This study focused on natural materials such as clinoptilolite (CLI), metakaolin (MK), marlstone (MRL) and phonolite (PH). Clinoptilolite is one of the most known and common natural minerals (zeolites) with a unique porous structure, metakaolin is calcined kaolin clay, marlstone is a sedimentary rock and phonolite is an igneous rock composed of alkali feldspar and other minerals. These natural materials are mainly used in the building industry (additions for concrete mixtures, production of paving, gravels) or for water purification, but the modification of their chemical, textural and mechanical properties makes these materials potentially usable in other industries, especially in the chemical industry. The modification of these natural materials and rocks was carried out by leaching using 0.1 M HCl (D1 samples) and then using 3 M HCl (D2 samples). This treatment could be an effective tool to modify the structure and composition of these materials. Properties of modified materials were determined by N2 physisorption, Hg porosimetry, temperature programmed desorption of ammonia (NH3-TPD), X-ray fluorescence (XRF), X-ray powder diffraction (XRD), diffuse reflectance infrared Fourier transform (DRIFT) and CO2 adsorption using thermogravimetric analysis (TGA). The results of N2 physisorption measurements showed that that the largest increase of specific surface area was for clinoptilolite leached using 3M HCl. There was also a significant increase of the micropore volume in the D2 samples. The only exception was marlstone, where the volume of micropores was zero even in the leached sample. Clinoptilolite had the highest acidity and sorption capacity of CO2. TGA showed that the amount of CO2 adsorbed was not significantly related to the increase in specific surface area and the opening of micropores. Hg porosimetry showed that acid leaching using 0.1 M HCl and 3 M HCl resulted in a significant increase in the macropore volume in phonolite, and during leaching using 3M HCl there was an increase of the mesopore volume. From the better properties, cost-efficient and environmental points of view, the use of these materials could be an interesting solution for catalytic and sorption applications.
Sulfur-free molybdenum carbides have the potential to replace the conventional sulfided catalysts used for hydrotreating. For these catalysts, it is not necessary to add sulfur to maintain their activity. This fact makes it worthwhile to continue working on improving their hydrotreating efficiency. According to our previous studies, the addition of Co or Ni promotes the hydrotreating activity, but only significant in the case of hydrodesulfurization efficiency (up to 30%). To increase the hydrodenitrogenation efficiency, other promoters, such as phosphorus, can be added. However, most of the published studies do not focus on coprocessing or only on hydrotreating of gas oil model molecules at a laboratory scale. In this paper, we build on our previous research by studying five sulfur-free phosphorus-modified MoCx/Al 2 O 3 catalysts (0.5, 1.5, 2.5, 3.5, and 4.5 wt %) for the hydrotreating of atmospheric gas oil and co-processing with rapeseed oil (5, 10, and 25 wt %) under industrial conditions (330−350 °C, 5.5 MPa, WHSV 1−2 h −1 ). A phosphorus content up to 1.5 wt % promoted the hydrodesulfurization (5− 10%) and the hydrodenitrogenation (10−25%) efficiencies of catalysts. Moreover, the triglycerides addition did not significantly decrease the catalyst activity during co-processing. Therefore, our results enable us to define the range of phosphorus addition that enhances MoCx activity using industrial conditions and commercial feedstocks, pointing the way to develop a suitable and sulfur-free alternative to conventional hydrotreating catalysts.
In this work, we studied the effect of alkali-activated zeolite foams modifications on properties and catalytic activity of cobalt phases in the process of catalytic decomposition of N2O. The zeolite foam supports were prepared by alkali activation of natural zeolite followed by acid leaching and ion exchange. The cobalt catalysts were synthesised by a different deposition technique (direct ion exchange (DIE) and incipient wetness impregnation (IWI) method of cobalt on zeolite foams. For comparison, catalysts on selected supports were prepared and the properties of all were compared in catalytic tests in the pellet form and as crushed catalysts to determine the effect of internal diffusion. The catalysts and supports were in detail characterized by a variety of techniques. The catalyst activity strongly depended on the structure of support and synthesis procedure of a cobalt catalyst. Ion exchange method provided active phase with higher surface areas and sites with better reducibility, both of these factors contributed to higher N2O conversions of more than 80% at 450 °C. A large influence can also be attributed to the presence of alkali metals, in particular, potassium, which resulted in a modification of electronic and acid base properties of the cobalt oxide phase on the catalyst surface. The promotional effect of potassium is better reducibility of cobalt species.
This study focuses on a comparison of alkali-activated materials based on natural zeolites without and with the addition of blast furnace slag and their subsequent modification by acid leaching. The addition of slag to alkali-activated mixtures is generally used to increase the strength. The subsequent modification of its chemical, textural and mechanical properties by acid leaching makes this material usable in other industries, especially in the chemical industry. This study aimed to examine the influence of the addition of blast furnace slag to alkali-activated mixtures based on natural zeolites and observe the effect of subsequent acid leaching on the chemical, textural and mechanical properties and CO2 adsorption capacity of these materials. The modification of alkali-activated materials was carried out by acid leaching using 0.1 M HCl and then using 3 M HCl. The properties of these materials were determined using N2 physisorption, Hg porosimetry, XRF, XRD, DRIFT, TGA and strength measurements. The results showed that the addition of blast furnace slag significantly increased the cutting-edge strength of the obtained materials and affected the textural properties, especially in leached samples. The presence of blast furnace slag generated a higher proportion of mesopores, which are attributed to the presence of the calcium silicate hydrate (C–S–H) phase and are easily removed by leaching, as shown by the XRF results. The obtained data showed an improvement in properties and extension of the potential applicability of these materials in the chemical industry, especially for catalytic and adsorption applications.
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