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Research Article
Heat and Mass Transfer in Reduction Zone of Sponge Iron Reactor
Bayu Alamsari,1 Shuichi Torii,1 Azis Trianto,2 and Yazid Bindar2
1 Department
2 Department
1. Introduction
Sponge iron product quality in direct Reduced iron (DRI)
plant can be increased by rising reduction gas temperature
and composition of reactant in reduction gas. The rising
of temperature will accelerate reaction flow rate which in
turn can raise reaction conversion as shown by Zhang and
Ostrovski [1]. However, the temperature rising can also bring
disadvantage due to the formation of total carbon on the
product. The increasing of reactant composition which is
consisted of H2 and CO in reduction gas will also increase
product quality as reported by many researchers (e.g., [2
4]). The optimum composition of reduction gas must be
determined to obtain the highest quality.
The investigation of temperature and composition of
reduction gas is carried out by analyzing the performance of
sponge iron reactor which in turn can predict the profitable
optimum condition of reactor. However, since the reactor
analysis is dicult to be executed directly in the field plant, it
will need a simulator as support instrument. This simulator
can be designed by arrangement of heat and mass transfer
equation inside the reactor to reproduce reactor data from
the field. By solving heat and mass transfer equations, the
eect of reduction gas on the performance of reactor is
studied.
Some iron ore reactor models are proposed in a few literatures. Iron ore reactor model proposed by Aguilar et al. [5]
is referred for fixed bed reactor. The model is derived based
on unsteady state condition. Parisi and Laborde [6] proposed
a model for moving bed counter current reactor. The model
is limited on reduction zone of iron ore reactor, and only
reduction reactions are considered in the model, in which
plug flow is used as an approach for the model.
Another related model is formulated on direct reduction
shaft furnace for producing sponge iron from iron ore as proposed by Takenaka et al. [7]. In their model, reduction rate
equations are derived from the three-interface model which
involves both mass and heat balances. Srinivasan [8] develops
a model for reduction iron oxides by carbon. This model in
which only the global direct reduction reactions are taken
into account and methane reforming and water gas shift
reaction are ignored, is formulated on a circulating fluidized
bed reactor.
The kinetics of direct reduction reaction plays an important role in sponge iron reduction zone mathematical model.
Unreacted core model proposed by Levenspiel [9] is widely
used for kinetics model of iron reduction in which the reaction occurs first at the outer skin of the particle. The zone
of reaction then moves into the solid and may leave behind
dCCH4
= rmethanation CH4 , H2 , Tgas ,
dz
ugas
dCH2
= rWGSR CO, Tgas
dz
(6)
(7)
ugas
dCCO
= rWGSR CO, Tgas
dz
2. Reactor Modeling
(8)
(1)
(2)
(3)
(4)
CO2 + H2 CO + H2 O.
(5)
Mathematical model of reduction zone in iron ore reactor is arranged on the gas and solid phases. Heat and mass
transfer equations are formulated to perform the temperature and concentration of gas and solid phases, respectively.
The modeling is also carried out by employing kinetics
model. Note that iron reduction, methane reforming, and
water gas shift reactions are taken into account in the model.
The mass and energy equations are formulated by
assuming (i) steady-state operating conditions, (ii) no heat
loss over the wall of reactor reduction zone, (iii) the
usolid
dCFe2 O3
= n p rFe2 O3 (CO, H2 , Tsolid ),
dz
(9)
usolid
dCFe3 O4
= n p rFe3 O4 (CO, H2 , Tsolid ),
dz
(10)
dCFeO
= n p rFeO (CO, H2 , Tsolid ),
dz
(11)
dCFe
= n p rFe (CO, H2 , Tsolid ),
dz
(12)
usolid
usolid
Asp h Tsolid Tgas
[Hi ri ]
dTsolid
=
.
dz
Msolid C psolid
Msolid C psolid
(14)
C pgas =
CH2
CCO
C pCO +
C pH2 , (15)
CCO + CH2
CCO + CH2
3
The values of standard reaction enthalpy at 298 K (HR(298) )
for each reaction are obtained from Chemical Sciences [12].
Reaction heat capacity (C pR ) is also calculated for each
reaction by using
5 Iron ore
Reduction
zone
C pR =
1
Reduction gas
6 Reduced iron
3
Isobaric
zone
Cooling
gas output
Cooling
zone
Cooling
gas input
Makeup
10 Sponge iron
product
where
2
3
4
5
C p(CO or H2 ) = a1 Tgas a2 Tgas
+ a3 Tgas
a4 Tgas
+ a5 Tgas
.
(16)
(17)
Hi ri =
HR(298)-methanation +
To
Tgas
HR(298)-WGSR +
Tgas
C pR dT rmethanation
To
C pR dT rWGSR ,
=
HR(298) CO-reduction +
To
HR(298) H2 -reduction +
Tsolid
C pR dT rCO-reduction
To
Tsolid
b j C p j-product ,
(20)
C pR dT rH2 -reduction .
(19)
(21)
EA+
RT
pCH4
.
p H2
(22)
T G1.56 5.67826.
h = 6.91 103 G0.75
f
cooling gas
bi C pi-reactant
where i and j refer to reactant and product number, respectively. Notation b is stoichiometric coecient for each reactant and product.
Heat transfer coecient, h, is determined by using the
correlation proposed by Furnas [14]. He investigates heat
transfer value from a stream of air to a bed of iron pellets
covered with a thin coating of iron oxides. The temperature
experiments are set up to 1023 K. The equation proposed by
Furnas [14] is as follows:
Sponge iron
from isobaric zone
EA+
RT
CH2
0.33
CCO2 .
(23)
Fe2 O3
Leave the pellet by
diusing through
gas film and ash
Product
CO2 and H2 O
R p rc
rc R p
Qgas
Qash
CCO or H2
Qdiusion =
1 dNgas
,
S dt
(27)
Qreaction =
Gas film
x
1 dNi
.
S dt
(28)
(24)
(25)
(26)
(1) Diusion through Gas Film Control (Steps (a) and (e)). If
gas CO or H2 diuses through a stagnant film onto surface of
ash as shown in Figure 3, the flux of material can be defined
as the flow of gas unit surface, or
Qgas =
1 dNCO or H2
D
C
=D
=
CCO or H2 Cash
S
dt
r
r
= kfilm CCO or H2 Cash ,
(29)
where S is surface area (m2 ), N is mole amount of CO
or H2 in mole (kfilm ) is gas film kinetic constant (m/sec),
C is concentration (mole/m3 ), and D is molecular diusion
coecient (m2 /sec). The same equation can also be applied
for diusion of gas product (CO2 and H2 O).
On the ash surface, the flux diusion can also be stated as
Qash =
1 dNCO or H2
= kash Cash ,
S
dt
(30)
Qgas = Qash ,
(31)
Therefore,
(a) Fe2 O3 :
Cash =
kfilm
CCO or H2 .
kfilm + kash
(32)
1 dNCO or H2
kfilm
= kash
CCO or H2
S
dt
kfilm + kash
1 dNFe2 O3
1 dNFe2 O3
=
= k1 CFe2 O3 ,
S dt
4R2c dt
= kGAS CCO or H2 ,
dCCO or H2
1 dNCO or H2
= e
,
S
dt
dr
dNCO or H2
dCCO or H2
= 4r 2 e
,
dt
dr
dNCO or H2
dt
Rc
Rp
dr
= 4 e
r2
CCO or H2 at R p
(42)
R2
1 dNFe
= 2c (Zk3 CFeO ).
A p dt
Rp
(43)
(e) CO:
(36)
1
1
=
2 4 e CCO or H2 = 2 e CCO or H2
4R p
Rp
R2
1 dNFeO
= 2c Y k2 CFe3 O4 + k3 CFeO .
A p dt
Rp
(d) Fe:
1 dNCO or H2 1
1
Ap
dt
RC R p
(37)
R2
b dNCO
= 2c V1 k1 CFe2 O3 + k2 CFe3 O4 + k3 CFeO . (44)
A p dt
Rp
(e) H2 :
R2
b dNH2
= 2c V2 k1 CFe2 O3 + k2 CFe3 O4 + k3 CFeO . (45)
A p dt
Rp
Notations X, Y , and Z shown in (41), (42), and (43), respectively, represent the weight coecient, while V1 and V2 on
(44) and (45) represent equilibrium conditions.
Kinetic reaction constants k1 , k2 , and k3 , respectively,
refer to reaction as
k
or
1
2Fe3 O4 + CO2 (H2 O)
3Fe2 O3 + CO(H2 )
1 dNCO or H2
Ap
dt
1
e CCO or H2 .
2
R p (1/Rc ) 1/R p
(41)
(35)
dCCO or H2 .
= 4 e CCO or H2 .
R2
1 dNFe3 O4
= 2c X k1 CFe2 O3 + k2 CFe3 O4 .
A p dt
Rp
dt
Rc R p
(40)
(c) FeO:
(34)
R2
1 dNFe2 O3
= 2c k1 CFe2 O3 .
A p dt
Rp
(b) Fe3 O4 :
(2) Diusion through Ash Layer Control (Steps (b) and (d)).
If the flux of gas within the ash layer is expressed by Ficks law
for equimolar counter diusion, then we will have
Q=
(39)
2
3FeO + CO2 (H2 O)
Fe3 O4 + CO(H2 )
(38)
3
FeO + CO(H2 )
Fe + CO2 (H2 O).
(46)
(47)
(48)
be CCO & H2
1 dNFe2 O3
= bkGAS CCO & H2 +
A p dt
R2p 1/Rc 1/R p
R2
+ b 2c k1(CO & H2 ) CFe2 O3
Rp
(49)
or
rFe2 O3 = A p bkGAS CCO & H2 +
A p be CCO & H2
R2
+ A p b C2 k1(CO & H2 ) CFe2 O3 .
Rp
(50)
ki = ko exp
(b) Fe3 O4 :
rFe3 O4
= A p bkGAS CCO & H2 +
+ Apb
A p be CCO & H2
R2C
X k1(CO & H2 ) CFe2 O3 + k2(CO & H2 ) CFe3 O4 .
R2p
(51)
(c) FeO:
A p be CCO & H2
R
+ A p b C2 Y k2(CO & H2 ) CFe3 O4
Rp
(52)
e =
(d) Fe:
R2p
1/RC 1/R p
R
+ A p b C2 Z k3(CO & H2 ) CFeO .
Rp
(53)
(e) CO:
+ Apb
82.06T
(57)
p D
.
p
(58)
RC =
A p be CCO
R2p
1/RC 1/R p
(f) H2 :
rH2 reduction
+ Apb
14700
R3p
Co Mw
n p 4
1/3
(59)
0
0
Co = CCO
CCO + CH
CH2 .
2
R2C
2 V1 k1(CO) CFe2 O3 + k2(CO) CFe3 O4 + k3(CO ) CFeO .
Rp
(54)
= A p bkGAS CH2 +
(56)
where
rCOreduction
= A p bkGAS CCO +
A p be CCO & H2
RT
Here, as for two variables unknown in (56), those are preexponential constant ko and activation energy EA . Note that
the corresponding values are dierent for each reduction
reaction by CO and H2 . Many literatures focus on the
comparison of EA values rather than ko , because the variation
of ko values is large and highly dependent on research
condition. The value of activation energy (EA ) is important
to get good result. The ko and EA values used in this research
are adopted from Aguilar et al. [5]. The formulations of each
ki are shown in Table 1.
Overall kinetic constant on gas film kGAS is calculated
based on formulation proposed by Parisi and Laborde [6] as
stated as
EA+
A p be CH2
R2p
1/RC 1/R p
R2C
2 V2 k1(H2 ) CFe2 O3 + k2(H2 ) CFe3 O4 + k3(H2 ) CFeO .
Rp
(55)
(60)
Fe2 O3 Fe3 O4
Fe3 O4 FeO
FeO Fe
Note
(1)
(2)
(3)
Correction factor f
Reaction constant rate
Rf
X
Y
Z
V1
V2
(4)
Methane
reforming
0.00199
0.02
0.02
40
14800
4.6E6
5.1E6
(1)
(2)
H2
ki(H2 ) = 45 exp[49884/RT]
ki(H2 ) = 0.36 exp[21616/RT]
ki(H2 ) = 9 exp[21616/RT]
(3)
(4)
Note
Reduction gas in the bottom of reduction zone
Temperature (K)
CH4 (% vol.)
H2 (% vol.)
CO (% vol.)
CO2 (% vol.)
N2 (% vol.)
H2 O (% vol.)
Reduction gas inlet
Temperature (K)
CH4 (% vol.)
H2 (% vol.)
CO (% vol.)
CO2 (% vol.)
N2 (% vol.)
H2 O (% vol.)
Leaking gas from isobaric
zone
Temperature (K)
CH4 (% vol.)
H2 (% vol.)
CO (% vol.)
CO2 (% vol.)
N2 (% vol.)
H2 O (% vol.)
Reduction gas wastes
Temperature (K)
CO2 (% vol.)
CH4 (% vol.)
CO (% vol.)
H2 O (% vol.)
N2 (% vol.)
H2 (% vol.)
Plant data
1193
Simulation results
Reduction Isobaric
zone
zone
1193
2.9
42.1
9.58
2.26
3.72
1.36
1203
3.7
71.86
16.5
3.8
1.8
2.34
1139
50.13
45.63
0.983
3.03
1.14
0.12
657.5
9.0
4.4
12.1
23.4
12
49.7
657.5
8.5
4.5
11.7
23.9
1.7
49.5
Adjust R f
Reduction
Input
T6
5
4
and T 5 Tref
?
Are T 4 Tref
Results
5
4
Are Mi4 Mi-ref
and Mi5 Mi-ref
?
T4
T5
1
6
MH
MFe
2
2 O3
4
MH
2
5
MFe
2 O3
1
6
MCO
MFe
3 O4
4
MCO
5
MFe
3 O4
1
MCO
2
1
MH2 O
1
MCH
4
1
MN
2
4
MCO
2
4
MH2 O
4
MCH
4
4
MN
2
5
MFeO
T1
u1
6
MFeO
6
MFe
6
Mgangue
6
MFe
2+
u6
u4
No
Yes
No
Finish
Yes
5
MFe
5
Mgangue
5
MFe
2+
u5
1200
1100
1000
900
800
700
600
500
400
300
200
100
0
80
Gas concentration (% volume)
Temperature (K)
70
60
50
40
30
20
10
0
2
3
4
Depth of reduction zone (m)
Solid
Gas
2
3
4
Depth of reduction zone (m)
CH4
CO
H2
N2
CO2
H2 O
(a)
(b)
100
80
60
40
20
0
0
2
3
4
Depth of reduction zone (m)
Fe2 O3
Fe3 O4
FeO
Fe
Gangue
Fe2+
Solid flow
Gas flow
(c)
Figure 5: Profiles of many variables as a function of the depth of reduction zone; (a) gas and solid temperature; (b) gas concentration; (c)
solid concentration.
9
Reduction
gas waste
5 Iron ore
Reduction
zone
1
6 Reduced iron
Adjust Mi6
Adjust T 6
No
T6
Mi6
u6
Flow 5
Solve
mathematical
model
Input
Results
simultaneously
New T 1
Flow 4
Mi1
T5
Mi5
u5
T4
Mi4
5
Is T 5 Tref
?
5
Are Mi5 Mi-ref
?
Yes
Finish
No
Yes
u4
u1
Figure 6: Simulation algorithm of reduction gas temperature eect on metallization degree of reduced iron.
0.97
0.96
0.95
0.94
0.93
0.92
1160
1180
1200
1220
1240
1260
1280
10
5 Iron ore
Reduction
zone
1
Reduction gas input
6 Reduced iron
3
Adjust Mi6
Adjust T 6
No
T6
Mi6
Solve
mathematical
u6
Input
T1
1
New MH
2
Flow 5
model
simultaneously
Results
Flow 4
T5
Mi5
u5
T4
5
Is T 5 Tref
?
5
Are Mi5 Mi-ref
?
Yes
No
Yes
Finish
Mi4
u4
New M 1
CO
1
MCO
2
1
MH
2O
1
MCH
4
1
MN
2
u1
Figure 8: Simulation algorithm of reduction gas composition eect on metallization degree of reduced iron.
Metallization degree
1
0.95
0.9
0.85
0.8
0.75
52/35
56/31
60/27
64/23
68/19
72/15
76/11
3.4. Composition. In general, hydrogen and carbon monoxide are good reducers for iron ore. The change in their composition in reduction gas will aect quality of the product.
Simulation of the eect of composition changes on metallization degree is performed on various composition of H2
and CO. Composition of other gas is maintained on the same
ratio.
Figure 8 shows the simulation algorithm of reduction gas
composition eect on metallization degree. Note that correction factor and other values resulted from the calculation in
reduction zone are used as the basis of calculation. By using
data at flow 1 and 6 as calculation input, we can solve the
model and get the new value for each data at flow 4 and 5.
Figure 9 depicts metallization degree as a function of
ratio H2 CO. One observes that an increase in H2 composition while an attenuation of CO will produce higher
metallization degree. This implies that H2 is better reducer
than CO. The same conclusion is reported by Bonalde et al.
[2], El-Geassy and Rajakumar [3], and Pineau et al. [4].
Bonalde et al. [2] analyze metallization degree produced by
using 100% H2 , 100% carbon monoxide, and midrex gas
(55% H2 -34% CO) as reducer, respectively. They reported
4. Conclusions
Reduction zone of iron reactor has been simulated. Kinetics
equation of reduction of hematite to iron metal, methane
reforming, and water gas shift reaction are taken into account
in the model. Simulation results are in good agreement with
the reference data.
Temperature profiles along reduction zone show an increase in gas and solid temperature from the direction of
solid flow. Gas concentration profiles show composition
changes which are caused by reactions in the gas phase. Gas
mole balance reaction for methane reforming, reduction,
and water gas shift reaction already have an agreement.
At the beginning of reduction zone inlet, solid concentration profile shows that total Fe in the ore is dominated
by Fe2 O3 . As reactions occur, Fe2 O3 is slowly reduced by
reduction gas to release oxygen. Reduced iron from reduction
zone produces metallization degree until 94.22%.
When an attenuation of CO yields, an increase in H2
composition produces higher metallization degree. Metallization degree is also increased with an increase in gas inlet
temperature. Reduction gas temperature over 1246 K is not
recommended because the formation of sticky iron will be
initiated.
Nomenclature
Asp :
11
Gas constant, Pam3 /moleK
Radius of unreacted core, m
Pellets radius, m
Relaxation factor
Temperature, K
Pore structure tortuosity
Superficial velocity, m/s
Coecients depending on weight
relationships and equilibrium conditions
X, Y , Z: Weight coecients
z:
Space variable inside reactor, m
solid: Solid
R:
Reaction.
R:
Rc :
Rp:
Rf :
T:
p:
u:
V:
Superscripts
+: Forward reaction
: Backward reaction.
Subscripts
1:
2:
3:
4:
i:
Reduction reaction by H2
Reduction reaction by CO
Methane reforming reaction
Water gas shift reaction
ith reaction.
References
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experimental results and kinetic modelling, Ironmaking and
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[2] A. Bonalde, A. Henriquez, and M. Manrique, Kinetic analysis
of the iron oxide reduction using hydrogen-carbon monoxide
mixtures as reducing agent, ISIJ International, vol. 45, no. 9,
pp. 12551260, 2005.
[3] A. A. El-Geassy and V. Rajakumar, Gaseous Reduction of
Wustite with H2 , CO and H2 -CO mixtures, Transactions of
the Iron and Steel Institute of Japan, vol. 25, pp. 449458, 1985.
[4] A. Pineau, N. Kanari, and I. Gaballah, Kinetics of reduction
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[5] J. Aguilar, R. Fuentes, and R. Viramontes, Simulation of iron
ore reduction in a fixed bed, Modelling and Simulation in
Materials Science and Engineering, vol. 3, no. 2, pp. 131147,
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[6] D. R. Parisi and M. A. Laborde, Modeling of counter current
moving bed gas-solid reactor used in direct reduction of iron
ore, Chemical Engineering Journal, vol. 104, no. 13, pp. 35
43, 2004.
[7] Y. Takenaka, Y. Kimura, K. Narita, and D. Kaneko, Mathematical model of direct reduction shaft furnace and its application
to actual operations of a model plant, Computers and Chemical Engineering, vol. 10, no. 1, pp. 6775, 1986.
[8] N. S. Srinivasan, Reduction of iron oxides by carbon in a
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[9] O. Levenspiel, Chemical Reaction Engineering, John Wiley &
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12
[10] K. Mondal, H. Lorethova, E. Hippo, T. Wiltowski, and S.
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[11] Y. Iguchi and S. Yokomoto, Kinetics of the reactions in carbon
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[14] C. C. Furnas, Heat transfer from a gas stream to a bed of
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[15] P. Munster and H. J. Grabke, Kinetics of the steam reforming
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[16] F. Bustamante, R. M. Enick, A. V. Cugini et al., High-temperature kinetics of the homogeneous reverse water-gas shift
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[18] Empowerment and Research Society Institution of Bandung
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