Mass spectrometric investigation of chemical conversion processes in flow reactors

连续反应器中化学转化过程的质谱研究

• 批准号: 239921178
• 负责人: Professorin Dr. Tina Kasper
• 金额: --
• 依托单位: Lehrstuhl für Thermodynamik
• 依托单位国家: 德国
• 项目类别: Research Units
• 财政年份: 2013
• 资助国家: 德国
• 起止时间: 2012-12-31 至 2022-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/239921178?language=en
• 关键词: Mass; spectrometric; investigation; chemical; conversion

The main objective of work in the research unit is to investigate the use of engines as flexible chemical reactors. In processes, referred to here as polygeneration, the engines should simultaneously provide higher-value chemicals, heat, and mechanical work. The planned work is the continuation of research performed in the project GV1 of the research unit FOR 1993.GV1 focusses on the investigation of the fundamental kinetic processes underlying the chemical conversion processes. In the third phase of the project, the main objective of the investigations is to assess the influence of ozone as additive on the formation of interesting chemicals because it is expected that ozone already activates the conversion reactions at very low concentrations. Fuel-rich gas mixtures are investigated in two types of flow reactors at temperatures between T = 300 – 1200 K, and high pressure (1 – 20 bar) for different residence times. The gas composition at the outlet of the reactor is analyzed by mass spectrometry and gas chromatography. Desired chemical conversion processes are all reactions that can potentially be used to store chemical energy, e.g. dehydrogenations, steam reforming, or C-C-coupling reactions, and partial oxidations. Conditions that lead to the formation of interesting products are identified by analyzing the product gas composition as function of the process parameters pressure, temperature or the residence time. Concentration profiles as function of reactor temperature or residence time serve as validation data for the development and testing of the “PolyMech” reaction mechanism developed in the research unit 1993. The reaction mechanism serves as a means of information transfer to apply results from the fundamental investigations to the application – the co-production of work and chemicals in the motor.The work in the third phase of the project relies on the methods already successfully implemented in the first two project phases and established collaborations. In the third project phase, biogenic fuels and additives (biogas, ethanol, methanol and oxymethylene ethers) will be used in addition to methane and natural gas to expand the accessible spectrum of products. The most important scientific question is, however, how the use of ozone as additive affects the chemical conversion processes. Ozone decomposes already at low temperature into reactive radicals and can activate the conversion reactions in this way. Since, in contrast to other additives, it does not compete with the fuel for the available oxygen, it does not limit the conversions of the fuel. Based on these observations, it will be investigated to what extent ozone can be used to improve the product yields and the selectivities of oxygenated and non-oxygenated products. As a result of the investigations, a fundamental kinetic understanding of the reaction mechanisms of ozone is generated.

研究单位的主要工作目标是研究发动机作为灵活化学反应堆的使用。在这里称为多联产的过程中，发动机应该同时提供更高价值的化学品，热量和机械功。计划的工作是1993年研究单位GV 1项目的继续。GV 1项目的重点是研究化学转化过程的基本动力学过程。在该项目的第三阶段，调查的主要目标是评估臭氧作为添加剂对形成感兴趣的化学品的影响，因为预计臭氧在非常低的浓度下就已经激活了转化反应。 富燃料气体混合物在两种类型的流动反应器中在T = 300 - 1200 K之间的温度和高压（1 - 20 bar）下对于不同的停留时间进行了研究。通过质谱和气相色谱分析反应器出口处的气体组成。所需的化学转化方法是可以潜在地用于储存化学能的所有反应，例如缩合、蒸汽重整或C-C偶联反应和部分氧化。通过分析作为工艺参数压力、温度或停留时间的函数的产物气体组成来识别导致感兴趣的产物形成的条件。作为反应器温度或停留时间函数的浓度曲线可作为1993年研究单位开发的“PolyMech”反应机制的开发和测试的验证数据。反应机制是将基础研究成果应用于实际应用的信息传递手段--发动机中的功和化学物质的联合生产。项目第三阶段的工作依赖于前两个项目阶段已经成功实施的方法和建立的合作关系。在项目第三阶段，除甲烷和天然气外，还将使用生物燃料和添加剂（沼气、乙醇、甲醇和甲醛醚），以扩大产品的可获得范围。然而，最重要的科学问题是，臭氧作为添加剂的使用如何影响化学转化过程。臭氧在低温下已经分解成活性自由基，并可以以这种方式激活转化反应。与其他添加剂相比，由于它不会与燃料竞争可用的氧气，因此它不会限制燃料的转化。基于这些观察结果，将研究臭氧在多大程度上可以用于改善含氧和非含氧产物的产物产率和选择性。作为调查的结果，臭氧的反应机制的基本动力学的理解产生。