PEPICO in combustion chemistry research II

PEPICO在燃烧化学研究II

• 批准号: 270672969
• 负责人: Professorin Dr. Tina Kasper
• 金额: --
• 依托单位: Institut für Verbrennungstechnik
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2015
• 资助国家: 德国
• 起止时间: 2014-12-31 至 2022-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/270672969?language=en
• 关键词: PEPICO; combustion; chemistry; research; II

A detailed knowledge of the most important reactions plays a key role for the development of a predictive understanding of combustion processes and it is particularly important for ignition processes and the mitigation of pollutants. The goal of this project is to investigate the initial steps of fuel destruction in detail. A key reaction is the formation of a fuel radical by hydrogen abstraction from the carbon frame of the fuel because it leads to isomeric radicals, which in subsequent reactions cause branching in the reaction network. To describe the complete reaction network correctly, the first branching steps must be understood. At low temperatures, the fuel radicals typically react by oxygen addition to peroxides and subsequently oxygenated intermediates. At high temperatures, beta-scissions and unimolecular decomposition form hydrocarbon intermediates. A combination of molecular-beam mass spectrometry (MBMS) and photoelectron-photoion-coincidence spectroscopy (PEPICO) is used to detect the reactive key species experimentally in laminar low pressure flames and in a plug-flow reactor. The experiments with photoionization at the Swiss Light Source are complemented with laboratory based MBMS experiments using electron ionization. The teams of both applicants showed that their flame experiment at the Swiss Light Source features exceptional sensitivity and can identify and quantify isomers better than comparable MBMS instruments. As a consequence, this experiment is ideally suited to detect the mostly radical species in the complex matrix of the flame gases. A Mercator-fellowship for Dr. Hemberger is requested to ensure a high quality of data evaluation. Because the pressure and the reaction times at a specified temperature can be controlled easier and more systematically in a flow reactor than in a model flame, it is one target of this project to build and connect a plug-flow reactor to the MBMS PEPICO system. The goal of these experiments is to characterize the intermediates formed via low-temperature reaction pathways in a wider parameter range by temperature-dependent concentration profiles.A combination of both experiments yields experimental data sets for a series of hydrocarbons (Propene, Propane, 1-Butene, 2-Butene, i-Butene, n-Butane, i-Butane, n-Heptane, Methylhexane, Propylbenzene und Propylcyclohexane) that can be used to develop and validate reaction mechanisms for low and high temperature combustion. The focus of the work in this project is the identification of intermediates that lead to branching in the initial steps of the reaction network. The experimental results obtained in this project will be provided to the scientific community and interpreted in cooperation with model developers.

对最重要反应的详细知识对于开发对燃烧过程的预测理解起着关键作用，这对于点火过程和缓解污染物尤为重要。该项目的目的是详细研究燃料破坏的初始步骤。一个关键的反应是从燃料的碳框架中抽象的燃料自由基形成，因为它导致异构体自由基在随后的反应中导致反应网络中的分支。为了正确描述完整的反应网络，必须了解第一个分支步骤。在低温下，燃料自由基通常会通过氧气加入过氧化物和随后的氧化中间体反应。在高温下，β-静态和单分子分解形成碳氢化合物中间体。 分子梁质谱法（MBMS）和光电子 - 光谱光谱（PEPICO）的组合用于在层状低压火焰中和塞孔反应器中实验检测反应性关键物种。使用电子电离的基于实验室的MBMS实验，在瑞士光源处进行光电离的实验。两位申请人的团队都表明，他们在瑞士光源的火焰实验具有出色的灵敏度，并且可以比可比的MBMS仪器更好地识别和量化异构体。结果，该实验非常适合检测火焰气体复杂基质中的基本激进物种。要求Hemberger博士的Mercator-Fellowship确保高质量的数据评估。由于与模型火焰中的压力和反应时间相比，在指定温度下的压力和反应时间可以更容易，更系统地控制，因此该项目的一个目标是构建和连接插头 - 流动反应器到MBMS Pepico系统。这些实验的目的是表征通过温度依赖性浓度曲线在更广泛的参数范围内通过低温反应途径形成的中间体。两种实验的组合产生了一系列烃（丙烯，丙烷，1--1-）的实验数据集丁烯，2-丁烯，I-丁烯，N-丁烷，I-丁烷，N-己烷，甲基己烷，丙烯苯和丙基环己烷），可用于开发和验证低温和高温燃烧的反应机制。该项目的工作重点是识别中间体，这些中间体在反应网络的初始步骤中导致分支。该项目中获得的实验结果将提供给科学界，并与模型开发人员合作。