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Anodic Oxidation of Textile Wastewaters On Boron Doped Diamond Electrodes
Anodic Oxidation of Textile Wastewaters On Boron Doped Diamond Electrodes
Anodic Oxidation of Textile Wastewaters On Boron Doped Diamond Electrodes
To cite this article: NourElHouda Abdessamad, Hanene Akrout & Latifa Bousselmi (2015) Anodic
oxidation of textile wastewaters on boron-doped diamond electrodes, Environmental Technology,
36:24, 3201-3209, DOI: 10.1080/09593330.2015.1056235
The objective of this study is to investigate the potential application of the anodic oxidation (AO) on two electrolytic
cells (monopolar (Cell 1) and bipolar (Cell 2)) containing boron-doped diamond electrodes on the treatment of real textile
effluents to study the reuse possibility of treated wastewater in the textile industry process. AO is applied in the flocculation
coagulation pretreatment of both upstream (BH) and downstream (BS) effluents. The chemical oxygen demand (COD)
results show that the final COD removal obtained for the BH effluent in the case of Cell 1 and Cell 2 is 800 and 150 mg
O2 L−1 after 5 and 6 h of electrolysis, respectively. The treatments of the BS effluent allow for obtaining a final COD of
76 mg L−1 for Cell 1 and a total mineralization for Cell 2. The obtained results demonstrate that the apparent mineralization
kinetics of both effluents when using Cell 2 are about four times faster than the one obtained by Cell 1 and highlight the
important contribution of the bipolar cell. Besides, the energy consumption values show that the treatment of the BH effluent
by Cell 1 consumes 865 kWh kg COD−1 against 411 kWh kg COD−1 by Cell 2. Therefore, the use of Cell 2 decreases the
energy cost by 2.1–6.65 times when compared to Cell 1 in the case of the BH and BS effluent treatment, respectively.
Keywords: anodic oxidation; BDD bipolar electrode; textile effluent; current efficiency; energy consumption; electrical
energy per order
Table 1. Physico-chemical characteristics of the BH and BS effluents, average and standards values.
(a)
(b) (c)
Figure 2. (a) Experimental setup: (1) reservoir, (2) electrochemical cell, (3) power supply and (4) peristaltic pump, (b) Cell 1 and (c)
Cell 2.
Cell 1 (mini diacell PS 500): It is a single compartment the wastewaters (Table 1) and under a current density of
with parallel plate electrodes. The anode is a monopolar-p- 40 mA cm−2 .
silicon covered by a BDD thin film (2–3 μm thick) with a
12.5 cm2 rectangular surface and the cathode is a stainless
steel. The inter-electrode gap is about 3 mm. 2.4. Analytic procedure
Cell 2: It contains three compartments and four elec- 2.4.1. Average current efficiency, energy consumption
trodes: two bipolar electrodes are coated with Si/BDD on and electrical energy per order
both sides and placed between two monopolar electrodes. The average current efficiency (ACE) of the effluent oxi-
The active surface is 70 cm2 per compartment and the dation is calculated using the COD values (in g L−1 ), by
inter-electrode gap is 1 mm. applying the following relationship [29]:
Figure 3. UV–visible absorption spectra of BH and BS effluents during AO on Cell 1 and Cell 2, pH natural, j = 40 mA cm−2 .
Faraday constant, 8 is the oxygen equivalent mass (g eq−1 ) of C, respectively, and Q is the water volume flow rate
and Vs is the solution volume (L). (m3 h−1 ).[31]
The EC per unit COD mass (kWh g−1 COD) at a time
t is determined as follows [30]:
IVt 3. Results and discussion
EC = , (R2)
((COD)0 − (COD)t )Vs 3.1. Decolourization of the textile effluent (BH and BS)
The dyeing wastewater is characterized by a high col-
where V is the average cell voltage (V).
oration level which is considered as the main limitation
The electrical energy per order (EE/O) is the elec-
for recycling the treated wastewater and its reuse in the
tric energy in kilowatt hours (kWh) required to degrade
process. The UV–visible spectra of the treated BH and
a contaminant (C) by one order of magnitude in 1 m3 of
BS effluents by AO on Cell 1 and Cell 2 during 6 and 5
contaminated water. The EE/O (kWh m−3 order−1 ) can be
h, respectively, are shown in Figure 3. The inset figures
calculated from the following equation of the recycling
represent only the visible area.
system [31]:
BH effluent presents two main absorption bands in the
EE P visible region at 430 and 602 nm. The absorption inten-
= , (R3) sity is not high due to the mixture of the dyeing effluents
O Q × log(c0 /cf )
with different rinsing wastewaters in the BH. Both adsorp-
where P is the rated power (kW) of the AO system, C0 tion bands are strongly decreased after the coagulation–
and Cf are the initial and final concentrations (mol L−1 ) flocculation pretreatment (BS effluent). The discoloration
Environmental Technology 3205
rates are about 74% and 65%, respectively, for 430 and
602 nm. This ratio is in agreement with the COD elimina-
tion by the flocculation coagulation process. The obtained
low absorption of BS can be linked to the low intensity of
the BH absorption bands in the visible region.
Similar results are obtained when the BH effluent is
treated by AO, after 5 and 6 h on Cell 1 and Cell 2, respec-
tively (Figure 3). A total discolouration is achieved only
after 60 min on Cell 1 and 20 min on Cell 2.
The BH effluent also presents a high absorption in
the UV region at 230 nm which is often linked to some
aromatic compounds such as dyes and detergents.
After the pretreatment, the BS effluent spectrum is still Figure 4. Absorbance at 290 nm during AO on Cell 1 and Cell
characterized by a high absorbance at the same absorbance 2 of BH effluent, pH natural, j = 40 mA cm−2 .
UV band (230 nm). The coagulation–flocculation process
appears to be inefficient in the elimination of the main aro-
Concerning the BS effluent, the behaviour of the
matic compounds despite the important COD degradation
hypochlorite ion absorption band is different from that
ratio calculated in Table 1 and equal to 69%.
observed in the case of the BH effluent. The absorp-
Nevertheless, the BH effluent AO had led to a high
tion at 290 nm decreases progressively until a rate of
decrease in the UV absorbance bands, especially at 230
86% by Cell 1 but it disappears totally by Cell 2. This
nm. However, only 25% of the absorbance removal is
could be explained by the low concentration of Cl− in
obtained by Cell 1 compared to 52% when using Cell 2
the BS effluent (Table 1), thus the formation of hypochlo-
after a treatment for 5 h. The obtained results with the BS
rite is lower. The presence and generation of OCl− dur-
effluent showed that the treatment achieved 92% of the
ing the electrolysis can have an impact on the pollution
absorbance removal by Cell 1 and a total removal by Cell 2.
oxidation.
Based on these results, Cell 2 appears to be more
efficient but further insights will be introduced in the
following part of this paper.
3.2. Removal of the COD
A particular behaviour is observed at 290 nm. This
band is attributed to the hypochlorite ions produced by the According to Table 1, the coagulation–flocculation pre-
chloride oxidation at the surface of BDD anodes according treatment allows a decrease of 69% of COD. The obtained
to the following equations [32]: concentration is higher than the sewage system discharge
standards values but it does not allow the recycling of the
2Cl− → Cl2 + 2e− , (1) pretreated wastewater.
Cl2 + H2 O → HOCl+H + Cl ,+ −
(2) Figure 5(a) depicts the evolution of the BH effluent
COD removal during the electrolysis time by the two cells.
HOCl → H+ + OCl− . (3) The AO of the BH effluent decreased the COD value
The absorption band intensity at 290 nm is higher for to 800 mg O2 L−1 which is equivalent to a 48% of COD
the BH effluent when compared to the BS effluent, which removal, after 6 h of electrolysis by Cell 1, such a reduction
is in agreement with the Cl− concentrations presented in is much lower than the one obtained by the pretreat-
Table 1. ment process adopted in the factory. The obtained value
In the case of BH effluent and during the AO by Cell also allows discharging the treated effluent in the sewage
1, the intensity band at 290 nm decreases progressively system but not yet its recycling. In Cell 2, 150 mg O2
during the first 60 min and then increases during the elec- L−1 of the COD is reached, this value corresponds to a
trolysis due to the production of OCl− on the BDD anode 90% removal after 5 h of treatment. The final concentra-
(Figure 4). tion obtained is higher than the discharge limit into the
By using Cell 2, the intensity band increases after 10 natural environment according to the Tunisian Legisla-
min and then decreases after 30 min to completely dis- tion standards (90 mg O2 L−1 ),[34] such a COD value can
appear at the end of the electrolysis step. This decrease be obtained by increasing the electrolysis time which is
in the band intensity corresponds to the degradation of related to the COD degradation kinetic.
the hypochlorite ions until its disappearance which is According to Figure 5(b), the COD degradation kinetic
explained by its reduction to Cl2 on the BDD cathode is fitting a pseudo-first order. This mineralization kinetic by
according to Equation (4).[13,32,33] This reaction is not Cell 2 (K BH,Cell2 = 8 × 10−3 min−1 ) is more rapid than the
possible on Cell 1 as the cathode is made of stainless steel one obtained by Cell 1 (K BH,Cell1 = 1.7 × 10−3 min−1 ).
The Cell 2 efficiency can be attributed to its active surface
2OCl− + 4H+ + 2e− → Cl2 + 2·H2 O. (4) which is 16.8 times larger than Cell 1’s. Besides, the BDD
3206 N. Abdessamad et al.
(a) (b)
Figure 5. Evolution of (a) COD removal and (b) ln(COD0 /COD) of BH effluent during AO on Cell 1 (♦) and Cell 2 (), pH natural,
j = 40 mA cm−2 , COD0 = 1538 mg O2 L−1 .
Table 3. Current efficiency, energy consumption per amount of amount of oxidized COD will be 0.158, 0.129, 0.114 and
COD oxidized (EC) and energy per order (EE/O). 0.052 DT m−3 order−1 , for the treatments of BH, Cell 1,
ta ACEb ECc EE/O
BH, Cell 2, BS, Cell 1 and BS, Cell 2, respectively.
(h) (%) (kWh kg COD−1 ) (kWh m−3 order−1 ) Therefore, it can be observed that in addition to the high
efficiency of the cell with bipolar BDD electrodes, the use
BH Cell 1 28 10 865 1.07 of Cell 2 decreases the energy cost per amount of oxidized
BH Cell 2 6 29 411 0.87
COD to 2.1 and 6.65 times when compared to Cell 1 in the
BS Cell 1 5 7 2860 0.77
BS Cell 2 2.33 20 430 0.35 case of the BH effluent treatment.
In conclusion, the obtained results show that the AO
a Necessary time to oxide COD to 90 mg L−1 .
has significant advantages for use as an effective method
b Current efficiency at t.
c Energy consumption per amount of oxidized COD
for dye removal. There is no consumption of chemicals
at t.
and no sludge build up. It shows efficient and economical
removal of dyes and a high efficiency for degradation of
recalcitrant pollutants. Currently, the textile dye treatment
necessary durations to achieve 90 mg O2 L−1 of COD are is by physical and chemical means. Although the dyes are
determined by applying the apparent first-order kinetic law removed, accumulation of concentrated sludge creates a
which are corresponding to 28 h by using Cell 1 and 6 h by disposal problem [41] and the quality of treated water is
using Cell 2. not adapted to recycling (Table 1).
In the case of the BS effluent, the final COD concen-
tration obtained is 76 mg O2 L−1 by Cell 1 while the treat-
ment by Cell 2 leads to a total mineralization. Therefore, 3.4. Evolution of inorganic ions
an energy estimation is also evaluated by considering the
The two treated effluents contain, in addition to the dyes
required time for the mineralization of the initial amount
and various other organic compounds, various inorganic
of COD to reach 90 mg L−1 (5 h by using Cell 1 and 2.33
ions such as nitrates, chlorides and sulphates.
h by using Cell 2).
The results given in Table 4 show the increase in the
Table 3 highlights the contribution of bipolar cells
sulphate concentration after treatment, particularly when
towards the current efficiency and the EC reduction. For
using Cell 2. This result is expected due to the mineraliza-
instance, the EC values show that the treatment of the BH
tion of sulphonated dyes and the release of sulphate ions.
effluent by Cell 1 consumes 865 kWh kg COD−1 against
However, the final concentration is not high (30 mg/L) and
41 kWh kg COD−1 required for treatment of the same
recycling options can be considered (e.g. rinsing water).
effluent by Cell 2.
In fact, the textile process and, particularly, dyeing step,
The better efficiency of Cell 2 can also be attributed to
needs a large quantity of salts as sulphate and nitrate which
its much higher electrode area (70 vs. 12.5 cm2 on Cell 1)
can exceed 0.6 kg L−1 . These salts allow and facilitate the
as the operating current density is the same. Also, the sepa-
penetration of dyes in fibre.[1,42]
ration between electrodes is different and this presupposes
The treatment of the BH and BS effluents by Cell 1
lesser ohmic drop in Cell 2 than in Cell 1, indicating lower
also leads to an increase in the nitrate concentration result-
EC.
ing from the oxidation of nitrogenous contaminants in the
Besides, the electric energy required for the mineral-
effluent. However, this increase is limited and lower for
ization of both effluents by Cell 1 and Cell 2 for their
Cell 2, which confirms the succession of a redox mecha-
reuse is given in Table 3. The EE/O values indicate that
nism on the BDD anode/cathode and thus reducing nitrate
the required electrical energy for the treatment of these
on NH+ −
4 , NO2 /N2 (g), NH3 (g) or N2 O(g), according to the
effluents is in the following order: BH, Cell 1 > BH, Cell
major electrochemical reactions involved in the electro-
2 > BS, Cell 1 > BS and Cell 2.
chemical nitrate reduction using BDD as a cathode and an
The energy per order also allows a comparison between
the different process or reactors and at variable conditions.
In fact, some studies [39,40] have shown that the treatment Table 4. Inorganic ion concentration of the BS and BH
of charged dyes by the UV/H2 O2 process is efficient for effluents before and after the AO by Cell 1 and Cell 2, pH
synthetic solutions treatments with electrical energy EE/O natural, j = 40 mA cm−2 .
between 0.4 and 5 kWh m−3 order−1 . In the studied case, −1 − −1 − −1
EE/O of the high polluted actual effluent is between 0.3 and SO2−
4 smg L ) Cl (mg L ) NO3 (mg L )
1 kWh−1 m−3 order−1 . BH 19.1 170.4 0
Finally, it is useful to relate the EC values found in BH Cell 1 17.4 67.8 6.4
this study to the treatment costs. The cost of the electric- BH Cell 2 28.7 6.6 4.4
ity, in Tunisia, is 0.148 DT (taxes included, 1 DT equal to BS 11.3 41.9 0
US$0.61587) per kWh, the contribution to the treatment BS Cell 1 12.1 4.2 2.3
BS Cell 2 28.9 1.9 0
cost obtained from the electrical energy and energy per
3208 N. Abdessamad et al.
anode material [43,44]: per amount of oxidized COD cost to 2.1 and 6.65 times
when compared to Cell 1 for the treatment of the BH and
NO− + − + −
3 + H2 O+6H + 8e → NH4 + 4OH , (5) BS effluents, respectively. The obtained results highlight
NO−
3 + H2 O+2e −
NO−
2
−
+ 2OH , (6) the interest and importance of the bipolar BDD electrodes
application for recycling the treated textile wastewater.
1
NO− −
3 + 3H2 O+5e → N2 + 6OH− , (7)
2
NO− − −
3 + ·6H2 O+8e → NH3 + 9OH . (8) Disclosure statement
No potential conflict of interest was reported by the authors.
Concerning chlorides ions, their concentration decrease
is related to their oxidation and then the formation of
hypochlorite and/or Cl2 by both cells. For Cell 2, the Funding
reduction reactions on the BDD cathode reduce greatly the
This research was undertaken with the support of International
chloride and nitrate concentrations. Foundation for Science (IFS), Sweden, by a research fellowship
to CP: HaneneAkrout – Baccour and in the frame of contract
objective with the Tunisian ministry in charge of Research.
4. Conclusion
The AO of real textile effluents for recycling purposes is
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