鲁西南煤矿区重金属元素环境地球化学特征研究
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摘要
煤在我国的能源结构中占主导地位,而且在很长的时间内其主体地位不会改变。在煤炭资源的开发、加工和利用过程中,已经产生地表沉陷、土壤及水体污染、大气污染、生态破坏等一系列环境问题,其中,煤、矸石及燃煤产物中微量重金属元素对土壤、水体、植物、大气构成严重的污染风险。鲁西南煤矿区是我国的14个大型煤炭生产基地之一,本论文选择鲁西南的兖州、济宁、滕州、宁汶煤矿区,基于煤田地质、地球化学、环境地质、环境影响评价以及数据统计等综合理论,综合采用ICP-MS、X-射线衍射分析、淋溶与浸出毒性实验等分析方法和实验手段,研究了鲁西南矿区煤及固体废物中重金属元素的环境地球化学特征,得到如下主要结论。
(1)鲁西南煤矿区煤中重金属元素(Pb、Cu、Zn)算术平均含量均高于华北和中国煤中微量元素算术平均含量,Pb、Cu、Zn在鲁西南矿区明显富集。
(2)以唐口煤矿为例,探讨了As、Pb、Cu、Zn等重金属元素在煤中的赋存状态。结果表明,Zn元素在3煤层和16煤层中多存在于有机硫化物中,在17煤层中主要以无机态形式存在,赋存于硫酸盐矿物中；Cu元素在3煤层和17煤层中主要存在于硫酸盐矿中,在16煤层煤中主要受有机硫的影响；Pb元素在3、16、17煤层中,除了以硫化物为主要载体外,还受到煤中有机硫的捕获作用；煤中硫元素及其相关矿物是As元素的存在载体。
(3)研究了不同煤田煤层矸石和不同煤层(3、12下、16煤层)矸石中As、Pb、Cu、Zn、Cd分布差异,与地壳元素丰度相比,确定Hg、Cd、As、Pb、Zn为鲁西南煤矿区矸石中富集程度较高重金属元素。而化学形态分析表明重金属元素在矸石中的生物有效态含量均较低,主要赋存在残渣态中。
(4)模拟研究了矸石在不同pH条件下淋溶析出和矸石浸出毒性,探讨了重金属累积毒性的潜在风险。对兖州矿区的北宿和东滩煤矿的表层土壤重金属含量研究表明,随距离矸石山由近到远,其浓度明显下降,而矿区土壤剖面中重金属元素随着土层深度的增加呈降低的趋势。以山东省土壤背景值为标准进行了矿区土壤质量评价,评价结果表明,研究区土壤污染在轻污染级～重污染级。
(5)研究了电厂燃煤产物微量元素As、Pb、Cu、Zn、F的分布规律,结果表明三个电厂灰与原煤的元素分布模式基本一致,煤燃烧后大部分重金属有害元素在电厂灰中富集,通过浸溶实验探讨了微量元素As、Pb、Cu、Zn、F在坏境中的迁移和分配规律,并进行了环境风险评价,上述成果为研究区煤炭资源开采和利用过程中重金属元素的释放机理和控制提供了科学依据。
The heavy metal contamination in coal mining industry and its environmental geochemistry are becoming research hotspots nowadays. Coal-mining area located at southwest of Shangdong Province is one of the13largest coal-production bases in China. Long-term mining exploitation and utilization caused mining subsidence, soil-water-air contamination, ecological disruption and other environmental problems. Heavy metal in coal, gangue and ash generated during burning led to serious pollution on soil, water, plants and air. Yanzhou, Jining, Tengzhou and Ningwen in southwest coal fields of Shandong Province were chosen as research areas. This study is based on coal-mining geology, geochemistry, environmental geology, environmental impact assessment and data statistics, to discuss the environmental geochemistry of heavy metal in coal and other solid wastes in the southwest of Shandong Province by using ICP-MS, X-ray diffraction, energy spectrum analysis, leaching toxicity test and other analytic-experimental methods. The conclusions are as follows:
(1) The mean values of trace heavy metals (Pb, Cu, and Zn) in coal mining area in southwest of Shandong Province are higher than in China and North China, which was indicating the higher accumulation in southwest of Shandong Province.
(2) Existence state of heavy metals (As, Pb, Cu, and Zn) in the coal was discussed (i.e., Tangkou coal mining). It indicated that Zn was consisted in inorganic sulphide in layer3and17, and in organic sulphide in layer16. Pb was consisted in sulphide in layers3,16, and17. In addition, Pb was captured by organic sulfur. As was consisted in sulfur and other related minerals.
(3)As, Pb, Cu, Zn, and Cd distribution in gangue from four coal fields and three layers of mining (layer3, layer12, and layer16) were studied seperatively. It was determined that concentrations of Hg, Cd, As, Pb, and Zn were the highest in the coal gangue in the southwest of Shandong Province. Bio-available fractions of these metals in the coal gangue were low according to form analysis. Majority of metals were in tailings.
(4) Toxicity of leaking from coal gangue under different pH was monitored. The risk of metals accumulation toxicities were evaluated. Concentrations of metals decreased with the distance from the coal gangue based on study of Yanzhou and Beisu coal mining area, and decreased in vertical direction with the increased depth. Coal mining soil was according to base value of the Shandong soil. The contamination level were between delight to high contamination.
(5) Distribution of trace metals including As, Pb, Cu, Zn, and F were determined. Results showed the agreement of metals distribution of the three ashes in the electric power plants with the mine run coal. Majority of heavy metals deposited in ash, and accumulated. Distribution and transportation of trace metals (i.e., As, Pb, Cu, Zn, and F) were studied. All these results were the fundamental for the heavy metal transportation and releasing mechanism in the mining process.
(1)鲁西南煤矿区煤中重金属元素(Pb、Cu、Zn)算术平均含量均高于华北和中国煤中微量元素算术平均含量,Pb、Cu、Zn在鲁西南矿区明显富集。
(2)以唐口煤矿为例,探讨了As、Pb、Cu、Zn等重金属元素在煤中的赋存状态。结果表明,Zn元素在3煤层和16煤层中多存在于有机硫化物中,在17煤层中主要以无机态形式存在,赋存于硫酸盐矿物中；Cu元素在3煤层和17煤层中主要存在于硫酸盐矿中,在16煤层煤中主要受有机硫的影响；Pb元素在3、16、17煤层中,除了以硫化物为主要载体外,还受到煤中有机硫的捕获作用；煤中硫元素及其相关矿物是As元素的存在载体。
(3)研究了不同煤田煤层矸石和不同煤层(3、12下、16煤层)矸石中As、Pb、Cu、Zn、Cd分布差异,与地壳元素丰度相比,确定Hg、Cd、As、Pb、Zn为鲁西南煤矿区矸石中富集程度较高重金属元素。而化学形态分析表明重金属元素在矸石中的生物有效态含量均较低,主要赋存在残渣态中。
(4)模拟研究了矸石在不同pH条件下淋溶析出和矸石浸出毒性,探讨了重金属累积毒性的潜在风险。对兖州矿区的北宿和东滩煤矿的表层土壤重金属含量研究表明,随距离矸石山由近到远,其浓度明显下降,而矿区土壤剖面中重金属元素随着土层深度的增加呈降低的趋势。以山东省土壤背景值为标准进行了矿区土壤质量评价,评价结果表明,研究区土壤污染在轻污染级～重污染级。
(5)研究了电厂燃煤产物微量元素As、Pb、Cu、Zn、F的分布规律,结果表明三个电厂灰与原煤的元素分布模式基本一致,煤燃烧后大部分重金属有害元素在电厂灰中富集,通过浸溶实验探讨了微量元素As、Pb、Cu、Zn、F在坏境中的迁移和分配规律,并进行了环境风险评价,上述成果为研究区煤炭资源开采和利用过程中重金属元素的释放机理和控制提供了科学依据。
The heavy metal contamination in coal mining industry and its environmental geochemistry are becoming research hotspots nowadays. Coal-mining area located at southwest of Shangdong Province is one of the13largest coal-production bases in China. Long-term mining exploitation and utilization caused mining subsidence, soil-water-air contamination, ecological disruption and other environmental problems. Heavy metal in coal, gangue and ash generated during burning led to serious pollution on soil, water, plants and air. Yanzhou, Jining, Tengzhou and Ningwen in southwest coal fields of Shandong Province were chosen as research areas. This study is based on coal-mining geology, geochemistry, environmental geology, environmental impact assessment and data statistics, to discuss the environmental geochemistry of heavy metal in coal and other solid wastes in the southwest of Shandong Province by using ICP-MS, X-ray diffraction, energy spectrum analysis, leaching toxicity test and other analytic-experimental methods. The conclusions are as follows:
(1) The mean values of trace heavy metals (Pb, Cu, and Zn) in coal mining area in southwest of Shandong Province are higher than in China and North China, which was indicating the higher accumulation in southwest of Shandong Province.
(2) Existence state of heavy metals (As, Pb, Cu, and Zn) in the coal was discussed (i.e., Tangkou coal mining). It indicated that Zn was consisted in inorganic sulphide in layer3and17, and in organic sulphide in layer16. Pb was consisted in sulphide in layers3,16, and17. In addition, Pb was captured by organic sulfur. As was consisted in sulfur and other related minerals.
(3)As, Pb, Cu, Zn, and Cd distribution in gangue from four coal fields and three layers of mining (layer3, layer12, and layer16) were studied seperatively. It was determined that concentrations of Hg, Cd, As, Pb, and Zn were the highest in the coal gangue in the southwest of Shandong Province. Bio-available fractions of these metals in the coal gangue were low according to form analysis. Majority of metals were in tailings.
(4) Toxicity of leaking from coal gangue under different pH was monitored. The risk of metals accumulation toxicities were evaluated. Concentrations of metals decreased with the distance from the coal gangue based on study of Yanzhou and Beisu coal mining area, and decreased in vertical direction with the increased depth. Coal mining soil was according to base value of the Shandong soil. The contamination level were between delight to high contamination.
(5) Distribution of trace metals including As, Pb, Cu, Zn, and F were determined. Results showed the agreement of metals distribution of the three ashes in the electric power plants with the mine run coal. Majority of heavy metals deposited in ash, and accumulated. Distribution and transportation of trace metals (i.e., As, Pb, Cu, Zn, and F) were studied. All these results were the fundamental for the heavy metal transportation and releasing mechanism in the mining process.
引文
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