Desalination 249 (2009) 279285

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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

Treatment of sea water using electrodialysis: Current efciency evaluation

Mohtada Sadrzadeh, Toraj Mohammadi
Research Center for Membrane Separation Processes, Department of Chemical Engineering, Iran University of Science and Technology (IUST), Narmak, Tehran, Iran

a r t i c l e

i n f o

a b s t r a c t
In this paper, desalination of seawater using a laboratory scale electrodialysis (ED) cell was investigated. At steady state operation of ED, the outlet concentration of dilute stream was measured at different voltages (26 V), ow rates (0.15.0 mL/s) and feed concentrations (500030,000 ppm). The electrical resistance of sea water solution in the dilute compartment was initially calculated using basic electrochemistry rules and average concentration of feed and dilute streams. Then, current intensity in each run was evaluated using Ohm's law. Finally, current efciency (CE) which is an important parameter in determining the optimum range of applicability of an ED cell was calculated. It was found out that, at ow rates larger than 1.5 mL/s, higher feed concentrations lead to larger values of CE. However, exactly opposite behavior was observed at lower ow rates. Increasing the feed ow rate increases CE to a maximum value then decreases it down to zero for all cell voltages and feed concentrations. In the case of higher feed concentrations, maximum values of CE are obtained at higher ow rates. As expected, in almost all experiments, CE increases by intensifying cell voltage. CE values of up to 48 indicate effective ion transfer across the ion exchange membranes in spite of low separation performance of the ED cell. 2009 Elsevier B.V. All rights reserved.

Article history: Accepted 27 October 2008 Available online 2 October 2009 Keywords: Electrodialysis Desalination Sea water Current efciency

1. Introduction Water is an important resource for use of mankind. It is essential for agricultural and industrial growth, as well as for supporting growing populations that require a safe drinking water supply. 97% of all water is found in oceans, 2% in glaciers and ice caps, and the rest in lakes, rivers and underground. Natural resources cannot satisfy the growing demand for low-salinity water with industrial development, together with the increasing worldwide demand for supplies of safe drinking water. This has forced mankind to search for another source of water. In addition, the rapid reduction of subterranean aquifers and the increasing salinity of these non-renewable sources will continue to exacerbate the international water shortage problems in many areas of the world. Desalination techniques are capable of providing the solution [1]. Desalination means the removal of fresh water from saline water. Many methods have been proposed for desalting saline water, but few were commercially used. The two most popular methods for classifying the well known desalination processes are as follows: 1. Processes in which desalination involves phase change. There are three main methods: Multi effect (ME) distillation Multistage ash (MSF) distillation Vapor compression (VC) distillation.

2. Processes in which desalination takes place without any phase change. These include the following two main methods: Reverse osmosis (RO) Electrodialysis (ED) ED is an electro-membrane process for separation of ions across charged membranes from one solution to another under the inuence of an electrical potential difference used as a driving force. This process has been widely used for production of drinking and process water from brackish water and sea water, treatment of industrial efuents, recovery of useful materials from efuents and salt production. The basic principles and applications of ED were reviewed in the literature [26]. CE is a key parameter that determines the optimum range of applicability of an ED cell. It also determines the required membrane area for a given application. CE takes into consideration all the undesirable phenomena occurring in the ED cell, such as the nonperfect permselectivity of membranes or physical leakage (leading to impurities in the products), that can be reduced by optimized ED cell design and membrane selection. CE is also lowered by shunt or stray currents running in the non-active cell areas. ED process can be operated at constant-current or constant-voltage modes. Literature review on investigation of ED process using CE values indicates that most researchers operated ED under constant-current mode [721]. ED cells with 220 compartments were applied and CE values were most frequently observed in the range of 6080 [713]. CE values near zero [1416], above 80 [1720] and even above 100 [21] were also reported. Most of the experiments were conducted at 298 K. In the present work, a constant-voltage mode was performed in a laboratory scale ED cell with three compartments. At rst, concentration

Corresponding author. Tel.: +98 21 77240496; fax: +98 21 77240495. E-mail address: torajmohammadi@iust.ac.ir (T. Mohammadi). 0011-9164/$ see front matter 2009 Elsevier B.V. All rights reserved. doi:10.1016/j.desal.2008.10.029

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of diluted middle compartment was measured using a conductometer. Then, electrical resistance of dilute stream and subsequently current intensity in each run were evaluated using basic electrochemistry rules. Finally, CE was calculated and applied along with SP for investigation of the ED cell performance at various operating conditions. 2. Theory CE is an important parameter that determines the optimum range of applicability of ED. CE is a measure of how effective ions are transported across the ion exchange membranes for a given applied current. It is calculated using the following equation: CE% = zFQ f Ci Co 100 NI 1

transport of species i, can be calculated from the molar ux of that species through the ED stack: ii = Fzi Ji 7

In an ideal ED membrane, all of the current is transported by the counterions. Their transport number is equal to 1, while the transport number of the excluded coions is equal to 0 [25]. Hence, neglecting coions transfer, the transport number of ions through a single ion exchange membrane is equal to CE [19,2629]. = ii = ti i 8

Where, Ci and Co are feed and dilute concentrations (mol/m3), respectively, z is the charge of ion, F is the Faraday constant (96,485 A s/mol), Qf is the dilute ow rate (m3/s), N is the number of cell pairs (1 in this study) and I is the current (A) [22,23]. It is also proven that the CE of a single ion exchange membrane is a measure of ionic transport across it for a given applied current. Based on the extended NernstPlanck equation, transport of ions through ion exchange membranes is determined by three contributions, an electrical migration, a diffusion and a convective term, respectively [3,24,25]: Ji = Ji;dif + Ji;ele + Ji;con Ji = Di dCi Fz C D dE + Ci Jv + i i i dx RT dx 2 3

For an ion exchange membrane pair, as in this study, CE is related to the transport number of cations and anions through CEM and AEM as follows [30,31]: CE% = t
CEM

+t

AEM

1 100

Assuming tCEM = tAEM = tIEM, the following equation is derived: t

IEM

zFQ f Ci Co + NI 2NI

10

Hence, it can be concluded that the transport number of ions through ion exchange membranes is itself dependent on CE, dilute ow rate and feed and dilute concentrations. 3. Materials and method 3.1. Materials An analytical grade salt (99.9% sodium chloride supplied by Merck) and deionized water were used in all experiments to produce solutions with wastewater qualities. The purpose of these experiments was to study the effects of voltage, ow rate and feed concentration on the ED cell performance. 3.2. Cell and membranes The ED cell was packed with a pair of cation and anion exchange membranes (CEM and AEM) and a pair of platinum electrodes (anode and cathode). Both electrodes were made of pure platinum. The area of each electrode was 4.2 4.2 cm2. The thickness of the dilution cell (center) was 4 mm and the thickness of each concentrate cell (left and right) was 3 mm. A schematic view of the applied ED cell is presented in Fig. 1. A sodium chloride solution is introduced into the three compartments. An applied direct current electric eld produces the transport of cations towards the cathode and anions towards the anode. During this transport, anions are able to permeate through the AEM, but are blocked by the CEM. The opposite behavior occurs with cations. As a result, water passing between the membranes is split into two streams. One is pure water (dilute), and the other is brine (concentrate). Since ED uses energy at a rate directly proportional to the quantity of salts to be removed, this process is more useful in desalting brackish water. AR204SXR412 and CR67, MK111 anion and cation exchange membranes supplied by Arak petrochemical complex and made by Ionics incorporated were used in all experiments. The effective area of each membrane was 6 6.5 cm2. IECs of anion and cation exchange membranes were 2.8 and 2.4 meq/g dry membrane, respectively. 3.3. ED setup ED setup consists of a feed tank (TK-01) where waste water is stored, two pumps (P-01 and P-02), a rectier (DC-01) and two globe valves (GB-01 and GB-02) to control the feed ow rate in three

Where Ci and Di are concentration and diffusion coefcients of species i. Neglecting diffusive and convective transport terms for commercially available membranes, only electromigration affects ion transport through ion exchange membranes: Ji = zi FCi Di dE dE = ui zi Ci F dx RT dx 4

Where, ui is ion mobility of species i. Transport number (ti) of a particular ion ( i) commonly expresses the fraction of current transported by these ions [25]: ti = zi Ji zi Ji
i

As can be noted from Eqs. (4) and (5), the transport number of an ionic species, depends on its concentration in solution (Ci) and its mobility (ui). Species with high mobilities and at high concentrations logically contribute most to the charge transport. The current density (i) of an ED cell, i.e. the electrical current (I) per area of one membrane sheet (Am) in the stack (cation or anion exchange membrane), is equivalent to the transport of electrical charges by the ion uxes through this membrane, as the ions are the carriers of the electrical charge inside the membrane stack. Every mobile ion species present in the stack contributes to the current density, as the electrical eld applied to the stack affects all charged species. Note that the ux of anions is in the opposite direction of that of cations, assuming that they both are only caused by the electrical eld. To calculate the current density from the ionic uxes, the charge zi of each species i has to be taken into account [25]: i = F z i Ji
i

The CE of an ED cell is dened as the ratio of the current used for an effective separation over the total current. The current used for the

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Fig. 3. Calibration curve of the conductometer. Fig. 1. Schematic view of an ED cell.

compartments of a self designed ED cell. A simplied diagram of the setup is shown in Fig. 2. As can be observed, the feed solution was passed through the dilute and concentrate compartments, based on once through operation. No cyclic regime was used. Concentrated streams were disposed of and diluted stream was collected for conductometric analysis. 3.4. Experimental design Experiments were conducted under the limiting current density at different feed concentrations (5000, 10,000, 20,000 and 30,000 ppm), ow rates (0.1, 0.3, 0.5, 0.75, 1, 1.5, 2, 3, 4 and 5 mL/s) and voltages (2, 4 and 6 V). Concentration of cations (Na+) only in the dilute compartment was measured at various operating conditions. Each experiment lasted for about 15 min to reach steady state condition. After that three samples were taken every 5 min and the average value was reported. Each experiment was repeated three times and the results were presented in average with a maximum deviation of 5%. 3.5. Analytical method In all the experiments, a conductometer (HANNA, model HI 8633, made in Portugal) was used to measure the amount of salt in the dilute aqueous solutions. Water conductivity directly depends on its salt content. This dependency (calibration curve of the conductometer) is shown in Fig. 3.

4. CE calculation In ED, the basic relations between current (I), effective electrical motive force (E) and system resistance (R) can be described by Ohm's law as I = E / NR. Now, mass transfer resistance in the cell should be considered. Four resistances can be taken into account in a single cell: Rcm, the resistance of cation exchange membrane; Ram, the resistance of anion exchange membrane; Rd, the resistance of dilute compartment and Rc, the resistance of concentrate compartment [3]. Neglecting the electrical resistance of ion exchange membranes compared with that of dilute and concentrate solutions, Rcm ; Ram Rd ; Rc , the cell resistance (R) can be expressed as follows: R = Rd + Rc 11

The electrical resistance of a solution can be expressed as a function of concentration. Electrical resistance increases with length and decreases with cross-sectional area [32,33]: R= h A 12

Where is the conductivity and proportional to concentration: = M Cave 13

Where Cave is the average concentration of feed and dilute streams (C = (Ci + Co) / 2) and M is the molar conductivity of the solution. For

Fig. 2. A simplied diagram of the ED cell.

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a concentrated solution of NaCl in water, as in this study, M is calculated by the following equation [34]: M = M 0:0082Cave + 0:0067Cave
0:5

14

Where M is the limiting molar conductivity, i.e. the molar conductivity in the limit of zero concentration (when the ions do not interact with each other). Kohlrausch expressed M as the sum of contributions of individual ions. If the limiting molar conductivity of cations is denoted + and that of anions is denoted , his law of the independent migration of ions is: M = v + v

15
Fig. 5. CE as a function of feed ow rate and concentration at cell voltage of 4 V.

Where + and are the numbers of cations and anions per an electrolyte molecule (e.g. + = = 1 for NaCl, CuSO4, PbSO4, NaNO3 etc.). Limiting molar conductivities of Na+ and Cl are 50.08 10 4 and 76.31 10 4 m2S/mol, respectively [34]. Substituting z = 1; N = 1; C0 = 0.0854, 0.1709, 0.3418 and 0.5128 mol/L; Qf = 0.1 10 6 5 10 6 m3/s; E = 2, 4 and 6 V in the above equations, CE values calculated to be in the range of 0.13 47.54. It should be noted that the dilute concentration was measured in each run. Low CE values indicate inefcient performance of the ED cell to separate salt ions which in itself is due to the poor combination of operating parameters, water splitting in the dilute or the concentrate streams, shunt currents between the electrodes, or back-diffusion of ions from the concentrate compartment to the dilute compartment. 5. Results and discussion As mentioned, with the aid of basic electrochemistry rules, the electrical resistance of sea water solution in the dilute compartment was calculated for each run. Then, current intensity was evaluated to be in the range of 1.7730.62 mA, using Ohm's law. By replacing current intensity, feed ow rate and feed and dilute concentrations in Eq. (1), current efciency in each run was nally calculated. The effect of ow rate on CE at various feed concentration and cell voltages is shown in Figs. 46. According to these gures, increasing the feed ow rate increases CE up to a maximum value then decreases it down to zero. The ow rate at which the maximum value of CE is obtained is completely dependent on the values of feed concentration and cell voltage. When feed concentration is in the range of 500020,000 ppm, maximum CE is achieved at ow rates lower than 1 mL/s. At higher feed concentrations (up to 30,000 ppm), CE reaches to a maximum value at ow rates larger than 1 mL/s. Using feed solutions with a concentration of 30,000 ppm, maximum values of CE were observed to be 17.4, 10.8 and 8.0 at 1.5, 1 and 1 mL/s and 6, 4 and 2 V, respectively. At a cell voltage of 6 V and ow rates lower than 1 mL/s, the maximum value of CE is obtained at minimum feed

concentration (5000 ppm). Decreasing cell voltage to lower than 4 V, feed concentration at which CE is maximized becomes larger (10,000 and 20,000 ppm). At ow rates higher than 1.5 mL/s, maximum CE is acquired using more concentrated feed solutions (30,000 ppm). Based on Eq. (1), this behavior is attributed to the dual effect of operating parameters on CE and separation performance of the ED cell (C iC o). It should be noted that, at all cell voltages, maximum and zero values of CE shift to the right (or the curves' domain becomes wider) at higher concentrations. As mentioned before, at higher cell voltages (i.e. 6 V), using dilute feed solutions results in larger CE values. It is due to this fact that applying high voltages during ED of concentrated solutions intensies the concentration polarization phenomena and consequently reduces CE values. Increasing feed ow rate obviously moderates the effect of concentration polarization. Hence, at higher ow rates CE increases with increasing feed concentration, which is logically expected due to the reduction of electrical resistance of the solution. At a constant cell voltage, reduction of electrical resistance accelerates the transfer rate of ions from the dilute compartment towards the concentrate compartment which subsequently decreases the outlet concentration of the dilute stream (Co). A decrease in the cell electrical resistance also leads to an increase in the current intensity (I) value at a constant cell voltage. However, the rate of ions transfer through ion exchange membranes is greater than that of current intensity increase. Hence, according to Eq. (1), CE increases. Figs. 79 indicate variation of CE with feed concentration at different cell voltages and at ow rates lower than 0.1 mL/s. As can be seen, when lower voltages are applied maximum values of CE is obtained at higher feed concentrations and vice versa. This result is attributed to the reduction of concentration polarization effects at these operating conditions as discussed before. Effect of cell voltage on CE at various feed concentrations and at ow rates smaller than 1 mL/s is shown better in Figs. 1013.

Fig. 4. CE as a function of feed ow rate and concentration at cell voltage of 6 V.

Fig. 6. CE as a function of feed ow rate and concentration at cell voltage of 2 V.

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Fig. 7. Effect of feed concentration on CE at various feed ow rate and cell voltage of 6 V.

Fig. 10. Effect of cell voltage on CE at feed ow rates smaller than 1 mL/s. Feed concentration = 5000 ppm.

According to these gures, increasing cell voltage (particularly from 4 to 6 V) enhances CE values at almost all ow rates and all feed concentrations except for 20,000 ppm. It should be noted that in the ED of a much concentrated solution (C > 20,000 ppm) at lower ow rates, increasing cell voltage has a negligible effect on CE. Hence, a slight decrease or increase in CE values when solutions with concentration of 20,000 and 30,000 ppm are treated is ascribed to experimental errors.

Taking a closer look at Figs. 1013, it is found out that increasing feed ow rate up to the higher values (Qf > 0.5 mL/s) leads to the logical behavior of ED cell with regard to voltage variation. This nding is conrmed in Figs. 14 and 15. According to these gures, increasing cell voltage increases CE values at ow rates larger than 1 mL/s, unexceptionably. Maximum value of CE was 47.54 which was obtained at 6 V cell voltage, 10,000 ppm feed concentration and 0.75 mL/s feed ow rate. It is worthy to say that, the operating conditions at which optimum

Fig. 8. Effect of feed concentration on CE at various feed ow rate and cell voltage of 4 V.

Fig. 11. Effect of cell voltage on CE at feed ow rates smaller than 1 mL/s. Feed concentration = 10,000 ppm.

Fig. 9. Effect of feed concentration on CE at various feed ow rate and cell voltage of 2 V.

Fig. 12. Effect of cell voltage on CE at feed ow rates smaller than 1 mL/s. Feed concentration = 20,000 ppm.

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CE as presented in Eq. (1) is directly dependent on feed concentration (Ci), separation performance (CiCo), ow rate of handled solution (Qf) and inversely dependent on cell voltage. When an ED cell handles a great deal of brine with the minimum cell voltage (minimum energy consumption) and this results in a minimum concentration of the dilute stream (optimum separation performance), CE reaches to its maximum value. As a result, it can be concluded that the nonlinear behavior of electrochemical processes such as ED, leads to the above mentioned conguration of operating conditions to reach the maximum value of CE. 6. Conclusion The effect of operating parameters (cell voltage and feed concentration and ow rate) on the CE of a laboratory scale ED cell was investigated. The electrical resistance of sea water in the dilute compartment was calculated at rst. Then current intensity and nally current efciency in each run were evaluated. It was found out that increasing ow rate and feed concentration increases CE to a maximum value and further increasing decreases it. In both cases the ow rate and feed concentration at which maximum CE is obtained, depend on the cell voltage. At higher cell voltages, using dilute solutions as well as lower feed ow rates, results in high values of CE and vice versa. Using higher cell voltages (>6 V), average feed ow rates (0.75 < Qf < 1 mL/s) and lower feed concentrations (5000 10,000 ppm) is recommended, for the applied cell in this study, to achieve optimum values of CE. Maximum value of CE (47.54) which is obtained at 6 V cell voltage, 10,000 ppm feed concentration and 0.75 mL/s feed ow rate, conrms effective transport of ions through the membranes in spite of the low value of separation percent (3.92). Notation CE t u J i D z F C I N E h A Qf R M M

Fig. 13. Effect of cell voltage on CE at feed ow rates smaller than 1 mL/s. Feed concentration= 30,000 ppm.

values of CE are obtained are not exactly those where optimum separation performance is achieved. In the present work, maximum separation percent, (CiCo) / Ci, was measured to be 8.72 at 6 V cell voltage, 5000 ppm feed concentration and 0.1 mL/s. The CE value measured at this condition was 13.87. Poor separation performance of the applied ED cell in this study is due to the thickness of the dilute compartment. It is 4 mm which is almost ten times larger than that in commercially developed ED cells.

Fig. 14. Effect of cell voltage on CE at feed ow rates larger than 1 mL/s. Feed concentration = 20,000 ppm.

Current efciency Transport number Ion mobility (m2/sV) Molar ux (mol/m2s) Current density (A/m2) Ion diffusivity (m2/s) Valence Faraday constant (C/mol) Concentration (mol/m3) Current intensity (A) Number of cell pairs Electrical potential (V) Thickness of dilute compartment (m) Effective area of ion exchange membrane (m2) Feed ow rate (m3/s) Electrical resistance () Conductivity (S/m) Molar conductivity (Sm2/mol) Limiting molar conductivity (Sm2/mol) Molar conductivity of ions (Sm2/mol) Stochiometric constant

Fig. 15. Effect of cell voltage on CE at feed ow rates larger than 1 mL/s. Feed concentration = 30,000 ppm.

Subscripts M Molar ave Average d Dilute compartment cm Cation exchange membrane am Anion exchange membrane c Concentrate compartment i Inlet, species i o Outlet

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