Hexagonal p-type semiconductor CuS nanoplates were synthesized via a hot injection method from bis(trimethylsilyl)sulfide and the ionic liquid precursor bis(N-dodecylpyridinium) tetrachloridocuprate(ii). The particles have a broad size distribution with diameters between 30 and 680 nm and well-developed crystal habits. The nanoplates were successfully incorporated into organic photovoltaic (OPV) cells as hole conduction materials. The power conversion efficiency of OPV cells fabricated with the nanoplates is 16% higher than that of a control device fabricated without the nanoplates.
5 December 2017 in European Journal of Inorganic Chemistry
We introduce a microwave (MW)-assisted heterogeneous catalytical setup, which we carefully examined for its thermal and performance characteristics. Although MW-assisted heterogeneous catalysis has been widely explored in the past, there is still need for attention towards the specific experimental details, which may complicate the interpretation of results and comparability in general. In this study we discuss technical and material related factors influencing the obtained data from MW-assisted heterogeneous catalysis, specifically in regards to the oxidation of carbon monoxide over a selected perovskite catalyst, which shall serve as a model reaction for exhaust gas aftertreatment. A high degree of comparability between different experiments, both in terms of setup and the catalysts, is necessary to draw conclusions regarding this promising technology. Despite significant interest from both fundamental and applied research, many questions and controversies still remain and are discussed in this study. A series of deciding parameters is presented and the influence on the data is discussed. To control these parameters is both a challenge but also an opportunity to gain advanced insight into MW-assisted catalysis and to develop new materials and processes. The results and discussion are based upon experiments conducted in a monomode MW-assisted catalysis system employing powdered solid-state perovskite oxides in a fixed bed reactor. The discussion covers critical aspects concerning the determination of the actual catalyst temperature, the homogeneity of the thermal distribution, time, and local temperature relaxation (i.e., thermal runaway effects and hotspot formation), particle size effects, gas flow considerations, and system design.
Potassium–oxygen batteries (KOBs) are a promising energy storage technology with high theoretical energy density, low overpotential and a long cycle life. The cathode microstructure plays a significant role in the electrochemical performance of KOB. In this article, hierarchical porosity was introduced to commercially available carbon paper cathodes by thermal pretreatment in air at different pretreatment times. This pretreatment modifies the properties, such as surface area, defects, oxygen functional groups, etc. The discharge performance was determined at three different current densities, i.e., 0.1 mA/cm2, 0.5 mA/cm2, and 1.0 mA/cm2. It has been found that an increase in specific surface area with the introduction of micropores and mesopores is beneficial for the improvement in the discharge capacity by enabling homogeneous discharge product, KO2 distribution and high degrees of pore filling over the volume of the cathode. A reduction in the discharge overpotentials was observed, which is attributed to the introduction of oxygenic functional groups and defects. Samples treated for the longest pretreatment time of 24 h showed the highest discharge capacity of 5 mAh/cm2 and lowest discharge overpotential of 0.03 V.
26 November 2024 in ACS Applied Materials & Interfaces
As a model for the energy-efficient aftertreatment of exhaust gas components, we studied microwave-assisted (MW) CO oxidation over a (La,Sr)CoO3-delta (LSC) perovskite oxide catalyst under dry and humidified conditions. We found that the use of a MW-based process can offer multiple advantages over traditional thermocatalysis in this scenario, as the nature of the MW-solid interaction offers quick, adaptive, and energy-efficient heating as well as improved yield and lower light-off temperatures. As found by combined CO and water MW-desorption experiments, the presence of technically relevant amounts of water leads to a competition for surface active sites and thus slows the reaction rate without indications for a fundamental change in the mechanism. Remarkably, the performance loss related to the presence of water was less pronounced in the MW-assisted process. Additionally, while we recorded a temperature-dependent degradation of the reaction rate in extended MW-catalysis experiments both in dry and humidified conditions, it quickly recovered after a short reactivation MW-treatment. Our study confirms that surface reaction can be driven by the use of MW-radiation in a similar magnitude that can be achieved by thermal activation at significantly higher temperatures. The nature of the effect of the MW-treatment on the structural and electronic surface properties of the LSC material was investigated by X-ray absorption (XAS) and X-ray photoelectron spectroscopy (XPS). We found evidence of a significant structural, chemical, and electronic reorganization of the oxide surface, possibly consistent with the occurrence of overheated surfaces or "hotspots" during MW-exposure, which may explain the increased catalytic and heating properties of the LSC after the MW-pretreatment. The good catalytic performance, quick response to MW-heating, and long-term stability of the catalyst all indicate the promising potential of a MW-based process for the energy-efficient exhaust aftertreatment using noble-metal-free oxide catalysts.
20 February 2024 in The Journal of Physical Chemistry C