燃烧温度对两淮烟煤中汞含量与赋存形态的影响
|
摘要
为了调查两淮烟煤中汞元素在不同燃烧温度下的地球化学行为,在两淮地区4个典型煤矿床分别采集了4个烟煤样品。采用程序升温石英管式炉获得400、500、600、700、800℃和900℃下的煤灰样品。利用ICP-MS测定了原煤及煤灰样品中Hg元素的含量,结合X射线衍射(XRD)和傅里叶转换红外光谱(FTIR)分析,取得如下成果:烟煤中Hg的丰度值约为0.1μg/g;烟煤中Hg主要以残渣态形式为主,其次为可交换态和碳酸盐结合态;烟煤中Hg主要挥发温度位于400~500℃间,仅有少量的Hg会赋存在灰渣之中;XRD实验表明,烟煤中黏土矿物含量变化与汞的变化关系密切;此外,残渣中固定碳的存在影响着其Hg含量变化;FTIR实验表明,烟煤中Hg含量与C=O官能团含量呈较好的正相关关系,表明煤中C=O含量可以用作检测煤中Hg含量的指示剂。
In order to investigate the geochemical behavior of mercury in two bituminous coal at different combustion temperature,4 samples of bituminous coal were collected from 4 typical coal mines in Huainan and Huaibei regions. The samples of coal ash at400 ℃, 500 ℃, 600 ℃, 700 ℃, 800 ℃ and 900 ℃ were obtained by a quartz tube furnace. The content of Hg element in coal and coal ash samples were determined using ICP-MS, combined with X ray diffraction(XRD)and Fourier transform infrared spectroscopy(FTIR)analysis. The results obtained are as follows: the abundance of Hg in bituminous coal is about 0.1 μg/g; Hg in bituminous coal is mainly in the form of residue, followed by exchangeable and carbonate binding states; volatile temperature of Hg in bituminous coal is at 400 ℃ to 500 ℃, a small amount of Hg is deposited in the slag; XRD experiments show that the variation of clay mineral content in bituminous coal is closely related to the variation of mercury; the presence of fixed carbon in the residue affects its Hg content; FTIR experiment shows that Hg content in bituminous coal has a good positive correlation with C=O functional group content,it indicates that the content of C=O in coal can be used as an indicator to detect the Hg content in coal.
In order to investigate the geochemical behavior of mercury in two bituminous coal at different combustion temperature,4 samples of bituminous coal were collected from 4 typical coal mines in Huainan and Huaibei regions. The samples of coal ash at400 ℃, 500 ℃, 600 ℃, 700 ℃, 800 ℃ and 900 ℃ were obtained by a quartz tube furnace. The content of Hg element in coal and coal ash samples were determined using ICP-MS, combined with X ray diffraction(XRD)and Fourier transform infrared spectroscopy(FTIR)analysis. The results obtained are as follows: the abundance of Hg in bituminous coal is about 0.1 μg/g; Hg in bituminous coal is mainly in the form of residue, followed by exchangeable and carbonate binding states; volatile temperature of Hg in bituminous coal is at 400 ℃ to 500 ℃, a small amount of Hg is deposited in the slag; XRD experiments show that the variation of clay mineral content in bituminous coal is closely related to the variation of mercury; the presence of fixed carbon in the residue affects its Hg content; FTIR experiment shows that Hg content in bituminous coal has a good positive correlation with C=O functional group content,it indicates that the content of C=O in coal can be used as an indicator to detect the Hg content in coal.
引文
[1]任建莉,周劲松,骆仲泱,等.煤中汞燃烧过程析出规律试验研究[J].环境科学学报,2002,22(3):289.
[2]傅丛,连进京,姜英,等.高汞煤燃烧过程中汞的析出规律试验研究[J].洁净煤技术,2007,13(6):62-65.
[3]李婷婷.贵州典型高汞煤温和热解过程中汞的释放及形态转化规律的研究[D].武汉:华中科技大学,2011:45-50.
[4]路文芳,田宇,战景明,等.我国大气汞污染对人体健康的影响[J].环境与健康杂志,2012,29(8):761.
[5]代世峰,任德贻,李丹,等.贵州大方煤田主采煤层的矿物学异常及其对元素地球化学的影响[J].地质学报,2006,80(4):589-597.
[6]黄晓雨,郑刘根,张强伟,等.卧龙湖煤矿岩浆蚀变煤层中汞的分布与赋存特征[J].高校地质学报,2015,21(2):280-287.
[7]姜萌萌.淮北卧龙湖岩浆侵入区煤中微量元素赋存规律与应用研究[D].合肥:中国科学技术大学,2011:56-62.
[8]Finkleman R.Health Impacts of Coal Combustion[J].Center for Integrated Data Analytics Wisconsin Science Center,2000:1-4.
[9]任德贻,赵峰华,张军营,等.煤中有害微量元素富集的成因类型初探[J].地学前缘,1999,6(5):17-22.
[10]郑刘根,刘桂建,齐翠翠,等.中国煤中汞的环境地球化学研究[J].中国科学技术大学学报,2007,37(8):953-963.
[11]曾凡桂,谢克昌.煤结构化学的理论体系与方法论[J].煤炭学报,2004,29(4):443-447.
[12]梁虎珍,王传格,曾凡桂,等.应用红外光谱研究脱灰对伊敏褐煤结构的影响[J].燃料化学学报,2014,42(2):129-137.
[13]刘大锰,杨起,汤达祯,等.华北晚古生代煤中硫及微量元素分布赋存规律[J].煤炭科学技术,2000,28(9):39-42.
[14]Tessier B,Reynaud J Y.Cataclysmic burial of Pennsylvanian Period coal swamps in the Illinois Basin[C]∥Contributions to Modern and Ancient Tidal Sedimentology:Proceedings of the Tidalites 2012 conference.John Wiley&Sons,Ltd,2016:102-110.
[15]丰芸,李寒旭,丁立明.利用XRD分析高温下淮南煤灰矿物质变化[J].安徽建筑大学学报,2008,16(5):53-57.
[16]刘国根,邱冠周,胡岳华.煤的红外光谱研究[J].中南大学学报(自然科学版),1999(4):371-373.
[17]邢莹莹.辽宁抚顺煤精官能团表征及热变异行为[J].光谱学与光谱分析,2017,37(6):1819-1825.
[2]傅丛,连进京,姜英,等.高汞煤燃烧过程中汞的析出规律试验研究[J].洁净煤技术,2007,13(6):62-65.
[3]李婷婷.贵州典型高汞煤温和热解过程中汞的释放及形态转化规律的研究[D].武汉:华中科技大学,2011:45-50.
[4]路文芳,田宇,战景明,等.我国大气汞污染对人体健康的影响[J].环境与健康杂志,2012,29(8):761.
[5]代世峰,任德贻,李丹,等.贵州大方煤田主采煤层的矿物学异常及其对元素地球化学的影响[J].地质学报,2006,80(4):589-597.
[6]黄晓雨,郑刘根,张强伟,等.卧龙湖煤矿岩浆蚀变煤层中汞的分布与赋存特征[J].高校地质学报,2015,21(2):280-287.
[7]姜萌萌.淮北卧龙湖岩浆侵入区煤中微量元素赋存规律与应用研究[D].合肥:中国科学技术大学,2011:56-62.
[8]Finkleman R.Health Impacts of Coal Combustion[J].Center for Integrated Data Analytics Wisconsin Science Center,2000:1-4.
[9]任德贻,赵峰华,张军营,等.煤中有害微量元素富集的成因类型初探[J].地学前缘,1999,6(5):17-22.
[10]郑刘根,刘桂建,齐翠翠,等.中国煤中汞的环境地球化学研究[J].中国科学技术大学学报,2007,37(8):953-963.
[11]曾凡桂,谢克昌.煤结构化学的理论体系与方法论[J].煤炭学报,2004,29(4):443-447.
[12]梁虎珍,王传格,曾凡桂,等.应用红外光谱研究脱灰对伊敏褐煤结构的影响[J].燃料化学学报,2014,42(2):129-137.
[13]刘大锰,杨起,汤达祯,等.华北晚古生代煤中硫及微量元素分布赋存规律[J].煤炭科学技术,2000,28(9):39-42.
[14]Tessier B,Reynaud J Y.Cataclysmic burial of Pennsylvanian Period coal swamps in the Illinois Basin[C]∥Contributions to Modern and Ancient Tidal Sedimentology:Proceedings of the Tidalites 2012 conference.John Wiley&Sons,Ltd,2016:102-110.
[15]丰芸,李寒旭,丁立明.利用XRD分析高温下淮南煤灰矿物质变化[J].安徽建筑大学学报,2008,16(5):53-57.
[16]刘国根,邱冠周,胡岳华.煤的红外光谱研究[J].中南大学学报(自然科学版),1999(4):371-373.
[17]邢莹莹.辽宁抚顺煤精官能团表征及热变异行为[J].光谱学与光谱分析,2017,37(6):1819-1825.