groundwater by electrodialysis
Cite as: AIP Conference Proceedings 1788, 030090 (2017); https://doi.org/10.1063/1.4968343
Published Online: 03 January 2017
Nasrul Arahman, Sri Mulyati, Mirna Rahmah Lubis, Ryosuke Takagi, and Hideto Matsuyama
The study of membrane formation via phase inversion method by cloud point and light
scattering experiment
AIP Conference Proceedings 1788, 030018 (2017); https://doi.org/10.1063/1.4968271
© 2016 Author(s).
Removal Performance of NO3- Ion from Groundwater by
Electrodialysis
Nasrul Arahman1, a), Sri Mulyati1, b), Mirna Rahmah Lubis1, c),
Ryosuke Takagi2, d), and Hideto Matsuyama2, e)
1
Department of Chemical Engineering, Syiah Kuala University, Banda Aceh 23111, Indonesia
2
Department of Chemical Engineering and Science, Kobe University, Rokkodai Cho, 1-1, Nada, Kobe, Japan
a)
Corresponding author: nasrular@unsyiah.ac.id
b)
sri_nafidz@unsyiah.ac.id
c)
mirna@che.unsyiah.ac.id
d)
takagi@harbor.kobe-u.ac.jp
e)
matuyama@kobe-u.ac.jp
Abstract. An excess amount of nitrate in drinking water is harmful to body health. A batch type of electrodialysis (ED)
which is consist of cation and anion exchange membrane has been used to separate a model of nitrate ion from
groundwater by using ten pairs of cation/anion exchange membrane. The objective of this research is to investigate the
effect of initial concentration feed solution on the separation performance of nitrate ion by electrodialysis. Also, the effect
of applied current in ED on the nitrate permeability is also studied. Experimental results indicated that the decrease of
nitrate concentration in the dilute compartment is significantly influenced by the applied current. The amount of nitrate
passing through the membrane increases linearly by increasing amount of current. The initial feed concentrations do not
influence on the removal rate of nitrate as a function of membrane surface area.
INTRODUCTION
Water is a basic necessity for humans and other living beings. To maintain a healthy life, humans need healthy
water that contains minerals in adequate amount as recommended by health standards. Water shortage has become a
serious issue that concerns humanitarian agencies all over the world [1]. Water shortage issue arises from the
scarcity of raw water sources that can be processed into clean water. Water scarcity is severely suffered by those
located in the areas affected by natural disasters such as floods and tsunami. In those areas, both surface and ground
water are often contaminated by some contaminants including fluoride and nitrate.
An appropriate content of ions or mineral in drinking water is necessary for human body. An example of
requiring ion for the human body is fluoride. It is an essential micronutrient for human beings, to strengthen the
apatite matrix of skeletal tissues and teeth [2]. Otherwise, an elevated level of fluoride in drinking water bring about
the negative impact on the human body. The maximum fluoride ion level in drinking water recommended by World
Health Organization (WHO) and the Indonesian drinking water standard is 1.5 mg/l [1,3]. High concentrations of
fluoride in drinking water result in fluorosis (dental/skeletal abnormalities), cognitive impairment problem, anxiety,
depression, and several neurological damages [2,4]. In many cases in the word, groundwater contains fluoride in
high concentration over the standard. Other ions such as nitrates are also found together in groundwater. These ions
should be considered as an affected parameter on removal efficiency of fluoride in water treatment processes by
electrodialysis. Nitrate concentrations in surface water and groundwater increase significantly in almost all regions
of the world as a result of penetration of nitrate from agricultural fertilizers into the soil [5,6]. The maximum limit of
nitrate concentration in drinking water recommended by the World Health Organization (WHO) is 50 mg/l for
adults and 15 mg/l for children [7]. Excessive consumption of nitrate in drinking water for adults can disrupt the
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reproduction system and increase the risk of cancer because of nitrosamines or nitrosamides. For infants,
overconsumption of nitrate can cause methemoglobinemia or well-known as blue-baby syndrome [5,7].
Separation of an ion from feed stream using membrane technology has been introduced widely in the treatment
of surface water or groundwater[8–10]. Electrodialysis is one of the useful methods for removal of ions from raw
water sources, which can provide higher removal rate and has a less fouling problem [11–13]. In this work, the study
is mainly focused on the removal of nitrate from groundwater by using a cation-anion exchange membrane. The
principle concept of desalination via cation-anion exchange membrane is illustrated in Fig. 1. The figure shows a
typical arrangement of electrodialysis cells, consisting of a series of anion and cation exchange membranes arranged
in an alternating pattern between an anode and a cathode to form individual cells. A cell consists of a volume with
two adjacent membranes. The schematic diagram of cation-anion exchange membrane in the industry is designed
with several pairs of cation and anion membrane. In this study, a batch system of electrodialysis apparatus is used
for removal of nitrate ion from water. The effect of initial feed concentration of nitrate and the applied current has
been investigated.
EXPERIMENTAL METHOD
Membrane Configuration
A standard cation/anion exchange membrane set provided by ASTOM Corp. Japan was used for ED experiment
to separate nitrate from synthetic groundwater. A selective monovalent anion membrane was also used for ED
module to remove nitrate from real groundwater. Before used, the membrane was rinsed for 24 hours in deionized
water produced by an Elix System (Milli-Q Water). Both standard and monovalent selective membranes consisted
of ten pieces of cation exchange membrane and ten pieces of anion exchange membrane. Those membranes were
configured in parallel as shown in Fig. 2.
Electrodialysis Procedure
Separation of nitrate ion from synthetic or real groundwater by using cation-anion exchange membrane was
carried out in mini scale electrodialysis apparatus provided by Astom Corp. Japan. All experiment series was set up
at room temperature (25 ± 1oC). A detail description of experimental design was shown in Fig. 3. This apparatus
was composed of a stack and three compartments of diluted, concentrated, and electrodes with the volume of 500
ml, respectively. The stack consisted of 10 pairs of anion and cation exchange membranes with each available
membrane surface area of 55 cm2. Nitrate sample in feed solutions was prepared by dissolving of NaNO3 (WAKO
Pure Chem. Ind., Osaka, Japan) in deionized water. NaNO3 (4 wt%) was also used as an electrolyte solution. Water
in dilute and concentrated compartments was collect every three minutes, and the concentration of nitrate was
analyzed by using an ion analyzer (IA-300, DKK-TOA Corp. Japan).
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FIGURE 2. Detail of electrodialysis system in membrane stack [14].
FIGURE 3. Electrodialysis apparatus consists of membrane stack and three solution compartments
NO3 Removal
Some removal ions from feed solution to the concentrated compartment is one of the key performances of the
desalination process. The concentration of ions in water samples such as fluoride, chloride, and nitrate in feed
compartment is expected to be decreased after passing the membrane in electrodialysis (ED). In this work, the
electrodialysis performance is studied by analyzing of nitrate concentration in the diluted and concentrated
compartments every three minutes.
6 10
(a) (b)
5
8
Change of NO (meq)
Change of NO (meq)
4
3
6
3
3
4
2
2
1 decrease of feed / meq decrease of feed / meq
increase of conc. / meq increase of conc. / meq
0 0
0 10 20 30 40 50 0 20 40 60 80 100
Time (min) Time (min)
FIGURE 4. Change of amount of nitrate ion during electrodialysis operation in the diluted and concentrated compartments.
Initial NO3 in feed solution of 0.01 eq/L (a), and 0.02 eq/L (b).
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The changes in nitrate concentration against operation time are shown in Fig. 4. The concentrations of initial
nitrate are 0.01 and 0.02 eq/L, and the applied current is 0.02 A. In the case of the initial concentration of nitrate was
0.01 eq/L, the tendency of ion decreases in the dilute compartment was exactly similar to the increases in ion
concentration in the concentrated compartment. However, a slight increase of the nitrate in the concentrated
compartment was noticed when the initial concentration of ion is 0.02 eq/L. Based on Fig. 4 (a) and (b), it can be
explained that the initial concentration of nitrate ions determined the desalination period. As shown in Fig 4(a),
desalination process was finished after 47 minutes when the initial concentration of nitrate was 0.01 eq/L. More
desalination time was required to separate the ion from dilute compartment to concentrated compartment when the
initial concentration of nitrate was 0.02 eq/L as shown in Fig 4(b). In this case, the concentration of nitrate in dilute
compartment reached zero after 81 minutes of the desalination process. Figure 4 also shows that in both initial
concentrations of nitrate, ions were removed from the diluted compartment linearly throughout time.
0.15
0.1
0.05
3
0
0 5 10 15 20
2
Applied current (A/m )
FIGURE 5. Nitrate versus applied current of ED in the difference of initial feed concentration.
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explains the effect of membrane type on the removal profile of nitrate by ED process. Nitrate ion migrates faster
through selective cation/anion exchange membrane. The initial concentration of nitrate in feed solution is 95.53
mg/L. In the final stage of ED process, amounts of nitrate remained in the dilute compartment are 4.95 and 0.39
mg/L by using standard and selective membrane, respectively. They correspond to removal efficiency of 94.82 and
99.90%.
120
Selective Membrane
100
NO concentration (mg/l)
Standard Membrane
80
60
40
3
20
0
-5 0 5 10 15 20 25
Time (min)
FIGURE 6. Time courses of the nitrate concentration during ED with different membrane type
CONCLUSION
Electrodialysis was performed to study the nitrate removal from synthetic and real groundwater. The study was
focused on the effect of applied current and initial concentration of an ion in a dilute compartment on the removal
performance of nitrate ions. It was found that the removal performance of nitrate through the membrane was only
affected by applied current. The permeability of ion was exactly similar to a system with an initial concentration of
0.01 and 0.02 eq/L. Furthermore, the ED module designed in this work was used to remove a high concentration of
nitrate from real groundwater. By using selective membrane for monovalent anion membrane, a 99.90 % nitrate was
successfully separate from the dilute compartment. Thus, the ED process in this work was useful to produce
drinking water.
ACKNOWLEDGEMENTS
We would like to thank the Directorate General of Higher Education, Ministry of Research, Technology, and
Higher Education, Indonesia for funding support of this research.
REFERENCES
1. World health organization (WHO), Guidelines for drinking-water quality, Guidel. Drink. Qual. Third Ed. Inc.
First Second Addenda, Vol. 1 Recomm. Geneva. (1997).
2. K.D. Brahman, T.G. Kazi, H.I. Afridi, S. Naseem, S.S. Arain, N. Ullah, Water Res. 47, 1005 (2013).
3. Permenkes, Regulation of The Minister of Health Republik Indonesia, No. 492/Menkes/PER/IV, (2010).
4. F. Liu, J. Ma, H. Zhang, P. Liu, Y.P. Liu, B. Xing, Physiol. Behav. 124, 1 (2014).
5. L.J. Banasiak, T.W. Kruttschnitt, A.I. Schafer, Desalination 205, 38 (2007).
6. K. Govindan, M. Noel, R. Mohan, J. Water Process Eng. 6, 58 (2015).
7. M.H. Ward, J.D. Brender, Drinking Water Nitrate and Health, Encyclopedia of Environmental Health. 167-178
(2011).
8. N. Arahman, S. Mulyati, M.R. Lubis, F. Razi, R. Takagi, H. Matsuyama, Membr. Water Treat. 4, 355 (2016).
9. N. Arahman, Int. J. Appl. Eng. Res. 9, 10453 (2014).
10. X. Shengji, L. Xing, Y. Ji, D. Bingzhi, Y. Juanjuan, Desalination. 222, 497 (2008).
11. C. Cheng, N. White, H. Shi, M. Robson, M.L. Bruening, , Polym. 55, 1397 (2014).
12. H.J. Lee, M.K. Hong, S.D. Han, S.H. Cho, S.H. Moon, Desalination. 238, 60 (2009).
030090-5
13. R. Takagi, S. Mulyati, N. Arahman, Y. Ohmukai, T. Maruyama, H. Matsuyama, Desalin. Water Treat. 34, 25
(2011).
14. ASTOM Corporation, Cautions on safety, Micro Acilyzer S3, Electrodialyzer, Operation Manual. (2009).
15. N. Parsa, A. Moheb, A. Mehrabani-Zeinabad, M.A. Masigol, Che. Eng. Res. Des. 98, 81(2015)
16. Z. Ma, Y. Yang, X. Lian, Y. Jiang, B. Xi, X. Peng, K. Yan, Sci. Total Environ. 563-564, 593 (2016).
17. Z. Zhang, A. Chen, Sep. Purif. Technol. 164, 107 (2016).
18. A. Me nció, J. Mas-Pla, N. Otero, O. Regàs, M. Boy-Roura, R. Puig, Sci. Total Environ. 539, 241 (2016).
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