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.
The remaining steps in the process were designed to effi-
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
the kiln as secondary air where it flows above the pellet bed
counter current to the flow of pellets through the kiln. The
gases from the kiln, including secondary air and combustion
products, are used to preheat and oxidize the pellet bed on a
traveling grate before the pellets are fed to the kiln.
Magnetite oxidation is exothermic, and occurs primarily
along the grate in the preheat h a c e where hot air is drawn
down through the porous bed of spherical pellets (Potts,
1991). Plant experience indicates that only a small fraction
of oxidation occurs in the kiln due to the relatively poor
mixing of the pellet bed with the freeboard gases. In addi-
tion, the gas to solids mixing in the rotary kiln is difficult to
model rigorously. Consequently, most models of the grate-
kiln iron ore pellet induration process have ignored oxida-
tion in the kiln by limiting this reaction to the grate in the
preheater and cooler (Thurlby, 1988; Young et al., 1979).
However, ignoring this reaction fails to account for the addi-
tional temperature rise in the kiln due to the heat released by
this exothermic oxidation reaction. According to Potts
(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
pellet bed temperature.
You may contact the author by E-mail: rdavis@d.umn.edu
Figure 1 -Grate-kiln system. Arrows indicate the countercurrent
flow of process gasses and pellet bed.
A simple, novel approach to simulating magnetite oxida-
tion in the kiln is presented here. For the purpose of demon-
stration, the magnetite oxidation model was incorporated
into a modified form of the one-dimensional rotary kiln heat
transfer model of Thornton and Batterham (1982). Concise
literature reviews of the shrinking core model applied to
magnetite oxidation and the heat and mass transfer models
of a rotary kiln precedes the theoretical development of the
magnetite oxidation model for a rotary kiln. This simple
rotary kiln magnetite oxidation model was found to provide
satisfactory results, while avoiding the complicated model-
ing of the gas to solids mixing in the kiln pellet bed (Young
et al., 1979).
Magnetite oxidation in the pellet
The overall reaction of oxygen with magnetite to form
hematite is
4 Fe304 + 0, + 6 Fe203 . . . . . . . . . . . . . . . . . . . . . (1)
The magnetite oxidation reaction may be assumed irre-
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)
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
unreacted magnetite core. Experimental evidence suggests
that the interface between the shrinking core and the ash
layer is sharp, and that the oxidation reaction is controlled
by the diffusion of 0, through the ash once the outside pel-
let surface is oxidized (Monson et al., 1994; Pape et al.,
1976; Papanastassiou and Bitsanes, 1973). By applying the
stationary-state approximation to the changing core size rel-
ative to the flow rate of 0, to the reacting interface, as out-
lined by Levenspiel (1992), the shrinking core model results
in the following expression for the rate of change in the core
radius.
drc
-_ - doe [0 2 ,3 ....................
where the subscript g refers to the conditions of the free-
board gas, De is the effective difisivity of 0, in the reacted
layer of Hematite, re is the radius of the unreacted magnetite
core, rp is the constant radius of the pellet, pc is the molar
density of magnetite in the core, and k is the mass transfer
coefficient for the convection of 0, from the bulk gas phase
to the surface of the pellet.
The shrinlung core model of oxidation within the pellet is
readily extended to models of magnetite oxidation in the
preheat furnace and cooler pellet beds where air is uniformly
drawn through the traveling grate (Thurlby, 1988; Young
et al., 1979). However, incorporation of the shrinking core
model into a rotary luln model is complicated by the unusual
gas to solids mixing and transport of 0, from the secondary
air to the cascading pellet bed in the kiln.
Heat and mass transfer theory
The one dimensional rotary kiln heat transfer model of
Thornton and Batterham (1982) was modified here to pre-
dict the 0, composition as well as the bed temperature pro-
file, both required in the magnetite oxidation model for a
rotary kiln. The principle heat transfer mechanism in the
kiln is radiation from the flame, followed by conduction
from the kiln wall, then convection from the secondary air.
Thermal energy is liberated during the combustion of natural
gas in the burner zone of the kiln, and by the exothermic
magnetite oxidation reaction. In this study, natural gas is
assumed to be pure methane. Approximately 10% of the sto-
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
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
Batterham's model used to demonstrate the magnetite oxi-
dation model are provided next. The details of the radiation
heat transfer model and solids mixing are described else-
where (Thornton and Batterham, 1982).
CONSERVATION OF ENERGY
For convenience, the gases in the luln are divided
between a flame stream and secondary air stream. The flame
and secondary air streams were assumed to be distinct, per-
fectly mixed, concentric flows, with no inter stream mixing,
THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996
except for a constant flux of entrained gas from the sec-
ondary air stream to the flame stream. It was recognized that
the flame shape is generally not symmetric about the kiln
centerline, and that some turbulent mixing of these streams
occurs. However, this description of the process was chosen
in order to simplify the mathematics of radiation heat transfer,
while providing reasonable results for gas and solids tem-
perature profiles, as described in the literature (Silcox and
Pershing, 1990; Barr et al., 1989; Gorog et al., 1983;
Thornton and Batterham, 1982, Jenkins and Moles, 1981).
The differential energy balances for the gas streams along
the length of the kiln, z, are of the form:
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
absolute temperature of the stream, q' is the net heat trans-
fer rate per unit length to the gas stream by either radiation
(as in the case of the flame stream) or convection (as for the
secondary air stream), and Ng, is an adjustable parameter for
the molar flux of gas from the secondary air stream
entrained into the flame stream. The parameter p = -1 for
the secondary air stream, p = 1 for the flame stream, depend-
ing on the direction of entrainment flux. The perimeter of
the flame stream, Pr is calculated from the local flame
stream radius.
This approach is similar to that of Jenkins and Moles
(1 98 l), Thornton and Batterham (1982), Gorog, et al. (1983),
and Silcox and Pershing (1990), except these authors
defined the flame dimensions a priori. The first two sets of
authors combined the flame and air streams into a single
well mixed stream upon complete combustion. Silcox and
Pershing (1990) treated the flame stream as a constant
radius plug flow surrounded by a secondary air stream, also
in plug flow. Here, the heat transfer model of Thornton and
Batterham (1982) was modified to allow for conveniently
adjusting the flux of gas between streams for reasonable
flame dimension and temperature profiles. The flame and
secondary air streams were also allowed to extend along the
entire length of the kiln, but the cross sectional area of the
flame stream was permitted to vary as a function of the
flame stream and secondary air stream volumetric flow rates
and temperatures. The two streams are mixed at the kiln
exit. Assuming ideal gas behavior and uniform pressure, the
cross sectional area of the flame is calculated as follows.
(4)
where the subscriptsf and g refer to the flame and secondary
air streams, respectively,and A, is the total cross sectional area
of the kiln above the pellet bed, normal to the flow direction:
~ , = r k 2 [ , - 0 . 5 ( 2 4 - s i n 2 4 ) ] . . . . . . . . . . . . . . . . .( 5 )
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
entrains the secondary air, the radius grows, increasing the
rate of entrainment. In the limit of z + 0, this model reduces
to the semi-empiricalexpression for gas entrainment by a jet
in a moving fluid derived by Ricou and Spalding ( 1961).
1005

i ‘
-
a
--------- - - ---_ ---.___
__ - - - --- -
-.-
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.
The differential thermal energy balance in the pellet bed
involves heat transfer between the bed and the kiln wall,
secondaw air, flame stream, and the heat released from the
exothekic reaction of magnetite oxidation (an additional
term not included in the original heat transfer model):
where the subscript b refers to the pellet bed, mb and 3.b are
the mass flow rate and specific heat of the pellet bed, respec-
tively; Tb is the pellet bed temperature at position z along the
length of the luln,qLb is the total heat transfer rate per unit
length to the pellet bed by convection and conduction from
the gas and kiln wall (Tscheng and Watlunson, 1979), qib is
the total net radiation per unit length to the bed from the
flame and wall (Thornton and Batterham, 1982), and qkx is
the rate of heat generated in the bed per unit length by the
magnetite oxidation reaction. The last term is the principal
contribution of this work. Note that the sign is negative
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:
CH, + 20, + CO, + 2H2O. . . . . . . . . . . . . . . . . . . .(7)
The change in composition of each individual species in
the flame and secondary air streams is governed by the com-
bustion reaction as well as the molar flux to the flame
stream. A stoichiometric amount of fuel is assumed to be
1006 THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996
completely combusted with the air entrained by the flame.
A differential material balance for each of the combustion
reactants and products in the flame stream uses 0, as the
reaction reference species:
.....
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
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:
dFo2, - dF02,b
. . . . . . . . . . . . . . . . . . (10)
---yo P N --
dz l f g dz
where Fo2,b is the molar flow rate of 0 2 to the bed where it
reacts with magnetite.
Model of magnetite oxidation
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-
tions of residence times in rotary kilns under conditions of
moderate to heavy kiln loading. In this approach it is
assumed that the freeboard gases, including O,, are periodi-
cally entrained by the revolving bed of tumbling pellets.
The entrained gases are carried around the bed along the arc
of rotation where the 0, reacts with the magnetite in the pel-
let core.
According to Saeman’s treatment, the average frequency
of cascades in the pellet bed may be calculated from the
superficial axial velocity of the pellet bed, ub, divided by the
average axial solids transport distance per cascade:
...............
where a is the bed angle of repose, usually around 40’
(Henein et al., 1983; Saeman, 1951), 6 is the kiln angle of
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
shown in Figure 2. Up to this point in Saeman’s derivation,
there is no distinction between the type of bed motion in the
kiln. Nevertheless, the mechanism of gas entrainment by the
tumbling pellets proposed here should exclude extreme bed
motion behavior, such as slipping or centrifuging, as
described by Henein et al. (1983).
Assuming that all of the 0, in the bed is reacted with
magnetite between cascades. the total molar flow rate of 0,
entrained by the bed is calculated by integrating the 0, con-
centration in the bed over the entire free bed volume:
Lk
Fo, ,h = C [0 2 1 , &bAbdZ . . . . . . . . . . . . . . . . . . . . . .
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
direction of flow. The local concentration of 0, in the bed is
calculated from an equation of state at the local conditions of
the bed temperature and secondary air partial pressure above
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
Equation (10) to account for magnetite oxidation:
. (13)
The heat generation rate per unit length from the mag-
netite oxidation in Equation (6) is now defined in terms of
the rate of 0, consumption by the bed and the heat of reac-
tion per mole of 0,, Hrxn:
dFO, ,b
qox = Hrxn 7 ...........................
The fraction of magnetite oxidized in the kiln bed is cal-
culated according to the stoichiometry of Equation (1) and
the rate of consumption of 0,. The total moles of 0, reacted
by the magnetite in the bed per solids residence time is:
. . . . . (15)
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:
dn, - 4c[02]bEbVb
--
........................
dz ub
where V, = L, A , is the pellet bed volume. The average dif-
ferential change in the magnetite core radius with oxidation
per unit length is calculated from the moles of 0, consumed
and the reaction stoichometry. Equation (16) may also be cast
differently in terms of the change in the magnetite core radius:
dnM - ( l - ~ ~ ) p ~ 42dr
-- zr,
2-. v,
.................
dz dz Vp
THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 74, DECEMBER, 1996
where Vp - 4nrp3/3 is the individual spherical pellet volume.
Equation (17) is rearranged in terms of the differential
change in r,:
2
drc - 1 P-dn, . . . . . . . . . . . . . . . . . . . . . .
d r - a l / h p c [ L c ) dz
(12) where a is the pellet surface area per unit bed volume,
a=- 3(l-€b) .............................. (19)
‘P
The total moles of magnetite oxidized per pellet is
The change in the unreacted core radius is calculated
from the total moles of magnetite oxidized:
rc =[(r:r -21 113
. . . . . . . . . . . . . . . . . . . . . . . . (21)
where rz is the average pellet core radius feeding into the
kiln.
Although Equations (13) and (14) are used in the kiln
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-
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
feed end of the kiln, due to the counter current flow of gas
and pellets through the kiln.
The assumption of complete 0, consumption in the bed
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-
tion conditions in the kiln. The differential 0, concentration
balance is proportional to the time gradient in the core radius:
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
between cascades is approximated as the average axial dis-
(16)
tance traveled per cascade divided by the superficial velocity
of the bed:
t = c-‘ . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . (23)
The gas entrained by the cascading bed of spheres is
assumed to be stagnant within the bed. The mass transfer coef-
ficient in Equation (2) was approximated from film theory:
k=-
.........................
6 ....
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
3.60 1000
3.55 --.A 800
0 5 10 15 20 25 30 35 40
(m)
Figure 3 -Temperature and magnetite core radius profiles in the
rotary kiln.
where D, is the difhivity of 0, in the kiln gas at the bed
conditions, and 6 is the gas film boundary layer thickness
around a spherical pellet. An estimate of the film thickness
was made from the hydraulic radius for the open, free space
between three, adjacent, connecting, spherical pellets in a
plane:
where the angle between the coordinate sphere centers, cp, is
d 3 radians. This estimate of the film thickness is considered
conservative because the expected smaller values of 6 will
result in larger mass transfer coefficients that yield higher
oxidation rates.
Results and discussion
The rotary kiln magnetite oxidation model results in a
coupled system of first-order, ordinary, differential equa-
tions describing the heat and mass transfer between the
flame, secondary air, pellet bed, as well as the magnetite
oxidation. The model equations were solved numerically by
an improved Euler method with two extrapolations, which
gives global error estimates and fourth order accuracy
(Hanna and Sandall, 1995). These simulation results apply
to a rotary kiln at the USS Minntac taconite pelletizing plant
(Potts, 1991). The plant operation parameters used in the
model calibration and simulation are listed in Table 1. The
gas entrainment flux in Equation (3) was adjusted for rea-
sonable model prediction agreement with the measured bed
and gas temperatures reported by Potts (1991). The gas
entrainment flux was found to be 4mole/m2.s. The result-
ing temperature profiles, shown in Figure 3, are in agree-
ment with plant data and other models for these operating
conditions (Thurlby, 1988; Thornton and Batterham, 1982;
Young et al., 1979).
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
occur in the kiln for the conditions of Table 1. T h s com-
pares favorably with the 5% maximum oxidation observed
in the plants (Potts, 1991). The shnnking core model was
used to test the assumption of complete 0, consumption in
the pellet bed between cascades. The equations were solved
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
average time between cascades of pellets in the rotating kiln
was estimated from Equation (23) to be 15 seconds. As
shown in Figure 4, the shrinking core model predicted that
most of the 0, is consumed in less than half the time
between cascades.
A novel approach to account for magnetite oxidation in a
rotary kiln was presented. The method gives results for the
fraction of magnetite oxidized that are in reasonable agree-
ment with plant experience. This model should be limited
to bed motion such as slumping, or cascading, where pel-
lets are turned over in the bed. It may be considered as an
upper limit to the extent of oxidation expected in extreme
bed motion, such as slipping or centrifuging. Further refme-
ments to this modeling approach to magnetite oxidation in
a rotary kiln should incorporate theory for the volume frac-
tion of cascading pellets exposed to the freeboard gas and
the effects of solids mixing between the outer mantle of
pellets and the inner bed core (Thornton and Batterham,
1982).

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

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Kilns,” in Proc. Chemeaca 82, Tenth Australian Chemical
c = pellet core or convection
Engineering Conference, Inst. of Engineers, Sydney, National
CH, = methane
CO, = carbon dioxide
publication no. 82/9, (1 982) pp. 260-266.
Thurlby, J. A,, “A Dynamic Mathematical Model of the Complete
e = effective property
Grate/Kiln Iron-Ore Pellet Induration Process,” Metall. Trans. B
f = to or in the flame stream
19B, 103-1 12 (1988).
g = from or in secondary air stream
Tscheng, S. H. and A. P. Watkinson, “Convective Heat Transfer in
H 2 0 = water
a Rotary Kiln,” Can. J. Chem. Eng. 57,433-443 (1979).
k = kiln
Young, R. W., M. Cross and R. D. Gibson, “Mathematical Model
M = magnetite
of Grate-Kiln-Cooler Process Used for Induration of Iron Ore
ox = magnetite oxidation
Pellets,” Ironmaking Steelmaking 1, 1-13 (1 979).
0, = oxygen
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