增压富氧气氛中煤燃烧及污染物生成特性研究
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摘要
近年来,为了捕集和封存大型燃煤电站产生的CO2,富氧燃烧(又称O2/CO2燃烧)技术正获得国内外学者越来越多的关注。但现有富氧燃烧技术的空气分离制氧与高浓度CO2烟气压缩过程均在高压下进行,而富氧燃烧却在常压下进行,系统压力经历升—降—升,能量损失必然严重。增压富氧燃烧是一种基于常压富氧燃烧的新型高效燃烧技术,即从空分制氧、煤燃烧与锅炉换热,直到烟气压缩捕集CO2的全过程均维持在高压下完成。由于系统全过程整体增压,锅炉热效率和汽轮机的输出功率得到了提高,减少了CO2冷却压缩液化的电能消耗,在一定程度上抵消了系统增压所增加的功率消耗；同时增压富氧燃烧大大提高了烟气中水蒸汽的凝结温度,增加了从锅炉排烟中回收的热量,提高了机组的整体发电效率。由于反应条件与常规燃烧存在明显差别,增压富氧气氛中煤的燃烧及污染物生成特性尚不清楚。本文针对增压富氧条件下的煤燃烧过程开展了相关实验和理论研究,主要内容和成果如下：
(1)利用常压热分析系统研究了煤粉热解行为与着火机理之间的关联特性,进而采用固定床反应器探讨了热解特性对燃煤NO生成规律的影响。煤粉中低温下的热解行为对其富氧气氛下的着火机理影响显著。热解特性不同的煤粉富氧燃烧时的着火机理有所区别。提高氧气浓度可改善煤粉的燃烧特性,但着火机理的转变对煤粉综合燃烧特性的影响较小。热解行为、氧气浓度和温度均对NO生成特性有一定程度影响。由于热解特性的差异,煤样燃烧时的NO释放过程和最终的燃料氮NO转化率差别明显。氧气浓度和温度对燃料氮NO转换率的影响主要取决于挥发分氮氧化反应与还原反应的相互竞争。
(2)利用加压热分析系统对煤粉在增压富氧气氛中的燃烧特性进行了研究。随着压力的升高,煤粉的着火机理首先由多相着火转变为均相着火,然后又逐渐向多相着火过渡,并最终完全转变为多相着火。在均相着火时,压力升高后,挥发分燃烧速率逐渐加快,煤粉热解程度逐步加深。由于不同压力下着火机理的转变,煤粉的着火和燃尽温度以及相应的可燃性和燃尽特性指数并非随着压力的升高而单调变化,因而导致煤粉的综合燃烧特性指数随着压力的增加先升高后降低。此外,提高反应气氛中的氧浓度,可使煤粉的燃烧特性得到改善,但对着火机理无影响。
(3)采用傅里叶红外变换多气体分析仪分析了增压富氧燃烧时燃料氮的迁移特性,同时结合扫描电子显微镜以及X-射线衍射物相分析对燃煤成灰的形貌特征与矿物转变过程进行了研究。由于氮氧化合物前驱体的生成机理不同,压力升高后,其转化率变化规律并不一致。随着压力升高后挥发分产量的增加,燃料氮的NO和NO2转化率迅速升高,虽然在3MPa时NO2的转化率略有降低,但燃料氮的NOx转化率仍是单调上升的。因为压力升高后燃烧过程中生成的高孔隙率焦炭破碎更为频繁,所以煤粉燃尽后生成煤灰的粒径较小。在增压富氧燃烧时,煤粉着火机理的转变伴随着燃烧温度的变化。常压多相着火时的燃烧温度较高,煤灰中有很多莫来石等高温矿物,而压力升高后均相着火时的燃烧温度较低,煤灰中出现了大量伊利石等低温矿物。压力继续升高,均相着火开始向多相着火过渡,燃烧温度升高,低温矿物逐渐向高温矿物转化。
(4)搭建小型增压富氧燃烧鼓泡床试验台,对增压富氧燃煤NO生成特性进行了研究。结果表明,氧气浓度对于增压燃烧时NO生成特性的影响至关重要。系统总压升高后,若氧气浓度较低,煤燃烧过程中消耗的氧气无法及时补充,导致颗粒周围的还原性气氛较强,燃料氮的NO转化率逐渐下降；若氧气浓度较高,消耗的氧气能快速得到补充,颗粒周围的氧化性气氛较强,随着系统总压的升高,燃料氮的NO转化率逐渐增加。
(5)基于精确求解的实际气体混合物物性,建立了煤粉颗粒初始加热阶段的传热模型,对煤粉颗粒周围气体的瞬时传热过程进行了分析。随着压力的升高,煤粉颗粒周围气体的温度逐渐上升,周围气体对颗粒的加热作用更强,颗粒温升更迅速,从而使得煤粉热解提前。环境气温的升高可在一定程度上提高煤粉颗粒周围的瞬态气温以及颗粒本身的温度,但气氛的改变对此影响较小。
In recent years, to capture and storage CO2generated from large scale stationary power plants, oxy-fuel combustion (O2/CO2combustion) has caused wide attention of scholars both at home and abroad. However, both air separation unit (ASU) and the compression unit (CPU) for oxy-fuel combustion are operated at evaluated pressure, whereas the combustion is nonpressurized, thus serious energy loss occurs due to the change of operating pressure in different subsystems. Pressurized oxy-fuel combustion (POFC) is a novel and efficient combustion technology that derived from basic oxy-fuel combustion. In the POFC cycle, the ASU, combustion and heat transfer and CPU are all operated under pressure. By operating at elevated pressure, the thermal efficiency of the boiler increased and the power consumption of CO2condensation reduced which in turn make up for the power consumption of pressurization. In addition, more latent heat from flue gas can be recovered owing to higher condensation temperature of water vapor under pressure, and hence a larger fraction of thermal energy of the flue gases can be recovered to generate steam and the plant efficiency is improved. There are uncertainties regarding the characteristics of combustion and pollutant emission in pressurized oxy-fuel atmosphere due to the markedly different reaction conditions between POFC and traditional combustion. Therefore, both experimental and theoretical analysis are developed to investigate the burning process of pulverized coal in pressurized oxy-fuel atmosphere, main contents and results of the study include as follows:
(1) The associative characteristics between pyrolysis behavior and ignition mechanism of pulverized coal were studied with a thermal analysis system at atmospheric pressure, and then the effect of pyrolysis characteristic on NO formation were discussed in a fixed-bed reactor. The pyrolysis behavior of pulverized coal at low and moderate temperatures has significant effects on the ignition mechanism in oxy-fuel atmosphere. The ignition mechanism varies with the pyrolysis characteristic of pulverized coal during oxy-fuel combustion. The combustion performance can be improved by increasing oxygen concentration, but the transformation of ignition mechanism has little influence on the combustion characteristic of pulverized coal. Pyrolysis behavior, oxygen concentration and temperature all have an influence on the NO formation laws. During burning process, there are obvious differences on both of the release procedures of NO and the NO conversion rates of coals with different pyrolysis characteristics. The impact of oxygen concentration and temperature on the NO conversion rate depends primarily on the volatile-N oxidation and reduction reactions competing with each other.
(2) The combustion characteristics of pulverized coal in pressurized oxy-fuel atmosphere were investigated with a pressurized thermal analysis system. With the increase of pressure, the heterogeneous ignition first converts to homogeneous ignition, then begins to change to heterogeneous ignition gradually, and finally becomes heterogeneous ignition. When the pulverized coal ignites homogeneously, the burning rate of volatile increases with the rise in pressure and more volatile is generated. For the change of the ignition mechanism at different pressures, the ignition temperature and burnout temperature and the corresponding flammability index and burnout index don't change linearly with pressure to a maximum value. As a result, the combustibility index increases firstly and then reduces with the rise in pressure. In addition, the increase of oxygen concentration can enhance the intensity of combustion but does not affect the ignition mechanism of pulverized coal.
(3) The conversion of fuel-N of POFC was studied with Fourier transform infrared spectroscopy (FTIR), and the morphological features and mineral conversions were investigated with the combination of scanning electron microscopy (SEM) and X-ray diffractometer (XRD). The conversion rates of precursors are different from each other with the rise in pressure due to the different formation principles. Along with the increase of pressure and the yield of volatiles, the conversion rates of NO and NO2rise rapidly. Although the NO2conversion rate drops somewhat, the NOx conversion rate rises linearly with pressure to a maximum value. With the increase of pressure, the porous char particles fracture frequently which lead to a large number of fine ash particles. The combustion temperatures may be different due to the different ignition mechanisms. Because of the higher combustion temperature of heterogeneous ignition at atmospheric pressure, some minerals, such as mullite, generate in the ash, while some other minerals, such as illite, are found in the ash owing to the lower combustion temperature of homogeneous ignition at elevated pressure. As the pressure continues rising, with increase of combustion temperature the homogeneous ignition transforms to the heterogeneous ignition and low temperature minerals converts to high temperature minerals.
(4) The emission characteristics of NO were investigated with a test bench of pressurized bubbling fluidized bed. The results indicate that oxygen concentration has a significant effect on NO emission characteristics. With the increase of system pressure, because of the low oxygen concentration the oxygen consumed during combustion process can not get prompt supplement. As a result, the conversion rate of NO gradually decreases due to the strongly reducing atmosphere around particles. However, the oxygen consumed can get prompt supplement with high oxygen concentration. Thus the NO conversion rate increases by degrees due to the strongly oxidation atmosphere.
(5) Based on the exact solution of physical properties of actual gas mixtures, a heat transfer model of initial heating stage was set up to study the transient heat transfer around a particle. The gas temperature around the particle increases gradually with the rise in pressure, which leads to remarkable effect of the heating of gas on the particle. Therefore, the particle temperature increases quickly and the pyrolysis of pulverized coal moves up. The increase of environmental temperature can raise the transient gas temperature around the particle and particle temperature, but the change of atmosphere has little effect.
(1)利用常压热分析系统研究了煤粉热解行为与着火机理之间的关联特性,进而采用固定床反应器探讨了热解特性对燃煤NO生成规律的影响。煤粉中低温下的热解行为对其富氧气氛下的着火机理影响显著。热解特性不同的煤粉富氧燃烧时的着火机理有所区别。提高氧气浓度可改善煤粉的燃烧特性,但着火机理的转变对煤粉综合燃烧特性的影响较小。热解行为、氧气浓度和温度均对NO生成特性有一定程度影响。由于热解特性的差异,煤样燃烧时的NO释放过程和最终的燃料氮NO转化率差别明显。氧气浓度和温度对燃料氮NO转换率的影响主要取决于挥发分氮氧化反应与还原反应的相互竞争。
(2)利用加压热分析系统对煤粉在增压富氧气氛中的燃烧特性进行了研究。随着压力的升高,煤粉的着火机理首先由多相着火转变为均相着火,然后又逐渐向多相着火过渡,并最终完全转变为多相着火。在均相着火时,压力升高后,挥发分燃烧速率逐渐加快,煤粉热解程度逐步加深。由于不同压力下着火机理的转变,煤粉的着火和燃尽温度以及相应的可燃性和燃尽特性指数并非随着压力的升高而单调变化,因而导致煤粉的综合燃烧特性指数随着压力的增加先升高后降低。此外,提高反应气氛中的氧浓度,可使煤粉的燃烧特性得到改善,但对着火机理无影响。
(3)采用傅里叶红外变换多气体分析仪分析了增压富氧燃烧时燃料氮的迁移特性,同时结合扫描电子显微镜以及X-射线衍射物相分析对燃煤成灰的形貌特征与矿物转变过程进行了研究。由于氮氧化合物前驱体的生成机理不同,压力升高后,其转化率变化规律并不一致。随着压力升高后挥发分产量的增加,燃料氮的NO和NO2转化率迅速升高,虽然在3MPa时NO2的转化率略有降低,但燃料氮的NOx转化率仍是单调上升的。因为压力升高后燃烧过程中生成的高孔隙率焦炭破碎更为频繁,所以煤粉燃尽后生成煤灰的粒径较小。在增压富氧燃烧时,煤粉着火机理的转变伴随着燃烧温度的变化。常压多相着火时的燃烧温度较高,煤灰中有很多莫来石等高温矿物,而压力升高后均相着火时的燃烧温度较低,煤灰中出现了大量伊利石等低温矿物。压力继续升高,均相着火开始向多相着火过渡,燃烧温度升高,低温矿物逐渐向高温矿物转化。
(4)搭建小型增压富氧燃烧鼓泡床试验台,对增压富氧燃煤NO生成特性进行了研究。结果表明,氧气浓度对于增压燃烧时NO生成特性的影响至关重要。系统总压升高后,若氧气浓度较低,煤燃烧过程中消耗的氧气无法及时补充,导致颗粒周围的还原性气氛较强,燃料氮的NO转化率逐渐下降；若氧气浓度较高,消耗的氧气能快速得到补充,颗粒周围的氧化性气氛较强,随着系统总压的升高,燃料氮的NO转化率逐渐增加。
(5)基于精确求解的实际气体混合物物性,建立了煤粉颗粒初始加热阶段的传热模型,对煤粉颗粒周围气体的瞬时传热过程进行了分析。随着压力的升高,煤粉颗粒周围气体的温度逐渐上升,周围气体对颗粒的加热作用更强,颗粒温升更迅速,从而使得煤粉热解提前。环境气温的升高可在一定程度上提高煤粉颗粒周围的瞬态气温以及颗粒本身的温度,但气氛的改变对此影响较小。
In recent years, to capture and storage CO2generated from large scale stationary power plants, oxy-fuel combustion (O2/CO2combustion) has caused wide attention of scholars both at home and abroad. However, both air separation unit (ASU) and the compression unit (CPU) for oxy-fuel combustion are operated at evaluated pressure, whereas the combustion is nonpressurized, thus serious energy loss occurs due to the change of operating pressure in different subsystems. Pressurized oxy-fuel combustion (POFC) is a novel and efficient combustion technology that derived from basic oxy-fuel combustion. In the POFC cycle, the ASU, combustion and heat transfer and CPU are all operated under pressure. By operating at elevated pressure, the thermal efficiency of the boiler increased and the power consumption of CO2condensation reduced which in turn make up for the power consumption of pressurization. In addition, more latent heat from flue gas can be recovered owing to higher condensation temperature of water vapor under pressure, and hence a larger fraction of thermal energy of the flue gases can be recovered to generate steam and the plant efficiency is improved. There are uncertainties regarding the characteristics of combustion and pollutant emission in pressurized oxy-fuel atmosphere due to the markedly different reaction conditions between POFC and traditional combustion. Therefore, both experimental and theoretical analysis are developed to investigate the burning process of pulverized coal in pressurized oxy-fuel atmosphere, main contents and results of the study include as follows:
(1) The associative characteristics between pyrolysis behavior and ignition mechanism of pulverized coal were studied with a thermal analysis system at atmospheric pressure, and then the effect of pyrolysis characteristic on NO formation were discussed in a fixed-bed reactor. The pyrolysis behavior of pulverized coal at low and moderate temperatures has significant effects on the ignition mechanism in oxy-fuel atmosphere. The ignition mechanism varies with the pyrolysis characteristic of pulverized coal during oxy-fuel combustion. The combustion performance can be improved by increasing oxygen concentration, but the transformation of ignition mechanism has little influence on the combustion characteristic of pulverized coal. Pyrolysis behavior, oxygen concentration and temperature all have an influence on the NO formation laws. During burning process, there are obvious differences on both of the release procedures of NO and the NO conversion rates of coals with different pyrolysis characteristics. The impact of oxygen concentration and temperature on the NO conversion rate depends primarily on the volatile-N oxidation and reduction reactions competing with each other.
(2) The combustion characteristics of pulverized coal in pressurized oxy-fuel atmosphere were investigated with a pressurized thermal analysis system. With the increase of pressure, the heterogeneous ignition first converts to homogeneous ignition, then begins to change to heterogeneous ignition gradually, and finally becomes heterogeneous ignition. When the pulverized coal ignites homogeneously, the burning rate of volatile increases with the rise in pressure and more volatile is generated. For the change of the ignition mechanism at different pressures, the ignition temperature and burnout temperature and the corresponding flammability index and burnout index don't change linearly with pressure to a maximum value. As a result, the combustibility index increases firstly and then reduces with the rise in pressure. In addition, the increase of oxygen concentration can enhance the intensity of combustion but does not affect the ignition mechanism of pulverized coal.
(3) The conversion of fuel-N of POFC was studied with Fourier transform infrared spectroscopy (FTIR), and the morphological features and mineral conversions were investigated with the combination of scanning electron microscopy (SEM) and X-ray diffractometer (XRD). The conversion rates of precursors are different from each other with the rise in pressure due to the different formation principles. Along with the increase of pressure and the yield of volatiles, the conversion rates of NO and NO2rise rapidly. Although the NO2conversion rate drops somewhat, the NOx conversion rate rises linearly with pressure to a maximum value. With the increase of pressure, the porous char particles fracture frequently which lead to a large number of fine ash particles. The combustion temperatures may be different due to the different ignition mechanisms. Because of the higher combustion temperature of heterogeneous ignition at atmospheric pressure, some minerals, such as mullite, generate in the ash, while some other minerals, such as illite, are found in the ash owing to the lower combustion temperature of homogeneous ignition at elevated pressure. As the pressure continues rising, with increase of combustion temperature the homogeneous ignition transforms to the heterogeneous ignition and low temperature minerals converts to high temperature minerals.
(4) The emission characteristics of NO were investigated with a test bench of pressurized bubbling fluidized bed. The results indicate that oxygen concentration has a significant effect on NO emission characteristics. With the increase of system pressure, because of the low oxygen concentration the oxygen consumed during combustion process can not get prompt supplement. As a result, the conversion rate of NO gradually decreases due to the strongly reducing atmosphere around particles. However, the oxygen consumed can get prompt supplement with high oxygen concentration. Thus the NO conversion rate increases by degrees due to the strongly oxidation atmosphere.
(5) Based on the exact solution of physical properties of actual gas mixtures, a heat transfer model of initial heating stage was set up to study the transient heat transfer around a particle. The gas temperature around the particle increases gradually with the rise in pressure, which leads to remarkable effect of the heating of gas on the particle. Therefore, the particle temperature increases quickly and the pyrolysis of pulverized coal moves up. The increase of environmental temperature can raise the transient gas temperature around the particle and particle temperature, but the change of atmosphere has little effect.
引文
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