199 research outputs found
Dissolution rate and diffusivity of lime in steelmaking slag and development of fluoride-free fluxes
A rotating disk technique was used to determine the dissolution rate and
diffusivity of CaO and MgO in slags. The dissolution rate was deduced from the
measured changes in concentration of oxides in slag with respect to reaction
time. The experimental set- up was initially tested with dissolution of magnesia in
the CaO – 55 wt% Al2O3 slag at 1430 ºC and a measured rate of 2.7 ´10 -5
g/cm2.s was obtained. The dissolution rate was increased by slag chemistry and
ranged from 6.5´10-5 to 2.1´10-4 g/cm2.s.
The dissolution rate of CaO was measured in CaO – 42 wt% Al2O3 – 8% SiO2
based slag. The measured dissolution rates were found to be strongly dependent
on the slag chemistry and temperature and ranged from 5.03´10 -5 to 3.3´10 -4
g/cm2.s.
The dissolution rates were strongly dependent on the rotation speed and results
indicate mass transfer in the slag phase to be rate- limiting step.
The diffusivity of MgO / CaO was calculated from the dissolution rate and
solubility data, using known mass transfer correlations. The diffusivity of MgO
in the calcium aluminate slag at 1430 ºC was found to be about 1.1´10-5 cm2/s.
Additions of 5 and 10 wt% Fe2O3 increased the diffusivity by a factor ~ 1.5 to 3,
respectively. However, with introduction of (CaF2 5 wt% + Fe2O3 5 wt%) and
(CaF2 5 wt% + Fe2O3 10 wt%) in the slag, the diffusivity increased considerably
by a factor of about 29 and 11, respectively.
The diffusivity of CaO in calcium aluminosilicate was measured to be in the
order of 10-6 to 10-5 over a temperature range of 1430 – 1600 ºC. CaF2 increased
the diffusivity by a factor of 3 to 5 while MnOx and FeOx, ilmenite and TiO 2
increased the diffusivity substantially and SiO2 had an opposite effect. The
measured diffusivities are in accord with published data on comparable systems
and are discussed with reference to Eyring theory.
It was concluded that MnOx, FeOx and ilmenite in the slag increase the
dissolution rate and diffusivity of lime, showing comparable results with respect
to CaF2
Carbon Capture Utilization and Storage in Methanol Production Using a Dry Reforming-Based Chemical Looping Technology
This further investigates the concept of gas switching dry reforming (GSDR) that efficiently converts the two major greenhouse gases (CO2 and CH4) into a valuable product (syngas) for gas-to-liquid (GTL) syntheses. The proposed GSDR is based on chemical looping technology but avoids external circulation of solids (metal oxides) by alternating the supply of reducing and oxidizing gas into a single fluidized bed reactor to achieve redox cycles. Each cycle consists of three steps where a metal oxide/catalyst is first reduced using GTL off-gases to produce CO2 (and steam) that is supplied to the next reforming step to produce syngas for GTL processes. The metal oxide is then reoxidized in the third step associated with heat generation (through the exothermic oxidation reaction of the metal oxide and air) to provide the heat needed for the endothermic dry methane reforming step. Experimental demonstrations have shown that a syngas H2/CO molar ratio between 1 and 2 suitable for methanol production could be achieved. A further demonstration shows that pressure has negative effects on gas conversion. Following the successful experimental campaign, process simulations were completed using ASPEN to show how the GSDR process can be integrated into a methanol (MeOH) production plant.publishedVersio
Comparison of particle-resolved direct numerical simulation and 1d modelling of catalytic reactions in a cylindrical particle bed
This work presents a comparative study of reactive flow in a realistically packed array of cylindrical particles on two widely different scales: particle-resolved direct numerical simulation (PR-DNS) and 1D modelling. PR-DNS directly simulates all transfer phenomena in and around the cylindrical particles, while 1D modelling utilizes closure models to predict system behaviour at a computational cost several orders of magnitude lower than PR-DNS. PR-DNS is performed on a geometry of ~100 realistically packed cylindrical particles generated using the discrete element method (DEM). Simulations are performed over a range of Thiele moduli, Prandtl numbers and reaction enthalpies. The geometry with particles of aspect ratio four is meshed with fine polyhedral elements both inside and outside the particles. Hence, we obtain accurate results for combined internal and external heat and mass transfer in the cylindrical particle array. These results are compared with a 1D packed bed reactor model incorporating appropriate models for intra particle diffusion and for external heat and mass transfer (applicable to cylindrical particles). Results document a good comparison for the heterogeneous first order catalytic simple reaction. Therefore, recommendations are made to guide future 1D modelling works involving reactive flows in packed beds of cylindrical particles
Integration of chemical looping combustion for cost-effective CO2 capture from state-of-the-art natural gas combined cycles
Chemical looping combustion (CLC) is a promising method for power production with integrated CO2 capture with almost no direct energy penalty. When integrated into a natural gas combined cycle (NGCC) plant, however, CLC imposes a large indirect energy penalty because the maximum achievable reactor temperature is far below the firing temperature of state-of-the-art gas turbines. This study presents a techno-economic assessment of a CLC plant that circumvents this limitation via an added combustor after the CLC reactors. Without the added combustor, the energy penalty amounts to 11.4%-points, causing a high CO2 avoidance cost of 93.8/ton) with an energy penalty of 8.1%-points. This conventional CLC plant would also require a custom gas turbine. With an added combustor fired by natural gas, a standard gas turbine can be deployed, and CO2 avoidance costs are reduced to 96.3/ton when a hydrogen cost of 90.3/ton by lowering the energy penalty to only 0.6%-points. An attractive alternative is, therefore, to construct the plant for added firing with natural gas and retrofit the added combustor for hydrogen firing when CO2 prices reach very high levels
Evaluation of a Lagrangian Discrete Phase Modeling Approach for Application to Industrial Scale Bubbling Fluidized Beds
Industrial scale bubbling fluidized bed simulations were carried out within the Kinetic Theory of Granular Flows (KTGF). The KTGF was applied within two different modelling frameworks, the traditional Two Fluid Model (TFM) and a new approach in the form of the Dense Discrete Phase Model (DDPM), in order to identify any differences in performance. Only the DDPM was able to attain fully grid independent results for industrial scale 2D simulations. In fact, the performance was sufficiently good to enable the completion of reasonably affordable full 3D simulations. These simulations revealed some differences between 2D and 3D, but the global system behaviour remained relatively similar. Comparisons to experimental pressure drop data for both 2D and 3D simulations were acceptable
The sensitivity of filtered Two Fluid Models to the underlying resolved simulation setup
Eulerian-Eulerian modelling based on the Kinetic Theory of Granular Flow has proven to be a promising tool for investigating the hydrodynamic and reactive behaviour inside fluidized beds. The primary limitation of this approach is the very fine grid size necessary to fully resolve the transient solid structures that are typical of fluidized bed reactors. It therefore remains impractical to simulate industrial scale fluidized bed reactors using resolved Two Fluid Model (TFM) simulations. For this reason, there is currently widespread interest in developing sub-grid (filtered) models that allow accurate simulations at coarser grids by correcting for the effects of unresolved solid structures. However, little attention has been paid to the importance of the choice of the underlying TFM closures during the derivation of the filtered models.
This paper follows a similar approach to an establish filtered TFM (1) to derive sub-grid closures for the interphase momentum exchange , solids viscosity and solids pressure in 2D periodic simulations. These corrections are obtained for different particle-particle restitution coefficients, frictional pressure models and drag models as a function of the particle phase volume fraction and the filter size. This reveals at which values of the markers the individual resolved TFM model choices have significant effects on the final expressions derived for filtered TFMs. Based on these findings suggestions are made regarding the derivation of new filtered TFMs and the use of the existing models.
1. Y. Igci and S. Sundaresan. Constitutive Models for Filtered Two-Fluid Models of Fluidized Gas–Particle Flows. Ind. Eng. Chem. Res., 50: 13190-13201, 2013
Evaluation of the minimum fluidization velocity at elevated temperature and pressure through experiments and modelling
The minimum fluidization velocity is an important measure used in the design and scale-up of fluidized beds. Due to its importance, a large number of experiments over a wide range of operating conditions have focused on this property. Despite this attention, the amount of data where the combined effect of elevated temperature and pressure on the minimum fluidization velocity was investigated is still limited.
In this study the minimum fluidization velocity is determined experimentally in a lab-scale fluidized bed reactor designed for use at elevated temperature and pressure. A central composite design (CCD) is used to design experiments where different operating parameters are varied over a wide range. This includes different particle sizes, pressures up to 5bar and temperatures up to 550°C. The collected data provides the basis for existing correlations, such as that given by Bi and Grace (1), to be evaluated at elevated temperature and pressure and allows for detecting any systematic deviations from the experimental data.
In addition to the experiments, the minimum fluidization velocity and the voidage at minimum fluidization is calculated numerically over the CCD using computational. Several different drag models are evaluated, allowing their relative performances to be assessed and any weaknesses to be identified. Recommendations are made for drag model selection in pressurized fluidized bed reactors.
1. H.T. Bi and J.R. Grace. Flow regime diagrams for gas-solid fluidization and upward transport. Int. J. Multiphase Flow, 21: 1229-1236, 1995.
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