中国煤中硒的分布、赋存状态和环境地球化学研究
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摘要
硒元素是人体一种必需的微量元素,摄入的过多或者过少都会影响人体的健康。世界大范围内环境中都是缺硒的,硒元素被加工成为各种营养品进行补充。中国是缺硒地方病高发区,同时也是硒中毒事件的高发区。其中,由于利用高硒煤而造成的燃煤型硒中毒事件,是最为突出的。硒在地壳中的丰度很低,而煤和黑色页岩被称为富硒沉积岩,是硒元素含量最为丰富的载体。由于硒元素较高的挥发性,燃煤过程中极易释放出来。燃煤释放的硒是大气中硒最主要的人为源,加之煤炭长久以来作为重要的能源,储量和用量巨大,即便是微量元素的释放亦不容忽视。
煤中硒的含量,分布和赋存状态直接影响到其在利用过程中的释放情况和迁移规律,通过改变环境中硒的含量和分布进而影响人类健康。中国煤炭储量丰富,并且成煤时代较长,沉积环境和成煤植物以及煤化作用相对复杂。系统性的研究中国煤中硒的含量水平,分布特征以及赋存状态特征,对于客观的评价和预测中国煤炭的利用可造成的环境影响具有重要意义。本次研究全面调查、收集和分析了国内外所报道的煤中硒的数据,针对不同赋煤地区、不同的成煤时代以及不同变质程度煤中硒的分布和含量特征进行了汇总和讨论。主要得出以下结论：1.中国不同省市地区煤中硒含量差异较大,几何平均值为3.91mg/Kg,按照省份划分了高硒区、中硒区和低硒区,高硒煤和低硒煤的分布具有一定的规律性；2.煤中硒的含量随着煤层成煤时代由老到新呈现降低趋势,古生代煤中硒的平均含量高于中生代和新生代；3.随着煤的变质程度逐渐升高,硒元素的赋存状态呈现一定的规律性变化。4.特殊煤种(高硫煤,高氯煤)中硒元素的赋存状态具有各自的差异性。
对于典型矿区的多个煤层进行系统的研究,有助于进一步了解煤中微量元素的分布和赋存规律。本次研究选取了高硒煤赋煤地区之一的安徽省淮北矿区作为研究区,采集了矿区内七个煤矿(祁东矿、桃园矿、任楼矿、海孜矿、百善矿、刘二矿和刘店矿)主采煤层的123个煤样和19个围岩样品,进行硒元素以及其他微量元素和常量元素的测试。考查了硒元素含量在矿区内垂直分布和水平分布规律,讨论了沉积环境与煤中硒元素含量的关系。采用相关性分析法对淮北煤中硒元素的赋存状态进行了总体上的评价,富铁粘土矿物和碳酸盐矿物是下石盒子组煤中硒元素的主要载体,山西组和上石盒子组煤中的硒元素主要与硫化矿物有关。淮北矿区广泛发育的断层可能是该地区煤中硒含量较高的原因之一。
过去国内外学者对于煤中易挥发元素硒的迁移转化行为研究关注较多,而对于煤矸石和煤泥的研究较少。事实上,煤中丰富的微量元素,在煤矸石和煤泥中同样存在甚至更加富集。加之低热值燃料相对于煤炭具有不同的物理特征,矿物构成及其微量元素的结合状态,弥补有关煤泥煤矸石低热值电厂的硒排放情形,对于火电厂整体的环境风险评价将更加具有科学性和准确性。对煤泥、煤矸石低热值电厂的不同燃料、除尘器飞灰及渣中痕量元素硒进行研究的结果表明,硒在除尘器飞灰中以不同程度富集,在底渣中显著亏损。分析可能的原因有两种：是脱硫剂石灰粉的使用,其在燃烧过程中产生的CaO不仅吸收了SO2还可与高温产生的Se02气体进行反应；二与飞灰的颗粒大小和形态有关,飞灰中存在的蜂窝状结构具有较大的比表面积,吸附能力显著提高。通过物质平衡计算,燃烧后的硒近80-90%存在于除尘器飞灰当中；6.60-15.23%的硒随气流和烟气细飞灰直接排放入大气；渣中硒含量较低,对于环境的影响很小。排放入大气的硒活性最高,并且随着电厂的运行,排放量亦非常显著,应进一步加以控制。根据地累积指数法的评价结果,除了个别样品之外,所研究区域矿区表层土壤中均受到不同程度的污染,最高污染程度达到中度污染。就硒元素而言,在2009年到2011年之间,受污染样品所占的比例,以及样品受污染的程度都有所加深。土壤剖面样品中硒元素的分布特征说明,硒元素在当地的土壤中具有一定的迁移性,地表接收到的硒元素会随着雨水的淋溶作用向下迁移；然而,此种迁移性不大,距地表约40cm以下即开始减退。水体中硒元素的分布在2009至2011年之间的变化不大且普遍含量亦较低,当前没有出现污染的迹象。然而沉积物中硒出现明显富集和污染迹象,污染水平主要呈中度污染,最高达到中重度污染水平。考虑到周边水体主要用于养鱼产业,底泥中的硒必将成为一个二次污染源,有必要对水产品进行周期性的监测,以保证食品安全和周边居民的人体健康。
As is well known, selenium (Se) is one of the essential elements of human beings at low concentrations but toxic at high concentrations. Se exists as a trace element in the Earth's crust, but coal and the black shale are known as the most Se-enriched carriers:so-called "Se-enriched sedimentary rock". An environmental lack of Se is prevalent in most of the world and as a result, various forms of extra Se-enriched nutrition are used among people. China not only has a high incidence of endemic Se-deficiency, but also has a high incidence of environmental Se-poisoning. Among the latter, Se-poisoning incidents caused by high-Se coal combustion are the most obvious forms. Selenium is readily released during coal-combustion due to the high volatility of Se. The huge consumption amount of coal has made coal-combustion the main artificial resource of Se in the atmosphere.
The content, distribution and mode of occurrence of Se in coals affects the release and migration of Se directly during the use of coal, and finally affects the environment and human health. China has abundant coal reserves produced by the long coal-forming period; thus, the sedimentary environment and coalification are comparatively complex. Systemic studies of Se in Chinese coals are meaningful work for objectively estimating the potential environmental effects of using Chinese coals. This study includes the following aspects:1. based on the collection of2,288coal samples, the average Se content in Chinese coal is3.91mg/kg;2. the Se content in Chinese coal varied remarkably with different provinces or areas, and three groups were defined upon Se content;3. contents of Se falls gradually over the coal-forming period, and the average content of Se in Paleozoic coals is higher than in the Mesozoic and Cenozoic coals;4. the content and modes of occurrence of Se in coals of different metamorphic grade were studied and discussed;5. the formation mechanism of Se in different kinds of coal was systemic discussed;6. Se in special coal samples (high-sulfur coal and high-chlorine coal) were also studied.
Systemic research on typical coal mining areas are helpful for further understanding of the distribution and enrichment mechanisms of trace elements in coal. Selenium contents in123coal and19surrounding rock channel samples, which were collected from the fresh working face of main coal seams in seven selected coal mines of the Huaibei coalfield (i.e. Qidong (QD), Taoyuan (TY), Renlou (RL), Haizi (HZ), Liudian (LD), Baishan (BS), and Liuer (LE)), were determined by hydride generation atomic fluorescence spectrometry. Compared with the average China and world coals, Huaibei coals were highly enriched in selenium. The depositional environment of the Permian coal-bearing strata in Huaibei coalfields was inferred by the Boron content in coal. Selenium was distributed unevenly both horizontally and vertically in this area. Pearson correlation coefficients are used to estimate the modes of occurrence of selenium in Huaibei coals. Iron-bearing clay minerals and carbonates were the dominant carriers of selenium in coals of the Lower Shihezi Formation. Selenium in coals from No.3and No.10coal seams was mainly associated with sulfide minerals. The well-developed faults in the Huaibei coalfield could contribute to the enrichment of selenium in Huaibei coals.
The transformation behavior of trace elements in coal during the combustion process has been a focus of interest for a long time, but few researchers have targeted the combustion of coal slime and coal gangue. In fact, the abundant trace elements in coals also exist in coal slime and gangue, which are even more enriched. Low heat value fuels have different physical characteristics, mineral components and modes of occurrence of trace elements. Study of the emission situation of Se from low heat value power plants would be helpful in estimating the environmental risk of the coal-fired power plants more scientifically and accurately. Therefore, Selenium in feed coal, fly ash and bottom ash samples which were collected from a low-heating power plant, were studied. Result showed that Se tends to be enriched by varied degrees in different kinds of fly ash samples. This kind of distribution is shaped by two factors:first, the use of desulfurizing agents produce CaO which may react with gaseous SeO2which is released by the high temperature; then, the honeycomb-like nature of the material and the tiny size could increase the adsorptive capacity by the enhanced specific surface area of the fly ash particles. Mass balance calculations of feed coal indicate that80-90%of selenium in coal is distributed in the fly ash, which is captured by an electrostatic precipitator.6.60-15.23%of the selenium may be disposed into the atmosphere directly or with the flue gas. The environmental impacts of bottom ashes may cause few environmental impacts because of the small proportions involved. The amount of selenium released into air could be very high over time, and further control is necessary for the potential environmental risk.
Surface soil samples of Huaibei coal mine area have been contaminated to various degrees, according to the result of the I-geo method. The most polluted soil sample belonged to the moderately polluted category. As far as Se is concerned, the proportion of the polluted sample and the level of Se pollution both have increased from2009to2011. Selenium mainly concentrated at the test site40cm below the surface, and then decreased with depth. This distribution pattern indicates the low immigration capacity of Se in local soils, and the high-Se site could be related to external Se sources.
The contents of Se in water samples collected in2009and2011did not show visible differences. Concentrations of Se in most of the water samples are very low without any pollution evident. But there is an obvious evidence of Se enrichment and pollution in sediments and the sediment samples are mainly moderately polluted. However, considering that those water bodies are mainly used for fish-farming, Selenium in the sediment could be secondary sources. Periodic monitoring is necessary for food safety and the health of local residents.
煤中硒的含量,分布和赋存状态直接影响到其在利用过程中的释放情况和迁移规律,通过改变环境中硒的含量和分布进而影响人类健康。中国煤炭储量丰富,并且成煤时代较长,沉积环境和成煤植物以及煤化作用相对复杂。系统性的研究中国煤中硒的含量水平,分布特征以及赋存状态特征,对于客观的评价和预测中国煤炭的利用可造成的环境影响具有重要意义。本次研究全面调查、收集和分析了国内外所报道的煤中硒的数据,针对不同赋煤地区、不同的成煤时代以及不同变质程度煤中硒的分布和含量特征进行了汇总和讨论。主要得出以下结论：1.中国不同省市地区煤中硒含量差异较大,几何平均值为3.91mg/Kg,按照省份划分了高硒区、中硒区和低硒区,高硒煤和低硒煤的分布具有一定的规律性；2.煤中硒的含量随着煤层成煤时代由老到新呈现降低趋势,古生代煤中硒的平均含量高于中生代和新生代；3.随着煤的变质程度逐渐升高,硒元素的赋存状态呈现一定的规律性变化。4.特殊煤种(高硫煤,高氯煤)中硒元素的赋存状态具有各自的差异性。
对于典型矿区的多个煤层进行系统的研究,有助于进一步了解煤中微量元素的分布和赋存规律。本次研究选取了高硒煤赋煤地区之一的安徽省淮北矿区作为研究区,采集了矿区内七个煤矿(祁东矿、桃园矿、任楼矿、海孜矿、百善矿、刘二矿和刘店矿)主采煤层的123个煤样和19个围岩样品,进行硒元素以及其他微量元素和常量元素的测试。考查了硒元素含量在矿区内垂直分布和水平分布规律,讨论了沉积环境与煤中硒元素含量的关系。采用相关性分析法对淮北煤中硒元素的赋存状态进行了总体上的评价,富铁粘土矿物和碳酸盐矿物是下石盒子组煤中硒元素的主要载体,山西组和上石盒子组煤中的硒元素主要与硫化矿物有关。淮北矿区广泛发育的断层可能是该地区煤中硒含量较高的原因之一。
过去国内外学者对于煤中易挥发元素硒的迁移转化行为研究关注较多,而对于煤矸石和煤泥的研究较少。事实上,煤中丰富的微量元素,在煤矸石和煤泥中同样存在甚至更加富集。加之低热值燃料相对于煤炭具有不同的物理特征,矿物构成及其微量元素的结合状态,弥补有关煤泥煤矸石低热值电厂的硒排放情形,对于火电厂整体的环境风险评价将更加具有科学性和准确性。对煤泥、煤矸石低热值电厂的不同燃料、除尘器飞灰及渣中痕量元素硒进行研究的结果表明,硒在除尘器飞灰中以不同程度富集,在底渣中显著亏损。分析可能的原因有两种：是脱硫剂石灰粉的使用,其在燃烧过程中产生的CaO不仅吸收了SO2还可与高温产生的Se02气体进行反应；二与飞灰的颗粒大小和形态有关,飞灰中存在的蜂窝状结构具有较大的比表面积,吸附能力显著提高。通过物质平衡计算,燃烧后的硒近80-90%存在于除尘器飞灰当中；6.60-15.23%的硒随气流和烟气细飞灰直接排放入大气；渣中硒含量较低,对于环境的影响很小。排放入大气的硒活性最高,并且随着电厂的运行,排放量亦非常显著,应进一步加以控制。根据地累积指数法的评价结果,除了个别样品之外,所研究区域矿区表层土壤中均受到不同程度的污染,最高污染程度达到中度污染。就硒元素而言,在2009年到2011年之间,受污染样品所占的比例,以及样品受污染的程度都有所加深。土壤剖面样品中硒元素的分布特征说明,硒元素在当地的土壤中具有一定的迁移性,地表接收到的硒元素会随着雨水的淋溶作用向下迁移；然而,此种迁移性不大,距地表约40cm以下即开始减退。水体中硒元素的分布在2009至2011年之间的变化不大且普遍含量亦较低,当前没有出现污染的迹象。然而沉积物中硒出现明显富集和污染迹象,污染水平主要呈中度污染,最高达到中重度污染水平。考虑到周边水体主要用于养鱼产业,底泥中的硒必将成为一个二次污染源,有必要对水产品进行周期性的监测,以保证食品安全和周边居民的人体健康。
As is well known, selenium (Se) is one of the essential elements of human beings at low concentrations but toxic at high concentrations. Se exists as a trace element in the Earth's crust, but coal and the black shale are known as the most Se-enriched carriers:so-called "Se-enriched sedimentary rock". An environmental lack of Se is prevalent in most of the world and as a result, various forms of extra Se-enriched nutrition are used among people. China not only has a high incidence of endemic Se-deficiency, but also has a high incidence of environmental Se-poisoning. Among the latter, Se-poisoning incidents caused by high-Se coal combustion are the most obvious forms. Selenium is readily released during coal-combustion due to the high volatility of Se. The huge consumption amount of coal has made coal-combustion the main artificial resource of Se in the atmosphere.
The content, distribution and mode of occurrence of Se in coals affects the release and migration of Se directly during the use of coal, and finally affects the environment and human health. China has abundant coal reserves produced by the long coal-forming period; thus, the sedimentary environment and coalification are comparatively complex. Systemic studies of Se in Chinese coals are meaningful work for objectively estimating the potential environmental effects of using Chinese coals. This study includes the following aspects:1. based on the collection of2,288coal samples, the average Se content in Chinese coal is3.91mg/kg;2. the Se content in Chinese coal varied remarkably with different provinces or areas, and three groups were defined upon Se content;3. contents of Se falls gradually over the coal-forming period, and the average content of Se in Paleozoic coals is higher than in the Mesozoic and Cenozoic coals;4. the content and modes of occurrence of Se in coals of different metamorphic grade were studied and discussed;5. the formation mechanism of Se in different kinds of coal was systemic discussed;6. Se in special coal samples (high-sulfur coal and high-chlorine coal) were also studied.
Systemic research on typical coal mining areas are helpful for further understanding of the distribution and enrichment mechanisms of trace elements in coal. Selenium contents in123coal and19surrounding rock channel samples, which were collected from the fresh working face of main coal seams in seven selected coal mines of the Huaibei coalfield (i.e. Qidong (QD), Taoyuan (TY), Renlou (RL), Haizi (HZ), Liudian (LD), Baishan (BS), and Liuer (LE)), were determined by hydride generation atomic fluorescence spectrometry. Compared with the average China and world coals, Huaibei coals were highly enriched in selenium. The depositional environment of the Permian coal-bearing strata in Huaibei coalfields was inferred by the Boron content in coal. Selenium was distributed unevenly both horizontally and vertically in this area. Pearson correlation coefficients are used to estimate the modes of occurrence of selenium in Huaibei coals. Iron-bearing clay minerals and carbonates were the dominant carriers of selenium in coals of the Lower Shihezi Formation. Selenium in coals from No.3and No.10coal seams was mainly associated with sulfide minerals. The well-developed faults in the Huaibei coalfield could contribute to the enrichment of selenium in Huaibei coals.
The transformation behavior of trace elements in coal during the combustion process has been a focus of interest for a long time, but few researchers have targeted the combustion of coal slime and coal gangue. In fact, the abundant trace elements in coals also exist in coal slime and gangue, which are even more enriched. Low heat value fuels have different physical characteristics, mineral components and modes of occurrence of trace elements. Study of the emission situation of Se from low heat value power plants would be helpful in estimating the environmental risk of the coal-fired power plants more scientifically and accurately. Therefore, Selenium in feed coal, fly ash and bottom ash samples which were collected from a low-heating power plant, were studied. Result showed that Se tends to be enriched by varied degrees in different kinds of fly ash samples. This kind of distribution is shaped by two factors:first, the use of desulfurizing agents produce CaO which may react with gaseous SeO2which is released by the high temperature; then, the honeycomb-like nature of the material and the tiny size could increase the adsorptive capacity by the enhanced specific surface area of the fly ash particles. Mass balance calculations of feed coal indicate that80-90%of selenium in coal is distributed in the fly ash, which is captured by an electrostatic precipitator.6.60-15.23%of the selenium may be disposed into the atmosphere directly or with the flue gas. The environmental impacts of bottom ashes may cause few environmental impacts because of the small proportions involved. The amount of selenium released into air could be very high over time, and further control is necessary for the potential environmental risk.
Surface soil samples of Huaibei coal mine area have been contaminated to various degrees, according to the result of the I-geo method. The most polluted soil sample belonged to the moderately polluted category. As far as Se is concerned, the proportion of the polluted sample and the level of Se pollution both have increased from2009to2011. Selenium mainly concentrated at the test site40cm below the surface, and then decreased with depth. This distribution pattern indicates the low immigration capacity of Se in local soils, and the high-Se site could be related to external Se sources.
The contents of Se in water samples collected in2009and2011did not show visible differences. Concentrations of Se in most of the water samples are very low without any pollution evident. But there is an obvious evidence of Se enrichment and pollution in sediments and the sediment samples are mainly moderately polluted. However, considering that those water bodies are mainly used for fish-farming, Selenium in the sediment could be secondary sources. Periodic monitoring is necessary for food safety and the health of local residents.
引文
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