Catalytic reaction in a circulating fluidized bed downer: Ozone decomposition

Catalytic ozone decomposition reaction was used to study the performance of a 76 mm i.d. and 5.8 m high gas–solid circulating fluidized bed (CFB) downer reactor. Optical fiber probes and an ultraviolet (UV) ozone analyzer were used to obtain comprehensive information about local solids holdup and ozone concentration profiles at different axial and radial positions at superficial gas velocity of 2–5 m/s and solids circulation rates of 50 and 100 kg/m² s. Axial ozone concentration profiles significantly deviated from the plug-flow behavior, with most conversion occurring in the entrance region or flow developing zone of the downer reactor. Strong correlation was observed between the spatial distributions of solids and extent of reaction; higher local solids holdups cause lower ozone concentrations due to higher reaction rates. Radial gradients of the reactant (ozone) concentrations increased in the middle section of the downer, and decreased with increasing superficial gas velocity and solids circulation rate. Contact efficiency, a measure of the interaction between gas and solids indicated high efficiency in the flow developing zone and decreased with height in the fully developed region.     

Radial gas mixing characteristics in a downer reactor

In a downer reactor (0.1 m-I.D.x3.5 m-high), the effects of gas velocity (1.6-4.5 m/s), solids circulation rate (0–40kg/m²s) and particle size (84, 164 Μm) on the gas mixing coefficient have been determined. The radial dispersion coefficient(D _r ) decreases and the radial Peclet number (Pe_r) increases as gas velocity increases. At lower gas velocities, D_r in the bed of particles is lower than that of gas flow only, but the reverse trend is observed at higher gas velocities. Gas mixing in the reactor of smaller particle size varies significantly with gas velocity, whereas gas mixing varies smoothly in the reactor of larger particle size. At lower gas velocities, D_r increases with increasing solids circulation rate (G_s), however, D_r decreases with increasing G_s at higher gas velocities. Based on the obtained D_r values, the downer reactor is found to be a good gas-solids contacting reactor having good radial gas mixing.     

Developments in the understanding of gas–solid contact efficiency in the circulating fluidized bed riser reactor:A review

In the last several decades, circulating fluidized bed reactors have been studied in many aspects including hydrodynamics, heat and mass transfer and gas–solid two phase contacting. However, despite the abundance of review papers on hydrodynamics, there is no summary paper on gas–solid contact efficiency to date, especially on high density circulating fluidized beds(CFBs). This paper gives an introduction to, and a review of the measurement of contact efficiency in circulating fluidized bed riser. Firstly, the popular testing method of contact efficiency including the method of heating transfer experiment and hot model reaction are discussed, then previous published papers are reviewed based on the discussed methods. Some key results of the experimental work are described and discussed. Gas–solid contact efficiency is affected by the operating conditions as well as the particle size distribution. The result of the contact efficiency shows that the CFB riser is far away from an ideal plug flow reactor due to the characteristics of hydrodynamics in the riser. Lacunae in the available literature have been delineated and recommendations have been made for further work.     

Modeling the hydrodynamics in a coupled high-density downer-to-riser reactor

A coupled high-density downer-to-riser (DtoR) reactor is proposed for the controlled reaction pathway in the fluid catalytic cracking (FCC) process with the desired products distribution, e.g., clean gasoline with less olefin content. Hydrodynamics in such a reactor coupling system is studied using a compressive model that considers the pressure balances around all the sub-units in the prototype. The continuity closure condition is used to determine the material balance of the solid particles flowing in the circulating fluidized bed system. The model predictions have good agreement with the experimental data in rather wide operating conditions, e.g., when the solids circulation rate goes to more than 400 kg/m² s. The effects of the solids inventory, the superficial gas velocity, the particle diameter and density, the inside diameter of risers, and the fractional opening of the control valve for the solids flow on the operation of the DtoR system, are investigated and discussed in detail. It is demonstrated that the model offers appropriate guidance for the design and the operation of the coupled circulating fluidized bed system.     

Bed-to-wall heat transfer in a downer reactor

The effects of superficial gas velocity (0.5 to 4.5 m/s), solid circulating rate (0 to 40 kg/m²·s), suspension density (0 to 19 kg/m³) and particle sizes (83, 103, 163, 236 μm) on the bed-to-wall heat transfer coefficient have been determined in a downer reactor (0.1 m I. D. × 3.5 m high). Bed-to-wall heat transfer coefficient increases with increasing suspension density. The heat transfer coefficient by gas convection played a significant role, especially at lower solid circulation rates or suspension densities and larger particle sizes. At a given particle suspension density in the downer reactor, the heat transfer coefficient increases with decreasing particle size. A model is proposed to predict the bed-to-wall heat transfer coefficient in a downer reactor.     

Modeling of the hydrodynamics of the fully developed region in a downer reactor

A mathematical model is developed to describe the hydrodynamics of the fully developed region in a downer reactor. The model is based on the energy-minimization and multi-scale (EMMS) principle. The influence of the friction coefficient, the solid flow rate and the superficial gas velocity on the flow pattern in the downer is simulated. The local solid concentration and gas/solid velocities are predicted. The model results show a good agreement with experimental data in literatures. In addition, cluster size and local slip velocity are discussed.     

A multiscale mass transfer model for gas-solid riser flows: Part II—Sub-grid simulation of ozone decomposition

This article is to test the EMMS-based multiscale mass transfer model through computational fluid dynamics (CFD) simulation of ozone decomposition in a circulating fluidized bed (CFB) reactor. Three modeling approaches, namely types A, B and C, are classified according to their drag coefficient closure and mass transfer equations. Simulation results show that the routine approach (type C) with assumption of homogeneous flow and concentration overestimates the ozone conversion rate, introduction of structure-dependent drag force will improve the model prediction (type B), while the best fit to experimental data is obtained by the multiscale mass transfer approach (type A), which takes into account the sub-grid heterogeneity of both flow and concentration. In general, multiscale behavior of mass transfer is more distinct especially for the dense riser flow. The fair agreement between our new model with literature data suggests a fresh paradigm for the CFB related reaction simulation.     

Hydrodynamics and reactor performance evaluation of a high flux gas‐solids circulating fluidized bed downer: Experimental study

Reactor performance of a high flux circulating fluidized bed (CFB) downer is studied under superficial gas velocities of 3–7 m/s with solids circulation rate up to 300 kg/m²s using ozone decomposition reaction. Results show that the reactant conversion in the downer is closely related to the hydrodynamics, with solids holdup being the most influential parameter on ozone decomposition. High degree of conversion is achieved at the downer entrance region due to strong gas‐solids interaction as well as higher solids holdup and reactant concentration. Ozone conversion increases with the increase of solids circulation rate and/or the decrease of superficial gas velocity. Overall conversion in the CFB downer is less than but very close to that in an ideal plug flow reactor indicating a good reactor performance in the downer because of the nearly “ideal” hydrodynamics in downer reactors. © 2014 American Institute of Chemical Engineers AIChE J, 60: 3412–3423, 2014     

Fluidization Characteristics of Circulating Fluidized Bed Boilers

The fluidization in the furnace of circulating fluidized bed (CFB) boilers is described. Data have been obtained from a 12 MW_th CFB boiler and from literature. The bottom bed is bubbling rather than fast or turbulently fluidized as is often assumed. There is an extended splash zone above this bed, in which particles are thrown up by the bubbles and fall back onto the bottom bed. Other particles are carried further into the transport zone, initially as a saturated gas flow, but some particles move into the wall layers and the density decays towards the exit. The density of the transport zone is low, and the circulation rate is relatively seen small. Therefore, this flow is in a state of dilute-phase transport and not in the fast fluidization regime, such as is often claimed.     

Flow behaviors in the downer of a large-scale triple-bed combined circulating fluidized bed system with high solids mass fluxes

The flow behaviors in the downer of a large-scale triple-bed circulating fluidized bed (TBCFB) gasifier cold model, which is composed of a downer (Φ 0.1 m×6.5 m), a bubbling fluidized bed (BFB, 0.75×0.27×3.4 m³), a riser (Φ 0.1 m×16.6 m) and a gas-sealing bed (GSB, Φ 0.158 m×5 m), were investigated. Sand particles with a density of 2600 kg/m³ and an average particle size of 128 μm were used as bed materials. Solids mass fluxes were in the range 113–524 kg/m² s. Average solids holdup in the developed region of the downer increased with increasing solids mass flux. The gas seal between the riser and the downer had a large effect on the solids holdup distribution in the downer. Compared with the solids holdup in the riser, a relatively low solids holdup was formed in the downer even at high solids loadings. A pressure balance model was set up to predict the solids mass flux for this TBCFB system. It was found that the static bed height in the GSB had a great effect on the solids mass flux. The possibilities of achieving a high density solids holdup in a downer were discussed.     

MULTI-SCALE MASS TRANSFER MODEL FOR GAS-SOLID TWO-PHASE FLOW

This article is devoted to analyzing the mass transfer in heterogeneous gas-solid flow by means of structure and process decomposition. A multi-scale mass transfer model was developed on the basis of the hydrodynamics calculated from the so-called EMMS model. This resulted in the predictions of the steady-state two-dimensional concentration distributions of sublimated substance as well as total mass transfer coefficient for circular concurrent gas-solid contactors. The predictions were validated by experimentally measured (via an on-line HP GC-MS system) axial concentration distributions of sublimated naphthalene in air in a circulating fluidized bed riser 3.0 m in height and 72 mm in diameter. The experiment also obtained mass transfer coefficients comparable to theoretical predictions under conditions with various gas velocities, solid circulation rates, particle sizes, and active material fractions in the particles. Both the theoretical and experimental results demonstrated that the heterogeneous flow structure prevailing in the concurrent gas-solid flow greatly influenced the flow's mass transfer.     

MULTI-SCALE MASS TRANSFER MODEL FOR GAS-SOLID TWO-PHASE FLOW

This article is devoted to analyzing the mass transfer in heterogeneous gas-solid flow by means of structure and process decomposition. A multi-scale mass transfer model was developed on the basis of the hydrodynamics calculated from the so-called EMMS model. This resulted in the predictions of the steady-state two-dimensional concentration distributions of sublimated substance as well as total mass transfer coefficient for circular concurrent gas-solid contactors. The predictions were validated by experimentally measured (via an on-line HP GC-MS system) axial concentration distributions of sublimated naphthalene in air in a circulating fluidized bed riser 3.0 m in height and 72 mm in diameter. The experiment also obtained mass transfer coefficients comparable to theoretical predictions under conditions with various gas velocities, solid circulation rates, particle sizes, and active material fractions in the particles. Both the theoretical and experimental results demonstrated that the heterogeneous flow structure prevailing in the concurrent gas-solid flow greatly influenced the flow's mass transfer.     

A multiscale mass transfer model for gas-solid riser flows: Part 1 — Sub-grid model and simple tests

The gas-solid mass transfer in circulating fluidized bed (CFB) riser flow is both structure-dependent and dynamic in nature. Recent progress in multiscale computational fluid dynamics (CFD) allows fresh insight into the dynamic flow structure, yet its influence on the mass transfer remains to be settled. To this end, a multiscale mass transfer model is established in this paper based on the extended framework of the energy-minimization multiscale (EMMS) model. The relevant algorithm named EMMS/mass is proposed for CFD-coupled mass transfer computation. Two testing cases accounting for sublimation of naphthalene and decomposition of ozone, respectively, are presented to demonstrate the characters of the model. It is shown that structural consideration can have significant effects on the model prediction. The normally used Reynolds number is not adequate to characterize these effects, while the combination of gas velocity and solids flux seems to capture the structural effects and allows to explain the variation of Sherwood number reported for CFB risers in the literature. Sub-grid coupling of this multiscale mass transfer model and CFD approach can be expected to provide a promising tool to probe the dynamic and structure-dependent nature of mass transfer in CFB risers.     

臭氧催化分解的研究

研究了多种单组分和双组分金属氧化物对臭氧催化分解的活性,单组分时催化分解活性次序为：Co＞Mn≈Ni＞Cr＞Fe＞Zn＞Mg＞Cu＞Ag＞Sn ＞Pb＞U＞Cd＞Al＞Si≈Bi≈Ce≈CaCO₃≈La＞Na。实验结果表明,几种双组分金属氧化物的催化分解活性主要由较高活性的金属氧化物所决定,并与两组分的比例有关。实验还表明,催化剂的催化分解活性与制备催化剂时的灼烧温度和时间有关,催化剂前驱体采用硝酸盐时比较合理的灼烧条件为：500 ℃,4 h。     

Hydrodynamic modeling of a circulating fluidized bed

Hydrodynamics plays a crucial role in defining the performance of circulating fluidized beds (CFB). The numerical simulation of CFBs is very important in the prediction of its flow behavior. From this point of view, in the present study a dynamic two dimensional model is developed considering the hydrodynamic behavior of CFB. In the modeling, the CFB riser is analyzed in two regions: The bottom zone in turbulent fluidization regime is modeled in detail as two-phase flow which is subdivided into a solid-free bubble phase and a solid-laden emulsion phase. In the upper zone core-annulus solids flow structure is established. Simulation model takes into account the axial and radial distribution of voidage, velocity and pressure drop for gas and solid phase, and solids volume fraction and particle size distribution for solid phase. The model results are compared with and validated against atmospheric cold bed CFB units' experimental data given in the literature for axial and radial distribution of void fraction, solids volume fraction and particle velocity, total pressure drop along the bed height and radial solids flux. Ranges of experimental data used in comparisons are as follows: bed diameter from 0.05-0.418 m, bed height from 5-18 m, mean particle diameter from 67-520 μm, particle density from 1398 to 2620 kg/m³, mass fluxes from 21.3 to 300 kg/m²s and gas superficial velocities from 2.52-9.1 m/s.As a result of sensitivity analysis, the variation in mean particle diameter and superficial velocity, does affect the pressure especially in the core region and it does not affect considerably the pressure in the annulus region. Radial pressure profile is getting flatter in the core region as the mean particle diameter increases. Similar results can be obtained for lower superficial velocities. It has also been found that the contribution to the total pressure drop by gas and solids friction components is negligibly small when compared to the acceleration and solids hydrodynamic head components. At the bottom of the riser, in the core region the acceleration component of the pressure drop in total pressure drop changes from 0.65% to 0.28% from the riser center to the core-annulus interface, respectively; within the annulus region the acceleration component in total pressure drop changes from 0.22% to 0.11% radially from the core-annulus interface to the riser wall. On the other hand, the acceleration component weakens as it moves upwards in the riser decreasing to 1% in both regions at the top of the riser which is an important indicator of the fact that hydrodynamic head of solids is the most important factor in the total pressure drop.     

Designing of primary air nozzles for large-scale CFB boilers in a combined numerical-experimental approach

The article presents a numerical-experimental approach for designing the primary air nozzles working with a large-scale Circulating Fluidized Bed (CFB) boiler. An analysis of the criteria that must be satisfied by CFB air grids has been made and it has been demonstrated that the existing correlations which are used in designing air grids are not possible to be utilized for determining the optimal nozzle design. On the example of a prototype nozzle design, based on the proposed design algorithm, the results of both numerical simulations and laboratory tests, whose aim was to determine the optimal geometry of a nozzle operating with a 235 MW_e asymmetric-design CFB boiler, are presented.     

Kinetic theory based computation of PSRI riser: Part II—Computation of mass transfer coefficient with chemical reaction

The design of circulating fluidized bed systems requires the knowledge of mass transfer coefficients or Sherwood numbers. A literature review shows that these parameters in fluidized beds differ up to seven orders of magnitude.To understand the phenomena, a kinetic theory based computation was used to simulate the PSRI challenge problem I data for flow of FCC particles in a riser, with an addition of an ozone decomposition reaction. The mass transfer coefficients and the Sherwood numbers were computed using the concept of additive resistances. The Sherwood number is of the order of 4 × 10⁻³ and the mass transfer coefficient is of the order of 2 × 10⁻³ m/s, in agreement with the measured data for fluidization of small particles and the estimated values from the particle cluster diameter in part one of this paper. The Sherwood number is high near the inlet section, then decreases to a constant value with the height of the riser. The Sherwood number also varies slightly with the reaction rate constant. The conventionally computed Sherwood number measures the radial distribution of concentration caused by the fluidized bed hydrodynamics, not the diffusional resistance between the bulk and the particle surface concentration. Hence, the extremely low literature Sherwood numbers for fluidization of fine particles do not necessarily imply very poor mass transfer.     

Fundamental studies on the hydrodynamics and mixing of gas and solid in a downer reactor

The effect of flow direction on hydrodynamics and mixing in the upflow and downflowcirculating fluidized beds is discussed in details.Similar profiles of gas and solids velocities andsolids concentration are found in both risers and downers.When the flow is in the direction ofgravity(downer),the radial profiles of gas and particle velocity are more uniform than that inthe riser,the solids mixing is very small and the flow pattern approaches plug flow,while theflow is against gravity(riser),the solids backmixing significantly increase and the flow pattern isfar from plug flow.Among many of factors the flow direction has the largest influence onhydrodynamics and axial mixing of gas and solids.     

Mass transfer in the core-annular and fast fluidization flow regimes of a CFB

In gas-solid reactors, particularly circulating fluidized beds (CFB) it is becoming increasingly more important to be able to predict the conversion and yield of reactant species given the ever rising cost of the reactants and the ever decreasing acceptable level of effluent contaminants. As such, the development and use of predictive models for the reactors is necessary for most processes today. These models all take into account, in some manner, the interphase mass transfer. The model developer, unless equipped with specific experimentally based empirical correlations for the reactor system under consideration, is required to go to the open literature to obtain correlations for the mass transfer coefficient between the solid and gas phases. This is a difficult task at present, since these literature values differ by up to 7 orders of magnitude. The wide variation in the prediction of mass transfer coefficients in the existing literature is credited to flow regime differences that can be identified in the cited literature upon careful inspection.A new theory is developed herein that takes into account the local hydrodynamics. The resulting model is compared with data generated in the NETL cold flow test facility and with values from the literature. The new theory and the experimental data agree quite well, providing a fundamentally based mass transfer model for predictive reactor simulation codes.     

Computation of the mass transfer coefficient of FCC particles in a thin bubbling fluidized bed using two- and three-dimensional CFD simulations

In this study, the standard kinetic theory based model with a modified drag correlation was successfully used to compute the mass transfer coefficients and the Sherwood numbers of FCC particles in a thin bubbling fluidized bed column using the additive diffusional and chemical reaction resistances concept. Also, the effects of the computational domain (two- or three-dimensional) and the reaction rate constant (low and high) are discussed.The computations show that the Sherwood numbers are in agreement with the measurement ranges for small particles in the fluidized bed system. The mass transfer coefficients and the Sherwood numbers are high near the inlet section, and decrease to a constant value with increasing height in the column. The two-dimensional computational domain simulations provide enough information to explain the phenomena inside a symmetrical system, but three-dimensional computational domain simulations are still needed for asymmetrical systems. Finally, the mass transfer coefficients and the Sherwood numbers increased with the larger reaction rate constant.