A REVIEW ON THE PHOTOCATALYTIC REMADIATION OF DYES IN WASTEWATER FOR THE PREVENSION OF ENVIRONMENT

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A REVIEW ON THE PHOTOCATALYTIC
REMADIATION OF DYES IN WASTEWATER
FOR THE PREVENSION OF ENVIRONMENT
*1Azad kumar, 2Shiv Mahendra Singh, 3Reena Verma, 4Mohiuddin Ansari
1, 4Department of Chemistry, M.L.K. (P.G.) College Balrampur, India
2Department of Botany, M.L.K. (P.G.) College Balrampur, India
3Department of Chemistry, Agra College Agra, India
Abstract
Textile dyes have a dangerous impact on the lives of marine animals and humans, when found in contaminated water. The
advancement of pollution control has been influenced by progress in nanoscience and technology. Several approaches and
nanomaterials were used effectively in recent times for the treatment of tint-contaminated polluted water. The Nanomaterials with
small sizes offer new possibilities to operate the technologies for the elimination of dyes from contaminated wastewater. The
potential application of Photo catalyst nanomaterials to the abatement of textile wastewater was investigated by the several
researchers.
Keyword: Photodegradation, Photocatalyst, Photocatalysis, dye, environment
1. Introduction
In various industries, teinting and textiles, teinting plays a major role. More than 100,000 commonly produced synthetic dyes are
some of the most commonly used in these industries. Typically, these dyes come from two main sources: coal tar and crude oil
intermediates, which produce over 7 to 105 tons per year. Every year around 15 percent of these not biodegradable textile dyes
(one thousand tonnes) are dumped into natural rivers and water bodies via textile industrial wastewaters. In dyeing process plants,
an average of 120-280 L of water is usually consumed for each kilogram of cloth [1-2]. Konstantinou and Albanis [3] have
confirmed that industrial dye materials and textile dyes are one of the largest classes of organic compounds hazardous. According
to World Bank figures, the significant determinants to textile and colouring industries are almost 17-20 percent water pollution.
According to Kant's report [4], 72 chemicals were released only through textile dyeing and nearly 30 of those chemicals were not
treated from major toxic wastewater chemicals.
Mostly the azo dyes and direct dyes show the very high toxicity. The acid dyes and reactive dyes are soluble in water which is
very bright coloured dyes and the most problematic dyes and it is not eliminate from water easily. The conventional methods and
aerobic treatment systems are ineffective for the elimination of these dyes from the waste water [5]. During the dyeing process,
the reactive dyes are absorbed on the surface of materials in the smallest quantity, so the residual dyes is released directly into the
waste water. Leena and Raj [6] reported that reactive dye wastewater has the potential to remain stable and unchanged in the
ecosystem for many years, i.e. hydrolysed reactive blue does have a half-life of approximately 46 years. Dispersed dyes should
not ionize in aqueous media to improve their ability to bioaccumulate in aquatic living organisms. Concerns concerning dye
effluents currently exist because many dyes are synthesized with known carcinogenic chemicals, such as aromatic and benzidine
agents [7].
The dye reduction in the gut ecosystem that led to the formation of toxic amines has been demonstrated by Chung et al [8]. In
addition, Azo dyes are quickly reduced to anaerobic treatment conditions to aromatic amines potentially toxic.
In addition to dye contamination, the manufacture of drying as well as scouring agents often results in pre-dying treatment in the
industrial processes such as mercerization, scouring, scale and bleaching [9]. However, the removal of dye from waste water is the
most complicated and complex process of all the above mentioned issues. Dyes are typically the first pollutant to be detected in
industrial wastewater, even in minute quantities, owing to its high visibility (<1ppm) [10-11]. These color waste water supplies
are a significant source of both eutrophication and non-esthetic emissions which can generate harmful by-products in the
wastewater environment by further degradation, oxygenation or other chemical reactions. It apart from the toxic effects of dyes in

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waste water sources, dyes can contribute to decreased light penetration, thereby rendering oxygen unappropriated for
biodegradation of microorganisms in water [12-14]. Besides textile, the textiles sector also leads to the presence of dyes in waste
water, such as the leather tanning sector, paper industry, food factories, hair colorants, photo electrochemicals cells and light
harvesters. Most dyes are poisonous and carcinogens in diverse industries, and thus pose significant threats for both the human
and aquatic environments. Consequently, the environmental effect of dyes has been widely researched in the past few years [15-
17]. The present article provides a review of recent changes to the oxidation of different dyes by the use of Tania based
nanocomposites as a probable photocatalyst.
2. Dye classification
Dyes typically have several structural varieties which are very difficult to classify thoroughly with regard to one factor and are not
useful in functional terms. However, 30 dyes are typically broken down into various groups and classes according to their source,
general coloration structure and fiber type, as seen in Figure 1.
Fig. 1. Classification of dyes on the basis of nature and synthesis.
Azo dyes are the largest category of colorants within the major groups of dyes, with over 50 per cent of azo dyes used throughout
industries [18]. Double bonding of azo-dyes (–N=N) is defined when at least one atom is attachable to an aromatic group Azo
Dyes (rings of naphthalene or benzene). In addition, owing to various functional groups of carboxyl, hydroxyl, amino and
sulfoxyl, which have amphoteric properties? Azo dyes can be anionic (acidic group deprotonation), cationic (amino group
protonation) or non-ionic based on the medium's pH [19]. Azo dyes are the most notable: acid dyes, base dyes, direct dyes,
dispersive dyes, reactive dyes, vat dyes, and sulphur dyes. The most important azo dyes are: dispersive dyes (non-ionic dyes) [20].
Dye can be classified as anionic, non-ionic and cationic dyes depending on general structure. Direct, acidic and reactive colors
primarily produce anionic dyes. Main non-ionic dyes are; dispersed dyes which do not ionizes in the aquaous environment and the
major cationic dyes contain simple and dispersed dyes. Acidic dyes are so called when commonly found in inorganic or organic
acid solutions on nitrogen fibers or fabrics [21-22]. Basic dyes give solution cations that are commonly used with acrylic and
modacrylic fibres. In the aqueous bath, direct dyes are added with ionic salts and electrolytes, which bind the electrostatic forces
with fibers and fabrics. Disperse dyes have poor water solubility, but, by shaping dispersed fragments, they can interfere with
polyester chains. The washing speed with dispersed teint varies depending on the kind of fiber used to teint, i.e. poor acetate
content and excellent polyester content. Reactive dyes are mostly used on celluloses but also on protein fibers and nylon, and they
form a covalent bond with the related textile feature. Sulphur fibers are used to create dark colors of marine, dark and brown on
cellulosic fibres. They have excellent fastness in most areas, but fades off when exposed to chlorine [23-25].

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3. Photocatalytic degradation of dyes
The conventionally chemical treatment such as activated carbon, adsorption, reverse osmosis, ultrafiltration can be used for dye
removal [26], biological [27] and adsorption [28] treatments have been applied for the removal of dyes from industrial waste
water but these processes are insufficient in removing dye contaminants.
Photodegradations is an innovative method of oxidation that provides multiple benefits over conventional wastewater
treatments such as chemical oxidation, activated carbon adsorption [29], biodegradation and microbiological or enzyme
decomposition therapy. Photocatalytic processes in this respect are useful for the elimination of toxins, even though low in
industrial wastewater concentration [30]. In addition, organic contaminants undertake complete oxidation within a few hours, also
in ppb level, without formation of highly active and secondary harmful products that can be used in special configuration reactor
systems [31].
Heterogeneous photocatalysis have been proved that it is very effective process for degrading environmental and aquatic
organic contaminants. In the presence of a photocatalyst device, sunlight tends to speed up the removal of organic contaminants
and the oxidation of highly active substances into less toxic biodegradable products like H2O, Ammonia, and CO2 etc.
Photocatalysis depends on the type of radiation used, i.e. pure TiO2, acts as good photocatalyst in presence of UV light (370–415
nm) [32–33] but it can be change the by doping and cooping and also designing the catalyst for the degradation of toxic
compounds. The visible light can be used, but the non-disposition of an appropriate catalyst and other contributor known as a less
effective irradiation operation. Dye molecules also have confounding reactions to TiO2 photocatalysts, and could be classified into
the following categories according to the photocatalysis products [34-35].
a) Photodecolourizations require basic photooxidation or photoreduction in which the dyes will either revert back or back
oxidization in the original form.
(b) Dye decomposition to form some stable materials in presence of photocatalyst. It is the most common term for the treatment of
toxic compounds photocatalytic decoloration.
c) Photomineralization is the process of complete decomposition of organic hazardous compound into CO2, H2O, N2, NO3, NO2,
etc.). Mineralization should be the target of ideal photocatalysis.
d) Photodecomposition could vary depending on the researchers, involving both photodegradation and mineralization. Although,
decolourization usually happens. The use of these terminologies as specifically as possible would be considered below in the
analysis. In general, CO2 formation and inorganic ions is determined [36] in order to measure the degree of color loss obtained
during therapy [37]. the precise concentration of these ions in actual wastewaters cannot however be determined. In these cases,
the degree of dye mineralization is measured by considering total organic carbon (TOC) and calculating the chemical oxygen
demand (COD) or biology oxygen demand (BOD). In general, at lower dye concentration and for compounds which do not form
stable intermediates, complete mineralization proceed with similar half-lives for parent dye and the intermediates but at higher
concentration intermediates mineralization is slower than the degradation of the parent dye [38]. To date most azo dyes have been
found to undergo complete mineralization except triazine containing dyes. The later does not undergo complete mineralization
due to high stability of triazine nucleus and the stable cyanuric acid intermediates. However, fortunately these intermediates are
not toxic. Usually COD or TOC values decrease with irradiation time whereas the amount of NH4+, Cl−, SO42− and NO3− ions
increase. For chlorinated dye molecules, Cl− ions are the first of the ions which appear during photocatalytic degradation. This
could be interesting in photocatalytic biological treatment which is generally not efficient for chlorinated compounds [39-40].
4. TiO2 as photocatalyst for dye treatment
Due to its high oxidation performance, non-toxicity, high photostability, chemical inertness and ecological friendliness,
titanium dioxide is a universally accepted photocatalyst [41]. It is a broad bandwidth semiconductor (~3.2 eV) which mineralizes
a wide variety of chemical contaminants in presence of UV radiation, such as herbicides, colorants, toxins, phenolic compounds,
tetracyclines, sulfamethazines, and others [42]. In photocatalytic processes the energy photon is absorbed by the TiO2, the holes
(h+) formed in the valence band and electrons (e−) in the conductive band, similarly or greater energy needed for the conduction

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than the band gap (3.2 eV). The absorb photon diffuses to the surface of TiO2 and participates in redox reactions of the adsorbed
substrates [43].
The TiO2 is a semi-conductor with wide band gap and hence ideal for photodegradation in presence of UV light. Meanwhile only
5% UV radiation in solar light, TiO2 is therefore not a good solar photocatalyst. Another disadvantage of TiO2 mediated
photocatalysis is an extra electron hole recombination. The Doping of metal ions in TiO2 host could to some degree overcome the
above disadvantages [44-45].
5. Basic principles and mechanism of photocatalysis for dye degradation
5.1. Indirect dye degradation mechanism
The indirect heterogeneous photocatalytic oxidation mechanism using semiconducting materials can be summarized as follows.
(a). Photoexcitation
Photocatalytic reaction is initiated when a photoelectron is promoted from the filled valence band of a semiconductor
photocatalyst i.e. TiO2 to the empty conduction band as a result of irradiation. The absorbed photon has energy (hυ) either equal or
greater than the band gap of the semiconductor photocatalyst [46].
The excitation process leaves behind a hole in the valence band (h+ vb). Thus as a net result, electron and hole pair (e−/h+) is
generated as indicated by the Equation 1 below.
TiO2 + hʋ → TiO2 [h+ (VB) + e- (CB)] (1)
Fig.2. Mechanism of formation of electron (in Conduction Band) and hole (in Valence band) in Titania.
(b). Ionization of water
The photogenerated holes at the valence band then react with water to produce OH• radical.
H2O (Ads) + h+ (VB) → OH• (Ads) + H+ (Ads) (2)
The HO• radical formed on the irradiated semiconductor surface are extremely powerful oxidizing agent. It attacks adsorbed
organic molecules or those that are very close to the catalyst surface non-selectively, causing them to mineralize to an extent
depending upon their structure and stability level. It does not only easily attack organic pollutants but can also attack
microorganisms for their enhanced decontamination [47].
(c). Oxygen ionosorption
While the photogenerated hole (h+ VB ) reacts with surface bound water or OH- to produce the hydroxyl radical, electron in the
conduction (e- CB) is taken up by the oxygen in order to generate anionic superoxide radical (O2•).
O2 + e- (CB) → O2-•(ads) (3)
This superoxide ion may not only take part in the further oxidation process but also prevents the electron-hole recombination, thus
maintaining electron neutrality within the TiO2 molecule [48].
(d). Protonation of superoxide
The superoxide (O2−•) produced gets protonated forming hydroperoxyl radical (HO2•) and then subsequently H2O2 which further
dissociates into highly reactive hydroxyl radicals (OH•).

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O2−• (Ads) + H+ ⇄ HOO• (Ads) (4)
2 HOO• (Ads) → H2O2 + O2 (5)
H2O2→ 2OH•(Ads) (6)
Dye + OH• → CO2 + H2O + (Dye Intermediate) (7)
Dye + h+ (VB) → Oxidation Products (8)
Dye + e- (CB) → Reduction products (9)
Both oxidation and reduction processes commonly take place on the surface of the photoexcited semiconductor photocatalyst. The
complete process has been represented by the Figure 3 [49].
Fig.3. Oxidation and reduction processes commonly take place on the surface of the photoexcited semiconductor photocatalyst.
5.2. Direct mechanism for dye degradation
Owing to their ability to easily absorb some of visible light, another mechanism of photocatalytic dye degradation can also occur
under visible light. This mechanism involves the dye excitation under visible light photon (λ 5 > 400 nm) from the ground state
(Dye) to the triplet excited state (Dye*). This excited state dye species is further converted into a semi-oxidized radial cation
(Dye•+) by an electron injection into the conduction band of TiO2. Due to reaction between these trapped electrons and dissolved
oxygen in the system superoxide radical anions (O2•−) are formed which in turn result into hydroxyl radicals (OH•) formation [50].
These OH• radicals are mainly responsible for the oxidation of the organic compounds represented by Figure 4 below.
Fig.4. Excitation of dye molecule with photocatalyst.
6. Photo-degradation of dyes
6.1. Photo-degradation of Eriochrome Black-T
The photocatalytic degradation of EBT has been studied in the presence of TiO2 nanoparticles at Different concentration
of dye which was prepared in 3:2 (V/V) ratio of water and alcohol. The photodegradation of EBT are shown in Fig.5. As obvious
from the graph, the % removal of dye decreases with increase in concentration. [51]. When the concentration of solution
increased, the number of dye molecule also increased therefore the effective number of photon penetrating the dye reached at the
catalyst surface also reduced, owing to hindrance in the path of light, thereby reducing the reactive hydroxyl and superoxide
radicals and decreasing the % degradation [52]. The Degradation rate of EBT was found to increase by increasing the dose of
photocatalyst from 50 mg/L to 200mg/L. this is due to the no active site increased. The results (Fig.5) show that degradation of
dye is highest in acidic medium (at pH = 2) while it decrease with increase in pH and ultimately becomes constant after pH 7. This
implies that acidic condition is favourable for formation of the reactive intermediate hydroxyl radicals. This further helps in
enhancing the reaction rate.

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-20 0 20 40 60 80 100 120 140 160 180 200
-10
0
10
20
30
40
50
60
70
80
90
33.3x10-5M
25.0x10-5M
20.0x10-5M
16.6x10-5M
% Photodegradation
Time (min)
(a)
1 2 3 4 5 6 7 8 9 10
10
20
30
40
50
60
70
80
90
100
33.3 x 10-5 M
25.0 x 10-5 M
20.0 x 10-5 M
16.6 x 10-5 M
% Photodegradation
pH of reaction mixture
(a)
-20 0 20 40 60 80 100 120 140 160 180 200
0
20
40
60
80
100
% Photodegradation
Reaction Time (min)
200 mg/L
100 mg/L
50 mg/L
(a)
Fig.5. Photo-degradation of Eriochrome Black-T at various condition
6.2. Photodegradation of Methyl Green Dye
The residual concentration of dye in the reaction mixture was measured spectrophotometrically. The results obtained for the
degradation of Methyl Green is shown in Fig. In presence of Titania the photodegradation of Methyl green dye was found 18%
and 3% at 25 and 100 ppm concentration of dye solution. But in presence of Ni0.10:La0.05:TiO2 the photodegradation was found
98.6 % and 56% at 25 ppm and 100ppm concentration of dye. With increasing concentration of Methyl Green the rate of
degradation was found to decrease. The photodegradation of Methyl Green was increased with increase irradiation time. The
photodegradation was found maximum in 50 min irradiation of visible light. Fig. 6 shows the effect of irradiation time on
photocatalytic degradation of Methyl Green. This is because of the interaction of dye molecule with the surface of photocatalyst.
The time of irradiation increase, the interaction of methyl green dye molecule increased with the surface of photocatalyst.
Therefore the photodegradation efficiency of photocatalyst was increased. The maximum photodegradation of Methyl Green dye
was found 17% and 88% in presence of TiO2 and Ni0.10:La0.05:TiO2 at neutral medium or 7 pH of solution. The reaction of
photodegradation was found low rates at acidic and basic ranges of pH. While at pH 7 or neutral medium, the photodegradation
was found maximum [53-54].
25 50 75 100
0
20
40
60
80
100 (a)
(b)
% Photodegradation
Concentration of dye (ppm)
300 400 500 600 700 800
0
1
2
3
4
5
Absorbance
Wavelength (nm)
10 min
50 min
Ni0.10:La0.05:TiO2
3 4 5 6 7 8 9 10
0
10
20
30
40
50
60
70
80
90 (a)
(b)
% Photodegradation
pH of solution
Fig.6. Photo-degradation of Methyl Green dye at various conditions
6.3. Photodegradation of Victoria Blue Dye
The photodegradation of cationic dyes (Victoria blue) was carried out under varying pH conditions from (2 to 9), by the
addition of H2SO4 and NaOH, keeping other parameters constant (concentration = 50 ppm, the amount of catalysts = 800 mg/L
and irradiation time = 120 min). The results show that degradation of dye Victoria blue is highest in basic medium (at pH = 10)
shown in Fig. 7. Under acidic conditions, it was found difficult to adsorb the cationic VB dye onto the TiO2 surface. The active
•OH radicals, formed in low concentrations, and hence the photodegradation process of VB remained slow. With higher pH
values, the formation of active •OH species is favoured, due to not only improved transfer of holes to the adsorbed hydroxyls, but
also electrostatic abstractive effects between the negatively charged TiO2 particles and the operating cationic dyes. Although the
VB dye can adsorb onto the TiO2 surface to some extent in alkaline media, when the pH value is too high (pH 11), the VB dye
molecules will change to a leuco-compound. Our results indicate that the TiO2 surface is negatively charged, and the VB adsorbs
onto the TiO2 surface through the positive ammonium groups. This is characteristic of heterogeneous photocatalysts, and the
results are in agreement with the earlier studies [55-56].

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2 4 6 8 10 12
0
10
20
30
40
50
60
70
80
90
100
(a)
(b)
(c)
Victoria Blue
% Degradation Efficiency
pH of the solution
30 60 90 120 150 180
0
10
20
30
40
50
60
70
80
90
100
Victoria Blue
(a)
(b)
(c)
% Degradation Efficiency
Irradiation Time (min)
0100 200 300 400 500 600 700 800
0
10
20
30
40
50
60
70
80
90
100
(a)
(b)
(c)
Victoria Blue
% Degradation Efficiency
Amount of Photocatalyst mg/L
Fig.7. Photodegradation of Victoria Blue Dye in presence of (a) TiO2 (b) TiO2/PPy and (c) TiO2/PPy/GO at various conditions.
6.4. Photodegradation of Rose Bengal Dye
The effect of the irradiation time on photodegradation of RB dye has been studied in presence of TiO2, TiO2/PAni and
TiO2/PAni/GO nanocomposite. The UV spectrum has been taken for TiO2, TiO2/PAni and TiO2/PAni/GO nanocomposite at
different irradiation time (30, 60, 90, 120 and 180 min) (Fig. 8). It is interesting to remark that the absorbance decreases with
increase of time with photocatalyst. At 120 minutes the photodegradation efficiency observed was 14, 93 and 97 % for TiO2,
TiO2/PAni and TiO2/PAni/GO nanocomposite respectively. The Titania was showed very low photodegradation efficiency in
visible light. This is due to high band gap energy (3.2 eV) which is not active in visible light region. Whereas TiO2/PAni and
TiO2/PAni/GO nanocomposite show very high photodegradation efficiency 93 and 97 %, this is due to the formation of sub band
in Titania. The coating of PAni and GO decrease the band gap energy of Titania and Titania becomes active in visible light [57].
The prominent degradation of Rose Bengal was found in 120 min study in the presence of TiO2/PAni/GO in comparison to the
prepared TiO2 and TiO2/PAni. This is due to the coating of polyaniline of Titania surface which provide the electron from the
HOMO to LUMO. The electrons of HOMO get excited into LUMO which is further jump into the conduction band of Titania.
20 40 60 80 100 120 140 160
10
20
30
40
50
60
70
80
90
100 Rose Bengal
(a)
(b)
(c)
% Degradation Efficiency
Irradiation Time (min)
2 4 6 8 10 12
0
10
20
30
40
50
60
70
80
90
100
Rose Bengal (a)
(b)
(c)
% Degradation Efficiency
pH of Solution
0200 400 600 800 10001200 1400 1600 1800
0
10
20
30
40
50
60
70
80
90
100
(a)
(b)
(c)
Rose Bengal
% Degradation Efficiency
Amount of Photocatalyst (mg/L)
Fig.8. Photodegradation of Rose Bengal Dye in presence of (a) TiO2 (b) TiO2/PPy and (c) TiO2/PPy/GO at various conditions.

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