基于实测的燃煤电厂氟排放特征
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摘要
选择我国4家电厂的6台煤粉锅炉,进行了烟气以及飞灰、底渣、脱硫石膏等燃煤副产物样品的采集和F(氟)含量分析,考察燃煤电厂F排放特征.结果表明:经过烟气除尘、脱硫及脱硝装置后,烟气中氟化物浓度明显降低;除尘器主要脱除烟气中颗粒态F,静电除尘器对烟气中氟化物的总脱除效率为19.50%~36.59%,布袋除尘器的脱除效率略高于静电除尘器;石灰石-石膏湿法脱硫装置可协同脱除烟气中94.19%的氟化物.燃煤中的F经过燃烧和烟气净化装置后,有0.83%~3.37%由底渣排放;1.20%~2.00%转移到脱硫废水中;13.45%~33.80%转移到飞灰中;59.60%~79.66%转移到脱硫石膏中;只有2.04%~5.00%通过烟囱排入大气.
Fluorine is a trace element in the coal and may cause environmental and human healthy problems during coal combustion.While coal-fired power plant is one of man-made sources of fluorine emissions in China,fluorine emission behaviors from coal-fired power plants have not been comprehensively investigated until now. A full-scale field study of fluorine emissions was conducted at six pulverized coal-fired boiler( PC) units of four coal-fired power plants in China. Flue gases were sampled from the inlets and outlets of the existing air pollutant control devices( APCDs) to investigate their effects on speciation and distribution of fluorine in the flue gas. Concurrent with flue gas,coal,bottom ash,fly ash and samples from the FGD process( desulfurization gypsum and waster water) were collected. Over96. 63% of fluorine contained in coal were released during the combustion process in the examined PC boilers,and fluorine compounds in flue gas were mainly in the form of HF. Wet FGD and dedusting devices were able to remove fluorine compounds in flue gas,wet FGD being more effective. Particulate bound fluorine in flue gas can be removed by dedusting devices. The removal efficiency of dedusting devices varied from 19. 50% to 36. 59% for fluorine compounds in flue gas. Bag-house filters were effective than electrostatic precipitators( ESP). Most of HF in flue gas can be removed by wet FGD devices and the average removal efficiency of wet FGD devices was 94. 19%.The fluorine released from coal combustion was transferred into slag,fly ash,desulfurization gypsum and the waste water after passing through the devices for air pollution control. Fluorine in slag ranged from 0. 83% to 3. 37%,and approximately about 13. 45%-33. 80%of fluorine were contained in fly ash. A proportion of 59. 60%-79. 66% of fluorine came into the gypsum while the waste water was kept1. 20%-2. 00% of the total fluorine. Only 2. 04%-5. 00% of fluorine were directly emitted into the atmosphere.
Fluorine is a trace element in the coal and may cause environmental and human healthy problems during coal combustion.While coal-fired power plant is one of man-made sources of fluorine emissions in China,fluorine emission behaviors from coal-fired power plants have not been comprehensively investigated until now. A full-scale field study of fluorine emissions was conducted at six pulverized coal-fired boiler( PC) units of four coal-fired power plants in China. Flue gases were sampled from the inlets and outlets of the existing air pollutant control devices( APCDs) to investigate their effects on speciation and distribution of fluorine in the flue gas. Concurrent with flue gas,coal,bottom ash,fly ash and samples from the FGD process( desulfurization gypsum and waster water) were collected. Over96. 63% of fluorine contained in coal were released during the combustion process in the examined PC boilers,and fluorine compounds in flue gas were mainly in the form of HF. Wet FGD and dedusting devices were able to remove fluorine compounds in flue gas,wet FGD being more effective. Particulate bound fluorine in flue gas can be removed by dedusting devices. The removal efficiency of dedusting devices varied from 19. 50% to 36. 59% for fluorine compounds in flue gas. Bag-house filters were effective than electrostatic precipitators( ESP). Most of HF in flue gas can be removed by wet FGD devices and the average removal efficiency of wet FGD devices was 94. 19%.The fluorine released from coal combustion was transferred into slag,fly ash,desulfurization gypsum and the waste water after passing through the devices for air pollution control. Fluorine in slag ranged from 0. 83% to 3. 37%,and approximately about 13. 45%-33. 80%of fluorine were contained in fly ash. A proportion of 59. 60%-79. 66% of fluorine came into the gypsum while the waste water was kept1. 20%-2. 00% of the total fluorine. Only 2. 04%-5. 00% of fluorine were directly emitted into the atmosphere.
引文
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[10]邓双,张辰,刘宇,等.基于实测的燃煤电厂氯排放特征[J].环境科学研究,2014,27(2):127-133.
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[20]齐庆杰,于贵生,刘建忠,等.石灰石石膏法烟气脱氟反应的动力学研究[J].燃料化学学报,2008,36(2):208-211.
[21]SILVA L F,JASPER A,ANDRADE M L,et al.Applied investigation on the interaction of hazardous elements binding on ultrafine and nano-particles in Chinese anthracite-derived fly ash[J].Sci Total Environ,2012,419:250-264.
[22]ALVAEWZ A E,QUEROL X.Stabilization of FGD gypsum for its disposal in landfills using amorphous aluminum oxide as a fluoride retention additive[J].Chemosphere,2007,69(2):295-302.
[23]CORDOBA P,FONT O,IZQUIERDO M,et al.Enrichment of inorganic trace pollutants in re-circulated water streams from a wet limestone flue gas desulphurisation system in two coal power plants[J].Fuel Processing Technology,2011,92:1764-1775.
[24]CORDOBA P,GONZALEZ R O,FONT O,et al.Partitioning of trace inorganic elements in a coal-fired power plant equipped with a wet flue gas desulphurisation system[J].Fuel,2012,92:145-157.
[25]SOLA P C,FONT O,IZQUIERDO M,et al.The retention capacity for trace elements by the flue gas desulphurisation system under operational conditions of a co-combustion power plant[J].Fuel,2012,102:773-778.
[26]国家环境保护总局.GB 16297—1996大气污染物综合排放标准[S].北京:中国标准出版社,1996.
[2]任德贻,赵峰华,代世峰,等.煤的微量元素地球化学[M].北京:科学出版社,2006.
[3]雒昆利,徐立荣,李日邦,等.中国华北地区和西北地区动力煤氟的排放量[J].科学通报,2002,47(11):873-876.
[4]陈成广,吴代赦,王五一,等.敞口地炉内燃烧煤泥饼时氟的逸出规律及控制[J].环境科学研究,2008,21(1):133-138.
[5]UKAWA N,OKINO S,IWAKI T.The effects of fluoride complexes in wet limestone flue gas desulfurization[J].Journal of Chemical Engineering of Japan,1992,25(2):146-151.
[6]齐庆杰,刘建忠,曹欣玉,等.煤燃烧过程中氟析出特性与生成机理[J].燃料化学学报,2003,31(5):400-404.
[7]刘建忠,齐庆杰,周俊虎,等.煤中氟化物在燃烧产物中的分布特征[J].环境科学,2003,24(4):127-130.
[8]LI Jing,ZHUANG Xinguo,QUEROL X,et al.Environmental geochemistry of the feed coals and their combustion by-products from two coal-fired power plants in Xinjiang Province,Northwest China[J].Fuel,2012,95:446-456.
[9]唐文伟,顾国维,曾新平.燃煤电厂氟的迁移转化与治理对策[J].环境保护,1999(2):13-15.
[10]邓双,张辰,刘宇,等.基于实测的燃煤电厂氯排放特征[J].环境科学研究,2014,27(2):127-133.
[11]国家环境保护总局.HJT 67—2001大气固定污染源F化物的测定离子选择电极法[S].北京:中国标准出版社,2001.
[12]US EPA.Determination of hydrogen halide and halogen emissions from stationary sources-isokinetic method,26A Method[S].Washington DC:US EPA,2001.
[13]US EPA.Determination of hydrogen halide and halogen emissions from stationary sources-non-isokinetic method,26 Method[S].Washington DC:US EPA,2001.
[14]李映日,邓双,王红梅,等.高温燃烧水解-淋洗液在线发生离子色谱法同时测定煤中氟和氯[J].环境工程,2011,29(5):130-134.
[15]BOUSKA V,PESEK J.Distribution of elements in the world lignite average and its comparison with lignite seams of the North Bohemian and Sokolov Basins[J].Geological,1999,42:1-51.
[16]CHOU C L.Abundances of sulfur,chlorine,and trace elements in Illinois Basin coals,USA[C]Proceedings of the 14thAnnual International Pittsburgh Coal Conference.Taiyuan:Taiyuan University of Technology:1997.
[17]吴代赦,郑宝山,唐修义,等.中国煤中氟的含量及其分布[J].环境科学,2005,26(1):7-11.
[18]TSUBOUCHI N,HAYASHI H,KAWASHIMA A,et al.Chemical forms of the fluorine and carbon in fly ashes recovered from electrostatic precipitator of pulverized coal-fired plants[J].Fuel,2011,90(1):376-383.
[19]CHENG C M,HACK P,CHU P,et al.Partitioning of mercury,Arsenic,Selenium,Boron and Chloride in a full-scale coal combustion process equipped with selective catalytic reduction,electrostatic precipitation,and flue gas desulfurization systems[J].Energy Fuels,2009,23(10):4805-4816.
[20]齐庆杰,于贵生,刘建忠,等.石灰石石膏法烟气脱氟反应的动力学研究[J].燃料化学学报,2008,36(2):208-211.
[21]SILVA L F,JASPER A,ANDRADE M L,et al.Applied investigation on the interaction of hazardous elements binding on ultrafine and nano-particles in Chinese anthracite-derived fly ash[J].Sci Total Environ,2012,419:250-264.
[22]ALVAEWZ A E,QUEROL X.Stabilization of FGD gypsum for its disposal in landfills using amorphous aluminum oxide as a fluoride retention additive[J].Chemosphere,2007,69(2):295-302.
[23]CORDOBA P,FONT O,IZQUIERDO M,et al.Enrichment of inorganic trace pollutants in re-circulated water streams from a wet limestone flue gas desulphurisation system in two coal power plants[J].Fuel Processing Technology,2011,92:1764-1775.
[24]CORDOBA P,GONZALEZ R O,FONT O,et al.Partitioning of trace inorganic elements in a coal-fired power plant equipped with a wet flue gas desulphurisation system[J].Fuel,2012,92:145-157.
[25]SOLA P C,FONT O,IZQUIERDO M,et al.The retention capacity for trace elements by the flue gas desulphurisation system under operational conditions of a co-combustion power plant[J].Fuel,2012,102:773-778.
[26]国家环境保护总局.GB 16297—1996大气污染物综合排放标准[S].北京:中国标准出版社,1996.