煤/生物质气化合成气燃烧特性的激光诊断研究
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摘要
由煤、生物质、有机废弃物的气化产生的合成气是一种很有前景的清洁高效燃料,主要组成为H2、CO、CH4、C02、02、N2等,与固体燃料直接燃烧相比,不仅能够提高能源利用效率,而且还能有效降低污染物排放,在未来的能源利用与转化方面具有极大的潜力。但是合成气的气体组成复杂、热值低、燃烧不稳定,加上其燃烧机理研究的不足,给实际应用带来很大挑战。因此,深入研究合成气的燃烧特性、高效清洁的利用合成气,是我国清洁能源战略的一个重要组成部分。
激光燃烧诊断技术具有不干扰流场、对恶劣的燃烧环境适应性强等优点,是研究火焰燃烧机理的理想手段。本文运用先进的激光燃烧诊断技术,对合成气的预混层流和湍流燃烧特性以及臭氧的强化燃烧展开了一系列的研究,形成了比较全面、系统的合成气燃烧理论,不仅为我国新型燃烧设备的发展与优化提供了重要的基础与工程实践指导,而且对未来的燃烧科学研究领域和工程设计也有着重要的意义。
本文先利用瑞利散射对烟煤气化合成气在稀薄预混条件下的层流火焰温度进行了定量测量,并与热电偶测量及CHEMKIN数值计算结果进行了对比分析；然后利用热流量法和热敏磷光测温法测量了两种典型合成气：5%H2-95%CO和20%H2-20%CO-60%N2的绝热层流火焰速度,并运用CHEMKIN的三种机理：GRI-Mech3.0, USC Mech Ⅱ和Davis'H2/CO进行了计算与对比验证。结果发现,氮气稀释对合成气的层流火焰速度有抑制作用,而预热温度的提高对火焰速度有促进作用；热流量法测合成气层流火焰速度的最小误差为0.5975cm/s；三种机理中Davis'H2/CO机理能够更好地预测H2/CO合成气的层流火焰速度。
接下来,本文模拟了真实组分的低热值煤／生物质气化合成气,利用OH-PLIF技术,对四种典型煤／生物质气化合成气的稀薄预混湍流火焰特性进行了试验研究与分析,包括湍流火焰结构、火焰前锋位置和湍流火焰速度等。研究表明,当量比、氢气含量、低热值和湍流强度对合成气火焰中OH自由基的强度分布、OH反应层的厚度、火焰长度、火焰前锋位置以及湍流火焰速度均有一定的影响；四种合成气中烟煤气化合成气的湍流火焰速度最大、更有利于燃烬；湍流强度可以压缩OH反应层的厚度,增强OH自由基的强度分布,从而强化了合成气的燃烧过程。
最后,本文利用热流量法精确测量了甲烷-空气预混气在有/无臭氧添加条件下的绝热层流火焰速度,研究了臭氧浓度变化对燃烧速度的影响,并改进了新的16步臭氧机理,运用CHEMKIN软件的PREMIX模块,对甲烷-空气-臭氧预混火焰的温度、主要自由基的分布、10个关键反应的敏感度分析以及火焰速度进行了计算与验证,确定了对臭氧增强火焰速度起关键作用的机理反应,进一步研究了臭氧分子的强化燃烧机理。研究表明,臭氧分子的加入,在火焰的预热区产生了大量的O自由基,从而激发了支链反应的发生,提高了火焰速度,强化了燃烧。
Syngas, derived from coal, biomass and organic waste gasification, is considered to be a more attractive fuel due to the cleanness and high efficiency. Compared with direct combustion of solid fuel, syngas (basis CO/H2/CH4/CO2/N2/O2) can not only enhance energy utilization efficiency but also reduce the toxic emission, which is very potential for further energy conversion and utilization. However, the complex gas composition, much lower low calorific value (LCV) and combustion instability of syngas as well as the shortage of combustion mechanism research, the practical application of syngas is faced with huge challenge. Therefore, it is necessary to investigate the combustion characteristic in depth, and efficiently and cleanly utilize the LCV syngas.
Laser diagnostics in combustion is a kind of ideal instrument for combustion mechanism investigation due to the noninterference for flow field and nice applicability for the abominable combustion environment. Premixed laminar and turbulent combustion characteristic of syngas and combustion enhancement of O3were investigated using advanced laser diagnostics technology and formed a relative comprehensive and systemic syngas combustion theory, which not only provide groundwork and guidance for the development and optimize of new combustion equipment, but also have great meaning for future combustion science and engineering design.
First, laminar flame temperatures of lean premixed bituminous coal gasification syngas were measured quantitatively using Rayleigh scattering and the results of thermocouple and CHEMKIN calculation were also carried out to compare with the experimental results; then adiabatic laminar flame speeds of two typical syngases:5%H2-95%CO and20%H2-20%CO-60%N2were accurately measured using improved Heat Flux method and thermographic phosphor. Three chemical kinetic mechanisms:GRI-Mech3.0, USC Mech Ⅱ and Davis'H2/CO were adopted to calculate and evaluate the experimental data. Results show that N2dilution restrain the flame speed of syngas while higher preheat temperature accelerate the flame speed. The smallest measurement uncertainty of the flame speed using heat flux method in present measurement was±0.5975cm/s. The Davis'H2/CO mechanism gives the best prediction among all the three models.
Then, lean premixed turbulent flame characteristics of several typical coal/biomass gasification syngases were investigated using OH planar laser induced fluorescence (PLIF) technology, including turbulent flame structure, flame front and turbulent flame speed etc. The syngases were prepared according to the actual gas composition of syngas. Results show that equivalence ratio, H2content, LCV and turbulence intensity are the most effective factors influencing the OH radical intensity distribution, thickness of OH reaction layer, flame length, flame front and turbulent flame speed. The bituminous coal gasification syngas has the fastest turbulent flame speed and tends to burn out easily. Through changes in thickness of the OH layers and signal intensities, the reaction layer can be compressed by intensifying turbulence and thereby the combustion processes of syngas.
In the end, the adiabatic laminar flame speeds of premixed methane/air flames with/without O3additive were accurately measured using the Heat Flux method, and the effect of O3on the enhancement of flame speed was investigated. An improved new16-step O3kinetic mechanism were proposed and adopted in the PREMIX module of CHEMKIN to calculate and validate the experimental results, including the premixed flame temperature, main radical distribution, sensitivity analysis of10key reactions and flame speed. The crucial reactions for the combustion enhancement by ozone additive were confirmed and the enhancement mechanism of ozone was investigated. Results show that Extra O radicals contributed by O3molecules in the pre-heat zone initiate and accelerate the chain-branching reactions and consequently increase the burning velocity.
激光燃烧诊断技术具有不干扰流场、对恶劣的燃烧环境适应性强等优点,是研究火焰燃烧机理的理想手段。本文运用先进的激光燃烧诊断技术,对合成气的预混层流和湍流燃烧特性以及臭氧的强化燃烧展开了一系列的研究,形成了比较全面、系统的合成气燃烧理论,不仅为我国新型燃烧设备的发展与优化提供了重要的基础与工程实践指导,而且对未来的燃烧科学研究领域和工程设计也有着重要的意义。
本文先利用瑞利散射对烟煤气化合成气在稀薄预混条件下的层流火焰温度进行了定量测量,并与热电偶测量及CHEMKIN数值计算结果进行了对比分析；然后利用热流量法和热敏磷光测温法测量了两种典型合成气：5%H2-95%CO和20%H2-20%CO-60%N2的绝热层流火焰速度,并运用CHEMKIN的三种机理：GRI-Mech3.0, USC Mech Ⅱ和Davis'H2/CO进行了计算与对比验证。结果发现,氮气稀释对合成气的层流火焰速度有抑制作用,而预热温度的提高对火焰速度有促进作用；热流量法测合成气层流火焰速度的最小误差为0.5975cm/s；三种机理中Davis'H2/CO机理能够更好地预测H2/CO合成气的层流火焰速度。
接下来,本文模拟了真实组分的低热值煤／生物质气化合成气,利用OH-PLIF技术,对四种典型煤／生物质气化合成气的稀薄预混湍流火焰特性进行了试验研究与分析,包括湍流火焰结构、火焰前锋位置和湍流火焰速度等。研究表明,当量比、氢气含量、低热值和湍流强度对合成气火焰中OH自由基的强度分布、OH反应层的厚度、火焰长度、火焰前锋位置以及湍流火焰速度均有一定的影响；四种合成气中烟煤气化合成气的湍流火焰速度最大、更有利于燃烬；湍流强度可以压缩OH反应层的厚度,增强OH自由基的强度分布,从而强化了合成气的燃烧过程。
最后,本文利用热流量法精确测量了甲烷-空气预混气在有/无臭氧添加条件下的绝热层流火焰速度,研究了臭氧浓度变化对燃烧速度的影响,并改进了新的16步臭氧机理,运用CHEMKIN软件的PREMIX模块,对甲烷-空气-臭氧预混火焰的温度、主要自由基的分布、10个关键反应的敏感度分析以及火焰速度进行了计算与验证,确定了对臭氧增强火焰速度起关键作用的机理反应,进一步研究了臭氧分子的强化燃烧机理。研究表明,臭氧分子的加入,在火焰的预热区产生了大量的O自由基,从而激发了支链反应的发生,提高了火焰速度,强化了燃烧。
Syngas, derived from coal, biomass and organic waste gasification, is considered to be a more attractive fuel due to the cleanness and high efficiency. Compared with direct combustion of solid fuel, syngas (basis CO/H2/CH4/CO2/N2/O2) can not only enhance energy utilization efficiency but also reduce the toxic emission, which is very potential for further energy conversion and utilization. However, the complex gas composition, much lower low calorific value (LCV) and combustion instability of syngas as well as the shortage of combustion mechanism research, the practical application of syngas is faced with huge challenge. Therefore, it is necessary to investigate the combustion characteristic in depth, and efficiently and cleanly utilize the LCV syngas.
Laser diagnostics in combustion is a kind of ideal instrument for combustion mechanism investigation due to the noninterference for flow field and nice applicability for the abominable combustion environment. Premixed laminar and turbulent combustion characteristic of syngas and combustion enhancement of O3were investigated using advanced laser diagnostics technology and formed a relative comprehensive and systemic syngas combustion theory, which not only provide groundwork and guidance for the development and optimize of new combustion equipment, but also have great meaning for future combustion science and engineering design.
First, laminar flame temperatures of lean premixed bituminous coal gasification syngas were measured quantitatively using Rayleigh scattering and the results of thermocouple and CHEMKIN calculation were also carried out to compare with the experimental results; then adiabatic laminar flame speeds of two typical syngases:5%H2-95%CO and20%H2-20%CO-60%N2were accurately measured using improved Heat Flux method and thermographic phosphor. Three chemical kinetic mechanisms:GRI-Mech3.0, USC Mech Ⅱ and Davis'H2/CO were adopted to calculate and evaluate the experimental data. Results show that N2dilution restrain the flame speed of syngas while higher preheat temperature accelerate the flame speed. The smallest measurement uncertainty of the flame speed using heat flux method in present measurement was±0.5975cm/s. The Davis'H2/CO mechanism gives the best prediction among all the three models.
Then, lean premixed turbulent flame characteristics of several typical coal/biomass gasification syngases were investigated using OH planar laser induced fluorescence (PLIF) technology, including turbulent flame structure, flame front and turbulent flame speed etc. The syngases were prepared according to the actual gas composition of syngas. Results show that equivalence ratio, H2content, LCV and turbulence intensity are the most effective factors influencing the OH radical intensity distribution, thickness of OH reaction layer, flame length, flame front and turbulent flame speed. The bituminous coal gasification syngas has the fastest turbulent flame speed and tends to burn out easily. Through changes in thickness of the OH layers and signal intensities, the reaction layer can be compressed by intensifying turbulence and thereby the combustion processes of syngas.
In the end, the adiabatic laminar flame speeds of premixed methane/air flames with/without O3additive were accurately measured using the Heat Flux method, and the effect of O3on the enhancement of flame speed was investigated. An improved new16-step O3kinetic mechanism were proposed and adopted in the PREMIX module of CHEMKIN to calculate and validate the experimental results, including the premixed flame temperature, main radical distribution, sensitivity analysis of10key reactions and flame speed. The crucial reactions for the combustion enhancement by ozone additive were confirmed and the enhancement mechanism of ozone was investigated. Results show that Extra O radicals contributed by O3molecules in the pre-heat zone initiate and accelerate the chain-branching reactions and consequently increase the burning velocity.
引文
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