城市固体废物焚烧过程二噁英与重金属排放特征及控制技术研究
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摘要
本论文主要针对我国实际工程领域内废物焚烧过程中二噁英与重金属的排放与控制，开展了一系列内容丰富的研究工作，得到了一些具有现实指导意义的研究结论。本文主要研究内容如下：
（1）对全国范围内垃圾焚烧设施进行基础资料调研，统计出了具有代表性的二噁英排放水平数据，即排放区间为0.0042-7.90ng I-TEQ/Nm~3，平均为0.561ng I-TEQ/Nm~3，85%排放可达到现行的国家排放标准1.0ng I-TEQ/Nm~3。然后对我国不同地区的8家典型生活垃圾焚烧设施开展现状调研与全面监测工作，从区域分布、焚烧技术、运营管理水平等方面总体上阐述了我国典型生活垃圾焚烧设施特征污染物（二噁英、重金属）的排放水平与排放特征。
（2）对我国典型垃圾焚烧设施的二噁英、重金属产生与排放的影响因素进行了系统研究。首先考察了不同焚烧工艺、工况（正常与非正常）以及管理水平等对二噁英/重金属排放的影响，得到运营管理不善导致的非正常工况运行排放了最高浓度水平的二噁英，范围8.01-181.69ng I-TEQ/Nm~3，平均78.18ng I-TEQ/Nm~3，而非正常工况运行不一定能导致重金属排放的增加；其次分析了生活垃圾组成中关键成分（含水率、热值、氯、硫含量、重金属自身含量与理化特性等）对二噁英/重金属排放的影响；接着研究了污染控制中的关键技术（急冷设备与活性炭的投加）对二噁英/重金属排放的影响，得到急冷设备能有效地降低二噁英的排放，主要能够抑制低氯代二噁英的生成，活性炭吸附能力也主要体现在对烟气中的低氯代二噁英的移除，短期内未投加活性炭对重金属同样具备高的移除效率；最后研究了焚烧炉启动不同阶段二噁英生成与排放，结果表明，启动阶段二噁英的排放要高于正常运行的，其中在投料阶段二噁英的排放最高，在稳定阶段，由于记忆效应的作用，二噁英排放并不能立刻降到正常值。
（3）研究了城市生活垃圾焚烧运行参数、常规污染指标与二噁英的关联关系。针对某个正常运行的垃圾焚烧设施，分析不同工况参数下二噁英排放量的变化规律，探讨了各种运行参数、常规污染因子与二噁英关联的可行性，与部分参数、因子建立了一定的线性相关性；采用多元线性回归分析法，建立了二噁英与多变量的关联性，相关系数达到0.9，能作为该焚烧设施二噁英的控制模型，并为污染物排放与工况参数的联动监测提供指导。
（4）研究了垃圾焚烧非正常工况下二噁英与重金属的排放。首先结合国内文献报道与实际监测数据，提供了全国范围内具有代表性的垃圾焚烧设施正常运行下二噁英排放因子，即0.0154-10.720μg I-TEQ/t-waste，平均1.602μg I-TEQ/t-waste；接着对非正常工况进行了分类，并研究了不同环节非正常工况下二噁英产生与排放特征，得到非正常工况运行会显著地增加二噁英的排放，随着非正常工况环节数的增加，二噁英的排放逐步增加，不同工况系列的异构体分布特征非常相似；非正常工况下二噁英的排放因子是正常工况下的2-3个数量级，并根据《二噁英和呋喃排放识别和量化标准工具包》对不同非正常工况系列二噁英排放因子作了校正推算；最后研究了非正常工况下重金属（Hg、Cd、Pb、Zn、Cr、Cu、Ni、Tl）的排放因子，得到重金属的排放因子随工况的变化没有任何规律性，但可以作为不同工况下垃圾焚烧重金属排放因子的数据参考。
（5）研究了5%、10%、15%与20%质量比的污泥与煤共焚烧过程中二噁英与重金属的排放、质量平衡与分布特征。结果表明，随着混合燃料中污泥含量的增加，二噁英的排放从7.00pg I-TEQ/Nm~3增加到32.72pg I-TEQ/Nm~3，混合燃料中高的硫含量以及相对低的氯含量能促进二噁英的排放降低；污泥中二噁英的异构体分布图与输出产物（烟气、底灰与飞灰）中的明显不同；二噁英负平衡说明煤粉炉电厂污泥与煤共焚烧不是二噁英的源头。烟气、飞灰与底灰中重金属的浓度与排放因子均随着混合燃料中重金属输入值的增加而增加，重金属的分布特征主要取决于自身的挥发性质，氯在一定程度上改变了重金属的分布特性。
The incineration technology is playing an increasingly important role in treatingmunicipal solid waste (MSW) in large-and-medium size cities due to its advantages includingvolume and mass reduction, detoxification, and energy recovery. Based primarily on fieldmeasurements, much detailed research work was conducted to investigate emission andcontrol of PCDD/F and heavy metal in municipal solid waste incinerators (MSWI). The maintopics of this dissertation are as follows:
(1) According to the survey about MSWI basic information in China, the representativePCDD/F emission levels ranged between0.0042and7.90ng I-TEQ/Nm~3, with a mean valueof0.561ng I-TEQ/Nm~3.85%emission values can meet Chinese dioxin emission standard(1.0ng I-TEQ/Nm~3), however, only42%under EU standard (0.1ng I-TEQ/Nm~3). Then theexhaustive research and monitoring were carried out in8typical MSWIs in China. Based onregional distribution, incineration technology and management level, the PCDD/F and heavymetal emission levels and characteristics were totally elaborated from Chinese typicalMSWIs.
(2) The important factors that affected PCDD/F and heavy metal emissions weresystemtically investigated. First, the influence of different incineration technology,conditions(normal and abnormal), and management level on PCDD/F and heavy metalemission were examined. It can be obtained that abnormal operating conditions resulted in thehighest PCDD/F emission concentrations under bad management, ranging from8.01to181.69ng I-TEQ/Nm~3with78.18ng I-TEQ/Nm~3on average, but abnormal conditions didn’tnecessarily lead to increasing heavy metal emission. Second, the effects of the key ingredientin MSW, such as moisture content, calorific value, sulphur and chlorine content, and heavymetal input, were analyzed. Third, the influence of key technologies in pollution control, suchas quencher and activated carbon injection(ACI), on PCDD/F and heavy metal formation andemissions were studied. Results indicated that the quencher resulted in lower PCDD/Femissions through inhibiting the formation of lower chlorinated PCDD/F, and ACI alsomainly removed lower chlorinated PCDD/F. Although no activated carbon was injected priorto bag filter in a short time, the high removal efficiency can be obtained. Last, PCDD/F andheavy emissions were investigated in different stages during incinerator start-up period.Results indicated that PCDD/F emissions during start-up period were higher than duringnormal operation. After waste was feed dioxin emissions reached the highest concentrations.Due to memory effect, PCDD/F emissions cannot immediately drop to normal values.
(3) The relationship between operation conditions, as well as regular parameters andPCDD/F emissions was studied in order to find the optimal conditions for minimizingPCDD/F emissions. Based on a normal operating MSWI, the change law of PCDD/Femission with different conditions and parameters was analyzed, and the correlativefeasibility was explored. So a significant linear correlation between partial conditions, as wellas parameters and PCDD/F emissions was established. Then through conducting a multipleregression analysis, the correlation between dioxin emission and multiple variables wasobtained. Thus a control model can be constructed and serve the purpose of determining howto reduce dioxin emissions.
(4) PCDD/F and heavy metal emissions were investigated under abnormal conditions.First, according to the related literatures and monitoring data, the representative dioxinemission factors were provided under normal conditions (range:0.0154–10.720μgI-TEQ/t-waste, average:1.602μg I-TEQ/t-waste). Second, different abnormal conditionswere classified, and PCDD/F formation and emission characteristics were studied in differentsorts of abnormal conditions. Results indicated that abnormal conditions of the MSWI werefound to considerably increase PCDD/F emission, and PCDD/F emissions increased withincreasing abnormal condition sorts. The PCDD/F congener profiles presented greatsimilarities for different abnormal conditions. The emission factors in abnormal conditionswere23order of magnitude than that in normal conditions. Then according to StandardizedToolkit for Identification and Quantification of Dioxin and Furan Releases, emission factorswere regulated and estimated in different sorts of abnormal conditions. Finally, heavy metalemission factors were examined under abnormal conditions. It can be obtained that heavymetal emission factors didn’t show regularity with the changes of conditions.
(5) The emission, mass balance, and distribution characteristics of PCDD/Fs as well asthose of heavy metals (Hg, Cd, Pb, Cr, and Cu) were investigated during the co-combustionof5%,10%,15%, and20%sewage sludge (SS) in a pulverized coal power plant. ThePCDD/F emissions increased from7.00pg I-TEQ/Nm~3to32.72pg I-TEQ/Nm~3as the amountof SS in the mixed fuel (MF) increased. High sulfur content and relatively low chlorine levelsin MF resulted in lower PCDD/F emissions. SS exhibited a remarkable difference in congenerprofiles compared with flue gas, bottom ash, and fly ash. The negative dioxin mass balanceindicated that the co-firing of SS with coal in power plants was not a source but a sink ofdioxins. The concentrations and emission factors of heavy metals in flue gas and bottom ash,as well as fly ash, all exhibited a tendency to increase with increasing input values of heavymetals in MF. The distribution characteristics of the investigated heavy metals were primarily dependent on the evaporative properties of these metals. The availability of chlorine couldalter the heavy metal distribution behavior.
（1）对全国范围内垃圾焚烧设施进行基础资料调研，统计出了具有代表性的二噁英排放水平数据，即排放区间为0.0042-7.90ng I-TEQ/Nm~3，平均为0.561ng I-TEQ/Nm~3，85%排放可达到现行的国家排放标准1.0ng I-TEQ/Nm~3。然后对我国不同地区的8家典型生活垃圾焚烧设施开展现状调研与全面监测工作，从区域分布、焚烧技术、运营管理水平等方面总体上阐述了我国典型生活垃圾焚烧设施特征污染物（二噁英、重金属）的排放水平与排放特征。
（2）对我国典型垃圾焚烧设施的二噁英、重金属产生与排放的影响因素进行了系统研究。首先考察了不同焚烧工艺、工况（正常与非正常）以及管理水平等对二噁英/重金属排放的影响，得到运营管理不善导致的非正常工况运行排放了最高浓度水平的二噁英，范围8.01-181.69ng I-TEQ/Nm~3，平均78.18ng I-TEQ/Nm~3，而非正常工况运行不一定能导致重金属排放的增加；其次分析了生活垃圾组成中关键成分（含水率、热值、氯、硫含量、重金属自身含量与理化特性等）对二噁英/重金属排放的影响；接着研究了污染控制中的关键技术（急冷设备与活性炭的投加）对二噁英/重金属排放的影响，得到急冷设备能有效地降低二噁英的排放，主要能够抑制低氯代二噁英的生成，活性炭吸附能力也主要体现在对烟气中的低氯代二噁英的移除，短期内未投加活性炭对重金属同样具备高的移除效率；最后研究了焚烧炉启动不同阶段二噁英生成与排放，结果表明，启动阶段二噁英的排放要高于正常运行的，其中在投料阶段二噁英的排放最高，在稳定阶段，由于记忆效应的作用，二噁英排放并不能立刻降到正常值。
（3）研究了城市生活垃圾焚烧运行参数、常规污染指标与二噁英的关联关系。针对某个正常运行的垃圾焚烧设施，分析不同工况参数下二噁英排放量的变化规律，探讨了各种运行参数、常规污染因子与二噁英关联的可行性，与部分参数、因子建立了一定的线性相关性；采用多元线性回归分析法，建立了二噁英与多变量的关联性，相关系数达到0.9，能作为该焚烧设施二噁英的控制模型，并为污染物排放与工况参数的联动监测提供指导。
（4）研究了垃圾焚烧非正常工况下二噁英与重金属的排放。首先结合国内文献报道与实际监测数据，提供了全国范围内具有代表性的垃圾焚烧设施正常运行下二噁英排放因子，即0.0154-10.720μg I-TEQ/t-waste，平均1.602μg I-TEQ/t-waste；接着对非正常工况进行了分类，并研究了不同环节非正常工况下二噁英产生与排放特征，得到非正常工况运行会显著地增加二噁英的排放，随着非正常工况环节数的增加，二噁英的排放逐步增加，不同工况系列的异构体分布特征非常相似；非正常工况下二噁英的排放因子是正常工况下的2-3个数量级，并根据《二噁英和呋喃排放识别和量化标准工具包》对不同非正常工况系列二噁英排放因子作了校正推算；最后研究了非正常工况下重金属（Hg、Cd、Pb、Zn、Cr、Cu、Ni、Tl）的排放因子，得到重金属的排放因子随工况的变化没有任何规律性，但可以作为不同工况下垃圾焚烧重金属排放因子的数据参考。
（5）研究了5%、10%、15%与20%质量比的污泥与煤共焚烧过程中二噁英与重金属的排放、质量平衡与分布特征。结果表明，随着混合燃料中污泥含量的增加，二噁英的排放从7.00pg I-TEQ/Nm~3增加到32.72pg I-TEQ/Nm~3，混合燃料中高的硫含量以及相对低的氯含量能促进二噁英的排放降低；污泥中二噁英的异构体分布图与输出产物（烟气、底灰与飞灰）中的明显不同；二噁英负平衡说明煤粉炉电厂污泥与煤共焚烧不是二噁英的源头。烟气、飞灰与底灰中重金属的浓度与排放因子均随着混合燃料中重金属输入值的增加而增加，重金属的分布特征主要取决于自身的挥发性质，氯在一定程度上改变了重金属的分布特性。
The incineration technology is playing an increasingly important role in treatingmunicipal solid waste (MSW) in large-and-medium size cities due to its advantages includingvolume and mass reduction, detoxification, and energy recovery. Based primarily on fieldmeasurements, much detailed research work was conducted to investigate emission andcontrol of PCDD/F and heavy metal in municipal solid waste incinerators (MSWI). The maintopics of this dissertation are as follows:
(1) According to the survey about MSWI basic information in China, the representativePCDD/F emission levels ranged between0.0042and7.90ng I-TEQ/Nm~3, with a mean valueof0.561ng I-TEQ/Nm~3.85%emission values can meet Chinese dioxin emission standard(1.0ng I-TEQ/Nm~3), however, only42%under EU standard (0.1ng I-TEQ/Nm~3). Then theexhaustive research and monitoring were carried out in8typical MSWIs in China. Based onregional distribution, incineration technology and management level, the PCDD/F and heavymetal emission levels and characteristics were totally elaborated from Chinese typicalMSWIs.
(2) The important factors that affected PCDD/F and heavy metal emissions weresystemtically investigated. First, the influence of different incineration technology,conditions(normal and abnormal), and management level on PCDD/F and heavy metalemission were examined. It can be obtained that abnormal operating conditions resulted in thehighest PCDD/F emission concentrations under bad management, ranging from8.01to181.69ng I-TEQ/Nm~3with78.18ng I-TEQ/Nm~3on average, but abnormal conditions didn’tnecessarily lead to increasing heavy metal emission. Second, the effects of the key ingredientin MSW, such as moisture content, calorific value, sulphur and chlorine content, and heavymetal input, were analyzed. Third, the influence of key technologies in pollution control, suchas quencher and activated carbon injection(ACI), on PCDD/F and heavy metal formation andemissions were studied. Results indicated that the quencher resulted in lower PCDD/Femissions through inhibiting the formation of lower chlorinated PCDD/F, and ACI alsomainly removed lower chlorinated PCDD/F. Although no activated carbon was injected priorto bag filter in a short time, the high removal efficiency can be obtained. Last, PCDD/F andheavy emissions were investigated in different stages during incinerator start-up period.Results indicated that PCDD/F emissions during start-up period were higher than duringnormal operation. After waste was feed dioxin emissions reached the highest concentrations.Due to memory effect, PCDD/F emissions cannot immediately drop to normal values.
(3) The relationship between operation conditions, as well as regular parameters andPCDD/F emissions was studied in order to find the optimal conditions for minimizingPCDD/F emissions. Based on a normal operating MSWI, the change law of PCDD/Femission with different conditions and parameters was analyzed, and the correlativefeasibility was explored. So a significant linear correlation between partial conditions, as wellas parameters and PCDD/F emissions was established. Then through conducting a multipleregression analysis, the correlation between dioxin emission and multiple variables wasobtained. Thus a control model can be constructed and serve the purpose of determining howto reduce dioxin emissions.
(4) PCDD/F and heavy metal emissions were investigated under abnormal conditions.First, according to the related literatures and monitoring data, the representative dioxinemission factors were provided under normal conditions (range:0.0154–10.720μgI-TEQ/t-waste, average:1.602μg I-TEQ/t-waste). Second, different abnormal conditionswere classified, and PCDD/F formation and emission characteristics were studied in differentsorts of abnormal conditions. Results indicated that abnormal conditions of the MSWI werefound to considerably increase PCDD/F emission, and PCDD/F emissions increased withincreasing abnormal condition sorts. The PCDD/F congener profiles presented greatsimilarities for different abnormal conditions. The emission factors in abnormal conditionswere23order of magnitude than that in normal conditions. Then according to StandardizedToolkit for Identification and Quantification of Dioxin and Furan Releases, emission factorswere regulated and estimated in different sorts of abnormal conditions. Finally, heavy metalemission factors were examined under abnormal conditions. It can be obtained that heavymetal emission factors didn’t show regularity with the changes of conditions.
(5) The emission, mass balance, and distribution characteristics of PCDD/Fs as well asthose of heavy metals (Hg, Cd, Pb, Cr, and Cu) were investigated during the co-combustionof5%,10%,15%, and20%sewage sludge (SS) in a pulverized coal power plant. ThePCDD/F emissions increased from7.00pg I-TEQ/Nm~3to32.72pg I-TEQ/Nm~3as the amountof SS in the mixed fuel (MF) increased. High sulfur content and relatively low chlorine levelsin MF resulted in lower PCDD/F emissions. SS exhibited a remarkable difference in congenerprofiles compared with flue gas, bottom ash, and fly ash. The negative dioxin mass balanceindicated that the co-firing of SS with coal in power plants was not a source but a sink ofdioxins. The concentrations and emission factors of heavy metals in flue gas and bottom ash,as well as fly ash, all exhibited a tendency to increase with increasing input values of heavymetals in MF. The distribution characteristics of the investigated heavy metals were primarily dependent on the evaporative properties of these metals. The availability of chlorine couldalter the heavy metal distribution behavior.
引文
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