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
The influence of pH on the partitioning behavior of REE at the water/particulate interface has been studied experimentally. At the beginning of colloid formation the adsorption of REE on iron hydroxide colloids is dom...The influence of pH on the partitioning behavior of REE at the water/particulate interface has been studied experimentally. At the beginning of colloid formation the adsorption of REE on iron hydroxide colloids is dominant, followed by REE desorption. Finally adsorption and desorption tend to reach equilibration. The capability of iron hydroxide colloids to adsorb the HREE is greater than that to adsorb the LREE. With increasing pH, LREE/HREE fractionations will take place between iron hydroxide colloids and water, leading to the reduction of their partition coefficient ratio (DLREE/DHREE). The DREE distribution patterns show Y anomalies (DY/DHo <1), with obvious REE tetrad effects appearing under low pH conditions. Experimental results have shown that there do exist REE tetrad effects in nature. In addition to pH, the chemical type of surface water and ion intensity are also the important factors controlling REE tetrad effects and leading to fractionations between particulate-adsorbed REE and dissolved REE.展开更多
The characteristics of water-soluble ions in size-resolved particulate matter were investigated usingion chromatography at Shangdianzi, a regional background station of Beijing, Tianjin, and Hebei. Seasonal total conc...The characteristics of water-soluble ions in size-resolved particulate matter were investigated usingion chromatography at Shangdianzi, a regional background station of Beijing, Tianjin, and Hebei. Seasonal total concentrations of ions （Na＋, Mg2＋, IC, Ca2＋, NH＋4, Cl-, SO2-4 and NO-3） were 75.5 ± 52.9 μg/m3 in spring, 26.5 ± 12.3 Bg/m3 in summer, 22.7 ± 20.4 μg/m3 in autumn, and 31.1 ± 23.9 μg/m3 in winter, respectively. The secondary ions （NO3, SO2-4 and NH＋4）, mainly associated with fine particles, accounted for 84.2% in spring, 82.1% in summer, 81.5% in autumn and 76.3% in winter of all ions. Strong correlations were found between NH＋4 and SO2-4 （r = 0.95, p 〈 0.01） as well as NH＋4 and NO-3 （r = 0.90, p 〈 0.01） in fine particles; while in coarse particles, correlations between Mg2＋ and NO-3 （r = 0.80, p 〈 0.01）, and Ca2＋ and NO2＋ （r = 0.85, p 〈 0.01） were found. The concentrations of Na＋, IC, Mg2＋, Ca2＋, NH＋4, Cl-, NO3, and SC2-4 were 2.02, 0.81, 0.36, 1.65, 9.58, 4.01, 18.9, and 18.4 μg/m3 in particulate matter from southeast-derived air masses, which were typically 1.58-3.37 times higher than in northwest trajectories. Thus, concentrations of water-soluble ions at this background station were heavily influenced by regional transport of serious pollution derived from biomass burning, coal combustion, industrial and vehicle exhaust emissions from Beijing, Tianjin, and Hebei.展开更多
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This work was supported by the State Outsanding Young Scientists Foundation (Grant No. 49625304) the Pre-selected Project under the State Climbing Program of China (Grant No. 95-39).
文摘The influence of pH on the partitioning behavior of REE at the water/particulate interface has been studied experimentally. At the beginning of colloid formation the adsorption of REE on iron hydroxide colloids is dominant, followed by REE desorption. Finally adsorption and desorption tend to reach equilibration. The capability of iron hydroxide colloids to adsorb the HREE is greater than that to adsorb the LREE. With increasing pH, LREE/HREE fractionations will take place between iron hydroxide colloids and water, leading to the reduction of their partition coefficient ratio (DLREE/DHREE). The DREE distribution patterns show Y anomalies (DY/DHo <1), with obvious REE tetrad effects appearing under low pH conditions. Experimental results have shown that there do exist REE tetrad effects in nature. In addition to pH, the chemical type of surface water and ion intensity are also the important factors controlling REE tetrad effects and leading to fractionations between particulate-adsorbed REE and dissolved REE.
基金supported by the National Environmental Protection Commonweal Research Project(No.201509062 and No.201409073)the National Natural Science Foundation of China(No.41105089)+1 种基金Research Project of Environmental Development Cenre(No.DY-2016-5)State Key Laboratory of Environmental Criteria and Risk Assessment,Chinese Research Academy of Environmental Sciences(No.SKLECRA201637)
文摘The characteristics of water-soluble ions in size-resolved particulate matter were investigated usingion chromatography at Shangdianzi, a regional background station of Beijing, Tianjin, and Hebei. Seasonal total concentrations of ions （Na＋, Mg2＋, IC, Ca2＋, NH＋4, Cl-, SO2-4 and NO-3） were 75.5 ± 52.9 μg/m3 in spring, 26.5 ± 12.3 Bg/m3 in summer, 22.7 ± 20.4 μg/m3 in autumn, and 31.1 ± 23.9 μg/m3 in winter, respectively. The secondary ions （NO3, SO2-4 and NH＋4）, mainly associated with fine particles, accounted for 84.2% in spring, 82.1% in summer, 81.5% in autumn and 76.3% in winter of all ions. Strong correlations were found between NH＋4 and SO2-4 （r = 0.95, p 〈 0.01） as well as NH＋4 and NO-3 （r = 0.90, p 〈 0.01） in fine particles; while in coarse particles, correlations between Mg2＋ and NO-3 （r = 0.80, p 〈 0.01）, and Ca2＋ and NO2＋ （r = 0.85, p 〈 0.01） were found. The concentrations of Na＋, IC, Mg2＋, Ca2＋, NH＋4, Cl-, NO3, and SC2-4 were 2.02, 0.81, 0.36, 1.65, 9.58, 4.01, 18.9, and 18.4 μg/m3 in particulate matter from southeast-derived air masses, which were typically 1.58-3.37 times higher than in northwest trajectories. Thus, concentrations of water-soluble ions at this background station were heavily influenced by regional transport of serious pollution derived from biomass burning, coal combustion, industrial and vehicle exhaust emissions from Beijing, Tianjin, and Hebei.
