Search results for: Al₂O₃

Authors: Masood Otarod, Ronald M. Supkowski

Abstract:

This abstract discusses a method that reduces the general dispersion model in cylindrical coordinates to a second order linear ordinary differential equation with constant coefficients so that it can be utilized to conduct kinetic studies in packed bed tubular catalytic reactors at a broad range of Reynolds numbers. The model was tested by 13CO isotope transient tracing of the CO adsorption of Boudouard reaction in a differential reactor at an average Reynolds number of 0.2 over Pd-Al2O3 catalyst. Detailed experimental results have provided evidence for the validity of the theoretical framing of the model and the estimated parameters are consistent with the literature. The solution of the general dispersion model requires the knowledge of the radial distribution of axial velocity. This is not always known. Hence, up until now, the implementation of the dispersion model has been largely restricted to the plug-flow regime. But, ideal plug-flow is impossible to achieve and flow regimes approximating plug-flow leave much room for debate as to the validity of the results. The reduction of the general dispersion model transpires as a result of the application of a factorization theorem. Factorization theorem is derived from the observation that a cross section of a catalytic bed consists of a solid phase across which the reaction takes place and a void or porous phase across which no significant measure of reaction occurs. The disparity in flow and the heterogeneity of the catalytic bed cause the concentration of reacting compounds to fluctuate radially. These variabilities signify the existence of radial positions at which the radial gradient of concentration is zero. Succinctly, factorization theorem states that a concentration function of axial and radial coordinates in a catalytic bed is factorable as the product of the mean radial cup-mixing function and a contingent dimensionless function. The concentration of adsorbed compounds are also factorable since they are piecewise continuous functions and suffer the same variability but in the reverse order of the concentration of mobile phase compounds. Factorability is a property of packed beds which transforms the general dispersion model to an equation in terms of the measurable mean radial cup-mixing concentration of the mobile phase compounds and mean cross-sectional concentration of adsorbed species. The reduced model does not require the knowledge of the radial distribution of the axial velocity. Instead, it is characterized by new transport parameters so denoted by Ωc, Ωa, Ωc, and which are respectively denominated convection coefficient cofactor, axial dispersion coefficient cofactor, and radial dispersion coefficient cofactor. These cofactors adjust the dispersion equation as compensation for the unavailability of the radial distribution of the axial velocity. Together with the rest of the kinetic parameters they can be determined from experimental data via an optimization procedure. Our data showed that the estimated parameters Ωc, Ωa Ωr, are monotonically correlated with the Reynolds number. This is expected to be the case based on the theoretical construct of the model. Computer generated simulations of methanation reaction on nickel provide additional support for the utility of the newly conceptualized dispersion model.

Keywords: factorization, general dispersion model, isotope transient kinetic, partial differential equations

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Authors: S. Toufigh Bararpour, Davood Karami, Nader Mahinpey

Abstract:

Dependence of global economics on fossil fuels has led to a large growth in the emission of greenhouse gases (GHGs). Among the various GHGs, carbon dioxide is the main contributor to the greenhouse effect due to its huge emission amount. To mitigate the threatening effect of CO₂, carbon capture and sequestration (CCS) technologies have been studied widely in recent years. For the combustion processes, three main CO₂ capture techniques have been proposed such as post-combustion, pre-combustion and oxyfuel combustion. Post-combustion is the most commonly used CO₂ capture process as it can be readily retrofit into the existing power plants. Multiple advantages have been reported for the post-combustion by solid sorbents such as high CO₂ selectivity, high adsorption capacity, and low required regeneration energy. Chemical adsorption of CO₂ over alkali-metal-based solid sorbents such as K₂CO₃ is a promising method for the selective capture of diluted CO₂ from the huge amount of nitrogen existing in the flue gas. To improve the CO₂ capture performance, K₂CO₃ is supported by a stable and porous material. Al₂O₃ has been employed commonly as the support and enhanced the cyclic CO₂ capture efficiency of K₂CO₃. Different phases of alumina can be obtained by setting the calcination temperature of boehmite at 300, 600 (γ-alumina), 950 (δ-alumina) and 1200 °C (α-alumina). By increasing the calcination temperature, the regeneration capacity of alumina increases, while the surface area reduces. However, sorbents with lower surface areas have lower CO₂ capture capacity as well (except for the sorbents prepared by hydrophilic support materials). To resolve this issue, a highly efficient alumina-aerogel support was synthesized with a BET surface area of over 2000 m²/g and then calcined at a high temperature. The synthesized alumina-aerogel was impregnated on K₂CO₃ based on 50 wt% support/K₂CO₃, which resulted in the preparation of a sorbent with remarkable CO₂ capture performance. The effect of synthesis conditions such as types of alcohols, solvent-to-co-solvent ratios, and aging times was investigated on the performance of the support. The best support was synthesized using methanol as the solvent, after five days of aging time, and at a solvent-to-co-solvent (methanol-to-toluene) ratio (v/v) of 1/5. Response surface methodology was used to investigate the effect of operating parameters such as carbonation temperature and H₂O-to-CO₂ flowrate ratio on the CO₂ capture capacity. The maximum CO₂ capture capacity, at the optimum amounts of operating parameters, was 7.2 mmol CO₂ per gram K₂CO₃. Cyclic behavior of the sorbent was examined over 20 carbonation and regenerations cycles. The alumina-aerogel-supported K₂CO₃ showed a great performance compared to unsupported K₂CO₃ and γ-alumina-supported K₂CO₃. Fundamental performance analyses and long-term thermal and chemical stability test will be performed on the sorbent in the future. The applicability of the sorbent for a bench-scale process will be evaluated, and a corresponding process model will be established. The fundamental material knowledge and respective process development will be delivered to industrial partners for the design of a pilot-scale testing unit, thereby facilitating the industrial application of alumina-aerogel.

Keywords: alumina-aerogel, CO₂ capture, K₂CO₃, optimization

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Authors: Mostafa Feiz, Hossein Hadizadeh, Mohammad Safari

Abstract:

The Chalpo copper area is located in northeastern Iran, which is part of the structural zone of central Iran and the back-arc basin of Sabzevar. This sedimentary basin accumulated in destructive-Oligomiocene sediments is named the Nasr-Chalpo-Sangerd (NCS) basin. The sedimentary layers in this basin originated mainly from Upper Cretaceous ophiolitic rocks and intermediate to mafic-post ophiolitic volcanic rocks, deposited as a nonconformity. The mineralized sandstone layers in the Chalpo area include leached zones (with a thickness of 5 to 8 meters) and mineralized lenses with a thickness of 0.5 to 0.7 meters. Ore minerals include primary sulfide minerals, such as chalcocite, chalcopyrite, and pyrite, as well as secondary minerals, such as covellite, digenite, malachite, and azurite, formed in three stages that comprise primary, simultaneously, and supergene stage. The best agents that control the mineralization in this area include the permeability of host rocks, the presence of fault zones as the conduits for copper oxide solutions, and significant amounts of plant fossils, which create a reducing environment for the deposition of mineralized layers. Statistical studies on copper layers indicate that Ag, Cd, Mo, and S have the maximum positive correlation with Cu, whereas TiO₂, Fe₂O₃, Al₂O₃, Sc, Tm, Sn, and the REEs have a negative correlation. The calculations of mass changes on copper-bearing layers and primary sandstone layers indicate that Pb, As, Cd, Te, and Mo are enriched in the mineralized zones, whereas SiO₂, TiO₂, Fe₂O₃, V, Sr, and Ba are depleted. The combination of geological, stratigraphic, and geochemical studies suggests that the origin of copper may have been the underlying red strata that contained hornblende, plagioclase, biotite, alkaline feldspar, and labile minerals. Dehydration and hydrolysis of these minerals during the diagenetic process caused the leaching of copper and associated elements by circling fluids, which formed an oxidant-hydrothermal solution. Copper and silver in this oxidant solution might have moved upwards through the basin-fault zones and deposited in the reducing environments in the sandstone layers that have had abundant organic matters. Copper in these solutions probably was carried by chloride complexes. The collision of oxidant and reduced solutions caused the deposition of Cu and Ag, whereas some stable elements in oxidant environments (e.g., Fe₂O₃, TiO₂, SiO₂, REEs) become unstable in the reduced condition. Therefore, the copper-bearing sandstones in the study area are depleted from these elements resulting from the leaching process. The results indicate that during the mineralization stage, LREEs and MREEs were depleted, but Cu, Ag, and S were enriched. Based on field evidence, it seems that the circulation of connate fluids in the reb-bed strata, produced by diagenetic processes, encountered to reduced facies, which formed earlier by abundant fossil-plant debris in the sandstones, is the best model for precipitating sulfide-copper minerals.

Keywords: Chalpo, oligo-miocene red beds, sandstone-hosted copper mineralization, mass change, LREEs, MREEs

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