Experimental Investigation On Metallic Droplet Behavior in Molten BOF Slag

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Experimental Investigation on Metallic Droplet

Behavior in Molten BOF Slag


YANNAN WANG, LINGLING CAO, MAARTEN VANIERSCHOT, BART BLANPAIN,
and MUXING GUO

In order to better understand the metallic droplet behavior during a slag treatment process, a
physical modeling based on the similarity principle was performed in a transparent scaled-down
vessel at room temperature. Paraffin oil, 20 wt pct copper sulfate solution, and compressed air
were used to simulate the molten slag, metallic droplet, and carrier gas, respectively. The
droplets injected into paraffin oil during the experiment were captured by a high speed camera
and were analyzed by Image Pro Plus software to obtain the droplet size distribution. The
critical droplet size in the physical modeling and slag treatment process is quantitatively
correlated. The results show that droplet breakage phenomenon is dominant over its
coalescence in the current industrial practice, and droplet breakage is enhanced with
increasing gas flow rate and/or lance depth. No significant effect of the nozzle configuration
was found on the droplet breakage and coalescence. The droplet size distribution varies with the
lance position. Gas flow rate and lance depth are the most important factors for droplet
breakage, the extent of which can be reduced through a proper selection of the operational
conditions. A linear relationship between the droplet size and the input energy flux is obtained.

https://doi.org/10.1007/s11663-019-01635-8
 The Minerals, Metals & Materials Society and ASM International 2019

I. INTRODUCTION probably due to the breakage of the large metallic


droplets into fine ones which cannot sediment fast
APPROXIMATELY 10 million tons of Basic Oxy- enough to the bottom of the slag pot and are hence
gen Furnace (BOF) slag are produced annually in trapped in the slag. Therefore, the study of metallic
Europe.[1,2] The BOF slag is conventionally disposed droplet behavior in molten slag is of significant impor-
through landfill or dumping, leading to land occupation, tance for increasing metal recovery after the hot-stage
environmental problems, and resource waste.[3,4] Many slag treatment.
efforts have been attempted to reuse BOF slag either as a There are a number of studies on the metallic droplet
secondary resource or as added value products.[3–6] behavior in molten slag. Those works were mainly
However, the application of BOF slag is restricted by its focused on the slag-metal-gas emulsion in the BOF
volume expansion due to the presence of free lime.[7,8] In steelmaking process[12–16] or copper slag cleaning pro-
order to stabilize BOF slag and to modify slag compo- cess.[17,18] The residence time of the metallic droplets in
sition for its high-added value applications, silica-rich the emulsified BOF slag has been investigated by low
additives are injected into the molten BOF slag with temperature physical modeling (e.g., mercury/glycerine
oxygen or nitrogen as carrier gas at high tempera- or water/oil systems),[13,14] high temperature experi-
ture.[9–11] However, a poor recovery of metallic iron is ments[14,15] and mathematical modeling,[15,16] respec-
found after this hot-stage slag engineering. This is tively. These studies help provide a better understanding
of the refining reactions and the separation of metallic
droplets from slag during metallurgical process. In the
copper slag cleaning process, electromagnetic stirring is
implemented to improve the coalescence of metallic
YANNAN WANG, BART BLANPAIN, and MUXING GUO are
with the Department of Materials Engineering, KU Leuven, 3000
droplets, leading to a higher copper recovery effi-
Leuven, Belgium Contact e-mail: muxing.guo@kuleuven.be ciency.[17,18] An advanced collision and coalescence
LINGLING CAO is with the State Key Laboratory of Advanced algorithm was developed, where the algorithm was
Metallurgy, University of Science and Technology Beijing, Beijing, coupled with the Euler–Lagrangian scheme and the
100083, China. Contact e-mail: meynell0809@gmail.com MAARTEN magneto-hydrodynamic module in the commercial code
VANIERSCHOT is with the Mechanical Engineering Technology
Cluster TC, Campus Group T Leuven, KU Leuven, 3000 Leuven, ANSYS FLUENT to predict the efficiency of copper
Belgium. recovery under the operational conditions of industrial
Manuscript submitted April 16, 2019. pilot plants.[18] This provides a numerical method to
Article published online July 9, 2019.

2354—VOLUME 50B, OCTOBER 2019 METALLURGICAL AND MATERIALS TRANSACTIONS B


understand the metallic droplet coalescence in the physical modeling dynamically similar to the proto-
molten slag, rendering references for copper recovery type.[19] The Weber number is also considered in this
in practice. study, since it is closely related with droplet breakage
However, the experimental work on the metallic and coalescence.[20,21] The modified Froude number and
droplet coalescence and breakage is limited due to the Weber number are given in Eqs. [1] and [2]:
opaque and high temperature environment in the
hot-stage slag engineering operations. This paper aims qg u2g
Frm ¼  ½1
to identify through physical modeling the main influ- ql  qg gH
encing factors of the hot-stage slag treatment operation,
such as gas flow rate, lance depth, lance position and
nozzle configuration, and to quantitatively understand
the behavior of metallic droplets, e.g., breakage and ql u2g d
We ¼ ½2
coalescence in molten slag. With this knowledge the r
operators may be able to optimize the process operation The experimental setup and the top view of CSS
to obtain a high metal recovery for the slag treatment. injection points are presented in Figure 2. The CSS
droplets were generated and introduced into the paraffin
oil in the vessel through five needles at equiangular
II. EXPERIMENTAL METHODOLOGY positions with a distance of half of the top vessel radius
to the vessel center. The purpose is to obtain a uniform
A tapered cylindrical vessel made of transparent dispersion of the initial droplets in the whole vessel.
plexiglass was designed and fabricated with a Images of the initial droplets with a 1504 9 1128 pixels
scale-down factor of 1/4. The geometrical shape of the resolution were captured by a high speed camera
vessel is maintained similar to the slag pot of a steel (REDLAKE HG-100K) at 1000 fps prior to the gas
plant in ArcelorMittal. The injection lance used in this injection. Subsequently, gas with a certain flow rate was
study is a glass pipe with one end closed. Three introduced to agitate the paraffin oil. After 10 minutes
equiangular holes were drilled at the closed end or at of gas blowing, images with the same resolution and
the side wall adjacent to the closed end to form two type frame rate were recorded. The imaging area was selected
nozzle configurations (types A and B). The bottom view around 100 mm below the oil surface and close to the
of a type A nozzle configuration and the front view of a vessel wall. This is because many droplets migrated to
type B nozzle configuration are shown in Figure 1. this area due to the recirculation flow according to
Paraffin oil, 20 wt pct copper sulfate solution (CSS), experimental observations. The imaging distance
and compressed air were used to simulate the molten between the captured droplets and camera lens is
slag, liquid iron phase and oxygen gas, respectively. around 1200 mm. It should be noted that the agitation
There are two reasons for using the CSS instead of time cannot be too long to avoid the mixing of small air
water. Firstly, the CSS-paraffin oil system has closer bubbles with the paraffin oil. The latter can deteriorate
density and viscosity ratios to those of the iron the image quality, leading to a difficulty in the image
droplet-slag system compared to the water–paraffin oil analysis. The lance position in the cross section of the
system (see Table I). Secondly, the CSS has a blue color, vessel and the lance depth from the oil surface can be
which makes imaging and analyzing easier. The mod- adjusted during the experiments. The input information
ified Froude number defined as a ratio of the inertial such as geometrical and operating parameters and
force to the buoyancy force is chosen to make this

Fig. 1—Nozzle configurations (a) bottom view of type A; (b) front view of type B.

METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 50B, OCTOBER 2019—2355


Table I. Input Values of Parameters for Slag Treatment
measuring known size polypropylene spheres
Process and the Physical Modeling in this Work (3.18 ± 0.05 mm), and the error level was confirmed
to be less than 3 pct. To determine the Droplet Size
Slag Treatment Process Distribution (DSD), a normalized frequency, Nf ,
obtained by dividing the frequency of droplet in each
Top diameter of the slag pot (mm) 3360 given size bin by the bin width was employed to
Bottom diameter of the slag pot (mm) 2390
eliminate the arbitrariness resulting from the choice of
Height of the slag pot (mm) 3558
Lance diameter (mm) 40 the bin size and number defined by the user.[23]
Height of slag level (mm) 3000 NXY
Submerged lance depth (mm) 300–1000 Nf ¼ ½3
Gas flowrate (Nm3 h1) 100–200 LY  LX
Slag density (kg m3) 3000
Slag viscosity (kg m1 s1) 0.1
Gas density (kg m3) 0.574¤
Gas viscosity (kg m1 s1) 5.87 9 105* III. RESULTS AND DISCUSSION
Metallic droplet density (kg m3) 7000
Metallic droplet viscosity (kg m1 s1) 0.007 A. Influence of Operational Parameters
Interfacial tension of slag/metallic droplet 1.27 Metallic droplet size is a significant parameter affect-
(N m1) ing droplet behavior in hot-stage slag engineering. In
Modified Froude number ðFrm Þ 0.043–0.600
order to precisely model the metallic droplet behavior in
the BOF slag, the critical droplet size dc in the physical
Physical Modeling
model and slag treatment process is correlated by
Top diameter of the model (mm) 840 analyzing the critical Weber number Wec . The droplet
Bottom diameter of the model (mm) 598 will break up under the given operational conditions
Height of the model (mm) 890 when the droplet size is larger than the critical droplet
Oil level (mm) 750 size. It was reported that the critical Weber number
Lance diameter (mm) 10 depends on the flow field,[20] which remains the same
Nozzle diameter (mm) 2 between the physical modeling and the slag treatment
Needle inner diameter (mm) 0.838
Submerged lance depth (mm) 200–600
process. Based on Eq. [2] the ratio of dc in physical
Lance position (mm) 0R–0.45R modeling to that in the slag treatment is expressed in
Gas flow rate (Nm3 h1) 0.46–3.6 Eq. [4]. The gas velocity ratio in Eq. [4] can be derived
Oil density (kg m3) 880 from Eq. [1], as shown in Eq. [5]. Compared to the liquid
Oil viscosity (kg m1 s1) 0.065 density, the gas density is much smaller. Therefore, the
Gas density, (g m3) 1.225 density difference between the liquid phase and the gas
Gas viscosity (kg m1 s1) 1.789 9 105 phase in Eq. [5] is simplified as the liquid density,
CuSO4 solution density (kg m3) 1194 resulting in Eq. [6]. After substituting Eqs. [6] into [4],
CuSO4 solution droplet viscosity (kg m1 s1) 0.0057 the correlation of the critical droplet size between the
Interfacial tension between oil and droplet 0.048w physical modeling and the slag treatment process is
(N m1)
Modified Froude number ðFrm Þ 0.044–2.668
quantitatively represented in Eq. [7].

‘‘¤’’, ‘‘*’’ and ‘‘w’’ indicate the calculated values based on the ideal dcm u2gp qlp rm
gas law, Sutherland’s law[22] and Antonoff’s rule, respectively. ‘‘R’’ ¼ ½4
indicates top radius of the vessel.
dcp u2gm qlm rp


u2gp qgm qlp  qgp Hp
¼  ½5
u2gm qgp qlm  qgm Hm
material properties are listed in Table I. It should be
mentioned that the present work is in the context of a
non-reactive slag stabilization process, and studies the
metallic droplet behavior in the molten BOF slag during u2gp qgm qlp Hp
the N2 gas injection. However, the study on chemical ¼ ½6
u2gm qgp qlm Hm
reactions between the gas phase and the metallic droplet
and/or slag phase will be necessary when the O2 gas, in
practice, is chosen as the carrier gas phase.
2
All the recorded images were analyzed using Image dcm qgm qlp Hp rm
Pro Plus (IPP) software. For the image analysis a plastic ¼ ½7
dcp qgp q2lm Hm rp
ruler attached to the vessel wall is used to transform the
pixels to physical dimensions. In order to obtain a Figure 3 shows droplet size distribution as a function
statistically reliable distribution approximately 800 of the gas flow rate. For comparison, the size distribu-
droplets for each experimental run were analyzed. The tion of the initial droplets is also plotted in the figure.
measurement quality of using IPP has been validated by The distribution curve moves to the left, indicating that

2356—VOLUME 50B, OCTOBER 2019 METALLURGICAL AND MATERIALS TRANSACTIONS B


Fig. 2—Experimental setup and the top view of CSS injection points.

the droplet size becomes smaller with increasing gas flow


rate. This can be understood from the changes in the
turbulent kinetic energy of the system with the gas flow
rate. Since the breakage is induced by the kinetic energy
of turbulent motion in a continuous phase, it occurs
when the kinetic energy is higher than the surface energy
required to form the daughter droplets.[24] It has been
proven that increasing gas flow rate augments the
turbulent kinetic energy and its dissipation rate.[25] This
favors droplet breakage.[26]
It is worth noting in Figure 3 that the frequency peak
decreases with the gas flow rate. This is probably
because (1) the droplet volume from each experimental
run was not conserved due to a fixed area for capturing
the droplet in the present work; (2) it is difficult to
capture the small droplets due to their mixed with gas
bubbles; and (3) the image analysis quality by the IPP
software is limited with tiny droplet. Fig. 3—Effect of the gas flow rate on DSD (Lance depth: 400 mm;
lance position: 0R; nozzle type: A).
In order to identify whether droplet coalescence takes
place during the process, an experiment with low gas flow
rate was also carried out. The obtained DSD curves are
presented in Figure 4(a), where the curve is on the right of finally coalesces into a larger droplet at t = 0.3 seconds.
the initial size distribution when the gas flow rate ranges This process consists of two steps, i.e., droplet collision and
from 0.46 to 1.0 Nm3 h1, and it moves to the left of the coalescence. The droplet interaction time ti is defined as the
initial curve as the gas flow rate increases up to time from droplet contact to droplet coalescence (i.e., from
1.8 Nm3 h1. This suggests there is a critical gas flow rate, 0.278 to 0.3 seconds), which is determined by observing the
which is close to 1.0 Nm3 h1, for droplet coalescence. The recorded figures frame by frame. Only if the interaction time
droplet coalescence occurs when the gas flow rate is less than is sufficient for the oil film thickness between the two
the critical value; otherwise, the droplet breakage takes colliding droplets h (see Eq. [8]) to be reduced to the critical
place during the process. This is attributed to an increase of value hc (see Eq. [9]), coalescence will take place.[27,28]
the droplet coalescence caused by a gentle agitation under Otherwise, the droplets bounce away from each other. The
the small gas flow rates. A vigorous agitation generated by time needed for the film being drained to the critical
large gas flow rate may result in a rebounding of the thickness is called the droplet drainage time. The schematic
colliding droplets or sliding and even droplet splitting. A of the coalescence and bouncing is shown in Figure 5. The
coalescence process is recorded in Figure 4(b), which shows interaction time in Figure 4(b) is approximately 0.022 sec-
that one droplet approaches closer to another droplet at onds. Since droplet coalescence occurs, the droplet drainage
t = 0.264 seconds, starts contact at t = 0.278 seconds and time is obviously less than 0.022 seconds. However, this

METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 50B, OCTOBER 2019—2357


 
drainage time cannot be determined by the experiment. 8rt
Based on the radii of colliding droplets in Figure 4(b) and h ¼ h0 exp ½8
qVr2
interface tension value in Table I, the critical film thickness
is calculated as 300 Å.
 
Areq 1=3
hc ¼ ½9
8pr
where
 
1 1 1 1
¼ þ ½10
req 2 ri rj
Figure 6 shows the DSD as a function of the
submerged lance depth for the gas flow rate of
3.0 Nm3 h1 at the lance position 0R. The distribution
curve gradually shifts to the left (i.e., the smaller size
distribution) as the lance depth increases from 200 to
600 mm. Increasing the lance depth favors droplet
breakage. Since this is a buoyancy-driven flow, the
energy input into this system is derived from the
potential energy of the rising gas bubbles. It has been
proven that the input energy is approximately propor-
tional to the lance depth.[29] Increasing lance depth
means more energy supplied into this system, leading to
greater droplet breakage.
Figure 7 shows the effect of the lance position on the
DSD for the gas flow rate of 3.0 Nm3 h1 at the lance
depth of 400 mm. For a given lance depth, the droplet
size decreases when the lance is moved from the center
to the vessel wall. This is believed to be connected with a
distinct flow pattern for a particular lance position.
When the lance is moved from the center to the vessel
wall, the stirring can be enhanced by eliminating
recirculation zone with low velocity in the vessel. This
increases the probability of droplet breakage, since
droplets in low velocity zones do not split.
Figure 8 shows a comparison of the DSD curves for
type A and B nozzle configurations. The two curves
approximately overlap with each other. This means that
Fig. 4—(a) Effect of the small gas flow rate on DSD (Lance depth: the considered nozzle modification does not affect the
300 mm; lance position: 0R, nozzle type: A). (b) Droplet coalescence droplet behavior. It is likely that changing the nozzle
process (Lance depth: 300 mm; lance position: 0R, nozzle type: A).

Fig. 5—Schematic of the coalescence and bouncing of two colliding Fig. 6—Effect of the submerged lance depth on DSD (Flow rate:
droplets. 3.0 Nm3 h1; lance position: 0R; nozzle type: A).

2358—VOLUME 50B, OCTOBER 2019 METALLURGICAL AND MATERIALS TRANSACTIONS B


Fig. 7—Effect of the lance position on DSD (Flow rate:
3.0 Nm3 h1; lance depth: 400 mm; nozzle type: A). Fig. 9—Relationship between the droplet behavior and input energy
flux.

Therefore, a normalized droplet size dN , which is defined


as the ratio of the average size of the resulting droplets
to the average size of the initial droplets (see Eq. [12]),
has been used to interpret the experimental results.
dN < 1 indicates that droplet breakage is dominant,
while dN > 1 means that droplet coalescence is domi-
nant. Figure 9 shows the relationship between the
normalized droplet size and the input energy flux.
Obviously, a coalescence region is found when the input
energy flux is lower than a critical value of approxi-
mately 9.0 kJ m2 s1. Once the input energy flux
exceeds this value, the droplet breakage predominates
over the droplet coalescence in the experiment. Actually,
the droplet breakage has been predominantly observed
under the present operational conditions of the indus-
trial hot-stage slag treatment. In the breakage region
(i.e., input energy flux EIn ranges from 12 to
Fig. 8—Effect of the nozzle configuration on DSD (Flow rate:
35 kJ m2 s1), by fitting the experimental data a linear
3.0 Nm3 h1; lance depth: 400 mm; lance position: 0R). relationship between the normalized droplet size and
input energy flux is obtained, as shown in Figure 9. The
configuration has little influence on the input energy and linear formula is given in Eq. [13]. Based on the result of
flow regime of the system when the experimental Figure 9, the operational conditions, such as gas injec-
conditions (such as the gas flow rate, lance depth, and tion rate and lance depth can be optimized to minimize
its position) are fixed. the breakage of the metallic droplets during the slag
treatment.
    
B. Correlation of Droplet Size with Input Energy Flux 1 q gH ql gH
EIn ¼ gQa qg u2 þ Qa Pa 2 ln 1 þ l  a
2 Pa Pa þ ql gH
Based on the experimental results of this work, the
droplet behavior is influenced by the input energy into ½11
the system. In order to quantitatively understand this
influence, the input energy flux under different experi-
mental conditions is calculated based on the formula di
derived by Schwarz[29] (see Eq. [11]). The conversion dN ¼  ½12
d0
efficiency, g, was deduced as 0.06 by Lehrer from a
similar gas-liquid experiment.[30] This value is adopted
in our calculation. Since the initial droplet size is 
different in each single factor experiment, it is not dN ¼ 0:0075EIn þ 0:887 R2 ¼ 0:964 ½13
possible to compare the resulting droplet size.

METALLURGICAL AND MATERIALS TRANSACTIONS B VOLUME 50B, OCTOBER 2019—2359


IV. CONCLUSIONS h0 Initial film thickness (mm)
hc Critical film thickness (mm)
A physical modeling experiment by using air-copper
H Submerged lance depth (m)
sulfate solution-paraffin oil has been performed to
g Gravitational acceleration (m/s2)
understand the mechanism of breakage and coalescence
LX Lower limit of a given bin (mm)
phenomena of the metallic droplets in molten slag
LY Upper limit of a given bin (mm)
during the hot-stage slag stabilization process. The main
Nf Normalized frequency (mm1)
conclusions are summarized as follows.
NXY Frequency in a given bin
(1) The critical droplet size in physical modeling and Pa Atmosphere pressure (Pa)
slag treatment practice is correlated by the analysis Qa Gas flowrate at pressure Pa (m3 s1)
of the critical Weber number. Therefore, the results r Radius of droplet (mm)
obtained by the physical modeling might quantita- req ; ri ; rj Equivalent radius, radius of droplet i and j,
tively describe the metallic droplet behavior in the respectively (mm)
slag stabilization treatment. R Top radius of the physical model (mm)
(2) The breakage and/or coalescence of the droplets t Time (s)
occur at different experimental conditions. The ti Interaction time (s)
droplet breakage was predominantly observed to be u Gas velocity (m s1)
greater than coalescence under the current opera- V Approach velocity (m s1)
tional conditions. The extent of the droplet breakage We Weber number
is enhanced with increasing gas flow rate and/or Wec Critical Weber number
lance depth. The droplet size distribution varies with
the lance position. The nozzle configuration has very
limited effect on the droplet size distribution.
(3) The gas flow rate and lance depth are the key factors GREEK SYMBOLS
influencing the droplet breakage.
(4) A droplet coalescence region is found when the in- g Conversion efficiency of kinetic energy
put energy flux into the system is lower than a l Viscosity, (Pa s)
critical value of 9.0 kJ/(m2 s). Once the input energy q Density (kg m3)
flux exceeds this critical value, the droplet breakage r Interfacial tension between paraffin oil and droplet
will be dominant in the process. In the breakage (N m1)
region, a linear relationship between the normalized
droplet size and the input energy flux is obtained.
(5) The present finding forms a basis for minimizing the
breakage of the metallic droplets during the slag SUBSCRIPTS
treatment by properly selecting the operational
conditions. d Droplet
g Gas phase
l Liquid phase
m Physical modeling
p Slag treatment process
ACKNOWLEDGMENTS
The financial support from an IWT project 140514 REFERENCES
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