Control and intensification of chemical reactions due to periodically operating distributors

该项目的目的是通过在膜分布器中添加反应物来提高所需烯烃的产率。在周期性操作的分布器中，应研究工业相关模型体系丙烷的氧化脱氢和热脱氢。为了最大限度地发挥协同效应，将在一个一体化的反应器中实现质量和能量的耦合，并对其进行评价。在热脱氢过程中，催化剂失活的缺点将通过在过程的每个阶段利用设备/催化剂的周期性操作来弥补。因此，必须基于合适的模型来估计随催化剂活性而变化的受控跨膜氧流量。分布式投药将有效地控制反应前沿的温度和速度。基于一维/二维的暂态计算研究，通过对复杂的温度和速度场的表征和评估，确定了最佳的投药剖面。此外，利用热重法和分段固定床反应器对催化剂的失活/再生进行了定量和数学描述。为了评估计划中的反应器规模，采用了详细的2D模型来研究膜反应器中投药概念对颗粒直径和孔隙率分布的影响。项目的时间发展受到不可预见的因素(前言)的影响，例如机械车间和中试车间大厅的电晕关闭。因此，重要的基于实验的工作包4-5还没有进展。这些存取点特别旨在按计划实现已开发的定期运行的分配器，不仅以解体(分离的温度效应)实现，而且以在试验规模上与物质和能量耦合完全结合的方式实现，它们对项目的圆满完成起着关键作用，其形式是对迄今在试验规模上取得的有希望的模拟结果进行实验验证。到目前为止，在该项目的成功过程中，已为国内和国际会议发表了9篇投稿(1个标价)，并发表了第一篇论文《丙烷氧化脱氢和热脱氢一体化耦合膜反应器分析》(另外2份出版物正在筹备中)。

Aim of the project is to increase the yield of desired olefins by means of reactant dosing in membrane distributors. In a periodically operating distributor the oxidative and thermal dehydrogenation of the industrial relevant model system propane should be investigated. With a view to exploiting maximum synergy effects a mass and energy coupling in one integrated reactor will be realized and evaluated.The disadvantage of catalyst deactivation in the thermal dehydrogenation is intended to be compensated by a periodically operation exploiting the apparatus/catalyst in each phase of the process. Thus, a controlled transmembrane oxygen flow, changing temporally with catalyst activity, has to be estimated based on suitable models. Control of temperature and velocity of reaction fronts will be efficiently adjusted by distributed dosing.Based on transient computational studies (1D/2D) optimal dosing profiles were identified by characterising and evaluating the complex temperature and velocity fields. Furthermore, the deactivation/regeneration of the catalyst by using thermogravimetry and a segmented fixed-bed reactor in a laboratory scale was quantified and mathematically described. Detailed 2D models implementing various approaches for heat transfer were applied to study the influence of particle diameter and porosity distribution by dosing concepts in membrane reactors in order to evaluated the planned reactor scale up.The temporal development of the project was influenced by unforeseeable factors (Preamble) e.g. the Corona shutdown of the mechanical workshop and the pilot plant hall. Thus, the important experimental based working packages 4-5 are not in progress yet. These APs aim in particular at the planned realization of the developed periodically operated distributors not only in a disintegrated (decoupled temperature effects) but also in a fully integrated way with material and energetic coupling in pilot scale They play an essential role for the successful overall conclusion of the project in the form of the experimental validation of the promising simulation results obtained so far on a pilot scale. Up to now, during the successful course of the project, 9 contributions to national and international conferences (1 poster price) and a first paper „Analysis of Membrane Reactors for Integrated Coupling of Oxidative and Thermal Dehydrogenation of Propane” (2 further publications in preparation) could be published.