多环芳烃在黄浦江水体的分布特征及吸附机理研究
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摘要
多环芳烃作为一种典型有毒有机化合物，具有持久性、难降解性和一定毒性，在环境中广泛分布。典型水体中多环芳烃的分布规律研究和迁移途径研究是当今环境科学领域研究的热点和难点。本研究以低分子量多环芳烃(LMW PAHs)为研究对象，建立一种高效灵敏、适合于水中痕量PAHs富集分析的方法，研究黄浦江流域PAHs的赋存状态和时空分布特征，分析以菲为代表的疏水性有机污染物在水／沉积物(腐殖酸)的吸附过程和吸附机制，揭示有机污染物在水环境中的存在、分布、迁移和归宿，以丰富和完善学科理论体系，为污染物控制技术研究和环境质量标准制定提供科学决策依据。
论文建立了适用于饮用水、饮用水源水和地表水等环境水样中痕量LMW PAHs富集分析的离线和在线SPE-HPLC法，并对两种方法进行了比较，结果表明；①离线固相萃取的优化条件为：水样体积为500mL，5mL四氢呋喃为洗脱溶剂，加入10％的甲醇作为有机改性剂；离线法对水样中LMW PAHs的回收率分别为95.22％-100.8％，相对标准偏差(RSD)为0.78％～6.68％，检测下限达0.06-0.24ng／L。②在线SPE-HPLC法测定LMW PAHs的优化条件为：C_(18)作为在线固相萃取柱吸附剂，液相流动相(乙腈：水=75：25)直接洗脱富集的多环芳烃，流速控制在5mL／min，在线萃取水样体积为25mL；在线法对水中痕量PAHs的回收率在92.98％～102.6％，相对标准偏差(RSD)为0.820％～5.76％，检测下限达0.01～0.13ng／L。③比较研究表明：在线SPE-HPLC法较离线法操作简便，工作效率增强，精密度和准确度提高，方法更为灵敏可靠，且对环境友好，可作为一般离线固相萃取法的替代方法，适合于水中痕量有机污染物的富集分析。
通过对上海市黄浦江8个断面表层水体中LMW PAHs为期1年的跟踪研究表明：①黄浦江表层水体中均有萘、芴、菲和蒽检出，平均浓度分别为60.79ng／L，50.90ng／L，35.17ng／L和7.64ng／L。相比较而言，黄浦江水体中LMW PAHs的含量在国内外河流中处于中等水平。②从空间分布特征上看，黄浦江水体PAHs浓度从上游到下游呈明显上升趋势，中下游段自徐浦大桥断面逐渐上升，到外滩断面达最高，进入吴淞口断面略有下降，这一空间分布特征与上海市工农业布局和城市分布存在一定的相关性。③从时间变化特征上看，监测期间4种
As a typical persistent organic pollutant (POPs), polycyclic aromatic hydrocarbons (PAHs) bearing the properties of persistent existence in the environment, refractory to degradation and noxious to living bodies is widely spread in the environment. The study on PAHs distribution character and transfer mechanism in typical aquatic environment is one of the difficulties and hotspots in environmental science research. This paper focused on the serious problem of POPs and studied the representative POPs, low molecular weight PAHs (LMW PAHs). Special research was conducted on the development of pre-treatment and analysis methods for LMW PAHs in aquatic environment, LMW PAHs distribution characters in Huangpu River, and the sorption process and mechanism of phenanthrene, a typical hydrophobic compound, between water and sediment (or humic acid) interface to uncover the existence, distribution, transfer and fate of POPs in aquatic environment which was developed for the study on POPs pollution control and the foundation of relevant environmental law making.
This paper developed off-line and on-line methods of solid phase extraction and high performance liquid chromatography (SPE-HPLC) for LMW PAHs in ultra-trace level of drinking water and surface water and compared the two methods, the results were stated as follows: ① The optimal conditions for off-line SPE method were: 10% methanol added in 500mL water sample as solvent conditioner, eluting solvent was tetradrofuran, amount of eluting solvent was 5mL with the average recoveries of off-line SPE method for LMW PAHs among 95.22% to 100.8%, relative standard deviations (RSD) among 0.78% to 6.68% and method detection limits ranged from 0.06ng/L to 0.24ng/L. ② The optimal conditions for on-line SPE method were: C_(18) as the on-line SPE column for the enrichment of PAHs in 25mL water sample, isocratic elution of 75:25 acetonitrile to water as mobile phase with 5mL/min flow rate with the average recoveries of on-line SPE-HPLC method for LMW PAHs among 92.98% to 102.6%, RSD among 0.82% to 5.76% and detection limits ranged from 0.01ng/L to 0.13ng/L. (3) Comparison results showed that with the improvement of convenience,
论文建立了适用于饮用水、饮用水源水和地表水等环境水样中痕量LMW PAHs富集分析的离线和在线SPE-HPLC法，并对两种方法进行了比较，结果表明；①离线固相萃取的优化条件为：水样体积为500mL，5mL四氢呋喃为洗脱溶剂，加入10％的甲醇作为有机改性剂；离线法对水样中LMW PAHs的回收率分别为95.22％-100.8％，相对标准偏差(RSD)为0.78％～6.68％，检测下限达0.06-0.24ng／L。②在线SPE-HPLC法测定LMW PAHs的优化条件为：C_(18)作为在线固相萃取柱吸附剂，液相流动相(乙腈：水=75：25)直接洗脱富集的多环芳烃，流速控制在5mL／min，在线萃取水样体积为25mL；在线法对水中痕量PAHs的回收率在92.98％～102.6％，相对标准偏差(RSD)为0.820％～5.76％，检测下限达0.01～0.13ng／L。③比较研究表明：在线SPE-HPLC法较离线法操作简便，工作效率增强，精密度和准确度提高，方法更为灵敏可靠，且对环境友好，可作为一般离线固相萃取法的替代方法，适合于水中痕量有机污染物的富集分析。
通过对上海市黄浦江8个断面表层水体中LMW PAHs为期1年的跟踪研究表明：①黄浦江表层水体中均有萘、芴、菲和蒽检出，平均浓度分别为60.79ng／L，50.90ng／L，35.17ng／L和7.64ng／L。相比较而言，黄浦江水体中LMW PAHs的含量在国内外河流中处于中等水平。②从空间分布特征上看，黄浦江水体PAHs浓度从上游到下游呈明显上升趋势，中下游段自徐浦大桥断面逐渐上升，到外滩断面达最高，进入吴淞口断面略有下降，这一空间分布特征与上海市工农业布局和城市分布存在一定的相关性。③从时间变化特征上看，监测期间4种
As a typical persistent organic pollutant (POPs), polycyclic aromatic hydrocarbons (PAHs) bearing the properties of persistent existence in the environment, refractory to degradation and noxious to living bodies is widely spread in the environment. The study on PAHs distribution character and transfer mechanism in typical aquatic environment is one of the difficulties and hotspots in environmental science research. This paper focused on the serious problem of POPs and studied the representative POPs, low molecular weight PAHs (LMW PAHs). Special research was conducted on the development of pre-treatment and analysis methods for LMW PAHs in aquatic environment, LMW PAHs distribution characters in Huangpu River, and the sorption process and mechanism of phenanthrene, a typical hydrophobic compound, between water and sediment (or humic acid) interface to uncover the existence, distribution, transfer and fate of POPs in aquatic environment which was developed for the study on POPs pollution control and the foundation of relevant environmental law making.
This paper developed off-line and on-line methods of solid phase extraction and high performance liquid chromatography (SPE-HPLC) for LMW PAHs in ultra-trace level of drinking water and surface water and compared the two methods, the results were stated as follows: ① The optimal conditions for off-line SPE method were: 10% methanol added in 500mL water sample as solvent conditioner, eluting solvent was tetradrofuran, amount of eluting solvent was 5mL with the average recoveries of off-line SPE method for LMW PAHs among 95.22% to 100.8%, relative standard deviations (RSD) among 0.78% to 6.68% and method detection limits ranged from 0.06ng/L to 0.24ng/L. ② The optimal conditions for on-line SPE method were: C_(18) as the on-line SPE column for the enrichment of PAHs in 25mL water sample, isocratic elution of 75:25 acetonitrile to water as mobile phase with 5mL/min flow rate with the average recoveries of on-line SPE-HPLC method for LMW PAHs among 92.98% to 102.6%, RSD among 0.82% to 5.76% and detection limits ranged from 0.01ng/L to 0.13ng/L. (3) Comparison results showed that with the improvement of convenience,
引文
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