滨岸城市大气湿沉降汞的时空分布特征及其物源辨析研究
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摘要
汞作为一种具有生物累积性和放大功能的全球性污染物,即使是在浓度非常低的情况下,它对人类和其它生物都具有相当大的毒性。所有形态的汞都经历着进入大气、形态转化并最终沉降进入水体或陆地生态系统而结束大气循环的过程。大气沉降是水体和陆地生态系统中有毒物质的一个重要来源,大气汞沉降与水生生态系统中鱼类的甲基汞含量具有直接的联系,在年降水日数多、降水量大的地区大气汞的湿沉降是沉降输入的主要类型。目前国外对湿沉降汞的研究较多,而被认为是世界上汞排放量最大的中国在该领域的研究较少,基础薄弱,仅在北京、贵州、长白山等地开展了零星的工作。上海地处长江三角洲东南隅,人口密度大,经济活动强度大,模型模拟显示该地区湿沉降汞的浓度、通量为全球之最；同时上海位于典型东亚季风控制区,存在着冬季风和夏季风的季节性变迁,并且夏季风受西南季风和东南季风交互控制,这造成水汽来源和大气汞输入源的季节性变化,上海又是海陆交互的重要边界带,气溶胶成分变化显著,既有大陆内陆沙尘气溶胶、陆地人类活动排放气溶胶,又有来自海洋的海盐气溶胶,多变的气溶胶成分为大气汞化学形态转化提供了多变的反应界面。因此,以上海市为例研究滨岸城市大气湿沉降汞的时空分布特征及其物源辨析具有重要的意义。
本文通过采集上海市市区、郊区、钢铁工业区、化学工业区和滨岸农业区不同功能区湿沉降样品以及市区和郊区的总沉降样品,分析、测试其中的离子、汞和其它金属元素的含量,理清上海市湿沉降汞的时空分布特征,通过数理统计分析、气流轨迹模型计算和同位素分析的方法对汞的来源进行研究,并对汞的危害进行简要分析,主要得出以下几点结论：
(1)上海市各功能区湿沉降总汞浓度、通量较高。市区、郊区、钢铁工业区、化学工业区和滨岸农业区湿沉降总汞浓度平均值分别为0.33μg·L-1(变化范围为0.06μg·L-1-1.18μg·L-1)、0.23μg·L-1、0.26μg·L-1、0.24μg·L-1、0.29μg·L-1,颗粒态汞占总汞比例分别为：48.5%、57.0%、50.0%、62.2%、64.2%；总汞沉降通量分别为447.67μg·m-2·y-1、233.55μg·m-2·y-1、284.46μg·m-2·y-1、296.97μg·m-2·y-1、296.97μg·m-2·y-1,总汞浓度变化规律分别为：夏季=冬季>秋季>春季、秋季>冬季>夏季=春季、秋季=冬季>春季>夏季、秋季>冬季>春季>夏季、秋季>春季>冬季>夏季。当API指数(空气污染指数)高时,湿沉降中的颗粒态汞浓度增大而溶解态汞浓度降低；湿沉降汞的浓度受降水量的影响不明显,而总汞沉降量与降水量呈现显著正相关关系。云下冲刷对上海市湿沉降中总汞浓度的贡献高于40.9%,局地污染物是湿沉降汞的重要来源之一。
(2)市区总沉降中总汞浓度体积加权平均浓度值为0.51μg·L-1,年沉降通量为654.42μg·m-2·y-1,以湿沉降为主,物质来源的多源性明显。郊区总沉降总汞浓度平均浓度值为0.46μg·L-1,沉降通量为466.77μg·m-2·y-1,干沉降的贡献约为一半,海洋来源对郊区总沉降中汞的贡献较大。市区和郊区总沉降中总汞浓度均为夏季最高,与湿沉降明显不同。不同季节干沉降的来源具有差别,在冬季风影响下,以西北风为主，低温干燥,大气中的活性单质汞被气溶胶粒子吸附反应的几率较小,所以在冬季气溶胶增多的情况下,汞的沉降量仍较低。在夏季风的控制的季节里,东南来源的气溶胶主要是海盐粒子为主,潮湿高温有利于大气活性单质汞在气溶胶表面的吸附反应,从而能够增加汞的沉降。
(3)湿沉降各离子的浓度较高,郊区总离子浓度(847.60μeq·L-1)远高于其它功能区(383.88-437.92μeq·L-1)。不同功能区湿沉降主要离子的体积加权平均值从大到小依次为：SO42->Ca2+>NH4+>Cl->NO3->Na+>Mg2+>F->K+,其中SO42-和Ca2+的浓度之和占总离子浓度的49.77%。离子浓度的时间变化规律Na+：冬季>秋季>春季>夏季,NH4+：春季>秋季>冬季>夏季,其余组分浓度：秋季>冬季>春季>夏季。各离子来源复杂,多源性明显,受人为活动影响严重,总离子组成的76.7%来自人为排放源,其中K+、Mg2+的来源以壳源为主,Na+、Cl-的来源以海源为主,Cl-也有42.2%的贡献来自人为源,Ca2+、NH4+、SO42-、NO3-、F-等组分均为人为排放源占主体。不同功能区各化学组分的浓度值存在较大的差别,但各来源的比例相对于浓度来讲差别较小。
(4)不同功能区各形态汞与其它元素的相关性分析和因子分析结果差异显著,汞可能的来源也有所不同。市区汞的来源是部分地表灰尘、建筑尘埃以及特殊源。郊区汞的来源主要是地壳源和特殊源。钢铁工业区汞的来源有化石燃料燃烧、地表灰尘、建筑尘埃及特殊源。化学工业区汞的来源主要是地表灰尘、建筑尘埃来源和特殊源。滨岸农业区汞的来源可能是特殊源。
(5)上海市市区水汽和低空气团来源在四季存在明显的不同,水汽来源方向：春季方向性不明显,秋季以西-北为主,夏季和冬季均以南-西为主；低空气团来源方向：夏季以东-南为主,春季、秋季和冬季均以北-东为主。湿沉降总汞浓度受水汽来源的影响较大：夏季由于温度高,水-气界面汞的交换通量较大,海盐中丰富的卤素元素能够使单质汞氧化成可溶性的二价汞,所以水汽来源于海域的湿沉降相对于来源于陆地的总汞浓度偏高,且颗粒态汞所占比例较大；其它季节中,大陆水汽蒸发进入雨云中的同时带入当地大气中的汞,水汽来源于内陆且运移距离较长的湿沉降在运移过程中吸收、溶解的气溶胶离子和微量元素较多,导致其湿沉降总汞浓度高、颗粒态汞所占比例小。低空气团的来源对汞的形态分布具有影响,源自海域的低空气团湿沉降中颗粒态汞所占总汞比例较低；低空气团为同一方向,在同时间内运移距离长的湿沉降总汞浓度较大。总汞浓度受降水日数和降水量的影响,当降水量少的时候,云下清除对湿沉降汞的贡献较大,湿沉降事件发生前几天的天气状况影响低空气溶胶的多寡,从而对湿沉降汞具有较大的影响。
(6)上海市区一年中各月δ18O同位素平均值变化范围范围在-12.16--3.00‰之间,年平均值为-8.11‰,春、夏、秋、冬四季的平均值分别为-5.58‰、-10.35‰、-7.45‰和-4.09‰；滨岸农业区各月δ18O同位素变化范围较在-10.66‰-+1.87‰之间,年平均值为-5.16‰。总体上δ18O同位素值呈现春冬高、夏秋低的特征。上海市区湿沉降样品同位素δ18O值与温度具有弱的负相关性,两者之间的关系为：δ18O=-0.20T-2.73；δ18O值存在明显的降水量效应,两者之间的关系式为：δ18O=-0.0603H-3.1841(H为降水量)。
具有相近水汽来源和运移路径的湿沉降中,在到达上海发生湿沉降事件前云团的降水量多少对湿沉降总汞的浓度具有影响,当之前的降水量较大时,同位素δ18O值较低,总汞浓度也较低,反之则相反。水汽携带的汞的多少对湿沉降总汞具有较大的影响,且在湿沉降发生时汞就像重同位素一样优先发生沉降,使后期降水云团中汞的含量减少。水汽来源、运移路径以及到达上海前降水量都基本相同的两次湿沉降水汽携带汞的量基本相同,湿沉降总汞的浓度主要受降水量效应的影响。
(7)水汽来源及路径对湿沉降汞浓度具有显著的控制作用,水汽的海陆来源差异和在相同时间内运移路径的长短均对影响着湿沉降汞浓度值的大小。具有相近水汽来源和运移路径的湿沉降中,在到达上海发生湿沉降事件前云团的降水量多少对湿沉降总汞的浓度具有影响,在湿沉降发生时汞就像重同位素一样优先发生沉降,使后期降水云团中汞的含量减少,所以当之前的降水量较大时,同位素δ18O值较低,总汞浓度也较低,反之则相反。
(8)以我国地表水质Ⅲ类水质(标准极限0.1μg·L-1)为标准,各功能区湿沉降汞的浓度平均值均高于0.1μg·L-1,利用潜在生物危害指数法评价,发现湿沉降汞的平均值均属于强生态危害范围,少数月份属于很强生态危害。通过饮水途径健康危害风险评价,发现市区湿沉降汞的健康危害风险最高而郊区最低；湿沉降汞的健康危害风险远高于上海及其它地区饮用水源地。
Mercury is a highly toxic, persistent and bioaccumulative trace element that is now exits in various environment media and food worldwide. Adversely may be taking place at lower concentrations than previously thought. All forms mercury is all experiencing the circulation of atmosphere with interacting transforming and transporting and ultimate entering waterbody or land ecosystem. In waterbody or land ecosystem, deposition is one of mainly source of toxic substance. It is direct connection in aquatic ecosystem that methyl mercury content in fish body and atmospherec deposition mercury. Atmospheric wet deposition mercury is the primary type at region that have much rainy days and precipitation. Now, wet deposition mercury has been much researched in abroad. China has been considered as the country where mercury emission ranks a maximum. The research is sporadic job in Beijing, Guizhou, Changbai mountain. Shanghai located in southeast in the Yangtze River delta, have large population density and economic activity intensity. The simulation shows that there is the maximum at wet deposition mercury concentration and flue over the world. Shanghai located in typical East Asia monsoon impacting area, where there exits existence seasonal transition for winter monsoon and summer monsoon, southwest monsoon and southeast monsoon interaction control in summer monsoon. Then this bring seasonal characteristic change of atmospheric vapour source and mercury inputs. Shanghai is at the border belt of sea and ground. Aerosol component change are observably. There are continent inland fine sand fling up in the air the aerosol, the aerosol discharging by human being and baysalt aerosol coming from ocean, variable aerosol constituent help atmospheric mercury interacts, transforms at reaction interface.
Wet depositon sample were collected at urban, suburban, steel industrial park, chemistry industrial park and coast agricultural region, sum deposition sample at urban and suburdan in Shanghai. Concentrations of ions, mercury and others elements were measured, and analysis space-time distribution characteristic, and mercury source has been proved by statistivs analyzing, air current trajectory model and isotope analysis, at last analysis the mercury damage on the human. Research distribution and source of atmospheric wet depositon mercury in shore city has importance therefore.
Following results have been acquired:
(1) Wet deposition mercury concentration and fluxes are higher in Shanghai. Wet depositon total mercury volume weighted average concentration at urban, suburban, steel industrial park, chemistry industrial park and coast agricultural region respectively is 0.33μg·L-1 (change range from 0.06μg·L-1 to 1.18μg·L-1),0.23μg·L-1, 0.26μg·L-1, 0.24μg·L-1 and 0.29μg·L-1, ratio of particle mercury accounted for the total mercury of 48.5%,57.0%,50.0%,62.2% and 64.2% concentrationrespectively, total mercury fluxes respectively is 447.67μg·m-2·y-1,233.55μg·m-2·y-1,284.46μg·m-2·y-1, 296.97μg·m-2·y-1 and 296.97μg·m-2·y-1, variation pattern of total mercury respectively is summer=winter>autumn>spring, autumn>winter>summer=spring, autumn=winter> spring>summer, autumn>winter>spring>summer, autumn>spring>winter>summer. Particle mercury concentration is enhancement and dissolve mercury concentration is reduce when API index increas. The correlation of wet deposition concentration and precipitation is unconspicuous, and they are positive correlation of total mercury concentration and precipitation. Wash under cloud take contribution over 40.9% in wet depositon tatal mercury concentration, local contaminant is one of major source in wet deposition mercury.
(2) Total depositon total mercury volume weighted average concentration is 0.51μg·L-1 at urban, and total mercury fluxes is 654.42μg·m-2·y-1, give first place to wet settlement, and the multisource source of matter obviously. Total mercury average concentration is 0.46μg·L-1 at suburban, and total mercury fluxes is 466.77μg·m-2·y-1, dry depositon conruibute half in total depositon, and sea source devoted largly in total depositon at suburban. Total mercury concentration is maximum in summer at urban and suburban, different that of wet depositon obviously. The source of dry deposition have difference, in witer season, north-west is mostly and low temperature and dry, mercury concentration lowly for Hg0 has been adsorbed from aerosol lessly. In summer season, sea salt particles priority to aerosol from south-east. It can add mercury deposition in summer for Hg0 has been adsorbed from aerosol easily in humid and high temperature weather.
(3) Every ions concentration in wet deposition are higher, total ions at suburban (847.60μeq·L-1) more than other functional zone (change range from 383.88μeq·L-1 to 437.92μeq·L-1). Ions volume weighted average concentration from higher to lower respectively is SO42->Ca2+>NH4+>Cl>NO3->Na+>Mg2+>F->K+,the sum concentration of SO42- and Ca2+ accounted for the total ions concentration of 49.77%. Temporal variation pattern of ion Na+ is winter>autumn>spring>summer, NH4+ is spring>autumn>winter>summer, the others ions are autumn>winter>spring>summer. Ions source is complicated and multisource obvious, ions concentration were large affected by artificial disturbance and 76.7% of ions concentration is source form artificial disturbance. In ions, K+, Mg2+ was mostly from land source, and Na+, Cl" was mostly from sea source, and 42.4% of Cl- was anthropogenic source. Ca2+, NH4+, SO42-, NO3- and F" were mostly from anthropogenic source. The concentration of ions in every functional zone exists difference obviously, but the ratio of each ion accounted for the total ions concentration less.
(4) It have different source of the mercury and other elements were identified by correlation and principal component factor analysis. Mercury source part from dust of surface and building, and part from special sources at urban, earthcrust and special at suburban, fossil fuel burning and dust of surface and building and special at steel industrial park, dust of surface and building and special at chemistry industrial park, special source at coast agricultural region.
(5) Source of vapour and low altitude air mass exist difference obviously at all seasons. At vapoure source, no mainly directivity in spring, North-west was mainly in autumn, North-west was mainly in summer and winter. At low altitude air mass, North-east was mainly directivity in summer, and North-east was mainly in the other seasons.
The wet deposition total mercury concentration was obviously influenced by vapour source. Wet depositon mercury concentration that vapour source from sea higher than what from land and particle mercury accounted for the total mercury oppositioned, for higher temperature and higher fluxes of the air-water mercury exchange quantities and Hg0 ready-made Hg2+ easy to be oxidized foe Hg0 chelated with halogen elements. Mercury concentration that vapour source from land with relatively long migration distance higher than that from relatively near sea or relatively shorter migration distance, and particle mercury concentration accounted for the total mercury to reduced, for absorption or dissolved aerosol ions and trace element, local air mercury enter into rain cloud on land more than on sea when vapour evaporation at seasons except for summer. Wet deposition speciation was obviously influenced by low altitude air mass source. Particle mercury concentration accounted for the total mercury that low altitude air mass source from sea lower than land, and total mercury concentration increased when relatively long migration distance at same time and low altitude air mass source from same direction.
Total mercury concentration was influenced by rainy days and precipitation. Wash under cloud take more contribution in mercury concentration when little precipitation. Mercury concentration was influenced by weather conditions the other day because low altitude aerosol interrelated with weather conditions.
(6)Isotopeδ18O ranges from-12.16‰to-3.00‰with season and annual average was-8.11‰at urban. spring, summer, autumn and winter season average respectively-5.58‰,-10.35‰,-7.45‰and-4.09‰at urban. Ranges from-10.66‰to+1.87‰with season and annual average was-5.16‰. Isotopeδ18O variation character was higer at spring and witer, lower at summer and autumn. Isotopeδ18O was negatively correlated with temperature, the line is fitted asδ18O=-0.20T-2.73. the precipitation effect ofδ18O in the precipitation is very pronounced, the line is fitted asδ18O=-0.0603H-3.1841 (H is precipitation)。
The wet deposition total mercury concentration has effected by precipitation that have homology vapour source and transporting before getting to Shanghai. Total mercury concentration and 18O have been reduced when precipitation generous. Be contrary on the contrary. Wet deposition mercury concentration has been effected by mercury of vapour carry-over. Mercury concentration in cloud has decreased at latter atage precipitation for mercury fall off prederential during the period of rain as heavy isotope. Total mercury concentration has been effected by precipitation when vapour source and transporting and precipitation before getting to Shanghai for mercury capacity of vapour carry-over homology.
(7)Wet deposition mercury concentration was controlled prominently by vapour source and transportation ways especially migration distance at same time. Total mercury concentration affected by precipitation before the time when the wet deposition happen on Shanghai in different wet deposition that have same vapour source and transportation ways. Isotopeδ18O and total mercury concentration to reduced when much precipitation happened before the cloud reached Shanghai for mercury as weightly isotope precedence fall when wet deposition happen lead to mercury concentration decrease in cloud.
(8) Each functional zone wet deposition mercury concentration higher than 0.1μg·L-1, sample was estimated by the method of Potential Ecological Risk Index and the earth's surface waterⅢkind standardwas chose as the estimated standard, the result show that wet deposition mercury was heavy degree ecological risk, and few month was significantly heavy degree ecologicl risk. Sample health risks associated with mercury in drinking water was estimated by Health Risks Associated Models, the result show that wet depositon mercury health risk more than drinking water region in Shangh and other areas and the highest risk at urban and lowest at suburban.
本文通过采集上海市市区、郊区、钢铁工业区、化学工业区和滨岸农业区不同功能区湿沉降样品以及市区和郊区的总沉降样品,分析、测试其中的离子、汞和其它金属元素的含量,理清上海市湿沉降汞的时空分布特征,通过数理统计分析、气流轨迹模型计算和同位素分析的方法对汞的来源进行研究,并对汞的危害进行简要分析,主要得出以下几点结论：
(1)上海市各功能区湿沉降总汞浓度、通量较高。市区、郊区、钢铁工业区、化学工业区和滨岸农业区湿沉降总汞浓度平均值分别为0.33μg·L-1(变化范围为0.06μg·L-1-1.18μg·L-1)、0.23μg·L-1、0.26μg·L-1、0.24μg·L-1、0.29μg·L-1,颗粒态汞占总汞比例分别为：48.5%、57.0%、50.0%、62.2%、64.2%；总汞沉降通量分别为447.67μg·m-2·y-1、233.55μg·m-2·y-1、284.46μg·m-2·y-1、296.97μg·m-2·y-1、296.97μg·m-2·y-1,总汞浓度变化规律分别为：夏季=冬季>秋季>春季、秋季>冬季>夏季=春季、秋季=冬季>春季>夏季、秋季>冬季>春季>夏季、秋季>春季>冬季>夏季。当API指数(空气污染指数)高时,湿沉降中的颗粒态汞浓度增大而溶解态汞浓度降低；湿沉降汞的浓度受降水量的影响不明显,而总汞沉降量与降水量呈现显著正相关关系。云下冲刷对上海市湿沉降中总汞浓度的贡献高于40.9%,局地污染物是湿沉降汞的重要来源之一。
(2)市区总沉降中总汞浓度体积加权平均浓度值为0.51μg·L-1,年沉降通量为654.42μg·m-2·y-1,以湿沉降为主,物质来源的多源性明显。郊区总沉降总汞浓度平均浓度值为0.46μg·L-1,沉降通量为466.77μg·m-2·y-1,干沉降的贡献约为一半,海洋来源对郊区总沉降中汞的贡献较大。市区和郊区总沉降中总汞浓度均为夏季最高,与湿沉降明显不同。不同季节干沉降的来源具有差别,在冬季风影响下,以西北风为主，低温干燥,大气中的活性单质汞被气溶胶粒子吸附反应的几率较小,所以在冬季气溶胶增多的情况下,汞的沉降量仍较低。在夏季风的控制的季节里,东南来源的气溶胶主要是海盐粒子为主,潮湿高温有利于大气活性单质汞在气溶胶表面的吸附反应,从而能够增加汞的沉降。
(3)湿沉降各离子的浓度较高,郊区总离子浓度(847.60μeq·L-1)远高于其它功能区(383.88-437.92μeq·L-1)。不同功能区湿沉降主要离子的体积加权平均值从大到小依次为：SO42->Ca2+>NH4+>Cl->NO3->Na+>Mg2+>F->K+,其中SO42-和Ca2+的浓度之和占总离子浓度的49.77%。离子浓度的时间变化规律Na+：冬季>秋季>春季>夏季,NH4+：春季>秋季>冬季>夏季,其余组分浓度：秋季>冬季>春季>夏季。各离子来源复杂,多源性明显,受人为活动影响严重,总离子组成的76.7%来自人为排放源,其中K+、Mg2+的来源以壳源为主,Na+、Cl-的来源以海源为主,Cl-也有42.2%的贡献来自人为源,Ca2+、NH4+、SO42-、NO3-、F-等组分均为人为排放源占主体。不同功能区各化学组分的浓度值存在较大的差别,但各来源的比例相对于浓度来讲差别较小。
(4)不同功能区各形态汞与其它元素的相关性分析和因子分析结果差异显著,汞可能的来源也有所不同。市区汞的来源是部分地表灰尘、建筑尘埃以及特殊源。郊区汞的来源主要是地壳源和特殊源。钢铁工业区汞的来源有化石燃料燃烧、地表灰尘、建筑尘埃及特殊源。化学工业区汞的来源主要是地表灰尘、建筑尘埃来源和特殊源。滨岸农业区汞的来源可能是特殊源。
(5)上海市市区水汽和低空气团来源在四季存在明显的不同,水汽来源方向：春季方向性不明显,秋季以西-北为主,夏季和冬季均以南-西为主；低空气团来源方向：夏季以东-南为主,春季、秋季和冬季均以北-东为主。湿沉降总汞浓度受水汽来源的影响较大：夏季由于温度高,水-气界面汞的交换通量较大,海盐中丰富的卤素元素能够使单质汞氧化成可溶性的二价汞,所以水汽来源于海域的湿沉降相对于来源于陆地的总汞浓度偏高,且颗粒态汞所占比例较大；其它季节中,大陆水汽蒸发进入雨云中的同时带入当地大气中的汞,水汽来源于内陆且运移距离较长的湿沉降在运移过程中吸收、溶解的气溶胶离子和微量元素较多,导致其湿沉降总汞浓度高、颗粒态汞所占比例小。低空气团的来源对汞的形态分布具有影响,源自海域的低空气团湿沉降中颗粒态汞所占总汞比例较低；低空气团为同一方向,在同时间内运移距离长的湿沉降总汞浓度较大。总汞浓度受降水日数和降水量的影响,当降水量少的时候,云下清除对湿沉降汞的贡献较大,湿沉降事件发生前几天的天气状况影响低空气溶胶的多寡,从而对湿沉降汞具有较大的影响。
(6)上海市区一年中各月δ18O同位素平均值变化范围范围在-12.16--3.00‰之间,年平均值为-8.11‰,春、夏、秋、冬四季的平均值分别为-5.58‰、-10.35‰、-7.45‰和-4.09‰；滨岸农业区各月δ18O同位素变化范围较在-10.66‰-+1.87‰之间,年平均值为-5.16‰。总体上δ18O同位素值呈现春冬高、夏秋低的特征。上海市区湿沉降样品同位素δ18O值与温度具有弱的负相关性,两者之间的关系为：δ18O=-0.20T-2.73；δ18O值存在明显的降水量效应,两者之间的关系式为：δ18O=-0.0603H-3.1841(H为降水量)。
具有相近水汽来源和运移路径的湿沉降中,在到达上海发生湿沉降事件前云团的降水量多少对湿沉降总汞的浓度具有影响,当之前的降水量较大时,同位素δ18O值较低,总汞浓度也较低,反之则相反。水汽携带的汞的多少对湿沉降总汞具有较大的影响,且在湿沉降发生时汞就像重同位素一样优先发生沉降,使后期降水云团中汞的含量减少。水汽来源、运移路径以及到达上海前降水量都基本相同的两次湿沉降水汽携带汞的量基本相同,湿沉降总汞的浓度主要受降水量效应的影响。
(7)水汽来源及路径对湿沉降汞浓度具有显著的控制作用,水汽的海陆来源差异和在相同时间内运移路径的长短均对影响着湿沉降汞浓度值的大小。具有相近水汽来源和运移路径的湿沉降中,在到达上海发生湿沉降事件前云团的降水量多少对湿沉降总汞的浓度具有影响,在湿沉降发生时汞就像重同位素一样优先发生沉降,使后期降水云团中汞的含量减少,所以当之前的降水量较大时,同位素δ18O值较低,总汞浓度也较低,反之则相反。
(8)以我国地表水质Ⅲ类水质(标准极限0.1μg·L-1)为标准,各功能区湿沉降汞的浓度平均值均高于0.1μg·L-1,利用潜在生物危害指数法评价,发现湿沉降汞的平均值均属于强生态危害范围,少数月份属于很强生态危害。通过饮水途径健康危害风险评价,发现市区湿沉降汞的健康危害风险最高而郊区最低；湿沉降汞的健康危害风险远高于上海及其它地区饮用水源地。
Mercury is a highly toxic, persistent and bioaccumulative trace element that is now exits in various environment media and food worldwide. Adversely may be taking place at lower concentrations than previously thought. All forms mercury is all experiencing the circulation of atmosphere with interacting transforming and transporting and ultimate entering waterbody or land ecosystem. In waterbody or land ecosystem, deposition is one of mainly source of toxic substance. It is direct connection in aquatic ecosystem that methyl mercury content in fish body and atmospherec deposition mercury. Atmospheric wet deposition mercury is the primary type at region that have much rainy days and precipitation. Now, wet deposition mercury has been much researched in abroad. China has been considered as the country where mercury emission ranks a maximum. The research is sporadic job in Beijing, Guizhou, Changbai mountain. Shanghai located in southeast in the Yangtze River delta, have large population density and economic activity intensity. The simulation shows that there is the maximum at wet deposition mercury concentration and flue over the world. Shanghai located in typical East Asia monsoon impacting area, where there exits existence seasonal transition for winter monsoon and summer monsoon, southwest monsoon and southeast monsoon interaction control in summer monsoon. Then this bring seasonal characteristic change of atmospheric vapour source and mercury inputs. Shanghai is at the border belt of sea and ground. Aerosol component change are observably. There are continent inland fine sand fling up in the air the aerosol, the aerosol discharging by human being and baysalt aerosol coming from ocean, variable aerosol constituent help atmospheric mercury interacts, transforms at reaction interface.
Wet depositon sample were collected at urban, suburban, steel industrial park, chemistry industrial park and coast agricultural region, sum deposition sample at urban and suburdan in Shanghai. Concentrations of ions, mercury and others elements were measured, and analysis space-time distribution characteristic, and mercury source has been proved by statistivs analyzing, air current trajectory model and isotope analysis, at last analysis the mercury damage on the human. Research distribution and source of atmospheric wet depositon mercury in shore city has importance therefore.
Following results have been acquired:
(1) Wet deposition mercury concentration and fluxes are higher in Shanghai. Wet depositon total mercury volume weighted average concentration at urban, suburban, steel industrial park, chemistry industrial park and coast agricultural region respectively is 0.33μg·L-1 (change range from 0.06μg·L-1 to 1.18μg·L-1),0.23μg·L-1, 0.26μg·L-1, 0.24μg·L-1 and 0.29μg·L-1, ratio of particle mercury accounted for the total mercury of 48.5%,57.0%,50.0%,62.2% and 64.2% concentrationrespectively, total mercury fluxes respectively is 447.67μg·m-2·y-1,233.55μg·m-2·y-1,284.46μg·m-2·y-1, 296.97μg·m-2·y-1 and 296.97μg·m-2·y-1, variation pattern of total mercury respectively is summer=winter>autumn>spring, autumn>winter>summer=spring, autumn=winter> spring>summer, autumn>winter>spring>summer, autumn>spring>winter>summer. Particle mercury concentration is enhancement and dissolve mercury concentration is reduce when API index increas. The correlation of wet deposition concentration and precipitation is unconspicuous, and they are positive correlation of total mercury concentration and precipitation. Wash under cloud take contribution over 40.9% in wet depositon tatal mercury concentration, local contaminant is one of major source in wet deposition mercury.
(2) Total depositon total mercury volume weighted average concentration is 0.51μg·L-1 at urban, and total mercury fluxes is 654.42μg·m-2·y-1, give first place to wet settlement, and the multisource source of matter obviously. Total mercury average concentration is 0.46μg·L-1 at suburban, and total mercury fluxes is 466.77μg·m-2·y-1, dry depositon conruibute half in total depositon, and sea source devoted largly in total depositon at suburban. Total mercury concentration is maximum in summer at urban and suburban, different that of wet depositon obviously. The source of dry deposition have difference, in witer season, north-west is mostly and low temperature and dry, mercury concentration lowly for Hg0 has been adsorbed from aerosol lessly. In summer season, sea salt particles priority to aerosol from south-east. It can add mercury deposition in summer for Hg0 has been adsorbed from aerosol easily in humid and high temperature weather.
(3) Every ions concentration in wet deposition are higher, total ions at suburban (847.60μeq·L-1) more than other functional zone (change range from 383.88μeq·L-1 to 437.92μeq·L-1). Ions volume weighted average concentration from higher to lower respectively is SO42->Ca2+>NH4+>Cl>NO3->Na+>Mg2+>F->K+,the sum concentration of SO42- and Ca2+ accounted for the total ions concentration of 49.77%. Temporal variation pattern of ion Na+ is winter>autumn>spring>summer, NH4+ is spring>autumn>winter>summer, the others ions are autumn>winter>spring>summer. Ions source is complicated and multisource obvious, ions concentration were large affected by artificial disturbance and 76.7% of ions concentration is source form artificial disturbance. In ions, K+, Mg2+ was mostly from land source, and Na+, Cl" was mostly from sea source, and 42.4% of Cl- was anthropogenic source. Ca2+, NH4+, SO42-, NO3- and F" were mostly from anthropogenic source. The concentration of ions in every functional zone exists difference obviously, but the ratio of each ion accounted for the total ions concentration less.
(4) It have different source of the mercury and other elements were identified by correlation and principal component factor analysis. Mercury source part from dust of surface and building, and part from special sources at urban, earthcrust and special at suburban, fossil fuel burning and dust of surface and building and special at steel industrial park, dust of surface and building and special at chemistry industrial park, special source at coast agricultural region.
(5) Source of vapour and low altitude air mass exist difference obviously at all seasons. At vapoure source, no mainly directivity in spring, North-west was mainly in autumn, North-west was mainly in summer and winter. At low altitude air mass, North-east was mainly directivity in summer, and North-east was mainly in the other seasons.
The wet deposition total mercury concentration was obviously influenced by vapour source. Wet depositon mercury concentration that vapour source from sea higher than what from land and particle mercury accounted for the total mercury oppositioned, for higher temperature and higher fluxes of the air-water mercury exchange quantities and Hg0 ready-made Hg2+ easy to be oxidized foe Hg0 chelated with halogen elements. Mercury concentration that vapour source from land with relatively long migration distance higher than that from relatively near sea or relatively shorter migration distance, and particle mercury concentration accounted for the total mercury to reduced, for absorption or dissolved aerosol ions and trace element, local air mercury enter into rain cloud on land more than on sea when vapour evaporation at seasons except for summer. Wet deposition speciation was obviously influenced by low altitude air mass source. Particle mercury concentration accounted for the total mercury that low altitude air mass source from sea lower than land, and total mercury concentration increased when relatively long migration distance at same time and low altitude air mass source from same direction.
Total mercury concentration was influenced by rainy days and precipitation. Wash under cloud take more contribution in mercury concentration when little precipitation. Mercury concentration was influenced by weather conditions the other day because low altitude aerosol interrelated with weather conditions.
(6)Isotopeδ18O ranges from-12.16‰to-3.00‰with season and annual average was-8.11‰at urban. spring, summer, autumn and winter season average respectively-5.58‰,-10.35‰,-7.45‰and-4.09‰at urban. Ranges from-10.66‰to+1.87‰with season and annual average was-5.16‰. Isotopeδ18O variation character was higer at spring and witer, lower at summer and autumn. Isotopeδ18O was negatively correlated with temperature, the line is fitted asδ18O=-0.20T-2.73. the precipitation effect ofδ18O in the precipitation is very pronounced, the line is fitted asδ18O=-0.0603H-3.1841 (H is precipitation)。
The wet deposition total mercury concentration has effected by precipitation that have homology vapour source and transporting before getting to Shanghai. Total mercury concentration and 18O have been reduced when precipitation generous. Be contrary on the contrary. Wet deposition mercury concentration has been effected by mercury of vapour carry-over. Mercury concentration in cloud has decreased at latter atage precipitation for mercury fall off prederential during the period of rain as heavy isotope. Total mercury concentration has been effected by precipitation when vapour source and transporting and precipitation before getting to Shanghai for mercury capacity of vapour carry-over homology.
(7)Wet deposition mercury concentration was controlled prominently by vapour source and transportation ways especially migration distance at same time. Total mercury concentration affected by precipitation before the time when the wet deposition happen on Shanghai in different wet deposition that have same vapour source and transportation ways. Isotopeδ18O and total mercury concentration to reduced when much precipitation happened before the cloud reached Shanghai for mercury as weightly isotope precedence fall when wet deposition happen lead to mercury concentration decrease in cloud.
(8) Each functional zone wet deposition mercury concentration higher than 0.1μg·L-1, sample was estimated by the method of Potential Ecological Risk Index and the earth's surface waterⅢkind standardwas chose as the estimated standard, the result show that wet deposition mercury was heavy degree ecological risk, and few month was significantly heavy degree ecologicl risk. Sample health risks associated with mercury in drinking water was estimated by Health Risks Associated Models, the result show that wet depositon mercury health risk more than drinking water region in Shangh and other areas and the highest risk at urban and lowest at suburban.
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