Desalination 491 (2020) 114540

Contents lists available at ScienceDirect

Desalination
journal homepage: www.elsevier.com/locate/desal

Developments and future prospects of reverse electrodialysis for salinity T

gradient power generation: Influence of ion exchange membranes and
electrodes
Jaewon Janga, Yesol Kanga, Ji-Hyung Hanb, Kyunghoon Janga, Chang-Min Kima, In S. Kima,
⁎

a
Global Desalination Research Center (GDRC), School of Earth Sciences and Environmental Engineering (SESE), Gwangju Institute of Science and Technology (GIST), 123
Cheomdangwagi-ro, Buk-gu, Gwangju 61005, Republic of Korea
b
Jeju Global Research Center, Korea Institute of Energy Research, 200 Haemajihean-ro, Gujwa-eup, Jeju 63357, Republic of Korea

ARTICLE INFO ABSTRACT

Keywords: Salinity gradient power can be a very attractive renewable energy system because electricity is generated by salt
Reverse electrodialysis concentration difference between two solutions without any pollutant emission. The representative example of
Ion exchange membrane salinity gradient power is reverse electrodialysis (RED), in which there are many variables such as ion exchange
Electrode membrane (IEM), electrode, stack configuration, the structure of flow pathway, spacer, and solution con-
Blue energy
centration. This paper focuses on IEMs and electrodes that have not been covered in the previous review papers,
Renewable energy
as well as on the fundamental of the RED system and plant development for commercialization. In the part of
IEM, the characteristics that need to be intensively studied are analyzed and the studies have been conducted to
improve membrane property are summarized. In addition, the properties of major commercial IEMs and tailor-
made membranes are compared and analyzed, and the relationship between properties affecting membrane
performance is studied. In the part of the electrode, the main issues and materials of the electrode part in the
RED system are presented, and the recent researches related to the electrode of a large-scale RED system for
commercialization are summarized. Finally, this review suggests the future prospects and expectations for
salinity gradient power using the RED system.

1. Introduction fluctuating electricity output depending on climate and time. This

Humankind lives in an era of rapid technological development with
consuming a huge amount of energy. A worldwide energy crisis, en-
vironmental pollution, and climate change caused by the process of
energy obtaining are important issues for global society [1–3]. The risk
of energy resource depletion has been raised from the 1970s, we have
succeeded in delaying the time of resource depletion through the in-
tensive efforts such as improvement of resource treatment technology
and resource diversification. However, the main energy source is still a
fossil fuel and the resources will be depleted someday. Therefore, many
researchers have been working on the development of renewable en-
ergy technologies that can both address the energy crisis and continue
to be sustainable in the future. Renewable energy refers to energy
sources excluding oil, coal, natural gas, and nuclear power. Typical
technologies of renewable energy include photovoltaic power, wind
power, hydropower, geothermal power, wave power, tidal power, and
biomass [3–10]. These technologies have a critical disadvantage of
drawback is the fatal obstacle to replacing coal-fired power plants. The
energy storage system (ESS) can be used to store excess power for re-
ducing the waste of electricity, and the disadvantages of renewable
energy mentioned above are also compensated by using ESS, but the
efficiency of the ESS is still insufficient and the extra cost of operation
and maintenance is needed. Above all, photovoltaic, wind, and wave
powers, the amount of energy source itself critically changes depending
on the climate. Salinity gradient power is slightly affected by the cli-
mate, but the amount of energy source of this determined by the con-
centration difference between the two feed solutions. Therefore, the
renewable energy system that does not require the installation of an ESS
is recommended to replace the typical energy system. In other words,
the promising renewable energy system should be no dependence on
climate and time. Also, it must be possible to generate power using
semi-permanent energy resources without pollutant emissions during
operation.
The renewable energy that satisfies all the conditions mentioned

⁎
Corresponding author.
E-mail address: iskim@gist.ac.kr (I.S. Kim).

https://doi.org/10.1016/j.desal.2020.114540
Received 31 March 2020; Received in revised form 16 May 2020; Accepted 18 May 2020
0011-9164/ © 2020 Elsevier B.V. All rights reserved.
J. Jang, et al.
above is the salinity gradient power generation by reverse electro-
dialysis (RED). The salinity gradient power was first introduced on
paper in 1954s by R.E. Pattle, and it is the technology that derives the
electricity by potential difference from the salinity gradient between
seawater and river water [11]. The salinity gradient power is very
beneficial technology because it can continue to produce electricity
permanently regardless of climate and time at the place where sea and
river are in contact with each other, and there is no need to construct a
dike facility such as a dam. In addition, the salinity gradient power does
not emit carbon dioxide and other pollutants since it uses concentrate
and dilute as a resource. The electricity of 2 MW can be produced per
ton of water by the salinity gradient power, the amount of electricity
would be multiplied with high concentrations of brine such as the Dead
Sea. Potential power generation is expected to be 1.4–2.6 TW with
considering entire regions where proper to operate the salinity gradient
power plant in the world [12,13]. This amount is about 20% of global
energy demand.
2. Fundamentals of reverse electrodialysis and stack
configuration
RED is a stacking structure that consists of endplates, electrodes, ion
exchange membranes (IEMs), and spacers/gasket (Fig. 1a). The cation
exchange membrane (CEM) and anion exchange membrane (AEM) are
alternately arranged in a stack configuration, and each IEM is divided
by a spacer/gasket. To operate the RED system, the concentrate and the
dilute solutions should be supplied alternately in the cell. Also, the
electrode solution (ES) is circulated in the electrode part with a con-
stant flow rate [13–15]. The cations and anions contained in the water
(a)
Electrode Gasket
AEM CEM
Effective area Spacer
End plate
(b)
CEM CEM CEM
e─
Cathode
AEM AEM
Circulating electrolyte solution
Fig. 1. (a) Scheme of RED stack configuration composed with endplates, electrodes, IEMs, gaskets, and spacers. (b) Simple operation mechanism of the RED system.
2
Desalination 491 (2020) 114540
are moved in opposite directions through the IEM placed alternately,
and a potential difference is induced between the electrodes [13].
Oxidation and reduction reactions occur at each electrode by potential
difference as a driving force, thereby the charge transfer (or ionic
current) is converted to electric current (Fig. 1b) [14,16].
Fe2+/3+ and ferri-/ferrocyanide are commonly used redox couples
in a lab-scale RED system. Their fast charge transfer rate is an important
factor to get maximum power in a lab-scale RED stack where the con-
tribution of electrode resistance to the total internal resistance is rela-
tively significant. The reaction formulas with standard electrode po-
tential are shown below [17]:
Fe3 + + e Fe 2 +, E = 0.771
Fe (CN )36 + e Fe (CN )64 , E = 0.361
In the salinity gradient power system using RED, each part has its
own importance but the specific factors such as the electrode, IEM, flow
pathway, number of repeat unit stacks, concentrations of brine and
diluent have a critical impact on power generation performances. The
concentration difference between the concentrate and dilute is a pre-
requisite for the salinity gradient power, which determines the amount
of electricity can be generated by assuming the size of module and other
conditions are fixed. When the concentration difference between the
concentrated solution and diluted solution is fixed, however, the IEMs
and electrodes govern performances of the RED system. The IEMs and
electrodes can affect the ion separation and electrochemical redox re-
action, respectively [13,14,16]. The materials, morphology, thickness,
surface condition, and structures determine the properties of the IEM
and electrode, thereby these engineering parameters critically affect the
Repeat unit
Dilute out
Concentrate out
AEM
Concentrate in
Dilute in
End plate
e─ flow
Cation
CEM Anion
Cation flow
Anion flow
High salinity
e─
Low salinity
Anode
AEM
J. Jang, et al.
(a) (b)
Anion exchange membrane Cation exchange membrane
Fig. 2. Scheme of (a) AEM in which fixed positive charge is uniformly dis-
tributed in the polymer matrix and (b) CEM in which fixed negative charge is
uniformly distributed in the polymer matrix.
salinity gradient power production [14,16,18–24]. Therefore, this re-
view explores in more detail the IEMs and electrodes that affect electric
power generated from the RED system.
3. Ion exchange membranes for the reverse electrodialysis system
3.1. Classification of ion exchange membrane
IEMs are classified into the AEM and CEM. They are semi-permeable
membranes that transport co-ions while obstructing counter-ions and
neutral molecules. Fig. 2 shows schematically the matrix of AEM and
CEM with fixed charges on its body and mobile ions in the solution.
AEM with positively charged groups allows anions to pass through but
preclude cations going through the membrane. CEM with negatively
charged groups permits the passage of cations but rejects the passage of
anions [25]. Also, the IEMs were separated into strong acid/base and
weak acid/base membrane depending on the type of fixed charged
groups. Strong acid contains sulfone groups (–SO2–) as a charged group;
however, carboxylic acid (–COOH) is the fixed charged group for weak
acid membranes [26,27]. In the case of the base membrane, strong and
weak base membranes have quaternary and tertiary amines, respec-
tively [26].
IEMs can be classified into homogeneous and heterogeneous structures
depending on its fabrication method and physical structure (Fig. 3a and b).
In homogeneous membrane, the ion exchange part is directly provided
into the polymer matrix during the fabrication process. Furthermore, it can
be categorized into two parts according to their manufacture procedure:
(1) polymerization or polycondensation of monomers, which should
contain cationic or anionic moiety at least one (e.g. styrene-divinylbenzene
based ion-exchange membranes in Fig. 3c) [28], (2) starting from polymer
state, for example, polymer film (e.g. improved by either directly grafting
functional monomers with/without ionic property) and polymer solution
(e.g. blending cationic or anionic moieties) [28–30]. Heterogeneous IEMs,
on the other hand, have non-uniform charge distribution resulted from its
preparation method of blending or melting the charged ion-exchange resin
into the uncharged binding polymer, followed by pressing or casting into
the membrane [26,31]. In general, therefore, its mechanical strength is
higher than the homogeneous membrane, whereas electrochemical prop-
erties such as ion exchange capacity (IEC), permselectivity and areal re-
sistance (AR) are comparatively lower than that of the homogeneous
membrane [32]. However, these days, it shows improved electrochemical
properties by modifying the membrane surface, changing compatible
material, including additives that can enhance the electrochemical prop-
erties, membrane post-treatment, and pre-treatment [33].
3
Desalination 491 (2020) 114540
3.2. Characteristics and major parameters of ion exchange membrane
The chemical/electrochemical properties of the IEM can be mod-
ified and optimized by engineering the key parameters for the RED
system. From the phenomenological point of view, the IEM should have
excellent ability of ion exchange and low AR. These properties vary
depending on the type of functionality/fixed charge, charge strength,
and the structure of the IEM. Basically, fixed charge density (FCD) is an
important parameter to make an effective IEM. Permselectivity is also
an important factor, which membrane ability to separate ions from the
mixed solution depending on the nature or character of ions. These
parameters influence the performance of the IEM through interaction.
The IEM that exhibits excellent performance not always means it has
superior properties in all perspectives. The FCD and IEC must be a level
of 1.0 meq L−1 and 0.7 meq g−1, respectively, at least or higher for the
IEM to work properly in the devices. After the minimum characteristics
are satisfied, the FCD or IEC values and the membrane performance are
not directly proportional. In this case, other properties of the membrane
such as AR and permselectivity can significantly affect RED perfor-
mances. When the FCD or IEC value reaches a minimum level men-
tioned above, the lower the AR of the membrane, the better the per-
formance because the ions can move smoothly within the membrane.
Especially, if the cations and anions need to be separated in opposite
directions as in the case of RED, permselectivity has a great influence on
the final performance.
FCD is the calculation of fixed charge groups attached to the
backbone of polymer [26]. Also, it determines the transport of counter-
ions and the exclusion of co-ions through IEMs [35]. In CEM, for ex-
ample, the fixed negatively charged groups are in electrical equilibrium
with the mobile cations (counter-ions); however, in AEM, the fixed
positively charged groups are in electrical equilibrium with the mo-
vable anions. FCD is expressed in mili-equivalents of fixed groups per
water volume in the membrane (meq L−1 H2O) [30,35]. FCD is calcu-
lated by dividing IEC into swelling degree (SD) (Eq. (1)).
IEC
FCD =
SD (1)
IEC is the ion exchange ability of membrane which related to the
functionalities and number of fixed charged groups inside of the IEM.
IEC is shown as milli-equivalents of fixed groups per gram of dry
membrane (meq g−1) [26]. IEC is estimated by a general experimental
method that determines the number of counter-ions, for example, a
titration method is available to measure the number of released hy-
drogen ions and chloride ions for CEMs and AEMs by phenolphthalein
solution as an indicator, respectively [36,37]. In the case of CEMs, the
membrane is equilibrated using HCl solution for a specific time at room
temperature, followed by rinsing in DI water. After that, CEM was
dipped into NaCl aqueous solution to exchange the equilibrated hy-
drogen ions into sodium ions (in some cases, CEM has directly im-
mersed in NaCl solution without HCl treatment). The displaced hy-
drogen ions from the membrane were titrated with NaOH solution
[36,38]. In the case of AEMs, the membrane is immersed in NaCl so-
lution for a specific time to make chloride ions, followed by washing
them using DI water to eliminate the excessive NaCl solution from the
membrane. It is equilibrated by Na2SO4 solution to exchange chloride
ions for sulfate ion groups, and then the released chloride ions are ti-
trated by the AgNO3 solution [36]. In some cases, AEM is directly ti-
trated with NaOH solution after immersing in NaCl solution [39].
Therefore, the IEC values of CEMs and AEMs were calculated by the
following equations, respectively (Eqs. (2) and (3)):
CNaOH × VNaOH
IEC for CEMs =
Wdry (2)
CAgNO3 × VAgNO3 CNaOH × VNaOH
IEC for AEMs = or
Wdry Wdry (3)
J. Jang, et al.
Fig. 3. Schematic illustration of IEMs; (a) a homogeneous membrane and (b) a heterogeneous membrane with ion-exchange resin and binder polymer [34]. (c)
Chemical reactions of CEM and AEM styrene-divinylbenzene based IEM [28].
where CNaOH is the concentration of aqueous NaOH solution, VNaOH is
the volume of aqueous NaOH solution which used in a titration, CAgNO3
is the concentration of aqueous AgNO3 solution, VAgNO3 is the volume of
aqueous AgNO3 solution which used in a titration, and Wdry is the
weight of the dried membrane.
Permselectivity (α) is an ability of how well the IEM separates the
counter-ions and co-ions from the mixture solution [16]. When the
membrane is in contact with an electrolyte or mixture solution,
counter-ions can pass without any interruption; however, co-ions
cannot pass through the membrane due to the repulsion of the fixed
charge groups (i.e. Donnan exclusion effect) [26]. It is usually calcu-
lated by the ratio of measured membrane potential (∆Vmeasured) and
theoretical membrane potential (∆Vtheoretical). The static potential
method for ∆Vmeasured is carried out by using a two-compartment cell
4
Desalination 491 (2020) 114540
separated by a membrane. Two different concentrations of sodium
chloride solutions (0.1 M and 0.5 M) are injected into each compart-
ment and circulated along the sides of the membrane. The experimental
potential of membrane is measured using an external potentiostat or
multimeter with two Ag/AgCl reference electrodes [16,32,40]. The
theoretical membrane potential can be calculated from the Nernst
equation. Consequently, permselectivity can be calculated as shown in
the following equation (Eq. (4)):
Vmeasured
(%) = × 100
Vtheoretical (4)
AR is directly related to the energy consumption and ability of ion
transport in the membranes [41,42]. It is decided by the ion exchange
ability and the mobility of ions from the membrane matrix, and also
J. Jang, et al. Desalination 491 (2020) 114540

operating temperature and relative humidity influence on the AR

[51,57]
[57,58]
[26,43,44]. In general, it is measured in such a way that a membrane is

[57]
[36]
[16]
[40]
[61]
[51]
[62]
[62]
[62]
[63]
[26]
[16]

[26]
[59]
[60]
[61]
Ref.
located between the two-compartments of a cell with two electrodes and
these two-compartments are filled with 0.5 M NaCl aqueous solution
[40,45]. The AR of the IEM can be measured by impedance spectroscopy

Power density (W m−2)

at various temperatures and relative humidity conditions in a frequency
range from 7 M to 0.01 Hz [28,40,44–47]. The following equation (Eq.
(5)) was adopted to calculate the AR of membrane (Rmem) [42,48]:

0.305–0.328

0.21–0.46

0.34–0.58

1.43–1.52
0.96–1.06
(5)

0.9–1.27
Rmem = (Rcell Rsol ) × A

< 0.39
< 1.5
1.36

N.A.
N.A.
N.A.
N.A.

N.A.
N.A.

N.A.
N.A.
N.A.
2
where Rmem is the areal resistance of membrane (Ω cm ), Rcell is the re-
sistance measured with the membrane in the cell, Rsol is the resistance of
electrolyte solution without membrane, and A is the surface area of the

AR (Ω cm2)
membrane.

0.71–1.32
0.82–2.05
0.76–1.34
0.23–0.32

0.72–0.76
2.59–3.3
2.5–3.5
< 7.5
1.84
2.35
2.44
0.68

1.22
<8

N.A.
N.A.
N.A.
3.3. Modification of ion exchange membrane

2.3
Recently, Jin Gi Hong et al. suggested that the physical and elec-

Perm-selectivity
trochemical properties of commercial and tailor-made IEMs had inter-
connected, influencing the RED performances [36]. This study said that

42.0–59.5
79.2–90.3

85.4–95.5
90.7–91.6
84.7–89.0

85.5–90.7
91.4–93.8
the AR of membrane is the most important property in the RED system

42–62

89–90
> 90
> 90
since it was directly contributed the results of gross power density (e.g.

91.8

88.4

93.8
91.7
N.A.
90
95
the highest power density value of 0.59 W m−2 came from the lowest
AR value of 6.72 Ω cm2 in the RED system); furthermore, they found
that the AR was influenced by physical properties such as the SD and

FCD (meq L−1 H2O)

the thickness of the membrane. Therefore, it is necessary to look at
what factors can be engineered in order to improve the electrochemical

1.45–2.00

1.00–2.35
5.50–10.7
performances of commercial and tailor-made IEMs.

1.25–1.6
1.0–1.2
3.4–5.4
IEMs were modified for many years to optimize them into the RED

N.A.

N.A.
N.A.
N.A.
N.A.
N.A.
N.A.
N.A.
N.A.

N.A.
N.A.
system. Especially, it started with the development of AEM due to its 5.4

weakness. Early in 2000, the fabrication of AEM was only focused on a

fuel-cell application, and further AEM was hard to apply in the RED

32.2–53.5

93.7–128
100–148

121–179
system than CEM since its low permselectivity and high SD eventually
SD (%)

33–40

32–59
19–30
10–34
< 65
< 65
56.6

N.A.

N.A.
reduced the FCD property. To apply AEM in the RED system, the
147

32
19
18
32

electrochemical properties of AEM should be modified by changing the

ratio and type of inert materials. In 2012, the first tailor-made mem-
brane for the RED application was studied [16]. From that moment on,
IEC (meq g−1)

the IEMs have been developed dramatically.

0.97–1.50
1.32–1.88

1.67–2.26

1.76–2.66
1.48–1.93
1.08–2.89
1.26–1.39
1.0–1.54
0.8–1.0
1.5–1.8

The modification methods can be classified into four categories: (1)

1.84
1.77
1.62

0.29

N.A.
N.A.

chemical reaction by cross-linking or grafting [49,50], (2) coating on

2.2

1.8

the membrane surface [51,52], (3) pores filling with an electrolyte and
Comparison of the commercial and custom-made AEMs properties in RED system.

a cross-linker [53–55], and (4) blending nanoparticles [32,35,56]. Re-

Thickness (μm)

cent studies demonstrated the fabrication of AEM by using different

amounts of cross-linker (4,40-diaminobenzophenone, DABP). Qua-
145–200
160–230
120–150

ternary-aminated polystyrene (QPS) and quaternary-aminated poly

33–130

90–108
70–120
70–120
70–120
< 450
< 450

(phenylene oxide) (QPPO) were used as monomers to increase the hy-

126
134

138

112

55

55
17

25

drophilicity of the polymer matrix. The resulting of AEM had a lower

AR (0.69–1.67 Ω cm−2) than commercial membrane (2.58 Ω cm−2),
Quaternary Ammonium Radel

corresponding to a maximum power density of 1.82 W m−2 using ar-

Photocured AA resin/ATAC

tificial seawater (0.599 M NaCl) and river water (0.00856 M NaCl) as

PSS/PEI coated CJMA-2

Pore-filled polyethylene

feed solutions [49]. Gao et al. developed the surface layer for AEMs via
PES/PE, strong base
PP/PE, strong base

layer-by-layer (LBL) method with negatively charged poly(styr-

Aminated PECH

enesulfonate) (PSS) and positively charged poly(ethyleneimine) (PEI)

polyelectrolytes. The fabricated membrane with 7.5 bilayers (CJMA-2-
aPPO-CxDy
PDDA/PVA
PDDA-PVA
Materials

Aromatic
Aromatic

7.5) exhibited the best permselectivity and anti-organic fouling char-

aPPO-z
N.A.
N.A.
N.A.

N.A.

N.A.

acteristics. The transport number ratio between Cl− and SO42−

(PSO42−Cl ) was improved from 1.10 (pristine, CJMA-2) to 2.44 and the
−

antifouling potential also increased 30.29% higher than the CJMA-2

membrane. Consequently, the power density generation of the RED
Asahi Glass Selemion AMV

MEGA RALEX AM(H)-PES

Asahi Glass Selemion APS
ASTOM NEOSEPTA AM-1
ASTOM NEOSEPTA AMX

MEGA RALEX AM(H)-PP

Hefei Chemjoy CJMA-2

system has been improved by up to 17% [51].

Manufacturer & model

FUJIFILM AEM type 1

Technol. Dev. JAM-II

In 2019, Yang et al. reported a one-time roll-to-roll (R2R) pore-

filling method including pretreatment, impregnation, photo-poly-
merization, and polishing steps to improve the performances of CEMs
Tailor-made

and AEMs. First, they optimized the process parameters for each step
Table 1

(e.g. changing the line speed, ratio of photo-initiator, and surfactant

type). After that, they fabricated pore-filling cation exchange

5
J. Jang, et al. Desalination 491 (2020) 114540

membranes (PCEMs) with a width of 62.0 cm and thickness of 16 μm at

[32,36]
a line speed of 1 m min−1, and pore-filling anion exchange membranes

[26]
[66]
[50]
[66]
[67]
[26]
[16]
[26]

[36]
[65]
[56]
[64]
[55]
[50]
[52]
[66]
[67]
Ref.
(PAEMs) with a width of 57.5 cm and a thickness of 39 μm at a line
speed of 0.3 m min−1. The pore filled membranes exhibited higher IEC,
permselectivity, and AR than commercial membranes even when they

Power density (W m−2)

were manufactured on an industrial scale [53,54].
The comparison between commercial and tailor-made AEMs was
presented in Table 1 [16,26,36,40,51,57–63]. Basically, tailor-made

0.48–0.59

0.28–0.46
0.36–0.48

0.87–0.99
3.50–4.32
AEMs show relatively better physical and electrochemical properties

0.75–1.3

< 1.5
compared to commercial AEMs. Tailor-made AEMs are usually few tens

1.17

0.42

4.19
N.A.
N.A.
N.A.
N.A.

N.A.

N.A.

N.A.
0.8
of μm thick, but commercial AEMs are thicker than 100 μm, resulting in
lower resistance of tailor-made AEMs than the commercial one. More-
over, tailor-made AEMs which modified by surface treatment or struc-

AR (Ω cm2)

0.97–1.09
0.35–0.63
0.85–1.87
1.31–2.11
0.45–0.70
1.11–4.04
tural engineering show better FCD, IEC, and SD values than commercial

1.73–125

0.61–1.3
0.3–1.3
AEMs. Therefore, tailor-made AEMs have a relatively good result

< 10

0.82
1.67

2.29
1.91
<8
<8

2.7
compared to commercial AEMs in many factors, thereby tailor-made

3
AEMs are sufficiently competitive and it is expected to improve the
performance of the RED system (Table 1).

Perm-selectivity
In the CEM cases, Pal et al. fabricated the IEMs by controlling the

84.4–87.7

79.1–86.5

89.9–95.3
ratio between monomers and cross-linking agents. They evaluated

53–97

81–87

86–88
homogeneous phase crosslinked poly(acrylonitrile-co-2-acrylamido-2-

> 92

> 90
97.2

98.8
95.1

N.A.

N.A.

N.A.
N.A.
N.A.
92
95
methyl-1-propanesulfonic acid) (PAN-co-PAMPS) co-network CEMs
with controlling the molar ratio of monomers (AN and AMPS). By using
a PAN-PAMPS-1 membrane including 15 mol% PAMPS, the mechanical

FCD (meq L−1 H2O)

ability (tensile strength of 16.4 MPa) and electrochemical performance
(FCD of 0.757 meq cm−3, transport number of 0.92) of CEM showed

0.69–0.757
good results due to its fast phase mixing of ionic domains and hydro-

1.68–4.54
5.0–5.4
2.5–4.2
2.6–4.7

4.6–5.5

1.4–9.9
1.1–2.1
phobic domains [50].

N.A.

N.A.
N.A.

N.A.

N.A.
N.A.

N.A.
4.3
6.5
Yongsheng Chen's groups have attempted to modify the IEMs.
Especially, they conducted the nanoparticle blending in IEMs that were 9

organic-inorganic nanocomposite CEMs [32,35,56] such as sulfonated

45.6–93.9
36.9–68.6

21.8–49.6
16.2–51.4
Iron (III) oxides (Fe2O3-SO42−) [32,35] and sulfonated silica (SiO2-

20–157
SD (%)

20–26
15–51
21–34

20–26
< 65
< 70
< 45
SO3H) [56] to improve the IEC, permselectivity, and resistance. And,

46.6
16
20
18
20
16

they fabricated the organic-organic hybrid CEMs and AEMs as the

method of a chemical reaction through the sulfated polyvinyl alcohol
IEC (meq g−1)

(sPVA) as a hydrophilic polymer to have synergistic effects (e.g. im-

proves the permselectivity, membrane AR, and power density) with
1.00–1.40
1.88–3.07
0.78–1.18

1.77–2.28
0.91–2.33

1.57–1.98
1.4–2.05

0.7–2.2
organic polymers (e.g. sulfonated poly (2,6-dimethyl-1,4-phenylene

16–3.1
> 2.2

0.84
1.62
2.01
1.04
2.2
2.4

oxide) (sPPO) for CEMs, and poly (diallyldimethylammonium chloride)

2.3

(PDDA) for AEMs) [36,40,64]. In addition, they adopt the multi-walled

carbon nanotubes (MWCNTs) as an inorganic filler to enhance the IEC,
Thickness (μm)
Comparison of the commercial and custom-made CEMs properties in RED system.

hydrophilicity, and ion conductivity [55].

In specific cases, the coating method is more usable when improving (Swollen)
119–147
< 150
< 450
< 450

the monovalent permselectivity and antifouling of RED. When using

47–70

63–81
135
178
133
158
101
100

420

100

natural complex feed solutions, multivalent ions like Mg2+ and SO42−
50
30
50

occurred negatively effects to open circuit voltage (OCV) and power

density due to the ‘uphill phenomenon’ that not only reduced the
Sulfonated PVDF/ETFE/styrene/VBS

Polypyrrole/chitosan/FU-JI CEMT1

permselectivity of monovalent ions but also improved the resistance of

membrane. By using polypyrrole (PPy) and chitosan (CS) composites
under different concentrations of pyrrole (0.025–1 M) and poly-
Sulfonated PPO/MWCNT

merization time (0–8 h), the passage of multivalent ions was prohibited;
Sulfonated Fe2O3/PPO
Per-fluorinated nafion

UV-oxidized PMP/sPS
Sulfonated SiO2/PPO
Sulfonated PVA/PPO
PES/PE, strong acid

therefore, the modified membranes showed enhancement of OCV and

PP/PE, strong acid

Sulfonated PS/PE

power density with > 20% and 42% improvement compared to pristine
PAN-co-PAMPS

membranes, respectively [52].

Strong acid
Materials

Table 2 shows the comparison of important properties of the CEMs

between commercial and tailor-made membranes including above
N.A.
N.A.
N.A.
N.A.

N.A.

mentioned cases [16,26,32,36,50,52,55,56,64–67]. The Nafion made in

DuPont showed overwhelming power density with low AR value, and
commercial CEM showed better properties of IEC and FCD than tailor-
Asahi Glass Selemion CMV
Asahi Glass Selemion CSO
MEGA RALEX CM(H)-PES
ASTOM NEOSEPTA CM-1
ASTOM NEOSEPTA CMX

MEGA RALEX CM(H)-PP

Hangzhou Ionsep-MC-C

made CEM.
Manufacturer & model

FUJIFILM CEM type 1

DuPont Nafion 117

3.4. The relations between key parameters

Tailor-made

Several key parameters are used to evaluate the performance of

Table 2

IEMs used in RED systems, including thickness, FCD, IEC, permselec-

tivity, SD, AR, and power density, as shown in the table above. When

6
J. Jang, et al. Desalination 491 (2020) 114540

(a) (b) (c)

1.6
6 1.5

Power density (W m‒2)

Resistance (ohm cm2)

Power density (W m‒2)

1.2
4
1.0
0.8
2
0.5 0.4
0
0.0 0.0
0 50 100 150 200 250 0 3 6 9 12 15 0.0 0.5 1.0 1.5 2.0
Thickness (µm) Resistance (ohm cm2) IEC (meq g‒1)
(d) 6 (e) (f) 5

Power density (W m‒2)

Resistance (ohm cm2)

4
Power density (W m‒2)
4
4
3 3

2 2 2

1 1
0
0
0
0 100 200 300 0 5 10 15 0.0 0.5 1.0 1.5 2.0
Thickness (µm) Resistance (ohm cm2) IEC (meq g‒1)

Fig. 4. The relations between the key factors of IEM; (a) AR versus thickness, (b) power density versus AR, (c) power density versus IEC of AEM. (d) AR versus
thickness, (e) power density versus AR, (f) power density versus IEC of CEM [16,26,32,36,40,50–52,55–67].

Mesh electrode changed by membrane thickness. However, if the membrane is made

very thin to reduce the AR, the mechanical strength of membrane
would be decreased and the overall property may be deteriorated.
Therefore, it needs to find the optimized thickness of membrane or to
make a composite membrane [68]. Also, it is confirmed that the power
density of the RED system was increased as overcoming a minimum IEC
level of > 1.0 meq L−1 (Fig. 4c and f). It can be seen that typical
Electrode Shielding polymer materials also improve the power density of the RED system by
connector membrane enhancing the IEC property through surface treatment or compounding
with nano-materials such as graphene and MXene [69–73].

Endplate 4. Electrode systems for reverse electrodialysis

Spacer
Fig. 5. Cross-sectional structure of the electrode part in the RED stack cell.
engineering or modifying a specific part of an IEM, however, not all of
the key properties are changed in the direction of improvement, and
sometimes there is a serious trade-off relationship. If we difficult to find
an optimum condition, one strategy is to abandon factors that have less
impact on the RED performance and focus on more important proper-
ties. To focus on the main characteristic of the membrane, it is im-
portant to quantitatively understand the relation between the major
parameters. The relation between the major parameters in the above
comparison table was summarized as a graph in Fig. 4
[16,26,32,36,40,50–52,55–67]. Fig. 4a–c and d–f summarizes the
characteristics of CEM and AEM, respectively. In both CEM and AEM,
the AR is decreased as decreasing membrane thickness (Fig. 4a and d),
and the power density is increased as decreasing AR (Fig. 4b and e). In
other words, surface treatment or structural engineering according to
the specific application conditions is important to change the mem-
brane properties, but basically AR which affects the power density is
4.1. Overview
The electrode system plays an important role in converting ionic
current to electric current via an electrochemical reaction. In general,
the voltage loss (I ∙ Relectrode) in the electrode system originates from the
thermodynamic electrode potential (Eeq), overpotential (η), concentra-
tion polarization (Rcp), resistance of shielding membrane (Rshield), and
solution resistance (Rs) (Eq. (6)) [74].
I Relectrode = Eeq + + I Rcp + I Rshield + I Rs (6)
Because of the electrode resistance (Relectrode) is constant regardless
of the number of the cell pairs, however, the contribution of Relectrode to
the total internal resistance decreases as the number of cell pairs in-
creases. Therefore, Ag/AgCl reference electrodes have been utilized to
measure the actual power without energy loss due to redox reaction at
the electrode in lab-scale RED systems [13,14,74–80], and the reports
[81,82] focusing on the electrode system are relatively fewer than those
discussing other components mentioned previously. Also, Relectrode has
not been regarded as an important factor in determining the perfor-
mance of large-scale RED, unlike general electrochemical cells (e.g.,
fuel cell and battery).
However, considering the high voltage of the large-scale RED

7
J. Jang, et al.
system and inherent structure of the RED stack where ions come in and
out through a shielding membrane placed between the electrode solu-
tion (ES) and feed solution (FS) (Fig. 5), interactions between the ES
and multivalent ions in natural FS are expected to occur [18,80,83,84].
As a result, scaling and fouling can take place, which leads to an in-
hibition of the electrochemical kinetics and an increase in internal re-
sistance. This issue is a critical factor in the long-term operation and the
power production efficiency of a pilot-scale plant. Therefore, the se-
lection of suitable conditions for the electrode system is important for
guaranteeing good and stable performances of the RED system [85,86].
4.2. Pros and cons of representative electrode reactions
The representative electrode reaction and electrode materials are
briefly introduced in this section. We focus on the pros and cons of
these electrode systems when applied to a large-scale RED system with
an emphasis on safety, health, technical feasibility, and economics for
real application. Here, a large-scale RED refers to a system consisting of
several hundreds or thousands of cell pairs [87].
Veerman et al. classified the electrode reaction designed for la-
boratory use into two groups: with or without opposite electrode reactions
[23], a concept that was introduced in the previous reviews [30,88].
The electrode system with opposite electrode reactions is not accom-
panied by a net chemical reaction, which means zero Eeq for the net
chemical reaction. Therefore, the biggest advantages are that there is no
energy consumption and gas production. Fe2+/Fe3+ and [Fe(CN)6]4−/
Fe(CN)6]3− with inert electrodes are representative examples
[85,89–96] and suitable for a lab-scale RED with a small number of cell
pairs. According to the charge of the redox couple, an AEM or a CEM is
used as a shielding membrane to confine the redox couples in the
electrode compartments. Because the [Fe(CN)6]4−/Fe(CN)6]3− couple
decomposes into cyanide under sunlight and oxygen, Fe2+/Fe3+ is
regarded as the more stable redox species in pilot-scale systems [82].
However, it should be noted that the redox reaction is in competition
with water electrolysis because the large-scale RED produces a high
membrane voltage on the order of tens of volts, which is much larger
than the overpotential (~1.8–2.6 V) for water electrolysis [97]. This
means that the precipitation of iron compounds occurs around the
cathode where the pH is very high because of water reduction. In ad-
dition, there is a continuous loss of reactants owing to the imperfect
permselectivity of the IEM. Because the electric power of a RED-based
iron redox couple is susceptible to changes in the concentrations of the
reactants [81,85], pH control and high concentrations of the reactants
are very important for stable long-term operation. It is a major dis-
advantage in terms of economics and maintenance expenses that pH
monitoring is needed at all times and large amounts of reagents are
used.
Table 3
Typical electrode systems of reverse electrodialysis.
Anode Cathode Electrolyte
2+ 3+
1. Ti/Ru-Ir 1. Ti/Ru-Ir Fe /Fe in NaCl or Na2SO4
2. Graphite 2. Graphite
1. Ti/Ru-Ir 1. Ti/Ru-Ir Fe(CN)63−/Fe(CN)64− in NaCl
2. Graphite 2. Graphite
1. Ti/Ru-Ir 1. Ti/Ru-Ir NaCl
2. Carbon 2. Carbon
Ti/Pt Ti/Pt Fe(CN)63−/Fe(CN)64− in Na2SO4
Ag/AgCl Ag/AgCl NaCl
8
Desalination 491 (2020) 114540
Another electrode reaction is water electrolysis that generates hy-
drogen and oxygen at the cathode and anode, respectively, and is
classified as a without opposite electrode reaction. Chlorine evolution by
oxidation of Cl− ion should also be considered because the Cl− ions in
the FS diffuse to the electrode compartment through the shielding
membrane, and the electrochemical kinetics of chlorine evolution is
faster than water oxidation [17]. One of the drawbacks is the high loss
of energy from a net chemical reaction; a significant number of cells
should be used to overcome the cell equilibrium voltage before elec-
tricity production is possible. Therefore, these electrode reactions are
suitable for the large-scale RED where the contribution of Relectrode to
the total internal resistance is very small. Gas evolution is another
disadvantage because the mixture of hydrogen and oxygen is ha-
zardous, and chlorine gas is toxic and corrosive. However, because the
current density of the RED is ten times smaller than that of ED [26,98],
the low-pressure gases are expected. Also, the membrane assembly with
a thickness of at least dozens of centimeters spatially separates hy-
drogen and oxygen. It is worth noting that the decoupling of hydrogen
and oxygen evolution during water splitting has received considerable
attention [99–101], and the inherent structure of the RED system can
overcome the gas-mixing issue. Besides, water as a reactant is a safe
chemical substance that is free from concentration polarization [84,85].
Various sources such as tap water and wastewater can be used as the ES
without any chemical reagents. The main disadvantage is that an abrupt
pH change occurs near the electrodes, which causes inorganic scaling
and degradation of the spacer and IEM [83]. Therefore, further research
on new designs of the electrode compartment for suppressing the
abrupt pH change and development of an IEM that is highly resistant to
strong acid/alkaline is required. Recently, Han et al. demonstrated that
using a bipolar membrane (BPM), as a shielding membrane, is a feasible
solution for suppressing inorganic scaling around the cathode [18];
water splitting at the bilayer structure of the BPM blocks the crossover
of hydroxide and multivalent ions owing to electroneutrality.
Reversible ion adsorption/desorption between the electrolyte and
electrode surface can convert ionic flow to electron flow, called capa-
citive RED (CRED). Vermaas et al. used activated carbon as an electrode
material for CRED [102]. This study showed that the power density of
CRED is close to that of the stack with conventional Pt-coated Ti elec-
trodes in the Fe(CN)64−/Fe(CN)63− redox couple when using 30 cell
pairs. While a periodic switching of feed solutions was necessary to
prevent saturation of the capacitive electrode in their study, Liu et al.
showed that flow electrodes consisting of graphite brushes allowed
continuous power generation without switching of feed solutions [103].
An important advantage of CRED is environment-friendliness; it is quite
free from the negative environmental impact caused by leakage and
chlorine generation. However, thus far, the development of electrode
materials has been limited to lab-scale systems. Further research on
Electrode reactions Ref.
2+ 3+ −
Anode: Fe → Fe +e [81,82,85,94]
Cathode: Fe3+ + e− → Fe2+
Net: nil.
Anode: Fe(CN)64− → Fe(CN)63− + e− [14,89,90,93,112]
Cathode: Fe(CN)63− + e− → Fe(CN)64−
Net: nil.
Anode: 2Cl− → Cl2 + 2e− [58,113]
Cathode: 2H2O + 2e− → H2 + 2OH−
Net: 2H2O + 2Cl− → H2 + 2OH− + Cl2
Anode: Fe(CN)64− → Fe(CN)63− + e− [15,114]
Cathode: Fe(CN)63− + e− → Fe(CN)64−
Net: nil.
Anode: Ag + Cl− → AgCl + e− [110,115]
Cathode: AgCl + e− → Ag + Cl−
Net: nil.
J. Jang, et al.
Fig. 6. Photographic image of a mesh-type Ti electrode.
large-scale RED is needed to prove that the capacitive electrode mate-
rials are robust under high-pressured stack assembly, exhibit good pH
stability, and possess side reaction and bubble resistance. In addition,
regarding the periodic switching of natural feed solutions, there is a
probability of fouling phenomena around the electrodes being more
severe because divalent cations and pH have a significant effect on
natural organic matter (NOM) adsorption on the surfaces and ag-
gregation of NOM in the solution [104–106]. A sudden change in the
pH around the electrodes by switching of feed solutions may increase
organic fouling rate along with a drastic change in the concentration of
divalent cations.
4.3. Recent studies of electrode materials and reactions
Typical electrode systems are classified in Table 3. Representative
electrode materials include metal oxide- (e.g., Ru/Ir) or noble metal-
(e.g., Pt) coated Ti mesh, so-called dimensionally stable anode (DSA)
type electrode (Fig. 6). DSA electrode is one of the famous and in-
tensively used electrodes in various electrochemical fields due to its low
electrical resistance and good thermal/chemical stabilities [107–109].
Graphite electrodes also have advantages over DSA electrodes in that
they do not consume precious metals and have a high overpotential for
a gas generation [23]. However, if the graphite electrode is used for a
long time operation, mechanical durability may be worse than that of
the DSA electrode. In addition, the AgCl electrode can be used in the
RED electrode system. Energy consumption of the electrode system
would be decreased with the use of an AgCl electrode and it is safer
than other electrodes because there is no oxygen and hydrogen pro-
duction [110]. For electrolyte, the system of Fe2+/Fe3+ in NaCl with
inert electrodes has been used to prevent the huge overvoltages by gas
generation. The iron hexacyanoferrate system was developed to cover
the unpractical character of the Fe2+/Fe3+ system because pH is
changed during system operation by diffusion of hydrogen ions and
oxidation of Fe2+. However, Fe(CN)63−/Fe(CN)64− redox couple has a
risk of contamination at the AEM by an accumulation of the negatively
charged hexacyanoferrate ions on the positive amino groups of AEM
[111]. It is the outer CEM that comes into direct contact with the
electrolyte, of course, but if the electrolyte leaks and mixes with the
feed solution between the outer CEM and the AEM, contamination may
occur on the AEM surfaces. To prevent the contamination problem at
the AEM surface, a pure NaCl solution can be used as an electrolyte in
the electrode compartments [23,58].
The development of highly active and cheap catalysts as electrode
materials is ongoing to overcome typical electrode systems [116–118].
9
Desalination 491 (2020) 114540
Recently, Jeong et al. synthesized molybdenum disulfide (MoS2) coated
rutile-phase TiO2 (rpTiO2) on Ti substrate and utilized this hetero-
structured electrocatalyst as a cathode of the RED system [116]. They
found that the MoS2 synthesis after sulfur modification of Ti surface
(MoS2/smrpTiO2/Ti) increases the gross power density and reduces
internal resistance of RED stack, indicating that interfacial engineering
between MoS2 and rpTiO2 improves both the catalytic activity and
charge transfer efficiency. They also fabricated thin film of MoS2 over
porous carbon substrate by chemical vapour deposition [117]. The
MoS2/carbon hybrid structure has abundant exposed edge sites, leads to
active electron transfer at the cathode of the RED system and high
power generation. Lee et al. investigated performance of Vulcan-coated
graphite foil electrode for RED applications [118]. This carbon-based
electrode showed the lowest material resistance and gained additional
5–10% in power density compared to other electrodes (Pt on Ti plate, Ir
on Ti mesh, graphite foil), indicating that the reversible electrode re-
action is mostly affected by porous Vulcan layers rather than graphite
foil.
The RED systems coupled with photocatalysts are being investigated
for electric power generation and chemical production. Xu et al.
achieved simultaneous production of H2O2 and salinity-gradient energy
by using ZnO/Zn photoanode, FeVO4/carbon felt cathode, and Fenton
system [119–121]. Tian et al. showed that the stack voltage of RED
accelerates the separation of photo-induced holes and electrons on the
TiO2 photoanode, which enhanced Rhodamine B degradation and H2O2
production [122]. Lee et al. proposed RED-assisted solar water splitting
system composed of a p-Si photocathode, a Ni foam anode, and a RED
stack [123]. In this system, the RED system serves not only as a se-
parator but also as an additional tunable power source to compensate
for the insufficient photovoltage produced by the photoelectrode. In
addition, the RED stacks were used to provide the electrical energy
needed to drive hydrogen gas or acid/alkali production in microbial
electrolysis cells (MECs), where exoelectrogenic microbes oxidize so-
luble wastewater organic and release electrodes on a bioanode
[124–126].
Zhu et al. integrated the RED stack with flow battery to improve
energy recovery from salinity gradients and energy storage [127]. They
used 2,6-dihydroxyanthraquinone (2.6-DHAQ) and ferrocyanide [Fe
(CN)64−] redox couples. During charge in the RED stack, Fe(CN)64− is
oxidized to Fe(CN)63− at the anode and 2,6-DHAQ is reduced to 2,6-
reDHAQ at the cathode. These two electrolyte solutions containing the
charged redox couples are then discharged in the flow battery. Kang
et al. investigated the potential of the application of a membrane
electrode assembly (MEA) to the RED system [128]. The MEA consists
of a CEM and two porous Ag/AgCl electrodes. Because equivalent cir-
cuit of MEA does not contain the resistances of the feed channels, high
power density (4.1 W m−2) was achieved. Kim et al. combined elec-
trode and Donnan potentials in a concentration flow cell by using
copper hexacyanoferrate (CuHCF) electrode and anion exchange
membrane [129]. The high power density of 12.6 W m−2 was achieved
with a concentration ratio of 30.
4.4. Electrode systems applied to a large-scale reverse electrodialysis
In this section, we discuss the reports focusing on electrode systems
applied to a large-scale RED. In their first of its kind study, D'Angelo
et al. evaluated the effect of the electrode reaction on the power output
in a pilot-scale RED plant with 500 cell pairs fed with real seawater
[85]. Two kinds of ES were employed; (1) 2.5 M NaCl solution (2) 0.3 M
FeCl2 and 0.3 M FeCl3 in a supporting electrolyte of 2.5 M Na2SO4 so-
lution for the Fe2+/3+ redox reaction. In the former case, water re-
duction/oxidation and chlorine evolution occurred. Both electrode re-
actions were effectively used to drive large-scale RED. The difference in
the maximum power was 13%, which indicated that the potential
penalty necessary to drive water electrolysis is higher than in the case
of the iron redox couples. On the other hand, Han et al. [84] reported
J. Jang, et al.
that in a large-scale RED with 1000 cell pairs, the difference in the
maximum power between water electrolysis and [Fe(CN)6]4−/Fe
(CN)6]3− is only 3% at a slow flow rate of ES (50 L h−1) for minimizing
the pumping energy. Therefore, the degree of potential penalty due to
water electrolysis depends on both the number of cell pairs and the flow
rate of ES. Because there is no energy loss caused by concentration
polarization in water electrolysis, with a low flow rate of ES, the dif-
ference in power between water electrolysis and reversible redox
couple decreases [81]. D'Angelo et al. conducted a long-term operation
for about four months in a real environment with the Fe2+/3+ redox
reaction. Although the reduction in the power output was very small,
instability of the ES was confirmed; there was a decrease in the con-
centration of redox couples by approximately 33% because of the for-
mation of an iron precipitate, and the pH increased from 2 to 4.
Nam et al. employed wastewater effluent as the ES in a large-scale
RED with 1000 cell pairs that were fed with natural seawater and
municipal wastewater effluent [83]. These authors reported that scale
formation is difficult to control; the spacer for electrode, shielding
membrane, and cathode are severely clogged by inorganic precipitates,
such as calcium carbonate and magnesium hydroxide. This indicates
that the Ca2+ and Mg2+ ions in seawater transfer to the cathode
chamber through the shielding membrane, and precipitates are formed
in the alkaline conditions (pH 11.3) caused by water reduction. As one
of the solutions for the prevention of scale formation, Han et al. sug-
gested that inorganic scaling and toxic Cl2 gas evolution can be sup-
pressed under a specific condition in which the outermost FS at both
electrodes and the ES is river water [84]. In this configuration, how-
ever, the electric power was reduced by > 20%. Considering that the
electric power increased when the electrode spacer was removed, the
authors verified that the bubbles inside the electrode spacer formed by
water reduction caused a significant power loss. In addition, they
confirmed that the open-type endplates with interconnected open
spaces could be used to address fluid congestion and abrupt changes in
pH, which are critical problems in conventional endplates with very
narrow spaces.
5. The expected applications of the RED components and systems
5.1. Wastewater treatment
The high membrane voltage of the RED system offers a possibility to
remove pollutants in the ES. The electrochemical abatement of pollu-
tants is one of the steps of the electrode reaction in the RED system
operation. D'Angelo et al. achieved a fast and complete removal of the
organic pollutant, Acid Orange 7 (AO7) without power loss of the large-
scale RED system [85]. H2O2 generated from oxygen reduction at the
cathode (Eq. (7)) is converted to hydroxyl radical at the anode via
classical Fenton's reaction (Eq. (8)). The hydroxyl radical can oxidize
AO7 in the solution. The reaction of Eq. (8) propagated through the
continuous electrogeneration of Fe2+ by reduction of Fe3+ (Eq. (9)).
Cathode reaction:O2 + 2H+ + 2e H2 O2 (7)
Anode reaction:H2 O2 + Fe2 + Fe3 + + OH + OH (8)
Cathode reaction:Fe3+ Fe 2+ (9)
Similarly, using a lab-scale RED with dozens of cell pairs, the
electrochemical abatement of other pollutants such as hexavalent
chromium and ammonia has been reported [130–132]. Considering the
high energy consumption of electrochemical treatment technique
[133], the RED system with proper redox processes could be an eco-
nomic and efficient way for the treatment of wastewater with the si-
multaneous generation of electric energy.
5.2. Desalination-RED hybrid system
Another possible use of the RED system is to minimize energy loss in
10
Desalination 491 (2020) 114540
desalination plants utilizing reverse osmosis (RO) [112,114,134–136]
or electrodialysis (ED) [137,138]. That is the most representative ap-
plication of the RED system. However, there have been few examples of
commercialization of desalination plants using the RED process, al-
though efforts have been made to use the desalination-RED hybrid plant
since the introduction of the salinity gradient power technology from
1954 [11]. The reason for this exertion is that if the RED system is
successfully applied to the desalination plant, the plant with less energy
consumption can be realized. The research on desalination plant using
the RED system was conducted in two ways: (i) hybrid of the RED
system and RO desalination process [134,135] and (ii) combination of
RED and ED system [137,138]. The integration of the RO plant and RED
system has different merits depending on the configurations. When a
solution that has been used to the RED process is adopted as a feed of
the RO process, the feed salinity is lowered appropriately, thereby the
energy consumption of the RO process can be reduced. Conversely, the
power density of the RED system can be improved by using the con-
centrated water which discharged from the RO process as a feed solu-
tion for the RED system. In the ED process, energy consumption has a
huge portion of total cost owing to the utilization of electricity, thereby
the energy recovery system is needed to merge with the ED process.
However, the production cost of electricity by renewable energy is often
much higher than that of the conventional energy source due to the
expensive cost for complicated equipment and its low energy produc-
tion. Therefore, the combination of ED and RED can be effective to
increase energy efficiency. In this ED-RED hybrid, RED and ED system
provides and accepts energy, respectively. To commercialize the hybrid
systems of RO-RED and ED-RED, the performance of the RED system
must be further optimized and the hybrid system itself needs to be more
developed. In addition to this, recently, a process study has been con-
ducted to produce water and energy simultaneously by grafting the
membrane capacitive deionization (MCDI) or direct contact membrane
distillation (DCMD) with the RED system to improve the energy effi-
ciency of the desalination process [112,114,136].
6. Commercial development and current status
In 2013, the world's first real pilot plant of 50 kW capacity was built
by cooperation of REDstack BV, Fuji-film manufacturing BV, and
Wetsus (European center of excellence for sustainable water tech-
nology) at the Afsluitdijk, Netherland. This plant produced electric
power using mixing salt water (28 g L−1) from the Wadden Sea and
freshwater (0.2–0.5 g L−1) from Lake IJssel [139,140]. However, in-
creasing the concentration difference between the high concentration
solution and low concentration solution to produce huge power can
lead to a drastic reduction of system efficiency because of the increased
internal resistance. Especially, when freshwater is used as a low con-
centration solution in the RED system to maximize the electromotive
force, the internal resistance of the stack is further increased, thereby
the system efficiency is going to be reduced. The system designed to
overcome the above disadvantage is the reverse electrodialysis alter-
native power (REAPower) system by using brackish water as a low
concentration solution for generating electricity. The REAPower plant
based on the RED technology was built at the saltworks of Ettore e
Infersa in Marsala (Trapani, Italy) as a part of the EU-FP7 REAPower
project in 2014. In this location, brackish water as dilute from a
shoreline well and saturated brine as concentrate from saltworks can be
obtained for feed steams. This pilot has consisted of 125 pairs of the
IEM (active area: 50 m2) [94,95].
In 2016, the nominal power capacity of 1 kW was demonstrated in a
large pilot plant operated through the system has a total IEM area of
400 m2 using artificial brine and brackish water. This scale-up plant
built by the University of Palermo in Italy and Wetsus was realized
because it was backed up by the large-scale technology of components
in the RED system, including IEM and electrode [95]. Also, many re-
searchers and companies have continuously made great efforts to
J. Jang, et al.
increase power production. Especially, some companies have achieved
remarkable progress in plant scaled power production, and have been
striving for sustainable development until now. A representative ex-
ample is REDstack BV (The Netherlands). Since launching a 5 kW pilot
project with Frisia Zout BV (a European salt company) in 2005 [140],
REDstack has been striving to enhance the performance and scale of the
RED pilot plant based on their technology and experience. However, we
need to improve much more not only the real power output but also the
power capacity of plant for adopting the salinity gradient power as the
commercial energy supply system. The RED pilot plant is expected to be
able to scale up to 5 MW later 2020 based on current performances
through various attempts [140]. If the salinity gradient power system is
used to power production for distributing the electricity on the city or
industrial factory with recovering the investment price, the power >
5 W m−2 must be produced from the RED plant with taking into ac-
count the area of the membrane used in the process [26,141]. Even in
the RED system of plant scale, continuous optimization of materials,
structures and geometric of stacks must be made to achieve maximum
performance while minimizing the efficiency decline.
Even many attempts have been made up to now to make progress of
the RED power plant, developing of the salinity gradient power system
using the RED plant was conducted by only a few countries in Europe.
Recently, however, the United States and Japan have joined the de-
velopment of salinity gradient power. The leading countries in salinity
gradient power such as the Netherlands, Italy, Norway, United States
and Japan are laying the foundation for commercialization through the
intensive research and construction of the plant [94,95,140,142–148].
Recently, South Korea is also researching salinity gradient power
through the global research center operated by the Korea Institute of
Energy Research (KIER) in Jeju island and is devoted to commerciali-
zation [83,149,150]. Especially, KIER has joined the integrated net-
work for energy from salinity gradient power (INES) and is showing a
desire to participate in international activities [151,152]. The countries
tried to commercialize the salinity gradient power has a plan to build
the plant has a capacity of MW level after 2025. If the commerciali-
zation is successful, it is expected to form a huge market of $ 16.4
trillion which estimated by using the world's top ten rivers. Also, the
carbon dioxides of 12 million tons can be reduced via operating the
salinity gradient power plant with a power generation of 30 TWh.
7. The challenges and future prospects
One of the chronic problems in the salinity gradient power system is
inorganic/organic fouling near the electrode part including endplate,
shielding membrane, spacer, and inner IEMs [85,86,153]. The transport
of counter ions through the membrane is disturbed due to the fouling
proceeds, leading to a decrease in power production. Therefore, effec-
tive pretreatment technique to remove foulants from the feed water and
component engineering to prevent the formation of dense fouling layer
are required. There is also a need to develop post-process to reduce the
fouling layer or to return the state prior to fouling formation.
In terms of the uniformity of high pressure for stack assembly,
moreover, a large-scale RED system is significantly different from a lab-
scale one. It is challenging to maintain a uniform pressure over the
entire area of a large-scale RED because the bolts and nuts are usually
located at the edge of the endplate. Non-uniform pressure leads to a
leakage problem of not only the inner parts but also the electrode
compartments. In addition, even the RED module pressurized uni-
formly, it requires further consideration of transport behaviour such as
non-ideal permselectivity of IEM and uphill transport which induces
unwanted reactions (e.g., inorganic precipitation and organic fouling)
around the electrodes and the inside of the stack. That kind of transport
problem is generated by a combination of water electrolysis and
chlorine evolution under high membrane voltage. Therefore, additional
research needs to be performed to better understand how the electrode
system is stable under the long-term operation of a large-scale RED
11
Desalination 491 (2020) 114540
system in real applications and to develop new strategies for stable
electrode systems.
On the other hand, in terms of research area management, it is
necessary to be recognized as a renewable energy technology in order
to further upgrade the status of salinity gradient power technology and
to become an important research field among the various energy
system. The salinity gradient power technology has not yet been listed
as the technology of marine renewable energy authorized by the United
Nations (UN). Therefore, local governments, companies, and research
institutes in various countries are making efforts to create INES and to
list the salinity gradient power as a renewable energy system. If the
RED technology and salinity gradient power system are recognized as
brand-new renewable energy systems, more intensive research will be
conducted than now and it will be possible to make a rapid technolo-
gical leap. In addition, the synergistic effect from collaborative research
will bring a paradigm shift, which cannot anticipate now.
8. Conclusions
Salinity gradient power based on RED system is an energy tech-
nology capable of sustainable development because it uses two kinds of
solutions with different salt concentrations as an energy source. And,
there is no concern of resource depletion and no emission of pollutants
during the power generation process. Although all the components of
the RED system have their own importance, this review highlighted key
issues and research regarding IEMs and electrodes.
IEMs are classified into AEM and CEM. They have a fixed charge in
the body, which rejects co-ions but passes counter-ions to generate ion
current in the RED system. In addition, IEMs can be classified into
homogeneous and heterogeneous IEMs. The fixed charges are uniformly
distributed in the body of the homogeneous IEM so that the counter-ion
movement is smooth but the mechanical strength of the membrane is
weak. On the contrary, the heterogeneous IEM has a non-uniform
charge distribution resulting in relatively low mobility of the counter-
ions but this membrane is mechanically strong. Therefore, it is neces-
sary to develop the IEMs having the advantages of both homogeneous
and heterogeneous IEMs.
Parameters for determining the performance of IEMs in RED sys-
tems are FCD, IEC, AR, and permselectivity. Most studies have focused
on improving these properties. Specifically, the methods such as (1)
chemical reaction by cross-linking or grafting, (2) surface treatment
(sulfonation and amination), (3) pore filling, and (4) blending particles
are mainly used to modification of IEMs.
Comparing the quantitative characteristics of commercial and
tailor-made IEMs, it is difficult to evaluate which one is superior due to
its unique physical and electrochemical advantages of each IEMs. In
addition, the performance of the IEM in the RED system is not only the
result of a combination of various factors but also some of the prop-
erties have a trade-off relation with each other. Thus, it does not mean
that the IEM has one or two excellent properties is the best IEM com-
pared to others. However, special tendencies are confirmed when
analyzing the relationship between some properties. The thinner IEM
shows lower AR compared to the thicker one, and the IEM has lower AR
exhibits high power density in the RED system. Also, higher power
densities were obtained at higher levels of IEC (1.5–2.0 meq g−1).
The electrode is also one of the very important elements in the RED
system because the electrode converts the ion current into an electric
current through an electrochemical reaction. Inorganic/organic fouling
phenomena around the electrode part, which reduce the electro-
chemical reaction rate and significantly increase the internal resistance
in the pilot-scale plant. The electrode system and fouling problem on
that are a critical factor in the amount of power production and module
lifetime. Optimization of the electrode system is essential, therefore,
such as the selection of an appropriate redox couple considering the
operating conditions and the engineering of the electrode material or
shielding membrane. In addition, the technology related to the pre-
J. Jang, et al.
treatment of feed water to exclude foulants and the post-treatment (or
cleaning) of the fouling layer formed on the RED components.
The salinity gradient power plant using the RED system was first
built in 2014 at the Netherlands and progressed steadily through a lot of
research. Improving power production or power capacity of the plant
can be achieved by increasing the size of IEMs, electrode systems, and
other RED components. Currently, the technology of RED-based salinity
gradient power is led by the United States, the Netherlands, Norway,
and Japan. These countries aim to build a plant with a capacity of the
MW scale of more after 2025. For the salinity gradient power system to
be responsible for the production of electricity for the actual urban or
industrial facilities, an output of above 5 W m−2 should be produced
with considering the area of the IEM used in the process. If the tech-
nology of salinity gradient power is commercialized, a huge market of
about $ 16.4 trillion is expected when the world's top ten rivers are
estimated as an energy source. And, it is expected to reduce carbon
dioxide of 12 million tons with power production of 30 TWh by salinity
gradient power.
Enlarging the size of the RED system to increase power production
inevitably leads to non-uniform pressure on the stack assembly. This
non-uniform pressure from inside the stack assembly would cause
leakage in the electrode system as well as in the water channel. Also,
non-ideal permselectivity or uphill transport problems in IEMs result in
side reactions inside the module, which can drastically degrade the
system performances. Therefore, large-scale research should always be
accompanied by concerns about the above-mentioned problems.
In terms of organizing the research area, it is expected that more
active and diversified research will be possible if the UN recognizes the
salinity gradient power as a renewable energy system as soon as pos-
sible. It is hoped that salinity gradient power based on RED will become
the main energy technology of the humankind in the future.
Declaration of competing interest
There are no conflicts to declare.
Acknowledgment
This work was supported by Korea Environment Industry &
Technology Institute (KEITI) through Industrial Facilities &
Infrastructure Research Program, funded by Korea Ministry of
Environment (MOE) (1485016165) and the National Research
Foundation of Korea (NRF) grant funded by the Korea government
(MSIT) (2019R1C1C1002847).
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