Available online at www.sciencedirect.
com Current Opinion in
ScienceDirect
Review Article
Ozone-based electrochemical advanced oxidation
processes
Irene Bavasso1, Daniele Montanaro2 and Elisabetta Petrucci1
Abstract
Novel processes have recently been developed that provide for
the enhancement of ozonation through combination with
electrochemical treatments. These are processes that can be
included among those defined as advanced oxidation pro-
cesses as they proceed via electrogeneration of highly
oxidizing radical species.
These processes are generally carried out by sparging ozone
in both divided and undivided electrochemical cells in order to
promote its decomposition through different mechanisms,
depending on the electrode materials adopted, and in some
cases still debated.
This mini review presents the most recent advances in the field
of electrochemically assisted ozonation.
In particular, the first section is focused on the process known
as electroperoxone (EP) where the ozone decomposition is
enhanced by the adoption of carbon-based cathodes, due to
the electrogeneration of hydrogen peroxide, while the second
section is focused on the process that implies ozonation in a
cell adopting metal-based cathodes.
Addresses
1 disinfectant action, the direct oxidation by ozone in-
Department of Chemical Engineering Materials Environment, Sapi-
enza University of Rome, Via Eudossiana, 18, 00184, Rome, Italy
2
ISPRA, Italian Institute for Environmental Protection and Research,
Via Vitaliano Brancati 48, 00144, Rome, Italy
Corresponding author: Petrucci, Elisabetta (elisabetta.petrucci@
uniroma1.it)
Current Opinion in Electrochemistry 2022, 34:101017
This review comes from a themed issue on Environmental Electro-
chemistry (2022)
Edited by Ernesto Calvo and Artur Motheo
For complete overview about the section, refer Environmental Electro-
chemistry (2022)
Available online 26 April 2022
https://doi.org/10.1016/j.coelec.2022.101017
2451-9103/© 2022 Elsevier B.V. All rights reserved.
Keywords
Ozonation, Electrolysis, Electroperoxone, Electrolysis-catalyzed ozon-
ation, Hydroxyl radical, Ozonide ion, Hydrogen peroxide, Scavenger,
Carbon-based cathodes, Metal-based cathodes.
Introduction
For the mineralization of recalcitrant and/or toxic organic
compounds, advanced oxidation processes (AOPs) are
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Electrochemistry
needed to overcome the limitations faced by conven-
tional treatments. This is a broad class of treatments
based on the decomposition of benign oxidizing agents
such as hydrogen peroxide (H2O2) and ozone through
metal catalysts or external sources of UV light or ultra-
sounds. Their effectiveness relies on the in-situ forma-
tion of highly oxidizing radicals.
Ozone is an unstable gas at room temperature that
rapidly decomposes into oxygen thus avoiding the risk of
secondary pollution (Eq. (1)).
O3 þ H2 O/2O2 þ 2H þ (1)
The Food and Drug Administration (FDA) recognizes,
under specific conditions, as a GRAS agent (Generally
Recognized As Safe).
However, despite the high redox potential (2.07 V vs
SHE in acidic solution), accounting for its strong
volves a slow degradation rate and poor mineralization of
the target compounds [1].
To enhance the effect of ozone, different approaches
have been tested including the adoption of alkaline
conditions, the co-dosage of H2O2, or coupling with UV
light sources. In all pathways, an indirect mechanism is
activated through the formation of secondary oxidants.
However, due to the limitations presented by the pre-
vious processes, especially in terms of costs and feasi-
bility, new routes are being explored. Recently, some
treatments based on the combination of ozonation with
electrochemical methods have been proposed.
Electrochemical processes are widely recognized as
being versatile, easily automatable, and environmentally
friendly. Considering the possibility of power supply
through renewable energy sources, it is not difficult to
understand why a renewed interest is growing in their
application also in hybrid treatment schemes.
This mini-review reports current orientations and
ongoing developments regarding the combined pro-
cesses between electrolysis and ozonation. The interest
is focused on the cathode processes which are less
energy-demanding than the anodic ones due to the lower
Current Opinion in Electrochemistry 2022, 34:101017
2 Environmental Electrochemistry (2022)
current intensities adopted. Because of the milder con-
ditions, the cathode processes also minimize the occur-
rence of parasitic reactions and guarantee a longer service
life of the adopted electrodes [2].
In these processes, depending on the electrode mate-
rials adopted, the occurrence of direct reduction of
ozone or its reaction with the electrogenerated H2O2
promotes the production of hydroxyl radicals which, as
known, are unselective and highly reactive oxidants
responsible for the rapid degradation and extensive
mineralization of a large number of molecules and
real effluents.
Electro-peroxone
The EP was proposed for the first time in 2013 [3] as an
evolution of the peroxone reaction where the addition of
H2O2 contributes to the HO2- formation (Eqs. (2)e(5))
thus speeding up the ozone decomposition process (that
is promoted at alkaline pH [4]) and formation of radical
oxidizing species (ROS) [5e7].
H2 O2 4 HO
2 þH
þ
(2)
O3 þ HO $ 
2 /HO þ O2 þ O2 (3)
O3 þ HO  $ rent. It is pivotal for the identification of the optimal
2 /O3 þ HO2 (4)
HO$2 þ OH  4O
2 þ H2 O (5)
Peroxone is an effective AOPs technique for the removal
of low reactive ozone species (i.e. ibuprofen, clofibric
acid, p-CBA, primidone, fluconazole, levetiracetam)
[8,9] and the prevention of secondary pollution
[10e14]. For the scale-up of the process, some draw-
backs are related to the use of an excess of reagents,
their storage, and transport. For this reason, more
attention has been paid to the EP based on the in-situ
H2O2 production.
Recent literature (2018e2021) is addressed to three
main themes: i) the comparison of the EP other AOPs;
ii) the investigation of the process set-up (reactor
configuration and cathodic materials; iii) the treatment
of emerging micropollutants in real water matrices and
the prevention of toxic by-products formation. As
regards the first theme, a significant number of articles
aim to demonstrate the effectiveness of the EP for the
ozonation and the electrochemical oxidation with in-situ
production of H2O2. In such a contest the effect of the
operative parameters as applied current density, ozone
flow rate, and pH is evaluated. In some cases, the
comparison involves other ozone-assisted treatments
Current Opinion in Electrochemistry 2022, 34:101017
with UV [15], or EP-assisted treatment with ultrasound
[16], UV [17], and catalysts [18,19].
The experimental set-up mainly adopted consists of an
undivided cell, in particular cylindrical reactors
[2,6,9,12,14e16,19e41], filter press cells [42e48], and
baffled ones [11,49,50]. Other configurations are
divided cells [51] and electrochemical filter [52]. As
regarding the ozone provision, usually an ozone gener-
ator fed with pure O2 is adopted and a mixture of O3/O2
is bubbled directly into the reactor [6,11,12,14e16,
19,20,22e24,26,29,31e35,37,39e41,43,44,47,49e51].
In a few articles, the ozone is produced in form of stock
solution and mixed with the water to be treated before
the entry into the reactor [9,28,36,38,42,46,48,52].
Alternative ways to produce ozone are proposed for
example from the air [2] or anodic oxidation reaction
(Eq. (6)) [25,30,53].
3H2 O / 6H þ þ 6e þ O3 (6)
The set-up also involves the selection of the cathodic
materials suitable for the electrochemical production of
H2O2. Carbon-based materials are known as highly
performant in terms of H2O2 production and whose
production rates are closely related to the applied cur-
current to be adopted because, although the increase of
the applied current deals with the increase of H2O2
production, it involves the occurrence of parasitic re-
actions. Jointly with the applied current, other operative
parameters influence the occurrence and the perfor-
mances of the EP. Several studies have demonstrated
the effectiveness of EP during the decomposition and
mineralization of organic molecules (dyes, pharmaceu-
tical, biocide) in a synthetic wastewater formulation
based with Na2SO4 as a supporting electrolyte with a
concentration in the range from 0.01 M to 0.2 M. Details
are summarized in Table 1.
Noteworthy are the discussions proposed in articles
whose aim is the treatment of real wastewater [24,25],
or the adoption of real water matrices where pharma-
ceutical molecules are spiked in a concentration com-
parable with those typical of micropollutants. In general,
these articles prove the effectiveness of the EP with
respect to ozonation since the formation of hydroxyl
radicals can enhance the degradation of products
(background water constituents) and by-products with
low ozone reactivity. The presence of dissolved organic
matter (DOM) in water can promote the ozonation
treatment due to the formation of hydroxyl radicals from
the ozone decomposition with electron-rich moieties
[15,37]. On the other hand, DOM, carbonates, and
ammonia (in secondary effluent) act as hydroxyl radicals
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Table 1

Ozone-based treatment adopting carbon-based cathode: Comparison of reactors and operative conditions in the treatment of synthetic wastewater (Na2SO4 as the supporting
electrolyte).

Pollutant Concentration pH Cathodic material (dimension) Ozone Applied current Ref.

Acid Orange 7 100–900 mg/L 3–11 Graphite (4 cm2) 20–46 mg/L 250–1000 mA [49]
Acid Orange 7 50 mg/L 3–9 Graphite felt (42 cm2) 15–41 mg/L 100–400 mA [16]
Acid Orange 7 50–900 mg/L 3–9 Graphite (4 cm2) 0.2–1 L/min 0–1000 mA [50]
Acid Violet 19 20–50 mg TOC/L 3 ferrite modified carbon nanotubes- 17.5 mg/min 15–30 mA cm-2 [42]
based GDE (5 cm2)
p-Aminobenzoic acid 10 mg/L 3–11 (3 cm × 1.5 cm x 0.5 cm; volumetric Ozonized gas 0.2 L min- 10–50 mA cm-2 [51]
area 517 cm-1) 1 (10–30 mg L-1 O3
Chloarmphenicol 20–50 mg/L 3–9 (7 cm × 8 cm x 4 mm) 17 mg/min 5–15 mA cm-2 [46]
2,4-Dichlorophenoxy 5–105 mg/L 2–10 Graphene (15 × 2 cm) 0.5–2.5 mg/L 250–1250 mA [17]
acetic
Diuron 40 mg/L 3–11 Carbon felt (5cm × 3 cm × 2 mm) 2–10 mg/L 50–550 mA [41]
Diuron 40 mg/L 3–10 RVC electrode (1 x 1 x 2.5 cm3) 17.4–260 mg/L h 25–250 mA [2]
Diuron 40 mg/L 3–9 CoFe2O4/carbonized-MIL-100(Fe) 0.2–1 L min-1 100–500 mA [6]
(20 mm × 35 mm 5 mm)
Fluconazone 20 mg/L 3–11 CNTs-PTFE gas diffusion 7.2–29.7 mg/L 10–60 A/cm2 [18]
electrode (2.5 × 3.5 cm)
Fluoroquinolones 20 mg/L 2.2–9.5 Graphite felt Ozonized gas 20–80 ml 0.07–0.28 A [33]
(enrofloxacin, min-1 (40.2 mg L-1
norfloxacin, ofloxacin) O3)
Levetiracetam – 3–11 Carbon felt modified with N-doped Ozonized gas 80 ml min- 70–350 mA [43]
Current Opinion in Electrochemistry 2022, 34:101017

rGO (5 cm × 2 cm × 2 mm) 1 (10–70 mg/L O3)

Levofloxacin 20–50 mg TOC/L 3 graphite felt placed on carbon 17.5 mg min-1 15–40 mA cm-2 [45]
cloth-PTFE GDE (3 cm × 8 cm x
0.25 cm, volumetric area 651 cm-
1)

Ozone-based EAOP Bavasso et al.

Oxalic Acid 2 mM 3–9 graphite 30 mg/L 20 mA [29]
sheet (2 cm × 4 cm)
Phenol 200 mg/L – Polyacrylonitrile-based carbon fiber 0.4 400 mA [20]
(brush) L/min
Reactive Black 5 50–250 mg/L 4–10 Graphite 2 g/h 100–400 mA [32]
Sodium oxalate 2 mM 9 graphite coated with g-C3N4/CNT 10–80 mg/L 10–50 mA [19]
(2 × 4 cm)

3
4 Environmental Electrochemistry (2022)
scavengers thus reflecting on the operative treatment
time and/or the reagent dosage [39]. Also, the presence
of chloride in real water matrices can affect the EP chain
reaction since the hypochlorous acid formed by anodic
oxidation of chloride may react with H2O2 thus reducing
its availability for ozone decomposition [8,37]. Finally,
depending on the reuse of the treated water (i.e.
drinking water, discharge in surface water bodies) the
evaluation of toxicity given by by-products or O3/H2O2
residual is fundamental [23]. Wang and collaborators
[15] reported that the treatment of the insecticide
thiamethoxam is enhanced by coupling the ozone with
in-situ H2O2 production or with UV which also avoids
the accumulation of the toxic aldehyde (such as form-
aldehyde) observed during the conventional ozonation.
Guo et al. [36] demonstrated the total inhibition of
bromate formation during the treatment of emerging
contaminants in groundwater with EP due to the
reduced availability of ozone and the quenching of
HOBr/BrO by H2O2.
Ozone electrolysis
Although among the combined treatments of ozone with
electrochemical methods the most investigated
currently is EP, the first attempts to support ozonation
with electrochemical methods have been made with
metal cathodes [54e56].
Unlike EP, this process has not even been assigned an
unequivocal name and different denominations can be
found in the various articles that have been published.
This technology represents a promising mostly unex-
plored niche also for the treatment of real [57e61] or
complex matrix effluents [62,63].
All the articles agree on defining the combination be-
tween ozone (obtained from pure oxygen except for [2])
and electrolysis as a synergistic process that benefits
from increasing current (Table 2). However, there is no
consensus in the literature on how the route leading to
the formation of OH radicals is initiated and proceeds
and on what species are involved. For these reasons, one
of the most debated topics in recent articles remains the
clarification of the reaction mechanisms also with the
use of scavengers capable of selectively reacting with
the radicals involved [2,64e66].
The postulated hypotheses consider that the dissolved
ozone is decomposed by: direct electron transfer from
the cathode via the formation of the ozonide radical ion
O3- [2,54,67] (Eqs. (7) and (8)).
O3 þ e /O
3 (7)
O $ 
3 þ H2 O4HO þ OH þ O2 (8)
Current Opinion in Electrochemistry 2022, 34:101017
reaction with the OH produced at the cathode by water
reduction [63,68] (Eqs. (8)e(11)).
O3 þ OH  /O $
2 þ HO2 (9)
HO$2 4 H þ þ O
2 ðpka ¼ 4:8Þ (10)
O3 þ O 
2 /O3 þ O2 (11)
reaction with the electrogenerated H2O2 by cathodic
reduction of dissolved oxygen on the surface of a DSA-type
cathode [61] and on the surface of particles of granular
activated carbon used as inter-electrode packing for the
realization of a 3D-electrode [60,65]. In addition to the
contribution of all three aforementioned reactions, the
possible involvement of radical species formed at the anode
[59,64]. Eq. (6) reminds Fenton’s reaction and similarly is
expected to be promoted by acidic conditions [2]. How-
ever, conflicting data can be found, and the effect of this
parameter is still debated in the recent articles examined.
In some cases, an optimal value of 5 is reported [65] while
in general neutral or alkaline values conditions appears
beneficial to the synergy. This behavior is explained
differently according to the proposed decomposition
routes. In particular, it is suggested that acid pH values.
i) Increase the absorption of Hþ on the cathode and
promote the occurrence of the hydrogen evolution
reaction which competes with the ozone depletion
[66].
ii) Reduce the thickness of the alkaline zone near the
cathode responsible for the decomposition of ozone
and favor the conversion of OH radicals to water
[68].
iii) Promote two-electrons ozone reduction with oxygen
formation to the detriment of radical species [67]
(Eq. (12)).
O3 þ H2 O þ 2e /2OH  þ O2 (12)
At present, it is not possible to compare the performance
of EP and ozone-electrolysis as there are only two arti-
cles dealing with this aspect that come to opposite
conclusions. In one article, where EP outperforms the
ozone-electrolysis process, the improvement is
explained by considering the increased absorption ca-
pacity of carbon-based materials that retain ozone thus
increasing the probability of its reduction [66]. How-
ever, Bavasso et al. [2] reported faster mineralization on
a SS cathode than in an RVC electrode. Moreover,
metal-based electrodes certainly exhibit greater dura-
bility. Yet this aspect as well as the optimization of the
fluidodynamic conditions of the electrochemical reactor
have not yet been thoroughly investigated.
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Table 2

Ozone-based treatment adopting metal-based cathode: Comparison of reactors and operative conditions.

Pollutant Concentration pH Cathodic material Cell Ozone Applied current Ref.

(dimension)

Atrazine in 1 mM fosfate 10 mg/L 7 C: SS (23.7 cm2) Undivided acrylic reactor From pure O2, 0.3 10 mA cm−2 [63]
buffer+chloride and A: BDD (23.7 cm2) (Vw = 0.47 L) L/min
bromate
Atrazine in 1 mM fosfate 10 mg/L 2–12 C: SS (2.5 × 5 cm2) Undivided acrylic reactor From pure O2, 0.3 10 mA cm−2 [68]
buffer +sulfate A: BDD (2.5 × 5 cm2) (Vw = 0.47 L) L/min
Concentrated 2 mM 9 C: SS (12 × 12 cm2) Undivided acrylic reactor From pure O2, 1 30 mA cm−2 [59]
Leachate A: RuO2/TiO2/ (Vw = 2.5 L) L/min
Ti(12 × 12 cm2)
Cu(II) organic 0.3 mM 4 C: Ti mesh (25 cm2) Undivided cylindrical From pure O2, 0.5 16 mA cm−2 [67]
complexes in 50 mM A: Ti mesh (25 cm2) reactor (Vw = 0.9 L) L/min
Na2SO4
1,4 dioxane in 20 mM 1.0 mM 3–7 C: SS (8.8 cm2) Ozone From pure O2, 0.2 L/min 2.5–10 mA cm−2 [67]
Na2SO4 A: IrO2/Ti (8.8 cm2) contactor+undivided
flow cell, cylindrical
reactor (flow
rate = 90 ml/min)
(Vw = 0.25 L)
Diuron in 50 mM 40 mg/L 3–10 C: SS electrode Undivided cylindrical From air, 17 mgO3L−1h- 25–250 mA [2]
Na2SO4 (2 × 2.5 cm2) reactor (Vw = 0.1 L) 1
1 and 260
A: Pt wire mgO3L−1h−1
NItrobenzene in 6 mg/L 6.6 C: Pt.plating Ti electrode Undivided cylindrical From pure O2, 0.1 300 mA [65]
Current Opinion in Electrochemistry 2022, 34:101017

100 mM Na2SO4 (5 × 3.5 cm2) reactor (Vw = 0.5 L) L/min

A: Pt.plating Ti
electrode
(5 × 3.5 cm2)
GAC packing

Ozone-based EAOP Bavasso et al.

Nitrobenzene in 100 mg/L 5.5 C: SS mesh (160 cm2) Divided flow reactor with From pure O2, 0.67 0–2 A [64]
Na2SO4 A: ceramic-base b ceramic diaphragm L/min
PbO2 BDD (160 cm2)
Petroleum 100–900 mg/L 9 C: RuO2/Ti(5 × 5 cm2) 2L, undivided cylindrical From pure O2, 0.5 L/min 30 mA cm−2 [61]
hydrocarbons A: RuO2/Ti(5 × 5 cm2) reactor (Vw = 1 L)
Pharmaceutical 13.475 mg TOC/L 12.8 C: SS(12 × 12 cm2) Undivided cylindrical From pure O2, 0.4 10–31 mA cm−2 [60]
wastewater A: RuO2/Ti(12 × 12 reactor (Vw = 0.5 L) L/min
cm2)

5
6 Environmental Electrochemistry (2022)
Current prospects and future developments
The combination of ozone with electrochemical treat-
ments aimed at promoting the formation of highly
oxidizing species for the mineralization of molecules of
environmental concern represents a promising technol-
ogy that involves no addition of external reagents and
the potential for full-scale implementation.
However, the viability of the process is unclear since the
current literature lacks a cost evaluation and optimiza-
tion. Ozone supply is usually operated by converting
oxygen and this can limit the application because of the
storage and cost of a gaseous source. Ozone from the air
or produced by anodic oxidation of oxygen from water
electrolysis can be considered a valid but still poorly
explored alternative.
A precise assessment of both emissions and release of
potentially harmful compounds is needed. It is also
necessary to intensify tests on real effluent where the
interferences deriving from the matrix do affect the final
removal efficiency.
In several articles, new cathode materials are proposed
but there are no standardized tests or patented mate-
rials to be considered for the critical evaluation of the
performances in view of the material commercialization.
A crucial disregarded topic is the service lifetime and
possible failure of the electrode materials that, though
exposed to low current density values, often work under
very acidic electrolytes and in the presence of a strongly
oxidizing environment.
Declaration of competing interest
The authors declare that they have no known competing
financial interests or personal relationships that could
have appeared to influence the work reported in
this article.
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* of special interest
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