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Fluid Flow and Bubble Behavior in the Aluminum Electrolysis Cell
Mr. Yufeng Wang, Prof. Lifeng Zhang, Mr. Xiangjun Zuo
Department of Materials Science and Engineering, Missouri University of Science & Technology, Rolla, MO 65401, USA,
Tel: +1-573-341-4776, Email: [email protected]
Keywords: Aluminum Electrolysis Cell, Fluid Flow, Bubbles, Water Modeling, LDV Measurement
Abstract
A full scale water model was established to investigate the
phenomena in aluminum reduction cells. The behavior of
bubbles under the anode is analyzed by both directly
observation and camera recording. Bubble under the anode
has a thick bubble front and a thin, long trail portion. With
0o tilted angle, hardly can the bubbles move forward, but
form a gas film under the anode. With non-zero tilted angle,
bubble motion under the anode is driven by the buoyancy
force, thus bubbles are easy to escape through the curved
end of the anode. LDV was used to investigate the fluid
flow pattern. The LDV measurements reveal a recirculation
flow pattern in side channel, similar to the observation of
the tracer dispersion. Larger tilted angle and larger gas flow
rate generate larger velocity and bigger turbulent energy,
especially in the region close to the end of the anode and
the top surface.
Introduction
Nowadays, most of the aluminum smelters are seeking
ways to increase the current and reduce energy
consumption. A transverse cross-sectional schematic of a
modern aluminum reduction cell is shown Figure 1. The
anodic gas bubbles in the Hall-Héroult cell are a very
important player in this process. The carbon anode is
consumed to give off approximately 2.5m3 of CO2 for
every kg of Al produced. 1)
It is generally accepted that gas
bubbles (predominantly CO2 with the basic chemical
reaction under the anode of Al2O3 + C = Al + CO2) formed
during normal operation provide some benefit by
contributing to electrolyte circulation and mixing. The
release of the anode gas from the horizontal anode surface
in a molten cryolitic electrolyte is not continuous, but
occurs in a cyclic fashion. The formation of the bubble
layer beneath the anode is one of the key factors for the
transport phenomena in the cell. The physics of bubble
dynamics includes its nucleation, departure, detachment,
coalescence, breakup, size and shape, sweeping, and escape
etc. Sloped anode must be also considered. This layer
contributes to the bath flow that is responsible for the
alumina dissolution and its transport into the interpolar
space. However, the bubble layer increases the voltage
drop and electric noise (voltage fluctuation) of the cell. The
bubble voltage could be as high as 300 mV depending on
the anode current density and alumina concentration. 2)
Also, the gas induces bath flow and bath turbulence, which
influence the current efficiency. The direct measurement of
the bubble layer 3)
is difficult due the harsh environment -
high temperature and corrosiveness of the bath. Physical
models have been used to study the phenomenon. 4)
There
are studies that have been made by numerical modeling
where only gas driven flow has been considered. 5)
.
Fig.1 Schematic phenomena in aluminum electrolysis
cell considering alumina addition 6)
Slotted anodes were first implemented in a Rio Tinto
Aluminium (RTA) managed plant in 1998. 7)
Slotted
anodes have been used in recent years by aluminum
smelters in order to reduce gas bubble resistance at the
anode/electrolyte interface.
Results of scientific investigations into aluminium
reduction cell gas bubbles and gas induced circulation were
made public over 30 years ago including, for example, see-
through cell studies 3)
and water modeling 4)
. A 2003 paper
by N. Richards et al. 8)
refers to at least 20 publications, by
a dozen different researchers, all focused on gas bubble
related phenomena. There are a few physical models of
slotted anodes 9, 10)
Water Model Experiments
The current study focuses on the water modeling of bubble
behavior and fluid flow in the reduction cell. The properties
of water and cryolite are shown in Table 1. Due to the
similar kinematic viscosity 11)
, the water-air system can be
used to model the aluminum electrolysis process (molten
581
aluminum and CO2 bubbles). Since the passage of four
electron through the circuit is necessary to release one
molecule of CO2, the correlation between the current
density and gas flow rate is 12)
10 kAm – 2
= 2.71 L m – 2
s – 1
(1)
Table 1. Properties of water and cryolite 12)
Liquids Cryolite Water
Temperature, oC 950 25
Density, kg/m3 2.1 1.0
Surface tension, Dynes cm2/s 60 70
Kinematic viscosity (Poise cm3/g) 1.5 1.0
The water model system used in the current study is shown
in Figure 3. A Plexiglas sided tank is used as container.
Two anodes are modeled by suspending two Plexiglas
boxes in the tank with a dimension of 150cm long, 17cm
wide and 43cm high. The distance between the anode and
the bottom of the tank, and the anode tilt angle are
adjustable in the current study. Gas evolution is simulated
by injecting air through 8 plastic pipes on each anode. In
low-temperature models, coalescence is the main growth
mechanism of bubbles. Small bubbles newly nucleating on
the anode surface do not significantly affect the motion of
large bubbles 13, 14)
, thus in the current study the pipes were
employed instead of porous plates under the anode.
Fig.3 Schematic of the water model
The operation parameters used in this study are listed in
Table 2. The anode cathode distance (ACD) is set to 40mm,
and the anode slope angle is various from 0 º to 1.1º. The
carbon anode is consumed to give off approximately 2.5m3
of CO2 for every kg of Al produced 1)
. It is generally
accepted that gas bubbles (predominantly CO2 with the
basic chemical reaction under the anode of Al2O3 + C = Al
+ CO2) formed during normal operation provide some
benefit by contributing to electrolyte circulation and mixing,
and there is a strict correlation between the current density
and gas flow rate15)
, as shown in Eq. (2). By the calculation,
the gas flow rate in the experiment was from 16.0 to 157
l/min, which equivalent to a current density of
0.2~1.0A/cm2.
4
iRTq
FP= 3 1 2[ ]m s m− − (2)
where i is the anodic current density, (Am-2
), R is gas, T is
Absolute temperature (K), F is Faraday’s constant, P is
pressure (Pa).
Table 2 Parameters in the water model
Items Value
Anode cathode distance (ACD) 40mm
Anode slope 0 º, 0.4 º, 1.1 º
Slot width 3mm
Side channel 390mm
Center channel 107mm
Gas flow rate 16.0~157l/min
Fifteen experiments were carried out (Table 3). The
different locations and views of the anode are recorded by
digital camera, as shown in Figure 4. The bubble behavior
at these locations is analyzed.
Table 3 Gas flow rate and anode tilted angle in the water
model experiments
Anode
slope
Current Density (A/cm2)
0.2 0.4 0.6 0.8 1.0
0º ▲ ▲ ▲ ▲ ▲
0.4 º ▲ ▲ ▲ ▲ ▲
1.1 º ▲ ▲ ▲ ▲ ▲
Location -1(Side)
Location -2(Side)
Location -3(Side)
Location -4(Bottom)
Location -5(Front)
Fig.4 Observation locations in the water experiments
Results and Discussion
The shape of bubbles
Every bubble below the anode has a thick bubble front and
a thin, long trail portion, as shown in Figure 5(a). If being
Anode
Anode
Anode
Anode
Anode
582
viewed from the bottom, as shown in Figure 5(b), the
largest dimension is transversal to the motion direction.
With the increase of current density, the thickness of the
bubble will increase, as confirmed by reference 11)
.
(a) Observion from the side
(b) Observation from the bottom
Fig.5 The shape of the bubble
When the size of the anode is large enough, big gas pockets
are formed by coalescence and during their passage they
sweep away smaller bubbles. The shape of these very big
gas pockets is not circular anymore, having a nearly
straight leading and trailing edge. While the thickness of
the bubble laden layer is generally determined by the
maximal possible height of a bubble under a solid surface,
these big gas pockets have a “head” at the leading edge
which is about twice thicker than the overall thickness of
the bubble layer.16)
The effect of the tilted angle
The gas flow rate is set to 125L/min·m2, and the anode
tilted angle is various from 0º to 1.1º. The bubble motion
velocity increases with increasing tilted angle. With 0o tilt
angle, lots of bubbles escape from the slot but not the
curved end of the anode. If the tilt angle is larger than 0.4º,
bubbles are mainly escape from the curved end of the
anode, as shown in Figure 6. With zero tilted angle, the gas
film coverage ratio of the anode bottom is largest compared
to non-zero tilted angle, and the coverage ratio decreases
with the increasing tilted angle. The liquid motion is also
greatly affected by the tilted angle. In the current
experiments, the ink tracer is injected into the system, as
shown in Figures 7. With 0º tilted angle, the tracer
stagnates under the anode for a long time. If the tilted angle
is larger than 0.4º, the ink tracer quickly enters the side
channel (between the end of the anode and the side wall of
the tank) and generates a recirculation flow in the side
channel. With larger tilted angle, the ink enters the side
channel more quickly and generates stronger recirculation.
Fig.6 Bubble motion viewed from the front of the anode:
upper- tilted angle 0º; lower- tilted angle 1.1º
583
Fig.7 Tracer dispersion at different time (tilted angle
0.4º)
Anode tilt dramatically affects the behavior of the bubble
layer. A tilt of a fraction of a degree is sufficient to induce
significant buoyancy driven motion of the gas bubbles. It
was found that 12)
the ACD has no effect on gas bubble
behavior. An increase in current density increased the
bubble size and thickness of the bubble front as well as gas
coverage of the anode face and bubble velocity. Current
density has no effect on bubble release frequencies. An
increase in electrolyte velocity decreased the bubble size
and the gas coverage and increased the bubble velocity and
release frequency. An increase in anode tilt decreased the
bubble size and gas coverage and increased the bubble
release frequency. Tilt has no effect on bubble velocity.
Behavior of the gas layer on a horizontal anode was
different than on an inclined anode. On a horizontal anode,
the process of bubble nucleation, growth, coalescence and
release involved no bubble motion and led to as gas layer
thickness of approximately 5 mm. 12)
On the inclined
surface, gas behavior was dominated by the motion of large
bubbles across the anode surface. Hydrodynamic effects
increase the maximum thickness of the bubbles to more
than 2cm. Figure 8 shows a possible mechanism of bubble
detachment from the bottom of a plate. When the anode
was slightly tilted(a fraction of a degree), large bubbles
formed and flowed beneath the anode with a leading edge
penetrating up to 2 cm into the electrolyte and a long tail as
seen in Figure 5a.
Fig.8 Possible mechanism of bubble detachment from
the bottom of a plate 17)
Figure 9 shows a picture taken with the PIV system for a
bubble moving on a liquid layer with a volume of 1.7 cm3
and an inclination of 5°. 17)
The PIV allows visualizing the
flow in two-dimensions around a moving bubble. In the
front of the bubble, the liquid is pushed away in the
direction normal to the interface. The depression in the rear
part of the bubble creates a counter flow to respect the
continuity. 17)
Fig.9 Flow around a moving bubble obtained with a PIV
system 17)
The effect of the gas flow rate
The tilted angle was set to 1.1º, and the gas flow rates
varies from 16.0-60.2l/min, which equals to a current
density of 0.2-1.0A/cm2. The gas release frequency
increases with increasing gas flow rate. The velocity of
recirculation flow in the side channel is accelerated with
increasing gas flow rate. So does the turbulence intensity
(Figure 10). Under 70L/min·m2 (equivalent 0.5A/cm
2) gas,
it takes ~ 6s for the tracer to move from the bottom to the
side, and under 157L/min·m2 (equivalent 1A/cm
2) gas, only
4s is needed.
(a) Flow rate of 70L/min·m
2, t=0s
(b) Flow rate of 70L/min·m
2, t=6s
(c) Flow rate of 157L/min·m
2, t=0s
584
(d) Flow rate of 157L/min·m
2, t=4s
Fig.10 Tracer dispersion (Tilted angle 1.1º)
LDV Measurement
In this current chapter, the fluid flow in the water model of
the aluminum electrolysis cell is characterized using a two-
component Laser Doppler Velocimetry (LDV) - TSI Model
9833 two-component LDV. Through LDV, the local
instantaneous velocity (u and v) at some points can be
measured. For each point measurement, the mean velocity
( u and v ) can be obtained by averaging the velocities of
1000 particles, approximately during the period of 5-8
minutes. The turbulent velocity fluctuation ( u′ and v′ )
can be calculated by
u u u′ = − v v v′ = − (4)
It is important to know the local value of the turbulent
energy because it provides useful information of the local
mixing intensity. The turbulent energy per unit mass, k
(m2/s
2), is calculated according to:
( )2 21 2 vk u′ ′= + (5)
The fluid flow features at two different locations was
measured: the region at side channel and the region under
the anode. At the side channel region more than 300 points
were measured and at the region under the anode more than
100 points were collected. LDV measurement is through
points to points. If it takes 6 minutes, then measuring 400
points needs at least 40 hours of pure measurement time
except for other experimental preparation time. Thus, in the
current study, only three groups of experiments were
carried out. Experimental details were listed in Table 4.
Table 4 Experimental parameters
Case 1 Case 2 Case 3
ACD, mm 40 40 40
Anode slope, ° 0 1.1 1.1
Gas flow rate, L/min 64.2 16 64.2
The measured mean velocity vector and the turbulent
energy for all the three cases in Table 4 are shown in
Figures 11-13. For all these three cases, the high
turbulence is located at the gas plume region near the end
of the anode and close to the liquid surface. The high
turbulent kinetic energy near the end of the anode is mainly
generated by the momentum transfer from rising bubbles to
the liquid. The turbulent kinetic energy close to the liquid
surface is due to energy dissipation of the waves, which is
induced by bubbles reaching the top surface.
With zero degree tilted angle (Fig.11), bubbles are not easy
to escape from the end of the anode, so the gas film
expands under the anode and rise up through the side wall
of the anode. the liquid follows the gas bubbles. Thus, the
velocity under the anode is very random and big at some
locations (Fig.11b). Occasionally there are bubbles rising
up the end of the anode, which generate a recirculation
flow pattern at the side channel (Fig.11a). With zero degree
tilt angle, larger gas flow rate does not always generate
larger velocity below the anode because the movement of
bubbles is driven by the expansion of the gas film instead
of buoyancy. The similar flow pattern is observed by water
model experiment before and validated by the stagnation of
tracer under the anode. Also the distribution of the
turbulent kinetic energy is different from those cases of
non-zero degree tilt angle. The larger turbulent kinetic
energy under the anode is the result of the generation of
dissipation of bubbles.
With 1.1o tilt angle (Figures 12-13), the fluid flow pattern
can be characterized as follows:
- Stable horizontal flow under the anode since almost all
bubbles escape through the end side of the anode;
- Similar but slight larger velocity in the side channel
region, especially near the anode and the top surface,
compared to the case of zero degree tilt angle;
- Eddy position is lower than the case of zero tilt angle;
- Larger gas flow rate generates larger turbulent energy,
especially around the top end of the anode, and
generates larger velocity under the anode, which is due
to the fact that large gas flow generates more bubbles.
a) Side Channel
b) Under Anode
Fig.11 Measured velocity and turbulent energy (Anode
tilted angle, 0°, Gas flow rate, 64.2L/min)
585
a) Side Channel
b) Under Anode
Fig.12 Measured velocity and turbulent energy (Anode
tilted angle, 1.1°, Gas flow rate, 16L/min)
a) Side Channel
b) Under Anode
Fig.13 Measured velocity and turbulent energy (Anode
tilted angle, 1.1°, Gas flow rate, 64.2L/min)
Summary
A full scale water model was established to investigate the
phenomena in aluminum reduction cells. The behavior of
bubbles under the anode is analyzed by both directly
observation and camera recording. Bubble under the anode
has a thick bubble front and a thin, long trail portion. With
0o tilted angle, hardly can the bubbles move forward, but
form a gas film under the anode. Although occasionally
bubbles escape from the curved end of the anode, they
mainly escape from the side wall of the anode. The large
gas film expands, which means high resistance and energy
consuming in aluminum reduction processes. With non-
zero tilted angle, bubble motion under the anode is driven
by the buoyancy force, thus bubbles are easy to escape
through the curved end of the anode. LDV was used to
investigate the fluid flow pattern. The LDV measurements
reveal a recirculation flow pattern in side channel, similar
to the observation of the tracer dispersion. With 0o degree
tilted angle, the recirculation flow pattern also exists.
However, larger tilted angle and larger gas flow rate
generate larger velocity and bigger turbulent energy,
especially in the region close to the end of the anode and
the top surface. The flow pattern under the anode is also
measured using LDV. With 0o degree tilted angle, the flow
pattern and turbulent kinetic energy are more random than
the cases with non-0o degree tilted angle.
The investigation can go further to optimize the operation,
such as the micro scale behavior of bubbles, the effect of
tilted angle, anode curve or slots in more detail. CFD
simulation of the multiphase flow is also necessary to
extend the results of the physical modeling to a whole cell.
References
1) X. Wang et al: Light Metals 2007, Proceedings of
136th TMS Annual Meeting, (2007), 299-304.
2) D. S. Severo et al, Light Metals 2007, Proceedings
of 136th TMS Annual Meeting, (2007), 287-292.
3) W. Haupin and W. McGrew, in Light Metals
Conference Proceedings, (1974), 37-47.
4) E. Dernedde and E. Cambridge, in Light Metals
Conference Proceedings, (1975), 111-122.
5) M. M. Bilek et al: Light Metals: Proceedings of
Sessions, TMS Annual Meeting, (1994), 323-331.
6) C. Droste: private communication, (2006).
7) G. Bearne et al: Light Metals 2007, Proceedings
of 136th TMS Annual Meeting, (2007), 305-310.
8) N. Richards, in Light Metals Conference
Proceedings, , (2003), 315-322.
9) M. A. Cooksey et al: Light Metals 2006, 135th
TMS Annual Meeting, (2006), 359-365.
10) J. J. J. Chen, et al: Chemical Engineering
Research & Design, (2001), 79 (A4), 383.
11) S.fortin et al: Light Metals, (1984), 721.
12) S. Fortin et al, in Light Metals Conference
Proceedings, (1984), 721-741.
13) F. N. Ngoya and J. Thonstad: Electrochim. Acta,
(1985), 30, 1659.
14) J. Zoric and A. Solheim: Jounral of Applied
Electrochmistry, (2000), 30, 787.
15) N. Zhou and X. Xia: Light Metal, (2004), (12), 26.
16) L. I. Kiss et al: Light Metals 2005, Proceedings of
TMS Annual Meeting, (2005), 559-564.
17) A. Perron et al: Light Metals 2005, Proceedings of
135th TMS Annual Meeting, (2005), 565-570.
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