摘要
微量元素在煤中的含量虽然比较少,但由于煤的大量使用,煤中有害成份可以通过多种途径进入环境,进而对环境和人体健康产生不良的影响。有些微量元素,例如汞,由于其有毒有害性,近几年收到国内外许多专家学者的特别关注。
本次研究以两淮矿区为例,通过对两淮矿区煤样、岩石样(包括岩浆岩样)、水样(包括地下水样和地表水)等多种样品进行系统采集,利用电感耦合等离子体发射光谱、电感耦合等离子质谱、冷蒸汽原子荧光光谱、扫描电镜等多种精细分析测试手段,系统分析了所采样品中矿物组成、微观结构及其中的微量元素的含量,尤其对相关样品中汞的含量进行了详细系统地分析,结合环境化学理论、元素地球化学理论、煤化学理论以及矿物学等多种交叉学科理论知识,系统探讨了微量元素在两淮矿区的环境地球化学特征,尤其对有害微量元素汞的环境地球化学行为进行了深入分析。通过对淮南矿区煤样品的采集与分析,系统研究了微量元素在淮南矿区煤中的含量、分布、赋存状态及其迁移转化规律,鉴定了淮南矿区煤中的矿物类型,特别地对淮南矿区煤中汞的含量进行了详细地计算分析,揭示了淮南矿区煤中汞的富集行为。通过对整个淮北矿区6个煤矿进行系统采样,评价了典型有害元素汞在整个淮北矿区煤中的含量,详细分析了影响淮北矿区汞富集的因素,深入探讨了有害元素汞在整个淮北矿区的空间分布规律以及迁移转化机制；通过对淮北矿区地表水进行采样测试,评价了有害元素汞在淮北矿区地表水中的含量；通过对淮北矿区不同层位地下水进行采样分析,研究了微量元素在不同层位地下水中的含量分布情况,探讨了微量元素(稀土元素)应用于地下水不同层位水源判别的有效性与实用性,并通过对地下水围岩样品的淋滤实验,测定围岩样品淋滤液中微量元素的含量,研究了深层地下水中微量元素的水岩交换作用及其相应的迁移机理。
微量元素地过量排放引发了一系列环境问题,对环境与人类健康产生了不良的影响。然而实际上,微量元素对环境的影响具有双面性,即既有不利的一面,也有有利的一面。微量元素及其化合物可以合成各种光催化剂,这些光催化剂能够有效利用太阳光对水体中的有机污染物进行高效地降解,从而达到净化污水的目的。设计、合成高效率的光催化剂已经成为环境污染控制领域热门的研究课题之一。本文以微量元素铋和钽为研究对象,合成了关于铋和钽的光催化剂化合物,并对其降解水体中的有机污染物进行了光降解测试,研究了该催化剂光催化性能以及表征了该光催化剂的形貌。
Because of widespread uses of coals many toxic elements including Hg have been released into the environment. Although many trace elements in coals are present in very small amounts, their environmental impacts and potential human health effects are of great concern because of the enormous amount of coal consumption. In this dissertation, some new findings related to the environmental geochemistry of trace elements from Two Huai coal mining districts were reported, including the abundance, distribution, modes of occurrence, enrichment factors, human health problems, and applications of trace elements in the environment.
With the aim of the better understanding of the geochemistry of trace elements in coal,416borehole samples of coal, one parting, two floor and two roof mudstones were collected from9minable coal seams in24boreholes drilled during exploration in the Huainan Coalfield, Anhui, China, and47elements were determined by various analytical techniques. The depositional environment, abundance, distribution, and affinity of elements were investigated. Results showed that the boron concentration in the coals indicates a brackish water depositional environment in this study region and the marine influence decreased from coal seam1to13-1. Some potentially toxic elements (e.g., Se, Cd) are higher in concentration than their averages for Chinese coals. The contents of some elements in the roof, floor and parting samples are higher than that in the coal seams. The minerals in the coals from the Huainan Coalfield were found to consist mainly of clays, carbonates and sulfides. The elements can be classified into two groups according to the stratigraphic distribution from coal seam No.1to No.13-1, and the characteristics of the groups are analyzed in detail. The elements may be classified into four groups (i.e., Group1to4) according to their correlation coefficients with ash yield. The elements in Group1, Group2, and Group3are strongly correlated with ash yield, while the elements in Group4have weak or negative correlation coefficients.
Mercury (Hg) and its compounds are among the most toxic pollutants in the environment. The combustion of some local coals has caused severe health problems which are linked to high Hg contents in coals. The Hg concentrations in84samples, comprising81coal samples,1igneous rock,2parting rock samples from the Huaibei Coal Mining District, China, were determined by cold-vapor atomic fluorescence spectrometry. The abundance and distribution of Hg in different coal mines and coal seams have been studied. The weighted average Hg concentration for all coal samples in the Huaibei Coalfield is0.42mg/kg, which is about twice that of Chinese average coals. From the southwestern to the northeastern coalfield in the Huaibei Coal Mining District, the Hg concentration shows a decreasing trend, which is presumably related to the magmatic activity and fault structures. Relatively high Hg levels are observed in coal seams Nos.6,7, and10in southwestern coal mines. Correlation analysis indicates that Hg in southwestern and southernmost coals with high Hg concentrations is associated with pyrite. Additionally, thirty-nine low-sulfur Permian coal samples were selected for the discussion of the geochemistry of Hg in Permian low-sulfur coals in the Zhuji Coal Mine, Huainan Coalfield, Anhui province, China. Mercury contents of coal samples were determined by cold-vapor atomic fluorescence spectrometry (CV-AFS). The average Hg content of the overall mine is71.2ng/g weighted by the estimated reserve of each coal seam. An increasing trend of Hg content was observed from bottom to top stratigraphically. As for Hg enrichment in some bench coal samples from No.3coal seam, magmatic activity is responsible for this phenomenon; the pyrite formed during seawater invasion possibly in return accumulated Hg from seawater and this mechanism is possibly responsible for the high Hg content in some coal samples from Nos.4to11-1coal seam. The mechanism that the organic matter can capture Hg from the leachable fractions of Hg for partings is possibly responsible for the Hg enrichment in some coal samples from No.11-2coal seam. Additionally, the anomalously high Hg levels coincide with high sulfur contents in this study, and the main contributor to the high Hg in these coals is presumably related to the sulfides such as pyrite.
The surface waters from ponds and stream creeks in the Huaibei coal mining subsidence areas in some coal mining districts have been used as drinking water and for breeding fish by the residents, so it is very important to assess the Hg concentration in these surface waters in the coal mining districts.24surface water samples were collected from the Huaibei Coal Mining District. The Hg concentrations in surface waters in the Huaibei Coal Mining District ranged from10to60ng/L, and displayed a decreasing trend with distance from a coal waste pile. However, the concentrations are lower than the regulated levels for Hg in drinking water. Although many publications have reported the geochemistry of trace elements in surface waters, few have reported about the geochemistry of trace elements in groundwater, partly due to the difficulty in sampling. In fact, the geochemistry of trace elements (e.g., rare earth elements) has been widely used to discriminate the source of groundwater. In this study, we especially analyzed the geochemistry of rare earth elements in groundwater. To investigate the distribution of trace elementsin groundwater, the concentrations of rare earth elements (REEs) were determined by ICP-MS for groundwater and aquifer limestone samples collected from the Taiyuan Formation limestone aquifer in the Wolonghu Coal Mine, Anhui province, China. The results showed that the groundwater is characterized by a warm temperature (ranging from35.8to39.1℃), roughly neutral pH (7.34-8.27) and high total dissolved solids (TDS,1380-2850mg/L). The REEs in groundwater are characterized by light rare earth elements (LREEs) depletion relative to heavy rare earth elements (HREEs), positive Eu anomalies and negative Ce anomalies. The fractionation of REEs in groundwater can be effected by the inorganic species of REEs. The negative anomalies of Ce possibly reflect the signatures of the aquifer rocks (limestone rocks), whereas positive Eu anomalies are probably attributed to the redox conditions. The similarities of REEs patterns between groundwater and aquifer rocks suggest that aquifer rocks play important roles in controlling the characteristics of REEs in groundwater. The characteristics of REEs and major ions in groundwater from the Taiyuan Formation aquifer are different from other aquifers in the Wolonghu Coal Mine. Although the groundwater from Taiyuan Formation limestone aquifer is not well discriminated from other aquifers by REEs in this study, the obtained results will provide important information for building the foundation of water source discrimination by using REEs in the Wolonghu Coal Mine in the future.
Compounds of trace elements have been widely used as photocatalysts for the degradation of pollutants in water. In this study, bismuth tantalum oxide is reported as a photocatalyst for the degradation of organic pollutants. Bismuth tantalum oxide is a potentially intelligent photocatalyst, which is able to perform a relatively good photocatalytic activity under visible light. Silver loaded bismuth tantalum oxide photocatalyst possess an orderly structure and uniform distribution in thickness, and shows a good photocatalytic activity for degradation of organic pollutants under visible light. Additionally, La doped bismuth tantalum oxide can also increase the photoactivity significantly in comparison with bismuth tantalum oxide.
引文
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