O_2/CO_2气氛下燃煤中硫与氮在热场中转化行为的研究
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摘要
煤燃烧过程中产生的SO_2、NO_X、CO_2引起的酸雨、光化学烟雾及温室效应等对环境造成了严重的危害。O_2/CO_2燃烧技术采用烟气再循环,以CO_2代替空气中的N_2参与煤燃烧,将烟气中CO_2的浓度提高到95%,使CO_2的回收极为方便,能同时实现对SO_2、CO_2、NO_X及其它污染物的控制,是一种环境友好型的新型燃烧技术。目前有关O_2/CO_2燃烧技术的研究主要集中在该技术的燃烧特性和经济性评价等方面,而有关O_2/CO_2燃烧技术下燃煤有关组分的化学转化过程的研究较少。燃煤中的污染组分如硫、氮及重金属等在O_2/CO_2燃烧方式下的转化特性的研究对于探索该方式下污染物SO_2、NO_X的综合控制机理具有重要意义。
本文首先综述了O_2/CO_2燃烧方式的原理及燃煤中SO_2及NO_X排放特性的研究进展,然后对O_2/CO_2燃烧方式下碳酸钙作为脱硫剂的有关反应特性及反应机理、燃煤中硫与氮的转化特性进行了研究,并采用CHEMKIN软件对硫、氮的转化动力学进行了计算。
研究了O_2/CO_2气氛下温度对脱硫剂CaCO_3与SO_2的反应特性的影响。研究结果表明当温度超过500℃时,燃烧气氛对CaCO_3与SO_2的反应产率(钙转化率)产生较大影响。1200℃以下,空气气氛下钙转化率高于O_2/CO_2气氛;1200℃以上,则相反;随温度提高,两种气氛下钙转化率差异减小,表明O_2/CO_2气氛有利于高温钙基脱硫。实验还发现提高SO_2浓度可增加钙转化率是由于SO_2对硫化反应的促进及对硫酸钙分解的抑制;表明O_2/CO_2燃烧技术所运用的烟气循环方式导致SO_2的富集是其喷钙脱硫效率优于传统空气燃烧方式的原因之一。
O_2/CO_2气氛下CO_2浓度对CaCO_3分解反应产物CaO的微观结构有重要影响。热重分析表明CO_2浓度增加使CaCO_3起始分解温度提高,并使CaCO_3的分解速率降低,低浓度CO_2表现为催化CaO烧结,高浓度CO_2抑制CaCO_3的分解。研究结果还表明在一定温度下CaCO_3分解反应速率与硫化反应速率相当,可避免CaO烧结,改善CaSO_4对孔的堵塞,存在一最优孔隙结构,这种优化的孔隙结构是O_2/CO_2燃烧技术在高温下脱硫效率高于空气气氛的重要原因。XRD分析发现O_2/CO_2气氛下硫化产物组成随温度变化,硫化反应机理不同于空气气氛下,既有直接硫化反应机理也有先分解后硫化的间接硫化反应机理。
研究了三种煤质特性不同的燃煤(合山煤、算盘山煤、短陂桥煤)在O_2/CO_2气氛下硫的静态转化特性。结果表明三种燃煤在该气氛下SO_2生成量均低于相应的空气气氛下,这是由于燃煤燃烧特性的变化及烟气中高浓度CO还原SO_2所致。研究还发现O_2/CO_2气氛下煤质特性对硫转化为SO_2的影响远低于空气气氛下。加入CaCO_3作为脱硫剂后,1000℃以下,空气气氛下脱硫率高于O_2/CO_2气氛;1000℃以上,反之,且在一定温度范围内脱硫率随温度升高而增加的幅度较空气气氛下大。
采用滴管炉实验装置在800℃-1300℃温度范围研究了O_2/CO_2气氛下合山煤中的硫的动态转化特性,探讨了CO_2浓度、温度等因素对SO_2生成的影响,并通过红外光谱及元素分析等手段研究了相关机理。研究结果表明CO_2浓度是影响燃煤中硫动态转化特性的重要因素,当CO_2为80%时,烟气中SO_2浓度远小于比空气气氛下;同时,元素分析结果发现底灰中硫含量高于空气气氛下,表明硫转化为SO_2的转化率降低。红外光谱表征结果表明O_2/CO_2气氛下燃煤中硫转化产物存在多种形式如COS等,SO_2只是众多转化产物的一种。研究还发现CO_2浓度对碳酸钙的最佳固硫温度有着重要影响。当CO_2浓度为分别40%和80%时,最佳的固硫温度则相应为900℃和1000℃。CHEMKIN动力学计算结果亦表明高温时硫的转化速率快于低温情况下的速率;SO_2含量的最终平衡值受反应温度和CO_2浓度的双重影响,COS的生成量随着气氛中CO_2浓度的增加而增加,与实验结果一致。
O_2/CO_2气氛下对不同煤质特性燃煤的氮的静态转化特性研究表明燃烧气氛对氮转化为NO_X的影响与温度有关。O_2/CO_2气氛下NO_X生成量明显降低。700℃到900℃是NO_X生成量随温度变化最敏感的温度区域,较之空气气氛,700℃时NO_X生成量降低近50%,是NO_X被CO还原所致。O_2/CO_2气氛下,CaCO_3对NO_X生成峰值的影响与温度密切相关。燃煤中氮含量仍是影响NO_X生成的重要因素,O_2/CO_2气氛更有利于降低高挥发份燃煤NO_X生成量。
探索了CO_2对气相中NO还原特性的影响。CO_2对NO还原率的影响与燃烧气氛的氧化或还原特性有关。氧化性气氛中CO_2的存在能促进NO的还原,且NO的还原率随CO_2浓度增而增加;而还原性气氛CO_2的存在不利于NO的还原。采用CHEMKIN软件对NO转化动力学进行了计算,计算结果与实验结果吻合较好。
The pollutants from coal combustion are harmful to environment.Among them,CO_2 is responsible for greenhouse effect,SO_2 is the cause of acid rain and NOx can form optical chemical fog.O_2/CO_2 combustion technology using CO_2 instead of N_2 for coal combustion with flue gas recirculation,which enriches CO_2 concentration up to 95%for easily CO_2 capture,can also reduce the emission of SO_2 and NO_x.So it is a promising advanced coal combustion technology which can simultaneously control CO_2,SO_2 and NO_x and friendly to environment.The main researches related to this technology focused on the coal combustion behavior and the economic evaluation.However,few papers have been reported on the coal's component transfer process under this technology.The investigation on the transfer behavior of some pollutant components such as sulfur and nitrogen is very important for clarity the mechanism of SO_2 and NO_x reduction under this technology.
In this work,the reaction characteristics and mechanism of calcium carbonate as desulphurization agent and the transfer characteristics of sulfur and nitrogen of coal in O_2/CO_2 mixtures were studied and the chemical kinetic simulation by CHEMKIN was also obtained.The main contents are as follows:
The effect of temperature on the characteristic of the reaction of CaCO_3 and SO_2 under O_2/CO_2 atmosphere was invesitigated.It was found that the atmosphere influenced the calcium conversion ratio when temperature was above 500℃.For instance,the calcium conversion ratio in O_2/CO_2 mixture was lower than that in air at 900℃and higher than that in air at 1200℃.The difference of calcium conversion ratio between O_2/CO_2 mixtures and air decreased with the temperature increasing.It indicated that high temperature was beneficial for SO_2 capture in O_2/CO_2 mixtures.The results also suggested that the calcium conversion ratio increased with increasing of SO_2 concentration for high SO_2 concentration contributed to the equilibrium of reaction of CaCO_3 - SO_2 and prevented the decomposition of CaSO_4.The enrichment of SO_2 in combustion atmosphere by flue gas recirculation is one of the reasons for higher desulphurization ratio under O_2/CO_2 combustion technology than that under air.
The CO_2 concentration influenced the microstructure of CaO in O_2/CO_2 atmosphere. The low CO_2 concentration catalyzed the sintering of CaO while the high concentration prevented the decomposition of CaCO_3.The kinetic and thermodynamics analysis suggested that high CO_2 concentration increased the decomposition temperature of CaCO_3 and decreased the CaCO_3 decomposition velocity.The results also indicated that CO_2 concentration had pronounced influence on the microstructure of product of sulfation reaction It has an optimum microstructure in calcium sorbent;in this case,the desulphurization ratio was the highest because the velocity of decomposition reaction and the sulfation reaction was approximately the same.The results also suggest that the conversion ratio can be increased by increasing the concentration of SO_2,which causeed the inhibition of CaSO_4 decomposition and shifting of the reaction equilibrium toward the products.XRD analysis of the product showed that the reaction mechanism was different at varied temperatures,i.e.CaCO_3 directly reacted with SO_2 at low temperatures and CaO from CaCO_3 decomposition reacted with SO_2 at higher temperatures.
The static sulfur transfer behaviors of three different coals(heshan,suanpanshan and duanpiqiao) under O_2/CO_2 atmosphere were obtained using fixed bed apparatus.From the results,the SO_2 emission was lower than ordinary air combustion and the SO_2 emission difference between O_2/CO_2 and air varied with the temperature,the maximum difference occurred at 700℃for the CO reduction effect.The coal property such as sulfur and volatile content influenced the SO_2 emission,but this effect was weaker under O_2/CO_2 compared with in air.When using CaCO_3 as SO_2 sorbent,the desulphurization ratio under O_2/CO_2 was higher than that in.air when the temperature above 1000℃and the enhancement extent of desulphurization ratio with temperature was also higher than that under air.
The dynamic sulfur transfer characteristics of Heshan high sulfur coal was carried out in a vertical tube electrical heating reactor at temperature range of 800℃-1300℃under O_2/CO_2.The effect of the CO_2 concentration and the temperature on the emission of SO_2 was investigated and the mechanism of the emission of SO_2 under O_2/CO_2 was revealed by FT-IR and elemental analysis.It was found that CO_2 in atmosphere decreased the emission of SO_2 and the lowest SO_2 emission occurred under 80%CO_2.The elemental analysis results showed that the sulfur in bottom ash was higher also suggested the lower transfer ratio from sulfur to SO_2 under O_2/CO_2.COS in flue gas suggested sulphur in coal could be transferred in different species under O_2/CO_2 and SO_2 is only one of them.The optimum temperature of limestone for desulphurization was affected by CO_2 concentration;it was 900℃under 40%CO_2 and 1000℃under 80%CO_2.The sulfur transfer chemical kinetics simulation which was performed with software CHEMKIN revealed that the final SO_2 concentration was affected by both temperature and the concentration of CO_2.The quantity of COS was increase with increasing the concentration of CO_2.The calculational results are consistent with the experimental data.
The static nitrogen transfer characteristics of different coals under O_2/CO_2 atmosphere were studied in a fixed bed tube-fumace.The results showed NO_x emission was affected markedly by temperature.High CO_2 concentration significantly decreased NO_x emission during coal combustion compared with conventional air condition due to the reduction of CO in O_2/CO_2.The effect of calcium carbonate on the NO_x peak value also related to the temperature.The NO_x emission was also influenced by the coal property and Ca/S molar. O_2/CO_2 atmosphere was beneficial for the decrease of NO_x emission of the coal with high volatility.
The effect of CO_2 on the reduction process of NO was conducted in bench-scale laminar CH_4 flames.NO reduction ratio related to the property of atmosphere.CO_2 accelerated the reduction of NO under oxidizing atmosphere,and the higher CO_2 concentration resulted in higher reduction ratio.However,reducing atmosphere is more promotional for the reduction process of NO.The chemical kinetics simulation results by CHEMKIN were consisted with that of the experiments.
本文首先综述了O_2/CO_2燃烧方式的原理及燃煤中SO_2及NO_X排放特性的研究进展,然后对O_2/CO_2燃烧方式下碳酸钙作为脱硫剂的有关反应特性及反应机理、燃煤中硫与氮的转化特性进行了研究,并采用CHEMKIN软件对硫、氮的转化动力学进行了计算。
研究了O_2/CO_2气氛下温度对脱硫剂CaCO_3与SO_2的反应特性的影响。研究结果表明当温度超过500℃时,燃烧气氛对CaCO_3与SO_2的反应产率(钙转化率)产生较大影响。1200℃以下,空气气氛下钙转化率高于O_2/CO_2气氛;1200℃以上,则相反;随温度提高,两种气氛下钙转化率差异减小,表明O_2/CO_2气氛有利于高温钙基脱硫。实验还发现提高SO_2浓度可增加钙转化率是由于SO_2对硫化反应的促进及对硫酸钙分解的抑制;表明O_2/CO_2燃烧技术所运用的烟气循环方式导致SO_2的富集是其喷钙脱硫效率优于传统空气燃烧方式的原因之一。
O_2/CO_2气氛下CO_2浓度对CaCO_3分解反应产物CaO的微观结构有重要影响。热重分析表明CO_2浓度增加使CaCO_3起始分解温度提高,并使CaCO_3的分解速率降低,低浓度CO_2表现为催化CaO烧结,高浓度CO_2抑制CaCO_3的分解。研究结果还表明在一定温度下CaCO_3分解反应速率与硫化反应速率相当,可避免CaO烧结,改善CaSO_4对孔的堵塞,存在一最优孔隙结构,这种优化的孔隙结构是O_2/CO_2燃烧技术在高温下脱硫效率高于空气气氛的重要原因。XRD分析发现O_2/CO_2气氛下硫化产物组成随温度变化,硫化反应机理不同于空气气氛下,既有直接硫化反应机理也有先分解后硫化的间接硫化反应机理。
研究了三种煤质特性不同的燃煤(合山煤、算盘山煤、短陂桥煤)在O_2/CO_2气氛下硫的静态转化特性。结果表明三种燃煤在该气氛下SO_2生成量均低于相应的空气气氛下,这是由于燃煤燃烧特性的变化及烟气中高浓度CO还原SO_2所致。研究还发现O_2/CO_2气氛下煤质特性对硫转化为SO_2的影响远低于空气气氛下。加入CaCO_3作为脱硫剂后,1000℃以下,空气气氛下脱硫率高于O_2/CO_2气氛;1000℃以上,反之,且在一定温度范围内脱硫率随温度升高而增加的幅度较空气气氛下大。
采用滴管炉实验装置在800℃-1300℃温度范围研究了O_2/CO_2气氛下合山煤中的硫的动态转化特性,探讨了CO_2浓度、温度等因素对SO_2生成的影响,并通过红外光谱及元素分析等手段研究了相关机理。研究结果表明CO_2浓度是影响燃煤中硫动态转化特性的重要因素,当CO_2为80%时,烟气中SO_2浓度远小于比空气气氛下;同时,元素分析结果发现底灰中硫含量高于空气气氛下,表明硫转化为SO_2的转化率降低。红外光谱表征结果表明O_2/CO_2气氛下燃煤中硫转化产物存在多种形式如COS等,SO_2只是众多转化产物的一种。研究还发现CO_2浓度对碳酸钙的最佳固硫温度有着重要影响。当CO_2浓度为分别40%和80%时,最佳的固硫温度则相应为900℃和1000℃。CHEMKIN动力学计算结果亦表明高温时硫的转化速率快于低温情况下的速率;SO_2含量的最终平衡值受反应温度和CO_2浓度的双重影响,COS的生成量随着气氛中CO_2浓度的增加而增加,与实验结果一致。
O_2/CO_2气氛下对不同煤质特性燃煤的氮的静态转化特性研究表明燃烧气氛对氮转化为NO_X的影响与温度有关。O_2/CO_2气氛下NO_X生成量明显降低。700℃到900℃是NO_X生成量随温度变化最敏感的温度区域,较之空气气氛,700℃时NO_X生成量降低近50%,是NO_X被CO还原所致。O_2/CO_2气氛下,CaCO_3对NO_X生成峰值的影响与温度密切相关。燃煤中氮含量仍是影响NO_X生成的重要因素,O_2/CO_2气氛更有利于降低高挥发份燃煤NO_X生成量。
探索了CO_2对气相中NO还原特性的影响。CO_2对NO还原率的影响与燃烧气氛的氧化或还原特性有关。氧化性气氛中CO_2的存在能促进NO的还原,且NO的还原率随CO_2浓度增而增加;而还原性气氛CO_2的存在不利于NO的还原。采用CHEMKIN软件对NO转化动力学进行了计算,计算结果与实验结果吻合较好。
The pollutants from coal combustion are harmful to environment.Among them,CO_2 is responsible for greenhouse effect,SO_2 is the cause of acid rain and NOx can form optical chemical fog.O_2/CO_2 combustion technology using CO_2 instead of N_2 for coal combustion with flue gas recirculation,which enriches CO_2 concentration up to 95%for easily CO_2 capture,can also reduce the emission of SO_2 and NO_x.So it is a promising advanced coal combustion technology which can simultaneously control CO_2,SO_2 and NO_x and friendly to environment.The main researches related to this technology focused on the coal combustion behavior and the economic evaluation.However,few papers have been reported on the coal's component transfer process under this technology.The investigation on the transfer behavior of some pollutant components such as sulfur and nitrogen is very important for clarity the mechanism of SO_2 and NO_x reduction under this technology.
In this work,the reaction characteristics and mechanism of calcium carbonate as desulphurization agent and the transfer characteristics of sulfur and nitrogen of coal in O_2/CO_2 mixtures were studied and the chemical kinetic simulation by CHEMKIN was also obtained.The main contents are as follows:
The effect of temperature on the characteristic of the reaction of CaCO_3 and SO_2 under O_2/CO_2 atmosphere was invesitigated.It was found that the atmosphere influenced the calcium conversion ratio when temperature was above 500℃.For instance,the calcium conversion ratio in O_2/CO_2 mixture was lower than that in air at 900℃and higher than that in air at 1200℃.The difference of calcium conversion ratio between O_2/CO_2 mixtures and air decreased with the temperature increasing.It indicated that high temperature was beneficial for SO_2 capture in O_2/CO_2 mixtures.The results also suggested that the calcium conversion ratio increased with increasing of SO_2 concentration for high SO_2 concentration contributed to the equilibrium of reaction of CaCO_3 - SO_2 and prevented the decomposition of CaSO_4.The enrichment of SO_2 in combustion atmosphere by flue gas recirculation is one of the reasons for higher desulphurization ratio under O_2/CO_2 combustion technology than that under air.
The CO_2 concentration influenced the microstructure of CaO in O_2/CO_2 atmosphere. The low CO_2 concentration catalyzed the sintering of CaO while the high concentration prevented the decomposition of CaCO_3.The kinetic and thermodynamics analysis suggested that high CO_2 concentration increased the decomposition temperature of CaCO_3 and decreased the CaCO_3 decomposition velocity.The results also indicated that CO_2 concentration had pronounced influence on the microstructure of product of sulfation reaction It has an optimum microstructure in calcium sorbent;in this case,the desulphurization ratio was the highest because the velocity of decomposition reaction and the sulfation reaction was approximately the same.The results also suggest that the conversion ratio can be increased by increasing the concentration of SO_2,which causeed the inhibition of CaSO_4 decomposition and shifting of the reaction equilibrium toward the products.XRD analysis of the product showed that the reaction mechanism was different at varied temperatures,i.e.CaCO_3 directly reacted with SO_2 at low temperatures and CaO from CaCO_3 decomposition reacted with SO_2 at higher temperatures.
The static sulfur transfer behaviors of three different coals(heshan,suanpanshan and duanpiqiao) under O_2/CO_2 atmosphere were obtained using fixed bed apparatus.From the results,the SO_2 emission was lower than ordinary air combustion and the SO_2 emission difference between O_2/CO_2 and air varied with the temperature,the maximum difference occurred at 700℃for the CO reduction effect.The coal property such as sulfur and volatile content influenced the SO_2 emission,but this effect was weaker under O_2/CO_2 compared with in air.When using CaCO_3 as SO_2 sorbent,the desulphurization ratio under O_2/CO_2 was higher than that in.air when the temperature above 1000℃and the enhancement extent of desulphurization ratio with temperature was also higher than that under air.
The dynamic sulfur transfer characteristics of Heshan high sulfur coal was carried out in a vertical tube electrical heating reactor at temperature range of 800℃-1300℃under O_2/CO_2.The effect of the CO_2 concentration and the temperature on the emission of SO_2 was investigated and the mechanism of the emission of SO_2 under O_2/CO_2 was revealed by FT-IR and elemental analysis.It was found that CO_2 in atmosphere decreased the emission of SO_2 and the lowest SO_2 emission occurred under 80%CO_2.The elemental analysis results showed that the sulfur in bottom ash was higher also suggested the lower transfer ratio from sulfur to SO_2 under O_2/CO_2.COS in flue gas suggested sulphur in coal could be transferred in different species under O_2/CO_2 and SO_2 is only one of them.The optimum temperature of limestone for desulphurization was affected by CO_2 concentration;it was 900℃under 40%CO_2 and 1000℃under 80%CO_2.The sulfur transfer chemical kinetics simulation which was performed with software CHEMKIN revealed that the final SO_2 concentration was affected by both temperature and the concentration of CO_2.The quantity of COS was increase with increasing the concentration of CO_2.The calculational results are consistent with the experimental data.
The static nitrogen transfer characteristics of different coals under O_2/CO_2 atmosphere were studied in a fixed bed tube-fumace.The results showed NO_x emission was affected markedly by temperature.High CO_2 concentration significantly decreased NO_x emission during coal combustion compared with conventional air condition due to the reduction of CO in O_2/CO_2.The effect of calcium carbonate on the NO_x peak value also related to the temperature.The NO_x emission was also influenced by the coal property and Ca/S molar. O_2/CO_2 atmosphere was beneficial for the decrease of NO_x emission of the coal with high volatility.
The effect of CO_2 on the reduction process of NO was conducted in bench-scale laminar CH_4 flames.NO reduction ratio related to the property of atmosphere.CO_2 accelerated the reduction of NO under oxidizing atmosphere,and the higher CO_2 concentration resulted in higher reduction ratio.However,reducing atmosphere is more promotional for the reduction process of NO.The chemical kinetics simulation results by CHEMKIN were consisted with that of the experiments.
引文
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