Minerals Engineering 149 (2020) 106238

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Minerals Engineering
journal homepage: www.elsevier.com/locate/mineng

CFD modeling and simulation of gas-phase extraction processes in fluidized T

bed reactor
⁎
Le Xie, Jundong Zhu, Jiang Hu, Chongwen Jiang
College of Chemistry and Chemical Engineering, and Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese Resources, Central South University,
Changsha 410083, Hunan, China

A R T I C LE I N FO A B S T R A C T

Keywords: Recently, the gas-phase organic ligand extraction of metals from low-grade sources using the fluidized bed
Computational fluid dynamics (CFD) reactor (FBR) technique has garnered significant attention owing to its simplicity and advantages in reducing
Binary-mixture particles energy costs. In this study, a computational fluid dynamics (CFD) coupled model including a three-phase
Minerals processing Eulerian model, kinetic theory of granular flow model, and reaction kinetics model was proposed to investigate
Extractive reaction
gas-phase extraction processes encountered in an FBR. The developed three-phase CFD coupled model was first
Fluidized bed reactor (FBR)
validated by comparing the obtained simulation results with the experimental data of cumulative iron extraction
at different reaction temperatures and the classical calculated data of the pressure drop. Subsequently, the effects
of the inlet gas velocity and particle phase holdup on the extraction were studied. Accordingly, both particle
fluidization behaviors and extractive reaction kinetics characteristics were obtained. The simulation results
indicated that the mentioned operating conditions significantly affected the distribution of particle phase holdup
and subsequently influenced the cumulative iron yield through an extractive reaction. Furthermore, the de-
veloped CFD coupled model is beneficial for optimizing gas-phase extractive reaction process in FBRs.

1. Introduction
A large number of slags serving as by-products in metallurgy pro-
cesses are produced annually worldwide (Liu et al., 2016; Piatak et al.,
2015; Sarfo et al., 2017; Shen and Forssberg, 2003). In general, these
slags should be handled with the utmost care because they contain
harmful or heavy metals that can cause environmental problems. Fur-
thermore, most slags that contain variable amounts of valuable metals
are in fact a secondary resource of metals. Therefore, it is crucial to
recover metals from these low-grade sources to recycle and reuse re-
sources, as well as for environmental protection (Piatak et al., 2015;
Shen and Forssberg, 2003).
In the last several decades, many types of conventional technolo-
gies, such as hydrometallurgy (Arslan and Arslan, 2002; Banza et al.,
2002; Petersen, 2016), pyrometallurgy (Gyurov et al., 2011; Sarfo et al.,
2017; Ye et al., 2003; Zhang et al., 2007), and bioleaching (Akcil et al.,
2007; Carranza et al., 2009; Potysz et al., 2018), have been proposed to
recover metals from slags. Such studies have confirmed that a higher
metal recovery rate can be realized, and the resulting data are useful for
the optimization of the recovery process. In addition, gas-phase ex-
traction has emerged as a powerful technique, and it is employed to
recover metals from their oxides. Volatile organic compounds serve as
extractants that pass through a heated feed material and react selec-
tively with metal oxides (Allimann-Lecourt and Bailey, 2002; Dyk et al.,
2010; Potgieter et al., 2006). Some experimental studies have been
performed on the effect of extractants on extraction efficiency
(Allimann-Lecourt and Bailey, 2002; Sun and Waters, 2014) and gas-
phase extraction reaction kinetics behaviors (Dyk et al., 2010; Potgieter
et al., 2006). Many detailed experimental investigations of the gas-
phase extraction of metals from oxides have been reported.
Generally, gas-phase extraction reactions are performed in fluidized
bed reactors (FBRs) owing to their excellent mass and heat transfer
performance. For gas-phase extraction in an FBR, oxide particles typi-
cally coexist with sand particles. When the gas velocity is higher than
the minimum fluidization velocity, the particle mixture starts to flow
(fluidization). Clearly, a gas-phase extraction system is a typical binary-
mixture particle system (gas–solid-solid three-phase) in which the
particle–particle mixing quality is critical in determining the gas-phase
extraction reaction rate. Therefore, it is crucial to comprehensively
understand the relationship between fluid flow and extraction reactions
to optimize this process, which is characterized by multiphase flow and
multiscale characteristics. As a supplement, computational fluid dy-
namics (CFD) simulations can provide flow field information that can
explain the experimental observations. Additionally, both the evolution

⁎
Corresponding author.
E-mail address: jcwcsu@csu.edu.cn (C. Jiang).

https://doi.org/10.1016/j.mineng.2020.106238
Received 3 June 2019; Received in revised form 20 January 2020; Accepted 30 January 2020
Available online 07 February 2020
0892-6875/ © 2020 Elsevier Ltd. All rights reserved.
L. Xie, et al.
Nomenclature
CD Drag coefficient, (-)
Cfr Friction coefficient, (-)
d Diameter of particles (m)
D Diffusion coefficient (m2 s−1)
e Restitution coefficient, (-)
F Interphase force (N m-3)
g Gravitational acceleration (m s−2)
g0 Radial distribution function, (-)
h Specific enthalpy, (kJ kg−1 K−1)
I Unit tensor, (-)
k reaction rate constant (s−1)
kΘ KTGF model parameter, (-)
mi Gas-solid drag model parameter, (-)
msp Interphase mass transfer, (kg m−3 s−1)
ni Gas-solid drag model parameter, (-)
Nc Courant number, (-)
p Pressure, (Pa)
Re Reynolds number, (-)
Si The source term of species i (kg m−3 s−1)
of fluidization and the gas-phase extraction reaction in an FBR can be
visualized by a CFD simulation.
Gas–solid hydrodynamic characteristics in FBRs can be numerically
investigated by many multiphase models, which include the multi fluid
model (MFM), dense discrete particle model (DDPM) and CFD-discrete
element model (CFD-DEM). A deep understanding of the advantages
and disadvantages of these models is inherently required for reliable
simulation results. In recent years, a considerable effort has been de-
voted to evaluating these different FBR modeling approaches (Chen and
Wang, 2014; Le Lee and Lim, 2017; Nikolopoulos et al., 2017;
Ostermeier et al., 2019a; 2019b; 2019c; Stroh et al., 2018; Wang et al.,
2013). The MFM and DDPM approaches require fewer computing re-
sources and have the potential for industrial applications. The CFD-
DEM approach can give more details about flow patterns. However, the
as-mentioned studies focused on gas–solid two-phase flow instead of
binary-mixture particle systems, which have received extensive atten-
tion in recent years (Benyahia, 2008; Chao et al., 2011; Das et al., 2008;
Jia et al., 2012; Mathiesen et al., 2000). Based on the kinetic theory of
granular flow (KTGF), Lu’s group proposed some constitutive relations
to calculate particle phase viscosity (Lu et al., 2000; 2001). The avail-
ability and suitability of the developed models were validated by ex-
perimental data from a riser (Lu and Gidaspow, 2003) and a bubbling
fluidized bed (Sun et al., 2005). In addition, other CFD simulations
focused on investigating the effects of numerical methods (i.e., DEM
and the Eulerian approach) (Cheng et al., 2014; Jalali and Hyppänen,
2010) and gas–solid/solid–solid interactions (Rong et al., 2014; Zhang
et al., 2017; Zhou and Wang, 2015) on the fluidization behaviors of
binary-mixture particles. These simulation results presented a com-
prehensive description of the distribution of solid particles in an FBR.
More recently, CFD models have been developed and employed to in-
vestigate the flotation process (Wang et al., 2018), including predicting
the flotation rate constant (Karimi et al., 2014a; 2014b) and de-
termining the gas dispersion characteristics and particle–bubble inter-
actions in flotation cells (Basavarajappa and Miskovic, 2016;
Hassanzadeh et al., 2018). The above studies provided a comprehensive
investigation of the fluidization behaviors of gas–solid binary-mixture
particles in FBRs. However, the relationship between the particle flui-
dization and the gas–solid reaction is still unclear because chemical
reactions are mostly ignored. In particular, the literature pertaining to
the gas-phase extraction of metals from oxides in FBR based on CFD
techniques is limited.
In this study, a CFD-KTGF model coupled with a reaction kinetics
2
Minerals Engineering 149 (2020) 106238
t Time, (s)
T Temperature, (K)
U Slip velocity, (m s−1)
v Velocity, (m s−1)
w Mass fraction (-)
y Yield (-)
Greek letters
α Volume fraction, (-)
ζ Inter-phase drag force coefficient, (kg m−3 s−1)
β Inter-phase drag force coefficient, (kg m−3 s−1)
γs Collisional dissipation energy, (kg m−1 s−3)
ρ Density, (kg m−3)
τ̄¯ Stress tensor, (Pa)
μ Viscosity, (Pa s)
Θ Granular temperature, (m2 s−2)
λ Solid bulk viscosity, (Pa s)
θ Angle of internal friction, (deg)
κ Thermal conductivity, (W m−1 K−1)
model was proposed for the first time to study the multiphase flow
reaction behaviors of the gas-phase extraction of iron from its oxide in
an FBR. The particle fluidization characteristics and gas-phase ex-
tractive reaction kinetics behaviors were investigated. The developed
model was validated by the experimental data of cumulative iron ex-
traction and the classical calculated data of pressure drops.
Subsequently, the CFD coupled model was employed to explore the
effect of inlet gas velocity and particle phase holdup. The hydro-
dynamic characteristics of the gas–solid-solid three-phase flow reaction
behaviors in an FBR were obtained.
2. Mathematical modeling and simulation details
To present a comprehensive description of the process of gas-phase
extraction in an FBR, a multiple model coupling approach is typically
required. In this study, the developed coupled model is composed of a
three-fluid CFD model (gas phase, oxide particle phase, and sand par-
ticle phase), a KTGF model, and a gas-phase extraction reaction kinetics
model. As the three-fluid CFD and KTGF models are widely applied in
simulating binary-mixture particle systems, herein, they are summar-
ized in Table 1.
As shown, each phase (three phases in total) has a set of governing
equations, which include the continuity equation, momentum equation,
energy equation, and species equation. For the solid phase, the extra
KTGF model is required to calculate solid phase properties, such as solid
pressure, solid shear viscosity, and solid bulk viscosity. For the species
equation, there are two independent equations in the gas phase.
Additionally, the volume fraction of the oxide particles should be cal-
culated. The interphase mass transfer (msp) can be calculated based on
the gas phase or solid phase. In this study, obviously, the interphase
mass transfer rate from the oxide particle phase to the gas phase just
equals the consumption rate of Fe2O3 particles, and it is integrated into
the CFD model using user-defined functions.
It should be noted here that, for the interphase force, only the drag
force is included in the momentum equation, and the proposed CFD
coupled model may be only suitable for a laboratory scale FBR. When it
is extended to industrial scale reactors, the drag model must be replaced
by the filtered drag correlations recommended by Sundaresan's group
(Milioli et al., 2013; Igci and Sundaresan, 2011). Additionally, an ap-
parent extraction reaction kinetics model was used for simplicity.
Therefore, an accurate reaction kinetics model based on the reaction
mechanism is of great importance for improving the accuracy of
L. Xie, et al. Minerals Engineering 149 (2020) 106238

Table 1
Governing equations of the three-liquid binary-mixture particle system.
Models Equations

Continuity equation
+ ∇·(αq ρq→
∂
(α ρ ) vq) = msp, q = s or g
∂t q q
2
αs + αg = ∑i = 1 αsi + αg = 1
Momentum equation →→ → →
(α ρ → + ∇·(αq ρq v v ) = −αq ∇p − ∇·τ¯q − msp v − F + αq ρq→
∂
v) g
∂t q q q q q q
→
τ¯g = αg μg [∇→
vg + (∇→
vg )T ] − αg μg ∇→
2
vg I
3
→
τ¯si = αsi μsi [∇→
vsi + (∇→
vsi )T ] + (λ si − μsi ) αsi ∇→
2
vsi I
3
Energy equation ∂ ∂pq →
(α ρ h ) + ∇·(αq ρq vq hq) = −αq + τ¯q: ∇ v − ∇·qq
∂t q q q ∂t q
n
+ ∑p = 1 (msp hsp − mps hps ), qq = −αq κ q ∇Tq
Species equation ∂
(α ρ w ) + ∇·(αq ρq vq wi ) = ∇·(Di ∇ (ρq wi )) + Si
∂t q q i
Granular temperature equation
[ (ρ α Θ ) + ∇·(ρsi αsi → ∇→
3 ∂
vsi Θsi )] = (−psi I¯ + τ¯si ): vsi + ∇·(k Θsi ∇Θsi )
2 ∂t si si si
− γΘsi − 3(βg − si + ζs, ij )Θsi
150ρsi dsi Θsi π 6 Θsi
k Θsi = [1 + αsi g0, ij (1 + es, ij )]2 + 2αsi2 ρsi dsi g0, ij (1 + es, ij )
384(1 + es, ij ) g0, ij 5 π
12(1 − es2, ij ) g0, ij
γΘs = ρsi αsi2 Θ1.5
si
dsi π
Solid pressure 2 dsi + dsj
Psi = αsi ρsi Θsi + 2αsi ρsi Θsi ∑ j = 1 [ ]3 (1 + es, ij ) g0, ij αsj
2dsi
gsi dsi + gsj dsj αs 3 2 α sj
g0, ij = , gsi = [1 − ( )1/3]−1 + dsi ∑ j = 1
dsi + dsj α s,max 2 dsj
α si,max
if mi ⩽
α si,max + (1 − α si,max ) α sj,max

dsj
αs,max = [αsi,max − αsj,max + (1 − )(1 − αsi,max ) αsj,max ]
dsi
mi
× [αsi,max + (1 − αsi,max ) αsj,max ] + αsj,max
α si,max
Packing limit dsj
else αs,max = (1 − )[αsi,max + (1 − αsi,max ) αsj,max ](1 − mi) + αsi,max
dsi
Solid bulk viscosity 4 Θsi
λ si = α ρ d g (1 + es, ij )
3 si si si 0, ij π
μsi = μsi, col + μsi, kin + μsi, fr
4 Θsi 0.5
μsi, col = αsi ρsi dsi go, ij (1 + es, ij )( )
5 π
α si dsi ρsi Θsi π 2
μs, kin = [1 + (1 + es, ij )(3es, ij − 1) αsi g0, ij ]
6(3 − es, ij ) 5
Solid shear viscosity psi sin θsi
μsi, fr = .
2 I
→
F = βg − si (→
vsi − →
Re −f (Re, αg )
vg ), βd = C α
24 d0 g
βg − si 0.5αg
= + 0.5(1 − αg ) ni2 + 0.5ni
βd ∑i2= 1 (mi / ni2)

f (Re,αg ) = 2.65(1 + αg ) − (5.3 − 3.5αg ) αg2 exp[−0.5(1.5 − log Re)2]

Gas-solid drag force model (Rong et al., 2014) αg ρg < d > Uslip 2 α si
Re = , < d > = [ ∑i = 1 (mi / di )]−1 , ni = di/ < d > , mi =
μg αs

Solid-solid drag force model (Syamlal, 1987) π π2

3(1 + es, ij )( + Cfr , ij ) α si ρsi α sj ρsj (dsi + dsj )2g0, ij
ζs, ij = 2 8
3 + ρ d3 ) |→
vsi − →
vsj|
2π (ρsi dsi sj sj

predictions. − ln(1 − y ) = kt (1)

2.1. Reaction kinetics model
At high temperatures, iron(III) oxide (Fe2O3) reacts readily with
acetylacetone; the stoichiometric equation is described as follows:
Fe2 O3 (s ) + 6H(C5 H7 O2) (g ) = 2Fe(C5 H7 O2)3 (g ) + 3H2 O (g )
This gas–solid reaction can be characterized by a noncatalytic
shrinking particle model, and no product layer is formed because the
products are gasified briefly under high-temperature conditions. In
general, the gas-phase extraction rate is determined by a chemical re-
action, mass transport, or both. Van Dyk et al. (2010) investigated the
effect of temperature, metal oxide concentration, and ligand flow rate
on extraction; they concluded that the gas-phase extraction reaction
obeys first-order kinetics the best. For an irreversible first-order reac-
tion, the following well-known equation can be used:
where y is the extraction rate of metallic Fe, and k is the reaction rate
constant which is a function of temperature. In this study, the reported
experimental data were employed to determine the apparent reaction
rate constant based on the least-squares method.
As shown in Fig. 1, high correlation coefficients (> 0.92) for the
extraction reactions were obtained when the experimental data were
fitted to a first-order rate equation. The slope of the line is the reaction
rate constant that is employed to determine the apparent activation
energy. The linear fitting results are shown in Fig. 2. The apparent
activation energy is 62.91 kJ/mol. It is worth noting that the apparent
reaction rate constant is dependent on the initial Fe2O3 charge (see
Fig. 1B). In this study, the determined reaction kinetics model should be
integrated into a CFD model to describe the reaction kinetics char-
acteristics.

3
L. Xie, et al.
Fig. 1. Results of the linear regression for cumulative iron extraction and reaction time under different operating conditions: (A) reaction temperature; (B) Fe2O3
charge.
Fig. 2. Results of the linear regression for apparent reaction rate constant and
reaction temperature.
2.2. Model coupling mechanism
Fig. 3 displays the coupling scheme of the proposed submodels. At
the beginning of the simulation, the velocity, pressure, phase holdup,
temperature, and species mass fraction in the FBR are initialized. The
KTGF model is solved to obtain the solid phase pressure and viscosity.
The gas–solid drag force is calculated based on the Rong model (Rong
et al., 2014) recommended by Zhang et al. (2017). Subsequently,
continuity and momentum equations can be solved to obtain the ve-
locity field information in each cell. Next, the temperature and species
mass fraction are transferred into the reaction kinetics model to cal-
culate the reaction rate, including the consumption rate of reactants
and the formation rate of products, which are the source terms of the
species transport equations. Additionally, these source terms should be
transferred into the CFD three-phase flow model (interphase mass
transfer). Subsequently, the species mass fraction distributions are up-
dated by solving these models. In this study, the coupled drag force
model and reaction kinetics model were written in C and were in-
tegrated into a CFD model using user-defined functions. The above
mentioned iterative process was performed repeatedly until a specific
criterion of physical time was satisfied. For more details about the
model coupling mechanism, please refer to Fig. 3.
4
Minerals Engineering 149 (2020) 106238
2.3. Simulation details
All simulations were performed in a two-dimensional (2D) FBR with
a diameter of 15 mm and a height of 500 mm. Acetylacetone was one of
the reactants and also served as a fluidizing agent. A sand particle has
an average size of approximately 64 μm, which is similar to that of an
Fe2O3 particle. However, these two particles are different in density
and, thus, are considered as two different solid phases. The two solid
phases had a total mass of 50 g, and the initial volume fraction of the
solid phase was 0.6. Therefore, when the Fe2O3 charge was 1 wt%, the
initial bed height was 0.2128 m. It should be noted that the volume
fraction of the solid phase was very low in this study. Therefore, we did
not evaluate the effect of frictional force on the mixing of solid parti-
cles. A constant solid–solid friction coefficient (Cfr =0.15) and a default
frictional viscosity model (Schaeffer model) were used in the CFD si-
mulation. The detailed settings, initial and boundary conditions and
model parameters are listed in Table 2.
The FBR was created and meshed by structured quadrilateral cells
using the commercial software GAMBIT 2.3.16 (Ansys Inc.). The cell
size was 0.0005 m. Consequently, 30,000 cells were selected for all the
CFD simulations. For binary-mixture particle systems, Coroneo et al.
(2011) recommended that a reasonable Courant number (Nc ) (see Eq.
(2)) should be in the range of 0.028–0.15. In this study, the gas velo-
city was 0.01–0.06 m/s, and the time step was 0.001 s. Therefore, the
Courant number was 0.02–0.12.
Δt
Nc = vg
Δcell (2)
In addition, the developed 2D CFD coupled model was solved by the
commercial code FLUENT (Ansys Inc.). The governing equations were
discretized by the QUICK scheme and solved under unsteady condi-
tions. The pressure-based solver with an absolute velocity formulation
was used. The gradient was computed by a Least Squares Cell Based
scheme. The pressure–velocity coupling was realized by the SIMPLE
scheme. In this study, the fixed time stepping method was used
(Δt = 0.001 s), and the convergence criterion was set at 1 × 10−6. All
CFD simulations were executed on a 2.2-GHz Intel 2 Central Processing
Unit (16 cores) with a 128 GB RAM. When the CFD Euler model, the
KTGF model, and reaction kinetics model were solved together, about
two weeks were needed to simulate the physical time of 120 min.
L. Xie, et al. Minerals Engineering 149 (2020) 106238

Fig. 3. Solution procedure for the CFD coupled model.

Table 2
Boundary conditions and model parameters.
Descriptions Values

Inlet boundary condition Velocity inlet

Outlet boundary condition Pressure outlet
Wall boundary condition No slip; constant temperature
Initial bed height 0.2016–0.2128 m
Initial volume fraction of solid phase 0.6
Reaction temperature 463–523 K
Inlet gas velocity 0.01–0.06 m/s
Solid-solid friction coefficient 0.15
Column diameter 15 mm
Column height 500 mm
Cell size 0. 5 mm
Convergence criteria 1 × 10−6
Time step 0.001 s

Fig. 5. Comparisons between simulation results (CFD) and experimental data

(Exp.) for the pressure drop.

3. Results and discussion

3.1. Model validation

3.1.1. Kinetics model validation

Fig. 4. Comparisons between simulation results (CFD) and experimental data
(Exp.) for cumulative iron extraction under four different reaction tempera-
tures.
To study the effect of reaction temperature on the gas-phase ex-
traction reaction kinetics behavior, experiments have been performed
in a FBR by Van Dyk et al. (2010). The experimental conditions used
were as follows: acetylacetone flow rate = 1 ml/min, Fe2O3
charge = 1 wt% (total mass of binary-mixture particles = 50 g), and
T = 190, 210, 230, 250 °C. In this study, CFD simulations were per-
formed under identical operating conditions and FBR structure para-
meters to compare the simulation results with the experimental data in
terms of cumulative iron extraction. It is worth noting that the inlet gas
velocity was determined by the ideal gas state equation. Fig. 4 displays
the predicted cumulative iron extraction profile along with the reaction
time.
From Fig. 4, the cumulative iron extraction is highly dependent on

5
L. Xie, et al.
Fig. 6. Time evolution of the volume fraction of the solid phase at the inlet gas
velocity of 0.035 m/s.
the reaction temperature. With an increase in reaction temperature
from 463 K to 523 K, the cumulative iron extraction increases from 12%
to 65% after 120 min. Therefore, FBR technology has similar ad-
vantages as other technologies when it comes to process efficiency.
Generally, advantages and disadvantages coexist for FBR technology.
Although FBR has excellent mass and heat transfer performance and is
convenient in operation, the solid phase has a considerable range of
residence time distribution, leading to polydispersed product distribu-
tion and low production yield; the operating air velocity should be
chosen carefully to ensure stable fluidization. Furthermore, complex
fluid mechanics and transport phenomena hinder the optimized design
and scale-up of FBRs. Therefore, it is of great importance to perform a
comprehensive investigation of the gas-phase extraction processes in
FBRs based on CFD technology.
Additionally, the simulation results revealed the same trend as the
experimental data. Potgieter et al. (2006) concluded that the gas-phase
extraction reaction corresponded to a first-order reaction, which was
derived based on the hypothesis that perfect mixing occurs. In this
study, a first-order reaction kinetics model was integrated into a CFD
model to describe the transport/dynamics of bubbles, particle fluidi-
zation, and reaction kinetics behaviors. In the CFD simulation, how-
ever, the distribution of Fe2O3 particles is instantaneous. As a result, the
distribution of the extraction rate changes spatially and temporally as
the reaction progresses. These differences are finally reflected in the
cumulative iron extraction. Therefore, an accurate reaction kinetics
model based on a reaction mechanism is inherently required to improve
the reliability of CFD simulation results.
3.1.2. Hydrodynamics characteristics validation
For binary-mixture particles in an FBR, bed pressure drop is an
important parameter in evaluating hydrodynamic performance.
Empirical equations are available to calculate the bed pressure drop
(Romeo et al., 2011; Singh et al., 2008):
ΔP = (1 − αg ) hmf (ρs − ρg ) g
(3)
In this study, the bed pressure drop calculated by the CFD model
6
Minerals Engineering 149 (2020) 106238
was compared with that obtained by an empirical equation (Eq. (3)) to
validate the proposed CFD coupled model. The comparison results are
shown in Fig. 5. Additionally, the time evolution of particle fluidization
is presented in Fig. 6. As shown, a steady fluidization can be developed
easily at the inlet gas velocity of 0.035 m/s. In a steady fluidization, the
bed height is ～0.321 m, and the calculated bed pressure drop is
2766 Pa. As shown in Fig. 5, the simulated results are in good agree-
ment with the calculated data, thus validating the CFD coupled model.
3.2. Model application
In this section, the effects of some key operating parameters (i.e.,
inlet gas velocity and particle phase holdup) on the particle fluidization
characteristics and reaction kinetics behaviors are investigated based
on the validated model.
3.2.1. Effects of the inlet gas velocity
The gas–solid drag force is an important interphase force de-
termining particle fluidization behaviors that can subsequently and
significantly affect the distributions of reaction rates and products.
Therefore, the inlet gas velocity should be addressed carefully ac-
cording to the established gas–solid drag force model (see Table 1). In
this section, the effect of the inlet gas velocity (0.01, 0.02, 0.04, and
0.06 m/s) on the results of the simulation cases is discussed. The time
evolutions of particle fluidization are obtained and shown in Fig. 7.
In general, with an increase in the inlet gas velocity, the particle bed
will pass through the fixed bed, critical fluidization, particulate ex-
pansion, bubbling fluidization, and fast fluidization, and so on. As
shown, the bed expansion height increases from 0.25 to 0.378 m with
an increase in inlet gas velocity from 0.01 to 0.06 m/s. From Fig. 7A
and 7B, when the inlet gas velocity is lower than 0.02 m/s, the particle
bed is in the state of particulate expansion, in which no bubbles are
formed and the particle bed is uniform. As the inlet gas velocity is in-
creased to 0.06 m/s, however, bubbling fluidization is observed (see
Fig. 7D). The bubble size increases gradually as it rises along the bed.
The fluidized bed reaches a steady fluidized state after ～4 s. For
binary-mixture particles, large and heavy particles tend to reside at the
bed bottom, while small and light particles are more easily con-
centrated on the bed surface (Zhou and Wang, 2015). In this study, the
oxide particles and sand particles are of a similar size but with different
densities. However, the segregation phenomenon of the binary-mixture
particles was not observed in this study. The extremely low levels of
oxide particles and the same size of oxide particles and sand particles
may be the possible reasons. Thus, a homogeneous mixing of the oxide
particle phase and sand particle phase was obtained.
Fig. 8 displays the time evolution of the bed expansion height. In the
particulate expansion state, the bed expansion height increases uni-
formly with flow time and finally stabilizes at a constant value. In the
bubbling fluidization state, the bed expansion height fluctuates owing
to the formation and movement of bubbles.
3.2.2. Effect of particle phase holdup
According to the developed CFD coupled model, particle phase
holdup is another important parameter determining the particle flui-
dization behaviors and reaction kinetics characteristics. In this section,
three Fe2O3 charges (i.e., 1%, 3%, and 10%) were selected from the
study by Van Dyk et al. (2010). For binary-mixture particle systems, it is
widely known that particle fluidization occurs with increased difficulty
with an increase in particle-phase holdup.
As shown in Fig. 9, when the Fe2O3 charge is 1%, the steady bed
expansion height is ～0.321 m. When the Fe2O3 charge increased to
10%, however, the steady bed expansion height was only 0.278 m. It is
noteworthy that the initial bed height cannot be ignored under different
Fe2O3 charges. The initial bed height declines by 0.011 m when the
Fe2O3 charge increases from 1% to 10%. The density of the oxide
particles is higher than that of the sand particles; thus, defluidization is
L. Xie, et al. Minerals Engineering 149 (2020) 106238

Fig. 7. Time evolutions of the volume fraction of the solid phase under different inlet gas velocities: (A) 0.01 m/s; (B) 0.02 m/s; (C) 0.04 m/s; and (D) 0.06 m/s.

Fig. 8. Time evolution of the bed expansion height under different inlet gas Fig. 9. Time evolution of the bed expansion height under three different Fe2O3
velocities. charges.

7
L. Xie, et al.
Fig. 10. Comparisons between simulation results (CFD) and experimental data
(Exp.) for cumulative iron extraction under three different Fe2O3 charges.
observed with an increase in oxide particle phase holdup.
Fig. 10 shows the time evolution of the cumulative iron extraction
under three different Fe2O3 charges. The CFD simulation conditions
were identical to the reported experimental conditions: the inlet gas
velocity was 0.0345 m/s, the total mass of the solid particles was 50 g,
and the reaction temperature was 250 °C. The CFD predictions are in
good agreement with the experimental data. As discussed above, the
gas-phase extraction reaction obeys the first-order kinetics best in terms
of the Fe2O3 charge under different reaction temperatures. Ad-
ditionally, these reaction kinetics characteristics are observed under
different Fe2O3 charges, while the apparent reaction rate constant de-
pends on the initial Fe2O3 charge. As shown in Fig. 10, the cumulative
iron extraction decreases with an increase in Fe2O3 charge. For an ir-
reversible first-order reaction, the extraction rate is independent of the
initial concentration of the reactant. Herein, the decreased reaction rate
with the increase in the initial Fe2O3 charge may indicate that the gas-
phase extraction reaction is reversible under high temperatures.
Therefore, it is necessary to develop a comprehensive mass transfer-
reaction kinetics model to gain a deep understanding of the relationship
between particle fluidization behaviors and reaction kinetics char-
acteristics.
Fig. 11. Contour plots of the reaction rate (kg/m3/s) in the FBR under different Fe2O3 charges: (A) 3% Fe2O3; (B) 10% Fe2O3.
8
Minerals Engineering 149 (2020) 106238
Fig. 11 displays the contour plots of the reaction rate in an FBR. As
shown, the distribution of the gas-phase extraction rate is highly de-
pendent on the distribution of the phase holdup of the Fe2O3 particles.
After the Fe2O3 charge increased from 1% to 3% and 10%, the average
reaction rates (the consumption rate of Fe2O3) were 0.000749,
0.002038, and 0.002526 kg/m3/s, respectively. Thus, the actual
amount of iron being extracted increased. Van Dyk et al. (2010) ob-
served that when the Fe2O3 charge was 10 wt%, the iron that was ex-
tracted was three times that obtained from a 1 wt% charge after 4 h.
4. Conclusions
A CFD coupled model involving a three-phase Eulerian model, KTGF
model, and reaction kinetics model was proposed to investigate gas-
phase extraction processes occurring in an FBR. The developed CFD
coupled model was validated by experimental data in terms of the cu-
mulative iron extraction at different reaction temperatures and the
classical calculated data of the pressure drop. Based on the validated
model, the effects of inlet gas velocity and particle phase holdup on the
extraction process were investigated. As the inlet gas velocity increased
from 0.01 to 0.06 m/s, the particles bed underwent particulate ex-
pansion into bubbling fluidization and the bed expansion height in-
creased from 0.25 to 0.378 m. Accordingly, both the particle fluidiza-
tion behaviors and extractive reaction kinetics characteristics were
obtained under three different Fe2O3 charges. Defluidization was ob-
served with an increase in oxide particle phase holdup. The simulation
results demonstrated that the distribution of the gas-phase extraction
rate was highly dependent on the distribution of Fe2O3 particle phase
holdup, and the cumulative iron extraction decreased with an increase
in Fe2O3 charges. Meanwhile, the average reaction rate and actual
amount of iron being extracted increased.
CRediT authorship contribution statement
Le Xie: Conceptualization, Methodology, Software, Writing - ori-
ginal draft. Jundong Zhu: Writing - review & editing. Jiang Hu:
Writing - review & editing. Chongwen Jiang: Supervision, Project
administration, Funding acquisition.
Declaration of Competing Interest
The authors declare that they have no known competing financial
L. Xie, et al.
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgements
The authors thank the National Natural Science Foundation of
China (No. 21476267) and Natural Science Foundation of Hunan
Province (No. 2018JJ2482) and the Center for High Performance
Computing, Shanghai Jiao Tong University for supporting this work.
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