氧/燃料燃烧方式下钙与铁对煤中氮释放特性的影响
摘要
煤炭作为目前我国最重要的常规能源,在燃烧过程中放出热量的同时,也向环境中排放了大量的污染物。在这些污染物中包括NOx、SOx、细微颗粒物、重金属等。研究表明,燃煤生成的NO和NO2是酸雨的前驱物,并且参与光化学烟雾污染的生成,N02还是一种温室气体。这些氮氧化物对人类的健康和生态环境都会产生严重的危害。NOx形成机理和释放特性的研究是进行氮氧化物危害评价、法规制定和排放控制的重要基础,因此开展这方面的研究具有重要的科学和实际意义。
氧/燃料燃烧技术是一种代替传统空气燃烧,有效减少CO2排放的燃煤新技术。在氧/燃料燃烧方式下,空气中分离出的氧气与循环烟气替代了传统煤粉燃烧方式下的空气,这样能得到高纯度的二氧化碳,从而降低了二氧化碳捕获的成本。在氧/燃料燃烧方式下,分子氮的量很低,这会抑制热力型NOx与快速型NOx的形成,从而降低整体NOx的排放率。普遍的结论是氧/燃料燃烧方式下NOx的排放量能减少到空气燃烧方式下的1/3到1/2,其主要原因与氧/燃料燃烧方式下的挥发份和煤焦有关。煤中含有大量矿物质,如Ca,Fe等,这些矿物质对煤热解及燃烧的过程都有很大的影响,它们对含氮物的释放特性也有各种不同的作用。本文从氧/燃料燃烧方式下NOx的排放量减少的原因着手,分析了CO2气氛下含氮物(HCN, NH3, NO和焦氮)的释放特性,以及煤焦燃烧和煤焦与循环烟气中NO反应的特性。并且在此基础上分析了钙和铁在反应过程中对含氮物释放特性的影响。本文主要内容如下：
应用酸洗的化学方法,以及物理混合和浸溶等矿物质添加方法来研究钙对煤热解过程含氮物释放特性的影响。在传统空气燃烧方式下,N2是主导气体。在氧/燃料燃烧方式下,循环后烟气中C02浓度可达90%以上。实验中煤粉热解气氛分别为N2和C02,用来研究热解气氛的不同引起的含氮物分布的差异。高浓度的N2会改变热解过程中的氮平衡,CO2气体会与NOx前驱物发生反应,所以这两个气氛对热解过程中含氮物释放特性分别会有很大的影响。同时在实验中也选用了不参与反应的惰性气体Ar为热解气氛,作为分析比较。结果发现,在分别添加(CH3COO)2Ca, Ca(OH)2和CaCl2时,焦产率随着钙的添加量的增加而降低。钙的添加对热解过程中HCN和NH3的生成的作用取决于添加钙的种类以及数量。Ar气氛下钙的添加能降低HCN和NH3的生成,而在N2气氛下钙的添加却能提高HCN和NH3的生成。在C02气氛下在热解气体中没有测量到NH3的浓度。但是在C02气氛下测量到了NO的浓度,而且NO的生成随着钙的添加量的增加而减少。
通过石英管式炉煤热解实验分析了不同热解气氛和不同氯化铁添加方式对含氮物释放特性的影响。氯化铁添加方式包含两种,一种是物理混合,另一种是煤样与氯化铁的水溶液混合。热解气氛有N2,C02和Ar。实验结果发现,在1000℃温度下,Ar气氛下热解时,酸洗煤添加氯化铁会抑制HCN的生成。但是在N2气氛下,HCN生成的量却增加,这是由于高浓度的N2抑制了氯化铁的作用。在C02气氛下,HCN的量明显降低,这是由于在C02气氛下氯化铁不仅促进挥发分的二次分解,还促进了焦氮的转化。在Ae和N2气氛下热解时,两种氯化铁的添加方式都能大幅度地降低NH3的生成。在C02气氛下没有测到NH3的量。
采用物理混合添加氧化铁,研究了铁对传统空气燃烧和氧/燃料燃烧方式下煤焦燃烧生成的NO的影响。在800℃温度下C02气氛中生成的煤焦颗粒尺寸比N2气氛下大,但是在1300℃时,煤焦颗粒却变小。这是由于煤焦与C02反生气化反应而引起的颗粒破碎。铁的添加能促进NO的转化率,而且铁的作用随着反应的进行而增强,并在最后保持稳定。实验结果表明,在氧/燃料燃烧方式下添加铁更能促进煤焦反应过程中NO的生成。
最后用高温沉降炉制焦,通过在石英管式炉中煤焦与NO的反应,研究了氧化铁对C02焦和NO反应的影响,并分析了CO对该反应的作用。实验结果表明,对于Ar焦与NO反应,添加氧化铁能促进反应的进行。煤焦中添加氧化铁后,NO释放的浓度的峰值比不添加氧化铁时要降低16%,而且从此开始,氧化铁对煤焦与NO反应的作用一直持续。煤焦与NO的反应是一个缓慢的长时间的过程,而其中氧化铁对反应的作用在一定条件下也是一个长期的作用。添加氧化铁后,CO释放曲线的峰值增加,这与NO释放曲线相互对应,是此消彼长的关系。
Coal as our most important conventional energy sources, while giving off heat in the combustion process, also releases a large number of pollutant emissions to the environment. These pollutants include NOx, SOx, fine particulate matter, trace metals and others. Studies have shown that coal-firing generated NO and NO2which are precursors of acid rain, and participate in the formation of photochemical smog pollution, and NO2is also a greenhouse gas. Nitrogen oxides will generate serious harm to human health and ecological environment. The understanding of NOx Formation Mechanism and Emission was an important foundation of the hazard assessment of nitrogen oxides, regulations and the emission control, to carry out research in this area has important scientific and practical significance.
Oxy-fuel combustion technology, insteading of traditional air combustion, is a new coal firing technology which can reduce the emission of CO2. In oxy-fuel combustion, O2which was seperated from air, and recycled flue gas took the place of air during traditional air combustion. It caused higher CO2concentration in flue gas, the cost of CO2capture would decrease as well. In oxy-fuel combustion, nitrogen was low, which would decrease the formation of thermal NOx and prompt NOx, so that the emission of NOx in whole would drop greatly. The general conclusion is that the emission of NOx in oxy-fuel combustion would decrease to1/3to1/2of that in air combustion, the main reason is related to volatile matter and char. There are lots of mineral matter, like Ca and Fe, which have great effect of coal pyrolysis and combustion. The mineral matter also have different effects on nitrogen species formation. The reason of NOx emission decrease in oxy-fuel combustion was analysed in this thesis, the nitrogen species(HCN, NH3, NO and char N)formation in CO2atmosphere was studied, the char combustion and the reaction of char in NO were studied too. The effects of Ca and Fe on nitrogen species formation were also analysed. The main contents were as follows:
With the methods of demineralization, mineral matter addition both of physically and with solution, the effects of Ca on nitrogen species distribution were studied. In conventional air combustion, N2is the dominant gas. The concentration of CO2would be higher than90%in oxy-fuel combustion with recycled flue gas. The pyrolysis atmospheres during experiments were N2and CO2, in order to study the effects of different atmospheres on nitrogen species formation. N2with high concentration would change nitrogen balance during pyrolysis, there is also reaction of CO2and precursors of NOx, which means that the two atmospheres have great effects on nitrogen species formation during pyrolysis. At the same time, Ar, which is inert, was choose as one pyrolysis atmosphere to analysis and compare. The results show that with three different Ca-based additives, i.e.,(CH3COO)2Ca, Ca(OH)2and CaCl2, char yield decreases with the increasing amount of Ca additives in all cases. The effect of Ca on HCN and NH3formation during pyrolysis depends on both the form of Ca and the amount of addition. HCN and NH3formation decreases with Ca addition in Ar, but increases in N2. There is no NH3detected during pyrolysis in CO2. In addition, NO concentration detected decreases sharply with increasing the amount of Ca addition in the atmosphere of CO2.
The effects of FeCl3addition on nitrogen distribution under different pyrolysis environments were studied by the experiments in horizontal tube furnace. Two mixing way were introduced, one was physically mixing, the other was mixing with a saturated aqueous solution of FeCl3. The results indicate that at the temperature of1000℃, FeCl3addition with DEM decreased HCN in pyrolysis atmosphere of Ar. In N2, FeCl3increased the release of HCN due to high concentration of N2. In atmosphere of CO2, the formation of HCN was much less than that in other environments, because of the effect of FeCl3on devolatilization and char conversion. In Ar or N2environments, NH3decreased sharply with FeCl3addition respectively. But there was no NH3measured under CO2.
The effects of Fe on NO formation under the reactions in air and oxy-fuel combustion were studied with the method of physically addition. The particle size of char generated at800℃in CO2is larger than that in N2. However, at1300℃, it is smaller in CO2atmosphere due to particle breaking by gasification of char and CO2. The Fe addition increases the NO conversion ratio, and the effect of Fe rises steeply with the process going until it becomes stable in the end. The results also indicate that the release of NO increases more significantly with the Fe addition in oxy-fuel environment.
Finally, the effect of Fe2O3on reaction of CO2-char and NO has been studied by experiments of devolatilization in high temperature drop tube furnace and the reaction of char and NO in horizontal tube furnace. It was found that the addition of Fe2O3promotes the reaction of Ar-char and NO. With Fe2O3addition, the peak of NO release dropped16%during the reaction of Ar-char and NO, from that point on, the effect of Fe2O3became stable. The reaction of char and NO was not a quick one, so the effect of Fe2O3was also lasting and effective. There was a strong connection between the release of NO and CO.
氧/燃料燃烧技术是一种代替传统空气燃烧,有效减少CO2排放的燃煤新技术。在氧/燃料燃烧方式下,空气中分离出的氧气与循环烟气替代了传统煤粉燃烧方式下的空气,这样能得到高纯度的二氧化碳,从而降低了二氧化碳捕获的成本。在氧/燃料燃烧方式下,分子氮的量很低,这会抑制热力型NOx与快速型NOx的形成,从而降低整体NOx的排放率。普遍的结论是氧/燃料燃烧方式下NOx的排放量能减少到空气燃烧方式下的1/3到1/2,其主要原因与氧/燃料燃烧方式下的挥发份和煤焦有关。煤中含有大量矿物质,如Ca,Fe等,这些矿物质对煤热解及燃烧的过程都有很大的影响,它们对含氮物的释放特性也有各种不同的作用。本文从氧/燃料燃烧方式下NOx的排放量减少的原因着手,分析了CO2气氛下含氮物(HCN, NH3, NO和焦氮)的释放特性,以及煤焦燃烧和煤焦与循环烟气中NO反应的特性。并且在此基础上分析了钙和铁在反应过程中对含氮物释放特性的影响。本文主要内容如下：
应用酸洗的化学方法,以及物理混合和浸溶等矿物质添加方法来研究钙对煤热解过程含氮物释放特性的影响。在传统空气燃烧方式下,N2是主导气体。在氧/燃料燃烧方式下,循环后烟气中C02浓度可达90%以上。实验中煤粉热解气氛分别为N2和C02,用来研究热解气氛的不同引起的含氮物分布的差异。高浓度的N2会改变热解过程中的氮平衡,CO2气体会与NOx前驱物发生反应,所以这两个气氛对热解过程中含氮物释放特性分别会有很大的影响。同时在实验中也选用了不参与反应的惰性气体Ar为热解气氛,作为分析比较。结果发现,在分别添加(CH3COO)2Ca, Ca(OH)2和CaCl2时,焦产率随着钙的添加量的增加而降低。钙的添加对热解过程中HCN和NH3的生成的作用取决于添加钙的种类以及数量。Ar气氛下钙的添加能降低HCN和NH3的生成,而在N2气氛下钙的添加却能提高HCN和NH3的生成。在C02气氛下在热解气体中没有测量到NH3的浓度。但是在C02气氛下测量到了NO的浓度,而且NO的生成随着钙的添加量的增加而减少。
通过石英管式炉煤热解实验分析了不同热解气氛和不同氯化铁添加方式对含氮物释放特性的影响。氯化铁添加方式包含两种,一种是物理混合,另一种是煤样与氯化铁的水溶液混合。热解气氛有N2,C02和Ar。实验结果发现,在1000℃温度下,Ar气氛下热解时,酸洗煤添加氯化铁会抑制HCN的生成。但是在N2气氛下,HCN生成的量却增加,这是由于高浓度的N2抑制了氯化铁的作用。在C02气氛下,HCN的量明显降低,这是由于在C02气氛下氯化铁不仅促进挥发分的二次分解,还促进了焦氮的转化。在Ae和N2气氛下热解时,两种氯化铁的添加方式都能大幅度地降低NH3的生成。在C02气氛下没有测到NH3的量。
采用物理混合添加氧化铁,研究了铁对传统空气燃烧和氧/燃料燃烧方式下煤焦燃烧生成的NO的影响。在800℃温度下C02气氛中生成的煤焦颗粒尺寸比N2气氛下大,但是在1300℃时,煤焦颗粒却变小。这是由于煤焦与C02反生气化反应而引起的颗粒破碎。铁的添加能促进NO的转化率,而且铁的作用随着反应的进行而增强,并在最后保持稳定。实验结果表明,在氧/燃料燃烧方式下添加铁更能促进煤焦反应过程中NO的生成。
最后用高温沉降炉制焦,通过在石英管式炉中煤焦与NO的反应,研究了氧化铁对C02焦和NO反应的影响,并分析了CO对该反应的作用。实验结果表明,对于Ar焦与NO反应,添加氧化铁能促进反应的进行。煤焦中添加氧化铁后,NO释放的浓度的峰值比不添加氧化铁时要降低16%,而且从此开始,氧化铁对煤焦与NO反应的作用一直持续。煤焦与NO的反应是一个缓慢的长时间的过程,而其中氧化铁对反应的作用在一定条件下也是一个长期的作用。添加氧化铁后,CO释放曲线的峰值增加,这与NO释放曲线相互对应,是此消彼长的关系。
Coal as our most important conventional energy sources, while giving off heat in the combustion process, also releases a large number of pollutant emissions to the environment. These pollutants include NOx, SOx, fine particulate matter, trace metals and others. Studies have shown that coal-firing generated NO and NO2which are precursors of acid rain, and participate in the formation of photochemical smog pollution, and NO2is also a greenhouse gas. Nitrogen oxides will generate serious harm to human health and ecological environment. The understanding of NOx Formation Mechanism and Emission was an important foundation of the hazard assessment of nitrogen oxides, regulations and the emission control, to carry out research in this area has important scientific and practical significance.
Oxy-fuel combustion technology, insteading of traditional air combustion, is a new coal firing technology which can reduce the emission of CO2. In oxy-fuel combustion, O2which was seperated from air, and recycled flue gas took the place of air during traditional air combustion. It caused higher CO2concentration in flue gas, the cost of CO2capture would decrease as well. In oxy-fuel combustion, nitrogen was low, which would decrease the formation of thermal NOx and prompt NOx, so that the emission of NOx in whole would drop greatly. The general conclusion is that the emission of NOx in oxy-fuel combustion would decrease to1/3to1/2of that in air combustion, the main reason is related to volatile matter and char. There are lots of mineral matter, like Ca and Fe, which have great effect of coal pyrolysis and combustion. The mineral matter also have different effects on nitrogen species formation. The reason of NOx emission decrease in oxy-fuel combustion was analysed in this thesis, the nitrogen species(HCN, NH3, NO and char N)formation in CO2atmosphere was studied, the char combustion and the reaction of char in NO were studied too. The effects of Ca and Fe on nitrogen species formation were also analysed. The main contents were as follows:
With the methods of demineralization, mineral matter addition both of physically and with solution, the effects of Ca on nitrogen species distribution were studied. In conventional air combustion, N2is the dominant gas. The concentration of CO2would be higher than90%in oxy-fuel combustion with recycled flue gas. The pyrolysis atmospheres during experiments were N2and CO2, in order to study the effects of different atmospheres on nitrogen species formation. N2with high concentration would change nitrogen balance during pyrolysis, there is also reaction of CO2and precursors of NOx, which means that the two atmospheres have great effects on nitrogen species formation during pyrolysis. At the same time, Ar, which is inert, was choose as one pyrolysis atmosphere to analysis and compare. The results show that with three different Ca-based additives, i.e.,(CH3COO)2Ca, Ca(OH)2and CaCl2, char yield decreases with the increasing amount of Ca additives in all cases. The effect of Ca on HCN and NH3formation during pyrolysis depends on both the form of Ca and the amount of addition. HCN and NH3formation decreases with Ca addition in Ar, but increases in N2. There is no NH3detected during pyrolysis in CO2. In addition, NO concentration detected decreases sharply with increasing the amount of Ca addition in the atmosphere of CO2.
The effects of FeCl3addition on nitrogen distribution under different pyrolysis environments were studied by the experiments in horizontal tube furnace. Two mixing way were introduced, one was physically mixing, the other was mixing with a saturated aqueous solution of FeCl3. The results indicate that at the temperature of1000℃, FeCl3addition with DEM decreased HCN in pyrolysis atmosphere of Ar. In N2, FeCl3increased the release of HCN due to high concentration of N2. In atmosphere of CO2, the formation of HCN was much less than that in other environments, because of the effect of FeCl3on devolatilization and char conversion. In Ar or N2environments, NH3decreased sharply with FeCl3addition respectively. But there was no NH3measured under CO2.
The effects of Fe on NO formation under the reactions in air and oxy-fuel combustion were studied with the method of physically addition. The particle size of char generated at800℃in CO2is larger than that in N2. However, at1300℃, it is smaller in CO2atmosphere due to particle breaking by gasification of char and CO2. The Fe addition increases the NO conversion ratio, and the effect of Fe rises steeply with the process going until it becomes stable in the end. The results also indicate that the release of NO increases more significantly with the Fe addition in oxy-fuel environment.
Finally, the effect of Fe2O3on reaction of CO2-char and NO has been studied by experiments of devolatilization in high temperature drop tube furnace and the reaction of char and NO in horizontal tube furnace. It was found that the addition of Fe2O3promotes the reaction of Ar-char and NO. With Fe2O3addition, the peak of NO release dropped16%during the reaction of Ar-char and NO, from that point on, the effect of Fe2O3became stable. The reaction of char and NO was not a quick one, so the effect of Fe2O3was also lasting and effective. There was a strong connection between the release of NO and CO.
引文
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