Journal of Environmental Chemical Engineering 9 (2021) 106555

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Journal of Environmental Chemical Engineering

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A full mechanistic and kinetics analysis of carbon tetrachloride (CCl4)

sono-conversion: Liquid temperature effect
Aissa Dehane a, Slimane Merouani b, Oualid Hamdaoui c, Magda H. Abdellattif d,
Byong-Hun Jeon e, Yacine Benguerba f, *, 1
a
Laboratory of Environmental Engineering, Department of Process Engineering, Faculty of Engineering, Badji Mokhtar – Annaba University, P.O. Box 12, 23000 Annaba,
Algeria
b
Laboratory of Environmental Process Engineering, Department of Chemical Engineering, Faculty of Process Engineering, University Salah Boubnider-Constantine 3, P.O.
Box 72, 25000 Constantine, Algeria
c
Chemical Engineering Department, College of Engineering, King Saud University, P.O. Box 800, 11421 Riyadh, Saudi Arabia
d
Department of Chemistry, College of Science, Taif University, PO Box 11099, Taif 21944, Saudi Arabia
e
Department of Earth Resources and Environmental Engineering, Hanyang University, Seoul 04763, Republic of Korea
f
Laboratoire des Matériaux Polymères Multiphasiques (LMPMP), University Ferhat Abbas Setif1, Setif, Algeria

A R T I C L E I N F O A B S T R A C T

Editor: Dr. GL Dotto In this study, a model of CCl4 sono-pyrolysis inside an acoustic bubble is used to provide a novel mechanistic and
kinetics study of CCl4 conversion. The impact of fluid temperature (10–50 ◦ C) on CCl4 conversion and the
Keywords: resulted products is illustrated for various aqueous CCl4 concentrations and acoustic intensities (0.7–1.5 W/cm2).
Sonochemistry With a concentration less than 3 × 10− 3 M, 1 W/cm2 is sufficient for the complete degradation of CCl4 at 20 ◦ C.
Carbon tetrachloride
However, at 10 ◦ C, 1.5 W/cm2 is much than enough to degrade CCl4 completely, regardless of its concentration
Liquid temperature
in solution. The generation of reactive chlorine species (RCS) increased proportionately with the temperature rise
OH radicals
Reactive chlorine species when the intensity was 0.7 W/cm2. In contrast, between 1 and 1.5 W/cm2, increasing the liquid temperature
from 10◦ to 40 ◦ C has a beneficial effect on the sonolytic activity of the cavity. However, this positive impact
continues to be observed only for⋅OH radicals when the bulk liquid temperature is greater than 40 ◦ C (the yield of
RCS, H⋅, HCl, and HOCl is amortized). According to the simulation results, it was concluded that the rapid sono-
degradation of nonvolatile pollutants in the presence of CCl4 was mainly due to the RCS and⋅OH radicals
generated at the efficient bubble collapse.

subsequent chemical reactions and produce light [17,18]. Furthermore,

1. Introduction the interaction on the bubble-solution interface or in bulk with hydroxy
radicals is most likely to remove hydrophilic/hydrophobic pollutants
Bescause of its devastating health effects on the liver, kidneys, brain, [19–22]. The pyrolysis of volatile pollutants such as CCl4, CHCl3, and
and lungs, CCl4 is one of the most hazardous organic pollutants found in benzene is mainly occurred in the bubble interior (gas phase) [11,12,
nature [1,2]. UV photolysis [3], photocatalytic degradation [4], modi­ 23–25]. However, the degradation rate is too slow to use in real appli­
fied Fenton’s reagent [5], and the thermally activated persulfate system cations, particularly for nonvolatile species [26]. CCl4 has, on the other
[6,7] have all been used to treat aqueous-phase CCl4. Sonolysis of CCl4 hand, been effectively used as a hydrogen atom scavenger to accelerate
was also applied as a promoter for the effective removal of this chemical the sonochemical degradation of nonvolatile organic contaminants in an
[8–14]. aqueous solution [27–30]. The frequency, acoustic intensity, liquid
The formed acoustic cavitation grows and collapses violently when a temperature, solution pH, and other experimental factors that impact
solution is sonicated [15]. As a result, at collapse, tremendous pressures CCl4 breakdown were studied in these studies.
(1000 atm) and temperatures (5000 K) are created within the bubble An increase in the temperature of the liquid adversely affects the
"hot spot" [16]. Within the bubble, steam and non-condensable gas temperature of bubbles because vapor penetrates bubbles during the
create a variety of radicals and reactive species that can initiate rarefaction phase, causing the bubble collapse to be cushioned (and

* Corresponding author.
E-mail addresses: [email protected], [email protected] (Y. Benguerba).
1
https://orcid.org/0000-0002-8251-9724

https://doi.org/10.1016/j.jece.2021.106555
Received 9 August 2021; Received in revised form 1 October 2021; Accepted 7 October 2021
Available online 14 October 2021
2213-3437/© 2021 Elsevier Ltd. All rights reserved.
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

Nomenclature Tmax Maximum temperature inside a bubble, (K).

T∞ Bulk liquid temperature, (K).
Af (Ar) Pre-exponential factor of the forward (reverse) reaction, x Thermal diffusivity inside the bubble (m2/s)
[(cm3 mol− 1 s− 1) for two body reaction and (cm6 mol− 2 Cp Heat capacity concentration inside the bubble (J/m3 K)
s− 1) for three body reaction]. MH2O Molar mass of water (Kg/mol).
bf (br) Temperature exponent of the forward (reverse) reaction. ṁ Evaporation-condensation rate of water (Kg/m2 s).
c Speed of sound in the liquid medium, (m s− 1). Q Energy transferred by heat exchange (J/s)
Eaf (Ear) Activation energy of the forward (reverse) reaction, (cal n Molar amount (mol).
mol− 1). PB Liquid pressure on the external side of the bubble wall. (Pa)
f Frequency of ultrasonic wave, (Hz). V Volume of the bubble (m3)
Ia Acoustic intensity of ultrasonic irradiation, (W m− 2).
kf (kr) Forward (reverse) reaction constant, [(cm3 mol− 1 s− 1) for Greek letters
two body reaction and (cm6 mol− 2 s− 1) for three body σ Surface tension of liquid water, (N m− 1).
reaction]. ρl Density of liquid water, (kg m− 3).
p Pressure inside a bubble, (Pa). ρg Density inside the bubble (kg m− 3).
pmax Maximum pressure inside a bubble (Pa). λmix Thermal conductivity of the mixture(W m− 1 K).
p∞ Ambient static pressure, (Pa). λi Thermal conductivity of species i (W m− 1 K).
PA Amplitude of the acoustic pressure, (Pa). μ Dynamic viscosity (Pa s).
Pv Vapor pressure of water, (Pa). α Accommodation coefficient.
R Radius of the bubble, (m). ρH2o Density of water vapor inside the bubble (Kg/m3).
Rmax Maximum radius of the bubble, (m). ρsat,H2o Saturated vapor density (Kg/m3).
R0 Ambient bubble radius, (m). υki Stoichiometric coefficient of the kth chemical species in the
Rg Ideal gas constant (J/mol K). ith reaction.
t Time, (s). U̇k Production rate of the kth species (mol/s m3).
T Temperature inside a bubble, (K).

sonochemical activity). Various behaviors are reported in the literature. CCl4 sono-pyrolysis and their relationship to liquid temperature and
These behaviors depend on the experimental conditions and character­ CCl4 concentration, and (iii) the process of improving the degradation of
istics of many species present in the solution. Merouani et al. [31] non-evolves by the sono-decomposition of CCl4.
measured the rate of triiodide production at four temperatures at
300 kHz: 25, 35, 45, and 55 ◦ C. They found that increasing the tem­ 2. Model and computational procedures
perature marginally affects the sonochemical yield of triiodide (i.e., the
chemical efficiency decreases by 20% with a temperature increase from It should be noted that there is just one bubble cavitation investi­
25◦ to 55◦ C). In addition, Weissler et al. [8] found that raising the fluid gated here, which excludes the numerous interactions between bubbles
temperature between 2 and 60 ◦ C affects CCl4 elimination at 1 MHz in the sonicated fluid. All simulations have been performed using argon-
(especially at temperatures over 40 ◦ C). Rajan et al. [32] at 25 kHz and saturated water with different CCl4 levels, resulting in an initial content
Wu et al. [33] at 20 kHz in the range of 20–60 ◦ C, as well as Spurlock of bubbles that combine these three species. Heat transport and liquid-
et al. [13] from 20◦ to 41◦ C, have made similar observations. Lim et al. vapor evaporation across the bubble/fluid interface and the heats of
[23] discovered that when the temperature rises from 10◦ to 40◦ C, the the chemical reaction are considered in the formulation of the bubble
degradation of CCl4 at 20 kHz decreases. Destaillats et al. [34], on the dynamics model. It is not taken into account that the bubble interface
other hand, discovered that the breakdown of trichloroethylene in­ CCl4 evaporation and condensation take place. Since they are less sol­
creases as the liquid temperature rises from 5◦ to 30◦ C, when the ul­ uble (5.2 ×10− 3 M at 20 ◦ C) and more volatile (91 mmHg at 20 ◦ C), CCl4
trasonic frequency used is 500 kHz (2 W/cm2). Over a temperature molecules are primarily present in the bubble at time zero (t = 0).
range of 6–19.4 ◦ C (20 kHz), Gaddam et al. [35] discovered an optimal Henry’s law was applied to determine the vapor pressure of CCl4 within
temperature of 14.2 ◦ C for 1,1,1 trichloroethane conversion. Sehgal the bubble.
et al. [36] showed that the rate of Thymine conversion increases from The mathematical model we used is based on the following modified
20◦ to 30◦ C, then goes through a horizontal temperature plateau from Keller-Miksis equation [37]:
30◦ to 55◦ C, before decreasing by raising the solution temperature to ( ) ( )
60 ◦ C. All of these results confirmed the complicated effect of liquid 1−
Ṙ
+
ṁ 3 2
RR̈ + Ṙ 1 −
Ṙ
+
2ṁ
temperature on the sonochemical degradation of volatile contaminants C C ρL 2 3C 3CρL
due to the various parameters influenced by the bulk liquid temperature ( )[ ( ( )) ] ( )
1 Ṙ R m̈R Ṙ ṁ
(viscosity, solubility of gases, surface tension, and vapor pressures) or = 1+ PB (t) − PA sin 2πf t + − P∞ + 1− +
ρL C C ρL C CρL
those modifying the temperature effect (e.g., frequency and intensity). ( )
Herein, using a novel model of ultrasonic decomposition of CCl4 in ṁ ṁ Ṙ ṁ R dPB
+ Ṙ + + +
aqueous solution (10− 3 M), the influence of bulk liquid temperature ρL 2ρL 2CρL CρL dt
(from 10◦ to 50◦ C) on the conversion of CCl4 is illustrated for concen­
(1)
trations of 0–5.2 mM. The effect of liquid temperature on CCl4 decom­
position products, bubble temperature, and dynamics is also thoroughly Where t, R, Ṙ, R̈, C, ρL, PB(t), PA f, P∞, are, respectively, the oscillation
discussed. All of these processes are investigated using a single bubble time, the bubble radius, the bubble wall velocity, the bubble wall ac­
sonochemistry model with a 355 kHz wave frequency. Three acoustic celeration, the sound speed in the water, the liquid pressure at the liquid
intensities, i.e., 0.7, 1, and 1.5 W/cm2, were used. The results obtained shell of the bubble, the ultrasonic amplitude, the wave frequency, and
disprove several conflicting literature findings, including (i) the impact the static pressure. PA= (2IaρLC)1/2 is the relationship between PA and
on CCl4 degradation of the liquid temperature, (ii) the main products of acoustic intensity Ia (or power per unit area). The external liquid

2
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

pressure PB(t) on the bubble wall is correlated to the internal pressure P

λmix
(t) as [38]: χ= (13)
Cp
2σ 4μṘ
PB (t) = P(t) − − (2) The heat capacity is given by the following equation [43]:
R R
∑fi + 2
Where σ and µ are the surface tension and the viscosity of liquid water, Cp = kB Ci NA (14)
2
respectively. To calculate P(t), the van der Waals equation is utilized:
The temperature (T) within the bubble may be estimated using the
nRg T an2 equation below [46]:
P(t) = + (3)
(V − nb) V 2 ( )
2
E + anV
With ’a’ and ’b’ are given as [38]:
T= (15)
⎧ ( ) ( ) ( ) ⎫ Cv nt
⎪
⎪ nH2 O nAr nCCl4 ⎪
⎪
⎨ &a = aH2 O nt
⎪ + aAr
nt
+ aCCl4
nt
⎪
⎬ The bubble’s internal energy change (ΔE) over time (Δt) accounts PV-
( ) ( ) ( ) (4) work, bubble chemical reaction heat, condensation/evaporation of
⎪
⎪ n n n ⎪
⎪
⎪ ⎪ water, and heat exchange through diffusion [47]:
H 2 O Ar CCl 4
⎩ &b = bH2 O + bAr + bCCl4 ⎭
nt nt nt
( )
Ṁ Tliq − T
where ’a’ and ‘b’ parameters of each species (H2O, CCl4, and Ar) are ΔE = − P(t).ΔV(t) + 4πR2 Δt
MH2 O
eH2O + 4π R2 Δtλ
Lth
available in [39]. (16)
4 3 ∑n
The Hertz-Knudsen formula is used to calculate the interfacial flow of − πR Δt i=1 ΔHi ri
3
evaporated and condensed water [40]:
{Psat [R] − Pv } eH2O = Cv,H2OT (17)
ṁ = α √̅̅̅̅̅̅̅̅̅̅̅̅ (5)
Table S1 (see supplementary data) consists of nineteen chemical
2π T[R] Rg
MH2 O
kinetic reactions and reverse reactions. The kinetic model is used for a
Psat [R], Pv : the water vapor saturated pressure, calculated at T[R] bubble initially containing CCl4, argon, and steam.
= Tliq, and the vapor pressure inside the bubble, respectively. The co­ The chemical reaction rate is defined as follows:
efficient of accommodation α is given as a function of the liquid tem­
∑K ∑K ′′ X
perature at the bubble wall (considered constant= Tliq) (Eq. (6)) [41]. ′
υ Xk ↔ υ
ki k
(18)
k=1 ki
Generally, this liquid is water, but even when another liquid is used (e.
k=1

g., methanol), α is considered the same for the reason of simplification as The rate of production U̇k is given as:
it was indicated by Yasui [42]:

⎧ ⎫
⎪
⎪
α= 0.35, for Tliq ≤ 350 K ⎪
⎪
⎪
⎪ ⎪
⎪
⎨ ( )2 ( )( )⎪
⎪
⎬(T )
Tliq Tliq Tliq
(6)
liq
α = 0.35 − 0.05 − 7 + 0.025 − 7 − 8 − 9 , for 350 ≤ Tliq ≤ 500K
⎪
⎪ 50 50 50 ⎪
⎪ 50
⎪
⎪ ⎪
⎪
⎪
⎩ ⎪
⎭
α= 0.05, for Tliq ≥ 500 K (6)

1 dnk ∑I
U̇ k = (υ′ ′ki − υ′ki )ri k = 1, …, K (19)
The heat exchange within and out of the bubble is calculated as [43]: V dt i=1

( )
Tliq − T with
Q̇ = 4π R2 λmix (7)
Lth ∏K υ′ki ∏K υ′ ′ki
ri = k f i [Xk ] − kr i [Xk ] (20)
{ √̅̅̅̅̅̅ } k=1 k=1
R Rχ
Lth = min , (8) and
π Q̇
( )
Ea fi
λmix, is calculated using the equation [44]: kf i = Af i T bf i exp − (21)
Rg T
( ) ( ) ( )
n H2 O nAr nCCl4
λmix = λH2 O (T) + λAr (T) + λCCl4 (T) (9) (
Eari
)
nt nt nt kr i = Ar i T bri exp − (22)
Rg T
The thermal conductivities are given by [38,45]:
The kinetic parameters are given in Tables S1 and S2 (see supple­
λH2 O (T) = 9.967213 10− 5 T − 1.1705 10− 2
(10) mentary data). The change in the water vapor quantity within the
bubble is given by:
λAr (T) = 3.5887 10− 5 T + 6.81277 10− 3
(11)
Ṁ
nH2 O (t + Δt) = nH2 O (t) + 4πR2 Δt + VΔtU̇ H2 O (23)
λCCl4 (T) = 3 10− 5 T + 2.2 10− 3
(12) MH2O
Except for Ar, the amount of each other species is given by:
and

3
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

nk (t + Δt) = nk (t) + VΔtU̇ k (24) employed. The FD integration method has been used by many re­
searchers in sonoluminescence and sonochemistry [48–52] due to its
Eq. (1) could be reduced in two first-order differential equations as high stability and robustness instead of the fourth-order Runge-Kutta
follows: (RK-4) method with adaptive step control. Dynamic bubble simulations
dR were performed under the same conditions as those used in the work of
= Ṙ (25) Kerboua et al. [53] to demonstrate the robustness and accuracy of the FD
dt

⎧ ( )[ ( ( )) ] ( ) ⎫
⎪
⎪ 1 Ṙ R m̈R Ṙ ṁ ⎪
⎪
⎪
⎪ 1+ PB (t) − PA sin 2πf t + − P∞ + 1− + + ⎪
⎪
⎪
⎨ ρL C C ρL C CρL ⎪
⎬
( ) ( )
⎪
⎪ ṁ ṁ ⎪
⎪
⎪
⎪ Ṙ ṁ R dPB 3 2 Ṙ 2ṁ ⎪
⎪
⎪
⎩ Ṙ + + + − Ṙ 1 − + ⎪
⎭
dṘ ρ L 2ρL 2CρL CρL dt 2 3C 3CρL
= ( ) (26)
dt
1 − CṘ + C ṁ ρ R
L

method. Their acoustic cavitation problem was solved using the RK-4
approach, utilizing almost the same phenomenological terms as our
For solving the set of differential Eqs. (15), (16), (19), (23), (24), model. Comparison of our results with those of Kerboua et al. [53] is
(25), and (26), the finite difference approach (more exactly forward shown in Fig. S3(a-c) in the supplemental material. As can be observed,
finite difference (FD) method with a fixed time step (i.e., 10− 10 s) is the development of our bubble dynamics is quite similar to that obtained

Fig. 1. Evolution of the bubble radius as function of time at around the maximum (Rmax) and the minimum (Rmin) bubble sizes for an acoustic intensity of 0.7 W/cm2
at liquid temperatures of 10 ◦ C [(a) and (b)] and 50 ◦ C [(c) and (d)]. The wave frequency is 355 kHz and the ambient bubble size is 3.2 µm.

4
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

Fig. 2. Evolution of the bubble radius as function of time at around the maximum (Rmax) and the minimum (Rmin) bubble sizes for an acoustic intensity of 1.5 W/cm2
at liquid temperatures of 10 ◦ C [(a) and (b)] and 50 ◦ C [(c) and (d)]. The wave frequency is 355 kHz and the ambient bubble size is 3.2 µm.

by the Kerboua et al. [53] model (using the Runge-Kutta technique) at sonochemistry and sonoluminescence fields [42,56,57]. Therefore, in
frequencies of 200, 300, and 500 kHz, respectively. Meanwhile, a the present paper, we use a mean value of ambient bubble radius
description of how well our entire numerical modeling approach per­ (3.2 µm) corresponding to an ultrasound frequency of 355 kHz, as
formed has been given in Text S1 of the Supplementary material, where demonstrated experimentally by Brotchie et al. [55]. Thus, the obtained
the model validation procedure is described in more detail. results in Figs. 1 and 2 give a good description of the real behavior
observed for the whole range of ambient bubble radii under a wave
3. Results and discussions frequency of 355 kHz (in the presence or absence of CCl4). Furthermore,
the solubility of CCl4 at liquid temperatures of 10–50 ◦ C is reported to be
All numerical simulations were carried out at a 355 kHz ultrasonic approximately 5.2 × 10− 3 M [58]. As a consequence, the CCl4 concen­
frequency. The acoustic intensity and liquid temperature were adjusted tration will vary from 0 to 5.2 × 10− 3 M to cover the range of concen­
to range from 0.7 to 1.5 W/cm2 and 10–50 ◦ C, respectively. The findings trations used in the various researches [9,12,25,28,32,59–61].
of numerous tests dealing with CCL4 degradation in the range of
300–800 kHz for maximal CCl4 conversion confirm this optimum fre­
3.1. Chemical mechanism
quency (355 kHz) [9,10,12,54]. However, in our study, we have focused
on the results of Lim et al. [9] whose found an optimum frequency of
When the bubble collapses, the chemical reaction becomes more
300 kHz for the degradation of CCl4 over a range of tested frequencies (i.
complex due to the presence of CCl4. The saturating gas has a further
e., 35–1000 kHz). We selected an operating frequency of 355 kHz
impact on its complexity. The selected reaction scheme (see Table S2 in
because of the availability of the experimental value of the ambient
the supplemental material) is entirely based on published experimental
bubble radius (R0), 3.2 µm [55], for this frequency. It should be noted
data. The chemical processes involving CCl4 and its derivatives have
that the bubbles population in the bulk solution is a range of active
been partially verified by shock-tube studies [62,63], RF thermal plasma
acoustic cavities rather than a fixed value. Nevertheless, to facilitate the
reactor tests [64,65], and discharge flow/resonance fluorescence in­
treatment of this population, we generally consider a mean value of
vestigations [66]. It should be noted that the contribution of electrons
bubbles radii, which represents a sample of all the population of bubbles
and electron transfer (if it is found) in bubble sonochemistry is neglected
radii existing in determining operational conditions (frequency, acoustic
according to the several theoretical works [67–69], whereas this is not
intensity, liquid temperature, etc.). This approach is the most adopted in
the case for bubble sonoluminescence, where harsher conditions of

5
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

temperature and pressure are attained within the bubble (see [70,71]).
Twelve more chemical reactions are triggered when CCl4 is intro­
duced into the argon bubble. The thermal dissociation, or pyrolysis, of
CCl4, is the first and most important process, which is thought faster
than the steam pyrolysis when bond energies are taken into account:
Cl–CCl3 has a bond energy of 288 kJ/mol, while H–OH has a bond en­
ergy of 497 kJ/mol. CCl4 is also believed to be an excellent hydrogen
atom scavenger [28,72], with k22 = 3.8 × 107 M− 1 s− 1 as the
second-order rate constant [58]. CCl4 has no interaction with⋅OH radi­
cals. This is confirmed especially by the work of Wang et al. [28], where
the increase of hydroxyterephthalate acid, i.e., a fluorescent molecule
resulting from the reaction of⋅OH radicals with terephthalic acid, for­
mation is found to be proportional to the amount of CCl4 added to the
solution and the time of sonocation. The addition of too much alcohol
does not influence the CCl4 rate of degradation and the⋅Cl formation,
according to Pétrier et al. [12]. However, the sonolysis of levofloxacin
[29] and p-nitrophenol [28] was prevented by adding t-butanol and
ethanol to the solution (<10 [CCl4]0). CCl4 is far more volatile than
alcohol molecules, which react with hydroxyl radicals inside the bubble.
The phenol hydroxylation leads to a significant increase in hydroqui­
none levels, validating the CCl4’s role as an⋅OH radical promoter [72].
During CCl4 sonolysis, hexachloroethane (C2Cl6) was shown to be
generated at a higher rate than tetrachloroethane (C2Cl4) [11,73]. The
trichloromethyl radical produces C2Cl6 due to its self-reaction (Reaction
16 of Table S2, see supplementary data). Due to the breakdown of tri­
chloromethyl radicals, dichlorocarbene (:CCl2) is detected after dis­
solving argon in the aqueous solution (Reaction 15 Table S2, see
supplemental data) [11]. The cleavage of hexachloroethane (Reactions
18–20 and 24 in Table S2, see supplementary data) generates tetra­
chloroethylene rather than the undesirable dichlorocarbene. Chlorine
radicals may recombine to form molecular chlorine (reaction 17 of
Table S2, see supplementary data). The primary sources of hypochlorous
and hydrochloric acids generation are reactions 21, 23, and 25 in
Table S2 (see supplemental data). In addition, it should be noted that the
production of Cl- during the breakdown of CCl4 (or chloroform, as in
[25]) is not always due to the attack of electrons on CCl4. In light of the
substantial quantities of HCl produced within and outside of the bubble
(Table S2) and the fact that (⋅Cl+H2O ⇌ HCl+⋅OH), a large amount of
Cl– is anticipated to be present in solution, as shown in Refs. [11,54,73],
as well as the findings of our earlier work [74].
Fig. 3. Effect of the liquid temperature (10–50 ◦ C) on the maximum bubble
3.2. Bubble dynamics as a function of CCl4 concentration and liquid temperature (i.e., attained at Rmin) as function of the concentration of CCl4 in
temperature the bulk liquid (0, 1 ×10− 5, 1 ×10− 4, 1 ×10− 3, 3 ×10− 3 and 5.2 ×10− 3 M), for
three acoustic intensities: (a) 0.7 W/cm2, (b) 1 W/cm2 and (c) 1.5 W/cm2.
The effect of CCl4 (5.2 ×10− 3 M) on the dynamic of the bubble radius
at around Rmax and Rmin bubble sizes is shown in Figs. 1 and 2 for two according to Yasui [44]. The Yasui’s effect occurs when the liquid
acoustic intensities, 0.7 and 1.5 W/cm2, respectively. The presence of temperature rises from 20◦ to 34◦ C while keeping the frequency con­
CCl4 in the bulk liquid reduces the expansion ratio (Rmax/R0) regardless stant at 20 kHz. Fig. 1(a,c) and 2(a,c) further show that when the
of the ambient temperature (10 or 50 ◦ C), as seen in Fig. 1(a,c) and 2(a, acoustic intensity rises from 0.7 to 1.5 W/cm2, the expansion ratio rises
c). This is because there is CCl4 within the cavitation, which prevents by 40% when the liquid temperature is fixed (10 or 50 ◦ C). This is true
additional vapor from entering the bubble during the rarefaction phase. for both CCl4 concentrations: 0 or 5.2 × 10− 3 M. As the acoustic power
This impact, however, is deemed insignificant since the expansion ratio increases from 0.7 to 1.5 W/cm2, more water evaporates into the bubble
drop for all treated instances is less than 0.35%. This effect is observed during the expansion phase than when the acoustic power was lower
even though CCl4 has a higher saturation pressure than water. The lower (0.7 W/cm2).
concentration of CCl4 can explain this in the bulk liquid (5.2 ×10− 3 M), In Fig. 1(b), the bubble compression ratio (Rmax/Rmin) is increased by
which suggests a lower beginning percentage of CCl4 within the bubble 2.3% when there’s CCl4 present at 10 ◦ C and 0.7 W/cm2 compared to an
(~0.09 for 5.2 ×10− 3 M, according to Henry’s law). Fig. 1(a,c) show argon bubble. Since CCl4 concentration increases when liquid temper­
that increasing the temperature from 10◦ to 50◦ C improves the ature rises to 50 ◦ C (Henry’s constant for CCl4 is 6624 Pa/m3 mol− 1
maximum bubble radius by 12.5% (In = 0.7 W/cm2) for an argon [58]), this amount has been increased to 11.4% (Fig. 1(d)). On the other
bubble. A 12.3% rise is seen in the same way for an argon bubble that hand, at 1.5 W/cm2 (Fig. 2(b)), the presence of CCl4 causes the
contains 5,2 × 10− 3 M CCl4. compression ratio to be increased by 12.5% (at 10 ◦ C) compared to the
Fig. 2(a) and 2(c) show that at 1.5 W/cm2, the maximum bubble case of argon bubble. However, the effect of CCl4 is reduced when the
radius rises by 10.2% and 10% for 0 and 5.2 × 10− 3 M of CCl4, liquid temperature is increased to 50 ◦ C (Fig. 2(d)). The compression
respectively. As the temperature of the liquid rises, more water vapor­ ratio is increased by 8.8% in the presence of CCl4 inside the bubble. This
izes inside the bubble, increasing Rmax. When the acoustic amplitude is behavior is due to the increase of the temperature (50 ◦ C) and the
reduced from 5 to 1.4 bar, the bubble radius increases from 3 to 6 µm,

6
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

3.3. Effect of liquid temperature and CCl4 concentration on the bubble

temperature

From 0.7–1.5 W/cm2, the bubble temperature for each [CCl4]0

increased proportionally. The maximum bubble temperature (Tmax)
varies from 2017 to 3210 K, 2587–4363 K, and 3030–5815 K, respec­
tively, for intensities of 0.7, 1, and 1.5 W/cm2. This trend of increased
bubble temperature with acoustic intensity has been obtained by Kant­
hale et al. [78] for various wave frequencies in addition to the increase
of bubble sonoluminescence intensity and H2O2 production. Fig. 3(a)
shows that the increase of the liquid temperatures (from 10◦ to 50◦ C)
positively affects the bubble temperature (In = 0.7 W/cm2). This is
observed for a CCl4 concentration lesser than 10− 3 M, which is explained
that as the liquid temperature increases, more vapor is trapped inside
the bubble. Consequently, the bubble collapse becomes violent pro­
portionally with the rise of the solution temperature. For this range of
CCl4 concentrations (i.e., 0–10− 4 M), the bubble temperature is not
affected by the endothermal dissociation and the lower polytropic index
of CCl4 (Cp/Cv=1.11). This is due to the low liquid concentration of CCl4
and bubble temperatures (2017–3210 K), in addition to the low applied
acoustic intensity (0.7 W/cm2). Because at the acoustic power of
0.7 W/cm2 [Fig. 3(a)] and CCl4 concentration < 10− 3 M, a small amount
of CCl4 is found in the bubble, especially at the end of bubble collapse
(low CCl4 and acoustic intensity). Therefore, the effect of CCl4 (increases
the heat capacity of the bubble) is reduced. Moreover, the relatively low
maximal temperature (2017–3210 K) attained at collapse minimizes the
conversion of CCl4 and its contribution to the decrease of bubble tem­
perature through its endothermal dissociation (see Table S2 in the
supplementary data). The same response is retrieved when the liquid
concentration of CCl4 is increased from 0–10− 5 M. In contrast, for a
liquid CCl4 concentration ≥ 10− 3 M, the effect of liquid temperature is
minimized (Fig. 3(a)), where a turning point at 20 ◦ C is observed. This is
mainly due to the relatively higher concentrations of CCl4 in the solu­
tion. The bubble temperature decreases due to endodermal dissociation
and CCl4’s lower polytropic index (1.11) than 1.33 for H2O and 1.67 for
Ar [79]. This is that more CCl4 is trapped in the bubble as the liquid
temperature rises.
Different behaviors are observed as the acoustic intensity is increased
to 1 W/cm2 (Fig. 3(b)). For the liquid concentrations of CCl4 lower than
10− 3 M (~ 0–1 ×10− 4 M), it is shown that the bubble temperature in­
creases with the increase of the liquid temperature, until the liquid
temperature of 40 ◦ C (optimal value), after that the bubble temperature
is decreased with a further rise in the bulk liquid temperature. The
Fig. 4. Maximal conversion of carbon tetrachloride as function of its concen­ negative effect of the liquid temperature above 40 ◦ C is explained by the
tration in the bulk liquid (0, 1 ×10− 5, 1 ×10− 4, 1 ×10− 3, 3 ×10− 3, 5.2 ×10− 3 more considerable amount of water evaporated inside the bubble during
M) and the temperature of the solution (10, 20, 30, 40 and 50 ◦ C). The the rarefaction phase for this case (1 W/cm2) compared to the previous
decomposition of CCl4 is calculated for three intensities: (a) 0.7 W/cm2, (b) one (0.7 W/cm2). As a result, the bubble collapse is cushioned, mainly
1 W/cm2 and (c) 1.5 W/cm2.
due to the molar heat of water vapor (6/2Rg) and its endodermal
dissociation. The same behavior is observed when the liquid concen­
acoustic intensity (1.5 W/cm2). The impact of CCl4 is hidden tration of CCl4 goes up to 1 × 10− 3 M, whereas, in this case, the optimal
(Ar-CCl4-bubble) by the tremendous amount of vapor evaporated into value of the bulk liquid is moved to 30 ◦ C, where a maximal bubble
the bubble during the rarefaction phase. The compression ratio is temperature of 3609 K is obtained. Similar behavior has been obtained
observed to increase by roughly 2-fold in each case if the liquid tem­ previously by Merouani et al. [57] for a single bubble at 300 kHz for the
perature is fixed (10 or 50 ◦ C) (Fig. 1(b,d) and 2(b,d), respectively). production of hydroxyl radicals (an indicator of bubble temperature)
Previously, the expansion ratio (Rmax/R0) showed a similar pattern. with an optimum point at 35 ◦ C (Tliq varies from 25◦ to 55◦ C).
At last, it should be mentioned that despite the slight differences Similarly, the increase of the liquid concentration of CCl4 to 3 × 10− 3
observed at each plot in Fig. 1 and Fig. 2, these slight differences in Rmax and 5.2 × 10− 3 M shifts the optimal temperature of the liquid to 20 ◦ C,
and Rmin (at each Tliq) have an important impact on the maximal bubble where the maximal bubble temperatures are 3016 and 2734 K, respec­
temperature (Tmax, see Fig. 3), CCl4 conversion (see Fig. 4), and the tively. It should be noted that for the liquid concentrations of CCl4
maximal bubble pressure and the wall velocity (results not shown). greater or equal to 1 × 10− 3 M, the decrease of bubble temperature
Consequently, the molar yield inside the bubble is automatically above the optimum liquid temperature is due to the molar heat of the
affected by the variation of bubble dynamics (see below sections). The water and its endothermal dissociation. The bubble’s due to CCl4’s
same behavior was observed in many theoretical works [37,76,77]. endothermal dissociation and its lower polytropic index.
As shown in Fig. 3(c), all CCl4 concentrations (from 0 to 5.2 ×10− 3
M) have a turning point at 1.5 W/cm2. As the liquid temperature in­
creases, the bubble temperature decreases. This is partly because the

7
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

bubble’s temperature is reduced due to the endothermal dissociation of M. The maximum conversion of CCl4 at a liquid temperature of 50 ◦ C,
water vapor and its molar heat. Furthermore, the presence of CCl4 for the concentrations 10− 5 and 10− 4 M are 99.3% and 97.6%, respec­
within the cavitation and its endothermal dissociation contribute to the tively. The maximal conversion inside the bubble is lower than 60% for
lowering of bubble temperature, which is amplified as the liquid tem­ CCl4 concentrations higher than 10− 4 M (for all the liquid
perature and CCl4 concentration rise. The negative effect of liquid temperatures).
temperature on that of a single bubble is observed through the decrease As the acoustic intensity is increased to 1 W/cm2 (Fig. 4(b)), the
of bubble sonoluminescence with the increase of liquid temperature conversion of CCl4 inside the bubble is improved for all the liquid
according to Hiller et al. (Tliq from 10◦ to 22◦ C) [80], Barber et al. (Tliq temperatures and CCl4 concentrations. It can be observed that the
from 1◦ to 40◦ C) [81] and Vazquez and Putterman (Tliq from 0◦ to 34◦ C) breakdown of CCl4 within the bubble is independent of the liquid tem­
[82]. perature for liquid concentrations less than 10− 3 M (100% conversion).
Similarly, for the CCl4 liquid concentration of 10− 3 M, the maximal
conversion for the liquid temperature of 40 and 50 ◦ C is 99.1% and
3.4. Effect of liquid temperature on CCl4 decomposition
98.7%, respectively (100% conversion for Tliq< 40 ◦ C). These higher
levels of CCl4 conversions are in good agreement with those obtained
The CCl4 conversion is shown in Fig. 4(a) to be proportional to the
experimentally by Wu et al. [33] (at 20 kHz), Hung and Hoffmann [73]
rise in the highest bubble temperature (Fig. 3(a)). The maximum
(at 20–1078 kHz), and Francony and P é trier (at 20 and 500 kHz) [54],
decomposition is obtained at 0.7 W/cm2 for CCl4 concentrations ≤ 10− 4

Fig. 5. The molar yield of the different species as function of the temperature of the bulk liquid (10, 20, 30, 40 and 50 ◦ C) and the concentration of carbon tet­
rachloride (0, 1 ×10− 5, 1 ×10− 4, 1 ×10− 3, 3 ×10− 3, 5.2 ×10− 3 M) in the bulk liquid. The evolution of production is given for three acoustic intensities: (a) 0.7 W/
cm2, (b) 1 W/cm2 and (c) 1.5 W/cm2. The ultrasound frequency is 355 kHz. RCS [Reactive chlorine species]:⋅Cl,⋅CCl3, :CCl2, Cl2 and HOCl.

8
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

Fig. 5. (continued).

where the removal efficiency of CCl4 is greater than 99% depending on between our model findings and the experimental temperature values
the operational conditions in these works. For the CCl4 concentrations determined by several types of research for different sonication condi­
greater than 10− 3 M, the decomposition of CCl4 is reduced significantly tions (see Table S3 and Fig. S1 of the supplementary material), a good
for the liquid temperatures greater than 20 ◦ C (turn point, Fig. 3(b)). concordance has been shown, confirming the efficiency of our model for
In terms of practical application, f = 355 kHz, 1 W/cm2, and Tliq predicting the bubble temperature under different sonication
= 20 ◦ C, appears to be sufficient for the full breakdown of CCl4 liquid circumstances.
concentrations < 3 × 10− 3 M (Fig. 4(b)) (the bubble temperature is Consequently, the conditions of 1.5 W/cm2 and 10 ◦ C can be used in
between 3569 and 4092 K). The acoustic intensity of 1.5 W/cm2 is experimental works to improve the optimal conditions for CCl4 degra­
demonstrated for the sound breakdown of CCl4 in Fig. 4(c). In com­ dation. It is worth mentioning that for the intensities 1 and 1.5 W/cm2,
parison to previous examples, higher amounts of CCl4 degradation are the high levels of CCl4 elimination observed in our study are in line with
found (Fig. 3(a) and 5(b)). The higher bubble temperatures at this in­ those resulting from the different experimental works [11,32,33].
tensity (4321 and 5771 K, Fig. 3(c)) can be explained by the fact that
CCl4 is fully converted at 10 ◦ C (for In = 1.5 W/cm2), regardless of the
3.5. Decomposition products of CCl4 as function of the bulk liquid
bulk liquid concentration. It should be noted that there is no available
temperature
study providing the bubble temperature in the presence of CCl4. As it
was demonstrated in Section 3.3, the CCl4 pyrolysis within the bubble
As is well established, the chemical activity of the acoustic bubble is
affect (reduce) its internal temperature. However, the bubble tempera­
fully localized towards the end of bubble collapse, where maximum
ture range retrieved in this study (from 2000 to ~ 5700 K, Fig. 3) is in
bubble compression is reached during the compression cycle of the
good line with that determined by several experimental and theoretical
acoustic wave [18,46,57,67,68,77,92–96]. In this region, the tempera­
investigations for pure water or aqueous alcohol solutions (please see
ture peak is reached when the minimum bubble radius (Rmin) is reached.
[83–88] and [89–91]). Besides, according to the comparison made
Fig. 5(a-c) show the molar yields achieved after the bubble collapse

9
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

Fig. 5. (continued).

(at Rmin, corresponding to the maximum bubble temperature). Fig. 5(a) temperature (Fig. 5(a)). This is most likely owing to its lesser yielding
shows that when the bulk CCl4 concentration and solution temperatures compared to HCl and the possibility of⋅Cl radical recombination. On the
rise, the production of all species (and the overall production) rises other hand, it is retrieved that the yield of hydrogen atoms increases as
proportionately, following the same pattern as the bubble temperature the liquid temperature rises from 10◦ to 50◦ C, with the generation of⋅H
at 0.7 W/cm2 (Fig. 3(a)). Also, regardless of the liquid temperature, the decreasing when the concentration of CCl4 in solution rises for each
production of RCS is higher than that of⋅OH radicals (Fig. 5(a)). Unre­ liquid temperature (Fig. 5(a)). This is related to the fact that CCl4 mol­
lated to the liquid temperature, the rise in RCS generation is due to the ecules consume the radical⋅H (reaction 22, Table S2, supplementary
liquid CCl4 and its bubble’s breakdown. The improved generation of⋅OH data).
radicals is due to the reaction of CCl4 molecules with hydrogen atoms A similar pattern is found for 1 W/cm2 (Fig. 5(b)) as in the preceding
within the bubble (reaction 22 of Table S2), preventing⋅OH and H⋅from example (0.7 W/cm2), where the yield of RCS,⋅OH,⋅H, HCl, and HOCl
recombination too quickly. In fact, CCl4 is regarded as an excellent increases as the liquid temperature rises from 10◦ to 50◦ C. This is despite
hydrogen atom scavenger [28,72]. Despite the increase in CCl4 liquid the fact that CCl4 conversion decreases with increasing liquid concen­
concentration (>10− 4 M) and temperature (>20 ◦ C), the production trations (>1 ×10− 3 M, see Fig. 4(b)). However, in this example (1 W/
of⋅OH radicals remains fairly steady (Fig. 5(a)). When the CCl4 mole cm2), it was retrieved that at a bulk liquid temperature of 50 ◦ C, RCS
fraction inside the bubble rises, vapor dissociation decreases due to a generation is little increased. When the liquid temperature is raised from
drop in bubble temperature (Fig. 3(a)), resulting from increased CCl4 30◦ to 40◦ C, the yield of RCS rises by 31.2% and 4.8%, respectively, for
concentration in the bulk liquid. It should be noted that at the liquid CCl4 liquid concentrations of 10− 5 and 5.2 × 10− 3 M (Fig. 5(b)).
concentration of CCl4 equal to 3 × 10− 3 M and Tliq> 20 ◦ C, a turning These percentages are moved to 13.8% and 3.7% (for the CCl4 con­
point of⋅OH production is observed at each liquid temperature (30, 40, centrations of 1 ×10− 5 and 5.2 ×10− 3 M, respectively), when the liquid
and 50 ◦ C) (Fig. 5(a)). This is due to a competition between the lowering temperature increases from 40◦ to 50◦ C. Consequently, the production
of bubble temperature (reduction of H2O dissociation) as the CCl4 mole of HCl and HOCl are affected by the decrease of RCS formation. For
fraction inside the bubble increases and the increasing generation of⋅OH example, when the liquid temperature increases from 30◦ to 40◦ C for the
radicals by reaction of CCl4 with hydrogen atoms (Reaction 22 of CCl4 concentration of 5.2(10–3 M), the yield of HCl and HOCl increases
Table 2). This suggests that the yield of⋅Cl radicals is more significant by 71% and 41.9%, respectively. Whereas, when the liquid temperature
than the yield of Cl2 molecules (as seen by the plot of production for each is raised from 40◦ to 50◦ C, these productions of HCl and HOCl go up by
species (data not shown)). 47.9% and 4.5%, respectively. For the production of H⋅and⋅OH radicals,
For liquid temperatures larger than 20 ◦ C, a turning point of HCl the same explanation applies to the previous case (i.e., 0.7 W/cm2).
production is seen at a CCl4 concentration of 3 × 10− 3 M, similar to Furthermore, when the liquid temperature increases from 40◦ to 50◦ C,
the⋅OH scenario (Fig. 5(a)). At each liquid temperature, competition the generation of OH radicals is somewhat reduced, compared to the
occurs between the rise of CCl4 mole fraction (as a source of⋅Cl radicals) RCS scenario, despite the reduction in bubble temperature (Fig. 3(b)).
within the bubble (by increasing its concentration in solution) and the For example, for the CCl4 concentration of 3 × 10− 3 M, the increase
reduction of its degradation yield and bubble temperature (Fig. 4(a) and of⋅OH production is 38% and 29.7% when the liquid temperature is
3(a)). The reduction in CCl4 breakdown (at each temperature, Fig. 4(a)) raised from 30◦ to 40◦ C and from 40◦ to 50◦ C, respectively. The same
appears not to affect the rise in HOCl generation at each liquid tendency is observed for the other CCl4 concentrations (especially

10
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

higher concentrations). The reason is that as the liquid temperature is concentration of CCl4 in solution is less than 3 × 10− 3 M, it has been
increased, more vapor is trapped inside the bubble during the rarefac­ determined that using a 1 W/cm2 (f = 355 kHz) intensity for a liquid
tion phase. Consequently, the quantity of⋅OH radicals continues to in­ temperature of 20 ◦ C is adequate for full degradation of CCl4. However,
crease even if the bubble temperature goes down. In addition, the it was shown that using a 1.5 W/cm2 intensity at a liquid temperature of
scavenging of hydrogen atoms by CCl4 inside the bubble promotes more 10 ◦ C is entirely sufficient for full CCl4 destruction, regardless of its
the production of⋅OH radicals. The yield amortization of RCS, HOCl, and content in solution. Finally, it was discovered that using a 355 kHz ul­
HCl is owing to the decrease of CCl4 decomposition (Fig. 4(b)) and the trasonic frequency and a 0.7 W/cm2 intensity, the production of RCS,⋅
bubble temperature (Fig. 3(b)), where the increase of the liquid tem­ OH,⋅H, HCl, and HOCl increases proportionately with the increase in
perature to 50 ◦ C seems to be inefficient for the production increase of liquid temperature (from 10◦ to 50◦ C). However, it has been found that
these species (RCS, HOCl and HCl). Therefore, it can be concluded that increasing the liquid temperature from 10◦ to 40◦ C influences the pro­
the increase of the bulk liquid temperature from 10◦ to 40◦ C for the duction (increased) of RCS and⋅OH radicals (in addition to⋅H, HCl, and
intensity of 1 W/cm2 has a positive impact on the generation of RCS HOCl) for intensities 1 and 1.5 W/cm2. However, when the bulk liquid
and⋅OH radicals. However, this positive effect is observed only for⋅OH temperature exceeds 40 ◦ C (the generation of RCS,⋅H, HCl, and HOCl is
radicals when the liquid temperature exceeds 40 ◦ C. Despite the increase amortized), this beneficial influence persists just for⋅OH radicals. In
in acoustic intensity from 1 to 1.5 W/cm2 (Fig. 5(c)), the same behavior addition, radicals from RCS and⋅OH were primarily responsible for the
was observed but with a better overall and molar yield of the different rapid breakdown of nonvolatile contaminants in the presence of CCl4.
species. This is due to an increase in the acoustic amplitude. As shown in The pH solution drop is due to the formation of HCl and HOCl molecules
Fig. 5(c), increasing the liquid temperature to 50 ◦ C did not significantly (formed within a bubble), with HCl being more important than HOCl
enhance RCS production. For a CCl4 concentration of 10− 3 M, increasing independent of the liquid temperature, CCl4 solution concentration, or
the liquid temperature from 30◦ to 40 ◦ C and then from 40◦ to 50 ◦ C solution intensity.
improves RCS production by 26.3% and 6.1%, respectively. The
reduction in both CCl4 decomposition (Fig. 4(c)) and bubble tempera­ CRediT authorship contribution statement
ture (Fig. 3(c)) explains this retrievement. In contrast, the production
of⋅OH radicals improves as seen in Fig. 5(c) for 1 W/cm2. Aissa Dehane: Investigation, Conceptualization, Methodology,
Finally, the drop in solution pH can be attributed to the formation of Writing – original draft. Slimane Merouani: Conceptualization, Meth­
HCl and HOCl within the bubble. Regardless of the liquid temperature, odology, Writing – review & editing, Supervision. Oualid Hamdaoui:
CCl4 content, or sonic intensity, the yield of HCl is more favored than Writing – review & editing, Supervision. Magda H. Abdellattif: Writing
that of HOCl. This is in line with the findings of several experimental – review & editing, Supervision. Byong-Hun Jeon: Writing – review &
investigations [19,32,97,98]. The interaction of⋅Cl radicals (produced editing, Supervision. Yacine Benguerba: Conceptualization, Method­
within the bubble) with water may increase HCl production in the bulk ology, Writing – review & editing.
liquid [99,100].
Exciting use of CCl4 as an intensifier of the sonochemical degradation
of nonvolatile organic pollutants can be developed. Because of the Declaration of Competing Interest
limited quantity of free radicals dispersed from the bubbles at the
collapse to the surrounding liquid, sonolytic destruction of nonvolatile The authors declare that they have no known competing financial
organic pollutants is low, as stated in the introduction (the degradation interests or personal relationships that could have appeared to influence
zone of nonvolatile contaminants). Dyes [20,101], phenolic compounds the work reported in this paper.
[27,28], ciprofloxacin [29] and levofloxacin [30] have all shown that
sonicating nonvolatile organic pollutant solutions in the presence of Acknowledgements
CCl4 greatly improves nonvolatile pollutant degradation. According to
the simulation results of Fig. 5(a-c), it can be concluded that these im­ The authors thank Taif University Researchers, supporting project
provements are mainly due to the conjunction of (i) the huge generation number TURSP-2020/91, Taif University, Taif, Saudi Arabia. The
of reactive chorine (RCS) and (ii) the increase of the yield of⋅OH when Algerian Ministry of Higher Education and Scientific Research (project
the sonolysis of nonvolatile contaminants is conducted in the presence of number. A16N01UN250320180001) and the General Directorate of
CCl4. Therefore, in addition to itself-degradation, CCl4 plays a dual role Scientific Research and Technological Development funded this
in that case: (i) RCS generator and (ii)⋅H scavenger, which release a research (GD-SRTD). This research was financed by the Algerian Min­
higher amount of⋅OH radicals (quench of the rapid recombination⋅OH istry of higher education and scientific research (MESRS) and the
+⋅H ⇋ H2O). However, as the yield of RCS is greater than that of⋅OH Directorate General of Scientific Research and Technological Develop­
radicals, it can be concluded that the contribution of the RCS could be ment (GD-SRTD) (project number. A16N01UN250320180001).
more appreciable. As shown in Fig. 5(a-c), this approach, which is
validated by experimental data [20,24,28–30,97,101,102], may be
applied to a wide range of liquid temperatures and aqueous CCl4 Compliance with ethical standards
concentrations.
• Funding:The Algerian Ministry of Higher Education and Scientific
4. Conclusion Research (project number A16N01UN250320180001) and the Gen­
ral Directorate of scientific Research and Technological Develop­
This study shows that the presence of CCl4 affects bubble dynamics ment (GD-SRTD) jointly sponsored this research
mainly towards the end of collapse (increase in the compression ratio) • Conflict of Interest:All Authors decleare that they have no conflict of
but that there is no significant influence on the expansion ratio interest
throughout the expansion phase. On the other hand, it has been • Author contribution:All Authors contribute equally in the work.
retrieved that at a frequency of 355 kHz and a power density of 0.7 W/
cm2, the bubble temperature rises proportionately to the rise in liquid
temperature. However, if the liquid concentration of CCl4 is raised, the Appendix A. Supporting information
ideal liquid temperature (for the maximum bubble temperature) shifts
toward lower values at 1 W/cm2. At 1.5 W/cm2, on the other hand, the Supplementary data associated with this article can be found in the
bubble temperature drops as the liquid temperature rises. When the online version at doi:10.1016/j.jece.2021.106555.

11
A. Dehane et al. Journal of Environmental Chemical Engineering 9 (2021) 106555

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