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Article history: For the FischerTropsch synthesis (FTS), this paper presents a numerical investigation in a 3D uidized bed reac-
Received 12 April 2017 tor. The effect of the operation parameters such as bed temperature, supercial gas velocities, particle size and
Received in revised form 17 May 2017 bed heights is discussed. A 3D-CFD model coupled with FTS chemical kinetics was set up. The computational re-
Accepted 19 May 2017
sults are compared with experimental data in terms of the components production rates, etc. The analysis shows
Available online xxxx
that the bed heights, the bed temperature, the supercial gas velocities and particle sizes affect the C5+ selectivity
Keywords:
and the reaction rates. Product yields are dependent on the operating conditions especially the temperature.
Fluidized bed 2017 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.
FischerTropsch synthesis
CFD
http://dx.doi.org/10.1016/j.cjche.2017.05.012
1004-9541/ 2017 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.
Please cite this article as: X. Zhang, et al., Effect of the operation parameters on the FischerTropsch synthesis in uidized bed reactors, Chin. J.
Chem. Eng. (2017), http://dx.doi.org/10.1016/j.cjche.2017.05.012
2 X. Zhang et al. / Chinese Journal of Chemical Engineering xxx (2017) xxxxxx
kinetics of the main reactions, the mass transfer equations and the heat includes a kinetic and a collisional term. The shear viscosity of particles
transfer equations. The Sasol R&D group developed a pilot plant for the is consisted of three parts, including the collision viscosity, the frictional
FTS [31], reporting similar selectivity and higher conversion than those viscosity and the kinetic viscosity [22].
in commercial CFBR. A transport equation for static enthalpy is used to describe the heat
CFD models are advantageous for the optimization of many complex ux in gas phase, and in solid phase the heat transfer is considered sim-
processes, especially for the gassolid ow in FRBs with close and com- ilar to a continuous phase [53]. The interphase heat transfer resistance is
plex interactions between the two phases and the heat and mass trans- regarded to be associated with the heat transfer coefcient and the tem-
fer, etc. The underlying physicochemical processes can be clearly perature difference [54] (Table 2).
understood through CFD simulation [3236]. The EulerianEulerian
models combined with the kinetic theory are the most popular method 2.3. Chemical model
for engineering simulation of gassolid ow. The main features of the
ows in uidized beds has been obtained by either laminar or turbu- There are many different authors proposed the kinetic mechanism
lence models [3740]. The turbulent interactions between the solid during the F-T synthesis, which can be roughly divided into two
and the gas phase have been elucidated by several authors [4143]. Re- categories: one is depended on the Langmuir Hinshelwood Hogan
cently, the turbulence model enforced in the CFD code MFIX (Multi- Watson(LHHW) model [55,56], while the other one is based on the
phase Flow with Interphase Exchanges) developed by Simonin's group power law of chemical rate expression [57,58]. The mechanism of the
has predicted dilute gassolid ows under an appropriate boundary Fe-HZSM5 Bifunctional Catalyst proposed by Marvast et al. [58].was
conditions reasonably [4446]. adopted in this study. It was supposed that the F-T reaction include
In this work, the FTS process in a three-dimension (3D) uidized bed CO, H2, CO2, H2O, CH4, C2H4, C2H6, C3H8, n-C4H10, i-C4H10, and C5+ spe-
reactor was numerically studied aiming to get a better description. Thus, cies. The following reactions (1)(8) were considered as dominating
a 3D model coupled with gassolid momentum, mass and heat trans- F-T reactions.
port, and FT reactions was employed. The operation parameters on
R1
the production rates, the temperature distribution and the selectivity CO 3H2 CH4 H2 O 1
were analyzed based on the simulations in this model.
R2
2CO 4H2 C2 H4 2H2 O 2
2. Models and Methods
R3
A 3D computational uid dynamics (CFD) model coupled with FTS 2CO 5H2 C2 H6 2H2 O 3
reaction which considered the uid ow, the heat transfer and the
R4
mass transfer mechanism was employed in this paper. 3CO 7H2 C3 H8 3H2 O 4
Constitutive correlations are required for closing the governing CO H2 OCO2 H2 WGS reaction 8
conservation equations. The gas-phase stress tensor always uses the
Newtonian closure. The gassolid momentum exchange coefcient The reactions (1)(7) are a general form for the rate equations. It is a
(i.e., the interphase drag coefcient), which is a crucial parameter for function of the yield pressures of hydrogen and carbon monoxide, are
the successful simulation, is taken the same as Syamlal et al. [47,48]. expressed as:
The solid stress tensor is calculated from the kinetic theory of the h i
1
granular [49], using two completely different models, for viscous shear- Ri ki exp Ei =RT P m ni
CO P H2
i
mol kg s1 9
ing and plastic regimes [47,48], where an algebraic expression of the
granular temperature m is used. The solid pressure, which considers where P is partial pressure and k is the apparent rate constant. Table 3
the normal forces because of particle-particle interactions [47,4952], presented the kinetic parameters.
Table 1
Conservation equations ([45,47])
Solid P
t
x m m U m j U mi g xg m xmij I gmi m m g i Rm gm m 1gm gm
m m U mi
t
j i j
U
g g tg U g j xg x g g xg g kgg gij xgi g g g
j
i
i
j
Solid m m tm U m j m
x m m 2 m
m m mij U mi
km m m m
x j x
i i x j
3=2
m 121e2 2m m g 0 dmp
Energy Gas T
g g C pg tg g T g qg Hgm H g Hgw
Solid T
g g C pg tg g T g qg Hgm H g Hgw
Species Gas and solid
t
ln l X ln l l X ln l Rln
Please cite this article as: X. Zhang, et al., Effect of the operation parameters on the FischerTropsch synthesis in uidized bed reactors, Chin. J.
Chem. Eng. (2017), http://dx.doi.org/10.1016/j.cjche.2017.05.012
X. Zhang et al. / Chinese Journal of Chemical Engineering xxx (2017) xxxxxx 3
Table 2
Constitutive relations ([45,47])
Table 3
Kinetic parameters for FTS reactions in Eqs. (1)(7)
Reaction no. ki Ei mi ni
r WGS 15:7 exp 45080=RT P CO P H2 O =P 0:5 0:5
H2 P CO2 P H2 =K WGS
h i 10
1 1:13 103 P CO P H2 O =P 0:5
H2
5078:0045
K WGS 5:8972089 13:958689 Fig. 1. Schematic diagram of the simulated uidized bed reactor.
T
104 T27:592844 108 T 2 11
To solve the transport and reaction for the model a suitable time
3. Simulation Setup step should be used, to ensure the accuracy and stability during
the calculation, was 0.00001 s in this study. The segregated solution
3.1. Reactor geometry strategy has been adopted to prevent the iterative divergent. In order
to eliminate the pressurevelocity coupling, The traditional SIMPLE
The simulated uidized bed is described in Fig. 1, the inner diameter method was used. Convective uxes of the transport equations were
of which is 30 mm and the height is 500 mm. all approximated by the Super bee spatial scheme with a second-
The synthesis gas enters from the bottom of the uidized bed which order accuracy. Linear discretization for the pressure was adopted. A
consists of CO and H2. The FischerTropsch synthesis takes place over convergence criterion of 1 105 was taken here for all the transport
the iron based catalyst powder, the effect is reected on the reaction ac- equations.
tivation energy. After the reactions, the products and reactant leave
from the outlet in the upper part of the reactor. All experiments were 3.3. Initial and boundary conditions
carried out at constant pressure conditions.
The gas distribution is assumed to be uniform at the reactor en-
3.2. Numerical method and parameters trance. In order to reach the desired bed expansion, the ow rate was
regulated based on the particle size. The inlet gas temperature is xed
In this study, the MFIX, which is described in Section 2, is used. The at a given value, and the reactor wall was assigned a series of given tem-
discretization of all the governing non-linear partial differential equa- peratures in different simulations. The gas phase used a no slip bound-
tions is accomplished using the nite volume method on the staggered ary and the solid phase used a free slip boundary. The outlet used a
grid. It is found that the grid size of 1.0 mm 1.0 mm 2.0 mm is suf- condition of the pressure outlet. Table 4 species the parameters in
cient for neglecting the numerical errors due to the grid resolution. these initial and boundary conditions and the particle properties.
Please cite this article as: X. Zhang, et al., Effect of the operation parameters on the FischerTropsch synthesis in uidized bed reactors, Chin. J.
Chem. Eng. (2017), http://dx.doi.org/10.1016/j.cjche.2017.05.012
4 X. Zhang et al. / Chinese Journal of Chemical Engineering xxx (2017) xxxxxx
Table 4
Operating conditions and material properties of the simulated uidized bed reactor
Parameters Value
Fig. 2. Methane production rates obtained from the simulation and from literature
(Rahmati [57]).
Please cite this article as: X. Zhang, et al., Effect of the operation parameters on the FischerTropsch synthesis in uidized bed reactors, Chin. J.
Chem. Eng. (2017), http://dx.doi.org/10.1016/j.cjche.2017.05.012
X. Zhang et al. / Chinese Journal of Chemical Engineering xxx (2017) xxxxxx 5
Fig. 5. Effect of catalyst particle diameter on the production selectivity and the production
Fig. 7. The production selectivity versus catalyst particle diameter (inlet gas temperature =
rates(inlet gas temperature = 560 K, inlet H2:CO mole ratio = 1.13, P = 1700 kPa, bed
560 K, inlet H2:CO mole ratio = 1.63, P = 1700 kPa, bed height = 50 cm, cooling
height = 50 cm, cooling temperature = 520 K).
temperature = 520 K).
of the particle diameter the selectivity rstly grows, the maximum value velocity is 8 times lower than Umf, the product rates are nearly linear
of 33.4% is achieved at 200 m diameter, which then slightly decreases. growth when the supercial gas velocity is growing, then decreases.
While the change trend of the methane production rate is opposite to it. For a uidized bed reactor, the rate-limiting step is usually decided by
The phenomena can be clearly explained by the axial temperature dis- mass transport or surface reaction kinetics [62,63]. It can be concluded
tribution of the gas phase as plotted in Fig. 6. It illustrates that the that when the syngas velocity is 8 times lower than Umf, the mass trans-
axial temperature difference is larger for smaller particle, which reaches port limits the process, but when velocity is 8 times over Umf, the limi-
the largest value of 65.0 K for 100 m particles, and the lowest value of tation is the reaction kinetics. When the syngas velocity is 8 times less
7.1 K for 200 m particles. The peak value of the temperature for 100 m than Umf, the C5+ selectivity and its production rate show the opposite
particles is also the maximum at 588.3 K. Because the FTS is a strong trend shown in Fig. 7(a).
exothermic reaction, the small particles tend to aggregate, which leads Fig. 8 shows the axial gas temperature distribution for different su-
to poor heat transfer. Meanwhile, smaller particles have higher reaction percial gas velocities. For smaller gas velocity, bed temperature is
activity [61]. These cause higher solid and gas temperature and uneven lower, which may explain the above phenomena. As the supercial
temperature distribution. As observed above, when the reaction tem- gas velocity grows, the gas residence time is shorter, which will reduce
perature is high, the C5+ production rate is low. This may explain that the reaction rate and the generation of the heat. Moreover, the heat
with the growth of the catalyst particle diameter, the production rates transfer rate among the gas and solid phase is higher.
sharply increase and then decrease, as shown in Fig. 5(b).
Fig. 8. Axial temperature distribution for different supercial gas velocity (inlet gas
temperature = 560 K, inlet H2:CO mole ratio = 1.63, P = 1700 kPa, bed height = 50 cm,
cooling temperature = 520 K).
Please cite this article as: X. Zhang, et al., Effect of the operation parameters on the FischerTropsch synthesis in uidized bed reactors, Chin. J.
Chem. Eng. (2017), http://dx.doi.org/10.1016/j.cjche.2017.05.012
6 X. Zhang et al. / Chinese Journal of Chemical Engineering xxx (2017) xxxxxx
Subscript
g gas phase
i,j indices to identify vector and tensor components
l liguid phase
m solid phase
WGS watergas shift
Fig. 9. Effect of bed height on the selectivity and rate of the products (inlet gas
temperature = 560 K, inlet H2:CO mole ratio = 1.13, P = 1700 kPa, Dp = 200 m,
supercial gas velocity = 8Umf, cooling temperature = 520 K). References
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Chem. Eng. (2017), http://dx.doi.org/10.1016/j.cjche.2017.05.012
X. Zhang et al. / Chinese Journal of Chemical Engineering xxx (2017) xxxxxx 7
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Please cite this article as: X. Zhang, et al., Effect of the operation parameters on the FischerTropsch synthesis in uidized bed reactors, Chin. J.
Chem. Eng. (2017), http://dx.doi.org/10.1016/j.cjche.2017.05.012