废弃印刷线路板高温燃烧特性及溴迁移转化特性
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摘要
废弃物处置的研究意义不仅在于无害化排放,更在于资源的循环利用。目前相关研究所关注的各种废弃印刷线路板处置方法中,以高温燃烧为特征的火法冶金工艺具有资源化程度最大的优点,因而非常具有研究价值。本研究选择了废弃印刷线路板高温燃烧处置过程两个关键问题,高温燃烧特性、溴的迁移转化规律,进行了深入研究。
采用热重-红外联用技术研究了不同阶段／温度区间内线路板热解、燃烧特性,研究首次发现：挥发份释放阶段相同温度区间,空气氛围下挥发份的释放量相对于氮气氛围明显减少,这与一般燃料的挥发份释放规律明显不同。此结果为线路板实际处理时燃烧过程的组织提供了有价值的信息：在燃烧初期,减少或不提供新鲜空气将有效促进挥发份的释放,从而保证顺利点火、促进稳定燃烧。此外升温速率增加,反应时间缩短,固定碳氧化程度也略有增加,燃烧更加完全。这对焚烧工艺的选择及燃烧室设计有一定价值。
率先采用小型连续进料的管式沉降炉研究了不同操作条件对燃烧完全性的影响,结果显示：燃烧效率取决于温度、过量空气系数、烟气高温区平均停留时间。研究首次发现,在CO转化过程中,温度的影响非常显著。在温度相对较低时HBr转化为Br2的过程抑制了CO的转化。当温度达到1200℃以后,烟气中CO浓度急剧下降。要实现完全燃烧,提高燃烧温度是必要条件。在自行设计的15kg/hr中试装置中,验证了上述试验结果。研究结果为线路板实际处理时燃烧过程的组织提供了理论依据。
线路板燃烧过程,样品中有机溴首先转化为HBr进入烟气,在有氧存在时大部分HBr转化Br2。随着温度升高,更多的有机溴转化为无机溴。当温度超过1200℃,过量空气系数达到1.6时,99.9%以上的有机溴被摧毁,转化为无机溴进入烟气。因此,提高燃烧温度能有效减少线路板燃烧过程溴代二嗯英高温气相生成、减少后燃区低温异相催化生成溴代二噁英的前驱物。利用中试装置烟气冷却系统研究了烟气冷却过程无机溴的转化规律,研究首次发现在冷却过程中,烟气中有较多溴化氢转化为分子溴,温度越低烟气中分子溴比例越高。研究结果对处理废弃线路板高温燃烧产生的烟气及研究后燃区溴代二嗯英生成特性有重要意义：1)实际生产中脱除烟气中无机溴时主要针对分子溴,这与含氯物质燃烧产生的烟气中酸性气体的脱除(主要是氯化氢)不同。2)提供了一条回收烟气中无机溴的线索：采用冷凝方法促进烟气中的无机溴在低温时以分子溴形式析出。3)后燃区烟气冷却过程,对溴代二嗯英生成活性较高的溴源(Br2)不断增加。对以气相中无机溴为溴源的溴代二嗯英生成过程而言,温度变化时反应物浓度是不断变化的。4)研究不同溴源(HBr、Br2)在澳代二嗯英生成过程中所起的作用时,气相中的HBr和Br2的分布随温度变化发生动态变化。
The significance of research on waste treatment lies in the recycle of resource. Among the present processing methods of waste printed circuit boards (PCBs), pyrometallurgical processing featuring high temperature combustion is most promising due to its high recycling ratio of resources contained in waste PCBs. High temperature combustion is a key during this PCBs recycling. Research on the two crucial technical challenge in the high temperature combustion of PCBs, the characteristics of high temperature combustion and the conversion of bromine during the whole combustion process, were conducted in present work.
The pyrolysis and combustion characteristics of waste PCBs in various stage during thermal treatment were investigated by using a thermogravimetric analyzer (TGA). For the first time, the study discovers that during same temperature range of volatiles evolution stage, compared with that under pyrolysis condition, the evolution of volatiles decreases by24.4%under combustion condition. This is quiet different with that of common fuel. The result shows that in the combustion organization practice of waste PCBs, reducing the oxygen supply during the early stage of combustion will promote the volatiles emission and thereby promote ignition and stable combustion.
The effect of operating condition on combustion completion of waste PCBs was investigated by using the continuous feeding drop tube furnace. The results show that combustion efficiency depends on temperature, excess air factor (EAF) and the mean residence time in high temperature zone. For the first time, the research discovers that temperature has the most significant effect on CO conversion. In the case of lower temperature combustion, the conversion of CO to CO2is inhibited due to the conversion of HBr to Br2, while at1200℃or higher the concentration of CO in flue gas decreases dramatically. High temperature is required to improve the combustion performance. These results were verified by further proven experiments conducted in the self-designing pilot. The research provides theoretical basis for the combustion organization practice of waste PCBs
During the combustion of PCBs. organic bromine converts to HBr firstly and transfer into flue gas, in the presence of oxygen, most of the HBr converts to Br2. With the temperature increasing, the conversion of organic bromine to inorganic bromine increases. At1200℃or higher, an EAF of1.6or more, organobrominated compounds are successfully decomposed (more than99.9%). Thereby, with increasing combustion temperature, the formation of brominated dioxin by high temperature homogenous reaction is decreased greatly and the precursor for bominated dioxin formed by the low temperature heterogeneous catalytic synthesis is reduced. Research on the conversion of inorganic bromine in flue gas during cooling was conducted using the pilot, and for the first time, it was discovered that much HBr in flue gas convert to Br2during flue gas cooling. This is very important for the practice process selection of inorganic bromine removal and the further study of bominated dioxin formation characteristics:the process should be more suitable for separation of Br2from flue gas rather than HBr; during the flue gas cooling, Br2, the more active bromine source in gas phase for brominated dioxin formation by fly ash catalyzed de novo synthesis, increases continuously with the decrease of temperature.
采用热重-红外联用技术研究了不同阶段／温度区间内线路板热解、燃烧特性,研究首次发现：挥发份释放阶段相同温度区间,空气氛围下挥发份的释放量相对于氮气氛围明显减少,这与一般燃料的挥发份释放规律明显不同。此结果为线路板实际处理时燃烧过程的组织提供了有价值的信息：在燃烧初期,减少或不提供新鲜空气将有效促进挥发份的释放,从而保证顺利点火、促进稳定燃烧。此外升温速率增加,反应时间缩短,固定碳氧化程度也略有增加,燃烧更加完全。这对焚烧工艺的选择及燃烧室设计有一定价值。
率先采用小型连续进料的管式沉降炉研究了不同操作条件对燃烧完全性的影响,结果显示：燃烧效率取决于温度、过量空气系数、烟气高温区平均停留时间。研究首次发现,在CO转化过程中,温度的影响非常显著。在温度相对较低时HBr转化为Br2的过程抑制了CO的转化。当温度达到1200℃以后,烟气中CO浓度急剧下降。要实现完全燃烧,提高燃烧温度是必要条件。在自行设计的15kg/hr中试装置中,验证了上述试验结果。研究结果为线路板实际处理时燃烧过程的组织提供了理论依据。
线路板燃烧过程,样品中有机溴首先转化为HBr进入烟气,在有氧存在时大部分HBr转化Br2。随着温度升高,更多的有机溴转化为无机溴。当温度超过1200℃,过量空气系数达到1.6时,99.9%以上的有机溴被摧毁,转化为无机溴进入烟气。因此,提高燃烧温度能有效减少线路板燃烧过程溴代二嗯英高温气相生成、减少后燃区低温异相催化生成溴代二噁英的前驱物。利用中试装置烟气冷却系统研究了烟气冷却过程无机溴的转化规律,研究首次发现在冷却过程中,烟气中有较多溴化氢转化为分子溴,温度越低烟气中分子溴比例越高。研究结果对处理废弃线路板高温燃烧产生的烟气及研究后燃区溴代二嗯英生成特性有重要意义：1)实际生产中脱除烟气中无机溴时主要针对分子溴,这与含氯物质燃烧产生的烟气中酸性气体的脱除(主要是氯化氢)不同。2)提供了一条回收烟气中无机溴的线索：采用冷凝方法促进烟气中的无机溴在低温时以分子溴形式析出。3)后燃区烟气冷却过程,对溴代二嗯英生成活性较高的溴源(Br2)不断增加。对以气相中无机溴为溴源的溴代二嗯英生成过程而言,温度变化时反应物浓度是不断变化的。4)研究不同溴源(HBr、Br2)在澳代二嗯英生成过程中所起的作用时,气相中的HBr和Br2的分布随温度变化发生动态变化。
The significance of research on waste treatment lies in the recycle of resource. Among the present processing methods of waste printed circuit boards (PCBs), pyrometallurgical processing featuring high temperature combustion is most promising due to its high recycling ratio of resources contained in waste PCBs. High temperature combustion is a key during this PCBs recycling. Research on the two crucial technical challenge in the high temperature combustion of PCBs, the characteristics of high temperature combustion and the conversion of bromine during the whole combustion process, were conducted in present work.
The pyrolysis and combustion characteristics of waste PCBs in various stage during thermal treatment were investigated by using a thermogravimetric analyzer (TGA). For the first time, the study discovers that during same temperature range of volatiles evolution stage, compared with that under pyrolysis condition, the evolution of volatiles decreases by24.4%under combustion condition. This is quiet different with that of common fuel. The result shows that in the combustion organization practice of waste PCBs, reducing the oxygen supply during the early stage of combustion will promote the volatiles emission and thereby promote ignition and stable combustion.
The effect of operating condition on combustion completion of waste PCBs was investigated by using the continuous feeding drop tube furnace. The results show that combustion efficiency depends on temperature, excess air factor (EAF) and the mean residence time in high temperature zone. For the first time, the research discovers that temperature has the most significant effect on CO conversion. In the case of lower temperature combustion, the conversion of CO to CO2is inhibited due to the conversion of HBr to Br2, while at1200℃or higher the concentration of CO in flue gas decreases dramatically. High temperature is required to improve the combustion performance. These results were verified by further proven experiments conducted in the self-designing pilot. The research provides theoretical basis for the combustion organization practice of waste PCBs
During the combustion of PCBs. organic bromine converts to HBr firstly and transfer into flue gas, in the presence of oxygen, most of the HBr converts to Br2. With the temperature increasing, the conversion of organic bromine to inorganic bromine increases. At1200℃or higher, an EAF of1.6or more, organobrominated compounds are successfully decomposed (more than99.9%). Thereby, with increasing combustion temperature, the formation of brominated dioxin by high temperature homogenous reaction is decreased greatly and the precursor for bominated dioxin formed by the low temperature heterogeneous catalytic synthesis is reduced. Research on the conversion of inorganic bromine in flue gas during cooling was conducted using the pilot, and for the first time, it was discovered that much HBr in flue gas convert to Br2during flue gas cooling. This is very important for the practice process selection of inorganic bromine removal and the further study of bominated dioxin formation characteristics:the process should be more suitable for separation of Br2from flue gas rather than HBr; during the flue gas cooling, Br2, the more active bromine source in gas phase for brominated dioxin formation by fly ash catalyzed de novo synthesis, increases continuously with the decrease of temperature.
引文
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