焚烧炉二恶英排放特性及关键控制技术研究
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摘要
近年来中国越来越多的生活垃圾、危险废物以及医疗垃圾焚烧炉在不断投入运行。然而,在运行过程中的剧毒性物质二恶英的超标排放是所有焚烧炉所不能忽略的问题,而且引起了一系列的社会问题。本文针对现今焚烧炉运行过程中的问题进行研究,对生活垃圾、危险废物以及医疗垃圾焚烧炉的二恶英排放特性进行了调查研究,并针对性地通过相关控制方法探讨了降低二恶英排放的主要因素。另外,开发了针对飞灰和烟气中二恶英减排的新型设备和技术,通过相关的实验论证了设备的可行性和控制效果。研究的主要结果如下：
(1)本文通过对典型的流化床生活垃圾焚烧炉二恶英排放特性进行调查分析,发现流化床在检测条件下当无活性炭喷射时其PCDD/Fs毒性浓度排放在0.073-14.8ng I-TEQ/Nm3之间,当有活性炭喷射时在0.064-4.70ng I-TEQ/Nm3之间,飞灰的PCDD/Fs浓度在254-8200ng I-TEQ/kg之间,新安装的布袋除尘器对PCDD/Fs的去除能力比旧布袋明显要高；烟气在锅炉中就存在异相催化生成的de novo反应,提高炉膛的燃烧温度对PCDD/Fs的生成有重要的作用,但不是影响PCDD/Fs排放的主要原因,烟气经净化设备的冷却过程是PCDD/Fs超标排放的主要原因；活性炭喷射能显著提高布袋除尘器的PCDD/Fs去除效率,而且新布袋条件下的去除效率要明显高于旧布袋条件,但是运行较久的布袋由于“记忆效应”的影响,即使活性炭喷射条件下也不能保证PCDD/Fs的达标排放；垃圾焚烧低负荷条件下的PCDD/Fs生成能力要强于高负荷条件,不同焚烧负荷也引起重金属的改变,其在飞灰中的重金属浓度除Cu外随焚烧负荷的增加而增加；
(2)本文研究的3个医疗废物焚烧炉烟气中PCDD/Fs排放差距较大,炉渣中的PCDD/Fs毒性浓度要比飞灰中小1-2个数量级,3个医疗废物焚烧炉的PCDD/Fs排放因子表明医疗废物焚烧炉的排放因子普遍要高于生活垃圾焚烧炉；危险废物焚烧炉处于活性炭长期喷射条件时,短暂停止喷射并不会造成出口尾气的PCDD/Fs浓度增加,但是对于长期无活性炭喷射的焚烧炉而言,活性炭的喷射对PCDD/Fs的去除效果比较明显,而且活性炭喷射量越大其去除效果也越加明显；危险废物焚烧炉在起炉过程中PCDD/Fs排放是总烟气排放的重要组成部分,本研究表明,焚烧炉起炉阶段PCDD/Fs在单位时间内的排放能力要比正常运行条件高56倍,Start-up阶段的PCDD/Fs排放量为年总排量的55.5%,I-TEQ排放量为50.5%；氯苯在起炉和正常运行条件下的排放特性跟PCDD/Fs类似,但是在浓度上要高PCDD/Fs两到三个数量级。对氯苯跟PCDD/Fs可能的关联研究发现,高氯代的氯苯如HxCBz同PCDD/Fs浓度的关联性较好；然而,同I-TEQ关联最好的是1.2,4,5-TeCBz,是实际危险废物焚烧炉的出口烟气排放中PCDD/Fs的最佳候选指示物。
(3)本文利用模拟飞灰研究SO2抑制二恶英生成的机理,发现当反应温度为300。C时PCDD/Fs的生成能力最强；SO：对反应中飞灰生成PCDD/Fs能力的抑制作用非常明显,而且随着温度的升高,其抑制作用增加；反应后通入SO2对PCDD/Fs抑制效果不是很明显,因此本文研究认为SO2对PCDD/Fs的抑制机理主要通过对催化剂如CuCl2的失活,而不是抑制气相的生成或者与PCDD/Fs本身参与反应；通过对反应过程中无机物质转归的模拟,发现当无SO2时,300℃前CuCl2能保持稳定,但是当温度继续增加后其分解,导致催化活性降低,模拟结果很好地印证了本实验中300℃时最大PCDD/Fs生成的现象；当有SO2时,模拟结果表明其抑制PCDD/Fs生成的机理是,一是将具有催化活性的CuCl2转变为无催化活性的CuSO4,二是减少主要反应元素C12的生成量,而且将最适生成温度从低温转移到高温。
(4)本文对危险废物焚烧飞灰(HFA)与生活垃圾焚烧飞灰(MFA)进行比较,发现HFA的比表面要远大于MFA, HFA具有更小的颗粒直径分布,而且在10μm以下的分布要远大于WFA；通过热释放化学动力学分析表明,飞灰在低温时发生反应的活化能较低,高温时的活化能较高,约为低温条件下的两个数量级,其可能发生残炭气化的化学反应。红外谱图分析表明,低温时产物主要是H2O和CO2,应该是物理的升温反应引起的气体的挥发；高温时残炭的气化生成H2O和CO2,在碳含量过高时,有部分的CO生成；飞灰在氮气气氛处理时PCDD/Fs的去除能力在300℃时便能满足大幅度降解的要求,温度增加时去除能力更为显著,PCDD/Fs去除的主要原因是脱氯和降解的反应的结果；气流速度提高能导致飞灰中PCDD/Fs去除效率的增加,但是在脱附烟气中,当流速度增加到4cm/s时,气相中PCDD/Fs浓度和I-TEQ浓度显著增加；而且不同种类的飞灰,尽管原始飞灰中PCDD/Fs浓度不大一致,热处理后的PCDD/Fs都较小,但是脱附至烟气中PCDD/Fs的浓度却明显不同；飞灰在热处理应用平台中的应用表明,热处理后PCDD/Fs浓度的总去除效率为66.9%, I-TEQ浓度的总去除效率为54.3%,PCDD/Fs主要分布在飞灰上,说明热处理技术在含有高浓度PCDD/Fs飞灰处理中应用的可行性。
(5)本文通过硫基抑制剂在实际危险废物焚烧炉中的应用,发现硫铁矿和硫酸铵作为抑制剂跟危险废物的掺烧能较大幅度增加烟气中的SO2浓度,能提高PCDD/Fs抑制剂的氛围浓度。硫基抑制剂的掺烧对烟气排放的PCDD/Fs减排能力相对较小,但是对整体的排放因子减量率为50%以上；基于飞灰热处理及硫基循环抑制二恶英生成与排放的应用平台的应用表明系统对SO2有一定程度的积累,而且外源硫基的添加能明显增加系统内的SO2浓度,硫铁矿作为外源硫基在系统内SO2积累能力要明显强于气体SO2作为外源硫基；应用平台初始运行下应用平台的运行虽然能在一定程度上降低PCDD/Fs排放的浓度,但是其降低程度有限。飞灰热处理的能力随着SO2积累能力的增加而提高,同时整体的PCDD/Fs排放因子也随着系统的运行而减少；应用平台在长期运行下布袋出口的PCDD/Fs排放会显著增加,可能的原因是“记忆效应”的影响,但是对于长期运行条件下的PCDD/Fs排放控制更具有效果,整体排放因子的减量率能达到80%以上,而且当硫铁矿作为外源硫基时,在10%的配比下能保证90%以上的PCDD/Fs排放因子减排,而且烟气的PCDD/Fs能保证在0.1ng1-TEQ/Nm3左右。
In recent years, more and more municipal solid waste, hazardous waste and medical waste incinerators continue to put into operation. However, excessive emissions of highly toxic substance of dioxin during combustion can't be ignored in all incinerators, and also raises some social problems. The problems during operation of incinerators nowadays in China were studied in the thesis, the dioxin emission characteristics in municipal solid waste, hazardous waste and medical waste incinerators was investigated, and the main factors to reduce the dioxin emission related to control methods were discussed in target. In addition, new equipment and technology for dioxin emission reduction in fly ash and flue gas were developed, and related experiments were carried out to demonstrate the feasibility of the device and the control effect. The main findings are as follows:
(1) The dioxin emission characteristics in typical fluidized bed municipal solid waste incinerators were surveyed and analyzed, and found that the emissions of toxic PCDD/Fs when activated carbon was not sprayed in the testing conditions was between0.073-14.8ng I-TEQ/Nm3. and between0.064-4.70ng I-TEQ/Nm3was found when was sprayed, the PCDD/Fs in fly ash was between254-8200ng I-TEQ/kg, and the newly installed bag filter was much better than aged one in relate to removal efficiency; heterogeneous catalysis formation of de novo synthesis already existed in boiler, the increase of combustion temperature in the furnace was important in the formation of PCDD/Fs, but not the main reason affecting the PCDD/Fs emissions, the cooling process of flue gas passing through air pollution control advices was the main reason for excessive emissions of PCDD/Fs; activated carbon spraying can significantly improve the removal efficiency of bag filter, and newly installed bag filter was more useful than aged one, however, due to "memory effect" existed in aged bag filter, the activated carbon spraying condition can't even guarantee that PCDD/Fs emission was lower than standard required; the PCDD/Fs formation ability under low combustion load was higher than the high combustion load, the different combustion loads could lead to the change of heavy metals emission, which was found that all concentrations of tested heavy metals except for Cu in fly ash increased with the increase of combustion load;
(2) The emission of PCDD/Fs among three experimented medical waste incinerators varied huge different, the toxic concentration PCDD/Fs in slag was1-2orders of magnitude lower than that in fly ash. the PCDD/Fs emission factors in three medical waste incinerators indicates that the emission factor in medical waste incinerators is generally higher than in municipal solid waste incinerators; if long-term spraying condition was operated in a hazardous waste incinerator, a brief suspension of spraying does not result in the increase of PCDD/Fs in stack, but for long-term non-activated carbon spraying condition, the spraying condition is obviously very important for the removal of PCDD/Fs. incinerator, and the removal efficiency increase with enhanced spraying amount; the PCDD/Fs emission during start-up process of the hazardous waste incinerator was most important part of total emission, the results in this study showed that the PCDD/Fs emissions capacity in per unit time during start-up process was56times higher than normal operating condition, the amout of PCDD/Fs emission in start-up stage was about55.5%of total annual emission, and the amout of I-TEQ emission in start-up stage was about50.5%of total annual emission; similar emission characteristics of chlorobenzenes under start-up and normal operating conditions was seen, but the concentration was two to three orders of magnitude higher than PCDD/Fs. The correlation of chlorobenzenes and PCDD/Fs was also studied, and found that the higher chlorinated chlorobenzenes such as HxCBz were much correlated with PCDD/Fs concentration; however, the best correlated chlorobenzenes with the I-TEQ was1,2,4.5-TeCBz, which turns out to be the best candidate of PCDD/Fs indicators at stack of real hazardous waste incinerator.
(3) A simulated fly ash was used to study the inhibition mechanism of SO2on dioxin, and found that when the reaction temperature was300C could generated most PCDD/Fs; SO2could obviously inhibit the PCDD/Fs formation in the fly ash, and the inhibition increased with the increase of reaction temperature; it was not very clear of inhibition effect when SO2reacted after fly ash reaction, which suggests that the inhibition mechanism of SO2on PCDD/Fs formation is mainly inactivating of catalyst, such as CuCl2, rather than inhibiting of gas phase formation or reacting with PCDD/Fs itself; rely on simulation of inorganic substances translation during the reaction, it was found that CuCl2could remain stable when temperature was lower than300C without SO2reaction, but it could decompose when the temperature continued to increase, which resulted in the reduction of catalytic activity, the simulation results confirms the phenomena in the experiment that maximum PCDD/Fs formation happened in300C very well; when SO2existed, the simulation results show that the PCDD/Fs inhibition mechanism is that, first to translate CuCl2with catalytic activity into non-catalytic activity of CuSO4. second to reduce the formation of Cl2which is the major element during reaction, and to transfer the optimum formation temperature from low to high temperature.
(4) Hazardous waste incinerator fly ash (HFA) and municipal solid waste incinerator fly ash (MFA) were compared and found that the specific surface area of the HFA is much larger than the MFA, HFA has a smaller particle diameter distribution, and the distribution which is less than10μm is much more than WFA; The analysis of thermal desorption chemical kinetics showed that the reaction of fly ash at low temperature with low activation energy, at high temperature with high activation energy, which is about two orders of magnitude higher than in the low-temperature condition, and possibly due to its gasification chemical reaction of residual carbon. IR spectra analysis showed that the main products at low temperature were H2O and CO2, which might be caused by the physical reaction of volatile gases; the main products at high temperature of residual carbon gasification were H2O and CO2and when the carbon content was high enough could generate partial CO; the PCDD/Fs removal efficiency in fly ash under N2atmosphere treated with thermal process shows that300C was able to meet the requirement of substantial degradation, and the removal efficiency elevated significantly with the increase of temperature, which mainly due to effects of dechlorination and degradation processes; the increase of flow rate could enhance the removal efficiency of PCDD/Fs in fly ash, but in the desorbed flue gas, when the flow rate increased to4cm/s, PCDD/Fs and I-TEQ concentrations in gas phase increased significantly; and with different types of fly ash, in spite of the different PCDD/Fs concentrations level in original fly ashes. PCDD/Fs concentrations could be reduced into low level after thermal treatment, but with obviously different PCDD/Fs concentrations which desorbed into the flue gas:the thermal treatment of fly ash in pilot scale plant showed that the removal efficiency of PCDD/Fs and I-TEQ concentration were66.9%and54.3%respectively, because the PCDD/Fs are mainly distributed in fly ash, it is feasible to thermal treat with fly ash with high concentration of PCDD/Fs.
(5) Sulfur-based inhibitors was used in a real hazardous waste incinerator, pyrite and ammonium sulfate as inhibitors co-combusted with the hazardous waste could increase the concentration of SO2in the flue gas. which could improve the inhibitor atmosphere. Co-combustion of sulfur-based inhibitors was relatively small effect to the PCDD/Fs emission reduction in flue gas, but the overall emission factor reduction efficiency could be larger than50%; the application of sulfur-based recycling and fly ash thermal treatment combination platform indicated a certain accumulation of SO2and the addition of exogenous sulfur-based inhibitors could increase the SO2concentration within the system, pyrite used as an exogenous sulfur could accumulate significantly more SO2in the system than gas SO2Although the debugging run under the new system test platform could reduce the PCDD/Fs emission in a certain extent but with limited extent. The thermal treatment capacity of fly ash increased with the increase of SO2accumulation capacity, at the same time, the whole PCDD/Fs emission factor reduced correspondingly; after long run, the PCDD/Fs emission in the outlet of pilot system increase significantly, which possibly due to "memory effect", but it was more effective of PCDD/Fs emission control for the long-term operating condition, the overall emission factor reduction efficiency could reach more than80%, and when pyrite was used as exogenous sulfur-based inhibitor could ensure more than90%reduction of PCDD/Fs emission factors and when the pyrite was10%to total treated fly ash, the PCDD/Fs emission could guarantee to lower than0.1ng I-TEQ/Nm3.
(1)本文通过对典型的流化床生活垃圾焚烧炉二恶英排放特性进行调查分析,发现流化床在检测条件下当无活性炭喷射时其PCDD/Fs毒性浓度排放在0.073-14.8ng I-TEQ/Nm3之间,当有活性炭喷射时在0.064-4.70ng I-TEQ/Nm3之间,飞灰的PCDD/Fs浓度在254-8200ng I-TEQ/kg之间,新安装的布袋除尘器对PCDD/Fs的去除能力比旧布袋明显要高；烟气在锅炉中就存在异相催化生成的de novo反应,提高炉膛的燃烧温度对PCDD/Fs的生成有重要的作用,但不是影响PCDD/Fs排放的主要原因,烟气经净化设备的冷却过程是PCDD/Fs超标排放的主要原因；活性炭喷射能显著提高布袋除尘器的PCDD/Fs去除效率,而且新布袋条件下的去除效率要明显高于旧布袋条件,但是运行较久的布袋由于“记忆效应”的影响,即使活性炭喷射条件下也不能保证PCDD/Fs的达标排放；垃圾焚烧低负荷条件下的PCDD/Fs生成能力要强于高负荷条件,不同焚烧负荷也引起重金属的改变,其在飞灰中的重金属浓度除Cu外随焚烧负荷的增加而增加；
(2)本文研究的3个医疗废物焚烧炉烟气中PCDD/Fs排放差距较大,炉渣中的PCDD/Fs毒性浓度要比飞灰中小1-2个数量级,3个医疗废物焚烧炉的PCDD/Fs排放因子表明医疗废物焚烧炉的排放因子普遍要高于生活垃圾焚烧炉；危险废物焚烧炉处于活性炭长期喷射条件时,短暂停止喷射并不会造成出口尾气的PCDD/Fs浓度增加,但是对于长期无活性炭喷射的焚烧炉而言,活性炭的喷射对PCDD/Fs的去除效果比较明显,而且活性炭喷射量越大其去除效果也越加明显；危险废物焚烧炉在起炉过程中PCDD/Fs排放是总烟气排放的重要组成部分,本研究表明,焚烧炉起炉阶段PCDD/Fs在单位时间内的排放能力要比正常运行条件高56倍,Start-up阶段的PCDD/Fs排放量为年总排量的55.5%,I-TEQ排放量为50.5%；氯苯在起炉和正常运行条件下的排放特性跟PCDD/Fs类似,但是在浓度上要高PCDD/Fs两到三个数量级。对氯苯跟PCDD/Fs可能的关联研究发现,高氯代的氯苯如HxCBz同PCDD/Fs浓度的关联性较好；然而,同I-TEQ关联最好的是1.2,4,5-TeCBz,是实际危险废物焚烧炉的出口烟气排放中PCDD/Fs的最佳候选指示物。
(3)本文利用模拟飞灰研究SO2抑制二恶英生成的机理,发现当反应温度为300。C时PCDD/Fs的生成能力最强；SO：对反应中飞灰生成PCDD/Fs能力的抑制作用非常明显,而且随着温度的升高,其抑制作用增加；反应后通入SO2对PCDD/Fs抑制效果不是很明显,因此本文研究认为SO2对PCDD/Fs的抑制机理主要通过对催化剂如CuCl2的失活,而不是抑制气相的生成或者与PCDD/Fs本身参与反应；通过对反应过程中无机物质转归的模拟,发现当无SO2时,300℃前CuCl2能保持稳定,但是当温度继续增加后其分解,导致催化活性降低,模拟结果很好地印证了本实验中300℃时最大PCDD/Fs生成的现象；当有SO2时,模拟结果表明其抑制PCDD/Fs生成的机理是,一是将具有催化活性的CuCl2转变为无催化活性的CuSO4,二是减少主要反应元素C12的生成量,而且将最适生成温度从低温转移到高温。
(4)本文对危险废物焚烧飞灰(HFA)与生活垃圾焚烧飞灰(MFA)进行比较,发现HFA的比表面要远大于MFA, HFA具有更小的颗粒直径分布,而且在10μm以下的分布要远大于WFA；通过热释放化学动力学分析表明,飞灰在低温时发生反应的活化能较低,高温时的活化能较高,约为低温条件下的两个数量级,其可能发生残炭气化的化学反应。红外谱图分析表明,低温时产物主要是H2O和CO2,应该是物理的升温反应引起的气体的挥发；高温时残炭的气化生成H2O和CO2,在碳含量过高时,有部分的CO生成；飞灰在氮气气氛处理时PCDD/Fs的去除能力在300℃时便能满足大幅度降解的要求,温度增加时去除能力更为显著,PCDD/Fs去除的主要原因是脱氯和降解的反应的结果；气流速度提高能导致飞灰中PCDD/Fs去除效率的增加,但是在脱附烟气中,当流速度增加到4cm/s时,气相中PCDD/Fs浓度和I-TEQ浓度显著增加；而且不同种类的飞灰,尽管原始飞灰中PCDD/Fs浓度不大一致,热处理后的PCDD/Fs都较小,但是脱附至烟气中PCDD/Fs的浓度却明显不同；飞灰在热处理应用平台中的应用表明,热处理后PCDD/Fs浓度的总去除效率为66.9%, I-TEQ浓度的总去除效率为54.3%,PCDD/Fs主要分布在飞灰上,说明热处理技术在含有高浓度PCDD/Fs飞灰处理中应用的可行性。
(5)本文通过硫基抑制剂在实际危险废物焚烧炉中的应用,发现硫铁矿和硫酸铵作为抑制剂跟危险废物的掺烧能较大幅度增加烟气中的SO2浓度,能提高PCDD/Fs抑制剂的氛围浓度。硫基抑制剂的掺烧对烟气排放的PCDD/Fs减排能力相对较小,但是对整体的排放因子减量率为50%以上；基于飞灰热处理及硫基循环抑制二恶英生成与排放的应用平台的应用表明系统对SO2有一定程度的积累,而且外源硫基的添加能明显增加系统内的SO2浓度,硫铁矿作为外源硫基在系统内SO2积累能力要明显强于气体SO2作为外源硫基；应用平台初始运行下应用平台的运行虽然能在一定程度上降低PCDD/Fs排放的浓度,但是其降低程度有限。飞灰热处理的能力随着SO2积累能力的增加而提高,同时整体的PCDD/Fs排放因子也随着系统的运行而减少；应用平台在长期运行下布袋出口的PCDD/Fs排放会显著增加,可能的原因是“记忆效应”的影响,但是对于长期运行条件下的PCDD/Fs排放控制更具有效果,整体排放因子的减量率能达到80%以上,而且当硫铁矿作为外源硫基时,在10%的配比下能保证90%以上的PCDD/Fs排放因子减排,而且烟气的PCDD/Fs能保证在0.1ng1-TEQ/Nm3左右。
In recent years, more and more municipal solid waste, hazardous waste and medical waste incinerators continue to put into operation. However, excessive emissions of highly toxic substance of dioxin during combustion can't be ignored in all incinerators, and also raises some social problems. The problems during operation of incinerators nowadays in China were studied in the thesis, the dioxin emission characteristics in municipal solid waste, hazardous waste and medical waste incinerators was investigated, and the main factors to reduce the dioxin emission related to control methods were discussed in target. In addition, new equipment and technology for dioxin emission reduction in fly ash and flue gas were developed, and related experiments were carried out to demonstrate the feasibility of the device and the control effect. The main findings are as follows:
(1) The dioxin emission characteristics in typical fluidized bed municipal solid waste incinerators were surveyed and analyzed, and found that the emissions of toxic PCDD/Fs when activated carbon was not sprayed in the testing conditions was between0.073-14.8ng I-TEQ/Nm3. and between0.064-4.70ng I-TEQ/Nm3was found when was sprayed, the PCDD/Fs in fly ash was between254-8200ng I-TEQ/kg, and the newly installed bag filter was much better than aged one in relate to removal efficiency; heterogeneous catalysis formation of de novo synthesis already existed in boiler, the increase of combustion temperature in the furnace was important in the formation of PCDD/Fs, but not the main reason affecting the PCDD/Fs emissions, the cooling process of flue gas passing through air pollution control advices was the main reason for excessive emissions of PCDD/Fs; activated carbon spraying can significantly improve the removal efficiency of bag filter, and newly installed bag filter was more useful than aged one, however, due to "memory effect" existed in aged bag filter, the activated carbon spraying condition can't even guarantee that PCDD/Fs emission was lower than standard required; the PCDD/Fs formation ability under low combustion load was higher than the high combustion load, the different combustion loads could lead to the change of heavy metals emission, which was found that all concentrations of tested heavy metals except for Cu in fly ash increased with the increase of combustion load;
(2) The emission of PCDD/Fs among three experimented medical waste incinerators varied huge different, the toxic concentration PCDD/Fs in slag was1-2orders of magnitude lower than that in fly ash. the PCDD/Fs emission factors in three medical waste incinerators indicates that the emission factor in medical waste incinerators is generally higher than in municipal solid waste incinerators; if long-term spraying condition was operated in a hazardous waste incinerator, a brief suspension of spraying does not result in the increase of PCDD/Fs in stack, but for long-term non-activated carbon spraying condition, the spraying condition is obviously very important for the removal of PCDD/Fs. incinerator, and the removal efficiency increase with enhanced spraying amount; the PCDD/Fs emission during start-up process of the hazardous waste incinerator was most important part of total emission, the results in this study showed that the PCDD/Fs emissions capacity in per unit time during start-up process was56times higher than normal operating condition, the amout of PCDD/Fs emission in start-up stage was about55.5%of total annual emission, and the amout of I-TEQ emission in start-up stage was about50.5%of total annual emission; similar emission characteristics of chlorobenzenes under start-up and normal operating conditions was seen, but the concentration was two to three orders of magnitude higher than PCDD/Fs. The correlation of chlorobenzenes and PCDD/Fs was also studied, and found that the higher chlorinated chlorobenzenes such as HxCBz were much correlated with PCDD/Fs concentration; however, the best correlated chlorobenzenes with the I-TEQ was1,2,4.5-TeCBz, which turns out to be the best candidate of PCDD/Fs indicators at stack of real hazardous waste incinerator.
(3) A simulated fly ash was used to study the inhibition mechanism of SO2on dioxin, and found that when the reaction temperature was300C could generated most PCDD/Fs; SO2could obviously inhibit the PCDD/Fs formation in the fly ash, and the inhibition increased with the increase of reaction temperature; it was not very clear of inhibition effect when SO2reacted after fly ash reaction, which suggests that the inhibition mechanism of SO2on PCDD/Fs formation is mainly inactivating of catalyst, such as CuCl2, rather than inhibiting of gas phase formation or reacting with PCDD/Fs itself; rely on simulation of inorganic substances translation during the reaction, it was found that CuCl2could remain stable when temperature was lower than300C without SO2reaction, but it could decompose when the temperature continued to increase, which resulted in the reduction of catalytic activity, the simulation results confirms the phenomena in the experiment that maximum PCDD/Fs formation happened in300C very well; when SO2existed, the simulation results show that the PCDD/Fs inhibition mechanism is that, first to translate CuCl2with catalytic activity into non-catalytic activity of CuSO4. second to reduce the formation of Cl2which is the major element during reaction, and to transfer the optimum formation temperature from low to high temperature.
(4) Hazardous waste incinerator fly ash (HFA) and municipal solid waste incinerator fly ash (MFA) were compared and found that the specific surface area of the HFA is much larger than the MFA, HFA has a smaller particle diameter distribution, and the distribution which is less than10μm is much more than WFA; The analysis of thermal desorption chemical kinetics showed that the reaction of fly ash at low temperature with low activation energy, at high temperature with high activation energy, which is about two orders of magnitude higher than in the low-temperature condition, and possibly due to its gasification chemical reaction of residual carbon. IR spectra analysis showed that the main products at low temperature were H2O and CO2, which might be caused by the physical reaction of volatile gases; the main products at high temperature of residual carbon gasification were H2O and CO2and when the carbon content was high enough could generate partial CO; the PCDD/Fs removal efficiency in fly ash under N2atmosphere treated with thermal process shows that300C was able to meet the requirement of substantial degradation, and the removal efficiency elevated significantly with the increase of temperature, which mainly due to effects of dechlorination and degradation processes; the increase of flow rate could enhance the removal efficiency of PCDD/Fs in fly ash, but in the desorbed flue gas, when the flow rate increased to4cm/s, PCDD/Fs and I-TEQ concentrations in gas phase increased significantly; and with different types of fly ash, in spite of the different PCDD/Fs concentrations level in original fly ashes. PCDD/Fs concentrations could be reduced into low level after thermal treatment, but with obviously different PCDD/Fs concentrations which desorbed into the flue gas:the thermal treatment of fly ash in pilot scale plant showed that the removal efficiency of PCDD/Fs and I-TEQ concentration were66.9%and54.3%respectively, because the PCDD/Fs are mainly distributed in fly ash, it is feasible to thermal treat with fly ash with high concentration of PCDD/Fs.
(5) Sulfur-based inhibitors was used in a real hazardous waste incinerator, pyrite and ammonium sulfate as inhibitors co-combusted with the hazardous waste could increase the concentration of SO2in the flue gas. which could improve the inhibitor atmosphere. Co-combustion of sulfur-based inhibitors was relatively small effect to the PCDD/Fs emission reduction in flue gas, but the overall emission factor reduction efficiency could be larger than50%; the application of sulfur-based recycling and fly ash thermal treatment combination platform indicated a certain accumulation of SO2and the addition of exogenous sulfur-based inhibitors could increase the SO2concentration within the system, pyrite used as an exogenous sulfur could accumulate significantly more SO2in the system than gas SO2Although the debugging run under the new system test platform could reduce the PCDD/Fs emission in a certain extent but with limited extent. The thermal treatment capacity of fly ash increased with the increase of SO2accumulation capacity, at the same time, the whole PCDD/Fs emission factor reduced correspondingly; after long run, the PCDD/Fs emission in the outlet of pilot system increase significantly, which possibly due to "memory effect", but it was more effective of PCDD/Fs emission control for the long-term operating condition, the overall emission factor reduction efficiency could reach more than80%, and when pyrite was used as exogenous sulfur-based inhibitor could ensure more than90%reduction of PCDD/Fs emission factors and when the pyrite was10%to total treated fly ash, the PCDD/Fs emission could guarantee to lower than0.1ng I-TEQ/Nm3.
引文
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