O_2/CO_2煤粉燃烧脱硫及NO生成特性实验和理论研究
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摘要
能源是人类赖以生存发展的基础，煤的燃烧是提供能源的主要方式。随经济的发展，燃煤与日俱增来满足能源的供给，而同时燃煤过程污染物排放又加重了环境的负担。其中CO_2是温室效应产生的根源，而SO_2、NOx导致了酸雨沉降。经济发展和环境保护相协调成为世界性的问题，开发高效低污染的煤粉燃烧技术势在必行。
近年来O_2／CO_2煤粉燃烧技术日渐得到世界各国的关注，许多研究机构陆续投入到相关的研究之中。该技术以纯氧代替空气，并与烟气再循环相结合。因为减少了占空气79％不支持燃烧的N_2所致的排烟热量损失，使燃烧效率得到很大提高，促进了能源的有效利用。此外，可以将排烟中CO_2浓度提高到95％，方便了CO_2的回收利用。基于此研究O_2／CO_2气氛下煤粉燃烧机理将为该技术的推广和应用提供理论基础。
本文研究了O_2／CO_2气氛下煤粉燃烧特性、SO_2钙基脱除的直接硫化特性及NOx燃煤排放特性，并对燃烧过程进行了数值模拟，主要工作概括为以下六个方面：
1．借用热重分析手段比较了空气和O_2／CO_2气氛下煤粉的燃烧特性，并就固硫特性作初步讨论。通过对莱阳煤、长广煤、太平煤三种煤种的着火温度、燃尽温度、及燃烧特性指数的分析，表明O_2／CO_2气氛下的燃烧优于空气，并从反应动力学数据得到证实。同时，借助定硫仪初步比较了煤粉在空气和O_2／CO_2两种气氛下的硫析出特性，结果表明后者脱硫效果有很大改善。
2．分别以热重仪及沉降炉研究了中等温度(800℃～900℃)和较高温(900～1250℃)下空气和O_2／CO_2两种气氛钙基脱硫特性。在热重分析仪上考察了中等温度下温度、O_2和SO_2浓度、粒径等主要因素对直接硫化CaCO_3-SO_2过程的影响，并求取了反应的活化能。在沉降炉上考察了较高温下O_2／CO_2气氛中温度、Ca／S、不同CO_2体积浓度、炉内停留时间、过量空气系数、煤种等参量的影响。
3．建立了高温条件下CaSO_4分解的吉布斯自由能与温度的函数关系，并求取了SO_2分解压力与分解温度之间的关系，在此基础上得到了CaSO_4高温热力学分解特性。并与直接硫化过程进行了对比，进而判断出O_2／CO_2气氛有利于阻止CaSO_4的热力分解。在热力学分析的基础上，借用热重分析评价CO_2、SO_2和O_2浓度对CaSO_4分解的影响，求取反应活化能。并采用不反应缩核模型比较O_2／CO_(2-)空气两种气氛下反应过程控制因素的变化特性。
4．借助压汞孔结构分析、电镜扫描及热重分析等手段，研究了Na2CO_3、K2CO_3、Al_2O_3及Cs_2CO_3对CaCO_3微观孔结构性质及硫化转化的影响，结果表明：Na_2CO_3、K_2CO_3、Al_2(SO_4)_3的加入优化了孔尺寸分布、增加了孔隙率和表面积，对直接硫化过程有促进作用。而Cs_2CO_3的作用正好相反。从灰熔点的分析得出Na_2CO_3
浙江大学博卜学位论文刘彦
摘要
的加入并没有导致结渣的加重。
5.用沉降炉分析了02/CO:煤粉燃烧中NOx的释放特性，得出煤粉燃烧过程
02/C氏气氛较空气下有助于抑制NOx的排放。考察了温度、不同煤种、过量空
气系数对NOx生成特性的影响。并以甲烷等混气模拟了炉内气氛，分析了燃料
氮、循环氮及两者同时存在对NOx生成的影响。
6.根据煤粉燃烧条件，选取合适的模型，借助Fluent软件对沉降炉内空气一02/c 02
两种气氛下煤粉燃烧及NOx污染物生成特性进行数值模拟，得到了炉内温度分
布特性、传热特性及污染物生成特性，并与实验数据作了比较。
7.初步讨论膜分离制氧的基本原理和方法，提出为了推广q/Cq煤粉燃烧技术
的应用，开发高效低耗的膜分离制氧的方法成为必要。
关键词:
仇/C 02气氛煤粉燃烧热重分析直接硫化压汞仪孔结构分析SEM电镜扫描
分析XRD测试添加剂调制NOx排放沉降炉Fluent软件模拟制氧膜分离
Combustion of coal is a main means to provide energy which is the foundation to our living. The use of coal combustion is increasing steadily to meet the need of economy development. And the pollutants from coal combustion influence reversely on environment, among them CO2 is greenhouse gas , while SO2 and NOx is the cause of acid rain. At present, how to harmonize the relation between economy development and environment protection become the focus internationally. Developing a technology with high efficiency and low pollution is imperative under the situation.Recently the technology of O2/CO2 recycled combustion is gradually paid attention internationally, and many organizations have ploughed into it. In the process air is replaced by pure oxygen, and flue gas is recycled. The heat loss resulted from N2 release is cut down, so the combustion efficiency is improved greatly. At the same time the CO2 concentration in the flue gas is increased to 95% and it will be easy to capture. Therefore, much research is necessary for a better understanding.In the work the characteristics of coal combustion in O2/CO2, the direct sulfation of CaCO3-SO2 and NOx emission were studied and the coal combustion numerical simulation carried out. The job consists of aspects as followings:1. Combustion characteristics of the pulverized coal was studied by thermogravime-tric analysis under the O2/CO2 atmosphere and the results were compared with traditional air conditions. The ignition temperature and burnout temperature of the pulverized coal are significantly lowered under O2/CO2 conditions, so the burning characteristics are improved greatly. The conclusion is confirmed by dynamic analysis. It is shown that calcium-based desulfurization efficiency increases in O2/CO2 atmosphere.2. Sulfation process under moderate and high different temperature in both atmosphere of air- O2/CO2 was studied by thermogravimetric analysis and one dimension drop-tube experiment. The influence of temperature,O2 and SO2 concentration, and grain diameter on desulfurization efficiency was investigated by thermogravimetric analysis. The effect of temperature,Ca/S,CO2 volume percent, residual time, excessive air coefficient and coal species on sulfation process was studied under one dimension drop-tube.3. The thermodynamics characteristics of CaSO4 decomposition was obtained by establishing the relation between Gibbs Free Energy and T, and the decomposition pressure of SO2 and T. CaSO4 decomposition in O2/CO2 is prevented compare to air. The influence of the concentration of CO2, SO2 and O2 on CaSO4 decomposition was evaluated, and the activation energy was obtained.The results from experiment and
calculation consistent with the thermodynamic conclusion.4. The effect on pore structure and direct sulfation of CaCCb added by K2CO3 A12(SO4)3 and Cs2CO3 was studied by Pore Master and SEM analysis. The results show that by adding Na2CO3,K2CO3 or Al2(SO4)3, the pore structure of CaCO3 was optimized, and sulfation effect is improved. The other way round is in CS2CO3. Ash melting point is not lowered by adding of Na2CO3.5. The characteristics of NOx release in O2/CO2 atmosphere was studied and compared with air, the law was summed up by analyzing the effect of coal species, temperature, excessive air coefficient et al on it. The effect of fuel-N, recycled-N and the combination of them on characteristics of NOx release was investigated.6. The coal combustion process and characteristics of NOx release in O2/CO2-air was simulated with the Fluent software, the temperature field, heat exchange characteristics and NOx concentration field were obtained and the results were consistent with experiment.7. Discussed the membrane separation process and the principle to produce oxygen, and believed that the technology of coal combustion in O2/CO2 will be applied widely to industry with improving of producing oxygen by membrane separation process.
近年来O_2／CO_2煤粉燃烧技术日渐得到世界各国的关注，许多研究机构陆续投入到相关的研究之中。该技术以纯氧代替空气，并与烟气再循环相结合。因为减少了占空气79％不支持燃烧的N_2所致的排烟热量损失，使燃烧效率得到很大提高，促进了能源的有效利用。此外，可以将排烟中CO_2浓度提高到95％，方便了CO_2的回收利用。基于此研究O_2／CO_2气氛下煤粉燃烧机理将为该技术的推广和应用提供理论基础。
本文研究了O_2／CO_2气氛下煤粉燃烧特性、SO_2钙基脱除的直接硫化特性及NOx燃煤排放特性，并对燃烧过程进行了数值模拟，主要工作概括为以下六个方面：
1．借用热重分析手段比较了空气和O_2／CO_2气氛下煤粉的燃烧特性，并就固硫特性作初步讨论。通过对莱阳煤、长广煤、太平煤三种煤种的着火温度、燃尽温度、及燃烧特性指数的分析，表明O_2／CO_2气氛下的燃烧优于空气，并从反应动力学数据得到证实。同时，借助定硫仪初步比较了煤粉在空气和O_2／CO_2两种气氛下的硫析出特性，结果表明后者脱硫效果有很大改善。
2．分别以热重仪及沉降炉研究了中等温度(800℃～900℃)和较高温(900～1250℃)下空气和O_2／CO_2两种气氛钙基脱硫特性。在热重分析仪上考察了中等温度下温度、O_2和SO_2浓度、粒径等主要因素对直接硫化CaCO_3-SO_2过程的影响，并求取了反应的活化能。在沉降炉上考察了较高温下O_2／CO_2气氛中温度、Ca／S、不同CO_2体积浓度、炉内停留时间、过量空气系数、煤种等参量的影响。
3．建立了高温条件下CaSO_4分解的吉布斯自由能与温度的函数关系，并求取了SO_2分解压力与分解温度之间的关系，在此基础上得到了CaSO_4高温热力学分解特性。并与直接硫化过程进行了对比，进而判断出O_2／CO_2气氛有利于阻止CaSO_4的热力分解。在热力学分析的基础上，借用热重分析评价CO_2、SO_2和O_2浓度对CaSO_4分解的影响，求取反应活化能。并采用不反应缩核模型比较O_2／CO_(2-)空气两种气氛下反应过程控制因素的变化特性。
4．借助压汞孔结构分析、电镜扫描及热重分析等手段，研究了Na2CO_3、K2CO_3、Al_2O_3及Cs_2CO_3对CaCO_3微观孔结构性质及硫化转化的影响，结果表明：Na_2CO_3、K_2CO_3、Al_2(SO_4)_3的加入优化了孔尺寸分布、增加了孔隙率和表面积，对直接硫化过程有促进作用。而Cs_2CO_3的作用正好相反。从灰熔点的分析得出Na_2CO_3
浙江大学博卜学位论文刘彦
摘要
的加入并没有导致结渣的加重。
5.用沉降炉分析了02/CO:煤粉燃烧中NOx的释放特性，得出煤粉燃烧过程
02/C氏气氛较空气下有助于抑制NOx的排放。考察了温度、不同煤种、过量空
气系数对NOx生成特性的影响。并以甲烷等混气模拟了炉内气氛，分析了燃料
氮、循环氮及两者同时存在对NOx生成的影响。
6.根据煤粉燃烧条件，选取合适的模型，借助Fluent软件对沉降炉内空气一02/c 02
两种气氛下煤粉燃烧及NOx污染物生成特性进行数值模拟，得到了炉内温度分
布特性、传热特性及污染物生成特性，并与实验数据作了比较。
7.初步讨论膜分离制氧的基本原理和方法，提出为了推广q/Cq煤粉燃烧技术
的应用，开发高效低耗的膜分离制氧的方法成为必要。
关键词:
仇/C 02气氛煤粉燃烧热重分析直接硫化压汞仪孔结构分析SEM电镜扫描
分析XRD测试添加剂调制NOx排放沉降炉Fluent软件模拟制氧膜分离
Combustion of coal is a main means to provide energy which is the foundation to our living. The use of coal combustion is increasing steadily to meet the need of economy development. And the pollutants from coal combustion influence reversely on environment, among them CO2 is greenhouse gas , while SO2 and NOx is the cause of acid rain. At present, how to harmonize the relation between economy development and environment protection become the focus internationally. Developing a technology with high efficiency and low pollution is imperative under the situation.Recently the technology of O2/CO2 recycled combustion is gradually paid attention internationally, and many organizations have ploughed into it. In the process air is replaced by pure oxygen, and flue gas is recycled. The heat loss resulted from N2 release is cut down, so the combustion efficiency is improved greatly. At the same time the CO2 concentration in the flue gas is increased to 95% and it will be easy to capture. Therefore, much research is necessary for a better understanding.In the work the characteristics of coal combustion in O2/CO2, the direct sulfation of CaCO3-SO2 and NOx emission were studied and the coal combustion numerical simulation carried out. The job consists of aspects as followings:1. Combustion characteristics of the pulverized coal was studied by thermogravime-tric analysis under the O2/CO2 atmosphere and the results were compared with traditional air conditions. The ignition temperature and burnout temperature of the pulverized coal are significantly lowered under O2/CO2 conditions, so the burning characteristics are improved greatly. The conclusion is confirmed by dynamic analysis. It is shown that calcium-based desulfurization efficiency increases in O2/CO2 atmosphere.2. Sulfation process under moderate and high different temperature in both atmosphere of air- O2/CO2 was studied by thermogravimetric analysis and one dimension drop-tube experiment. The influence of temperature,O2 and SO2 concentration, and grain diameter on desulfurization efficiency was investigated by thermogravimetric analysis. The effect of temperature,Ca/S,CO2 volume percent, residual time, excessive air coefficient and coal species on sulfation process was studied under one dimension drop-tube.3. The thermodynamics characteristics of CaSO4 decomposition was obtained by establishing the relation between Gibbs Free Energy and T, and the decomposition pressure of SO2 and T. CaSO4 decomposition in O2/CO2 is prevented compare to air. The influence of the concentration of CO2, SO2 and O2 on CaSO4 decomposition was evaluated, and the activation energy was obtained.The results from experiment and
calculation consistent with the thermodynamic conclusion.4. The effect on pore structure and direct sulfation of CaCCb added by K2CO3 A12(SO4)3 and Cs2CO3 was studied by Pore Master and SEM analysis. The results show that by adding Na2CO3,K2CO3 or Al2(SO4)3, the pore structure of CaCO3 was optimized, and sulfation effect is improved. The other way round is in CS2CO3. Ash melting point is not lowered by adding of Na2CO3.5. The characteristics of NOx release in O2/CO2 atmosphere was studied and compared with air, the law was summed up by analyzing the effect of coal species, temperature, excessive air coefficient et al on it. The effect of fuel-N, recycled-N and the combination of them on characteristics of NOx release was investigated.6. The coal combustion process and characteristics of NOx release in O2/CO2-air was simulated with the Fluent software, the temperature field, heat exchange characteristics and NOx concentration field were obtained and the results were consistent with experiment.7. Discussed the membrane separation process and the principle to produce oxygen, and believed that the technology of coal combustion in O2/CO2 will be applied widely to industry with improving of producing oxygen by membrane separation process.
引文
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