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.

固定的离子液体（ILS）是用于催化的有吸引力的材料，例如，对于受支持的离子液相（SILP）概念，其中包含均质催化剂的IL被固定在固体支持上。该应用的重点是水气（WGS）反应。对于具有RU-SILP催化剂的WGS，已经证明了孔填充度的孔填充度和IL中催化剂浓度对有效活性的影响，但仅被了解。通常，均质催化剂的稳定性取决于进料气体。因此，通过还原与H2的金属络合物观察到RU纳米颗粒的形成。在技​​术过程中，通常仅通过测量活性减少来观察催化剂停用。仅随后对催化剂（表面，成分等）进行研究，才能推断出可能的原因。在设想的项目中，将首次研究基于基于接触式的射频（RF）对WGS反应的SILP催化剂的Operando状态监测。选择了WGS反应，因为它具有重要意义（例如NH3合成），并且由于我们已经在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RF方法是否适合连续过程监测的程度。计划的调查基于三个支柱：1）杰西集团对WGS反应与SILP的初步工作，2）关于Moos集团在基于RF的基于RF的状态监测排气催化剂的状态监测的经验，以及3）关于SILP气体干燥系统的基于RF的水负荷检测的联合工作。在项目中，应系统地研究包含IL和催化剂的支撑物的介电材料特性，这是孔填充度和IL的催化剂载荷的函数。还应考虑温度的影响。还应阐明纯IL的介电特性与SILP的介电特性有多大不同，以及催化材料对介电材料特性的影响。伴随WGS反应的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。这将用于监视SILP催化剂操作。还设想了化学反应过程及其在介电材料参数上的相互作用的建模。这种联系将使反应室中的过程可以从测量的RF数据中使用空间和时间分辨率来理解和定量描述。