Mass spectrometric investigation of chemical conversion processes in flow reactors

研究单位的主要工作目标是研究使用发动机作为柔性化学反应器。在这里称为多联产的过程中，发动机应该同时提供高价值的化学物质、热量和机械功。计划的工作是继续1993年研究单位的GV1项目所进行的研究。GV1侧重于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，调查的主要目的是评估臭氧作为添加剂对有趣化学品形成的影响，因为预计臭氧在极低浓度下已经激活了转化反应。在两种类型的流动反应器中，在T = 300 - 1200 K的温度和高压（1 - 20 bar）的不同停留时间下，研究了富燃料气体混合物。用质谱法和气相色谱法分析反应器出口的气体成分。期望的化学转化过程是所有可能用于储存化学能的反应，例如脱氢，蒸汽重整，或c -c偶联反应和部分氧化。通过分析产品气体成分作为工艺参数压力、温度或停留时间的函数来确定导致有趣产品形成的条件。浓度曲线作为反应器温度或停留时间的函数，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。反应机理作为一种信息传递手段，将基础研究的结果应用于电机中功和化学物质的共同生产。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已建立的合作关系。在第三个项目阶段，除甲烷和天然气外，还将使用生物燃料和添加剂（沼气、乙醇、甲醇和甲氧基醚），以扩大可获得的产品范围。然而，最重要的科学问题是，使用臭氧作为添加剂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，并以这种方式激活转化反应。因为，与其他添加剂相比，它不与燃料竞争可用的氧气，它不限制燃料的转化。根据这些观察结果，将研究臭氧在多大程度上可以用来提高产品产量和氧化和非氧化产品的选择性。作为研究的结果，对臭氧的反应机制产生了基本的动力学理解。

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.