城市生活垃圾焚烧飞灰熔融特性及重金属赋存迁移规律的研究
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摘要
垃圾焚烧电厂产生的焚烧飞灰中含有大量毒性重金属及其化合物,且具有高浸出率,属于危险废物,飞灰熔融处理技术可有效地控制焚烧飞灰中重金属污染,是焚烧飞灰无害化处理的主要技术之一。本文系统地研究了垃圾焚烧飞灰的基本特性、在高温管式炉和旋风熔融炉中的熔融特性及重金属的行为特性,并分析探讨了流化床煤气化-旋风熔融集成处理系统的各种因素对焚烧飞灰中重金属行为的影响。
本文选取我国华东地区三个典型城市正在运行的垃圾焚烧发电厂的布袋除尘器飞灰作为研究对象,系统地分析了它们的化学组成特性、物理特性、微观形貌、矿物组成特性、浸出特性等,结果表明,垃圾焚烧飞灰的成分相当复杂,其主要成分是SiO_2、CaO、Al_2O_3和Fe_2O_3,其次为Na_2O、K_2O、MgO、氢氧化物、氯化物,还有少量重金属,如Cd、Cr、Cu、Pb、Zn等,其中Pb、Zn等重金属严重超出危险废物鉴别标准;三种飞灰粒径呈近似的正态分布,飞灰粒径的主要范围在10-100μm之间;焚烧飞灰熔融处理过程为吸热过程,包括晶体物相转变阶段和熔融阶段。各阶段的温度范围、吸收热量及熔融反应的起始温度与飞灰成分有着密切关系,其熔点受成分的影响最为显著,SiO_2+Al_2O_3含量的高低直接影响飞灰的熔点,三种飞灰的熔点由高到低依次为:FA3>FA2>FA1。焚烧飞灰由大量的不规则状结晶相和非晶相组成,外观上较为松散,呈球状、椭球状或片状层叠在一起,孔隙率较高,比表面积较大。焚烧飞灰是高浸出毒性的危险废弃物,其中Cd、Cr、Pb、Cu、Zn的质量分数均比土壤中高出很多,三种飞灰中Pb、Cr,FA1和FA2中的Zn的浸出值均超过标准值,须对焚烧飞灰进行稳定化、无害化处理。三种飞灰浸出前后溶液的pH值的变化规律较接近,浸出液的pH值以5.3为分界点,分界点之前浸出液的pH值上升较快,之后变化明显减慢。
在掌握了焚烧飞灰基本特性基础上,采用高温管式电炉对焚烧飞灰进行静态熔融试验,研究了飞灰熔融前后试样的微观形貌、矿物特性、重金属分布、浸出毒性、添加剂对熔融特性的影响,并探讨了熔融温度、熔融时间、碱基度、添加剂、气氛等多种因素变化对飞灰熔融过程中重金属的固溶、挥发特性的影响。研究表明:1400℃时试样已完全熔融,熔融体表观结构平整光滑,具有较高的硬度,其断面具有光泽且无明显孔隙产生;熔融体呈结晶状态,且结晶相数量随着温度的升高呈增加趋势;熔融产物中Zn、Cr、Pb、Cu、Cd、Hg等重金属浸出率均非常低;在空气气氛下熔融时,SiO_2、CaO、Al_2O_3三种添加剂对熔融效果的影响次序:SiO_2>CaO>Al_2O_3。熔融温度对重金属的行为影响显著;熔融时间对各种重金属的固溶挥发行为影响差异较大;碱基度变化对重金属的固溶率影响显著。熔融过程中适当地掺入SiO_2有利于重金属固溶率提高。氧化气氛下,Cr、Ni、Cu、As的固溶率随其熔沸点的升高而依次升高,低沸点金属Pb、Cd、Hg、Zn在熔融过程中挥发性较高;还原气氛下,Ni、Cr大部分固溶在熔渣中,还原性气氛有利于Ni、Cr、Cu和As的固溶,而Hg、Cd、Zn更容易挥发,熔融温度对它们挥发率影响较小,但还原性气氛对Pb的挥发有抑制作用。
根据垃圾焚烧飞灰管式熔融炉熔融特性和重金属行为特性的试验研究结果,提出了一种新型工艺——煤气化-旋风熔融集成处理工艺,自行设计建造了处理能力为6kg·h-1的试验系统,首先采用燃油作为热源对旋风熔融炉进行了焚烧飞灰动态熔融试验,研究了熔融温度、CaO、SiO_2和MgO添加剂对焚烧飞灰熔融特性及重金属赋存迁移规律的影响,获得了焚烧飞灰动态熔融处理特性及重金属赋存迁移规律。结果表明,在1400℃条件下,飞灰试样在旋风炉中也可完全转化为玻璃态;在飞灰中掺入CaO、SiO_2和MgO,同样可有效地改进焚烧飞灰熔融特性:CaO可有效地控制飞灰熔点,CaO对焚烧飞灰的助熔作用应根据飞灰的成分进行适当的调整;添加SiO_2有利于降低飞灰的熔点,随着SiO_2添加量的增加,熔渣稳定性增强;MgO对飞灰中硅酸盐或硅铝酸盐中的网状结构有破坏作用,MgO添加量>5%时,对试样达到较好的熔融效果具有促进作用。在1250-1400℃范围内,Ni、Cr、Cu、Co、Mn的固溶率随熔融温度的升高而缓慢增长,熔融温度变化对As、Pb、Cd、Zn的固溶率有显著影响,对Hg的挥发影响甚微;CaO的添加对Cr、Cu、Mn、As、Zn、Pb的固溶有抑制作用;添加SiO_2对重金属的固溶率有促进作用;MgO的添加有利于重金属的固溶,尤其是对于Zn、As、Cd、Pb的固溶率提高更为显著;三种添加剂对重金属的固溶作用:MgO最好,SiO_2次之,CaO较差。在不同熔融温度下,烟气中挥发性重金属对熔融温度较敏感,随温度增加呈先减后增的趋势;CaO添加量为5%时可减少熔融过程中挥发性重金属的排放,继续增加CaO将对重金属固溶产生负面影响;烟气挥发性重金属含量随SiO_2添加量的增加而减少;MgO的介入对烟气中重金属含量有显著影响。
最后将流化床煤气化炉和旋风熔融炉联接起来进行集成试验,研究了空气-煤质量比、蒸汽-煤质量比、床层温度、添加剂种类等因素对焚烧飞灰熔融过程中重金属元素赋存迁移规律的影响。结果表明:在不同空煤比条件下,Ni、Cr的固溶率最高,Cu、Mn、Co的固溶率随空煤比增加呈缓慢上升的趋势;挥发性重金属的固溶率随空煤比的增加基本呈上升趋势。固溶率超过30%的重金属主要有As和Zn;Hg的固溶率随空煤比的变化基本维持不变。随着汽煤比的增加,Co、Cr、Cu、Mn、Ni的固溶率及挥发性重金属的固溶率均呈先增后减的趋势,且在汽煤比为0.41kg·kg-1时,固溶率达到最高,Cr、Ni的固溶率在不同工况下均大于90%;当床层温度在860-920℃之间时,Mn的固溶率随床温的升高略有降低,Co、Cr、Cu、Ni的固溶率与床层温度呈正相关,固溶率大小依次为:Ni>Cr>Cu>Mn>Co;Zn的固溶率与床层温度呈反比,Pb、Cd的固溶率随床层温度的升高而升高;Hg的固溶率随床温变化不明显。添加MgO对Ni、Cr固溶较为有利;CaO、SiO_2、MgO的添加对于Mn的固溶率均无明显提高;对于Cu,SiO_2的固溶效果最好,MgO次之,CaO稍差;添加MgO时Co的固溶率最高,SiO_2次之,CaO最差;MgO、SiO_2的添加相对无添加剂时重金属的固溶率提高较为明显。对于As、Zn、Cd、Pb,MgO的效果优于SiO_2、CaO;三种添加剂对飞灰熔融过程中重金属固溶率提高的次序依次为:MgO>SiO_2>CaO。
在试验研究的基础上,基于重金属元素在熔融过程中挥发特性,建立了重金属的挥发扩散模型及重金属元素从飞灰颗粒内释放模型,模型中考虑了气固反应、颗粒间传热传质、重金属的扩散等因素的影响,并对不同熔融温度下焚烧飞灰中重金属的固溶率进行了数值模拟,总体模拟结果与实验结果,趋势一致,数值相近。
Fly ashes from municipal solid waste (MSW) incinerator contain a great deal of toxic heavy metals and their compounds. They are defined as hazardous waste because these fly ashes in having high leaching ratios of heavy metals. Melting technology can effectively control emission of heavy metals in fly ashes from MSW incinerator. It is one of the major techniques of fly ashes innocent treatment. The basic properties of fly ashes from MSW incinerator are systematically investigated. The fly ashes are carried out the melting characteristics and the behavior of heavy metals in fixed tube furnace and swirling furnace. At the same time, the factors of the system on coal gasification and fly ashes melting are explored.
The fly ashes of bag filters from three typical running municipal solid waste powder plants in east China were studied to explore the chemical composition, physical properties, changes of microstructure, mineralogical composition, leaching characteristics of fly ashes samples. The results show that the compositions of fly ashes are very complexes. The major components contain silicon dioxide, calcium oxide, alumina, ferric oxide, hydrate, and chloride. There are a small amount of heavy metals, such as cadmium, chromium, copper, lead, zinc and so on. The content of zinc and lead are grievously outside of the identification standard for hazardous wastes. The particles size distributions of three fly ashes are approximately normal school. The primary range of particles sizes is 10 to 100 micron. The melting process of fly ash is an endothermic process. It is comprised materials phases transformation and melting reaction. The temperature range, endothermic amount and initiative temperature of melting reaction in each process rest with the compositions of fly ashes. The melting points of fly ash are distinctly affected by the compositions. The temperature of melting point is determined by the content of silicon dioxide and alumina in fly ash. The order of melting point on three fly ashes is FA3> FA2> FA1. The major constitutes of fly ash are composed by plentiful crystal and amorphous materials. They have higher porosity and BET. The fly ash is higher leaching rate of hazardous waste. The mass fractions of cadmium, chromium, lead, copper, zinc are higher than these of soil. The leaching rates of lead, chromium in three fly ashes and zinc in FA1, FA2 go beyond the values of standards. Therefore, it is obligatory for fly ash to immobilize and detoxify. The change rules of pH values in leachate of before and after three fly ashes are very analogical. The pH value of leachate in 5.3 is a critical point. When pH value is less than 5.3, it would sharply raise. On the contrary, the change of leachate pH value becomes smooth. These conclusions will provide the important theory bases for the farther research treatment harmlessly of fly ashes.
The fly ashes from MSW incinerator were conducted in a tube melting furnace in this study. The changes of microstructure, mineralogical composition, heavy metals distribution, leaching characteristics of samples before and after melting treatment were explored. The emphasis is on the effects additives on the melting characteristics and heavy metals distribution. Simultaneity, influences of melting temperature, melting time, basicity, additives, different atmosphere on the immobility and volatilization behavior of heavy metals during melting process. The results show that the melting temperature is an important factor on the melting treatment of fly ashes from MSW incinerator. At 1400℃, the molten sample became full smooth, much hard in surface structure, while the section of the molten sample had lustrous or no apparent aperture, the sample fly ash had completely melted. The slag melted is crystalloid. The amounts of crystalsincrease with the melting temperature elevation. The leaching rates of zinc, chromium, lead, copper, cadmium, mercury was very low in the products melted. The gaseous volatile of mercury, cadmium and lead is captured. The effect of heavy metals immobility was in sequence of silicon dioxide>calcium oxide>alumina. Melting temperature has an important impact on the behavior of heavy metals. There is a great difference for the behavior of immobility and volatilization of various heavy metals. The changes of basicity will give birth to the marked influence on the fixation rate of heavy metals. The proper additive rate of silicon dioxide will be propitious to enhance the fixation rate on the heavy metals. The fixation rates of chromium, nickel, copper and arsenic in melted samples would increase with the elevation of their melting point and boiling point at oxidizing atmosphere. The volatilization rates of lead, cadmium and mercury with low boiling points are very high during melting process. The reducing atmosphere would be propitious to enhancing the fixation rates of chromium, nickel, copper and arsenic. It is confirmed that mercury, cadmium, and zinc are more easily vaporized under reducing atmosphere, but the volatilization rate of lead would be inhibited at the same condition.
Based on the previous experimental results, the different fly ashes were melted in the self-developed swirling melting furnace system. The melting characteristics and behavior of heavy metals of fly ashes were investigated in detail under different operation runs. Influences of melting temperature, calcium oxide, silicon dioxide, magnesia additional reagent on the melting characteristics and behavior of heavy metals were studies during fly ashes melting process. The dynamic melting treatment characteristics and occurrence and transference of heavy metals in samples were concluded. Experimental results indicate that the fly ashes will transform into vitrification state at 1400℃. The higher melting temperature will redound to fly ashes melting treatment. There are marked differences on the influences of calcium oxide, silicon dioxide, magnesia additional reagent on the melting characteristics. Adding calcium oxide may effectively control melting point of fly ash. If adding less than 15 percent, it would be propitious to melting treatment. The melting-aid effect of calcium oxide should appropriately adjust base on composition of fly ash. Adding silicon dioxide in fly ash would redound to reducing the melting point of fly ash and advance the liquidity of sample. With the adding amount increasing of silicon dioxide, the glassy amorphous materials in the melted sample would enhance. The higher adding amount of silicon dioxide, the better is the stability of melted slag. The netlike structures of silicates in fly ash would be destroyed by the adding magnesia. The glutinosity of melted sample reduces with increasing adding amount of magnesia. The sample would achieve the better melting effect when the adding amount is less than 5 percent in fly ash sample. The glassy materials in slag would enhance and the crystal phases take place transform with adulterating magnesia. The crystals in sample are enveloped by the amorphous slag. The fixation rates of nickel, chromium, copper, cobalt, and manganese in slag increase with melting temperature heightening between 1250 and 1400 degree centigrade. With the exception of mercury, the change of melting temperature would markedly affect on the fixation rates of arsenic, lead, cadmium, zinc. The fixation rates of chromium, copper, manganese are decreased by adding calcium oxide during melting process. The lower is the fixation rate of arsenic, zinc, and lead, the more is adding calcium oxide. It is beneficial for the improvement fixation rate of heavy metals to add silicon dioxide. With the exception of mercury, the fixation rates of residual heavy metals would improve with adding amount increasing. The fixation rates of zinc, arsenic, cadmium, and lead would distinctly enhance. Adding amount being controlled at 10 percent for FA3 would achieve the optimal fixation effect. The volatile heavy metals are sensitive to melting temperature. With melting temperature increasing, the content of them takes on the increasing first and after reducing in flue gas. When calcium oxide adding amount is 5 percent, the content of volatile heavy metals would lessen in flue gas of melting treatment. It would give birth to negative effect for fixation heavy metals once calcium oxide adding exceeding 5 percent. With the increasing of silicon dioxide adding amount, the content of heavy metals in flue gas would reduce, but the content of mercury is ruleless. The adding magnesia in flyash has remarkable influence on the content of heavy metals in flue gas.
At last, the gas products of coal gasification were used as the substitutive fuel on melting treatment of fly ashes. The fly ashes were conducted in the experimental system associating coal gasification with melting treatment. The effects of air/coal ratio, steam/coal ratio, bed temperature and additives on the occurrence and transference of heavy metals during melting process on swirling furnace was systemically investigated. The fixation rates of nickel and chromium achieve the maximal value above 90 percent at different air/coal ratio condition. With increasing air/coal ratio, the fixation rates of copper, manganese, and cobalt enhance steadily, the fixation rates of volatile heavy metals take on the ascending. The fixation rates of arsenic and zinc is above 30 percent in slag, the fixation rate of cadmium becomes increasing first and after reducing in slag. That of mercury keeps stable. The fixation rates of cobalt, chromium, copper, manganese, nickel and volatile heavy metals increase first then reduce in slag with increasing steam/coal ratio, and fixation rates of them achieve the maximum at steam/coal ratio 0.41 kg·kg-1, those of chromium and nickel is above 90 percent. With the exception of manganese, the fixation rates of cobalt, chromium, copper, and nickel enhance with increasing bed temperature. The order of fixation rate is Ni>Cr>Cu>Mn>Co. With bed temperature increasing, the fixation rates of lead and cadmium aggrandize, the fixation rate of zinc is reductive, mercury keep stable. The adding magnesia in sample would conduce to increasing the fixation rate of nickel and chromium. The adding calcium oxide, silicon dioxide, magnesia would not be helpful to fixation of manganese. For copper, the fixation effect of silicon dioxide is the best, the magnesia is the better, calcium oxide is the worse. For cobalt, the order of fixation effect is magnesia>silicon dioxide>calcium oxide. The fixation rates of heavy metals would remarkably enhance when adding magnesia and silicon dioxide. For the volatile heavy metals such as arsenic, zinc, cadmium, and lead, the fixation effect of magnesia is better than that of silicon dioxide and calcium oxide. The fixation rates order of heavy metals is magnesia>silicon dioxide>calcium oxide. These conclusions will offer the experimental bases and theoretic references for further comprehending the melting treatment technology of fly ash.
Based on the experimental results and existent states of heavy metals in fly ashes and slag, the gas-solid reaction theory during the melting process, heat and mass transfer of particles in fly ashes, chemical dynamics theory such as volatile heavy metals diffuseness, the plentiful experimental datum were analyzed. The melting reaction model and the volatility model of heavy metals in particles during fly ashes melting process have been constructed. The results simulated from the predicted model are basically consistent with the measured values of experiments.
本文选取我国华东地区三个典型城市正在运行的垃圾焚烧发电厂的布袋除尘器飞灰作为研究对象,系统地分析了它们的化学组成特性、物理特性、微观形貌、矿物组成特性、浸出特性等,结果表明,垃圾焚烧飞灰的成分相当复杂,其主要成分是SiO_2、CaO、Al_2O_3和Fe_2O_3,其次为Na_2O、K_2O、MgO、氢氧化物、氯化物,还有少量重金属,如Cd、Cr、Cu、Pb、Zn等,其中Pb、Zn等重金属严重超出危险废物鉴别标准;三种飞灰粒径呈近似的正态分布,飞灰粒径的主要范围在10-100μm之间;焚烧飞灰熔融处理过程为吸热过程,包括晶体物相转变阶段和熔融阶段。各阶段的温度范围、吸收热量及熔融反应的起始温度与飞灰成分有着密切关系,其熔点受成分的影响最为显著,SiO_2+Al_2O_3含量的高低直接影响飞灰的熔点,三种飞灰的熔点由高到低依次为:FA3>FA2>FA1。焚烧飞灰由大量的不规则状结晶相和非晶相组成,外观上较为松散,呈球状、椭球状或片状层叠在一起,孔隙率较高,比表面积较大。焚烧飞灰是高浸出毒性的危险废弃物,其中Cd、Cr、Pb、Cu、Zn的质量分数均比土壤中高出很多,三种飞灰中Pb、Cr,FA1和FA2中的Zn的浸出值均超过标准值,须对焚烧飞灰进行稳定化、无害化处理。三种飞灰浸出前后溶液的pH值的变化规律较接近,浸出液的pH值以5.3为分界点,分界点之前浸出液的pH值上升较快,之后变化明显减慢。
在掌握了焚烧飞灰基本特性基础上,采用高温管式电炉对焚烧飞灰进行静态熔融试验,研究了飞灰熔融前后试样的微观形貌、矿物特性、重金属分布、浸出毒性、添加剂对熔融特性的影响,并探讨了熔融温度、熔融时间、碱基度、添加剂、气氛等多种因素变化对飞灰熔融过程中重金属的固溶、挥发特性的影响。研究表明:1400℃时试样已完全熔融,熔融体表观结构平整光滑,具有较高的硬度,其断面具有光泽且无明显孔隙产生;熔融体呈结晶状态,且结晶相数量随着温度的升高呈增加趋势;熔融产物中Zn、Cr、Pb、Cu、Cd、Hg等重金属浸出率均非常低;在空气气氛下熔融时,SiO_2、CaO、Al_2O_3三种添加剂对熔融效果的影响次序:SiO_2>CaO>Al_2O_3。熔融温度对重金属的行为影响显著;熔融时间对各种重金属的固溶挥发行为影响差异较大;碱基度变化对重金属的固溶率影响显著。熔融过程中适当地掺入SiO_2有利于重金属固溶率提高。氧化气氛下,Cr、Ni、Cu、As的固溶率随其熔沸点的升高而依次升高,低沸点金属Pb、Cd、Hg、Zn在熔融过程中挥发性较高;还原气氛下,Ni、Cr大部分固溶在熔渣中,还原性气氛有利于Ni、Cr、Cu和As的固溶,而Hg、Cd、Zn更容易挥发,熔融温度对它们挥发率影响较小,但还原性气氛对Pb的挥发有抑制作用。
根据垃圾焚烧飞灰管式熔融炉熔融特性和重金属行为特性的试验研究结果,提出了一种新型工艺——煤气化-旋风熔融集成处理工艺,自行设计建造了处理能力为6kg·h-1的试验系统,首先采用燃油作为热源对旋风熔融炉进行了焚烧飞灰动态熔融试验,研究了熔融温度、CaO、SiO_2和MgO添加剂对焚烧飞灰熔融特性及重金属赋存迁移规律的影响,获得了焚烧飞灰动态熔融处理特性及重金属赋存迁移规律。结果表明,在1400℃条件下,飞灰试样在旋风炉中也可完全转化为玻璃态;在飞灰中掺入CaO、SiO_2和MgO,同样可有效地改进焚烧飞灰熔融特性:CaO可有效地控制飞灰熔点,CaO对焚烧飞灰的助熔作用应根据飞灰的成分进行适当的调整;添加SiO_2有利于降低飞灰的熔点,随着SiO_2添加量的增加,熔渣稳定性增强;MgO对飞灰中硅酸盐或硅铝酸盐中的网状结构有破坏作用,MgO添加量>5%时,对试样达到较好的熔融效果具有促进作用。在1250-1400℃范围内,Ni、Cr、Cu、Co、Mn的固溶率随熔融温度的升高而缓慢增长,熔融温度变化对As、Pb、Cd、Zn的固溶率有显著影响,对Hg的挥发影响甚微;CaO的添加对Cr、Cu、Mn、As、Zn、Pb的固溶有抑制作用;添加SiO_2对重金属的固溶率有促进作用;MgO的添加有利于重金属的固溶,尤其是对于Zn、As、Cd、Pb的固溶率提高更为显著;三种添加剂对重金属的固溶作用:MgO最好,SiO_2次之,CaO较差。在不同熔融温度下,烟气中挥发性重金属对熔融温度较敏感,随温度增加呈先减后增的趋势;CaO添加量为5%时可减少熔融过程中挥发性重金属的排放,继续增加CaO将对重金属固溶产生负面影响;烟气挥发性重金属含量随SiO_2添加量的增加而减少;MgO的介入对烟气中重金属含量有显著影响。
最后将流化床煤气化炉和旋风熔融炉联接起来进行集成试验,研究了空气-煤质量比、蒸汽-煤质量比、床层温度、添加剂种类等因素对焚烧飞灰熔融过程中重金属元素赋存迁移规律的影响。结果表明:在不同空煤比条件下,Ni、Cr的固溶率最高,Cu、Mn、Co的固溶率随空煤比增加呈缓慢上升的趋势;挥发性重金属的固溶率随空煤比的增加基本呈上升趋势。固溶率超过30%的重金属主要有As和Zn;Hg的固溶率随空煤比的变化基本维持不变。随着汽煤比的增加,Co、Cr、Cu、Mn、Ni的固溶率及挥发性重金属的固溶率均呈先增后减的趋势,且在汽煤比为0.41kg·kg-1时,固溶率达到最高,Cr、Ni的固溶率在不同工况下均大于90%;当床层温度在860-920℃之间时,Mn的固溶率随床温的升高略有降低,Co、Cr、Cu、Ni的固溶率与床层温度呈正相关,固溶率大小依次为:Ni>Cr>Cu>Mn>Co;Zn的固溶率与床层温度呈反比,Pb、Cd的固溶率随床层温度的升高而升高;Hg的固溶率随床温变化不明显。添加MgO对Ni、Cr固溶较为有利;CaO、SiO_2、MgO的添加对于Mn的固溶率均无明显提高;对于Cu,SiO_2的固溶效果最好,MgO次之,CaO稍差;添加MgO时Co的固溶率最高,SiO_2次之,CaO最差;MgO、SiO_2的添加相对无添加剂时重金属的固溶率提高较为明显。对于As、Zn、Cd、Pb,MgO的效果优于SiO_2、CaO;三种添加剂对飞灰熔融过程中重金属固溶率提高的次序依次为:MgO>SiO_2>CaO。
在试验研究的基础上,基于重金属元素在熔融过程中挥发特性,建立了重金属的挥发扩散模型及重金属元素从飞灰颗粒内释放模型,模型中考虑了气固反应、颗粒间传热传质、重金属的扩散等因素的影响,并对不同熔融温度下焚烧飞灰中重金属的固溶率进行了数值模拟,总体模拟结果与实验结果,趋势一致,数值相近。
Fly ashes from municipal solid waste (MSW) incinerator contain a great deal of toxic heavy metals and their compounds. They are defined as hazardous waste because these fly ashes in having high leaching ratios of heavy metals. Melting technology can effectively control emission of heavy metals in fly ashes from MSW incinerator. It is one of the major techniques of fly ashes innocent treatment. The basic properties of fly ashes from MSW incinerator are systematically investigated. The fly ashes are carried out the melting characteristics and the behavior of heavy metals in fixed tube furnace and swirling furnace. At the same time, the factors of the system on coal gasification and fly ashes melting are explored.
The fly ashes of bag filters from three typical running municipal solid waste powder plants in east China were studied to explore the chemical composition, physical properties, changes of microstructure, mineralogical composition, leaching characteristics of fly ashes samples. The results show that the compositions of fly ashes are very complexes. The major components contain silicon dioxide, calcium oxide, alumina, ferric oxide, hydrate, and chloride. There are a small amount of heavy metals, such as cadmium, chromium, copper, lead, zinc and so on. The content of zinc and lead are grievously outside of the identification standard for hazardous wastes. The particles size distributions of three fly ashes are approximately normal school. The primary range of particles sizes is 10 to 100 micron. The melting process of fly ash is an endothermic process. It is comprised materials phases transformation and melting reaction. The temperature range, endothermic amount and initiative temperature of melting reaction in each process rest with the compositions of fly ashes. The melting points of fly ash are distinctly affected by the compositions. The temperature of melting point is determined by the content of silicon dioxide and alumina in fly ash. The order of melting point on three fly ashes is FA3> FA2> FA1. The major constitutes of fly ash are composed by plentiful crystal and amorphous materials. They have higher porosity and BET. The fly ash is higher leaching rate of hazardous waste. The mass fractions of cadmium, chromium, lead, copper, zinc are higher than these of soil. The leaching rates of lead, chromium in three fly ashes and zinc in FA1, FA2 go beyond the values of standards. Therefore, it is obligatory for fly ash to immobilize and detoxify. The change rules of pH values in leachate of before and after three fly ashes are very analogical. The pH value of leachate in 5.3 is a critical point. When pH value is less than 5.3, it would sharply raise. On the contrary, the change of leachate pH value becomes smooth. These conclusions will provide the important theory bases for the farther research treatment harmlessly of fly ashes.
The fly ashes from MSW incinerator were conducted in a tube melting furnace in this study. The changes of microstructure, mineralogical composition, heavy metals distribution, leaching characteristics of samples before and after melting treatment were explored. The emphasis is on the effects additives on the melting characteristics and heavy metals distribution. Simultaneity, influences of melting temperature, melting time, basicity, additives, different atmosphere on the immobility and volatilization behavior of heavy metals during melting process. The results show that the melting temperature is an important factor on the melting treatment of fly ashes from MSW incinerator. At 1400℃, the molten sample became full smooth, much hard in surface structure, while the section of the molten sample had lustrous or no apparent aperture, the sample fly ash had completely melted. The slag melted is crystalloid. The amounts of crystalsincrease with the melting temperature elevation. The leaching rates of zinc, chromium, lead, copper, cadmium, mercury was very low in the products melted. The gaseous volatile of mercury, cadmium and lead is captured. The effect of heavy metals immobility was in sequence of silicon dioxide>calcium oxide>alumina. Melting temperature has an important impact on the behavior of heavy metals. There is a great difference for the behavior of immobility and volatilization of various heavy metals. The changes of basicity will give birth to the marked influence on the fixation rate of heavy metals. The proper additive rate of silicon dioxide will be propitious to enhance the fixation rate on the heavy metals. The fixation rates of chromium, nickel, copper and arsenic in melted samples would increase with the elevation of their melting point and boiling point at oxidizing atmosphere. The volatilization rates of lead, cadmium and mercury with low boiling points are very high during melting process. The reducing atmosphere would be propitious to enhancing the fixation rates of chromium, nickel, copper and arsenic. It is confirmed that mercury, cadmium, and zinc are more easily vaporized under reducing atmosphere, but the volatilization rate of lead would be inhibited at the same condition.
Based on the previous experimental results, the different fly ashes were melted in the self-developed swirling melting furnace system. The melting characteristics and behavior of heavy metals of fly ashes were investigated in detail under different operation runs. Influences of melting temperature, calcium oxide, silicon dioxide, magnesia additional reagent on the melting characteristics and behavior of heavy metals were studies during fly ashes melting process. The dynamic melting treatment characteristics and occurrence and transference of heavy metals in samples were concluded. Experimental results indicate that the fly ashes will transform into vitrification state at 1400℃. The higher melting temperature will redound to fly ashes melting treatment. There are marked differences on the influences of calcium oxide, silicon dioxide, magnesia additional reagent on the melting characteristics. Adding calcium oxide may effectively control melting point of fly ash. If adding less than 15 percent, it would be propitious to melting treatment. The melting-aid effect of calcium oxide should appropriately adjust base on composition of fly ash. Adding silicon dioxide in fly ash would redound to reducing the melting point of fly ash and advance the liquidity of sample. With the adding amount increasing of silicon dioxide, the glassy amorphous materials in the melted sample would enhance. The higher adding amount of silicon dioxide, the better is the stability of melted slag. The netlike structures of silicates in fly ash would be destroyed by the adding magnesia. The glutinosity of melted sample reduces with increasing adding amount of magnesia. The sample would achieve the better melting effect when the adding amount is less than 5 percent in fly ash sample. The glassy materials in slag would enhance and the crystal phases take place transform with adulterating magnesia. The crystals in sample are enveloped by the amorphous slag. The fixation rates of nickel, chromium, copper, cobalt, and manganese in slag increase with melting temperature heightening between 1250 and 1400 degree centigrade. With the exception of mercury, the change of melting temperature would markedly affect on the fixation rates of arsenic, lead, cadmium, zinc. The fixation rates of chromium, copper, manganese are decreased by adding calcium oxide during melting process. The lower is the fixation rate of arsenic, zinc, and lead, the more is adding calcium oxide. It is beneficial for the improvement fixation rate of heavy metals to add silicon dioxide. With the exception of mercury, the fixation rates of residual heavy metals would improve with adding amount increasing. The fixation rates of zinc, arsenic, cadmium, and lead would distinctly enhance. Adding amount being controlled at 10 percent for FA3 would achieve the optimal fixation effect. The volatile heavy metals are sensitive to melting temperature. With melting temperature increasing, the content of them takes on the increasing first and after reducing in flue gas. When calcium oxide adding amount is 5 percent, the content of volatile heavy metals would lessen in flue gas of melting treatment. It would give birth to negative effect for fixation heavy metals once calcium oxide adding exceeding 5 percent. With the increasing of silicon dioxide adding amount, the content of heavy metals in flue gas would reduce, but the content of mercury is ruleless. The adding magnesia in flyash has remarkable influence on the content of heavy metals in flue gas.
At last, the gas products of coal gasification were used as the substitutive fuel on melting treatment of fly ashes. The fly ashes were conducted in the experimental system associating coal gasification with melting treatment. The effects of air/coal ratio, steam/coal ratio, bed temperature and additives on the occurrence and transference of heavy metals during melting process on swirling furnace was systemically investigated. The fixation rates of nickel and chromium achieve the maximal value above 90 percent at different air/coal ratio condition. With increasing air/coal ratio, the fixation rates of copper, manganese, and cobalt enhance steadily, the fixation rates of volatile heavy metals take on the ascending. The fixation rates of arsenic and zinc is above 30 percent in slag, the fixation rate of cadmium becomes increasing first and after reducing in slag. That of mercury keeps stable. The fixation rates of cobalt, chromium, copper, manganese, nickel and volatile heavy metals increase first then reduce in slag with increasing steam/coal ratio, and fixation rates of them achieve the maximum at steam/coal ratio 0.41 kg·kg-1, those of chromium and nickel is above 90 percent. With the exception of manganese, the fixation rates of cobalt, chromium, copper, and nickel enhance with increasing bed temperature. The order of fixation rate is Ni>Cr>Cu>Mn>Co. With bed temperature increasing, the fixation rates of lead and cadmium aggrandize, the fixation rate of zinc is reductive, mercury keep stable. The adding magnesia in sample would conduce to increasing the fixation rate of nickel and chromium. The adding calcium oxide, silicon dioxide, magnesia would not be helpful to fixation of manganese. For copper, the fixation effect of silicon dioxide is the best, the magnesia is the better, calcium oxide is the worse. For cobalt, the order of fixation effect is magnesia>silicon dioxide>calcium oxide. The fixation rates of heavy metals would remarkably enhance when adding magnesia and silicon dioxide. For the volatile heavy metals such as arsenic, zinc, cadmium, and lead, the fixation effect of magnesia is better than that of silicon dioxide and calcium oxide. The fixation rates order of heavy metals is magnesia>silicon dioxide>calcium oxide. These conclusions will offer the experimental bases and theoretic references for further comprehending the melting treatment technology of fly ash.
Based on the experimental results and existent states of heavy metals in fly ashes and slag, the gas-solid reaction theory during the melting process, heat and mass transfer of particles in fly ashes, chemical dynamics theory such as volatile heavy metals diffuseness, the plentiful experimental datum were analyzed. The melting reaction model and the volatility model of heavy metals in particles during fly ashes melting process have been constructed. The results simulated from the predicted model are basically consistent with the measured values of experiments.
引文
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