Tag: Liquid Metal

Schematic diagram of overlapping powder particles.

Because the particle size of the powder used for HP-LPBF is much smaller than 100 μm, the effect of van der Waals forces must be considered. Therefore, the cohesive force �jkr of the Hertz–Mindlin model was used instead of van der Waals forces,⁷² with the following expression:�jkr=−4��0�*�1.5+4�*3�*�3,

(4)1�*=(1−��2)��+(1−��2)��,

(5)1�*=1��+1��,

(6)

where �* is the equivalent Young’s modulus in GPa; �* is the equivalent particle radius in m; �0 is the surface energy of the powder particles in J/m²; α is the contact radius in m; �� and �� are the Young’s modulus of the unit particles � and �⁠, respectively, in GPa; and �� and �� are the Poisson’s ratio of the unit particles � and �⁠, respectively.

2. Model building

Figure 2 shows a 3D powder bed model generated using DEM with a coarse powder geometry of 1000 × 400 × 30 μm³. The powder layer thickness is 30 μm, and the powder bed porosity is 40%. The average particle size of this spherical powder is 31.7 μm and is normally distributed in the range of 15–53 μm. The geometry of the fine powder was 1000 × 400 × 20 μm³, with a layer thickness of 20 μm, and the powder bed porosity of 40%. The average particle size of this spherical powder is 11.5 μm and is normally distributed in the range of 5–25 μm. After the 3D powder bed model is generated, it needs to be imported into the CFD simulation software for calculation, and the imported geometric model is shown in Fig. 3. This geometric model is mainly composed of three parts: protective gas, powder bed, and substrate. Under the premise of ensuring the accuracy of the calculation, the mesh size is set to 3 μm, and the total number of coarse powder meshes is 1 704 940. The total number of fine powder meshes is 3 982 250.

FIG. 2.

Three-dimensional powder bed model: (a) coarse powder, (b) fine powder.

FIG. 3.

Geometric modeling of the powder bed computational domain: (a) coarse powder, (b) fine powder.

B. Modeling of fluid mechanics simulation

In order to solve the flow, melting, and solidification problems involved in HP-LPBF molten pool, the study must follow the three governing equations of conservation of mass, conservation of energy, and conservation of momentum.⁷³ The VOF method, which is the most widely used in fluid dynamics, is used to solve the molten pool dynamics model.

1. VOF

VOF is a method for tracking the free interface between the gas and liquid phases on the molten pool surface. The core idea of the method is to define a volume fraction function F within each grid, indicating the proportion of the grid space occupied by the material, 0 ≤ F ≤ 1 in Fig. 4. Specifically, when F = 0, the grid is empty and belongs to the gas-phase region; when F = 1, the grid is completely filled with material and belongs to the liquid-phase region; and when 0 < F < 1, the grid contains free surfaces and belongs to the mixed region. The direction normal to the free surface is the direction of the fastest change in the volume fraction F (the direction of the gradient of the volume fraction), and the direction of the gradient of the volume fraction can be calculated from the values of the volume fractions in the neighboring grids.⁷⁴ The equations controlling the VOF are expressed as follows:𝛻��+�⋅(��→)=0,

(7)

where t is the time in s and �→ is the liquid velocity in m/s.

FIG. 4.

Schematic diagram of VOF.

The material parameters of the mixing zone are altered due to the inclusion of both the gas and liquid phases. Therefore, in order to represent the density of the mixing zone, the average density �¯ is used, which is expressed as follows:⁷²�¯=(1−�1)�gas+�1�metal,

(8)

where �1 is the proportion of liquid phase, �gas is the density of protective gas in kg/m³, and �metal is the density of metal in kg/m³.

2. Control equations and boundary conditions

Figure 5 is a schematic diagram of the HP-LPBF melting process. First, the laser light strikes a localized area of the material and rapidly heats up the area. Next, the energy absorbed in the region is diffused through a variety of pathways (heat conduction, heat convection, and surface radiation), and this process triggers complex phase transition phenomena (melting, evaporation, and solidification). In metals undergoing melting, the driving forces include surface tension and the Marangoni effect, recoil due to evaporation, and buoyancy due to gravity and uneven density. The above physical phenomena interact with each other and do not occur independently.

FIG. 5.

Schematic diagram of HP-LPBF melting process.

Laser heat sourceThe Gaussian surface heat source model is used as the laser heat source model with the following expression:�=2�0��2exp(−2�12��2),(9)where � is the heat flow density in W/m², �0 is the absorption rate of SS316L, �� is the radius of the laser focal spot in m, and �1 is the radial distance from the center of the laser focal spot in m. The laser focal spot can be used for a wide range of applications.
Energy absorptionThe formula for calculating the laser absorption �0 of SS316L is as follows:�0=0.365(�0[1+�0(�−20)]/�)0.5,(10)where �0 is the direct current resistivity of SS316L at 20 °C in Ω m, �0 is the resistance temperature coefficient in ppm/°C, � is the temperature in °C, and � is the laser wavelength in m.
Heat transferThe basic principle of heat transfer is conservation of energy, which is expressed as follows:𝛻𝛻𝛻�(��)��+�·(��→�)=�·(�0��)+��,(11)where � is the density of liquid phase SS316L in kg/m³, �� is the specific heat capacity of SS316L in J/(kg K), 𝛻� is the gradient operator, t is the time in s, T is the temperature in K, 𝛻�� is the temperature gradient, �→ is the velocity vector, �0 is the coefficient of thermal conduction of SS316L in W/(m K), and �� is the thermal energy dissipation term in the molten pool.
Molten pool flowThe following three conditions need to be satisfied for the molten pool to flow:
- Conservation of mass with the following expression:𝛻�·(��→)=0.(12)
- Conservation of momentum (Navier–Stokes equation) with the following expression:𝛻𝛻𝛻𝛻��→��+�(�→·�)�→=�·[−pI+�(��→+(��→)�)]+�,(13)where � is the pressure in Pa exerted on the liquid phase SS316L microelement, � is the unit matrix, � is the fluid viscosity in N s/m², and � is the volumetric force (gravity, atmospheric pressure, surface tension, vapor recoil, and the Marangoni effect).
- Conservation of energy, see Eq. (11)
Surface tension and the Marangoni effectThe effect of temperature on the surface tension coefficient is considered and set as a linear relationship with the following expression:�=�0−��dT(�−��),(14)where � is the surface tension of the molten pool at temperature T in N/m, �� is the melting temperature of SS316L in K, �0 is the surface tension of the molten pool at temperature �� in Pa, and σdσ/ dT is the surface tension temperature coefficient in N/(m K).In general, surface tension decreases with increasing temperature. A temperature gradient causes a gradient in surface tension that drives the liquid to flow, known as the Marangoni effect.
Metal vapor recoilAt higher input energy densities, the maximum temperature of the molten pool surface reaches the evaporation temperature of the material, and a gasification recoil pressure occurs vertically downward toward the molten pool surface, which will be the dominant driving force for the molten pool flow.⁷⁵ The expression is as follows:��=0.54�� exp ��−��0��,(15)where �� is the gasification recoil pressure in Pa, �� is the ambient pressure in kPa, �� is the latent heat of evaporation in J/kg, �0 is the gas constant in J/(mol K), T is the surface temperature of the molten pool in K, and T_e is the evaporation temperature in K.
Solid–liquid–gas phase transitionWhen the laser hits the powder layer, the powder goes through three stages: heating, melting, and solidification. During the solidification phase, mutual transformations between solid, liquid, and gaseous states occur. At this point, the latent heat of phase transition absorbed or released during the phase transition needs to be considered.⁶⁸ The phase transition is represented based on the relationship between energy and temperature with the following expression:�=��,(�<��),�(��)+�−��−��,(��<�<��)�(��)+(�−��)��,(��<�),,(16)where �� and �� are solid and liquid phase density, respectively, of SS316L in kg/m³. �� and �� unit volume of solid and liquid phase-specific heat capacity, respectively, of SS316L in J/(kg K). �� and ��⁠, respectively, are the solidification temperature and melting temperature of SS316L in K. �� is the latent heat of the phase transition of SS316L melting in J/kg.

3. Assumptions

The CFD model was computed using the commercial software package FLOW-3D.⁷⁶ In order to simplify the calculation and solution process while ensuring the accuracy of the results, the model makes the following assumptions:

It is assumed that the effects of thermal stress and material solid-phase thermal expansion on the calculation results are negligible.
The molten pool flow is assumed to be a Newtonian incompressible laminar flow, while the effects of liquid thermal expansion and density on the results are neglected.
It is assumed that the surface tension can be simplified to an equivalent pressure acting on the free surface of the molten pool, and the effect of chemical composition on the results is negligible.
Neglecting the effect of the gas flow field on the molten pool.
The mass loss due to evaporation of the liquid metal is not considered.
The influence of the plasma effect of the molten metal on the calculation results is neglected.

It is worth noting that the formulation of assumptions requires a trade-off between accuracy and computational efficiency. In the above models, some physical phenomena that have a small effect or high difficulty on the calculation results are simplified or ignored. Such simplifications make numerical simulations more efficient and computationally tractable, while still yielding accurate results.

4. Initial conditions

The preheating temperature of the substrate was set to 393 K, at which time all materials were in the solid state and the flow rate was zero.

5. Material parameters

The material used is SS316L and the relevant parameters required for numerical simulations are shown in Table I.^46,77,78

TABLE I.

SS316L-related parameters.

Property	Symbol	Value
Density of solid metal (kg/m³)	�metal	7980
Solid phase line temperature (K)	��	1658
Liquid phase line temperature (K)	��	1723
Vaporization temperature (K)	��	3090
Latent heat of melting (⁠ J/kg⁠)	��	2.60×105
Latent heat of evaporation (⁠ J/kg⁠)	��	7.45×106
Surface tension of liquid phase (N /m⁠)	�	1.60
Liquid metal viscosity (kg/m s)	��	6×10−3
Gaseous metal viscosity (kg/m s)	�gas	1.85×10−5
Temperature coefficient of surface tension (N/m K)	��/�T	0.80×10−3
Molar mass (⁠ kg/mol⁠)	M	0.05 593
Emissivity	�	0.26
Laser absorption	�0	0.35
Ambient pressure (kPa)	��	101 325
Ambient temperature (K)	�0	300
Stefan–Boltzmann constant (W/m² K⁴)	�	5.67×10−8
Thermal conductivity of metals (⁠ W/m K⁠)	�	24.55
Density of protective gas (kg/m³)	�gas	1.25
Coefficient of thermal expansion (/K)	��	16×10−6
Generalized gas constant (⁠ J/mol K⁠)	R	8.314

III. RESULTS AND DISCUSSION

With the objective of studying in depth the evolutionary patterns of single-track and double-track molten pool development, detailed observations were made for certain specific locations in the model, as shown in Fig. 6. In this figure, P1 and P2 represent the longitudinal tangents to the centers of the two melt tracks in the XZ plane, while L1 is the transverse profile in the YZ plane. The scanning direction is positive and negative along the X axis. Points A and B are the locations of the centers of the molten pool of the first and second melt tracks, respectively (x = 1.995 × 10⁻⁴, y = 5 × 10⁻⁷, and z = −4.85 × 10⁻⁵).

FIG. 6.

Schematic diagram of observation position.

A. Single-track simulation

A series of single-track molten pool simulation experiments were carried out in order to investigate the influence law of laser power as well as scanning speed on the HP-LPBF process. Figure 7 demonstrates the evolution of the 3D morphology and temperature field of the single-track molten pool in the time period of 50–500 μs under a laser power of 100 W and a scanning speed of 800 mm/s. The powder bed is in the natural cooling state. When t = 50 μs, the powder is heated by the laser heat and rapidly melts and settles to form the initial molten pool. This process is accompanied by partial melting of the substrate and solidification together with the melted powder. The molten pool rapidly expands with increasing width, depth, length, and temperature, as shown in Fig. 7(a). When t = 150 μs, the molten pool expands more obviously, and the temperature starts to transfer to the surrounding area, forming a heat-affected zone. At this point, the width of the molten pool tends to stabilize, and the temperature in the center of the molten pool has reached its peak and remains largely stable. However, the phenomenon of molten pool spatter was also observed in this process, as shown in Fig. 7(b). As time advances, when t = 300 μs, solidification begins to occur at the tail of the molten pool, and tiny ripples are produced on the solidified surface. This is due to the fact that the melt flows toward the region with large temperature gradient under the influence of Marangoni convection and solidifies together with the melt at the end of the bath. At this point, the temperature gradient at the front of the bath is significantly larger than at the end. While the width of the molten pool was gradually reduced, the shape of the molten pool was gradually changed to a “comet” shape. In addition, a slight depression was observed at the top of the bath because the peak temperature at the surface of the bath reached the evaporation temperature, which resulted in a recoil pressure perpendicular to the surface of the bath downward, creating a depressed region. As the laser focal spot moves and is paired with the Marangoni convection of the melt, these recessed areas will be filled in as shown in Fig. 7(c). It has been shown that the depressed regions are the result of the coupled effect of Marangoni convection, recoil pressure, and surface tension.⁷⁹ By t = 500 μs, the width and height of the molten pool stabilize and show a “comet” shape in Fig. 7(d).

FIG. 7.

Single-track molten pool process: (a) t = 50 ��⁠, (b) t = 150 ��⁠, (c) t = 300 ��⁠, (d) t = 500 ��⁠.

Figure 8 depicts the velocity vector diagram of the P1 profile in a single-track molten pool, the length of the arrows represents the magnitude of the velocity, and the maximum velocity is about 2.36 m/s. When t = 50 μs, the molten pool takes shape, and the velocities at the two ends of the pool are the largest. The variation of the velocities at the front end is especially more significant in Fig. 8(a). As the time advances to t = 150 μs, the molten pool expands rapidly, in which the velocity at the tail increases and changes more significantly, while the velocity at the front is relatively small. At this stage, the melt moves backward from the center of the molten pool, which in turn expands the molten pool area. The melt at the back end of the molten pool center flows backward along the edge of the molten pool surface and then converges along the edge of the molten pool to the bottom center, rising to form a closed loop. Similarly, a similar closed loop is formed at the front end of the center of the bath, but with a shorter path. However, a large portion of the melt in the center of the closed loop formed at the front end of the bath is in a nearly stationary state. The main cause of this melt flow phenomenon is the effect of temperature gradient and surface tension (the Marangoni effect), as shown in Figs. 8(b) and 8(e). This dynamic behavior of the melt tends to form an “elliptical” pool. At t = 300 μs, the tendency of the above two melt flows to close the loop is more prominent and faster in Fig. 8(c). When t = 500 μs, the velocity vector of the molten pool shows a stable trend, and the closed loop of melt flow also remains stable. With the gradual laser focal spot movement, the melt is gradually solidified at its tail, and finally, a continuous and stable single track is formed in Fig. 8(d).

FIG. 8.

Vector plot of single-track molten pool velocity in XZ longitudinal section: (a) t = 50 ��⁠, (b) t = 150 ��⁠, (c) t = 300 ��⁠, (d) t = 500 ��⁠, (e) molten pool flow.

In order to explore in depth the transient evolution of the molten pool, the evolution of the single-track temperature field and the melt flow was monitored in the YZ cross section. Figure 9(a) shows the state of the powder bed at the initial moment. When t = 250 μs, the laser focal spot acts on the powder bed and the powder starts to melt and gradually collects in the molten pool. At this time, the substrate will also start to melt, and the melt flow mainly moves in the downward and outward directions and the velocity is maximum at the edges in Fig. 9(b). When t = 300 μs, the width and depth of the molten pool increase due to the recoil pressure. At this time, the melt flows more slowly at the center, but the direction of motion is still downward in Fig. 9(c). When t = 350 μs, the width and depth of the molten pool further increase, at which time the intensity of the melt flow reaches its peak and the direction of motion remains the same in Fig. 9(d). When t = 400 μs, the melt starts to move upward, and the surrounding powder or molten material gradually fills up, causing the surface of the molten pool to begin to flatten. At this time, the maximum velocity of the melt is at the center of the bath, while the velocity at the edge is close to zero, and the edge of the melt starts to solidify in Fig. 9(e). When t = 450 μs, the melt continues to move upward, forming a convex surface of the melt track. However, the melt movement slows down, as shown in Fig. 9(f). When t = 500 μs, the melt further moves upward and its speed gradually becomes smaller. At the same time, the melt solidifies further, as shown in Fig. 9(g). When t = 550 μs, the melt track is basically formed into a single track with a similar “mountain” shape. At this stage, the velocity is close to zero only at the center of the molten pool, and the flow behavior of the melt is poor in Fig. 9(h). At t = 600 μs, the melt stops moving and solidification is rapidly completed. Up to this point, a single track is formed in Fig. 9(i). During the laser action on the powder bed, the substrate melts and combines with the molten state powder. The powder-to-powder fusion is like the convergence of water droplets, which are rapidly fused by surface tension. However, the fusion between the molten state powder and the substrate occurs driven by surface tension, and the molten powder around the molten pool is pulled toward the substrate (a wetting effect occurs), which ultimately results in the formation of a monolithic whole.^38,80,81

FIG. 9.

Evolution of single-track molten pool temperature and melt flow in the YZ cross section: (a) t = 0 ��⁠, (b) t = 250 ��⁠, (c) t = 300 ��⁠, (d) t = 350 ��⁠, (e) t = 400 ��⁠, (f) t = 450 ��⁠, (g) t = 500 ��⁠, (h) t = 550 ��⁠, (i) t = 600 ��⁠.

The wetting ability between the liquid metal and the solid substrate in the molten pool directly affects the degree of balling of the melt,^82,83 and the wetting ability can be measured by the contact angle of a single track in Fig. 10. A smaller value of contact angle represents better wettability. The contact angle α can be calculated by�=�1−�22,

(17)

where �1 and �2 are the contact angles of the left and right regions, respectively.

FIG. 10.

Schematic of contact angle.

Relevant studies have confirmed that the wettability is better at a contact angle α around or below 40°.⁸⁴ After measurement, a single-track contact angle α of about 33° was obtained under this process parameter, which further confirms the good wettability.

B. Double-track simulation

In order to deeply investigate the influence of hatch spacing on the characteristics of the HP-LPBF process, a series of double-track molten pool simulation experiments were systematically carried out. Figure 11 shows in detail the dynamic changes of the 3D morphology and temperature field of the double-track molten pool in the time period of 2050–2500 μs under the conditions of laser power of 100 W, scanning speed of 800 mm/s, and hatch spacing of 0.06 mm. By comparing the study with Fig. 7, it is observed that the basic characteristics of the 3D morphology and temperature field of the second track are similar to those of the first track. However, there are subtle differences between them. The first track exhibits a basically symmetric shape, but the second track morphology shows a slight deviation influenced by the difference in thermal diffusion rate between the solidified metal and the powder. Otherwise, the other characteristic information is almost the same as that of the first track. Figure 12 shows the velocity vector plot of the P2 profile in the double-track molten pool, with a maximum velocity of about 2.63 m/s. The melt dynamics at both ends of the pool are more stable at t = 2050 μs, where the maximum rate of the second track is only 1/3 of that of the first one. Other than that, the rest of the information is almost no significant difference from the characteristic information of the first track. Figure 13 demonstrates a detailed observation of the double-track temperature field and melts flow in the YZ cross section, and a comparative study with Fig. 9 reveals that the width of the second track is slightly wider. In addition, after the melt direction shifts from bottom to top, the first track undergoes four time periods (50 μs) to reach full solidification, while the second track takes five time periods. This is due to the presence of significant heat buildup in the powder bed after the forming of the first track, resulting in a longer dynamic time of the melt and an increased molten pool lifetime. In conclusion, the level of specimen forming can be significantly optimized by adjusting the laser power and hatch spacing.

FIG. 11.

Double-track molten pool process: (a) t = 2050 ��⁠, (b) t = 2150 ��⁠, (c) t = 2300 ��⁠, (d) t = 2500 ��⁠.

FIG. 12.

Vector plot of double-track molten pool velocity in XZ longitudinal section: (a) t = 2050 ��⁠, (b) t = 2150 ��⁠, (c) t = 2300 ��⁠, (d) t = 2500 ��⁠.

FIG. 13.

Evolution of double-track molten pool temperature and melt flow in the YZ cross section: (a) t = 2250 ��⁠, (b) t = 2300 ��⁠, (c) t = 2350 ��⁠, (d) t = 2400 ��⁠, (e) t = 2450 ��⁠, (f) t = 2500 ��⁠, (g) t = 2550 ��⁠, (h) t = 2600 ��⁠, (i) t = 2650 ��⁠.

In order to quantitatively detect the molten pool dimensions as well as the remolten region dimensions, the molten pool characterization information in Fig. 14 is constructed by drawing the boundary on the YZ cross section based on the isothermal surface of the liquid phase line. It can be observed that the heights of the first track and second track are basically the same, but the depth of the second track increases relative to the first track. The molten pool width is mainly positively correlated with the laser power as well as the scanning speed (the laser line energy density �⁠). However, the remelted zone width is negatively correlated with the hatch spacing (the overlapping ratio). Overall, the forming quality of the specimens can be directly influenced by adjusting the laser power, scanning speed, and hatch spacing.

FIG. 14.

Double-track molten pool characterization information on YZ cross section.

In order to study the variation rule of the temperature in the center of the molten pool with time, Fig. 15 demonstrates the temperature variation curves with time for two reference points, A and B. Among them, the red dotted line indicates the liquid phase line temperature of SS316L. From the figure, it can be seen that the maximum temperature at the center of the molten pool in the first track is lower than that in the second track, which is mainly due to the heat accumulation generated after passing through the first track. The maximum temperature gradient was calculated to be 1.69 × 10⁸ K/s. When the laser scanned the first track, the temperature in the center of the molten pool of the second track increased slightly. Similarly, when the laser scanned the second track, a similar situation existed in the first track. Since the temperature gradient in the second track is larger than that in the first track, the residence time of the liquid phase in the molten pool of the first track is longer than that of the second track.

FIG. 15.

Temperature profiles as a function of time for two reference points A and B.

C. Simulation analysis of molten pool under different process parameters

In order to deeply investigate the effects of various process parameters on the mesoscopic-scale temperature field, molten pool characteristic information and defects of HP-LPBF, numerical simulation experiments on mesoscopic-scale laser power, scanning speed, and hatch spacing of double-track molten pools were carried out.

1. Laser power

Figure 16 shows the effects of different laser power on the morphology and temperature field of the double-track molten pool at a scanning speed of 800 mm/s and a hatch spacing of 0.06 mm. When P = 50 W, a smaller molten pool is formed due to the lower heat generated by the Gaussian light source per unit time. This leads to a smaller track width, which results in adjacent track not lapping properly and the presence of a large number of unmelted powder particles, resulting in an increase in the number of defects, such as pores in the specimen. The surface of the track is relatively flat, and the depth is small. In addition, the temperature gradient before and after the molten pool was large, and the depression location appeared at the biased front end in Fig. 16(a). When P = 100 W, the surface of the track is flat and smooth with excellent lap. Due to the Marangoni effect, the velocity field of the molten pool is in the form of “vortex,” and the melt has good fluidity, and the maximum velocity reaches 2.15 m/s in Fig. 16(b). When P = 200 W, the heat generated by the Gaussian light source per unit time is too large, resulting in the melt rapidly reaching the evaporation temperature, generating a huge recoil pressure, forming a large molten pool, and the surface of the track is obviously raised. The melt movement is intense, especially the closed loop at the center end of the molten pool. At this time, the depth and width of the molten pool are large, leading to the expansion of the remolten region and the increased chance of the appearance of porosity defects in Fig. 16(c). The results show that at low laser power, the surface tension in the molten pool is dominant. At high laser power, recoil pressure is its main role.

FIG. 16.

Simulation results of double-track molten pool under different laser powers: (a) P = 50 W, (b) P = 100 W, (c) P = 200 W.

Table II shows the effect of different laser powers on the characteristic information of the double-track molten pool at a scanning speed of 800 mm/s and a hatch spacing of 0.06 mm. The negative overlapping ratio in the table indicates that the melt tracks are not lapped, and 26/29 indicates the melt depth of the first track/second track. It can be seen that with the increase in laser power, the melt depth, melt width, melt height, and remelted zone show a gradual increase. At the same time, the overlapping ratio also increases. Especially in the process of laser power from 50 to 200 W, the melting depth and melting width increased the most, which increased nearly 2 and 1.5 times, respectively. Meanwhile, the overlapping ratio also increases with the increase in laser power, which indicates that the melting and fusion of materials are better at high laser power. On the other hand, the dimensions of the molten pool did not change uniformly with the change of laser power. Specifically, the depth-to-width ratio of the molten pool increased from about 0.30 to 0.39 during the increase from 50 to 120 W, which further indicates that the effective heat transfer in the vertical direction is greater than that in the horizontal direction with the increase in laser power. This dimensional response to laser power is mainly affected by the recoil pressure and also by the difference in the densification degree between the powder layer and the metal substrate. In addition, according to the experimental results, the contact angle shows a tendency to increase and then decrease during the process of laser power increase, and always stays within the range of less than 33°. Therefore, in practical applications, it is necessary to select the appropriate laser power according to the specific needs in order to achieve the best processing results.

TABLE II.

Double-track molten pool characterization information at different laser powers.

Laser power (W)	Depth (μm)	Width (μm)	Height (μm)	Remolten region (μm)	Overlapping ratio (%)	Contact angle (°)
50	16	54	11	/	−10	23
100	26/29	74	14	18	23.33	33
200	37/45	116	21	52	93.33	28

2. Scanning speed

Figure 17 demonstrates the effect of different scanning speeds on the morphology and temperature field of the double-track molten pool at a laser power of 100 W and a hatch spacing of 0.06 mm. With the gradual increase in scanning speed, the surface morphology of the molten pool evolves from circular to elliptical. When � = 200 mm/s, the slow scanning speed causes the material to absorb too much heat, which is very easy to trigger the overburning phenomenon. At this point, the molten pool is larger and the surface morphology is uneven. This situation is consistent with the previously discussed scenario with high laser power in Fig. 17(a). However, when � = 1600 mm/s, the scanning speed is too fast, resulting in the material not being able to absorb sufficient heat, which triggers the powder particles that fail to melt completely to have a direct effect on the bonding of the melt to the substrate. At this time, the molten pool volume is relatively small and the neighboring melt track cannot lap properly. This result is consistent with the previously discussed case of low laser power in Fig. 17(b). Overall, the ratio of the laser power to the scanning speed (the line energy density �⁠) has a direct effect on the temperature field and surface morphology of the molten pool.

FIG. 17.

Simulation results of double-track molten pool under different scanning speed: (a) � = 200 mm/s, (b) � = 1600 mm/s.

Table III shows the effects of different scanning speed on the characteristic information of the double-track molten pool under the condition of laser power of 100 W and hatch spacing of 0.06 mm. It can be seen that the scanning speed has a significant effect on the melt depth, melt width, melt height, remolten region, and overlapping ratio. With the increase in scanning speed, the melt depth, melt width, melt height, remelted zone, and overlapping ratio show a gradual decreasing trend. Among them, the melt depth and melt width decreased faster, while the melt height and remolten region decreased relatively slowly. In addition, when the scanning speed was increased from 200 to 800 mm/s, the decreasing speeds of melt depth and melt width were significantly accelerated, while the decreasing speeds of overlapping ratio were relatively slow. When the scanning speed was further increased to 1600 mm/s, the decreasing speeds of melt depth and melt width were further accelerated, and the un-lapped condition of the melt channel also appeared. In addition, the contact angle increases and then decreases with the scanning speed, and both are lower than 33°. Therefore, when selecting the scanning speed, it is necessary to make reasonable trade-offs according to the specific situation, and take into account the factors of melt depth, melt width, melt height, remolten region, and overlapping ratio, in order to achieve the best processing results.

TABLE III.

Double-track molten pool characterization information at different scanning speeds.

Scanning speed (mm/s)	Depth (μm)	Width (μm)	Height (μm)	Remolten region (μm)	Overlapping ratio (%)	Contact angle (°)
200	55/68	182	19/32	124	203.33	22
1600	13	50	11	/	−16.67	31

3. Hatch spacing

Figure 18 shows the effect of different hatch spacing on the morphology and temperature field of the double-track molten pool under the condition of laser power of 100 W and scanning speed of 800 mm/s. The surface morphology and temperature field of the first track and second track are basically the same, but slightly different. The first track shows a basically symmetric morphology along the scanning direction, while the second track shows a slight offset due to the difference in the heat transfer rate between the solidified material and the powder particles. When the hatch spacing is too small, the overlapping ratio increases and the probability of defects caused by remelting phenomenon grows. When the hatch spacing is too large, the neighboring melt track cannot overlap properly, and the powder particles are not completely melted, leading to an increase in the number of holes. In conclusion, the ratio of the line energy density � to the hatch spacing (the volume energy density E) has a significant effect on the temperature field and surface morphology of the molten pool.

FIG. 18.

Simulation results of double-track molten pool under different hatch spacings: (a) H = 0.03 mm, (b) H = 0.12 mm.

Table IV shows the effects of different hatch spacing on the characteristic information of the double-track molten pool under the condition of laser power of 100 W and scanning speed of 800 mm/s. It can be seen that the hatch spacing has little effect on the melt depth, melt width, and melt height, but has some effect on the remolten region. With the gradual expansion of hatch spacing, the remolten region shows a gradual decrease. At the same time, the overlapping ratio also decreased with the increase in hatch spacing. In addition, it is observed that the contact angle shows a tendency to increase and then remain stable when the hatch spacing increases, which has a more limited effect on it. Therefore, trade-offs and decisions need to be made on a case-by-case basis when selecting the hatch spacing.

TABLE IV.

Double-track molten pool characterization information at different hatch spacings.

Hatch spacing (mm)	Depth (μm)	Width (μm)	Height (μm)	Remolten region (μm)	Overlapping ratio (%)	Contact angle (°)
0.03	25/27	82	14	59	173.33	30
0.12	26	78	14	/	−35	33

In summary, the laser power, scanning speed, and hatch spacing have a significant effect on the formation of the molten pool, and the correct selection of these three process parameters is crucial to ensure the forming quality. In addition, the melt depth of the second track is slightly larger than that of the first track at higher line energy density � and volume energy density E. This is mainly due to the fact that a large amount of heat accumulation is generated after the first track, forming a larger molten pool volume, which leads to an increase in the melt depth.

D. Simulation analysis of molten pool with powder particle size and laser focal spot diameter

Figure 19 demonstrates the effect of different powder particle sizes and laser focal spot diameters on the morphology and temperature field of the double-track molten pool under a laser power of 100 W, a scanning speed of 800 mm/s, and a hatch spacing of 0.06 mm. In the process of melting coarse powder with small laser focal spot diameter, the laser energy cannot completely melt the larger powder particles, resulting in their partial melting and further generating excessive pore defects. The larger powder particles tend to generate zigzag molten pool edges, which cause an increase in the roughness of the melt track surface. In addition, the molten pool is also prone to generate the present spatter phenomenon, which can directly affect the quality of forming. The volume of the formed molten pool is relatively small, while the melt depth, melt width, and melt height are all smaller relative to the fine powder in Fig. 19(a). In the process of melting fine powders with a large laser focal spot diameter, the laser energy is able to melt the fine powder particles sufficiently, even to the point of overmelting. This results in a large number of fine spatters being generated at the edge of the molten pool, which causes porosity defects in the melt track in Fig. 19(b). In addition, the maximum velocity of the molten pool is larger for large powder particle sizes compared to small powder particle sizes, which indicates that the temperature gradient in the molten pool is larger for large powder particle sizes and the melt motion is more intense. However, the size of the laser focal spot diameter has a relatively small effect on the melt motion. However, a larger focal spot diameter induces a larger melt volume with greater depth, width, and height. In conclusion, a small powder size helps to reduce the surface roughness of the specimen, and a small laser spot diameter reduces the minimum forming size of a single track.

FIG. 19.

The International Journal of Advanced Manufacturing Technology (2023)Cite this article

Simulation results of double-track molten pool with different powder particle size and laser focal spot diameter: (a) focal spot = 25 μm, coarse powder, (b) focal spot = 80 μm, fine powder.

Table V shows the maximum temperature gradient at the reference point for different powder sizes and laser focal spot diameters. As can be seen from the table, the maximum temperature gradient is lower than that of HP-LPBF for both coarse powders with a small laser spot diameter and fine powders with a large spot diameter, a phenomenon that leads to an increase in the heat transfer rate of HP-LPBF, which in turn leads to a corresponding increase in the cooling rate and, ultimately, to the formation of finer microstructures.

TABLE V.

Maximum temperature gradient at the reference point for different powder particle sizes and laser focal spot diameters.

Laser power (W)	Scanning speed (mm/s)	Hatch spacing (mm)	Average powder size (μm)	Laser focal spot diameter (μm)	Maximum temperature gradient (×10⁷ K/s)
100	800	0.06	31.7	25	7.89
100	800	0.06	11.5	80	7.11

IV. CONCLUSIONS

In this study, the geometrical characteristics of 3D coarse and fine powder particles were first calculated using DEM and then numerical simulations of single track and double track in the process of forming SS316L from monolayer HP-LPBF at mesoscopic scale were developed using CFD method. The effects of Marangoni convection, surface tension, recoil pressure, gravity, thermal convection, thermal radiation, and evaporative heat dissipation on the heat and mass transfer in the molten pool were considered in this model. The effects of laser power, scanning speed, and hatch spacing on the dynamics of the single-track and double-track molten pools, as well as on other characteristic information, were investigated. The effects of the powder particle size on the molten pool were investigated comparatively with the laser focal spot diameter. The main conclusions are as follows:

The results show that the temperature gradient at the front of the molten pool is significantly larger than that at the tail, and the molten pool exhibits a “comet” morphology. At the top of the molten pool, there is a slightly concave region, which is the result of the coupling of Marangoni convection, recoil pressure, and surface tension. The melt flow forms two closed loops, which are mainly influenced by temperature gradients and surface tension. This special dynamic behavior of the melt tends to form an “elliptical” molten pool and an almost “mountain” shape in single-track forming.
The basic characteristics of the three-dimensional morphology and temperature field of the second track are similar to those of the first track, but there are subtle differences. The first track exhibits a basically symmetrical shape; however, due to the difference in thermal diffusion rates between the solidified metal and the powder, a slight asymmetry in the molten pool morphology of the second track occurs. After forming through the first track, there is a significant heat buildup in the powder bed, resulting in a longer dynamic time of the melt, which increases the life of the molten pool. The heights of the first track and second track remained essentially the same, but the depth of the second track was greater relative to the first track. In addition, the maximum temperature gradient was 1.69 × 10⁸ K/s during HP-LPBF forming.
At low laser power, the surface tension in the molten pool plays a dominant role. At high laser power, recoil pressure becomes the main influencing factor. With the increase of laser power, the effective heat transfer in the vertical direction is superior to that in the horizontal direction. With the gradual increase of scanning speed, the surface morphology of the molten pool evolves from circular to elliptical. In addition, the scanning speed has a significant effect on the melt depth, melt width, melt height, remolten region, and overlapping ratio. Too large or too small hatch spacing will lead to remelting or non-lap phenomenon, which in turn causes the formation of defects.
When using a small laser focal spot diameter, it is difficult to completely melt large powder particle sizes, resulting in partial melting and excessive porosity generation. At the same time, large powder particles produce curved edges of the molten pool, resulting in increased surface roughness of the melt track. In addition, spatter occurs, which directly affects the forming quality. At small focal spot diameters, the molten pool volume is relatively small, and the melt depth, the melt width, and the melt height are correspondingly small. Taken together, the small powder particle size helps to reduce surface roughness, while the small spot diameter reduces the forming size.

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좁은 간격 가스 텅스텐 아크 용접의 용융 풀 거동에 대한 수치 시뮬레이션

Numerical simulation on molten pool behavior of narrow gap gas tungsten arc welding

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Abstract

As a highly efficient thick plate welding resolution, narrow gap gas tungsten arc welding (NG-GTAW) is in the face of a series of problems like inter-layer defects like pores, lack of fusion, inclusion of impurity, and the sensitivity to poor sidewall fusion, which is hard to be repaired after the welding process. This study employs numerical simulation to investigate the molten pool behavior in NG-GTAW root welding. A 3D numerical model was established, where a body-fitted coordinate system was applied to simulate the electromagnetic force, and a bridge transition model was developed to investigate the wire–feed root welding. The simulated results were validated experimentally. Results show that the molten pool behavior is dominated by electromagnetic force when the welding current is relatively high, and the dynamic change of the vortex actually determines the molten pool morphology. For self-fusion welding, there are two symmetric inward vortices in the cross-section and one clockwise vortex in the longitudinal section. With the increasing welding current, the vortices in the cross-section gradually move to the arc center with a decreasing range, while the vortex in the longitudinal section moves backward. With the increasing traveling speed, the vortices in the cross-section move toward the surface of the molten pool with a decreasing range, and the horizontal component of liquid metal velocity changes in the longitudinal section. For wire–feed welding, the filling metal strengthens the downward velocity component; as a result, the vortex formation is blocked in the cross-section and is strengthened in the longitudinal section.

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Data availability

The raw/processed data required cannot be shared at this time as the data also forms part of an ongoing study.

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Figure 5 A schematic of the water model of reactor URO 200.

Physical and Numerical Modeling of the Impeller Construction Impact on the Aluminum Degassing Process

알루미늄 탈기 공정에 미치는 임펠러 구성의 물리적 및 수치적 모델링

Kamil Kuglin,¹ Michał Szucki,² Jacek Pieprzyca,³ Simon Genthe,² Tomasz Merder,³ and Dorota Kalisz^1,^*

Mikael Ersson, Academic Editor

Author information Article notes Copyright and License information Disclaimer

Associated Data

Data Availability Statement

Abstract

This paper presents the results of tests on the suitability of designed heads (impellers) for aluminum refining. The research was carried out on a physical model of the URO-200, followed by numerical simulations in the FLOW 3D program. Four design variants of impellers were used in the study. The degree of dispersion of the gas phase in the model liquid was used as a criterion for evaluating the performance of each solution using different process parameters, i.e., gas flow rate and impeller speed. Afterward, numerical simulations in Flow 3D software were conducted for the best solution. These simulations confirmed the results obtained with the water model and verified them.

Keywords: aluminum, impeller construction, degassing process, numerical modeling, physical modeling

1. Introduction

Constantly increasing requirements concerning metallurgical purity in terms of hydrogen content and nonmetallic inclusions make casting manufacturers use effective refining techniques. The answer to this demand is the implementation of the aluminum refining technique making use of a rotor with an original design guaranteeing efficient refining [1,2,3,4]. The main task of the impeller (rotor) is to reduce the contamination of liquid metal (primary and recycled aluminum) with hydrogen and nonmetallic inclusions. An inert gas, mainly argon or a mixture of gases, is introduced through the rotor into the liquid metal to bring both hydrogen and nonmetallic inclusions to the metal surface through the flotation process. Appropriately and uniformly distributed gas bubbles in the liquid metal guarantee achieving the assumed level of contaminant removal economically. A very important factor in deciding about the obtained degassing effect is the optimal rotor design [5,6,7,8]. Thanks to the appropriate geometry of the rotor, gas bubbles introduced into the liquid metal are split into smaller ones, and the spinning movement of the rotor distributes them throughout the volume of the liquid metal bath. In this solution impurities in the liquid metal are removed both in the volume and from the upper surface of the metal. With a well-designed impeller, the costs of refining aluminum and its alloys can be lowered thanks to the reduced inert gas and energy consumption (optimal selection of rotor rotational speed). Shorter processing time and a high degree of dehydrogenation decrease the formation of dross on the metal surface (waste). A bigger produced dross leads to bigger process losses. Consequently, this means that the choice of rotor geometry has an indirect impact on the degree to which the generated waste is reduced [9,10].

Another equally important factor is the selection of process parameters such as gas flow rate and rotor speed [11,12]. A well-designed gas injection system for liquid metal meets two key requirements; it causes rapid mixing of the liquid metal to maintain a uniform temperature throughout the volume and during the entire process, to produce a chemically homogeneous metal composition. This solution ensures effective degassing of the metal bath. Therefore, the shape of the rotor, the arrangement of the nozzles, and their number are significant design parameters that guarantee the optimum course of the refining process. It is equally important to complete the mixing of the metal bath in a relatively short time, as this considerably shortens the refining process and, consequently, reduces the process costs. Another important criterion conditioning the implementation of the developed rotor is the generation of fine diffused gas bubbles which are distributed throughout the metal volume, and whose residence time will be sufficient for the bubbles to collide and adsorb the contaminants. The process of bubble formation by the spinning rotors differs from that in the nozzles or porous molders. In the case of a spinning rotor, the shear force generated by the rotor motion splits the bubbles into smaller ones. Here, the rotational speed, mixing force, surface tension, and fluid density have a key effect on the bubble size. The velocity of the bubbles, which depends mainly on their size and shape, determines their residence time in the reactor and is, therefore, very important for the refining process, especially since gas bubbles in liquid aluminum may remain steady only below a certain size [13,14,15].

The impeller designs presented in the article were developed to improve the efficiency of the process and reduce its costs. The impellers used so far have a complicated structure and are very pricey. The success of the conducted research will allow small companies to become independent of external supplies through the possibility of making simple and effective impellers on their own. The developed structures were tested on the water model. The results of this study can be considered as pilot.

2. Materials and Methods

Rotors were realized with the SolidWorks computer design technique and a 3D printer. The developed designs were tested on a water model. Afterward, the solution with the most advantageous refining parameters was selected and subjected to calculations with the Flow3D package. As a result, an impeller was designed for aluminum refining. Its principal lies in an even distribution of gas bubbles in the entire volume of liquid metal, with the largest possible participation of the bubble surface, without disturbing the metal surface. This procedure guarantees the removal of gaseous, as well as metallic and nonmetallic, impurities.

2.1. Rotor Designs

The developed impeller constructions, shown in Figure 1, Figure 2, Figure 3 and Figure 4, were printed on a 3D printer using the PLA (polylactide) material. The impeller design models differ in their shape and the number of holes through which the inert gas flows. Figure 1, Figure 2 and Figure 3 show the same impeller model but with a different number of gas outlets. The arrangement of four, eight, and 12 outlet holes was adopted in the developed design. A triangle-shaped structure equipped with three gas outlet holes is presented in Figure 4.

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Figure 1

A 3D model—impeller with four holes—variant B4.

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Figure 2

A 3D model—impeller with eight holes—variant B8.

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Figure 3

A 3D model—impeller with twelve holes—variant B12.

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Figure 4

A 3D model—‘red triangle’ impeller with three holes—variant RT3.

2.2. Physical Models

Investigations were carried out on a water model of the URO 200 reactor of the barbotage refining process (see Figure 5).

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Figure 5

A schematic of the water model of reactor URO 200.

The URO 200 reactor can be classified as a cyclic reactor. The main element of the device is a rotor, which ends the impeller. The whole system is attached to a shaft via which the refining gas is supplied. Then, the shaft with the rotor is immersed in the liquid metal in the melting pot or the furnace chamber. In URO 200 reactors, the refining process lasts 600 s (10 min), the gas flow rate that can be obtained ranges from 5 to 20 dm³·min⁻¹, and the speed at which the rotor can move is 0 to 400 rpm. The permissible quantity of liquid metal for barbotage refining is 300 kg or 700 kg [8,16,17]. The URO 200 has several design solutions which improve operation and can be adapted to the existing equipment in the foundry. These solutions include the following [8,16]:

URO-200XR—used for small crucible furnaces, the capacity of which does not exceed 250 kg, with no control system and no control of the refining process.
URO-200SA—used to service several crucible furnaces of capacity from 250 kg to 700 kg, fully automated and equipped with a mechanical rotor lift.
URO-200KA—used for refining processes in crucible furnaces and allows refining in a ladle. The process is fully automated, with a hydraulic rotor lift.
URO-200KX—a combination of the XR and KA models, designed for the ladle refining process. Additionally, refining in heated crucibles is possible. The unit is equipped with a manual hydraulic rotor lift.
URO-200PA—designed to cooperate with induction or crucible furnaces or intermediate chambers, the capacity of which does not exceed one ton. This unit is an integral part of the furnace. The rotor lift is equipped with a screw drive.

Studies making use of a physical model can be associated with the observation of the flow and circulation of gas bubbles. They require meeting several criteria regarding the similarity of the process and the object characteristics. The similarity conditions mainly include geometric, mechanical, chemical, thermal, and kinetic parameters. During simulation of aluminum refining with inert gas, it is necessary to maintain the geometric similarity between the model and the real object, as well as the similarity related to the flow of liquid metal and gas (hydrodynamic similarity). These quantities are characterized by the Reynolds, Weber, and Froude numbers. The Froude number is the most important parameter characterizing the process, its magnitude is the same for the physical model and the real object. Water was used as the medium in the physical modeling. The factors influencing the choice of water are its availability, relatively low cost, and kinematic viscosity at room temperature, which is very close to that of liquid aluminum.

The physical model studies focused on the flow of inert gas in the form of gas bubbles with varying degrees of dispersion, particularly with respect to some flow patterns such as flow in columns and geysers, as well as disturbance of the metal surface. The most important refining parameters are gas flow rate and rotor speed. The barbotage refining studies for the developed impeller (variants B4, B8, B12, and RT3) designs were conducted for the following process parameters:

Rotor speed: 200, 300, 400, and 500 rpm,
Ideal gas flow: 10, 20, and 30 dm³·min⁻¹,
Temperature: 293 K (20 °C).

These studies were aimed at determining the most favorable variants of impellers, which were then verified using the numerical modeling methods in the Flow-3D program.

2.3. Numerical Simulations with Flow-3D Program

Testing different rotor impellers using a physical model allows for observing the phenomena taking place while refining. This is a very important step when testing new design solutions without using expensive industrial trials. Another solution is modeling by means of commercial simulation programs such as ANSYS Fluent or Flow-3D [18,19]. Unlike studies on a physical model, in a computer program, the parameters of the refining process and the object itself, including the impeller design, can be easily modified. The simulations were performed with the Flow-3D program version 12.03.02. A three-dimensional system with the same dimensions as in the physical modeling was used in the calculations. The isothermal flow of liquid–gas bubbles was analyzed. As in the physical model, three speeds were adopted in the numerical tests: 200, 300, and 500 rpm. During the initial phase of the simulations, the velocity field around the rotor generated an appropriate direction of motion for the newly produced bubbles. When the required speed was reached, the generation of randomly distributed bubbles around the rotor was started at a rate of 2000 per second. Table 1 lists the most important simulation parameters.

Table 1

Values of parameters used in the calculations.

Parameter	Value	Unit
Maximum number of gas particles	1,000,000	–
Rate of particle generation	2000	1·s⁻¹
Specific gas constant	287.058	J·kg⁻¹·K⁻¹
Atmospheric pressure	1.013 × 10⁵	Pa
Water density	1000	kg·m⁻³
Water viscosity	0.001	kg·m⁻¹·s⁻¹
Boundary condition on the walls	No-slip	–
Size of computational cell	0.0034	m

In the case of the CFD analysis, the numerical solutions require great care when generating the computational mesh. Therefore, computational mesh tests were performed prior to the CFD calculations. The effect of mesh density was evaluated by taking into account the velocity of water in the tested object on the measurement line A (height of 0.065 m from the bottom) in a characteristic cross-section passing through the object axis (see Figure 6). The mesh contained 3,207,600, 6,311,981, 7,889,512, 11,569,230, and 14,115,049 cells.

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Figure 6

The velocity of the water depending on the size of the computational grid.

The quality of the generated computational meshes was checked using the criterion skewness angle Q_EAS [18]. This criterion is described by the following relationship:

QEAS=max{βmax−βeq180−βeq,βeq−βminβeq},

(1)

where β_max, β_min are the maximal and minimal angles (in degrees) between the edges of the cell, and β_eq is the angle corresponding to an ideal cell, which for cubic cells is 90°.

Normalized in the interval [0;1], the value of Q_EAS should not exceed 0.75, which identifies the permissible skewness angle of the generated mesh. For the computed meshes, this value was equal to 0.55–0.65.

Moreover, when generating the computational grids in the studied facility, they were compacted in the areas of the highest gradients of the calculated values, where higher turbulence is to be expected (near the impeller). The obtained results of water velocity in the studied object at constant gas flow rate are shown in Figure 6.

The analysis of the obtained water velocity distributions (see Figure 6) along the line inside the object revealed that, with the density of the grid of nodal points, the velocity changed and its changes for the test cases of 7,889,512, 11,569,230, and 14,115,049 were insignificant. Therefore, it was assumed that a grid containing not less than 7,900,000 (7,889,512) cells would not affect the result of CFD calculations.

A single-block mesh of regular cells with a size of 0.0034 m was used in the numerical calculations. The total number of cells was approximately 7,900,000 (7,889,512). This grid resolution (see Figure 7) allowed the geometry of the system to be properly represented, maintaining acceptable computation time (about 3 days on a workstation with 2× CPU and 12 computing cores).

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Figure 7

Structured equidistant mesh used in numerical calculations: (a) mesh with smoothed, surface cells (the so-called FAVOR method) used in Flow-3D; (b) visualization of the applied mesh resolution.

The calculations were conducted with an explicit scheme. The timestep was selected by the program automatically and controlled by stability and convergence. From the moment of the initial velocity field generation (start of particle generation), it was 0.0001 s.

When modeling the degassing process, three fluids are present in the system: water, gas supplied through the rotor head (impeller), and the surrounding air. Modeling such a multiphase flow is a numerically very complex issue. The necessity to overcome the liquid backpressure by the gas flowing out from the impeller leads to the formation of numerical instabilities in the volume of fluid (VOF)-based approach used by Flow-3D software. Therefore, a mixed description of the analyzed flow was used here. In this case, water was treated as a continuous medium, while, in the case of gas bubbles, the discrete phase model (DPM) model was applied. The way in which the air surrounding the system was taken into account is later described in detail.

The following additional assumptions were made in the modeling:

—The liquid phase was considered as an incompressible Newtonian fluid.
—The effect of chemical reactions during the refining process was neglected.
—The composition of each phase (gas and liquid) was considered homogeneous; therefore, the viscosity and surface tension were set as constants.
—Only full turbulence existed in the liquid, and the effect of molecular viscosity was neglected.
—The gas bubbles were shaped as perfect spheres.
—The mutual interaction between gas bubbles (particles) was neglected.

2.3.1. Modeling of Liquid Flow

The motion of the real fluid (continuous medium) is described by the Navier–Stokes Equation [20].

dudt=−1ρ∇p+ν∇2u+13ν∇(∇⋅ u)+F,

(2)

where du/dt is the time derivative, u is the velocity vector, t is the time, and F is the term accounting for external forces including gravity (unit components denoted by X, Y, Z).

In the simulations, the fluid flow was assumed to be incompressible, in which case the following equation is applicable:

∂u∂t+(u⋅∇)u=−1ρ∇p+ν∇2u+F.

(3)

Due to the large range of liquid velocities during flows, the turbulence formation process was included in the modeling. For this purpose, the k–ε model turbulence kinetic energy k and turbulence dissipation ε were the target parameters, as expressed by the following equations [21]:

∂(ρk)∂t+∂(ρkvi)∂xi=∂∂xj[(μ+μtσk)⋅∂k∂xi]+Gk+Gb−ρε−Ym+Sk,

(4)

∂(ρε)∂t+∂(ρεui)∂xi=∂∂xj[(μ+μtσε)⋅∂k∂xi]+C1εεk(Gk+G3εGb)+C2ερε2k+Sε,

(5)

where ρ is the gas density, σ_κ and σ_ε are the Prandtl turbulence numbers, k and ε are constants of 1.0 and 1.3, and G_k and G_b are the kinetic energy of turbulence generated by the average velocity and buoyancy, respectively.

As mentioned earlier, there are two gas phases in the considered problem. In addition to the gas bubbles, which are treated here as particles, there is also air, which surrounds the system. The boundary of phase separation is in this case the free surface of the water. The shape of the free surface can change as a result of the forming velocity field in the liquid. Therefore, it is necessary to use an appropriate approach to free surface tracking. The most commonly used concept in liquid–gas flow modeling is the volume of fluid (VOF) method [22,23], and Flow-3D uses a modified version of this method called TrueVOF. It introduces the concept of the volume fraction of the liquid phase f_l. This parameter can be used for classifying the cells of a discrete grid into areas filled with liquid phase (f_l = 1), gaseous phase, or empty cells (f_l = 0) and those through which the phase separation boundary (f_l ∈ (0, 1)) passes (free surface). To determine the local variations of the liquid phase fraction, it is necessary to solve the following continuity equation:

dfldt=0.

(6)

Then, the fluid parameters in the region of coexistence of the two phases (the so-called interface) depend on the volume fraction of each phase.

ρ=flρl+(1−fl)ρg,

(7)

ν=flνl+(1−fl)νg,

(8)

where indices l and g refer to the liquid and gaseous phases, respectively.

The parameter of fluid velocity in cells containing both phases is also determined in the same way.

u=flul+(1−fl)ug.

(9)

Since the processes taking place in the surrounding air can be omitted, to speed up the calculations, a single-phase, free-surface model was used. This means that no calculations were performed in the gas cells (they were treated as empty cells). The liquid could fill them freely, and the air surrounding the system was considered by the atmospheric pressure exerted on the free surface. This approach is often used in modeling foundry and metallurgical processes [24].

2.3.2. Modeling of Gas Bubble Flow

As stated, a particle model was used to model bubble flow. Spherical particles (gas bubbles) of a given size were randomly generated in the area marked with green in Figure 7b. In the simulations, the gas bubbles were assumed to have diameters of 0.016 and 0.02 m corresponding to the gas flow rates of 10 and 30 dm³·min⁻¹, respectively.

Experimental studies have shown that, as a result of turbulent fluid motion, some of the bubbles may burst, leading to the formation of smaller bubbles, although merging of bubbles into larger groupings may also occur. Therefore, to be able to observe the behavior of bubbles of different sizes (diameter), the calculations generated two additional particle types with diameters twice smaller and twice larger, respectively. The proportion of each species in the system was set to 33.33% (Table 2).

Table 2

Data assumed for calculations.

No	Rotor Speed (Rotational Speed) rpm	Bubbles Diameter m	Corresponding Gas Flow Rate dm³·min⁻¹	No	Rotor Speed (Rotational Speed) rpm	Bubbles Diameter m	Corresponding Gas Flow Rate dm³·min⁻¹
A	200	0.016	10	D	200	0.02	30
0.008	0.01
0.032	0.04
B	300	0.016	10	E	300	0.02	30
0.008	0.01
0.032	0.04
C	500	0.016	10	F	500	0.02	30
0.008	0.01
0.032	0.04

The velocity of the particle results from the generated velocity field (calculated from Equation (3) in the liquid ul around it and its velocity resulting from the buoyancy force ub. The effect of particle radius r on the terminal velocity associated with buoyancy force can be determined according to Stokes’ law.

ub=29 (ρg−ρl)μlgr2,

(10)

where g is the acceleration (9.81).

The DPM model was used for modeling the two-phase (water–air) flow. In this model, the fluid (water) is treated as a continuous phase and described by the Navier–Stokes equation, while gas bubbles are particles flowing in the model fluid (discrete phase). The trajectories of each bubble in the DPM system are calculated at each timestep taking into account the mass forces acting on it. Table 3 characterizes the DPM model used in our own research [18].

Table 3

Characteristic of the DPM model.

Method	Equations
Euler–Lagrange	Balance equation: dugdt=FD(u−ug)+g(ϱg−ϱ)ϱg+F. F_D (u − u_p) denotes the drag forces per mass unit of a bubble, and the expression for the drag coefficient F_D is of the form FD=18μCDReϱ⋅gd2g24. The relative Reynolds number has the form Re≡ρdg\|ug−u\|μ. On the other hand, the force resulting from the additional acceleration of the model fluid has the form F=12dρdtρg(u−ug), where u_g is the gas bubble velocity, u is the liquid velocity, d_g is the bubble diameter, and C_D is the drag coefficient.

Method

Equations

Euler–Lagrange

Balance equation:
dugdt=FD(u−ug)+g(ϱg−ϱ)ϱg+F.
F_D (u − u_p) denotes the drag forces per mass unit of a bubble, and the expression for the drag coefficient F_D is of the form
FD=18μCDReϱ⋅gd2g24.
The relative Reynolds number has the form
Re≡ρdg|ug−u|μ.
On the other hand, the force resulting from the additional acceleration of the model fluid has the form
F=12dρdtρg(u−ug),
where u_g is the gas bubble velocity, u is the liquid velocity, d_g is the bubble diameter, and C_D is the drag coefficient.

3. Results and Discussion

3.1. Calculations of Power and Mixing Time by the Flowing Gas Bubbles

One of the most important parameters of refining with a rotor is the mixing power induced by the spinning rotor and the outflowing gas bubbles (via impeller). The mixing power of liquid metal in a ladle of height (h) by gas injection can be determined from the following relation [15]:

pgVm=ρ⋅g⋅uB,

(11)

where p_g is the mixing power, V_m is the volume of liquid metal in the reactor, ρ is the density of liquid aluminum, and u_B is the average speed of bubbles, given below.

uB=n⋅R⋅TAc⋅Pm⋅t,

(12)

where n is the number of gas moles, R is the gas constant (8.314), A_c is the cross-sectional area of the reactor vessel, T is the temperature of liquid aluminum in the reactor, and P_m is the pressure at the middle tank level. The pressure at the middle level of the tank is calculated by a function of the mean logarithmic difference.

Pm=(Pa+ρ⋅g⋅h)−Paln(Pa+ρ⋅g⋅h)Pa,

(13)

where P_a is the atmospheric pressure, and h is the the height of metal in the reactor.

Themelis and Goyal [25] developed a model for calculating mixing power delivered by gas injection.

pg=2Q⋅R⋅T⋅ln(1+m⋅ρ⋅g⋅hP),

(14)

where Q is the gas flow, and m is the mass of liquid metal.

Zhang [26] proposed a model taking into account the temperature difference between gas and alloy (metal).

pg=QRTgVm[ln(1+ρ⋅g⋅hPa)+(1−TTg)],

(15)

where T_g is the gas temperature at the entry point.

Data for calculating the mixing power resulting from inert gas injection into liquid aluminum are given below in Table 4. The design parameters were adopted for the model, the parameters of which are shown in Figure 5.

Table 4

Data for calculating mixing power introduced by an inert gas.

Parameter	Value	Unit
Height of metal column	0.7	m
Density of aluminum	2375	kg·m⁻³
Process duration	20	s
Gas temperature at the injection site	940	K
Cross-sectional area of ladle	0.448	m²
Mass of liquid aluminum	546.25	kg
Volume of ladle	0.23	M³
Temperature of liquid aluminum	941.15	K

Table 5 presents the results of mixing power calculations according to the models of Themelis and Goyal and of Zhang for inert gas flows of 10, 20, and 30 dm³·min⁻¹. The obtained calculation results significantly differed from each other. The difference was an order of magnitude, which indicates that the model is highly inaccurate without considering the temperature of the injected gas. Moreover, the calculations apply to the case when the mixing was performed only by the flowing gas bubbles, without using a rotor, which is a great simplification of the phenomenon.

Table 5

Mixing power calculated from mathematical models.

Mathematical Model	Mixing Power (W·t⁻¹) for a Given Inert Gas Flow (dm³·min⁻¹)
	10	20	30
Themelis and Goyal	11.49	23.33	35.03
Zhang	0.82	1.66	2.49

The mixing time is defined as the time required to achieve 95% complete mixing of liquid metal in the ladle [27,28,29,30]. Table 6 groups together equations for the mixing time according to the models.

Table 6

Models for calculating mixing time.

Authors	Model	Remarks
Szekely [31]	τ=800ε−0.4	ε—W·t⁻¹
Chiti and Paglianti [27]	τ=CVQl	V—volume of reactor, m³ Ql—flow intensity, m³·s⁻¹
Iguchi and Nakamura [32]	τ=1200⋅Q−0.4D1.97h−1.0υ0.47	υ—kinematic viscosity, m²·s⁻¹ D—diameter of ladle, m h—height of metal column, m Q—liquid flow intensity, m³·s⁻¹

Figure 8 and Figure 9 show the mixing time as a function of gas flow rate for various heights of the liquid column in the ladle and mixing power values.

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Figure 8

Mixing time as a function of gas flow rate for various heights of the metal column (Iguchi and Nakamura model).

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Figure 9

Mixing time as a function of mixing power (Szekly model).

3.2. Determining the Bubble Size

The mechanisms controlling bubble size and mass transfer in an alloy undergoing refining are complex. Strong mixing conditions in the reactor promote impurity mass transfer. In the case of a spinning rotor, the shear force generated by the rotor motion separates the bubbles into smaller bubbles. Rotational speed, mixing force, surface tension, and liquid density have a strong influence on the bubble size. To characterize the kinetic state of the refining process, parameters k and A were introduced. Parameters k, A, and u_B can be calculated using the below equations [33].

k=2D⋅uBdB⋅π−−−−−−√,

(16)

A=6Q⋅hdB⋅uB,

(17)

uB=1.02g⋅dB,−−−−−√

(18)

where D is the diffusion coefficient, and d_B is the bubble diameter.

After substituting appropriate values, we get

dB=3.03×104(πD)−2/5g−1/5h4/5Q0.344N−1.48.

(19)

According to the last equation, the size of the gas bubble decreases with the increasing rotational speed (see Figure 10).

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Figure 10

Effect of rotational speed on the bubble diameter.

In a flow of given turbulence intensity, the diameter of the bubble does not exceed the maximum size d_max, which is inversely proportional to the rate of kinetic energy dissipation in a viscous flow ε. The size of the gas bubble diameter as a function of the mixing energy, also considering the Weber number and the mixing energy in the negative power, can be determined from the following equations [31,34]:

—Sevik and Park:

dBmax=We0.6kr⋅(σ⋅103ρ⋅10−3)0.6⋅(10⋅ε)−0.4⋅10−2.

(20)

—Evans:

dBmax=⎡⎣Wekr⋅σ⋅1032⋅(ρ⋅10−3)13⎤⎦35 ⋅(10⋅ε)−25⋅10−2.

(21)

The results of calculating the maximum diameter of the bubble d_Bmax determined from Equation (21) are given in Table 7.

Table 7

The results of calculating the maximum diameter of the bubble using Equation (21).

Model	Mixing Energy ĺ (m²·s⁻³)	Weber Number (We_kr)
0.59	1.0	1.2
Zhang and Taniguchi d_max	0.1	0.0167	0.0230	0.026
0.5	0.0088	0.0121	0.013
1.0	0.0067	0.0091	0.010
1.5	0.0057	0.0078	0.009
Sevik and Park d_B_max	0.1	0.265	0.36	0.41
0.5	0.139	0.19	0.21
1.0	0.106	0.14	0.16
1.5	0.090	0.12	0.14
Evans d_B_max	0.1	0.247	0.340	0.38
0.5	0.130	0.178	0.20
1.0	0.098	0.135	0.15
1.5	0.084	0.115	0.13

3.3. Physical Modeling

The first stage of experiments (using the URO-200 water model) included conducting experiments with impellers equipped with four, eight, and 12 gas outlets (variants B4, B8, B12). The tests were carried out for different process parameters. Selected results for these experiments are presented in Figure 11, Figure 12, Figure 13 and Figure 14.

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Figure 11

Impeller variant B4—gas bubbles dispersion registered for a gas flow rate of 10 dm³·min⁻¹ and rotor speed of (a) 200, (b) 300, (c) 400, and (d) 500 rpm.

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Figure 12

Impeller variant B8—gas bubbles dispersion registered for a gas flow rate of 10 dm³·min⁻¹ and rotor speed of (a) 200, (b) 300, (c) 400, and (d) 500 rpm.

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Figure 13

Gas bubble dispersion registered for different processing parameters (impeller variant B12).

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Figure 14

Gas bubble dispersion registered for different processing parameters (impeller variant RT3).

The analysis of the refining variants presented in Figure 11, Figure 12, Figure 13 and Figure 14 reveals that the proposed impellers design model is not useful for the aluminum refining process. The number of gas outlet orifices, rotational speed, and flow did not affect the refining efficiency. In all the variants shown in the figures, very poor dispersion of gas bubbles was observed in the object. The gas bubble flow had a columnar character, and so-called dead zones, i.e., areas where no inert gas bubbles are present, were visible in the analyzed object. Such dead zones were located in the bottom and side zones of the ladle, while the flow of bubbles occurred near the turning rotor. Another negative phenomenon observed was a significant agitation of the water surface due to excessive (rotational) rotor speed and gas flow (see Figure 13, cases 20; 400, 30; 300, 30; 400, and 30; 500).

Research results for a ‘red triangle’ impeller equipped with three gas supply orifices (variant RT3) are presented in Figure 14.

In this impeller design, a uniform degree of bubble dispersion in the entire volume of the modeling fluid was achieved for most cases presented (see Figure 14). In all tested variants, single bubbles were observed in the area of the water surface in the vessel. For variants 20; 200, 30; 200, and 20; 300 shown in Figure 14, the bubble dispersion results were the worst as the so-called dead zones were identified in the area near the bottom and sidewalls of the vessel, which disqualifies these work parameters for further applications. Interestingly, areas where swirls and gas bubble chains formed were identified only for the inert gas flows of 20 and 30 dm³·min⁻¹ and 200 rpm in the analyzed model. This means that the presented model had the best performance in terms of dispersion of gas bubbles in the model liquid. Its design with sharp edges also differed from previously analyzed models, which is beneficial for gas bubble dispersion, but may interfere with its suitability in industrial conditions due to possible premature wear.

3.4. Qualitative Comparison of Research Results (CFD and Physical Model)

The analysis (physical modeling) revealed that the best mixing efficiency results were obtained with the RT3 impeller variant. Therefore, numerical calculations were carried out for the impeller model with three outlet orifices (variant RT3). The CFD results are presented in Figure 15 and Figure 16.

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Figure 15

Simulation results of the impeller RT3, for given flows and rotational speeds after a time of 1 s: simulation variants (a) A, (b) B, (c) C, (d) D, (e) E, and (f) F.

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Figure 16

Simulation results of the impeller RT3, for given flows and rotational speeds after a time of 5.4 s.: simulation variants (a) A, (b) B, (c) C, (d) D, (e) E, and (f) F.

CFD results are presented for all analyzed variants (impeller RT3) at two selected calculation timesteps of 1 and 5.40 s. They show the velocity field of the medium (water) and the dispersion of gas bubbles.

Figure 15 shows the initial refining phase after 1 s of the process. In this case, the gas bubble formation and flow were observed in an area close to contact with the rotor. Figure 16 shows the phase when the dispersion and flow of gas bubbles were advanced in the reactor area of the URO-200 model.

The quantitative evaluation of the obtained results of physical and numerical model tests was based on the comparison of the degree of gas dispersion in the model liquid. The degree of gas bubble dispersion in the volume of the model liquid and the areas of strong turbulent zones formation were evaluated during the analysis of the results of visualization and numerical simulations. These two effects sufficiently characterize the required course of the process from the physical point of view. The known scheme of the below description was adopted as a basic criterion for the evaluation of the degree of dispersion of gas bubbles in the model liquid.

Minimal dispersion—single bubbles ascending in the region of their formation along the ladle axis; lack of mixing in the whole bath volume.
Accurate dispersion—single and well-mixed bubbles ascending toward the bath mirror in the region of the ladle axis; no dispersion near the walls and in the lower part of the ladle.
Uniform dispersion—most desirable; very good mixing of fine bubbles with model liquid.
Excessive dispersion—bubbles join together to form chains; large turbulence zones; uneven flow of gas.

The numerical simulation results give a good agreement with the experiments performed with the physical model. For all studied variants (used process parameters), the single bubbles were observed in the area of water surface in the vessel. For variants presented in Figure 13 (200 rpm, gas flow 20 and dm³·min⁻¹) and relevant examples in numerical simulation Figure 16, the worst bubble dispersion results were obtained because the dead zones were identified in the area near the bottom and sidewalls of the vessel, which disqualifies these work parameters for further use. The areas where swirls and gas bubble chains formed were identified only for the inert gas flows of 20 and 30 dm³·min⁻¹ and 200 rpm in the analyzed model (physical model). This means that the presented impeller model had the best performance in terms of dispersion of gas bubbles in the model liquid. The worst bubble dispersion results were obtained because the dead zones were identified in the area near the bottom and side walls of the vessel, which disqualifies these work parameters for further use.

Figure 17 presents exemplary results of model tests (CFD and physical model) with marked gas bubble dispersion zones. All variants of tests were analogously compared, and this comparison allowed validating the numerical model.

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Figure 17

Compilations of model research results (CFD and physical): A—single gas bubbles formed on the surface of the modeling liquid, B—excessive formation of gas chains and swirls, C—uniform distribution of gas bubbles in the entire volume of the tank, and D—dead zones without gas bubbles, no dispersion. (a) Variant B; (b) variant F.

It should be mentioned here that, in numerical simulations, it is necessary to make certain assumptions and simplifications. The calculations assumed three particle size classes (Table 2), which represent the different gas bubbles that form due to different gas flow rates. The maximum number of particles/bubbles (Table 1) generated was assumed in advance and related to the computational capabilities of the computer. Too many particles can also make it difficult to visualize and analyze the results. The size of the particles, of course, affects their behavior during simulation, while, in the figures provided in the article, the bubbles are represented by spheres (visualization of the results) of the same size. Please note that, due to the adopted Lagrangian–Eulerian approach, the simulation did not take into account phenomena such as bubble collapse or fusion. However, the obtained results allow a comprehensive analysis of the behavior of gas bubbles in the system under consideration.

The comparative analysis of the visualization (quantitative) results obtained with the water model and CFD simulations (see Figure 17) generated a sufficient agreement from the point of view of the trends. A precise quantitative evaluation is difficult to perform because of the lack of a refraction compensating system in the water model. Furthermore, in numerical simulations, it is not possible to determine the geometry of the forming gas bubbles and their interaction with each other as opposed to the visualization in the water model. The use of both research methods is complementary. Thus, a direct comparison of images obtained by the two methods requires appropriate interpretation. However, such an assessment gives the possibility to qualitatively determine the types of the present gas bubble dispersion, thus ultimately validating the CFD results with the water model.

A summary of the visualization results for impellers RT3, i.e., analysis of the occurring gas bubble dispersion types, is presented in Table 8.

Table 8

Summary of visualization results (impeller RT3)—different types of gas bubble dispersion.

No Exp.	A	B	C	D	E	F
Gas flow rate, dm³·min⁻¹	10	30
Impeller speed, rpm	200	300	500	200	300	500
Type of dispersion	Accurate	Uniform	Uniform/excessive	Minimal	Excessive	Excessive

Tests carried out for impeller RT3 confirmed the high efficiency of gas bubble distribution in the volume of the tested object at a low inert gas flow rate of 10 dm³·min⁻¹. The most optimal variant was variant B (300 rpm, 10 dm³·min⁻¹). However, the other variants A and C (gas flow rate 10 dm³·min⁻¹) seemed to be favorable for this type of impeller and are recommended for further testing. The above process parameters will be analyzed in detail in a quantitative analysis to be performed on the basis of the obtained efficiency curves of the degassing process (oxygen removal). This analysis will give an unambiguous answer as to which process parameters are the most optimal for this type of impeller; the results are planned for publication in the next article.

It should also be noted here that the high agreement between the results of numerical calculations and physical modelling prompts a conclusion that the proposed approach to the simulation of a degassing process which consists of a single-phase flow model with a free surface and a particle flow model is appropriate. The simulation results enable us to understand how the velocity field in the fluid is formed and to analyze the distribution of gas bubbles in the system. The simulations in Flow-3D software can, therefore, be useful for both the design of the impeller geometry and the selection of process parameters.

4. Conclusions

The results of experiments carried out on the physical model of the device for the simulation of barbotage refining of aluminum revealed that the worst results in terms of distribution and dispersion of gas bubbles in the studied object were obtained for the black impellers variants B4, B8, and B12 (multi-orifice impellers—four, eight, and 12 outlet holes, respectively).

In this case, the control of flow, speed, and number of gas exit orifices did not improve the process efficiency, and the developed design did not meet the criteria for industrial tests. In the case of the ‘red triangle’ impeller (variant RT3), uniform gas bubble dispersion was achieved throughout the volume of the modeling fluid for most of the tested variants. The worst bubble dispersion results due to the occurrence of the so-called dead zones in the area near the bottom and sidewalls of the vessel were obtained for the flow variants of 20 dm³·min⁻¹ and 200 rpm and 30 dm³·min⁻¹ and 200 rpm. For the analyzed model, areas where swirls and gas bubble chains were formed were found only for the inert gas flow of 20 and 30 dm³·min⁻¹ and 200 rpm. The model impeller (variant RT3) had the best performance compared to the previously presented impellers in terms of dispersion of gas bubbles in the model liquid. Moreover, its design differed from previously presented models because of its sharp edges. This can be advantageous for gas bubble dispersion, but may negatively affect its suitability in industrial conditions due to premature wearing.

The CFD simulation results confirmed the results obtained from the experiments performed on the physical model. The numerical simulation of the operation of the ‘red triangle’ impeller model (using Flow-3D software) gave good agreement with the experiments performed on the physical model. This means that the presented model impeller, as compared to other (analyzed) designs, had the best performance in terms of gas bubble dispersion in the model liquid.

In further work, the developed numerical model is planned to be used for CFD simulations of the gas bubble distribution process taking into account physicochemical parameters of liquid aluminum based on industrial tests. Consequently, the obtained results may be implemented in production practice.

Funding Statement

This paper was created with the financial support grants from the AGH-UST, Faculty of Foundry Engineering, Poland (16.16.170.654 and 11/990/BK_22/0083) for the Faculty of Materials Engineering, Silesian University of Technology, Poland.

Author Contributions

Conceptualization, K.K. and D.K.; methodology, J.P. and T.M.; validation, M.S. and S.G.; formal analysis, D.K. and T.M.; investigation, J.P., K.K. and S.G.; resources, M.S., J.P. and K.K.; writing—original draft preparation, D.K. and T.M.; writing—review and editing, D.K. and T.M.; visualization, J.P., K.K. and S.G.; supervision, D.K.; funding acquisition, D.K. and T.M. All authors have read and agreed to the published version of the manuscript.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Data are contained within the article.

Conflicts of Interest

The authors declare no conflict of interest.

Footnotes

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