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ae

Current Organic Chemistry, 2017, 21, 1068-1073

REVIEW ARTICLE
ISSN: 1385-2728
eISSN: 1875-5348

Advanced Oxidation Processes for the Removal of Impact

Factor:
1.949

Food Dyes in Wastewater

BENTHAM
SCIENCE

Vincenzo Vaianoa, Giuseppina Iervolinoa, Luigi Rizzob,* and Diana Sanninoa

a
Department of Industrial Engineering, University of Salerno, Via Giovanni Paolo II, 132, 84084 Fisciano (Salerno), Italy;
b
Department of Civil Engineering, University of Salerno, Via Giovanni Paolo II, 132, 84084 Fisciano (Salerno), Italy

ARTICLE HISTORY
Received: July 26, 2016
Revised: September 12, 2016
Accepted: November 22, 2016
DOI:
10.2174/1385272821666170102163307
Current Organic Chemistry
Abstract: Many synthetic food dyes and their by-products, such as aromatic amines and phenolic compounds,
occurring in industrial wastewater, are toxic to aquatic environment and, because of their carcinogenic and
mutagenic nature, they result in a risk for the environment and human health when wastewater is reused or
released into environment. Therefore, an effective wastewater treatment is required before effluent possible
reuse or disposal. In the last years, advanced oxidation processes (AOPs) have been successfully investigated
in the removal of a wide range of organic and inorganic contaminants from water and wastewater because of
their capacity to promote the formation of highly reactive radicals (especially hydroxyl radicals). However,
most of the studies available in scientific literature have been focused on the application of AOPs in the
degradation of organic dyes from textile industries rather than food dyes. Therefore, while the literature about
dye treatment by AOPs in textile wastewater is consolidated, less information is available for food dyes.
Accordingly, this manuscript summarizes the main results related to the removal of food dyes by AOPs. In

particular, conventional methods (biological and adsorption processes) are shortly introduced before to focus
this mini-review on consolidated (namely, ozonation and homogeneous Fenton/photo-Fenton) and new
(namely heterogeneous photocatalytic processes) AOPs.

Keywords: Food dyes, advanced oxidation processes, ozonation, photo-Fenton, heterogeneous photocatalysis.

1. INTRODUCTION 1.1. Organic Dyes in the Environment

Wastewaters coming from domestic and industrial sectors are
very critical from environmental point of view [1]. Therefore, an
effective wastewater treatment is required to reduce their toxicity
before disposal in the environment. The increased amount of
wastewater produced in the developed countries requires suitable
treatments [2]. The main concern related to environment pollution
and human health is related to the production of dangerous waste-
water from different industrial sectors such as tannery, pharmaceu-
tical, textile and agricultural runoffs [3, 4]. Unfortunately, industrial
wastewaters containing dyes are difficult to treat due to dyes char-
acteristics and properties [5]. Conventional biological processes,
typically used in urban wastewater treatment, are not or poorly
effective in industrial wastewater treatment due to the high pollut-
ing loadings in terms of COD, poor biodegradability and high toxic-
ity, therefore suitable advanced methods are required.
This mini-review is focused on the treatment of wastewater
containing food dyes. In particular, the effect of consolidated
(namely, ozonation and homogeneous Fenton/photo-Fenton) and
new (namely heterogeneous photocatalytic processes) advanced
oxidation processes (AOPs) on food dyes wastewater will be
reviewed.
*Address correspondence to this author at the Department of of Civil Engineering,
University of Salerno, Via Giovanni Paolo II, 132, 84084 Fisciano (Salerno),
Italy; Tel/Fax: ++39-089-96-30; E-mail: l.rizzo@unisa.it
Organic dyes are used in a wide range of industrial applications
such as textiles, cosmetics, pharmaceuticals or paper printing but
also in food products [6]. Synthetic dyes are the largest groups of
additives used in the food industry. Generally, these substances
impart color to food and beverages but they do not add any nutri-
tional value and, moreover, they are also present as contaminants in
the process effluents [7].
There are different ways for the classification of commercial
dyes in terms of structure, colour and use (such as textile and food
dyes). Unlike textile dyes, food ones do not result in allergic reac-
tions. On the contrary, textile dyes can cause skin hypersensitivity
and allergy and they are not used as food dyes [8]. However, syn-
thetic food dyes and their by-products, such as aromatic amines and
phenolic compounds, are toxic for the aquatic environment and,
because of their carcinogenic and mutagenic nature [9-11] and pos-
sible transfer through food chain, they represent a risk for human
health. In addition, synthetic food dyes generally contain organic
and inorganic groups that are recalcitrant, thus promoting bioaccu-
mulation in the various food chain steps. In particular, the colour
change obtained by the addition of dyes interferes with the trans-
mission of light in the polluted water, thus reducing the photosyn-
thetic activity of aquatic organisms and increase in the biochemical
oxygen demand [7]. These factors may induce an anaerobic activity
and the consequential formation of sulfides and mercaptans result-
ing in the emission of unpleasant odours [12-14].

15-/17 $58.00+.00 2017 Bentham Science Publishers

Advanced Oxidation Processes for the Removal of Food Dyes
1.2. Conventional Processes: Adsorption and Biological Oxi-
dation
Adsorption is the most used method for the treatment of col-
oured effluents [15] because of (i) high efficiency in terms of colour
removal, (ii) design simplicity, (iii) easy operation and (iv) insensi-
tivity to toxic substances [16]. However, adsorption has several
disadvantages including (i) a progressively decreased adsorbent
capacity to remove the target contaminants as the number of cycle
increases and (ii) pH adjustment is required before or after the
treatment. Moreover, due to the extensive number of aromatic rings
present in some of the food dye molecules, conventional biological
oxidation, typically used in wastewater treatment plants, is ineffec-
tive in treating food dye contaminated water [17-19] and therefore
more effective processes are needed.
1.3. Advanced Oxidation Processes
AOPs have been widely and successfully investigated in the
removal of several contaminants occurring in water and wastewater
[20]. AOPs as those processes that involve the generation of highly
reactive radicals, especially hydroxyl radicals (HO) [21] at near
ambient temperature and pressure. Hydroxyl radicals are extraordi-
narily reactive species that attack most of the organic molecules.
Hydroxyl radicals are also characterized by a low selectivity, which
is an attractive feature for an oxidant to be used in wastewater
treatment. AOPs, such as heterogeneous photocatalysis, ozonation
and photo-Fenton have been investigated for the treatment of waters
contaminated with organic dyes [22-25]. However most of these
studies deal with the application of AOPs in the degradation of
organic dyes from textile industries, while only a few papers in the
scientific literature deal with the removal of food dyes. For this
reason, this review summarizes the main results reported in scien-
tific papers concerning the removal of dyes used in food industries
with the aim to up-date the state of the art in the study of AOPs as
alternative to the traditional methods. According to the relevant
literature available, the following processes were reviewed: ozona-
tion, homogeneous Fenton/photo-Fenton and heterogeneous photo-
catalytic processes.
2. FOOD DYES DEGRADATION BY OZONATION
Ozone (O3) is a strong oxidant effective in many applications,
such as colour removal, disinfection, smell and taste removal, iron
and manganese oxidation and organic contaminants removal [26].
In standard conditions of temperature and pressure, ozone has a low
solubility in water, it is unstable [27] and it has an average life of a
few minutes. Therefore, to have the necessary amount of ozone in
the reaction medium, a greater dose should be used. Ozone has a
high oxidizing power, second only to that of fluorine and HO.
Although included among classical chemical treatments, the ozona-
tion of dissolved compounds in water can also constitute an AOP
by itself as HO are generated from the decomposition of ozone,
which is catalyzed by HO or initiated by the presence of traces of
other substances, such as transition metal cations [28]. Ozonation is
used in many drinking water plants as a tertiary treatment and also
for the oxidation of emerging contaminants [29]. In water solution,
ozone can react with organic compounds via: (1) direct 1,3-dipolar
cycloaddition to double bonds (C=C, C=N, N=N) and (2) in situ
generation of HO [29, 30].
In the case of dyes degradation, ozone selectively attacks the
chromophoric functional group of a dye molecule resulting in a
rapid colour removal [25]. The degradation of the food dye Brilliant
Blue by ozone in aqueous solution has been recently studied [31].
Current Organic Chemistry, 2017, Vol. 21, No. 12 1069
Experimental results showed the high efficiency of ozonation in the
decolourization of aqueous solutions containing the Brilliant Blue,
whereas total organic carbon (TOC) measurements revealed that the
mineralization of the intermediates generated by an initial attack of
HO (generated via the decomposition of ozone), occurred in a
limited extent [31]. The use of ozonation as a decolourization step
was also applied to aqueous solutions of the commonly used food
colorants 2-naphthalenesulfonic acid (Red 40), tartrazine (Yellow
5) and erioglaucine (Blue 1) [32], identifying a number of carbonyl
compounds as major by-products. The results suggested ring-
opening reactions during colorant decomposition, typical of the
interaction between ozone and aromatic compounds [33, 34].
Experiments of degradation of Ponceau 4R azo dye in pure water
were carried out by applying the ozonation process [35]. Almost
complete apparent colour removal was obtained. However, a partial
mineralization of the investigated azo dye and its intermediates, as
well as negligible chemical oxygen demand (COD) removal from
wastewater was observed [35]. The ozone treatment of aqueous
samples containing food Red 17 dye has also been recently studied
[36]. In this case, in contrast with previous studies, ozonation at low
temperature (30 C) was effective not only in the decolourization
but also in the COD removal [36].
3. FOOD DYES DEGRADATION BY PHOTO-FENTON AND
HETEROGENEOUS PHOTOCATALYSIS
3.1. Photo-Fenton Oxidation
It is well known that ferrous ion (as homogeneous catalyst)
combined with hydrogen peroxide (Fentons reagent) reacts
stoichiometrically to give HO [37]. The oxidizing power of the
Fenton reaction can be greatly enhanced by irradiation with UV
light. This effectiveness has been proven with the total mineraliza-
tion of many organic compounds in aqueous solution. The reason
for the positive effect of irradiation on the degradation rate is due to
the photo-reduction of Fe3+ to Fe2+ ions, which produce new HO
radicals with H2O2 [38, 39].
Recently the homogeneous photo-Fenton process has been stud-
ied in the degradation of Tartrazine [40]. Tartrazine is a synthetic
lemon yellow azo dye used in food colorants industry and it seems
to cause most of the allergic and intolerance reactions of all the
food azo dyes, particularly among asthmatics patients and those
with aspirin intolerance [40]. Photo-Fenton process has led to the
total dye disappearance with a TOC removal of 80%.
In the photo Fenton process, the degradation mechanism of
food dyes occurs thanks to the presence of HO formed according
to the following equations [40]:
Fe2++H2O2= Fe3++HO + OH- Eq. 1
Fe3++H2O= Fe(HO)2+ + H+ Eq. 2
2+ 2+
Fe(HO) +h
= Fe + HO Eq. 3
Hydroxyl radicals initiate the first step of the degradation:
R1-N=N-R2+ HO = oxidation intermediates Eq. 4
HO + oxidation intermediates = CO2+ H2O + other inorganic
products Eq. 5
The dye removal rate increased as H2O2 concentration increased
up to an optimum value. Beyond this value, the photo-Fenton activ-
ity decreased due to H2O2 scavenging effect on generated HO radi-
cals [40]. The photo-Fenton reaction with the ferrous gluconate as
homogeneous catalyst showed best results in the degradation of
food dye Acid Green 25 when compared to the Fenton reaction
[41]. Photo-Fenton reaction carried out with Fe2+ ions was also
1070 Current Organic Chemistry, 2017, Vol. 21, No. 12
120
100
80
TOCremoval[%]
60
40
20
0
2.20% 4.50%
Amountofactivephase[wt%]
Fig. (1). Mineralization of Red Allura (RED) and Tartrazine (TRZ) by photo-Fenton oxidation on LaFeO3 based structured photocatalysts after 60 min of
irradiation time [49].
effective in the degradation of Carmoisine dye, a food dye having
low level of beta naphthylamine that is a well known carcinogen
[42]. In this case, the comparison between dye removal efficiency
of Fenton and photo-Fenton processes showed that the latter is a
little more efficient but more expensive; accordingly, the authors
concluded that the Fenton method is more appropriate than the
photo Fenton for Carmoisine removal [42].
Drawbacks of homogeneous photo-Fenton process, such as low
pH (
3), production of Fe containing sludge, and deactivation can
be overcome by heterogeneous photo-Fenton process [43-46]. In
heterogeneous photo-Fenton process, catalysts have been used as
suspended particles in the aqueous solution [47]. Nevertheless, the
suspended catalysts should be removed before effluent disposal,
making necessary a subsequent separation process which increases
investment and operating costs. The use of structured catalysts
could be the solution to avoid an expensive separation process, thus
saving money for wastewater treatment [48, 49]. In particular
heterogeneous photo-Fenton process with structured catalyst was
investigated in the removal of two typical food azo dyes, Red
Allura (RED) and Tartrazine (TRZ) [49]. The photocatalyst used
was LaFeO3 perovskite supported on honeycomb monoliths (corun-
dum). The authors evaluated dyes decolourization and minerali-
zation (through TOC measurements) and they found that the
presence of the structured catalyst plays a crucial role in the miner-
alization of both dyes. In particular the influence of LaFeO3 loading
on corundum honeycomb monolithic support was evaluated. In
spite of complete decolourization was observed for all LaFeO3
loadings investigated and for both dyes (data not shown), the best
efficiency in terms of dye mineralization was observed at 4.5% wt
% LaFeO3 loading for RED dye (87% of TOC removal after 60 min
of irradiation time), and a lower LaFeO3 loading (2.2% wt %) for
TRZ dye (total TOC removal in 60 min of irradiation time) (Fig. 1).
3.2. Heterogeneous Photocatalysis
Heterogeneous photocatalysis can be seen as a green technol-
ogy because it is able to work at ambient temperature and atmos-
pheric pressure. Its operating principle is based on the simultaneous
action of a light source (such as solar light) and a catalyst (semi-
conductor), which allows the degradation of organic pollutants
without any damage to the surrounding environment [49, 50].
Vaiano et al.
RED TRZ
10% 17%
Heterogeneous photocatalysis has been shown to be effective in the
conversion of solar energy into chemicals [51-56], fuels [57-60],
electricity [61], and in the removal of pollutants from wastewater
[62-65] and gaseous streams [66, 67]. Heterogeneous photocatalysis
has been also investigated in the degradation of food dyes. Bukallah
et al. [68] report the photocatalytic degradation of Coomassie Bril-
liant Blue with a commercial TiO2 (Degussa P25) irradiated with a
UV lamp. Unfortunately, they only focused on dye decolourization,
showing that the photocatalytic performances decreased with the
increase in initial Coomassie Brilliant Blue concentration, probably
because of light transfer limitation phenomena occurring in the used
photoreactor [69]. Nanostructured photocatalytic solgel TiO2 films
were used for the degradation of Lissamine Green B dye as a model
pollutant with the predominant irradiation wavelength of 365 nm,
showing that decolourization was almost completed in 2 h while the
total mineralization of the target dye was not achieved [70]. Inter-
estingly, TiO2 was studied as catalyst in the photo-bleaching of
many organic dyes in aqueous dispersions using visible light [71].
The mechanism for bleaching during photocatalytic oxidation with
TiO2 is believed to proceed according to the following equations
[71]:
TiO2+h
= TiO2 (e-+h+) Eq. 6
TiO2 (h+) + H2O= TiO2 + HO+ H+ Eq. 7
TiO2 (e-) + O2 = TiO2+O2- Eq. 8
In addition to the photocatalytic oxidation mechanism,
photosensitizing oxidation mechanism has been considered [71].
This mechanism suggests that the electron from the excited dye
molecule is injected into the conduction band of the TiO2, and the
cation radical formed at the surface quickly undergoes degradation
to yield products:
Dye+h
= Dye* Eq. 9
Dye*+TiO2= Dye++ TiO2 (e-) Eq. 10
TiO2 (e-)+ O2 = TiO2+ O2- Eq. 11
The authors concluded that the used food dyes (Food Red 12,
Food Yellow 13, Food Blue 1, Food Green 3, Food Red 9 and Food
Red 17) were, in general, relatively easier to be bleached than the
other dyes [71].
In a very recent paper, the photocatalytic activity of TiO2 at dif-
ferent morphologies (nanosheets, nanotubes or spherical TiO2) was
Advanced Oxidation Processes for the Removal of Food Dyes
100
90
Decolourizationormineralization[%]
80 decolourization
70
mineralization
60
50
40
30
20
10
0
TiO2
Fig. (2). Decolourization and mineralization of Patent Blue V dye by heterogeneous photocatalysis with TiO 2 and Au/TiO2 after 3 hours of UV irradiation
[22].
tested for the degradation of three food dyes (yellow sunset, red
allura and red carmoisine) underlining that the morphology strongly
affects photocatalyst selectivity. The optimum degradation of sun-
set yellow was achieved by TiO2 nanosheets, by spherical TiO2 for
allura and by TiO2 nanotubes for carmoisine. The authors suggested
that their results present the potential for tuning the morphology of
TiO2 based on the dye to be removed [72]. Despite the very inter-
esting results presented in the cited literature, it must consider that
photocatalysts suffer for the layout of photocatalytic plants, where
the main limitation regards the low activity of photocatalysts sam-
ples and the effective transferring of the light towards the overall
amount of photocatalyst [49]. Therefore a key parameter for a suc-
cessful implementation of photocatalytic processes at large scale is
the reduction of reaction time [49]. In order to improve the photoac-
tivity of the semiconductor, many strategies, such as noble metal
addition, have been employed [54, 67]. The presence of noble met-
als decreased the electron-hole recombination, thus improving the
TiO2 efficiency in the photocatalytic reactions [54, 67]. Very
recently, photocatalytic removal of Patent Blue V food dye has
been verified on Au/TiO2 and Pt/TiO2 catalysts [22]. It was ob-
served that the presence of Au or Pt on TiO2 enhanced the Patent
Blue V photodegradation and that the noble metal particle size and
the distribution on TiO2 surface are important factors influencing
the dye removal. In particular, the highest dye degradation was
observed over the Au/TiO2 catalyst obtaining a decolourization
equal to 93% after 3 hours of UV irradiation, and the mineralization
was equal to 67% (Fig. 2).
It is noteworthy that the most of the photocatalysts formulations
proposed are only active under ultraviolet (UV) radiation, which is
only a little fraction (5%) of solar light [73]. Therefore, to improve
process efficiency, the absorption of the semiconductors should be
within the visible light (43%) of the electromagnetic radiation
reaching the planets surface. Accordingly, a suitable photocatalyst
should work in the visible-light region with a band gap of less than
3 eV [73]. Interesting visible photocatalytic activity results were
found using N-doped TiO2, both under visible irradiation and under
Current Organic Chemistry, 2017, Vol. 21, No. 12 1071
Au/TiO2
solar simulated radiation, in the removal of different pollutants such
as emerging contaminants [62] and bacteria [74]. To increase the
photocatalytic performances, N-doped TiO2 photocatalyst was cou-
pled with light carriers, such as light emitting phosphorescent parti-
cles (phosphors), and UVA-LEDs was used as light source to im-
prove radiation emission and to decrease the optical path of irradia-
tion towards the photocatalyst [73]. A further enhancement of
photocatalytic activity was achieved by combining the N-doped
TiO2 with up-conversion phosphors (OP), able to convert low-
energy into high-energy photons. In this context, the photoactivity
of visible active N-doped TiO2 in the photocatalytic mineralization
of spiramycin was found to be significantly enhanced in the pres-
ence of OP in the catalyst formulation [62]. This optimized
photocatalytic system has been recently tested also with two food
dyes (Tartrazine and Red Allura) finding a strong increase of the
photocatalytic activity with N-doped TiO2 supported on OP
(NdT/OP) with respect to unsupported N-doped TiO2 (NdT) in
presence of visible light emitted by white LEDs (Fig. 3) [73].
The authors believe that NdT supported on the OP surface is
excited both by the blue component of the emission spectrum of the
white LEDs, and by the blue emission of the phosphors (OP),
excited in turn by the green component emitted by the white LEDs
[73].
CONCLUSION
This review summarizes the main results available in scientific
literature dealing with the removal of food dyes by AOPS as alter-
native to traditional methods (such as biological and adsorption
processes) for the treatment of coloured wastewater from food
industries. The mini-review was focused on: ozonation, photo-
Fenton oxidation and heterogeneous photocatalysis. Ozonation is
able to induce the decolourization in a very short treatment time but
it is ineffective in the mineralization.
Quite interesting results have been achieved in photo-Fenton
treatment using a structured photocatalyst made by LaFeO3
1072 Current Organic Chemistry, 2017, Vol. 21, No. 12 Vaiano et al.

100
TRZ(NdT/OP)

TRZ(NdT)

80 RED(NtD/OP)

RED(NdT)

Decolourization[%]
60

40

20

0
0 20 40 60 80 100 120 140
Irradiationtime[min]

Fig. (3). Decolourization of Red Allura (RED) and Tartrazine (TRZ) by heterogeneous photocatalysis under visible light on unsupported N-doped TiO2 (NdT)
and on NdT supported on organic phosphors (NdT/OP) [73].

perovskite, supported on honeycomb monoliths; in this case, high
levels of decolurization and mineralization degree have been
observed. Moreover, the use of structured catalysts instead of the
suspended ones, allows avoiding expensive separation processes
after treatment.
In the case of heterogeneous photocatalysis, the optimization of
the photocatalyst formulation to enhance photons transfer inside the
reactor is the key parameter for process upscale in the removal of
food dyes.
CONFLICT OF INTEREST
The authors confirm that this article content has no conflict of
interest.
ACKNOWLEDGEMENTS
Declared none.
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