Light Metals 2009 Edited by: Geoff Bearne TMS (The Minerals, Metals & Materials Society), 2009

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: zhanglife@mst.edu 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-Hroult 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 Fig.1 Schematic phenomena in aluminum electrolysis cell considering alumina addition 6) 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).

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, seethrough 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

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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.

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. iRT (2) [m3 s 1m 2 ] q=
4 FP

where i is the anodic current density, (Am-2), R is gas, T is Absolute temperature (K), F is Faradays constant, P is pressure (Pa). Table 2 Parameters in the water model Items Value Anode cathode distance (ACD) 40mm Anode slope 0 , 0.4 , 1.1 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 Current Density (A/cm2) slope 0.2 0.4 0.6 0.8 1.0 0 0.4 1.1
Anode

Location -1(Side)
Anode

Location -2(Side)
Anode

Location -3(Side)
Anode

Fig.3

Schematic of the water model

Location -4(Bottom)
Anode

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 to 1.1. 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

Fig.4

Location -5(Front) 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

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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).

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 0 tilted angle, the tracer stagnates under the anode for a long time. If the tilted angle is larger than 0.4, 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.

(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/minm2, and the anode tilted angle is various from 0 to 1.1. 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 0.4, 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

Fig.6 Bubble motion viewed from the front of the anode: upper- tilted angle 0; lower- tilted angle 1.1

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part of the bubble creates a counter flow to respect the continuity. 17)

Fig.9 Fig.7 Tracer dispersion at different time (tilted angle 0.4)

Flow around a moving bubble obtained with a PIV system 17)

The effect of the gas flow rate The tilted angle was set to 1.1, 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/minm2 (equivalent 0.5A/cm2) gas, it takes ~ 6s for the tracer to move from the bottom to the side, and under 157L/minm2 (equivalent 1A/cm2) gas, only 4s is needed.

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.

(a) Flow rate of 70L/minm2, t=0s

(b) Flow rate of 70L/minm2, t=6s

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

(c) Flow rate of 157L/minm2, t=0s

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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.

(d) Flow rate of 157L/minm2, t=4s Fig.10 Tracer dispersion (Tilted angle 1.1) LDV Measurement In this current chapter, the fluid flow in the water model of the aluminum electrolysis cell is characterized using a twocomponent 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/s2), is calculated according to:

k = 1 2 ( u 2 + v 2 )

(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 ACD, mm 40 40 Anode slope, 0 1.1 Gas flow rate, L/min 64.2 16 Case 3 40 1.1 64.2

a) Side Channel

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

b) Under Anode Fig.11 Measured velocity and turbulent energy (Anode tilted angle, 0, Gas flow rate, 64.2L/min)

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a) Side Channel

consuming in aluminum reduction processes. With nonzero 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) 2) 3) 4) 5) X. Wang et al: Light Metals 2007, Proceedings of 136th TMS Annual Meeting, (2007), 299-304. D. S. Severo et al, Light Metals 2007, Proceedings of 136th TMS Annual Meeting, (2007), 287-292. W. Haupin and W. McGrew, in Light Metals Conference Proceedings, (1974), 37-47. E. Dernedde and E. Cambridge, in Light Metals Conference Proceedings, (1975), 111-122. M. M. Bilek et al: Light Metals: Proceedings of Sessions, TMS Annual Meeting, (1994), 323-331. C. Droste: private communication, (2006). G. Bearne et al: Light Metals 2007, Proceedings of 136th TMS Annual Meeting, (2007), 305-310. N. Richards, in Light Metals Conference Proceedings, , (2003), 315-322. M. A. Cooksey et al: Light Metals 2006, 135th TMS Annual Meeting, (2006), 359-365. J. J. J. Chen, et al: Chemical Engineering Research & Design, (2001), 79 (A4), 383. S.fortin et al: Light Metals, (1984), 721. S. Fortin et al, in Light Metals Conference Proceedings, (1984), 721-741. F. N. Ngoya and J. Thonstad: Electrochim. Acta, (1985), 30, 1659. J. Zoric and A. Solheim: Jounral of Applied Electrochmistry, (2000), 30, 787. N. Zhou and X. Xia: Light Metal, (2004), (12), 26. L. I. Kiss et al: Light Metals 2005, Proceedings of TMS Annual Meeting, (2005), 559-564. A. Perron et al: Light Metals 2005, Proceedings of 135th TMS Annual Meeting, (2005), 565-570.

b) Under Anode Fig.12 Measured velocity and turbulent energy (Anode tilted angle, 1.1, Gas flow rate, 16L/min)

a) Side Channel

6) 7) 8) 9) 10)

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

11) 12) 13) 14) 15) 16) 17)

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