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Controlled foam generation using cyclic diphasic flows through a constriction

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DOI: 10.1016/j.ijmultiphaseflow.2017.02.009

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Accepted Manuscript

Controlled foam generation using cyclic diphasic flows through a

constriction

T. Gaillard, M. Roché, C. Honorez, M. Jumeau, A. Balan,

C. Jedrzejczyk, W. Drenckhan

PII: S0301-9322(16)30212-9
DOI: 10.1016/j.ijmultiphaseflow.2017.02.009
Reference: IJMF 2549

To appear in: International Journal of Multiphase Flow

Received date: 8 April 2016

Revised date: 20 February 2017
Accepted date: 22 February 2017

Please cite this article as: T. Gaillard, M. Roché, C. Honorez, M. Jumeau, A. Balan, C. Jedrzejczyk,
W. Drenckhan, Controlled foam generation using cyclic diphasic flows through a constriction, Interna-
tional Journal of Multiphase Flow (2017), doi: 10.1016/j.ijmultiphaseflow.2017.02.009

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 ACCEPTED MANUSCRIPT

Controlled foam generation using cyclic diphasic flows

through a constriction
T.Gaillarda , M.Rochéa,b , C.Honoreza , M.Jumeaua , A.Balana ,

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C.Jedrzejczyka , W.Drenckhana

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a
Laboratoire de Physique des Solides, CNRS UMR 8502 and Université Paris Sud,
Bâtiment 510, 91405 Orsay Cedex, France
b
Now at Laboratoire Matière et Systèmes Complexes, CNRS UMR 7057 and Université

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Paris Diderot, Bâtiment Condorcet, 75205 Paris Cedex 13, France

Abstract
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Numerous industrial and academic applications of liquid foams require a fine
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control over their bubble size distribution and their liquid content. A particu-
lar challenge remains the generation of foams with very small bubbles and low
liquid content. A simple technique which fulfils these different criteria, the
“double syringe technique”, has been exploited for decades in hospital appli-
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cations. In this technique, the foaming liquid and gas are pushed repeatedly
back and forth through the constriction that connects two syringes. After
having motorised the technique we investigate here the influence of the differ-
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ent processing conditions on the obtained foam properties in a quantitative

manner. We show that this technique is unique in producing foams with the
same characteristic bubble size distributions over a wide range of processing
conditions (tubing, fluid velocities,...), making it an ideal tool for controlled
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foam generation. In contrast to other techniques, the liquid fraction in the

double syringe technique can be varied without impacting the bubble size
distribution. Using high-speed imaging we show that bubbles are dispersed
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in the aqueous phase at two different places in the device. Through an anal-
ysis based on the estimation of the characteristic dimensionless numbers of
the flow we bring some insights on the potential hydrodynamic instabilities
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at play in the dispersion process. We compare our experimental results with

bubble size distributions predicted by hydrodynamic fractionation processes.
Keywords: Foam generation, Diphasic Flow, Bubble size distribution,
Flow pattern, Hydrodynamic instabilities

Preprint submitted to International Journal of Multiphase Flow February 22, 2017

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1. Introduction
Liquid foams consist of closely packed gas bubbles within a continuous
liquid phase. Due to their rich properties they are at the core of numerous
fundamental research problems [4, 37, 25] and of a wide range of applica-

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tions [32]. The properties of foams depend on the average bubble size, the
bubble size distribution and on the liquid fraction, φ (given by the ratio of the

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liquid volume over foam volume), and thus depend on the mechanism used
to generate the bubbles in the liquid phase. A wide range of foaming tech-

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niques are routinely applied in research laboratories or for applications [11],
ranging from physical (break-up of bubbles under shear, phase transitions,
etc.), via chemical (gas releasing reactions) to biological techniques (yeast).
A major issue in the use of these techniques is the fact that bubble size and

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liquid fraction are not only tightly coupled, but that it is also inherently
difficult to obtain control and reproducibility over the foam properties. Last
but not least, a key challenge lies in the reliable generation of small bubble
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foams with low liquid fraction. A promising technique - at least for small
foam volumes - has been developed about 40 years ago for foam-based scle-
rotherapy in hospitals [39]. As shown in Figure 1, the technique consists
of two connected syringes containing a well-defined volume of gas VG and
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liquid VL , which are connected by a short piece of tubing. The foam is then
generated by pushing both liquid and gas repeatedly through the connecting
tube. Similar techniques are used for the generation of emulsions [30, 31].
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Figure 2 shows that foams obtained with the double syringe technique
have the visual appearance of a typical white shaving foam: the foam scat-
ters light indicating the presence of numerous small bubbles. When care
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is taken to avoid the destabilisation of the foam during and just after its
generation, we finds the characteristic bubble size to be of the order of 20
microns for the three foams shown in Figure 2. Traditionally, these foams are
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generated “by hand”. Nevertheless, most users have reported an astound-

ing reproducibility in the foam properties obtained for different experimental
runs, different experimentalists and even different syringes and connectors.
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One main goal of our work was therefore to characterise the foams obtained
with the double-syringe technique under various conditions. For this purpose
we automated the technique to obtain precise control over the processing pa-
rameters.
In Section 2 we describe how we performed our experiments using two dif-
ferent devices. The first of these devices applies a sinusoidal velocity profile

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Figure 1: Principle of the two-syringes technique (a) Initial state (b) After one push:
bubbly Liquid with tiny bubbles (c) Foam after several pushes. The liquid fraction is
defined as the ratio between the liquid volume VL and the foam volume VL + VG with VG
the gas volume.
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to the fluids while the second one applies a squared velocity profile. The
frequency of these profiles is adjustable leading to different pushing veloc-
ities U . We used these machines to investigate the influence of the device
parameters (Section 3.1) and of the foam formulation (Section 3.2). We con-
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firm the robustness of the bubble size distribution. In Section 4 we report

high-speed observations of the foaming process within the device from which
we suggest possible bubbling mechanisms. A better understanding of these
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mechanism may lead to the design of efficient and well-controlled foaming

techniques to provide foams of adjustable bubble size and liquid fraction,
ideally in a continuous manner to remove the finite foam volume restriction
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currently imposed by the use of the syringes.

2. Materials and Methods

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2.1. Materials
Most of the experiments were conducted with solutions of the anionic
surfactant Sodium Dodecyl Sulfate (SDS, Sigma-Aldrich, used as received).
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The solutions were prepared by dissolving SDS in ultra-pure water at 23 g/L

which corresponds to ten times the critical micellar concentration (CMC).
Ultra-pure water with a resistivity greater than 18 M Ω.cm was obtained
from a Millipore Simplicity 185 filtering device. For each experiment freshly
prepared solutions were used to avoid surfactant hydrolysis. To probe the im-
portance of the foaming liquid we varied the viscosity of the SDS solution by

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Figure 2: Typical foams obtained for various liquid fractions φ using the double syringe
technique of Figure 1. (a) φ = 30% (b) φ = 10% (c) φ = 3%.

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adding different amounts of glycerol (Fischer Scientific, purity > 99%). So-
lutions were made of 30 wt% and 50 wt% of glycerol, which leads to solution
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viscosities of 2.4 mPa.s and 5.8 mPa.s respectively (at room temperature).
In order to establish the influence of the foam stabiliser we used different sur-
factant mixtures. These include the cationic surfactant TTAB (at 10 CMC),
the non-ionic sugar-based surfactant β − C12 G2 (at 10 CMC), a surfactant
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mixture known to make very rigid interfaces and highly stable foams (the
“Bulgarian mixture” [18]), and the commercial dishwashing liquid “Fairy”
(at 10 wt%). Common names together with abreviations, values of the crit-
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ical micelle concentrations, and equilibrium surface tension of all these sta-
bilising agents are summarised in Table 1. Nearly all experiments were done
using nitrogen gas with traces of C6 F14 (Sigma-Aldrich) in order to reduce
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gas exchange between bubbles. Finally to compare the influence of the gas
on the foaming mechanism as well as on the ageing of the foam during the
generation experiments were conducted using pure C2 F6 or CO2 (Air Liq-
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uide).

2.2. Foam generation

To generate the foams, the entire body of one syringe (60 mL, Codan
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Medical) is filled with both the solution (volume VL ) and the gas (volume VG )
in proportions corresponding to the initial liquid fraction, i.e φ = VL /(VL +
VG ). In the case of the pure gases the gas is introduced in the syringe by
simply connecting it to the gas tank of interest, whereas in the case of C6 F14 ,
which is liquid at room temperature but extremely volatile, the syringe is

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Surfactant Abbreviation CMC (g/l) Surface tension γ (mN/m)

Sodium Dodecyl Sulfate [22] SDS 2.3 36
Tetradecyl Trimethyl Amonium Bromide [21] TTAB 1.3 38
β − C12 G2 [17] C12 G2 0.1 34
SLES+betaine+MAc [18] Bulgarian mixture - 23.8

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Fairy dishwashing Liquid [10] Fairy - 31

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Table 1: Stabilising agents.

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connected to a bottle containing the liquid C6 F14 and some gas is bubbled
slowly through it in to the syringe.

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It is important to note that the liquid fraction φf of the obtained foam has a
lower limit, i.e. if too much gas is placed in the syringe the generated foam
will not fill completely the syringe and therefore the final liquid fraction of the
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generated foam will not correspond to the initially placed liquid fraction in
the syringe. In most experiments the gas finally gets entirely included within
the liquid, so that φf = φ and we will discuss (in Section 3.1) how this
initial liquid fraction φ influences the foaming mechanism. Both syringes are
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horizontal and this first syringe is then connected to the second one, whose
piston is in the fully closed position, as shown in Figure 3a. In our case this
connection is ensured by a tubing of variable length and diameter connected
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to the outlet of the syringes. For most cases we use rigid PVC tubing with an
inner diameter of 3.5 mm and a length of 20 cm. The outlets of the syringes,
being of a diameter smaller than the tubing used, form constrictions in the
flow path (Figure 17). Foaming action occurs upon repeatedly pushing the
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gas/liquid mixture through the connection.

In order to automate this pushing action we built two types of machines.
The first one (Figure 3a) is made of two hydraulic pistons going alternatively
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back and forth at a constant velocity that can be set between 10 and 50
mm.s−1 . The second device, shown in Figure 3b, is made of two rotating
arms which perform the pushing action on the pistons. The piston velocity
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varies therefore in a sinusoidal manner and depends on the frequency f . We

use two frequencies, f = 1/3 s−1 and f = 1/6 s−1 . Since the piston path in
the syringe is 100 mm long, this gives a pushing velocity which goes up to
about 100 mm.s−1 (resp. 50 mm.s−1 ) at the point of maximum velocity and
an average velocity of 66 mm.s−1 (resp. 33 mm.s−1 ).

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Figure 3: Photographs of the two devices which are used for foam generation: (a) Two

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hydraulic pistons which perform a pushing action on the syringe pistons at constant, but
adjustable, velocity (10 - 50 mm.s−1 ). (b) Crankshaft set-up. Typical rotation frequencies
1/6-1/3 s−1 . The average piston velocities used here are then 33 and 66 mm.s−1 , leading
to peak velocities of 50 and 100 mm.s−1 , respectively.
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2.3. Bubble size measurement

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After the generation, a small amount of foam is deposited rapidly on a

microscope cover slide together with a few drops of the foaming solution.
These drops ensure a good separation of the bubbles when the second mi-
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croscope slide is put on the top to spread the foam. The two microscope
slides are separated by plate spacers of height 150 µm as sketched in the
inset of Figure 4a. Separating the bubbles in this way is not only helpful
for the imaging purpose, but it also reduces foam ageing effects during the
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capture of the image. To provide good statistics on the bubble size distri-
bution we ensured the measurement of at least a thousand of bubbles, with
a typical count of 10000. To do so we use a digital microscope (Keyence
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VHX Series 2000) that scans a complete layer of thousand of bubbles with
micrometric resolution. A small section of a typical image is shown in Figure
4a. To obtain the size of the bubbles, the images are first thresholded and
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then processed by combining binarisation with a watershed algorithm using

the ImageJ software (freely available at http://imagej.nih.gov/ij/). After
this procedure the bubbles appear as black circles (Figure 4b), which are
then detected by the “Analyze particle” tool of the ImageJ software in order
to obtain the corresponding bubble radius distribution. Bubbles which are
larger than the spacing between the two microscope cover slides (150 µm)

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are flattened into pancake shape and a small correction must be done to
obtain their true volume. More details on this correction can be found in a
previous paper [14]. The resolution of the image processing is reliable down
to bubble of radius of 3 µm. The full processing finally gives bubble size
distributions like the on shown in Figure 4c. These distributions are then

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converted into probability density functions (PDF) in number (PDFN ) or in

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volume (PDFV ), defined respectively as:

N (R < RB < R + ∆R )
PDFN = , (1)

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Ntot ∆R
and
V (R < RB < R + ∆R )
PDFV = , (2)

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where N (R < RB < R + ∆R ) is the number of bubbles of radius RB be-
tween R and R + ∆R , V (R < RB < R + ∆R ) the total volume of the bubbles
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of radius RB between R and R + ∆R , Ntot the total number of bubbles, Vtot
the total volume of the bubbles, and ∆R the bin size of the histogram.
When considering the physical properties of the generated foam it is more
relevant to discuss volume distributions rather than number distributions.
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However as our interest is mostly to understand the mechanisms of genera-

tion of the bubbles we will mainly discuss the number distributions (designed
simply as PDF from now on). Moreover our imaging technique cannot cap-
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ture both small (20 µm) and big bubbles (1 mm) so volume distribution and
number distribution appear to be quite similar. These will be discussed in
Section 3.3.
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3. Results
Using both setups described in Section 2.2 we investigate a set of param-
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eters likely to affect the foam generation. In Section 3.1 using exclusively
SDS-stabilised foams we investigate the role of the pushing velocity U and
of the number of pushing cycles N , together with the influence of the initial
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liquid fraction φ incorporated in the syringe. We then explore the influence

of both the length L and the diameter D of the tubing connecting the two sy-
ringes. In Section 3.2 we investigate the influence of the physical-chemistry of
the system, including the viscosity η of the liquid and the nature of the foam
stabiliser. All results are complemented in Section 4 by observations obtained

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Figure 4: Bubble size measurement technique: (a) Cropped image obtained using the
Keyence microscope (b) Corresponding image after binarisation in combination with a

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Watershed algorithm. (c) Obtained bubble size distribution.
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with high-speed imaging and an analysis of the associated non-dimensional
numbers.

3.1. Dependence of the bubble size distribution on device parameters

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Initial liquid fraction φ and number of pushing cycles N : In both

devices foam is generated already during the first pushing cycle, whatever
the pushing conditions. If the initial liquid fraction φ in the syringe is high
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enough, the entire syringe is filled with foam right after the first cycle. This
is shown in Figure 5a for the example of φ = 15%. However, if only a small
amount of liquid is present, it takes several cycles N to incorporate all the
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gas into the liquid. For example N = 15 for φ = φf = 3% as shown on

Figure 5a. The precise number of cycles depends not only on the amount of
liquid, but also on the pushing speed U . The higher U , the more rapidly the
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gas is fully integrated into the liquid.

It is interesting to analyse the bubble size distribution of the generated
foam. After the first cycle, a few large bubbles (about 1 mm) are present in
the foam, surrounded by numerous tiny bubbles. Since the few large bubbles
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are two orders of magnitude larger than the small bubbles, we cannot image
both populations simultaneously. This is why they do not appear in the dis-
tributions, even though at low pushing speed they may take up a significant
volume of the foam during the first cycles.The bubble size distribution of the
small bubbles are shown in Figure 5b for both devices, after different num-

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bers of cycles and for φ = 15%. After about 10 - 15 cycles all large bubbles
have typically disappeared. When taking into account only the population
of small bubble, a general trend can be observed already after the first cycle.
A characteristic size distribution appears which shows a nearly exponential
decay towards larger bubbles and a steep fall-off towards smaller bubbles

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defining a peak at a characteristic bubble size of 10 - 20 µm. This peak

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seems more pronounced for the sinusoidal device. With increasing number of
cycles N and for N < 12, the distribution becomes slightly narrower while the
peak position remains constant, leading to a small drop in the average bubble

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radius hRB i. This evolution is shown in Figure 5c for the sinusoidal device
for two different liquid fractions (φ = 3% and φ = 15%). Interestingly, the
normalised bubble size distributions (Figure 5d) seem fairly invariant during

devices.
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the first 1-12 cycles, even though one can see a difference between the two

After about 10 cycles (depending on the device and pushing speed), the
distribution remains narrow but the cut-off becomes smoother and the peak
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shifts to slightly larger bubble sizes. Both peak and average bubble radius
increase with increasing number of cycles reaching a constant values around
15 cycles. We think that foam ageing does not play an important role in
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fixing the initial distribution (after the first cycle), but ultimately it shoulds
balance the foam generation mechanisms and have a role in fixing this equi-
librium distribution. These foam aggeing effects are discussed in more details
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in Appendix 6.1. The bubble size distribution after a large number of cycles,
which we shall from now on call the “equilibrium distribution”, depends lit-
tle on the foaming device and the liquid fraction of the foam, as shown in
Figure 6. Moreover, when this equilibrium distribution is reached, there are
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no more big bubbles within the foam.

Pushing velocity U : Let us now discuss the influence of the piston ve-
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locity U on the bubble size distribution obtained after the first push N = 1.
This is shown in Figure 7 for both devices for a liquid fraction of φ = 15%. In
both of them it seems that the characteristic peak position does not vary sig-
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nificantly with the pushing velocity. The width of the distribution however
decreases with increasing pushing velocity in the constant velocity device.
While an influence of the pushing velocity may be detected during the first
cycles, it has negligible influence on the equilibrium distribution after a large
number of cycles.

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(a) (b)

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(c) (d)

Figure 5: (a) Filling fraction (foam volume / syringe volume) as a function of the number
of cycles N for two different liquid fractions for the sinusoidal device (f = 1/3 s−1 ). (b)
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Influence of the number of cycles N and pushing type (constant velocity or sinusoidal
velocity) on the obtained bubble size distributions for φ = 15%. (c) Evolution of the
average bubble size < RB > and the peak value with the number of cycles N in the
sinusoidal device (f = 1/3 s−1 ) for two different liquid fractions. (d) Normalised bubble
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size distributions from (b) in semi-log scale for both devices (U = 50 mm.s−1 and f =
1/3 s−1 ).
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The influence of the velocity U on a foaming process is often capture via

the power input PI of the process. For our devices we may define it as

PI = Q∆P = U SP ∆P, (3)

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Figure 6: “Equilibrium” distributions for both devices (U = 50 mm.s−1 and f = 1/3 s−1 )
after 15 cycles for different liquid fractions.
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Figure 7: Influence of the pushing type and speed on the bubble size distribution after 1
cycle in the constant-velocity device (top) and in the sinusoidal-velocity device (bottom)
for φ = 15 %.
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where ∆P is the pressure difference between the syringes, Q is the aver-

age flow rate and SP the cross-section of the syringe. Because of the friction
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of the pistons on the wall of the syringes the motion of the two piston is
not perfectly synchronised and the gas is compressed. We can calculate that
∆P ≈ 1.2 bar. We find that during the first cycle, this value depends little
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on the pushing velocity. We can therefore estimate the power input to vary
from 5 Watt at 10 mm.s−1 to 20 Watt at 50 mm.s−1 . This is a variation by a
factor of four, which does not seem to be correlated with the obtained bubble
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sizes. However the effect of an higher power input might be to generate more
bubbles during a cycle which is indeed what we observe since more cycles are
needed to produce the foam at lower pushing velocity.
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Tubing dimensions: In order to investigate the influence of the di-

mensions of the tubing which connects the syringes, we used tubing of two
different lengths L = 20 − 40 mm and of three different inner diameters
D = 1.6 − 3.5 − 4.6 mm. The obtained bubble size distributions are shown
in Figure 8 for φ = 15 % and for N = 15. Within the experimental error the

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equilibrium size distribution seems quite independent of the tubing geometry.

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Figure 8: Influence of the tubing length and diameter at φ = 15% and U = 50 mm.s−1 on
the equilibrium bubble size distribution.
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In summary, all our results seem to show that the key features of the bub-
ble size distributions are, to first order, independent of the device parameters
- at least in the range we investigated. This means that foam generation
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with this double-syringe technique is highly reproducible: independently of

the number of cycles, the pushing velocity, the initial liquid fraction, or the
tubing dimensions, the generated bubbles are very small (peak between 10
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and 20 µm) with a polydispersity of 30 to 40 %. Finally a very important

feature of this technique is that the bubble size is not a function of the liquid
fraction. While bubble size and liquid fraction are correlated in most foaming
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technique [11, 16], the double syringe technique makes wet and dry foams
with the same bubble size distributions.

3.2. Dependency of the bubble size distribution on the foam formulation

Viscosity: In order to investigate the influence of the foam formulation
on the equilibrium distribution we varied systematically the viscosity of the

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foaming liquid by adding glycerol. Figure 9a shows how the bubble size dis-
tribution after N = 10 cycles depends on the liquid viscosity (η = 1 mPa.s,
2.4 mPa.s, or 5.8 mPa.s) for two different liquid fractions (15 % and 30 %) in
the constant velocity device (U = 50 mm.s−1 ). With increasing viscosity the
distribution becomes clearly narrower and the characteristic peak position

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decreases from 20 µm for η = 1 mPa.s down to 7.5 µm for η = 5.8 mPa.s.

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Figure 9b shows the evolution of the distribution with liquid fraction for
η = 5.8 mPa.s. Contrary to our observation made with a surfactant solution
with viscosity η = 1 mPa.s, the bubble size distributions here depends on

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liquid fraction: the decay towards larger bubbles steepens for lower liquid
fractions. Nevertheless, Figures 9c and 9d show that the shape of the nor-
malised distribution of RB / < RB > is roughly independent of the viscosity
and of the liquid fraction.
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In the inset of Figure 9b we show the evolution of the average bubble
radius with number of cycles for two different viscosities (1 and 5.8 mPa.s)
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for a liquid fraction of 15% . This data shows that when the viscosity of
the solution is increased the mean bubble size varies less with the number of
pushing cycle. However, while the final bubble size distribution is obtained
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after less cycles, the final foam volume is actually obtained with more cycles.
i.e with increasing viscosity it takes longer to create the foam. In that sense
reducing the initial amount of liquid or increasing the viscosity seems to have
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a similar effect on the foaming mechanism. More importantly, with increas-

ing viscosity it becomes more difficult to fill the entire syringe with foam, i.e.
to incorporate all the gas into the liquid even after many cycles. This leads
to a minimum achievable liquid fraction φmin which can be obtained with
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this technique for a given viscosity. This minimum liquid fraction depends
sensitively on the pushing speed: the larger the pushing speed, the larger the
minimum liquid fraction becomes (Figure 10). Interestingly, the data scales
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with the capillary number Ca2/3 = (ηU/γ)2/3 , which may indicate that this
final minimum liquid fraction may be fixed by friction between the foam and
the wall [9].
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Foam stabiliser: An important question arises regarding the influence

of the nature of the stabilising agent on the final foam properties. While all
the experiments up to now have been done with SDS, we investigate here
a range of commonly used foam stabilisers. For this purpose we choose a
liquid fraction of 15 % and we compare again the equilibrium distributions

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(a) U = 50 mm.s−1
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(c) U = 50 mm.s−1 (d) f = 0.34 s−1

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Figure 9: (a) Bubble size distributions after 10 cycles at U = 50 mm.s−1 for two different
liquid fractions and three different viscosities η. Inset: Images of a layer of bubbles for
each viscosity. (b) Bubble size distribution after 10 cycles for sinusoidal pushing velocity
(f = 1/3 s−1 ) for different liquid fractions. Inset: Evolution of the mean bubble radius
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< R > with cycle number N for two viscosities. (b) PDF of RB / < RB > in semi-log of
the results shown in (a). (d) PDF of RB / < RB > in semi-log of the results shown in(c).

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Figure 10: Minimum liquid fraction φmin as a function of the viscosity η of the foaming
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solution for different pushing velocities U in the constant velocity device.
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(N = 15) obtained in both devices. One can see in Figure 11 that the foam
formulation has a non-negligible influence on the final bubble size distribu-
tions. The peak in the obtained bubble sizes can be pushed down below 10
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µm. As shown in Figure 12 the obtained bubble size distributions for each
stabilising agent are again very reproducible and quite insensitive to the liq-
uid fraction and the device parameters, as discussed in detail for the SDS
foams in Section 3.1. Yet there is no direct correlation between the surface
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tension of the stabiliser and the typical size of the bubble, and it is sur-
prising to find out that foams made from SDS surfactant and the Bulgarian
Mix have the closest characteristic bubble size while their surface properties
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(Bulgarian Mix are known to make rigid interfaces) are very different [18, 36].

In summary, we have seen that while the device parameters have a negligi-
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ble influence on the obtained bubble size distributions, the foam formulation
(liquid viscosity and stabilising agent) seems to play a role in fixing the bub-
ble sizes.

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Figure 11: Influence of the foam stabiliser on the bubble size distributions after 10 cycles
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in both devices at φ = 15%.
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3.3. Number VS Volume distribution

Our results focused entirely on the bubble size distribution in number
as our goal is to obain insight into the generating mechanism. However, for
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most users, the physical properties of the obtained foams will be of great
interest. For this purpose, it is often more appropriate to use the bubble
size distributions by volume (Section 2.3). We therefore compare here the
two types of distributions (Figures 13) for different liquid fractions and for
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the different stabilising agents - all obtained in the equilibrium regime. As

mentioned earlier no millimetric bubbles remain in the foam at this stage, so
that both number and volume distributions are very similar.
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4. Discussion
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In Section 3 we have evidenced some of the key features of the double sy-
ringe device. In particular, we have seen that the foaming mechanism seems
to be fairly independent of the device parameters at least in the ranges we
tested. Neither the type/amplitude of the pushing velocity nor the liquid
fraction nor the tubing dimensions seems to play a major role in fixing the

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(a) TTAB (b) Fairy
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(c) C12 G2 (d) Comparison of various stabilisers

Figure 12: Bubble size distributions obtained after 10 cycles for different stabilising agents.
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(a) Number distribution. (b) Volume distribution.
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(c) Number distribution. (d) Volume distribution.

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Figure 13: (a) Number and (b) Volume distributions of SDS-stabilised foams for various
liquid fractions after 15 cycles in both devices. (c) Number and (d) Volume distributions
of foams stabilised by various surfactant at a liquid fraction φ = 15% after 15 cycles in
both devices.
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obtained bubble-size distributions. On the contrary the effect of the foam

formulation (viscosity and stabilising agent) is significant. This indicates
the presence of a physical foaming mechanism which is controlled rather
by the physico-chemical properties of the gas/liquid dispersion, than by the
properties of the device. We advance here some hypothesis on the potential

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mechanisms.

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Before entering into a more detailed discussion, let us note that any dis-
cussion on foaming needs to take into account the potential influence of foam

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ageing effects (bubble ripening or coalescence) on the obtained bubble size
distributions. In order not to confuse the reader, this is discussed in the
Appendix 6.1. There we provide different experimental investigations and

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arguments to demonstrate that the main features of the measured bubble
size distributions are expected to be the result of the generating mechanism,
rather than of foam ageing effects.
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4.1. Description of foaming mechanisms
It is tempting to think that the mechanism of foam production in this
system is related to bubble break-up under shear. In such a scenario large
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bubbles are produced during the first cycles and are then broken up repeat-
edly in the following cycles by the shear arising in both constriction and
tubing. The mean bubble size should then decrease with increasing number
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of cycles. However, even though this mechanism probably happens, it cannot

be the major contribution to the bubble size distribution as the characteristic
distribution is already obtained after one single push.
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The goal of this section is therefore to describe the bubbling mechanisms

observed within this device and to suggest two mechanisms likely to control
the final distributions. For this purpose we work with a high-speed cam-
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era to provide images of the process (Photron Fastcam SA3). Visualisation

experiments are done with the constant-velocity device and during the first
push of the process. The set-up was simplified to allow us to observe what
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happens in the channel. It now consists of only one syringe containing the
surfactant solution and the gas which are then pushed through the syringe
constriction connected to the tubing. The rigid tubing is replaced by a flex-
ible and transparent one of equal length and diameter. Figure 14 compares
the bubble size distribution obtained with this simplified set-up with those
obtained with two syringes after one cycle. These distributions being almost

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Figure 14: Comparison of bubble size distribution after one push between one syringe and
two syringes
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identical we assume that we can use only one syringe and focus on the mech-
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anisms happening within the constriction and the tubing.

Figure 15 shows images of the flow within the constriction and all along
the tube for two different liquids (pure water and surfactant solution) and
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at two different pushing speeds, for an initial liquid fraction of φ = 50%.

We observe a complex foaming behavior which can be divided into two main
steps: one foaming mechanism within the constriction and one at the en-
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trance of the tubing. Both are discussed in detail in the following.

Within the constriction millimetric bubbles are formed in a repro-

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ducible way whatever the pushing velocity and the formulation. This phe-
nomenon is shown in Figure 15 and detailed in Figure 16. As it is known from
numerous micro- and millifluidic applications [16, 15, 24, 13] a configuration
where a millimetric bubble grows inside a channel is not stable indefinitely:
the bubble will detach from the injection point due to a capillary-driven in-

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Figure 15: Images of the flow within the constriction (0 mm) and the connecting tube (10, 75,and 150 mm) for pure water
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and surfactant solutions at two different speeds U = 10 mm.s−1 and U = 50 mm.s−1 .
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Figure 16: A millimetric bubble is created in the constriction of the syringe whose rear end
breaks into many tiny bubbles just after detachment. The created bubbles are too small
to be resolved by the camera but they strongly scatter light which is why they appear as
dark zones in the image.
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stability. During this detachment an interesting phenomenon happens: the

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downstream end of the bubble seems to “explode” into many tiny bubbles
during the few milliseconds of the detachment process. The tiny bubbles
are too small to be resolved by the camera, but one can see their presence
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due to their efficient light scattering that creates the black, blurry zones in
the images. While this effect is small at low pushing velocities, it becomes
more important at higher pushing velocities. The critical pushing velocity
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at which we begin to observe this phenomenon varies with the presence of

surfactant. This effect is reproducible and occurs at the rear of each bubble.
The precise mechanism which leads to this break-up phenomenon is not clear
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to us but preliminary results suggest that the geometry of the constriction

has an important role to play.
The second foaming mechanism takes place at the exit of the constriction,
i.e at the entrance of the tubing. This corresponds to the position z = 10
mm in Figure 15. While diphasic flows and air entrapment into pure water
in pipes or microchannels have been extensively studied [1, 38, 35, 33, 27],

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we describe here a system where the presence of surfactant influence the flow
pattern and the bubble generation. Whereas at U = 10 mm.s−1 with pure
water and air an annular flow is formed which then destabilises in a slug
flow further in the tubing (z = 75 mm and z = 150 mm), the presence of
surfactant stabilises the big bubbles formed in the constriction which then

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accumulate to form a bubbly flow down the tubing. We note the presence
of tiny bubbles. At U = 50 mm.s−1 air and water keep forming annular

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flow at the outlet of the constriction, and the generation of tiny bubbles
is clearly noticable. This annular flow then destabilises into a bubbly flow

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which generates a large quantity of tiny bubbles turning the tubing black
due to strong light scattering.
At first sight one may take this observation as a cavitation effect [20, 2].

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Using gases of different solubility we show in the Appendix 6.2 that this
could be excluded as potential mechanism.

4.2. Analysis of foaming mechanism

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Bubbling in two-phase flow is a vast subject [8, 1]. A wide number of flow
conditions - and the associated instabilities of the air/liquid interface - are
known to produce bubbles with characteristic sizes and size distributions [34,
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28, 29]. Due to the complexity of the flow conditions in our set-up, we are
not able yet to identify clearly the physical instabilities at the origin of our
process. We nevertheless give some first qualitative analysis here.
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We shall use the following dimensionless numbers

Capillary number Ca = ηhui

γ
Reynolds number Re = ρhuiL
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η
ηhui2 L
Weber number We = γ
,

in order to compare the relative importance of the viscous, inertial and

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capillary stresses at different locations in our setup. Here γ is the surface

tension, ρ the density, hui the mean velocity of the fluid of interest, and L
the characteristic length scale over witch the flow occurs. We calculate the
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non-dimensionless numbers for each of the fluid phases.

The syringes have a large cross-section (Ds = 24 mm) compared to the

smallest cross-section of the constriction (Dc = 1.6 mm) and the tubing
(Dt = 3.5 mm) (Figure 17a). This leads to high aspect ratios: (Ds /Dc )2 =
225, (Ds /Dt )2 ≈ 50 and (Dc /Dt )2 ≈ 5 - and hence to abrupt and significant

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Figure 17: (a) Sketch of the geometry of the constriction of diameter Dc and the tubing of
diameter Dt , in which an annular flow occurs. (b) Sectional view of the annular flow. Dg
and el are calculated making the approximation that gas and liquid flow have the same
cross-section. Di is the diameter of the tube at a given position.
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changes in the average flow velocity < u >. Since we see that the water level
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in the syringe remains constant during foaming at roughly half the diameter
of the syringe, we assume in the following that the flow rate of the liquid and
of the gas are roughly equal and constant, i.e. Ql ≈ Qg ≈ const. (considering
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the gas as incompressible). The cross-section of the gas and of the liquid in
the constriction and in the tubing adjust to the flow conditions. Inspired by
our experimental observations, we shall assume in the following that the flow
is annular and that both cross-sections are roughly equal. As illustrated in
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Figure 17b, this allows us to fix the characteristic length scale L of the gas
flow as the diameter of the thread of the annular flow Dg , and the one of the
liquid flow as the thickness el of the layer in contact with the wall .
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Using these length scales and the average velocity U imposed by the
syringe piston, we can calculate the different dimensionless numbers for the
gas and the liquid in the constriction and in the tubing. These are listed in
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Table 2.
Because of the high aspect ratio between the cross-section of the sy-
ringe and the constriction ((Ds /Dc )2 = 225), gas and liquid are greatly
accelerated in the constriction. For example, flow velocities < u > of the
order of 10 m.s−1 are reached in the constriction for a pushing velocity

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In the constriction In the tubing

Piston Velocity U = 10 mm.s−1 U = 50 mm.s−1 U = 10 mm.s−1 U = 50 mm.s−1
Phase Liquid Gas Liquid Gas Liquid Gas Liquid Gas
< u > (m.s−1 ) 2.2 2.2 11.3 11.3 0.5 0.5 2.3 2.3
−4
Capillary number Ca 8.10 1
9.10 4.10 2
5.10−3 1.10 −2
2.10−4 6.10 −2
10−3

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2 2 3
Reynolds number Re 5.10 2.10 3.10 9.102 2.10 2
8.101 103
4.102

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Weber number W e 3.101 2.10−1 8.102 4 3 2.10−4 8.101 4.10−1

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Table 2: Flow velocity and corresponding dimensionless numbers calculated at the outlet
of the construction (Dc = 1.6 mm) and within the tubing (Dt = 3.5 mm).

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U = 50 mm.s−1 . This leads to an increasing importance of inertial effects
(high Re and W e numbers). Moreover, as one can see in Figure 16, the
cross-section of the gas thread in the constriction goes periodically to zero
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during pinch-off process of the big bubble. Since both the gas and the liq-
uid flow rate remain roughly constant during this process, this means, that
the average liquid velocity reduces slightly, while the average gas velocity in-
creases dramatically. Inertial effects may therefore lead to a destabilisation
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of the gas thread during pinch-off, resulting in the explosive generation of

tiny bubbles observed within the constriction (Figure 16).
The second foaming mechanism arises when the fluids enter into the tub-
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ing. Here the average velocity decreases by a factor of five with a much more
significant decrease of the liquid velocity due to the angular flow geometry.
The associated capillary number of the liquid decreases significantly from
Cal << 1 in the constriction to Cal >> 1 in the tubing. At the same time,
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the W e number decreases by a factor of 10. Hence, while the flow is clearly
dominated by the inertial and viscous stresses within the constriction, capil-
lary stresses become much more important at the entrance of the tubing. In
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many situations of free interface flows it has been shown that these kind of
transitions are likely to lead to air entrainment [26, 7, 6].
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Since we cannot visualise the air entrainment process in our setup, it is

interesting to analyse more closely the obtained bubble size distributions as
these may be revelatory of the underlying mechanism. Two different types
of mechanisms are commonly considered in fragmentation-type processes.
These are best known in the case of droplet generation, but Eggers and

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Villermaux state in their review [12] that “there is no reason to think that
the same phenomenology and ideas should not apply to the opposite situ-
ation of bubbles forming in a continuous liquid phase”. In the first case,
thin ligaments of gas are formed within the liquid which - below a critical
thickness - destabilise into small bubbles. This process leads to a Gamma

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distribution which is given by [40]

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β α α−1
fGamma (x, α, β) = x exp(−βx), (4)
Γ(α)

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where α and β are the shape and rate parameters, respectively, and
R +∞
Γ(x) = 0 tx−1 et dt the Gamma function.
In the second case, a cascade of break-ups occurs, in which larger bubbles

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break into smaller bubbles, which then break again into smaller bubbles etc.
Taking into account a certain probability of coalescence events which reunites
bubbles, such a process leads to a Lognormal distribution which is given
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by [19]  
1 (ln(x) − µ)2
fLognormal (x, µ, σ) = √ exp − , (5)
xσ 2µ 2σ 2
P q P
where µ = n n ln(x) and σ = n1 n (ln(n) − µ)2 .
1
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In Figure 18 we fit these distributions to a selection of experimental distribu-

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tions obtained in both setups (i.e. constant or sinusoidal pushing velocity)

after the first cycle and after ten cycles. After the first cycle, the distributions
are captures slightly better by the Lognormal distribution, which may be a
signature of a breakup process via cascades. After 10 Cycles, both distribu-
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tions fit equally well. Moreover, the dependency of bubble size on viscosity
is similar to what has been observed in liquid jet fragmentation [12, 23]:
a higher liquid viscosity slows down the break-up of the thin gas threads
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since they remain stable for a longer time, resulting in narrower Gamma-
distributions. Combining these different observations, it is impossible at this
stage to draw any reliable conclusions from bubble size distribution. More-
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over, foam ageing and the presence of surfactants may have a non-negligible
influence on the obtained distributions. Future work should therefore aim
for a direct visualisation of the foaming process in order to elucidate the
underlying mechanisms.

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(a) U = 50 mm.s−1 Ncycle = 1
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(c) f = 1/3 s−1 Ncycle = 1 (d) f = 1/3 s−1 Ncycle = 10

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Figure 18: Comparison of experimental results with Lognormal (Equation 5) and Gamma
distributiona (Equation 4) for both constant and sinusoidal piston velocity.

5. Conclusion and Outlook

We have shown here how a simple technique - the “double syringe tech-
nique” - can produce small-bubble foams whose bubble sizes are of the order

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of 10 − 20 µm. The bubble size distributions have a well-defined peak with

a nearly exponential decay towards larger bubbles. These distributions are
highly reproducible and, most importantly, independent of the liquid frac-
tion. This is the only foaming technique known to us in which the liquid
fraction can be varied independently of the bubble size distribution. The

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double syringe technique is therefore an ideal tool to produce well-controlled,

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small-bubble foams.

We have been able to show that a characteristic bubble size distribution is

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obtained after the first pushing action, i.e. we are not dealing with a progres-
sive break-up of bubbles under shear in the constriction, as one may naively
expect (even though the foam initially contains some millimetric bubbles).

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We see, however, that the distribution changes slightly with number of cy-
cles, leading to an ”equilibrium distribution” after a certain number of cycles
which is again independent of the liquid fraction. We expect foam ageing to
play a role in fixing this distribution. However, it is not clear to us why the
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strong dependence of foam ageing effects on liquid fraction does not show up
in the distributions.
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We have systematically tested the influence of a wide range of parameters

on the obtained foam properties. We find that the parameters of the device
(pushing speed, pushing type, tubing length and diameter, ...) have very lit-
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tle influence on the obtained foam properties. The foam formulation (foam
stabiliser and liquid viscosity), on the contrary, influences non-negligibly the
obtained bubble size distributions. In particular, the bubble sizes decrease
measurably with the viscosity of the liquid. This viscosity also sets a well-
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defined minimum liquid fraction which can be produced. Since this minimum
liquid fraction increases strongly with liquid viscosity, the double syringe
technique is not appropriate for foaming high viscosity liquids.
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Using high-speed imaging, we attempted to identify the foaming mech-

anism and found two different mechanisms in the device, both related to
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hydrodynamic instabilities. The first mechanism arises in the constriction

in which the rear end of millimetric bubbles ”explodes” into numerous tiny
bubbles during pinch-off. The second mechanism, which seems the domi-
nating one, is visible at the entrance of the tubing, where a large quantity
of tiny bubbles seems to be generated in an annular-type flow. Analysis of
the associated non-dimensional numbers indicates that the mechanism in the

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constriction may be dominated by inertia, while the mechanism in the tubing

should also be sensitive to capillary stresses. Comparison of the bubble size
distributions with those known from the literature does not provide conclu-
sive indications about the nature of these mechanisms. Moreover, it is not
clear to us how foam ageing and the presence of surfactants may influence

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the bubble size distributions in comparison to those obtained from purely

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hydrodynamic effects.

Due to the coupling of hydrodynamics, physical chemistry and foam age-

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ing, future work should therefore aim for direct visualisation of the process,
potentially with simplified model experiments. A major step would then be
to export the acquired understanding in order to exploit this mechanism in

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a continuous process, rather than a periodic cycling between two syringes
which can only provide a small foam volume at a time. Moreover, it would
be desirable to find a device parameter which provides explicit control over
the obtained size distributions.
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However, even without this fine understanding of the foaming mecha-
nism, the double seryinge technique can already be used reliably in order to
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generate well-controlled, small-bubble foams with variable liquid fraction for

research purposes or applications.
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Acknowledgment
We thank Florence Elias and the members of the ANR SAMOUSSE in
whose context this work was inspired and regularly discussed. We thank
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Emmanuelle Rio, Anniina Salonen, Dominique Langevin, Benjamin Dollet,

Arnaud Saint-Jalmes, Jens Eggers, Christophe Josseran, Stéphane Popinet,
Thomas Séon, Frédéric Moisy, and Marc Rabaud for fruitful discussions.
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We thank Marc Bottinot, Vincent Klein, Jérémy Sanchez and Rémi Brauge
for building the foaming devices. We also thank Christophe Poulard for
letting us use excessively his Keyence Microscope, and Alain Cagna and
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Séverine Besson from TECLIS for additional stimulation of this work from
an applied perspective. Funding is greatfully acknowledged from the Euro-
pean Research Counsil (ERC) in form of an ERC Starting Grant (agreement
307280-POMCAPS) and from the French Agence Nationale de la Recherche
(project SAMOUSSE, ANR-11-BS09-001).

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6. Appendix
6.1. Foam ageing
To discuss the potential foaming mechanism one needs to quantify the in-
fluence of the foam stability on the obtained bubble size distributions. Foams

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are known to be inherently unstable: bubbles can dissolve in the surround-
ing liquid (“dissolution”), bubbles can exchange gas due to the difference in

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internal pressures (“coarsening”) and thin films between bubbles can break
(“coalescence”). These different ageing mechanisms are particularly rapid for

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small-bubble foams [3] and can lead to non-negligible changes in the bubble
size distributions. In our case we need to worry about this in two different
situations: foam ageing may arise in the syringes during foam generation

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and/or after foam generation during the time it takes to take the image of
the bubbles after their deposition in a monolayer (Section 2.3).

In order to verify the influence of the second process, we investigated the

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evolution of the bubble size distribution of an SDS foam containing nitrogen
bubbles with with traces of C6 F14 after deposition, taking images of the same
foam after t = 300 s, 2400 s, and 4500 s. t = 0 s corresponds to the mo-
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ment when the bubbles are deposited in the monolayer, as shown in Fig 4.a.
The results are shown in Figure 19. Since bubbles cannot coalesce in this
configuration, the ageing is essentially due to coarsening. One can see that
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it takes about one hour for the peak to double its maximum position. This
slow evolution is due to the presence of the C6 F14 . Since it takes us about 3
minutes to take the first image we can therefore assume that the bubble size
has not evolved more than a few micrometers between foam generation and
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imaging.

The analysis of the influence of foam ageing effects during foam gener-
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ation is more involved. Since bubbles are in close contact within the foam,
all ageing mechanism are accelerated with respect to the evolution shown in
Figure 19. Hence, it is certain that foam ageing has an influence on the final
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size distribution - the question being to what extent. A selection of obser-

vations tells us that the key features of the distributions we observe should
be a result of the generating mechanism - rather than of the foam stability.
A first indication is the fact that the distributions depend very little on the
liquid fraction. Foam ageing effects increase drastically with decreasing liq-
uid fraction - hence we should observe much larger bubbles for lower liquid

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Figure 19: Ageing of a bubble monolayer deposited between two glass plates, made from
a SDS solution at a concentration of 10CMC and with air having C6 F14 traces
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fractions, which is not the case. It shows even the opposite behaviour for
more viscous foaming liquids: the bubble size is more peaked for low liq-
uid fraction. Equally, the type of foam stabiliser plays an important role in
controlling foam stability. If foam ageing was a key parameter in fixing the
bubble size distributions, more stable foams would have narrower size distri-

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butions. Looking at Figures 11 and 12, this is not at all the case. “Fairy”

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and the “Bulgarian Mix” are expected to make the most stable foams but
do not have at all the narrowest bubble size distribution.

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To sum up: even though we expect foam stability to have an influence
on the size distributions, we believe that the controlling factor must be in
the generation mechanism. At this stage we are not able to quantify the

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influence of foam ageing. However, we expect it to be small enough so that
our key observations can be assigned to the foaming mechanism which we
discuss in the following.
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6.2. Cavitation
If cavitation was playing a role in the foam formation, the foaming ef-
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ficiency should depend on the solubility of the gas. We therefore repeated

the experiment under the same conditions using either pure C2 F6 (poorly
soluble in water) or pure CO2 (highly soluble in water). Figures 20b and 20c
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show that the bubbling mechanism with these two gases is undistinguishable
from the one with air+C6 F14 , which is why we consider the origin of this
observation to be of hydrodynamic nature [5]. Unfortunately we cannot ob-
serve directly what happens due to the strong light scattering by the tiny
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bubbles present on the walls of the tube. The fact that this mechanism is
much less efficient with pure water - which has a much higher surface tension
(0.072 N/m) than the SDS solution (0.034 N/m) (Figure 15, U = 50 mm.s−1 )
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suggests that surface tension- and therefore capillarity effects - may play an
important role in the foaming mechanism.
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(a) Air and C6 F14 traces
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(b) C2 F6
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(c) CO2
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Figure 20: Bubble generation in pure water at the entrance of the tubing for three gases
with very different solubilities in water to test a potential influence of cavitation.

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[2] Brennen, C. E. (2013). Cavitation and bubble dynamics. Cambridge

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