Ultrasonics Sonochemistry 29 (2016) 420–427

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Ultrasonics Sonochemistry
journal homepage: www.elsevier.com/locate/ultson

Characterization of HIFU transducers designed for sonochemistry

application: Acoustic streaming
L. Hallez a, F. Touyeras a, J.-Y. Hihn a,⇑, Y. Bailly b
a
Institut UTINAM/SRS, UMR 6213, CNRS, University of Bourgogne Franche-Comté, Besançon, France
b
Institut FEMTO-ST/ENISYS, UMR 6174, CNRS, University of Bourgogne Franche-Comté, ENSMM, UTBM, Belfort, France

a r t i c l e i n f o a b s t r a c t

Article history: Cavitation distribution in a High Intensity Focused Ultrasound sonoreactors (HIFU) has been
Received 8 March 2014 extensively described in the recent literature, including quantification by an optical method
Received in revised form 5 October 2015 (Sonochemiluminescence SCL). The present paper provides complementary measurements through the
Accepted 27 October 2015
study of acoustic streaming generated by the same kind of HIFU transducers. To this end, results of mass
Available online 27 October 2015
transfer measurements (electrodiffusional method) were compared to optical method ones (Particle
Image Velocimetry). This last one was used in various configurations: with or without an electrode in
Keywords:
the acoustic field in order to have the same perturbation of the wave propagation. Results show that
HIFU
Acoustic streaming
the maximum velocity is not located at the focal but shifted near the transducer, and that this shift is
Hydrodynamic behavior greater for high powers. The two cavitation modes (stationary and moving bubbles) are greatly affect
Cavitation the hydrodynamic behavior of our sonoreactors: acoustic streaming and the fluid generated by bubble
Bubbles behavior motion. The results obtained by electrochemical measurements show the same low hydrodynamic activ-
ity in the transducer vicinity, the same shift of the active focal toward the transducer, and the same
absence of activity in the post-focal axial zone. The comparison with theoretical Eckart’s velocities
(acoustic streaming in non-cavitating media) confirms a very high activity at the ‘‘sonochemical focal”,
accounted for by wave distortion, which induced greater absorption coefficients. Moreover, the equiva-
lent liquid velocities are one order of magnitude larger than the ones measured by PIV, confirming the
enhancement of mass transfer by bubbles oscillation and collapse close to the surface, rather than from
a pure streaming effect.
Ó 2015 Elsevier B.V. All rights reserved.

1. Introduction synthesized under ultrasonic irradiation and selective oxidation

of pyrrole on oxydable metals.
In the first part of this study [1], we have described the cavita- Characterization of this kind of transducer is rather complex
tion distribution in a sonoreactor equipped with High Intensity due to the presence of cavitation bubbles in the acoustic field. As
Focused Ultrasound (HIFU) and quantified them with an optical predictive tools are not available for cavitation phenomenon,
method (SCL). The use of HIFU enables generation of very intense experimental studies had to be conducted to describe their specific
acoustic intensities at high frequencies, which is not possible with behavior. In a previous paper [1], the dynamics of cavitation bub-
classical flat transducers. This large density of acoustic energy had bles can be defined in two modes: ‘‘stationary bubbles” (bubbles
already paved the way for very interesting medical applications, trapped in the pressure antinodes of the standing wave) and ‘‘mov-
allowing specific innovations in therapeutics [2,3]. More recently, ing bubbles” (bubbles in motion in the acoustic field). The present
prospects have emerged in surface treatments such as selective work concerns the acoustic streaming generated by HIFU.
ablation of polymers [4], study of cavitation and hydrodynamic The flows generated by ultrasound are nearly always present in
effects on the selective stripping of acrylic coatings, selective poly- all sonoreactors, along with cavitation and other induced effects.
merization known as ‘‘acoustic masking” [5,6], or modification of Such flows are well known to enhance mass transfer in processes
compactness and ions repartition of polypyrrole coatings electro- limited by diffusion [7,8], to favor heat exchanges [9,10] or indeed
to perform mixing or micromixing [11,12]. Wave propagation in a
viscous fluid induces a transfer of energy between the acoustic
wave and the propagation media, leading to a large scale flow com-
⇑ Corresponding author.
monly called ‘‘acoustic streaming” [13]. In a non-cavitating media,
E-mail address: [email protected] (J.-Y. Hihn).

http://dx.doi.org/10.1016/j.ultsonch.2015.10.019
1350-4177/Ó 2015 Elsevier B.V. All rights reserved.
 L. Hallez et al. / Ultrasonics Sonochemistry 29 (2016) 420–427 421

two kinds of acoustic streaming can be seen: Eckart’s streaming (or electrodes; the working electrode can be located at various dis-
quartz wind), generated in the bulk by the Reynolds tensions tances from the transducer. This limiting current density can be
resulting from wave absorption in a viscous media, and Rayleigh linked to an equivalent circulation of electrolyte Ueq, able to pro-
streaming where the Reynolds tensions act on the hydrodynamic duce the same electrochemical signal in silent conditions, using
limiting layer in the vicinity of the reactor wall [14]. In cavitating equations of mass transfer and mass balance. Pollet and Hihn pro-
media (heterogeneous media), a variety of factors are involved in posed the following equation [23]:
global agitation. The present work is based on experimental mea-
1
surements using optical method (Particle Image Velocimetry) and U eq ¼ D4=3 m1=3 Relec j~jD j2lim ;
electrochemical method to describe the global agitation generated ð0:45nFC sol Þ2
by HIFU.
where m is the kinematic viscosity.
All experiments were conducted by a Tacussel PGZ 301
2. Experimental details potensiostat.

2.1. Instrumentation
3. Results and discussion
All experiments were conducted using two composite HIFUs
3.1. Velocity vector fields measured by PIV
designed by IMASONIC (Besançon, France). The first operates at
3 MHz (Tfc3000) with a 40 mm geometrical focal length, while
The PIV method was previously used in many configurations
the second operates at a frequency of 750 kHz (Tfc750) with a
with an interesting sensitivity [25,26]. Indeed the behavior of cav-
100 mm geometrical focal length. Transducers were set on the ves-
itation bubble field is dependent on many parameters such as
sel’s bottom. The geometrical focal corresponds to the center of
acoustic power, reflector nature, i.e. whether the surface facing
spherical cap of the emitting surface characterized by its radius
the transducer is free (case of a liquid without obstacle) or not
[15]. The reactor (750 mL) consists of a double walls cylindrical
(electrode surface) [4] and even on wave generation mode (contin-
Pyrex vessel (92 mm diameter) equipped with a displacement sys-
uous or pulsed). Therefore, first tests consisted in irradiating a free
tem with four degrees of freedom [1]: three translations guided by
surface, whereas in the second test, an electrode was located in the
micrometric screws and one rotation axis to avoid reflections
acoustic field (giving an opportunity to compare with electrochem-
toward the transducer.
ical measurements). It was observed that the polyamide particles
(Rilsan 30 lm diameter) used as tracers formed cavitation germs,
2.2. Operating procedures
thus leading to a decrease in cavitation threshold (reach here for
the lowest available powers instead of a few Watts in previous
In the present work, streaming velocities were measured by
works [1]. The values of the axial velocity (fluid velocity on the
two methods. Particle Image Velocimetry (PIV) is an optical visual-
acoustic axis) measured by PIV were averaged with a MATLAB
ization method dedicated to velocity measurements by determin-
post-treatment software, over a 5
5 mm2 window, centered on
ing particle displacement over time using a double-pulsed laser
the propagation axis, and sliding by steps from the vicinity of the
technique [16,17]. The liquid media was seeded by tracers, which
transducer up to the free surface.
have a density close to water (microparticles of Rilsan 30 lm). A
light sheet, generated by a laser Continuum Nd-Yag (532 nm)
and an optical system with cylindrical lenses, illuminates the 3.2. Irradiation of a free surface
acoustic axis plane. Particle locations are recorded in this plane
using a CDD camera (Sensicam PCO 12 bits, 1280
1024 pixels). The velocity vector fields obtained by PIV measurements for
A fraction of a second later, a second image of the particle was both HIFU transducers (Tfc750 and Tfc3000) for 20 W (acoustic
taken and from these two images, analysis algorithms allowed to power measured by calorimetry) are shown in Fig. 1. A conical
obtain the particle displacements for the entire flow region shape is visible in both cases, with the same global pattern as
mapped. For each experiment, 50 pairs of images were recorded the distribution of the active bubbles observed in a previous study
and post-treated using INSIGHT 3D software. [1]. Velocities reach their maximum values in the acoustic axis, and
The second method was the determination of mass transfer by a whirlpool recirculating flow is visible close to the walls in the
cyclic voltammetry using the well-known quasi reversible redox upper part of the reactor.
couple Fe(CN)3 4 The average vectors are plotted as a function of transducer dis-
6 /Fe(CN)6 . The work of Coury et al. [18–20] and
Compton et al. [21] investigated mass-transfer phenomena under tance at various powers. Fig. 2a gives the results for the Tfc750
sonication. Sonication decreases the diffusion layer thickness d transducer. Velocities increase with distance and irrespective of
power maximum values are reached of between 70 and 80 mm,
(m) and increases the limited current of diffusion j~jD j (A m2) lim slightly above the acoustic focal (90 mm), which corresponds to
attributed to the stirring effect in the reactor, its mean acoustic
the maximum cavitation activity previously observed [1,27]. After
streaming and microjets generated by bubble collapses in cavitat-
the maximum, the presence of a large number of bubbles and the
ing media. Stirring in the neighborhood of the electrode can be
divergence of the acoustic field lead to fluid decelerations. Never-
expressed by the dimensionless Sherwood number [22–24]:
theless, dependence of axial velocity on power is low, seemingly
j~jD jlim Relec reaching a kind of saturation beyond 20 W and around
Sh ¼ ; 120 mm s1. On the contrary, an increase in axial velocity vs.
nDFC sol
power is noticeable in the zone close to the transducer. For exam-
Relec = 103 m is the electrode radius, DFeðCNÞ4 ¼
6 ple, if we look at its evolution at a given distance of 20 mm from
10
ð5:60  0:21Þ  10 2 1
m s the diffusion coefficient of the species the transducer, velocity evolves from a few mm s1 at 10 W to
determined with a rotating electrode, F the Faraday constant, and more than 60 mm s1 at 40 W. Results for the Tfc3000 transducer
Csol the concentration of the species. are shown in Fig. 2b. The same global trends are observed, i.e.
Experiments were carried out with a concentration in ferri- the average value of the axial component of the velocity vectors
ferrocyanide [Fe(CN)3 4
6 ] = [Fe(CN)6 ] = 5 mM in a background salt increases as a function of distance to the horn up to a maximum
NaOH = 0.2 M. We used a classical setup with 3 platinum of between 45 and 50 mm, but located just beyond the acoustic
422 L. Hallez et al. / Ultrasonics Sonochemistry 29 (2016) 420–427

HIFU HIFU

Fig. 1. Velocity vector fields of acoustic streaming generated by HIFU (Tfc750 and Tfc3000) at 20 W.

Fig. 2a. Evolution of the axial average velocity of acoustic streaming vs. distance from the transducer for various powers (Tfc750).

Fig. 2b. Evolution of the axial average velocity of acoustic streaming vs. distance from the transducer for various powers (Tfc3000).
 L. Hallez et al. / Ultrasonics Sonochemistry 29 (2016) 420–427 423

focal (40 mm). In this case, the decrease in recorded velocities is in cavitating media, and concerns a huge bubble motion relative to
slow and velocities remain at a high value up to the reactor top. the liquid. This bubble motion appears suddenly and is triggered
This last phenomenon is certainly due to fewer and less active cav- by the loss of equilibrium between forces acting on bubbles. The
itation bubbles at this frequency. On another hand, a singular power increase affected the radiation and Bjerknes forces as well
behavior is observed for the highest power (20 W), resulting in a as the Eckart’s streaming. We can assume than the high number
sudden increase in the fluid velocity just after the acoustic focal. of bubbles which move to the top of the reactor contributes to
To understand this better, the dependence of the maximum of axial the global motion of the fluid itself, through viscous friction.
velocities on acoustic powers is plotted on Fig. 3, where we can To compare PIV results to equivalent velocities obtained by
observe a break in the curve of fluid velocities, particularly clear electrochemistry, it appears necessary to add measurements in
for the 3 MHz Tfc 3000 transducer. In this case, axial velocity presence of an obstacle (electrode).
increases regularly as a function of acoustic power up to 20 W. This
corresponds to the Eckart theory where streaming is proportional 3.3. Presence of an obstacle in the acoustic field (Pt-PTFE electrode)
to acoustic intensity. Beyond this power, a steep increase is
observed, related to the sudden bubble motion: these are bubbles Fig. 4 shows velocity vector fields obtained by PIV measure-
that were trapped in the pressure antinodes of the standing wave ments for both HIFU transducers (Tfc750 and Tfc3000) at 20 W
at low powers. Nevertheless, the power threshold value is difficult when an electrode is located at the acoustic focal. Far from pre-
to determine with accuracy due to its randomness. As a germina- venting liquid circulation, an intense activity is noticeable in the
tion phenomenon, water purity (bear in mind tracer presence) or electrode vicinity, directly in the zone facing the transducer and
shocks on the vessels can trigger irreversibly the global fluid all along the electrode body. In all cases, the presence of the elec-
motion. Once this phenomenon is activated, this additional contri- trode leads to a major perturbation.
bution to the convection flow (Eckart streaming) is rapidly satu- The agitation generated close to the electrode is the most
rated for the higher powers. important phenomenon, because it is directly linked to the mass
In the case of Tfc 750, the same behavior is observed but at transfer measurements, which will be undertaken later on. The
lower powers (2 W) and most of the time is hardly noticeable. This average velocities (normal and tangential components of the vec-
was expected because cavitation occurs sooner at low frequencies. tor fields) are calculated in a zone (5
5 mm2) in the vicinity of
Then, for higher powers (beyond 2 W), velocities are no longer the electrode, and plotted as a function of the location of the elec-
dependent on power and the curve reaches a plateau, which illus- trode in the reactor (moving from the transducer to the free surface
trates saturation. on the acoustic axis). Results are shown in Fig. 5a (Tfc750) and
These results go hand in hand with observation of bubble Fig. 5b (Tfc3000). As previously observed without an obstacle for
dynamics in an acoustic field: at low powers, bubbles are in levita- the Tfc 750 transducer, the maximum values for tangential and
tion in the standing wave at pressure antinodes, whereas they start normal velocity are reached when the electrode is located at the
to move at higher powers [1,15]. It is clear that two factors of focal (around 90 mm from the transducer). For the Tfc 3000, the
hydrodynamic agitation (motion of fluid itself relative to the ves- maximum values are also found at the focal (around 40 mm from
sel) exist. The first, in the stationary bubble mode or in cavitation the transducer), which was not the case in electrode absence. At
less conditions, corresponds to the convective flow described by 750 kHz, cavitation activity is intense and bubbles act as a reflec-
Eckart equations. We recall that this flow is directed following tor, ever for low powers, and the electrode will not introduce any
the wave propagation axis and results from energy transfer changes. Although this is not systematically the case at higher fre-
between the acoustic wave and the propagation media through quencies, the electrode will reflect the waves, introducing a
presence of viscous forces. Even if bubbles can move relatively to marked change in the cavitation field and inducing an increase in
the liquid in an oscillating mode, which can therefore be pushed stirring. It seems that electrode presence tends to displace the
back and forth by the bubbles [28], the liquid itself is only con- maximum velocities in the direction of the transducer, a type of
cerned by a very little average motion. The second is observed only behavior already observed for bubble distribution by luminol mea-
surements in HIFU [1].
The higher velocities observed at 750 kHz than at 3 MHz attract
our attention. Indeed, Eckart’s theory predicts a velocity 16 times
lower for a frequency 4 times lower, as the absorption coefficient
is propositional to the square of frequency [13,29]. This discrep-
ancy can be attributed to a huge modification of the absorption
coefficient due to the presence of bubbles, which are numerous
at lower frequencies.
To conclude, the values of acoustic winds measured by PIV in
the present work are within the range of magnitude as previously
measured in the case of low frequency plane transducers [25], i.e. a
few cm s1, but with a distribution specific to HIFU geometries.

3.4. Electrochemical measurement: mass transfer and expression of an

equivalent velocity

3.4.1. Mass transfer measurement

This measurement helps us to understand the influence of local
agitation at the electrode surface, yielding quantitative informa-
tion on bubble dynamics and flow circulation. Fig. 6 shows the evo-
lution of the cathodic current vs potential decrease (linear sweep
Fig. 3. Evolution of the axial maximum velocity of acoustic streaming vs. distance
voltammetry) by positioning the working electrode in the propaga-
from the transducer for various powers (Tfc750 and Tfc3000): detection of the tion axis of the Tfc750. Ultrasound and voltammetry start simulta-
cavitation mode. neously. Firstly, current increases with potential (0–0.05 V/Pt)
424 L. Hallez et al. / Ultrasonics Sonochemistry 29 (2016) 420–427

HIFU
HIFU

Fig. 4. Velocity vector fields of acoustic streaming in presence of an electrode located at the acoustic focal (Tfc750: 10 W; Tfc3000: 20 W).

Fig. 5a. Average normal and tangential velocity components in the reactor axis determined by PIV in presence of an electrode at various distances from the emitting surface
(Tf750:10 W).

corresponding to the limitation by electron transfer kinetics, before chemical measurement, thus it is possible to switch from the sta-
a slowdown attributed to the limitation by mass transfer as already tionary cavitation mode to the motion of cavitation bubbles
observed in many cases for this kind of technique [23,24]. Usually mode. It can occur at any value of the potential. It is well known
for reversible electrochemical systems, the current reaches a pla- at low frequencies (20–60 kHz) that mass-transfer limited currents
teau proportional to agitation. It is interesting to note that, after under ultrasonic agitation included a steady state and time-
about 30 s where stationary cavitation bubbles appear (corre- dependent component (oscillating around the average plateau cur-
sponding to 0.09 V/Pt at 150 mV min1 scan rate), the current rent value) [18,19,23,25]. These peaks are more difficult to observe
increases slightly. This contribution to agitation is the result of at high frequencies, because cavitation is usually less violent [30].
the motion of bubbles around their average position, in equilib- Moreover, this leads some authors to prefer high frequencies as
rium in the pressure antinode of the acoustic wave. On the con- mechanical effects are reduced [5,6], while chemical effects remain
trary, in a random manner or triggered by an external event at high levels [31]. HIFU therefore ensures a broader range of mag-
(impact on the vessel, electrode motion in the field, etc.), the nitude of bubble dynamics, from stationary bubbles (available only
strength maintaining the bubbles in equilibrium is broken and a at high frequencies) to moving bubbles with very high velocities
large flow is directed toward the electrode. This phenomenon is (possible in both HIFU and low frequencies) [1]
similar to what observed by PIV (Fig. 3). This corresponds to a glo-
bal bubble motion leading to a significant increase in current aver- 3.4.2. Distribution of the Sherwood number in the sonoreactor
age level (global convective flow) and to current spikes indicating This operating mode with stationary bubbles is interesting, as it
that a strong cavitation event has occurred. The transition between may be useful for several applications where the destructive effects
the two modes of cavitation is totally independent of the electro- of cavitation must be avoided. Agitation was systematically
 L. Hallez et al. / Ultrasonics Sonochemistry 29 (2016) 420–427 425

Fig. 5b. Average normal and tangential velocity components in the reactor axis determined by PIV in presence of an electrode at various distances from the emitting surface
(Tf3000: 20 W).

Fig. 6. Voltammetry study of different cavitation modes (5 W).

mapped by moving the working electrode into the acoustic field in detail in the comparison between equivalent velocities and Eck-
a plane containing the acoustic axis (distribution of agitation in our art’s theoretical velocities.
cylindrical reactor was considered as axisymmetric). All experi-
ments were conducted with great care to prevent bubble motion, 3.4.3. Equivalent velocity
i.e. 10 W and ultrapure water. Fig. 7 shows the evolution of the agi- To simplify the comparison between theoretical and experi-
tation level in the Tfc750 field expressed in Sherwood numbers mental values, previous results were expressed in equivalent
versus longitudinal and axial directions. This allows to map the velocities (Fig. 8). Theoretical Eckart’s velocities U were calculated
complete reactor volume facing the transducer. Sherwood num- from the modeling [13,29] with the acoustic intensity distribution
bers were calculated with the value of the limited current density calculated in a previous work [1] with the Rayleigh’s integral
j~
jD j
lim obtained with mass transfer measurement. The stirring (Ultrasim module of Matlab developed at the University of Oslo).
effects are distributed with the same global shape as predicted This equation contains a geometrical factor G(r) dependent on
by the previous method, and maximum agitation is observed the acoustic beam Rb and the vessel (Rv = 46mm) radii. The absorp-
before the acoustic focal just as for the PIV measurements. More tion coefficient is estimated experimentally.
original is the experimental detection of the marked agitation
decrease at 60 mm from the transducer on the propagation axis, aIa r2t
U¼ GðrÞ
due to destructive interferences. This point will be described in gc
426 L. Hallez et al. / Ultrasonics Sonochemistry 29 (2016) 420–427

Fig. 7. Mapping of the distribution of Sherwood number on a half-plane adjacent to the transducer acoustic axis (Tfc750: 10 W).

Fig. 8. Comparison between the equivalent velocity determined by electrochemistry and the theoretical Eckart’s velocity at the stationary cavitation mode (Tfc750: 10 W).

With tion of simulated velocities fit surprisingly well with the experi-
      
2 R2 2 mental equivalent ones in the propagation axis; in particular, the
GðrÞ ¼ 12 1  Rr 2  1  2Rb2 1  Rr 2  log RRvb for 0 6 r 6 Rt
b v v presence of the destructive interferences predicted by theory is
     
R2 2 experimentally confirmed. On another hand, the experimental
And GðrÞ ¼ 1  2Rb2 1  Rr 2  log Rrv for Rt 6 r 6 Rv
v v maximum velocity is shifted toward the transducer. This has been
The acoustic beam radius is calculated as a function of z already observed in a previous work ([1] – Fig. 12a), where the
(distance of a point on the acoustic axis to the transducer’s center) light emitted by sonochemiluminescence SCL was recorded at dif-
and r = 0 (on the acoustic axis). ferent locations in the reactor. The highest SCL values were
Fig. 8 shows that close to the transducer, the effects of ultra- obtained in a zone centered on 73 mm of the emitting surface,
sound are not significant, and a noticeable velocity can be detected slightly upstream from the acoustic focal (we had named this zone:
only beyond 20 mm from the transducer. A marked decrease then the sonochemical focal). For powers upper than 10 W, there is an
occurs at 60 mm, resulting from the destructive interferences due absence of SCL at the focal and in the post-focal zone, immediately
to the phase shift between each transducer component. Beyond downstream from the focal. Our first assumptions were that the
this point, it then increases again up to a maximum at the acoustic high concentration of bubbles in this zone would favor interactions
focal. Equivalent velocities were calculated from electrochemical between them, such as coalescence or clustering in the case of sta-
measurements and plotted vs transducer to electrode distance. tionary cavitation, or, on the contrary, when they reach high
Both curves present the same global pattern in the prefocal zone speeds in a viscous fluid, that their deformation would induce
(0–70 mm from the transducer). It is important to note that asymmetric collapses. Some authors [32] have recently shown that
velocity calculated from Eckart’s equation are strongly dependant gentle additional agitation in the cavitation field minimizes this
of the absorption coefficient (not easy to evaluate in presence of quenching. This tends to prove that SCL absence at the focal is
cavitation), and therefore should be considered cautiously from linked to clustering or coalescence of bubbles. In fact, this cloud
the point of view of their absolute values. Nevertheless, the evolu- of bubbles directly at the focal is a possible reason for the shift
 L. Hallez et al. / Ultrasonics Sonochemistry 29 (2016) 420–427 427

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