This paper presents a study aimed at optimizing the composition of a Co-2(CO)(8): promoter catalytic complex for the ethylene carboalkoxylation reaction in order to maximize the yield and purity of propyl propionate. The following promoters were used: pyridine, dimethylaniline, triethylamine and dimethylaminopyridine. It was found that pyridine and dimethylaminopyridine have the highest catalytic activity. The use of these promoters makes it possible to achieve ethylene conversion of up to 97 % with selectivity for the target product equal to 95 % for pyridine and 90 % for dimethylaminopyridine. It was also found that for the catalytic system Co-2(CO)(8): pyridine the addition of hydrogen to the reaction stock leads to an increase in the target product yield, while for the catalytic system Co-2(CO)(8): dimethylaminopyridine, this activity leads to the opposite effect. In addition, the optimal ratio of the catalytic system Co-2(CO)(8): dimethylaminopyridine was determined to be 14:1. This ratio allows achieving a conversion of 94 % and selectivity for propyl propionate of 93 %.
Catalysts for steam conversion of carbon monoxide of the composition 44 wt
Here we report the synergistic effect of OMS-2 catalysts tested in ethanol oxidation, and the effects produced by both the addition of an Fe modifier in the catalyst preparation stage, and the introduction of Ag on its surface by the impregnation method. To analyze the action of each component, the Fe-modified, Ag-containing OMS-2 catalysts with different Mn/Fe ratios were prepared. Combined XPS and XRF elemental analysis confirms the states and distribution of the Ag- and Fe-containing species between the surface and bulk of the OMS-2 catalysts, which form highly dispersed Ag species on the surface of 0.05Fe–OMS-2, and are also incorporated into the OMS-2 crystalline lattice. The cooperative action of Ag and Fe modifiers improves both reoxidation ability (TPO results) and the amount of adsorbed oxygen species on the catalyst surface. The introduction of Ag to the OMS-2 and 0.05 Fe–OMS-2 surface allows a high level of activity (T80 = 150–155 °C) and selectivity (SAc80 = 93%) towards the acetaldehyde formation.
Abstract The effect of the amount of Mn (II) in the precursor of manganese-aluminium oxide catalysts for the complete oxidation of hydrocarbons on the phase composition and kinetic parameters of the reaction was studied. It was shown that an increase in the amount of manganese in the catalysts results in an increase in the constants of C1-C3 hydrocarbons oxidation reaction rates. An increase in the number of carbon atoms in the alkane leads to an increase in the reaction rate and a decrease in the energy of reaction activation. Promising catalysts for the catalytic combustion of hydrocarbons were identified.
Process of pyrolysis 1, 2 dichloropropane to a allyl chloride have been studied. The reaction was carried out both homogeneously without a catalyst and using catalysts: quartz, waterless CaCl2; 15% mass. Cu/SiO2, 15% mass. CaCl2/Al2O3. It is shown that at 1, 2 dichloropropane conversion 15-40 % main pyrolysis byproducts were DCP is (cys-, trans-) 1-CP and 2-CP with trans-1-CP in most. At that parameters of pyrolysis, it is possible to achieve productivity by an allyl chloride 0.5-0.7 g/(ml⋅h).
Was studied how preparation method influences phase composition, oxide particle size and catalytic activity of the binary NiO–ZrO2 systems. The processes taking place under the thermal influence while NiO–ZrO2 catalysts are formed from precursors, obtained using a variety of methods, were determinated using the methods of simultaneous TGA-DTG/DSC analysis and XFA. Was studied the influence of the precursor preparation method upon the catalysts' phase composition, sizes of the nickel oxide and zirconium dioxide particles. The research revealed that preparation of precursor using coprecipitation method makes it possible to obtain a binary system, where nickel oxide has minimal size, determined by CSR, and monoclinic phase prevails in ZrO2, after heating it to 800 °C. The research unearthed that the catalyst exhibiting maximal catalytic activity by deep oxidation of methane is nickel oxide-zirconium dioxide, containing equal amounts of monoclinic and tetragonal phases of ZrO2.
A new method has been proposed for the synthesis of catalytically active 80 wt % SnO 2 + 20 wt % CeO 2 materials supported on glass fiber, which involves the use of an ethanolic film-forming solution based on cerium(III) nitrate and salicylic acid, with the addition of tin(IV) chloride. We have studied the morphology of the materials thus prepared and assessed their catalytic activity for the deep oxidation of methane. The results indicate that the appreciable catalytic activity of the materials is ensured by their uniform distribution over the support surface and the small oxide aggregate size ( 10 μm), which is due to the use of the filmforming solution of the proposed composition.
Studying the properties of nanomaterials is an important task, but nanomaterials with desired properties is a promising direction. The aim of this work is to investigate the influence of the value of the concentration of the modifier (ions Mn2+) on the structural and functional properties of modified aluminum oxyhydroxide. In this paper, using methods such as the X-ray diffraction studies, differential thermal analysis, electron microscopy, chromatography. The paper found that increasing the concentration of the modifier result in significant changes in the morphology, the appearance of metallic aluminum, which is well seen on X-ray data samples. The influence of thermal effects on a modified aluminum oxyhydroxide argon. Set the phase transition temperatures in the synthesized samples. It is shown that with increasing sodeozhaniya manganese in the composition of the synthesized samples decreases the value of specific surface area. Study of the functional properties showed that the synthesized material has catalytic properties in the oxidation of methane. It is shown that the effective sample is a sample with a manganese content of 2.7 wt. %. By XRD results calcined in air samples modified aluminum oxyhydroxide was shown that only in the sample with a manganese content of 2.7 wt. % MnAl2O4 phase is formed, which is catalytically active phase.
Oxidative transformations of C1-C4 alkanes into olefins on oxide manganese catalysts were under study. We also studied oxidative coupling of methane (OCM) into ethylene on deposited and applied on the silicon dioxide catalysts. We studied the influence of chemical composition of catalyst and promotors on the OCM. Adding a little amount of ethane and propane hydrocarbons to methane allows increasing the concentration of ethylene in gases and significantly increasing productivity in ethylene. The study also shows the impact of the amount of manganese and promotors applied on SiO2 on the yield of olefins during the conversion of C3-C4 alkanes.
The influence of the concentration of Mn2+ in a solution for the hydrolysis of nanosized aluminum powder on the phase composition of the precursor and the content of manganese in samples of aluminum hydroxide is studied. Stages of the formation of catalysts from the precursors are studied by means of synchronic thermogravimetric (TG)-differential scanning calorimetry (DSC) analysis and X-ray phase analysis (XPA). The influence of the number of manganese ions in aluminum hydroxide on the phase composition and catalytic properties of MnO x -Al2O3 systems in the reaction of the deep oxidation of methane is also studied. It is shown that an increase in the concentration of manganese ions in the solution for hydrolysis raises the content of unreacted aluminum and X-ray amorphous hydroxides in the precursors of the catalysts. It is established that the phase composition of the catalyst and the catalytic activity in the reaction of the deep oxidation of methane depend on the content of manganese in the precursor.
The authors have synthesized nanofibrous aluminum oxyhydroxide (AlOOH), modified with different amounts of manganese ions (II), which is the precursor for methane deep oxidation catalysts. It was shown that the catalytic activity of the manganese-based system obtained depends on manganese amount and thermal activation conditions. It is approved that as the catalyst for deep oxidation of hydrocarbons the system with manganese content of 10.5 wt. % is the most perspective despite the fact that the oxidation rate of methane is lower in it than in the catalyst with Mn content of 5.7 wt. %. As opposed to the catalyst with Mn content of 5.7 wt. %., where the aluminium oxide is in metastable form (s-Al 2 O 3 ), the catalyst with manganese content of 10.5 wt. % contains in its structure a thermodynamically and thermally stable α-Al 2 O 3 phase.
The effect of a promoter on the acidic and catalytic properties of aluminum oxide in the reaction of acetic acid ammonolysis has been studied. It has been shown that the promotion of γ-Al 2 O 3 with phosphorus-oxygen compounds results in a change in the porous structure, an increase in the concentration of acid sites, and site strength redistribution, thereby enhancing the activity and selectivity of the catalyst. The change in the acid properties of γ-Al 2 O 3 surface has a significant effect on the second stage of the process, the dehydration of acetamide.
The influence of principal parameters (reaction temperature, ratio of acetic acid and ammonia, composition of reactionary mixture and promotion of catalysts) on the selectivity and yield of the desired product was studied in the reaction of catalytic acetonitrile synthesis by ammonolysis of acetic acid. The processing of γ-Al2O3 by phosphoric acid increases amount of the centers, on which carries out reaction of acetamide dehydration. The kinetic model of a limiting stage of reaction – the acetamide dehydration to acetonitrile was suggested. In the process of ammonolysis of acetic acid it was demonstrated that the use of catalysts promoted by phosphoric acid and ratio NH3:CH3COOH=(3-4):1 at temperatures of a reactor 360-390°С leads to the increase of acetonitrile productivity to 0.7-0.8g/cm3·h and allows to minimize formation of by-products.
Catalysts containing 15 wt % Ni on MgО-Cr 2 О 3 supports with different ratios of magnesium and chromium oxides were prepared. The catalysts were tested in the reactions of partial oxidation and of carbon dioxide and combined reforming of methane into syngas. The phase composition of the catalysts was studied by X-ray diffraction analysis, and the concentration of base sites on the catalyst surface was determined by temperature-programmed CO 2 desorption. The 15 wt % Ni/MgО·Cr 2 O 3 catalyst ensures the highest output of syngas in combined reforming of methane.
Aluminum oxyhydroxide nanofibers modified by manganese ions (II) was shown to have catalytic properties in a reaction of methane deep oxidation. It was established that the catalytic activity was increased at heating the samples in air at 850 degrees C, which is associated with the formation of the manganese oxide phases on the surface of aluminum oxide. The most promising catalyst for the high-temperature combustion of methane was found to be the system with manganese content in a catalyst of 5.7 wt. %.
The effect the method of preparation has on the formation, phase composition, porous structure, and catalytic properties of the 10% Ni-ZrO2 system during the partial oxidation of methane into syngas is studied. Stages of the formation of catalysts from precursors and the effect the method of preparation has on the phase composition, particle size, and catalytic properties of the active component during the partial oxidation of methane into syngas are investigated by means of synchronous TG-DTG/DSC and X-ray diffraction. The synthesis of a catalyst precursor via coprecipitation is shown to yield a monophase system with high nickel dispersion, catalytic activity, and stability.
Catalysts containing 15 wt % Ni on MgO-Cr2O3 supports with different ratios of magnesium and chromium oxides were prepared. The catalysts were tested in the reactions of partial oxidation and of carbon dioxide and combined reforming of methane into syngas. The phase composition of the catalysts was studied by X-ray diffraction analysis, and the concentration of base sites on the catalyst surface was determined by temperature-programmed CO2 desorption. The 15 wt % Ni/MgO·Cr2O3 catalyst ensures the highest output of syngas in combined reforming of methane.