Journal of Water Process Engineering 37 (2020) 101378

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Journal of Water Process Engineering

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Understanding of ultrasound enhanced electrochemical oxidation of T

persistent organic pollutants
Ritesh Patidar*, Vimal Chandra Srivastava*
Department of Chemical Engineering, Indian Institute of Technology Roorkee, Roorkee 247667, Uttarakhand, India

ARTICLE INFO ABSTRACT

Keywords: Advanced oxidation processes have gained attention recently due to their effectiveness in mineralizing toxic
Cavitation recalcitrant pollutants. In this paper, studies on combined sonolysis and electroxidation techniques have been
Sonoelectroxidation reviewed for the degradation of the persistent organic pollutants, and real industrial wastewater. The effects of
Hydroxyl radicals various parameters such as ultrasonic power, current density, initial pH, and electrolyte concentration have been
Electrode
elucidated. Critical analysis of the studies (1996-2020) on the treatment of various synthetic and real wastewater
Reactive oxygen species
using the sono-electroxidation process has been considered. Ultrasound, in combination with electrochemical
technology, is an attractive option for the treatment of industrial wastewater. The application of ultrasound gives
the synergistic effect by virtue of the physical and chemical effects of cavitation. Coupling these two techniques
increases the mineralization degree by increasing the mass transport rate and the chemical reaction rate, and
reduce the electrode passivation and fouling problem. Woking with an optimized sonoelectrochemical reactor
design with low power ultrasound with pulsed mode can remarkably decrease the energy cost and increase the
economic viability of the treatment method. Challenges associated with the process are documented in this
paper.

1. Introduction
Industrial wastewater pollution is a worldwide environmental issue
because of the complex composition and other challenging character-
istics of wastewater generated from various industries such as food,
cosmetics, textile, pharmaceutical, pulp and paper industries [1]. Also,
industrial waste containing volatile organic compounds (VOCs), phar-
maceutical and personal care products (PPCPs), petroleum constituents,
and aromatics in wastewater, such as 4-methyl benzylidene camphor
(4-MBC), octocrylene (OC), norfloxacin, ciprofloxacin, triclosan, ben-
zophenone-3 (BP-3, UV filter), galaxolide and tonalide (polycyclic
musk), dankly ethers, methyl-t-butyl ether (MTBE), are frequently re-
leased into the river, ponds, lakes and ultimately contaminating
groundwater and creating a risk for the human health [2]. As far as the
occurrence of these POPs in the wastewater is concerned, it also comes
from the municipal sewage treatment plants. These micropollutants are
mutagenic and hazardous, and their derivatives are even more toxic
than parent compounds. Therefore, the removal of these persistent or-
ganic pollutants (POPs) in wastewater has grown attention among the
scientific community [3]. Various conventional physio-chemical and
biological treatment methods have been applied for the removal of
POPs. However, these methods have their own limitation in terms of
secondary waste generation and poor degradation/mineralization effi-
ciency for the pollutant. The problem of secondary solid waste can be
solved by employing energy-based techniques such as sonolysis (US)
[4], electrochemical (EC) [5,6], and photocatalysis [7] which are called

Abbreviations: AOPs, advanced oxidation processes; ARB, acid red B; BDD, boron doped diamond electrode; BG, brilliant green; CBZ, carbamazepine; CIRB-8, C.I.
Reactive black 8; COD, chemical oxygen demand; DCF, diclofenac; DMP, dimethyl phthalate; DOC, dissolved organic carbon; DSA, dimensionally stable electrode;
EC, electrochemical; %H, hydrogen atom; H2O2, hydrogen peroxide; IBU, ibuprofen; LG-B, lissamine green B; MB, methylene blue; MG, malachite green; MMO, mixed
metal oxide; MR, methyl red; OEP, oxygen evolution potential; OG, orange G; PA, phthalic acid; POPs, persistent organic pollutants; PPCPs, pharmaceutical and
personals care products; PWW, pharmaceutical wastewater; RB-19, reactive blue -19; RB-52, reactive blue -52; RO-7, reactive orange-7; ROS, reactive oxygen species;
RY-125, reactive yellow-125; SE, synergistic effect; SMX, sulfamethoxazole; SSE, stainless steel electrode; TCAA, trichloroacetic acid; TOC, total organic carbon; US,
sonolysis; US-EC, sonoelectroxidation; k, pseudo first order rate constant; kEC, pseudo first order rate constant of electrolysis (min−1); kUS, pseudo first order rate
constant of sonolysis (min−1); kUS-EC, pseudo first order rate constant of sono-electrolysis (min−1); t1/2, half-life time (min); $, dollar; %, percentage; %OH, hydroxyl
radicals; 1O2, singlet oxygen; 2-4-D, 2-4-dichlorophenoxyacetic acid; 2-4-DC-Phenol, 2,4,dichlorophenol; 3O2, triplet oxygen; F, frequency; Hr, hour
⁎
Corresponding authors.
E-mail addresses: riteshpatidar@gmail.com (P. Ritesh), vimal.srivastava@ch.iitr.ac.in, vimalcsr@yahoo.co.in (V.C. Srivastava).

https://doi.org/10.1016/j.jwpe.2020.101378
Received 18 March 2020; Received in revised form 12 May 2020; Accepted 15 May 2020
Available online 18 June 2020
2214-7144/ © 2020 Elsevier Ltd. All rights reserved.
P. Ritesh and V.C. Srivastava
advanced oxidation processes (AOPs) [8]. The most commonly used
AOPs for the removal of POPs in wastewater are Fenton and Fenton-like
[9], EC [10], photocatalyst [7,11], ultrasound-based oxidation [12],
ozonation [13], etc. These all AOPs generate the different reactive
oxygen species (ROS) such as hydroxyl radicals (OH%), singlet oxygen
(1O2), triplet oxygen (3O2), etc. [14–16]. Oxidation potential of these
radicals (such as standard redox potential of %OH is E° = +2.8 V vs.
SHE) towards the pollutant degradation is high [17]. Therefore, these
radicals can degrade most of the organic pollutants with the rate of the
order of 106–109 L (mol.s)−1 [18]. As an individual technique, ultra-
sound takes a long time for the complete mineralization of the pollutant
[19], and EC techniques suffered from the electrode passivation, in-
activation, and polarization problem [20–22]. Recently sonoelectrox-
idation (US-EC), an integrated technology of ultrasound and EC, has
gained attention as a new hybrid AOP for the removal of recalcitrant
organic pollutants. A significant improvement in the oxidation effi-
ciency of the pollutant have been reported using the US-EC technique in
the literature. Apart from pollutant oxidation, the US prevents the de-
position of the by-product on the electrode surface, increases the mass
transfer rate and current efficiency, and reduces the energy consump-
tion for the complete mineralization of the pollutant [23]. Therefore,
the coupling of ultrasound with EC technology not only provides the
enhanced efficiency for the pollutant degradation but also increases the
life of the electrode and reduces the cost of the treatment. Over the past
decades, several studies have been devoted to the removal of POPs
using US-EC techniques [1,8,23–27]. These techniques reported that
ultrasound induces the chemical, biological, and mechanical changes in
the medium due to the physical and chemical effect of the cavitation
[26]. Hence ultrasound could effectively make up the shortcoming of
the EC techniques alone.
In this review paper, progress in US-EC technology for the de-
gradation/mineralization of the various organic waste in the last
decade has been reviewed, and various challenges are discussed in
depth.
2. Sonoelectrolysis and its Mechanism
2.1. Mechanism of sonolysis
Sonolysis is an advanced oxidation process in which ultrasound
waves are used for the degradation of the pollutants present in the
wastewater. Ultrasound is nothing but a sound wave having a frequency
higher than the human audible frequency of 16 kHz [27]. Fig. 1 shows
Fig. 1. Sonolysis degradation mechanism of organic pollutants.
2
Journal of Water Process Engineering 37 (2020) 101378
US degradation mechanism of organic pollutants.
Ultrasound mechanism for the degradation of pollutants based on
acoustic cavitation, which is a phenomenon of formation, growth, and
transient collapse of microbubble in the liquid medium [28]. When
ultrasonic wave passes through the irradiating medium, compression,
and expansion cycles of ultrasonic waves continuously exerted positive
and negative pressure on the liquid [29]. During the negative pressure,
microbubble expand, and during positive pressure, microbubble com-
press. This expansion and compression cycle continues till negative
pressure sufficiently is large enough to pull the liquid molecules from
each other to the threshold limit. Hence, cavities filled with gas and
vapor get formed, cavitation bubble gets formed, and the bubble grows
in size over a few-cycle, and finally, explosive collapse occurs. This
transient collapse generates a temperature of 5000 K and pressure 1000
atm leading to the thermal dissociation of water molecules into %OH
and %H radicals (as shown in Eq. 1–5) [30–32]. Sonolysis reaction oc-
curs inside the cavitation bubble at the interface of the cavitation
bubble as well as in bulk. At the surface of the transient bubble, the
concentration of the %OH radicals is comparatively high. At the time of
the collapse, these radicals eject to the bulk medium where it reacts
with the pollutant and decomposes it. Another mechanism of US oxi-
dation is the pyrolysis of the organic pollutant, which takes place under
high temperature and pressure inside the cavitation microbubble. Hy-
drophobic types of the pollutants get inside the microbubble where
oxidation of the pollutant takes place under higher temperatures (500
K) and pressure (1000 atm) [28].
H2O +))) (Ultrasound)→ %OH + %H (1)
%
OH + H→ H2O
%
(2)
%
H + O2→ %HO2 (3)
%
OH +%OH → H2O2 (4)
2 HO2→ H2O2+O2
%
(5)
O2+)))→ 2 O %
(6)
2.1.1. Limitations of US alone
Few studies have been reported which show the degradation of
organic pollutants using the US alone [33–38]. However, complete
mineralization of pollutants such as phenol, and its derivative, PPCPs
products, and nitrogenous compounds (nitrobenzene, aniline, and
pyridine) is not well-reported using the US alone [8]. US alone is not an
P. Ritesh and V.C. Srivastava
efficient process for the degradation of all types of recalcitrant pollu-
tants because %OH radicals generated from the collapse of microbubble
gets recombined at the gas-liquid interface before being ejected into the
bulk solution. Therefore, oxidation of the pollutants will not take place
in the bulk medium by %OH radicals. Nature of the pollutant (hydro-
phobic or hydrophilic) and its degradation mechanism (inside cavita-
tion bubble, gas-liquid interface, and bulk medium) is important for the
complete mineralization of the pollutants using the US alone [29].
Further hydrophilic pollutants do not get inside the cavitation bubble
due to which direct pyrolysis of the pollutants does not occur inside the
cavitation bubble. Therefore, complete degradation of the pollutant will
not occur using the US alone. Further energy consumption limitation at
the higher frequency ultrasonic horn and higher ultrasonic power re-
strict the application of ultrasound in the low-frequency range
(20−100 kHz) and low ultrasonic power range (40−120 W) due to
which wide application of US alone on variety of pollutants is not
feasible.
2.2. Synergistic mechanism of US-EC techniques
EC process, individually, also suffers from the limitation of the mass
transport passivation of the electrode, which decreases the efficiency of
the electrode. Therefore, coupling ultrasound with electrochemical
technology can be a viable option to overcome the weakness of the US
and EC alone [39]. Fig. 2 shows the sono-electroxidation degradation
mechanism of refractory organic pollutants. Ultrasound, in combination
with the EC, provides the synergistic effect via physical and chemical
effects of ultrasound. Irradiation of the electrochemical cell using ul-
trasound produces physical effects such as microjet, shock wave, tur-
bulence and acoustic streaming of ultrasound provide in-situ cleaning
of electrodes, increase the rate of chemical reaction, increase the mass
transfer of the pollutants across the electrodes and reduce the diffusion
layer thickness to several micrometers. Simultaneous effect of all these
significantly increase the mineralization degree, reduce the passivation,
and increases the life of the electrode. Further chemical effects of ul-
trasound increase the rate of formation of reactive hydroxyl radicals (%
OH), which react with the pollutant either in bulk medium or at the gas-
liquid interface [40]. Therefore a positive synergistic effect always
Fig. 2. Sono-electroxidation degradation mechanism of refractory organic pollutants.
3
Journal of Water Process Engineering 37 (2020) 101378
exists when ultrasound is used in combination with electrolysis. Fur-
ther, due to the physical effect, some part of the ultrasound energy gets
absorbed by the liquid medium. This results in the mechanical mo-
mentum of the liquid (acoustic streaming) due to which Faradaic cur-
rent and mass transfer of electroactive compound increases [39]. The
transient cavitation results in uneven and violent motion of the solution
due to the mutual interaction of collapsing and oscillating bubbles. The
ultrasound increases the mass transport of the reactant to the electrode
surface, enhances the efficiency of the electrochemical cell, and keeps
the electrode clean and activated [39]. Ultrasonic frequency and anode
material play an important role in the synergism of the process. It was
reported by Compton et al. [41] that higher ultrasonic frequency favor
the chemical effect of the ultrasound, i.e., higher rate of formation of
the %OH radicals while low frequency supports the mechanical effects
such as the generation of a shock wave which results in an enhancement
in the mass transfer and in-situ activate the electrode [42]. This effect
results in an enhancement in electrolysis current due to which yield of
electrolysis changes, i.e., more than one reaction pathway with dif-
ferent rates.
2.2.1. Sono-electrocoagulation
Electrocoagulation (ECG) is a versatile technique for the treatment
of a variety of wastewaters such as oil tanning [43], car-washing [44],
gray [45], olive-oil mill [46] pulp and paper mill [47] distillery
[48,49], terephthalic acid [50], dairy [51], and dye [52–55] However,
electrode passivation, which increases the resistance and reduces the
releases of the coagulation material, has been reported to be the main
electrode problem during the treatment. Electrode passivation increases
the cell voltage and decreases the current efficiency due to which the
cost of treatment increases. Many investigators have coupled the ul-
trasonic process with ECG to prevent passivation. [44,45,56,57]. Li
et al. [57] reported the beneficial effects of the US in combination with
the ECG technique. US significantly improved the phosphorus removal
efficiency (99.6 %) from synthetic wastewater as compared to 81.3 %,
using ECG only. The synergistic effect of the US in combination with the
ECG was attributed to: (i) the mechanical effect of the US, which de-
structs the dense layer of byproduct deposition on the electrode surface,
and (ii) enhanced hydroxide formation with increased adsorption of
P. Ritesh and V.C. Srivastava
pollutants. Vianney et al. [54] studied the degradation of azo dyes
(methyl red and congo red) from aqueous solutions using US-ECG
process. US alone gave 9.55 % decolorization, ECG gave 40.75 %, and
US-ECG gave 100 % decolorization of congo red dye in 20 min. The
higher performance of US-ECG was attributed to the increased pro-
duction of the %OH radicals by the US process, which attack the N]N
bond of azo dye. In another study, Raschitor et al. [55] reported 92 %
rhodamine 6 G removal efficiency with US-ECG as compared to 60 %
efficiency in the ECG process in 5 h treatment time. Turbidity removal
of the wastewater also found to increase with the coupling of the US
with the ECG process. He et al. [56] reported that the US-ECG increases
the removal efficiency of RB19 by 7 % over the conventional electro-
coagulation process. The author also reported that during the ECG
process, electrode impedance increased while it decreased during the
US-ECG. This indicated that the passive film gets removed from the
sacrificial electrode using the US due to which sacrificial electrode can
generate more coagulant metal. Besides, the US also decreased the size
of the metal hydroxide, which adsorb more pollutants in wastewater.
Dizge et al. [48] worked on brewery wastewater treatment using US-
ECG, which enhanced the COD removal to 60.5% as compared to 46.5%
using ECG alone at the optimum condition of 100 A m−2, pH 7 and
reaction time of 60 min. US enhanced radicals generation rate, there-
fore higher reaction rate and pollution removal efficiency was obtained.
Further US also affects the particle size, formation of refractory com-
pounds, and organic material structure.
Some studies report negative impacts of US in combination with
ECG as well. Lakshmi and Sivashanmugam [43] reported the treatment
of oil tanning effluent by US assisted ECG technique using aluminum
(Al) and iron (Fe) sacrificial electrodes. In this study, the US showed an
adverse effect on the mineralization efficiency. COD removal of 90 %
was obtained using ECG, which decreased to 86 % using US-ECG;
however, sludge generation increased from 0.49 kg m−3 using ECG to
0.9 kg m−3 using US-ECG. US didn’t allow the formation of flocs, and
only anodic dissolution and mixing was occurring, which decreased the
COD removal efficiency. The increase in sludge generation was attrib-
uted to the fact that the US reduced the diffusion layer thickness at the
electrode surface and increased the current efficiency, thus increasing
the formation of metal ions, thereby enhancing metal hydroxide gen-
eration. In another reported study, the US couldn’t significantly influ-
ence the COD removal efficiency for the treatment of greywater [45]
3. Sonoelectroxidation of organic pollutant
A number of researchers have worked on the degradation of the
pollutants using the US-EC process [1,8,23–26,58,59]. This section
presents the work done on the degradation of dyes, pharmaceutical
compounds, aromatics, and phthalates employing the US-EC method. A
conventional US-EC reactor which described the simultaneous removal
of pollutant is shown in Fig. 3.
3.1. Dyes
Textile industries are considered as the primary source of the dye
wastewater, producing units that pollute the natural streams [60]. Dyes
are difficult to remove by conventional physicochemical methods [61].
Therefore, as an alternative, AOPs such as photocatalytic degradation
[62], ozonation [63], and EC [5] are found to be prominent techniques
that can successfully mineralize the dyes containing industrial effluents.
Percentage degradation of the dyes through the US, EC, and US-EC
process reported in different studies are depicted in Fig. 4. It was found
that the US alone is not accomplished enough for the removal of these
dye. The EC process has shown some restrictions on the scale-up of the
process due to the limitation of the mass transfer, electrode fouling, and
passivation problem [64–66]. Therefore, the coupling of ultrasound
with EC oxidation can be a viable technique, which provides a sy-
nergistic effect (SE) on degradation efficiency. Many studies reported
4
Journal of Water Process Engineering 37 (2020) 101378
almost 90 % removal of dyes using the US-EC oxidation process
[8,42,67,68]. Table 1 presents a comparative assessment of studies on
the degradation of dyes using the US-EC process [69–81]. Some re-
cently published literature for mineralization of dyes using the US-EC
process is discussed herein.
Lorimer et al. [81] showed degradation of the sandolan yellow dyes
through ultrasonic assisted electroxidation with platinum and carbon
electrode. Ultrasound, when operated alone, at two different fre-
quencies of 20 kHz, and 40 kHz, did not decolorize the acidic sandolan
yellow dyes; moreover, the dye also resisted 0.5 mol dm−3 of H2O2.
Decolorization of sandolan yellow was obtained using the addition of a
sodium hypochlorite solution. The rate of decolorization was much
quicker by electrolysis alone using a platinum electrode as compared to
the carbon electrode.
The effect of different types of electrode (Ti, Cu, Al, Ni, graphite,
and stainless steel) on the degradation of cyanide ions was studied by
Iordache et al. [80]. Highest electroxidation efficiency (22 %) was
obtained using the graphite electrode and lowest 10% with the Ti
electrode. US-EC efficiency was the highest 60% with aluminum elec-
trode while the lowest using graphite (Fig. 5). Aluminum was found
most efficient electrode with sonoelectro-chlorination with 78% effi-
ciency, and graphite was found to be the least efficient electrode. The
efficiency of the electrodes was in the order: graphite < Ti < Inox <
Ni < Cu < Al for the sono electroxidation of cyanide ions. In another
study by Chua et al. [79], the mineralization of cyan ink effluent was
carried out using two-step treatment. Step one used combined oxidation
of the ultrasound-assisted EC process, and step second used chemical
oxidation process, which involved FeSO4 and H2O2. The US alone
provided no significant reduction in response to COD, copper content,
and color removal after 3 h treatment time. US, in combination with the
Fenton process, provide 45 % COD removal that was more than Fen-
ton’s process alone. In the two-step treatment of cyan ink effluent, a 65
% reduction of copper content, 20 % COD reduction with 98 % re-
duction in sludge generation was reported in 3 h treatment time. Fen-
ton’s process alone produced 6.7 g COD−1 sludge due to the less
amount of FeSO4 requirement at the second stage, and highly acidic
conditions of the treated effluent lead to higher solubility of the product
for iron sludge. Treated effluent by the two-stage process also met the
copper discharge limit with less disposal cost of sludge, which is an
advantage over Fenton’s process. Rivera et al. [78] removed acid black
24 (AB-24), LG-B, MO, and trupocor red (TR) dyes using the US-EC
technique with a graphite electrode. The application of the ultrasound
(for degassing and activation of electrode surface), in combination with
the EC techniques, increased the decolorization and COD removal of the
various dyes. Degradation of AB-24 was higher (50.18 %) using the US-
EC process as compared to the EC treatment alone (20.76 %). COD
removal was 19.05 % and 14.28 % using US-EC and EC techniques. LG-
B degradation was also observed in the continuous mode of the US-EC
technique and found that LG-B decolorization was 95 % at the optimum
condition of 0.0025 mol L−1 of Na2SO4 with total reflux of 4.5 mL
min−1 after 2 h treatment which was almost four times than EC
treatment. The difference in the removal percentage of these dyes was
due to the types of chromophore present in dye structure. Mono-azo
(LG-B) can be easily breakable than di-azo (AB-24). On the other hand,
Ai et al. [77] investigated the decolorization of rhodamine B (RhB) azo
dye using the US-EC process. The decolorization of RhB using the US
alone is not possible. However, 24.5 % of decolorization was obtained
using electrolysis alone, and 91.4 % degradation was reported using the
sono-electroxidation process. Reported results clearly showed the SE of
the combined process. Since the lower frequency of ultrasound were
used in the study, therefore, %OH radicals produced were less, and only
chemical effect of ultrasound is not enough for the synergetic de-
gradation, roll of physical effect was also important which improved
the decolorization rate by an increase in the activity at the surface of
electrode (cleaning and peeling) and increased the reaction rate of mass
transfer. Siddique et al. [76] investigated the decolorization of RB-19
P. Ritesh and V.C. Srivastava
Fig. 3. Conventional US-EC reactor for the treatment of refractory organic pollutants.
Fig. 4. Percentage degradation of various dye pollutants using ultrasound, EC,
and US-EC technique. RB-5 (Reactive Black 5), OG (Orange-G), CIRB-49, (CI
Reactive Blue49), RB-49, (Reactive Blue-19) [71,76,78].
using the PbO2 electrode for the US-EC process. His research group
found that the US-EC process is an effective technique in terms of en-
ergy consumption and decomposition of RB-19. About 90 % decolor-
ization with 56 % TOC removal was reported at the optimum condition
of pH 8, 80 kHz ultrasonic frequency, 120 min treatment time, and 50
mg L−1 dye concentration. 81 % TOC removal was observed with hy-
drolyzed dye. Reported results confirmed the synergism in the com-
bined strategies of the US-EC process.
Wu et al. [75] did studies on operation parameters (current density,
pH, initial dye concentration, and electrolyte concentration) for deco-
lorization of CI reactive black 8 (CIRB-8) by Ti/RuO2-IrO2 anodic oxi-
dation with and without ultrasound. With ultrasound alone, negligible
color removal was obtained. Later Siddique et al. [76] also reported
only 13 % degradation of RB-19 dyes using the US alone. Wu et al. [75]
found COD removal of 32.4 % and CIRB-8 removal efficiency of 62.9 %
at optimum condition of 31.7 mA cm−2 current density for initial dye
concentration of 100 mg L-1, 5.4 pH, 90 min treatment time, ultrasonic
power of 100 W L-1 and 0.1 mol L-1 electrolyte concentration. En-
hancement factor (ratio of the rate constant of the US-EC process to EC
process) using the US-EC process was greater than one, which shows
that ultrasound irradiation enhanced the decolorization with EC oxi-
dation process. Observed enhancement was due to the increase in tur-
bulence and mass transfer of the pollutants [82]. Somayajula et al. [74]
worked on the decolorization of reactive red 195 (RR-195) by the US-
5
Journal of Water Process Engineering 37 (2020) 101378
EC method with the MMO mesh type electrode. About 91 % decolor-
ization was found with the EC process, and 99 % decolorization was
reported with the US-EC process after 120 min treatment time. Lounis
et al. [70] reported only 3 % decolorization of OG using ultrasound
alone while 90 % removal after 30 min with EC treatment. Somayajula
et al. [74] reported COD removal of 23 % using US-EC and 14 % using
EC alone. The effect of electrolytes concentration on decolorization was
also investigated. NaCl and KCl provided 99 % decolorization of RR-
195 in 120 min as compared to 52 % and 39 % decolorization with
Na2SO4 and Na2CO3, respectively. The increase in treatment efficiency
with the use of electrolytes was the production of hypochlorite ions by
NaCl and KCl. Wu et al. [75] also reported that the presence of a high
concentration of Na2SO4 in solution results in the scavenging of O%H
radicals by the sulfate ions.
Yang et al. [73] assessed the effect of the nano-coating electrode on
the degradation efficiency of methylene blue (MB) using the US-EC
process. At the optimum condition (45 kHz frequency, 50 W power, and
600 mA current), TOC removal efficiency was 92 % with a nano-coated
electrode while under the same operating condition. 70 % TOC removal
was obtained using a conventional electrode. Shestakova et al. [67], for
the first time, analyzed the modified electrode for the degradation of
the MB dyes. His research group assessed the sono-electrocatalytic re-
moval of the MB dye using the Ti/Ta2O5-SnO2 electrode prepared using
the drop-casting technique. About 100 % removal of MB was reported
at the optimum frequency of 850 kHz after 45 min treatment while the
US alone took 90 min, and electrolysis alone took 180 min for complete
removal of MB dye. COD removal was 78.9 %, 40.4 %, and 85.4 % using
electrolysis, US, and US-EC process, respectively. The energy con-
sumption of the process was found to be 141.26 kW h m−3 for 0.025
mM MB dye. These published studies were in agreement with the study
reported by Barros et al. [68]. They found almost 90–95 % color re-
moval of amaranth dyes using BDD anode after 90 min US-EC treat-
ment, while only 8 % amaranth dyes removal was seen using the US
alone. The performance of the US-EC process at lower current density
(10−25 mA cm-2) was found to be more effective. Therefore energy
requirement of the process at lower current density was also found to be
less (20 kW h kg-1 dye removed) compared to the reported by Shesta-
kova et al. [67], which is about 141.26 kW h m−3. On the other hand,
 Table 1
Typical studies of US-EC oxidation of various dyes.
Pollutant
Dyes
C.I Reactive Blue 49
Alizarin Red S (ARS)
Orange-G (OG)
CI Reactive Blue 49 (RB-49)
Methylene Blue (MB)
Amaranth Dye
6
Amaranth Dye
Methylene Blue (MB)
Reactive Red 195
CI Reactive Black 8
Reactive Blues -19
Rhodamine B solution (Rh –B)
Trupocor Red, Reactive Black
5,
Lissamine Green B, Methyl
Orange and Acid Black 24
Experimental Conditions
Electrodes
Anode:- Platinum
Cathode:- Carbon
Anode:-Boron Doped Diamond
Electrode
Cathode:-Stainless Steel
Anode:- Platinum grid
Cathode:- Carbon Felt Dimension (6 ×
2.5 × 1.1 cm)
Anode:- Carbon Electrode, auxiliary
electrode:- Platinum
Anode:-Ti/Ta2O5-SnO2
Cathode:-Ti plate
Anode:-Boron Doped Diamond
Electrode Cathode:-Platinum wire
Electrode:- Anode:-Boron Doped
Diamond Electrode
Cathode:-Platinum wire
Anode:-RuO2-IrO2-TiO2/Ti
Cathode:- Stainless steel.
Electrode:- MMO Mesh type surface
area 42 cm2
Anode:-Ti/RuO2-IrO2 (31.5 cm2)
Cathode:-Stainless Steel (31.5 cm2)
Anode:- Lead oxide (14 × 15cm2)
Cathode:-Stainless Mesh Steel
Anode : Pt sheet (2 cm2), Cathode :
Active Carbon Fiber (ACF) (3.0 cm2)
Electrode:-Graphite (Effective 7 cm2)
Ultrasound
f =35 kHz, P = 150 W cm-2
f = 20 kHz, P = 100 W
f =22.5 kHz, P = 15 W
f=35 kHz
P = 150 W cm-2
f = 20 kHz (Probe)
40 kHz (Bath)
f = 20 kHz (probe)
ultrasonic intensity = 523 W
cm-2,
f = 20 kHz \ultrasonic
intensity = 523 W cm-2,
P = 250W
f =45 kHz, P = 250 W
f = 850 kHz, P = 39.54
f = 20 kHZ, P = 250 W
f = 80 kHz
US Source : f =22 kHz, P =
400 W
f = 20 kHz, P = 60% with
cycle 10%,
Other condition
pH = 8.3, concentration of dye = 10 mg
L−1, voltage = 0.7 V and t = 80.6 min
ARS = 100 mg L-1, 0.05 M Na2SO4
electrolyte, T=30 °C and pH = 4.97
t=3 h.
OG = 0.04 mM, V = 150 mL, pH = 3.0,
Na2SO4 = 0.05 M, electric
Current = 100 mA, voltage = 4.0 V, Fe(II)
= 0.05 mM
RB-49 = 10 mg L-1, H2O2 = 3 mol L-1, t
=90 min.
T =25 °C, Current 20 mA,
MB = 0.025 mM and 0.1 M Na2SO4
T = 25 °C Current Densities:-10-50 mA cm-
2
, Amarant Dyes = 100 mg L-1 in 0.05 M
K2SO4
T = 25 °C
Densities:-10-50 mA cm-2, Dyes = 100 mg
L-1 in 0.05 mol L-1 K2SO4, pH = 12, t =90
min.
MB = 200 mg L-1, V = 600 mL, current
intensity = 600 mA.
Current Density = 1 to 5 mA cm-2,
RR-195 = 100 ppm, t = 50 min,V = 500
mL, electrolyte = 1.51 g L-1
T = 20 °C, RB8 = 100 mg L-1,
Na2SO4 = 0.1 mol L-1, Current Density
=31.7 mA cm-2, pH = 5.4, Electrode gap
= 3.8 cm
RB-19 = 50 mg L-1, pH = 8,T =120 min
pH = 7, T = 25 °C (bath) Na2SO4 = 21.3 g
L-1 applied potential 4.0 V
Na2SO4 = 0.0025 mol L-1 and total reflux
4.5 mL min-1
Treatment Efficiency References
4% removal using US, 53.4% removal using EC and 91% removal using [69]
P. Ritesh and V.C. Srivastava
US-EC
100% color removal and 86.07% COD removal [1]
3% degradation using the US alone. [70]
90% degradation was obtained with electrolysis.
100% degradation using US-EC oxidation.
99% decolorization and 87% TOC removal using US-EC with H2O2. [71]
95% decolorization and 76.2% COD removal using US-EC without H2O2.
64% decolorization using US with H2O2 at pH 2.0 51% decolorization
using EC with H2O2
85.4% COD removal with US-EC [67]
78.9% using electrolysis
40.4% using US process.
38.4% TOC removal using US-EC.
99% color removal using US-EC process. [72]
50% decoloration obtained using EC process.
92.1% TOC removal using EC process.
95.1% TOC removal using the US-EC process.
8% removal using the US process. [68]
90% removal using US-EC treatment.
98% TOC removal using the US-EC process.
96% TOC removal using EC process
92% TOC removal using the US-EC method with Nano coated electrode [73]
while 70% TOC removal with non-Nano-scale electrode.
50% TOC removal with EC process with both types of electrode.
99% Decolorization using the US-EC method. [74]
91% decolorization using EC process
58.3% COD removal using the EC method
63.74% COD removal using US-EC.
32.4% COD removal and 62.9% degradation with US-EC process. [75]
90% Color Removal and 56% TOC removal using US-EC method. [76]
91.4% decolorization of RhB using US-EO within 6 min while complete [77]
decolorization in 12 min at optimum condition.
0.4% decolorization using the US alone.
24.5% using Electroxidation process
Acid Black 24 : 50% decolorization and 19% COD reduction. Lissamine [78]
Green B : 95% decolorization and 60% COD reduction,
Methyl Orange : 84% decolorization and 27% COD reduction, Reactive
Black 5 : 73% decolorization and 21.5% COD reduction, Trupocor Red :
80% decolorization and 24% COD reduction
(continued on next page)
Journal of Water Process Engineering 37 (2020) 101378
P. Ritesh and V.C. Srivastava Journal of Water Process Engineering 37 (2020) 101378

References

[79]

[80]

[81]
98% reduction in the amount of sludge generated after 3 hours two-step

22% electroxidation efficiency using graphite electrode and 10% using Ti

97% decolorization by addition of sodium hypochlorite solution.

65% reduction in copper content and 20% COD reduction.

60% US-EC efficiency using aluminium electrode.

No decolorization with ultrasound alone.

Fig. 5. Percentage degradation of cyanide using different electrodes by EC and

US-EC process. Al (Aluminium), Cu (Copper), Ni (Nickel Inox), Ti (Titanium),
Source [80].

Steter et al. [72] reported 100 % decolorization of amaranth dyes using

the BDD electrode at lower current densities of 35 mA cm-2. Energy
Treatment Efficiency

consumption was found to be 5.3 kW h m-3 using a US-EC reactor. The

TOC removal was 92.1 % using EC and 95.1 % for the US-EC process at
the optimal current density of 35 mA cm-2. Steter et al. [72] found that
electrode.
treatment

at low current densities (10−25 mA cm-2), the apparent rate constant

was higher for US-EC techniques (10-1 min-1) as compared to EC alone
(10−3 min-1). With an increase in the current density from 10 to 50 mA
pH = 7.0, H2O2 = 35 wt percentage, T =

cm-2, current efficiency decreased from 55 % to 20 %. The positive

CN- = 0.1 mg mL NaCl = 0.1 mg mL ,
-1

Current 100 mA, Supporting electrolyte

synergetic effect was found at lower current densities as compared to a

higher current density due to saturation of the solution by oxygen and
Current Density = 0.03 A dm-2

proxy radicals, which increased the formation of oxidizing species like

H2O2 and oxygen. Lounis et al. [70] investigated the effect of operating
parameters such as ultrasonic power, current density for degradation of
NaCl = 0.2 mol dm-3.

OG dyes using the US-EC reactor. Platinum (anode) and carbon felt
-1

(cathode) was used as an electrode. It was found that with an increase

T = 30 to 35 °C
Other condition

in the ultrasonic power from 4 to 15 W, removal efficiency increased to

T = 60 °C

100 % at 15 W within 8 min. However, a further increase in power

showed no significant effect on the mineralization of OG dye. Ai et al.
25 °C

[77] also assessed the ultrasonic power effect on rhodamine B (RhB)

decolorization. It was found that with an increase in ultrasonic power
f =35 kHz (bath), P = 240

from 100 to 400 W, decolorization of RhB increased while further in-

f = 20 kHz and 40 kHz,

crease in power up to 800 W decreased the decolorization. This may be

due to the delay in the growth of the cavitation bubble and long col-
lapse duration leading to scavenging and recombination of O%H radi-
cals, ultimately decreasing the degradation at the higher ultrasonic
Ultrasound

f =37 kHz

P = 22 W

power. Lounis et al. [70] reported that with an increase in the pH value
from 3 to 6, OG decolorization decreased due to the reduction in the
W

oxidation potential of hydroxyl radical. At pH 3, USEC degradation was

higher than at pH 2 due to the scavenging of O%OH radicals by hy-
Anode:-Mild steel (Grade SS41) 15 cm

Electrode:- Ti, Cu, Al, Ni, Graphite and

length and 3 mm thickness and 24 mm

stainless steel with 0.5 dm3 surface

drogen ion at lower pH. Lounis et al. [70] also studied the effect of
Cathode:- 15 cm length and 3 mm

Electrodes: -Carbon and platinum

pollutant concentration on the performance of US-EC reactor. They

thickness and 37 mm width

found that OG percentage removal decreases from 92 % to 87 %, with

Experimental Conditions

an increase in the concentration of the dye (0.6 mM to 0.8 mM). Wu

et al. [75] reported that with an increase in the concentration of dyes
from 50 to 200 mg L-1, the rate-constant value decreased from 0.0098
min-1 to 0.0081 min-1 for electroxidation process while values de-
Electrodes

creased from 0.0113 min-1 to 0.0101 min-1 for US-EC process. These
width

results were found opposite to that reported by Ai et al. [77] during the
study of the degradation of RhB dyes. They reported that by changing
the initial concentration of RhB dye from 10 to 50 mg L-1, the efficiency
of removal of RhB was not affected. Barros et al. [68] reported pseudo-
Synthetic Cyan Ink Effluent

first-order kinetic constant value of 4.6 × 10-2 min-1 for US-EC treat-
ment and 3.5 × 10-2 min-1 for electroxidation treatment. Mineraliza-
Table 1 (continued)

Sandolan Yellow

tion efficiency was 95 % for the US-EC process, and 80 % for the EC
process. Ultrasound enhanced the mineralization of the pollutant.
While the US alone was not able to mineralize the pollutant as TOC
Pollutant

Cyanides

removal of 19 % only was observed. Ai et al. [77] also reported that the
US alone is not enough to degrade the textile dyes such as RhB.

7
P. Ritesh and V.C. Srivastava
Lounis et al. [70] show that with increases in current (30 to 100
mA), OG removal percentage increases. Results obtained were in
agreement with the study of Yang et al. [73] they reported that with an
increase in current (150 to 600 mA) mineralization increases while
further increases in the current slightly increase in TOC reduction. The
possible reason is that the high applied current increases the rate of
H2O2 generation, which further decomposed to O%H radicals through
the cavitation phenomena. Similarly, with increases in the concentra-
tion of Fe (II) ion (0.03 to 0.05 mM) degradation rate was increased
from 8 μM min−1 to 13.6 μM min−1. The increases in removal rate due
to the increase in the production of O%H radicals by electro Fenton
while it was also seen that further increases in the concentration of the
Fe(II) ions from 0.05 mM to 0.5 mM OG degradation decreases due to
scavenging of O%H radicals by Fe(II). Giray et al. [83] look ahead for
degrading the real textile wastewater using the sonoelectrofenton pro-
cess and reported 98.12 % TOC removal. The effect of water matrices,
such as seawater, pure water, and mineral water, was also reported by
Lounis et al. [70]. About 100 % degradation was obtained after 8 min in
seawater because of a high amount of NaCl (35 g L−1), which lead to
the production of hypochlorite ions while 94 % was obtained in 20 min
for mineral water with US-EC treatment. These results were in agree-
ment with the studies of Ai et al. [77]. They reported the effect of
electrolyte concentration on decolorization of RhB. They found that
with 21.3 g L−1 Na2SO4 electrolyte concentration, 100 % decoloriza-
tion was obtained in 12 min.
Radi et al. [71] studied the removal of CIRB-49 with a carbon
electrode. 64 % decolorization of CIRB-49 at optimum pH 2 using so-
nochemical treatment while the US-EC process enhanced the decolor-
ization to 99 % at pH 7 after 90 min of treatment. The addition of 3 mol
L−1 H2O2 slightly increased the decolorization while significantly in-
creased the COD reduction from 76.2 % (in the absence of H2O2) to
87.8 %. They reported that because of the addition of H2O2, the rate of
generation of %OH radicals increased due to self-decomposition under
ultrasound irradiation, and reduction of H2O2 in the conduction band
produces additional %OH. A SE in COD removal under ultrasonic irra-
diation at optimum condition was found, which showed the hy-
bridization of the US with electrolysis increased the mineralization of
the pollutant. Radi et al. [71] studied the degradation of CIRB-49 dye
using the US-EC process. Results demonstrated that carbon (working
electrode) and platinum electrode (auxiliary electrode) successfully
decolorized (97.2 %) dyes and reduced 91 % COD at the optimum
condition of 8.3 pH, 80 min treatment time and 10 mg L−1 initial dye
concentration. A synergism of 63.2 % was reported in combined stra-
tegies of these two techniques. This large positive SE is due to the en-
hancement of the mass transfer and continuous activation of the elec-
trode by ultrasound application [84]. Zhu et al. [1] also studied the
degradation of alizarin red S (ARS) using US-EC techniques. It was in-
vestigated that at the optimum condition of 0.05 M Na2SO4 electrolyte
concentration and pH = 4.97 value, 100 % color removal and 86.07 %
COD removal was found. Lower temperature was favorable for the US-
EC techniques, while higher temperatures (above 45 °C) was favorable
for EC with a higher rate of degradation.
3.2. Pharmaceuticals and personal care compounds
Pharmaceuticals and personal care products (PPCPs) are the new
class of emerging pollutants. The presence of these types of con-
taminants in wastewater treatment plants, groundwater, seawater,
surface water, soil, and sludge has been reported [85–87]. Conventional
methods have a limitation of sludge generation, partial removal, and
high chemical requirements, which increases the operating cost of the
treatments. Therefore, AOPs, including US, photolysis, and electrolysis,
have been studied for remediation of PPCPs such as IBP, TCS, and SMX
from the aqueous system. Percentage degradation of some pharma-
ceutical compound using these techniques are depicted in Fig. 6. Some
of the recent studies on PPCPs pollutants using the US-EC process are
8
Journal of Water Process Engineering 37 (2020) 101378
Fig. 6. Percentage degradation of pharmaceuticals compounds using ultra-
sound, EC, and US-EC. IBU (Ibuprofen), DU (Diuron), SMX (Sulfamethoxazole)
[89,93,107].
present in Table 2 [88–95].
Ren et al. [95] reported the parametric study on Triclosan (TCS)
degradation using different combinations of electrode with higher fre-
quency ultrasound (850 kHz). It was found that a diamond-coated
niobium electrode (DCNE) was found best for the EC degradation of
TCS, which was 24 % comparatively 9 % with silicon carbide electrode
(SCE) and 6 % using stainless steel electrode (SSE) as shown in Fig. 7.
About 35 % SE was observed with SSE using the US-EC system com-
pared to 25 % with SCE and 8 % with DCNE. The highest 82 % TCS
degradation was reported using sulfuric acid electrolyte and DCNE
electrode, while 63 % using sodium sulfate and 41 % using sodium
hydroxide. Effect of initial concentration of TCS on degradation effi-
ciency was also seen and found that with an increase in the TCS con-
centration from 1 to 10 mg L−1, degradation efficiency decreased from
90 % to 69 % in 15 min treatment time. Energy efficiency increased,
and the highest energy efficiency observed was 1.312-mmol kW h−1.
The effect of different electrolytes on the percentage degradation of TCS
and phenol also reported by Rean et al. [95]. It was found that NaOH
gave the highest percentage of degradation as compared to H2SO4 and
Na2SO4 electrolyte. An overview of AOPs for the mineralization of TCS
is shown in Fig. 8. Almost all types of AOPs can successfully degrade the
TCS from the wastewater. Tran et al. [92] observed the degradation of
Carbamazepine (CBZ) using Ti/PbO2 anode and Ti cathode by the US-
EC method. About 90 % removal using the US-EC process was reported
at optimum condition of 180 min time, 38 W ultrasonic power, and 4 A
current for 10 mg L−1 carbamazepine. However, this optimal condition
was applied for the mineralization of the municipal wastewater ef-
fluent, which contains 10 μg L−1. They found 93 % removal of CBZ, 60
% reduction of TOC, and a 93 % reduction of COD.
Finkbeiner et al. [94] performed the mineralization of diclofenac
(DCF) with the US-EC process and found 90 % degradation within 5
min. The effect of various operating parameters such as applied voltage,
electrode gap, immersion depth of electrode, and pH was also studied.
DCF degradation decreased from 96.8 to 85.1%, with an increase in the
pH value from 4.4 to 9.9. They reported that this decrease in the de-
gradation was due to the fact that at lower pH value, diclofenac exists in
nonpolar molecular form, which is more hydrophobic and can easily be
oxidized at the boundary layer of cavitation bubble compares to non-
polar form at higher pH value. Higher voltage lead to higher degrada-
tion of the DCF, which is 93 % at 7.2 V as compared to 54 % at 2.8 V.
Overview of different AOPs for diclofenac degradation is depicted in
Fig. 9. It can be observed that almost all types of AOPs able to degraded
the diclofenac from the wastewater without any generation of sec-
ondary waste. It shows that AOPs can successfully applied for the mi-
neralization of the pharmaceuticals pollutants. Thokchom et al. [93]
studied the IBP degradation kinetics with different electrolytes using a
US-assisted EC oxidation process. It was found that the ultrasound as an
individual treatment process was most effective using H2SO4 (rate
constant 0.0326 min−1) as an electrolyte because of the non-volatile
property of IBP and hydrophobic nature in the case of H2SO4. EC
treatment was most effective with NaOH (rate constant 0.032 min−1)
because of the hydrophilic form of the IBP at 10.75 pH. Similar results
were reported by Ciriaco et al. [96] who used NaOH for the
 Table 2
Typical studies of US-EC oxidation of various pharmaceutical and personal care pollutants.
Pollutant Experimental Conditions Treatment Efficiency References
P. Ritesh and V.C. Srivastava

Electrodes Ultrasound Other condition

Pharmaceutical Compounds
Ibuprofen (IBU)
Sulfamethoxazole (SMX)
Carbamazepine (CBZ)
Cephalosporin Pharmaceutical
Wastewater
Anode:- Platinum f =37 kHz IBU = 5 mg L-1, t = 60 min, US = 13.8% removal [88]
Cathode:- carbon black-coated carbon P = 320 W Applied current: 0.03 A. EC = 58%
cloth US-EC = 84
Anode:- Platinum (2 × 2 cm2) f =40 kHz, SMX = 10 mg L-1,V = 100 mL, Electrode gap = 1.5 cm, T 83% degradation with sonoelectrolysis. [89]
Cathode:- Graphite (d = 6 mm) P = 100 W =30 °C, Na2SO4 = 0.1 mM, Current density = 2-20 mA cm- 10% degradation with electrolysis
2
, pH = 6 3% degradation with the US.
Synergy factor = 14.7
Anode:-Titanium Coated with lead f = 520 kHz CBZ = 10 mg L-1 Electrode Gap = 20 mm,Na2SO4 = 0.01 99.5% CBZ degradation with Sono EC process. [90]
oxide (Ti/PbO2) (working surface area mol L-1
1100 mm2)
Cathode:- Titanium (700 mm2 Solid P = 40 W T = 20 °C, 91% with EC process.
area) Current intensity = 1A, t = 180 min 45% degradation using the US.
33.45% synergistic effect.
Anode:-RuO2-IrO2/Ti (50 cm2), f =45 kHz, P = 100 Current Density = 8 mA cm-2, pH = 6.3, t =30 min, COD = 94% COD removal efficiency was obtained with US-EC [91]
Cathode:- Stainless Steel W 326.9 mg L-1, treatment technology with nanocoated electrode.
70% COD removal was found with traditional electrode
using US/EO

9
Ibuprofen (IBU) Anode:- Titanium Coated with lead
Oxide (Ti/PbO2) (Solid Area 280 cm2,
Void Area = 120 cm2)
Cathode:- Titanium (solid area 420 cm2
and void area 180 cm2),
Ibuprofen (IBP) Anode:- Platinum (6 × 8 cm2)
Cathode:-Stainless Steel (7 × 8cm2)
Diclofenac(DCF) Anode:-Boron doped diamond Electrode
(50 mm × 30 m m × 1.5 mm) (5 μm
diamond layer on niobium)
Cathode: Boron doped diamond
Electrode (50 mm × 30 mm × 1.5 mm)
Triclosan 1.Diamon Coated niobium electrode
(DCNE) (50 mm × 30 mm × 1.5 mm)
(Coating 5 μ,)
2.Silicon carbide electrode (SCE) (50
mm × 30 mm × 1.5 mm)
3.Stainless Steel Electrode (SSE) (50
mm × 30 mm × 1.0. 8 mm)
50% COD removal nanocoated electrode in the absence of
the US.
f = 520 kHz (Bath), IBP = 10 mg L-1, V = 1 L, Electrode gap = 2.0 cm, T = 20 84% TOC removal was obtained using US-EC process [92]
°C, Current Densities = 3.6 -35.7 mA cm-2, t =120 min,
P = 40 W 84.74% removal of IBP using US-EC process with synergy
degree of 5.26%.
5% Degradation using US.
75% degradation using electrolysis.
f = 1000 kHz (bath), IBP = 0.01 Mm V = 30 V, T =25 °C, t = 60 min, pH = 6.85 89.32% degradation using US/EO/NaOH. [93]
Power density = 100 81.85% using US/EO/H2SO4.
W L-1 88.7% using US/EO/Deionized water
81.22% using US
21.46% using electrolysis
f = 850 kHz, DCF = 50 μg L-1,V = 500 mL, pH = 5.8, Na2SO4 = 30 mM, 90% degradation of diclofenac with US-EC process. [94]
T =22 °C, t = 5 min,
P = 120 W power Electrode immersion depth = 2.1 cm, Electrode gap = 1 cm. Synergy index 1.127
density = 94.1 W L-1
f = 850 kHz, TCS = 5 mg L-1, Electrode gap = 1 cm, T =25 °C, H2SO4 = 92% degradation of TCS was obtained at optimum condition [95]
0.16 g L-1, Electric Voltage 10, Solution Conductivity =1 mS using DCNE electrode with sono EC system while using SCE
cm-2,t =15 min. TCS solution =400 mL, pH = 2.5 electrode 25% and using SSE electrode 9%.
P = 170W 35% synergistic effect was observed.
Journal of Water Process Engineering 37 (2020) 101378
P. Ritesh and V.C. Srivastava
Fig. 7. Percentage degradation of triclosan using different electrodes by ultra-
sound, EC, and US-EC. Source: [95].
Fig. 8. Percentage degradation of Triclosan using different advanced oxidation
processes [132–136].
Fig. 9. Percentage degradation of Diclofenac using different advanced oxida-
tion processes [94,137–144].
Fig. 10. Percentage degradation of ibuprofen using different electrolytes by
ultrasound, EC, and US-EC process. Source: [93].
mineralization of IBP with a modified electrode. As depicted in Fig. 10,
the combined US-EC of IBP provided 89.32 % degradation using NaOH
and 81.85 % using H2SO4 and 88.70 % using deionized water. Tran
10
Journal of Water Process Engineering 37 (2020) 101378
et al. [97] worked on titanium-coated PbO2 electrode for the de-
gradation of IBP using US-EC process and reported 84.74 % removal of
IBP using US-EC process with synergy degree of 5.26 % which was
lower than that reported by Ren et al. [84] while degrading phenol with
US-EC process (75 %) in which SSE was used for 400 mL treatment
volume. They found a synergy degree of 60 % using the US-EC process.
This discrepancy in synergism was due to the difference in power im-
posed for the degradation of pollutants. Tran et al. [97] imposed 244 W
g−1 of IBU, while Ren et al. [84] delivered 4521 Wg-1 of phenol. An-
other reason is that the IBU structure is more complex than phenol for
the oxidation; therefore, it was quite difficult to degrade IBU as com-
pared to phenol. Tran et al. [97] reported that IBP mineralization in-
creased up to 84.2 %, with an increase in ultrasonic power from 5 to 40
W. Villaroel et al. [98] reported that the degradation rate increased
with increases in power for the degradation of acetaminophen in water.
Madhavan et al. [99] also assessed similar outcomes during the oxi-
dation of DCF pollutants using the sonochemical process. Tran et al.
[97] reported 89 % IBU removal and 84 % TOC removal with a current
intensity of 10 A. Ciriaco et al. [96] also reported 60–95% COD removal
and 48–92% TOC removal of IBU using electroxidation by Ti/Pt/PbO2/
BDD anode electrode while da Silva Duarte et al. [100] reported 95 %
rifampicin removal in 3 h using the BDD anode electrode.
Yang et al. [91] studied combined ultrasound EC degradation of
actual pharmaceutical wastewater (PWW) by nanocoated electrode
(RuO2-IrO2/Ti). A significant improvement in the mineralization of the
pollutant was reported using a nanocoated electrode. The current
density effect (2–8 mA cm−2) was found to be positive because of an
increase in %OH radical generation and diffusion with an increase in
current density. 94 % COD removal of PWW was reported using US-EC
treatment at optimum condition of current density = 8 mA cm−2, ul-
trasonic power = 100 W, and 45 kHz frequency. However, using the
traditional electrode at the same operating condition, only 70 % COD
removal was obtained. The difference in COD removal between nano-
coated electrode and conventional coated electrode, a higher number of
active sites are available in the nanocoated electrode as compared to
the conventional coated electrode. Therefore, ultrasound enhanced the
mass transport inside the bulk and increased the generation of %OH
radicals from the surface of the nanocoated electrode. Due to the higher
rate of %OH radicals generation, the rapid reaction of pollutants with %
OH radicals takes place. Ultimately higher mineralization takes place.
In the absence of ultrasound, COD removal was 50 % for both types of
electrodes. It was also observed that the presence of ultrasound en-
hanced the oxidation activity of chlorine. Tran et al. [101] studied
chlortetracycline degradation using Ti/PbO2 electrode. 73.3 % de-
gradation was found at optimum condition of current = 3.92 A, ul-
trasonic power = 20 W, frequency = 500 kHz, and 90 min treatment
time. At this optimum condition, 61.4 % mineralization (TOC removal)
was reported. Effectiveness of the US-EC process was also evaluated by
employing the real municipal wastewater and found that up to 98 %
oxidation of the chlortetracycline. Due to the presence of the chloride
ion in the real wastewater, both direct (due to %OH radicals) and in-
direct (hypochlorous acid formed by chloride oxidation) anodic oxi-
dation involved in the mineralization of the pollutants. Zaviska et al.
[102] also reported similar studies during the mineralization of real
wastewater contaminated with BPA and 465 mg L-1 chloride ions. They
reported that within 30 min treatment time, complete degradation of
BPA took place in municipal wastewater while it took 100 min for the
complete degradation of synthetic wastewater using Na2SO4 as an
electrolyte.
Huang et al. [89] adopted a common platinum and graphite elec-
trode for SMX degradation using the US-EC oxidation method. The US
alone showed a marginal degradation of SMX, while electrolysis gave
10 % degradation, and sonoelectrolysis provided 83 % removal of SMX.
The synergism of 14.7 at the optimum condition was reported. Direct
anodic oxidation and %OH radicals were both found to be responsible
for this synergism. Tran et al. [90] reported CBZ degradation with
P. Ritesh and V.C. Srivastava Journal of Water Process Engineering 37 (2020) 101378

titanium coated PbO2 (Ti/PbO2) electrode and found 99.5 % degrada-

References
tion at optimum condition using the US-EC process. 91 % of CBZ de-

[104]

[105]

[106]

[107]

[108]

[109]

[110]
gradation was obtained using the EC process at the same condition in
30 days. The synergy degree increased with an increase in the power of
ultrasound. The highest synergy degree of 33.5 % was obtained at 40 W

while with US-EC process power consumption decreases

Fractional conversion = 97%, degradation efficiency =

consumption from 227.4 kW h m-3 to 455.4 kW h m-3
100% removal of thiaram using US-EC process in 5 h.
power. Dominguez et al. [103] also assessed electroxidation miner-

Almost 50% oxidation of 2,4-D solution in 60 second

The Arrhenius constant was 8 h-1, and the activation
100% herbicide degradation and 91% TOC removal
Apperant rate constant was found to be 10-3 min-1.
alization of CBZ using the Ti/BDD electrode. Ti/BDD electrode caused

26%, selectivity = 0.92, current efficiency = 8%

while fully degradation was obtained in 600 sec.

complete degradation of CBZ at the optimal condition. The highest

The electrolysis process increases the power

synergy degree of 25.36 % and lowest synergy of -9.31 % was reported

from 325.4 kW h m-3 to 302.3 kW h m-3.

72.8% degradation using the EC process.
93.3% degradation using US-EC process,
by Tran et al. [90] at 1 A and 15 A, respectively. Huang et al. [89] also

43% mineralization kinetics increased.

performed parametric studies for the degradation of SMX. His research
found that SMX degradation increased with an increase in applied
current density up to 20 mA cm−2. Above 20 mA cm−2, the rate of

energy was 7.7 kJ mol-1.

degradation slightly decreased. This is because, at higher current,

37% synergistic effects.

Treatment Efficiency
oxygen evolution takes place near the electrode, which inhibits the
direct oxidation of the pollutant. Effect of the addition of different
electrolytes such as Na2SO4, NaNO3 and NaCl, Fe2+, and H2O2 on US-

using US-EC.
EC and EC system was also observed. NaNO3 gave the highest rate
constant value with 83 % removal, while NaCl gave the lowest value.
An additional effect of Fe2+ was also investigated and found that the
US-EC-Fe2+ system was found to be the best among others employed

Diuron = 18 mg L-1, V = 250 mLCurrent Density = 60

T = 20 °C, Na2SO4 = (0.5 gL ), 2,4-D = 0.25-1.5 mM,

T =25 °C, Na2SO4 = (0.5 g L-1), 2,4-D = 0.25-1.5 mM,

CPS = 900 mg L-1, V = 400 mL, Na2SO4 = 2 mg L-1, T

electrode gap = 9 mm, BDD coating film thickness = 2

mA cm-2, pH = 12, T =10 °C, t = 8 h. Na2SO4 = 10 g

2,4-DCP = 0.35-1.5 mM, pH = 3, Fe2+ = 0.5 to 50 m,

mm, Distance between probe and electrode = 1.8 cm
L-1, and Electrode gap = 5 cm, Probe diameter = 13
for the mineralization of the SMX. Tran et al. [90] also examined the

2,4-D = 100 mg dm-3,V = 1.2 dm3, NaCl = 3 gL-1,

morphology of the electrode pre- and post-treatment using scanning
electron microscopy, EDS analysis, and EIS measurement. It was found

K2SO4 = 0.05 mol L-1, j = 10-50 mA cm-2

that the surface of the electrode used in the US-EC process does not

pH = 2.7, T = 25 °C, Na2SO4 = 20 mM

contain any impurities, while the surface of the electrode used in the

Thiaram = 100 mg L-1, t =120 min,

2,4-DCP = 0.35-1.5 mM, pH = 3,

electroxidation process contains impurities. Hence, the promotional
role of ultrasound in cleaning and peeling of the electrode was ob-

-1
mm, resistivity = 100 mΩcm.
served. Soltani et al. [88] studied the degradation of ibuprofen using
platinum and carbon black-coated carbon cloth as a cathode with US-

= 15-35 °C, t =1 h.
EC techniques. The US alone gave 13.8 % degradation, EC alone gave

H2O2 = 30 mM
58 % degradation, and US-EC gave 84.2 % degradation of the IBU in-
Other condition

dicate that the coupling of ultrasound using the US-EC process en-
hanced the degradation of the IBU. The effect of the presence of organic
and inorganic compounds on the US-EC reactor was also investigated. It
was found that methanol and ethanol both decreased the removal ef-
ficiency of IBP up to 47.2 % and 71.7 %, respectively. This is due to the
f =40 kHz, P = 200 W

f = 20 kHz, P = 523 W

f = 20 kHz, P = 75 W
US Source : f =24 kHz
Typical studies of US-EC oxidation of various herbicides, fungicides, and insecticides pollutants.

f = 20 kHz,P = 55 W
scavenging of %OH radicals by alcoholic compounds. While the presence f = 20 kHz (probe)

(horn), P = 200 W
of inorganic such as carbonate and chloride increased the degradation
efficiency of up to 95.3 % and 88.4%, respectively. The presence of
P = 200 W

P = 750 W
Ultrasound

f =24 kHz

chloride ions generated the chlorine-free radicals (Cl%) and increased

the degradation rate of IBU.

cm- 2
cm-2

3.3. Herbicide, fungicides, and insecticides

Anode:-Boron doped Diamond Electrode

cylindrical segments (11 mm radius and

cylindrical segments(11 mm radius and
Electrode:- Nickel Foil in the form of

Electrode:- Nickel Foil in the form of

Anode – Stainless steel (3140 mm2)

Few studies have been reported for the degradation of the herbicide,
Cathode:- Boron doped Diamond
(11.4 cm2 Effective anodic area)
(Circular,geometric area70 cm2)

fungicides, and insecticides using the US-EC process. Table 3 presents a

Boundary Electrode :-Si/BDD,

comparative assessment of these studies for the degradation of herbi-

Experimental Conditions

cide and fungicide [104–110].

Cathode- Stainless steel

Cathode:- Pt plate

Titanium, Pt wire

3.3.1. Herbicide
20 mm height)

20 mm height)
Anode :- BDD

Bringas et al. [107] worked on diuron (herbicide) mineralization

Electrodes

Electrode

using the BDD electrode by ultrasound-assisted EC oxidation process.

100 % degradation of herbicide was obtained after 7 h. Dissolved or-
ganic carbon (DOC) removal was 69 % using EC and 91 % using US-EC
after 8 h treatment. A SE of 43 % at the optimum condition of 60 mA
Diuron (N-(3,4-dichlorophenyl)-N,N-

(2,4-D), and 2,4-Dichlorophenol

(2,4-D), and 2,4-Dichlorophenol

Pesticides, Herbicides Pollutants

cm−2, 20 kHz, pH 12, and 10 °C was reported. Guo et al. [111] reported
2,4-Dichlorophenoxyacetic acid

2,4-Dichlorophenoxyacetic acid

a 10 % degradation of 2, 4 – dinitrophenol using low-frequency ultra-

Trichlolroacetic acid (TCAA)

sound in 4 h treatment. Abu-Hassan et al. [112] reported 80 % de-

gradation and 20–25 % mineralization of sodium dodecylbenzene sul-
fonate, Souza et al. [106] reported 100 % degradation of 2,4-
dimethyl-urea)
Chlorpyrifos (CPS)

dichlorophenoxyacetic acid (2,4–D) herbicide using US-EC process. All

2,4-D herbicide

studies show that the US-EC process can mineralize herbicides. Kinetic
Pollutant

study results revealed that high pH favors fast mineralization due to the
Thiram
Table 3

accumulation of hypochlorite that acts as a redox agent. Canizares et al.

[113] observed similar results during the degradation of chlorophenols.

11
P. Ritesh and V.C. Srivastava
Some cases of successful pesticide mineralization by means of US-EC-
oxidation are also reported. Yasman et al. [109] investigated the de-
gradation of chloro-organic compounds with the sonoelectrocatalytic
process. A common herbicide 2, 4-D and 2, 4-dichlorophenol (2, 4-DC-
phenol) was selected as a model pollutant. The application of Pd and
Pd-Fe powder in the sonoelectrocatalytic process allowed the complete
removal of the complex chlororganic compounds. About 65 % de-
gradation of 2, 4-D in 30 sec, and complete conversion was obtained in
10 min using the Pd electrode. Yasman et al. [110] evaluated the per-
formance of the US-EC Fenton process for the decomposition of (2, 4-D)
and (2,4-DC-phenol) and found that the efficiency of sono-electro-
Fenton process for the mineralization of the pollutant is much higher
than the other process. 50 % removal of 2, 4-D solution in 60 seconds
while complete degradation was obtained in 600 sec. Esclapez et al.
[108] investigated the improved EC route of TCAA (a pesticide) de-
gradation using ultrasound. A continuous flow US-EC device on the
pilot scale was used for the degradation of an organic compound. High
conversion (95 %) with high current efficiency (10 %), selectivity of
0.92, and degradation efficiency of 26 % was reported. They also found
that the TCAA degradation got enhanced using high-frequency ultra-
sound by means of dissociative adsorption/incineration that occurred
on both the electrodes.
3.3.2. Fungicides and insecticides
Steter et al. [105] observed the degradation of thiram (fungicide)
using the BDD electrode by the US-EC method. Operating parameter
effects on degradation kinetics were evaluated. With an increase in
current density from 10 to 50 mA cm−2, current efficiency decreased
from 25.88 to 11.27 %, whereas energy consumption increased from
27.70 to 55.27 kW h m-3. Ren et al. [104] reported the degradation of
chlorpyrifos (insecticides) using the US-EC technique by SSE. 50.98 %
removal using the US, 72.8 % removal using the EC system, and 93.3 %
removal using the US-EC process was reported. A synergism of 37 %
using the combined system was reported. Sodium sulfate was selected
as an electrolyte so that the pH of the solution is not affected by the
addition of the electrolyte.
3.4. Aromatic compounds
Aromatic compounds are persistent organic pollutants in the en-
vironment. These compounds accumulate in high concentrations near
the oil distillation plants [114]. The decomposition of these organic
complexes from the wastewater is still a changing task for the re-
searcher. The degradation of the various aromatic pollutants using US,
EC, and US-EC are shown in Fig. 11. Table 4 presents a comparative
assessment of studies on aromatics compound degradation using the
US-EC process [115–121]. Trabelsi et al. [26] reported the degradation
of phenol using the US-EC process and found only 3 % phenol de-
gradation using the US alone while 75 % degradation was obtained
after 10 min using the US-EC process with 20 kHz ultrasound fre-
quency. At the optimum conditions, 95 % degradation was obtained
with the same treatment time using a 540 kHz ultrasound frequency
with no toxic product. Lima Leite et al. [121] investigated the de-
gradation of 2,4 dihydroxybenzoic acid (2,4-DHBA) under two
Fig. 11. Percentage degradation of aromatic compounds using ultrasound, EC,
and US-EC process [116,123,145].
12
Journal of Water Process Engineering 37 (2020) 101378
ultrasonic frequencies, 20 kHz, and 500 kHz. Under the optimum
condition, 47 % TOC degradation was reported using the US-EC tech-
nique. De Lima Leite et al. [122] reported that the electrolysis is able to
degrade the pollutant, but under low concentration, and this technique
is not efficient. Lima Leite et al. [121] investigated the combination of
ultrasound and electro-oxidation and found that under the combined
technique, pollutants can be effectively removed in low concentration
at low ultrasound frequency. The mass transfer rate and adsorption and
desorption mechanisms got accelerated under ultrasound irradiation.
Zhao et al. [120] studied the decomposition of the phenol and phthalic
acid (PA) in the presence of ultrasound using the BDD electrode (anode)
and titanium foil (cathode). Only 1.5 % COD removal of phenol and 1.3
% COD removal of phthalic acid was reported after 3 h using the US
alone. Zhao et al. [120] combined ultrasound and EC oxidation pro-
cesses for the degradation of phenol and PA and reported 100 % COD
removal. The promotional role of the ultrasound by virtue of chemical
and physical effect of ultrasound was clearly observed. Another inter-
esting result was found that the variation in energy consumption was
lower in the case of the US-EC process as compared to EC alone for both
the pollutants. This reflects that the US can reduce the EC energy re-
quirement for the complete mineralization of the pollutants. Mass
transport coefficient, kd, increased with the application of ultrasound,
and it was found to be 2.0 × 10−5 m s-1 in case of the US-EC process for
both the pollutant; as compared to 6.7 × 10-6 m s-1 for PA and 5.4 ×
10-6 m s-1 for phenol with EC alone. This clearly shows that the kd value
of the US-EC system is higher than the EC system alone. This is because
the application of ultrasound in combination with EC increased the
adsorption/desorption process on the electrode surface. EC alone gets
difficult to desorb intermediates from the electrode surface, while in the
US-EC process, desorption of intermediates was easy. Zhao et al. [24]
assessed the effect of the BDD electrode and Pt electrode for phenol
degradation. Only 1.5 % degradation of phenol using ultrasound was
found in 3 h. They investigated that the oxidation efficiency of phenol
on the BDD electrode was faster than the Pt electrode. 39 % COD re-
moval was investigated using a Pt electrode, while 69 % COD removal
was reported using a BDD electrode. Garbellinil et al. [123] also in-
vestigated the valuable effect of ultrasound for the degradation of
pentachlorophenol using the BDD electrode. They reported 19.8 %
degradation using US, 70.8 % degradation using electrolysis, and 82.6
% degradation using the US-EC process. Zhao et al. [24] reported that
the BDD shows higher OEP as compared to the Pt electrode. Therefore,
higher degradation was obtained using the BDD electrode than the Pt
electrode. Average current efficiency was also investigated and found
that in the EC process, it was 6.5 % using a Pt electrode while it was
12.3 % using the BDD electrode. The average current efficiency in-
creased to 9.7 % in the US-EC process using a Pt electrode and increased
to 24.6 % using the BDD electrode. About 100 % US-EC degradation of
phenol was obtained in 3 h using the BDD electrode while it took 4 h
using the Pt electrode.
Ren et al. [84] published a study on phenol degradation by low-cost
SSE using higher frequency (850 kHz) ultrasound for the economic
performance and found 16%, 32 %, and 99 % removal of phenol using
US, EC, and US-EC process. They reported that with an increase in
electrolyte concentration from 0.39 to 4.26 g L−1, percentage de-
gradation increased from 24 to 67 %, energy consumption increased
from 0.180 kW h to 0.198 kW h, and energy efficiency increased from
0.520 to 1.354 mmol kWh−1. An increase in the percentage removal
with an increase in the electrolyte concentration was due to an increase
in the conductivity of the solution. Souza et al. [118] also assessed the
complete mineralization of dimethyl phthalate (DMP) using the US-EC
process by employing a conductive diamond electrode. Chen et al.
[117] reported that the enhancement in TOC removal by combined
strategies by virtue of ultrasound, which increases the mass transfer
rate across the electrode. The influence of operational parameters on
TOC removal efficiency was also investigated and found that with an
increase in temperature, TOC removal decreases. 94 % TOC removal
 P. Ritesh and V.C. Srivastava

Table 4
Typical studies of US-EC oxidation of various aromatics pollutants.
Pollutant Experimental Conditions Treatment Efficiency References

Electrodes Ultrasound Other condition

Aromatic compounds
Bisphenol-A BDD Electrode (5 μm diamond layer on niobium) f =24 kHz, Electrode gap = 2-3 cm, T = 20 °C, BPA 93% degradation of Bisphenol A with sonoeletroxidation process. [115]
= 1 mg L-1, t =30 min
Nitrobenzene Anode:-Ti/Sb-SnO2 (Effective area = 18cm2) f =22 kHz, P = T =30 °C, Electrode gap = 2.5 cm, Pulse 63% degradation of nitrobenzene with EC process and 78% [116]
Cathode:- Titanium electrode 48W mode of TUS = 50 ms,TECD = 50 ms, pH = degradation with EC-US process while 80% nitrobenzene
3, Na2SO4 = 0.1M degradation was obtained using dual pulse US-ECD coupling
process.
Nitrotoluenes Platinum (20 mm × 20 mm × 1 mm) f =120 kHz, pH = 0.1,O2 = 150 mL min-1, T =30 °C, 15% TOC removal with US alone, 69% with electrolysis and 94% [117]
150 mg L-1 ferrous ions, Electrode TOC removal with sonoelectrolysis process. 99% TOC removal
Potential = 6 V with sonoeletro-fenton process compare to 73% using electro-
Fenton and 15% using US process.
Phenol Anode:-Stainless steel spherical net (surface area = f = 850 kHz,P = T =1 hr,Na2SO4 = 4.26 g L-1, Electric 16% degradation of phenol using sonication and 32% phenol [84]
4950 mm2, mesh size = 0.16 mm2) Cathode:- 170 W Voltage = 30 V,T =25 °C, Conductivity = removed by EC method.
Stainless steel ring (Diameter 50 mm,thick = 2.8 4000 μS cm-2

13
mm)
Dimethyl Phthalate Conductive diamond electrode (p-Si-boron doped f =24 kHz, P = 200 Inter electrode gap 9 mm Na2SO4 = [118]
diamond) (78 cm2 geometric area) W DMP = 1.6-161.8 mg dm-3
P-Substitued Phenol Anode:-BDD or PbO2 (Geometric area 4 cm2) f =40 kHz, P = 50 Current Density = 20 mA cm-2, T =25 °C, At the BDD electrode p- substituted phenol percentage degradation [119]
Cathode:- Stainless Steel W Na2SO4 = 0.2 M, Electrode gap = 10 mm increases in the range of 73-83%, and COD removal was 60-70%
while at PbO2 anode 50-70% p-substituted phenol disappearance
and only 5-25% COD removal increases.
Phenol and Phthalic acid Anode-BDD (24 cm2 immersed area), Cathode:- f =33 kHz,P = 50 Current Density = 20 mA cm-2, pH = 3.0 1.5% of COD removal of phenol,1.3% COD removal of phthalic [120]
Titanium Foil, Diamond Film Thickness =1 μm, W. adjusted using 2 M H2SO4 acid for ultrasound alone
Electrode Gap = 1 cm. 100% COD removal was obtained in 3.4 h and 3.2 h for phthalic
acid (PA) and phenol, respectively, using the US-EC process.
Phenol Anode:-BDD, Pt (immerse area = 24cm2) f =33 kHz, P = 50 Interelectrode Gap = 1 cm, Current 100% degradation of phenol on BDD electrode using US-EC [24]
Cathode:- Titanium Foil (immerse area = 24cm2) W Density = 20 mA cm-2, Na2SO4 = 0.05 process after 3 h while on Pt Electrode 4 h. COD removal increase
mM H2SO4 = 0.2 M, T =10 °C to 98% using US-EC process on BDD electrode while for Pt
electrode COD removal increase to 54%.
Phenol Anode:- Platinised titanium grid (Surface area 147 f = 540 kHz and 20 T =27 °C, Nacl = 0.5 g L-1, Current Only 5% phenol degraded after 3 h with US alone while 95% [26]
cm2) kHz, P = 50 W intensity = 1 A, Current Density = 68 A degradation of phenol in 10 min at 540 kHz ultrasound with US-EC
Cathode:- Nickel Foam m-2 process with no toxic aromatic product.
2,4 Dihydroxybenzoic acid (2,4- Electrode:-Platinum rotating disk (3.14 mm2) f = 20 kHz, and 500 Disk RPM = 2000.T =30 °C, pH = 2, Complete degradation of pollutant was obtained using low [121]
DHBA) kHz. Na2SO4 = 0.1M frequency US at 1.3 Ah of US-EC process
P = 150 W and 100 2,4-DHBA = 100 or 300 mg L-1
W
Journal of Water Process Engineering 37 (2020) 101378
P. Ritesh and V.C. Srivastava
was obtained at the lowest temperature of 30 °C. This was due to a
higher yield of H2O2 results in a higher rate of generation of O%OH
radicals at a lower temperature. A stronger acidic medium was favor-
able for a higher TOC removal rate. Effect of oxygen dosage and ferrous
ion concentration was also investigated and found that with increases in
oxygen dosage, TOC removal increases while at 150 mg L−1 ferrous
ions concentration 99 % TOC removal reported. Xia et al. [116] studied
a dual pulse ultrasonic enhanced EC process for the degradation of
nitrobenzene and found that dual pulse US-EC process has a better ef-
ficiency in terms of degradation and energy consumption. 63 % de-
gradation of nitrobenzene using the EC process and 78 % degradation
using the US-EC process was reported. 80 % nitrobenzene degradation
was obtained using a dual pulse US-EC coupling process. Observed re-
sults are due to pulse mode diminished interference of ultrasound on EC
degradation. Energy used by the dual pulse US-EC method was only
46.5 % of the conventional US-EC method. They also reported that the
acidic condition was more favorable for the dual pulse US-EC process
than alkaline conditions. Aquinoneto et al. [124] also reported the si-
milar results that organic compound oxidation is more favorable in
acidic medium. This is because lower value of pH diminishes the
oxygen evolution reaction. Further, electrolyte concentration increased
the removal efficiency due to an increase in the conductivity of the
solution. Ultrasonic power has a positive effect on the pulsed process
with increased ultrasonic power. Nitrobenzene degradation increased
due to the enhancement in the cavitation activity of the bubble. Chen
et al. [117] considered the degradation of nitrotoluenes using a com-
monly used platinum electrode by the US-EC process. Synergism was
reported using TOC removal efficiency. 15 %, 69 %, and almost com-
plete mineralization, 94 % TOC removal were reported using US,
electrolysis, and sonoelectrolysis process. Dietrich et al. [123] worked
on the mineralization of BPA by combing the BDD electrode with a
lower frequency (20 kHz) ultrasound. 38 % BPA degradation at 25 μm
ultrasonic amplitude and 61 % BPA degradation at 125 μm ultrasonic
amplitude was reported. Increases in the amplitude increases the per-
centage removal. This may be because of increasing hydroxyl radicals
by higher amplitude ultrasound. Dietrich et al. [115] also studied the
effect of sonotrode immersion depth and found that with decreased
immersion depth of sonotrode from 8.1 cm to 3.1 cm, the BPA de-
gradation decreases from 61 % to 29 %. 93 % degradation of BP-A was
reported at the optimum condition of 2 cm electrode gap, 24 kHz fre-
quency, and 5 V power. A synergistic index of 2.26 was investigated
using 125 μm amplitude. The percentage degradation of BPA using
different methods is depicted in Fig. 12. Dietrich et al. [115] evaluated
0.024, 0.016, and 0.090 min−1 rate constant value for the US, EC, and
US-EC process, respectively.
Some researchers also employed different types of electrode for
degradation of persistent pollutants such as Zhu et al. [119] reported
the removal of p-substituted phenol using BDD and PbO2 electrode. The
study showed that ultrasonic irradiation increases the COD removal
efficiency by virtue of mass transfer enhancement. Trabelsi et al. [26]
and Lima Leite et al. [121] also reported the enhancement in EC oxi-
dation of phenol at Pt and BDD electrode due to improved mass transfer
rate by ultrasound. BDD electrode showed higher rate of removal of p-
Fig. 12. Percentage degradation of Bisphenol-A using different AOPs
[115,121,122,146–153].
14
Journal of Water Process Engineering 37 (2020) 101378
substituted phenol (73–83 % removal and 60–70 % COD removal)
compare to the PbO2 electrode (50–70 %, 5–25 % COD removal).
3.5. Chlorinated compounds
Chlorinated compounds have been reported as a strong recalcitrant
class of pollutants, among others found in the aqueous life [125]. Due
to the poor performance of the biological methods toward the de-
gradation of the chlorinated compounds, the researchers have studied
alternative techniques such as catalytic hydrogenation, photolysis, and
the US. Table 5 presents a comparative assessment of these studies for
the degradation of chlorinated and other miscellaneous compounds
[126–130]. Saez et al. [127] studied the degradation of per-
chloroethylene, which is used as a chlorinated solvent in many in-
dustries. 55 % degradation efficiency and 100 % fractional conversion
of perchloroethylene were reported using Pb and PbO2 electrodes under
low ultrasonic intensity. Energy consumption with the US-EC process is
less as compared to the sonochemical treatment because of the sig-
nificant reduction in the time using a pulsed mode flow reactor. In
another study by Saez et al. [128], decomposition of perchloroethylene
were carried out without electrolyte. They reported that low con-
ductivity wastewater could be successfully mineralized using an ultra-
sound-assisted EC process. Ultrasound cavitation increases the mass
transfer of ion across the electrodes, which avoids the use of extra
chemicals. About 100 % dechlorination was obtained at high ultrasonic
power.
3.6. Other
Recovery of silver from the photographic effluents is a major pro-
blem. Industrially, various techniques have been employed, such as ion
exchange, electrolysis, bacterial digestion to recover silver from pho-
tographic processing solution. Pollet et al. [130] investigated the re-
covery of silver from photographic processing using ultrasound-assisted
electroxidation and found that under 20 kHz ultrasonic frequency,
silver recovery increased with an increase in ultrasonic intensity. The
effect of the location of the ultrasound generator and electrode was also
studied. A higher rate constant for the removal of silver was observed
when the ultrasonic horn was kept parallel to the electrode as compared
to an upright position with respect to the electrode. They also employed
a rotating cylinder as a working electrode and found that with an in-
crease in the rotation speed of the cylinder, silver recovery increased. In
another study, Pollet et al. [131] worked on the oxidation of thiosul-
phate with stainless steel and platinum electrode. They found that ul-
trasound has a good impact on the degradation of thiosulphate. This is
because the cavitation activity of microbubble increased mass transfer,
which reduced the diffusion layer thickness. However, thiosulphate
degradation using sonication alone was found to be negligible.
Shetakova et al. [126] coupled higher frequency ultrasound with
Ti/Ta2O5-SnO2 electrode prepared by thermal decomposition and drop-
casting technique for the degradation of formic acid. They reported 97
% removal of formic acid using ultrasonic frequency of 1176 kHz and
current of 20 mA under 120 min treatment time while sonication alone
had no effect on degradation of FA as only 3 % degradation after 2 h
was reported. FA degradation of 92.8 % using electrolysis and 99 %
degradation using US-EC degradation at the optimum condition of
frequency = 381 kHz, 20 mA, and 0.02 W cm−3 ultrasonic power was
reported. Reported results stated that lower frequency provided higher
removal of FA as compared to a higher frequency.
Sundarapandiyan et al. [129] also investigated the decomposition of
organic pollutants in saline wastewater using the US-EC method and
found that ultrasound alone was not sufficient in the degradation of the
pollutant. Only 29.91 % COD reduction and 69.35 % total Kjeldahl
nitrogen (TKN) reduction was obtained while 69.23 % COD reduction
and 93.4 % TKN reduction was reported using the electrolysis process.
A complete reduction of TKN was achieved using the US-EC process.
P. Ritesh and V.C. Srivastava Journal of Water Process Engineering 37 (2020) 101378

This shows that ultrasound alone is unable to degrade the toxic pollu-
References
tants.

[126]

[127]

[128]

[129]

[130]
4. Energy consumption estimation in US-EC techniques
97 % mineralization of FA using US-EC degradation and 99 % degradation

100 % fractional Conversion and degradation efficiency around 55 % using

sonoelectro rate constant = 1.9 × 10−3 s−1 and electrolysis rate constant
US and EC technology were found to be relatively inefficient in
100 % degradation efficiency of PCE at higher ultrasonic power level.

100 % COD Reduction and total Kjeldahl nitrogen (TKN) reduction.

terms of energy consumption for the degradation of the wastewater

Thiosulphate degradation was observed first order kinetics with

containing refractory organic pollutants. Therefore, both the techniques
are not economically attractive or feasible alone for scale-up. Several
authors estimated the energy consumption in EC and US-EC and found
that the US, in combination with EC, generally reduces the energy

= 3.8 × 10−5 s−1 with stainless steel electrode,

consumption per unit mass of pollutant mineralized by increasing the
rate of reaction [74,76,92,93,120,126,129]. Typical studies of energy
consumption of the US, EC, and US-EC technique are shown in Table 6.
Siddique et al. [74] reported that the US-EC techniques for decom-
position and decolorization of RB-19 dye is more effective in terms of
of FA using sono EC degradation.

energy requirement. It was found that US-EC techniques reduce energy

requirement to half as compared to the electrolysis and US techniques
alone. The effect of ultrasonic frequency (40−80 kHz) on energy con-
Treatment Efficiency

sumption was also reported. It was found that with an increase in the
US-EC treatment

frequency from 40 to 80 kHz, energy consumption decreased from 1.14

to 0.75 kW h L−1 while decomposition of dye increased from 49 to 65
% for US-EC techniques. Further EC alone required energy consumption
of 1.20 kW h L−1 for 39 % decomposition of RB-19 dye during 120 min
treatment time, which is higher than the US-EC technique. Somayajula
et al. [74] calculated the energy consumption for the degradation of
Sodium Thiosulphate = 220 g dm−3
Electrode Gap = 1 cm, FA = 250 mg

T =45 min, Current density = 0.01

T = 20 °C, PCE = 60 ppm, current

reactive red 195. EC technique required 72.3 kW h kg of COD removed

A cm−2, Salt concentration 4%.

−1
for 58.3 % COD removal while the US-EC technique consumed 65.7
kW h kg of COD removed−1 with 63.74 % COD removal, which clearly
density =3.5 mA cm−2

shows that US-EC technique reduces the energy consumption for the
L−1, NaCl = 3 g L−1

mineralization of the dye by accelerating the rate of reaction. Sundar-

Other condition

apand et al. [129] reported that the energy consumption in the US-EC
process is inversely proportional to the power of ultrasound. The author
reported that with an increase in the ultrasonic power from 0 to 100 W,
energy consumption reduced from 0.51 kW h (kg of COD removal)−1 to
0.27 kW h (kg of COD removed)−1. However, the energy consumption
f =38 kHz (Bath) 20

became constant with further increase in ultrasonic power. Hence, an

f = 381 kHz, P =

optimum ultrasonic power can reduce the energy consumption of US-

f = 20 kHz, P =

f = 20 kHz, P =

f = 20 kHz, P =
0.270 W cm−3

0.270 W cm−3

EC techniques because at optimum power sufficient number of cavity

0.02 W cm−2

kHz (Horn)
Ultrasound

formed by OO%H radicals, which react with the pollutant and miner-
alize it. Zhao et al. [120] studied the mineralization of phenol and
400W

phthalic acid on the BDD electrode. It was reported that ultrasound was
found to reduce the energy required for the complete mineralization of
cm) Cathode:-lead (4.5 cm × 2.5 cm × 0.3

cm) Cathode:-lead (4.5 cm × 2.5 cm × 0.3

Anode:-lead dioxide (4 cm × 2.7 cm × 0.6

Anode:-lead dioxide (4 cm × 2.7 cm × 0.6

cm2), Counter Electrode:-Platinum (1 cm2)

lead, manganese, and tantalum (200 cm2)
Working electrode:- Platinum wire (0.157
2

Electrode:-Titanium coated with oxide of

surface area) Cathode:-Ti plate (2.2 cm2)

the pollutants by 69 % for phthalic acid and by 74 % for phenol. Energy

Anode electrode:-Ti/Ta2O5-SnO2 (2.2 cm

consumption during phthalic acid treatment by EC was 395 Wh (g of

COD removed)−1 while that for US-EC, it was 123 Wh (g of COD re-
moved)−1. Similarly, energy consumption for phenol mineralization by
Typical studies of US-EC oxidation of miscellaneous pollutants.

EC was 435 Wh (g COD removed)−1, while for US-EC, it was reduced to

Experimental Conditions

112 Wh (g COD removed)−1.

However, few studies have reported that the application of ultra-
sound in combination with the EC technology increases the energy re-
quired for the degradation of the pollutants [68,116]. Shestakova et al.
Electrodes

[126] worked on the effect of current on energy consumption of the EC

process and found that with an increase in the current from 10 to 30
cm)

cm)

mA, energy consumption increased from 675 to 700 kW h m−3 for 90 %

degradation of the formic acid. Further, the effect of ultrasonic fre-
Perchloroethylene in sodium sulfate

quency on energy consumption was also considered using the US-EC

Perchloroethylene aqueous media

Protein (Bovine serum albumin)

process, and it was found that at the highest frequency of 1176 kHz,
energy consumption was 4346 kW h m−3. The application of ultra-
aqueous media (PCE)

sound with EC techniques increased the energy requirement as well as

mineralization degree (97 %). Barros et al. [68] reported that the ap-
plication of ultrasound in combination with EC techniques increases the
Thiosulphate

energy consumption. At the highest current density of 50 mA cm-2, EC

Formic Acid

(PCE)
Pollutant

required 102.7 kW h kg−1, while US-EC required 337.3 kW h kg−1

Table 5

though the overall rate of oxidation increased with the application of

ultrasound, but energy consumption increased. Xia et al. [116] reported

15
P. Ritesh and V.C. Srivastava Journal of Water Process Engineering 37 (2020) 101378

the dual pulse ultrasound approached to minimize the energy con-

References
sumption in the US-EC technique. It was found that EC, US-EC, and dual
[126]

[129]

[119]
[120]

[116]
pulse US-EC technique consumed energy of 0.0812 kW h L-1, 0.3039 kW

[68]

[74]

[76]

[97]

[93]
h L-1, and 0.1413 kW h L-1, respectively, for 63, 77 and 80 % removal of
nitrobenzene in 30 min, respectively. Hence, energy used in the de-

However, the decrease in energy consumption was linear from 0 to 100 W, beyond which, the energy consumption remains

During the US-EC of IBU, the energy consumption (including electrolysis and sonolysis) linearly varied between 1.0 and 10

The US-EC technique using platinum and stainless-steel electrodes and cup horn-type transducer is highly efficient in terms
Ultrasound increases the rate of electrochemical oxidation of amaranth dye, but the process is less efficient in terms of
gradation of nitrobenzene using dual pulsed US-EC techniques was only
The COD removal efficiency was obtained 58.3 % and 63.74 % in electrochemical and sonoelectrochemical process,

The total energy consumption reduced to half as compared with simple electrolysis/ sonochemical decomposition.
Energy consumption was found to decrease with the increase in the power of ultrasound during electro-oxidation.
about 46.5 % that of conventional US-EC techniques. This study shows
The time required for achieving the same degradation efficiency was reduced about twice in sonoelectrochemical

that energy consumption in the US-EC method can be significantly re-

duced by dual pulsed ultrasound over the conventional US-EC techni-
ques for the mineralization of the refractory organic wastewater.
Higher energy consumption in US-EC techniques and limited scale-
up potential hindered the development of US-EC techniques. For better
understanding, the energy consumption, more aspects like the design of
suitable ultrasound producers, electrode material must be taken in to
For complete mineralization, energy consumption decreased by 69 % using ultrasound.
For complete mineralization, energy consumption decreased by 74 % using ultrasound.

Pulsed ultrasound reduces energy consumption by 20 % over continuous ultrasound.

account at comparable conditions so that this technique can be devel-
oped.

5. Summary and future perspectives

EC technologies, in combination with ultrasound, are found to be

promising techniques for the enhancement in the degradation of the
POPs due to their environmental compatibility, amenability of auto-
mation, high-energy efficiency, versatility, and safe operation under
mild operation condition. Ultrasound increases the pollutant mass
transport across the electrode surface and eliminates the electrode
fouling by virtue of the physical and chemical effects of cavitation, such
as micro-jet and shock waves. US-EC techniques in-situ generate oxi-
dizing agent without any chemical addition and eliminate any passi-
vation layer from the electrode surface, which also enhanced direct
A, from 1.43 to 85.7 kW h m−3

oxidation of the pollutants on the surface of the electrode. The use of

US-EC techniques also reduces the energy required for the complete
of energy consumption.
Additional information

mineralization of the pollutants. Further, degradation rate kinetics is

energy consumption.

also higher in the US-EC system. However, the energy required for the
complete removal of the organic pollutant is still a crucial issue in the
experiments.

respectively.

scale-up of the geometry of the reactor for the industrial application.

This can be addressed by using lower ultrasonic intensity equipment in
stable.

the pulse mode. More contact between pollutants and ROS is the es-
sential criterion. Ultrasound frequency is a vital parameter in assessing
the synergism. More scientific studies on ultrasonic frequency is re-
123 Wh gCOD removed−1
112 Wh gCOD removed−1

quired in order to optimize it. The electrode material activity in the

65.7 kW h kg of COD

presence of ultrasound needs to be further evaluated so as to compete

0.31 kW h kg COD
337.3 kW h Kg AD

with more expensive metal oxides such as IrO2 and RuO2. Both theo-
−1
56.57 kW h m−3

0.123 kW h m−3
1785 kWh m−3

0.44 kW h L−1

0.1413 kW h L

retical and experimental studies are required for giving a guideline for
removed−1

removed−1

removed−1

selecting a proper set of electrodes. Further, the conversion of electrical

energy into cavitation energy is inefficient. About 30–40 % supplied
Typical studies of energy consumption of US, EC and US-EC technique.
US-EC

electrical energy is actually transferred to producing the desired final

effect. This issue needs to be addressed and planned in order to over-
come the energy barrier. Optimum design and shape of the reactor
395Wh gCOD removed−1
435Wh gCOD removed−1

along with the position of electrode and ultrasound generator are the
two essential aspects of the US-EC reactor, which needs to be carefully
72.3 kW h kg COD

0.51 kW h kg COD
−1

−1

addressed so that the scale-up of the reactor for the industrial appli-
700 kW h m−3

102.7 kW h Kg

0.86 kW h L−1

0.0812 kW h L

cation can be possible. Novel electrode materials such as Ta and Sn for

removed−1

removed−1

organic compound degradation are the best alternative of expensive

electrode of Pt group metal such as Ir and Ru. Thus, the operating cost
EC

of the process can be minimized by electrode surface modification using

a suitable precursor that can also provide high over-potential for
oxygen formation. Pilot-scale studies on the US-EC reactor is not much
reported yet. The power density used in reported studies is high. It is
Organic Pollutants in Saline

recommended to use a low power density of approximately 0.05 Wm

Reactive Red 195(RR-195)

Reactive Blue 19 (RB-19)

L−1 in order to make the process economically viable at industrial

Amaranth dye (AD)

scale. A vast majority of the research has been performed in a labora-

Nitrobenzene (NB)
Phthalic acid (PA)
Formic Acid (FA)

tory only with the traditional design of the US-EC reactor in which
Ibuprofen (IBU)

Ibuprofen (IBU)
Wastewater

electrode is dipped in the US bath or ultrasonic horn dipped in EC cell.

Phenol (Ph)
Pollutant

It is must require to develop a new geometry of the US-EC reactor by

Table 6

incorporating the above issues so that these techniques can be im-

plemented in industries for the wastewater treatment. Overall

16
P. Ritesh and V.C. Srivastava
contribution from the field of electrochemistry, sonochemistry, physics,
and chemical engineering can provide valuable input for the true op-
timization of US-EC reactor geometries. It should also be noted that this
technology is in the developing phase. Once it will developed the cost of
the treatment would decrease.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgment
One of the authors (Ritesh Patidar) acknowledges to quality im-
provement program supported by All India Council for Technical
Education (AICTE), Government of India, for providing the scholarship
for pursuing this research at the Indian Institute of Technology Roorkee.
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