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Keywords: Selective separation of both inorganic and organic particles by flotation process involving air bubbles has wide
Flotation, bubble rise velocity application areas which critically depends on the particle laden bubble rise velocity. In this study, the rising
Drag coefficient behaviour of particle-laden bubbles (particle diameter dp ~ 114 μm, bubble diameter dB = 2.88 ± 0.07 mm) at
bubble surface loading (BSL)
various surfactant concentrations (Sodium Dodecyl Sulphate, 0 % − 25 % cmc) was investigated. Bubble ve
Surfactant
Bubble-particle aggregates
locity, aspect ratio and bubble surface loading (BSL) parameters were quantified by high-speed imaging. A
regime map was proposed to determine the effect of particles and surfactant on the observed bubble surface
mobility condition. Also, an unsteady-state mathematical model based on force balance approach with appro
priate drag correction factor was developed to predict the rise velocity of a particle-laden bubble. The model
produced reasonable agreement with the experiment specifically in the high surfactant concentration cases
where the bubble shape became nearly spherical.
* Corresponding author.
E-mail address: Subhasish.mitra@newcastle.edu.au (S. Mitra).
https://doi.org/10.1016/j.ces.2024.119812
Received 10 September 2023; Received in revised form 15 January 2024; Accepted 22 January 2024
Available online 24 January 2024
0009-2509/© 2024 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
A. Wang et al. Chemical Engineering Science 288 (2024) 119812
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 2. Schematic diagram of the experimental setup for determining bubble rising behaviour.
dominant mechanisms behind the bubble surface rigidity; iii) propose motor speed (see Fig. 2). The chosen particle size was typical to the
both drag coefficient and rise velocity correction factor in the identified coarse end of the particle size distribution commonly encountered in the
regimes; and finally iv) quantify the transient rise velocity for particle- conventional mineral flotation process which was convenient for
laden bubbles using a force balance based mathematical model incor handling and visualisation. The glass particles were rendered a contact
porating the proposed drag correction factor sub-model. angle of ~ 53◦ after hydrophobicisation using 2 % hydrophobic solution
prepared by mixing a commercial hydrophobic agent NG1010 in RO
2. Experimental water (Wang et al., 2021).
Once the required bubble surface coverage level was attained, the
2.1. Materials screw feeder was stopped, and air injection was resumed by turning on
the syringe pump to dislodge the particle-laden bubble from the nozzle
Six different solutions in aqueous medium were prepared using So tip. Details of the bubble surface loading level from the captured images
dium Dodecyl Sulphate (SDS) surfactant with concentration ranging are presented in section 2.3.
from 0 to 25 % cmc where 100 % cmc of SDS equals to 8.2 × 10-3 mol/L High-speed imaging was performed to capture the rising dynamics of
(Markarian et al., 2005) to modify bubble surface mobility. Surface a particle-laden bubble using a Phantom v311 camera in shadowgraphy
tension parameter of these solutions was measured by a Sigma Force mode at 1000 frames per second and 65 µs exposure time. Proper
tensiometer 700 (Biolin Scientific) which varied in the range from 70.9 backlight illumination was provided by placing a diffuser screen in front
mN/m at 0 % cmc to 47.6 mN/m at 25 % cmc (592 ppm). The surface of a bright halogen light source (12 V, 50 W) placed at a sufficient dis
tension as a function of surfactant concentration cs was fitted for inter tance from the apparatus to avoid any heating yet ensuring high contrast
polation purpose for any intermediate concentration as follows (see images. The field of view (FoV) in the images was kept at 512 × 800
Fig. 1): pixels with a pixel resolution of ~ 29 µm/pixel.
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 3. Identification of bubble surface loading from a raw image of a rising particle laden bubble (Wang et al., 2021).
ellipsoidal bubble. Details of the image processing algorithm for surface The bubble rise velocity UBP was determined by dividing the shift in the
loading identification and ellipsoidal surface reconstruction procedure bubble centroids in the two successive images by the corresponding time
can be found in Wang et al. (2021). difference as follows:
Subsequently, the equivalent bubble diameter from the raw images
was calculated as: yB,i+1 − yB,i
UBP = (4)
Δt
( )1/3
dB = 2 ab2 (2)
Determining change in the bubble centroids calculated using Eq. (4)
Following bubble detachment from the nozzle, bubble size measure involved around two pixels error. For a pixel resolution of ~ 29 µm/
ments were performed once the initial surface oscillations subsided. The pixel, and time resolution Δt of 5 × 10-3 s, the measurement error in the
average diameter of the bubbles generated in various surfactant solu estimated bubble rise velocity UBP was ~ 0.0116 m/s.
tions was dB = 2.88 ± 0.07 mm. It is important to mention that this Assuming a monolayer of particles at bubble interface, bubble sur
bubble size was found convenient to generate in a consistent manner. face loading (BSL) parameter was determined as a ratio of the surface
Bubbles of this size were quite stable at the nozzle tip allowing sufficient area of the particles covered bottom ellipsoidal cap (marked by the
time for particles to settle and coat a layer of particles on the bubble dashed magenta line) Scap to that of the whole surface area of the bubble,
surface. Generating any smaller bubble size using a smaller size nozzle Sbubble:
was very difficult to stabilise at the nozzle tip for the same duration in Scap
BSL = (5)
the presence of surfactant. Utilising the major and minor diameter ob Sbubble
tained from the images, the bubble aspect ratio AR was calculated as
a wherein the surface area of the bubble Sbubble, was expressed as:
AR = (3)
b
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 4. Temporal evolution of rise velocity for bare bubbles in various SDS surfactant concentration.
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 5. Validation of the terminal velocity model (Eq. (7)) of bare bubbles with the experimental data.
gμ4L (ρL − ρB ) experimental data (deviation < 10 % and the root-mean-square devia
Mo = (8)
ρ2L σ 3 tion (RMSD) = 0.020). Error bars for each surface tension case were also
plotted herein but those are not distinguishable because of small errors
wherein σ = gas–liquid surface tension, ρB = bubble density. involved (standard deviations ~ 1.2 × 10-4 to 6.2 × 10-4). Based on the
The variable J in Eq. (7) is a stepwise function which is written as: agreement obtained, Eq. (7) was used as the base model in Section 3.2
{ for development of a velocity correction factor to account for the pres
0.94H 0.757 (2 < H⩽59.3)
J= (9) ence of particles on bubble surface.
3.42H 0.441 (H > 59.3)
A small jump in the experimentally measured terminal rise velocity
can be noted as the surface tension parameter increases from 0.0533 to
wherein the variable H is expressed as:
0.0566 N/m corresponding to SDS concentration decreasing from 15 %
4 0.14
(10) cmc to 10 % cmc. This behaviour could be attributed to the transition of
H = EoMo− 0.149
(μL /μw )−
3 bubble surface mobility from rigid to partially rigid state with less
adsorption of surfactant on the surface in the 10 % cmc case causing
ρ gd2
where μw = liquid viscosity at wall and Eötvös number Eo = L σ B . larger shape oscillations. The rise velocity correlation model in Eq. (7) in
Fig. 5 shows good agreement of the model prediction with the the 10 % cmc case however predicted a smoother velocity increase
without capturing this jump pattern which is attributed to inaccuracy in
the Clift model itself to capture variability in the rise velocity data for
Table 1
ellipsoidal shape bubbles of size around 3 mm due to oscillatory
Empirical models for drag coefficients of a bare bubble.
behaviour in the bubble shape.
Researchers Models To predict the temporal velocity of a bare bubble as it ascends from
its stationary state, a rise velocity model was proposed based on New
{ [ 24 18.7 ]
Peebles and Garber CD,B = max max , ,
ReB Re0.68 ton’s second law comprising gravity, virtual mass, buoyancy and drag
(1953) [ ]} B
0.0275EoWe2 , force as follows:
min
0.82Eo0.25 We0.5
{ 24 ( [ ]} ∫ Ut ∫t
) 8 2 FB,B − FG,B − FD,B
Ishii and Chawla (1979) CD,B = max 1 + 0.1Re0.75 , min , Eo0.5
ReB B
3 3 dUB = dt (11)
{ 24 ( ) 8 Eo
} 0 0 m′B
Tomiyama et al. (1998) CD,B = max 1 + 0.15Re0.687
B ,
ReB 3 (Eo + 4)
[( )2 ]0.5 where the modified bubble mass m′B is expressed as sum of the actual and
Zhou et al. (2020) CD,B = CD,Mei + (CD (Eo) )2 CD,Mei =
virtual mass of a single bubble:
{ [ ( )] }
1
16 8 1 3.315 −
1+ + 1 + 0.5 CD (Eo) = 4 4
ReB ReB 2 ReB m′B = πR3B ρB + Cv πR3B ρL (12)
⎧ ⎫
3 3
(− 1.23log(Eo)+0.37log(Mo)+1.6 )
⎪
⎨ 10 , ⎪
⎬
max [
4Eo 8Eo
] where virtual mass coefficient was selected as Cv = 0.5.
⎩ min
⎪ ⎪
,
(Eo + 9.5) 3(0.8726Eo + 4.887)
⎭
FB,B in Eq. (11) denotes the bubble buoyancy force which is given as:
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 6. Comparison of theoretical and experimental rise velocity of a bare bubble in a) 0 % cmc; b) 10 % cmc; c) 15 % cmc; and d) 25 % cmc. Water densityρL = 998
kg/m3, Bubble densityρB = 1.18 kg/m3.
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 7. Rising of particle-laden bubbles in pure water and 15% cmc case for different initial bubble surface loading (BSL) values.
into multiple spherical harmonics. Their results showed that the pres rear vortices of rising bubble due to low particle Stokes number (St =
ence of particles at bubble surfaces decreases the damping rate of the ρP UB d2P /(9μL dB ) ~ 0.25 to 0.36) and are randomly dispersed in the
dominant harmonic significantly while having a minor influence on the trailing vortices. These factors together contribute to the observed de
√̅̅̅̅̅̅̅
oscillation frequency which can be scaled approximately as ρ σd3 . Since viation between the initial and final BSL values.
The temporal evolution of bubble surface loading levels reported in
L B
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 8. Evolution of BSL over time in a) 0% cmc case (initial BSL: 0.29, average BSL: 0.27) and b)15% cmc case (initial BSL: 0.27, average BSL: 0.25).
pure water case. Such increase in the BSL parameter is ascribed to the The summary of bubble terminal velocity obtained at various BSLs
interaction of the particle layer with the trailing vortices which stretches and surfactant concentrations in Fig. 10 confirms this observation. The
a bubble in the equatorial direction (Wang et al., 2021). decreasing terminal velocity profiles with BSL as an independent
The lower increasing rate of BSL value in the presence of surfactant parameter can be categorized into three groups according to surfactant
can be attributed to Marangoni effect. When bubbles rise, the absorbed concentration: Cs = 0 % cmc, 5 % to 10 % cmc, and 15 % cmc and above,
surfactant on bubble surface is swept down to the rear part increasing respectively. In the first category (Cs = 0 % cmc) wherein the bubble
surfactant concentration. The resultant concentration gradient gener surface is mobile, Fig. 10 shows a non-linear decreasing trend of ter
ates Marangoni stress in the tangential direction which tends to retard minal velocity with the BSL parameter. This decreasing trend is attrib
surface motions. Consequently, particles at the interface slow down uted to higher drag force resulting from the decreasing buoyancy or due
when they are pushed towards the bubble equator by the trailing to presence of particles on bubble surface. In the second category (Cs = 5
vortices (Wang et al., 2021) leading to relatively lower expansion of the % to 10 % cmc), such decreasing trend of the rise velocity profiles be
instantaneous BSL boundary. comes more linear wherein slope (UBP/BSL) is directly affected by the
In general, it is noted that BSL value increases for the initial BSL level BSL parameter. Increasing bubble surface loading levels decreases
< 0.4 and gradually becomes steady for the initial BSL > 0.4 (not bubble rise velocity due to increased gravity and drag forces. It can be
shown). The threshold value BSL ~ 0.40 obtained in this study is in noted that the lowest rise velocity occurred in the 10 % cmc case which
agreement with our previous study (Wang et al., 2021) involving pure had the largest BSL ~ 0.55 among all other cases.
water (no surfactant case) which confirms that such threshold is inde Although the degree of contamination on bubble surface by surfac
pendent of the surfactant concentration. tant is difficult to measure (Clift et al., 1978; Legendre et al., 2009), it
The time evolution of aspect ratio (AR) and rise velocity of particle- can be postulated from these trends that bubble surface is partially rigid
laden bubbles UBP quantified in three different surfactant concentrations (partial slip condition) in the presence of surfactant, and the surface
are shown in Fig. 9. In the absence of surfactant (Fig. 9a), The aspect rigidity increases with more particles loaded onto bubble surface leading
ratio of the particle-laden bubble at a high BSL value ~ 0.42 remains to increased drag force. The third category involves a lower slope of rise
steady at ~ 0.75, significantly higher than the aspect ratio value ~ 0.35 velocity at higher surfactant concentration which indicates bubble sur
at BSL = 0.00 and 0.23. In all cases, bubble rise velocity is observed to be face becomes more rigid from adsorption of larger amount of surfactant
inversely correlated to its aspect ratio and bubble surface loading. High (no-slip condition) and consequently bubble velocity becomes less
BSL values also suppress oscillations in the bubble rise velocity profiles. dependent on the BSL parameter.
As the surfactant concentration increases (Fig. 9b-c), the effect of BSL Given the importance of bubble surface rigidity in affecting the
parameter on the steady state aspect ratio (AR) becomes somewhat bubble rise velocity in the three surfactant concentration categories
insignificant, fluctuating around a steady value of 0.80 which indicates described in Figs. 9 to 10, a regime map of bubble surface rigidity in the
bubble surface elasticity achieved by the adsorption of surfactant, is not presence of surfactant and loaded particles is proposed in Fig. 11. In
amenable to any further shape change by bubble surface loading. It can Regime I at both BSL = 0 and Cs = 0 % cmc, bubble surface is free of
be also observed that once BSL reaches beyond ~ 0.24, with increasing surfactant and particles and therefore is mobile. In Regime II at BSL <
surfactant concentration Cs, the difference between bubble terminal 0.5 and 0 < Cs < 15 % cmc, bubble becomes partially rigid under the
velocity at different BSLs in the steady region reduces (Fig. 9b) and combined effect of loaded particles and surfactant. In Regime III bubble
becomes almost negligible at 15 % cmc (Fig. 9c). surface can become rigid from the contributions of loaded particles at
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 9. Rise velocity and instantaneous aspect ratio of particle-laden bubble in a) pure water; b) 10% cmc and c) 15% cmc case.
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 10. Terminal velocity of particle-laden bubbles vs bubble surface loading for different surfactant concentrations.
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 12. Velocity modification factor as a function of bubble surface loading in various surfactant concentrations: a) 0% cmc; b) 5% − 10% cmc; c) 15% − 25% cmc.
BSL ≥ 0.5 and 0 < Cs < 15 % cmc, or from the adsorbed surfactant at 3.2.2. Bubble rise velocity model
BSL < 0.5 or combinedly from contribution of both particles and A velocity correction factor αBP,U was introduced to modify the rise
adsorbed surfactant at BSL ≥ 0.5 and Cs ≥ 15 % cmc. velocity of a bare bubble of same diameter dB in the presence of a sur
Although surfactant plays an important role in controlling bubble factant of concentration Cs in the aqueous medium. Applying Eq. (7), the
rise velocity (Davis and Acrivos, 1966; Griffith, 1962; Takagi and Mat rise velocity of a particle-laden bubble was written as:
sumoto, 2010) as shown in Figs. 9 to 11, developing an analytical model μL
from first principles to determine the bubble rise velocity including UBP = αBP,U 1.05 Mo− 0.149
(J − 0.857) (16)
ρL dB
surfactant effect is a challenging problem. This is due to the combined
complexity posed by the distribution of surfactant on bubble surface and where the Morton number Mo in Eq. (7) is correlated to ρBP the density
the corresponding slip condition, deforming gas–liquid interface and of bubble-particle aggregate, namely the air bubble with the attached
bubble Reynolds number which usually falls in the intermediate flow particles. Mo was calculated as follows:
regime rather than the ideal flows defined by the Stokes or potential
flow field (Wang et al., 2021) for which no straightforward solutions Mo =
gμ4L (ρL − ρBP )
(17)
exist. ρ2L σ3
To the best of the authors’ knowledge, limited studies are reported
on the analytical modelling of rise velocity of a particle-laden bubble in ρBP was calculated by dividing the volume of single bubble into the sum
the presence of a surfactant. The model proposed by Yan et al. (2021) is of the bubble mass and loaded particle mass, as shown in the following
only suitable for pure water condition due to the assumption that the equation:
loaded particles have the same effect on the bubble surface mobility as a ρB dB3 + NP ρP dP3
surfactant. Nevertheless, this study shows that in presence of surfactant, ρBP = (18)
dB3
bubble surface becomes partially or even fully rigid even without any
particles however both parameters affect the bubble rise velocity when As the particles form a monolayer on the surface of the bubble, the
surfactant concentration is below a threshold value. In this context, the change in total volume of the bubble has very little difference between
models of rise velocity and drag coefficient of a single bubble accounting the bare bubble case and loaded bubble > 1 %. The volume of particles
for both particles and surfactant concentrations are presented in the therefore was ignored when determining the volume of the particle-
following sub-sections. laden bubble.
The number of loaded particles, NP in Eq.(18) was determined ac
cording to Wang et al., (2020) as:
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 13. Drag correction factor as a function of bubble surface loading for various surfactant concentrations: a) 0% cmc; b) 5 to 10% cmc; c) 15 to 25% cmc.
4πdB2 (ϕBSL)
NP = (19) 3.2.3. Drag coefficient model
πdP2
The drag correction factor αBP,U which represents the effect of bubble
surface loading on
where ϕ is the packing factor of the particle loading region and was
assigned a value of 0.8 (Gallegos-Acevedo et al., 2006; Huang et al., 24 ( )
CD,BP = αBP,D 1 + 0.15Re0.687 (21)
2011). ReBP BP
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
Fig. 14. Comparison of predicted and experimental rise velocity of particle-laden bubbles in a) 0 % cmc; b) 10 % cmc; c) 15 % cmc; and d) 25 % cmc of SDS solution.
Liquid densityρL = 998 kg/m3, bubble densityρB = 1.18 kg/m3.
4 however suggests that Model Eq. (27) predicts the correction factor
FG,P = π R3P ρP gNP (26) reasonably well even for bubble diameter as small as ~ 1 mm obtained
3
from Huang et al. (2011). Although no other experimental data is
where the number of loaded particles, NP, was calculated using Eq. (19). available to verify other bubble diameters, the reasonable agreement of
The force balance model presented in Eq.(23) was used to determine the proposed correlation down to 1 mm size bubble indicates that the
the drag coefficient for particle laden bubble (CD,BP) using the experi models developed in this study is also applicable within the range 1 ≤dB
mentally measured rise velocity (UBP). Then, the drag correction factor ≤ 2.88 mm and aspect ratio AR ≥ 0.5. It should be noted that the data for
(αBP,D ) was determined by comparing CD,BP with the Schiller-Naumann bare bubble in pure water was not included in Fig. 13 as its aspect ratio
drag model (Schiller et al., 1935) in Eq. (21) by replacing the bare was lower (~0.3) than the threshold selected for Eq. (27). This proposed
bubble rise velocity (UB) with the particle laden bubble rise velocity model of drag coefficient factor presented in Eq. (27) covers a reason
(UBP). The model of the empirical drag correction factor αBP,D was then able range of surfactant concentration and serves as an extension to the
developed by fitting it to the measured BSL data. It needs to be noted drag correction model earlier reported in Wang et al., (2021).
that use of experimentally measured bubble rise velocity in determining The rise velocity model for the bare bubble case presented in Eq. (11)
the velocity and drag correction factor decouples the interdependency of was suitably modified to account for the presence of particles by
these parameters which are otherwise related to each other through the including the drag coefficient correction factor αBP,D as follows:
force balance model. ∫ Ut ∫t
FB,B + FB,P − FG,B − FG,P − FD,BP
The drag modification factor αBP,D is presented in Fig. 13 for mobile- dUBP = dt (28)
surface bubble (Cs = 0 % cmc Fig. 13a), partial rigid bubble (Cs = 5 % 0 0 m′BP
and 10 % cmc, Fig. 13b) and rigid bubble (Cs ≥15 % cmc, Fig. 13c). where the modified mass m′BP is equal to the addition of the mass of
Similar to the velocity correction factor, the drag correction factor αBP,D loaded particles to the modified mass of a bare bubble m′B calculated
also shows distinctive behaviours in the three different bubble surface using Eq. (12) in Section 3.1 as below:
regime for near-spherical bubbles (BSL≤0.50 and AR ≥ 0.5) which can
be best fitted by the following expressions: 4 4 4
m′BP = πR3B ρB + πR3P ρP NP + Cv πR3B ρL (29)
⎧ 3 3 3
⎨ 0.29 + 2.56BSL (Cs = 0%, in pure water)
αBP,D = 1.11 + 0.81 BSL (0% < Cs < 15% cmc) (27) The rise velocity of a particle-laden bubble UBP predicted using Eq. (28)
⎩
1.44 (Cs ⩾15% cmc) for various surfactant concentrationCs = 0 to 25 % cmc is presented in
Fig. 14. Overall, a reasonable prediction was obtained from the model
It can be noted that in this study, only a single nozzle size was used to
when compared with all experimental cases (average RMSD ~ 0.028). In
produce bubbles of averaged diameter 2.88 ± 0.07 mm. Fig. 13a
the transition period, relatively larger deviations were observed in the
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
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A. Wang et al. Chemical Engineering Science 288 (2024) 119812
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