废物焚烧及工业金属冶炼烟气中二噁英的排放水平及同系物分布
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摘要
为掌握二噁英(PCDD/Fs)排放重点行业的二噁英排放特性与工艺影响因素,为相关行业的二噁英排放治理提供基础性数据支持,采用同位素稀释高分辨气相色谱质谱法对生活垃圾焚烧(MWI)、危险废物焚烧(HWI)、再生有色金属冶炼(SNP)和铁矿石烧结(SNT)烟气中的二噁英的排放特征进行比较,并讨论了物料组成、含氧量、含氯量、催化离子、尾气处理装置及处理量对二噁英排放特征的影响。结果表明,生活废弃物焚烧排放烟气质量浓度最低,危险废弃物燃烧、再生有色金属冶炼次之,铁矿石烧结烟气的二噁英质量浓度最高。危险废物焚烧、再生有色金属冶炼和铁矿石烧结三者烟气中二噁英的同系物分布吻合度较高,均以PCDFs为主,推断二噁英的合成机理均以从头合成为主。4种烟气来源的氯化度均高于6,主要为高氯代产物。物料来源与组成的复杂性为二噁英提供了良好的合成环境。高含氧量及使用水幕除尘装置会增加二噁英的生成,但含氧量约高于18%时可抑制PCDD/Fs的产生。而高含氯量和高含量的催化金属离子则有助于PCDFs的生成。
This paper is aimed to present an analysis of 25 groups of flue gas monitoring data in the different industries in Chongqing in hoping to work out the dioxin emission profiles and the processing influential factors of dioxin( PCCD/Fs) emission in the principal industrial branches and provide a basic data support for its emission management strategy. The said principal industrial branches are the municipal solid waste incinerator( MWI),the hazardous waste incinerator( HWI),the secondary nonferrous production( SNP),and the iron ore sinter( SNT),the top of the 4 branches belonging to the greatest dioxins emission ones in the country. While it is hoped to test and measure the concentrations of the 17 kinds of PCDD/Fs through the isotope dilution high resolution so as to work out the gas chromatography mass spectrometry,it is necessary to identify and determine the emission profile and the corresponding influential factors of PCDD/Fs through analyzing the similarities and differences of the data from the aforementioned 4 branches of industries. So far as we know,the lowest PCDD/Fs concentrations can be found in the flue gas from MWI,followed by HWI and SNP. Among them,the highest dioxin concentration rates have been discovered in the flue gas from the SNT. In comparison with the domestic and international research results,the dioxin concentration rates of the said 4 industries can be regarded as in the intermediate level,in which HWI,SNP and SNT can be assessed of a similar dioxin emission feature,with PCDFs( especially with 1,2,3,4,6,7,8-Hp CDF) being of the major pollutants, for whose synthesis mechanism is generally taken as de novo synthesis. All the above mentioned 4 types of dioxin source consist of high chlorinated dioxin,with an average chlorination pollution level being higher than 6. Besides,the paper has also made a further discussion of the effects of its material composition of chlorinity,the oxygen content,the catalytic ions,the tail-gas treatment and handling capacity. Since the impurities of the dioxin source enjoy a better material condition for the dioxin synthesis,it is favorable for such synthesis. What is more,its high oxygen content is also beneficial for PCDD/Fs formulation.In spite of this,if the oxygen content is beyond 18%,it would be possible to impede the formation of dioxin. In such a case,it would be convenient to promote the dioxin emission concentration with a water dedusting device as the tail-gas treatment promoter,compared with a bag filter. High catalytic ion content rate and high chlorinity rate can then be found to promote the PCDFs generation. In addition,since the handling capacity ought to serve as a complicated influential factor,it wouldn't be easy to forecast the dioxin emission rate accurately in case to make profit of its handling capacity only.
This paper is aimed to present an analysis of 25 groups of flue gas monitoring data in the different industries in Chongqing in hoping to work out the dioxin emission profiles and the processing influential factors of dioxin( PCCD/Fs) emission in the principal industrial branches and provide a basic data support for its emission management strategy. The said principal industrial branches are the municipal solid waste incinerator( MWI),the hazardous waste incinerator( HWI),the secondary nonferrous production( SNP),and the iron ore sinter( SNT),the top of the 4 branches belonging to the greatest dioxins emission ones in the country. While it is hoped to test and measure the concentrations of the 17 kinds of PCDD/Fs through the isotope dilution high resolution so as to work out the gas chromatography mass spectrometry,it is necessary to identify and determine the emission profile and the corresponding influential factors of PCDD/Fs through analyzing the similarities and differences of the data from the aforementioned 4 branches of industries. So far as we know,the lowest PCDD/Fs concentrations can be found in the flue gas from MWI,followed by HWI and SNP. Among them,the highest dioxin concentration rates have been discovered in the flue gas from the SNT. In comparison with the domestic and international research results,the dioxin concentration rates of the said 4 industries can be regarded as in the intermediate level,in which HWI,SNP and SNT can be assessed of a similar dioxin emission feature,with PCDFs( especially with 1,2,3,4,6,7,8-Hp CDF) being of the major pollutants, for whose synthesis mechanism is generally taken as de novo synthesis. All the above mentioned 4 types of dioxin source consist of high chlorinated dioxin,with an average chlorination pollution level being higher than 6. Besides,the paper has also made a further discussion of the effects of its material composition of chlorinity,the oxygen content,the catalytic ions,the tail-gas treatment and handling capacity. Since the impurities of the dioxin source enjoy a better material condition for the dioxin synthesis,it is favorable for such synthesis. What is more,its high oxygen content is also beneficial for PCDD/Fs formulation.In spite of this,if the oxygen content is beyond 18%,it would be possible to impede the formation of dioxin. In such a case,it would be convenient to promote the dioxin emission concentration with a water dedusting device as the tail-gas treatment promoter,compared with a bag filter. High catalytic ion content rate and high chlorinity rate can then be found to promote the PCDFs generation. In addition,since the handling capacity ought to serve as a complicated influential factor,it wouldn't be easy to forecast the dioxin emission rate accurately in case to make profit of its handling capacity only.
引文
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[5]KONG Sifang(孔丝纺),LIU Hui(刘惠),ZENG Hui(曾辉),et al.The mechanism and influence factors of dioxin formation during asste incineration[J].Environmental Engineering(环境工程),2012,30(S2):249-254.
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[8]RAO Qinquan(饶钦全),WANG Hui(王晖),XU Fangxi(徐方曦).Study on monitoring and sampling of dioxin in exhaust gas from pollution sources[J].Environmental Science and Management(环境科学与管理),2017,42(7):116-120.
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[11]ZHAO Wei(赵伟),SONG Hongjun(宋红军),ZHANG Lijuan(张丽娟),et al.Polychlorinated dibenzo-p-dioxins/furans in fly ash from a secondary aluminum metallurgy factory[J].Environmental Pollution and Control(环境污染与防治),2016,38(2):59-62.
[12]LU Yi(卢益),ZHANG Xiaoling(张晓岭),GUO Zhishun(郭志顺),et al.Atmospheric emission of PCDD/Fs from secondary aluminum metallurgy industry in the Southwest Area,China[J].Environmental Science(环境科学),2014,35(1):30-34.
[13]FISHER R,FRAY T A T,ANDERSON D R.Investigation of the formation of dioxins in the sintering process[C]∥The Chinese Society for Metals.Proceedings of 2nd International Congress on the Science and Technology of Ironmaking and 57th Ironmaking Conference.Beijing:The Chinese Society for Metals,1998:1183-1193.
[14]WU H L,LU S Y,YAN J H,et al.Thermal removal of PCDD/Fs from medical waste incineration fly ash—effect of temperature and nitrogen flow rate[J].Chemosphere,2011,84(3):361-367.
[15]HJ 77.2—2008 Ambient air and flue gas—determination of polychlorinated dibenzo-p-dioxins(PCDDS)and polychlorinated dibenzofurans(PCDFs)—isotope dilution HRGC-HRMS(环境空气和废气——二噁英类的测定——同位素稀释高分辨气相色谱-高分辨质谱法)[S].
[16]YU Mingfeng(俞明锋),FU Jianying(付建英),ZHAN Mingxiu(詹明秀),et al.The research of PCDD/Fs emission characteristics in flue gas from municipal solid waste incinerations[J/OL].Acta Scientiae Circumstantiae(环境科学学报),2018,38(5):1983-1988.
[17]LIN W Y,WU Y L,TU L K,et al.The emission and distribution of PCDD/Fs in municipal solid waste incinerators and coal-fired power plant[J].Aerosol&Air Quality Research,2010,10(6):519-532.
[18]LIU Jinsong(刘劲松),LIU Weiping(刘维屏),GONG Hongping(巩宏平),et al.Source identification for PCDD/Fs in ambient air and soil in the vicinity of a municipal solid waste incinerator[J].Acta Scientiae Circumstantiae(环境科学学报),2010,30(10):1950-1956.
[19]YANG Yanyan(杨艳艳),HAN Jinglei(韩静磊),QING Xian(青宪),et al.PCDD/Fs pollutions in exhaust gases from typical industries of the Pearl River Delta[J].China Environmental Science(中国环境科学),2013,33(S1):186-190.
[20]ZHAN M,CHEN T,LIN X,et al.Suppression of dioxins after the post-combustion zone of MSWIs[J].Waste Management,2016,54:153-161.
[21]CHEN Jia(陈佳),CHEN Tong(陈彤),WANG Qi(王奇),et al.PCDD/Fs emission levels of hazardous and medical waste incineration in China[J].Acta Scientiae Circumstantiae(环境科学学报),2014,34(4):973-979.
[22]FERRHUGUET N,NADAL M,SCHUHMACHER M,et al.Environmental impact and human health risks of polychlorinated dibenzo-p-dioxins and dibenzofurans in the vicinity of a new hazardous waste incinerator:a case study[J].Environmental Science&Technology,2006,40(1):61-66.
[23]BA T,ZHENG M,ZHANG B,et al.Estimation and characterization of PCDD/Fs and dioxin-like PCBs from secondary copper and aluminum metallurgies in China[J].Chemosphere,2009,75(9):1173-1178.
[24]LI H W,LEE W J,HUANG K L,et al.Effect of raw materials on emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans from the stack flue gases of secondary aluminum smelters[J].Journal of Hazardous Materials,2007,147(3):776-784.
[25]AITTOLA J P,PAASIVIRTA J,VATTULAINEN A,et al.Formation of chloroaromatics at a metal reclamation plant and efficiency of stack filter in their removal from emission[J].Chemosphere,1996,32(1):99-108.
[26]CHEN Zurui(陈祖睿),YAN Mi(严密),BAI Sihong(白四红),et al.Inhibition effect of thiourea on dioxin emission from iron ore sintering process[J].Energy Engineering(能源工程),2014,(4):48-52.
[27]BOSCOLO M,PADOANO E.Investigations into dioxin emissions at Italian iron ore sintering plant[J].Ironmaking&Steelmaking,2013,35(5):338-342.
[28]JIANG T,HWANG J Y,SCHLESINGER M E,et al.Comprehensive emission reduction of sintering exhaust gas pollutant with addition of urea[M].Hoboken:John Wiley&Sons,Inc.,2014:353-360.
[29]ANDERSON D R,FISHER R,JOHNSTON S,et al.Investigation into the effect of organic nitrogen compounds on the suppression of PCDD/Fs in iron ore sintering[J].Organohalogen Compounds,2007,69:2470-2473.
[30]GB 18485—2014 Standard for pollution control on the municipal solid waste incineration(生活垃圾焚烧污染物控制标准)[S].
[31]GB 18484—2001 Pollution control standard for hazardous wastes incineration(生活垃圾焚烧污染物控制标准)[S].
[32]GB 31574—2015 Emission standards of pollutants for secondary copper,aluminum,lead and zink industry(再生铜、铝、锌、铅工业污染物排放标准)[S].
[33]GB 28662—2012 Emission standard of pollutants for sintering and pelletizing of iron and steel(钢铁烧结、球团工业大气污染物排放标准)[S].
[34]YUE Changsheng(岳昌盛),PENG Ben(彭犇),ZHANG Yibo(张艺伯),et al.Research process of dioxin emission reduction in metallurgical sintering process[J].Environmental Engineering(环境工程),2015,33(12):155-158.
[35]EVERAERT K,BAEYENS J.The formation and emission of dioxins in large scale thermal processes[J].Chemosphere,2002,46(3):439-448.
[36]HUNG P C,CHANG S H,BUEKENS A,et al.Continuous sampling of MSWI dioxins[J].Chemosphere,2016,145:119-124.
[37]THOMPSON D,OOI T C,ANDERSON D R,et al.The polychlorinated dibenzofuran fingerprint of iron ore sinter plant:Its persistence with suppressant and alternative fuel addition[J].Chemosphere,2016,154:138-147.
[38]WANG Mengjing(王梦京),WU Susu(吴素愫),GAO Xinhua(高新华),et al.Formation mechanism and emission profiles of PCDD/Fs in iron ore sintering[J].Environmental Chemistry(环境化学),2014,33(10):1723-1732.
[39]STANMORE B R.The formation of dioxins in combustion systems[J].Combustion&Flame,2004,136(3):398-427.
[40]ADDINK R,OLIE K.Mechanisms of formation and destruction of polychlorinated dibenzo-p-dioxins and dibenzofurans in heterogeneous systems[J].Environmental Science&Technology,1995,29(6):1425-1435.
[41]HUANG H,BUEKENS A.On the mechanisms of dioxin formation in combustion processes[J].Chemosphere,1995,31(9):4099-4117.
[42]REN Yue(任玥),TIAN Honghai(田洪海),LI Nan(李楠),et al.Analysis of the influencing factors for dioxin emission from municipal solid waste incinerators by the analytic hierarchy process[J].Environmental Chemistry(环境化学),2011,30(1):391-398.
[43]ZHANG Hailong(张海龙),LI Xiangping(李祥平),QI Jianying(齐剑英),et al.Analysis of composition characteristics of municipal solid waste in South China[J].Environmental Science(环境科学),2015,36(1):325-332.
[44]LI Jialing(李家玲),ZHANG Zhengjie(张正洁).Causes of dioxin generation during secondary aluminum production process and the whole process pollution control technology[J].Environmental Protection Science(环境保护科学),2013,39(2):42-46.
[45]WANG L C,LEE W J,LEE W S,et al.Effect of chlorine content in feeding wastes of incineration on the emission of polychlorinated dibenzo-p-dioxins/dibenzofurans[J].Science of the Total Environment,2003,302(1/2/3):185-198.
[46]TANG Yuhui(唐雨慧),REN Man(任曼).Distribution characteristic of PCDD/Fs and PBDD/Fs in flue gas from municipal solid waste incinerators[J].Environmental Engineering(环境工程),2015,33(11):78-82.
[47]LI Dinglong(李定龙),WANG Kaiquan(王凯全).Solid waste disposals and environmental dioxins[J].Journal of Changzhou University:Natural Science Edition(常州大学学报:自然科学版),2001,13(2):62-65.
[2]FIEDLER H.National PCDD/PCDF release inventories under the Stockholm convention on persistent organic pollutants[J].Chemosphere,2007,67(9):96-108.
[3]ZHENG Minghui(郑明辉),SUN Yangzhao(孙阳昭),LIU Wenbin(刘文彬).Study of China dioxin persistent organic pollutant emission inventory(中国二噁英类持久性有机污染物排放清单研究)[M].Beijing:China Environmental Science Press,2008.
[4]OLIE K,VERMEULEN P L,HUTZINGER O.Chlorodibenzo-pdioxins and chlorodibenzofurans are trace components of fly ash and flue gas of some municipal incinerators in The Netherlands[J].Chemosphere,1977,6(8):455-459.
[5]KONG Sifang(孔丝纺),LIU Hui(刘惠),ZENG Hui(曾辉),et al.The mechanism and influence factors of dioxin formation during asste incineration[J].Environmental Engineering(环境工程),2012,30(S2):249-254.
[6]TONG H Y,KARASEK F W.Comparison of PCDD and PCDF in flyash collected from muncipal incinerators of different countries[J].Chemosphere,1986,15(9/10/11/12):1219-1224.
[7]BRENNER K S,MADER H,STEVERLE H,et al.Dioxin analysis in stack emissions and in the wash water circuit during high-temperature incineration of chlorine-containing industrial wastes[J].Bulletin of Environmental Contamination and Toxicology,1984,33(1):153-162.
[8]RAO Qinquan(饶钦全),WANG Hui(王晖),XU Fangxi(徐方曦).Study on monitoring and sampling of dioxin in exhaust gas from pollution sources[J].Environmental Science and Management(环境科学与管理),2017,42(7):116-120.
[9]VERMEULEN I,CANEGHEM J V,VANDECASTEELE C.Indication of PCDD/F formation through precursor condensation in a full-scale hazardous waste incinerator[J].Journal of Material Cycles&Waste Management,2014,16(1):167-171.
[10]KARADEMIR A.Health risk assessment of PCDD/F emissions from a hazardous and medical waste incinerator in Turkey[J].Environment International,2004,30(8):1027-1038.
[11]ZHAO Wei(赵伟),SONG Hongjun(宋红军),ZHANG Lijuan(张丽娟),et al.Polychlorinated dibenzo-p-dioxins/furans in fly ash from a secondary aluminum metallurgy factory[J].Environmental Pollution and Control(环境污染与防治),2016,38(2):59-62.
[12]LU Yi(卢益),ZHANG Xiaoling(张晓岭),GUO Zhishun(郭志顺),et al.Atmospheric emission of PCDD/Fs from secondary aluminum metallurgy industry in the Southwest Area,China[J].Environmental Science(环境科学),2014,35(1):30-34.
[13]FISHER R,FRAY T A T,ANDERSON D R.Investigation of the formation of dioxins in the sintering process[C]∥The Chinese Society for Metals.Proceedings of 2nd International Congress on the Science and Technology of Ironmaking and 57th Ironmaking Conference.Beijing:The Chinese Society for Metals,1998:1183-1193.
[14]WU H L,LU S Y,YAN J H,et al.Thermal removal of PCDD/Fs from medical waste incineration fly ash—effect of temperature and nitrogen flow rate[J].Chemosphere,2011,84(3):361-367.
[15]HJ 77.2—2008 Ambient air and flue gas—determination of polychlorinated dibenzo-p-dioxins(PCDDS)and polychlorinated dibenzofurans(PCDFs)—isotope dilution HRGC-HRMS(环境空气和废气——二噁英类的测定——同位素稀释高分辨气相色谱-高分辨质谱法)[S].
[16]YU Mingfeng(俞明锋),FU Jianying(付建英),ZHAN Mingxiu(詹明秀),et al.The research of PCDD/Fs emission characteristics in flue gas from municipal solid waste incinerations[J/OL].Acta Scientiae Circumstantiae(环境科学学报),2018,38(5):1983-1988.
[17]LIN W Y,WU Y L,TU L K,et al.The emission and distribution of PCDD/Fs in municipal solid waste incinerators and coal-fired power plant[J].Aerosol&Air Quality Research,2010,10(6):519-532.
[18]LIU Jinsong(刘劲松),LIU Weiping(刘维屏),GONG Hongping(巩宏平),et al.Source identification for PCDD/Fs in ambient air and soil in the vicinity of a municipal solid waste incinerator[J].Acta Scientiae Circumstantiae(环境科学学报),2010,30(10):1950-1956.
[19]YANG Yanyan(杨艳艳),HAN Jinglei(韩静磊),QING Xian(青宪),et al.PCDD/Fs pollutions in exhaust gases from typical industries of the Pearl River Delta[J].China Environmental Science(中国环境科学),2013,33(S1):186-190.
[20]ZHAN M,CHEN T,LIN X,et al.Suppression of dioxins after the post-combustion zone of MSWIs[J].Waste Management,2016,54:153-161.
[21]CHEN Jia(陈佳),CHEN Tong(陈彤),WANG Qi(王奇),et al.PCDD/Fs emission levels of hazardous and medical waste incineration in China[J].Acta Scientiae Circumstantiae(环境科学学报),2014,34(4):973-979.
[22]FERRHUGUET N,NADAL M,SCHUHMACHER M,et al.Environmental impact and human health risks of polychlorinated dibenzo-p-dioxins and dibenzofurans in the vicinity of a new hazardous waste incinerator:a case study[J].Environmental Science&Technology,2006,40(1):61-66.
[23]BA T,ZHENG M,ZHANG B,et al.Estimation and characterization of PCDD/Fs and dioxin-like PCBs from secondary copper and aluminum metallurgies in China[J].Chemosphere,2009,75(9):1173-1178.
[24]LI H W,LEE W J,HUANG K L,et al.Effect of raw materials on emissions of polychlorinated dibenzo-p-dioxins and dibenzofurans from the stack flue gases of secondary aluminum smelters[J].Journal of Hazardous Materials,2007,147(3):776-784.
[25]AITTOLA J P,PAASIVIRTA J,VATTULAINEN A,et al.Formation of chloroaromatics at a metal reclamation plant and efficiency of stack filter in their removal from emission[J].Chemosphere,1996,32(1):99-108.
[26]CHEN Zurui(陈祖睿),YAN Mi(严密),BAI Sihong(白四红),et al.Inhibition effect of thiourea on dioxin emission from iron ore sintering process[J].Energy Engineering(能源工程),2014,(4):48-52.
[27]BOSCOLO M,PADOANO E.Investigations into dioxin emissions at Italian iron ore sintering plant[J].Ironmaking&Steelmaking,2013,35(5):338-342.
[28]JIANG T,HWANG J Y,SCHLESINGER M E,et al.Comprehensive emission reduction of sintering exhaust gas pollutant with addition of urea[M].Hoboken:John Wiley&Sons,Inc.,2014:353-360.
[29]ANDERSON D R,FISHER R,JOHNSTON S,et al.Investigation into the effect of organic nitrogen compounds on the suppression of PCDD/Fs in iron ore sintering[J].Organohalogen Compounds,2007,69:2470-2473.
[30]GB 18485—2014 Standard for pollution control on the municipal solid waste incineration(生活垃圾焚烧污染物控制标准)[S].
[31]GB 18484—2001 Pollution control standard for hazardous wastes incineration(生活垃圾焚烧污染物控制标准)[S].
[32]GB 31574—2015 Emission standards of pollutants for secondary copper,aluminum,lead and zink industry(再生铜、铝、锌、铅工业污染物排放标准)[S].
[33]GB 28662—2012 Emission standard of pollutants for sintering and pelletizing of iron and steel(钢铁烧结、球团工业大气污染物排放标准)[S].
[34]YUE Changsheng(岳昌盛),PENG Ben(彭犇),ZHANG Yibo(张艺伯),et al.Research process of dioxin emission reduction in metallurgical sintering process[J].Environmental Engineering(环境工程),2015,33(12):155-158.
[35]EVERAERT K,BAEYENS J.The formation and emission of dioxins in large scale thermal processes[J].Chemosphere,2002,46(3):439-448.
[36]HUNG P C,CHANG S H,BUEKENS A,et al.Continuous sampling of MSWI dioxins[J].Chemosphere,2016,145:119-124.
[37]THOMPSON D,OOI T C,ANDERSON D R,et al.The polychlorinated dibenzofuran fingerprint of iron ore sinter plant:Its persistence with suppressant and alternative fuel addition[J].Chemosphere,2016,154:138-147.
[38]WANG Mengjing(王梦京),WU Susu(吴素愫),GAO Xinhua(高新华),et al.Formation mechanism and emission profiles of PCDD/Fs in iron ore sintering[J].Environmental Chemistry(环境化学),2014,33(10):1723-1732.
[39]STANMORE B R.The formation of dioxins in combustion systems[J].Combustion&Flame,2004,136(3):398-427.
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