Determination of Transient Reaction Kinetics for Unsteady-State Methanation of CO2 on Ruthenium Catalysts using Periodic Experimentation

使用定期实验测定钌催化剂上 CO2 非稳态甲烷化的瞬态反应动力学

• 批准号: 525949581
• 负责人: Professor Dr.-Ing. Robert Güttel
• 金额: --
• 依托单位: Institut für Chemieingenieurwesen
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/525949581?language=en
• 关键词: Determination; Transient; Reaction; Kinetics; Unsteady

The integration of renewable energies into the chemical value chain requires the design of chemical reactors that can respond flexibly to temporal fluctuations in the availability, quality and composition of the raw materials. On the one hand, a constant product quality should be achieved and, on the other hand, safe operation should be guaranteed even under highly dynamic conditions. Chemical processes that take place on solid catalysts are particularly relevant, as they account for by far the largest share in the chemical industry in terms of value creation. Essential for the design and dimensioning of chemical reactors are the reaction kinetics, which are implemented in suitable mathematical reactor models and represent the catalytic processes at the solid surface. The reactor models are now used to simulate and optimize the reactors with regard to load characteristics, product yield and other aspects. For highly dynamic operation mode, kinetics are required that also adequately represent the transient behavior of the catalysts. However, in most cases, such transient reaction kinetics are not known or only to some extent, since steady-state experiments have usually been performed to obtain kinetic information so far. The proposed project aims to obtain transient kinetic information by means of highly dynamic periodic experiments and model-based evaluation of experimental data. The hydrogenation of CO2 to methane on ruthenium-based catalysts under technically relevant conditions serves as an example reaction with technical relevance. It will be demonstrated that the periodic step response of a chemical reactor contains the corresponding kinetic information and that such information can be determined from the experimental results on the basis of a dynamic reactor model. In particular, the limit cycle that is established during periodic operation will be investigated. The focus is on the development of a methodology for the determination of the transient kinetics from periodic step responses, which includes an adequate experimental procedure and a strategy for model-based evaluation. For this purpose, an application-relevant example reaction from the class of heterogeneously catalyzed gas phase reactions is selected, which offers sufficient complexity with respect to the elementary reactions involved to provide generalizable conclusions.

将可再生能源纳入化学品价值链需要设计能够灵活应对原材料供应、质量和成分随时间波动的化学反应器。一方面，应实现恒定的产品质量，另一方面，即使在高度动态的条件下也应保证安全操作。在固体催化剂上进行的化学过程特别重要，因为它们在价值创造方面占化学工业的最大份额。化学反应器的设计和尺寸的关键是反应动力学，它是在合适的数学反应器模型中实现的，并代表固体表面的催化过程。反应器模型现在用于模拟和优化反应器的负载特性，产品收率和其他方面。对于高度动态的操作模式，需要动力学也充分地表示催化剂的瞬态行为。然而，在大多数情况下，这样的瞬态反应动力学是未知的或仅在某种程度上，因为稳态实验通常已经进行，以获得动力学信息到目前为止。拟议项目旨在通过高动态周期性实验和基于模型的实验数据评估获得瞬态动力学信息。在技术相关的条件下，在铼基催化剂上将CO2氢化成甲烷用作具有技术相关性的示例反应。它将被证明，化学反应器的周期性阶跃响应包含相应的动力学信息，这种信息可以从实验结果的基础上确定的动态反应器模型。特别是，将研究在周期性操作期间建立的极限环。重点是从周期性的阶跃响应，其中包括一个足够的实验程序和基于模型的评估策略的瞬态动力学的确定方法的发展。为此目的，从多相催化气相反应的类别中选择与应用相关的示例反应，其提供关于所涉及的基元反应的足够复杂性以提供可概括的结论。