Unsupported cobalt catalysts promoted with barium (symbol Co/Ba), cerium (Co/Ce) or both (Co/Ce/ Ba) were synthesized and tested in ammonia synthesis at 6.3 MPa. The Ba-free Co and Co/Ce oxide forms of the catalysts were prepared by precipitation/co-precipitation and a subsequent calcination at 500°C. The Co and Co/Ce powders were impregnated with an aqueous solution of barium nitrite. Nitrogen physisorption and H 2 chemisorption measurements revealed that cerium and barium play the role of structural promoters, which hinder the sintering of cobalt oxide during calcination and stabilize the surface of cobalt under reduction conditions. It seems that barium also modifies the surface of the active phase, i.e., cobalt. The kinetic studies of NH 3 synthesis have shown that the co-promoted material (Co/Ce/Ba) is about 2-3 times more active than the system doped with barium (Co/Ba) and more than ten times as active as that with Ce. At 400°C and at low conversion (1% NH 3 ), the ammonia synthesis rate (TOF) over Co/Ce/Ba proved to be almost 60% as high as that obtained for the commercial iron catalyst (KMI, H. Topsøe) commonly used in ammonia plants all over the world. Moreover, at the same temperature and a high ammonia concentration (8%) the co-promoted cobalt catalyst is over two times more active than the fused iron catalyst. Another asset of the cobalt catalyst is its high thermal stability.
In this laboratory experiment, the synthesis of a supported solid catalyst (Cu/SiO 2 ) and its application in the dehydrogenation of cyclohexanol performed under flow conditions was studied. The experiment was planned for a group of two or three students for two 6 h long sessions. The copper catalyst was synthesized using incipient wetness impregnation of the silica support with copper(II) nitrate trihydrate as the precursor of the active phase. It was then dried, calcined, and reduced. Each step of the synthesis was characterized by color change. The catalytic reaction was performed as a continuous process in a flow reactor, and the postreaction mixture was analyzed using gas chromatography. The laboratory experiment showed practical aspects of heterogeneous catalysis and encouraged students to seek alternative, environmentally friendly methods of organic compound synthesis.
AbstractThere is a strong need for transformative sanitation systems in the areas of the world where open defecation habits and/or inadequate sewage treatment methods and facilities exist. This paper describes an innovative thermally efficient solid waste treatment process as a basis for an off-the-grid, non-sewered toilet in order to address this need. Human feces are combusted in a continuous-cyclic manner using two stages of smoldering and catalytic oxidation. It has been shown that thermal coupling of the two stages creates a self-sustained reactor that can combust wet fecal material containing up to 3.2 parts water to 1 part dry matter – equivalent of water content in healthy human feces – without the need for external heating, known as the ultimate challenge in direct combustion of human feces. Furthermore, it has been shown that air flow rate can be reliably used as a controlling mechanism for fecal destruction rate which means the same reactor could be operated for various and varying input rates. The present work demonstrates the potential for manufacturing low-cost, low-energy consuming sanitation systems that are more easily accessible to communities in need of such systems.
Although heterogeneous monometallic gold catalysts are commonly more active when the gold particles are smaller, this study shows that the reverse is true in the case of liquid phase catalytic transfer hydrogenation of acetophenone with 2-pentanol. Higher catalytic activity of larger gold particles, i.e., over 30 nm in diameter, than of smaller particles of average 4 nm in size was observed. Moreover, this effect was contradictory to that observed for supported monometallic silver catalysts in which the interaction with the support and hence particle size was shown to cause drastic changes in the activity in this reaction, with the large particles being completely inactive and tiny ones being the most active system studied. In this reaction, the ceria-zirconia solid solutions were used as the supports for the catalysts and both zirconium doped ceria, as well as cerium doped zirconia carriers were tested. The supports themselves exhibited little activity in this reaction. It was shown that the activity of the supports and catalysts depends on the Ce/Zr ratio and potassium content. Both types of catalysts showed excellent selectivity to 1-phenylethanol and conversion of acetophenone, although it was noted that a high loading of potassium carbonate in the gold catalysts propelled undesired reactions, thereby reducing the selectivity to 1-phenylethanol.
The influence of the lanthanum and barium addition on the physicochemical properties and catalytic behavior of the Ru/C catalyst for CO methanation was investigated. The catalyst was doped with La or with La plus Ba. It was found out that there are various ways the additives were applied in the study, thus changing the catalytic performance of the basic material and influencing the susceptibility of the carbon support in relation to undesired methanation. The highest catalytic activity, 23.46 (mmol CO/gC+Ru × h), was achieved for the LaRu/C system, with methane selectivity exceeding 80% over the whole temperature range. Ba addition caused a significant decrease in activity. TG-MS studies revealed that both La and Ba improved the resistance of the carbon support to undesired methanation. Detailed characterization methods, employing XRPD, Raman spectroscopy, CO chemisorption, and SEM-EDX, showed that the catalytic behavior of the studied catalysts was attributed to lanthanum distribution over the Ru/C materials surface and structural changes in the carbon support affecting electron supply to the metallic active phase.
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