Operando monitoring of Supported Ionic Liquid Phase (SILP) catalysts by microwave-based methods exemplarily investigated for the water gas shift reaction

通过基于微波的方法对负载型离子液体相 (SILP) 催化剂进行操作监测，对水煤气变换反应进行了示例性研究

• 批准号: 522590549
• 负责人: Professor Dr.-Ing. Andreas Jess
• 金额: --
• 依托单位: Lehrstuhl für Chemische Verfahrenstechnik
• 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/522590549?language=en
• 关键词: Operando; monitoring; Supported; Ionic; Liquid

Immobilized ionic liquids (ILs) are attractive materials for catalysis, e.g., for the Supported Ionic Liquid Phase (SILP) concept, where the IL that contains a homogeneous catalyst is immobilized on a solid support. The application focuses on the water gas shift (WGS) reaction. For WGS with a Ru-SILP catalyst, the influence of the pore filling degree of the support and the catalyst concentration in the IL on the effective activity has been demonstrated, but is only incompletely understood. Often, the stability of the homogeneous catalyst depends on the feed gas. Thus, Ru nanoparticle formation was observed by the reduction of the metal complex with H2. In technical processes, catalyst deactivation is often observed only by measuring the decrease in activity. Only subsequent investigations of the catalyst (surface, composition, etc.) allow to deduce possible reasons for this. In the envisaged project, the contactless radio frequency (RF)-based operando state monitoring of SILP catalysts for the WGS reaction will be investigated for the first time under process conditions. The WGS reaction was selected, because of its significance (e.g. NH3 synthesis) and because we have already gained good experience with SILP systems. Preliminary studies show that the RF method can be used to diagnose the state of the SILP catalyst. The overall objective is therefore to determine whether and to what extent the non-contact RF method is suitable for continuous process monitoring. The planned investigations base on three pillars: 1) on the preliminary work of the Jess group on the WGS reaction with SILP, 2) on the experience of the Moos group on RF-based state monitoring of exhaust gas catalysts, and 3) on joint work on RF-based water loading detection of SILP gas drying systems. In the project, the dielectric material properties of the support that contains the IL and the catalyst are to be systematically investigated as a function of the pore filling degree and the catalyst loading of the IL. The influence of temperature is also to be taken into account. It should also be clarified how much the dielectric properties of the pure IL differ from those of the SILP and how much the catalytic material influences the dielectric material properties. Accompanying kinetic studies of the WGS reaction are essential. The RF method will eventually be used to establish a relationship between the decrease in catalytic "performance" and changes in RF resonance parameters. This will be used to monitor the SILP catalyst operando. Modeling of the chemical reaction processes and their interactions on the dielectric material parameters is also envisioned. This linkage would allow the processes in the reaction chamber to be understood and quantitatively described with spatial and temporal resolution from the measured RF data.

固定化离子液体 (IL) 是一种有吸引力的催化材料，例如，对于负载型离子液体相 (SILP) 概念来说，其中包含均相催化剂的 IL 被固定在固体载体上。该应用重点关注水煤气变换 (WGS) 反应。对于使用 Ru-SILP 催化剂的 WGS，载体的孔填充度和 IL 中的催化剂浓度对有效活性的影响已得到证实，但尚未完全了解。通常，均相催化剂的稳定性取决于原料气。因此，通过用H 2 还原金属络合物观察到Ru纳米颗粒的形成。在技​​术过程中，催化剂失活通常仅通过测量活性下降来观察。只有随后对催化剂（表面、成分等）的研究才能推断出可能的原因。在设想的项目中，将首次在工艺条件下研究用于 WGS 反应的 SILP 催化剂的基于非接触式射频 (RF) 的操作状态监测。选择 WGS 反应是因为它的重要性（例如 NH3 合成）并且因为我们已经在 SILP 系统方面获得了良好的经验。初步研究表明，RF方法可用于诊断SILP催化剂的状态。因此，总体目标是确定非接触式射频方法是否以及在何种程度上适合连续过程监控。计划的调查基于三个支柱：1) Jess 小组在 WGS 与 SILP 反应方面的初步工作，2) Moos 小组在基于 RF 的废气催化剂状态监测方面的经验，以及 3) 联合研究致力于 SILP 气体干燥系统的基于 RF 的水负载检测。在该项目中，将系统地研究包含离子液体和催化剂的载体的介电材料特性，作为离子液体的孔填充度和催化剂负载量的函数。温度的影响也要考虑在内。还应该澄清纯 IL 的介电性能与 SILP 的介电性能有何不同，以及催化材料对介电材料性能的影响有多大。 WGS 反应的伴随动力学研究至关重要。 RF方法最终将用于建立催化“性能”下降与RF共振参数变化之间的关系。这将用于监控 SILP 催化剂操作。还设想了化学反应过程及其对介电材料参数的相互作用的建模。这种联系将使反应室中的过程能够通过测量的射频数据的空间和时间分辨率来理解和定量描述。