Desalination 260 (2010) 23–28

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Desalination
j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / d e s a l

Removal of Mn2+ ions from synthetic wastewater by electrocoagulation process

Ashraf Shafaei a,⁎, Maryam Rezayee a,1, Mokhtar Arami b,2, Manouchehr Nikazar a,3
a
Chemical Engineering Department, Amirkabir University, Hafez Ave, Tehran, Iran
b
Textile Engineering Department, Amirkabir University, Hafez Ave, Tehran, Iran

a r t i c l e i n f o a b s t r a c t

Article history: Electrocoagulation (EC) process has been used as an effective method for the removal of a variety of
Received 20 January 2010 contaminants, especially heavy metal ions, from water and wastewater effluents. In this study, the removal
Received in revised form 3 May 2010 of Mn2+ ions from solutions has been studied by EC process with aluminium electrodes. The effect of
Accepted 4 May 2010
influential parameters such as initial pH, applied current density, electrolysis time, solution conductivity and
Available online 2 June 2010
initial metal concentration on the performance of EC process has been investigated. It was found that the
optimum initial pH to remove Mn2+ ions was 7.0. Also, the results indicated that increasing the current
Keywords:
Heavy metal
density and electrolysis time has a positive effect on the Mn2+ removal efficiency. The removal of Mn2+ ions
Manganese ion was not influenced by the solution conductivity but the electrical energy consumption decreased with an
Wastewater increase in the solution conductivity. In addition, the results of our study revealed that Mn2+ removal rate
Electrocoagulation process decreased with increasing the initial concentration of the contaminant. The by-products obtained from the
electrocoagulation process were analyzed and explained using SEM, EDAX and XRD.
© 2010 Elsevier B.V. All rights reserved.

1. Introduction The most widely used method for the treatment of metal polluted
wastewater is precipitation with alkaline solution and coagulation
Wastewaters containing heavy metal pollutants come from with Fe2(SO4)3 or Al2(SO4)3 with subsequent time-consuming
different industrial activities such as mining, power plants, plating sedimentation. Although precipitation is shown to be quite efficient
facilities and electrical equipment manufacturing. All heavy metals in treating industrial effluents, the chemical coagulation may induce
are toxic and non-biodegradable and should be separated from secondary pollution caused by the added chemical substances. These
wastewaters [1]. Manganese (Mn) is the second most abundant metal disadvantages encouraged many studies to use electrocoagulation for
in nature. It is an essential metal for the human system and many the treatment of several industrial effluents [14]. Electrocoagulation
enzymes are activated by manganese. Manganese has a variety of (EC) is an electrochemical wastewater treatment technology. Treat-
applications in ceramics, dry battery cells, and electrical coils and ment of wastewater by EC has been practiced for most of the 20th
manganese is an alloying element of many alloys. Intake of higher century with limited success and popularity. In the last decade, this
concentrations of manganese causes manganese psychosis, an technology has been increasingly used in the world for treating the
irreversible neurological disorder [2–4]. It is characterized by industrial wastewater and many studies conducted to optimize this
uncontrollable laughter, sexual excitement and impotence [2]. It is process for specific problems [15].
also reported to cause ‘manganese pneumonia’. Like most of the The EC process is based on the in-situ production of a coagulant by
metallic species, excessive supply of Mn to plants has detrimental anodic dissolution and, subsequently, produces aluminium or iron
effects [5]. Therefore, before the disposal of Mn containing industrial hydroxides in the contaminated water. In addition, cathodic reactions
wastes, their manganese content should be eliminated. There are allow for the pollutant removal either by deposition on cathode
several ways for the removal of manganese from water and electrode or by flotation (evolution of hydrogen at the cathode)
wastewater [6–13]. [16,17]. It has been shown that EC is able to eliminate a variety of
pollutants from water and wastewaters, such as suspended particles
[18], industrial wastewater [19], phenolic wastewater [20], refractory
organic pollutants including surfactants [21], COD removal [22], NOM
removal [23], dyes [24,25], restaurant wastewater [26], oil–water
⁎ Corresponding author. Tel.: + 98 21 64543200; fax: + 98 21 66405847. emulsions [27], fluoride [28] and heavy metal-containing solution
E-mail addresses: [email protected] (A. Shafaei), [email protected] [14,29–33].
(M. Rezayee), [email protected] (M. Arami), [email protected] (M. Nikazar).
1
Tel.: + 98 21 64543200; fax: + 98 21 66405847.
The electrolytic dissolution of the anode produces the cationic
2
Tel.: + 98 21 64542614; fax: + 98 21 66405847. monomeric species such as Al3+ and Fe3+. A range of coagulant
3
Tel.: + 98 21 64543192; fax: + 98 21 66405847. species and hydroxides is formed which destabilize and coagulate the

0011-9164/$ – see front matter © 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2010.05.006
24 A. Shafaei et al. / Desalination 260 (2010) 23–28

suspended particles or precipitate and adsorb the dissolved con-

taminants. It is well known that, in EC process, the main reactions
occurring at the aluminium electrodes during electrolysis are [17]:

(a): Anodic reactions:

3þ −
Al→Al þ 3e ð1Þ
þ −
2H2 O→O2ðgasÞ þ 4HðaqÞ þ 4e ð2Þ

(b): Cathodic reactions:

− −
2H2 O þ 2e →H2ðgasÞ þ 2ðOHÞðaqÞ : ð3Þ

Likewise, direct electrochemical reduction of metal cations (Mn+)

may occur at the cathode surface [14]:
nþ − 0
M þ ne →nM : ð4Þ
Furthermore, the hydroxide ions formed at the cathode increase
the pH of the wastewater thereby inducing the precipitation of metal Fig. 1. A schematic of EC cell.
ions as corresponding hydroxides and co-precipitation with alumin-
ium hydroxides [14]:
Dimensions of electrodes were 50 mm ×30 mm ×2 mm and the distance
nþ −
M þ nOH →MðOHÞn ↓ ð5Þ between two electrodes in EC cell was 10 mm in all experiments. The
electrodes were directly connected to a DC power supply (ESCORT, 3060
In addition, the electrolytic dissolution of the aluminium anode
TD Dual Tracking, Taiwan) providing 0–30 V (0–6 A) with galvanostatic
produces the cationic monomeric species such as Al3+ and Al(OH)2+
operational options for controlling the current density.
at low pH, which, at appropriate pH values, are transformed initially
into Al(OH)3 and finally polymerized to Aln(OH)3n according to the
2.3. Procedure
following reactions [15]:
3þ þ Before each experiment, the electrodes were abraded with sand
ALðaqÞ þ 3H2 O→AlðOHÞ3 þ 3HðaqÞ ð6Þ
paper, then dipped in HCL solution, cleaned with water, dipped in
nAlðOHÞ3 →Aln ðOHÞ3n : ð7Þ acetone for 5 min and finally put in oven in 110 °C for 30 min.
250 mL of the samples containing Mn2+ ion was transferred to the
However, depending on the pH of the aqueous medium, other EC cell. A steady temperature of 25 °C was maintained for all test runs.
ionic species such as dissolved Al(OH)2+, Al2(OH)4+ and Al(OH)4− The air speed was found to be sufficient to provide good mixing in the
hydroxide complexes may also be present in the system. The electrolytic cell and yet not strong enough to break up the flocs
suspended aluminium hydroxides can remove pollutants from the formed during the treatment process. The operation started when the
solution by sorption, co-precipitation or electrostatic attraction, current density was adjusted to a desired value. The samples were
followed by coagulation [14]. taken at regular time intervals, then filtered through 0.2 µm syringe
The aim of this research is to study the removal of Mn2+ ions by filter paper and the solution concentration was analyzed using atomic
the electrocoagulation process. The effect of important parameters absorption spectrophotometer (model Varian CP3800). Absorbance
such as time, initial pH, initial solution conductivity and applied was measured at the wavelength of 279.5 nm and spectral bandwidth
current density was examined. By-products obtained from the EC bath of 0.5 nm.
were characterized by SEM, EDAX and XRD analysis.
3. Results and discussion
2. Experiment
The data of different conditions were obtained and analyzed using
2.1. Materials and methods the parameter Re, as the C removal fraction (or efficiency in Re %) as:
 
Manganese sulfate monohydrate from Riedl-de Haën Company C0  C
Re = × 100 ð8Þ
was used to prepare the synthetic wastewater solutions. Sodium C0
chloride salt (Merck, 99.9% purity) was used to adjust the initial
solution conductivities. Initial pH of solutions was adjusted by NaOH where C0 and C are concentrations of Mn2+ ions at initial and time t in
and HCl solutions 0.1 molar (Merck). mg/L, respectively.

2.2. EC cell 3.1. Effect of pH

Experiments were carried out in a double-walled Pyrex batch One of the important parameters in the electrochemical process is
cylindrical EC cell with 250 mL capacity of aqueous solution. Water the initial pH of the solution. It has been established that pH has a
was circulated in jacket to keep the internal temperature of reactor considerable influence on the performance of EC process [16,20]. To
solution in the range of 25±2 °C. The cell lid was provided with ports for evaluate its effect, the pH of the samples was adjusted to the desired
the inlet and outlet of gases and sampling port. The solution was value by sodium hydroxide or sulfuric acid solution. The current
continuously aerated during the EC process. The experimental set-up is density was fixed at 6.25 mA/cm2 and the Mn2+ concentration was
shown in Fig. 1. Two aluminium (Arak Alopars Co. with 98% purity) 100 mg/L. The Mn2+ removal efficiency after 30 min of electrolysis, as
rectangular shape electrodes were installed vertically in the cell. a function of pH, is shown in Fig. 2. It can be seen that the initial pH has
 A. Shafaei et al. / Desalination 260 (2010) 23–28 25

Fig. 3. Effect of current density on the Mn2+ removal efficiency: tEC = 30 min;
Fig. 2. Effect of initial pH on the Mn2+ removal efficiency: CD = 6.25 mA/cm2; pH0 = 7.0; C0 = 100 mg/L.
tEC = 30 min; C0 = 100 mg/L.

aluminium and hydroxide ions generated at a given time, within the

a significant effect on the removal efficiency especially at low pH. As electrocoagulation cell and the current flow:
illustrated in Fig. 2, the removal efficiencies (Re) of manganese
reached the value as high as 70% when pH exceeded 4 but removal ItM
m= ð9Þ
yield lower than 13% was achieved at pH = 2. When the initial pH is zF
increased above 4, an insignificant change is seen in Re values.
The decrease of Re at a pH less than 4 and higher than 8 was where I is the current intensity, t is the time, M is the molecular weight
observed by many investigators and was attributed to an amphoteric of aluminium or hydroxide ion (g mol− 1), z is the number of electrons
behavior of Al(OH)3 which led to soluble Al3+ cations when the initial transferred in the reaction (3 for aluminium and 1 for hydroxide) and
pH is low, and to monomeric anions Al(OH)− 4 when the initial pH is F is the Faraday's constant (96,486 Cmol− 1). To study the effect of
high. These soluble species have insignificant effect on the EC current density on the Mn2+ removal efficiency, EC process was
performance. When the initial pH was kept in the range of 4–8, all carried out using various current densities in the range of 1.5–9.4 mA/
aluminium cations produced at the anode formed polymeric species cm2.
Al13O4(OH)7+24 and precipitated Al(OH)3 leading to a more effective Fig. 3 shows the Re against current density applied to the
treatment [18,33]. The Mn2+ removal efficiency exceeds higher than aluminium electrodes in the EC process. The Mn2+ removal efficiency
99.5% at pH N7.0, the results of which are not shown in Fig. 2. This increased from 35.8% at 1.5 mA/cm2 to 87.9% at 9.4 mA/cm2.
phenomenon might be ascribed to the precipitation of Mn hydroxide According to Faraday's law, the amount of Al3+ species formed by
at the cathode, which started at pH ∼7–8. the dissolution of the anode increases with the current density in the
In Table 1, the final pH of the treated samples after 30 min is EC cell. Therefore, higher current density will generate significant
reported. As observed by other investigators [33], the treatment amount of flocs, which in turn will trap the Mn2+ ions and enhance
induced an increase in pH when the initial pH was low. This might be the EC removal efficiency. The effect of current density on the removal
explained by the excess of hydroxyl ions produced at the cathode in efficiency of different contaminants was studied by other researchers
sufficiently acidic conditions and by the liberation of OH− due to the and the similar results were observed [19–33].
occurrence of a partial exchange of Cl− with OH− in Al(OH)3 [26].
3.3. Effect of operation time
3.2. Effect of current density
As mentioned, the efficiency of EC process depends directly on the
concentration of aluminium ions, which is produced by the electrode
In electrochemical processes, current density determines the
dissolution. In addition, the production rate of Al3+ ions is related to
coagulant production rate and the size and rate of the bubble
the time and current flow in the EC cell, according to Faraday's law
production and hence affects the growth of flocs on the EC [25]. The
(Eq. (9)). Fig. 4 shows the effect of electrolysis time on the Mn2+
Faraday's law explains the relationship between the amounts of
removal efficiency. The results indicated that the efficiency of Mn2+
removal increases from 34.1% after 10 min to 94.4% after 60 min.
Because when the operation time increases, an increase occurs in
concentration of Al3+ ions and their hydroxide flocs so the EC process
Table 1 yield is enhanced [25].
pH variation after EC (tEC = 30 min).

Initial pH Final pH 3.4. Effect of solution conductivity

2.3 5.21
4.0 6.47 The effect of solution conductivity on the removal efficiency of Mn2+
5.0 6.61 has been investigated using NaCl salt as supporting electrolyte. The
6.0 7.1 initial conductivity of solution was adjusted in the range 2.5–7 mS/cm
7.0 6.97
by adding NaCl. As seen in Fig. 5, the solution conductivity had little
26 A. Shafaei et al. / Desalination 260 (2010) 23–28

Fig. 4. Effect of operation time on the Mn2+ removal efficiency: CD = 6.25 mA/cm2; Fig. 6. Effect of solution conductivity on the cell voltage.
pH0 = 7.0; C0 = 100 mg/L.

positive effect on treatment efficiencies. The increasing Re can be related 3.5. Effect of initial Mn2+ ion concentration
to the increase of chloride ions in the solution. Chloride ions not only
increase the solution conductivity, but also decrease the passivity of the The removal efficiencies of Mn2+ ions after 30 min from the
electrodes by removing the passivating oxide layer form on electrode solutions of manganese sulfate at different initial concentrations by EC
surface [30] due to its catalytic action. It increases the availability of are shown in Fig. 8. It shows that after 30 min of EC with initial
aluminium hydroxide in solution. Therefore, it is expected that in the concentrations, 25, 50, 100, 150 and 400 mg/L about 98.1, 94.8, 78.2,
presence of higher Cl− ions, the concentration removal of Mn2+ ions 73.8 and 36.2% of Mn2+ ions are removed from aqueous solution.
should be more. Therefore, the Mn2+ removal efficiency is reduced by increasing the
In addition, it should be noted that the conductivity of the solution initial Mn2+ concentration. In addition, decreasing the efficiency of EC
affects the cell voltage and electrical energy consumption in EC cells. is considerable in higher initial concentration of Mn2+ (400 mg/L).
Figs. 6 and 7 show the effect of solution conductivity on the cell Even though the removal efficiency of process has decreased, the
voltage and electrical energy consumption, respectively. It is clear that amount of Mn2+ removed has increased when the initial concentration
the cell voltage decreased with an increase in the conductivity at of solutions increased. In other words, after 30 min of EC under identical
constant current density. When the conductivity of solution increases, operating conditions, 24.5, 47.3, 78.2, 110.7 and 144.8 mg of Mn2+ ions
IR-drop decreases, so the necessary voltage to reach on optimum are removed from the solutions when initial Mn2+ loadings were 25, 50,
current density will be diminished, and consequently the consumed 100, 150 and 400 mg, respectively. This can be explained by the fact that
electrical energy is decreased [25]. the amount of aluminium electrodes dissolution is not affected by the
initial Mn2+ concentration and at higher initial Mn2+ loading, number
density of Mn2+ ions is higher and consequently these ions have higher
chances of being trapped and removed (sweep coagulation) from the
solution by the hydroxide matrices. This is a probable cause for a slightly
higher removal of Mn2+ in case of higher initial concentration. In the

Fig. 5. Effect of solution conductivity on the Mn2+ removal efficiency: CD = 6.25 mA/
cm2; tEC = 30 min; pH0 = 7.0; C0 = 100 mg/L. Fig. 7. Effect of solution conductivity on the electrical energy consumption.
 A. Shafaei et al. / Desalination 260 (2010) 23–28 27

Fig. 10. SEM image of EC by-product.

surface, as it was shown in Fig. 9. As can be seen from this figure the
amount of deposited Mn on cathode surface is too low.
Fig. 8. Effect of initial concentration on the Mn2+ removal efficiency: CD = 6.25 mA/
cm2; pH0 = 7.0; tEC = 30 min.. 3.6.2. Characterization of the EC by-product
A gray precipitate was formed at the end of the EC process. To
study of Golder et al. on the removal of Cr3+ ions with EC, the similar illustrate the presence and the structure of the Mn particles which
results on the effect of initial Cr3+ concentration were observed [30]. were removed from the aqueous solution, the dried by-product was
characterized by SEM, EDAX and XRD analyses. The SEM image and
3.6. Characterization of the cathode surface and the EC by-products EDAX analysis graph of by-product are shown in Figs. 10 and 11. The
results show that the surface of this by-product was coated with a
The cathode surface was characterized by EDAX after EC process. layer of Mn species. Also, it was seen that the by-product was
The precipitate (solid phase) that formed during EC process was composed of elements like Al, Cl and Mn and the amount of
separated by filter paper at the end of the process. It was dried in an aluminium hydroxides was much higher than manganese element
oven and then ground to a fine powder. The by-product obtained from present in the EC by-product.
the EC cell was characterized by SEM, EDAX and XRD analyses. The EC by-product was analyzed by XRD to investigate the
Microscopic observation of dried solid by-product was carried out by a structure of manganese and aluminium components which was
scanning electron microscope (Philips XL30, Holland). The elemental removed from the aqueous solution. Fig. 12 shows the XRD pattern of
composition of the cathode surface and EC by-products was identified EC by-product. The results revealed that no peaks related to the
by energy dispersive X-ray analysis (EDAX) that was available in the manganese components have been observed in this spectrum. Also,
scanning electron microscope (SEM). the peaks related to the aluminium component are broad and diffuse.
The crystalline phase of the EC by-product was examined by XRD Therefore, the XRD results indicated that the manganese and
analysis. Powder XRD patterns were recorded by the use of an aluminium components which were formed in the EC flocs are
automatic powder X-ray diffractometer (Philips, PC-APAD, Diffraction amorphous [20,21].
software) using Cu Kα (λ = 1.5418 A°) radiation. The XRD scans were
recorded from 5° to 90° 2θ, with 0.08° step-width. 4. Conclusion

3.6.1. Characterization of the cathode surface In this study, the removal of Mn2+ ions from aqueous solution by
The objective of performing EDAX analysis on the cathode surface electrocoagulation was investigated using aluminium electrodes. The
is to investigate the possibility of direct deposition of Mn on cathode

Fig. 9. EDAX analysis graph of the cathode surface after EC process. Fig. 11. EDAX analysis graph of EC by-product.
28 A. Shafaei et al. / Desalination 260 (2010) 23–28

this project. The authors gratefully acknowledge Dr. M. Mirzazadeh

for the kind help on editing this manuscript.

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