ISIJ International, Vol. 50 (2010), No. 6, pp.

797–803

Interfacial Phenomena in Metal–Slag–Gas System during AOD

Process

Timo FABRITIUS,1) Jaana RIIPI,1) Mika JÄRVINEN,2) Olli MATTILA,1), Eetu-Pekka HEIKKINEN,1) Aki KÄRNÄ,1)
Jari KURIKKALA,1) Petri SULASALMI1) and Jouko HÄRKKI1)

1) Laboratory of Process Metallurgy, University of Oulu, P.O.Box 4300, FIN-90014 Finland.

2) Helsinki University of Technology, Department of Energy Technology, Energy Engineering and Environmental Protection,
P.O. Box 4400, 02015 TKK, Finland.
(Received on June 29, 2009; accepted on March 8, 2010 )

Significance of interfacial phenomena and properties such as surface tension are essential in iron and
steelmaking processes due to chemical reactions occurring on the interfaces including elements transfer
through the phase boundaries. In this study, the influences of surface tensions of slag and metal and interfa-
cial tension between slag and metal on the behavior of metal–slag–gas system were analysed based on the
energy bound to system surfaces. Effects of reactions between slag and steel on the behavior of
metal–slag–gas system during AOD process were evaluated by two cases: evaluation of top slag–steel melt
system and single bubble rising in the metal bath.
Simulations for metal–top slag system show that there are no possibilities to form metal film around the
gas bubbles when they penetrate through metal–slag interface. Behavior of system is also independent of
intensity of reactions between slag and steel. According to the calculations during intensive metal–slag re-
actions metal droplets are disintegrated more easily into top slag layer. If there are no metal–slag reactions
metal droplets are attached into the gas bubbles.
Calculations prove that, when reactive oxygen gas bubble forming oxides is injected into steel bath, slag
film can be formed around the gas bubble if the intensity of reactions between the slag and the metal is
high. During effective oxidation reactions at the vicinity of nozzles formed micro slag is attached with the ris-
ing gas bubble.
KEY WORDS: interfacial tension; surface tension; metal–slag–gas system; interfacial phenomena; flotation;
film formation.

face during reactions weakens the balance between the

1. Introduction
Significance of interfacial phenomena properties are es-
sential in iron and steelmaking processes since most of the
chemical reactions are heterogeneous and thus involve sep-
arate phases that are divided by phase boundaries through
which the elements must transfer.
In order to succeed in the production effectiveness, phys-
ical interactions on metal–slag–gas boundary are necessary
to understand. Although the equilibrium interfacial tension
plays an essential role while considering the phenomena on
the metal–slag–gas interface, it is equally important to be
familiar with the surface properties of individual phases
(i.e. surface tension) and the effect of reactions on system
in order to understand the behavior of considered sys-
tems.1,2) Minto and Davenport3) and El Gammal et al.4) have
analyzed behavior of metal droplets in liquid slag layer by
minimization of the interfacial energy but they have only
focused on the equilibrium conditions.
According to the literature, reactions in the gas–metal5–7)
and metal–slag8–13) interface can influence dramatically on
the value of interfacial tension between studied phases de-
pending on the reaction rate. Mass transfer across the inter-
phases at the interface. Kapilashrami et al.5–7) studied the
effect of reaction between CO–CO2–Ar atmosphere and liq-
uid iron on the interfacial phenomena using silica, corun-
dum and mullite as substrates. Ooi et al.8) studied effect of
reaction on the interfacial tension between CaO–SiO2–
Al2O3 slag and carbon saturated iron containing sulfur.
They measured 0.5 N/m decrease in interfacial tension
when rate of sulfur transfer is more than 3 · 10⫺6
mol/min/cm2. During intensive mass transfer between the
slag and the metal, the interfacial tension decreased to very
low value and remained low level until the system ap-
proached its chemical equilibrium.8) Riboud and Lucas9) re-
searched reactions between slag and iron containing oxidiz-
able alloying elements (Al, Ti, Si and Cr) and found out
that dynamic interfacial tension tends to zero when oxygen
flow is more than 0.1 mol/m2/s. Dynamic interfacial tension
during reaction between Fe–Al alloy and CaO–SiO2–Al2O3
slag was 0.274–0.44 N/m lower than equilibrium value ac-
cording to the Rhamdhani et al.12)
Since the reactions have an essential role when consider-
ing the interfacial phenomena in metallurgical metal–slag–
gas systems, it is necessary to take the influence of reac-

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 ISIJ International, Vol. 50 (2010), No. 6
tions into account when modeling the processes (e.g. AOD
process). Therefore, the purpose of this work was to study
the influence of chemical reactions on the interfacial phe-
nomena occurring in metal–slag–gas system during AOD
process. The behaviour of three-phase system was analysed
based on the energy bound to the system surfaces. Surface
tension of slag14) and metal15) were calculated using previ-
ously published models and determination of interfacial
tension between slag and steel based on Girifalco and
Good’s16) equation.
2. AOD Process
Argon Oxygen Decarburization (AOD) is a process
which main function is carbon removal from melt. This is
done in AOD converter by means of blowing oxygen con-
taining gas from bottom nozzles, and in some stages of the
process, also from top lance. In bottom blowing a diluting
gas (argon and nitrogen) is used to lower the partial pres-
sure of carbon monoxide, thus making carbon removal
more efficient. Carbon and chromium contents of the stain-
less steel as a function of blowing time in the AOD process
are presented in Fig. 1. It is seen from Fig. 1 that decarbur-
ization takes place in four stages. The final stage of the
Table 1. Composition of injected gas during AOD process.17)
Fig. 1. Change of metal phase composition during processing of austenitic stainless steel in AOD.17)
Table 2. Typical compositions of the stainless steel and the slag in AOD process. Estimated compositions of top slag during decarbur-
ization are marked with *.
© 2010 ISIJ
AOD process is the combined desulphurization and reduc-
tion of the slag in which the oxidized chromium is reduced
from the slag with ferrosilicon or ferromanganese during
argon injection. Used ratios between oxygen and inert gas
are presented in Table 1.
Compositions of the top slag and the stainless steel melt
in AOD process are presented in Table 2. Progress of the
composition of top slag during decarburization was esti-
mated based on the literature18) but the final composition of
top slag was measured.
3. Metal–Slag–Gas System
Three-phase system including gas, metal and slag is
formed when gas is injected into liquid bath during AOD
process. Depending on the interfacial energies of the sys-
tem there exists either stable surface film or ruptured sur-
face film when gas bubble penetrates metal–slag interface.
Ruptured surface film generates droplets which can be
attached with gas bubbles or they can be disintegrated
depending on the interfacial tensions.3) Stability of the film
is described by film coefficient (Q ) and droplets attach-
ment with gas bubble by flotation coefficient (D).3,4) Coeffi-
cients are evaluated in detail in the study of Minto and
Davenport.3)
Behavior of metal–slag–gas system was analyzed based
on the energy bound to the system surfaces. Non-turbulent
circumstances in the bath where metal, slag and gas are in
contact were assumed.3,4) Behavior of three-phase system in
the AOD was studied by two cases: A) evaluation of top
slag–steel melt system and B) evaluation of single bubble
rising in the metal bath (Fig. 2).
798
 ISIJ International, Vol. 50 (2010), No. 6
3.1. Top Slag–Metal System
Metal droplets can be entrained into the slag phase when
gas bubbles pass through the molten metal–slag interface.
The behavior of system when metal droplets are suspended
into liquid slag (situation A) can be divided into three types
according to the Fig. 3.
Case A1
The gas bubble delivers metal film into the slag layer if
film coefficient (Q m) is bigger than zero according to the
Eq. (1).3,4)
Q m⫽s slag–gas⫺s metal–gas⫺s metal–slag⬎0 ............(1)
where s slag–gas, s metal–gas and s metal–slag are surface tension of
slag and metal and interfacial tension between metal and
slag, respectively.
Case A2
The metal film ruptures and forms droplets that are at-
tached to gas bubble when the flotation coefficient (D m) is
bigger than zero (Eq. (2)).3,4)
D m⫽s slag–gas⫺s metal–gas⫹s metal–slag⬎0 .............(2)
Case A3
The metal film ruptures and disperses into the slag layer
Fig. 2. Schematic picture of studied cases: A) top slag–metal
system and B) single gas bubble rising in liquid steel
bath.
Fig. 3. Schematic picture of metal droplets suspended into liquid slag.
Fig. 4. Schematic picture of slag droplets that are emulsified into liquid metal.
799
when flotation coefficient is lower than zero (i.e. D m⬍0).
3.2. Single Gas Bubble Rising in the Metal Bath
When oxygen is injected through the submerged nozzles
into the stainless steel bath it reacts forming metal oxides
(micro slag) and CO gas. Behavior of micro slag droplets in
liquid metal (situation B) can be evaluated using the above-
mentioned approach. Mathematical descriptions of cases
(B1–B3) are presented in Eqs. (3)–(5) and described in Fig.
4.
Slag film forms around the gas bubble if Q s⬎0 (B1)3,4):
Q s⫽s metal–gas⫺s slag–gas⫺s metal–slag⬎0 .............(3)
Slag droplets attach to gas bubble during flotation when
D s⬎0 (B2)3,4):
D s⫽s metal–gas⫺s slag–gas⫹s metal–slag⬎0..............(4)
Slag droplets disperse into the metal bath without coales-
cence to bubble when D s⬍0 (B3)3,4):
D s⫽s metal–gas⫺s slag–gas⫹s metal–slag⬍0..............(5)
4. Modeling of Interfacial Properties of Metal–Slag–
Gas System
4.1. Surface Tension of Metal
In the present work, the surface tension of metal includ-
ing surface active elements oxygen, sulfur and nitrogen has
been calculated using modified form of Butler’s equation.19)
Butler’s equation uses the concepts of equating the chemi-
cal potential of a component on the interface to that of the
bulk phase added with the value of the surface energy. It
can be expressed as
RT ⎛ aim ⎞
σ metal–gas ⫽ σ i0 ⫹ ln ⎜ ⎟ ..................(6)
Si ⎝ ai ⎠
where s i0 is the surface tension of the pure component i, aim
is the activity of the surface component i and ai is the activ-
ity of the component i of the bulk phase, Si is the molar sur-
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 ISIJ International, Vol. 50 (2010), No. 6

face area of the component i, T is temperature and R is the ⫺ ΔGmetal–slag

a

molar gas constant. Used model for Fe–O–S–N system has Φ⫽ ................(12)
[ΔGmetal–gas
c
⋅ ΔGslag–gas
c
]0.5
been presented in detail in the previous work.15)
DG ametal–slag is free energy of adhesion between the metal
4.2. Surface Tension of Slag and the slag. DG metal–gas
c
and DG slag–gas
c
are geometric mean
Surface tension model for oxide system derived by of free energy of cohesion of the separate metal and slag
Tanaka et al.14) are based also on the Butler’s equation.19) phases respectively. Interaction between two phases is de-
The model considers the ratio of the ionic radii of the com- scribed by the proportionality factor (F ) in Eq. (12). F is
ponents as the model parameters and uses surface tension a semi-empirical correction factor and it in general varies
and molar volumes of pure oxide components. The model between 0.32 and 1.15 but for most liquids between 0.55–
can be extended to calculate the surface tension of molten 0.75.16) Higher value of the proportionality factor (F ) indi-
multi-component slag. In this work the model was applied cates a stronger attraction between the phases. Cramb and
to the calculation of the surface tension of oxide melts as a Jimbo13) have developed model for SiO2–CaO–Al2O3 and
function of chemical composition. CaO–CaF2–Al2O3 slags which provides 0.5–0.6 values for
The surface tension (s slag–gas) of the AX–BY–CZ molten F with typical metallurgical slag compositions. According
slag can be calculated as follows to the study of Gay et al.21) the proportionality factor (F )
varies between 0.4–0.6 for SiO2–CaO–Al2O3–CaF2 system.
RT Ms If FeO is added into the slag, F increases in which case the
σ slag–gas ⫽ σ AX
0
⫹ ln AX .................(7)
AAX b
M AX maximum value of F ⫽0.82 is achieved with very high FeO
contents.13) Tanaka and Hara22) have found out for steel–
RT Ms slag system that F is related to FeO content by Eq. (13).
σ slag–gas ⫽ σ BY
0
⫹ ln BY
b
.................(8)
ABY M BY
F ⫽0.5⫹0.3 · XFeO...........................(13)
RT Ms
σ slag–gas ⫽ σ CZ
0
⫹ ln CZ
b
..................(9) Where XFeO is mass fraction of FeO in slag. Combining the
ACZ M CZ Eqs. (1) and (2) with the Eqs. (11) and (13), the film coeffi-
( RA / RX ) ⋅ N AX
s/b cient (Q m) and the flotation coefficient (D m) for the metal in
s/b
M AX ⫽ the top slag layer (Case A) during AOD process can be pre-
( RA / RX ) ⋅ N AX
s/b
⫹( RB / RY ) ⋅ N BY
s/b
⫹( RC / RZ ) ⋅ N CZ
s/b
sented by Eqs. (14) and (15).
.........................................(10)
Q m⫽(1⫹0.6 · XFeO)[s metal–gas · s slag–gas]0.5⫺2s metal–gas
Equations for MBY and MCZ, in the bulk and surface, can be .........................................(14)
formulated equally.
The symbols presented in Eqs. (7)–(10) are as follows: D m⫽2s slag–gas⫺(1⫹0.6 · XFeO)[s metal–gas · s slag–gas]0.5
s i0 represents the surface tension of pure component i; .........................................(15)
equals N01/3Vi2/3 (N0 is Avogadro’s number and Vi represents
the molar volume of pure component i); T is absolute tem- Film coefficient (Q s) and the flotation coefficient (D s) for
perature; R is gas constant; NiP is a mole fraction of compo- the slag in the metal bath (Case B) can be presented respec-
nent i in either bulk (P⫽bulk) or surface (P⫽surface); and tively using the Eqs. (3), (4), (5), (11) and (13).
the ionic radius fractions MiP can be calculated using Eq.
(10). Subscripts A, B and C represent cations, whereas sub- 4.4. Validation of Presented Approach
scripts X, Y and Z represent anions. Superscript s indicates Validity of the presented approach was tested by using
surface and b indicates bulk. RA and RX are radii of cations laboratory measurements made by Han and Holappa.23)
and anions, respectively. Superscript 0 indicates properties They have studied iron entrainment mechanism into slag
of pure molten components. Modeling of the surface ten- due to the rising gas bubbles. They analyzed behavior
sion of multi component oxide melts has been presented in of metal–slag system in the laboratory scale under argon
the previous study.20) gas injection by X-ray imaging method. Metal (contain-
ing 4 ppm C, 8 ppm S and 100 ppm O) was covered by
4.3. Slag–Metal Interfacial Tension 50%Al2O3–50%CaO slag. They presented that surface ten-
Interfacial tension between slag and metal is calculated sion of metal was 1.7 N/m and interfacial tension between
using Girifalco and Good’s equation which is shown in Eq. metal and slag was 1.27 N/m calculated by Cramb’s equa-
(11). Girifalco and Good16) consider the interfacial tension tion.13) They have also estimated from literature that the
between two liquids to be due to London dispersion forces surface tension of slag is 0.55 N/m. They observed that
and postulated that free energy of adhesion between the flu- when a bubble hit the interface it rested under the interface
ids might be given by geometric mean of free energy of co- for a shorter or longer time depending on its size. During
hesion.13) the resting time the bubble was still covered by a thin metal
film. The bubble finally broke through the interface at the
s metal–slag⫽s metal–gas⫹s slag–gas⫺2F [s metal–gas · s slag–gas]0.5 initiation of film rupture moved into the slag phase and
.........................................(11) metal droplets were entrained into the slag phase.
The behavior of above-mentioned metal–slag–gas system
where,
was evaluated by Eqs. (1) and (2). According to the calcula-
tion (Eq. (1)) metal film cannot be formed because the film

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 ISIJ International, Vol. 50 (2010), No. 6
coefficient for metal film is lower than 0 (Q m⫽⫺2.43). This
agrees well with the experimental observations presented
by Han and Holappa.23) When adhesion of metal droplets
with gas bubbles were analyzed, one can notice that the
flotation coefficient (D m) for metal droplets is bigger than
zero (D m⫽0.13) which means that droplets can be attached
with gas bubbles. This disagrees with the experimental
findings but one has to remember that used Eq. (2) ignores
the kinetic drags that have also effect on the behavior of the
gas bubble and the metal droplets on the metal–slag inter-
face. Furthermore, value of (D m) approaches zero which in-
dicates that behavior of system can change easily.
5. Results and Discussion
Surface tension of top slag at different blowing stages
during AOD process was calculated using Eqs. (7)–(10).
According to the calculations surface tension of the top slag
varies between 0.48–0.56 N/m (Table 3). Value of the pro-
portionality factor (F ) is approximately 0.55 when the ef-
fect of FeO content of the top slag is taken into account by
the Eq. (13). Based on the information presented in Table 3
the top slag surface tension is assumed to be s slag–gas⫽
0.5 N/m and the proportionality factor F ⫽0.55 in AOD
process.
5.1. Effect of Reactions on the Interfacial Tension in
the Considered Systems
Effects of reactions between the slag and the metal on the
interfacial phenomena in the metal–slag–gas system were
evaluated using different values for slag–metal interfacial
tension based on the observations made in experimental
studies.8–13) Intensity of reactions and mass transfer be-
tween the slag and the metal were demonstrated by decreas-
Table 3. Top slag surface tension and proportionality factor
during AOD process.
Fig. 5. Effect of reaction intensity on the behavior of three phase
system.
801
ing slag–metal interfacial tension. For example in Fig. 5
marking ‘D with s s⫽0.5 N/m, F ⫽0.55 reaction with
⫺99%’ describes situation where reactions are very inten-
sive and in calculations value for the slag–metal interfacial
tension is 1% of equilibrium state value.
Effect of reaction intensity on the flotation coefficient is
described in Fig. 5. If system is in the equilibrium state
metal droplets are attached with gas bubbles. Figure 5 also
shows that during very intensive reaction between slag and
steel it is possible that behavior of the system changes and
the metal droplets disperse into the slag phase without coa-
lescence to the bubbles.
Figure 6 shows that the intensity of reactions has no ef-
fect on the film formation. Metal film can be formed only
with unrealistic low surface tension of metal and during
very intensive slag–metal reactions. In the case of AOD
metal film is not formed.
5.2. Top Slag–Metal System
Top slag is homogeneous and liquid only during the slag
reduction period in AOD and this causes uncertainty for the
calculations especially when the behavior of the system
during decarburization is evaluated.
Film coefficient (Q m) for metal droplet in liquid top slag
was calculated as a function of steel surface tension using
Eq. (14). Intensity of slag–metal reactions has demon-
strated using two different values of interfacial tensions:
50% of the equilibrium value and 1% of the equilibrium
value. Operating area of AOD is described in Fig. 7 by box.
Surface tension of metal calculated by Eq. (6) based on the
estimation of contents of surface active elements during
AOD process.17) Simulations show that there are no possi-
bilities to form metal film around the gas bubbles when
they penetrate through the metal–slag interface. It is also
independent of reaction intensity between the slag and the
steel.
Flotation coefficient for the metal droplet (D m) as a func-
tion of steel surface tension are presented in Fig. 8. Accord-
ing to the calculations during intensive reactions metal
droplets are disintegrated more easily into the top slag
layer. The increase of reaction intensity increases tendency
of disintegration. Calculations also show that metal droplets
are attached with the gas bubbles with equilibrium values
Fig. 6. Effect of reaction intensity on the behavior of three phase
system.
© 2010 ISIJ
 ISIJ International, Vol. 50 (2010), No. 6
Fig. 7. Film coefficient (Q m) for metal film in liquid top slag.
Fig. 8. Flotation coefficient (D m) for metal droplet in liquid top
slag.
of slag surface tension (D m⬎0).
5.3. Single Gas Bubble Rising in Metal Bath
The behavior of a single bubble including reactive oxy-
gen gas injected into stainless steel melt in AOD converter
has been studied by Järvinen et al.24) Reactions between gas
bubble and stainless steel melt were simulated by detailed
model that describes the chemical reactions, mass transfer
and heat transfer taking place on the surface of a single gas
bubble in liquid steel.24) According to the simulations oxy-
gen reacted very rapidly (t⬍0.05 s) and it was mainly con-
sumed to form Cr2O3 which was reduced by dissolved car-
bon by forming CO during bubble rising in melt bath.
Composition of the micro slag is assumed to be 80 wt%
Cr2O3, 10 wt% MnO and 10 wt% FeO in calculations.18,24,25)
According to the calculations slag film can be formed
around the gas bubble if the intensity of reactions between
the slag and the metal is high (Fig. 9). It must be remem-
bered that the formation of the slag film requires fully liq-
uid slag. Although, the melting points of the individual ox-
ides are remarkable higher than temperature used in AOD
process, slags as multi component oxides have much lower
liquidus and solidus temperatures than individual oxides.
During effective oxidation reactions at the vicinity of
© 2010 ISIJ
Fig. 9. Film coefficient (Q s) for micro slag film in liquid metal
bath.
Fig. 10. Flotation coefficient (D s) for micro slag droplet in metal
bath.
nozzles formed micro slag is attached with gas bubble (Fig.
10). Due to the high liquidus temperature of the formed ox-
ides, slag film cannot form although the slag film coeffi-
cient is higher than zero if reactions occur (Q s⬍0). Thick-
ness of the formed slag film is approximately 0.4–3 m m de-
pending on the formed oxide and temperature if oxygen
bubble (10 mm diameter) is reacted to form oxides. If the
formed slag film is very narrow (i.e. tens of nanometres),
thermodynamic properties of the film can differ remarkable
from the pure material values. Based on the used method it
can be said that it is correct to assume the micro slag at-
tachment with the gas bubbles. Attachment is required for
reduction of formed Cr2O3 and it is very important fact
when economy of the AOD process is analyzed.
6. Conclusions
In this study, the effects of surface tension of slag and
metal and interfacial tension between slag and metal on the
behavior of metal–slag–gas system in AOD process were
analysed based on the energy bound to system surfaces. Be-
havior of three-phase system in the AOD was studied by
two cases: evaluation of top slag–steel melt system and sin-
gle bubble rising in the metal bath. Effects of reactions on
802
 ISIJ International, Vol. 50 (2010), No. 6
the behavior of metal–slag–gas system were simulated by
using lowered values of the metal–slag interfacial tension
despites of the equilibrium ones.
Simulations for the metal–top slag system showed that
there are no possibilities to form metal film around the gas
bubbles when penetrating metal–slag interface. Behavior of
system is also independent of the intensity of reactions be-
tween slag and steel. According to the calculations during
intensive reactions metal droplets are disintegrated more
easily into top slag layer. The increase of reaction intensity
increases disintegration. If there are no slag–metal reactions
metal droplets are attached into the gas bubbles.
Calculations proved that, when reactive gas bubble is in-
jected into steel bath, slag film can be formed around the
gas bubble if the intensity of reactions between the slag and
the metal is high. It must be remembered that the formation
of the slag film requires fully liquid slag. During effective
oxidation reactions at the vicinity of nozzles formed micro
slag is attached with gas bubble.
Acknowledgements
Authors would like to thank Mr. Pentti Kupari, Dr. Paavo
Hooli, Mr. Veikko Juntunen and Mr. Topi Ikäheimonen
from Outokumpu Stainless for many discussions and com-
ments concerning the topic. Furthermore, Mr. Petri Mure
from Outokumpu Stainless is acknowledged due to the help
of figure processing. This research was partly funded by
Finnish Funding Agency for Technology and Innovation
(TEKES) and it is a part of the Energy Efficiency & Lifecy-
cle Efficient Metal Processes (ELEMET) research program
coordinated by Metals and Engineering Competence Clus-
ter (FIMECC).
803
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