Characteristics of phenanthrene and pyrene’s sorption and desorption on two local soils in solutions of simulated groundwater, simulated lung fluid, and simulated saliva were studied with batch equilibrium experiments to understand the fate of PAHs in the karst region of southwestern China and to assess the environmental exposure and the health risk of PAHs. The results showed that the sorption and desorption isotherms of phenanthrene and pyrene on two target soils in the three solution systems could be adequately described by the Freundlich model, while the fitted isotherm parameters for the simulated groundwater solution distinguished notably from those for the simulated body fluid solutions. For the sorption experiments, in the simulated groundwater, the n values were 0.722 and 0.672 for phenanthrene and were 0.724 and 0.663 for pyrene, respectively, on the yellow soil and the limestone soil; The log KF values were 3.118 and 3.323 for phenanthrene and were 3.648 and 3.846 for pyrene, respectively, on the yellow soil and the limestone soil. In the simulated body fluids, the n values for phenanthrene and pyrene ranged from 0.622 to 0.836 and from 0.590 to 0.865, respectively, and the log KF values of phenanthrene and pyrene ranged from 2.845 to 3.327 and from 3.344 to 3.779, respectively. For the desorption experiments, in the simulated groundwater, the n values were 0.662 and 0.744 for phenanthrene and were 0.702 and 0.647 for pyrene, respectively, on the yellow soil and the limestone soil. The log KF values were 3.666 and 3.686 for phenanthrene and were 4.128 and 4.225 for pyrene, respectively, on the yellow soil and the limestone soil. In the simulated body fluids, the n values for phenanthrene and pyrene ranged from 0.612 to 0.668 and from 0.631 to 0.819, respectively, and the log KF values of phenanthrene and pyrene ranged from 3.134 to 3.407 and from 3.533 to 3.839, respectively. The limestone soil had relatively higher log KF values but lower KOC values compared to those of the yellow soil, indicated that the nature of sorbent soils played the dominant role in sorption and desorption behaviors of PAHs. The experimental results showed a remarkable differences in sorption and desorption behaviors of PAHs in simulated body fluids and groundwater. The nonlinearities of measured isotherms and the measured sorption capacities of soils in simulated body fluids were significantly lower than corresponding those in the simulated groundwater, and HI values for simulated body fluids systems were significantly smaller than corresponding those for the simulated groundwater systems. The results underscore cautions in assessing environmental exposure and health risks of PAHs based on their sorption–desorption data in simulated groundwater as this is traditionally done.
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超高效液相色谱法检测地下水中苯并(a)芘 总被引：3，自引：2，他引：1
通过对荧光检测器波长、色谱柱温的选择,建立了超高效液相色谱测定地下水中苯并(a)芘的简便方法。采用Acquity C18色谱柱,流动相为甲醇,流速为0.40 mL/min,方法线性范围为0.082~200 ng/mL,检出限为0.033 ng/mL。在此分析条件下,苯并(a)芘保留时间仅为0.61 min。应用超高效液相色谱法和高效液相色谱法对地下水中苯并(a)芘的测定结果进行比较,超高效液相色谱在分析速度、分辨率和灵敏性方面,特别是在节省时间与溶剂消耗上具有显著的理论优势。 相似文献
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在不同照射时间、pH和溶解氧浓度下,研究了从加拿大魁北克省Rimouski河提取的黄腐酸(RRFA)在模拟太阳光照射过程中对苯并(α)芘结合性质的影响.结果表明,RRFA经模拟太阳光照射后,其与苯并(α)芘的结合系数KOC下降.光化过程中RRFA的相对分子质量或SUVA270与KOC之间有良好的指数回归关系.在pH 4.1～8.0范围内,以光照后的pH条件下测定照射样品的KOC,KOC平均下降47.4%±17.4%;以光照前的pH条件下测定照射样品的KOC,KOC平均下降48.7%±16.9%.溶解氧浓度的升高能加速RRFA的光氧化降解过程,与相应的未照射样品相比,空气饱和与氧气饱和条件下照射后的KOC分别下降30%和74%,氮气饱和条件下照射后的KOC升高122%. 相似文献
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高效液相色谱法测定地下水中苯并(a)芘的不确定度评定 总被引：1，自引：1，他引：0
通过对高效液相色谱法测定地下水中苯并(a)芘含量的全过程分析,确定了测定结果不确定度的来源。采用不确定度连续传递模型,对引入的不确定度分量进行评定,并采用最小二乘法对标准曲线进行拟合,确定了地下水中苯并(a)芘含量标准不确定度由样品取样量、样品定容体积及测定体积、样品重复性测定、标准溶液浓度和标准曲线拟合误差6部分不确定度合成。通过对2个不同含量样品测定结果不确定度评定,证明苯并(a)芘含量越低,测定结果的相对标准不确定度越大;且样品重复性测定和标准曲线拟合误差是测定结果不确定度的重要来源。 相似文献
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地下水中苯并[a]芘来源探讨 总被引：1，自引：0，他引：1
采用色谱质谱法对2000~2002年地下水中苯并[a]芘含量进行了分析,在分析苯并[a]芘在地下水环境中迁移特征的基础上,初步探讨了地下水中苯并[a]芘的来源。结果表明,苯并[a]芘在潜水含水层、200m的承压含水层以及500m的煤系地层和1000m以上的岩溶水中都有检出,含量低,为数个ng/L;由于苯并[a]芘的辛醇-水分配系数kow很大,为106个数量级,具有很强的憎水性,会强烈地被吸附在土壤颗粒物的有机碳上,因此苯并[a]芘很难从表层土壤中迁移进入地下水,土壤和沉积物是其主要的环境归宿;从理论上看,地下水中的苯并[a]芘是天然来源。 相似文献
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提出了一种氢化物发生—原子荧光光谱法测定地质样品(水系沉积物)中Sb(Ⅲ)和Sb(Ⅴ)的方法.选取4.8 mol/L HC1为提取剂,采用超声波辅助提取,以6 g/mL柠檬酸钠作为Sb(Ⅴ)的掩蔽剂,在0.24 mol/L的HC1介质中选择性测定Sb(Ⅲ),用差减法求得Sb(Ⅴ).Sb(Ⅲ)的方法检出限为0.075×10-6,Sb(Ⅴ)的方法检出限为0.097×10-6.对40 ng/mL的Sb(Ⅲ)和Sb(Ⅴ)分别连续测定11次,得到相对标准偏差分别为1.1％和0.64％.应用该方法对地质样品中的Sb(Ⅲ)和Sb(Ⅴ)进行分析测定,并与王水溶解值相比较,该方法测定的总Sb提取率在80％以上,Sb(Ⅲ)和Sb(Ⅴ)的加标回收率分别为83％ ～ 107％和98％ ～ 114％. 相似文献
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苯并[a]芘是多环芳烃中毒性最大的一种物质,具有三致作用。基于对淮河流域平原区四千余组水样的统计分析,阐述研究区内地下水中BaP分布现状,指出淮河流域平原地区浅层地下水（埋深小于50 m）及中深层地下水（埋深不小于50 m）中BaP分布现状,并分析其成因。浅层地下水中BaP检出率为1.85%,零散分布于整个研究区内,其中皖北豫东能源基地及河南部分人口密集乡镇超标点相对集中深层地下水中BaP检出率0.38%,主要分布于豫东皖北地区。流域内浅层水中BaP成因众多,其中煤炭燃烧、秸秆燃烧、生活排污是主要成因。在现状评价及成因分析基础上,提出开发利用地下水中避免BaP危害的措施。 相似文献
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以水中5种微量苯类化合物为对象，考察了固相微萃取器的聚二甲基硅氧烷纤维头萃取条件以及对水中非极性有机物的吸附萃取特性，并将固相微萃取-气相色谱法与顶空-气相色谱法和液液萃取-气相色谱法相比较，固相微萃取-气相色谱法分析水中5种苯类化合物，样品量为10mL时，方法的检出限为0．01～0．02μg／L，低于其它两种方法，测定水中低含量有机污染物有一定优势。 相似文献
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固相萃取-气相色谱法测定饮用水中的多氯联苯 总被引：2，自引：2，他引：0
研究了饮用水中84种多氯联苯的气相色谱分析方法。讨论了洗脱曲线、水样的pH值、甲醇加入量、含盐量、萃取流速等实验条件,并与经典的液-液萃取方法进行了对比。确定了样品在pH值为3,以5 mL/min的流速经大体积样品采样器-C18固相萃取柱富集,7 mL丙酮和5 mL乙腈洗脱,氮吹蒸发浓缩后正己烷定容至1.0mL,加入内标后使用电子捕获检测器气相色谱仪测定,并在选定的色谱条件下以选择离子监测方式进行验证。84种多氯联苯的方法检出限为1.2～15.0 ng/L,加标回收率为74.8%～126.8%,相对标准偏差为1.1%～14.8%。由于采用了大体积样品采样器,可实现多个样品的同时萃取富集,方法快速、低污染,低成本,可用于批量水样品中多氯联苯的分析测定。 相似文献
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在分析废旧金属拆解场地浅层地下水中芘的检出和分布特征的基础上,对地下水中芘的污染来源、污染途径和污染控制因素进行了探讨.研究结果表明,场地中心和地下水下游2km范围内芘污染明显,垂直于地下水流向芘迁移距离较小,一般小于0.5km.芘在地下水中的迁移转化受地下水中pH、Eh及DO等因素的控制,弱酸性或中性环境以及厌氧强还原条件下,芘易于检出和迁移,一般难以生物降解. 相似文献
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高锰酸盐指数(CODMn)、硝酸根(NO-3)、铵根(NH+4)是判断水体是否受到三氮污染的重要指标。对于测定这三个指标的水样保存方式和时间,地质行业标准和国内外主要国家标准间存在明显差异。地质行业标准规定地下水样品原水室温保存,CODMn和NH+4在3天内测定;NO-3在20天内测定;国家标准和美国标准推荐样品硫酸酸化,避光或冷藏保存,在2~7天内完成CODMn和NO-3和1~7天内完成NH+4测试。为了分析各类标准在样品保存要求上的差异对检测结果的影响,确保检测数据能真实地反映水体污染状况,找寻简便的保存方式,本文在广州地区采集地下水,按照地质行业标准与国家标准进行处理和保存,并在不同时间段对三个指标进行测试。分析验证结果表明:地质行业标准与国家和美国标准关于水样的保存方法均非常可靠。地质行业标准主要针对静态地下水,保存方法相对宽松;国家标准和美国标准适用范围除了地下水,还包括动态的地表水和废水,采样对象成分更为复杂,更不稳定,更容易受外界影响发生变化,故保存条件高于地质标准。在广州地区,采用原水室温避光保存水样,CODMn、NH+4保存时间可为5天,NO-3保存时间可为30天;采用酸化水室温保存水样,CODMn、NO-3和NH+4保存时间可长达30天。这两种方式均比地质行业标准和国家标准推荐的有效时间长,且原水和酸化水室温保存方式相对于冷藏保存方式更为方便。本文提出,如果采集的水样能方便、快速送达实验室,可采用原水保存;如果不能在短时间内送达实验室检测,可采用硫酸酸化保存。 相似文献
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In order to better understand the compositional and structural complexity of dissolved organic matter (DOM) macromolecules and provide mechanistic information on the binding of hydrophobic organic contaminants (HOCs) to DOM, we fractionated large amounts of lake water into three hydrophobic DOM-fractions. The variation of the partitioning coefficients (K DOC) of pyrene at different pH levels was examined by florescence quenching titration. Results show that, relative to the more polar acidic DOM-fractions, the hydrophobic neutral fraction exhibits a higher sorption ability to pyrene. Generally, the sorption of pyrene to the three hydrophobic fractions is strongly pH-dependent. The K DOC values of pyrene generally increase with decreasing pH levels, which is especially obvious in the sorption of pyrene to the fulvic acid fractions, suggesting that the binding is controlled by hydrophobic interactions. The mechanisms underlying the binding of pyrene to the hydrophobic fractions were also discussed. Our data are beneficial to further understanding the binding of HOCs to DOM and how it has been affected, which may result in more accurate predictions of K DOC. 相似文献
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This work reports the application of thermodynamic models, including equations of state, to binary (salt-free) CH4-H2O fluid inclusions. A general method is presented to calculate the compositions of CH4-H2O inclusions using the phase volume fractions and dissolution temperatures of CH4 hydrate. To calculate the homogenization pressures and isolines of the CH4-H2O inclusions, an improved activity-fugacity model is developed to predict the vapor-liquid phase equilibrium. The phase equilibrium model can predict methane solubility in the liquid phase and water content in the vapor phase from 273 to 623 K and from 1 to 1000 bar (up to 2000 bar for the liquid phase), within or close to experimental uncertainties. Compared to reliable experimental phase equilibrium data, the average deviation of the water content in the vapor phase and methane solubility in the liquid phase is 4.29% and 3.63%, respectively. In the near-critical region, the predicted composition deviations increase to over 10%. The vapor-liquid phase equilibrium model together with the updated volumetric model of homogenous (single-phase) CH4-H2O fluid mixtures (Mao S., Duan Z., Hu J. and Zhang D. (2010) A model for single-phase PVTx properties of CO2-CH4-C2H6-N2-H2O-NaCl fluid mixtures from 273 to 1273 K and from 1 to 5000 bar. Chem. Geol.275, 148-160), is applied to calculate the isolines, homogenization pressures, homogenization volumes, and isochores at specified homogenization temperatures and compositions. Online calculation is on the website: http://www.geochem-model.org/. 相似文献
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Pyromorphite Pb5(PO4)3Cl and mimetite Pb5(AsO4)3Cl are isostructural minerals with apatite. Due to their high environmental stability, they have gained considerable attention as metals sequestration agents in water treatment and contaminated soil remediation. Pyromorphite and mimetite can form a continuous solid solution series in near-Earth surface environments. Precipitation of the end members and intermediate members of the series is likely to occur in the areas where the cost-effective in situ immobilization reclamation method, based on phosphate amendments, is applied. In contrast to the widely studied thermodynamic parameters of pyromorphite and mimetite, knowledge of the thermodynamics of their solid solutions is sparse. To supplement the data, a number of compounds from the pyromorphite-mimetite series were synthesized at room temperature using a method to simulate the conditions in the near-Earth surface environments. Afterwards, batch dissolution and dissolution-recrystallization experiments of seven synthesized precipitates were conducted at 25 °C, pH = 2 and in a 0.05 M KNO3 background electrolyte. The experiments were carried out for a period of 6 (dissolution) and 14 (dissolution-recrystallization) months. A plateau in the [Pb] evolution patterns was used to determine equilibrium. All seven dissolutions were congruent, and the ionic activity products (IAP) of the minerals from the pyromorphite-mimetite solid solution series were calculated based on the dissolution reaction: . The IAPs for pyromorphite and mimetite exhibit a significant difference in values over three orders of magnitude between approximately 10−79 for pyromorphite and approximately 10−76 for mimetite. The series appeared to be ideal, and Lippmann and Roozboom diagrams were used for better understanding of its thermodynamics. The results indicated a strong tendency of pyromorphite to partition into the solid phase in the series, which explains some of the naturally observed phenomena. The improvement of the lattice stability of the mimetite due to isostructural phosphate substitutions in anionic sites was observed. The thermodynamic data reported in this study supplement existing databases used in geochemical modeling. 相似文献
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Zhaosheng Qian Hui Feng Wenjing Yang Yingjie Wang 《Geochimica et cosmochimica acta》2010,74(4):1230-1032
In this paper, the structure of the Al30O8(OH)56(H2O)2618+(Al30) polyoxocation in aqueous solution is investigated, including an exploration of its water-exchange reaction using a supramolecular model. Thirty-one solvent water molecules were explicitly included in the supramolecular model to approximate the influence of the solvent. The calculated results indicated that both the gas-phase and the supramolecular models could correctly reproduce the structure of the Al30 polyoxocation, but the supramolecular model described the structure more accurately. Using the supramolecular model, we calculated the 27Al NMR chemical shifts of various aluminum atoms using HF and GIAO methods, and they compared well to the chemical shifts determined experimentally. The water-exchange reaction of the Al30 polyoxocation could not be simulated with the gas phase model because of a proton-transfer reaction that is induced by the highly positive charge of the Al30 polyoxocation. However, the inclusion of an explicit second solvation sphere lowered the acidity of the coordinated water molecules and allowed simulation of the water exchange reaction. 相似文献
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