Search Results (6)

Gold catalysts, with different particle sizes ranging from 19 to 556 Å, and supported on SBA-15 mesoporous silica, were prepared by using deposition-precipitation, co-precipitation, and impregnation methods. All samples were characterised by TEM, EXAFS, XPS, XRD, CFR (Continuous Flow Reactor), and TPR. The sample which proved to have the highest activity was characterised by TAP (Temporal Analysis of Products) as well. XPS, wide-angle XRD, EXAFS, and H₂-TPR measurements and data analysis confirmed that gold was present as Au⁰ only on all samples. The size of the Au nanoparticle was determined from TEM measurements and confirmed through wide-angle XRD measurements. EXAFS measurements showed that as the Au-Au coordination number decreased the Au-Au bond length decreased. TEM data analysis revealed a dispersion range from 58% (for the smallest particle size) to 2% (for the highest particle size). For Au particles’ sized lower that 60 Å, the Au dispersion was determined using a literature correlation between the dispersion and EXAFS Au-Au coordination number, and was in good agreement with the dispersion data obtained from TEM. The Au dispersion decreased as the particle size increased. CFR experiments validated the relationship between the size of the gold particles in a sample and the sample’s catalytic activity towards acetone oxidation. The lowest temperature for the acetone 100% conversion, i.e., 250 °C, was observed over the reduced catalyst sample with the smallest particle size. This sample not only showed the highest catalytic activity towards acetone conversion, but, at the same time, showed high reaction stability, as catalyst lifetime tests, performed for 25 h in a CFR at 270 °C for the as-synthesised sample, and at 220 °C for the reduced sample, have confirmed. TAP (Temporal Analysis of Products) measurements and data analysis confirmed a weak competitive adsorption of acetone and oxygen over the Au/SBA-15 sample. Based on TAP data, a combination of Eley–Rideal and Langmuir–Hinshelwood mechanisms for acetone complete oxidation was proposed. Full article

Time series of vegetation indices can be utilized to capture crop phenology information, and have been widely used in land cover and crop classification, phenological feature extraction, and planting structure monitoring. This is of great significance for guiding agricultural production and formulating agricultural policies. According to the characteristics of the GF-6 satellite’s newly-added red edge bands, wide field view and high-frequency imaging, the time series of vegetation indices about multi-temporal GF-6 WFV data are used for the study of land cover and crop classification. In this study, eight time steps of GF-6 WFV data were selected from March to October 2019 in Hengshui City. The normalized difference vegetation index (NDVI) time series and 10 different red edge spectral indices time series were constructed. Then, based on principal component analysis (PCA), using two feature selection and evaluation methods, stepwise discriminant analysis (SDA) and random forest (RF), the red edge vegetation index of normalized difference red edge (NDRE) was selected. Seven different lengths of NDVI, NDRE and NDVI&NDRE time series were reconstructed by the Savizky-Golay (S-G) smoothing algorithm. Finally, an RF classification algorithm was used to analyze the influence of time series length and red edge indices features on land cover and crop classification, and the planting structure and distribution of crops in the study area were obtained. The results show that: (1) Compared with the NDRE red edge time series, the NDVI time series is more conducive to the improvement of the overall classification accuracy of crops, and NDRE can assist NDVI in improving the crop classification accuracy; (2) With the shortening of NDVI and NDRE time series, the accuracy of crop classification is gradually decreased, and the decline is gradually accelerated; and (3) Through the combination of the NDVI and NDRE time series, the accuracy of crop classification with different time series lengths can be improved compared with the single NDVI time series, which is conducive to improving the classification accuracy and timeliness of crops. This study has fully tapped the application potential of the new red edge bands of GF-6 WFV time series data, which can provide references for crop identification and classification of time series data such as NDVI and red edge vegetation index of different lengths. At the same time, it promotes the application of optical satellite data with red edge bands in the field of agricultural remote sensing. Full article

Conventional fossil fuels such as gasoline or diesel should be substituted in the future by environmentally-friendly alternatives in order to reduce emissions in the transport sector and thus mitigate global warming. In this regard, iso-butanol is very promising as its chemical and physical properties are very similar to those of gasoline. Therefore, ongoing research deals with the development of catalytically-supported synthesis routes to iso-butanol, starting from renewably-generated methanol. This research has already revealed that the dehydrogenation of ethanol plays an important role in the reaction sequence from methanol to iso-butanol. To improve the fundamental understanding of the ethanol dehydrogenation step, the Temporal Analysis of Products (TAP) methodology was applied to illuminate that the catalysts used, Pt/C, Ir/C and Cu/C, are very active in ethanol adsorption. H₂ and acetaldehyde are formed on the catalyst surfaces, with the latter quickly decomposing into CO and CH₄ under the given reaction conditions. Based on the TAP results, this paper proposes a reaction scheme for ethanol dehydrogenation and acetaldehyde decomposition on the respective catalysts. The samples are characterized by means of N₂ sorption and Scanning Transmission Electron Microscopy (STEM). Full article

In the development of catalytic materials, a set of standard conditions is needed where the kinetic performance of many samples can be compared. This can be challenging when a sample set covers a broad range of activity. Precise kinetic characterization requires uniformity in the gas and catalyst bed composition. This limits the range of convecting devices to low conversion (generally <20%). While steady-state kinetics offer a snapshot of conversion, yield and apparent rates of the slow reaction steps, transient techniques offer much greater detail of rate processes and hence more information as to why certain catalyst compositions offer better performance. In this work, transient experiments in two transport regimes are compared: an advecting differential plug flow reactor (PFR) and a pure-diffusion temporal analysis of products (TAP) reactor. The decomposition of ammonia was used as a model reaction to test three simple materials: polycrystalline iron, cobalt and a bimetallic preparation of the two. These materials presented a wide range of activity and it was not possible to capture transient information in the advecting device for all samples at the same conditions while ensuring uniformity. We push the boundary for the theoretical estimates of uniformity in the TAP device and find reliable kinetic measurement up to 90% conversion. However, what is more advantageous from this technique is the ability to observe the time-dependence of the reaction rate rather than just singular points of conversion and yield. For example, on the iron sample we observed reversible adsorption of ammonia and on cobalt materials we identify two routes for hydrogen production. From the time-dependence of reactants and product, the dynamic accumulation was calculated. This was used to understand the atomic distribution of H and N species regulated by the surface of different materials. When ammonia was pulsed at 550 °C, the surface hydrogen/nitrogen, (H/N), ratios that evolved for Fe, CoFe and Co were 2.4, 0.25 and 0.3 respectively. This indicates that iron will store a mixture of hydrogenated species while materials with cobalt will predominantly store NH and N. While much is already known about iron, cobalt and ammonia decomposition, the goal of this work was to demonstrate new tools for comparing materials over a wider window of conversion and with much greater kinetic detail. As such, this provides an approach for detailed kinetic discrimination of more complex industrial samples beyond conversion and yield. Full article

The aim of this study was to compare the applicability and the correlation between three commercially available instruments capable of detection, quantification, and characterization of ultrafine airborne particulate matter in the industrial setting of a tapping area in a silicon alloy production plant. The number concentration of ultrafine particles was evaluated using an Electric Low Pressure Impactor (ELPI^TM), a Fast Mobility Particle Sizer (FMPS^TM), and a Condensation Particle Counter (CPC). The results are discussed in terms of particle size distribution and temporal variations linked to process operations. The instruments show excellent temporal covariation and the correlation between the FMPS and ELPI is good. The advantage of the FMPS is the excellent time- and size resolution of the results. The main advantage of the ELPI is the possibility to collect size-fractionated samples of the dust for subsequent analysis by, for example, electron microscopy. The CPC does not provide information about the particle size distribution and its correlation to the other two instruments is somewhat poor. Nonetheless, the CPC gives basic, real-time information about the ultrafine particle concentration and can therefore be used for source identification. Full article

Aiming at an improved mechanistic understanding of the preferential oxidation of CO on supported Au catalysts, we have investigated the competition between CO and H₂ for stable, active oxygen (O_act) species on a Au/TiO₂ catalyst during the simultaneous exposure to CO and H₂ with various CO/H₂ ratios at 80 °C and 400 °C by quantitative temporal analysis of products (TAP) reactor measurements. It is demonstrated that, at both higher and lower temperature, the maximum amount of active oxygen removal is (i) independent of the CO/H₂ ratio and (ii) identical to the amount of active oxygen removal by CO or H₂ alone. Hence, under preferential CO oxidation (PROX) reaction conditions, in the simultaneous presence of CO and H₂, CO and H₂ compete for the same active oxygen species. In addition, also the dependency of the selectivity towards CO oxidation on the CO/H₂ ratio was evaluated from these measurements. Consequences of these findings on the mechanistic understanding of the PROX reaction on Au/TiO₂ will be discussed. Full article