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Automatically simplified chemical kinetics and molecular transport and its applications in premixed and non-premixed laminar flame calculations 自动简化化学动力学和分子传递及其在预混和非预混层流火焰计算中的应用
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80440-2
T. Blasenbrey, D. Schmidt, U. Maas

Among many other methods for simplifying chemical kinetics for laminar and turbulent flame calculations, the method of intrinsic low-dimensional manifolds (ILDM) has shown to be an efficient tool for the development of reduced kinetic schemes. Based on a numerical analysis, it identifies and decouples the fast relaxing timescales of the chemical system. The results, for example, the thermokinetic state of the system or the reaction rates, are then stored in terms of a small number of parameters (mixture fraction, reaction progress variables) for subsequent use in reacting flow calculations. Furthermore, together with the reduced mechanism, information about the coupling of the chemical kinetics with the physical processes (molecular transport, turbulent mixing) is obtained.

In this paper, we present a method that allows an efficient implementation of the ILDM method in flame calculations and overcomes several problems that had been discussed in previous work. It is based on three ingredients: A robust numerical method to calculate the ILDM, a storage scheme that allows an easy implementation in CFD codes, and a model for the coupling of the chemical kinetics with transport processes. In this way, not only the chemistry can be calculated beforehand but also a reduced set of diffusion coefficients. The method is verified by simulations of laminar syngas-air flames with an emphasis on the non-premixed case.

在许多其他简化层流和湍流火焰化学动力学计算的方法中,本然低维流形(ILDM)方法已被证明是开发简化动力学方案的有效工具。在数值分析的基础上,识别并解耦了化学系统的快速弛豫时间尺度。结果,例如,系统的热力学状态或反应速率,然后以少量参数(混合物分数,反应过程变量)的形式存储,以便随后用于反应流计算。此外,结合简化的机理,获得了化学动力学与物理过程(分子输运、湍流混合)耦合的信息。在本文中,我们提出了一种方法,允许在火焰计算中有效地实现ILDM方法,并克服了以前工作中讨论的几个问题。它基于三个要素:一种强大的计算ILDM的数值方法,一种易于在CFD代码中实现的存储方案,以及一种化学动力学与传输过程耦合的模型。这样,不仅可以事先计算出化学性质,而且可以简化扩散系数集。通过层流合成气-空气火焰的数值模拟验证了该方法的有效性,并以非预混情况为重点。
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引用次数: 23
Kinetic investigations of the reactions of toluene and of p-xylene with molecular oxygen between 1050 and 1400 K 甲苯和对二甲苯在1050 ~ 1400k间与分子氧反应的动力学研究
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80407-4
R.A. Eng , C. Fittschen , A. Gebert , P. Hibomvschi , H. Hippler , A.-N. Unterreiner
<div><p>The reaction of toluene with molecular oxygen was studied behind reflected shock waves. Mixtures of 0.5–1 mol% toluene and 5–10% oxygen in argon were investigated in the temperature range between 1050 and 1400 K at total pressures between 2 and 4 bar. We followed the rate of formation of the benzyl radicals by time-resolved UV absorption at 257 nm. The measured concentration-time profiles of the benzyl radicals were numerically reproduced using a simple reaction mechanism. For the initial reaction<span><span><span><math><mrow><msub><mo>C</mo><mn>6</mn></msub><msub><mo>H</mo><mn>5</mn></msub><mo>C</mo><msub><mo>H</mo><mn>3</mn></msub><mo>+</mo><msub><mo>O</mo><mn>2</mn></msub><mo>→</mo><msub><mo>C</mo><mn>6</mn></msub><msub><mo>H</mo><mn>5</mn></msub><mo>C</mo><msub><mo>H</mo><mn>2</mn></msub><mo>+</mo><mo>H</mo><msub><mo>O</mo><mn>2</mn></msub><mo>(</mo><mo>R</mo><mn>1</mn><mo>)</mo></mrow></math></span></span></span> a rate coefficient<em>k</em><sub>1</sub> of <span><span><span><math><mrow><msub><mi>k</mi><mn>1</mn></msub><mo>=</mo><mn>3</mn><mo>×</mo><msup><mrow><mn>10</mn></mrow><mrow><mn>14</mn></mrow></msup><mo>exp</mo><mrow><mo>[</mo><mrow><mfrac><mrow><mo>−</mo><mn>180</mn><mo>kj</mo><mo>/</mo><mo>mol</mo></mrow><mrow><mi>R</mi><mi>T</mi></mrow></mfrac></mrow><mo>]</mo></mrow><mfrac><mrow><msup><mo>cm</mo><mn>3</mn></msup></mrow><mrow><mo>mol</mo><mo>s</mo></mrow></mfrac><mo>(</mo><mn>1050</mn><mo>K</mo><mo><</mo><mi>T</mi><mo><</mo><mn>1400</mn><mo>K</mo><mo>)</mo></mrow></math></span></span></span>was determined with an accuracy of 30%. The rate constant <em>k</em><sub>2</sub>of the subsequent reaction <span><span><span><math><mrow><msub><mo>C</mo><mn>6</mn></msub><msub><mo>H</mo><mn>5</mn></msub><mo>C</mo><msub><mo>H</mo><mn>3</mn></msub><mo>+</mo><mo>H</mo><msub><mo>O</mo><mn>2</mn></msub><mo>→</mo><msub><mo>C</mo><mn>6</mn></msub><msub><mo>H</mo><mn>5</mn></msub><mo>C</mo><msub><mo>H</mo><mn>2</mn></msub><mo>+</mo><msub><mo>H</mo><mn>2</mn></msub><msub><mo>O</mo><mn>2</mn></msub><mo>(</mo><mo>R</mo><mn>2</mn><mo>)</mo></mrow></math></span></span></span>was determined to be.<span><span><span><math><msub><mi>k</mi><mn>2</mn></msub><mo>=</mo><mn>3</mn><mo>×</mo><msup><mn>10</mn><mrow><mn>14</mn></mrow></msup><mo>exp</mo><mo>⁡</mo><mrow><mo>[</mo><mrow><mfrac><mrow><mo>−</mo><mn>92</mn><mo>kj</mo><mo>/</mo><mo>mol</mo></mrow><mrow><mi>R</mi><mi>T</mi></mrow></mfrac></mrow><mo>]</mo></mrow><mfrac><mrow><msup><mo>cm</mo><mn>3</mn></msup></mrow><mrow><mo>mol</mo><mo>s</mo></mrow></mfrac><mo>(</mo><mn>1150</mn><mo>K</mo><mo><</mo><mi>T</mi><mo><</mo><mn>1250</mn><mo>K</mo><mo>)</mo></math></span></span></span>The reaction of <em>p</em>-xylene with molecular oxygen was investigated using the same technique. Mixtures of 0.25–0.5 mol % <em>p</em>-xylene and 2.5–10 mol% oxygen in argon were shock-heated to temperatures between 1130 and 1380 K. We followed the formation of <em>p</em>-methyl-benzyl radicals by time-resolved UV a
研究了甲苯与分子氧在反射激波下的反应。在1050 ~ 1400k的温度范围内,在2 ~ 4bar的总压力下,研究了0.5 ~ 1mol %甲苯和5 ~ 10%氧在氩气中的混合物。我们用时间分辨紫外吸收法在257 nm处跟踪了苯自由基的形成速度。用简单的反应机理数值再现了测量到的苯自由基的浓度-时间分布。对于初始反应c6h5ch3 +O2→C6H5CH2+HO2(R1),速率系数k1为k1=3×1014exp[−180kj/molRT] cm3mools (1050K<T<1400K),准确度为30%。测定了后续反应C6H5CH3+HO2→C6H5CH2+H2O2(R2)的反应速率常数k2为,k2=3×1014exp (- 92kj/molRT) cm3mol (1150K<T<1250K)。在氩气中,0.25-0.5 mol%的对二甲苯和2.5-10 mol%的氧的混合物被冲击加热到1130 - 1380 K之间。我们用时间分辨紫外吸收法在265 nm处观察对甲基苄基自由基的形成。然而,我们发现对甲基苄基自由基的产率很低,我们将其归因于这些自由基与分子氧的快速反应。根据这一低产率,我们估计了反应的速率常数k3/k4的上限为:p−CH3C6H4CH3+O2→p−CH3C6H4CH2+HO2(R3)p−CH3C6H4CH2+O2→p−CH2C6H4CH2+HO2(R4)。
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For the initial reaction&lt;span&gt;&lt;span&gt;&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;mn&gt;6&lt;/mn&gt;&lt;/msub&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;5&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;O&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;→&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;mn&gt;6&lt;/mn&gt;&lt;/msub&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;5&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;O&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mo&gt;R&lt;/mo&gt;&lt;mn&gt;1&lt;/mn&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt; a rate coefficient&lt;em&gt;k&lt;/em&gt;&lt;sub&gt;1&lt;/sub&gt; of &lt;span&gt;&lt;span&gt;&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;msub&gt;&lt;mi&gt;k&lt;/mi&gt;&lt;mn&gt;1&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;=&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;mo&gt;×&lt;/mo&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mn&gt;10&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;14&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;mo&gt;exp&lt;/mo&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mfrac&gt;&lt;mrow&gt;&lt;mo&gt;−&lt;/mo&gt;&lt;mn&gt;180&lt;/mn&gt;&lt;mo&gt;kj&lt;/mo&gt;&lt;mo&gt;/&lt;/mo&gt;&lt;mo&gt;mol&lt;/mo&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;R&lt;/mi&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;/mrow&gt;&lt;/mfrac&gt;&lt;/mrow&gt;&lt;mo&gt;]&lt;/mo&gt;&lt;/mrow&gt;&lt;mfrac&gt;&lt;mrow&gt;&lt;msup&gt;&lt;mo&gt;cm&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msup&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;mol&lt;/mo&gt;&lt;mo&gt;s&lt;/mo&gt;&lt;/mrow&gt;&lt;/mfrac&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mn&gt;1050&lt;/mn&gt;&lt;mo&gt;K&lt;/mo&gt;&lt;mo&gt;&lt;&lt;/mo&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;mo&gt;&lt;&lt;/mo&gt;&lt;mn&gt;1400&lt;/mn&gt;&lt;mo&gt;K&lt;/mo&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;was determined with an accuracy of 30%. The rate constant &lt;em&gt;k&lt;/em&gt;&lt;sub&gt;2&lt;/sub&gt;of the subsequent reaction &lt;span&gt;&lt;span&gt;&lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;mn&gt;6&lt;/mn&gt;&lt;/msub&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;5&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;O&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;→&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;mn&gt;6&lt;/mn&gt;&lt;/msub&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;5&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;C&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;msub&gt;&lt;mo&gt;H&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;msub&gt;&lt;mo&gt;O&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mo&gt;R&lt;/mo&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;was determined to be.&lt;span&gt;&lt;span&gt;&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mi&gt;k&lt;/mi&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;=&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;mo&gt;×&lt;/mo&gt;&lt;msup&gt;&lt;mn&gt;10&lt;/mn&gt;&lt;mrow&gt;&lt;mn&gt;14&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;mo&gt;exp&lt;/mo&gt;&lt;mo&gt;⁡&lt;/mo&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mfrac&gt;&lt;mrow&gt;&lt;mo&gt;−&lt;/mo&gt;&lt;mn&gt;92&lt;/mn&gt;&lt;mo&gt;kj&lt;/mo&gt;&lt;mo&gt;/&lt;/mo&gt;&lt;mo&gt;mol&lt;/mo&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;R&lt;/mi&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;/mrow&gt;&lt;/mfrac&gt;&lt;/mrow&gt;&lt;mo&gt;]&lt;/mo&gt;&lt;/mrow&gt;&lt;mfrac&gt;&lt;mrow&gt;&lt;msup&gt;&lt;mo&gt;cm&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msup&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;mol&lt;/mo&gt;&lt;mo&gt;s&lt;/mo&gt;&lt;/mrow&gt;&lt;/mfrac&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mn&gt;1150&lt;/mn&gt;&lt;mo&gt;K&lt;/mo&gt;&lt;mo&gt;&lt;&lt;/mo&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;mo&gt;&lt;&lt;/mo&gt;&lt;mn&gt;1250&lt;/mn&gt;&lt;mo&gt;K&lt;/mo&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/math&gt;&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;The reaction of &lt;em&gt;p&lt;/em&gt;-xylene with molecular oxygen was investigated using the same technique. Mixtures of 0.25–0.5 mol % &lt;em&gt;p&lt;/em&gt;-xylene and 2.5–10 mol% oxygen in argon were shock-heated to temperatures between 1130 and 1380 K. We followed the formation of &lt;em&gt;p&lt;/em&gt;-methyl-benzyl radicals by time-resolved UV a","PeriodicalId":101203,"journal":{"name":"Symposium (International) on Combustion","volume":"27 1","pages":"Pages 211-218"},"PeriodicalIF":0.0,"publicationDate":"1998-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0082-0784(98)80407-4","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"98416850","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 21
Ignition and combustion of levitated magnesium particles in carbon dioxide 悬浮镁颗粒在二氧化碳中的点火和燃烧
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80093-3
Benjamin Legrand , Evgeny Shafirovich , Michaël Marion , Christian Chauveau , Iskender Gökalp

This paper considers ignition and combustion of small (50–100 μm) single particles of magnesium and 50-50 magnesium-aluminum alloy in the atmosphere of carbon dioxide or its mixtures with argon. This investigation is of interest for both basic combustion science and applications to rocket engines, including those using Martian CO2 as an oxidizer, An experimental setup with an electrodynamic levitator inside a high-pressure chamber was employed. A CO2 laser was used for heating to ignition of the particles. The laser was switched off after ignition. The experiments were conducted with the oxidizer at room temperature over the range of pressures from 0.1 to 2 MPa. Effects of the CO2 concentration and pressure on the critical ignition conditions, ignition delay times, and burning times have been determined for Mg particles. The results clearly indicate that ignition of Mg in CO2 is controlled by chemical kinetics and that its combustion is controlled by diffusion in gas phase. Quantitative disagreement of the observed critical ignition pressures with previous experimental data on ignition of Mg disks in CO2 is explained by the differences in heat-loss mechanisms. The measured values of the burning rate correlate well with previous experimental results on combustion of 2-mm particles and with a quasi-steady model of Mg particle burning in CO2. In contrast to pure Mg and Al, particles of Mg−Al alloy did not ignite in CO2 under the present experimental conditions.

本文研究了50-100 μm镁和50-50镁铝合金在二氧化碳或其与氩气混合的气氛中的点火和燃烧。这项研究对基础燃烧科学和火箭发动机的应用都很有兴趣,包括那些使用火星二氧化碳作为氧化剂的火箭发动机。在高压室内采用了一个电动悬浮器的实验装置。用CO2激光器加热点燃颗粒。激光在点火后被关闭。实验是在室温下,在0.1 ~ 2mpa的压力范围内用氧化剂进行的。测定了CO2浓度和压力对Mg颗粒临界点火条件、点火延迟时间和燃烧时间的影响。结果表明,Mg在CO2中的着火受化学动力学控制,燃烧受气相扩散控制。在CO2中观察到的临界点火压力与先前的Mg盘点火实验数据的定量差异可以用热损失机制的差异来解释。燃烧速率的测量值与以往2-mm颗粒燃烧的实验结果以及Mg颗粒在CO2中燃烧的准稳态模型吻合良好。与纯Mg和纯Al相比,在本实验条件下,Mg−Al合金颗粒在CO2中不着火。
{"title":"Ignition and combustion of levitated magnesium particles in carbon dioxide","authors":"Benjamin Legrand ,&nbsp;Evgeny Shafirovich ,&nbsp;Michaël Marion ,&nbsp;Christian Chauveau ,&nbsp;Iskender Gökalp","doi":"10.1016/S0082-0784(98)80093-3","DOIUrl":"10.1016/S0082-0784(98)80093-3","url":null,"abstract":"<div><p>This paper considers ignition and combustion of small (50–100 μm) single particles of magnesium and 50-50 magnesium-aluminum alloy in the atmosphere of carbon dioxide or its mixtures with argon. This investigation is of interest for both basic combustion science and applications to rocket engines, including those using Martian CO<sub>2</sub> as an oxidizer, An experimental setup with an electrodynamic levitator inside a high-pressure chamber was employed. A CO<sub>2</sub> laser was used for heating to ignition of the particles. The laser was switched off after ignition. The experiments were conducted with the oxidizer at room temperature over the range of pressures from 0.1 to 2 MPa. Effects of the CO<sub>2</sub> concentration and pressure on the critical ignition conditions, ignition delay times, and burning times have been determined for Mg particles. The results clearly indicate that ignition of Mg in CO<sub>2</sub> is controlled by chemical kinetics and that its combustion is controlled by diffusion in gas phase. Quantitative disagreement of the observed critical ignition pressures with previous experimental data on ignition of Mg disks in CO<sub>2</sub> is explained by the differences in heat-loss mechanisms. The measured values of the burning rate correlate well with previous experimental results on combustion of 2-mm particles and with a quasi-steady model of Mg particle burning in CO<sub>2</sub>. In contrast to pure Mg and Al, particles of Mg−Al alloy did not ignite in CO<sub>2</sub> under the present experimental conditions.</p></div>","PeriodicalId":101203,"journal":{"name":"Symposium (International) on Combustion","volume":"27 2","pages":"Pages 2413-2419"},"PeriodicalIF":0.0,"publicationDate":"1998-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0082-0784(98)80093-3","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"104606756","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 41
Simultaneous rayleigh, raman, and LIF measurements in turbulent premixed methane-air flames 同时瑞利,拉曼和LIF测量湍流预混甲烷-空气火焰
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80470-0
J.H. Frank , R.S. Barlow

Instantaneous measurements of temperature, major species, OH, CO, and NO are performed in turbulent premixed flames using simultaneous Rayleigh scattering, Raman scattering, and laser-induced fluorescence (LIF). Temperature is determined from Rayleigh scattering, and concentrations of CH4, O2, N2, H2O, CO2, and H2 are obtained from Raman scattering. Linear LIF is used to measure OH and NO, while two-photon LIF is used to determine CO concentrations. The two-photon CO-LIF system provides significant improvements over CO-Raman measurements. This combination of diagnostic techniques is used to investigate the detailed compositional structure of turbulent lean premixed methane-air flames. Three turbulent flames having different equivalence ratios are considered. The ratio of rms velocity to laminar flame speed ranges from approximately 6 to 17. The correlation of major species, OH, and CO concentrations with temperature are similar to those predicted by one-dimensional laminar flame calculations. However, NO concentrations in the leaner flames are higher than the predicted values.

使用瑞利散射、拉曼散射和激光诱导荧光(LIF)在湍流预混火焰中进行温度、主要物质、OH、CO和NO的瞬时测量。温度由瑞利散射测定,CH4、O2、N2、H2O、CO2和H2的浓度由拉曼散射测定。线性LIF用于测量OH和NO,而双光子LIF用于测定CO浓度。双光子CO-LIF系统提供了CO-Raman测量的显著改进。这种诊断技术的组合用于研究湍流贫预混甲烷-空气火焰的详细组成结构。考虑了三种不同等效比的湍流火焰。均方根速度与层流火焰速度之比约为6 ~ 17。主要物质、OH和CO浓度与温度的相关性与一维层流火焰计算预测的结果相似。然而,较细火焰中的NO浓度高于预测值。
{"title":"Simultaneous rayleigh, raman, and LIF measurements in turbulent premixed methane-air flames","authors":"J.H. Frank ,&nbsp;R.S. Barlow","doi":"10.1016/S0082-0784(98)80470-0","DOIUrl":"10.1016/S0082-0784(98)80470-0","url":null,"abstract":"<div><p>Instantaneous measurements of temperature, major species, OH, CO, and NO are performed in turbulent premixed flames using simultaneous Rayleigh scattering, Raman scattering, and laser-induced fluorescence (LIF). Temperature is determined from Rayleigh scattering, and concentrations of CH<sub>4</sub>, O<sub>2</sub>, N<sub>2</sub>, H<sub>2</sub>O, CO<sub>2</sub>, and H<sub>2</sub> are obtained from Raman scattering. Linear LIF is used to measure OH and NO, while two-photon LIF is used to determine CO concentrations. The two-photon CO-LIF system provides significant improvements over CO-Raman measurements. This combination of diagnostic techniques is used to investigate the detailed compositional structure of turbulent lean premixed methane-air flames. Three turbulent flames having different equivalence ratios are considered. The ratio of rms velocity to laminar flame speed ranges from approximately 6 to 17. The correlation of major species, OH, and CO concentrations with temperature are similar to those predicted by one-dimensional laminar flame calculations. However, NO concentrations in the leaner flames are higher than the predicted values.</p></div>","PeriodicalId":101203,"journal":{"name":"Symposium (International) on Combustion","volume":"27 1","pages":"Pages 759-766"},"PeriodicalIF":0.0,"publicationDate":"1998-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0082-0784(98)80470-0","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"96604349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 31
Modeling the temperature and pressure dependence of the reaction HO+CO ixHOCO ixH+CO2 模拟反应HO+CO ixHOCO ixH+CO2的温度和压力依赖性
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80402-5
Jürgen Troe

The bimolecular reaction HO+CO ixH+CO2 involves the intermediate formation of HOCO. As a consequence, the rate coefficient shows a complicated temperature and pressure dependence. An optimized E- and J-resolved rigid activated complex RRKM theory, with simplified E- and J-resolved pressure-dependent collision efficiencies, fits the available experimental data and allows for extrapolations to unexplored conditions. Experiments between 80 and 2370 K, between 10−3 and 103 bar in the bath gas He, and below 1 bar in Ar, N2, CF4 SF6, and H2O at 298 K, serve as the database. A limiting low-pressure rate constant for HO removal of ko=[1.0×1013 exp(−8050 K/T)+9.0×1011 exp(−2300 K/T)+1.01×1011 exp (−30 K/T)] cm3 mol−1 s−1 and a limiting high-pressure rate constant of k=[1.23×1015 exp (−7520 K/T)+1.1×1013 exp(−1850 K/T)+8.0×1011 exp(−120 K/T] cm3 mol−1 s−1 will reproduce the results. The pressure dependence of the rate coefficient as a function of the temperature is represented for the bath gases He, Ar, N2, CF4, SF6, and H2O. Rate coefficients for HOCO formation and HOCO dissociation are also given.

双分子反应HO+CO ixH+CO2参与了HOCO的中间生成。因此,速率系数表现出复杂的温度和压力依赖关系。优化的E-和j -分辨刚性活化复合物RRKM理论,简化了E-和j -分辨压力相关碰撞效率,符合现有实验数据,并允许对未探索条件进行外推。在80 - 2370 K, 10 - 3 - 103 bar的浴气He,以及低于1 bar的Ar, N2, CF4 SF6和H2O中298 K的实验作为数据库。ko去除HO的极限低压速率常数=[1.0×1013 exp(−8050 K/T)+9.0×1011 exp(−2300 K/T)+1.01×1011 exp(−30 K/T)] cm3 mol−1 s−1,K∞的极限高压速率常数=[1.23×1015 exp(−7520 K/T)+1.1×1013 exp(−1850 K/T)+8.0×1011 exp(−120 K/T)] cm3 mol−1 s−1,将重现结果。对于浴液气体He, Ar, N2, CF4, SF6和H2O,速率系数作为温度函数的压力依赖性表示。给出了HOCO形成和HOCO解离的速率系数。
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引用次数: 30
Two-dimensional failure waves and ignition fronts in premixed combustion 预混合燃烧的二维失效波与点火锋面
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80444-X
T.G. Vedarajan , J. Buckmaster , P. Ronney

This paper is a continuation of our work on edge-flames in premixed combustion. An edge-flame is a two-dimensional structure constructed from a one-dimensional configuration that has two stable solutions (bistable equilibrium). Edge-flames can display wavelike behavior, advancing as ignition fronts or retreating as failure waves. Here we consider two one-dimensional configurations: twin deflagrations in a straining flow generated by the counterflow of fresh streams of mixture; and a single deflagration subject to radiation losses. The edge-flames constructed from the first configuration have positive or negative speeds, according to the value of the strain rate. But our numerical solutions strongly suggest that only positive speeds (corresponding to ignition fronts) can exist for the second configuration. We show that this phenomenon can also occur in diffusion flames when the Lewis numbers are small. And we discuss the asymptotics of the one-dimensional twin deflagration configuration, an overlooked problem from the 70s.

本文是对预混燃烧中边缘火焰研究的延续。边缘火焰是由一维构型构成的二维结构,具有两个稳定解(双稳态平衡)。边缘火焰可以表现出波浪式的行为,作为点火锋面前进或作为失效波后退。这里我们考虑两种一维结构:由新鲜混合流逆流产生的应变流中的双爆燃;单次爆燃会造成辐射损失。根据应变速率的值,由第一种配置构造的边缘火焰具有正或负速度。但我们的数值解强烈表明,只有正速度(对应于点火前沿)可以存在于第二种配置。结果表明,当刘易斯数较小时,扩散火焰也会出现这种现象。讨论了一维双爆燃构型的渐近性,这是70年代以来一个被忽视的问题。
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引用次数: 24
Pyrolysis product absorption by burning benzene droplets 热解产物通过燃烧吸收苯滴
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80033-7
Nathan D. Marsh, Delin Zhu, Mary J. Wornat

By burning droplets of benzene in a single-droplet combustor and performing phase-discriminating sampling of the liquid and gas phases of the droplet system, we have found that gas-phase pyrolysis products arise in the liquid phase of the droplet. The experiments are conducted at 1000 K and 21 mol % O2 in the postcombustion gas from an oxygen-rich premixed methane flame. Disruptive burning, which has not previously been reported for a pure hydrocarbon in normal gravity conditions, is observed at the end of the droplet residence time (∼92 ms). Samples of the liquid phase have been taken at various times throughout the combustion lifetime and analyzed by high-pressure liquid chromatography. Compositional analysis using ultraviolet-visible absorbance spectra of the separated components of the samples reveals a wide variety of pure polycyclic aromatic hydrocarbons (PAH), substituted PAH, and cyclopenta-fused PAH. In addition, recent synthesis of new reference standards has enabled identification of cyclopenta-fused PAH—cyclopent[hi]acephenanthrylene, cyclopenta[cd]fluoranthene, and dicyclopenta[cd, jk]pyrene—which have never before been identified as benzene products. Because the droplet remains relatively cold (∼350 K) with respect to the gas phase in the oxygen-deficient zone between the droplet and the flame (∼2000 K), we conclude that these compounds are gas-phase pyrolysis products that are obsorbed into the droplet, rather than products of reactions within the droplet. These heavier species may play a role in observed terminal disruptive burning events by acting as additional droplet components that promote multicomponent effects. Analysis of species concentrations over time reveals the dominance of both ring rupture pyrolysis products such as phenylacetylene, triacetylene, and acenaphthylene, and biaryl pyrolysis products such as biphenyl. These four products in particular represent 70% of the identified mass of absorbed pyrolysis products, which accounts for up to 5% of the droplet mass at the end of its lifetime.

通过在单液滴燃烧器中燃烧苯液滴,并对液滴体系的液相和气相进行分相取样,我们发现液滴的液相中产生气相热解产物。实验是在1000 K和21 mol % O2的富氧甲烷火焰燃烧后气体中进行的。在液滴停留时间(~ 92 ms)结束时,观察到先前未在正常重力条件下对纯碳氢化合物进行破坏性燃烧的报道。在整个燃烧寿命的不同时间取了液相样品,并用高压液相色谱法进行了分析。利用紫外-可见吸收光谱对样品分离组分进行成分分析,发现了多种纯多环芳烃(PAH)、取代多环芳烃和环五芳烃。此外,最近合成了新的参考标准,使得以前从未被鉴定为苯产品的环五[cd]芴和环五[cd, jk]芘得以鉴定。由于液滴与火焰之间缺氧区(~ 2000 K)的气相温度相对较低(~ 350 K),因此我们得出结论,这些化合物是被液滴吸收的气相热解产物,而不是液滴内部反应的产物。这些较重的物种可能在观察到的终端破坏性燃烧事件中发挥作用,作为促进多组分效应的附加液滴组分。对物种浓度随时间变化的分析显示,环断裂热解产物(如苯乙炔、三乙炔和苊)和联芳基热解产物(如联苯)都占主导地位。这四种产物占热解吸收产物鉴定质量的70%,在其寿命结束时占液滴质量的5%。
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引用次数: 11
Effects of stretch on the local structure of preely propagating premixed low-turbulent flames with various lewis numbers 拉伸对不同刘易斯数预混合低湍流火焰局部结构的影响
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80480-3
Bruno Renou, Abdelkrim Boukhalfa, Daniel Puechberty, Michel Trinité

An experimental investigation of the flame response to strain rate in the case of unsteady premixed low-turbulent flames is presented. In order to point out the fundamental aspects of the mutual interaction between combustion and turbulence, measurements of local flame properties (curvature, displacement speed) and tangential strain rate were performed under varying conditions of Lewis number and turbulence.

Three different mixtures (methane/air, propane/air, and hydrogen/air) were successively spark ignited in a vertical wind tunnel. The expanding flame freely propagated in a grid-generated decaying turbulent flow. An advanced field imaging technique coupling high-speed laser tomography and cross-correlation particle image velocimetry (PIV) was used to measure the temporal evolution of local flame stretch exerted by the turbulent cold flow.

Local flame curvature and local displacement speed were calculated from flame-front contours. Curvature probability density functions (PDFs) were negatively skewed, especially for nonunity Lewis numbers, and displacement speed distributions underlined the influence of local stretch and thermodiffusive effects on flame-speed variations. Tangential strain rate was determined by using the velocity field in the neighborhood of the flame front and appears to be independent of the Lewis numbers. A strong correlation between local flame curvature and tangential strain rate was demonstrated, underlining the cold flow effects on the local flame structure. The influences of turbulence and Lewis number were evaluated and compared with numerical simulations. Then, local flame stretch distributions were determined versus time, indicating that a significant proportion of the flame was under compression.

本文研究了非定常预混低湍流火焰对应变速率的响应。为了指出燃烧和湍流相互作用的基本方面,在不同的刘易斯数和湍流条件下进行了局部火焰特性(曲率、位移速度)和切向应变率的测量。三种不同的混合物(甲烷/空气、丙烷/空气和氢气/空气)在垂直风洞中先后被火花点燃。膨胀的火焰在网格生成的衰减湍流中自由传播。采用一种先进的场成像技术,结合高速激光层析成像和相互关联粒子图像测速(PIV)技术,测量了湍流冷流作用下局部火焰拉伸的时间演变。根据火焰前轮廓计算火焰的局部曲率和局部位移速度。曲率概率密度函数(pdf)呈负偏态,特别是对于非统一Lewis数,位移速度分布强调了局部拉伸和热扩散效应对火焰速度变化的影响。切向应变率由火焰前缘附近的速度场确定,与路易斯数无关。局部火焰曲率与切向应变率之间存在很强的相关性,表明冷流动对局部火焰结构的影响。对湍流和刘易斯数的影响进行了评估,并与数值模拟进行了比较。然后,确定了局部火焰拉伸随时间的分布,表明有很大一部分火焰处于压缩状态。
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引用次数: 92
On pulsating and cellular forms of hydrodynamic instability in liquid-propellant combustion 液体推进剂燃烧中流体动力不稳定性的脉动和细胞形式
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80089-1
Stephen B. Margolis

An extended Landau-Levich model of liquid-propellant combustion, one that allows for a local dependence of the burning rate on the (gas) pressure at the liquid-gas interface, exhibits not only the classival hydrodynamic cellular instability attributed to Landau but also a pulsating hydrodynamic instability associated with sufficiently negative pressure sensitivities. Exploiting the realistic limit of small values of the gas-to-liquid density ratio p, analytical formulas for both neutral sability boundaries may be obtained by expanding all quatities in appropriate powers of p in each of three distinguished wave-number regimes. In particular, composite analytical expressions are derived for the neutral stability boundaries Ap(k), where Ap is the pressure sensitivity of the burning rate and k is the wave number of the disturbance. For the cellular boundary, the results demonstrate explicitly the stabilizing effect of gravity on long-wave disturbances, the stabilizing effect of viscosity (both liquid and gas) and surface tension on short-wave perturbations, and the instability associated with intermediate wave numbers for negative values of Ap, which is characteristic of many hydroxylammoninum nitrate-based liquid propellants over certain pressure ranges. In contrast, the pulsating hydrodynamic stability boundary is insensitive to gravitational and surface-tension effects but is more sensitive to the effects of liquid viscosity because, for typical nonzero values of the latter, the pulsating boundary decreases to larger negative values of Ap as k increases through O(1) values. Thus, liquid-propellant combustion is predicted to be stable (that is, stealy and planar) only for a range of negative pressure sensitivities that lie below the cellular boundary that exists for sufficiently small negative values of Ap and above the pulsating boundary that exists for larger negative values of this parameter.

一种扩展的液体推进剂燃烧朗道-列维奇模型,允许燃烧速率局部依赖于液气界面处的(气体)压力,不仅表现出归因于朗道的分类流体动力细胞不稳定性,而且还表现出与足够负压敏感性相关的脉动流体动力不稳定性。利用气液密度比p的小值的现实极限,可以通过在三种不同的波数状态中展开p的适当幂的所有质量来获得两个中性稳定边界的解析公式。特别推导了中性稳定边界Ap(k)的复合解析表达式,其中Ap为燃速的压力灵敏度,k为扰动的波数。对于细胞边界,研究结果明确地证明了重力对长波扰动的稳定作用,粘度(液体和气体)和表面张力对短波扰动的稳定作用,以及与Ap负值的中间波数相关的不稳定性,这是许多硝酸羟胺基液体推进剂在一定压力范围内的特征。相比之下,脉动流体动力稳定性边界对重力和表面张力效应不敏感,但对液体粘度的影响更敏感,因为对于后者的典型非零值,随着k的增加,脉动边界通过O(1)值减小到较大的负值。因此,预测液体推进剂燃烧是稳定的(即,隐蔽的和平面的),只有在负压灵敏度范围内,该范围位于细胞边界以下,存在足够小的负Ap值,并高于脉动边界,存在较大的负Ap值。
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引用次数: 9
Measurement of the resolved flame structure of turbulent premixed flames with constant reynolds number and varied stoichiometry 恒定雷诺数和不同化学计量的湍流预混火焰分解火焰结构的测量
Pub Date : 1998-01-01 Epub Date: 2007-09-25 DOI: 10.1016/S0082-0784(98)80473-6
Armin Soika, Friedrich Dinkelacker, Alfred Leipertz

Wire-stabilized premixed methane-air flames have been studied in a grid-generated homogeneous turbulent flow field in order to identify different burning regimes. The planar Rayleigh scattering technique was used with two parallel laser light sheets, which allows the detection of three-dimensional temperature gradients. For a detailed investigation of the flame structure and topology, the modification of the local temperature gradients at different progress variables c due to the turbulent motion was studied by varying the flame stoichiometry and thereby the Karlovitz number Ka while keeping the turbulent Reynolds number Ret constant at 87 or 134. Because of a nearly Gaussian shaped statistical distribution of the thermal gradients, the 50% median and the width of the distribution are suitable measures used to characterize the flame response. Compared with laminar unstrained calculations, especially very lean flames (<0.55) marked with the highest Karlovitz number (Ka=4.6) revealed a reduction of the flame thickness of about 30%. This is in contrast to the expected burning regime but fits well with laminar strained calculations. Subsequently, detailed investigations were made to examine the influence of curvature on local thermal gradients. It was found that negatively curved cusps (concave toward the reactants) show a steepening of the flame-temperature profile, while positively curved flame elements can be identified by a retardation of the overall reaction process. In terms of a statistical examination, the widths of the thermal gradient distribution conditioned at different reaction progress variables c were regarded, finding a decrease of the spread with increasing Ka independent of Ret and c. Based on different curvature radii and perturbation frequencies of the detected flames, we assume that in our experiments the flame response depends more on flame curvature than on effects caused by modification of Ka.

为了识别不同的燃烧形式,在网格均匀湍流流场中研究了线稳定预混甲烷-空气火焰。利用平面瑞利散射技术对两个平行激光片进行了三维温度梯度检测。为了详细研究火焰的结构和拓扑结构,在保持湍流雷诺数Ret恒定在87或134的情况下,通过改变火焰的化学计量,从而改变Karlovitz数Ka,研究了湍流运动对不同进程变量c下局部温度梯度的影响。由于热梯度的统计分布近似高斯分布,50%的中位数和分布的宽度是表征火焰响应的合适度量。与层流无应变计算相比,特别是Karlovitz数(Ka=4.6)最高的极细火焰(<0.55)显示火焰厚度减少了约30%。这与预期的燃烧状态相反,但很适合层流应变计算。随后,详细研究了曲率对局部热梯度的影响。结果发现,负弯曲的尖峰(向反应物凹)表明火焰温度曲线变陡,而正弯曲的火焰元素可以通过整个反应过程的延迟来识别。在统计检验方面,考虑了不同反应过程变量c条件下的热梯度分布宽度,发现随着Ka的增加,传播减少与Ret和c无关。基于检测到的火焰的不同曲率半径和扰动频率,我们假设在我们的实验中火焰响应更多地取决于火焰曲率而不是Ka修饰引起的影响。
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引用次数: 87
期刊
Symposium (International) on Combustion
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