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Mathematical Model of Magnetite Oxidation in a

Rotary Kiln furnace


R. A. DAVIS

Department of Chemical Engineering, University of Minnesota Duluth, Duluth, MN 55812, U.S.A.


A novel method of accounting for the oxidation of magnetite during iron ore pellet induration in a rotary kiln is pre-
sented. The technique is based on the mathematical description of a cascading bed of pellets in a rotary kiln by Saeman
(1951). For the purpose of illustration, this method was incorporated into a simple one-dimensional model of heat and
mass transfer in a natural gas fired rotary kiln fkmace. The model predicts a fraction of magnetite oxidation less than
5%, which is in agreement with plant observations.

On presente une nouvelle methode pour tenir compte de I’oxydation de la magnetite lors de l’induration de pastilles
de minerai de fer dans un four rotatif. La technique s’appuie sur la description mathematique de Saeman (1 95 1) d’un lit
en cascade gami de pastilles dans un four rotatif. A des fins d’illustration, on a applique cette methode a un modele uni-
dimensionnel simple de transfert de chaleur et de matiere dans un four rotatif alimente au gaz naturel. Le modele predit
une fraction de l’oxydation magnetique a moins de 5%, ce qui est en accord avec les observations en usine.

Keywords: taconite pellet induration, magnetite oxidation, rotary kiln, mathematical model.

mpart
Aperatures
s of the taconite iron ore pellet induration process,
agnetite in the pellet is oxidized to hematite at tem-
high
with oxygen from air. The grate-kiln system is com-
Proh.ator/Grnta Rotary Kiln
n

monly used for this purpose (Ball et al., 1973; Potts, 1991).
The grate-kiln taconite pellet induration system involves sev- v
eral stages of heat and oxygen transfer to a traveling bed of To Dryer Cooler
spherical taconite pellets, as shown in Figure 1. At the heart of
the process is the rotary kiln where pellets are heated to tem- Secondary air to 1st stage I

peratures in excess of 1600 K with a high temperature flame. Figure 1 -Grate-kiln system. Arrows indicate the countercurrent
The remaining steps in the process were designed to effi- flow of process gasses and pellet bed.
ciently recover thermal energy from the pellet bed. The pellets
exiting the kiln are cooled by an updraft of ambient air through
the pellet bed traveling along a grate in a revolving two stage
cooler. Hot air from the first stage of the cooler is passed to A simple, novel approach to simulating magnetite oxida-
the kiln as secondary air where it flows above the pellet bed tion in the kiln is presented here. For the purpose of demon-
counter current to the flow of pellets through the kiln. The stration, the magnetite oxidation model was incorporated
gases from the kiln, including secondary air and combustion into a modified form of the one-dimensional rotary kiln heat
products, are used to preheat and oxidize the pellet bed on a transfer model of Thornton and Batterham (1982). Concise
traveling grate before the pellets are fed to the kiln. literature reviews of the shrinking core model applied to
Magnetite oxidation is exothermic, and occurs primarily magnetite oxidation and the heat and mass transfer models
along the grate in the preheat h a c e where hot air is drawn of a rotary kiln precedes the theoretical development of the
down through the porous bed of spherical pellets (Potts, magnetite oxidation model for a rotary kiln. This simple
1991). Plant experience indicates that only a small fraction rotary kiln magnetite oxidation model was found to provide
of oxidation occurs in the kiln due to the relatively poor satisfactory results, while avoiding the complicated model-
mixing of the pellet bed with the freeboard gases. In addi- ing of the gas to solids mixing in the kiln pellet bed (Young
tion, the gas to solids mixing in the rotary kiln is difficult to et al., 1979).
model rigorously. Consequently, most models of the grate-
kiln iron ore pellet induration process have ignored oxida- Magnetite oxidation in the pellet
tion in the kiln by limiting this reaction to the grate in the
preheater and cooler (Thurlby, 1988; Young et al., 1979). The overall reaction of oxygen with magnetite to form
However, ignoring this reaction fails to account for the addi- hematite is
tional temperature rise in the kiln due to the heat released by
this exothermic oxidation reaction. According to Potts 4 Fe304 + 0, + 6 Fe203 . . . . . . . . . . . . . . . . . . . . . (1)
(1991), up to 5% of the magnetite is oxidized in the kiln,
which can result in as much as a 10% increase in the kiln The magnetite oxidation reaction may be assumed irre-
pellet bed temperature. versible for the kiln conditions in this analysis (Papanastassiou
and Bitsanes, 1973). Taconite pellets are roughly spherical
with magnetite evenly distributed throughout the pellet. The
well known shrinking core model (Levenspiel, 1972)
You may contact the author by E-mail: rdavis@d.umn.edu applied to taconite pellets, assumes a retreating reaction

1004 THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996
interface between an outer ash layer of hematite and an except for a constant flux of entrained gas from the sec-
unreacted magnetite core. Experimental evidence suggests ondary air stream to the flame stream. It was recognized that
that the interface between the shrinking core and the ash the flame shape is generally not symmetric about the kiln
layer is sharp, and that the oxidation reaction is controlled centerline, and that some turbulent mixing of these streams
by the diffusion of 0, through the ash once the outside pel- occurs. However, this description of the process was chosen
let surface is oxidized (Monson et al., 1994; Pape et al., in order to simplify the mathematics of radiation heat transfer,
1976; Papanastassiou and Bitsanes, 1973). By applying the while providing reasonable results for gas and solids tem-
stationary-state approximation to the changing core size rel- perature profiles, as described in the literature (Silcox and
ative to the flow rate of 0, to the reacting interface, as out- Pershing, 1990; Barr et al., 1989; Gorog et al., 1983;
lined by Levenspiel (1992), the shrinking core model results Thornton and Batterham, 1982, Jenkins and Moles, 1981).
in the following expression for the rate of change in the core The differential energy balances for the gas streams along
radius. the length of the kiln, z, are of the form:

drc
-_ - doe [0 2 ,3 .................... z4hi
dT
= 41 - c dF:
( - p p f ~ , Y i )... . . . . . . . (3)
H ~2
dz

where Fi,Ai,Hi, yi are molar flow rate, heat capacity,


enthalpy and mole fraction of species i, respectively, T is the
where the subscript g refers to the conditions of the free- absolute temperature of the stream, q' is the net heat trans-
board gas, De is the effective difisivity of 0, in the reacted fer rate per unit length to the gas stream by either radiation
layer of Hematite, re is the radius of the unreacted magnetite (as in the case of the flame stream) or convection (as for the
core, rp is the constant radius of the pellet, pc is the molar secondary air stream), and Ng, is an adjustable parameter for
density of magnetite in the core, and k is the mass transfer the molar flux of gas from the secondary air stream
coefficient for the convection of 0, from the bulk gas phase entrained into the flame stream. The parameter p = -1 for
to the surface of the pellet. the secondary air stream, p = 1 for the flame stream, depend-
The shrinlung core model of oxidation within the pellet is ing on the direction of entrainment flux. The perimeter of
readily extended to models of magnetite oxidation in the the flame stream, Pr is calculated from the local flame
preheat furnace and cooler pellet beds where air is uniformly stream radius.
drawn through the traveling grate (Thurlby, 1988; Young This approach is similar to that of Jenkins and Moles
et al., 1979). However, incorporation of the shrinking core (1 98 l), Thornton and Batterham (1982), Gorog, et al. (1983),
model into a rotary luln model is complicated by the unusual and Silcox and Pershing (1990), except these authors
gas to solids mixing and transport of 0, from the secondary defined the flame dimensions a priori. The first two sets of
air to the cascading pellet bed in the kiln. authors combined the flame and air streams into a single
well mixed stream upon complete combustion. Silcox and
Heat and mass transfer theory Pershing (1990) treated the flame stream as a constant
radius plug flow surrounded by a secondary air stream, also
The one dimensional rotary kiln heat transfer model of in plug flow. Here, the heat transfer model of Thornton and
Thornton and Batterham (1982) was modified here to pre- Batterham (1982) was modified to allow for conveniently
dict the 0, composition as well as the bed temperature pro- adjusting the flux of gas between streams for reasonable
file, both required in the magnetite oxidation model for a flame dimension and temperature profiles. The flame and
rotary kiln. The principle heat transfer mechanism in the secondary air streams were also allowed to extend along the
kiln is radiation from the flame, followed by conduction entire length of the kiln, but the cross sectional area of the
from the kiln wall, then convection from the secondary air. flame stream was permitted to vary as a function of the
Thermal energy is liberated during the combustion of natural flame stream and secondary air stream volumetric flow rates
gas in the burner zone of the kiln, and by the exothermic and temperatures. The two streams are mixed at the kiln
magnetite oxidation reaction. In this study, natural gas is exit. Assuming ideal gas behavior and uniform pressure, the
assumed to be pure methane. Approximately 10% of the sto- cross sectional area of the flame is calculated as follows.
ichiometric air required for complete combustion is pre-
mixed with the fuel in the burner (Zahl et al., 1995). The rest
of the oxygen required for complete combustion is supplied (4)
as secondary air. The combustion rate and flame shape are
governed by the flux of air to the flame stream from the sec-
ondary air stream. Only those modifications to Thornton and where the subscriptsf and g refer to the flame and secondary
Batterham's model used to demonstrate the magnetite oxi- air streams, respectively,and A, is the total cross sectional area
dation model are provided next. The details of the radiation of the kiln above the pellet bed, normal to the flow direction:
heat transfer model and solids mixing are described else-
where (Thornton and Batterham, 1982). ~ , = r k 2 [ , - 0 . 5 ( 2 4 - s i n 2 4 ) ] . . . . . . . . . . . . . . . . .( 5 )

CONSERVATION OF ENERGY where 4 is the solid fill angle and rk is the inside kiln refrac-
tory radius, as defined in Figure 2. As the flame stream
For convenience, the gases in the luln are divided entrains the secondary air, the radius grows, increasing the
between a flame stream and secondary air stream. The flame rate of entrainment. In the limit of z + 0, this model reduces
and secondary air streams were assumed to be distinct, per- to the semi-empiricalexpression for gas entrainment by a jet
fectly mixed, concentric flows, with no inter stream mixing, in a moving fluid derived by Ricou and Spalding ( 1961).

THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996 1005
completely combusted with the air entrained by the flame.
A differential material balance for each of the combustion

i ‘ reactants and products in the flame stream uses 0, as the


reaction reference species:

.....
-
a

where uiis the combustion reaction coefficient for species i


in terms of one mole of 0, reacting ( U C H ~= -1/2, uo, = -1,
uco,= 112, VH,O = l), and yo, is the mole fraction of 0, in
the secondary air stream. The initial flame stream tempera-
ture is assumed to be the adiabatic flame temperature for
--------- - - ---_ ---.___
__ - - - --- -
complete combustion of the primary air mixed with the fuel.
-.- The differential species balance for the non-combustion
Bed species in the flame stream, and the secondary air stream
.............................................. species is:

5
! = py,prlVg .............................. (9)
dz

where yi is the mole fraction of species i. There is one addi-


tional term in the 0, balance for the secondary air stream to
account for the consumption of 0, by the magnetite oxida-
tion reaction in the pellet bed:
Figure 2 -(a) Inclined kiln angle of inclination, 0, (b) angle of
bed surface from the centerline, ty,and (c) bed fill angle, 4, and bed
angle of repose, a. dFo2, - dF02,b
. . . . . . . . . . . . . . . . . . (10)
---yo P N --
dz l f g dz
The differential thermal energy balance in the pellet bed
involves heat transfer between the bed and the kiln wall, where Fo2,b is the molar flow rate of 0 2 to the bed where it
secondaw air, flame stream, and the heat released from the reacts with magnetite.
exothekic reaction of magnetite oxidation (an additional Model of magnetite oxidation
term not included in the original heat transfer model):
The model of magnetite oxidation in a rotary h l n devel-
oped here is based Saeman’s (195 1) mathematical descrip-
tion of a cascading bed in a rotary kiln. Kohav et al. (1995)
demonstrated that Saeman’s method gives accurate predic-
where the subscript b refers to the pellet bed, mb and 3.b are tions of residence times in rotary kilns under conditions of
the mass flow rate and specific heat of the pellet bed, respec- moderate to heavy kiln loading. In this approach it is
tively; Tb is the pellet bed temperature at position z along the assumed that the freeboard gases, including O,, are periodi-
length of the luln,qLb is the total heat transfer rate per unit cally entrained by the revolving bed of tumbling pellets.
length to the pellet bed by convection and conduction from The entrained gases are carried around the bed along the arc
the gas and kiln wall (Tscheng and Watlunson, 1979), qib is of rotation where the 0, reacts with the magnetite in the pel-
the total net radiation per unit length to the bed from the let core.
flame and wall (Thornton and Batterham, 1982), and qkx is According to Saeman’s treatment, the average frequency
the rate of heat generated in the bed per unit length by the of cascades in the pellet bed may be calculated from the
magnetite oxidation reaction. The last term is the principal superficial axial velocity of the pellet bed, ub, divided by the
contribution of this work. Note that the sign is negative average axial solids transport distance per cascade:
because the gases and solids move in counter current flow
through the kiln.
...............
CONSERVATION OF MASS

For complete methane combustion, the reaction stoi-


chiometry is equimolar: where a is the bed angle of repose, usually around 40’
(Henein et al., 1983; Saeman, 1951), 6 is the kiln angle of
CH, + 20, + CO, + 2H2O. . . . . . . . . . . . . . . . . . . .(7) inclination, w is the angle between the top of the bed and the
kiln centerline, and Wb is the width of the top of the bed, as
The change in composition of each individual species in shown in Figure 2. Up to this point in Saeman’s derivation,
the flame and secondary air streams is governed by the com- there is no distinction between the type of bed motion in the
bustion reaction as well as the molar flux to the flame kiln. Nevertheless, the mechanism of gas entrainment by the
stream. A stoichiometric amount of fuel is assumed to be tumbling pellets proposed here should exclude extreme bed

1006 THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996
motion behavior, such as slipping or centrifuging, as where Vp - 4nrp3/3 is the individual spherical pellet volume.
described by Henein et al. (1983). Equation (17) is rearranged in terms of the differential
Assuming that all of the 0, in the bed is reacted with change in r,:
magnetite between cascades. the total molar flow rate of 0,
entrained by the bed is calculated by integrating the 0, con- 2
centration in the bed over the entire free bed volume: drc - 1 P-dn, . . . . . . . . . . . . . . . . . . . . . .
d r - a l / h p c [ L c ) dz
Lk

Fo, ,h = C [0 2 1 , &bAbdZ . . . . . . . . . . . . . . . . . . . . . . (12) where a is the pellet surface area per unit bed volume,
0 defined as follows.

where L, is the kiln length, &b is the pellet bed porosity, and
A , is the cross sectional area of the bed, perpendicular to the a=- 3(l-€b) .............................. (19)
direction of flow. The local concentration of 0, in the bed is ‘P
calculated from an equation of state at the local conditions of
the bed temperature and secondary air partial pressure above The total moles of magnetite oxidized per pellet is
the bed. The justification for the stationary-state approxima-
tion in the shrinking core model is also assumed to apply in
the bed; thus allowing the composition of the gas in the free
bed volume to instantaneously match the freeboard gas
composition. Equation (12) was differentiated to give the
local flow rate of 0, per unit length to the bed, required by The change in the unreacted core radius is calculated
Equation (10) to account for magnetite oxidation: from the total moles of magnetite oxidized:

. (13)
rc =[(r:r -21 113
. . . . . . . . . . . . . . . . . . . . . . . . (21)

The heat generation rate per unit length from the mag- where rz is the average pellet core radius feeding into the
netite oxidation in Equation (6) is now defined in terms of kiln.
the rate of 0, consumption by the bed and the heat of reac- Although Equations (13) and (14) are used in the kiln
tion per mole of 0,, Hrxn: material and energy balances to account for 0, consump-
tion, Equation (2 1) is used directly to calculate the effect of
oxidation on the core radius in the kiln. This avoids an iter-
dFO, ,b
qox = Hrxn 7 ........................... ative trial and error solution for rc at the pellet discharge end
of the kiln that would be required to match the calculated
initial pellet core radius with the known value for ( at the
The fraction of magnetite oxidized in the kiln bed is cal- feed end of the kiln, due to the counter current flow of gas
culated according to the stoichiometry of Equation (1) and and pellets through the kiln.
the rate of consumption of 0,. The total moles of 0, reacted The assumption of complete 0, consumption in the bed
by the magnetite in the bed per solids residence time is: between cascades was evaluated by solving the shrinking
core model for the bed 0, concentration during the time
between cascades, at typical temperature and gas composi-
. . . . . (15) tion conditions in the kiln. The differential 0, concentration
balance is proportional to the time gradient in the core radius:

The total moles of magnetite oxidized in the kiln per res-


idence time is nM = 4n0,. The differential form of Equation
(1 5), with substitution from Equation (12) for Fo2,b, gives
the differential change in the moles of magnetite reacted per
unit kiln length: where the rate of change in the core radius is calculated
based on the shrinking core model in Equation (2).
According to Saeman’s mathematical description, the time
dn, - 4c[02]bEbVb
--
........................ between cascades is approximated as the average axial dis-
(16)
dz ub tance traveled per cascade divided by the superficial velocity
of the bed:
where V, = L, A , is the pellet bed volume. The average dif-
ferential change in the magnetite core radius with oxidation t = c-‘ . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (23)
per unit length is calculated from the moles of 0, consumed The gas entrained by the cascading bed of spheres is
and the reaction stoichometry. Equation (16) may also be cast assumed to be stagnant within the bed. The mass transfer coef-
differently in terms of the change in the magnetite core radius: ficient in Equation (2) was approximated from film theory:

dnM - ( l - ~ ~ ) p ~ 42dr
-- zr,
2-. v,
................. k=-
dz dz Vp .........................
6 ....

THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996 1007
TABLE1
Rotary kiln process simulation parameters
pellet feed rate
pellet radius
bed porosity
mb
'P
E~
141 kg/s
0.0062
0.4
m n
magnetite concentration
fuel feed rate
kiln length Lk
% 9 I 00 m0i/m3
100 molh (1 0% stoich. air)
40m
refractory inside radius rk 3m
bed angle of repose 4 0.7 rad
kiln angle of inclination 6' 0.052 rad
bed angle of repose a 0.7 rad

1800
3.75

-E 1600 -Y t (s)
E 3.70
v
c Figure 4 - O2 consumption between cascades.
L"
1400

3.65
1200 gas entrainment flux in Equation (3) was adjusted for rea-
sonable model prediction agreement with the measured bed
3.60 1000 and gas temperatures reported by Potts (1991). The gas
entrainment flux was found to be 4mole/m2.s. The result-
3.55 --.A 800 ing temperature profiles, shown in Figure 3, are in agree-
0 5 10 15 20 25 30 35 40 ment with plant data and other models for these operating
(m) conditions (Thurlby, 1988; Thornton and Batterham, 1982;
Figure 3 -Temperature and magnetite core radius profiles in the Young et al., 1979).
rotary kiln. The shrinking magnetite core radius profile is plotted
along with the process temperature profiles in Figure 3.
Approximately 3 3% of the oxidation was calculated to
where D, is the difhivity of 0, in the kiln gas at the bed occur in the kiln for the conditions of Table 1. T h s com-
conditions, and 6 is the gas film boundary layer thickness pares favorably with the 5% maximum oxidation observed
around a spherical pellet. An estimate of the film thickness in the plants (Potts, 1991). The shnnking core model was
was made from the hydraulic radius for the open, free space used to test the assumption of complete 0, consumption in
between three, adjacent, connecting, spherical pellets in a the pellet bed between cascades. The equations were solved
plane: for the case of an 0, partial pressure of 20 kPa above the
bed, and pellet bed temperatures of 1000, 1200, 1400, and
1600 K. The 0, diffusion coefficient was calculated from
the correlation of Wilke and Lee (Reid et al., 1987). The
effective diffusivity was calculated based on pellet porosity
and pore tortuosity, D,=Do, Ep/t (Shigeno et al., 1990). The
where the angle between the coordinate sphere centers, cp, is average time between cascades of pellets in the rotating kiln
d 3 radians. This estimate of the film thickness is considered was estimated from Equation (23) to be 15 seconds. As
conservative because the expected smaller values of 6 will shown in Figure 4, the shrinking core model predicted that
result in larger mass transfer coefficients that yield higher most of the 0, is consumed in less than half the time
oxidation rates. between cascades.
A novel approach to account for magnetite oxidation in a
Results and discussion rotary kiln was presented. The method gives results for the
fraction of magnetite oxidized that are in reasonable agree-
The rotary kiln magnetite oxidation model results in a ment with plant experience. This model should be limited
coupled system of first-order, ordinary, differential equa- to bed motion such as slumping, or cascading, where pel-
tions describing the heat and mass transfer between the lets are turned over in the bed. It may be considered as an
flame, secondary air, pellet bed, as well as the magnetite upper limit to the extent of oxidation expected in extreme
oxidation. The model equations were solved numerically by bed motion, such as slipping or centrifuging. Further refme-
an improved Euler method with two extrapolations, which ments to this modeling approach to magnetite oxidation in
gives global error estimates and fourth order accuracy a rotary kiln should incorporate theory for the volume frac-
(Hanna and Sandall, 1995). These simulation results apply tion of cascading pellets exposed to the freeboard gas and
to a rotary kiln at the USS Minntac taconite pelletizing plant the effects of solids mixing between the outer mantle of
(Potts, 1991). The plant operation parameters used in the pellets and the inner bed core (Thornton and Batterham,
model calibration and simulation are listed in Table 1. The 1982).

1008 THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996
Acknowledgements References

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Zahl, R. K., L. A. Haas and J. Engesser, “Formation of NO, in Iron
p = pellet Oxide Pelletizing Furnaces,” US Bureau of Mines, NRRI, St.
r = radiation
Paul, Minnesota DNR final report, September 29 (1 995).
mn = reaction

Superscripts
’ = initial condition Manuscript received May 21, 1996; revised manuscript received

= per unit length, m-1 September 23, 1996; accepted for publication October 2, 1996.

THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996 1009