i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3

Available online at www.sciencedirect.com

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Review Article

Sonolytic and ultrasound-assisted techniques for

hydrogen production: A review based on the role of
ultrasound

Nourhane Merabet a,b, Kaouther Kerboua a,*

a
Higher School of Industrial Technologies, Department of Engineering, P.O. Box 218, 23000 Annaba, Algeria
b
Laboratory of Technologies of Energetic Systems E3360100, Higher School of Industrial Technologies, Annaba,
Algeria

highlights

Sonochemical and ultrasound assisted techniques for H2 production are reviewed.

Sonophysical effects are the predominant mechanism for H2 production improvement.

The controlling parameters of ultrasound-assisted H2 production are discussed.

In sonoelectrolysis, of energy efficiency increases by 1% to 25% due to sonication.

Technological challenges and limits of H2 production using ultrasound are reported.

article info abstract

Article history: Among the cleanest combustibles, hydrogen represents the energy carrier of the near
Received 2 January 2022 future, thereby, techniques for hydrogen synthesis have been the subject of several
Received in revised form research studies. The integration of ultrasound to several techniques as a promising
1 April 2022 combination has known in recent years an increasing interest owing to the physical and
Accepted 12 April 2022 chemical roles of sonication and the eventual created synergetic effects. The present re-
Available online 6 May 2022 view aims to inspect the various techniques using ultrasound as a direct or auxiliary
pathway for the generation of hydrogen. Experimental and numerical studies related to the
Keywords: use of power ultrasound as an isolated technique are reviewed in terms of approaches,
Sonication configurations, and qualitative and quantitative observations. The combination of power
Sonochemistry ultrasound with other techniques such as electrolysis, catalysis, and photolysis, is then
Physical effects examined and discussed, particularly in regards to the role of ultrasound in the “ultra-
Hydrogen sound-assisted” hydrogen production, but also the expected magnitude of the kinetics
Parameters enhancement and energy-saving when integrating ultrasound. It was reported in several
Scale works that the use of ultrasound for hydrogen generation may lead to an increase in the
rate of produced hydrogen achieving 25%, and an improvement in energy efficiency in the
range of 5e18%, while some other studies reported limited enhancement in the order of
1%. Overall, ultrasound irradiation has the advantages of enhancing mass transport,
bubbles detachment from catalysts and electrodes surfaces, efficient degassing, and
cleaning effect. The technological state of the art and the engineering designs are also

* Corresponding author.
E-mail address: k.kerboua@esti-annaba.dz (K. Kerboua).
https://doi.org/10.1016/j.ijhydene.2022.04.108
0360-3199/© 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
17880 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3

reported with the perspective of adopting the sono-production of hydrogen at the indus-
trial scale.
© 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

Contents

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17880
The sonolytic pathway of hydrogen production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17881
The experimental approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17881
The modeling approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17882
Effect of ultrasound frequency and waveform . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17883
Effect of static pressure and acoustic amplitude . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17883
Effect of acoustic intensity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17883
Effect of the nature of the liquid medium and dissolved gases . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17884
Ideal and real gas assumptions for modeling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17884
The ultrasound-assisted pathway for hydrogen production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17885
Sonoelectrolysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17885
Sonocatalysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17886
Sonoelectrocatalysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17888
Sonophotolysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17888
Sonophotocatalysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17888
Controlling parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17889
The technological state of the art . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17890
Observations and conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17891
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17891
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17891

the mixture i.e., it consists of the gasification of the raw ma-

Introduction
In recent times, the scarcity of fossil fuels and climate change
represent the most important challenging topics of global
impact. Hence, finding a new, clean and concise source of
energy is one of the main tough objectives of the scientific and
engineering communities. Fortunately, hydrogen has proved
to respond to the main criterion of the green fuel, with a
specific heat capacity of 140 MJ/kg, it is expected to be the fuel
of the near future [1].
The synthesis of hydrogen can be achieved through several
technologies, such as steam reforming, partial oxidation,
renewable liquid and bio-oil processing, biomass, and coal
gasification [2]. Steam reforming is a well-established method
for hydrogen generation, in which, the most widely used feed
materials are natural gas and light hydrocarbons, methanol,
and other oxygenated hydrocarbons [3]. Steam methane
reforming for hydrogen production has proved to be the most
efficient, safe, and cost-effective technology based on several
infrastructure criteria, according to Chau et al. [4]. Another
excellent pathway for hydrogen generation is the partial
oxidation process, which is a nano catalytic technology to
produce hydrogen from hydrocarbons, namely heavy oil,
methane, and biogas. Partial oxidation systems add a small
amount of air to the fuel to partially oxidize the fuel and heat
terials in the presence of oxygen and possibly steam, at tem-
peratures that range from 1300 to 1500  C and pressures in the
range of 3e8 MPa [3,5]. Hydrogen can also be generated via
plasma reforming from several hydrocarbon fuels. This
method is known to achieve almost 100% of conversion effi-
ciency. In this technology, required energy and free radicals
are provided by plasma, generally from electricity or heat.
There are mainly two forms of plasma reforming, namely
thermal and non-thermal reforming [3]. Biomass is an excel-
lent feedstock for renewable hydrogen processes as well,
indeed, an alternative route for hydrogen generation is the
gasification of biomass. This later is based on partial oxidation
of the primary material into a mixture of hydrogen, methane,
higher hydrocarbons, carbon monoxide, carbon dioxide, and
nitrogen [6]. In contrast to the former techniques, gasification
can be performed at relatively low temperatures below 700  C
with lower CO2 emissions [7].
While the combustion of hydrogen remains clean, by
resulting exclusively in water and heat, the carbon footprint
and risks related to the process of hydrogen production vary
according to the technique itself and the energy source
involved in the technique. The carbon footprint related to
hydrogen generation increases in industries that use natural
gas and hydrocarbons as feedstock [8]. For instance, approxi-
mately 50% of the global demand for hydrogen is currently
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
produced through steam reforming of natural gas, and around
30% from oil/naphtha reforming from refinery/chemical in-
dustrial off-gases [9]. These conventional techniques for
hydrogen generation (steam reforming of hydrocarbons)
generate an extremely high amount of carbon dioxide and
greenhouse gases emissions that can reach 7.05 Kg CO2/Kg of
H2 in the case of methane and 10.621 Kg CO2/Kg of H2 using
natural gas, which significantly contributes in the carbon
footprint [3,10]. The electrolytic pathway for hydrogen pro-
duction presents the most basic method to split water into
hydrogen and oxygen through the application of continuous
current (circulation of electrons via an outer circuit) [11].
While alkaline and proton exchange membrane (PEM) elec-
trolyzers are the most well-established electrolytic pathways,
4% of the worldwide hydrogen generation is made using the
electrolytic technique. Another possible pathway for
hydrogen generation is the electrocatalytic process where
catalysts are parts of the electrodes used in water splitting via
an electrochemical process. However, this later suffers from
cost limitations related to metals used as catalysts, or from
the proprieties of the catalyst (stability and durability) [12].
Renewable energy systems of water electrolysis, namely wind
and PV (photovoltaic) electrolysis, are considered promising
pathways for clean hydrogen production [13]. In addition,
thermochemical water splitting and hybrid thermochemical
cycles (e.g. CueCl, SeI, and MgeCl) also provide interesting
environmental results [14]. Besides, photolysis is a method
that consists of the cleavage of water into hydrogen and ox-
ygen using light or solar radiation [15]. This technique could be
enhanced by the employment of catalysts using metals such
as semiconductors. In fact, the exposition of the metal to light
irradiation initiates the catalytic activity of this metal. How-
ever, the high cost of catalysts and the low ratio of hydrogen
production compared to energy consumption in photolysis
are the main challenges facing this method.
The need for decarbonization or semi-decarbonization of
hydrogen generation suggested the introduction of ultra-
sound for its pure chemical effects, i.e., sonochemistry, and as
an auxiliary technique in ultrasound-assisted processes for
hydrogen production, such as sonoelectrochemistry. It is
known that the propagation of ultrasonic waves in a liquid
medium generates two major phenomena, namely acoustic
streaming, and acoustic cavitation. Acoustic cavitation, which
is defined as the nucleation, growth, and violent implosion of
micro-bubbles, remains the dominant effect of this propaga-
tion [16]. During the propagation of ultrasound waves in
aqueous mediums, each cavitation bubble behaves as a local
‘hot spot’, causing a dramatic increase in temperature and
pressure exceeding 5000  C and 2000 atm, and inducing the
apparition of several chemical reactions, which is known as
sonochemistry [17]. Owing to the multiple reactions evolving
within the cavitation bubble, several species are produced,
while the main products are hydroxyl radicals HO
, H
and
H2 O2 : Usually, in the case of pure sonolysis, chemical effects
associated with sonication, namely sonochemistry, are
responsible of the production of hydrogen. Acoustic stream-
ing and acoustic cavitation result in other important proper-
ties such as high shear stress near the bubble wall, increased
heating and cooling yields, micro-jets, microstreaming, gen-
eration of shock waves, and turbulent flow. These physical
17881
effects promote stirring and mass transfer and increase the
current in ultrasound-assisted electrolysis owing to the
erosion of the electrode surface under the effect of the
shockwave phenomena, offering a new reactive surface.
Cavitation is a phenomenon that is highly dependent on the
operating parameters and the geometry of the reactor. Basi-
cally, the reaction pathway and global yields of sonochemical
reactions are dependent on the temperature, the acoustic
frequency and intensity, and the static pressure of the fluid
[18].
The physical and chemical effects originating from
acoustic cavitation in water irradiated by ultrasound waves
have been reported in detail in several research studies
[19e21]. In terms of the sonochemical hydrogen production,
and according to Edwin and Henglein [22] and Maritza et al.
[23], the generation of hydrogen takes place through the
recombination of two H
radicals. Merouani et al. [21]
demonstrated that the main pathway of hydrogen production
inside the bubble remains the recombination of HO
and H
.
Despite the challenging question of the exact mechanism of
hydrogen production via water sonolysis, the technique is
presented as a promising technology for clean hydrogen
generation [1,21].
In terms of ultrasound-assisted pathways for hydrogen
generation, the considerable progress in the combination of
ultrasound power to several conventional processes (elec-
trolysis, photolysis, catalysis, photocatalysis, and electro-
catalysis) has animated important scientific debates on the
hybrid processes’ efficiencies [24]. On this subject, tens of
experimental works could be found in the literature, in which
the adoption of sonication in silent techniques has come with
encouraging results that could attend the 100% of enhance-
ment [25].
In the present review, we shed light on the important re-
sults that are provided from literature studies, particularly
from the last five years, dealing with sonochemistry and ul-
trasound-aided techniques for hydrogen generation, and
highlight the mechanism behind the observed effects. The
review aims to examine the configurations of the techniques
and their relative performances; and elucidate the conver-
gence and divergence points, particularly in terms of plausible
mechanisms and achieved efficiencies and energy saving. The
review will also reveal the challenges facing sonolysis and
ultrasound-assisted techniques as eventual technologies for
hydrogen production. It will also clarify some future orienta-
tions for research and development in this specific field of
application. The present review covers sonolysis, sonoelec-
trolysis, sonocatalysis, sonoelectrocatalysis, sonophotolysis,
and sonophotocatalysis techniques from a mechanistic point
of view to bring insights to researchers expecting to combine
sonication with conventional techniques for the production of
hydrogen.
The sonolytic pathway of hydrogen production
The experimental approach
Despite being a clean, environmentally friendly, and safe so-
lution for hydrogen production, the experimental
17882 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3

investigations of water sonolysis for hydrogen production are
few in the literature. An early experimental study of Henglein
et al. [26] was conducted under 300 kHz and 35 W/cm2 under
atmospheres of argon, oxygen, and argon-oxygen mixtures.
Hydrogen was then detected for the first time as the main
product of sonolysis with hydrogen peroxide. Since then, and
to the best of our knowledge, no experimental study has been
conducted on sonolytic hydrogen generation for several de-
cades. Very recently, Kerboua et al. [27] carried out a combined
study based on modeling and experimental approaches for
hydrogen production through the sonolytic pathway, in which
the acoustic frequencies have been varied over the range of 20,
210, 326, and 488 kHz. The experimental approach revealed
that the highest percentage of conversion of electric energy to
acoustic energy was estimated at 61.25% under 20 kHz. In the
same study, Kerboua et al. [27] suggested several metrics
allowing the estimation of the efficiency of the process. For
instance, the mass-to-energy ratio corresponding to both
microscopic and macroscopic scales was calculated, as well as
the rate of hydrogen production via water sonolysis. The
study revealed an optimum ratio of hydrogen molar yield to
acoustic intensity of 5.50  107 mol/J at reactor scale, ach-
ieved at 210 kHz and considering a common acoustic intensity
of 0.48 W/cm2 at all the studied frequencies. In terms of
electric energy consumption, the highest ratio was recorded
under 20 kHz with a value of 1.08  1010 mol/J of electric
energy, for a common electrical consumption of 87 ± 5 W at all
the frequencies. This value decreases with the increase of
ultrasound frequency. It is worthy to note that the modeling
and simulation results revealed that at the multi-bubble scale,
the highest ratio of hydrogen yield to electric energy con-
sumption was observed at 20 kHz. In the same study, both
approaches demonstrated a perfect agreement.
The modeling approach
In contrast with the experimental approaches, the literature
counts tens of works that deal with the modeling and simu-
lation of the sonochemical hydrogen production. Numerous
studies presented mathematical models to explain the
mechanism of water cleavage using ultrasound power. A
considerable number of these studies has been gathered in
Table 1, which reports the examined parameters, the scanned
range, the studied scale, and the main observations. Most of
these investigations adopted the so-called “single bubble
model”, which is regarded as the representative unit of the
sonicated medium [21,28e32]. Merouani et al. [21] proposed a
numerical modeling work describing a single argon bubble, to
explain the mechanism of hydrogen generation during the
sonication of water. This model combines the bubble dy-
namics with the chemical kinetics consisting of 25 reversible
chemical reactions evolving during the collapse phase. The

Table 1 e Synthesis of the principal modeling works dealing with the sonochemical production of hydrogen.
Parameter Author scale Range Observed optimum
Frequency Merouani et al. [36] Single bubble 140, 213, 355, 515, 647, 875, 1000 kHz 140 kHz
Brotchie et al. [37] Single bubble 213, 355, 647, 875, 1056, 1136 kHz 355 kHz
Kerboua et al. [38] Single bubble 200,300 and 500 kHz 200 kHz using a sine wave and 500 kHz
when using a sum of six successive
harmonics
Kerboua et al. [31] Single bubble 200,300,500 kHz 200 kHz
Kerboua et al. [27] Single bubble 20, 210, 326 and 488 kHz 20 kHz
Multi-bubble 20, 210, 326 and 488 kHz 210 kHz
Amplitude/acoustic Merouani et al. [29] Single bubble 0.5, 0.75, 1 W/cm2 1 W/cm2
intensity Dehane et al. [39] Single bubble 0.3e2 atm 0.7 atm at 355 kHz and 0.5 atm at
515 kHz
Dehane et al. [40] Single bubble 1.5, 2, 3 atm 3 atm
Saturating gas Merouani et al. [29] Single bubble 20, 140, 213, 355, 515, 647,1000, 1100 kHz Ar gas
Gielen et al. [46] Single bubble 47,248 kHz Ar gas and an optimum frequency of
247 kHz
Kerboua et al. [45] Single bubble 20 kHz Ar gas
Kerboua et al. [27] Multi-bubble 20 kHz Ar atmosphere
Ambient radius Dehane et al. [40] Single bubble 355, 500 and 1000 kHz 500 kHz
Modeling Kerboua et al. [32] Single bubble 200, 300,500 and 1000 kHz Higher rates were obtained when
assumptions using the equation of Van der Waals at
low acoustic amplitude while higher
rates were observed using ideal gas
law at high acoustic amplitude
Kerboua et al. [41] Single bubble 200, 300,500 and 1000 kHz The introduction of reaction heats
induces a reduction in the harsh
conditions within the bubble owing to
their endothermic nature
Waveform Kerboua et al. [31] Single bubble 200,300,500 kHz The signal composed of the sum of six
harmonics demonstrated a clear
enhancement in hydrogen production.
Kerboua et al. [38] Single bubble 200,300 and 500 kHz The square wave proved to enhance
the yield of reactants for the chemical
process
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
production of hydrogen through water sonolysis occurs when
the liquid medium, generally water, is exposed to an ultra-
sonic wave, which in turns provokes the formation, growth
and violent collapse of microscopic bubbles. Accordingly,
during the rarefaction phase of the ultrasonic wave, the bub-
ble expands attaining a resonance size, then, the violent
collapse of the bubble during the compression phase leads to
the reduction of the bubble size until it attains a minimum
size. A series of successive expansions occurs and generates
extreme conditions of temperature and pressure within the
bubble, offering a specific environment where high energy
chemical reactions take place and many chemical products
are formed, namely, H2, O2, H2O2, H
, HO
, O and HO2
via the
thermal cleavage of water vapor and its associated reactions
[21]. Though the mechanism of hydrogen generation inside
the bubble remains debatable, according to the author, H2
kinetics evolution achieves its maximum at the end of the
bubble explosion, H2 constitutes then 35.3% of the bubble
content at 20 kHz and more than 17.2% at 355 kHz. Merouani
et al. [21] concluded after analysing the chemical kinetics re-
sults and the high consumption of H
and HO
radicals, that
more than 99% of hydrogen is generated within the gas phase
inside the bubble volume through the recombination of H

and HO
according to the equation H
þ HO
4H2 þ O
.
The sonochemistry of hydrogen production depends not
only on the chemical mechanism, but also on the sonication
pathway (direct or indirect), ultrasound irradiation modes
(pulsed or continuous), diverse configurations (by modifica-
tion of the amount and positions of ultrasonic wave sources)
[33e35], and several other parameters. In a recent paper,
Merouani and Hamdaoui [20] reviewed the available studies
dealing with ultrasound production of hydrogen and the pa-
rameters influencing its production. While Torres et al. [33]
presented a chapter that tackled the different applications of
ultrasound in water and the influence of the different oper-
ating parameters on the sonochemical reactions, and implic-
itly on the sonochemical hydrogen generation. Numerous
studies retrieved in the literature examined the impact
of the operational parameters on the overall sonochemical
hydrogen production.
Effect of ultrasound frequency and waveform
One of those parameters that have been widely investigated is
the ultrasound frequency. Merouani et al. [36] inspected the
impact of ultrasound frequency (200, 300, 500, 1000 kHz) and
acoustic amplitude (1.5, 2, 2.5, 3 atm) on the optimal equilib-
rium size of bubbles to maximize hydrogen production. Mer-
ouani et al. [36] explained that the optimum ambient radius
for hydrogen production decreases when the ultrasound fre-
quency increases. These results match perfectly with the
previous findings of Brotchie et al. [37]. Additionally, Merouani
et al. [29] performed a simulation study under different fre-
quencies (20, 140, 213, 355, 515, 647, 1000, 1100 kHz), saturating
gases (Argon and air) and acoustic intensities (0.5, 0.75 and
1 W/cm2). The same research group [30] proposed another
numerical simulation assessing the effect of ultrasound fre-
quency in the interval ranging from 213 to 1100 kHz under
different saturating gases (O2, air, N2, and H2), and it was found
that hydroxyl radicals HO
were the main product among the
created radicals (H
HO2
and O) during the strong explosion of
17883
the bubble. While at lower frequencies, the amount of
hydrogen would be predominant. Kerboua et al. [38] investi-
gated the effect of the waveform on the sonochemical pro-
duction of hydrogen. They modified the sine wave into a
square wave by summing harmonics of regressive amplitude
and using ultrasonic waves with frequencies of 200, 300, and
500 kHz at an acoustic amplitude of 2 atm. When comparing
the results of the aforementioned work, it was deduced that
the more the waveform approaches the square shape, the
higher the molar yield of the produced hydrogen. It was also
observed that with the same waveform, the increase of ul-
trasound frequency leads to a decrease in the rate of hydrogen
produced at the single acoustic cavitation scale. The effect of
frequency is related to the fact that at higher frequencies, the
evolution of the reaction system inside the bubble is limited
and the bubble implodes very quickly, hence, only a few of the
emerging free radicals combine and can be converted to
hydrogen.
Effect of static pressure and acoustic amplitude
Very recently, Dehane et al. [39] investigated the effect of the
static pressure (0.2e3 atm) on the bubble size and conse-
quently on hydrogen production, for frequencies in the range
of 355, 500, and 1000 kHz. The results showed that the
decrease of the pressure has the same impact as the increase
of the acoustic power, while the augmentation of the static
pressure lowers the maximal temperature of bubbles at
collapse. Overall, it was revealed that the production rate of
hydrogen was favored at conditions leading to high collapse
temperatures exceeding 8500 K. In another study, Dehane
et al. [40] varied the range of ambient radius, acoustic fre-
quency (355, 500, and 1000 kHz) and acoustic amplitude
(1.5e3 atm) in the aim of investigating the impact of mass
transfer, heat exchange and chemical reactions heat on the
sonochemical hydrogen production. As expected, it was
revealed that the rate of produced hydrogen achieved its
maximum at a lower frequency and higher acoustic ampli-
tude, as demonstrated previously in several studies [29,32,41].
This trend was verified independently of the adopted hy-
potheses. A higher rate of hydrogen was retrieved when
eliminating the heat of the reaction owing to the removal of
the endothermic reactions participating in the chemical
mechanism and causing the considerable reduction of the
temperature within the bubble during the implosion. On the
other hand, the mass transport phenomenon has proved its
important role in the enhancement of sono-hydrogen pro-
duction. The lowest rate of production was recorded in the
absence of mass transport. The approach of Dehane et al. [40]
was based on the inspection of the effects of the adopted
assumption on the simulated evolution of sono-hydrogen
production.
Effect of acoustic intensity
Some other studies dealt with the acoustic intensity instead of
the acoustic amplitude. The previous research work of Mer-
ouani et al. [29] reported a considerable improvement in the
amount of hydrogen produced at the single bubble level when
acoustic intensities increased due to the general increase in
the sonochemical activity. The same trend was reported by
several researchers [20,33,42]. Dehane et al. [40] observed an
17884 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
increase in the bubble's temperature due to the increase in the
acoustic intensity. This was explained by the acceleration of
the bubble wall during the collapse stage, resulting in a more
violent collapse at the end of the compression stage. As a
result, the overall sonochemical generation of hydrogen
within the bubble is improved. In another study, Dehane et al.
[43] reported an increase in hydrogen production rate when
increasing acoustic frequency under Xe, Ar and He saturated
water. Moreover, Merouani et al. [36] investigated the impact
of acoustic intensity on the size of the bubble. Similarly, the
researchers observed an increase in hydrogen activity when
increasing the acoustic intensity. While Labouret et al. [44]
observed an expansion in the bubble radius at higher acoustic
intensities. According to Merouani et al. [29], a higher acoustic
intensity promotes the bubble core temperatures and the
amount of trapped water vapor which enlarges the radius
interval of the acoustic cavitation bubble, improving hydrogen
production. The increase of the amount of trapped water
vapor enhances the formation of free radicals since hydrogen
results mainly from the decomposition of water vapor mole-
cules inside the bubble. The implosion of the larger bubbles is
stronger at higher acoustic intensities and, therefore, these
bubbles become more active and generate H2 by the recom-
bination of free radicals.
Effect of the nature of the liquid medium and dissolved gases
In terms of the liquid medium composition and its effect on
the sonochemical hydrogen production, a numerical study
has been performed by Kerboua et al. [28] to investigate the
efficiency of methanol degradation in wastewater and its
conversion into hydrogen via the sonolysis pathway under an
argon-oxygen atmosphere. According to the authors,
hydrogen amount was ~104 higher in the presence of an
aqueous solution of methanol, as compared to pure water.
Furthermore, the optimum rate of hydrogen was recorded
under a 40% argon atmosphere within a solution of 20% vol/
vol of methanol with a value of 9.9  107 mol/s. Overall, the
produced hydrogen yield was improved when increasing
methanol concentration in the medium until reaching an
optimum at 40%, the rate of hydrogen drops then for the
concentrations above 40%.
Kerboua et al. [45] also investigated numerically the effect
of dissolved gases on the kinetic mechanism of the sono-
chemical production of hydrogen. The numerical simulation
was conducted at 20 kHz and 0.1 MPa of acoustic amplitude
under 4 dissolved gases, namely N2 O2, Ar, and air, and
demonstrated that at the single bubble scale, the highest
hydrogen amount was recorded under argon atmosphere
which is an inert gas that intervenes only as a third body in the
reaction mechanism. This was in perfect accordance with the
conclusions of Gilen et al. [46] who investigated the impact of
dissolved gases on free radicals formation and sonolumi-
nescence under the same gaseous atmospheres at 47 and
248 kHz. It was also in good agreement with the findings of
Merouani et al. [29] in terms of the nature of dissolved gases
for the optimal sonochemical production, in which the author
found that the highest amount of hydrogen is produced under
an argon atmosphere, and attributed this to the thermal pro-
prieties of the dissolved gas, specifically its polytropic index
and thermal conductivity. Merouani et al. [29] explained that a
greater polytropic index increases the temperature inside the
bubble at the collapse, while a lower thermal conductivity
reduces the heat dissipation, hence inducing the augmenta-
tion of the temperature and improving the sonochemical
activity.
Recently, Dehane et al. [43] investigated the influence of
saturated gases on sono-hydrogen generation under different
operational parameters of frequency (213, 355, and 515 kHz),
acoustic intensity (1, 1.5, and 2 W/cm2), and the nature of
saturating gas (Ar, Xe, and He). The study revealed that an
optimum hydrogen production rate, as well as optimum radii,
were observed under xenon-saturated water, followed by Ar
and He atmospheres. This was due to the fact that the
increased thermal conductivity of the saturating gas affects
negatively the intensity of the bubble collapse and its molar
efficiency, which was in good agreement with several previ-
ous works.
Ideal and real gas assumptions for modeling
This approach has been treated by Kerboua et al. in regards to
the effects of gas state [32] and reaction heat [41]. In the first
study [32], two approaches were adopted to assess the
hydrogen production rate under different operating conditions
of acoustic amplitude (1.5, 2, 2.5, and 3 atm) and frequencies
(200, 300,500, and 1000 kHz). The adoption of the ideal gas
approach revealed that the amount of hydrogen increases with
the augmentation of acoustic amplitude and the decrease of
ultrasound frequency reaching the value of 1.30  1016 mol
under 200 kHz and 3 atm, per single bubble and over one
acoustic cycle. The approach using the real gas model resulted
in the highest amounts of hydrogen at low acoustic amplitude
and high frequencies, the highest gap due to both approaches
in terms of hydrogen molar yield was observed at 1.5 atm and
1000 kHz. This was attributed to the fact that when gas is
considered real, the reached temperature within the bubble at
the end of the collapsing phase is higher (around 6000 K), which
leads to higher hydrogen production. In the second study,
Kerboua and Hamdaoui [41] studied the impact of reaction heat
on the variation of radius, temperature, pressure, and chemical
species rates, including hydrogen, using both aforementioned
approaches. The temperature appeared to be a frequency-
acoustic amplitude-dependent variable, which increases with
the decrease of the frequency and the augmentation of the
acoustic amplitude. However, when introducing the reaction
heat, the value of the pressure increases, in contrast to the
bubble volume and the temperature that drop down, particu-
larly with the decrease of the frequency and the increase of the
amplitude. Overall, these variations demonstrated a negative
impact of the reaction heat on the rates of chemical species,
and consequently hydrogen production. Even more, the results
revealed that the temperature is the dominant parameter in
the chemical mechanism inside the bubble, the sonochemical
production of hydrogen was then proved to be mainly a
temperature-dependent kinetics.
Despite the encouraging results of the considerable num-
ber of studies regarding sonochemical hydrogen production, it
is worthy to mention that this technique is still limited at a
laboratory scale owing to several factors. To focus on one of
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3 17885

the main limitations in terms of modeling, the single bubble
model, generally adopted by researchers, prevents the
comprehension of the phenomenon at the macroscopic scale
and thus the scaling up of the technique. In fact, at the
macroscopic scale, the bubbles interact with each other in the
medium, and the single acoustic cavitation bubble is no longer
a representative unit of the population. In a recent review,
Kerboua and Hamdaoui [1] discussed the factors influencing
the development of sonochemical as well as ultrasound-
assisted pathways for hydrogen production. The authors
suggested as a perspective of the review to explore new axes
of research regarding the impact of static, acoustic, and me-
dium factors on the size distribution of the bubbles, shape
stability, lifetime, bubbles' number density, and interaction.
Beyond the single bubble scale, the recent study of Kerboua
et al. [27] examined for the first time the energy efficiency of
sonochemical hydrogen production. The study was based on
laboratory-scale experiments, and numerical modeling at the
single bubble and reactor scale to assess the mass efficiency
and mass-to-energy metrics at both single and multi-bubble
scales. For instance, under a similar acoustic intensity of
0.48 W/cm2 for the same irradiation time of 50 ms, the greatest
hydrogen production was estimated at 2.36  1017 mol under
an acoustic frequency of 20 kHz while the highest H2 molar
yield was recorded at 20 kHz with 1.16  1010 mol/J of internal
energy variation. This value seemed to decrease with the in-
crease of the ultrasonic frequency.
The ultrasound-assisted pathway for hydrogen
production
Sonoelectrolysis
Among the different ultrasound-based techniques for
hydrogen generation, sonoelectrolysis is the technique known

Table 2 e Synthesis of the principal experimental works dealing with sono-electrolysis for hydrogen production.
Author Type of Type of Acoustic Observed improvement Interpretation of the effect
electrolysis sonication conditions
Cataldo [51] Acidic NaOH and Ney Ultrasonik 30 kHz and an Hydrogen yield increased by The main phenomenon
Acidic HCl 100 ultrasonic acoustic intensity 11% in 5 M NaOH/1.1 M HCl occurred under sonication is
solutions bath. estimated in the solution using carbon rod the degassing effect owing to
range of (1e2W/cm2) electrodes. the coalescence of bubbles
which prevents the
accumulation of bubbles on the
surface of the electrode and
hence improves hydrogen and
chlorine yields
Walton [52] Sulfuric acid Julabo U S F 38 kHz Voltammogram measures of Sonication power improved
H2SO4 solution Ultrasonic bath hydrogen and oxygen under hydrogen production by
silent and ultrasonic irradiation contributing to the efficient
showed an improvement in the bubbles' removal from
working current electrodes
McMurray [53] Na2SO4 solution (Ti) tip sonotrode 20 kHz and 26 W/cm2 Voltammetry measurements at Enhancement of mass
the cathode and the anode transport under ultrasound
showed an improvement in the power that leads to the increase
current density in the presence in the rate of hydrogen gas
of ultrasound produced
Budischak [54] Alkaline KOH Ultrasonic bath 42 kHz Voltammetry measurements at Ultrasound irradiation cleans
solution Quantrex 310 by the anode and the cathode the surface of the electrode
L&R Ultrasonics showed an improvement in the from bubbles to create more
working current active sites
Li et al. [55] Alkaline (0.1, 0.5 Ultrasound 60 kHz and 50 W 10% to 25% of energy-saving The quick removal of the
and 1.0 M) NaOH generator and 5e18% improvement in the bubble from the electrode
solution energy efficiency of hydrogen surface without any
production coalescence so that the active
sites are recharged to form a
new gas bubble.
Zadeh [57] Alkaline 0.1 M ultrasonic 20 kHz H2 production was improved by Bubble detachment from the
NaOH/0.1 M KOH transducer 14 and 25% for NaOH and KOH electrode prepares the surface
solutions solutions, in addition to an for new electrochemical
enhancement of 4.5% in reactions.
production efficiency and 1.3%
in energy efficiency.
Lin et al. [58] Alkaline KOH An ultrasonic 133 kHz Ultrasound sonication
solution shakes machine (225,450,675,900 W) contributes to the acceleration
(GE-900 W) of ions vibration and diffusion
and increases the deviation of
the bubble from the electrodes
and accelerates
17886 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
as associating ultrasound with electrolysis. This technique
proved to be efficient by several researchers, Table 2 reports
the main research studies retrieved in the literature in this
field. Pollet is the pioneering researcher in the field of sonoe-
lectrolysis, Pollet and coworkers presented numerous works
to explain the impact of ultrasound on the reduction of the
overpotential and the drop of ohmic voltage, which
conducts to higher hydrogen generation rates [47e49].
Pollet [48] reported in a book entitled “Power Ultrasound in
Electrochemistry: From Versatile Laboratory Tool to Engi-
neering Solution” the application of ultrasound power in
electrochemistry. Pollet discussed, reviewed, and analyzed
the different works and results of sonoelectrolysis and high-
lighted the role of ultrasound waves in the decrease of over-
potential. Similarly, Islam et al. [49], from the same research
group, presented the sonoelectrochemical pathway for
hydrogen production and explained how do ultrasound in-
fluence the mass transport and electrode cleaning through the
combined effect of microjets and microstreaming as well as
the drop of the over potential that is caused by the degassing
effects and/or the modifications of the surface of the electrode
[50]. Islam suggested deeper investigations of H2 quantifica-
tion for a better comprehension of the impact of different
parameters of sonoelectrochemistry for hydrogen production,
for the upgrade of the process. Cataldo [51] was one of the first
to study the effect of ultrasound on water electrolysis for
hydrogen production. Using different solutions of 6 M NaCl,
6 M HCl, and acidified solution of 0.5NaCl/1.1 HCl under
30 kHz. It was found that the presence of ultrasound increased
the rate of chloride and hydrogen gases due to the induced
degassing effect. Walton et al. [52] used 38 kHz of ultrasound
frequency to study its effect on hydrogen evolution from
1 M H2SO4 solution at a platinized platinum electrode. In their
study, Walton et al. [52] reported that the effect of sonication
on the removal of gases from the electrode surface improves
the rate of hydrogen evolution. This positive effect of ultra-
sound on hydrogen evolution during electrolysis was also
proved by Mc Murray et al. [53], who used a 20 kHz and 26 W/
cm2 ultrasound generator at a titanium tip sonotrode. In their
study, McMurray et al. [53] assumed that the enhancement in
hydrogen evolution and oxygen reduction is mainly caused by
the enhancement of mass transport. Budischak et al. [54]
coupled a 42 kHz and 300 W ultrasound generator with KOH
electrolysis using platinum electrodes. The results showed
that ultrasound increased the efficiency of the electrolyzer,
especially at intermediate current densities.
Li et al. [55] exposed water alkaline solutions of different
concentrations of NaOH (0.1, 0.5, and 1 M) at a RuO2 and IrO2
plated Ti electrode. Their study demonstrated that an
enhancement in the efficiency of hydrogen generation of the
order of 5% to 18% is achieved. Moreover, 10% to 25% of energy
consumption was saved at high current densities and low
electrolyte concentrations. Similar studies were conducted by
Symes [56] and Zadeh [57] under 20 kHz from mild acidic
(H2SO4) and alkaline solutions (KOH and NaOH) at different
electrode materials (platinum, glassy carbon, industrial car-
bon, 316 stainless steel, and nickel-based electrodes). The re-
sults of both studies showed an enhancement in hydrogen
production due to the increase in mass transport, electrode
cleaning, and degassing. Zadeh [57] observed an improvement
in H2 generation of 14% and 25% for NaOH and KOH electro-
lytes, respectively, when coupling ultrasound to electrolysis
process.
Lin et al. [58] investigated the polarization impedance
phenomenon in water sonoelectrolysis at different concen-
trations of KOH solution, using nickel electrodes. The study
revealed that the sonoelectrolysis process is mainly affected
by ultrasonic power, electrode gap, and electrolyte concen-
tration. The sonication proved to reduce the concentration
polarization and increase the mass transfer. In the same
study, Lin et al. [58] highlighted the importance of lowering
the consumption of electric power and invoked economic
power efficiency, they concluded that even though the inte-
gration of an ultrasound field in electrolysis requires more
material, it still increases the efficiency of hydrogen produc-
tion and decreases energy consumption.
We suggest examining the configurations of the experi-
mental setups adopted in the studies mentioned previously,
Fig. 1 reports the schematics of the different setups.
The analysis of the presented setups reveals that direct
sonication is usually used in sonoelectrolysis. However, each
configuration has its particularity and consequently its
intrinsic effect on the process. For instance, the physical
separation of the anodic and cathodic compartments in the
first configuration (a) [57] improves the purity of the produced
hydrogen, however, it limits the passage of ions within the
electrolytic solution and hence reduces the overall efficiency
of the process. On the other hand, the absence of the physical
separation in the configurations (b), (c), (d), and (f) influences
negatively the purity of hydrogen and may create HHO mix-
tures at an industrial scale.
Furthermore, in configuration (e) [55], the horizontal
placement of the ultrasonic transducer reduces the bubble
detachment from the electrode surface as well as the di-
aphragm's lifetime due to the direct exposition of the dia-
phragm to the ultrasound action and the risk of erosion. To
ensure the effective removal of bubbles from the electrode
surface, the vertical configuration is preferred in such
situations.
Overall, it was proved from the sonoelectrolysis studies
that the effects of ultrasound in the improvement of hydrogen
production yield are rather physical. Therefore, there is an
agreement that in the case of sonoelectrolysis, the combina-
tion of ultrasound irradiation enhances mass transfer [53],
bubble detachment from electrodes surface [52,54,55]
degassing effect [59], and desorption effect [48].
Sonocatalysis
Sonocatalysis is another ultrasound-assisted technique that
is employed for hydrogen generation, based on the combi-
nation of sonication and the catalytic effect of solid catalysts.
This method has been the subject of a few articles reported in
Table 3. Wang et al. [61] investigated the efficiency of
hydrogen generation using the sonication of a methanol/
water solution at 40 kHz and 50 W, in the presence of Au/TiO2
catalyst. Wang et al. [61] assumed that the formation of
hydrogen passes mainly by three pathways: (1) two H

recombined after the cleavage of water molecules, (2) H-
abstraction from methanol by H
produced by water division,
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3 17887

Fig. 1 e Schematics of different setups of sonoelectrolysis for hydrogen production adopted by Zadeh et al. [57] (a), McMurray
et al. [53] (b), Pollet et al. [60] (c) and (d), Li et al. [55] (e), and Lin et al. [58] (f).

and finally, (3) thermal reforming of methanol. Furthermore,
the authors affirmed that Au/TiO2 increased the energy effi-
ciency of the ultrasonic treatment due to its high activity for
the thermal splitting of water and the thermal reforming of
methanol. On the other hand, Singh et al. [62] observed zero
hydrogen production in the dark in the presence of ultra-
sound and CdS (Cadmium sulfide) based catalyst. In addition,
Zhao et al. [63] reported that the introduction of CdS nano-
rods as a catalyst did not change the rate of hydrogen pro-
duced via sonolysis.
17888 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
Table 3 e Synthesis of the principal experimental works dealing with sonocatalysis for hydrogen production.
Author Catalyst Acoustic conditions
Wang et al. [61] Catalyst Au/TiO2 40 kHz and 50 W
Singh et al. [62] rGO supported CdS catalyst 20 kHz, 10e40 W
Zhao et al. [63] CdS nanorods 21, 27, 50 and 68 kHz.
Based on our analysis of the results, the positive effect
recorded in the study of Wang et al. [61] is mainly due to the
chemical effects of sonication which occur under the hot spot
conditions characterized by high temperature and pressure
during the violent collapse of the cavitation bubbles. Thus, the
enhancement in the rate of produced hydrogen was attributed
to the improvement in thermal cleavage of water and reform-
ing of the alcohols. In contrast, Zhao's study [63] revealed that
the combination of ultrasound and catalysts in the absence of
light shows no effect on the hydrogen production process.
Sonoelectrocatalysis
Sonoelectrocatalysis is a hybrid technique known as the
combination of ultrasound and electrocatalysis. Only
recently, this method has been the subject of experiments for
direct hydrogen production, thus, few research studies related
to this topic are available in the literature. For instance, Pollet
et al. [60] realised an experimental work aiming to report the
impact of ultrasound power on hydrogen evolution reaction at
a platinum (Pt) polycrystalline disc electrode in 0.5 M of H2SO4
solution under 26 kHz, and up to 100% acoustic amplitude (up
to 75 W/cm2). Pollet and coworkers [60] stated that under
sonication, the current intensity shifted to a higher value with
an order of about 250% at maximum sonication power, while
the overvoltage decreased with 41.3% at 100% of acoustic
amplitude. Consequently, the hydrogen evolution reaction
was enhanced. According to the authors, this improvement
was attributed to the effect of ultrasound in the detachment of
bubbles from the electrode surface, which diminishes the
bubble coverage of the electrodes and catalysts.
Sonophotolysis
The concept of associating ultrasound and light to enhance
the chemical reaction of hydrogen production was treated by
Cotana et al. [64], who combined sonication at 22.5 kHz and
50 W with simulated sunlight irradiations using a xenon lamp
whose spectrum is very close to sunlight under different static
pressure values (1, 2, and 3 atm). It was observed that at a low
static pressure of 1 atm, hydrogen production increased when
coupling power ultrasounds to light. However, and similarly to
the sonocatalysis technique, sonophotolysis for hydrogen
production faces divergent results. For instance and in
contrast with the aforementioned study, Harada [65] assumed
that the introduction of ultrasound in the sonophotolysis of
Sonicated observation
medium
methanol/water In the presence of Au/TiO2 as a catalyst in
solution addition to methanol as a sacrificial reagent,
the amount of hydrogen evolution increased
Aqueous solution of No hydrogen was detected in the presence of
4 mM Na2SO3 and ultrasound and catalyst and the absence of
10 mM Na2S light
Water The use of CdS as a catalyst in sonolysis does
not change the rate of the produced hydrogen
water results in the reduction of produced hydrogen by
approximately 13.1%.
Recently, Escobar et al. [66] invoked an experimental work
for hydrogen generation using a novel approach by laser
irradiation of metals in water. According to the author, the
proposed technique allows the production of H2 of high purity,
using Ti, Si, Al, Mg, and AleMg alloy metals under 40 kHz and
1064 nm of the laser. In another study, Escobar et al. [25] used
laser ablation and ultrasound under the same conditions of
ultrasound frequency and laser in ambient static conditions,
while the sed materials were Al, Mg, and AleMg alloys with
different Al/Mg ratios. In this study, Escobar assumed that the
simultaneous application of ultrasound and laser ablation
metal enhanced hydrogen production by ~100%, leading to a
production of 23.2 mmol/min per g of metal. The observed
effect was interpreted by the removal of the oxide layer and
the increased temperature on the metal surface inducing
higher activation energy, which leads at its turn to an
improvement in water-metal reaction rate. Therefore, it was
affirmed in another study that a synergy between sonolysis
and photolysis was confirmed and both phenomena assist
each other for hydrogen production [67].
Sonophotocatalysis
The beginning of the sonophotocatalytic decomposition of
water for hydrogen production was with Harada [65], who
combined ultrasonic irradiation of 200 kHz and 200 W and
light, and used powdered TiO2 catalyst. It was observed that
the hybrid process reduces the amount of produced
hydrogen by 26.68% compared to the sonolysis process
(0.796 cm3/h and 1.086 cm3/h using sonophotocatalysis and
sonolysis respectively). Sasikala et al. [68] carried out a
similar experience using an aqueous solution of methanol
and different types of catalysts (metallic, semiconductor
photocatalyst, transition metal oxide, mixed oxide, or insu-
lator material). Under 40 kHz and 200 W, the hydrogen rate
was enhanced due to the increased number of cavitation
bubbles produced in the presence of the suspended mate-
rials, and the efficiency of the scavenging of HOC radicals by
methanol. Luigi et al. [69] investigated the hydrogen pro-
duction by heterogeneous photocatalysis, sonocatalysis, and
sonophotocatalysis in water-ethanol solutions using 0.4 g of
new solid solutions of lanthanum, gallium, and indium ox-
ides suspended in 200 ml and 1100 ml of water/ethanol (10%
vol/vol) solutions. The sonication was performed under
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
38 kHz and 50 W. In their study, Luigi et al. [69] assumed that
the hybrid action of ultrasound waves and light improves the
synergistic effect of hydrogen production, which was
enhanced at high concentrations of suspensions. The syn-
ergetic effect leads, according to the authors, to an
enhancement of 200 times as compared to the photocatalysis
pathway. This effect was even more accentuated within the
200 mL solution, this was attributed to the fact that reducing
the amount of water-ethanol solution decreases the dissi-
pation of mechanical energy of ultrasound in the form of
heat which is useless for water cleavage owing to shearing
movements of the molecules in the medium and viscous
forces. Luigi et al. [69] estimated the value of sound absorp-
tion coefficient which is proportional to the fraction of power
of ultrasound converted into heat.
The enhancement of H2 yield through the sonophotocata-
lytic pathway was also demonstrated by Rossi et al. [67], who
used 38 kHz and 50 W sonication, and ethanol as a sacrificial
agent. Rossi et al. [67] observed a considerable improvement
in the H2 rate which was more pronounced with high con-
centrations of catalyst. The authors noticed an effective syn-
ergy between the sonolytic and the photolytic effects. In the
same context, Penconi et al. [15] investigated the effect of ul-
trasound on water photolysis and compared it to each isolated
process of sonolysis and photolysis. The study revealed that
ultrasound enhanced hydrogen generation, the addition of
ethanol accentuated this enhancement, for instance, the
addition of 20% vol/vol of ethanol in water accelerated
hydrogen production with a factor of 1.4.
Zhao et al. [63] studied the generation of hydrogen via
ultrasound-assisted photocatalytic method under different
ultrasonic frequencies (21, 27, 50, and 68 kHz) using CdS
nanorod arrays as a catalytic. The highest amount of hydrogen
was recorded at the frequency of 27 kHz, which has been
possibly attributed to the fact that 27 kHz is the closest fre-
quency to the resonance frequency of the nanorods used in
the experiments. In the same study, it was affirmed that the
synergy of photoacoustic hydrogen production in the presence
of a catalyst is attributed to the force applied by the ultrasound
source on the photo-generated electrons and holes to move
along opposite directions, respectively, which promotes the
local density of free electrons on the surface of the catalyst.
Similarly, Abbood et al. [70] investigated the possible synergy
of the combination of ultrasound with photocatalysis for
hydrogen production under different ultrasonic frequencies
(55, 45, 55, and 25 kHz). The authors found that the highest rate
of hydrogen was recorded under 45 kHz, they consequently
assumed that 45 kHz is the nearest value to the resonance
frequency of the prepared nanosheets. The study of Abbood
et al. [70] examined the efficiency of hydrogen evolution re-
action using different thicknesses of CdS nanosheet (Accord-
ing to the changes in dimensioning of samples by varying the
amounts of DL-dithiothreitol, the nanosheets fabricated by
adding 0, 2, 4, and 6 mmol of DL-dithiothreitol were denoted as
0-CdS, 2-CdS, 4-CdS, and 6-CdS). The maximum photocatalytic
H2 production was estimated at 1293.62 mmol/g.h and was
detected using the thinnest product 4-CdS. This optimum was
attributed to the increase of the catalytic activity of 4-CdS
under solar and ultrasonic vibrations compared to the other
samples. This was explained by the fact that the combination
17889
of light and ultrasound induces a synergetic effect that en-
hances the photoactivity due to an increase in the active
surface area and the charge separation. The results also
showed that no hydrogen is produced under visible-light
irradiation in the presence of CdS nanorods, while no differ-
ence has been detected in the amount of hydrogen produced
through sonolysis and sonocatalysis. However, the rate of
hydrogen generated from the combination of ultrasound and
visible-light in the presence of Cds increased significantly.
In another study of Singh et al. [62], ultrasound was
coupled to photocatalysis using rGO supported CdS catalyst
under a frequency of 20 kHz at different input powers from 10
to 40 W, in 4 mM and 10 mM of Na2SO3 and Na2S aqueous
solution. An enhancement of 40% was recorded when intro-
ducing acoustic power to the photocatalysis system for
hydrogen production under 20 kHz and 35 W due to the
improvement of mass transfer of hydrogen from the surface
of the catalyst to the bulk. Accordingly, this enhancement was
attributed to the mechanical energy associated with ultra-
sound that causes the detachment of hydrogen bubbles from
the surface of the photocatalyst, making a larger free surface
for higher adsorption of reactants and reactive sites. The ef-
fect of temperature was also inspected in the same study [62],
which reported an enhancement of 70% during sonophoto-
catalysis of water for an increase in temperature from 299 K to
318 K. The authors [62] assumed that the shockwaves and the
mechanical energy generated during the collapse of acoustic
cavitation bubbles are the reasons for the rise in the hydrogen
production rate.
Dharmarathane et al. [71], however, examined the use of
sonoluminescence and sonochemiluminescence generated
from cavitation as in situ photon sources in photocatalysis for
hydrogen production. Using an ultrasound transducer of
355 kHz and 60 W. It was found that sonoluminescence ap-
pears to be an efficient in-situ photon source for photo-
catalytic hydrogen generation. Nevertheless, according to the
authors, the combination of photocatalysis with sonication
remains a complex process from a chemical point of view,
since several side reactions can evolve and limit the optimi-
zation of the overall process.
Controlling parameters
The operating parameters and process configuration should
be carefully selected in order to ensure good performance of
the hybrid process and significant gain in terms of kinetics of
hydrogen production, energy efficiency, and energy-saving for
scale-up applications. The ultrasonic frequency is the major
factor that must be taken into consideration when integrating
sonication into a given technique for hydrogen production. It
is assumed that the mechanical forces exerted by sonication
are directly dependent upon the ultrasonic frequency. The
greatest mechanical effect is generated under low frequencies
[10]. The decrease of ultrasound frequency favors the physical
effects of ultrasound, while at higher acoustic frequency, the
chemical effects of ultrasound remain the dominant mecha-
nisms explaining the role of sonication in the hybrid process.
Accordingly, the optimal ultrasound frequencies applied
during the ultrasound-assisted techniques are of low value
(20, 30, 38, 40, 42 kHz), since in most of the applications, the
17890 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
physical effect of ultrasound would be more required than
sonochemistry. For instance, with sonoelectrolysis and
sonocatalysis, the mechanical energy released from sonicat-
ion exceeds the surface tension force and facilitates the
removal of hydrogen bubbles from the surface, providing a
larger fraction of catalyst and electrode surface for adsorption
[62].
Dissolved gases were frequently used in earlier experi-
ments of sonophotolysis, sonocatalytic, and sonophotocata-
lytic for hydrogen production [67,69,72]. For instance, in
sonoelectrolysis, free volumes of the vessel are usually filled
with argon gas, while electrolytes could be purged with argon
or nitrogen for a specific period during the electrolysis in order
to remove air bubbles from the cell [57,62]. It is established
that the proprieties of dissolved gases influence directly the
sonochemical activity and the kinetics of hydrogen produc-
tion. Basically, the polytropic index and the thermal conduc-
tivity of the gas are the main factors that influence the
thermodynamic conditions of the acoustic cavitation bubble,
and hence, the kinetics of hydrogen production. Overall, an
atmosphere filled with saturated gas of a higher polytropic
index leads to an increase in the temperature of the bubbles at
the instant of collapse, which promotes the sonochemical
activity. Similarly, a lower thermal conductivity decreases the
heat dissipation, which increases the temperature of the
bubble at the collapse [10]. Singh et al. [62] carried out exper-
iments where the electrolyte solution was purged with
hydrogen, and with nitrogen in the presence of a catalyst. It
was observed that in the case of an atmosphere filled with
hydrogen, the total hydrogen production declined dramati-
cally. On the opposite, in the case of the electrolyte solution
purged with nitrogen, the rate of hydrogen production
increased drastically. When the concentration of hydrogen
augments, the rate of desorption of hydrogen significantly
decreased, owing to the progressive accumulation of
hydrogen in the system over time [62].
In addition, sacrificial reagents are commonly used in
sonophotocatalytic, sonocatalytic, and sonophotacalytic pro-
cesses for hydrogen production. The sacrificial reagent should
be selected as a chemical compound that can be oxidized
easier than oxygen and that can reactivate the photocatalyst.
Ethanol and methanol have proved to be the most efficient
reagents for hydrogen evolution reactions [61,67]. The exper-
imental studies dealing with sonophotocatalytic, sonocata-
lytic, and sonophotacalytic assisted with sacrificial reagents
reported an increase in the rate of produced hydrogen
[62,67,69,72]. This was attributed to the fact that sacrificial
reagents, namely methanol, and ethanol, can easily enter the
cavitation bubble, capture H
and scavenge HO
radicals. In
addition, Hydrogen may also be produced through thermal
reforming of methanol and ethanol at the high temperatures
achieved at the hot spots [61].
In terms of energy consumption and possible cost-saving,
and compared to silent technologies for hydrogen produc-
tion, Islam et al. [10] reported that the energy required to
produce 1 m3 of hydrogen is 5.96 kWh with alkaline water
electrolysis, while it may be lowered to 5.06 kWh when it is
combined with ultrasound, which is equivalent to 14%
reduction in energy consumption. Zadeh [57] reported in a
comparative study based on alkaline electrolysis for hydrogen
production that the energy-saving is in the order of 1.3% when
integrating sonication. On the other hand, Li et al. [55]
demonstrated that the energy-saving for H2 production when
combining the ultrasonic field to the electrolysis is about
10e25% for a certain concentration of the electrolyte, with a
high current density. When dealing with pure electrolysis,
Kerboua et al. [27] reported in their study that, for a constant
electric power of 87 ± 5 W feeding the ultrasonic generator, a
molar yield of hydrogen of 5.65 mmol is recorded after 10 mi-
nutes. Clearly, the reported gains in terms of energy con-
sumption per molar unit of produced hydrogen in the
ultrasound-assisted processes are rather explained by the
physical contribution of ultrasound in the combined process,
and not the sonochemical production.
The technological state of the art
Hydrogen being a crucial reactive element in the industry
and energy sector, it has attracted the attention of re-
searchers for several decades. However, the generation of
this substitute using ultrasound at a large scale is limited due
to multiple factors. Ultrasound technology is also known to
be an expensive technique as the cost of sonication equip-
ment is high, nevertheless, with the advancement of the
technology, this cost has been considerably decreased [47]. At
present, ultrasound has been incorporated in a few patents
as ultrasound-based hydrogen production. In 2010, Kirchoff
et al. [73] elaborated a sonoelectrolysis equipment for
hydrogen production designed to reduce the energy con-
sumption as well as increase the mass and volume of the
produced hydrogen. In 2014, Burjanadze [74] invented a
cavitation-electrolysis for hydrogen generation. Burjanadze
assumed that the developed device can enhance the effi-
ciency of hydrogen production and minimize the cost of
hydrogen generation. The presented patents and the previ-
ous results of scientists suggest the use of ultrasound tech-
niques for hydrogen generation as primary methods to be
incorporated in the industrial sector to solve the issues of
energy generation and ensure the independency of fossil
fuels. Although most scientists agree on the positive effect of
ultrasound on chemical reactions in hydrogen production as
an environmentally friendly process, energy efficiency has
often been neglected as a key element to the development of
the technology. In addition, to the best of our knowledge,
literature suffers from the lack in techno-economic analysis
for an industrial application of hydrogen generation using
ultrasound.
Several research articles focused on the design aspects and
geometry of sonochemical reactors as a key for scaling up the
technology. Gogate et al. [75] provided unified selection
criteria for major operating parameters for any feasible
physicochemical changes. Gogate and coworkers assumed
that the distribution of cavitational activity [18], geometric
parameters [76], physicochemical characteristics of the liquid
phase, hydrodynamics, mixing time and mass transfer char-
acteristics are important aspects of the design of the sono-
chemical reactors.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 7 ( 2 0 2 2 ) 1 7 8 7 9 e1 7 8 9 3
Observations and conclusion
The use of ultrasound for hydrogen production as a sono-
chemical process or combined methods has shown several
valuable results, particularly in terms of kinetic efficiency. The
present review gathers the most important findings of re-
searchers in the context of water sonication and ultrasound-
aided pathways for hydrogen production. It is important to
notice that most of the studies related to the combination of
sonication with electrolysis refer to indirect sonication
through an ultrasonic bath, and most of the investigations
applied low acoustic frequencies in the process (20, 30, 38, and
42 kHz). Overall, according to these studies, integrating ul-
trasound power to electrolysis enhances the mass transport,
diminishes the diffusion layer thickness to increase the
limiting current [50], and facilitates the bubble removal from
the electrodes’ surfaces which leads to the drop in the over
voltage, thus enhances the rate of the produced hydrogen.
According to our analysis of results in the case of sonopho-
tocatalysis for hydrogen production, the effects of ultrasound
irradiation are rather physical. These effects are explained by
the improvement of the photoactivity through the augmen-
tation of the active surface area and the charge separation,
which enhances the mass transfer of hydrogen from the
surface of the catalyst to the bulk, and provokes the detach-
ment of hydrogen bubbles from the catalyst surface. This also
augments the adsorption proprieties and reactive sites, due to
the shockwaves and the mechanical energy generated during
the collapse of acoustic cavitation bubbles. It is also worthy to
mention that the literature suffers from the lack of studies
related to sonocatalysis and sonophotolysis techniques which
makes the estimation of the efficiencies of these methods
harder to establish. It is also noticeable that most of the
studies do not tackle the energy efficiency aspects of hydrogen
production. Thus, this track requires deeper investigation in
order to make a clearer vision of the future of sonochemical
and ultrasound-assisted techniques for hydrogen production
from a techno-economic perspective. Finally, it is recom-
mended to carry out more experimental works in the case of
water sonolysis, which was significantly studied through nu-
merical models but very poorly explored through experi-
ments. On the contrary, theoretical investigations should be
developed to describe ultrasound-assisted technologies for
hydrogen production, since most of the works retrieved in the
literature are rather experimental. The scaling up of hybrid
technologies for hydrogen production integrating ultrasound
should pay special attention to the controlling parameters,
based on the judicious selection of operating parameters ac-
cording to the desired physical or chemical effect contributing
to the enhancement of the kinetics of hydrogen production
and the energy efficiency.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
17891
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