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An experimental and kinetic modeling study of the pyrolysis and oxidation of n-C3C5 aldehydes in shock tubes

机译：冲击管中n-C3C5醛热解和氧化的实验和动力学建模研究

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Due to the increasing interest in the use of biofuels for energy production, it is of great importance to better understand the combustion and thermal decomposition characteristics of species such as aldehydes.\udThese are known to be key intermediate products of transport fossil and bio-fuels combustion and are also dangerous pollutants emitted from combustion in internal combustion engines and from gasification\udof biomasses. In this study, an experimental and kinetic modeling investigation of propanal, n-butanal and n-pentanal pyrolysis and oxidation in two shock tube facilities was carried out. Experiments were\udperformed in a single pulse shock tube to determine the speciation profiles of the fuels and intermediate species under pyrolysis conditions for mixture of pure propanal/n-butanal/n-pentanal (3%)–Ar (97%), at\udaveraged reflected pressure of 1.9 atm and at reflected shock temperatures of 972–1372 K. Additionally, ignition delay times for mixtures of pure propanal/n-butanal/n-pentanal (1%)–O2/Ar were measured in\udthe temperature range 1136–1847 K, at pressures of 1 and 3 atm, and at equivalence ratios of 0.5, 1.0 and 2.0.\udA comprehensive sub-mechanism for the high temperature kinetics of the three aldehydes was developed. This scheme was then coupled with NUIG (National University of Ireland, Galway) and POLIMI\ud(Politecnico di Milano) C0AC4 kinetic schemes. The inclusion of the aldehydes sub-mechanism in two different kinetic environments, required modifications for the H-abstraction reactions, due to different rate\udrules in use in the two kinetic environments, and due to differences in the C0AC4 kinetic schemes. Both of the models were validated and showed good agreement with the new experimental data. The mechanisms\udare also satisfactorily compared with ignition delay times, speciation profiles and laminar burning velocities previously published in literature. Reaction pathways and sensitivity analyses were also performed\udto highlight the important reaction steps involved in the pyrolysis and oxidation processes. The major differences between the models and the experiments have to be attributed to the chemistry\udof the smaller species, more than to aldehyde specific reactions. This work further highlights the relevant role of the C0AC4 sub-mechanism, mainly in terms of a unification process that needs to start from the\udsmaller species chemistry in order to obtain an unambiguous description of any fuel investigated.
机译：由于人们越来越关注使用生物燃料进行能源生产，因此，更好地了解醛等物质的燃烧和热分解特性至关重要。\ ud这些物质是运输化石和生物燃料的关键中间产品燃烧，并且也是内燃机燃烧以及生物质气化\ udud排放的危险污染物。在这项研究中，在两个激波管设施中进行了丙醛，正丁醛和正戊醛的热解和氧化的实验和动力学模型研究。在单脉冲激波管中进行实验以测定纯丙醛/正丁醛/正戊醛（3％）– Ar（97％）混合物在热解条件下燃料和中间物质的形态分布，平均反射压力为1.9 atm，反射冲击温度为972–1372K。此外，在\温度范围内测量了纯丙醛/正丁醛/正戊醛（1％）– O2 / Ar混合物的点火延迟时间。在1和3 atm的压力下，以及当量比为0.5、1.0和2.0的情况下，产生了1136–1847K。\ ud针对三种醛的高温动力学开发了一种综合的子机制。然后将该方案与NUIG（爱尔兰国立大学，戈尔韦分校）和POLIMI \ ud（米兰理工大学）的C0AC4动力学方案结合。由于在两种动力学环境中使用不同的速率/规则，并且由于CO 2动力学方案的差异，所以在两种不同的动力学环境中包括醛亚机理，需要对H-抽象反应进行修饰。两种模型均经过验证，并与新的实验数据显示出良好的一致性。与以前在文献中发表过的点火延迟时间，形态分布和层流燃烧速度相比，该机理也令人满意。还进行了反应途径和敏感性分析，以突出热解和氧化过程中涉及的重要反应步骤。模型和实验之间的主要差异必须归因于较小物种的化学反应，而不是醛特异性反应。这项工作进一步突出了C0AC4子机制的相关作用，主要是在统一过程中，该过程需要从较小的物种化学开始，以获得对所研究燃料的明确描述。

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