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A Study of Pollutant Formation from the Lean Premixed Combustion of Gaseous Fuel Alternatives to Natural Gas.

机译:天然气替代燃料的稀薄预混燃烧中污染物形成的研究。

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摘要

The goal of this research is to identify how nitrogen oxide (NO x) emissions and flame stability (blowout) are impacted by the use of fuels that are alternatives to typical pipeline natural gas. The research focuses on lean, premixed combustors that are typically used in state-of-the-art natural gas fueled systems. An idealized laboratory lean premixed combustor, specifically the jet-stirred reactor, is used for experimental data. A series of models, including those featuring detailed fluid dynamics and those focusing on detailed chemistry, are used to interpret the data and understand the underlying chemical kinetic reasons for differences in emissions between the various fuel blends. An ultimate goal is to use these data and interpretive tools to develop a way to predict the emission and stability impacts of changing fuels within practical combustors.;All experimental results are obtained from a high intensity, single-jet stirred reactor (JSR). Five fuel categories are studied: (1) pure H 2, (2) process and refinery gas, including combinations of H2, CH4, C2H6, and C3H8, (3) oxygen blown gasified coal/petcoke composed of H2, CO, and CO2, (4) landfill and digester gas composed of CH4, CO2, and N2, and (5) liquified natural gas (LNG)/shale/associated gases composed of CH4, C2H6, and C3 H8. NOx measurements are taken at a nominal combustion temperature of 1800 K, atmospheric pressure, and a reactor residence time of 3 ms. This is done to focus the results on differences caused by fuel chemistry by comparing all fuels at a common temperature, pressure, and residence time. This is one of the few studies in the literature that attempts to remove these effects when studying fuels varying in composition. Additionally, the effects of changing temperature and residence time are investigated for selected fuels. At the nominal temperature and residence time, the experimental and modeling results show the following trends for NOx emissions as a function of fuel type: 1.) NOx emissions decrease with increasing H2 fuel fraction for combustion of CH4/H2 blends. This appears to be caused by a reduction in the amount of NO made by the prompt pathway involving the reaction of N2 with hydrocarbon radicals as the CH4 is replaced by H2. 2.) For category 2 (the process and refinery blend) and category 5 (the LNG, shale, and associated gases), NOx emissions increase with the addition of C2 and C3 hydrocarbons. This could be due to an increased production of free radicals resulting from increasing CO production when higher molecular weight hydrocarbons are broken down. 3.) For category 3 (the O2 blown gasified coal/petcoke), NOx emissions increase with increasing CO fuel fraction. The reason for this is attributed to CO producing more radicals per unit heat release than H2. When CO replaces H2, an increase in NOx emissions is seen due to an increase in the productivity of the N2O, NNH, and Zeldovich pathways. 4.) For category 4 (the landfill gas) the addition of diluents such as CO2 and N2 at constant air flow produces more NOx per kg of CH4 consumed, and N2 is more effective than CO 2 in increasing the NOx emission index. The increase in emission index appears to be due to an enhancement of the prompt NOx pathway as the diluents are added and the mixture moves towards stoichiometric. In addition, the presence of CO2 as a diluent catalyzes the loss of flame radicals, leading to less NOx formation than when an equivalent amount of N2 is used as a diluent.;For a selected set of fuels, detailed spacial reactor probing is carried out. At the nominal temperature and residence time, the experimental results show the following trends for flame structure as a function of fuel type: 1.) Pure H2 is far more reactive in comparison to CH4 and all other pure alkane fuels. This results in relatively flat NO x and temperature profiles; whereas, the alkane fuels drop in both temperature and NOx production in the jet, where more fresh reactor feed gases are present. 2.) For category 2 (the Process and Refinery blends), H 2 addition increases reactivity in the jet while decreasing overall NOx emissions. The increased reactivity is especially evident in the CO profiles where the fuels blended with C2H6 and H2 have CO peaks on jet centerline and CO emissions for pure CH 4 peaks slightly off centerline. 3.) For category 3 (the O2 blown gasified coal/petcoke), the temperature profiles for the gasification blend and pure H2 are nearly identical, which is likely due to the high reactivity of H2 dominating the relatively low reactivity of CO. Despite a small temperature difference, the addition of CO causes an increase in NOx production. 4.) For category 4 (the landfill gas), the temperature profiles are virtually indistinguishable. However, the addition of diluent decreases reactivity and spreads out the reaction zone with the CO concentration peaking at 2 mm off of centerline instead of 1 mm. Diluent addition increases NOx production in comparison to pure CH4 for reasons explained above. 5.) For category 5 (the LNG, shale, and associated gases), the temperature profiles are all very similar. The increased reactivity of C2H6 is evident from looking at the CO profiles. Increased C2H6 promotes CO production on jet centerline which is indicative of the hydrocarbon material breaking down earlier in the jet.;At temperatures and residence times other than the nominal conditions, the experimental results show the following trends: 1.) The NOx emissions from LPM combustion of pure CH4, H2, C 2H6, and C3H8 are shown to vary linearly with residence time and in an Arrhenius fashion with temperature. This occurs because (1) more reaction time leads to more NOx formation, and (2) NOx formation is a strong, non-linear function of temperature. 2.) The addition of both H2 and C2H6 to a LPM CH4 flame is effective at extending its lean blowout limit.;The results of both two and three dimensional CFD simulations are presented to illustrate the general flow, temperature, and species structure within the reactor. Since the two dimensional model is far more computationally efficient, it is employed to study various fuel mixtures with more sophisticated chemical mechanisms. The CFD results from the LPM combustion of H2, H2/CO, and CH4 with NOx formation are presented.;A three dimensional CFD simulation is run for LPM CH4 combustion that uses a global CH4 oxidation mechanism. While this model does not predict intermediate radicals and NOx, the CO contours and flow field can be used as guidelines to develop a chemical reactor network (CRN), which can incorporate detailed chemistry. In addition, this model runs quickly enough that it is a good way to initialize the temperature and flow field for simulations that do incorporate more complex chemistry.;The two dimensional model is used to illustrate the difference in combustion behavior between the various fuels tested. In particular, it illustrates the geometric locations of the super-equilibrium radical fields and shows where and through which pathways NOx is formed. The pathway breakdowns show good agreement with the CRN modeling results.;The main goal of the CFD modeling is to use the results of each model to develop Chemical Reactor Networks, CRNs, that are customized for a particular burner. The CRN can then be used to estimate the impacts due to fuel variation.
机译:这项研究的目的是确定使用燃料替代典型的管道天然气会如何影响氮氧化物(NO x)的排放和火焰稳定性(井喷)。该研究的重点是通常在最新的天然气燃料系统中使用的稀薄,预混燃烧器。理想的实验室贫油预混燃烧器,特别是喷射搅拌反应器,用于实验数据。一系列模型,包括那些具有详细的流体动力学特征的模型和侧重于详细化学特征的模型,被用来解释数据并理解各种燃料混合物之间排放差异的潜在化学动力学原因。最终目标是使用这些数据和解释工具来开发一种方法来预测实际燃烧器内变化燃料的排放和稳定性影响。;所有实验结果均来自高强度单喷射搅拌反应器(JSR)。研究了五种燃料类别:(1)纯H 2,(2)工艺和炼厂气,包括H2,CH4,C2H6和C3H8的组合,(3)吹氧气化的煤/石油焦,由H2,CO和CO2组成(4)由CH4,CO2和N2组成的垃圾填埋场和消化池气体,以及(5)由CH4,C2H6和C3 H8组成的液化天然气(LNG)/页岩/伴生气。在标称燃烧温度为1800 K,大气压力和3 ms反应堆停留时间的条件下进行NOx测量。通过比较在相同温度,压力和停留时间下的所有燃料,可以将结果集中在燃料化学性质造成的差异上。这是文献中为数不多的试图研究组成不同的燃料时消除这些影响的研究之一。此外,还针对选定的燃料研究了温度和停留时间变化的影响。在标称温度和停留时间下,实验和建模结果显示出NOx排放随燃料类型变化的以下趋势:1.)NOx排放随着CH4 / H2混合物燃烧时H2燃料分数的增加而降低。这似乎是由于当CH4被H2取代时,涉及N2与烃基反应的快速途径所产生的NO减少所致。 2.)对于第2类(过程和炼油厂混合物)和第5类(LNG,页岩和伴生气),NOx排放随着C2和C3碳氢化合物的添加而增加。这可能是由于当较高分子量的烃被分解时,由于CO产量增加而导致自由基的产量增加。 3.)对于第3类(吹氧气化的煤/石油焦),NOx排放随着CO燃料分数的增加而增加。究其原因,是因为单位热量释放的CO比H2产生更多的自由基。当CO替代H2时,由于N2O,NNH和Zeldovich途径的生产率提高,NOx排放量增加。 4.)对于第4类(垃圾填埋气),在恒定空气流量下添加稀释剂(例如CO2和N2)会产生每千克所消耗的CH4更多的NOx,并且N2在提高NOx排放指数方面比CO 2更有效。排放指数的增加似乎是由于在添加稀释剂且混合物朝化学计量方向移动时,NOx即时途径的增强。此外,CO2作为稀释剂的存在催化了火焰自由基的损失,与使用等量的N2作为稀释剂相比,导致NOx的形成更少。;对于所选的一组燃料,进行了详细的空间反应堆探测。在标称温度和停留时间下,实验结果表明,火焰结构随燃料类型变化的趋势如下:1.)与CH4和所有其他纯烷烃燃料相比,纯H2具有更高的反应活性。这导致NOx和温度曲线相对平坦。相反,在有更多新鲜反应器进料气的射流中,烷烃燃料的温度和NOx产量均下降。 2.)对于第2类(过程和炼油厂混合物),H 2的添加增加了射流的反应性,同时降低了总的NOx排放量。反应性的提高在CO曲线中尤为明显,其中与C2H6和H2混合的燃料在射流中心线处具有CO峰,而纯CH 4峰的CO排放则稍稍偏离中心线。 3.)对于第3类(吹入氧气的气化煤/焦炭),气化混合物和纯氢气的温度曲线几乎相同,这很可能是由于氢气的高反应性主导了CO的相对较低的反应性。温度差小时,添加CO会增加NOx的产生。 4.)对于第4类(垃圾填埋气),温度曲线几乎无法区分。然而,稀释剂的添加降低了反应性并扩展了反应区,CO浓度在距中心线2 mm而不是1 mm处达到峰值。由于上述原因,与纯CH4相比,稀释剂的添加增加了NOx的产生。 5.)对于第5类(LNG,页岩和伴生气),温度曲线都非常相似。通过观察CO曲线可以明显看出C 2 H 6的反应性增加。 C2H6的增加促进了射流中心线上的CO生成,这表明碳氢化合物在射流中较早分解。在标称条件以外的温度和停留时间下,实验结果显示出以下趋势:1.)LPM的NOx排放结果表明,纯CH4,H2,C 2H6和C3H8的燃烧随停留时间线性变化,并随温度呈阿伦尼乌斯(Arrhenius)方式变化。发生这种情况是因为(1)更多的反应时间导致更多的NOx形成,以及(2)NOx的形成是温度的强非线性函数。 2.)在LPM CH4火焰中同时添加H2和C2H6可以有效地延长其稀薄喷出极限。;二维和三维CFD模拟的结果均用于说明内部的一般流动,温度和物质结构反应堆。由于二维模型具有更高的计算效率,因此可用于研究具有更复杂化学机理的各种燃料混合物。提出了H2,H2 / CO和CH4的LPM燃烧并形成NOx的CFD结果。;对LPM CH4燃烧进行了三维CFD模拟,它使用了整体CH4氧化机理。尽管此模型无法预测中间自由基和NOx,但CO轮廓和流场可以用作开发化学反应器网络(CRN)的指南,该网络可以包含详细的化学反应。此外,该模型运行速度足够快,这是初始化包含更复杂化学反应的模拟的温度和流场的好方法。;二维模型用于说明测试的各种燃料之间燃烧行为的差异。特别是,它说明了超平衡自由基场的几何位置,并显示了在何处以及通过哪些途径形成NOx。路径分解显示出与CRN建模结果良好的一致性。CFD建模的主要目标是利用每个模型的结果来开发针对特定燃烧器定制的化学反应器网络CRN。然后,可以使用CRN来估计由于燃料变化而产生的影响。

著录项

  • 作者

    Fackler, Keith Boyd, Jr.;

  • 作者单位

    University of Washington.;

  • 授予单位 University of Washington.;
  • 学科 Alternative Energy.;Engineering Mechanical.;Energy.
  • 学位 Ph.D.
  • 年度 2011
  • 页码 207 p.
  • 总页数 207
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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