汞矿区中汞和大气中重金属污染的评估
摘要
本论文包括两个部分。第一部分为绪论,介绍了汞的性质、主要用途和汞污染来源,概述了汞环境污染现状、汞污染对人类健康的危害与汞污染防治,评述了汞分析方法研究的进展。第二部分为研究报告,研究了旬阳汞矿区域内水样、土壤样品、沉积物样品和植物样品中汞的分布,测定了旬阳汞矿区域水样中溶解汞和颗粒汞的含量,探讨了汞在炼汞地区环境中迁移、转化和富集的环境地球环境化学行为和规律。同时测定了多伦多市和耶罗纳夫市大气湿沉降中重金属及甲基汞含量,比较两城市间重金属含量及甲基汞所占汞含量比例。
本文选择陕西旬阳汞矿区作为地区研究对象,主要是考虑到旬阳汞矿是一处仍然在运行的汞矿,比起其它已经关闭的汞矿更具有研究意思。论文研究了受采矿活动影响后,该地区河流、土壤、沉积物以及植物中的总汞分布,以及河流中存在的其它形态汞的含量;同时探讨了汞在植物中的迁移富集行为,揭示了该地区植物受到采矿活动的影响。此外,还研究了汞和其他重金属之间的关系,揭示了汞污染与其它重金属污染伴随的情况。同时测定了Toronto市和Yellowknife市大气湿沉降中重金属及甲基汞含量,比较两城市间重金属含量及甲基汞所占汞含量比例。通过详细研究,本论文主要得出以下结论:
1)旬阳汞矿区域河流中总汞含量处在0.12-25.57μg L~(-1)范围内,平均浓度为6.35μg L~(-1),其中颗粒汞浓度较高,平均值为2.08μg L~(-1),占总汞含量50%以上(平均值为64%)。说明在该地区颗粒汞是受汞污染水体的主要形态传输途径。通过测定一系列采用点水样,发现水体中总汞含量随距离汞矿距离呈现一定的变化规律:①在公馆区域中,水中总汞含量随距离公馆汞矿距离的增加呈现先下降后上升的趋势;②在青铜沟区域,水中总汞含量随距离青铜沟距离的增加呈现一直下降的趋势。
2)旬阳汞矿区域采集的土壤样品中总汞含量在1.3-752.1 mg kg~(-1)范围中,平均含量为106.6 mg kg~(-1)。5号和12号采样点所采集土壤中含汞量比较高,分别为518 mg kg~(-1)和752.1 mgkg~(-1),这是由于这两个采样点距离汞矿很近,5号采样点距公馆汞矿较近,而12号采样点距青铜沟汞矿较近。因此我们可以认为如此高的汞含量可能是由于以下两个原因造成的:其一,是由于处于矿区本身地壤中汞含量较高;其二是由于炼汞厂排放大量的汞进入大气中,其中一部分沉降到土壤中。土壤中汞含量随距离汞矿距离变化趋势呈现出与在河流中相似的规律。在研究土壤中汞含量纵向变化中发现,汞含量随着垂直距离的加深呈现递减的趋势。
3)旬阳汞矿区域中采集的沉积物中总汞含量在59.7-2100 mg kg~(-1)范围中,平均值为580mg kg~(-1),这一值远远高于报道的背景区域中采集的沉积物的汞含量,由于沉积物受流水的搅动较小,其汞较易沉积下来,造成了沉积物中汞含量远远高于河流中汞含量。研究表明,沉积物中汞含量量随距离汞矿距离变化趋势呈现出与在河流、土壤中相似的规律。
4)旬阳汞矿区域中采集的植物样品(白菜和小麦苗)总汞含量在58-5370 ng g~(-1)(湿重)范围中变化,其平均值为1163 ng g~(-1)。根部和叶部总汞含量分别为62-4210 ng g~(-1)和58-3420 ngg~(-1),且根部中汞含量大于叶部中汞含量。在该地区采集的植物样品总汞含量远远大于中国国家食品标准机构所允许的最大汞含量20 ng g~(-1)。这说明了该地区的植物明显受到汞污染。根据FTt分析可知,汞的迁移形式是从土壤到根部再到叶部。
5)在对水样、土样和沉积物样品中其它重金属(Se,Pb,Sb)分析后发现,汞和这些元素存在一定的相关性,随着汞含量的增加这些元素的含量也呈现增加的趋势。在水样中,这些重金属和汞表现出良好的相关性,而在沉积物中只有Sb和汞表现出一定的相关性。这说明该地区其他重金属含量受到炼汞活动的影响。
6)在对Toronto市和Yellowknife市大气湿沉降(雨水和雪)中重金属和甲基汞含量分析中发现,雨水中重金属含量普遍高于雪中重金属含量,其中Al,Fe,Pb,Cu,Zn在大气中的含量明显高于其他元素;雨水中甲基汞所占比例较雪中甲基汞所占比例高。通过与其他城市大气中重金属含量比较发现,Toronto市和Yellowknife市大气中重金属污染并不严重。
This thesis includes two parts:a review and a research report.
In the first part,the characteristics and applications of mercury and the sources of mercury pollution were introduced.The status and prevention of mercury pollution and the effects of mercury on human health were reviewed.The development in analytical methods of total mercury was extensively presented.
In the second part,a mercury mine in Xunyang County in Shaanxi Province,the largest mercury mine currently in operation in China,was selected as a case for the study.The concentrations and distributions of mercury species were studied in surface water,soil,sediment and plants(cabbage and wheat seedling) in the region affected by mercury mining activities.The environmental geochemistry behaviors and modes of transport,transformation,and enrichment of mercury in mercury mining environments were thoroughly discussed.The behaviors and modes of transport and enrichment of mercury in plants are also discussed.The data obtained indicate that the plants which grow in the region are contaminated by mercury mining.In addition,the relationship between mercury and other metals was studied.The results indicate that the contamination of mercury is accompanied by the contamination of other metals.The concentration of heavy metals and methyl mercury in wet deposition(rain and snow) was determined.Compare the percentage of methyl mercury in rain and snow samples between city of Toronto and Yellowknife.The main conclusions are as follows:
1.In Xunyang mercury mining area,the total mercury concentration in surface water ranged from 0.12 to 25.57μg L~(-1),with the average value of 2.08μg L~(-1) and the particulate mercury typically exceeded 50%(with the average of 64%) of total mercury in the stream water.This indicates that the main transportation of mercury was performed by particulate mercury in surface water.The result showed that the concentration of total mercury dropped sharply in several kilometres from the Gongguan furnace,climbed when approaching the Qingtonggou furnace;decreased rapidly with increasing distance from the Qingtonggou mining and smelting location.
2.The total mercury contents in soil samples collected from Xunyang mercury mining area ranged from 1.3 to 752.1 mg kg~(-1),with the average value of 106.6 mg kg~(-1).The most contaminated sites appeared at sites No.5 and No.12 with the values of 518 mg kg~(-1) and 752.1 mg kg~(-1), respectively.It was attrubited the fact that site No.5 was closed to Gongguan melting furnace and site No.12 was closed to Qinggonggou melting furnace.The total mercury content in soil samples was attrubited to two factors.The first one was the high mercury contents in local soil.The second one was that the mercury released from mercury smelting furnace could get into atmosphere and then a part of mercury could deposit to the soil in the area.Similar as in surface water,the total mercury contents in soil dropped first and then climbed in Gongguan area and decreased with an increase of the distance from the Qingtonggou mercury smelting furnace in Qingtonggou area.It was clearly seen that the mercury contents decreased with an increase of vertical depth at sites No.1 and No.22.
3.In the Xunyang mercury mining area,the total mercury contents in sediment ranged from 59.7 to 2100 mg kg~(-1),with the average value of 580 mg kg~(-1),which was much higher than the mercury value from background area.It was attrubited the fact that the mercury easily deposited into sediment.The distribution of mercury content in sediment showed the similar tendency as in surface water and soil.
4.The total mercury contents in plants(cabbage and wheat seedling) samples collected from Xunyang mining area ranged from 58-5370 ng g~(-1)(wet weight) with an average value of 1163 ng g~(-1).The total mercury contents in the roots and leaves samples ranged from 62 to 4210 ng g~(-1) and 58 to 3420 ng g~(-1),respectively.The mercury levels in root were generally higher than those in leaf. These values were much higher than the maximum value of 20 ng g~(-1) recommended by the Chinese National Agency for food sources.It indicated that the plants(cabbage and wheat seedling) were significantly contaminated by mercury mining activities.The Fit values suggested that mercury translocation into the plants from roots to aerial part occurred and the mercury source was mainly derived from soil rather than atmosphere.
5.The contents of other metals(Se,Pb,Sb) in surface water,soil and sediment samples showed a common lithological correlation with mercury.There are positive correlations between mercury and other metals in surface water,rather than in sediments.It was found there was only a strong tight correlation between the contents of mercury and Sb.It indicated that the activities of mining affected the contents of other metals in this study area.Actions should be taken to clean the contaminated riverbed,manage waste discharges,and reduce the exposure of mercury to the local residents by issuing advisory for consuming the agricultural products grown in the area.
6.The contents of heavy metals including Cd,Fe,Mn,Ni,Pb,T1,Zn,Co,Cu,Hg and Al in wet deposition(rain and snow) in Toronto and Yellowknife,Cannada,showed that the contents of heavy metals in rain samples were much higher than that in snow samples.The contents of Al,Fe, Pb,Cu,Zn were much higher than that of others such as Cd,Mn,Ni,T1,Co,Hg in both rain and snow samples.The percentage of methyl mercury in rain samples was higher than that in snow samples in Toronto and Yellowknife.The contamination of heavy metals in atomosphere in both Toronto and Yellowknife cities was not serious compared with other cities.
本文选择陕西旬阳汞矿区作为地区研究对象,主要是考虑到旬阳汞矿是一处仍然在运行的汞矿,比起其它已经关闭的汞矿更具有研究意思。论文研究了受采矿活动影响后,该地区河流、土壤、沉积物以及植物中的总汞分布,以及河流中存在的其它形态汞的含量;同时探讨了汞在植物中的迁移富集行为,揭示了该地区植物受到采矿活动的影响。此外,还研究了汞和其他重金属之间的关系,揭示了汞污染与其它重金属污染伴随的情况。同时测定了Toronto市和Yellowknife市大气湿沉降中重金属及甲基汞含量,比较两城市间重金属含量及甲基汞所占汞含量比例。通过详细研究,本论文主要得出以下结论:
1)旬阳汞矿区域河流中总汞含量处在0.12-25.57μg L~(-1)范围内,平均浓度为6.35μg L~(-1),其中颗粒汞浓度较高,平均值为2.08μg L~(-1),占总汞含量50%以上(平均值为64%)。说明在该地区颗粒汞是受汞污染水体的主要形态传输途径。通过测定一系列采用点水样,发现水体中总汞含量随距离汞矿距离呈现一定的变化规律:①在公馆区域中,水中总汞含量随距离公馆汞矿距离的增加呈现先下降后上升的趋势;②在青铜沟区域,水中总汞含量随距离青铜沟距离的增加呈现一直下降的趋势。
2)旬阳汞矿区域采集的土壤样品中总汞含量在1.3-752.1 mg kg~(-1)范围中,平均含量为106.6 mg kg~(-1)。5号和12号采样点所采集土壤中含汞量比较高,分别为518 mg kg~(-1)和752.1 mgkg~(-1),这是由于这两个采样点距离汞矿很近,5号采样点距公馆汞矿较近,而12号采样点距青铜沟汞矿较近。因此我们可以认为如此高的汞含量可能是由于以下两个原因造成的:其一,是由于处于矿区本身地壤中汞含量较高;其二是由于炼汞厂排放大量的汞进入大气中,其中一部分沉降到土壤中。土壤中汞含量随距离汞矿距离变化趋势呈现出与在河流中相似的规律。在研究土壤中汞含量纵向变化中发现,汞含量随着垂直距离的加深呈现递减的趋势。
3)旬阳汞矿区域中采集的沉积物中总汞含量在59.7-2100 mg kg~(-1)范围中,平均值为580mg kg~(-1),这一值远远高于报道的背景区域中采集的沉积物的汞含量,由于沉积物受流水的搅动较小,其汞较易沉积下来,造成了沉积物中汞含量远远高于河流中汞含量。研究表明,沉积物中汞含量量随距离汞矿距离变化趋势呈现出与在河流、土壤中相似的规律。
4)旬阳汞矿区域中采集的植物样品(白菜和小麦苗)总汞含量在58-5370 ng g~(-1)(湿重)范围中变化,其平均值为1163 ng g~(-1)。根部和叶部总汞含量分别为62-4210 ng g~(-1)和58-3420 ngg~(-1),且根部中汞含量大于叶部中汞含量。在该地区采集的植物样品总汞含量远远大于中国国家食品标准机构所允许的最大汞含量20 ng g~(-1)。这说明了该地区的植物明显受到汞污染。根据FTt分析可知,汞的迁移形式是从土壤到根部再到叶部。
5)在对水样、土样和沉积物样品中其它重金属(Se,Pb,Sb)分析后发现,汞和这些元素存在一定的相关性,随着汞含量的增加这些元素的含量也呈现增加的趋势。在水样中,这些重金属和汞表现出良好的相关性,而在沉积物中只有Sb和汞表现出一定的相关性。这说明该地区其他重金属含量受到炼汞活动的影响。
6)在对Toronto市和Yellowknife市大气湿沉降(雨水和雪)中重金属和甲基汞含量分析中发现,雨水中重金属含量普遍高于雪中重金属含量,其中Al,Fe,Pb,Cu,Zn在大气中的含量明显高于其他元素;雨水中甲基汞所占比例较雪中甲基汞所占比例高。通过与其他城市大气中重金属含量比较发现,Toronto市和Yellowknife市大气中重金属污染并不严重。
This thesis includes two parts:a review and a research report.
In the first part,the characteristics and applications of mercury and the sources of mercury pollution were introduced.The status and prevention of mercury pollution and the effects of mercury on human health were reviewed.The development in analytical methods of total mercury was extensively presented.
In the second part,a mercury mine in Xunyang County in Shaanxi Province,the largest mercury mine currently in operation in China,was selected as a case for the study.The concentrations and distributions of mercury species were studied in surface water,soil,sediment and plants(cabbage and wheat seedling) in the region affected by mercury mining activities.The environmental geochemistry behaviors and modes of transport,transformation,and enrichment of mercury in mercury mining environments were thoroughly discussed.The behaviors and modes of transport and enrichment of mercury in plants are also discussed.The data obtained indicate that the plants which grow in the region are contaminated by mercury mining.In addition,the relationship between mercury and other metals was studied.The results indicate that the contamination of mercury is accompanied by the contamination of other metals.The concentration of heavy metals and methyl mercury in wet deposition(rain and snow) was determined.Compare the percentage of methyl mercury in rain and snow samples between city of Toronto and Yellowknife.The main conclusions are as follows:
1.In Xunyang mercury mining area,the total mercury concentration in surface water ranged from 0.12 to 25.57μg L~(-1),with the average value of 2.08μg L~(-1) and the particulate mercury typically exceeded 50%(with the average of 64%) of total mercury in the stream water.This indicates that the main transportation of mercury was performed by particulate mercury in surface water.The result showed that the concentration of total mercury dropped sharply in several kilometres from the Gongguan furnace,climbed when approaching the Qingtonggou furnace;decreased rapidly with increasing distance from the Qingtonggou mining and smelting location.
2.The total mercury contents in soil samples collected from Xunyang mercury mining area ranged from 1.3 to 752.1 mg kg~(-1),with the average value of 106.6 mg kg~(-1).The most contaminated sites appeared at sites No.5 and No.12 with the values of 518 mg kg~(-1) and 752.1 mg kg~(-1), respectively.It was attrubited the fact that site No.5 was closed to Gongguan melting furnace and site No.12 was closed to Qinggonggou melting furnace.The total mercury content in soil samples was attrubited to two factors.The first one was the high mercury contents in local soil.The second one was that the mercury released from mercury smelting furnace could get into atmosphere and then a part of mercury could deposit to the soil in the area.Similar as in surface water,the total mercury contents in soil dropped first and then climbed in Gongguan area and decreased with an increase of the distance from the Qingtonggou mercury smelting furnace in Qingtonggou area.It was clearly seen that the mercury contents decreased with an increase of vertical depth at sites No.1 and No.22.
3.In the Xunyang mercury mining area,the total mercury contents in sediment ranged from 59.7 to 2100 mg kg~(-1),with the average value of 580 mg kg~(-1),which was much higher than the mercury value from background area.It was attrubited the fact that the mercury easily deposited into sediment.The distribution of mercury content in sediment showed the similar tendency as in surface water and soil.
4.The total mercury contents in plants(cabbage and wheat seedling) samples collected from Xunyang mining area ranged from 58-5370 ng g~(-1)(wet weight) with an average value of 1163 ng g~(-1).The total mercury contents in the roots and leaves samples ranged from 62 to 4210 ng g~(-1) and 58 to 3420 ng g~(-1),respectively.The mercury levels in root were generally higher than those in leaf. These values were much higher than the maximum value of 20 ng g~(-1) recommended by the Chinese National Agency for food sources.It indicated that the plants(cabbage and wheat seedling) were significantly contaminated by mercury mining activities.The Fit values suggested that mercury translocation into the plants from roots to aerial part occurred and the mercury source was mainly derived from soil rather than atmosphere.
5.The contents of other metals(Se,Pb,Sb) in surface water,soil and sediment samples showed a common lithological correlation with mercury.There are positive correlations between mercury and other metals in surface water,rather than in sediments.It was found there was only a strong tight correlation between the contents of mercury and Sb.It indicated that the activities of mining affected the contents of other metals in this study area.Actions should be taken to clean the contaminated riverbed,manage waste discharges,and reduce the exposure of mercury to the local residents by issuing advisory for consuming the agricultural products grown in the area.
6.The contents of heavy metals including Cd,Fe,Mn,Ni,Pb,T1,Zn,Co,Cu,Hg and Al in wet deposition(rain and snow) in Toronto and Yellowknife,Cannada,showed that the contents of heavy metals in rain samples were much higher than that in snow samples.The contents of Al,Fe, Pb,Cu,Zn were much higher than that of others such as Cd,Mn,Ni,T1,Co,Hg in both rain and snow samples.The percentage of methyl mercury in rain samples was higher than that in snow samples in Toronto and Yellowknife.The contamination of heavy metals in atomosphere in both Toronto and Yellowknife cities was not serious compared with other cities.
引文
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