency and high energy consumption of conventional electrochemical systems was also emphasized. This review identified several major knowledge gaps and challenges in the scalability and adaptability of efficient electrochemical systems for PFAS remediation. Materials science and system design developments are forging a path toward sustainable treatment of PFAS-contaminated water through electrochemical technologies.展开更多
提出了滤过型固相萃取柱净化-超高效液相色谱-串联质谱法同时测定鸡蛋中全氟丁酸、全氟戊酸、全氟己酸、全氟庚酸、全氟辛酸、全氟壬酸、全氟癸酸、全氟十一酸、全氟十二酸、全氟十三酸、全氟十四酸、全氟丁烷磺酸、全氟己烷磺酸、全氟...提出了滤过型固相萃取柱净化-超高效液相色谱-串联质谱法同时测定鸡蛋中全氟丁酸、全氟戊酸、全氟己酸、全氟庚酸、全氟辛酸、全氟壬酸、全氟癸酸、全氟十一酸、全氟十二酸、全氟十三酸、全氟十四酸、全氟丁烷磺酸、全氟己烷磺酸、全氟庚烷磺酸、全氟辛烷磺酸等15种全氟化合物含量的方法。鸡蛋样品(2 g)中加入0.1 mL 20.0μg·L^(-1)同位素内标混合溶液,经10 mL 80%(体积分数)乙腈溶液振荡和超声提取后,离心;分取5 mL滤液,直接过滤过型Captive EMR-Lipid柱净化,收集流出液,氮吹至近干,加入500μL甲醇复溶,经涡旋、离心处理后测定。采用Agilent Eclipse Plus C_(18)RRHD色谱柱(100 mm×2.1 mm,1.8μm)分离,以不同体积比的2 mmol·L^(-1)乙酸铵溶液和甲醇的混合溶液梯度洗脱,在电喷雾离子源负离子扫描模式下,以多反应监测模式检测,同位素内标法定量。结果表明:15种全氟化合物标准曲线的线性范围均为0.125~20.0μg·L^(-1),测定下限(10S/N)为0.05~0.16μg·kg^(-1);在0.500,4.00,16.0μg·kg^(-1)加标浓度水平下,15种目标物的回收率为78.0%~111%,测定值的相对标准偏差(n=6)为0.87%~14%。展开更多
New and efficient proposed to treat perfluorinated reactor systems were compounds via catalytic decomposition. One system has a single reactor （S-1）, and another has a series of reactors （S-2）. Both systems are c...New and efficient proposed to treat perfluorinated reactor systems were compounds via catalytic decomposition. One system has a single reactor （S-1）, and another has a series of reactors （S-2）. Both systems are capable of producing a valuable CaF2 and eliminating toxic HF effluent and their feasibility was studied at various temperatures with a commercial process simulator, Aspen HYSYS. They are better than the conventional system, and S-2 is better than S-1 in terms of CaF2 production, a required heat for the system, natural gas usage and CO2 emissions in a boiler, and energy consumption. Based on process simulation results, preliminary economic analysis shows that cost savings of 12.37% and 13.55% were obtained in S-2 at 589.6 and 621.4℃compared to S-1 at 700 and 750 ℃, respectively, for the same amount of CaF2 production.展开更多
Per-and polyfluorinated alkyl substances(PFASs) are commonly used in industrial processes and daily life products.Because they are persistent, they accumulate in the environment, wildlife and humans.Although many stud...Per-and polyfluorinated alkyl substances(PFASs) are commonly used in industrial processes and daily life products.Because they are persistent, they accumulate in the environment, wildlife and humans.Although many studies have focused on two of the most representative PFASs, PFOS and PFOA, the potential toxicity of short-chain PFASs has not yet been given sufficient attention.We used a battery of assays to evaluate the toxicity of several four-carbon and six-carbon perfluorinated sulfonates and carboxyl acids(PFBS,PFHxS, PFBA and PFHxA), with a human mesenchymal stem cell(hMSC) system.Our results demonstrate significant cyto-and potential developmental toxicity for all the compounds analyzed, with shared but also distinct mechanisms of toxicity.Moreover, the effects of PFBS and PFHxS were stronger than those of PFBA and PFHxA, but occurred at higher doses compared to PFOS or PFOA.展开更多
12 perfluorinated compounds（PFCs） in human blood from workers in a textile mill in Shandong province and several barbershops in Tianjin were analyzed in this study. It was found that perfluorooctanesulfonate（PFOS）...12 perfluorinated compounds（PFCs） in human blood from workers in a textile mill in Shandong province and several barbershops in Tianjin were analyzed in this study. It was found that perfluorooctanesulfonate（PFOS） and perfluorooctanoate（PFOA） were the most prominent PFCs, with average concentrations of 5.73 mg/L and 5.46 mg/L for textile workers, and 2.55 mg/L and 2.84 mg/L for barbers.PFOS and perfluorohexanesulfonate（PFHxS） concentrations revealed a positive correlation in blood samples（p 〈 0.01）, and concentrations among PFOS, perfluorononanoic acid（PFNA） and perfluorodecanoic acid（PFDA） also revealed positive correlations（p 〈 0.01）. The influence of gender and age on PFC concentration in blood was also investigated, and the results showed that there was no statistically significant difference between the male and female samples, as well as in samples from people with different ages. Generally speaking, the textile workers展开更多
基金supported by the NQI Project of National key R&D Program of China (No.2016YFF0201102)the project for the“Development of analytical method and certified reference materials for tracing air pollutant source” (No.21AKY1514)from the National Institute of Metrology,Beijing,China。
文摘A method of quantification of perfluorinated compounds(PFCs)from atmospheric particulate matter(APM)is described.A single step pretreatment method,selective pressurized liquid extraction(SPLE),was developed to reduce the high matrix background and avoid contamination from commonly used multiple sample pretreatment steps.An effective sorbent was selected to purify the PFCs during SPLE,followed by liquid chromatography-tandem mass spectrometry(LC–MS/MS),for quantification of PFCs.Conditions affecting the SPLE efficiency,including temperature,static extraction time,and number of extraction cycles used,were studied.The optimum conditions were found to be 120℃,10 min,and 3 cycles,respectively.LC-MS/MS method was developed to obtain the optimal sensitivity specific to PFCs.The method detection limits(MDLs)were 0.006 to 0.48 ng/g for the PFCs studied and the linear response range was from 0.1 to 100 ng/g.To ensure accurate values were obtained,each step of the experiment was evaluated and controlled to prevent contamination.The optimized method was tested by performing spiking experiments in natural particulate matter matrices and good rates of recovery and reproducibility were obtained for all target compounds.Finally,the method was successfully used to measure 16 PFCs in the APM samples collected in Beijing over five years from 2015 to 2019.It is observed that some PFCs follow the trend of total PFC changes,and can be attributed to the environment influencing events and policy enforcement,while others don't seem to change as much with time of the year or from year to year.
基金supported by the National Natural Science Foundation of China (No.22276221,and 21675176)the Fundamental Research Funds for the Central Universities,and South-Central Minzu University (No.CZP21002)。
文摘Perfuorinated compounds(PFCs)are toxic and widely present in the environment,and therefore effective adsorbents are required to remove PFCs from environmental water.In the present study,a new type of fuorinated biomass materials was synthesized via an ingenious fuorosilanization reaction.These adsorbents were applied for the adsorption of 13typical PFCs,including perfuorocarboxylic acids(PFCAs)and perfuorosulfonic acids(PFSAs).By comparing their adsorption performance,Fluorinated cedar slag(FCS)was discovered to have the best absorption efficiency and enabled highly efficient enrichment of PFCs.The adsorption recovery of FCS with the investigated PFCs is greater than 90%under the optimal adsorption condition.Ascribed to the high affinity of F-F sorbent-sorbate interaction,FCS had good adsorption capacities of PFCs from aqueous solution,with the maximum adsorption capacity of 15.80 mg/g for PFOS and 10.71 mg/g for PFOA,respectively.Moreover,the adsorption time could be achieved in a short time(8 min).Using the FCS absorbent,an innovative FCS-solid phase extraction assisted with high performance liquid chromatography-electrospray-tandem mass spectrometry(FCS-SPE-HPLC-ESI-MS/MS)method was first developed to sensitively detect PFCs in the environmental water samples.The intra-day and inter-day recovery rates of the 13 compounds ranged from 90.7%-104.3%,with the RSD of 2.1%-4.7%(intra-day)and 2.5%-8.5%(inter-day),respectively.This research demonstrates the potential of the newly fuoro-functionalized plant biomass to adsorb PFCs from environmental water,with the advantages of high adsorption efficiencies,high antiinterference,easy operation and low economic cost.
基金supported by the National Natural Science Foundation of China(No.52170068 and U21A20161)the Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(No.QAK202108).
文摘Per- and polyfluoroalkyl substances (PFAS) pose serious human health and environmental risks due to their persistence and toxicity. Among the available PFAS remediation options, the electrochemical approach is promising with better control. In this review, recent advances in the decontamination of PFAS from water using several state-of-the-art electrochemical strategies, including electro-oxidation, electro-adsorption, and electro-coagulation, were systematically reviewed. We aimed to elucidate their design principles, underlying working mechanisms, and the effects of operation factors (e.g., solution pH, applied voltage, and reactor configuration). The recent developments of innovative electrochemical systems and novel electrode materials were highlighted. In addition, the development of coupled processes that could overcome the shortcomings of low efficiency and high energy consumption of conventional electrochemical systems was also emphasized. This review identified several major knowledge gaps and challenges in the scalability and adaptability of efficient electrochemical systems for PFAS remediation. Materials science and system design developments are forging a path toward sustainable treatment of PFAS-contaminated water through electrochemical technologies.
文摘提出了滤过型固相萃取柱净化-超高效液相色谱-串联质谱法同时测定鸡蛋中全氟丁酸、全氟戊酸、全氟己酸、全氟庚酸、全氟辛酸、全氟壬酸、全氟癸酸、全氟十一酸、全氟十二酸、全氟十三酸、全氟十四酸、全氟丁烷磺酸、全氟己烷磺酸、全氟庚烷磺酸、全氟辛烷磺酸等15种全氟化合物含量的方法。鸡蛋样品(2 g)中加入0.1 mL 20.0μg·L^(-1)同位素内标混合溶液,经10 mL 80%(体积分数)乙腈溶液振荡和超声提取后,离心;分取5 mL滤液,直接过滤过型Captive EMR-Lipid柱净化,收集流出液,氮吹至近干,加入500μL甲醇复溶,经涡旋、离心处理后测定。采用Agilent Eclipse Plus C_(18)RRHD色谱柱(100 mm×2.1 mm,1.8μm)分离,以不同体积比的2 mmol·L^(-1)乙酸铵溶液和甲醇的混合溶液梯度洗脱,在电喷雾离子源负离子扫描模式下,以多反应监测模式检测,同位素内标法定量。结果表明:15种全氟化合物标准曲线的线性范围均为0.125~20.0μg·L^(-1),测定下限(10S/N)为0.05~0.16μg·kg^(-1);在0.500,4.00,16.0μg·kg^(-1)加标浓度水平下,15种目标物的回收率为78.0%~111%,测定值的相对标准偏差(n=6)为0.87%~14%。
文摘New and efficient proposed to treat perfluorinated reactor systems were compounds via catalytic decomposition. One system has a single reactor （S-1）, and another has a series of reactors （S-2）. Both systems are capable of producing a valuable CaF2 and eliminating toxic HF effluent and their feasibility was studied at various temperatures with a commercial process simulator, Aspen HYSYS. They are better than the conventional system, and S-2 is better than S-1 in terms of CaF2 production, a required heat for the system, natural gas usage and CO2 emissions in a boiler, and energy consumption. Based on process simulation results, preliminary economic analysis shows that cost savings of 12.37% and 13.55% were obtained in S-2 at 589.6 and 621.4℃compared to S-1 at 700 and 750 ℃, respectively, for the same amount of CaF2 production.
基金supported by the National Natural Science Foundation of China (Nos.21876197, 21577166, 21707160)the Chinese Academy of Sciences (Nos.XDB14040301, 29[2015]30, QYZDJ-SSW-DQC017)the K.C.Wong Education Foundation.
文摘Per-and polyfluorinated alkyl substances(PFASs) are commonly used in industrial processes and daily life products.Because they are persistent, they accumulate in the environment, wildlife and humans.Although many studies have focused on two of the most representative PFASs, PFOS and PFOA, the potential toxicity of short-chain PFASs has not yet been given sufficient attention.We used a battery of assays to evaluate the toxicity of several four-carbon and six-carbon perfluorinated sulfonates and carboxyl acids(PFBS,PFHxS, PFBA and PFHxA), with a human mesenchymal stem cell(hMSC) system.Our results demonstrate significant cyto-and potential developmental toxicity for all the compounds analyzed, with shared but also distinct mechanisms of toxicity.Moreover, the effects of PFBS and PFHxS were stronger than those of PFBA and PFHxA, but occurred at higher doses compared to PFOS or PFOA.
基金supported by the National Natural Science Foundation of China (Nos. 41023005, 21377145, 21321004)the State Environmental Protection Welfare Scientific Research Project (No. 201009026)
文摘12 perfluorinated compounds（PFCs） in human blood from workers in a textile mill in Shandong province and several barbershops in Tianjin were analyzed in this study. It was found that perfluorooctanesulfonate（PFOS） and perfluorooctanoate（PFOA） were the most prominent PFCs, with average concentrations of 5.73 mg/L and 5.46 mg/L for textile workers, and 2.55 mg/L and 2.84 mg/L for barbers.PFOS and perfluorohexanesulfonate（PFHxS） concentrations revealed a positive correlation in blood samples（p 〈 0.01）, and concentrations among PFOS, perfluorononanoic acid（PFNA） and perfluorodecanoic acid（PFDA） also revealed positive correlations（p 〈 0.01）. The influence of gender and age on PFC concentration in blood was also investigated, and the results showed that there was no statistically significant difference between the male and female samples, as well as in samples from people with different ages. Generally speaking, the textile workers
