) 105–111 (2014)

1696-013-0426-5

ORIGINAL PAPER

Kinetics of tartrazine photodegradation by UV/H2O2 in aqueous

solution

Petruta Oancea, Viorica Meltzer*

Department of Physical Chemistry, Faculty of Chemistry, University of Bucharest, Bd. Regina

Elisabeta, 4–12, Bucharest 030018, Romania

Received 4 February 2013; Revised 9 April 2013; Accepted 12 April 2013

In the present work, kinetics of tartrazine decay by UV irradiation and H 2O2 photolysis, and the removal of
total organic carbon (TOC) under specific experimental conditions was explored. Irradiation experiments were
carried out using a photoreactor of original design with a low-pressure Hg vapour lamp. The photodegradation
rate of tartrazine was optimised with respect to the H 2O2 concentration and temperature for the constant dye
concentration of 1.035 × 10−5 M. Tartrazine degradation and the removal of TOC followed the pseudo-first-
order kinetics. The much higher kobs value for tartrazine degradation (7.91 × 10−4 s−1) as compared with the
TOC removal (2.3 × 10−4 s−1) confirmed the presence of reaction intermediates in the solution. 2013 Institute
of Chemistry, Slovak Academy of Sciences

Keywords: tartrazine, dyes, photodegradation, advanced oxidation process (AOP), water treatment

Introduction water (Da Silva et al., 2011; Gupta et al., 2012a,

Synthetic dyes are complex aromatic compounds
that are rather difficult to degrade. These highly
structured organic substances are widely used in
textile and food industries. Azo dyes, characterised
by the presence of one or more azo groups (R 1—N
——N—R2) (Khehra et al., 2006) represent about
60–70 % of all synthetic dyes produced worldwide.
They are resistant to biodegradation under aerobic
conditions (Pagga & Taeger, 1994). A wide range of
methods for the removal of synthetic dyes from
aqueous solutions, including physical adsorption,
electrochemical oxidation, chemical oxidation, and
chemical coagulation/precipitation, have been
proposed (Daneshvar et al., 2002, 2003; El Qada et
al., 2008). These methods are not destructive and
they only transfer the pollutant from one phase to
another. One promising method consists in the use
of advanced oxidation processes (AOPs) involving
the generation of highly reac-
. and Fe(III) catalysts and observed higher tartrazine
tive oxygen species (HO ) in sufficient quantities to
oxidise the majority of organic compounds in waste
2012b).
Over the past 20 years, numerous publications
recommended UV/H2O2 as an effective process for
the removal of pollutants from aqueous solutions
(El-Dein et al., 2003; Behnajady et al., 2004; Shu &
Chang, 2005; Daneshvar et al., 2004). H2O2 is an
environmentally friendly oxidant and the UV/H 2O2
process has several advantages such as no sludge
production, simplicity of operation, and low cost.
Tartrazine (known as E102, C.I. 19140, or
FD&C Yellow 5) is a synthetic lemon yellow azo
dye used as food colourant, in cosmetics and in the
textile industry. Out of all azo dyes, tartrazine seems
to cause the most allergic and intolerance reactions,
particularly among asthmatic patients and those with
aspirin intolerance (Alvarez Cuesta et al., 1981).
There are very few studies concerning tartrazine
degradation. Salem and Gemeay (2000) examined
the oxidation kinetics of tartrazine with
peroxydisulfate in the presence and absence of Ag(I)
conversion in alkaline media. Fragoso et al. (2009)
investigated the

*Corresponding author, e-mail: viomel@gw-chimie.math.unibuc.ro

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106 P. Oancea, V. Meltzer/Chemical Papers 68 (1) 105–111 (2014)
Fig. 1. Molecular structure of tartrazine.
degradation of tartrazine by oxidation with H 2O2 in
an alkaline solution. Mittal et al. (2007) studied the
removal of tartrazine using waste material-hen
feathers as the adsorbent. Patel and Suresh (2006)
investigated the decolourisation of azo dyes using a
magnesium/palladium system, while Gupta et al.
(2011) removed tartrazine by photodegradation on a
titanium dioxide surface.
In the present work, the decay kinetics of
tartrazine by UV light induced by H 2O2 photolysis at
pH ∼ 6, and the degree of mineralisation under
specific experimental conditions were explored and
the effect of the dye and hydrogen peroxide initial
concentrations as well as of the temperature (not
studied by this process until now) were evaluated.
Experimental
Tartrazine (Fig. 1) and stabilised H 2O2 (30 %)
were purchased from Merck and used without
further purification. Aqueous solutions were
prepared by dissolving the required dye quantity in
double distilled water. [Fe(C2O4)3]K3 ·3H2O for
actinometry was prepared in our laboratory.
The irradiation experiments were carried out in a
photoreactor built in our laboratory, using a
lowpressure Hg vapour lamp. The distance of the
UV lamp from the surface of the sample was
maintained at 75 mm. The lamp emits
predominantly UV radiation of the wavelength of
254 nm. The total incident photon flow was 1.92 ×
10−6 E−1, as determined by ferrioxalate actinometry
(Hatchard & Parker, 1956).
The tartrazine concentration was determined
spectroscopically using a Pye Unicam α Helios
UVVIS spectrophotometer (UK) and the pH data
were recorded on a Radiometer Copenhagen pH-
meter (Denmark).
The total organic carbon (TOC) was measured
using an Analyzer Multi N/C 3100 (Analytic Jena,
Germany). All experiments were performed in
duplicate and the maximum difference between the
measured values was 0.9 %.
Results and discussion
Reaction rate expression and UV-VIS spectral
studies
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Photolysis of H2O2 in pure water was studied
extensively in order to elucidate the reaction
mechanism (Bielski et al., 1985; Buxton et al.,
1988). It is well known that the UV irradiation of
H2O2 in aqueous solution leads to the production of
hydroxyl radicals (HO.) (Eq. (1)). These radicals
react with the substrate (S, tartrazine) forming
intermediates (INT) which further react with HO.
and are mineralised (Eqs. (2) and (3)). Other
reactions involved are illustrated by Eqs. (3)–(7).
.
(1)
H2O2 + hν → 2HO
.
(2)
S + HO → INT
.
(3)
INT + HO → Final products
. .
(4)
H2O2 + HO → HO2 + H2O
H O
. .
(6)
HO2 + HO → H2O + O2
. .
(7)
HO + HO → H2O2
Because the oxidation potential of the peroxyl
radical is much lower than that of the hydroxyl
radical, they can be neglected. The photooxidation
of tartrazine with H2O2 in the presence of UV
radiation is thought to be a pseudo-first-order
reaction with respect to the tartrazine concentration:
.
(S); kobs = k2C(HO )
where C(S) represents the tartrazine concentration, t
is the irradiation time, k2 is the second-order rate
constant characterising the reaction of the hydroxyl
radical with the dye (S), and C(HO.) is the hydroxyl
radical concentration. El-Dein et al. (2003) and Shu
et al. (2004) revealed that the degradation rate
follows the pseudo-first-order kinetics with respect
to the dye concentration. Integration of Eq. (8)
resulted in Eq.
(9):
The UV-VIS spectrum of tartrazine exhibited
absorption bands at 257 nm and 428 nm, as shown
in Fig. 2. The band at 428 nm can be assigned to the
n– π∗ transitions of the N——N, C——N, and C
——O groups, responsible for the colour of the dye.
The band at 257 nm was attributed to the π–π∗
transition, showing the aromatic character of the
dye. These wavelengths were used for monitoring of
the dye degradation. The degradation of tartrazine
by UV irradiation is presented in Fig. 2. Samples
 P. Oancea, V. Meltzer/Chemical Papers 68 (1) 105–111 (2014)
(each of 3 mL) were taken at fixed time intervals
and analysed using UVVIS spectrophotometry.
Fig. 2. UV-VIS spectra of tartrazine aqueous solution during its
degradation with UV/H2O2; initial concentrations (C0)
of tartrazine and H2O2 were 1.035 × 10−5 M and
4.14 × 10−4 M, respectively; irradiation time (t): 0 min
(1) 5 min (2), 8 min (3), 10 min (4), 15 min (5), 20 min
(6), 25 min (7), 30 min (8), 40 min (9), 50 min (10), 60
min (11).
Fig. 3. First-order reaction kinetics for the degradation of
tartrazine by UV/H2O2; C0 of tartrazine and H2O2 are as
given in Fig. 2.
It can be seen that an increase of the irradiation
time resulted in a decrease in the dye concentration.
This allowed computing the rate constant of
tartrazine degradation. As shown in Fig. 3, a plot of
ln(C0(S)/C(S)) versus the irradiation time (t) (Eq.
(2)) provided a straight line with the slope equal to
kobs = 7.91 × 10−4 s−1 and the correlation coefficient
R2 = 0.9947.
Effect of initial H2O2 concentration
Fig. 4 shows the dependence of the degradation
degree (A/A0) of the dye solution on the time of
action of H2O2, UV, or UV/H2O2.
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107
No measurable degradation effect was observed
for tartrazine in the presence of H 2O2 alone.
However, UV
•
Fig. 4. Effect of UV irradiation ( ), H2O2 oxidation ( ), or
UV/H2O2 action () on the photodegradation of
tartrazine; A0 is the tartrazine absorbance at t = 0 min; A
is the tartrazine absorbance at different irradiation time
(t = 5–60 min); C0 of tartrazine and H2O2 are as given in
Fig. 2.
Fig. 5. First-order reaction kinetics for the degradation of
tartrazine by UV/H2O2; C0 of tartrazine: 1.035 × 10−5
◦
M; H2O2 concentration: 4.140 × 10−4 M ( ), 6.750 ×
4
10− M ( M
( ), 1.035 × 10−4 M (); A and A0 mean absorbances as
given in Fig. 4.
irradiation degraded about 30 % of the dye within 60
min. Similar results were obtained by Ince et al.
(1997) for the degradation of remazol Black-B and
Elmorsi et al. (2010) for the decolouration of
Mordant red 73. Significant degradation of tartrazine
(83 %) was observed when the sample was
irradiated with UV light in the presence of H 2O2. By
generating HO. radicals via direct photolysis of
108 P. Oancea, V. Meltzer/Chemical Papers 68 (1) 105–111 (2014)

H2O2, Rott and Minke (1999) and Georgiou et al.
(2002) obtained the tartrazine degradation of 80 %
within 60 min.
The degradation of 1.035 × 10−5 M tartrazine was
investigated at different concentrations of H 2O2 in
the range of 1.035–6.75 × 10−4 M and the results
obtained at various irradiation times are presented in
Fig. 5.
Table 1. Kinetic parametersa of the photodegradation process of tartrazine at different H2O2 concentrations
To study the UV/H2O2 degradation, experiments
using different concentrations of tartrazine and
constant H2O2 concentration (optimum value of
4.140 × 10−4 M) were performed. The obtained
results are shown in Fig. 6.
It should be emphasised that the rate constants
decreased from 14.7 × 10−4 to 4.53 × 10−4 s−1 when
the initial dye concentration increased from 0.52 ×

Ctart/M CHP/M Ctart/CHP ratio kobs/s−1 t1/2/s η/%

1.035 × 10−−55 1.035 × 10−−44 2.47 × 10−−44

1.035 × 10 5 1.035 × 2.070 × 10 4 3.105 × 1 : 10 3.63 × 10 4 2806 60

1 : 20 1900 73
10−−5 10−−4 1 : 30 4.44 × 10−−4 1554 80
1 : 40 876 97
1.035 × 10−5 4.140 × 10−4 1 : 50 7.91 × 10−4 920 93

1.035 × 10 6.750 × 10 7.80 × 10

a) Ctart – concentration of tartrazine; CHP – concentration of hydrogen peroxide; kobs – pseudo-first-order rate constant; t1/2 – half-time degradation
time; η – degradation efficiency.

Table 2. Kinetic parametersa of the photodegradation process at different tartrazine concentrations

Ctart/M CHP/M kobs/s−1 t1/2/s η/%

0.520 × 10−55 1.035 × 4.140 × 10−44 1.47 × 10−34

10−−5 4.140 × 10−−4 7.91 × 10−−4 471 99

876 97
2.070 × 10−5 4.140 × 10−4 6.48 × 10−4 1069 85
1372 80
4.140 × 10 5 4.140 × 10 4 5.05 × 10 4 1530 78

8.280 × 10− 4.140 × 10− 4.53 × 10−

10−5 to 8.28 × 10−5 M (Table 2). A similar behaviour
a) For symbols and abbreviations, see Table 1.
was found by other authors (Gao et al., 2003;
Muruganandham & Swaminathan, 2004;
The concentration of H2O2 was approximately Modirshahla & Behnajady, 2006) for the
constant during the process. degradation of other dyes. A possible explanation of
The rate constant increased with the increasing
the dependence of the rate constants on the initial
H2O2 concentration in the aforementioned range, but
decreased at 6.750 × 10−4 M. Similar effects were concentration of tartrazine is that HO. radicals are
reported by other authors (Aleboyeh et al., 2003; consumed not only in the reactions with the dye, but
ElDein et al., 2003) for various dyes. This trend can also in those with the degradation
be explained by the presence of an excess of H 2O2
causing increased consumption of HO. radicals (Eqs.
(4), (5)), thus decreasing the rate constant of
tartrazine degradation. The optimum range of H2O2
concentrations seems to be 3.105–6.750 × 10−4 M
and therefore, the value of 4.140 × 10−4 M was
selected for the determination of the optimum
reaction conditions. Kinetic parameters obtained
under these conditions are presented in Table 1.

Effect of initial tartrazine concentration

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 P. Oancea, V. Meltzer/Chemical Papers 68 (1) 105–111 (2014) 109

Fig. 6. Effect of different initial concentrations of tartrazine Fig. 7. Effect of temperature (T: 295 K ( ), 305 K (

• ◦
(( C0), 2.070(tartrazine− 10): 0.520−5 M (×10), 4.140−5 M (×), K (), 325 K ()) on the degradation of tartrazine by •
1.03510−5 M (×10)−, and5 M UV/H2O2; A0 is the tartrazine absorbance at t = 0 min;
A is the tartrazine absorbance at different irradiation
time (t = 5–90 min); C0 of tartrazine and H2O2 are as
given in Fig. 2.
8.280 × 10×5 M ( )) on the UV/H2O2 degradation;

A0 is the tartrazine absorbance at t = 0 min; A is the

tartrazine absorbance at different irradiation time (t = 0–
180 min).

products. Another explanation of these phenomena

is that at high initial dye concentration, the path
length of the photons entering the solution decreases
and the amount of HO radicals formed in the
solution also decreases. This affects the production
of HO by photolysis of H2O2. Kinetic parameters
obtained under these conditions are presented in
Table 2.

Effect of temperature
Fig. 8. Arrhenius plot of the photodegradation of tartrazine; R2 =
0.9912; C0 of tartrazine and H2O2 are as given in Fig. 2.
Tartrazine degradation was studied at various
temperatures in the range of 295–325 K. Fig. 7
shows
Table 3. Kinetic parametersa of the tatrazine photodegradation the dependence of the degradation (A/A0 ratio) on the
process at various temperatures (T)
temperature. The rate constant (kobs) and halflife
T/K kobs/s−1 t1/2/s η/% degradation time (t1/2) were calculated from these
data and are shown in Table 3.
7.91 × 10−−44
295 876 97
305 9.02 × 10−4 768 98
315 648 99
325 10.70 × 10−4 603 99
11.50 × 10
a) For symbols and abbreviations, see Table 1.

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110 P. Oancea, V. Meltzer/Chemical Papers 68 (1) 105–111 (2014)

•
Fig. 9. Tartrazine degradation ( ) and TOC removal ( ) by the

UV/H2O2 process; C0 of tartrazine and H2O2 are as given

in Fig. 2.

The value of the rate constant increased with the

increasing temperature. According to the rate
constants obtained at various temperatures, the
activation energy (Ea) for the degradation of
tartrazine by UV/H2O2 was calculated using the
Arrhenius equation. The Arrhenius plot of lnkobs
versus 1/T is presented in Fig. 8.
Fig. 10. First-order reaction kinetics for the removal of TOC by
The computed activation parameters are: Ea =
UV/H2O2; kobs = 2.3 × 10−4 s−1; R2 = 0.9948; C0 of
10.08 kJ mol−1, ∆H# = 9.213 kJ mol−1, ∆S# = 55.54 J
mol−1 K−1, and ∆G# = −7.16 kJ mol−1. tartrazine and H2O2 are as given in Fig. 2.

These values indicate that the oxidative process is

spontaneous and has small energetic requirements.
They also reveal the endothermic nature of the
system with only a little change in the three
dimensional arrangement of the transition state of
the molecules (Fragoso et al., 2009).
Kinetics of total organic carbon removal
It is known that the oxidation of azo dyes can
lead to the formation of intermediates which are
more toxic than the initial compounds. For this
reason it was necessary to evaluate the
mineralisation level induced by the UV/H2O2
process.
Kinetic results obtained by tartrazine
concentration monitoring by UV-VIS analysis and
the decrease in the TOC content during irradiation
are presented in Fig. 9. The differences between
UV-VIS and TOC results are caused by the presence
of intermediates. It can be seen that tartrazine
degradation was much higher than TOC removal
after 60 min.
The kobs value for TOC removal was calculated
from the plot ln(C0(TOC)/Ct(TOC)) versus tir, where
Ct(TOC) and C0(TOC) are the TOC concentration
values at reaction times t and 0, respectively, and tir
is the irradiation time (Fig. 10). The straight-line
shape (R2 = 0.9948) of this plot confirms the first-
order reaction kinetics. The value of 2.3 × 10−4 s−1
obtained for kobs is lower than kobs for tartrazine
degradation (7.91
× 10−4 s−1). This observation confirms the presence of
reaction intermediates in the solution.
Although tartrazine dye was degraded by 83 %,
the removal of TOC was only 54 % after 60 min of
irradiation. Advanced degradation and
biodegradable products formation can be achieved
by prolonging the irradiation time.
Conclusions
Evaluation of the tartrazine degradation by the
UV/H2O2 process showed that: i) effective
photodegradation by UV/H2O2 is possible, however,
at 54 % mineralisation efficiency and prolonged
irradiation time; ii) kinetics of tartrazine degradation
and TOC removed follow the pseudo-first-order
kinetics; iii) degradation rate is positively influenced
by the increasing temperature in the tested range; iv)
rate constant of the degradation increases with the
increasing H2O2 concentration up to 4.140 × 10−4 M.
Above this value, the rate constant decreases due to
the scavenging effect of excess H 2O2 and HO.
radicals; v) the value of kobs for tartrazine, which is
much higher than kobs for TOC, confirms the
presence of reaction intermediates in the solution.
Acknowledgements. This work was supported by the
strategic grant POSDRU/89/1.5/S/58852, Project “Postdoctoral
programme for training scientific researchers” co-financed by the
European Social Fund within the Sectorial Operational Program
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