Desalination 299 (2012) 115

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Desalination
journal homepage: www.elsevier.com/locate/desal

Trends in electro-Fenton process for water and wastewater treatment: An overview

P.V. Nidheesh, R. Gandhimathi
Department of Civil Engineering, National Institute of Technology, Tiruchirappalli, Tamilnadu, India

a r t i c l e

i n f o

Article history:
Received 29 February 2012
Received in revised form 3 May 2012
Accepted 5 May 2012
Available online 14 June 2012
Keywords:
Electro Fenton
Wastewater treatment
Degradation
Organic pollutant

a b s t r a c t
Organic compound, especially aromatic compound is the main pollutant in industrial efuent. Conventional
wastewater treatment processes are inefcient for the removal of these types of toxic and hazardous pollutants from wastewater. Electro Fenton is one of the powerful and environmentally friendly emerging technologies for the remediation of wastewaters containing organic, especially aromatic compounds. This paper
reviews the fundamentals and recent developments in electro Fenton process. Electro Fenton process utilizes
different electrolytic reactors such as bubble reactor, lter press reactor, divided double-electrode electrochemical cell, divided three-electrode electrochemical cell and double compartment cell. Different cathodes
as working electrode and anodes as counter electrode used in this process are analyzed. The effects of various
operating parameters and their optimum ranges for maximum pollutant removal and mineralization are
reviewed. Also various pollutants removed by this process are evaluated. Quick removal and mineralization
of pollutants and their intermediate reaction products were reported.
2012 Elsevier B.V. All rights reserved.

Contents
1.
2.

3.
4.
5.

6.

7.

Introduction . . . . . . . . . . . . . . . . . . . . . . . . .
E-Fenton reactors . . . . . . . . . . . . . . . . . . . . . .
2.1.
Bubble reactor (BR) (A) . . . . . . . . . . . . . . . .
2.2.
Filter press reactor (FPR) (B) . . . . . . . . . . . . . .
2.3.
Divided double-electrode electrochemical cell (DDEC) (C)
2.4.
Divided three-electrode electrochemical cell (DTEC) (D) .
2.5.
Double compartment cell (DCC) (E) . . . . . . . . . .
Electrode materials . . . . . . . . . . . . . . . . . . . . . .
Kinetics of E-Fenton process . . . . . . . . . . . . . . . . .
Affecting factors . . . . . . . . . . . . . . . . . . . . . . .
5.1.
pH . . . . . . . . . . . . . . . . . . . . . . . . . .
5.2.
Oxygen sparging rate . . . . . . . . . . . . . . . . .
5.3.
Temperature . . . . . . . . . . . . . . . . . . . . .
5.4.
Applied current density . . . . . . . . . . . . . . . .
5.5.
Fe 2+ concentration . . . . . . . . . . . . . . . . . .
5.6.
Hydrogen peroxide concentration and feeding mode . . .
5.7.
Distance between the electrodes . . . . . . . . . . . .
5.8.
Nature of the supporting electrolyte . . . . . . . . . .
Applications . . . . . . . . . . . . . . . . . . . . . . . . .
6.1.
Dyes . . . . . . . . . . . . . . . . . . . . . . . . .
6.2.
Pesticides and herbicides. . . . . . . . . . . . . . . .
6.3.
Phenolic compounds. . . . . . . . . . . . . . . . . .
6.4.
Leachate . . . . . . . . . . . . . . . . . . . . . . .
6.5.
Drugs . . . . . . . . . . . . . . . . . . . . . . . . .
6.6.
Others . . . . . . . . . . . . . . . . . . . . . . . .
Degradation pathway of organic pollutants . . . . . . . . . .

Corresponding author. Tel.: + 91 431 2503171; fax: + 91 431 2500133.

E-mail address: rgmathii@nitt.edu (R. Gandhimathi).
0011-9164/$ see front matter 2012 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2012.05.011

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PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

8.
Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

1. Introduction
The focus on waste minimization and water conservation in the
recent years resulted in the discovery of various treatment processes,
one of them being Advanced Oxidation Processes (AOPs). These refer
to the chemical treatment processes which follow oxidation route
and are particularly employed to degrade biologically toxic and non
degradable chemicals [1]. AOPs have been broadly dened as near
ambient temperature treatment processes based on highly reactive
radicals, especially the hydroxyl radical (OH) as the primary oxidant
[2]. Many processes such as chemical oxidation, Fenton and photoFenton processes, ultraviolet (UV)-based processes, photo-catalytic
redox processes, supercritical water oxidation, sonolysis, and electron
beams and -ray irradiation come under advanced oxidation techniques [1]. The main function of AOPs is the generation of highly reactive free radicals. Hydroxyl radicals (HO) are effective in destroying
organic chemicals because they are reactive electrophiles (electron
preferring) that react rapidly and non-selectively with nearly all
electron-rich organic compounds [3].
Among AOPs, oxidation using Fenton's reagent is an attractive and
effective technology for the degradation of a large number of hazardous and organic pollutants because of the lack of toxicity of the reagents, eventually leaving no residues and the simplicity of the
technology [4]. Maleic acid oxidation was the rst Fenton process
reported by Fenton [5]. The main steps involved in the Fenton process
are (i) Oxidation, (ii) Neutralization, (iii) Flocculation and (iv) Sedimentation. The Fenton process is most effective at pH near to 3 [6].
Normally the organic substances are removed at two stages of oxidation and coagulation [7]. Oxidation of organic substances is due to
OH radicals and coagulation is ascribed to the formation of ferric
hydroxo complexes [8]. The degradation mechanism of organic pollutants by Fenton reaction is given in Eqs. (1) to (4) [9,10]. The
main advantages and disadvantages of Fenton process are given in
Table 1.
2

Fe

H2 O2 Fe

OH HO

RH HO R H2 O

1
2

where, RH denoting organic pollutants

R Fe
2

Fe

R Fe

HO Fe

[2224]. Moreover, electricity as a clean energy source is used in the

process, so the overall process does not create secondary pollutants
[21]. Since E-Fenton process is not using any harmful reagents, it is
an environment friendly method for water and wastewater
treatment [25]. The typical mechanism of E-Fenton process is illustrated in Fig. 1.

O2 2H 2e H2 O2

This review reports on the most recent experimental studies and

developments in the eld of E-Fenton process. Fundamentals, experimental setups, main reactions, the parameters that affect these processes and various applications are discussed in detail. Different
cathodes and anodes used for E-Fenton process are also analyzed in
this work.
2. E-Fenton reactors
Electrolytic reactor is one of the essential parts of E-Fenton process. There are several types of electrolytic cells used by researchers.
Some of the important types of such cells are explained below.
2.1. Bubble reactor (BR) (Fig. 2A)
The E-Fenton bubble reactor (a glass cylindrical reactor) having working volume of 0.675 L was operated in batch mode with
total reux or continuous mode by Rosales et al. [27]. The cathode
and anode bars were placed at a distance of 30 mm and 270 mm
above the bottom of the cell, respectively. Steel bars having a total
contact surface area of 3.14 cm 2 or graphite bars having a total contact surface area of 1.27 cm 2 were used. A constant potential difference (15 V) was applied with a power supply and the process was
monitored with a multimeter.
2.2. Filter press reactor (FPR) (Fig. 2B)
Prabhakaran et al. [28] used lter press reactor of capacity 2 L for
the removal of resin efuents. The uid ow circuit consists of a reservoir, a magnetically driven self priming centrifugal pump, a ow
meter and the electrolytic cell. The electrical circuit consists of a

OH

Electrochemical advanced oxidation processes (EAOPs) based on

Fenton's reaction chemistry are eco-friendly methods that have recently received much attention for water remediation [18]. The
most popular EAOP is the electro Fenton (E-Fenton) process [19]. EFenton process has two different congurations. In the rst one,
Fenton reagents are added to the reactor from outside and inert electrodes with high catalytic activity are used as anode material while in
the second conguration, only hydrogen peroxide is added from outside and Fe 2+ is provided from sacricial cast iron anodes [20]. Compared to the conventional Fenton process, the electro-Fenton process
has the advantage of allowing better control of the process and
avoiding the storing and transport of the H2O2 [21]. In this approach,
H2O2 is continuously supplied to the contaminated solution by a twoelectron oxygen reduction in an acidic medium according to Eq. (5)

Table 1
Advantages and disadvantages of the Fenton process.
Advantages

Disadvantages

No energy input is necessary to

activate hydrogen peroxide [11]
Fenton's reagent is relatively
inexpensive and the process is
easy to operate and maintain [13]

Ferrous ions are consumed more rapidly

than they are regenerated [12]
Treatment of the sludge-containing Fe
ions at the end of the wastewater
treatment is expensive and needs large
amount of chemicals and manpower [14]
It is limited by a narrow pH range
(pH 23) [16]
Iron ions may be deactivated due to
complexion with some iron complexing
reagents such as phosphate anions and
intermediate oxidation products [16]
Additional water pollution caused by
the homogeneous catalyst that added
as an iron salt, cannot be retained in the
process [11]

Short reaction time among all

advanced oxidation processes [15]
There is no mass transfer limitation
due to its homogeneous catalytic
nature [17]
There is no form of energy involved
as catalyst [17]

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

Fig. 1. Reaction mechanism of E-Fenton process [26].

regulated D.C. power supply; ammeter and the cell with the voltmeter are connected in parallel to the reactor.

volume. A digital DC power supply was connected to the electrodes.

1 N H2SO4 solution was used to adjust the pH between 3 and 5.

2.3. Divided double-electrode electrochemical cell (DDEC) (Fig. 2C)

2.4. Divided three-electrode electrochemical cell (DTEC) (Fig. 2D)

Reactor consisting of a 0.5 L glass beaker equipped with iron cathode

and anode, installed in parallel was used by Kurt et al. [29]. Electrodes
having a total effective electrode area of 45.0 cm2 were plunged into
the beaker, containing tannery wastewater with a 0.4 L working

Zhou et al. [30] used DTEC reactor for the removal of methyl red
from aqueous solution. This type of reactor contains a saturated calomel
electrode (SCE) as reference electrode in addition to DDEC. Potential
controlled electrolysis is the main purpose of SCE in DTEC.

(6)

(1)

(4)

(8)
(7)

(1)

(5)

(9)
(2)

(3)

(6)

(A)
A

(10)

(6)

(B)
(1)

(1)

(1)

(4)
(13)
(3)

(11)

(C)

(3)

(3)

(12)
(4)

(11)

(D)

Compartment 1

Compartment 2

(E)

Fig. 2. Schematic diagram of electrolytic reactors (A) BR [27] (B) FPR [28] (C) DDEC [29] (D) DTEC [30] (E) DCC [31] (1) power supply, (2) air compressor, (3) cathode, (4) anode, (5)
control unit, (6) pumps, and (7) reux (8) rotameter (9) reservoir (10) electro chemical reactor (11) magnetic stirrer (12) oxygen tank (13) SEC.

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

Fig. 3. Recent citations of E-Fenton reactors.

2.5. Double compartment cell (DCC) (Fig. 2E)

DCC contains two compartments for electrolytic action. Yuan et al.
[31] conducted experiments with DCC type of reactor for the degradation of Rhodamine B. Anode (Pt akes) and cathode (Pt akes) were
placed in compartment 1, whereas in compartment 2 only cathode
was placed. Direct current was provided by a power supply. Salt
bridge lled with saturated K2SO4 and agar was used to connect the
compartments. Micro bubbles of H2 and O2 were generated in compartment 1 by water electrolysis. Excess production of H + compared
with OH results in lowering of pH in between 2 and 3. Cathode 2 in
compartment 2 was used as a bypass to accumulate OH and to neutralize the low pH efuent from compartment 1 [31].
The recent citation of above reactors is shown in Fig. 3. From Fig. 3,
it is observed that DDEC and DTEC reactors were used in the E-Fenton
process by many researchers.
3. Electrode materials
Selection of anode and cathode material is one of the signicant
steps in E-Fenton process. For example, selection of unstable anode
will cause deterioration of electrode in electrolytic cells. High-oxygen

Fig. 4. Comparison of recently used anodes in E-Fenton process.

Fig. 5. Comparison of recently used cathodes in E-Fenton process.

overvoltage anode can produce hydroxyl radicals in E-Fenton process

as in Eq. (6) [32],

H2 OHO H e

Pt has been used for a long time as an electrode material due to its
good conductivity and chemical stability even at high potentials and
in very corrosive media [33]. Pt anode was used in more numbers
for the degradation of pollutants in E-Fenton system (Fig. 4). The different forms of Pt anodes such as Pt sheet [19,3439], Pt gauze
[25,4042], Pt foil [43], Pt akes [31], Pt grid [44,45], platinum
plate [46], Pt mesh [39] etc. were used for the degradation of pollutants. But it is rarely used for a practical purpose because of its high
cost. The various anodes other than Pt being recently used are
shown in Fig. 4. Boron-doped diamond (BDD) electrode synthesized
by the hot lament chemical vapor deposition technique on singlecrystal p-type Si (100) wafers was used by Isarain-Chavez et al. [47]
for the mineralization of atenolol. Borra's et al. [48], zcan et al.
[44], Pozzo et al. [49] and Sire's et al. [39] used BDD as an anode for
wastewater treatment. Feasibility of Titanium (Ti) rod coated with
IrO2/RuO2 in the E-Fenton process has been studied by Huang et al.
[50] and Prabhakaran et al. [28]. RuO2/Ti mesh [51] and Iron [52] are
some other types of anodes being used recently in E-Fenton process.
Efciency of E-Fenton system depends more on efciency of cathode. Hence it is also known as working electrode. The various cathode
materials used for laboratory-scale and pilot-scale are shown in Fig. 5.
Commercial graphite felt [34], carbon felt [35,38,40,42,46,53], BDD
plate [54],carbon-polytetrauoroethylene (PTFE) [37,39,43], graphitePTFE [30], graphite [55], reticulated vitreous carbon (RVC) [25,41],
activated carbon ber (ACF) [51], Pt akes [31], carbon sponge [44],
stainless steel [28,48,49], and titanium [52] are some of the recently
used working electrodes in wastewater treatment. The details of anode
and cathode including cell conguration are summarized in Table 2.
Different congurations of cathode were also used by various researchers. The usage of composite electrodes is the emerging trend
in E-Fenton system. Fan et al. [64] prepared Fe-CHI/Ni|ACF|Fe-CHI/
Ni sandwich lm cathode for the removal of Rhodamine B (Note:
Fe-CHI Fe 2+-chitosan, Ni Nickel). Fe@Fe2O3/ACF [19], Cu2O/
CNTs/PTFE (Note: CNT Carbon Nanotubes) [36] and Fe@Fe2O3/
CNT [65] were also used as composite cathodes in E-Fenton process.
Wang et al. [66] used platinum wire anode placed inside a hollow cylindrical cathode (2.9 cm diameter and 7 cm height), composed of
one layer of polyacrylonitrile (PAN) based activated carbon ber
cloth held by two plastic screens. This design makes the primary

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

Fig. 6. Pathway of Acid Red 97 degradation products using carbon felt cathode and Pt anode [40].

current or potential distribution more uniform. The oxygen gas from

an oxygen cylinder was dispensed directly at the bottom of the hollow cylindrical cathode [66].
Different congurations were used for the application of electrochemical remediation techniques and the electrodes could be made
of different materials. A signicant interest in the effectiveness of different electrode materials has recently arisen, with the use of stainless steel, graphite, platinum, PbO2, titanium compounds, boron
doped diamond, and ceramics [27]. Oxidation capacity and removal
efciency of different electrodes were also compared by different researchers. Sire's et al. [39] evaluated and compared the oxidizing
power of the four E-Fenton systems to mineralize chlorophene solutions from the Total Organic Carbon (TOC) decay. Four different EFenton systems are: (i) a Pt/O2 diffusion cell (ii) a BDD/O2 diffusion
cell (iii) a Pt/carbon felt cell and (iv) a BDD/carbon felt cell. A

continuous, but slow, TOC abatement with 52% of mineralization

has been observed in the Pt/O2 diffusion cell after 660 min of electrolysis at 300 mA. But BDD/O2 diffusion cell has a removal efciency of
100% with rapid and total mineralization by applying high currents.
This indicates that BDD has greater oxidation ability than that of Pt
[39]. Isarain-Chavez et al. [56] also reported a same trend for degradation of atenolol from aqueous solution. The study demonstrated that
BDD/carbon felt cell has higher oxidizing power than Pt/carbon felt
cell to decontaminate the solution completely in a shorter time [56].
Siminiceanu et al. [37] reported better performances by the replacement
of Pt with BDD anode. The mineralization current efciency becomes
1.53 to 3.25 times higher; whereas specic energy consumption is 1.43
to 2.81 times lower for BDD than that of Pt [37]. zcan et al. [44] reported
that the formation rate of hydroxyl radicals and the decay rate of organics
are faster on BDD anode than that of Pt. Hammami et al. [67] also

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

Table 2
Specications of anodes and cathodes used in E-Fenton process.
No Reactor conguration

Anode specication

Cathode specication

Reference

Pt sheet of 99.99% purity

Carbon-PTFE, carbon felt of area 3 cm2

[56]

Cylindrical Pt mesh or a 25 cm2 thin-lm

boron-doped diamond Ti/RuO2

Carbon-felt of size 14 cm 5 cm each side

and 0.5 cm in width
Stainless steel
Iron of size 2.0 mm 6.0 cm 7.5 cm
Graphite of size 75 mm 30 mm 6 mm and
having an effective electrode area of 22 cm2.
Carbon felt of dimensions 6 cm 8 cm 0.6 cm
and 6 cm 17 cm 0.6 cm.
Carbon felt having an area of 60 cm2
(15 cm 4 cm)
Stainless steel cylinder with an inside
diameter of 8 cm and a height of 17.5 cm
Carbon felt of size 3 cm 5 cm.
A 3 cm2 carbon-PTFE and 70 cm2
(17 cm 4.1 cm) carbon felt

[57]

2
3
4
5
6

Open and undivided tank reactor containing

100 mL of solution
A small, open and undivided cylindrical glass
cell of 6 cm diameter and 250 mL capacity
A glass reactor of capacity 600 mL
0.5 L glass beaker with a 0.4 L working volume.
Borosil glass of capacity 0.5 L

0.40 L open and undivided cylindrical glass

cell of internal diameter 60 mm
Open undivided cylindrical glass cell of 6 cm diameter
and 500 mL capacity
Reservoir of capacity 5 L

9
10

Glass reactor of capacity 300 mL

Glass cell of 6 cm diameter and 250 mL capacity

11

An undivided cylindrical glass cell of capacity

0.175 L
Open undivided cylindrical glass cell of 6 cm
diameter and 250 mL capacity
Open undivided cylindrical glass cell of 500 mL
capacity
Cylindrical cell of 250 mL capacity
An open undivided cylindrical glass cell of
100 mL capacity
A divided thermostatic cell of 150 mL in volume
Undivided glass electrochemical cell of 600 mL
capacity
An open and undivided cell with a capacity
of 0.55 L
An undivided glass electrochemical cell of
capacity 500 mL
Glass beakers of capacity 250 mL

12
13
14
15
16
17
18
19
20

Iron plate of size 6.0 cm 7.5 cm

Iron plate of size 55 mm 40 mm
Cylindrical Pt grid
4.5 cm2 Pt cylindrical mesh

[61]

[63]

Pt sheet of 1 cm2 area

Graphite felt of thickness = 0.4 cm, having

an area of 9.5 cm2
Carbon felt of size 12.5 cm 4 cm
BDD plate having geometric area of 2 cm2

[34]

Cu2O/CNTs/PTFE having an area of 3.0 cm2

Reticulated vitreous carbon (RVC) sheet of
an area of 35 cm2 and thickness of 0.9 cm.
20 cm2 area of ACF felt

[36]
[25]

RVC sheet of dimensions 5 cm 7 cm 0.9 cm

[41]

Pt akes of size 1 1 cm

[31]

Pt gauze of area 6 cm2

Platinum (geometric area, 4 cm2)
Pt sheet (purity: 99.99%) of area 2.0 cm2
Platinum gauze of an area 3.8 cm2
RuO2/Ti mesh of area 20 cm2
Platinum gauze of an area 3.8 cm

Pt akes of size 1 1 cm

4. Kinetics of E-Fenton process

The decay of organic pollutants via E-Fenton process can be represented as:

[60]

Titanium rod coated with RuO2/IrO2 with an

outside diameter of 1.5 cm and a height of 16 cm.
Platinum gauze
3 cm2 Pt sheet, 3 cm2 BDD thin-lm deposited
on conductive single crystal p-type Si wafers
and a 4.5 cm2 Pt cylindrical mesh
BDD thin-lm electrode which is deposited on
Carbon sponge of size 1.0 cm 1.0 cm 4.0 cm
both sides of a niobium substrate (3.0 cm 4.0 cm)
2
A 60 cm2 carbon felt
4.5 cm Pt cylindrical mesh

reported similar results for BDD and Pt anodes in the E-Fenton process.
Wang et al. [51] compared the efciency of activated carbon ber and
graphite cathodes for removing azo dye and Acid Red 14 from aqueous
solution. For ACF cathode, after 360 min of electrolysis under the operating conditions of 0.36 A current, 1 mmol/L Fe2+ at pH 3, 70% TOC removal and 100% color removal were achieved. For the same operating
conditions, graphite cathode shows less removal efciency than that of
ACF [51]. Sudoh et al. [68] reported that the graphite was the best cathode material for electrogeneration of H2O2 while metal cathodes such
as copper, stainless steel, lead and nickel were likely to decompose
H2O2. This agrees with the results reported by Rosales et al. [27] for lissamine green B dye (LGB) removal from aqueous solution using graphite
and stainless steel electrodes. The graphite electrodes have the highest
LGB discoloration rate, with total discoloration after 10 h. Moreover,
gradual corrosion was detected in stainless steel electrodes [27]. zcan
et al. [44] compared the propham degradation rate for BDD//Pt, Pt//CS
(Note: CS Carbon Sponge) and BDD//CS systems in acidic media. The
decay rate of propham was higher in BDD//CS system than in BDD//Pt
system. This result indicates that H2O2 production ability of CS was
higher than that of Pt. A slight increase in removal rate was observed in
the case of BDD//CS compared to Pt//CS system [44].

RH OH Oxidation products

[58]
[29]
[59]

[32]
[62]
[39]

[44]

[40]
[54]

[51]

treatment [69]. The rate of decay of organic pollutants can be written

as:
d RH k RHOH 
abs
dt

Since [OH] is constant at steady state, kabs [OH] is equal to kapp.

Where kabs and kapp are absolute and apparent rate constants, respectively. The value of kabs can be determined by kinetic competition
method using the benzoic acid as standard substrate having a kabs
value of 4.3 10 9 L mol 1 s 1 [70,71]. Eq. (8) can be rewritten as:
d RH k RH
app
dt

Integration of Eq. (9) gives the rst order kinetic equation of EFenton process as:
In

RHo
kapp t
RHt

10

Where [RH]0 and [RH]t are the concentration of organic pollutant

at beginning and time t, respectively. The kapp can be determined analytically from the slope of concentration vs. time plot in accordance
with the above equation. The second order kinetic equation of EFenton is given as [4]:

As OH is a very reactive species it does not accumulate in the solution, and its concentration takes a steady-state value during

RHt
1

RHo 1 ktRHo

11

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

Table 3
Optimum pH values of E-Fenton process in various studies.
No

Pollutant

Electrodes

Optimum pH

Efciency (%)

Time (min)

Reference

1
2
3
4
5
6
7

Dyeing wastewater
LGB
Methyl red
Sunset yellow FCF
Dyeing wastewater
Rhodamine B
Biologically treated coking wastewater

Activated carbon ber-Pt wire

Steel-graphite
Graphite PTFE-Pt
RVC-Pt
Graphite-Pt/Ti
Fe@Fe2O3/CNT-Pt
ACF-Ti/RuO2

3
2
3
3
3
3
4

75.2
40
80
100
70
99.6
55

240
120
20
120
150
120
480

[66]
[27]
[30]
[25]
[55]
[65]
[79]

process is reported in Table 3. From Table 3, it was found that the optimum pH for E-Fenton process varies from 2 to 4.

5. Affecting factors
5.1. pH

5.2. Oxygen sparging rate

The pH is one of the most important factors for the E-Fenton
process. Generally Fenton process was conducted in acidic medium. Most of the studies reported that the optimum pH of Fenton
process is around 3 [25,30,55,65]. In traditional Fenton process,
iron species begin to precipitate as ferric hydroxides at higher
pH values. On the other hand, iron species form stable complexes
with H2O2 at lower pH values, leading to deactivation of catalysts.
Consequently, the oxidation efciency dramatically decreases [66].
Acidic medium is the favorable condition for the production of
H2O2 (Eq. (5)) [66]. However, a low pH also promotes hydrogen
evolution, as given in Eq. (12), reducing the number of active
sites for generating hydrogen peroxide [66]. In addition, at pH
below 3, hydrogen peroxide would remain steady according to
the formation of oxonium ion (e.g., H3O2+ as in Eq. (13)) [30].
Due to the regeneration of Fe 2+, through reaction between Fe 3+
and H2O2, Fenton process becomes less effective at pH b 3
[72,73]. At higher pH, the efciency of E-Fenton process decreases
rapidly, especially pH > 5. This is due to the fact that H2O2 is unstable in basic solution. H2O2 rapidly decomposes to oxygen and
water at neutral to high pH with rate constant of 2.3 10 2
and 7.4 10 2 min 1 at pH 7.0 and 10.5, respectively [74,75].

H2 O2 2H 2e 2H2 O

12

13
H2 O2 H H3 O2
The increase in pH during E-Fenton process leads to electrocoagulation whereby pollutants are removed by electrostatic attraction and/or complexation of reactions due to the conversion of Fe 2+
and Fe 3+ to Fe(OH)n type structures [76]. Ting et al. [77] reported
that 2,6-dimethylaniline concentration decreased from 36% to 25%
in 2 h when pH was increased from 1.5 to 2.0. The complete removal
of 2,6-dimethylaniline was achieved after 140 min at pH 2. Also a further increase of pH from 2 to 4 increased 2,6-dimethylaniline concentration from 25% to 85%. Daneshvar et al. [78] suggested the
perchloric acid instead of hydrochloric or sulfuric acid to adjust the
optimal pH value to obtain optimal removal of dyes. But the optimum
pH value shows the disadvantage of E-Fenton process because the pH
of most wastewater samples is not within the optimal range. The optimum pH necessary for the different pollutant removal by E-Fenton

Oxygen is one of the major factors that limit the performance of EFenton system, because increasing the oxygen sparging rate can increase the dissolved oxygen concentration and the mass transfer
rate of dissolved oxygen and nally increase the production of hydrogen peroxide [66]. Chen and Lin [80] reported that the electrochemical oxidation of TOC correlates well with the hydrogen peroxide
generated at the cathode, wherein the saturated solubility of oxygen
in wastewater has been almost achieved at the oxygen ow rate of
100 mL/min. But the color removal efciency remained almost constant at a current density of 68 A/m 2 even when the oxygen sparging
rate increased from 0.3 to 0.4 L/min [55]. The results indicate that
color removal began to be controlled by the kinetics of the production
of hydrogen peroxides when the oxygen sparging rate exceeded
0.3 L/min [55]. Similar results are reported by Wang et al. [66] after
the oxygen sparging rate was over 150 L/min for COD removal.
5.3. Temperature
Although temperature has a positive effect on the treatment efciency in Fenton and related processes, the increase in organic compound removal due to temperature is relatively small compared to
the other factors. Too low and too high temperatures negatively impact the process efciency. An optimal temperature of 30 C has
been reported by Guedes et al. [81] for the degradation of cork
cooking wastewater. Temperature between 20 and 30 C can be considered as an optimum range because of relatively higher treatment
efciency in this temperature range [82]. Zhang et al. [83] reported
that COD removal efciency of Fenton process increased slightly as
the temperature increased from 15 to 36 C. Wang [4] reported that
the rate of dye degradation was lower at low temperature and the extent of degradation was higher at 2030 C before 100 min. On the
other hand Wu et al. [84] found an optimal temperature of 45 C for
the degradation of humic acid. Also up to 100% degradation of
diisopropanolamine at 60 C has been reported by Khamaruddin et
al. [85]. Temperature has two effects on the accumulated H2O2 concentration during the electrolysis. First one is the decrease of O2 solubility in water with increase of the temperature and second one is the
low stability of H2O2 at high temperatures [86]. Dye degradation rate
has been decreased when the temperature was greater than 30 C

Table 4
Optimum temperatures of E-Fenton process in various studies.
No Pollutant

Electrodes

Experimental conditions

Pt-PAN-based activated
carbon ber
Graphite-Pt/Ti

Current density = 3.2 mA/cm2; oxygen sparging rate = 150 cm3/min;

20
pH = 3; [Fe2+] = 2 mM.
pH = 3; oxygen sparging rate = 0.3 L/min; applied current density = 68 A/ 45
m2; [Fe2+] = 15 mM.
40
Electrode potential = 6 V, O2 = 100 mL/min, pH = 0.2, [Fe2+] = 15 mg/L.

2
3

Dyeing
wastewater
Dyeing
wastewater
Nitrotoluenes

PtPt

Temperature
(C)

Removal
efciency (%)

Reference

75

[66]

70.6

[55]

~ 100

[80]

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

due to decomposition of H2O2 at a higher temperature [4]. The negative effect of temperature on the pollutant removal percentage can
also be explained by the lower concentration of dissolved oxygen
and the self-decomposition of hydrogen peroxide at higher temperatures [66]. Namely, the concentration of hydrogen peroxide decreased
as the temperature increased because increasing temperatures can decrease oxygen solubility in the wastewater [66]. In addition, the rate
of self decomposition of hydrogen peroxide to water and oxygen increased with the temperature [55,66]. But Hameed and Lee [87]
reported that degradation of malachite green increased from 85.59 to
98.14% as a consequence of increasing the temperature from 30 to
50 C within the rst 10 min of Fenton process. Also Homem et al.
[88] reported that the reaction rate of amoxicillin degradation was increased by increasing the temperature (in between 22 and 57 C).
Zazo et al. [89] reported that increasing the temperature clearly improves both the oxidation rate and the degree of mineralization of phenol by Fenton oxidation allowing working with reduced amounts of
H2O2 and Fe2+. This may be due to the fact that the increase in reaction
rate between hydrogen peroxide and any form of ferrous/ferric iron
(chelated or not) at higher temperature increases the rate of generation
of oxidizing species such as OH radical or high-valence iron species
[90]. The optimum temperatures and corresponding removal efciencies reported by various researchers are given in Table 4.
5.4. Applied current density
The applied current is the driving force for the reduction of oxygen
leading to the generation of hydrogen peroxide at the cathode. Higher
applied current increases the quantum of hydrogen peroxide produced, thus increasing the number of hydroxyl radicals in the electrolyte medium, which are highly reactive and responsible for the
degradation [91]. Higher applied current density means higher applied voltage on the electrochemical system [66]. Also higher
electro-regeneration of ferrous ion from ferric ion (Eq. (14)) with increasing current increased the efciency of Fenton chain reactions [32].
3

Fe

e Fe

14

The efciency of E-Fenton will be less at higher current density efciency. This is due to the competitive electrode reactions in the electrolytic cell. The discharge of oxygen at anode (Eq. (15)) and the
evolution of hydrogen at cathode (Eq. (16)) occur at a higher current.
These reactions inhibit main reactions such as reactions (6) and (14)
[32], which lead to decrease in efciency of E-Fenton.

2H2 O4H O2 4e

15

2H 2e H2

16

The degradation rate of organic pollutants is constant after

300 mA. This is due to the formation of H2O as in Eq. (17) [42].

4H O2 4e 2H2 O

17

Some studies indicated that the current density in the E-Fenton

process should be no larger than 10 A/m 2, while others indicated
that the upper limit value should be 6.4 A/m 2 [92]. The optimum current or current densities and corresponding removal efciencies of EFenton process are given in Table 5.
5.5. Fe 2+ concentration
Suitable ferrous ion concentration is an important prerequisite in
the E-Fenton process [30]. Generally the efciency of E-Fenton process increases with Fe 2+ concentration because the concentration of
hydroxyl radical, which is the main oxidizing agent in the E-Fenton
process increases with the increase in Fe 2+ concentration (Eq. (1)).
Also the oxidizing power of hydrogen peroxide was not enough to destroy large molecules, such as dyestuffs in real dyeing wastewater in
the absence of ferrous ions [66]. The color removal efciency was
markedly increased from 9% to 46% by externally adding a small
amount of ferrous ions (5 mM) [55]. Wang et al. [66] reported that
the presence of Fe 2+ signicantly improved the COD removal percentage. The COD removal percentage markedly increased from
19.8% to 43.1% by externally adding a Fe 2+ concentration of
0.33 mM [66]. Zhou et al. [30] reported that the removal of methyl
red increased from 45% to 75% in 10 min in the presence of Fe 2+.
Wang et al. [51] observed an increase in the rate of TOC decay by EFenton process, when initial Fe 2+ concentrations were increased
from 0 to 1 mM. However, ferrous ions in the electrolyte solution,
when present in excess, could consume the hydroxyl radicals and affect the extent of degradation [91]. The plausible interpretation is
given by a competitive reaction between hydroxyl radicals and ferrous ions, which could diminish the concentration of hydroxyl radicals as in Eq. (4) [93,94]. The effect of Fe 2+ concentration on the
kinetic rate constants, for 2,6-dimethylaniline degradation was studied by Ting et al. [77]. The kinetic rate constant increased with increasing Fe 2+ concentration from 1.0 to 1.5 mM and does not
increase signicantly as the dosage of ferrous ions increased from
1.5 to 2.0 mM [77]. The optimum Fe 2+ concentrations and
corresponding E-Fenton process removal efciencies are given in
Table 6.

Table 5
Optimum current/current densities of E-Fenton process in various studies.
No Pollutant

Electrodes

Experimental conditions

Applied current or Removal

Reference
current density
efciency (%)

1
2
3

o-Chlorophenol
4-Nitrophenol
Dyeing
wastewater
Acid Red 14
Dyeing
wastewater
Picloram

Stainless steel Pt gauze

Stainless steel Ti/RuO2/IrO2
Pt-PAN based activated carbon
ber
RuO2/Ti ACF
Graphite Pt/Ti

[Pollutant] = 80 mg/L, [Fe2+] = 0.5 mg/L, electrolysis time = 60 min

[Pollutant] = 200 mg/L, [H2O2] = 9.12 mmol/L, Fe(II)/H2O2 = 0.050
Oxygen sparging rate = 150 cm3/min; pH = 3; [Fe2+] = 2 mM;
temperature = 20 C
[Pollutant] = 200 mg/L, [Na2SO4] = 0.05 M, pH = 3, [Fe2+] = 1 mM
pH = 3; oxygen sparging rate = 0.3 L/min; [Fe2+] = 15 mM

600 mA
1A
3.2 mA/cm2

59.12
65.0
75.2

[91]
[32]
[66]

0.50 A
68 A/m2

73.3
70

[51]
[55]

Carbon felt Pt

2,4,6Trinitrotoluene
2,6Dimethylaniline

Pt carbon felt

[Pollutant] = 0.125 mM; [Fe3+] = 0.1 mM; [Na2SO4] = 50 mM;

pH = 3
[TNT]0 = 0.2 mM, [Fe2+] = 0.2 mM

4
5
6
7
8

Ti-RuO2/IrO2 stainless steel

[Pollutant] = 1 mM; [Fe

2+

] = 1 mM; [H2O2] = 20 mM; pH = 2.0

300 mA
250 mA
10.6 A/m

100

[42]

99

[61]

91

[77]

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

Table 6
Optimum Fe2+ concentrations of E-Fenton process in various studies.
No

Pollutant

Electrodes

Experimental conditions

Fe2+ concentration

o-Chlorophenol

Stainless steel Pt gauze

2 mg/L

80.4

[91]

Dyeing wastewater

2 mM

75

[66]

Methyl red

Pt-PAN-based activated
carbon ber
Graphite PTFE Pt

0.25 mM

75

[30]

4
5
6

Sunset yellow FCF

Acid Red 14
Dyeing wastewater

RVC Pt
RuO2/Ti ACF
Graphite Pt/Ti

[Pollutant] = 80 mg/L, applied current = 60 mA,

electrolysis time = 60 min
Current density = 3.2 mA/cm2; oxygen sparging
rate = 150 cm3/min; pH = 3; temperature = 20 C.
pH = 3.0, [Na2SO4] = 0.1 M, [pollutant] = 100 mg/L,
oxygen ow rate = 0.4 L/min
[pollutant] = 0.2 mM, [Na2SO4] = 0.05 M, pH = 3
[pollutant] = 200 mg/L, [Na2SO4] = 0.05 M, pH = 3
pH = 3; oxygen sparging rate = 0.3 L/min; applied
current density = 68 A/m2

0.1 mM
1 mM
15 mM

100
68.2
70

[25]
[51]
[55]

Removal efciency (%)

Reference

5.6. Hydrogen peroxide concentration and feeding mode

5.7. Distance between the electrodes

The initial concentration of H2O2 plays an important role in the EFenton process [77]. Removal of pollutants increases with increase in
H2O2 concentration. The increase in the removal efciency was due to
the increase in hydroxyl radical concentration as a result of the addition of H2O2 (Eq. (1)) [77]. Zhang et al. [32] reported that efciency of
hydrogen peroxide for removing organic materials in the leachate decreased with the increase of Fenton's reagent dosage. At a high dosage
of H2O2, the decrease in removal efciency was due to the hydroxyl
radical scavenging effect of H2O2 (Eqs. (18) and (19)) and the recombination of the hydroxyl radical (Eq. (20)) [95].

In the E-Fenton process, distance between electrodes is another

important factor that affects the removal of pollutants. The decrease
of the distance between the electrodes leads to a decrease of the
ohmic drop through the electrolyte and then an equivalent decrease
of the cell voltage and energy consumption [97]. Zhang et al. [12]
reported that the COD removal efciency from landll leachate
remained the same for electrode distance between 1.3 and 2.1 cm.
The removal efciency of E-Fenton system was less for the shorter
or larger distance. This is because electro-regenerated Fe 2+ could be
easily oxidized to ferric ion at the anode, when the electrodes were
placed too short [12]. Longer distance causes the limiting mass transfer of ferric ion to the cathode surface that governs ferrous ion regeneration [12,98]. Atmaca [20] reported that the changes in the distance
between the electrodes have an insignicant effect on treatment efciency. Use of long electrode distance in E-Fenton reactor causes a signicant increase in energy consumption [20].

HO H2 O2 HO2 H2 O

HO2 HO H2 O O2

2HO H2 O2

18
19
20

Improvement of E-Fenton process efciency by feeding Fenton's

reagent in multiple steps or continuous mode was reported by
Zhang et al. [12]. Anotai et al. [96] compared the one-step and the
two-step addition with H2O2 for aniline degradation. The results indicated that the aniline oxidation for the system of one-step addition
with H2O2 was similar to that of the two-step. In both cases aniline
oxidation was about 95% after reacting for 60 min. The removal efciency of COD in the one-step addition with H2O2 was similar to
that in the two-step. On the other hand, the TOC removal efciency
and remaining Fe 2+ concentrations were not affected by the H2O2
feeding mode [96].
Effect of H2O2 addition in a single step and in continuous mode on
the degradation of 4-nitrophenol was reported by Zhang et al. [32]. It
has been reported that decreasing feeding time increased the initial
COD removal rate. The optimum COD removal has been reached
when H2O2 was applied in a single step. But for continuous mode,
the concentration of H2O2 increased with decrease in feeding time
during the initial period. This will cause the production of more hydroxyl radicals as in Eq. (1) and increases the efciency of E-Fenton
process. The nal COD removal efciency increased with the decreasing feeding time and reached highest when feeding time was 60 min.
But due to side reactions, the efciency of E-Fenton process decreases
with further decrease of feeding time [32]. The concentration of hydrogen peroxide during the initial period would be higher when hydrogen peroxide was added in a single step or fed more quickly in a
continuous mode, the produced hydroxyl radicals would be scavenged by hydrogen peroxide. This reaction leads to the production
of hydroperoxyl radical (Eq. (18)), a species with much weaker oxidizing power compared to hydroxyl radical [32].

5.8. Nature of the supporting electrolyte

Electrolyte improves the solution conductivity, and accelerates the
electron transfer, thus beneting the E-Fenton reaction. Therefore,
supporting electrolyte is necessary, especially in the solution without
enough conductivity [21]. In E-Fenton process, sodium sulfate is commonly used as the supporting electrolyte. Zhou et al. [30] reported
that higher Na2SO4 concentration led to higher current density,
which resulted in faster and larger production of hydrogen peroxide
and increases the efciency of E-Fenton system. But Diagne et al.
[99] observed a faster methyl parathion degradation rate in the presence of NO3 than that of SO42. Daneshvar et al. [78] also reported
that the change in Na2SO4 concentration from 0.05 to 0.1 M did not
have any effect on H2O2 accumulation. Ghoneim et al. [25] reported
that optimal Na2SO4 concentration for sunset yellow FCF is 0.05 M.
But Pt-graphite PTFE electrolytic system has an optimal Na2SO4 concentration of 0.1 M for the degradation of methyl red [30]. Also the
authors noticed a signicant drop in efciency of the system at
0.2 M Na2SO4 concentration. This may be due to the consumption of
the generated hydroxyl radical by high SO42 concentration as in
Eq. (21) [30].

HO SO4 HO SO4

21

Efciency of 0.05 M Na2SO4, 0.05 M NaCl and 0.05 M KCl as

supporting electrolyte was compared by Ghoneim et al. [25] and
reported that aqueous solutions with SO42 have the highest rate of
decolorization of sun set yellow compared to Cl electrolytes of the
same concentration. But approximately 100% removal of the azodye was achieved for all electrolytes. The time taken for the removal
of dye is 120, 180 and 180 min respectively for 0.05 M Na2SO4,

10

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

In recent years there is a great interest in the development of practical electrochemical methods for the destruction of toxic and biorefractory organic pollutants for wastewater treatment [91]. The EFenton process is widely used to treat non-biodegradable or refractory
organic compounds with moderate energy costs [100]. The applications of E-Fenton process is explained below.

rhodamine B in aqueous solution was evaluated by Ai et al. [36].

The study reported that degradation of rhodamine B reached 80.2%
and 89.3% in 120 min at neutral pH and pH 3, respectively [36].
Zhou et al. [30] reported that the degradation of methyl red was accomplished at two different stages, and the consumption of ferrous
ion and formation of hard-to-treat intermediates led to the slower
degradation in the second stage. Under the optimal conditions, the
initial methyl red concentration of 100 mg/L could be degraded 80%
in 20 min [30]. Ghoneim et al. [25] reported that for a contact time
of 120 min, complete color removal and signicant mineralization
(approximately 97%) of sunset yellow FCF have been achieved. 70%
TOC removal for 500 mL of a 200 mg/L Acid Red 14 after 360 min of
electrolysis was reported by Wang et al. [51]. El-Desoky et al. [41] applied optimized E-Fenton system successfully for complete degradation and signicant mineralization (approximately 8590%) of
Levax blue and red reactive azo-dyes in real industrial wastewater
samples of textile dyeing house. The removal efciency of color
from real dyeing wastewater in the cathodic chamber reached 70.6%
under specied operation conditions in 150 min [55]. This study
reported that the best oxygen contact mode for removing the color
was the three-phase contact mode, resulting in the optimal transference of the dissolved oxygen to the electrode surface [55]. COD removal efciency from real dyeing wastewater by using Fe 2+ in
combination with electrogenerated hydrogen peroxide at the polyacrylonitrile based activated carbon ber cloth cathode was studied by
Wang et al. [66]. In this study, the highest COD removal efciency
(75.2%) was achieved at an applied current density of 3.2 mA/cm 2.

6.1. Dyes

6.2. Pesticides and herbicides

The dyes used in the textile dyeing and printing industries not
only can impart color to water sources but also can cause environmental damage to living organisms by stopping the reoxygenation capacity of water and also blocking sunlight, thereby disturbing the
natural growth activity of aquatic life [4]. Some of the dyes are also
toxic and carcinogenic in nature [101]. Presence of very small
amounts of dyes in water (less than 1 ppm for some dyes) is highly
visible and undesirable [102]. Synthetic dyes are used extensively
by several industries including textile dyeing (60%), paper (10%)
and plastic matter (10%) [35]. It is estimated that 1015% of the dye
is lost in the efuent during dyeing processes [103]. Presently, more
than 10,000 types of different commercial dyes and pigments are
available [101], and more than 7 10 5 t per year are produced worldwide [102].
E-Fenton process has been identied as a powerful tool for removal of dye from wastewater very effectively. Guivarch et al. [35] studied
the degradation of the three azo dyes azobenzene, methyl orange and
p-methyl red by the E-Fenton and concluded that this process is efcient for azo dye degradation, achieving an efcient removal (over
80%) of COD. The degradation mechanism begins with the azo bond
cleavage and is followed by the hydroxylation of the aromatic ring
[35]. A synthetic dye wastewater sample composed of yellow
drimaren, Congo red and methylene blue and having an initial COD
of 3782 mg O2 L 1 was successfully mineralized using E-Fenton process by Lahkimi et al. [38] with the COD abatement ratio of 89% after
10,000 C of electrical charge passed. Decolorization of acid yellow 36
in acidic aqueous medium was studied by Cruz-Gonzlez et al. [54]
and reported 97.8% of acid yellow 36 removal at optimum conditions
such as Fe 2+ of 0.24 mmol/L, current density of 23 mA/cm 2 and electrolysis time of 48 min. Complete mineralization of indigo carmine of
220 mg/L concentration is feasible when E-Fenton is carried out with
a BDD anode [43]. The degradation of different dyes by E-Fenton oxidation was carried out successfully in a continuous reactor by Rosales
et al. [27]. The reactor was very efcient for dye removal and high discoloration percentage depends on the residence time. The operational
problems of the reactor were also very less [27]. Degradation of

Due to the extensive utilization in agricultural activities, pesticides

and herbicides are widely detected in many surface water, groundwater and wastewater efuents and are among the most frequently
found organic pollutants in natural waters [104,105]. Many of these
pesticides are utilized in amounts over 50,000 kg/year [106]. Relatively high pesticide and herbicide contamination levels are found in
groundwater and surface water: 0.10.3 g/L in US groundwater
and 0.030.5 g/L in European groundwater [107,108]. Similar results
have been observed in India also. The residue levels of persistent
chlorinated pesticides such as HCH (hexachlorocyclo-hexane) isomers and DDT (dichlorodiphenyltrichloroethane) compound samples
from the river Kaveri, Tamil Nadu, South India have been reported by
Rajendran and Subramanian [109]. River Ganges in Kanpur contains
high concentrations of -HCH (0.259 g/l) and malathion (2.618 g/l)
[110]. -HCH, malathion and dieldrin concentrations of 0.900,
29.835 and 16.227 g/l, respectively were detected in ground water
samples [110]. Sanghi et al. [111] reported that the endosulfan concentrations in the human milk were the highest and exceeded the
S-HCH, chlorpyrifos, and malathion concentrations by 3.5-, 1.5-,
and 8.4-fold, respectively. Similarly Jani et al. [112] reported an average concentration of alpha-HCH, gamma HCH, beta HCH, p,p-DDE
(Note: DDE-Dichlorodiphenyldichloroethylene), and p,p-DDT as
17.51, 1.62, 205.48, 244.71, and 53.43 g/kg, respectively in human
milk. Also dairy milk and buffalo milk from Jaipur city were contaminated
with DDT and its metabolites (DDE and p,p-dichlorodiphenyldichloroethane DDD), isomers of hexachlorocyclohexane (HCH; alpha,
beta, and gamma), heptachlor and its epoxide, and aldrin [113].
This situation is considered as a pervasive problem because these
compounds usually have direct adverse effects on the living organisms [114]. The E-Fenton process has been proved to be powerful
enough to degrade hazardous pesticides and herbicides. Yatmaz and
Uzman [52] reported that E-Fenton reaction by using both Fe electrodes with supply of H2O2 is the most efcient method for the degradation of monocrotophos in acidic medium. Monocrotophos was
rapidly degraded within 5 min and the energy consumption of complete degradation was 0.834 kWh/kg [52]. Boye et al. [108] reported

0.05 M NaCl and 0.05 M KCl solution [25]. Pimentel et al. [60] compared the efciency of iron, cobalt, manganese, and copper salts to
provide the metal cations as catalyst of Fenton reaction to produce
hydroxyl radicals and concluded that ferrous ions were the most effective catalysts with optimum concentration of 0.1 mM. 0.1 mM of
soluble FeSO4 supplied the optimum catalytic condition, allowing
100% removal of TOC of aqueous phenol solutions [60]. But during
E-Fenton process, degradation of some other compounds using iron
as catalyst may lead to formation of complexes and changing iron
concentration in the media [60]. zcan et al. [86] reported that the
production of H2O2 is lower in the case of NaCl than that of NaNO3
and NaSO4. Signicantly a faster decrease of Orange II in the NaClO4
media than in Na2SO4 or NaCl media has been noticed by Daneshvar
et al. [78]. Concentration of electrolyte also affects the efciency of
E-Fenton process. But Daneshvar et al. [78] reported that the concentration of supporting electrolyte does not have any effect in orange II
degradation, when the NaClO4 concentration has been increased from
0.05 to 0.1 M.
6. Applications

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

80% mineralization of herbicide 4-chlorophenoxyacetic acid. zcan et

al. [44] compared the propham removal efciency of BDD, CS and Pt
electrodes as anode and/or cathode at four different congurations
in the E-Fenton process. The authors reported that the highest TOC
removal efciency and the lowest mineralization current efciency
values were observed at 500 mA in the presence of 0.2 mM Fe 3+.
The best mineralization current efciency value of 81% was obtained
at 100 mA in the presence of 0.2 mM Fe 3+ for 30 min treatment
[44]. Edelahi et al. [46] reported 93% COD removal within 10 min by
degrading diuron using E-Fenton process. This process is also efcient
for imazapyr degradation and the COD removal was found to be
higher than 95% [115]. The degradation of herbicide chlortoluron in
aqueous medium by E-Fenton process using a carbon felt cathode
and a platinum anode was studied by Abdessalem et al. [69]. Even
the degradation of 0.05 mM chlortoluron happened within 4 min,
98% of TOC removal was recorded only after 8 h [69]. Similar results
were also reported by zcan et al. [42] for the removal of picloram.
Kaichouh et al. [116] reported that the imazaquin is degraded more
quickly than the imazapyr. But 97% mineralization of each herbicide
was reached after 3.5 h of treatment under optimal operating conditions of I = 0.2 A and [Fe 2+]0 = 0.1 mM [116]. E-Fenton with a Pt
anode, stainless steel sheet cathode and 1 mmol/L Fe 2+ as catalyst
yields the quickest and complete depollution of amitrole [49]. A comparative study of a mixture of three pesticides (chlortoluron,
carbofuran and bentazon) has been investigated by Abdessalem et
al. [117]. It was reported that based on cost, E-Fenton process is
much more interesting than photo-Fenton process [117].
6.3. Phenolic compounds
Among the various wastes, phenolic compounds constitute a family of pollutants particularly toxic to the aquatic fauna and ora. These
compounds are released in the surface water by a considerable number of industries, mainly, by pharmaceutical plants, oil reneries, coke
plants, pulp, and food-processing industries and several other chemical plants [118,119]. Nitrophenols are anthropogenic, toxic, inhibitory and biorefractory organic compounds used extensively in chemical
industries for the manufacture of pesticides, pharmaceuticals and
synthetic dyes [120]. Chlorophenols have been detected during the
manufacture of pesticides, bleaching of industrial wastewater, and
chlorination of drinking water [121]. Phenolic compounds are very
toxic to human health and aquatic life. Consequently, removal of
them from wastewater is an environmental concern. These compounds are removed very effectively by E-Fenton process. Pimentel
et al. [60] reported that total mineralization of phenol was obtained
at optimum experimental conditions. The degradation of various
chlorophenols by E-Fenton method was carried out by Song-hu and
Xiao-hua [122]. The degradation sequence of various chlorophenols
were in the following order: 2,4-dichlorophenol>2,4,6-trichlorophenol>pentachlorophenol>4-chlorophenol. This order is different from
other AOP studies. The degradation pathways of chlorophenols were proposed as ortho- and para-reaction by hydroxyl attack and direct
dechlorination by cathode reduction [122]. Further oxidation was
preceded by hydroxyl radical. Most of the residual chlorine was left in
the ring opening low molecule compounds [122]. 280.7 C electrical
charge was consumed during 450 min of electrolysis to attain
degradation of 4-chloro-2-methylphenol and 14.9% TOC removal and
89.3% dechlorination have been reported by Irmak et al. [62]. The kinetics
of the oxidative degradation of several chlorophenols, such as monochlorophenols (2-chlorophenol and 4-chlorophenol), dichlorophenols
(2,4-dichlorophenol and 2,6-dichlorophenol), trichlorophenols (2,3,5trichlorophenol and 2,4,5-trichlorophenol), 2,3,5,6-tetrachlorophenol,
and pentachlorophenol by the E-Fenton process have been investigated
using a carbon felt cathode [123]. It was demonstrated that the number and the position of the chlorine atoms in the aromatic ring significantly inuence the oxidation. The degradation followed a pseudo-

11

rst-order kinetics and the apparent rate constant follows the

sequence 4-chlorophenol > 2-chlorophenol > 2,4-dichlorophenol > and
2,6-dichlorophenol >2,3,5-trichlorophenol >2,4,5-trichlorophenol >2,3,
5,6-tetrachlorophenol >pentachlorophenol. It was also observed that
the mineralization rate of chlorophenols decreased with increasing the
number of chlorine atoms in the aromatic ring, conrming that the
more chlorinated phenols are, the more difcult to mineralize [123]. EFenton process is highly efcient for the degradation of o-chlorophenol
[91]. Sankara Narayanan et al. [91] concluded that the non-availability
of sufcient concentrations of ferrous ions with electrolysis time limits
the efciency of the process. Under optimized conditions it is possible
to achieve more than 70% degradation and addition of goethite as a catalyst did not show any signicant increase in the degradation of ochlorophenol. Irmak et al. [62] reported that in E-Fenton application,
degradation of the refractory aromatic ring was quite straightforward
but decomposition of all aliphatic products into carbon dioxide and
water, i.e. complete mineralization is time and energy consuming. On
the other hand, release of chlorine atoms from organic structure into
the aqueous solution as chloride ions takes place almost simultaneously
with the breaking-up of the aromatic ring. In other words, toxicity related to the organochlorine structures is diminished in the early stages of
the E-Fenton treatment. Therefore, one can advise to continue to treat
the aqueous system by using cheaper conventional techniques following
the breakdown of aromatic structures and in situ release of most of the
chlorine as chloride ions [62]. Degradation of 4-nitrophenol was carried
out in batch recirculation mode by Zhang et al. [32]. It was reported that
even under successful COD removal, E-Fenton process induces a synergetic effect on COD removal. Treatment of high concentration of 4nitrophenol in the undivided cell removed more than 98% of 4nitrophenol and about 13% of TOC [124]. Negligible quantity of nitrate
and nitrite ions detected indicates that there is no direct release of
NO2 and NO groups from 4-nitrophenol and its degradation intermediates [124].
6.4. Leachate
Landlls are ubiquitous in modern society, and the proper management of their potential environmental impact is of the highest priority [125]. Landll leachate is dened as those aqueous streams
generated as a consequence of rainwater percolation through wastes,
biochemical processes in the wastes' cells and the inherent water
content of the wastes themselves [126]. Leachate may contain large
amounts of organic matter, of which humic-type constituents are an
important group, as well as ammonia-nitrogen, heavy metals and
chlorinated organic and inorganic salts. The removal of organic
material based on COD, biological oxygen demand and ammonium
from leachate is the usual prerequisite before discharging the leachate into natural waters [126]. Only a few works on leachate treatment
by E-Fenton are reported. Altin [127] reported more than 90% color
removal efciency by E-Fenton process. 87% PO4P and 26% NH4N
removal from landll leachate under optimum conditions was
reported by Atmaca [20]. Also this study reported 72% COD and 90%
color removal. Mohajeri et al. [128] achieved 94% COD removal and
95.8%color removal from landll leachate. Treatment of high strength
landll leachate by E-Fenton process was studied by Zhang et al. [12].
Ti/RuO2 and IrO2 type electrodes were used as anode. They reported
that the process was very fast in the rst 30 min and then slowed
down till it was complete in 75 min. Atmaca [20] studied the characteristics of sludge produced from landll leachate treatment by EFenton process. The author reported that the sedimentation characteristics of the waste are fairly good [20].
6.5. Drugs
A large number of pharmaceutical drugs have been recently
detected in water sources. For example chlorophene, a widespread

12

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

Table 7
Various pollutants removed by E-Fenton process.
No

Pollutant/purpose

Research highlights

Reference

Aniline

[131]

Petrochemical wastewater

Biological coking wastewater

Industrial wastewater containing morpholine and

diethylethanolamine, as well as sodium salts of naphthalene
sulfonic acid and of ethylenediamine tetraacetic acid
Dinitrotoluenes and 2,4,6-trinitrotoluene

After 6 h of electrolysis at 100 mA 68% of TOC removal achieved.

A fast aniline mineralization
Ammonium ions (7580% of initial nitrogen) were generated
More than 50% of COD removal efciency
E-Fenton method is effective in treating this wastewater
Optimum parameters were: pH 4, 1.8 h reaction time, 0.6 mM of Fe2+
and 3.7 mA/cm2 of current density
55% TOC removal
Up to 64.5% of running costs can be cut when E-Fenton used
100% current efciency in solutions polluted by organic substances

2,4,6-Trinitrotoluene

2,6-Dimethylaniline

Nonylphenol polyethoxylate

9
10

COD reduction of rayon industry wastewater

COD reduction of leather tanning industry wastewaters

11

Benzene sulfonic acid

Nearly complete decomposition of nitrotoluenes under the optimal conditions

of electrode potential = 6 V, T = 303 K, O2 = 100 mL/min and iron(II) = 15 mg/L.
After 5 min electrolysis, 70 and 99% of the initial TNT content were degraded
for 60 and 250 mA current intensity values
Minimum 22% of aromatic rings were cleaved at TNT disappearance time
35% of initial material reached the last step before mineralization,
60% TOC removal efciency
Oxalic acid was the major intermediate detected from 2,6-dimethylaniline degradation
Around 50% COD reduction
95% nonylphenol polyethoxylate removal was achieved in 5 min for aqueous
solution and 10 min for wastewater treatment
88% COD was reduced in 50 min
COD was reduced by 6070% within 10 min
Over 70% COD removal for pH 3.
At a neutral pH, greater than 60% COD removal
Sulde concentration in the tannery industry wastewater was almost 100%
removed in 10 min
64% of TOC removal

broad-spectrum antimicrobial pharmaceutical has been detected at

concentrations up to 50 mg/L in activated sludge sewage systems
and up to 10 mg/L in sewage treatment plant efuents and rivers
[39]. This pollution is originated from emission from production
sites, direct disposal of over plus drugs in households, excretion
after drug administration to humans and animals and treatments
throughout the water in sh and other animal farms [129]. Some of
the drugs are carcinogenic and mutagenic [130]. To avoid the dangerous health effects of such pollutants, potent oxidation methods are
needed to remove drugs and their metabolites from wastewaters
[56]. E-Fenton is one of such powerful tool for removing drugs from
wastewater. The catalytic behavior of the Fe 3+/Fe 2+ system in the
E-Fenton degradation of the antimicrobial drug chlorophene mainly
depends on the cathode [39]. The authors reported that that EFenton is a viable environmentally friendly technology for the remediation of wastewaters containing chlorophene. The removal efciency of chlorophene by Pt/O2 diffusion, BDD/O2 diffusion, BDD/carbon
felt and Pt/carbon felt E-Fenton systems was compared. Maximum removal of chlorophene is in the order of Pt/carbon felt system followed
by BDD/carbon felt, BDD/O2 diffusion and Pt/O2 diffusion systems
[39]. Isarain-Chvez et al. [47] used two-electrode cells with a Pt or
boron-doped diamond anode and an air-diffusion cathode for H2O2
electrogeneration, and four-electrode combined cells containing the
above pair of electrodes coupled in parallel to a Pt anode and a
carbon-felt cathode, to degrade the pharmaceutical blocker atenolol by E-Fenton. Compared with the single cells, the corresponding
novel four-electrode combined systems enhance strongly the mineralization rate of atenolol in E-Fenton. Because of the fast Fe 2+ regeneration at the carbon-felt cathode favoring: (i) the production of
more amounts of OH from Fenton's reaction that destroy more rapidly aromatic pollutants and (ii) the formation of Fe(II) complexes
with nal carboxylic acids such as oxalic and oxamic, which are
more quickly oxidized with OH [47]. Solutions of about 0.25 mM
of the -blocker metoprolol tartrate (100 mg/L total organic carbon)
with 0.5 mM Fe 2+ in the presence and absence of 0.1 mM Cu 2+ with
pH 3.0 have been degraded under single and combined E-Fenton

[132]
[79]

[133]

[80]
[61]

[77]
[134]

[59]
[29]

[135]

conditions [56]. The study reported that the combined cell was
much more potent than the single one by the larger OH generation
from the continuous Fe 2+ regeneration at the carbon felt cathode,
accelerating the oxidation of organics. Total mineralization was feasible using the combined cell in the presence of 0.1 mM Cu 2+, because of the parallel quick oxidation of Cu(II) carboxylate
complexes by OH [56].
6.6. Others
Many other pollutant degradation was carried out successfully by
E-Fenton process. The details are given in Table 7. From Table 7, it is
very clear that E-Fenton is a very powerful and environmentally
friendly tool for wastewater treatment.
7. Degradation pathway of organic pollutants
One of the main advantages of E-Fenton process is the complete
mineralization and degradation of organic compounds. High performance liquid chromatography (HPLC) analysis and Gas chromatographymass spectrometry (GCMS) of electrolyzed wastewater
revealed the formation of different oxidation products. The decay kinetics for initial pollutants can be monitored by reversed-phase
HPLC. The proposed reaction sequence for the degradation of dye
Acid Red 97 using carbon felt cathode and Pt anode [40] is shown
in Fig. 6. The oxidation of Acid Red 97 under the action of OH gives
1,2-naphthalenediol, 1,1-biphenyl-4-amino-4-ol, 2-naphthalenol diazonium and 2-naphthalenol by the reduction of azo bonds. These
products undergo further oxidation and release 2,3-dihydroxy-1,4naphthalenedion, phthalic anhydride, 1,2-benzenedicarboxylic acid,
phthaldehyde, 3-hydroxy-1,2-benzenedicarboxylic acid, 4-aminobenzoic acid and 2-formyl-benzoic acid. During this reaction most
of the nitrogen element went away from the dye structure as
NO3 and NH4+ ions or nitrogen. After that gradual cleavage of aromatic ring occurs, and this leads to the formation of CO2 as nal
product [40].

PV. Nidheesh, R. Gandhimathi / Desalination 299 (2012) 115

8. Conclusions
The application of E-Fenton on organic pollutant removal from
wastewater has received increased attention in the last decade. Different types of electrolytic reactors were used for E-Fenton study. Efciencies of various anode and cathode were evaluated and
compared. This process is very much dependent on pH, oxygen sparging rate, temperature of solution, applied current density, Fe 2+ concentration, hydrogen peroxide concentration and feeding mode,
distance between the electrodes and nature of the supporting electrolyte. Removal of various organic pollutants including dyes, drugs, herbicides and pesticides, leachate, phenolic compounds etc. by this
process was evaluated. Overall, E-Fenton process is a promising technology for applications in wastewater treatment.
Acknowledgments
The authors are thankful to K. Sharath, Ranjith Kumar and T.G.
Parameswaran for the great support.
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