生物质热解油雾化燃烧及气化的实验研究与数值模拟
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摘要
能源危机及环境问题随着人类社会的快速发展日益严重,迫切需要开发可再生能源并实现产业化应用。生物质能作为唯一可再生碳源,具有可储存运输的特点,通过快速热解可以转化为生物油、可燃气以及炭粉。生物油的品质较差,与传统化石燃料具有较大差异且不能互溶,最为经济和方便的应用方法是直接燃烧,最具有前景的高品位应用方法是生物油分散制造、集中气化合成车用燃料。基于此背景,本学位论文通过实验和数值模拟技术较为系统地研究了生物油的雾化燃烧及气化特性,设计建立了生物油燃烧和气化应用装置。
在空气气氛下采用热失重技术研究生物油及其与小分子醇的混合燃料的燃烧性能,并与柴油和重油的燃烧性能进行对比。结果表明：生物油及其与小分子醇的混合燃料的燃烧都可分为三个阶段,即轻组分挥发、重组分裂解和焦炭燃烧；混合燃料中小分子醇质量分数不宜超过26%,否则其燃烧段的活化能增大,且热解焦炭所含有机官能团强度变弱,燃烧性能反而变差；生物油挥发性能及其焦炭燃烧性能均优于重油。
采用相位多普勒粒子分析仪,研究生物质热解油喷雾特性。生物油的索特平均直径沿着轴向距离的增加呈先减小后增大的趋势,而沿着径向呈单向增大的趋势；随着气液质量流量比的增加,液滴的平均直径不断减小,但减小趋势变缓；柴油雾化性能最好,生物油最差,添加甲醇或乙醇能增强生物油的雾化性能；利用试验数据拟合得到了生物油索特平均直径的经验公式。
利用流体力学软件FLUENT分别对重油和生物油在旋流燃烧室内的燃烧进行了数值模拟,对比研究了两种燃料的燃烧和污染物排放特性,考察了旋流强度对生物油燃烧特性的影响。模拟结果表明：旋流燃烧室内存在中心回流区,生物油燃烧时回流区面积和回流量均小于重油；重油燃烧的气体组分分布的模拟结果与文献测量值较吻合,炉膛最高温度比生物油燃烧高300K,CO和NO的排放量均比生物油高；随着空气旋流强度的增加,生物油燃烧时炉膛内回流区和回流量增大,CO的排放得到有效抑制,而NO排放量先升高后降低；生物油可以替代重油燃烧应用于很多工业场合。
对实验室自砌小型窑炉装置内生物油的燃烧进行三维数值模拟,获得了炉膛流场、温度场、组分分布、火焰形状及污染物排放的详细信息,揭示了炉膛内部流动、燃烧及传热传质过程的特点。模拟结果与试验数据吻合良好,验证了模型的可靠性。根据实验和模拟结果对窑炉燃烧系统进行优化,缩小了炉膛体积,简化了炉膛结构,更换了雾化喷嘴。进一步的燃烧实验和模拟结果表明：改造后的窑炉燃烧系统达到同样雾化效果所需的雾化空气量显著降低；虽然生物油流量减小,但燃烧室的最高温度(1450K)高于改造前的窑炉；雾化空气流量的增加可以减小雾化平均粒径、增强油气混合,从而缩短液相停留时间,增加燃尽程度；但雾化空气流量过大时,会携带燃料快速移动,导致部分未燃尽组分直接逃逸出炉膛；空气雾化流量2.0kg/h时,烟气中的一氧化碳浓度最小随着过量空气系数的增加,区域内氧气浓度、混合气体的速度增加,湍流和燃烧质量提高,CO浓度不断降低,NO浓度升高；在最佳过量空气系数1.22时,CO和NO浓度都在一个较低的水平。温度和污染物的排放浓度的模拟值和测量值吻合较好。
根据生物油燃烧特性的研究结果设计建立了一套模拟燃油锅炉的生物油燃烧装置,并进行了燃烧实验,获得了最佳运行参数。生物油燃烧前需要将炉膛预热到250℃,在有明火的条件下喷入生物油,即可点燃,但此时的燃烧不稳定,火焰位置较靠下游。随着燃烧时间的增加,火焰向前移动,监测点的温度增加,当燃烧约25分钟后,距喷口1.5m处的温度基本保持不变,此时燃烧稳定,污染物排放低于排放标准。
生物油在氮气下的热失重曲线表明气化分为挥发和热解两个阶段,升温速率的增加能减少固定碳的生成,增加气化效率。建立了生物油小型气化装置,通过实验和FLUENT模拟研究生物油的气化特性。气化炉内温度分布的模拟结果与实验值吻合较好；相同生物油流量下,载气可以阻止生物油组分间的反应炭化,但载气较大时会减小气化气体反应时间,使得气化不完全；通过计算,气体停留时间约1s以上时气化质量较高。部分供氧气化试验结果表明,CO2的产率随着当量比增加而线性增加,可燃气体产率随着当量比的增加先减小后增加,碳转化率提高,这是因为氧化反应使得局部区域反应温度上升。实验和模拟结果表明,部分生物油完全燃烧为其他生物油的气化提供热源是实现自热式高效气化的关键。
对生物质热解液化技术进行了经济性分析,证明了该技术实现产业化后具有良好的经济性：生物油替代化石燃油燃烧应用具有较好的经济效益；在费托合成工厂规模较大时,生物油气化替代生物质气化制备合成气的成本较低。此外,生物油的生产和利用还将带来显著的社会效益和环境效益。
With the rapid development of human society, increasing environmental concerns and the rising demand for fossil fuel have increased the necessity in developing and manufacturing alternative source of energy, which is renewable in nature. Biomass is the only renewable carbon source that can be storage and handling. Solid Biomass can be converted into carbon-rich liquid bio-oil, solid chars and non-condensable gas through a process called pyrolysis. The chemical and physical properties of bio-oil have much more differences with traditional fossil fuel and cannot dissolve each other. The most simple and feasible application of bio-oil is combustion. The most promising refined technology of bio-oil is to produce syngas via gasification, after that syngas is used to synthesize high-grade vehicle fuel. Based on this background, a series of experiments and numerical simulation were presented to integrally investigate bio-oil spraying properties, combustion and gasification characteristic. The bio-oil combustion and gasification plants were design and built.
Thermal weight loss curves of bio-oil and its blends with low molecular weight alcohols were determined by TG-DTA method in the oxygen atmosphere and compared with traditional fossil fuel diesel and heavy fuel oil. The thermo gravimetric cures of bio-oil and its blends with alcohols can be divided into three steps:volatilization, secondary char formation, and char combustion. With the increasing of alcohols content in the blend fuels, the active energies of volatilization and char combustion both decreased first and then increased. The mass fraction of alcohols should not exceed26%, otherwise the active energy of char combustion increased and the contained organic function groups in char decreased, which indicated higher stability and lower combustibility of the char. The volatility and char combustibility of bio-oil is better than heavy fuel oil.
The spray characteristics of bio-oil for combustion were investigated with Phase Doppler Anemometry (PDA) with Sauter mean diameter (SMD) as evaluating indicator. The results showed that SMD of bio-oil spray droplets exhibited a tendency to first decrease and then increase along axial direction and increased continuously along radial direction. The SMD diminished with the increase of gas-liquid flow ratio and had little variation when the gas-liquid flow ratio exceeded a certain value. Among three kinds of fuels, the atomizing quality of diesel was the best, while that of the bio-oil was the worst. By adding methanol or ethanol to the bio-oil, the atomizing quality was improved. The empirical equation for the SMD was derived. The predicted results were found to be in a good agreement with the experiment results.
FLUENT was used to simulate the combustion process of bio-oil and heavy fuel oil with the same heating value flow in a swirl combustion chamber. Combustion and emission characteristics of them were comparative study to provide useful data for the application of bio-oil, and the effects of swirl number on the bio-oil combustion were simulated. The results indicate that there existed central recirculation region, the recirculation area and flow of bio-oil combustion were smaller than heavy fuel oil combustion. The maximum furnace temperature of heavy fuel oil combustion is300K higher than bio-oil. The predicted gas species distributions of heavy fuel oil combustion were found to be in a reasonable agreement with the measurements, and heavy fuel oil release more CO and NO than bio-oil combustion in the flue gas. With the increase of swirl number, the recirculation area and flow increased, and the formation of CO can be effectively reduced, but the NO concentration in the outlet increased at first and then decreased. Bio-oil can replace heavy fuel oil combustion in the boiler.
Three-dimensional numerical simulation performed to obtain detailed information to reveal the characteristics of the flow, combustion, heat and mass transfer process in the kiln. The simulation results agreed well with the experimental results, which confirmed the reliability of the model. According to the experimental and simulated results, the kiln experimental combustion system optimized for reducing size and simplifying structure, a new atomizing nozzle employed. Combustion experiments and simulation results show that atomizing air flow rate achieving the same spraying quality significantly reduces. Although the oil flow rate decrease, measured combustion temperature (exceeds1450K) is higher than original kiln. Changing the atomizing air flow rate can be an optimizing factor in improving atomizing quality and liquid-oxygen mixing in central axis lead to short residence time to burn-out. The minimum CO and maximum NO concentration in flue gas obtained when air atomizing flow rate is2.0kg/h. With the increasing of equivalence ratio, the reacting oxygen concentration, turbulence and combustion quality is increased, combustion zone get downstream. The CO concentration in flue gas inhibited, while the formation of NO is increased. The optimum equivalence ratio is 1.22that CO and NO emissions both within a low level. The predicted temperature, CO and NO concentrations were in a reasonable agreement with the experiment data, which confirmed the reliability of the model.
Based on experimental and simulation results, taking into account the fuel characteristics of bio-oil, a bio-oil combustion device was build. The bio-oil could be ignited while the combustion chamber was preheated up to about250℃and existed naked flame. The flame was not stable at the beginning because the temperature of furnace was too low to evaporate bio-oil quickly. With the increase of burn time, the flame move downstream. After25min, the temperature at location1.5m from injection slightly increased from900K to1350K, the combustion flame became steady and the pollutant emissions were lower than emission standard.
The thermo gravimetric cures of bio-oil in the nitrogen atmosphere can be divided into two steps:volatilization and carbonization. The increasing of heating rate can reduce the formation of carbon, increase gasification efficiency. A bio-oil gasification device was build, a serious of experiments and simulation by FLUENT were presented. The experimental and predicted temperatures in gasification reactor are in reasonable agreement. The carrier gas N2inhibit the carbonization reaction between bio-oil components, but the high flow rate of carrier gas lead bio-oil gasification reaction time and gasification efficiency reduce. The gasification reaction time need be more than1s. With the increase of equivalence ratio, the combustible gas production decrease firstly and then increase, CO2production and carbon conversion increase because the oxidation reaction increase the gasification temperature. The experimental and simulation results indicate that part of the bio-oil complete combustion is the key to achieve effectively auto thermal gasification.
The economic analysis of biomass pyrolysis technology proves that the technology has a good economy for industrialization. The combustion application of bio-oil as a substitute for fossil fuel oil has good economic benefits. In a large Fischer-Tropsch synthesis plant, the cost of bio-oil gasification to produce synthesis gas is lower than biomass gasification. The production and utilization of bio-oil will bring significant social and environmental benefits.
在空气气氛下采用热失重技术研究生物油及其与小分子醇的混合燃料的燃烧性能,并与柴油和重油的燃烧性能进行对比。结果表明：生物油及其与小分子醇的混合燃料的燃烧都可分为三个阶段,即轻组分挥发、重组分裂解和焦炭燃烧；混合燃料中小分子醇质量分数不宜超过26%,否则其燃烧段的活化能增大,且热解焦炭所含有机官能团强度变弱,燃烧性能反而变差；生物油挥发性能及其焦炭燃烧性能均优于重油。
采用相位多普勒粒子分析仪,研究生物质热解油喷雾特性。生物油的索特平均直径沿着轴向距离的增加呈先减小后增大的趋势,而沿着径向呈单向增大的趋势；随着气液质量流量比的增加,液滴的平均直径不断减小,但减小趋势变缓；柴油雾化性能最好,生物油最差,添加甲醇或乙醇能增强生物油的雾化性能；利用试验数据拟合得到了生物油索特平均直径的经验公式。
利用流体力学软件FLUENT分别对重油和生物油在旋流燃烧室内的燃烧进行了数值模拟,对比研究了两种燃料的燃烧和污染物排放特性,考察了旋流强度对生物油燃烧特性的影响。模拟结果表明：旋流燃烧室内存在中心回流区,生物油燃烧时回流区面积和回流量均小于重油；重油燃烧的气体组分分布的模拟结果与文献测量值较吻合,炉膛最高温度比生物油燃烧高300K,CO和NO的排放量均比生物油高；随着空气旋流强度的增加,生物油燃烧时炉膛内回流区和回流量增大,CO的排放得到有效抑制,而NO排放量先升高后降低；生物油可以替代重油燃烧应用于很多工业场合。
对实验室自砌小型窑炉装置内生物油的燃烧进行三维数值模拟,获得了炉膛流场、温度场、组分分布、火焰形状及污染物排放的详细信息,揭示了炉膛内部流动、燃烧及传热传质过程的特点。模拟结果与试验数据吻合良好,验证了模型的可靠性。根据实验和模拟结果对窑炉燃烧系统进行优化,缩小了炉膛体积,简化了炉膛结构,更换了雾化喷嘴。进一步的燃烧实验和模拟结果表明：改造后的窑炉燃烧系统达到同样雾化效果所需的雾化空气量显著降低；虽然生物油流量减小,但燃烧室的最高温度(1450K)高于改造前的窑炉；雾化空气流量的增加可以减小雾化平均粒径、增强油气混合,从而缩短液相停留时间,增加燃尽程度；但雾化空气流量过大时,会携带燃料快速移动,导致部分未燃尽组分直接逃逸出炉膛；空气雾化流量2.0kg/h时,烟气中的一氧化碳浓度最小随着过量空气系数的增加,区域内氧气浓度、混合气体的速度增加,湍流和燃烧质量提高,CO浓度不断降低,NO浓度升高；在最佳过量空气系数1.22时,CO和NO浓度都在一个较低的水平。温度和污染物的排放浓度的模拟值和测量值吻合较好。
根据生物油燃烧特性的研究结果设计建立了一套模拟燃油锅炉的生物油燃烧装置,并进行了燃烧实验,获得了最佳运行参数。生物油燃烧前需要将炉膛预热到250℃,在有明火的条件下喷入生物油,即可点燃,但此时的燃烧不稳定,火焰位置较靠下游。随着燃烧时间的增加,火焰向前移动,监测点的温度增加,当燃烧约25分钟后,距喷口1.5m处的温度基本保持不变,此时燃烧稳定,污染物排放低于排放标准。
生物油在氮气下的热失重曲线表明气化分为挥发和热解两个阶段,升温速率的增加能减少固定碳的生成,增加气化效率。建立了生物油小型气化装置,通过实验和FLUENT模拟研究生物油的气化特性。气化炉内温度分布的模拟结果与实验值吻合较好；相同生物油流量下,载气可以阻止生物油组分间的反应炭化,但载气较大时会减小气化气体反应时间,使得气化不完全；通过计算,气体停留时间约1s以上时气化质量较高。部分供氧气化试验结果表明,CO2的产率随着当量比增加而线性增加,可燃气体产率随着当量比的增加先减小后增加,碳转化率提高,这是因为氧化反应使得局部区域反应温度上升。实验和模拟结果表明,部分生物油完全燃烧为其他生物油的气化提供热源是实现自热式高效气化的关键。
对生物质热解液化技术进行了经济性分析,证明了该技术实现产业化后具有良好的经济性：生物油替代化石燃油燃烧应用具有较好的经济效益；在费托合成工厂规模较大时,生物油气化替代生物质气化制备合成气的成本较低。此外,生物油的生产和利用还将带来显著的社会效益和环境效益。
With the rapid development of human society, increasing environmental concerns and the rising demand for fossil fuel have increased the necessity in developing and manufacturing alternative source of energy, which is renewable in nature. Biomass is the only renewable carbon source that can be storage and handling. Solid Biomass can be converted into carbon-rich liquid bio-oil, solid chars and non-condensable gas through a process called pyrolysis. The chemical and physical properties of bio-oil have much more differences with traditional fossil fuel and cannot dissolve each other. The most simple and feasible application of bio-oil is combustion. The most promising refined technology of bio-oil is to produce syngas via gasification, after that syngas is used to synthesize high-grade vehicle fuel. Based on this background, a series of experiments and numerical simulation were presented to integrally investigate bio-oil spraying properties, combustion and gasification characteristic. The bio-oil combustion and gasification plants were design and built.
Thermal weight loss curves of bio-oil and its blends with low molecular weight alcohols were determined by TG-DTA method in the oxygen atmosphere and compared with traditional fossil fuel diesel and heavy fuel oil. The thermo gravimetric cures of bio-oil and its blends with alcohols can be divided into three steps:volatilization, secondary char formation, and char combustion. With the increasing of alcohols content in the blend fuels, the active energies of volatilization and char combustion both decreased first and then increased. The mass fraction of alcohols should not exceed26%, otherwise the active energy of char combustion increased and the contained organic function groups in char decreased, which indicated higher stability and lower combustibility of the char. The volatility and char combustibility of bio-oil is better than heavy fuel oil.
The spray characteristics of bio-oil for combustion were investigated with Phase Doppler Anemometry (PDA) with Sauter mean diameter (SMD) as evaluating indicator. The results showed that SMD of bio-oil spray droplets exhibited a tendency to first decrease and then increase along axial direction and increased continuously along radial direction. The SMD diminished with the increase of gas-liquid flow ratio and had little variation when the gas-liquid flow ratio exceeded a certain value. Among three kinds of fuels, the atomizing quality of diesel was the best, while that of the bio-oil was the worst. By adding methanol or ethanol to the bio-oil, the atomizing quality was improved. The empirical equation for the SMD was derived. The predicted results were found to be in a good agreement with the experiment results.
FLUENT was used to simulate the combustion process of bio-oil and heavy fuel oil with the same heating value flow in a swirl combustion chamber. Combustion and emission characteristics of them were comparative study to provide useful data for the application of bio-oil, and the effects of swirl number on the bio-oil combustion were simulated. The results indicate that there existed central recirculation region, the recirculation area and flow of bio-oil combustion were smaller than heavy fuel oil combustion. The maximum furnace temperature of heavy fuel oil combustion is300K higher than bio-oil. The predicted gas species distributions of heavy fuel oil combustion were found to be in a reasonable agreement with the measurements, and heavy fuel oil release more CO and NO than bio-oil combustion in the flue gas. With the increase of swirl number, the recirculation area and flow increased, and the formation of CO can be effectively reduced, but the NO concentration in the outlet increased at first and then decreased. Bio-oil can replace heavy fuel oil combustion in the boiler.
Three-dimensional numerical simulation performed to obtain detailed information to reveal the characteristics of the flow, combustion, heat and mass transfer process in the kiln. The simulation results agreed well with the experimental results, which confirmed the reliability of the model. According to the experimental and simulated results, the kiln experimental combustion system optimized for reducing size and simplifying structure, a new atomizing nozzle employed. Combustion experiments and simulation results show that atomizing air flow rate achieving the same spraying quality significantly reduces. Although the oil flow rate decrease, measured combustion temperature (exceeds1450K) is higher than original kiln. Changing the atomizing air flow rate can be an optimizing factor in improving atomizing quality and liquid-oxygen mixing in central axis lead to short residence time to burn-out. The minimum CO and maximum NO concentration in flue gas obtained when air atomizing flow rate is2.0kg/h. With the increasing of equivalence ratio, the reacting oxygen concentration, turbulence and combustion quality is increased, combustion zone get downstream. The CO concentration in flue gas inhibited, while the formation of NO is increased. The optimum equivalence ratio is 1.22that CO and NO emissions both within a low level. The predicted temperature, CO and NO concentrations were in a reasonable agreement with the experiment data, which confirmed the reliability of the model.
Based on experimental and simulation results, taking into account the fuel characteristics of bio-oil, a bio-oil combustion device was build. The bio-oil could be ignited while the combustion chamber was preheated up to about250℃and existed naked flame. The flame was not stable at the beginning because the temperature of furnace was too low to evaporate bio-oil quickly. With the increase of burn time, the flame move downstream. After25min, the temperature at location1.5m from injection slightly increased from900K to1350K, the combustion flame became steady and the pollutant emissions were lower than emission standard.
The thermo gravimetric cures of bio-oil in the nitrogen atmosphere can be divided into two steps:volatilization and carbonization. The increasing of heating rate can reduce the formation of carbon, increase gasification efficiency. A bio-oil gasification device was build, a serious of experiments and simulation by FLUENT were presented. The experimental and predicted temperatures in gasification reactor are in reasonable agreement. The carrier gas N2inhibit the carbonization reaction between bio-oil components, but the high flow rate of carrier gas lead bio-oil gasification reaction time and gasification efficiency reduce. The gasification reaction time need be more than1s. With the increase of equivalence ratio, the combustible gas production decrease firstly and then increase, CO2production and carbon conversion increase because the oxidation reaction increase the gasification temperature. The experimental and simulation results indicate that part of the bio-oil complete combustion is the key to achieve effectively auto thermal gasification.
The economic analysis of biomass pyrolysis technology proves that the technology has a good economy for industrialization. The combustion application of bio-oil as a substitute for fossil fuel oil has good economic benefits. In a large Fischer-Tropsch synthesis plant, the cost of bio-oil gasification to produce synthesis gas is lower than biomass gasification. The production and utilization of bio-oil will bring significant social and environmental benefits.
引文
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