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.

最重要的反应的详细知识起着关键作用的发展预测的理解燃烧过程，它是特别重要的点火过程和减轻污染物。该项目的目标是详细调查燃料销毁的初步步骤。一个关键的反应是通过从燃料的碳框架中提取氢来形成燃料自由基，因为它导致异构自由基，其在随后的反应中引起反应网络中的分支。为了正确描述完整的反应网络，必须理解第一个分支步骤。在低温下，燃料自由基通常通过向过氧化物和随后的氧化中间体添加氧而反应。在高温下，β-分裂和单分子分解形成烃中间体。 结合分子束质谱（MBMS）和光电子-光离子符合光谱（PEPICO）被用来检测实验中的层流低压火焰和活塞流反应器中的反应性的关键物种。在瑞士光源的光电离实验的补充与实验室为基础的MBMS实验，使用电子电离。两个申请人的团队表明，他们在瑞士光源的火焰实验具有卓越的灵敏度，并且可以比可比的MBMS仪器更好地识别和量化异构体。因此，该实验非常适合于检测火焰气体的复杂基质中的主要自由基物质。为确保高质量的数据评价，要求为Hemberger博士提供墨卡托研究金。由于在特定温度下的压力和反应时间可以在流动反应器中比在模型火焰中更容易和更系统地控制，因此本项目的目标之一是构建活塞流反应器并将其连接到MBMS PEPICO系统。这些实验的目的是在较宽的参数范围内通过温度依赖的浓度分布来表征通过低温反应途径形成的中间体，这两个实验的组合产生了一系列烃类的实验数据集（丙烯，丙烷，1-丁烯，2-丁烯，异丁烯，正丁烷，异丁烷，正庚烷，甲基己烷，丙苯和丙基环己烷），可用于开发和验证低温和高温燃烧的反应机理。该项目的工作重点是识别在反应网络的初始步骤中导致分支的中间体。该项目获得的实验结果将提供给科学界，并与模型开发人员合作进行解释。