Process Biochemistry 43 (2008) 1352–1358

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Process Biochemistry
journal homepage: www.elsevier.com/locate/procbio

Electricity production during the treatment of real electroplating wastewater

containing Cr6+ using microbial fuel cell
Zhongjian Li, Xingwang Zhang, Lecheng Lei *
Institute of Environmental Pollution Control Technologies, Xixi Campus, Zhejiang University, Hangzhou 310028, PR China

A R T I C L E I N F O A B S T R A C T

Article history: Microbial fuel cell (MFC) was employed to dispose Cr6+ in real electroplating wastewater and generate
Received 30 January 2008 electricity simultaneously. The experiments were carried out in a dual-chamber MFC. Under the
Received in revised form 11 July 2008 condition of pH 2 and using graphite paper as the cathode electrode chromium removal and power
Accepted 8 August 2008
density were highest. Moreover, increasing initial concentration of Cr6+ could enhance the power density.
The results indicated that when treating a real electroplating wastewater containing Cr6+ with the initial
Keywords:
concentration of 204 ppm in the MFC, the maximum power density of 1600 mW/m2 was generated at a
Microbial fuel cell (MFC)
columbic efficiency of 12%. In addition, 99.5% Cr6+ and 66.2% total Cr were removed through reduction of
Electroplating wastewater
Chromium
Cr2O72 to Cr2O3 precipitating on the surface of cathode electrode. MFC was proved to be a promising
Electricity generation technology for removing Cr6+ from electroplating wastewater.
XPS ß 2008 Elsevier Ltd. All rights reserved.
SEM

1. Introduction fuel cells are of interest as a technology for the conversion of

One of the critical pollution problems arising from the
electroplating industry is the generation of wastewater containing
heavy metals such as cadmium, copper and chromium [1]. Heavy
metals especially chromium pose a serious risk to human, animals,
and the environment. Hexavalent chromium usually occurs as
highly soluble and highly toxic chromate anions, and is suspected
carcinogens and mutagens. The accumulation of Cr6+ in living
tissues throughout the food chain causes many serious health
problems. Potable waters containing more than 0.05 mg/l Cr6+ are
considered toxic [2,3]. Therefore, it is necessary to treat electro-
plating wastewater containing chromium prior to its discharge.
Several treatment techniques such as chemical precipitation,
coagulation–flocculation, ion exchange, membrane filtration [4]
and biosorption [5] have been applied to dispose chromium in
electroplating wastewater. Although conventional metal removal
techniques are effective, they encountered with some major
disadvantages including high energy requirements, excessive
chemicals consumption, and generation of a large quantity of
toxic waste sludge.
It is proposed here that electroplating wastewater containing
Cr6+ can be treated using microbial fuel cells (MFCs) which have
been developed to generate electricity from wastewater. Microbial
* Corresponding author. Tel.: +86 571 88273090; fax: +86 571 88273693.
E-mail address: lclei@zju.edu.cn (L. Lei).
chemical energy to electricity [6–9]. The most commonly used
MFCs in the laboratory are dual-chamber MFCs, which consist of an
anode chamber and a cathode chamber separated by a proton
exchange membrane (PEM). Microorganisms grow at the anode
under anaerobic conditions. These microorganisms oxidize the
organic matter and transfer electrons to the anode that then pass
through an external circuit to the cathode producing current.
Protons migrate through the proton exchange membrane to the
cathode where they combine with oxygen and electrons to form
water [7]. Recently, MFCs have been developed to generate
electricity directly from complex organic wastewater such as food
wastewater [10,11], domestic wastewater [12–14], swine waste-
water [15], chemical wastewater [16,17] and other wastewaters
[18–23]. Min et al. [15] treated swine wastewater by a dual-
chamber MFC. They found that 86% removal of COD and 83%
removal of NH4–N was achieved and the maximum power density
was 45 mW/m2. Liu et al. [24] employed a single-chamber MFC to
treat domestic wastewater. The maximum power density gener-
ated during the treatment process was 26 mW/m2 and 80% COD
was removed. Previous studies have demonstrated that the
energy-efficient treatment of wastewater is one of the most
promising applications of MFCs. However, in most of those
systems, wastewater as the electron donors was treated in the
anode chamber by microorganisms. The effect of cathode chamber
on electricity generation was just to form the pass way for
electrons and protons. Oxygen [8,9,25], hexacynoferrate [26] or
permanganate [27] was commonly used as electron acceptors.

1359-5113/$ – see front matter ß 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.procbio.2008.08.005
 Z. Li et al. / Process Biochemistry 43 (2008) 1352–1358
Therefore, if using certain pollutant with the ability of accepting
electrons and protons as oxidant, the cathode chamber of MFCs, as
well as the anode chamber could harvest considerable energy from
pollutants. This would greatly enhance the environmental benefit
of MFCs [28]. Based on this hypothesis, electroplating wastewater
containing Cr6+ was chosen as the cathodic electron acceptor in
this study. Under acidic conditions, Cr6+ ion accepts six electrons
and thus is reduced to Cr3+ ion as illustrated in the following
equations:
Cr2 O7 2 þ 8Hþ þ 6e ¼ Cr2 O3 þ 4H2 O; 1:33 V
Cr2 O3 þ 6Hþ ¼ 2Cr3þ þ 3H2 O
The equations indicated that in acidic environment Cr6+ has higher
oxidation potential (1.33 V vs. SHE) than oxygen (1.23 V) and
hexacynoferrate (0.36 V) [26]. So it can be deduced that potassium
dichromate is a more favorable electron acceptor theoretically. To
the best of our knowledge, potassium dichromate has not been
used as the cathodic electron acceptor in MFCs.
In this work, the objective is to produce electricity directly from
electroplating wastewater using a MFC combined with accom-
plishing wastewater treatment. Therefore, several factors that
might affect the removal of chromium and electricity generation
including pH, initial Cr6+ ion concentration and different electrode
materials were investigated using synthetic wastewater in a dual-
chamber MFC. Also, to demonstrate the feasibility of this novel
MFC treatment process, we examined the treatment efficiency of a
real electroplating wastewater containing Cr6+. The reduced
production of Cr6+ was analyzed by SEM and XPS.
2. Materials and methods
2.1. MFC construction
The experimental set-up was shown in Fig. 1. MFC comprised two (anode and
cathode) 220 ml (h = 11 cm, w ¼ 4 cm, l = 5 cm, effective volume = 200 ml) plex-
iglass rectangular chambers. The chambers were physically separated by proton
exchange membrane (NafionTM 117, Dupont Co.) with a 45 cm2 surface area. The
Fig. 1. Schematic prototype of the MFC used to generate electricity from
electroplating wastewater.
1353
PEM which was sequentially boiled in H2O2 (30%), deionized water, 0.5 M H2SO4,
and then deionized water (each time for 1 h) as described by Liu and Logan [29] was
held between the two rectangular chambers with a rubber gasket to prevent
leakage. The anode chamber sealed with a rubber stopple was mixed with a
magnetic stir bar. Plain carbon felt (2 cm  5 cm, 2 mm thick, Liaoning, China) with
rough surface and porosity was placed in the anode chamber to accumulate the
electron-transferring bacteria. Plain graphite paper (2 cm  5 cm, 0.2 mm thick,
Jiangsu, China) was inserted into the cathode chamber to act as a cathode (except as
noted). The electrodes were connected with a copper wire coming out of the rubber
stopple to provide the connection points for the external circuit. An air-sparger was
fixed in the bottom of cathode chamber for air sparging during inoculation or
nitrogen sparging during the wastewater treatment.
(1)
2.2. Inoculation
(2)
Inoculation was conducted in the dual-chamber MFC mentioned above.
Anaerobic sludge collected from the anaerobic digester of SiBao wastewater
treatment plant in Hangzhou, China, was used as an inoculum in the anode
chamber. Anaerobic sludge has been shown to be a suitable biocatalyst for
electricity production [24,26]. For inoculation, a mixed solution of 50 ml anaerobic
sludge with 150 ml sodium acetate medium was injected into the anode chamber.
The anode medium contained the following (per liter): KH2PO4, 13.60 g;
CH3COONa, 1.00 g; NaCl, 11.70 g; NaOH, 2.33 g [15]; NH4Cl, 0.45 g; MgCl26H2O,
0.17 g; FeCl36H2O, 1.00 mg; MnCl24H2O, 23.0 mg; CaCl2, 15.0 mg [7] and 1 ml of a
trace element solution as reported by Logan et al. [25]. The cathode medium
contained the following (per liter): KH2PO4, 13.60 g; NaCl, 11.70 g; NaOH, 2.33 g.
KH2PO4 and NaOH were added in both anode and cathode medium forming PBS (pH
7). And NaCl was added to increase the solution conductivity. The cathode chamber
was sparged with air (80 ml/min) using an air pump, during the inoculation stage.
The electrodes were connected via an external circuit containing a single resistor
(R = 1000 V). Experiments were conducted in a 35 8C temperature-controlled box
(SPX-250B-Z, Shanghai, China). The anode chamber was added with 80 mg sodium
acetate every day until the stable output voltage increase to 240–260 mV, which
indicated bacteria have colonized the electrodes.
2.3. Operation of MFC
After the inoculation was finished, the anode chamber was refilled with 200 ml
anode medium which was sparged with N2 for 0.5 h (60 ml/min) to remove dissolved
oxygen. Synthetic wastewater was refilled in the cathode chamber and continuously
sparged with N2 (80 ml/min) to fully mix the cathode medium. The synthetic
wastewater (per liter) contained KH2PO4, 13.6g and NaCl, 11.7 g with different
amount of K2Cr2O7. The pH was adjusted with H2SO4 (50%). Plain graphite paper
(2 cm  5 cm, 0.2 mm thick) was used as the cathode electrode except where stated
otherwise. Electrodes were connected via a circuit containing a resistance of 1000 V
(except as noted) to measure electricity generation and Cr6+ removal. To determine
the effect of various parameters on power generation and Cr6+ removal, pH (1–6) and
initial concentration of Cr6+ (50–500 ppm), different electrode materials including
graphite paper, carbon paper (120, Toray Co., Japan) and carbon felt were investigated.
Different external resistance (10–9000 V) was applied in order to obtain polarization
curve for determination of the maximum power generation.
2.4. Calculations
Voltage was measured using a multimeter with a data acquisition system (UNT
UT-70B, China) and converted to power density, P (W/m2), according to
y2
P¼
RA
where R is the resistance, y is the voltage, and A is the cross-sectional area
(projected) of the anode. The Columbic efficiency was calculated as
CP
Ec ¼  100%
CT
where Cp is the total coulombs calculated by integrating the current over time. CT is
the theoretical amount of coulombs that can be produced from sodium acetate,
calculated as
bCVF
CT ¼
M
where F is Faraday’s constant (96485 C/mol e), M is relative molecular mass (82 g/
mol by sodium acetate), b is the number of mol of electrons produced per mol of
substrate (b = 8 mol e/mol based on sodium acetate), C (mg/l) is the overall
removal of sodium acetate, y (200 ml) is the anode liquid volume.
2.5. Analytical methods
Acetate was analyzed using ion chromatograph (IC1000 Techcomp, China)
equipped with an anion separation column (SI-90 Shodex, Japan). Samples were
1354 Z. Li et al. / Process Biochemistry 43 (2008) 1352–1358

filtered through a 0.22 mm pore diameter membrane. Cr6+ was determined by

colorimetry using diphenylcarbazide. Total chromium was analyzed using atom
absorption spectrometry (AA-6800 Shimadzu, Japan). Microorganisms on anodic
electrodes and cathodic electrodes were examined using a scanning electron
microscope (SEM) (XL-30 Philips, Holland). Determination of the chemical
composition of cathodic reduced products was done by using an X-ray
photoelectron spectrometer (XPS) (PHI 5000C ESCA System, USA).

3. Results and discussion

3.1. The start up of MFC using Cr6+ ion as the electron acceptor

During the start-up stage, stable power generation was

obtained after two cycles. Fig. 2 showed the output voltage
(R = 1000 V) steadily increased from 100 mV at 232.4 h to about
240 mV at 233.5 h when the anode chamber was refilled with the
fresh anode medium (point A). And then the synthetic wastewater
containing 50 ppm potassium dichromate (pH 2) was refilled the
cathode chamber and N2 was continuously sparged at a flow rate of Fig. 3. SEM image of electron-transfer bacteria attached to the surface of the anode.
80 ml/min (point B). This led to a substantial increase of voltage
to 605 mV. Such a sharp increase of voltage was most likely due
to the high redox potential (1.33 V) of Cr2O72 in acidic conditions
as illustrated in Eq. (1). The SEM images (Fig. 3) shows that
anodic electrode surface is covered by bacilliform bacteria which
are responsible for electron transfer and current generation in
the MFC.

3.2. Effects of pH on power density and removal efficiency of Cr6+ ion

To determine the effect of pH, the power density and the

removal of chromium were examined using a synthetic waste-
water containing 50 ppm potassium dichromate. The pH of
synthetic wastewater was adjusted to 1–6 with H2SO4 (50%).
Fig. 4 illustrates that Cr6+ removal increases from 28% to 98.3%, as
the pH decreases from 6 to 2. And green deposit could be evidently
observed on the surface of cathode. However, the removal was not
further increased at lower pH (pH 1). This was attributed to the H+
in cathode chamber diffused to anode chamber at pH 1, leading to a
decrease in pH of anodic medium from 6.8 to 1.8 over the course of
experiment. The low pH of anodic medium deactivated the
microorganism and reduced the performance of MFC. The removal
of total chromium followed a similar trend. The highest removal of
49.1% total chromium was achieved at pH 2, while removal
decreasing to 18% at pH 6 and to 0 at pH 1. We supposed that Cr3+
Fig. 4. Maximum power density generated and chromium removal as a function of
pH (50 ppm potassium dichromate).
was removed in the form of trivalent chromium oxides depositing
on the surface of cathode. Moreover, trivalent chromium oxides
dissolved in the cathode medium pH 1. Fig. 4 also shows the effect
of pH on the maximum power density. The maximum power
density was increased from 67.6 to 705 mW/m2 as pH decreased
from 6 to 1. This revealed that low pH played a positive effect on
power generation when potassium dichromate was used as
electron acceptor in the MFC. The conclusion was confirmed by
the power density generated over 9 h experiments with an
external resistance of 1000 V (Fig. 5). The sharp decrease of
power density at pH 1 observed in Fig. 5 was possibly due to the
diffusion of H+ to anode chamber mentioned above.

3.3. Effects of initial Cr6+ concentration on output power density

and cathode potential

To determine the effect of initial Cr6+ concentration on the

Fig. 2. Electricity generation by MFCs during startup using potassium dichromate.
(A) Refill the anode chamber with fresh anode medium. (B) Refill the cathode
chamber with synthetic wastewater containing 50 ppm potassium dichromate,
pH 2.
performance of MFC, Cr6+ concentration was set in the range of 50–
500 ppm. Based on the above-mentioned results, the pH of cathode
medium was adjusted to 2 and then the effect of Cr6+ concentration
on cathode OCP was examined by placing a saturated calomel
electrode in the cathode chamber. Fig. 6 shows that increasing the
initial Cr6+ concentration from 50 to 500 ppm increases the
maximum power density by a factor of 3.54 from 602 to 2116 mW/
m2 and the OCP increases from 619 mV to 814 mV. The
 Z. Li et al. / Process Biochemistry 43 (2008) 1352–1358
Fig. 5. Comparison of power generated in different pH (50 ppm potassium
dichromate, R = 1000 V).
Fig. 6. Maximum power density and open circle cathode potential as a function of
initial concentration of potassium dichromate (pH 2).
improvement in maximum power density might be due to the
increase of cathode OCP which was influenced by Cr6+ concentra-
tion and pH. The phenomena were generally consistent with the
trends expected from analysis using the Nernst equation based on
Eq. (1):
E ¼ 1:33 þ 0:01 log½Cr2 O7 2   0:08 pH
Another reason for the increase in maximum power density might
be the decrease in internal resistance as a result of increase in ionic
strength [30]. At 50 ppm Cr6+, the internal resistance was 300 V
and then decreased to 100 V as the Cr6+ concentration increased to
500 ppm. You et al. adopted 100 ppm potassium permanganate as
the electron acceptor in a dual-chamber MFC. And a maximum
power density of 115.6 mW/m2 was generated [27]. Gu et al.
revealed that a maximum power density of 12.4 mW/m2 was
generated using 50 ppm chlorophenol as the electron acceptor
[28]. In contrast to potassium permanganate and chlorophenol,
potassium dichromate was a more favorable electron acceptor,
showing a higher power density of MFC.
3.4. Effects of different electrode materials on power density and
removal of Cr6+
Graphite paper, carbon paper and carbon felt were chosen as
the cathode electrodes in this investigation. A synthetic waste-
1355
Fig. 7. Comparison of power generated using different cathode materials (50 ppm
potassium dichromate, pH 2, R = 1000 V).
water containing 50 ppm potassium dichromate at optimal pH of 2
was used to assess the effect of different electrode materials on the
performance of MFC. As shown in Fig. 7, the power density of
graphite paper cathode slowly increased to the maximum
(348 mW/m2) at the first 2 h, and gradually decreased to
5.7 mW/m2 in the next 7 h as Cr6+ was reduced. For carbon paper
cathode, the power density of achieved the maximum value
(291.6 mW/m2) in 10 min, and decrease slowly to 13.3 mW/m2
within the next 8.5 h. As for the carbon felt cathode, the maximum
power density (678.9 mW/m2) was generated in 10 min, and
decrease sharply to a low level (<50 mW/m2). The sharp decrease
could be ascribed to some changes on the surface of carbon felt,
which were induced by electricity and oxidation effects. The
internal resistances kept about 300 V, not affected by the electrode
materials. The maximum power density of graphite paper, carbon
paper and carbon felt were 616, 408.3 and 761 mW/m2,
respectively, for an external resistance of 300 V.
From Fig. 8, it can be seen that the removal of Cr6+ in 9 h is 98.3%
for graphite paper cathode, 86.3% for carbon paper and 40.6% for
carbon felt. The graphite paper had the best performance on
removing Cr6+. Moreover, 49% of total chromium could be reduced
using graphite paper, while only 26.2% and 27.6% total chromium
could be removed using carbon paper and carbon felt, respectively.
After 9 h, a green precipitate could be observed on the surface of
Fig. 8. Chromium removal obtained using different cathode materials (50 ppm
potassium dichromate, pH 2).
1356 Z. Li et al. / Process Biochemistry 43 (2008) 1352–1358

graphite paper and carbon paper, while few precipitate could be

found on carbon felt. The removal of Cr6+ and total chromium was
related with the output power density. Higher power density
produced faster removing of chromium. During 9 h treatment, the
redox potential of NAD+/NADH in the anode varied between 320
and 355 mV, which was similar to that reported by Rabaey and
Verstraete [31]. Hence, compared with carbon paper and carbon
felt, the MFC using graphite paper cathode with higher cathode
potential showed the highest power density and the most efficient
removal of chromium.

3.5. Treatment of real electroplating wastewater using MFC system

To demonstrate the feasibility of this new type of MFC

treatment process, we examined the treatment of a real electro-
plating wastewater. All the real wastewater used in this study was
collected from an actual electroplating plant. The concentration of
potassium dichromate was about 204 ppm and the pH was 2.5.
After 25 h treatment, the removal of Cr6+ and total chromium Fig. 9. Power generated in the MFC using real electroplating wastewater as electron
reached 99.5% and 66.2%, respectively. Table 1 compared the acceptor (pH 2, R = 1000 V).

removal of Cr6+ in the literatures with that obtained in this study.

In contrast to other treatment process, the main advantages of MFC
for electroplating wastewater treatment were (1) simultaneous
electricity generation, (2) higher Cr6+ concentration tolerance
compared to other biological treatment and (3) no toxic waste
sludge production. The power density generated over the process
was showed in Fig. 9. The maximum power density was 1600 mW/
m2 at a current density of 0.4 mA/cm2 with an external resistance
of 100 V (Fig. 10). The obtained maximum power density was
higher than that reported by other researchers in the treatment of
wastewater using MFC, e.g. the maximum of 142.41 mW/m2 was
obtained during the chemical wastewater treatment using MFC
reported by Mohan et al. [17], 25 mW/m2 generated during urban
wastewater treatment reported by Rodrigo et al. [14] And the
maximum of 218 mW/m2 generated during domestic wastewater
treatment reported by Min and Angelidaki [39]. The columbic
efficiency of the system was 12% which was comparable to <15%
reported by Liu et al. [9], indicating there was substantial COD
removal that was not associated with power generation. With
Fig. 10. Power generation as a function of the current density using potassium
respect to reaction mechanism, the removal of Cr6+ was dichromate (pH 2).
accomplished by the whole MFC system, including the proton
and electron generation phase. Under anaerobic condition,
microorganisms in anode chamber oxidized acetate to generate cathode chamber through the PEM. Cr6+ was reduced by the
protons and electrons (Eq. (3)): protons and electrons as illustrated in Eq. (1). The reduction of
Cr6+ is strongly dependent on pH. Therefore, decreasing the pH
CH3 COO þ 4H2 O ! 2HCO3  þ 9Hþ þ 8e (3) makes the reaction more favorable. For practical application, the
wastewater containing Cr6+ can be mixed with acid cleaning
And then electrons were transferred to anode and finally to wastewater which is also discharged from electroplating
cathode through the circuit, while proton was transferred to industry to decrease the pH value. Thus, no additional chemicals
are needed in the treatment process. Also, a continuous operation
Table 1 was conducted in sequencing batch model for three cycles
Cr6+ removal reported in the literatures and that obtained in this study without significant reduction in capacity for power generation
Methods Initial Removal Reference and Cr6+ removal. These suggested that MFC should be an
concentration (%) economical and sustainable method for removing Cr6+ from
(mg/l) electroplating wastewater. The electricity produced by MFC can
Nanofiltration 17.09 96.6 [32] be used for monitoring the process. The high output power
Biosorption 30 86.61–91.03 [33] density and efficient removal of chromium makes this MFC
Biosorption 100 95 [34] treatment process useful not only for treating pollutants but also
Fluidized zero valent 534 99.9 [35] for electricity production. In addition, trivalent chromium oxide
iron process
recovered in MFC treatment systems following purification can
Combined electrocoagulation– 10 97 [36]
electroflotation have additional market value. Thus, the system may also be
Electrocoagulation 24 92 [37] applied in a metal recovery process. The system used here was a
Biosorption by surfactant 20 96 [38] very basic type of MFC that has been used to examine factors that
modified coconut coir pith
can increase power generation in these types of applications.
Microbial fuel cells 204 99.5 This study
However, the development of an economical treatment system
 Z. Li et al. / Process Biochemistry 43 (2008) 1352–1358
Fig. 11. SEM image of (A) plain cathode and (B) surface of cathode in the MFC using
potassium dichromate as electron acceptor (500 ppm potassium dichromate pH 2,
reacting time of 35 h).
will require a system architecture that is scaleable. Improve-
ments in system architecture are under investigation and will be
reported in due course.
3.6. Characteristics of the cathode surface
SEM images clearly show deposits formed on the surface of the
cathode (Fig. 11). To identify the chemical form of those deposits
Fig. 12. XPS analysis for the surface of the cathode (500 ppm potassium dichromate
pH 2, reacting time of 35 h).
1357
on the graphite paper, XPS analysis was applied. As shown in
Fig. 12, binding energies peaks corresponded to 575.6 eV, pointing
to a fact that Cr2O3 was the main cathode products [40].
4. Conclusion
Treatment of electroplating wastewater containing Cr6+ and
production electricity was carried out successfully in the cathode
chamber of dual-chamber microbial fuel cell. pH value affected the
power density and chromium removal obviously and the optimal pH
value was 2. In addition, higher concentration of Cr6+ could enhance
the power density. Compared with carbon paper and carbon felt
cathode, the graphite paper cathode showed the best performance
on chromium removal and electricity generation. During the 25 h
treatment of real electroplating wastewater containing 204 ppm
Cr6+, the maximum power density generated was up to 1600 mW/
m2 accompanied by 99.5% of Cr6+ and 66.2% of total chromium
removal, respectively. The removal of chromium from wastewater
was mainly due to the deposition of Cr2O3 on the surface of cathode.
The considerable high power density, higher Cr6+ concentration
tolerance compared to other biological treatment and no hazardous
waste sludge production demonstrated that microbial fuel cell
was a promising technology to treat electroplating wastewater and
simultaneously generate electricity.
Acknowledgements
The authors would like to acknowledge financial support for
this work provided by the National Science Foundation of China
(Nos. 20576120, 90610005 and U0633003), project of Zhejiang
Province (No. 2007C13061) and ‘‘86300 project of China (No.
2007AA06Z339).
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