碱性钼尾矿及其影响水体中重金属迁移转化规律研究
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摘要
含多金属硫化矿物的尾矿形成的碱性排水,仍会携带特定的重金属至水体而引发严重的环境污染。本文以辽西铝矿区为例,分析了其尾矿形成碱性排水的原因,建立了尾矿铝等重金属释放迁移模式,探讨了水体中重金属的迁移转化规律及生态风险等问题。为尾矿渗流水质评价、水体水质动力学模拟、污染控制及环境管理提供科学依据。
尾矿矿物学地球化学研究表明,辽西钼尾矿为低硫低碳酸盐尾矿。尾矿库表层硫化矿物发生氧化,但碳酸盐等矿物的酸中和效应使尾矿形成碱性排水(Paste pH 7.3-8.24)。Fe、Cu和Zn以及SO42-在氧化带底部呈现含量峰值,分别是表层的1.4、2.4、3.2和3.4倍。重金属Mo的含量却随深度逐渐增大,钻孔2 m处含量是表层的2倍左右。重金属地球化学形态比例指示,硫化矿物氧化释放的Fe、Cu和Zn在迁移过程中受沉淀、络合吸附、同沉淀等机制控制。重金属Mo的迁移不受沉淀、络合吸附等机制控制。钻孔2 m处各金属的生物有效态含量比例顺序为：Mo>>Fe～Cu～Zn。碱性条件成为Fe、Cu和Zn等元素滞留于尾矿中的自然因素,但却有效地促进了Mo的释放迁移。
尾矿释放动力学特征表明,重金属释放量受酸中和效应控制,释放的重金属以Mo为主。尾矿氧化时间、模拟液pH、温度、粒径和氧气浓度对尾矿释放重金属Mo的影响,进一步揭示了尾矿重金属Mo的释放迁移规律。钼尾矿酸碱潜力评价显示,尾矿未来不会呈酸性环境。这表明滞留于尾矿库氧化带底部的Fe、Cu和Zn未来也不会迁移出尾矿。重金属Mo将持续迁移出尾矿进入下游水体。
流经矿区的女儿河重金属地球化学对比研究表明,矿区及下游各采样点Fe、Cu、Zn和Mo的含量一致大于参照点S0处的含量。水相Mo浓度高于生活饮用水卫生标准1.86-16.66倍。沉积物中各金属含量在矿区段呈现峰值,分别超过S0处含量7.30倍、10.75倍、11.42倍和494.33倍。沉积物中Fe、Cu和Zn元素的含量高值源于尾矿的降水冲蚀和风蚀,Mo的含量高值更主要源于尾矿的淋滤释放。水体中重金属Fe、Cu和Zn的分配系数>>Mo的分配系数。沉积物因吸附机制成为Fe、Cu和Zn元素的归宿,但不能完全吸附重金属Mo。水库还原环境可有效滞留Mo,但各采样点沉积物中重金属Mo生物有效态仍达18-58%。
结论表明,酸碱条件是控制各重金属迁移转化的主要因素。碱性环境促进重金属Mo从钼尾矿中迁移释放,并易在河流水体中迁移。沉积物中的Mo具有中等以上的生态危害。
The alkaline mine drainage may be caused in mine tailings contained polymetallic sulfide minerals for depletion of carbonate minerals through consumption by acid-neutralization reactions. However, some special metals can also transport into water with the alkaline mine drainage in elevated levels and result in serious impact on environment. The paper, based on a case study on Molybdenum mine area in western Liaoning, analyses the forming causation of the alkaline mine drainage, establishes the release and transport model of heavy metals, investigates the migration and transformation of heavy metals in water and ecological risk caused by heavy metals. The results can provide scientific basis for seepage quality assessment, dynamics simulation of water quality, heavy metal pollution control and environmental management.
The mineralogical and geochemical results showed Mo tailings in western Liaoning were low sulfide and low carbonates tailings. The sulfide minerals in surface tailings pond were oxidized but the alkaline mine drainage was formed because of carbonate neutralization (Paste pH 7.3-8.24). The hydrolytic equilibrium of HCO3- and CO32- controlled the acid-base environment. The peak concentrations of Fe, Cu, Zn and SO42- were presented at the bottom of oxidation zone, which were 1.4,2.4,3.2 and 3.4 times higher than that of in surface tailings pond, respectively. The Mo concentration increased gradually with depth and the Mo concentration at 2 m depth was 2 times higher than that of in surface tailings pond (1090-1146μg/g). Geochemical species of heavy metals indicated that precipitation, co-precipitation and complexing adsorption mechanism controlled Fe, Cu and Zn released from sulfide minerals in migration process, but not for Mo. The proportion of those four metals of bioavailable fraction at 2 m depth in tailings pond followed the order:Mo>>Fe～Cu～Zn. The alkaline conditions played a crucial role in retention of Fe, Cu and Zn, but promoted effectively the leaching and migration of Mo.
The results of batch experiments of leaching kinetics with tailings demonstrated that elution quantity of heavy metals was controlled by neutralization of minerals and heavy metal Mo was major metal in leachate. Oxidation time, pH of simulated solution, temperature, particle size and O2 concentration had effect on the release of Mo from tailings, which further prove the release transport of Mo in tailings. The acid producing potential revealed that acidic condition in tailings would not been formed. Fe, Cu and Zn remaining in the bottom of oxidation zone would not leach from tailings ponds due to the alkaline conditions, but heavy metal Mo would leach from tailings ponds into environment downstream of Mo mining area.
The geochemical results of samples from water body in mining area and downstream of mining area indicated that the concentrations of Fe, Cu, Zn and Mo in water were higher than in S0. Mo concentrations in aqueous phase were much higher than the health standard for domestic drinking water by 1.86-16.66 times. All the concentrations of heavy metals in sediments of mining area and downstream of mining area were higher than that of heavy metals at SO by 7.30,10.75,11.42 and 494.33 times, respectively. The high concentration values of heavy metals in sediments had a close relationship with Mo mining activity. The partition coefficients of heavy metals of Fe, Cu and Zn were higher than that of Mo. Sediments did not become the bearing medium for Mo but for Fe, Cu and Zn due to adsorption mechanism. The reduction condition in reservoir sediments played an important role for retention Mo, but the bioavailable Mo fraction presented 18-58% in the Nver River.
The conclusions suggested that the pH condition controlled the migration and transformation of heavy metals in different phase. Heavy metal Mo migrated easily in mine tailings and in the Never River for the alkaline condition. The ecological risk from Mo was higher than medium grade in sediments.
尾矿矿物学地球化学研究表明,辽西钼尾矿为低硫低碳酸盐尾矿。尾矿库表层硫化矿物发生氧化,但碳酸盐等矿物的酸中和效应使尾矿形成碱性排水(Paste pH 7.3-8.24)。Fe、Cu和Zn以及SO42-在氧化带底部呈现含量峰值,分别是表层的1.4、2.4、3.2和3.4倍。重金属Mo的含量却随深度逐渐增大,钻孔2 m处含量是表层的2倍左右。重金属地球化学形态比例指示,硫化矿物氧化释放的Fe、Cu和Zn在迁移过程中受沉淀、络合吸附、同沉淀等机制控制。重金属Mo的迁移不受沉淀、络合吸附等机制控制。钻孔2 m处各金属的生物有效态含量比例顺序为：Mo>>Fe～Cu～Zn。碱性条件成为Fe、Cu和Zn等元素滞留于尾矿中的自然因素,但却有效地促进了Mo的释放迁移。
尾矿释放动力学特征表明,重金属释放量受酸中和效应控制,释放的重金属以Mo为主。尾矿氧化时间、模拟液pH、温度、粒径和氧气浓度对尾矿释放重金属Mo的影响,进一步揭示了尾矿重金属Mo的释放迁移规律。钼尾矿酸碱潜力评价显示,尾矿未来不会呈酸性环境。这表明滞留于尾矿库氧化带底部的Fe、Cu和Zn未来也不会迁移出尾矿。重金属Mo将持续迁移出尾矿进入下游水体。
流经矿区的女儿河重金属地球化学对比研究表明,矿区及下游各采样点Fe、Cu、Zn和Mo的含量一致大于参照点S0处的含量。水相Mo浓度高于生活饮用水卫生标准1.86-16.66倍。沉积物中各金属含量在矿区段呈现峰值,分别超过S0处含量7.30倍、10.75倍、11.42倍和494.33倍。沉积物中Fe、Cu和Zn元素的含量高值源于尾矿的降水冲蚀和风蚀,Mo的含量高值更主要源于尾矿的淋滤释放。水体中重金属Fe、Cu和Zn的分配系数>>Mo的分配系数。沉积物因吸附机制成为Fe、Cu和Zn元素的归宿,但不能完全吸附重金属Mo。水库还原环境可有效滞留Mo,但各采样点沉积物中重金属Mo生物有效态仍达18-58%。
结论表明,酸碱条件是控制各重金属迁移转化的主要因素。碱性环境促进重金属Mo从钼尾矿中迁移释放,并易在河流水体中迁移。沉积物中的Mo具有中等以上的生态危害。
The alkaline mine drainage may be caused in mine tailings contained polymetallic sulfide minerals for depletion of carbonate minerals through consumption by acid-neutralization reactions. However, some special metals can also transport into water with the alkaline mine drainage in elevated levels and result in serious impact on environment. The paper, based on a case study on Molybdenum mine area in western Liaoning, analyses the forming causation of the alkaline mine drainage, establishes the release and transport model of heavy metals, investigates the migration and transformation of heavy metals in water and ecological risk caused by heavy metals. The results can provide scientific basis for seepage quality assessment, dynamics simulation of water quality, heavy metal pollution control and environmental management.
The mineralogical and geochemical results showed Mo tailings in western Liaoning were low sulfide and low carbonates tailings. The sulfide minerals in surface tailings pond were oxidized but the alkaline mine drainage was formed because of carbonate neutralization (Paste pH 7.3-8.24). The hydrolytic equilibrium of HCO3- and CO32- controlled the acid-base environment. The peak concentrations of Fe, Cu, Zn and SO42- were presented at the bottom of oxidation zone, which were 1.4,2.4,3.2 and 3.4 times higher than that of in surface tailings pond, respectively. The Mo concentration increased gradually with depth and the Mo concentration at 2 m depth was 2 times higher than that of in surface tailings pond (1090-1146μg/g). Geochemical species of heavy metals indicated that precipitation, co-precipitation and complexing adsorption mechanism controlled Fe, Cu and Zn released from sulfide minerals in migration process, but not for Mo. The proportion of those four metals of bioavailable fraction at 2 m depth in tailings pond followed the order:Mo>>Fe～Cu～Zn. The alkaline conditions played a crucial role in retention of Fe, Cu and Zn, but promoted effectively the leaching and migration of Mo.
The results of batch experiments of leaching kinetics with tailings demonstrated that elution quantity of heavy metals was controlled by neutralization of minerals and heavy metal Mo was major metal in leachate. Oxidation time, pH of simulated solution, temperature, particle size and O2 concentration had effect on the release of Mo from tailings, which further prove the release transport of Mo in tailings. The acid producing potential revealed that acidic condition in tailings would not been formed. Fe, Cu and Zn remaining in the bottom of oxidation zone would not leach from tailings ponds due to the alkaline conditions, but heavy metal Mo would leach from tailings ponds into environment downstream of Mo mining area.
The geochemical results of samples from water body in mining area and downstream of mining area indicated that the concentrations of Fe, Cu, Zn and Mo in water were higher than in S0. Mo concentrations in aqueous phase were much higher than the health standard for domestic drinking water by 1.86-16.66 times. All the concentrations of heavy metals in sediments of mining area and downstream of mining area were higher than that of heavy metals at SO by 7.30,10.75,11.42 and 494.33 times, respectively. The high concentration values of heavy metals in sediments had a close relationship with Mo mining activity. The partition coefficients of heavy metals of Fe, Cu and Zn were higher than that of Mo. Sediments did not become the bearing medium for Mo but for Fe, Cu and Zn due to adsorption mechanism. The reduction condition in reservoir sediments played an important role for retention Mo, but the bioavailable Mo fraction presented 18-58% in the Nver River.
The conclusions suggested that the pH condition controlled the migration and transformation of heavy metals in different phase. Heavy metal Mo migrated easily in mine tailings and in the Never River for the alkaline condition. The ecological risk from Mo was higher than medium grade in sediments.
引文
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