Recently, a laboratory setup for microwave-based characterization of powder samples at elevated temperatures and different gas atmospheres was presented. The setup is particularly interesting for operando investigations on typical materials for exhaust gas aftertreatment. By using the microwave cavity perturbation method, where the powder is placed inside a cavity resonator, the change of the resonant properties provides information about changes in the dielectric properties of the sample. However, determining the exact complex permittivity of the powder samples is not simple. Up to now, a simplified microwave cavity perturbation theory had been applied to estimate the bulk properties of the powders. In this study, an extended approach is presented which allows to determine the dielectric properties of the powder materials more correctly. It accounts for the electric field distribution in the resonator, the depolarization of the sample and the effect of the powder filling. The individual method combines findings from simulations and recognized analytical approaches and can be used for investigations on a wide range of materials and sample geometries. This work provides a more accurate evaluation of the dielectric powder properties and has the potential to enhance the understanding of the microwave behavior of storage materials for exhaust gas aftertreatment, especially with regard to the application of microwave-based catalyst state diagnosis.
Recently, radio frequency (RF) technology was introduced as a tool to determine the oxygen storage level of a three-way catalyst (TWC) for gasoline vehicles. Previous studies on the investigation of commercial catalysts mostly use only the resonant frequency to describe the correlation of oxygen storage level and RF signal. For the first time this study presents a comparison under defined laboratory conditions considering both, resonance frequency and also the quality factor as measurands. Furthermore, various advantages over the sole use of the resonant frequency in the technical application are discussed. Experiments with Ø4.66’’ catalysts and Ø1.66’’ catalyst cores with alternating (rich/lean) gas compositions showed that the relative change in signal amplitude due to a change in oxygen storage is about 100 times higher for the inverse quality factor compared to the resonant frequency. In addition, the quality factor reacts more sensitively to the onset of the oxygen-storage ability, and delivers precise information about the necessary temperature, which is not possible when evaluating the resonant frequency due to the low signal amplitude. As investigations on aged catalysts confirm, the quality factor also provides a new approach to determine operando the ageing state of a TWC.
This study reassesses an overview of the potential of the radio frequency (RF)-based state diagnostics of three-way catalysts (TWC) based on a previous study with an emphasis on the defect chemistry of the catalyst material during reoxidation and reduction. Some data are based on the previous works but are newly processed, and the signal parameters resonant frequency and inverse quality factor are evaluated with respect to applicability. The RF-based method uses electromagnetic resonances in a cavity resonator to provide information on the storage level of the oxygen storage component. The analysis focuses on a holistic investigation and evaluation of the major effects influencing the RF signal during operation. On the one hand, the response to the oxygen storage behavior and the resolution of the measurement method are considered. Therefore, this study merges original data from multiple former publications to provide a comprehensive insight into important measurement effects and their defect chemistry background. On the other hand, the most important cross-sensitivities are discussed and their impact during operation is evaluated. Additionally, the effect of catalyst aging is analyzed. The effects are presented separately for the two resonant parameters: resonant frequency and (unloaded) quality factor. Overall, the data suggest that the quality factor has a way higher signal quality at low temperatures (<400 °C) and the resonant frequency is primarily suitable for high operating temperatures. At most operating points, the quality factor is even more robust against interferences such as exhaust gas stoichiometry and water content. Correctly estimating the catalyst temperature is the most important factor for reliable results, which can be achieved by combining the information of both resonant signals. In the end, the data indicate that microwave-based state diagnosis is a powerful system for evaluating the oxygen storage level over the entire operating range of a TWC. As a research tool and in its application, the system can therefore contribute to the improvement of the emission control of future gasoline vehicles.
An important process of chemical engineering is the removal of moisture from natural gas and process gases by fixed-bed adsorption. Experiments were conducted to design (ad)sorption columns, predict breakthrough behavior, and determine the velocity of the (ad)sorption front. The data obtained from these adsorption experiments served as input parameters for modeling by the linear driving force approach. In this study, the supported ionic liquid (SILP) 1-ethyl-3-methylimidazolium methanesulfonate ([EMIM][MeSO3]), coated on porous silica, was used as drying agent in fixed-bed adsorption. A novel method for the operando monitoring of (ad)sorption fronts in fixed-bed adsorbers is the radio-frequency-based cavity perturbation method. Here, the adsorber forms a cavity resonator. A model based on S-shaped advancing sorption profiles that is represented by a cumulative Gaussian distribution (CDF) is applied. Furthermore, it is shown that the modeled (ad)sorption fronts lead to resonance parameters measured via the microwave-based cavity perturbation method with high precision. It is demonstrated that the breakthrough curves in SILPs can be accurately reproduced both by the new radio-frequency-based method and by a classical chemical engineering tool such as the linear driving force model.