A R C H I T E C T U R E C I V I L E N G I N E E R I N G E N V I R O N M E N T

T h e S i l e s i a n U n i v e r s i t y o f Te c h n o l o g y N o. 4 / 2 0 1 6

DISCOLORATION OF DYE WASTEWATER

BY MODIFIED UV-FENTON PROCESS WITH SODIUM PERCARBONATE

Barbara PIECZYKOLAN a*, Izabela PŁONKA b, Krzysztof BARBUSIŃSKI c

a PhD; The Silesian University of Technology, Institute of Water and Wastewater Engineering, Konarskiego 18,
44-100 Gliwice, Poland
* E-mail address: barbara.pieczykolan@polsl.pl
b PhD; The Silesian University of Technology, Institute of Water and Wastewater Engineering, Konarskiego 18,
44-100 Gliwice, Poland
c Prof.; The Silesian University of Technology, Institute of Water and Wastewater Engineering, Konarskiego 18,
44-100 Gliwice, Poland
Received: 18.10.2016; Revised: 26.10.2016; Accepted: 7.11.2016

Abstract
A modified Fenton process using sodium percarbonate (SP), as an alternative source of H2O2, and UV radiation was inves-
tigated to discoloration of dye wastewater containing Acid Green 16 (concentration 100 mg/dm3). This acid dye is charac-
terized by the harmful effect on aquatic organisms and it may cause adverse effects in the aquatic environment. The exper-
iments were carried out in two systems, in which two lamps were used as a UV radiation source: low pressure (system I) and
medium pressure (system II). The effect of SP dosage (100-400 mg/dm3 – system I; and 100-250 mg/dm3 – system II),
Fe2+/SP ratio (from 0.2 to 0.4), reaction pH (3 and 4) and reaction time (from 10 to 30 min) on colour removal efficiency
was examined. The modified Fenton process was found to be very efficient for discoloration of simulated wastewater. For a
system with a low pressure UV lamp the optimal doses of SP and Fe2+/SP ratio were 400 mg/dm3 and 0.2, respectively at
pH 3 and 20 minutes reaction time. For a system with a medium pressure UV lamp the optimal doses of SP and Fe2+/SP
ratio were 200 mg/dm3 and 0.33, respectively at pH 3 and 20 minutes reaction time. In both cases, at described conditions
total visual discoloration was achieved. Better results of colour removal (concentration of Acid Green 16 was in the range
of 0.64-0.96 mg/dm3) were achieved when the initial pH value equalled 3.0 than at initial pH value of 4.0 (concentration of
Acid Green 16 was in the range of 0.80-6.87 mg/dm3).

Streszczenie
W procesie odbarwiania ścieków zawierających barwnik Acid Green 16 (o stężeniu 100 mg/dm3) zastosowano zmody-
fikowany proces Fentona z nadwęglanem sodu, jako alternatywnym źródłem nadtlenku wodoru, wspomagany
promieniowaniem UV. Barwnik ten zaliczany do grupy barwników kwasowych charakteryzuje się szkodliwym działaniem na
organizmy wodne, a także może wywoływać niekorzystne zmiany w tym środowisku. Badania prowadzono w dwóch układach
wyposażonych w lampy UV: niskociśnieniową (system I) i średniociśnieniową (system II). Podczas badań zastosowano dawki
nadwęglanu sodu w zakresie (100-400 mg/dm3 – układ I oraz 100-250 mg/dm3 – układ II), wartości stosunku
Fe2+/nadwęglan (od 0.2 do 0.4), pH reakcji (3 i 4), a także czas naświetlania (od 10 do 30 min). Zmodyfikowany proces
Fentona okazał się bardzo skuteczny w odbarwianiu badanych ścieków. Dla układu I z lampą niskociśnieniową najkorzy-
stniejsza dawka nadwęglanu sodu oraz stosunek Fe2+/nadwęglan wynosiły odpowiednio 400 mg/dm3 i 0.2, przy pH=3 i cza-
sie naświetlania 20 minut. Dla układu II (lampa średniociśnieniowa) najkorzystniejsza dawka nadwęglanu sodu wynosiła
200 mg/dm3 i stosunek Fe2+/nadwęglan 0.33, przy pH=3 i czasie naświetlania 20 minut. W obu przypadkach dla tych para-
metrów uzyskano wizualne odbarwienie ścieków. Lepsze efekty odbarwienia uzyskano dla pH=3 w porównaniu z pH=4
(stężenie barwnika odpowiednio 0.64-0.96 mg/dm3 i 0.80-6.87 mg/dm3).

K e y w o r d s : Fenton reagent; UV-Fenton; Acid Green 16; sodium percarbonate; Discoloration.

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 B . P i e c z y k o l a n , I .
1. INTRODUCTION
The consumption lifestyle and an increased demand
on various colored textile, paper, cosmetic and food
products contributes to generation of increasing
amounts of wastewater containing dyes [1]. There are
many different methods for industrial wastewater
treatment. One group of them are oxidation process-
es. Among the innovative methods of industrial
wastewater treatment special interest focuses on
investigations of advanced oxidation processes
(AOPs). Between the various AOPs, Fenton reagent
(mixture of hydrogen peroxide and ferrous iron) is
one of the most effective methods of the oxidation of
organic pollutants [2, 3]. Therefore, the Fenton
reagent has been found to be effective in treating var-
ious industrial wastewater components including aro-
matic amines [4], pesticides [5, 6], surfactants [7, 8], a
wide variety of dyes [9, 10] and many other sub-
stances. Fenton reagent may also be used to improve
the efficiency of aerobic digestion of sewage sludge
[11, 12]. For this reason, Fenton reagent has been
applied to treat a variety of wastes such as those asso-
ciated with the chemical and textile industries [13-15].
Recently, beside the classical Fenton reagent
(H2O2/ferrous salt) a lot of studies have focused espe-
cially on investigation of the Fenton process with
alternative H2O2 or iron sources. Research carried
out by Barbusiński [16-17] showed that this alterna-
tive sources of H2O2 could be calcium and magne-
sium peroxides (CaO2, MgO2) as well as sodium per-
carbonate (sodium carbonate peroxyhydrate) [18-19].
As a most reasonable in practice, it is considered to
use for this purpose commercial products containing
calcium peroxide (PermeOx, PermeOx Plus, Ixper
75C) and magnesium peroxide (Drillox 35M). The
essence of these modifications consists in releasing
H2O2 from CaO2, MgO2 or sodium percarbonate in
acidic condition at the presence of ferrous salt. The
released H2O2 reacts with Fe2+ ions (the Fenton
reaction) and generates OH• radicals which have a
great oxidizing potential. For example, sodium per-
carbonate in the aqueous solution is decomposed
into hydrogen peroxide and sodium carbonate
according to the equation 1:
2Na2CO3  3H2O2 → 2Na2CO3 + 3H2O2 (1)
The authors of this publication have conducted earli-
er studies on discoloration of wastewater using a
modified Fenton process in the H2O2/swarf system.
In this system heterogeneous catalyst (steel swarf), as
an alternative source of iron ions, was investigated
for degradation of dye Acid Green 16 [20]. The
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P ł o n k a , K . B a r b u s i ń s k i
experiments were carried out in continuously-flow
reactor with a column filled with steel swarf. The con-
tinuous Fenton process was found to be very efficient
for discoloration of simulated wastewater.
The present study is a continuation of the use of var-
ious modifications of Fenton reagent for efficient dis-
coloration of dye wastewater. The aim of this study
was to determine the most favorable values of para-
meters of modified Fenton reagent, with sodium per-
carbonate (SP) and UV radiation (UV/SP process),
in order to obtain visual discoloration of wastewater
containing dye Acid Green 16. The effect of experi-
mental factors such as SP dosage, Fe2+/SP ratio, ini-
tial pH and reaction time was tested. UV radiation
was used to increase the amount of OH• radicals such
as in the UV-Fenton system.
2. MATERIALS AND METHODS
2.1. Dye Wastewater
The simulated dye wastewater was prepared by dilu-
tion of commercial dye Acid Green 16 (BORUTA-
KOLOR, Poland) and meat peptone (Aminobak-
pepton, BTL, Poland) with water. The dye was of
high purity and used without further purification.
Concentration of dye and peptone was 100 mg/dm3
and 100 mg/dm3 respectively. Thus prepared waste-
water was characterized with an intensive dark-green
color, high clarity and COD = 320 mg O2/dm3. Acid
Green 16 (Fig. 1) is characterized by the harmful
effect on aquatic organisms and it may cause adverse
effects in the aquatic environment [20-21].
Figure 1.
Structure of the dye Acid Green 16 (C.I. 44025)
2.2. Experimental Procedure
The procedure of Fenton’s reaction was as follows:
the wastewater was put into reactors of 0.5 dm3 vol-
ume, and then acidified with H2SO4 (1+1) to the
selected values of pH, as a Fenton reaction is effec-
tive in acidic range. After that, the various amounts
of sodium percarbonate (SP) and FeSO47H2O (1%
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solution) were added and continuous magnetical stir-
ring was applied. Next, the pH of the wastewater was
again adjusted due to alkaline nature of sodium per-
carbonate. Prepared wastewater was introduced into
a suitable reactor equipped with a low (system I) or
medium (system II) pressure UV lamp. The labora-
tory UV reactor (Wedeco) with a low-pressure (LP)
lamp (15 W) and the UV reactor (UV-Consulting
Peschl) with a medium-pressure (MP) lamp (150 W)
were used. After appropriate time the wastewater
was neutralized with 0.1 N NaOH up to about pH 9
in order to prevent further generation of hydroxyl
radicals. Then, the samples were centrifuged at 3000
rpm (2.5 min) and analyzed at the λ = 590 nm, using
a WPA COLOR WAVE CO7000 Medical
Colorimeter.
The scope of research was divided into three stages,
which included: selection of SP dose and the reaction
time, indication of the most favorable weight ratio of
Fe2+/SP and the value of reaction pH (Table 1). The
selection of the most favorable parameters was made
on the basis of changes in dye Acid Green 16 concen-
tration in the wastewater after the oxidation process
and visual discoloration of wastewater. The concen-
tration of the dye was measured with a colorimetric
method based on a standard curve of dye [22-24].
Table 1.
Parameters of the discoloration process
The range The range Reaction
The kind of
of SP doses, of Fe2+/SP
pH
time,
UV lamp reaction
mg/dm3 ratio minutes
Low
100-400 0.2; 0.33; 0.4 3; 4 10; 20; 30
Pressure
Medium
100-250 0.2; 0.33; 0.4 3; 4 10; 20; 30
Pressure
3. RESULTS AND DISCUSSION
3.1. Effect of SP dosage and radiation time
During the first stage of the experiment, the most
favorable value of SP dose was examined. For both
types of UV lamps with increasing dose of SP (at con-
stant values of other process parameters) a gradual
decrease of the concentration of dye in the treated
wastewater was observed. In case of the system I, the
greatest increase of process efficiency was observed
when the dose of SP increased from 100 to
150 mg/dm3. At the dose of 100 mg SP/dm3 the con-
centration of Acid Green 16 was equaled to
19.03 mg/dm3 (after 10 minutes of reaction) and at
the dose of 150 mg SP/dm3, the dye content was only
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7.65 mg/dm3 (also after 10 minutes of radiation).
E N V I R O N M E N T
Further increase of SP value up to 400 mg/dm3 con-
tributed to a reduction in the concentration of dye to
0.64 mg/dm3 (10 min of radiation). A similar effect of
treatment efficiency was also observed in the case of
the medium pressure lamp. At the dose of 100 mg
SP/dm3, the concentration of Acid Green 16 was
11.17 mg/dm3, while at 150 mg SP/dm3, the concen-
tration of the dye after the process was only
3.16 mg/dm3. Further increase in SP dose to
250 mg/dm3 allowed for reducing the concentration
of Acid Green 16 in the effluent to a value of
1.29 mg/dm3 (10 minutes of radiation).
The obtained results concerning the effect of radia-
tion time on the discoloration efficiency showed that
the highest concentration change was achieved in the
first 10 minutes of reaction for both types of UV
lamps (Fig. 2 and 3). For example, in the system I (LP
lamp) at the dose of 100 mg SP/dm3, the concentra-
tion of the dye was reduced from 100 to
19.03 mg/dm3. Increased reaction time contributed to
further decrease in dye concentration to 13.37 and
10.53 mg/dm3, after 20 and 30 minutes of radiation
respectively. A similar relationship between dye con-
centration and reaction time was observed in the sys-
tem II (MP lamp). It was also noted that for all SP
doses, in both research systems, when reaction time
increased, the efficiency of discoloration also
increased. This is because the longer exposure time
to a UV radiation causes a larger amount of Fe2+ions
produced by reduction of Fe3+ ions according to the
reaction 2 [25]. It should be noted, however, that the
visual discoloration of wastewater was only obtained
after 20 and 30 minutes of reaction in the whole
range of examined SP doses. Therefore, in further
investigations the reaction time of 20 minutes was
used.
Fe3+ + H2O2 + hv → Fe2+ + OH• + H+ (2)
The research results also showed that in the system I,
higher doses of SP were required to ensure visual dis-
coloration than in the system II (Fig. 2 and 3). When
the LP lamp was used as a source of UV radiation,
visual discoloration of the wastewater was achieved
only at 400 mg SP/dm3. The application of the MP
lamp allowed for visual discoloration of wastewater
already at dose of 200 mg SP/dm3. It indicates that,
the power of UV lamps plays a key role in the effi-
ciency of UV/Fenton process. Low pressure lamps
are mainly used in the disinfection process and gen-
erate radiation with a wavelength of 254 nm [26]. In
contrast, medium pressure UV lamps generate radia-
tion in length of 240-600 nm, which has a much high-
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 B . P i e c z y k o l a n , I .
er energy. Therefore, this kind of radiation can oxi-
dize the contaminants directly. Moreover, both types
of UV lamp are often used in wastewater treatment
processes, particularly in the AOPs technologies
[27-30]. To further stage of research (i.e. selection of
the most favorable weight ratios of Fe2+/SP) doses of
400 and 200 mg/dm3 were chosen in the system with
LP and MP UV lamp, respectively. Furthermore,
basing on the results obtained in the first stage of the
study, 20 minutes was selected as the most favorable
radiation time for both systems.
Figure 2.
Changes of Acid Green 16 concentration in dependence of SP
doses during UV/Fenton process with LP UV lamp (pH 3,
Fe2+/SP=0.33)
Figure 3.
Changes of Acid Green 16 concentration in dependence of SP
doses during UV/Fenton process with MP UV lamp (pH 3,
Fe2+/SP=0.33)
3.2. Effect of Fe2+/SP
In both systems, the effect of three values of the
weight ratio of Fe2+/SP was examined. It was shown
that as the value of Fe2+/SP increased, the efficiency
of the purification process also increased (Fig. 4). In
the system I with the LP UV lamp, visual discol-
oration of wastewater was obtained for Fe2+/SP
ratio = 0.2 and at dye concentration 0.64 mg/dm3.
The increase of iron quantity (sequentially to 0.33
and 0.4 of Fe2+/SP ratio) caused almost linear
decrease of the dye concentration, to 0.48 mg/dm3
(Fe2+/SP=0.33) and 0.32 mg/dm3 (Fe2+/SP=0.4),
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P ł o n k a , K . B a r b u s i ń s k i
respectively. In the system II, visual discoloration of
wastewater was obtained at value of Fe2+/SP ratio
equal 0.33 (dye concentration = 0.96 mg/dm3). Using
lower dose of iron ions did not allow to achieve the
effective removal of Acid Green 16 (visual discol-
oration was not obtained).
In addition, it was seen that the greater efficiency of
the process was observed in the system I. However, it
should be noted, that in the case of the purification
system with LP UV lamp the dose of SP was twice
higher than in the system with MP UV lamp.
Therefore, basing on the results obtained during that
stage of the study as a most favorable ratio of Fe2+/SP
following values were chosen: 0.2 in system I and 0.33
in the system II. These were the minimum values of
Fe2+/SP ratio at which the visual discoloration of the
wastewater was obtained.
Figure 4.
Changes of Acid Green 16 concentration in dependence of
Fe2+/SP ratio values: system with LP UV lamp (pH 3, SP dose
400 mg/dm3); system with MP UV lamp (pH 3, SP dose
200 mg/dm3)
3.3. Effect of pH
Experiments conducted in both systems showed that
as reaction pH increased from 3.0 to 4.0, the efficien-
cy of the removal of the dye Acid Green 16 decreased
(Fig. 5). In the case of LP UV lamp the dye concen-
trations were equaled to 0.64 and 0.80 mg/dm3, at
pH 3.0 and 4.0 respectively. However, in the system II
with MP UV lamp, the effect of pH on discoloration
efficiency was much more significantly. When the
process was conducted at pH 3.0 the concentration of
Acid Green 16 was equaled to 0.96 mg/dm3. At pH
4.0 the dye content increased up to 6.87 mg/dm3.
Such differences in the effect of pH on the effective-
ness of discoloration in both systems may result from
the difference in SP doses. In the system I the dose of
SP was twice higher than in system II. It is also known
that as the pH increases quantity of H2O2 released
from SP decreases. Generally, the higher dose of SP,
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the greater quantity of H2O2 is released from SP into
the treated wastewater. Therefore the dose of SP
could have such a large impact on the process effect.
Figure 5.
Effect of pH on the reduction of Acid Green 16 concentration:
system I – LP UV lamp (Fe2+/SP=0.2, dose of SP
400 mg/dm3); system II – MP UV lamp (Fe2+/SP=0.33; dose
of SP 200 mg/dm3
4. CONCLUSIONS
The study of treatment of synthetic dye wastewater
using a modified UV-Fenton process (in the modifi-
cation with sodium percarbonate) allowed to formu-
late the following conclusions:
• It is possible to effectively decolorize wastewater
containing Acid Green 16 using the modified
Fenton reagent with sodium percarbonate in com-
bination with UV radiation.
• The type and power of the UV lamp, which is a
source of radiation, has a significant impact on the
effectiveness of decolorizing. In the case of MP
lamp a visual discoloration of wastewater was
obtained at a dose of 200 mg SP/dm3. When the LP
UV lamp was used, twice higher dose of SP
(400 mg/dm3) was required. It can be assumed that
in the case of system II beyond oxidation of the
dye by Fenton reagent, direct photo-oxidation the
Acid Green 16 can also occur (due to a wider
range of wavelengths of the radiation emitted by
the MP UV lamp).
• In both systems, the impact of individual parame-
ters of UV-SP process on the effectiveness of dis-
coloration of dye wastewater was noted. As the
dose of SP increased, the efficiency of discol-
oration increased. The same impact of radiation
time and Fe2+/SP ratio on discoloration effective-
ness was observed. As the values of these para-
meters increased the removal of Acid Green 16
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also increased.
E N V I R O N M E N T
• In the whole range of Fe2+/SP ratio, better results
of discoloration were obtained in the system I.
That phenomenon may be connected with using
twice higher dose of SP in that system in compari-
son with system II.
• In both systems, the color removal efficiency was
lower at pH 4 compared with pH 3.
• The results of the study showed that better results
were obtained when system II with MP UV lamp
was used. The visual discoloration of treated
wastewater was achieved when following process
parameters were used: dose of SP 200 mg/dm3,
Fe2+/SP ratio 0.33, radiation time 20 minutes and
pH 3.
ACKNOWLEDGEMENTS
The authors wish to thank Ms. A. Krzon and
Ms. A. Niestrój for their technical and analytical
assistance.
This research was supported by the research fund of
Silesian University of Technology in Gliwice (Poland)
through the project BK-270/RIE-4/2015.
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