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Mixed-Control Kinetic Model of Magnesia-Based Flux Dissolution in BOF

Steelmaking Slags: Part 1 — Model Formulation and Validation With
Literature Data

Article in Iron & Steel Technology · January 2023

DOI: 10.33313/TR/0123

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236 AIST Transactions Vol. 20, No. 1 DOI 10.33313/TR/0123

Mixed-Control Kinetic Model of Magnesia-Based Flux Dissolution

in BOF Steelmaking Slags: Part 1 — Model Formulation and
Validation With Literature Data
Author
Kanan Kumar Sahoo
Assistant General Manager-WRM-II-
Operations, Visakhapatnam Steel Plant,
Visakhapatnam, India
kanansahoo@vizagsteel.com
In basic oxygen furnace (BOF) steelmaking, it is very important to understand the dissolution
mechanism of magnesia-based flux to improve the productivity of BOF vessels by increasing the
refractory lining life and reducing the downtime of vessels. In the present study, a mixed-control
kinetic model for the dissolution of calcined dolomite and calcined magnesite is presented. The
model considers the formation of both dicalcium silicate (2CaO.SiO2 = C 2 S) solid solution on
unreacted CaO and magnesiowüstite (MgO.FeO = MF′) solid solution on unreacted MgO in the
case of calcined dolomite, and only magnesiowüstite (MgO.FeO = MF′) solid solution formation
on MgO in the case of calcined magnesite. A general mixed-control kinetic model has been
proposed taking the two diffusing components in BOF steelmaking slag as SiO 2 and FeO (to
estimate the dissolution rate of calcined dolomite) and only FeO (to estimate the dissolution rate
of calcined magnesite); various slag compositions generally produced during BOF steelmaking
are considered. The rate equation for mixed-control kinetics has been proposed and solved by
using a computer program to find the dissolution rate. The predicted values of the dissolution
rates are validated with experimental and operating plant data available in the literature, with
encouraging results.

B asic oxygen furnace (BOF) steel-

making is a high-temperature
multi-phase, multi-reaction pro-
cess that occurs with continuous
variation of temperature, and com-
positions of liquid iron and slag,
throughout the blow, which makes
the process very complex. This
complex and severe nature makes
it difficult to take measurements
of the evolution of metal and slag
compositions. To overcome these
difficulties, mathematical modeling
not only helps to predict the evolu-
tion of metal and slag throughout
the process but also guides process
understanding. Generally, there are
two types of mathematical models
available for the BOF process: static
and dynamic modeling. In static
modeling, the end blow conditions
I IRON & STEEL TECHNOLOGY I AIST.ORG
the metal and slag evolution as
functions of time can be predicted
throughout the blowing process by
considering the hot metal weight,
temperature and composition, oxy-
gen flowrate, lance height, flux and
coolant addition as input variables.
Since a dynamic model predicts the
slag composition throughout the
blow, thorough knowledge of flux
dissolution is essential.
Generally, there are three types
of dynamic model for BOF steel-
making. The first is thermodynamic
modeling, providing information on
the equilibrium distribution of spe-
cies between phases, the behavior
(activity) of species in solution and
the heat generated or consumed by
these reactions. It also deals with
feasibility of each individual oxida-

such as temperature, weight of steel, tion reaction and its subsequent

and oxygen gas consumption are
predicted from the weight, tempera-
ture and composition of hot metal
as the main input variables. The
static model does not predict metal
and slag evolution during refining;
it is generally used to define the ini-
tial blowing and input conditions to
JAN 2023
effects on further purification of
impurities.1–3 Equilibrium calcula-
tions are performed using the Gibbs
free energy minimization technique.
The second model type is kinetic
modeling, dealing with the rate of
reactions occurring in the bath.4–11
It provides information about not

predict the endpoint steel composi- only the required reaction condi-
tion. However, in dynamic modeling tions but also the factors that govern

the rates of reactions and the reaction mechanisms.
The third model type is a decarburization model
based on offgas analysis, which is widely used in the
steelmaking industry and provides slopping predic-
tion and calculation of oxygen accumulation in the
BOF vessel; an oxygen mass balance is used to esti-
mate the amounts of FeO, Fe2O3 and MnO in the slag
during blowing. The oxygen level in the system can
be used as an indicator of progress of a reaction since
the accumulated oxygen controls the P and Mn con-
tents of steel and the total iron content of slag at the
end of the blow.12–19 Another type of kinetic model is
the droplet model that considers liquid iron droplet
generation by impingement of the supersonic oxygen
gas jet onto the liquid iron surface, greatly increasing
slag-metal interface area, enhancing the rates of heat
and mass transfer.20–23 Computational fluid dynamics
(CFD) modeling provides graphical representations
of fluid flow in terms of swirls and turbulent motion
along with the cavity formation. Due to the availability
of powerful digital computers, the time required for
simulations has been reduced.24–30
The evolution of slag composition is important
not only for the oxidation of impurities in the liquid
iron (such as Si, Mn and P) into their corresponding
oxides that are absorbed by the slag, but also for the
dissolution of lime and magnesia-containing flux. It
is quite important to understand the dissolution of
magnesia-containing fluxes in steelmaking slag, to
ensure MgO-saturated slag throughout the blow to
protect the MgO-C refractory lining of the vessel with-
out hindering refining.
It is well known that reactions between solid CaO
with SiO2 and solid MgO with FeO in iron-silicate
type slag results in the formation of dicalcium silicate
(2CaO.SiO2 = C2S), tricalcium silicate (3CaO.SiO2 =
C3S) and magnesiowüstite (MgO.FeO=MF'), respec-
tively, as illustrated in Eqs. 1 and 2. The experimental
evidence of formation of the solid solutions is found
in the studies of several researchers.31–36
(Eq. 1)
(Eq. 2)
The formation of C2S and C3S depends on the slag
basicity (CaO/SiO2) and FeO content. The similarity
in ionic radius of Mg2+ (0.72Å) and Fe2+ (0.63Å) ions37
enables Fe2+ to readily substitute Mg2+ ions, creating
an unlimited solid solution called magnesiowüstite
(MF'). Calcined dolomite is a mixture of CaO and
MgO particles. Reactions at these two phases produce
237
C2S and MF' as separate phases. Further reaction
between the CaO and MgO particles with SiO2 and
FeO present in the slag requires the diffusion of SiO2
and FeO through the C2S and MF' solid solution
layers. In the case of calcined magnesite, diffusion
of only FeO through the MF' solid solution layer is
required.
A majority of experimental and modeling studies
on cylindrical samples of burnt/calcined dolomite
and sintered/calcined magnesite assumed diffusion
through the slag film to be rate-controlling.31–33,38,39
The experimental studies of Umakoshi et al.31,32 and
Takoka et al.39 concluded that the observed increase
in dissolution with increasing rotation rate of cylindri-
cal samples confirms that slag-film diffusion is rate-
controlling, but this may also occur under mixed con-
trol. Takoka et al.39 concluded from their microscopic
analysis of slag samples that there are many small
undissolved MgO particles (<100 μm) scattered in the
molten slag when MgO clinker was used. Williams et
al.33 concluded that in the presence of MgO in the slag,
the fluxing properties of MgO in the slag increases by
lowering the fusion temperature of slag with increase
in slag viscosity so that the kinematic viscosity (ϑk) of
slag remains almost constant. Furthermore, Satyoko
et al.37 reported magnesia refractory dissolution in
steelmaking slag. However, binders are used during
manufacturing of refractory; these may alter the dis-
solution rate of MgO from the refractory.
Tromel et al.40 studied the solubility of MgO as MF'
in CaO-SiO2-FeO slag as a function of FeO concen-
tration and slag basicity at 1,600°C and concluded
that the solubility of MgO decreases as the basicity of
slag increases (at constant FeO content), and that the
MgO solubility increases with decrease in FeO con-
centration. Huang et al.41 experimentally dissolved
solid MgO in MgO-SiO2-B2O3 and FeO-SiO2-CaO slag
stirred with argon and reported that the formation
and decomposition of C2S and MF' solid solution lay-
ers are rate-controlling steps; they concluded that the
dissolution of solid MgO particles in CaO-SiO2-FeO
slag strongly depends on the composition of the MF'
solid solution. Cheremisina et al.42 studied the kinet-
ics of lime dissolution containing different amounts of
MgO (4.3–7.6 wt. %) in steelmaking for temperatures
of 1,300–1,600°C. They found that the lime dissolu-
JAN 2023
tion rate decreases with an increase in MgO content;
they concluded that the formation of high-temper-
I IRON & STEEL TECHNOLOGY I AIST.ORG
ature solid compounds (Ca2SiO4 and (Fe,Mg)2SiO4)
and solid solutions based on MgO (like MF') within
the lime particles is responsible for decreasing the dis-
solution rate of lime.
These results show that a general conclusion regard-
ing the overall rate of dissolution of magnesia-con-
taining flux cannot be drawn. Furthermore, in actual
steelmaking processes, where conditions such as
temperature and slag composition vary continuously
238 AIST Transactions

throughout the refining period, it is not likely that a

J i* = ni − N i ni − N i ∑ j =2 n j
k
single mechanism would control the dissolution rate
of magnesia-containing fluxes over the entire refin-
ing period. Thus, a mixed-control model43,44 would be (Eq. 4)
more appropriate for calculating dissolution rates of
magnesia-containing flux in steelmaking slag. Neglecting the cross or other species diffusion as
Sarkar et al.44 developed a mixed-control model for given in the third term in the right-hand side of Eqs. 3
estimating the dissolution rate of lime in BOF steel- and 4 yields:
making slag, giving a better model to predict dynamic
lime dissolution during BOF steelmaking. However,
they considered diffusion of only one component
(SiO2) into the lime particles, which would only be
the case for lime dissolution. In the present paper, a
similar mixed-control model has been formulated, (Eq. 5)
but considering the diffusion of two components
(SiO2 and FeO) for dissolution of calcined dolomite where
and one component (FeO) for dissolution of calcined
magnesite. A cylindrical particle geometry is used for Ni = the mole fraction of the ith species in the slag
comparing the magnesia flux dissolution with the phase,
results of Umakoshi et al.,31,32 and a spherical geom- Ci = the molar concentration of the ith species in the
etry for comparing dissolution of dolomite during slag solution and
BOF steel refining with the results Cicutti et al.,45 with C = the molar density of the slag.
encouraging results.
Dissolution of Cylindrical Calcined Dolomite Particles: In the
present model, a shell mass balance for diffusion of
Model Development for Magnesia-Containing Flux species i through a cylindrical shell in the slag-film
Particles of radius r, thickness dr and length L is considered
as illustrated in Fig. 1a. This yields a pseudo-steady
The mixed-control kinetic model considers three state assumption in the product layer diffusion.44,46
kinetic steps: (i) slag-film diffusion: diffusion of SiO2 Considering the interfacial reaction as pseudo mono-
and FeO from the bulk slag through the slag-film molecular in nature results in the following expression:
boundary layer around CaO and MgO particles to
form C2S and MF' solid solutions; (ii) product-layer
diffusion: diffusion of SiO2 and FeO through the C2S
and MF' layers that surround the unreacted core of (Eq. 6)
CaO and MgO; and (iii) interfacial reaction: SiO2
and FeO, after diffusing through C2S and MF', react Rearranging and taking limit dr → 0 by dividing
with bulk CaO and MgO (for calcined dolomite), or 2πδrL yields:
only FeO (after diffusion through MF') reacts with
bulk MgO (for calcined magnesite). These steps are
in series and hence are combined to achieve the inte-
grated mixed-control kinetic model as mentioned by
Sarkar et al.44 In the present model, one-dimensional (Eq. 7)
diffusion of SiO2 and FeO is considered.43 Schematic
diagrams of these steps (for cylindrical and spherical From the definition of first derivative, Eq. 7 can be
calcined dolomite and calcined magnesite particles) rewritten as:
I IRON & STEEL TECHNOLOGY I AIST.ORG

are shown in Fig. 1.

Derivation of Mixed-Control Rate Equations — The molar

diffusion flux (J*i ) defined as the difference between
molar flux (n·i) and the rate of bulk transport (cross (Eq. 8)
diffusion) of the ith species in the jth direction is
given by Eqs. 3 and 4: Substituting Eq. 5 into Eq. 8 and integrating, Eq. 9
may be developed:
J i* = ni − N i ∑ j =1 n j
k
JAN 2023

(Eq. 3)
 239
Figure 1

(a) (b)

JAN 2023
I IRON & STEEL TECHNOLOGY I AIST.ORG

(c) (d)

Schematic diagram of the cylindrical geometry for dissolution of a calcined dolomite particle (a), schematic diagram of the
spherical geometry for dissolution of calcined dolomite (b), schematic diagram of dissolution of cylindrical calcined magnesite
(c), and schematic diagram of dissolution of spherical calcined magnesite (d).
240 AIST Transactions
(Eq. 9)
In the calculations, it is assumed that the initial
radius of calcined dolomite flux particle is the same
as that of CaO and MgO particles, i.e., r 0CD = r 0CaO =
r 0MgO . The boundary conditions for SiO2 diffusion are:
at r = r 0CaO ; CS = CSe and at r = (r 0CaO + δC); CS = CbS . For
FeO diffusion, at r = r 0MgO ; C F = CFe and at r = (r 0MgO +
δM); C F = CFb (see Fig. 1a). Eqs. 1 and 2 are used to find
the molar flux of CaO and MgO particle dissolution
from the molar fluxes of SiO2 and FeO into the cal-
cined dolomite flux particle, integrating over the vari-
ables of change in radius of the particle with respect
to change in time. The rate equations for slag-film
diffusion control results in the fractional dissolution
(f ) of CaO and MgO being given as Eq. 10.
The general rate equation for dissolution of CaO
and MgO present from a calcined dolomite particle
under slag-film diffusion control may be given as: f =
kcsf .t where kcsf is defined as the rate constant for slag-
film diffusion (m/second) for a cylindrical particle
Equations 10, 11
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JAN 2023
and is the diffusion time of SiO2 and FeO into their
respective CaO and MgO particle(s).
In a similar manner, the rate equations for the
product-layer diffusion control may be obtained,
using the appropriate boundary conditions: for SiO2
diffusion, at r = rCaO ; CS = CSe and at r = r 0CaO ; CS = CbS
and for FeO diffusion: at r = rMgO ; C F = CFe and at r =
r 0MgO ; C F = CbF . The fractional dissolution (f ) of CaO
and MgO from a cylindrical particle is given in Eq. 11.
The general rate equation for dissolution of CaO
and MgO present in the calcined dolomite flux par-
ticle under product-layer diffusion control may be
given as: f + (1 – f )ln(1 – f ) = kcpl.t where kcpl is the rate
constant for product-layer diffusion for a cylindrical
particle (m/second) and is the diffusion time of SiO2
and FeO into their respective CaO and MgO particles.
The rate equations for interfacial reaction control
for dissolution of CaO and MgO in steelmaking slag
may be obtained as shown in Eqs. 12 and 13.
Integrating over the variable of change in radius of
the particle with respect to change in time, the rate
equations for the interfacial reaction control may be
obtained. The fractional dissolution of CaO and MgO
is given in Eq. 14.
(Eq. 10)
(Eq. 11)

Equations 12–15
The general rate equation for dissolution of CaO
and MgO present in the calcined dolomite flux par-
ticle under interfacial reaction control may be given
as: 1 – (1 – f )1/2 = kcir.t where kcir is the rate constant
for interfacial reaction of a cylindrical particle (m/
second) and t is the reaction time (seconds).
By combining all the three steps in series and rear-
ranging the terms, one can get the algebraic form of
the mixed-control rate equation for dissolution of a
cylindrical calcined dolomite particle in steelmaking
slag as shown in Eq. 15.
Dissolution of Spherical Calcined Dolomite Particles: The dis-
solution rates of spherical particles can similarly be
found shown in Eqs. 16–19.
Eq. 16 shows the dissolution rate for slag-film diffu-
sion control. This can be written as f = kssf .t where kssf is
the rate constant of slag-film diffusion for a spherical
particle (m/second).
241
(Eq. 12)
(Eq. 13)
(Eq. 14)
(Eq. 15)
Eq. 17 shows the dissolution rate for product-layer
diffusion control. This can be written as: 1 – 2/3f –
(1 – f )2/3 = kspl.t where kspl is the rate constant for prod-
uct-layer diffusion for a spherical particle (m/second).
Eq. 18 shows the dissolution rate for interfacial reac-
tion control. This can be written as: 1 – (1 – f )1/3 = ksir.t
where ksir is the reaction rate constant for interfacial
reaction of a spherical particle (m/second) and t is
the reaction time (seconds).
JAN 2023
The mixed-control rate equation for spherical par-
ticles dissolving in steelmaking slag is then given in
I IRON & STEEL TECHNOLOGY I AIST.ORG
Eq. 19.
Dissolution of Cylindrical and Spherical Calcined Magnesite
Particles: Following similar concepts as for dissolution
of calcined dolomite particles, the mixed-control
model for dissolution of cylindrical and spherical
calcined magnesite particles (Figs. 1c and 1d) can
be developed by considering FeO as the only dif-
fusing species into the MgO particle. The resulting
242 AIST Transactions
Equations 16–19
I IRON & STEEL TECHNOLOGY I AIST.ORG
mixed-control model equations are shown in Eqs. 20
and 21.
In these expressions, Ci is the molar concentration
SiO2 and FeO (mol/m3), J*i is the molecular flux in
the ith direction (mol/m2.s), r 0CaO and r 0MgO are the
JAN 2023
initial radius of the CaO and MgO flux particle (m), t
is the dissolution time (seconds), CbS , CFb and CeS , CFe are
(Eq. 16)
(Eq. 17)
(Eq. 18)
(Eq. 19)
the molar concentrations of SiO2 and FeO in the bulk
and at the interfaces between the C2S and MF' solid
solution phases and the slag film (mol/m3), δC and
δM are the concentration boundary layer thickness
around the CaO and MgO particles (m), DS , DF and
DpS , DpM are the diffusivity of SiO2 and FeO in the slag
and in C2S and MF' solid solution phases respectively

(m2/second), rS is the apparent density of flux particle
(kg/m3), and kCf and kMf are the modified forward reac-
tion rate constant for the reactions 2CaO(s) + SiO2 =
2CaO.SiO2 (i.e. C2S) and MgO(s) + FeO = MgO.FeO
(i.e. MF') respectively (m/second).
Estimation of Model Parameters
In the present study, the concentration boundary
layer thickness (δi) was estimated as a function of slag
properties using the empirical formula of Kosaka et
al.47 They reported the correlation for dissolution of
a rotating steel cylinder into liquid Zn and Al as: δi =
4.76dS1.5NRe–0.62NSC
–0.35 where N , N
SC Re and NSh are the
Schmidt number, Reynolds number and Sherwood
number, respectively, and dS is the cylinder diameter.
The Ranz-Marshall’s48 correlation is used for dissolu-
tion of spherical particles: NSh = 2.0 + 0.6NRe1/2. By
applying the definitions of these dimensionless num-
bers the concentration boundary layer thickness (δi)
can be estimated as a function of slag properties as:
d S/δ = 2.0 + 0.6η –1/6r 1/6D –1/3ϑ 1/2 where D is the dif-
i s s i k i
fusivity of SiO2 in CaO (DS) and C2S (DpS) and diffu-
sivity of FeO in MgO (DF) and MF' (DpF), respectively.
The temperature dependence of diffusivity was
assumed to follow an Arrhenius relationship with
temperature: Di or Dpi = D 0exp(– Ed/RT) where D 0 is
the pre-exponential factor (m2/second), Ed is the
activation energy for diffusion of SiO2 and FeO in
slag (kcal/mol), and T is the temperature of slag (K).
The diffusivity at 1,500°C was calculated using the
correlation of Dolan et al.49 Due to unavailability of
data in the literature for diffusion of SiO2 into the C2S
solid solution and FeO into the MF' solid solution, it
is assumed that (DpS = DS/2) (for diffusion of SiO2 into
C2S) and (DpF = DF/2) for diffusion of FeO into MF', to
obtain good agreement between model predictions
and experimental values. This assumption seems to
be valid because the formed C2S de-polymerizes the
silicate structure forming more stable and simple
silicate ions as SiO44–, thereby reducing the Si/O ratio
to a smaller value of 1/4, which reduces the mobil-
ity or diffusion coefficient of SiO2 in the C2S solid
solution.50 For the case of FeO diffusion into MF'
the growth of MF' involves counterdiffusion of Fe2+
and Mg2+ ions.51–53 MF' has a rock-salt structure with
two fcc lattices, one consisting of the O2- anions and
the other consisting of Fe2+ and Mg2+ cations. In this
structure, the mobility of O2- anions is small, due to its
larger size in comparison to that of either Fe2+ or Mg2+.
Therefore, the diffusion of O2- anions is very slow or
the diffusion coefficient of FeO in MF' is smaller.51
The C2S solid solution is monoclinic with an atomic
packing factor of 0.25, much less than in the rock salt
structure of MF' solid solution (atomic packing factor
243
of 0.79), contributing to the smaller diffusivity of FeO
into MF' compared with that of SiO2 into C2S.
The viscosity of slag was estimated with Urbain’s
viscosity model54 as: ηs = ATexp(1000.B/T) where A and
B are constants found from an empirical relationship.
The activity coefficients of SiO2 and FeO in steel-
making slag was estimated with the regular-solution
model proposed by Ban-ya et al.55 as: RTlnγi = ΣjaijX 2j +
ΣjΣk(aij + aik – ajk)XjXk + I ' where γi is the activity coef-
ficient of ith component in the slag, Xi , Xj and Xk were
the cation fraction of ith, jth and kth components in
the slag, and aij, aik and ajk are the interaction ener-
gies between (i cation)-O-(j cation), (j cation)-O-(k
cation) and (i cation)-O-(k cation), and I ' is the con-
version factor of activity coefficient from the hypo-
thetical regular solution and a real solution.
Results and Discussion
The algebraic Eqs. 15, 19, 20 and 21 were solved to
get the fractional dissolution (f ), using computer
code written in MATLAB® 2018 a. The driving force
for SiO2 and FeO diffusion was estimated for the
CaO-SiO2-FeO ternary system by considering inter-
sections between the liquidus line and a straight line
to C2S. The thermodynamic data used in the model
calculations has been adopted from the standard data
sources.56
For validation of the model, predicted dissolution
of cylindrical calcined dolomite and calcined mag-
nesia particles dissolution was modeled for the slags
given in Table 1 and compared with experimental
data of Umakoshi et al.31,32 For dissolution of spheri-
cal calcined dolomite and calcined magnesite par-
ticles in steelmaking slag during the BOF steelmak-
ing, slags shown in Table 2 were used for comparison
with the plant operating data of Cicutti et al.45 The
input parameters to the model are given in Table 3.
Furthermore, a complete analysis and discussion has
Table 1
Slag Composition Used in the Present Model for
Dissolution of Cylindrical Geometry Magnesia-Based Flux
JAN 2023
Slag composition (wt. %) Umakoshi et al.31,32
Slag No. FeO CaO SiO2 Basicity
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A 20 40 40 1.0
B 30 35 35 1.0
C 40 30 30 1.0
D 50 25 25 1.0
E 60 20 20 1.0
F 70 15 15 1.0
G 20 30 50 0.6
244 AIST Transactions

Table 2 been made regarding the predicted magnesia flux

dissolution compared with operating trial data from
Slag Composition Used in the Present Model for
Dissolution of Spherical Geometry Magnesia-Based Flux
the Visakhapatnam Steel Plant as illustrated in Fig. 2.
Slag composition during the blow (wt. %) Cicutti et al.45
Blow Effect of Process Variables on the Dissolution Rate of Magnesia-
time CaO FeO SiO2 Basicity Based Flux — The effect of process variables such as
2 31 47 22 1.4 temperature, revolution speed, slag composition and
4 31 44 25 1.2
porosity present in the magnesia-based flux particles
on dissolution rate of calcined dolomite and calcined
7 38 37 25 1.5
magnesite in BOF model slag available in the litera-
10 47 24 29 1.6 ture is illustrated in the following section.
12 50 24 27 1.9
15 52 29 19 2.8
Effect of Temperature on Dissolution Rate: The effect of
temperature on fractional dissolution of calcined
18 53 28 19 2.9
dolomite and calcined magnesite has been predicted
for comparison with experimental data of Umakoshi
et al.1,2 as given in Fig. 3 for slag A (20 wt. %FeO-40 wt.
%CaO-40 wt. %SiO2), apparent porosity of φ = 24.85%
Table 3
and speed of revolution of 200 r.p.m., and tempera-
Input Parameters Used in the Present Mixed-Control Model tures of 1,350, 1,375, 1,400 and 1,425°C. The figures
Parameters Units Values show increased dissolution rates of calcined dolomite
Initial radius of cylindrical calcined dolomite and calcined magnesite with increased temperature;
m 0.0009
and calcined magnesite particles (r0) in all the cases the predicted dissolution rate of cal-
Length of cylindrical calcined dolomite and cined dolomite is higher than the experimental data
m 0.03 of Umakoshi et al.31 The error was calculated as the
calcined magnesite particles (L)
Modified forward reaction rate constant for the
root mean square error (RMSE) as:
3.2 x 10-4 and
reaction CaO with SiO2 and MgO with FeO (kCf moles/sec
1.5 x 10–3
and kMf )
Activation energy for SiO2 and FeO diffusion 58.45 and
kcal/mol
in slag (Ed) 71.00
Diffusivity of SiO2 and FeO through a solid D pS = DS/2 and
m2/sec (Eq. 20)
solution of C2S and MF' D pF = DF/2

where

Figure 2 ŷ 1, ŷ 2, ŷ 3, …. = the predicted values,

y1, y2, y3, …. = the measured values and
n = the number of observations.

The estimated errors for calcined dolomite disso-

lution were 0.78, 0.83, 0.66 and 0.69 for the case of
temperatures 1,350, 1,375, 1,400 and 1,425°C, respec-
tively. For calcined magnesite dissolution at the same
temperatures the errors are 0.34, 0.19, 0.14 and 0.15.
A reason for overestimation of calcined dolomite
dissolution may be an error in the prediction of the
I IRON & STEEL TECHNOLOGY I AIST.ORG

boundary layer thickness dC and dM for the formation

of C2S and MF' around the CaO and MgO particles;
it may also be due to incorrect estimation of diffusion
coefficients of SiO2 and FeO (DS (also DpS) and DF (also
DpM)) from Dolan et al.49
The model prediction of the dissolution of calcined
magnesite agrees with the experimental data of
Umakoshi et al.32 The model variables such as C, CeS ,
Ternary plot of CaO-FeO-SiO2 showing slag evolution data of CeF, γi , kCf , kMf, DS (also DpS), DF (also DpM), ϑk , δC , δM and
JAN 2023

Visakhapatnam steel plant. rS depend on temperature. However, over the range of

temperature considered the values of C and rS do not
 245
Figure 3
2.5 3.0
Present model: Calcined Dolomite Present model: Calcined Dolomite
Umakoshi et al.: Calcined Dolomite Umakoshi et al.: Calcined Dolomite
Decrease in Flux Particle Radius (mm)

Decrease in Flux Particle Radius (mm)

Present model: Calcined Magnesite Present model: Calcined Magnesite
Umakoshi et al.: Burnt Magnesite 2.5 Umakoshi et al.: Burnt Magnesite
2.0
Slag A; 1,350°C; 200 rpm; ϕ 24.85% Slag A; 1,375°C; 200 rpm; ϕ 24.85%

2.0
1.5

1.5

1.0
1.0

0.5
0.5

0 0
0 10 20 30 40 50 0 10 20 30 40 50
Immersion Time (min) Immersion Time (min)
(a) (b)
3.5 4.0
Present model: Calcined Dolomite Present model: Calcined Dolomite
Umakoshi et al.: Calcined Dolomite Umakoshi et al.: Calcined Dolomite
Decrease in Flux Particle Radius (mm)

Decrease in Flux Particle Radius (mm)

3.0 Present model: Calcined Magnesite 3.5 Present model: Calcined Magnesite
Umakoshi et al.: Burnt Magnesite Umakoshi et al.: Burnt Magnesite

Slag A; 1,400°C; 200 rpm; ϕ 24.85% 3.0 Slag A; 1,425°C; 200 rpm; ϕ 24.85%
2.5

2.5
2.0
2.0
1.5
1.5
1.0
1.0

0.5
0.5

0 0
0 10 20 30 40 50 0 5 10 15 20 25 30 35 40 45
Immersion Time (min) Immersion Time (min)
(c) (d)

Effect of temperature on the model predicted dissolution rate for calcined dolomite and calcined magnesite flux in comparison
with experimental data of Umakoshi et al.:31,32 1,350°C (a), 1,375°C (b) 1,400°C (c), and 1,425°C (d).

change much. Since the interfacial reaction does not km ∝ Di0.65ϑk –0.35
have a significant effect on the overall reaction rate,
the effect of temperature on the reaction rate con- (Eq. 21)
stants, i.e., kCf , kMf have been chosen as constant. The
activity coefficients γS of SiO2 decreases with tempera- The diffusion coefficients DS (also DpS) and DF (also
ture and the activity coefficient γF of FeO increases DpM) increase exponentially with temperature and the
with temperature, whereas CeS and CFe vary a little with kinematic viscosity of slag (ϑk) decreases exponential-
JAN 2023

temperature. However, their combined effect is signif- ly with temperature, both causing the mass transfer
icant role on the driving force for calcined dolomite coefficient (km) to increase. Therefore, the dissolution
I IRON & STEEL TECHNOLOGY I AIST.ORG

(C – CeS) and calcined magnesite dissolution (C – CFe ). rate of both calcined dolomite and calcined magne-
The diffusivity of SiO2 and FeO in the slag, i.e., DS site increases with increased temperature as shown in
(also DpS) and DF (also DpM), the kinematic viscosity of Fig. 3. The dissolution rates of both calcined dolomite
slag (ϑk) and the boundary layer thickness of product and calcined magnesite follow the Arrhenius-type
layers, i.e., δC , δM also vary significantly with tem- relationship with temperature as illustrated in Fig. 4a
perature. These affect the mass transfer coefficient and 4b.
as estimated from the empirical relation of Kosaka et Fig. 4 shows that the predicted temperature depen-
al.47 as follows: dence of the dissolution rate for calcined dolomite and
calcined magnesite is comparable to experimental
246 AIST Transactions
Figure 4
-5.80 -6.1
Dissolution rate (log(-dr/dt)): Model prediction Dissolution rate ((-dr/dt)): Model ...
-5.85 Dissolution rate (log(-dr/dt)): Umakoshi et al. Dissolution rate ((-dr/dt)): Umakoshi et al.
Dissolution Rate (log(-dr/dt)) (m/s)

Dissolution Rate (log(-dr/dt)) (m/s)

-5.90

-5.95
-6.2
-6.00

-6.05

-6.10
-6.3
-6.15

-6.20

-6.25

-6.30 -6.4
5.80 5.85 5.90 5.95 6.00 6.05 6.10 6.15 6.20 5.85 5.90 5.95 6.00 6.05 6.10 6.15 6.20
(1/T) x 10 (1/K)
4
(1/T) x 104 (1/K)

(a) (b)

Model prediction results for the effect of temperature on dissolution rate of calcined/burnt dolomite (a) and calcined/sintered
magnesite (b), compared with experimental data of Umakoshi et al.31,32

data, reflecting to equivalent activation energy (Ed) Effect of Revolution Speed on Dissolution Rate: The revo-
in the model prediction and the experimental data of lution speed of the magnesia flux samples in the
Umakoshi et al.31,32 The model predicted the effective molten slag can be directly related to the boundary
activation energy for dissolution of calcined dolomite layer thickness (δC) and (δM) as described in model
to be 43 kcal/mol and that of calcined magnesite to Eqs. 15 and 19. The effect of revolution speed on the
be 45 kcal/mol, compared with the activation energy fractional dissolution (f ) of calcined dolomite and
values of 50 and 48 kcal/mol given by Umakoshi et magnesite has been estimated from the present model
al.31,32 The slight difference in these values might be equations and compared with the experimental data
attributed to errors in estimation of diffusion coeffi- of Umakoshi et al.31,32 in Figs. 5a and 5b (for slag A of
cients of SiO2 and FeO, i.e., DS (also DpS) and DF (also composition 20 wt. %FeO-40 wt. % CaO-40 wt. %SiO2,
DpM) from the expressions of Dolan et al.49 apparent porosity of φ = 30.2%, at 1,400°C). It can be

Figure 5
0.6 0.4
Fractional Calcined Dolomite Dissolution (f)

Fractional Calcined Dolomite Dissolution (f)

Model prediction: 400 rpm Model prediction: 400 rpm

Umakoshi et al.: 400 rpm Umakoshi et al.: 400 rpm
Model prediction: 300 rpm
0.5 Model prediction: 200 rpm
Umakoshi et al.: 300 rpm
Model prediction: 200 rpm Umakoshi et al.: 200 rpm
0.3 Model prediction: 100 rpm
Umakoshi et al.: 200 rpm
0.4

0.3 0.2
I IRON & STEEL TECHNOLOGY I AIST.ORG

0.2

0.1
0.1
Slag A; ϕ –30.2%; 1,400°C Slag A; ϕ –30.2%; 1,400°C

0 0
0 10 20 30 40 50 0 10 20 30 40 50 60 70
Immersion Time (min) Immersion Time (min)

(a) (b)
JAN 2023

Model predictions of fractional dissolution of calcined dolomite (a) and calcined magnesite (b) for the rotating cylindrical
samples compared with the experimental data of Umakoshi et al.31,32 at different rotating speeds.

observed from Fig. 5a and 5b that the present model
predicts reasonably good for higher revolution speeds
of 400 and 300 rpm. However, for lower revolution
speeds of 200 and 100 rpm, the model prediction
results are relatively poor as compared to the experi-
mental values although it shows the similar trend. The
estimated RSME for calcined dolomite dissolution
were 0.08, 0.15 and 0.17 for the revolution speeds
of 400, 300 and 200 rpm, respectively, while the
estimated RSME for calcined magnesite dissolution
were 0.03, 0.05 and 0.12 for their revolution speeds
of 400, 200 and 100 rpm, respectively. The reason for
such deviations might be due to error in estimation
of boundary layer thickness (δC) and (δM) for lower
revolution speeds. At low revolution speeds, the value
of boundary layer thickness is expected to be high,
which results in much slower diffusion of SiO2 and
FeO through the slag-film. Under such conditions,
the diffusion in slag film may be the rate-controlling
step. It is interesting to observe from Figs. 5a and 5b
that the difference between the model prediction
results and experimental data of Umakoshi et al.31,32
for the estimation of fractional dissolution rate (f ) of
both calcined dolomite and calcined magnesite fluxes
is less at the highest revolution speed (400 rpm).
Effect of Slag Basicity on the Dissolution Rate: The effect of
slag basicity (wt. % CaO/wt. % SiO2) on the dissolu-
tion rates of calcined dolomite and magnesite is inves-
tigated as illustrated in Fig. 6 for slags A–G as listed in
Table 1: apparent porosity of ϕ = 24.8, speed of revolu-
tion of 200 r.p.m. and 1,400°C. The dissolution of cal-
cined dolomite and calcined magnesite flux particles
depends significantly on activity or concentration
difference of SiO2 and FeO, i.e., the driving force (C –
CeS) and (C – CeF) of the present model Eqs. 15 and 19.
The activity coefficients of both SiO2 (γS) and FeO (γF)
decreases with increase in slag basicity up to certain
extent then it becomes more or less constant. The slag
basicity has a marked effect on the kinematic viscosity
of slag (ϑk). From Fig. 6a it is evident that with increase
in slag basicity from 0.6 to 1 the dissolution rate pre-
dicted by the present model and the experimental
data of Umakoshi et al.31 for both calcined dolomite
and calcined magnesite flux particle decreases. No
experimental data on the effect of slag basicity on the
dissolution rate of calcined dolomite is available for
basicities >1.0, and no experimental data on the effect
of basicity on the dissolution rate of calcined magne-
site is available in Umakoshi et al.32
Effect of Slag FeO Content on the Dissolution Rate: The
activities or concentration of slag components SiO2
and FeO, i.e., the driving force (C – CeS) and (C – CeF),
directly affect the dissolution rate of magnesia flux
particle as shown by Eqs. 15 and 19. The effect of FeO
content of slag on the dissolution rate of calcined
247
dolomite and calcined magnesite has been studied by
keeping basicity constant for the slags A–F as given in
the experimental data of Umakoshi et al.31,32 for an
apparent porosity of ϕ = 25.6 and revolution speed
of 200 r.p.m. at 1,400°C; see Figs. 7a and 7b. With
an increase in the FeO content of the slag, the activ-
ity coefficients of both SiO2 and FeO, i.e., γS and γF
increase (changing their saturation concentrations CeS
and CeF), but the overall effect on the driving force for
dissolution is small. However, the FeO content of slag
has marked effect on the kinematic viscosity of slag
(ϑk), decreasing the kinematic viscosity decreases sig-
nificantly up to 30 wt. % FeO;3 there is no significant
decline in kinematic viscosity with further increases
in FeO content. Thus, the mass transfer coefficient
(km) increases with a decrease in kinematic viscosity
of slag (ϑk) up to 30 wt. % FeO content in slag; after
that it remains almost constant. Figs. 7a and 7b show
that the dissolution rate of calcined dolomite and
calcined magnesite increases when the FeO content
of slag increases in the range of 20–30 wt. %, beyond
which the dissolution rate of calcined dolomite found
to decease (Fig. 7a); the dissolution rate of calcined
magnesite flux particle becomes more or less constant
beyond 30% FeO (in Fig. 7b). The reason behind it
might be an in the solid boundary layer thickness δM
with increasing %FeO, and increasing (%FeO) in the
magnesiowüstite (MF').40 However, the experimental
data of Umakoshi et al.31,32 shows a generally increas-
ing dissolution rate for burnt magnesite in the range
of 20–40 wt. % FeO. A possible reason for the discrep-
ancy might be slight errors in the estimation of satura-
tion concentrations of SiO2 and FeO from the CaO-
SiO2-FeO ternary diagram for FeO concentrations
Figure 6
4.0
Model predictions for cal. dolomite
Umakoshi et al.
Dissolution Rate (-dr/dt) x 106 (m/s)
3.5 Model predictions for cal. magnesite
Slag A B
FeO 20 30 40 50
C D E F G
60 70 20
3.0
CaO 40 35 30 25
SiO2 40 35 30 25
20 15 30
20 15 50
2.5 Umakoshi et al.31,32
2.0
JAN 2023
1.5
1.0
I IRON & STEEL TECHNOLOGY I AIST.ORG
0.5
0
0.5 0.6 0.8 0.9 1.0 1.1 1.3
Basicity (wt.% CaO/wt.% SiO2)
Model predictions of the effect of slag basicity on dissolution
rate of calcined dolomite and calcined magnesite compared
with the experimental data of Umakoshi et al.31,32
248 AIST Transactions
Figure 7
2.5
(-dr/dt) Model prediction 1.4 (-dr/dt) Model prediction
(-dr/dt) Umakoshi et al. (-dr/dt) Umakoshi et al.
Dissolution Rate of Calcined Dolomite

Dissolution Rate of Calcined Dolomite

2.0
1.1
(-dr/dt) x 106 (m/s)

(-dr/dt) x 106 (m/s)

1.5

0.8
1.0

0.5
0.5

0 0.2
10 20 30 40 50 60 70 80 15 25 35 45 55
wt.% FeO in Slag wt.% FeO in Slag

(a) (b)

Model predictions for the effects of FeO content of slag on dissolution of calcined dolomite (a) and calcined magnesite (b)
compared with the experimental data of Umakoshi et al.31,32

above 30 wt. %. Further investigation of these devia- (f ) of these fluxes with the experimental data of
tions is necessary. Umakoshi et al.31,32 for porosity levels of 20, 24.4, and
30.4% for slag A *20 wt. %FeO-40 wt. % CaO-40 wt.
Effect of Flux Particle Porosity on Dissolution Rate: The effect %SiO2), speed of revolution of 200 r.p.m., and 1,400°C
of flux particle porosity (ϕ) on the dissolution of cal- as illustrated in Fig. 8.
cined dolomite and calcined magnesite in terms of The experimental work of Umakoshi et al.31,32
their fractional dissolution rate (f ) can be related to showed that the dissolution mass flux hardly changed
the apparent density of the particle (rS) that appears with increasing apparent porosity (ϕ); the dissolution
in model Eqs. 15 and 19. The effect of different par- rate increased by only 20%. The stated reason was
ticle porosity (ϕ) levels has been studied by comparing the increase in penetration of molten slag into burnt/
the model predicted values of fractional dissolution calcined dolomite samples with increase in apparent

Figure 8
0.7 0.40
Fractional Dissolution of Calcined Dolomite (f)

Fractional Dissolution of Calcined Magnesite (f)

Model prediction: 200 rpm, ϕ = 20% Model prediction: 200 rpm, ϕ = 28.2%
Umakoshi et al.: 200 rpm, ϕ = 20% Umakoshi et al.: 200 rpm, ϕ = 28.2%
0.6 0.35 Model prediction: 200 rpm, ϕ = 13%
Model prediction: 200 rpm, ϕ = 24.4%
Umakoshi et al.: 200 rpm, ϕ = 24.4% Umakoshi et al.: 200 rpm, ϕ = 13%
Model prediction: 200 rpm, ϕ = 30.4% 0.30
0.5 Umakoshi et al.: 200 rpm, ϕ = 30.4%

0.25
0.4
0.20
0.3
I IRON & STEEL TECHNOLOGY I AIST.ORG

0.15

0.2
0.10

0.1 0.05

0 0
0 5 10 15 20 25 30 35 40 45 0 10 20 30 40 50 60 70 80
Immersion Time (min) Immersion Time (min)
(a) (b)
JAN 2023

Effect of apparent porosity (ϕ) on the dissolution of calcined dolomite (a) and calcined magnesite (b) compared with the
experimental data of Umakoshi et al.31,32

porosity (ϕ). However, micrographs of their samples
show little penetration of slag into the samples
of burnt dolomite. The present model prediction
results also show a slight increase in dissolution with
increased porosity in the range of 20–30%, for cal-
cined dolomite (Fig. 8a) but not for calcined magne-
site (Fig. 8b). This may be due to the formation of con-
tinuous magesiowüstite (MF') layer upon exposure of
the calcined magnesite to the slag.
Conclusions
In the present investigation of the dissolution of
magnesia-containing flux in steelmaking slags, a
mixed-control kinetic model has been developed by
taking into account the dissolution variables such as
slag composition, temperature and stirring intensity.
The model predictions provide better insight and
quantitative estimation of flux dissolution by consid-
ering all the factors affecting the dissolution. The
following conclusions can be drawn from the present
investigation:
1. The dissolution rate of both the calcined
dolomite and calcined magnesite increases
with an increase in temperature, for constant
slag composition and stirring intensity. The
apparent activation energy for dissolution
of calcined dolomite and calcined magne-
site were found to be 43 and 45 kcal/mol,
respectively.
2. The dissolution rate of both calcined dolo-
mite and calcined magnesite increases with
an increase in stirring speed. However, it was
also found that their dissolution decreases
with increasing slag basicity.
3. The effect of the FeO content of the slag on
the dissolution rate of calcined dolomite and
calcined magnesite flux by keeping the basic-
ity of slag as a constant parameter has been
investigated and found that, with an increase
in FeO content of slag up to 30 wt. %, the dis-
solution of calcined dolomite and calcined
magnesite increases due to a decrease in
kinematic viscosity (ϑk), which results in an
increase of the mass transfer coefficient (k m).
However, with a further increase in FeO con-
tent of the slag beyond 30 wt. %, the impervi-
ous magnesiowüstite (MF') layer thickness
increases, thereby decreasing the dissolution
of both calcined dolomite and calcined mag-
nesite in the steelmaking slag. Furthermore,
the effect of variations in the flux particle
porosity on their is negligible, both for the
present mixed-control prediction model and
the experimental work of Umakoshi.
249
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51. W.E. Ranz and W.R. Marshall Jr., Chem. Eng. Prog., Vol. 48, 1952, pp. 173–
180.

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