煤热解中微量元素迁移规律的再探索
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摘要
为探寻煤热解过程中微量元素活动的普适规律,对河南义马煤和山东兖州煤在不同温度下热解时煤的微量元素迁移规律进行了再探索。结果发现:在非自然的人工煤热解过程中,煤中微量元素的挥发率和富集率变化趋势总体上符合元素周期律。并据此,在1 000℃以下的范围内,对河南义马煤的难挥发元素分为3类:第1类,为最难挥发的元素,有V,Cr,Co,Cu,Ga,Zr,La,Pr,Nd,Tm等10个元素;第2类,为难挥发元素,有稀土元素Sm,Eu,Gd,Tb,Dy,Ho,Ta等7个元素;第3类,为较难挥发的元素,有Li,Ge,Nb,Mo,Er等5个元素。在煤热解过程中,镧系元素的转化总体上也遵从镧系元素地球化学效应。
The re-exploration about the law of trace elements migration during pyrolysis of coal samples,which were collected from Yima mining and Yanzhou,mining districts,were done by authors for studying pervasive law of trace element activity in this processes. It was discovered that in general,change trend on evaporation rate and enrichment rate of trace elements in coal,during the pyrolysis of coal,are comply with periodic law of elements. For this reason,difficult volatile elements in coal from Yima mining were divided into three categories within 1 000 ℃. V,Cr,Co,Cu,Ga,Zr,La,Pr,Nd,Tm are most difficult elements in volatile which belongs to the first sort one; Second sort of elements,there are 7 elements from Sm to Ho in REE and Ta,are more difficult ones; the third sorts of elements are relatively difficult ones in which there are Li,Ge,Nb,Mo,Er. In pyrolysis of coal,transformation of the lanthanide obeys geochemical effect of rare earth elements( REE).
The re-exploration about the law of trace elements migration during pyrolysis of coal samples,which were collected from Yima mining and Yanzhou,mining districts,were done by authors for studying pervasive law of trace element activity in this processes. It was discovered that in general,change trend on evaporation rate and enrichment rate of trace elements in coal,during the pyrolysis of coal,are comply with periodic law of elements. For this reason,difficult volatile elements in coal from Yima mining were divided into three categories within 1 000 ℃. V,Cr,Co,Cu,Ga,Zr,La,Pr,Nd,Tm are most difficult elements in volatile which belongs to the first sort one; Second sort of elements,there are 7 elements from Sm to Ho in REE and Ta,are more difficult ones; the third sorts of elements are relatively difficult ones in which there are Li,Ge,Nb,Mo,Er. In pyrolysis of coal,transformation of the lanthanide obeys geochemical effect of rare earth elements( REE).
引文
[1]李美芬,曾凡桂,孙蓓蕾,等.低煤级煤热解H2生成动力学及其与第一次煤化作用跃变的关系[J].物理化学学报,2009,25(12):2597-2603.Li Meifen,Zeng Fangui,Sun Beilei,et al.Evolution kinetic of hydrogen generation from low rank coal pyrolysis and its relation to the first coalification junp[J].Acta Physico-Chimica Sinica,2009,25(12):2597-2603.
[2]周淑芬,杨建丽,刘振宇.煤热解过程焦中硫的残留及煤中硅、铝、碳的研究[J].燃料化学学报,2010,38(6):652-655.Zhou Shufen,Yang Jianli,Liu Zhenyu.Sulfur retention in char during coal pyrolysis and influence of silicon,aluminum and carbon in coal[J].Journal of Fuel Chemistry and Technology,2010,38(6):652-655.
[3]段钰锋,刘玲,王卉,等.煤热解过程中汞析出与汞吸附特性研究[J].太原理工大学学报,2010,41(5):619-626.Duan Yufeng,Liu ling,Wang Hui,et al.Experiment study on mercury release and adsorption during coal pyrolysis[J].Journal of Taiyuan University of Technology,2010,41(5):619-626.
[4]谢建军,杨学民,吕雪松,等.煤热解过程中硫氮分配及迁移规律研究进展[J].化工进展,2004,23(11):1214-1218.Xie Jianjun,Yang Xuemin,LüXuesong,et al.Progress on transformation behavior of sulfur and nitrogenduring coal prolysis[J].Chemical Industry and Engineering Progress,2004,23(11):1214-1218.
[5]赵炜,常丽萍,冯志华,等.煤热解过程中生成氮化物的研究[J].燃料化学学报,2002,30(5):408-412.Zhao Wei,Chang Liping,Feng Zhihua,et al.Formation of nitrogenous species during coal pyrolysis[J].Journal of Fuel Chemistry and Technology,2002,30(5):408-412.
[6]骆艳华,崔平,胡润桥.义马煤的热解及产物分布的研究[J].安徽工业大学学报,2006,23(2):160-168.Luo Yanhua,Cui Ping,Hu Runqiao.Research of Yima coal pyrolysis and its products range[J].Journal of Anhui University of Technology,2006,23(2):160-168.
[7]鞠付栋,陈汉平,杨海平,等.不同变质煤热解和气化中燃料氮的转化规律[J].煤炭转化,2011,34(3):21-26.Ju Fudong,Chen Hanping,Yang Haiping,et al.Fuel nitrogen evolution of different coal rank during pyrolysis and gasification[J].Coal Conversion,2011,34(3):21-26.
[8]魏晓飞,张国平,李玲,等.黔西南高砷煤热解过程中微量元素释放规律研究[J].中国环境科学,2011,31(12):2005-2012.Wei Xiaofei,Zhang Guoping,Li Ling,et al.volatility of trace elements during pyrolysis of high arsenic coal from southwestern Guizhou[J].China Environmental Science,2011,31(12):2005-2012.
[9]吴爱坪,潘铁英,史新梅,等.中低阶煤热解过程中自由基的研究[J].煤炭转化,2012,35(2):1-5.Wu Aiping,Pan Tieying,Shi Xinmei,et al.Study on free radicals in low rank coal pyrolysis process[J].CoalConversion,2012,35(2):1-5.
[10]王锦平,张德祥,高晋生.煤热解过程中氯的脱除研究[J].煤炭学报,2002,27(4):402-405.Wang Jinping,Zhang Dexiang,Gao Jinsheng.Chlorine removal on the process of coal pyrolysis[J].Journal of China Coal Society,2002,27(4):402-405.
[11]王云鹤,李海滨,黄海涛,等.重金属元素在煤热解过程中的分布迁移规律[J].煤炭转化,2002,25(3):37-42.Wang Yunhe,Li Haibin,Huang Haitao,et al.Distribution and transport of heavy metal elements during coal pyrolysis[J].Coal Conversion,2002,25(3):37-42.
[12]尹浩,刘桂建,刘静静.煤热解过程中含硫气体的释放特征[J].环境化学,2012,31(3):330-334.Yin Hao,Liu Guijian,Liu Jingjing.Release of sulfur containing gases during coal pyrolysis[J].Environmental Chemistry,2012,31(3):330-334.
[13]杨会民,王美君,张玉龙,等.添加物对宁夏煤热解气相产物生成的影响[J].煤炭学报,2010,35(8):1364-1368.Yang Huimin,Wang Meijun,Zhang Yulong,et al.Effect on addictives of Ningxia coal pyrolysis behavior[J].Journal of China Coal Society,2010,35(8):1364-1368.
[14]张永发,张慧荣,田芳,等.无烟粉煤成型块炭化行为及热解气体生成规律[J].煤炭学报,2011,36(4):670-675.Zhang Yongfa,Zhang Huirong,Tian Fang,et al.The characteristics of anthracite briquette carbonization and regularity of pyrolysis gas generation during carbonization[J].Journal of China Coal Society,2011,36(4):670-675.
[15]Chen Yiwei,Liu Guijian,Gong Yanming,et al.Release and enrichment of 44 elements during coal pyrolysis of Yima coal,China[J].Journal of Analytical and Applied Pyrolysis,2007,80:283-288.
[16]陈怡伟.热解过程煤中某些微量元素转化行为研究[D].合肥:中国科技大学,2008.
[17]黄文辉,杨起.燃煤过程中有害元素转化机理研究进展[J].地质科技情报,1999,18(1):71-74.Huang Wenhui,Yang Qi.Novel development of study on the transformation mechanism of hazard elements during coal combustion[J].Geological Science and Technology Information,1999,18(1):71-74.
[18]Yang Jianye.The periodic law of trace elements in coal—A case study of the No.5 coal from the Weibei Coalfield[J].Science China,2011,54(10):1542-1550.
[19]崔晓丽,童汝亭.元素标准摩尔规定熵值周期表[J].化学研究与应用,1998,10(3):320-322.Cui Xiaoli,Tong Ruting.Periodic table for standard molar convention entropy of elements[J].Chemical Research and Application,1998,18(3):320-332.
[20]杨建业.镧系元素的煤地化效应——以渭北中熟煤为例[J].中国稀土学报,2008,26(4):486-490.Yang Jianye.The effect on coal-geochemistry of rare earth elements——An example of middle rank coal from Weibei[J].Journal of Rare Earths,2008,26(4):486-490.
[2]周淑芬,杨建丽,刘振宇.煤热解过程焦中硫的残留及煤中硅、铝、碳的研究[J].燃料化学学报,2010,38(6):652-655.Zhou Shufen,Yang Jianli,Liu Zhenyu.Sulfur retention in char during coal pyrolysis and influence of silicon,aluminum and carbon in coal[J].Journal of Fuel Chemistry and Technology,2010,38(6):652-655.
[3]段钰锋,刘玲,王卉,等.煤热解过程中汞析出与汞吸附特性研究[J].太原理工大学学报,2010,41(5):619-626.Duan Yufeng,Liu ling,Wang Hui,et al.Experiment study on mercury release and adsorption during coal pyrolysis[J].Journal of Taiyuan University of Technology,2010,41(5):619-626.
[4]谢建军,杨学民,吕雪松,等.煤热解过程中硫氮分配及迁移规律研究进展[J].化工进展,2004,23(11):1214-1218.Xie Jianjun,Yang Xuemin,LüXuesong,et al.Progress on transformation behavior of sulfur and nitrogenduring coal prolysis[J].Chemical Industry and Engineering Progress,2004,23(11):1214-1218.
[5]赵炜,常丽萍,冯志华,等.煤热解过程中生成氮化物的研究[J].燃料化学学报,2002,30(5):408-412.Zhao Wei,Chang Liping,Feng Zhihua,et al.Formation of nitrogenous species during coal pyrolysis[J].Journal of Fuel Chemistry and Technology,2002,30(5):408-412.
[6]骆艳华,崔平,胡润桥.义马煤的热解及产物分布的研究[J].安徽工业大学学报,2006,23(2):160-168.Luo Yanhua,Cui Ping,Hu Runqiao.Research of Yima coal pyrolysis and its products range[J].Journal of Anhui University of Technology,2006,23(2):160-168.
[7]鞠付栋,陈汉平,杨海平,等.不同变质煤热解和气化中燃料氮的转化规律[J].煤炭转化,2011,34(3):21-26.Ju Fudong,Chen Hanping,Yang Haiping,et al.Fuel nitrogen evolution of different coal rank during pyrolysis and gasification[J].Coal Conversion,2011,34(3):21-26.
[8]魏晓飞,张国平,李玲,等.黔西南高砷煤热解过程中微量元素释放规律研究[J].中国环境科学,2011,31(12):2005-2012.Wei Xiaofei,Zhang Guoping,Li Ling,et al.volatility of trace elements during pyrolysis of high arsenic coal from southwestern Guizhou[J].China Environmental Science,2011,31(12):2005-2012.
[9]吴爱坪,潘铁英,史新梅,等.中低阶煤热解过程中自由基的研究[J].煤炭转化,2012,35(2):1-5.Wu Aiping,Pan Tieying,Shi Xinmei,et al.Study on free radicals in low rank coal pyrolysis process[J].CoalConversion,2012,35(2):1-5.
[10]王锦平,张德祥,高晋生.煤热解过程中氯的脱除研究[J].煤炭学报,2002,27(4):402-405.Wang Jinping,Zhang Dexiang,Gao Jinsheng.Chlorine removal on the process of coal pyrolysis[J].Journal of China Coal Society,2002,27(4):402-405.
[11]王云鹤,李海滨,黄海涛,等.重金属元素在煤热解过程中的分布迁移规律[J].煤炭转化,2002,25(3):37-42.Wang Yunhe,Li Haibin,Huang Haitao,et al.Distribution and transport of heavy metal elements during coal pyrolysis[J].Coal Conversion,2002,25(3):37-42.
[12]尹浩,刘桂建,刘静静.煤热解过程中含硫气体的释放特征[J].环境化学,2012,31(3):330-334.Yin Hao,Liu Guijian,Liu Jingjing.Release of sulfur containing gases during coal pyrolysis[J].Environmental Chemistry,2012,31(3):330-334.
[13]杨会民,王美君,张玉龙,等.添加物对宁夏煤热解气相产物生成的影响[J].煤炭学报,2010,35(8):1364-1368.Yang Huimin,Wang Meijun,Zhang Yulong,et al.Effect on addictives of Ningxia coal pyrolysis behavior[J].Journal of China Coal Society,2010,35(8):1364-1368.
[14]张永发,张慧荣,田芳,等.无烟粉煤成型块炭化行为及热解气体生成规律[J].煤炭学报,2011,36(4):670-675.Zhang Yongfa,Zhang Huirong,Tian Fang,et al.The characteristics of anthracite briquette carbonization and regularity of pyrolysis gas generation during carbonization[J].Journal of China Coal Society,2011,36(4):670-675.
[15]Chen Yiwei,Liu Guijian,Gong Yanming,et al.Release and enrichment of 44 elements during coal pyrolysis of Yima coal,China[J].Journal of Analytical and Applied Pyrolysis,2007,80:283-288.
[16]陈怡伟.热解过程煤中某些微量元素转化行为研究[D].合肥:中国科技大学,2008.
[17]黄文辉,杨起.燃煤过程中有害元素转化机理研究进展[J].地质科技情报,1999,18(1):71-74.Huang Wenhui,Yang Qi.Novel development of study on the transformation mechanism of hazard elements during coal combustion[J].Geological Science and Technology Information,1999,18(1):71-74.
[18]Yang Jianye.The periodic law of trace elements in coal—A case study of the No.5 coal from the Weibei Coalfield[J].Science China,2011,54(10):1542-1550.
[19]崔晓丽,童汝亭.元素标准摩尔规定熵值周期表[J].化学研究与应用,1998,10(3):320-322.Cui Xiaoli,Tong Ruting.Periodic table for standard molar convention entropy of elements[J].Chemical Research and Application,1998,18(3):320-332.
[20]杨建业.镧系元素的煤地化效应——以渭北中熟煤为例[J].中国稀土学报,2008,26(4):486-490.Yang Jianye.The effect on coal-geochemistry of rare earth elements——An example of middle rank coal from Weibei[J].Journal of Rare Earths,2008,26(4):486-490.