Degradation of Dyes From Aqueous Solution by Fenton Processes

Environ Sci Pollut Res (2013) 20:20992132
DOI 10.1007/s11356-012-1385-z
REVIEW ARTICLE
Degradation of dyes from aqueous solution

by Fenton processes: a review
Puthiya Veetil Nidheesh & Rajan Gandhimathi &
Srikrishnaperumal Thanga Ramesh
Received: 10 October 2012 / Accepted: 29 November 2012 / Published online: 22 January 2013
# Springer-Verlag Berlin Heidelberg 2013
Abstract Several industries are using dyes as coloring

agents. The effluents from these industries are increasingly
becoming an environmental problem. The removal of dyes
from aqueous solution has a great potential in the field of
environmental engineering. This paper reviews the classification, characteristics, and problems of dyes in detail.
Advantages and disadvantages of different methods used
for dye removal are also analyzed. Among these methods,
Fenton process-based advanced oxidation processes are an
emerging prospect in the field of dye removal. Fenton
processes have been classified and represented as Fenton
circle. This paper analyzes the recent studies on Fenton
processes. The studies include analyzing different configurations of reactors used for dye removal, its efficiency, and
the effects of various operating parameters such as pH,
catalyst concentration, H2O2 concentration, initial dye concentration, and temperature of Fenton processes. From the
present study, it can be conclude that Fenton processes are
very effective and environmentally friendly methods for dye
removal.
Tamil Nadu, India reached up to US$ 2,500 million in the

years 20082009 (Srivastava et al. 2011). Due to the higher
production of garments, the effluent production is also very
high. India may be the major contributor of textile wastewater in South Asia (Verma et al. 2012). More than
100,000 m3/day of textile effluent was generated from 800
dyeing, bleaching, and textile-processing industries situated
in Tirupur (Ranganathan et al. 2007). Treatment of these
effluents is becoming a headache for environmental engineers and studies show that Fenton-based advanced oxidation process is one of the efficient and environmentally
friendly tool for the treatment of dye effluent (Nidheesh
and Gandhimathi 2012; Brillas et al. 2009).
This review paper highlights the problems of various
dyes. The main objective of this study is to present a general
survey on dye removal by Fenton processes. Recent developments in the field of Fenton processes for dye removal are
analyzed and critical analysis of different Fenton processes,
mechanisms, advantages, and disadvantages are included in
this article. Factors affecting Fenton processes are also described in this article.
Keywords Dye . Decolorization . Fenton . Advanced

oxidation process
Dye and its classification
Introduction
Increase in population demands an increase in commodities
or products. This law is applicable in the case of textile
industry also. For example, garment export from Tirupur,
Responsible editor: Vinod Kumar Gupta
P. V. Nidheesh : R. Gandhimathi (*) : S. T. Ramesh
Department of Civil Engineering, National Institute of Technology,
Tiruchirappalli, Tamil Nadu, India
e-mail: rgmathii@nitt.edu
A dye is a colored organic compound that strongly absorbs

light in the visible region and can firmly attach to the fiber
by virtue of chemical and physical bonding between the
groups of the dye and groups of the fibers. To be of commercial importance, a dye should be fast to light, rubbing
and water. Any colored compound may not always be a Dye
or Dyestuff. Colour is a physiological sensation associated
with the wavelength of light striking the retina of the eye.
The sensation of colour is produced when light having a
wavelength within the visible region of electromagnetic
spectrum strikes the retina of the eye (Iqbal 2008).
2100
Dye molecules comprise of two key components: the

chromophores, responsible for producing color, and the
auxochromes, which cannot only supplement the chromophore but also render the molecule soluble in water and give
enhanced affinity (to attach) toward the fibers (Gupta and
Suhas 2009). Chromophores determine the color of the dye
while the auxochromes determine the intensity of the color
(Moussavi and Mahmoudi 2009). The chromophore group
is a radical configuration consisting of conjugated double
bonds containing delocalized electrons. The chromogen,
which has an aromatic structure normally contain benzene,
naphthalene, or anthracene rings, is a part of chromogen
chromophore structure along with an auxachrome. The presence of ionizing groups known as auxochromes results in a
much stronger alternation of the maximum absorption of the
compound and provides a bonding affinity (Allen and
Koumanova 2005). Some common auxochrome groups include NH3, COOH, HSO3, and OH (Al-Ghouti 2004).
Dyes can be classified (Iqbal 2008) in many ways. The
organic chemists classify them according to their common
parent structure (Chemical Classification). The dyer, who is
only interested in fixing the dye to the fiber, classifies them
according to their method of application (Iqbal 2008). The
classifications of dyes are given in Table 1. Dyes used in
textile industries are classified (Sharma et al. 2011) into
three classes: (a) anionic (direct, acid, and reactive dyes),
(b) cationic (all basic dyes), and (c) nonionic (dispersed
dyes).
Problems of dyes
The rapid development of the textile industries results in the
dyes becoming one of the main sources of severe water
pollution. The discovery of synthetic dyes overwhelmed the
role of natural dyes in the society due to its low production
cost, brighter colors, better resistance towards environmental
factors, and easy-to-apply factor (Wan Ngah et al. 2011). This
has led to a higher consumption of synthetic dyes over natural
dyes for most types of industrial applications (Wan Ngah et al.
2011). Many industries like textiles, leather, cosmetics, paper,
printing, plastics, etc. use many synthetic dyes to color their
products. Thus, effluents from these industries contain various
kinds of synthetic dye stuffs (Sharma et al. 2011). Over
100,000 commercially available dyes exist and more than
7105 t per year are produced annually (Pearce et al. 2003;
McMullan et al. 2001). It has been reported that nearly 40,000
dyes and pigments are listed, which consist of more than
7,000 different chemical structures (Demirbas 2009).
However, it is reported that 1015 % of the used dyes enter
the environment through wastes (Hai et al. 2007; Husain
2006). Typical textile industry wastewater characteristics can
be summarized by a chemical oxygen demand (COD) range
from 150 to 12,000 mg/L, total suspended solids between

2,900 and 3,100 mg/L, total Kjeldahl nitrogen from 70 to
80 mg/L, and BOD range from 80 to 6, 000 mg/L leading to
a biochemical oxygen demand (BOD)/COD ratio of around
0.25, showing that it contains large amounts of nonbiodegradable organic matter (Oller et al. 2011).
Presence of color and color-causing compounds has always been undesirable in water for any use (Sharma et al.
2011). The presence of very small amounts of dyes in water
(less than 1 ppm for some dyes) is highly visible and
undesirable (Robinson et al. 2001; Banat et al. 2003).
They may also be toxic to some aquatic life due to the
presence of metals, chlorides, etc. in them (Clarke and
Anliker 1980). Most of them are toxic, mutagenic, and
carcinogenic. Lethal levels may be reached, affecting aquatic systems and associated flora and fauna (Gupta et al.
2007a). Moreover, they are unusually resistant to degradation due to their complex structure and xenobiotic properties
(Cristovao et al. 2011; Gupta et al. 2007b). Wastewater
containing dyes is difficult to treat since dyes are recalcitrant
organic molecules, resistant to aerobic digestion and are
stable to light, heat, and oxidizing agents (Sun and Yang
2003). The environmental impacts of dyes are given in
Fig. 1. The application and problems posed by the different
types of dyes are given in Table 2.
Methods for dye removal

In the last few years, however, more information on the environmental consequences of dyestuff usage has become available and the dye manufacturers, users, and government
themselves are taking substantial measures to treat the dyecontaining wastewater (Gupta and Suhas 2009). A wide range
of methods has been developed for the removal of dyes from
water and wastewater to decrease their impact on the environment (Forgacs et al. 2004). Generally, the treatments of the
dyestuff effluents can be classified into three major categories,
namely, biological, chemical, and physical treatment (Monash
and Pugazhenthi 2009). Various physical and chemical techniques such as adsorption (Gupta et al. 2007d, 2010b, 2011b,
2012b, c; Gandhimathi et al. 2012), photo-catalysis (Gupta et
al. 2011c, d, 2012d; Saleh and Gupta 2011, 2012a), adsorptional photocatalytic degradation (Gupta et al. 2012e), ozonation (Cuiping et al. 2011; Tizaoui and Grima 2011), coagulation
(Beltrn-Heredia et al. 2011; Ellouze et al. 2011; Chafi et al.
2011), electrocoagulation (Balla et al. 2010; Chafi et al. 2011;
Daneshvar et al. 2007; Kobya et al. 2007; Zaroual et al. 2006),
electro chemical methods (Aquino et al. 2011; Jain et al. 2005;
Mohan et al. 2007), membrane separation (Ciardelli et al. 2000;
Ellouze et al. 2011; Srivastava et al. 2011), sonolysis
(Berberidou et al. 2007; Li et al. 2010; Martinez and Uribe
2012), jet cavitation (Wang et al. 2011a, b), wet air oxidation
2101
Table 1 Classification of dyes (Iqbal 2008)

No.
Dye type
I. According to chemical structure

1
Nitro dyes
2
Azo dyes
3
4
Diphenlymethane dyes
Triphenylmethane dyes
Xanthene dyes
6
Phthaeleins
7
Indigoid and Thioindigoid dyes
8
Anthraquinoid dyes
II. According to method of application
1
Direct dyes
Mordant dyes
Vat dyes
Ingrain dyes
Disperse dyes
Characteristics
Examples
Polynitro derivatives of phenols containing at least one

nitro group ortho or para to the hydroxyl group.
The azo dyes represent the largest and the most
important group of dyes. They are characterized by
the presence of one or more azo groups (N0N),
which form bridges between two or more aromatic rings.
Picric acid, Maritus yellow and

Naphthol yellow S
Aniline yellow, Butter yellow,
Chrysoidine, Methyl Orange,
Orange II, Para Red, Resorcin
Yellow, Disperse Red 1, Congo
Red.
Auramine O
Malachite Green, Pararosaniline,
Rosaniline, Crystal Violet
Central carbon atom is joined to two benzene

rings and to p-quinoid group. Triphenylmethane
dyes are not fast to light or washing, however,
except when applied to acrylic fibers. They are
used in large quantities for coloring paper, and
typewriter ribbons where fastness to light is
not so important.
Obtained by condensing phenols with phthalic
anhydride in the presence of zinc chloride,
sulphuric acid, or anhydrous oxalic acid.
Phthaleins are related to xanthene dyes
Indigoid is the parent compound of indigoid dyes.
A p-quinoid group is fused to two other benzene rings.
These contain acidic or basic groups and
combine with polar groups in the fiber.
Such dyes color a fabric directly when
the fiber is immersed in a hot aqueous
solution of the dye.
This class of dyes requires a pretreatment of
the fiber with a mordant material designed
to bind the dye. The mordant becomes
attached to the fiber and then combines with
the dye to form an insoluble colored complex.
This complex is called a lake. Commonly
used mordant are the oxides of aluminum,
iron and chromium.
These dyes are insoluble in water, but on reductin
with sodium hydrosulphite yield alkali soluble
forms (Leuco-compounds) which may be colorless.
It is in this form they are introduced into the fabric.
The reducing operation was ormerly carried out in
wooden vats, giving rise to the name Vat Dyes.
After the reduced dye has been absorbed in the
fiber, the original insoluble colored dye is reformed
by oxidation with air or chemicals.
These dyes are synthesized within the fa bric, and
may be applied to any type of fiber.
These are insoluble in water, but are capable of
dissolving certain synthetic fibers. Disperse dyes
are usually applied in the form of a dispersion of
finely divided dye in a soap solution in the presence
of some solublising agent such as phenol, cresol, or
benzoic acid. The absorption into the fiber is carried
out at high temperatures and pressures.
(Ovejero et al. 2011; Hua et al. 2013), liquid emulsion membrane (Das et al. 2008; Othman et al. 2011; Djenouhat et al.
2008; Das and Hamdaoui 2010), etc. were applied
Fluorescein, eosin, and

Rhodamine B.
Phenolphthalein,
Tyrian Purple, Thioindigo
Alizarin
Naphthol Yellow S and
Martius Yellow
Alizarin
Indigo
Azo dyes
Celliton Fast Pink B and
Celliton Fast Blue B
successfully for the treatment of various dyes. These techniques

are effective and economic only in the case where the solute
concentrations are relatively high (Sharma et al. 2011; Panswed
2102
Fig. 1 Schematic representation of the effect of textile wastewater into the environment (Verma et al. 2012)
and Wongchaisuwan 1986; Malik and Saha 2003; Koch et al.

2002; Ciardelli et al. 2000; Gupta and Suhas 2009). Some of
these methods are costly and sometimes produce hazardous
byproducts (Yang et al. 2011). Biological processes applied for
decolorization of textile effluents are based on anaerobic and
aerobic processes (Yasar et al. 2012). Reactors like, rotating
biological contactor (Pakshirajan and Kheria 2012), upflow
anaerobic sludge blanket reactor (Senthilkumar et al. 2011),
enzyme membrane reactors (Katuri et al. 2009), anaerobic/
aerobic fixed-bed sequencing batch biofilm reactor (Hosseini
Koupaie et al. 2013), fluidized bed reactor (Andleeb et al.
2010), and species like fungi (Agnes Mariya Dorthy et al.
2012; Andleeb et al. 2010), yeast (Charumathi and Das
2010), bacteria (Senthilkumar et al. 2012; Kaushik and Malik
2009), fungalbacterial consortium (Lade et al. 2012), anoxic
aerobicanoxic microenvironment (Venkata Mohan et al.
2012), etc. were used successfully for decolorizing the colored
wastewater recently. Even though biological treatment is the
most economical alternative when compared with other physical and chemical processes, their application is often restricted
because of technical constraints (Crini 2006). Biological methods are time consuming and they are often ineffective in
removing dyes which are highly structured polymers with
low biodegradability and cannot be applied to most textile
wastewaters due to the toxicity of most commercial dyes to
the organisms used in the process (Mohan et al. 2007; Zaroual
et al. 2006). The methods of dye removal can also be classified
as destructive and nondestructive methods (Fig. 2; Fernndez et
al. 2010). Table 3 summarizes the advantages and disadvantages of the various methods used for dye removal.
Fenton process
The development of novel treatment methods encompasses
investigations of advanced oxidation processes (AOPs),
which are characterized by the production of hydroxyl radical (OH) as a primary oxidant (Hua and Hoffmann 1997).
OH is the second highest powerful oxidant after fluorine
(Table 4). These radicals are very reactive, attack most of the
organic molecules, and are not highly selective (Skoumal et
al. 2006; Rosenfeldt et al. 2007). OH reacts with most of
the organic compounds at near diffusion-limited rates
(Arantes and Milagres 2007). These hydroxyl radicals attack
organic molecules by either abstracting a hydrogen atom or
adding hydrogen atom to the double bonds (Mohajerani et
al. 2009). It makes new oxidized intermediates with lower
molecular weight or carbon dioxide and water in case of
complete mineralization (Mohajerani et al. 2009).
The Fenton reaction is a catalytic process for the generation of hydroxyl radicals from hydrogen peroxide and is
based on an electron transfer between H2O2 and iron ions
acting as homogeneous catalyst (Barbusiski and Majewski
2003). The Fenton process was reported by Fenton (1884)
over 100 years ago for maleic acid oxidation. The Fenton
reaction is based on the formation of OH, a nonspecific
oxidant with a high E0 value that can degrade pollutants
efficiently (Hsing et al. 2007). Fenton process is performed
in four stages, which are pH adjustment to low acidic
values, oxidation reaction, neutralization, and coagulation
(Meric et al. 2004). Lowering the pH is an important step in
the Fenton process because degradation of organic matter is
most effective at pH 3 (Kochany and LipczynskaKochany 2009). Also, H2O2 and ferrous ions are more
stable at lower pH (Meric et al. 2004). In Fenton process,
both ferrous and ferric ions can act as coagulants; therefore,
they have dual functions of oxidation and coagulation in
treatment process (Kang et al. 2002a). Fenton technology is
widely studied and reported as an interesting alternative for
the treatment of industrial wastewater containing nonbiodegradable organic pollutants (Hassan and Hameed 2011). The
degradation mechanism of organic pollutants by Fenton
Anthraquinone dye
Vat dye, indigoid dye
Remazol Brilliant Blue R
Indigo Carmine
Textile industry (Hadibarata et al. 2012), used to screen fungi

for lignolytic activity (Zhang et al. 2007a).
Mainly used in the textile industry for the dyeing of polyester
fibers and denim (Gutirrez-Segura et al. 2009). Used in
Widely used in textile industry for dyeing silk, wool, jute leather
and cotton (Cuiping et al. 2011), It is also a useful analytical
reagent for the detection and determination of metals (Gupta
et al. 2004, 2010a)
Basic dye, Xanthene

dye
Triphenylmethane
cationic dye
Malachite green
Used in biology to stain cells (Lv et al. 2011), printing calico,

dyeing, printing cotton and tannin, indicating oxidationreduction, and dyeing leather, and in purified zinc-free form,
it is used as an antiseptic and for other medicinal purposes
(Gupta et al. 2004)
Extensively used all over the world in the fish farming industry
as fungicide, ectoparasiticide and disinfectant (Gong et al.
2006). Used as medical disinfectant and coloring agent on
silk, wool, jute, leather, cotton, paper, and acrylic (Culp and
Beland 1996)
Rhodamine B
Cationic dye
Methylene blue
Used widely in the textile industry (Deniz and Karaman 2011)

Used for dying silk, wool, leather, jute, cotton, biological stain,
dermatological agent, veterinary medicine, green ink
manufacture, intestinal parasites, fungus textile dying and
paper printing (Ghaedi et al. 2011)
It is the active ingredient in Grams stain, and is employed as a

bacteriostatic agent (Bale 1981). The dye is used as an external
skin disinfectant in humans and animals (Ryan 1992; Saji et al.
1995). It is widely used as a purple dye for textiles such as
cotton and silk, and in paints and printing ink (Au et al. 1979).
Being used for various purposes: a biological stain, a
dermatological agent, a veterinary medicine, an additive to
poultry feed to inhibit propagation of mold, intestinal parasites
and fungus etc. It is also extensively used in textile dying and
paper printing (Adak et al. 2005)
Azo dyes
cationic dye
Acid Yellow 220

Brilliant green
Uses
Crystal violet (basic violet 3, Triphenylmethane

cationic dye
gentian violet, and methyl
violet)
Type
Dye
Table 2 Uses and problems of different dyes
Affects the aquatic life and causes detrimental effects in

the liver, gill, kidney, intestine and gonads (Srivastava
et al. 2004). In humans, it may cause irritation to the
gastrointestinal tract and even cancer upon ingestion
(Garg et al. 2004). Skin contact with malachite green
causes irritation redness and pain (Vijayakumaran and
Arivoli 2012). Contact with the eye can lead to
permanent injury in humans and laboratory animals
(Khataee et al. 2009; Kumar et al. 2005)
Toxic to mammalian cells and is a mutagen and a mitotic
poison (Fan et al. 2011). The dye is responsible for causing
moderate eye irritation, causing painful sensitization to
light. It can cause permanent injury to the cornea and
conjunctiva since the product contains a cationic dye and
such dyes have been reported to cause toxicity to
mammalian cells (Thomas and MacPhee 1984; Jone and
Falkinham 2003). It may be absorbed in harmful amounts
through the skin and cause skin irritation and digestive
tract irritation. In extreme cases it may lead to respiratory
and kidney failure and permanent blindness (Mittal et
al. 2010a)
May cause carcinogenic and teratogenic effects on public
health (Gupta and Suhas 2009). The carcinogenicity,
reproductive and developmental toxicity, neurotoxicity
and chronic toxicity towards humans and animals have
been experimentally proven (Jain et al. 2007)
An important class of toxic and recalcitrant
organopollutants (Hadibarata et al. 2012).
A highly toxic indigoid dye and might cause skin and eye
irritations to human beings. It can also cause permanent
Toxic, mutagenic and carcinogenic (Saratale et al. 2011)

Causes irritation to the gastrointestinal tract; symptoms
include nausea, vomiting and diarrhea (Mittal et al.
2008), irritation to the respiratory tract, leading to cough
and shortness of breath (Mane and Vijay Babu 2011).
Skin contact causes irritation with redness and pain
(Mittal et al. 2008), it can cause permanent injury to
eyes, a mutagen in microorganisms (Rehman et al. 2011),
may form hazardous products like carbon oxides, nitrogen
oxides, and sulfur oxides when heated to decomposition
(Mane et al. 2007)
Acute exposure to Methylene blue will cause increased
heart rate, vomiting, shock, Heinz body formation,
cyanosis, jaundice, quadriplegia, and tissue necrosis in
humans (Hameed and Ahmad 2009)
Problems

2103
Mono Azo dye
Diazo dye
Azo dye
Azo dye
Acid dye
Triaminotriphenylmethane Widely used as coloring agent for textile and leather materials
dye
(Gupta et al. 2008). It is also used to stain collagen, muscle,
mitochondria, and tubercle bacillus (Luna 1968)
Direct red 23
Acid Orange 7
Chrysoidine Y
Quinoline yellow
Basic fuchsin, Magenta II
Used in coloring fibers, leather, paper, agrochemicals, fertilizers,

detergents, wood, ink, externally applied cosmetics, etc. (Gupta
et al. 2005)
Used widely in the textile industry (Mittal et al. 2010b)
Used for dyeing a variety of materials such as nylon,

aluminum, detergents, cosmetics, wool, and silk
(Gupta et al. 2006a; Greluk and Hubicki 2011)
Textile, tannery, paper, soap, cosmetics, polishes, wax

(Abdelwahab et al. 2005)
Textile, tannery, paper, soap, cosmetics, polishes, wax

(Malik 2003)
food industry, cosmetics industries, as a diagnostic aid, as

a redox indicator in analytical chemistry, and as a microscopic
stain in biology (Lakshmi et al. 2009)
Acid Yellow 36
Uses
Type
Dye
Table 2 (continued)
injury to cornea and conjunctiva (Mittal et al. 2006), is

carcinogenic and can lead to reproductive, developmental,
neuro and acute toxicity. It has also been established that
the dye leads to tumors at the site of application (Barka
et al. 2008). Indigo carmine causes irritation to the
gastrointestinal tract leading to nausea, vomiting and
diarrhea. It may also cause irritation to the respiratory
tract such as coughing and shortness of breath (Lakshmi
et al. 2009)
Toxic and carcinogenic nature, Acute toxicity to
heteropneustes fossilis (Malik 2003), loss of body weight,
changes in body colors, restlessness, jerky and random
movements to fish (Mall and Kishore 1995; Goel and
Gupta 1995)
Toxicity and carcinogenic nature, dose will not allow
sunlight to pass through and thereby affects the
photosynthesis of aquatic plants (Abdelwahab et al. 2005)
It is highly toxic, and its ingestion can cause eye, skin,
mucous membrane, and upper respiratory tract irritation;
severe headaches; nausea; water-borne diseases such as
dermatitis; and loss of bone marrow leading to anemia
(Anliker 1986). Its consumption can also prove fatal,
as it is carcinogenic in nature and can lead to tumors
(Cartwright 1983)
Carcinogenic (Cartwright et al. 1983). Chrysoidine Y may
also undergo reduction followed by a chain of reactions
leading to formation of other toxic compounds, which
are potentially harmful to humans and animals (Mittal
et al. 2010b). Oral administration of Chrysoidine Y
results in liver-cell adenomas, carcinomas and leukemia
in animals (IARC Monog. 1975)
Carcinogenic and can also cause tumor and allergy (Lu
and Lavallee 1964; Oettel et al. 1965). Though it is
considered less toxic than its spirit soluble counterpart,
its oral consumption is prohibited, particularly for
infants and children (Coleman 1991)
Inflammable in nature (Gupta et al. 2008), The physical
contact with the dye may cause severe eye and skin
irritation (Churchman 1923). Its ingestion may cause
gastrointestinal irritation with nausea, vomiting, and
diarrhea and the inhalation of the dye causes irritation
to the respiratory tract (Fisher 1980). Inhalation or
ingestion may also cause damage to the organs such
as blood, liver, spleen, and thyroid (Crandall et al. 1929;
Ball 1972; Rogers et al. 1978). Repeated exposure to the
dye may affect the nervous system with headache,
Problems
2104
Azo dye
Triphenylmethane dye
Metanil Yellow
Brilliant Blue FCF
Amaranth
Azo Dye
Xanthene dye
Erythrosine
Safranin-T
Type
Dye
Table 2 (continued)
Problems
dizziness, lethargy, and muscle contraction. In humans

and animals, its toxicity includes carcinogenic and
mutagenic effects (Littlefield, et al. 1985)
May affect thyroid activity (Gupta et al. 2006b), one
Used for coloring pharmaceuticals, food products, wool, silk, nylon,
of the causes of atopic diseases (Uysal and Aral 1998).
drugs, cosmetics, cocktails, tinned cherries and fruits, biscuits,
Its consumption can also prove fatal, as it is carcinogenic
chocolates, garlic sausages, salmon spreads, scotch eggs, stuffed
in nature and can lead to tumors (Borzelleca and Hallagan
olives, sweets, bakery items, snack foods, chewing gums, jellies,
1987; Sasaki et al. 2002). The comet assay on the glandular
wines, drugs, ice creams, etc. (Jain et al. 2005; Gupta et al. 2006b;
stomach, colon, liver, kidney, urinary bladder, lung, brain,
Ozsoy and Araman 1993; Tripathi et al. 2004). It is also being used
and bone marrow was performed and it was found that
for coloring food, in printing inks and lipstick, as a biological stain,
erythrosine induced DNA damage in the gastrointestinal
a dental plaque disclosing agent, and a radio plaque medium
organs even at a low dose (Pereira et al. 2000). Moreover
(Ishikawa et al. 2003; Desiderio et al. 1998)
research has proved that long term use of erythrosinecontaining lipsticks by Indian women of lower economic
background may lead to abnormal embryonic development
(Mailman and Lewis 1987). In addition the food color
erythrosine was hypothesized to be a neurotoxicant because
it disrupted neurotransmitter uptake in vitro (Augustine
Jr.and Levitan 1980; Tanaka 2001). Moreover it is a
xenoestrogen, which enhances the effect of estrogens
(Vidaeff and Sever 2005)
Widely used as a colorant in sweet meat, ice creams, soft drinks and
It causes toxic methaemoglobinaemia (Sachdeva et al.
beverages. Due to its orange-yellow color, the dye is also extensively
1992) and cyanosis (Chandro and Nagaraja 1987) in
used for coating turmeric. It is widely used in leather, paper and
humans, while skin contact results into allergic dermatitis
textile industries (Seth et al. 2000) and also as a stain and colorant
(Hausen 1994). Metanil Yellow also has tumor-producing
for thewool (OConnor 1997; Fierz-David and Blangey 1949). It is
effects and can also create intestinal (Ramachandani et al.
also used as coloring material for lacquers and cosmetic products.
1997) and enzymic (Das et al. 1997) disorders in human
The dye is highly suitable for the preparation of colored water-fast
body. Though it is not mutagenic but can alter the
inks (Zimmerman 1933) and can also be employed for determining
expression of genes (Gupta et al. 2003)
trace amounts of Mo(VI) (Wang and Du 1996). Apart from all these,
MetanilYellowcan act as an indicator for the determination of H+ ion
concentration in the pH range of 1.22.3 (Fay 1911)
Used as a colorant in textile and leather, a common food additive in
It is toxic and carcinogenic (Gupta et al. 2006c). It causes
beverages, dairy products, powders, jellies, confections, icings,
severe allergies and anaphylactic reactions in living beings
syrups, extracts and condiments (Gupta et al. 2006c)
(Mortelmans et al. 1986; Metheny 2002)
Used as food dye in flavoring and coloring candies and cookies,
It can cause eye irritation and can also create permanent injury
used for dyeing tannin, cotton, bast fibers, wool, silk, leather and
to the cornea and conjunctiva in human and rabbit eyes. It
paper (Zaghbani et al. 2008; Gupta et al. 2006d, 2011a)
also causes skin and respiratory tract irritation (Gupta et al.
2007c, 2011a)
It is widely used for coloring textile materials, paper, wood, leather
It is toxic and carcinogenic (Gupta et al. 2012a). A prolong
etc. (Gupta et al. 2012a; Mittal et al. 2005)
intake of Amaranth can result to tumors, allergy, respiratory
problems and birth defects (Koutsogeorgopoulou et al. 1998;
Lockey 1959; Talmage 1992; Bantle et al. 1990)
Uses

2105
2106
Fig. 2 Methods for dye

removal (Fernndez et al. 2010)
reaction is shown below (Neyens and Baeyens 2003; Ma et

al. 2005; Gu et al. 2012):
Fe2 H2 O2 ! Fe3 OH HO
RH HO ! R H2 O
RH denotes dyes
R Fe3 ! R Fe2
Fe2 HO ! Fe3 OH
Ferrous ions are regenerated in Fenton process by the

reaction between ferric ion and H2O2 (Eqs. (5) and (6)) in
acidic aqueous medium (Walling 1975; Chen and Pignatello
1997; Kang et al. 2002b). These reactions increase advantages of Fenton processes because the regenerated Fe2+ will
undergo further Fenton reactions.
Fe3 H2 O2 ! Fe2 H HO2
Fe3 HO2 ! Fe2 O2 H
When ferric salts are used instead of ferrous salts in

Fenton process, the hydroxyl radical is produced in a
two-stage process with the slow reaction between ferric
ion and hydrogen peroxide (Eqs. (7) and (8)) followed
by the rapid reaction between the produced ferrous ion
and additional hydrogen peroxide (Bishop et al. 1968;
Kiwi et al. 1993).
Zero-valent iron also undergoes Fenton reactions.

Zero-valent iron metal (Fe0) is a very promising reactive
medium due to its low cost, effectiveness, ability to
degrade contaminants, and its accessibility (Hardy and
Gillham 1996; Deng et al. 2000). In acidic conditions,
the surface of the zero-valent iron corrodes and generates
in situ ferrous ions, which can leads to Fenton reactions
in the presence of hydrogen peroxide (Eq. (9); Fu et al.
2010a). This Fe2+ subsequently reacts with H2O2 as in
the traditional Fenton reaction (Pagano et al. 2011).
There is a considerable interest in the development of
transition metalligand complexes that can perform hydrogen peroxide decomposition with the production of
reactive oxygen species such as hydroxyl radicals (Bali
and Karagzolu 2007). Transition metals like copper
(Pecci et al. 1997) can undergo Fenton-based reaction
as shown in the following general equation (Eq. (10)):
Fe0 H2 O2 ! Fe2 2OH
Mn1 H2 O2 ! Mn HO OH
10
Fe3 H2 O2 ! FeO2 H2 H
where, M is a transition metal.

The generation of ferrous ions in the Fe0/H2O2 system
may be influenced by the addition of metal ions such as Fe3+
and Cu2+ (Pagano et al. 2011). Although Fe3+ ions are
generated by the Fenton reaction itself, an excess of these
ions may enhance the production of Fe2+ (Eq. (11); Pagano
et al. 2011).
FeO2 H2 ! HO2 Fe2
Fe0 2Fe3 ! 3Fe2
11
2107
Table 3 Advantages and disadvantages of dye removal methods from wastewater

Technology
Advantages
Disadvantages
Coagulation
flocculation
Simple, economically feasible (Crini 2006)
Ozonation
No change in effluent volume (Robinson et al. 2001)
Photochemical
No sludge generation (Robinson et al. 2001), Rapid

process and good sorption capacity for dyes
(Mirkhani et al. 2009)
Economically attractive, publicly acceptable
treatment (Crini 2006)
Causes extra pollution due to the undesired reactions

in treated water and produces large amounts of
sludge (Kobya et al. 2007)
High production cost of ozone and the low ozone
utilization due to poor mass transfer rate of ozone
(Gao et al. 2005; Boilyky and Associates 1981),
short half-life (20 min; Robinson et al. 2001)
Formation of byproducts (Robinson et al. 2001),
High energy costs (Mirkhani et al. 2009)
Biodegradation
Adsorption on
activated carbon
High adsorption capacity (Mittal et al. 2010b) and no

chemical degradation (Saleh and Gupta 2012b), it
can handle fairly large flow rates, producing a high
quality of water without producing notorious sludge,
residual contaminants, etc. (Gupta et al. 2007e)
Electrochemical
Additional chemical is not required, easy implementation

and the high removal rates (Aquino et al. 2011),
nonhazardous end products (Robinson et al. 2001)
No loss of sorbent on regeneration, effective
(Crini 2006)
Ion - exchange
Membrane filtration
Oxidation
Advanced oxidation
process
Adsorption/biosorption
Electrocoagulation
Biomass
Sonolysis
Environmentally friendly (Pearcea et al. 2003), removes

all dye types, produce a high-quality treated effluent
(Crini 2006)
Rapid and efficient process (Crini 2006)
Neither transfer pollutants from one phase to the other nor
produce massive amounts of hazardous sludge
(Dojcinovic et al. 2011), Little or no consumption of
chemicals, and efficiency for recalcitrant dyes (Crini
2006), and organic contaminants are commonly
oxidized to CO2 (Gupta et al. 2012f)
Easy operation, insensitivity to toxic substances, ability to
treat concentrated forms of the dyes, and the possibility of
reusing the spent adsorbent via regeneration (Dobrowski
2001), Fast, inexpensive, ecofriendly and recycling of
waste materials (Gupta et al. 2010c, 2011e; 2012g; Gupta
and Sharma 2003; Nidheesh et al. 2011, 2012a, b; Ali and
Gupta 2006; Gupta and Rastogi 2008, 2009; Gupta and
Ali 2008; Jain et al. 2004)
High efficiency at low capital and operation costs, simplicity
and compactness of the equipment required and easiness of
process control that result in robustness (Chafi et al. 2011).
Eliminates or reduces the need for additional chemicals,
and decrease drastically sludge production in comparison to
coagulation (Balla et al. 2010). Additional chemical is not
required and no sensitivity to toxicity (Daneshvar et al. 2007)
Low operating cost, good efficiency and selectivity, no toxic
effect on microorganisms (Crini 2006)
No Extra sludge production (Adewuyi 2001; Arslan-Alaton
2003)
But numerous competitive reactions are also occurring in

the Fenton process (Eqs. (1215)). These reactions
Slow process, necessary to create an optimal favorable

environment, maintenance and nutrition requirements
(Crini 2006)
Relatively high operation costs, which hamper its
large-scale application (Mittal et al. 2010b), Ineffective
against disperse and vat dyes, the regeneration is
expensive and results in loss of the adsorbent,
non-destructive process (Crini 2006)
High cost of electric energy (Robinson et al. 2001)
Economic constraints, not effective for disperse dyes

(Crini 2006), Less efficient for column or flow
adsorption systems (Slokar and Le Marechal 1997)
Concentrated sludge production (Robinson et al. 2001),
High pressures, expensive, incapable of treating large
volumes (Crini 2006)
Produces some very toxic products such as
organochlorine compounds (Daneshvar et al. 2007)
Operation is quite expensive (Comninellis et al. 2008),
Treatment efficiency is inadequate because of the
large variability of the composition of textile
wastewaters (Kobya et al. 2007)
Requires chemical modification, non-destructive

process (Crini 2006). Regeneration and reactivation
processes often result in the degradation of the
adsorption properties of the carbon, which
subsequently affects the economic viability of the
operation (Gupta et al. 2011f)
High water conductivity is required to reduce power

requirements (Chafi et al. 2011). Lack of general
design of batch or continuous electrocoagulation
reactors (Mollah et al. 2001). Complexity of the
mechanisms involved in pollution abatement
(Chafi et al. 2011)
Slow process, performance depends on some
external factors (pH, salts) (Crini 2006)
Requires a lot of dissolved oxygen, High cost
(Adewuyi 2001; Arslan-Alaton 2003)
negatively affect the oxidation process (Walling 1975;

Kang et al. 2002b; Bielski et al. 1985; Buxton et al. 1988;
2108
Table 4 Oxidizing potential of some oxidizing agents (Parsons and

Williams 2004)
Oxidizing agent
Fluorine
Hydroxyl radical
Atomic oxygen
Ozone
Hydrogen peroxide
Hypochlorite
Chlorine
Chlorine dioxide
Molecular oxygen
Oxidation potential (E0) (V)

3.06
2.80
2.42
2.06
1.78
1.49
1.36
1.27
1.23
Fig. 4 Fenton circle
Bergendahl and Thies 2004; Burbano et al. 2005).

HO H2 O2 ! HO2 H2 O
12
HO Fe2 ! Fe3 HO
13
HO2 H2 O2 ! O2 HO OH
14
HO2 Fe2 ! Fe3 HO

2
15
The overall classification of Fenton processes is shown in

Fig. 3. Based on the usage of external energy for dye
degradation, Fenton process can be divided into two.
External energy includes ultrasound, light, and electricity.
These sources will enhance the degradation capacity of the
AOP systems. Conventional Fenton process is the only one
process, which is not using external energy. Extended
Fenton processes and hybrid Fenton processes are the two
Fenton systems using energy for the degradation of dyes.
Hybrid system is the combination of extended Fenton systems. These classifications can also describe using primary
colors and its combinations as in Fig. 4. For example, sonoFig. 3 Classification of Fenton
process
Fenton and electro-Fenton processes are represented using

the primary colors green and red, respectively. Sono electroFenton process, which is a combination of sono-Fenton and
electro-Fenton processes, is represented by yellow color.
Yellow is the combination of green and red. This pictorial
representation is known as Fenton Circle. Exceptional
case in the Fenton circle is conventional Fenton process,
which is located at the center of the Fenton circle. It is
shown as white in Fenton circle, which is a combination
of all primary colors.
The Fenton reaction has a short reaction time among all
advanced oxidation processes and it has other important
advantages (Gotvajn and Zagorc-Konan 2005). The other
advantage is that no energy input is required to activate
H2O2 and therefore it offers a cost effective source of
hydroxyl radicals using easy-to-handle reagents (Bautista
et al. 2007). The major advantage of Fenton process is that
highly complicated apparatus and pressurized systems are
not required for the oxidation process (Kavitha and
Palanivelu 2004). Iron and H2O2 are economic and nontoxic; there is no mass transfer limitations due to its homogenous catalytic nature, there is no energy involved as catalyst,
and the process is easy to run and control (Gotvajn and
Zagorc-Konan 2005). Complete destruction of contaminants to carbon dioxide, water, and inorganic salts is achievable using Fenton process (Neyen and Baeyens 2003).
However, several limitations may hamper the conventional Fenton system into becoming commercial application
(Fu et al. 2010b). In many cases, since target contaminants
in real wastewater are at high levels, the treatment of which
correspondingly demands a proportional increase in the
starting concentrations of both Fenton reagents for a deep
mineralization of the compounds (Gu et al. 2012). This will
increase the operational cost of the system. Transport and
handling of commercial concentrated H2O2 is very difficult
(Fu et al. 2010b). Fentons oxidation may not be applicable
to alkaline solutions or sludge with strong buffering capacities (Dutta et al. 2001). Regeneration of catalyst is impossible in Fenton process and requires narrow range of pH
values for reaction (Dukkanc et al. 2010). Massive iron
sludge produced in the form of Fe(OH)3 requires proper
disposal, which needs additional investment for appropriate
design and operation of the whole system (Fu et al. 2010b).
To overcome the disadvantages of Fenton type processes,
heterogeneous Fenton and Fenton-like catalysts have recently
received much attention (Hassan and Hameed 2011;
Karthikeyan et al. 2011). It is well-accepted that the advantages of heterogeneous Fenton processes are complete mineralization of organic compounds at ambient temperature and
easy separation of the heterogeneous catalysts from the treated
wastewater (Rodriguez et al. 2010). In heterogeneous Fenton
process, iron salts are adsorbed onto the surface of supported
catalysts and in a suitable aqueous medium, the reduction
oxidation reactions between Fe2+/Fe3+ take place in the presence of hydrogen peroxide which promotes the formation of
reactive components such as (OH) and hydroperoxyl (OOH)
radicals (Daud and Hameed 2009; Hassan and Hameed 2011).
The radicals generated by the decomposition of hydrogen
peroxide can oxidize organic compounds adsorbed over the
catalyst or degrade soluble organic compounds in the vicinity
of active iron ions present at both the catalyst surface and in
the bulk liquid phase. Thus, the Fe3+/Fe2+ complex formed on
the surface of support can react with H2O2 thus allowing iron
ions to participate in the Fenton catalytic cycle (Sum et al.
2004; Hassan and Hameed 2011). Several materials such as
zeolite (Aleksi et al. 2010; Rodriguez et al. 2010; Idel-aouad
et al. 2011), carbon nanotubes (Rodriguez et al. 2010), carbon
nanofibers (Rodriguez et al. 2010), hydrotalcite (Rodriguez et
al. 2010), mesoporous silica (Rodriguez et al. 2010), silica
(Rodriguez et al. 2010), silica xerogel (Rodriguez et al. 2010),
sepiolite (Rodriguez et al. 2010), natural graphite tailing
(Cuiping et al. 2012), iron-impregnated activated carbon
(Rodriguez et al. 2010; Mesquita et al. 2012; Duarte et al.
2012, 2013), and natural vanadiumtitanium magnetite
(Liang et al. 2010) were used as heterogeneous Fenton catalysts for the dye removal from aqueous solutions.
Few study results of dye removal by Fenton reaction are
summarized in Table 5. From Table 5, it can be concluded that
very less working volume of the dye solution has been
2109
considered for the experimental work. Works on high volume

dye degradation are necessary for practical applications. The
cost estimation of Fenton process is also very essential. Most
of the works are carried out in batch mode. But Su et al. (2011)
studied the degradation of textile wastewater using fluidized
bed reactor with a working volume of 1.35 l (Fig. 5). PukdeeAsa et al. (2011) conducted homogeneous and heterogeneous
degradation of three azo dyes in fluidized bed reactor. Chicago
Sky Blue degradation through packed bed filled with ironimpregnated activated carbon was successfully carried out by
Mesquita et al. (2012). A pilot scale study for dye degradation
was carried out by Gu et al. (2012). Two staged Fenton rectors
of volume 2 m3 and oxidation time of 60 min was used by the
authors for treating real naphthalene dye intermediate
wastewater.
The dye degradation by Fenton process is affected by
several factors, like initial dye concentration, pH of the
solution, initial catalyst concentration, H2O2 concentration,
temperature, mixing rate, and inhibitors. The optimum values of some of these parameters are also given in Table 5.
The optimum pH of the solution was reported as 3 or near to
3 in all the cases. Hameed and Lee (2009) reported 38.29
93.22 % dye removal for a pH increase from 2.5 to 3.4. Fu et
al. ( 2010a, b) observed an increase in residual pH for Acid
Red 73 degradation. But Hameed and Lee (2009) reported,
contradicting to the above results that, optimal concentration
of H2O2 in most of the cases is in a range of 2 mM. The
optimal initial concentration of a catalyst varies with respect
to the nature of the catalyst.
Kinetic study is an important step in all the processes.
Wang (2008) reported an nth order kinetic equation for
Fenton oxidation as:
dC
kC n
dt
16
Where, C represents the dye concentration, n the order of

the reaction, k the reaction rate coefficient, and t the time.
From the above equation, the first- and second-order kinetic
equation can be derived as (Wang 2008; Emami et al. 2010)
C C0 ekt
C0
1 kC0 t
17
18
Wang (2008) proposed a combined first- and secondorder kinetics by combining the above two equations as:
C C10 ek1 t C20 ek2 t
19
where, C10 and C20 are the initial dye concentrations of two
independent first-order reactions and k1 and k 2 are the
reaction rate constants, respectively.
2110
Table 5 Recent studies of dye removal by Fenton process

Dye
Working
volume
Optimum factors
Major findings
Reference
Malachite green
200 mL
pH03.4, [Fe2+]00.1 mM,

temperature040 C
Hameed and Lee (2009)
Acridine orange
100 mL
pH03, [H2O2]02 mM,

[Fe2+]00.3 mM
Acid Red 1
200 mL
[Fe2+]01.0 wt.%,
[catalyst]05.0 g/l, pH03,
temperature050 C
100 % Removal for 20 mg/L solution after 50 min

Reduction in pH after reaction has been observed
After a period of 35 min there was no significant
increase in degradation efficiency % on increasing
the [H2O2]0
93.2 % Dye removal at optimum pH
98.4 % Dye removal after 60 min at 0.5 mM of Fe2+
Chloride ion had a negative impact on the decolorization
Degradation is much higher than TOC removal
99 % Decolorization was achieved within 180 min.
With continuous increasing of H2O2 concentration more
than 12 mM, the decolorization rate was reduced.
Acid Red 73
200 mL
[Fe0] 0 0.3 g/l, [H2O2] 0

2.5 mM, pH03
Methylene blue
50 mL
[LiFe(WO4)2]010 g/l,
pH03
Reactive Blue 19
50 mL
pH03, [Fe2+]01 mM,

[H2O2]02 mM
Methyl red
50 mL
pH03.2
Fig. 5 Fluidized bed reactor for

Fenton process (Su et al. 2011)
Decolorization efficiency increased with the initial

dye concentration
[Fe0] do not have any effect on dye removal after
30 min.
Increase in residual pH has been observed
Dye removal increases with mixing rate
95.2 % Removal after 90 min was obtained for
500 mg/L dye solution
Complete removal after 90 min for 500 mg/L dye
solution, [LiFe(WO4)2]010 g/L and [H2O2]0
0.10.2 M
Chloride and sulfate ions have a negative impact
on the decolorization of dyes by Fenton oxidation.
First- and second-order kinetic model fits the
experimental data better than the classical constructs.
As the dye concentration increased, dye removal
percentage decreased. But the initial rate of
degradation increased with dye concentration
The inhibition effects of ions is in the order of NO3
~SO42 <Cl <I <F <Br <CO32 <oxalate<EDTA~
Ophen
Chen et al. (2009a)
Hassan and Hameed

(2011)
Fu et al. (2010a, b)
Ji et al. (2011)
Emami et al. (2010)
Whebi et al. (2010)
2111
But, Emami et al. (2010) proposed a new combined firstand second-order kinetic model by assuming, c CC0t
Ct
C1
2
; k kapp k2 C1
. This equation is given below.

ln
C
1C

kt
20
Even though both of these authors proposed two different

equations, they reported that the combined first- and secondorder rate model fits the results best.
First-order rate constants for the degradation of dyes
reported by various authors are given in Table 6. The rate
constant depends mostly on the concentrations of the catalyst and dye. The rate constant decreases with increase in
dye concentration. For example, Lucas et al. (2007) reported
that the rate constant for a Reactive black 5 concentration of
100 mg/L is approximately double than that of the concentration of 200 mg/L, and 10 times higher than the Reactive
black 5 concentration of 500 mg/L. The rate of dye degradation also depends on the type of catalyst and dye. Acid
orange II degradation rate varies with the supporting catalyst
(Rodriguez et al. 2010). Swaminathan et al. (2003) reported
the order of degradation rate of dyes as: H acid>Red M5B>
Blue MR.
O2 2H 2e ! H2 O2
21
The reduction of ferric ions to ferrous ions may occur

simultaneously at the cathode as shown in Eq. (22) (Chen
and Lin 2009)
Fe3 e ! Fe2
22
In other respect, the water molecule may be oxidized into

oxygen at the anode (Chen and Lin 2009)
Electro-Fenton process
Recently, there is an increasing interest in the use of electrochemical methods such as anodic oxidation, indirect
electro-oxidation methods with H2O2 electrogeneration and
so-called electrochemical advanced oxidation processes
(EAOPs), which can produce HO as the main oxidizing
agent by different ways (Brillas et al. 2000; Kraft et al.
Table 6 First order kinetic rate

constants of dye degradation
2003). Environmental compatibility is the main advantage

of these methods. Their main reagent is an electron, which is
an inherently clean species whose energy can be carefully
controlled by means of an applied potential, thus avoiding
parallel reactions (Peralta-Hernndez et al. 2009). Among
these EAOPs, Fenton-based electrochemical method has
attracted much interest. This process consists of either adding Fe2+ or reducing Fe3+ electrochemically with the simultaneous production of H2O2 on the reduction of O2 on the
electrodes (Yuan et al. 2006). Hydrogen peroxide is electrogenerated in acidic solutions by two-electron reduction of
oxygen on the cathode surface according to the Eq. (21)
(Panizza and Cerisola 2009). This will create a platform for
further Fenton reactions. Fe2+ added to the system (normally
in the form of FeSO4) reacts with H2O2 to form strong HO
(Fenton reaction).
2H2 O ! O2 4H 4e
23
The above reaction will supply more O2 to the system.

This will create more H2O2 at cathode and consequently the
concentration of HO increase. High-oxygen overvoltage
anode can produce hydroxyl radicals from water oxidation
Dye and its concentration
Catalyst and its concentration
k (min1)
Reference
100 mg/L Reactive black 5

100 mg/L Acid Red 73
8.25 mg/L Fe2+

0.3 g/L zero-valent iron
1.225
0.1571
Lucas et al. (2007)

Fu et al. (2010a)
600 mg/L Methyl Orange

4104 Acridine orange
Orange II
50 mg/L Acid Red 14
Acid orange II
Acid orange II
Acid orange II
Acid orange II
Acid orange II
Acid orange II
Acid orange II
Acid orange II
Acid orange II
20 g/L Fe2O3SiO2 composite

2.75 mg/L Fe2+
5 mg/L zero-valent iron
15 g/L Fe(II)-Y Zeolite
2 g/L hydrotalcite
2 g/L zeolite USY
2 g/L Active carbon
2 g/L carbon nanofibers
2 g/L carbon nanotubes
2 g/L mesoporous silica
2 g/L silica
2 g/L silica xerogel
2 g/L sepiolite
3.36102
0.0113
0.0350
0.9051
0.0108
0.0120
0.1228
0.0358
0.0046
0.0068
0.0717
0.0131
0.0620
Panda et al. (2011)

Chen et al. (2009a)
Moon et al. (2011)
Idel-aouad et al. (2011)
Rodriguez et al. (2010)
2112
in electro-Fenton process as in Eq. (24) (Zhang et al.

2007b),
H2 O ! HO H e
24
The overall reactions that occur in the cathode and anode

of the electro-Fenton system are given in Eqs. (25) and (26),
respectively (Oturan 2000).
O2 3H 3e ! H2 O HO
25
H2 O $ 2H 0:5O2 2e
26
So the balanced overall reaction of electro-Fenton process results in the production of HO can be summarized as
in Eq. (27) (Oturan 2000).
0:5O2 H2 O ! 2HO
27
Besides HO, hydroperoxyl (HO2)-free species also can

be produced in an electro-Fenton system. This sequential
pathway consists of the following reactions (Eqs. (2831))
(Vatanpour et al. 2009):
HO H2 O2 ! H2 O
HO2
28
Fe3 HO2 ! Fe2 O2 H
29
Fe2 HO2 ! Fe3 HO

2
30
Fig. 6 Schematic diagram of major reactions occurs in an electroFenton system (Oturan 2000)
studies. It will increase the cost of the treatment. The optimum pH of the treatment is same as that of the conventional
Fenton process (pH03). But as exception from this, is the Fe
alginate gel bead (Rosales et al. 2012)-like materials, which
show a wide range of operational pH.
Sono-Fenton process
Fe
HO ! Fe
HO
31
The main mechanisms of electro-Fenton process are

shown in Fig. 6. The electro-Fenton process has several
advantages: H2O2 can be continuously generated on site
whenever needed, which eliminates the needs for acquisition, shipment, and storage; a dilute H2O2 solution is safe to
handle; the production process can be simply conducted at
ambient pressure and temperature; Fe2+ can be electrochemically regenerated at the cathode, which minimizes the
quantity of iron sludge (Qiang et al. 2002).
Some of the recent studies on dye removal by electroFenton process (EF) process were summarized in Table 7.
From Table 7, it can be concluded that EF is an efficient tool
for dye removal. Complete decolorization and significant
percentage of mineralization were reported in most of the
cases. The decolorization rate is very much higher than that
of mineralization. Some of the inhibition reactions will
reduces the mineralization rate (Oturan et al. 2008a). But
most of the studies used less working volume, even though
the work was carried out at higher initial dye concentration.
Also, Pt was used as the anode material in most of the
Sonochemical oxidation makes use of ultrasound that

results in the cavitation phenomenon, which is defined
as the formation, growth, and subsequent collapse of
microbubbles or cavities occurring in an extremely small
interval of time (microseconds), releasing large magnitudes of energy at millions of such locations in the
reactor (Gogate and Padit 2004). Acoustic cavitation
results in high temperature (in the range of 1,000
15,000 K) and pressure (in the range of 5005,000 bar)
in the reactor (Suslick 1990). This cavitation will result
in the production of hotspots, strong acoustic streaming
(liquid circulation), high shear stress near the bubble
wall, formation of microjets near the solid surface (due
to asymmetric collapse of bubbles), generation of highly
reactive free radicals and turbulence resulting in enhanced transport properties of the species (Mason and
Lorimer 2002; Leighton 1994; Young 1999).
Thermal dissociation of water and dissolved oxygen
molecules in the cavities will convert them into reactive
species such as OH, hydrogen atoms (H), O atoms and
hydroperoxyl radicals (OOH) in a cavitation bubble (Eqs.
Dye
Lissamine Green B
and Azure B
Cationic red X-GRL
Methyl red
Alizarin Red
Acid Yellow 36
Acid Orange 7
No.
carbon-felt-Pt gauze
BDD-Pt
Carbon PTFE/Pt
Graphite-PTFE- Pt
ACF or GraphiteRuO2/Ti mesh
Graphitegraphite
Electrodes
Table 7 Recent studies of dye removal by EF process
Undivided cell with a volume of 250 mL

was used for experiments; initial dye
concentration0120 mg/L
An open, undivided, and cylindrical glass
cell of 100 mL capacity was used for
experiments; electrode gap02.5 cm;
pH03; initial dye concentration060 mg/L
0.25 L undivided cylindrical glass cell
of diameter of 6 cm equipped with two
electrodes was used for experiments;
mixing rate0500 rpm; pH03; ionic
strength050 mM
Three electrode electrochemical cell;

electrode gap03 cm
An open, undivided glass vessel; working

volume01 L; solution temperature0271 C;
electrode gap05 cm.
Undivided two electrode system; working

volume00.15 L; electrode gap06 cm;
initial FeSO47H2O concentration0150 mg/L;
initial Fe alginate gel beads quantity08.69 g;
pH02; [Lissamine Green B]08.5 mg/L;
[Azure B]04.83 mg/L
Equipment details
Degradation kinetics and mineralization

efficiency were increased by increasing
the applied current and decreasing the
concentration of Fe3+ ions as catalyst
Complete decolorization at 3 min
Complete destruction of dye and its
aromatic byproducts achieved within 1 h
Quasi complete mineralization of dye was
achieved in 8 h
97.8 % decolorization was achieved at

[Fe2+]00.24 mmol/L, current density0
23 mA/cm2 and electrolysis time048 min
Fe alginate gel beads eliminate the negative

effect of iron sludge generated in classical
Fentons oxidation process at higher pH
values.
It is possible for Fe alginate gel beads to
operate in a wide range of solution pH
(from 2 to 8).
Fe alginate gel beads improved the dye
decolorization of electro-Fenton technique
ACF is more suitable than graphite as
cathode material.
The optimum concentration of Fe2+ was
5 mM with a decolorization efficiency
of 97.62 % after 180 min reaction time.
Cu2+ and Mn2+ were more effective than
Fe2+ in catalyzing the degradation of
the dye
NaCl is more efficient than Na2SO4 as
supporting electrolyte
In the NaCl medium, the removal of dye
seemed to be less sensitive to pH
variations compared with that of Na2SO4
medium
High electrolyte concentration promoted
dye removal 90 % COD removal after
4 h electrolysis
90% COD removal after 4hr electrolysis
Highlights of the work
zcan et al. (2009)
Cruz-Gonzlez et al. (2010)
Panizza and Cerisola (2009)
Ma and Zhou (2009)
Lei et al. (2010)
Rosales et al. (2012)
Reference

2113
Oturan et al. (2008a)

Total decolorization obtained after 22 min
Total mineralization obtained at 9 h.
Mineralization rate was decreased after
240 min due to inhibition reactions
Hammami et al. (2007)

98 % of TOC removal was obtained after 6 h
Ghoneim et al. (2011)
Malachite green
10
Carbon felt-Pt
Direct orange 61
9
Carbon felt-Pt
Sunset Yellow FCF

8
Reticulated vitreous
carbonplatinum gauze
An undivided glass electrochemical cell of 600-mL

volume was used for experiments; pH03;
working volume0450 mL; [Na2SO4]00.05 M;
[FeSO4]00.1 mM; mixing rate0400 rpm;
temperature0252 C
An undivided glass electrochemical cell of
250 mL volume was used for experiments;
pH03; cathode area060 cm2; anode area05.5 cm2
An open, cylindrical and undivided glass cell of 6 cm
diameter and 250 mL capacity was used for
experiments; anode area04.5 cm2; cathode
area060 cm2; initial dye concentration00.5 mM;
[Na2SO4]00.05 mM; [Fe3+]00.2 mM; pH03
Complete decolorization and 9095 %

mineralization of dyes
Complete decolorization and 8590 %
mineralization of real wastewater
containing Levafix Blue CA and Levafix
Red CA
Complete decolorization and approximately
97 % mineralization of the dye
Optimal operational parameters : 0.05 M
Na2SO4, pH 3 and 0.1 mM FeSO4
An undivided glass electrochemical cell
of 500 ml volume was used for experiments;
working volume0250 mL; pH03; initial
dye concentration0200 mg/L; [Fe2+]00.5 mM;
mixing rate0400 rpm
Levafix Blue CA and
Levafix Red CA
7
Reticulated vitreous
carbon-platinum gauze
Highlights of the work

Equipment details
Electrodes
Dye
No.
Table 7 (continued)
El-Desoky et al. (2010)
Reference
2114
(3236)) (Pang et al. 2011). These radicals will enhance the

degradation of pollutants under the ultrasound.
H2 O ! HO H
32
O2 ! 2O
33
HO O ! HO2
34
O H2 O ! 2HO
35
O2 H ! HO2
36
Combination of Fenton with sonolysis or sono-Fenton

processes can be applied to increase the mineralization of
the organic compounds (Ranjit et al. 2008). The oxidation
power of low concentration of iron in Fenton could be
significantly enhanced by ultrasonic irradiation (Sun et al.
2007). H2O2 production potential of ultrasonic irradiation is
another important advantage for sono-Fenton process
(zdemir et al. 2011). Thus, the H2O2 dosages necessary
for the reaction may also be reduced (zdemir et al. 2011).
Fe3+ to Fe2+ conversion rate in Fenton process also increases
in the presence of ultrasound (Mehrdad and Hashemzade
2010).
Schematic diagram of sono-Fenton process (SF) experimental setup for dye removal is shown in Fig. 7. Zhang et al.
(2009) used this type of reactor for the removal of Acid
Orange 7 from aqueous solution. H2O2 and Fe2+ were added
in required quantity to the pH adjusted dye solution. The
probe of sonicator was inserted 2 cm below the top of the
dye solution. The temperature of the dye was kept constant
by a water circulation around the reactor. The authors
reported that the presence of dissolved gas will enhance
color removal and the enhancement is more significant
when dissolved oxygen is present. But air supply is optional
for SF process. Also, decolorization rate increases with the
increase of hydrogen peroxide concentration and power
density, but decreases with the increase of initial pH value
(Zhang et al. 2009). Of the acid black 1 degradation,
98.83 % of was achieved by SF process (Sun et al. 2007).
Using SF process, Sundararaman et al. (2009) removed
82 % COD and 95 % of color from Reactive Yellow 16
solution. Similarly, 51 % of COD and 95 % of color removal
was reported by zdemir et al. (2011). The authors also
reported that the reaction occurred more rapidly by the
combination of Fenton process with ultrasound and the
decolorization improved even at low H2O2 dosages, compared to Fenton process. Effect of inorganic anions on dye
removal by SF process was investigated by Sun et al.
2115
Fig. 7 Experimental setup of

SF process (Zhang et al. 2005)
(2007). The authors listed the effect in decreasing order as:

SO32 >CH3COO >Cl >CO32 >HCO3 >SO42 >NO3.
Photo-Fenton process
Photo-Fenton process is a combination of UV radiation with
Fenton reagents, produces more hydroxyl radicals in comparison to the conventional Fentons reagent and promoting
the rates of degradation of organic pollutants (Ahmadi et al.
2008). Since the OH is the major oxidant of the photoFenton process, the dye removal behavior is highly related
with the OH formation (Kang et al. 2000). The use of UV
light in Fenton process will reduce the amount of sludge
produced (Poyatos et al. 2010). The conceptual redox reaction mechanism of photo-Fenton reaction is shown in Fig. 8.
The main advantage of photo-Fenton process is the possibility of using solar irradiation (i.e., sensitivity to 1
600 nm) which considerably reduces the costs of the process, especially when applying photo-Fenton for the treatment of high volumes of water (Petrovic et al. 2011). In
photo-Fenton process, in addition to Fenton reactions, the
formation of hydroxyl radical also occurred by the following reactions (Eqs. (37) and (38); Muruganandham and
Swaminathan 2004; Will et al. 2004; Tamimi et al. 2008).
Fe3 H2 O hv ! HO Fe2 H
37
H2 O2 hv ! 2HO l < 300 nm
38
At acidic pH (2.55), the main compounds absorbing

light in the photo-Fenton system are ferric ion complexes,
e.g., Fe(OH)2+ and Fe(RCO2)2+, which produce additional
Fe2+ (Eqs. (39) and (40)) (Sagawe et al. 2001). This will
enhance the further Fenton reactions.
FeOH2 hv ! Fe2 HO l < 450 nm
39
FeRCO2 2 hv ! Fe2 R CO2 l < 500 nm
40
The rate of dye removal by photo-Fenton process can

also be accelerated by the use of ferrioxalate as mediator
reaction. In acidic medium, ferrioxalate produces CO2 and
Fe2+ or Fe2+ complexes (Hatchard and Parker 1956). This
provides a continuous source of Fentons reagent as demonstrated by equations below (Carneiro et al. 2007)

3

2

FeC2 O4 3
hv ! FeC2 O4 2
C2 O4
41

3

2
C2 O
! FeC2 O4 2
C2 O2
4 FeC2 O4 3
4 2CO2
42
Fig. 8 Conceptual reaction pathways in photo-Fenton reaction (Liao et
al. 2004)

C2 O
4 O2 ! O2 2CO2
43
2116
It is possible to reduce the size of the photo-Fenton reactor

because the velocity of reaction in this case is very high
(Poyatos et al. 2010). However, an industrial application of
this technique requires a previous study with a pilot plant with
continuous addition of reagents as well as demands a high
degree of mineralization (Durn et al. 2011).
Schematic diagrams of UV-assisted photo-Fenton process (PF) process experimental setup used for dye removal
are shown in Fig. 9. Kusic et al. (2006) conducted experiments using water jacketed PF reactor (Fig. 9a) of capacity
800 mL, for the removal of Acid Orange 7. The UV lamp
was placed in a quartz tube and kept vertically in the middle
of the reactor. With use of water jacket, temperature in the
reactor was maintained near 25 C. The authors attained a
complete decolorization of dye using this reactor. Multilamp
photo reactor (Fig. 9b) containing eight numbers of mercury
lamps was used by Muruganandham and Swaminathan
(2004) and Selvam et al. (2007). The reaction chamber
contains specially designed reflectors made of highly polished aluminum and a built in cooling fan at the bottom.
Open borosilicate glass tube of 82 mL capacity, 36 cm
height, and 1.7 cm diameter was used as a reaction vessel.
Magnetic stirrer was used for the effective mixing of solution. Remazol Brilliant Orange 3R removal from aqueous
solution using heterogeneous PF process was studied by
Tekbas et al. (2008) using 500 mL capacity quartz photo
reactor as in Fig. 9c. Six lamps were used for the experiments. The authors reported that in comparison with homogeneous PF process, heterogeneous PF is found to be
superior because of the reusability of the catalyst. Also some
of the authors attained more than 90 % of dye removal
within 60 min. photo-Fenton process using 12 number of
Fig. 9 UV-assisted PF reactors;
1 power supply, 2 thermometer,
3 water outlet, 4 quartz jacket, 5
solution inlet, 6 magnetic
stirrer/stirring bar, 7 water inlet,
8 UV lamp, 9 glass water
jacketed reactor, 10 solution
outlet, 11 cooling fan, 12 air
inlet, 13 ice bath, 14 lamp
assembly, 15 quartz batch
reactor, 16 flow meter, 17
pump, 18 mixer (Kusic et al.
2006; Muruganandham and
Swaminathan 2004; Selvam et
al. 2007; Tekbas et al. 2008; Liu
et al. 2007)
mercury lamps (Fig. 9d) was carried out by Liu et al. (2007)
for the degradation of textile dyes. A variable speed mixer
was used for the effective mixing of the dye solution.
Schematic diagrams of solar-assisted PF process experimental setup used for dye removal are shown in Fig. 10.
Chen et al. (2009b) used double-glass cylindrical jacket
reactor (Fig. 10a) of 500 mL capacity for the heterogeneous
photo-Fenton degradation of reactive brilliant orange X-GN.
Halogen lamp was used as the light source. Under the
conditions of a reaction temperature of 30 C, pH 3.0,
4.9 mmol/L H2O2, 0.6 g/L of catalyst, after 140 min treatment under visible irradiation, 98.6 % decolorization, and
52.9 % TOC, removal was reported by Chen et al. (2009b).
Modified solar PF reactor (Fig. 10b) using multiple borosilicate glass trays was used by Ganesan and Thanasekaran
(2011) for the degradation of real textile wastewater. H2O2
added wastewater was pumped to the reactor using a peristaltic pump. The reactor was filled with steel scrap as
catalyst. The authors reported that compared to classical
solar PF reaction and solar PF reaction with alternative iron
sources, the new modified solar PF process has clear advantages. This process is relatively economical because the steel
scrap can be used as a discard material. The modified solar
PF process is easy to operate allowing it to retain the catalyst
in the process and thus the catalyst (steel scrap) can be used
repeatedly (Ganesan and Thanasekaran 2011). PF process
for dye removal using compound parabolic concentrator
(CPC) reactor (Fig. 10c) was studied by Monteagudo et al.
(2010), Durn et al. (2008), and Prato-Garcia and Buitrn
(2012). Durn et al. (2008) obtained 100 % decolorization,
82 % COD removal, and 23 % TOC removal using CPC
reactor.
2117
Fig. 10 Solar PF reactors (Chen et al. 2009a, b; Ganesan and Thanasekaran 2011; Prato-Garcia and Buitrn 2012)
Photo-electro Fenton process (PEF)

This advanced oxidation process system coupling the
advantages of electro-Fenton process and photo-Fenton process for the removal of organic pollutants. In this technique,
the solution is treated under EF conditions and simultaneously irradiated with UV light to accelerate the degradation rate of organics (Khataee et al. 2010a). Instead of UV,
solar light also had been used in PEF process by many
researchers. The synergistic degradation action of irradiation
can be associated with (1) a higher regeneration rate of Fe2+
and production of additional OH from photolysis of [Fe
(OH)]2+ through photo reduction reaction (Eq. (44)) and (2)
the photolysis of complexes of Fe3+ with generated carboxylic acids through reaction (Eq. (45)) (Brillas et al. 2009).
The main reactions in a PEF process are shown in Fig. 11.
FeOH2 hv ! Fe2 HO
44
FeOOCR2 hv ! Fe3 CO2 R
45
Typical schematic diagrams of a PEF reactors setup are

shown in Fig. 12. Khataee et al. (2010b) conducted experiments
at room temperature in an open, undivided and cylindrical glass
cell of 1,000 mL capacity and at a constant current (Fig. 12a).
Carbon nanotubepolytetrafluoroethylene and Pt sheet were
used as cathode and anode, respectively. The authors compared
the efficiencies of EF and PEF processes for the removal of
Basic Red 46 from aqueous solution and reported that color
removal was higher in the case of PEF. They observed 35 and
29.8 % decolorization within 1 h for PEF and EF, respectively.

Similarly, Wang et al. (2008) reported 6070 and 94 % TOC
removal for EF and PEF process respectively for the removal of
Acid Red 14. Peralta-Hernndez et al. (2008) used batch cum
recirculation PEF reactor (Fig. 12b) for removing Orange II azo
dye. They conducted the study using graphite electrodes. Total
volume of 400 mL at a recirculation flow rate of 100 mL/min
was used for their study. They compared the efficiency of EF
and PEF at Fe2+ concentrations of 0.2 and 0.5 mM. They
observed a best performance for PEF with an 80 % TOC
removal at 1 h for 0.2 mM Fe2+ concentration. But EF showed
a 63 % TOC removal for the same conditions. Salazar et al.
(2011) used solar PEF (SPEF) process (Fig. 12c) for the removal
Fig. 11 Generation of free hydroxyl radicals by means of EF and PEF

processes (Peralta-Hernndez et al. 2009)
2118
Fig. 12 Schematic diagram of a PEF batch reactor (Khataee et al. 2010b), b batch recycle reactor (Peralta-Hernndez et al. 2008), and c SPEF
reactor (Salazar et al. 2011)
Disperse Red 1 and Disperse Yellow 3 using BDD anode and

carbonPTFE cathode. A working volume of 2.5 L was used for
the study. This solution was circulated again using a peristaltic
pump. The solution was further passed through two heat
exchangers (to maintain the temperature at 35 C), an electrochemical reactor and solar photo reactor, and was finally
returned to the reservoir. They compared the efficiencies of EF
and SPEF and reported that SPEF is more potent than EF for the
dye removal, with higher current efficiency and lower energy
consumption. Total decolorization, complete dye removal, and
almost overall mineralization for both dye solutions using SPEF
were observed by the authors. Also, they reported that the
oxidizing power of SPEF was enhanced by the additional production of hydroxyl radicals from the photolysis of Fe(III)
hydrated species and the photodecomposition of Fe(III) complexes with intermediates by UV light of solar irradiation
(Salazar et al. 2011). Ruiz et al. (2011a, b) also reported the
same results for the degradation of Acid Yellow 36, Acid Red 88
and Acid Yellow 9.
So, many dye removal studies were conducted by combining PEF and photo catalysis. 91.6 % of Basic Red 46 decolorization at 60 min of PEF/TiO2 process was observed by
Zarei et al. (2010). Similarly, 93.7 % of Acid Red 17 decolorization was reported by Khataee et al. (2010b). Khataee et
al. (2010a) observed 93.8 % of decolorization efficiency at
60 min for PEF/Oxalate process. Similarly, higher dye removal was observed by Khataee and Zarei (2011a, b) by adding
ZnO nanoparticles in PEF process.
Sono-electro Fenton process
Sono-electro Fenton process (SEF) is the coupling process
of SF and EF. Its high performance arises from the
coupling between ultrasound irradiation and the in situ

electrogeneration of Fentons reagent (Oturan et al.
2008b). Also continuous cleaning and activation of electrodes will occur in the presence of ultrasound irradiation
(Li et al. 2010). The improvement of dye degradation rate
in SEF is due to (Brillas et al. 2009): (1) the enhancement
of the transfer of reactants Fe3+ and O2 towards the
cathode for the electrogeneration of Fe2+ and H2O2, as
well as the transfer of both products to the solution
increasing OH production by Fentons reaction and accelerating the destruction process; (2) the additional generation of OH by sonolysis; and (3) the pyrolysis of
organics due to cavitation promoted by ultrasound irradiation. Ultrasonic irradiation improved the H2O2 production rate of EF reactor (Li et al. 2010). Yasman et al.
(2004) reported that the efficiency of the SEF process is
tentatively much higher than the reference degradation
methods and the time required for full degradation is
considerably shorter. SEF process appeared to be very
efficient technique in terms of energy consumption and
decomposition rate of dyes (Siddique et al. 2011). So SEF
is a promising, efficient, and environmentally friendly
method for dye removal.
The schematic diagram of SEF experimental setup is
shown in Fig. 13. Li et al. (2010) used this type of reactor
for the removal of cationic red X-GRL from aqueous solution. An open, undivided glass vessel of size 13080
170 mm was used for the experiments. ACF and RuO2/Ti
mesh of size 10090 mm were used as cathode and anode,
respectively. The probe of transducer was inserted at a depth
of 20 mm from top of the solution. The authors reported that
compared with the electro-Fenton process, a higher decolorization efficiency, and TOC removal efficiency for the dye
Fig. 13 Schematic diagram of SEF experimental setup (modified from

Yasman et al. (2004))
solution can be achieved with ultrasonic irradiation. 85 % of

COD removal by SEF was reported by Martinez and Uribe
(2012). The authors also reported that SEF is twofold efficient than that of conventional Fenton process. Siddique et
al. (2011) used bath type ultrasonic instrument for the degradation Reactive blue 19 by SEF process. The authors
reported that 90 % color removal and a maximum of 56 %
TOC removal for 50 mg/L dye concentration of unhydrolyzed dye was achieved at an ultrasonic frequency of
80 kHz, pH of 8 after 120 min. Also, 81 % of TOC removal
was obtained for hydrolyzed dye.
Sono-photo-Fenton process
This process is the combination of SF and PF. This will
improve the degradation rate of dyes. The most common
problem in photo catalytic oxidation is the reduced efficiency of photo catalyst with continuous operation, possibly attributable to the adsorption of contaminants on the
2119
surface and blocking of the active sites (Gogate and

Pandit 2004). Ultrasound irradiation will rectify this problem by cleaning the catalyst surface during the operation
itself (Gogate and Pandit 2004). Studies reported that the
coupled Sono-photo-Fenton process (SPF) system appears
as a promising process for dye wastewater treatment
(Zhong et al. 2011).
Berberidou et al. (2007) studied the degradation of
Malachite green using a cylindrical 20060 mm Pyrex
glass vessel (Fig. 14a). A 350 mL of working volume was
used for the study. Horn-type ultrasound generator operating at a fixed frequency of 80 kHz was used as ultrasonic source. The bottom of the vessel was fitted with a
glass cylindrical tube housing the light source. Then,
appropriate amounts of hydrogen peroxide followed by
ferric ions were added in the acidified Malachite green
solution. After that, the solution was radiated with ultraviolet and ultrasound. The authors reported that when SPF
removed the dye within 1520 min; the increase in the
degradation rate from PF was only marginal. But the
photochemical decomposition rate of azure-B is markedly
increased in the presence of ultrasound (Vaishnave et al.
2012). The authors also reported complete mineralization
of azure-B at experimental conditions.
Acid Orange 7 removal using the mesoporous silica
supported nanosized iron oxide particles (Fe2O3/SBA-15)
as catalyst was studied by Zhong et al. (2011; Fig. 14b).
Used for the study was 200 mL of 100 mg/L dye solution.
Ultrasonic transducer was used as the ultrasonic source.
Temperature was controlled at 202 C during the ultrasound and UV irradiation. The authors reported that after
60 min reaction, 32.6 % COD removal was achieved
while the decolorization efficiency was as high as
84.9 % at optimal conditions as hydrogen peroxide concentration of 8 mmol/L, Fe2O3/SBA-15 addition of 0.3 g/
L, ultrasonic power of 80 W, and pH2.
Fig. 14 SPF reactors used for dye removal (Berberidou et al. 2007; Zhong et al. 2011)
2120
Factors affecting Fenton processes

pH
The actual dye wastewater has a wide range of initial pH
values and the solution pH is an important operating parameter affecting dye removal efficiency in Fenton processes (Fu
et al. 2010a). The most suitable range for Fenton processes is
pH3. This is due to the higher H2O2 production (Zhou et al.
2007). At pH3.5, the solubility equilibrium is controlled by
Fe3+ and Fe(OH)3 for Fe-H2O system. For the solution pH
higher than 3.5, this equilibrium is controlled only by Fe
(OH)3. Under this condition, the removal of pollutant is mainly due to coagulation or sorption process and not by Fenton
process. In contrary to this, if Fe3+ controls the equilibrium
and Fenton process is responsible for the pollutant removal at
pH<3.5. As the dye degradation proceeds, the formation of
organic acids in Fenton processes leads to a drop of the pH of
the solution (Idel-aouad et al. 2011). At low pH (pH<2.0), the
reaction of hydrogen peroxide with Fe2+ could be slowed
down because H2O2 can stay stable probably by solvating a
proton to form an oxonium ion (e.g., H3O2+) as presented by
Eq. (46) (Hassan and Hammed 2011). Also at low pH, the
excess H+ ions will react with hydroxyl radical as in Eq. (47)
(Tang and Huang 1996). In the case of pH>3, the oxidation
efficiency decreased rapidly due to the stability of H2O2 which
rapidly starts to decompose into molecular oxygen without the
formation of appreciable amounts of hydroxyl radicals
(Hassan and Hammed 2011). Also at higher pH, the reduction
of OH will occur due to the formation of ferric hydroxide
complexes (Ji et al. 2011). This was confirmed by Chen et al.
(2009a) at pH56 during Fenton process. But Idel-aouad et al.
(2011) reported that after 6 min, the decolorization efficiency
of heterogeneous Fenton system is independent of its initial
solution pH. The various forms of Fe3+ species in the solution
at different pH are given in Table 8. On the other hand, pH
readjustment usually done after Fentons treatment in order to
neutralize the pH and to remove iron from the oxidized
effluent may result in an additional coagulation and precipitation effect (ISO 8192 1986).
H2 O2 H ! H3 O
2
46
HO H e ! H2 O
47
Table 8 Various hydrated Fe3+ species in

solution as a function of
pH (Gomathi Devi et al.
2009; Neamtu et al.
2003)
Fe3+ species
Fe[H2O]63+
Fe[OH][H2O]52+
Fe[OH]2[H2O]4+
Fe[OH]3
pH range
12
23
34
710
For electro-Fenton oxidation process, the solution pH is

not only a crucial factor for Fenton oxidation efficiency, but
also a chief parameter for electrogeneration of H2O2 (Wang
et al. 2010). Normally, the change in pH of the solution in
EF process is very minimal. This is because the protons
consumed at the cathode are balanced by water oxidation
reaction at the anode (El-Desoky et al. 2010). At low pH,
two side reactions other than that in conventional Fenton
process also occurs at cathode (Eqs. (48) and (49)) (Wang et
al. 2010). These reactions also reduce the efficiency of EF
system at low pH.
H2 O2 2H 2e ! 2 H2 O
48
2H 2e ! H2
49
On the contrary, H2O2/UV process is independent of pH

condition, according to Eq. (38) (Kang et al. 2000). In other
words, the PF process can remove pollutants under both
acidic and neutral conditions (Kang et al. 2000). Chen and
Zhu (2007) reported that even up to initial an pH9.0, the
heterogeneous photo-Fenton process could proceed
effectively.
The optimum pH necessary for the removal of various
dyes via Fenton processes is given in Table 9. From Table 9,
the optimum pH for Fenton process is in between 3 and 3.5.
In the case EF, the optimum pH is 3 as expected earlier. PF
shows optimum pH range in between 2 and 3.5. But most of
the cases reported optimum as 3. Similarly, in the case of SF
and PEF, most of the researchers reported 3 as optimum pH
for dye removal. But Zhang et al. (2009) and Wang et al.
(2008) reported deviations from the above value. In contradictory to all, the optimum pH reported for SPF is 2 in all
the cases.
Concentration of H2O2
H2O2 plays the role of an oxidizing agent in Fenton
processes (Hassan and Hammed 2011). The existence of
an optimum H 2 O 2 concentration is well known in
Fentons oxidation (Dukkanc et al. 2010). Generally, the
dye removal increases with increase in H2O2 concentration until optimum H2O2 concentration. This is due to the
fact that at higher H2O2 concentration, enough hydroxyl
radicals are produced leading to almost complete decolorization (Panda et al. 2011). In contradiction to this, Alaton
and Teksoy (2007) reported that color removal will not
take place in the absence of H2O2 and decolorization
efficiency will not increase for H2O2 concentrations above
30 mM. But after a particular concentration of H2O2, the
removal of dye will decrease with increase in H2O2 concentration. H2O2 acts as a scavenger of highly potent HO
radicals to produce perhydroxyl radical at higher concentration (Eq. (12)), which is rather innocent towards redox
2121
Table 9 Optimum pH obtained for dye removal by various Fenton processes

No. Process
1
2
3
4
Dye
Optimum pH Results
Reference
3.5
3
3
3
87 % COD and 99 % color removal

24 % COD and 92 % Color removal
99 % color removal
99.7 % color removal
Meric et al. (2004)

Alaton and Teksoy (2007)
Hassan and Hammed (2011)
Ji et al. (2011)
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
Fenton
Reactive Black 5
Fenton
Acid dyebath effluent
Fenton
Acid Red 1
Heterogeneous
methylene blue
Fenton-like
Fenton
Acridine Orange Dye
Fenton
textile wastewater
EF
Real dyeing wastewater
EF
Levafix CA
EF
methyl red
PF
Reactive Red 120
PF
Reactive Yellow 84
Solar PF
Eosin Y
Heterogeneous PF Reactive brilliant orange X-GN
PF
Azure-B
SF
Acid Orange 7
SF
Acid black 1
SF
Acid Orange 7
PEF
Acid Red 14
PEF/ZnO
Basic Yellow 28
3
3.5
3
3
3
2
3
3.5
3
2.2
3
3
2
3.97
3

40 % COD removal
75 % COD removal
100 % color removal
80 % color removal
99 % color removal
99 % color removal
90 % color removal
Rate of dye removal is 2.98103 s1
91 % color removal
82 % color removal
97 % mineralization
97 % color removal
Chen et al. (2009a)

Kos et al. (2010)
Wang et al. (2010)
El-Desoky et al. (2010)
Zhou et al. (2007)
Neamtu et al. (2003)
Neamtu et al. (2003)
Zheng et al. (2007)
Chen et al. (2009b)
Vaishnave et al. (2012)
Zhang et al. (2005)
Sun et al. (2007)
Zhang et al. (2009)
Wang et al. (2008)
Iranifam et al. (2011)
20
21
22
PEF/ZnO
SPF
SPF
3
2
2.1
90 % color removal
Khataee and Zarei (2011a)
Zhong et al. (2011)
Rate of dye removal is 4.39103 s1 Vaishnave et al. (2012)
Direct Yellow 12
Acid Orange 7
Azure-B
act (Dutta et al. 2001). The hydroperoxyl radicals are

much less reactive and do not contribute to the oxidative
degradation of the organic substrate which takes place
only through the reaction with OH (Ji et al. 2011).
Also, so many other reactions of hydroperoxyl radicals
in Fenton system will occur as in Eqs. (1315). Therefore,
it is important to control the initial concentration of H2O2
since the high concentration would be adverse to the
decolorization of dye and would increase the cost of the
wastewater treatment (Hassan and Hammed 2011).
For the degradation of pollutants, H2O2 addition is not
required for EF related processes. This is mainly due to the
cathodic in situ generation of H2O2 keeps alive the H2O2
concentration throughout the EF process. But if the pollutant
strength of wastewater is very high, H2O2 addition to EF
system is required to reduce the electrolysis time. If H2O2 is
added to an EF system, it is known as Fered Fenton process.
The Fered-Fenton process, also called EF-Fere, consists of
the addition of either Fe2+ orFe3+ to the initial wastewater
along with the continuous injection of H2O2 during the
treatment in an undivided electrolytic cell (Brillas et al.
2009). Fered Fenton process increases the efficiency and
reduces the electrolysis time of EF process. Therefore, for
the mineralization of real high strength textile wastewater
Fered Fenton process is better than EF process.
Catalyst concentration
Catalyst (Fe2+/Fe3+/Fe0) is an important parameter affecting
the efficiency of all Fenton processes. Generally, dye removal
is directly proportional to the catalyst concentration. This is
mainly because, increase in the active sites to produce OH
promotes the degradation efficiency of pollutants (Ji et al.
2011). Also, the oxidizing power of hydrogen peroxide is
not enough to destroy dyestuffs in real dyeing wastewater in
the absence of ferrous ions (Wang et al. 2010). This was
experimentally proved by Lei et al. (2010) and Alaton and
Teksoy (2007). In heterogeneous Fenton system, increase in
catalyst dose increases the presence of active sites in catalyst
surface for H2O2 decomposition and dye adsorption (Idelaouad et al. 2011; Liang et al. 2010). In addition to above
reasons, in SF, SPF, and SEF processes, with the increase in
catalyst concentration a higher rate of cavities formation due
to the presence of gas nuclei in the pores of the catalyst will
occur (Kim et al. 2007). However, an excess of catalyst can
result in a decrease in overall number of photons that can
reach H2O2 molecules (Li et al. 2006). So, this will reduce the
concentration of hydroxyl radical in the solution and thus,
reduce the removal efficiency of the system.
But there exists an optimum catalyst concentration for
Fenton processes. Wang et al. (2010) reported an optimum
2122
Fe2+ concentration (2 mM) for EF process. This is due to, at

higher concentration, Fe2+ will react with OH and produce
Fe3+ as in Eq. (13) (Kang and Hwang 2000). Additionally,
the active sites on the cathode surface are presumably occupied by Fe3+, leading to the reduction of the number of
effective sites on the cathode surface for producing hydrogen peroxide (Wang et al. 2010). Panizza and Oturan (2011)
and Zhou et al. (2007) reported an optimum Fe2+ concentration of 0.2 mM for dye degradation by electro-Fenton
process. These optimum values indicate that the optimum
concentration of catalyst is depends more on experimental
conditions and nature of dye.
El-Desoky et al. (2010) reported an optimal Fe3+ concentration of 0.1 mM for Levafix CA removal by EF process.
This is because at higher concentration, Fe3+ ions could
react with H2O2 to produce hydroperoxyl radicals of less
oxidation capability (Eqs. (7) and (8)) resulting in decrease
in the rate of oxidation of the dye by the electro-generated
Fentons reagent (Neyens and Baeyens 2003; Benitez et al.
2001; Wang et al. 2005).
Gomathi Devi et al. (2011) reported that increase in catalyst
concentration in PF process not only decreases the percentage
of degradation, but also changes the final pH of the solution
from 3.5 to 4.4, leading to yellow coloration. This will increase
the turbidity of the dye solution, which will reduce the penetration of light through the solution. This will result in decrease
in efficiency of PF, PEF, and SPF processes at higher catalyst
concentration. A precipitation of iron oxyhydroxide was observed for Fe2+ concentrations in between 75 and100mg/L by
Gomathi Devi et al. (2011). Therefore, Fe2+ concentration
should be controlled properly to gain the desired decolorization during the reaction period (Zheng et al. 2007). But longer
time is required for dye degradation at lower catalyst concentration (Muruganandham and Swaminathan 2004).
Hassan and Hameed (2011) observed an induction period
in heterogeneous Fenton process. This is due to two reasons,
First, it is due to an activation process of surface iron species,
which are enabled to form complexes with the dyes before the
oxidation process can occur. Second, it is attributed to the time
needed to dissolve enough iron for homogeneous Fenton
reaction to take place (Hassan and Hameed 2011). In contradiction to this, Zhou et al. (2007) reported another two-step
process. The Fenton oxidation was very rapid at the initial

stage and this was followed by a much slower process.
Initial dye concentration
Initial concentration of dye is an important parameter in
practical applications (Fu et al. 2010a). The concentration
range of dyes usually found in the textile industry wastewaters
is in between 50 and 250 mg/L (Idel-aouad et al. 2011).
Generally, the degradation of dyes decreases as the initial
dye concentration increases because, at higher dye concentration, the generation of OH radicals on the surface of the
catalyst is reduced since the active sites may be occupied by
dye ions and because the number of dye molecules is increased but not the OH radical molecules number (Idel-aouad
et al. 2011). In addition, the intermediate products formed
during dye-oxidation probably compete with the dye molecules for the available Fe2+ active sites (Panda et al. 2011).
Thus, the reaction between the catalyst and the H2O2 was
inhibited, thereby decreased the degradation efficiency (Ji et
al. 2011). Contradictory to this, Hassan and Hameed (2011)
reported that the dye removal increases with increasing initial
dye concentration. The authors gave reason for this phenomenon based on collision theory. That is, by increasing the
quantity of dyes molecules per volume unit the probability
of collision between organic matter and oxidizing species is
logically enhanced, thereby leading to an increase in the
decolorization efficiency (Kitis and Kaplan 2007).
Temperature
Temperature is an important parameter influencing the degradation of dyes by Fenton processes. There exists an optimum
temperature for Fenton processes as in the case of other
factors. Too low and too high temperatures negatively impact
the process efficiency (Nidheesh and Gandhimathi 2012). But
textile effluents have unusually high temperature compared to
most of the industrial wastewaters and during the dyeing
process, rinse water temperature can increase up to 90 C
(Lin and Peng 1994). The increase in degradation of dyes
with increase in temperature is due to the increase of the
reaction rate of the OH formation (Idel-aouad et al. 2011).
Table 10 Optimum temperature obtained for dye removal by Fenton processes

No Process
Dye
Fenton
Reactive Black 5
2
3
4
5
Fenton Like
Methylene Blue
Heterogeneous Fenton Acid Red 14
EF
Alizarin red
Heterogeneous PF
Reactive brilliant orange X-GN
Optimum temperature (C) Removal efficiency (%) Reference

40
26
60
35
40
COD079
Color099
Color 100
Color099
COD 90
Color098.4
Meric et al. (2004)

Dutta et al. (2001)
Idel-aouad et al. (2011)
Panizza and Cerisola (2009)
Chen et al. (2009b)
2123
The rate constant increment is attributed to increased corrosion rates and collisions between the dye and hydroxyl radicals (Fu et al. 2010a, b). But at higher temperatures, the
removal of dyes by Fenton processes decreases. This is due
to the thermal decomposition of the hydrogen peroxide
resulted in the reduction of its effective concentration towards
making hydroxyl radicals, and this was possibly the reason
behind lower conversion of the dye at higher reaction temperatures (Dutta et al. 2001). The thermal decomposition of H2O2
is given in Eq. (50) (Panizza and Cerisola 2009). Also, destabilization of flocs resulted in increased ferrous ions which
scavenged OH radicals during Fentons reactions (Benitez et
al. 2001). But Wang et al. (2010) reported an opposing result
to this. The authors reported that the COD removal by EF
process is decreases with increase in temperature. This negative effect of temperature on the COD removal percentage
can be explained by the lower concentration of dissolved
oxygen and the self-decomposition of hydrogen peroxide at
higher temperatures. Namely, the concentration of hydrogen
peroxide decreased as the temperature increased because increasing temperatures can decrease oxygen solubility in the
wastewater. In addition, the rate of self decomposition of the
hydrogen peroxide to water and oxygen increased with the
temperature (Wang et al. 2010). This negative effect was
experimentally proved by zcan et al. (2008). Higher temperature also affects the efficiency of sono-related Fenton processes. Because in the process of ultrasound, generally, higher
temperatures are likely to facilitate bubble formation due to an
increase in the equilibrium vapor pressure; nevertheless, this
beneficial effect is compensated by the fact that bubbles
contain more vapor which cushions bubble implosion and
consequently reduces the maximum temperature obtained
during bubble collapse (Psillakis et al. 2004). The optimum
temperatures and corresponding dye removal efficiencies
reported by various researchers are given in Table 10.
H2 O2 ! H2 O 0:5O2
50
Fenton in future
Currently, Fenton and related processes are well established.
So many works on theoretical and application-oriented
Fenton-related processes have been applied. Dyes were
successfully mineralized using all Fenton-related processes.
But most of the works carried out in batch mode. Apart from
this, developments of successful Fenton pilot plants capable
of treating large quantity of dye effluents are required.
Fluidized bed reactor is one of the most suitable reactors
for Fenton, PF, SF, and SPF processes. Sono-related Fenton
processes will work very well in fluidized bed reactors.
Because the efficiency of ultrasound-related process will
enhance with increase in the fluid depth, there may be a
chance for the production of Ferrate ions in all the Fenton

processes. Ferrate ions are the iron ions in higher than 3+
oxidation states. If the production of ferrate ions is there in
Fenton system, the effect of these ions on the efficiency of
the Fenton system should be evaluated. Experiments on EFrelated Fenton processes working in AC power system
should be a good trend in this field. Because, EF-related
Fenton processes working in DC power have reduction in
efficiency due to the settlement of iron ions on cathode. The
usage of AC instead of DC will rectify this problem.
Combination of all Fenton processes, i.e., sono-photo
electro-Fenton process is also enhances the efficiency of
Fenton system. More works on heterogeneous Fenton and
Fenton-like reactions are also required for selecting best
method for dye degradation.
Conclusions
Dyes are one of the major pollutants threaten to our environment. It is very harmful to all the species on earth and it
will destroy the ecosystem if it is not removed before entering into the aquatic system. Fenton processes are the one of
the powerful tool for removing dyes from aqueous solution.
Total mineralization of dyes has been achieved in many
processes. Different types of reactors have been used for
this purpose. All these processes very much depends on pH,
catalyst concentration, H2O2 concentration, initial dye concentration, and temperature. There exists an optimal value
for pH, catalyst concentration, H2O2 concentration, and
temperature in all the process. Hence, Fenton processes are
one of the best methods for dye degradation.
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