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Separation and Purification Technology 61 (2008) 391397

An alternative type of photoelectro-Fenton process for

the treatment of landfill leachate
Ahmet Altin
Z. Karaelmas University, Department of Environmental Engineering, 67100 Zonguldak, Turkey
Received 12 July 2007; received in revised form 5 November 2007; accepted 4 December 2007

Abstract
An alternative type of photoelectro-Fenton (PEF) process has been proposed to remove COD, color and phosphate from the landfill leachates.
The process was improved by combining the different type of electro-Fenton (EF) process with UV irradiation. The efficiency of the process
and settling characteristics of waste sludge produced from the process were investigated by changing some operating parameters such as initial
pH, H2 O2 and current. In addition, the proposed process was compared with other treatment processes such as electro-coagulation (EC), electroFenton and UV/H2 O2 in terms of treatment efficiency. The high removal efficiencies were observed at the initial pH 3, initial H2 O2 concentration,
3000 mg L1 ; current, 2.5 A; and treatment time, 20 min. Removal of COD, color and phosphate under the reported conditions were 94%, 97%,
96%, respectively. The obtained results from the comparative experiments revealed that the proposed PEF process is more effective than the other
treatment processes for the landfill leachate.
2007 Elsevier B.V. All rights reserved.
Keywords: Landfill leachate; Fentons reagent; Photoelectro-Fenton; Wastewater treatment

1. Introduction
Advanced oxidation processes (AOPs) are frequently used
to oxidize complex organic constituents found in wastewaters,
which are difficult to be degraded biologically into simpler end
products [1]. In these processes, free hydroxyl radical (OH ) is
used as a strong oxidant to destroy the complex organic compounds. Fentons reagent (an aqueous mixture of Fe2+ and H2 O2
that produces OH ) stand out among the most promising AOPs
for the treatment due to its high oxidation power [2]. In this
process (called as Fenton oxidation), oxidation of the organics
occurs generally by means of the following chain reactions [3]:
Fe2+ + H2 O2 Fe3+ + OH + OH

(1)

Fe2+ + OH Fe3+ + OH

(2)

RH + OH H2 O + R

(3)

R + Fe3+ R+ + Fe2+

(4)

Tel.: +90 372 257 4010; fax: +90 372 257 4023.
E-mail address: aaltin@karaelmas.edu.tr.

1383-5866/$ see front matter 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.seppur.2007.12.004

Recently, there are several applications of electro-Fenton process. According to Zhang et al. [4], these can be generally
divided into four categories as applying of Fenton reagents externally to electrochemical reactor or its in situ generations. In the
first category, ferrous ion is externally applied, and hydrogen
peroxide is concurrently generated on the surface of a cathode
such as mercury pool [5], carbon felt [6], reticulated vitreous carbon [7], graphite [8], activated carbon fiber [9], stainless steel
plate [10] or carbon-PTFE [11]. In the second category, hydrogen peroxide is externally applied while a sacrificial iron anode
is used as ferrous ion source [12]. In the third category, hydrogen
peroxide is externally applied and ferrous ion is electrogenerated
via the reduction of ferric ion or ferric hydroxide sludge [13]. In
the fourth category, both ferrous ion and hydrogen peroxide are
electrogenerated at sacrificial anode and cathodes [14]. When all
these electro-Fenton applications are evaluated in terms of cost,
simplicity of operation and effectiveness, it can be said that each
one has advantages and disadvantages to each other.
The catalytic effect of Fe2+ in the electro-Fenton process can
be enhanced by solution irradiation with UV light. Hence, it
is called photoelectro-Fenton (PEF) process that can produce a
large regeneration rate of Fe2+ [15].
(FeOH)2+ + hv Fe2+ + OH

(5)

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A. Altin / Separation and Purication Technology 61 (2008) 391397

This reaction increases oxidative capability of the process

due to the rise of the OH in the process [2]. In addition to all of
these mechanisms in the PEF process, two OH can be produced
from H2 O2 by photocatalytic effect of UV light (253 nm) [16].
H2 O2 + hv 2OH

(6)

Environmental application of the PEF process is fairly a

new topic and previous studies are quite limited. The most part
of these studies have comprised to treatability of some specific pollutants such as some kinds of herbicides [11,1719],
some kinds of dyes [20,21] and some kinds of organics [14,22].
In addition, Flox et al. [23] have recently used solar energy
as photon source, and reduced operating costs of the process,
substantially. However, in order to increase the environmental application of the process, researchers should focus on real
wastewaters.
In treatment of landfill leachates, biological treatment systems are frequently used. Even though, these systems ensure
a high BOD removal efficiency, they are usually insufficient
in degrading high molecular weight fractions and decoloring
[24]. Electro-Fenton method for treatment of landfill leachate
was used in the studies performed by Zang et al. [4] and Lin
and Chang [12]. In a study performed by Lin and Chang [12],
they found that electro-Fenton process (the second type application of the process) achieved 67.3% COD removal. In the
study conducted by Zang et al. [4], COD removal was 87.2%
in case of using a pair of Ti/RuO2 and IrO2 type electrodes.
The PEF process performed by using DSA anode and titanium
cathode was reported by Tauchert et al. [25] for the treatment
of landfill leachate, and they found that the decolorization and
the COD removal were extended to 90% and 60%, respectively.
The following paper presents an alternative type of the PEF
process to remove COD, color and phosphate from landfill
leachates. The proposed process was improved by combining the
second type of electro-Fenton [4,12] with UV irradiation. The
pH in the process, which gradually increases during the experiments, also provides electro-coagulation of Fe ions released
from electrodes at the end of the treatment. To increase efficiency of the process, operating parameters such as initial pH,
initial H2 O2 concentration, and applied current were optimized
and the effects of these parameters on the settling properties
of waste sludge produced in the PEF reactor were also investigated. After these studies, the proposed process was compared
with other processes such as electro-coagulation (EC), electroFenton (EF) and UV/H2 O2 in terms of treatment efficiency by
using similar experimental conditions.
2. Experimental
2.1. Equipments and chemicals
The PEF process was carried out in a quartz glass reactor having 1.0 L capacity equipped with a magnetic stirrer
(Fig. 1). Two pairs of the cast iron anode and cathode
electrodes (4.0 cm 5.0 cm 0.4 cm) were positioned approx-

Fig. 1. Experimental apparatus used in the experiments.

imately 1.0 cm apart from each other. The current input was
controlled by a DC power supply (Good Will-4303). Ultraviolet (UV) radiation was provided by two low-pressure UV lamps
(4 W, Philips-miniTUV-PL4). The UV intensity of the lamps at
253.7 nm was 1.4 W m2 .
In the EF, EC and UV/H2 O2 comparative experiments, some
components of the PEF reactor (DC power supply and electrodes for UV/H2 O2 experiments, UV lamps for EF and EC
experiments) were not used.
All chemicals, obtained from Merck, used in the experiments
were of analytical grade. The removal efficiency of organics
was monitored by COD determinations using a closed reflux
colorimetric method described in standard methods [26]. Color
changes were followed at 400 nm using a UVvisible spectrophotometer (Jenway-6105). The conductivity and pH were
measured with a WTW-330 EC meter and Orion-250A pH meter.
In the phosphate (PO4 P) measurements, colorimetric test kits
obtained from Merck were utilized. Sludge settling properties
were evaluated by using sludge volume index (SVI) described
in standard methods [26].
2.2. Experimental procedure
In the PEF experiments, leachate samples (0.5 L), collected
from landfill area, were transferred into the PEF reactor after
the filtration. The pH of the samples were then adjusted
to different pHs by drop wise addition of 0.1 molar H2 SO4
and NaOH and H2 O2 added at different concentrations. The
PEF experiments were started under a constant DC current.
The sample was mixed at 200 rpm with a magnetic stirrer
to provide homogeneity during the experiments. Time interval samples were taken from the reactor at 5th, 10th, 20th,
30th and 45th minutes of the treatment times. These samples
were centrifuged at 5000 rpm for 15 min prior to analytical controls.
In all comparative experiments, initial pH was used as 3. Initial H2 O2 concentration was selected as 2000 mg L1 for the
EF and UV/H2 O2 experiments. 3 A constant DC current were
applied to the electrodes for the EF and EC experiments. For
the experiments conducted in this study, since the color removal
generated by adding H2 O2 at the pervious stage of the experiments were low level (approximately 10%), all color removal
efficiencies were attributed to the reactions taken place in all
treatment process.

A. Altin / Separation and Purication Technology 61 (2008) 391397

393

Fig. 2. The effects of the initial pH on treatment efficiency: (a) COD removal; (b) color removal. (Test conditions: UV intensity, 1.4 W cm2 ; initial H2 O2 ,
2000 mg L1 ; current, 2.0 A.)

2.3. Characteristics of landll leachate

Landfill leachates generated from solid waste disposal area
of City of Sivas (Turkey) have been discharged to Kzlrmak
River at 500 m distance through a surface flow. Samples
used in the experiments were taken from a point just before
the discharge of the leachate to the river, and stored at
+4 C in the laboratory conditions. Their main characteristics
were: pH, 8.36 (0.08); conductivity, 10.51 mS cm1 (0.56);
COD, 2350 mg L1 (310); BOD5 , 915 mg L1 (110); color
as absorbance, 1.143 (0.105); NH4 N, 310 mg L1 (56);
PO4 P, 10.25 mg L1 (2.0).
3. Results and discussion
In a PEF process, many useful and interfere reactions, which
have effects on the treatment efficiency, can take place. It is
possible to keep the useful reactions dominant in the PEF reactor
by controlling the operating parameters such as initial pH, initial
H2 O2 concentration and applied current, etc. For an effective
Fenton oxidation, the pH of the solution should be adjusted to
low values. According to Zang et al. [3], optimum pH range
for wastewater treatment should be between 2 and 4. A high
concentration of the main oxidizing agent, OH , is expected to be
produced from Fentons reaction within this range, thus yielding
a rapid mineralization of pollutant [18]. However, in the PEF
treatment, OH can also be produced from the reaction (6) in the
pH interval 2.55 [18,27], and the reaction (8) [16]. Therefore,
this part of our work was focused on the effect of initial pH on the
treatment efficiency. In order to determine optimum initial pH
of the process, the samples were treated at different pHs within
the range of 28 using a constant current of 2 A and a H2 O2
concentration of 2000 mg L1 . The COD and the color removal
efficiencies obtained from the experiments were given in Fig. 2.
It is also observed in Fig. 2 that the COD removal efficiencies
decrease with rise of the initial pH (except that for pH 2). The
low efficiencies seen in the initial pH 2 can be explained that
the effectiveness removal of reaction (5) is limited by low concentration of Fe(OH)2+ in the solution. In addition, the highest
COD removal efficiency is found at the initial pH 2.5, whereas

the best color removal efficiency is observed at the initial pH

with in the range of 24.
For initial pH 8, the COD and the color removal efficiencies
of PEF process are relatively lower than the others, because this
pH value is out of the effective pH interval for Fentons reaction.
The color and the COD removal observed at this initial pH can be
the results of the EC and UV/H2 O2 processes taken place in the
reactor. Another important result can be concluded from Fig. 2
that considerable amount of the COD removal observed within
first 20 min of the treatment time. The rises in the efficiencies
after this time are unimportant. This phenomenon is related to
the final pH of the solution in the reactor, which is outside of the
effective pH interval of Fentons reactions (Fig. 3).
In addition, high color removal efficiencies were observed
within the first 5 min of the treatment time. After 20th minute,
the efficiencies slightly decreased. This result can be explained
by increment of the Fe ions (ferric and ferrous ions) in the
solutions, causing a color generation between green and brown.

Fig. 3. The initial and the final pH values observed in the initial pH experiments.
(Test conditions are same as that of the Fig. 2.)

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A. Altin / Separation and Purication Technology 61 (2008) 391397

Fig. 4. The effects of initial H2 O2 concentration on treatment efficiency: (a) COD removal; (b) color removal. (Test conditions: UV intensity, 1.4 W cm2 ; initial
pH, 3.0; current, 2.0 A.)

Another interesting result found from the experiments that the

decreases seen after the 20th minute of the treatment time for
the COD removal could be ascribed to the slow dissolution of
organics coagulated with Fe(OH)n flocs. Similar results were
also reported in a previous work by Lin and Chang [12].
It is well known that main source of OH radical is H2 O2 used
in the PEF process. Therefore, the effects of initial H2 O2 concentration on the treatment efficiency also were investigated in
this part of the study. In order to determine optimum initial H2 O2
concentration of the process, the samples were treated at different H2 O2 concentrations within the range of 15003000 mg L1
using a constant current (2 A) and an initial pH (3). The results
obtained from the experiments are given in Fig. 4.
As seen in Fig. 4, COD removal efficiencies raised significantly by increasing initial concentration of the H2 O2 , whereas
decolorization rates did not change for first 20 min of the
treatment time. For the treatment of landfill leachate via electroFenton process, Lin and Chang [12] reported that COD removal
efficiencies increased only 5% when H2 O2 concentration was
increased from 500 to 1250 mg L1 . It can be concluded from
these results that the production of the OH in the PEF process
is higher than that of the electro-Fenton process, since large
amount of H2 O2 can be catalyzed by means of reactions (5)
and (6). However, after the 20th minute, both color and COD

removal efficiencies decreased with similar decrements were

also observed in the initial pH experiments.
The amount of Fe2+ ions dissolved from the sacrificial iron
anodes increases (reaction (7)), when a DC current applied to
the electrochemical reactor increases.
Fe Fe2+ + 2e

(7)

This phenomenon is the most important to increase the efficiency of PEF process, since high level of Fe2+ in the rector
propagates to Fentons reaction. However, for high DC current
values, the removal efficiency of the process may not change
considerably or even may decrease due to some competitive or
inhibiting reactions. Therefore, the current density used in the
experiments should be chosen, precisely. In order to determine
optimum current value of the process, the samples were treated
at different current values within the range of 0.53 A using initial pH (3) and initial H2 O2 (3000 mg L1 ) and the results are
given in Fig. 5.
As seen in Fig. 5 an increment in the COD removal was progressively observed by rising the current up to 2 A. However, the
speed of this increase decreased significantly, when the current
was raised up to 2.5 A. This decay can be described by excessive
rise of Fe2+ concentration in the reactor. Recent studies show that

Fig. 5. The effects of applied current on treatment efficiency: (a) COD removal; (b) color removal. (Test conditions: UV intensity, 1.4 W.cm2 ; initial H2 O2 ,
3000 mg L1 ; initial pH, 3.0.)

A. Altin / Separation and Purication Technology 61 (2008) 391397

Fig. 6. Phosphate removal efficiencies of the PEF process vs. initial pH, current
and initial H2 O2 concentration. (Test conditions, for initial pH experiments; UV
intensity, 1.4 W cm2 ; initial H2 O2 concentration, 2000 mg L1 ; current, 2.0 A.
For current experiments: UV intensity, 1.4 W cm2 ; initial H2 O2 concentration,
3000 mg L1 ; initial pH, 3. For initial H2 O2 concentration experiments: UV
intensity, 1.4 W cm2 ; initial pH, 3; current, 2.0 A.)

an increment of the Fe2+ can inhibit the degrading rate of the

organics due to the competitive reaction (2) [17,28,29].
Another result derived from Fig. 5 showed that the required
time for the treatment reduced with the increment of the applied
DC current. Especially, the required time was drastically shortened, when the applied current were raised from 1.5 A to 2.0 A.
When a high level of phosphorus compounds is discharged
into an aquatic environment, eutrophication problem, described
as the dramatic growth of algs, can be seen [30]. Therefore, in
this part of our study, the effects of the initial pH, the initial H2 O2
concentration and the applied current on the phosphate removal
from landfill leachate via the PEF process were investigated and
the results obtained from the experiments are given in Fig. 6.
According to the results seen in Fig. 6, it is concluded that
the PEF process can be used for the phosphate removal from
the leachates, effectively. The best phosphate removal (98%)
were obtained at the end of treatment time (45th min) for the
initial pH 2.5, initial H2 O2 3000 mg L1 and the DC current
2.5 A. It was also observed that the increment of the applied
current is quietly affected to the treatment efficiency, whereas the
variations of the initial pH and H2 O2 concentration affected to
removal efficiencies, slightly. This phenomena can be described
by the increment of both pHs and dissolved Fe ions in the reactor
which cause to form Fe(OH)n flocks that remove the pollutant
by either complexation or by electrostatic [31].
One of the most important advantages of electrochemical
methods compared to the conventional biological and chemical
treatment methods is low sludge production and high settling
quality of produced sludge. In this study, to determine the set-

395

tling quality of PEFs waste sludge, sludge volume index (SVI)

parameters were measured at the end of each run and results are
given in Fig. 7.
Fig. 7 shows the effects of the initial pH, the initial concentration of H2 O2 and the applied current on SVI parameter. As seen
in Fig. 7, SVI values decreased with the increment of the applied
current, caused to rise the entrance speed of the Fe ions into reactor, while these values raised with the increment of the initial
H2 O2 concentration which caused the decomposing of Fe(OH)n
flocks structure. However, some increases were observed in the
SVI value, when the initial pH was higher and lower than 3. This
may be a result of the end pH and/or the final Fe2+ concentration in the solution. It is well known that Fe(OH)n flocks is large
and more stabile for slightly alkali conditions and the suitable
concentrations of Fe ions.
Based on the aforementioned results, it can be concluded that
the PEF process used in the study can be an alternative for the
treatment of the landfill leachate. Besides, in order to describe
the reactions in the PEF with more detail, and to determine superiorities of the PEF process over the other treatment processes
such as EC, EF and UV/H2 O2 taken place simultaneously in
the PEF reactor, more comparative experiments should be performed. Therefore, several experiments were conducted under
similar conditions used in the PEF process in order to compare
the COD and color removal efficiencies of the PEF process with
those of the EC, EF and UV/H2 O2 processes. Results were given
in Fig. 8.
As seen in Fig. 8a, the COD removal of the EF, UV/H2 O2
and PEF processes are high at the first 10 min of the treatment
time, and then the speed of the COD removal starts to decrease.
When the optimum treatment time is assumed as 20th minutes,
the COD removal efficiency of the PEF process is 28% and 10%

Fig. 7. Sludge volume index (SVI) values of treated solutions vs. initial pH,
current and initial H2 O2 concentration. (Test conditions are same as that of the
Fig. 6.)

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A. Altin / Separation and Purication Technology 61 (2008) 391397

Fig. 8. COD (a) removal and color (b) removal efficiencies of the different treatment processes. (Test conditions: for UV/H2 O2 process; UV intensity, 1.4 W cm2 ;
initial H2 O2 concentration, 2000 mg L1 ; initial pH, 3. For electro-coagulation process: current, 2.0 A; initial pH, 3. For electro-Fenton process: initial H2 O2
concentration, 2000 mg L1 ; initial pH, 3; current, 2.0 A. For PEF process: UV intensity, 1.4 W cm2 ; initial H2 O2 concentration, 2000 mg L1 ; initial pH, 3; current,
2.0 A.)

higher than those of UV/H2 O2 and EF processes, respectively.

It is derived from these results that the main Fenton reaction, the
reaction (1), is more effective in the reactor for initial pH 3 and
first 20 min than the reaction (8) which is the main reaction of the
UV/H2 O2 . In addition, the reaction (1) can also be propagated
by the reaction (8) which is an important source for ferrous ion
generation in the high hydrogen peroxide concentration, and
reaction (9) in which ferric ions are reduced to ferrous ions at
the cathode surface.
Fe3+ + e Fe2+

(8)

Fe3+ + H2 O2 H2 O + H+ + Fe2+

(9)

In addition, 10% difference in the COD removal efficiency

between the PEF and the EF process can be described by the
reaction (5), which is another promoting reaction of the hydroxyl
radical production by UV light, and the reaction (8). However,
these reactions are more effective at initial pH 2.5 (89% COD
removal efficiency seen in Fig. 2a) than initial pH 3.0 (80% COD
removal efficiency seen in Fig. 8a).
Another result can be derived from Fig. 8a that the COD
removal efficiency of the EC process for landfill leachate is relatively lower than those of the other process. This phenomena
can be a result of the high soluble organics concentration in the
solution causing the low removal efficiency in the EC process,
and/or the final pH in the rector that is the effective solution pH
of the process should be higher than 4.
Fig. 8b shows color removal efficiencies obtained from comparative experiments. As seen from Fig. 8b that the best color
removal efficiencies were obtained in the PEF experiments.
However, the important decrements were seen in the efficiencies of the PEF and the EF experiments after the 20th minutes
and the 30th minutes, respectively. It is thought that the reason
of this phenomenon is color generation in the solution due to
the excessive ferrous ions produced from the reactions (5) and
(8) for the PEF process, and the reaction (9) for the EF process.
In the EC experiment, color removal efficiencies drastically rise
by increasing the solution pH. High color removal efficiencies

reveal that a large amount of the color in the landfill leachate

is colloidal pollutants. This judgement is also supported by the
relatively low removal efficiencies observed in the UV/H2 O2
experiments.
4. Conclusions
Based on the obtained results, it may be concluded that the
described PEF process can be proposed as a promising approach
for high removal of COD, color and phosphate from the landfill
leachates. Besides its high removal efficiency, the method provides waste sludge having low amount and high settling quality
compared to conventional treatment. In addition, when it is compared with EC, UV/H2 O2 and EF processes, it is determined that
the proposed PEF process is more effective than the other treatment in terms of treatment efficiency. The results also revealed
that the operating parameters such as pH, H2 O2 concentration,
and applied current should be taken into consideration to obtain
an effective treatment in the process. Although, the high operating costs of the process due to high concentrations of used H2 O2
which limits its commercial usage, it can be applied for the treatment of wastewaters heavily polluted with organic compounds
which are not readily biodegradable.
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