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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
a r t i c l e i n f o a b s t r a c t
Article history: Disposal of saline effluent from desalination plants, agricultural drainage water, and other industries is an
Received 9 August 2010 increasing problem worldwide. Saline effluent has long been considered waste brine and traditional approaches
Received in revised form 17 December 2010 to its disposal have included evaporation ponds, deep wells, and coastal discharge. However, such effluent is now
Accepted 17 December 2010
being considered as a saline resource; therefore, alternative approaches have been developed to extract available
Available online 15 January 2011
salts and to recover purified water. In this study, techniques to dispose of rejected brine were investigated and
Keywords:
alternative salt recovery methods that have been developed and widely employed were reviewed. Evaporation
Desalination and cooling to extract salts from retentate has been widely used worldwide, but use of the membrane separation
Salt recovery techniques technique has been increasing rapidly owing to the development of cheaper and higher performance membranes.
Retentate Electrodialysis, ion-exchange, eutectic freezing, and chemical processing can also be used to recover salts from
Effluent retentate. Currently, hybrid systems that combine two or more techniques, such as the nanofiltration
(pretreatment)–reverse osmosis (concentration)–thermal processes (crystallization), are being developed and
used actively to increase the amount of extracted salt and reduce the final volume of rejected brine. Economic
analysis of concentrate utilization in comparison with disposal was performed in this study. Based on the cost of
producing salts, the multi-stage flash (MSF) distillation and electrodialysis and Dow chemical process were
relatively expensive when compared to nanofiltration and membrane crystallization, evaporation, and ion-
exchange techniques. However, technical developments for increasing the performance efficiency must be
further investigated to reduce the cost of desalting processes.
© 2010 Elsevier B.V. All rights reserved.
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Treatment and disposal of waste brine . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3. Salt recovery techniques . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3.1. Evaporation and cooling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3.2. Membrane separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.3. Electrodialysis (ED) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.4. Ion exchange . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.5. Eutectic freezing crystallization (EFC). . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.6. Chemical processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.7. Combination of techniques . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
4. Economic analysis of concentrate utilization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
5. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
Abbreviations: ADW, agricultural drainage water; BWRO, brackish water reverse osmosis; ED, electrodialysis; EDR, electrodialysis reversal; EFC, eutectic freezing crystallization;
IX, ion-exchange; MCr, membrane crystallizer; MEE, multiple-effect evaporation; MSF, multi-stage flash; NF, nanofiltration; RO, reverse osmosis; UF, ultrafiltration; VC, vapor
compression.
⁎ Tel.: +82 33 250 6496; fax: +82 33 255 6406.
E-mail address: daekim@kangwon.ac.kr.
0011-9164/$ – see front matter © 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.desal.2010.12.041
2 D.H. Kim / Desalination 270 (2011) 1–8
concentrate wastewater as a pretreatment for calcinations [11] and to produced by chemical industries [39,40], and treatment of agricultural
supply brine to a solar pond [31]. drainage water (ADW) for non-agricultural purposes [41]. To recover
fresh water from ADW, an aerated lagoon and a two stage RO system
3.2. Membrane separation was used and the retentate was sent to an evaporation pond for
disposal [41]. Membrane technology was also used to recover sodium
If a solution such as salt water is placed on one side of a semi- chloride from waste brine at a sugar decolorization plant [9]. RO
permeable membrane and water is placed on the other side, then coupled with NF was found to be more economical than a multiple
there is a natural tendency for water to diffuse through the membrane effect evaporator for salt recovery from textile effluents [42].
to the solute side until an equilibrium osmotic pressure is achieved Economically, RO is relatively inexpensive to install, operate, and
(osmosis). In a process known as reverse osmosis (RO), pressure maintain, and it consumes less energy than other desalination methods.
substantially greater than the osmotic pressure is applied to the solute However, membrane separation always produces a relatively large
side, then water diffuses from the solution through the membrane to volume of concentrate that must be disposed off or receive further
the fresh water side. This process is continuous and separates the feed processing.
fluid into two streams without the need to regenerate the membrane. Reverse osmosis is generally not selective for a specific target
Specifically, a concentrate stream containing the impurities and a high compound. Accordingly, other constituents present may also need to
purity water stream known as the permeate are produced. be separated. As a result, RO is not-cost effective as an add-on process
RO is a high-pressure, energy-efficient technique for dewatering for a specific target compound after other compounds have been
process streams, concentrating low-molecular-weight substances in eliminated during pretreatment. Determination of the correct
solution, or purifying wastewater. RO has the ability to concentrate all materials is the most important factor when developing RO
dissolved and suspended solids, while producing a permeate that desalination plant equipment to ensure that a long operation life is
contains a very low concentration of dissolved solids. attained.
The nanofiltration (NF) technique is primarily used for the
removal of bivalent and monovalent ions such as heavy metals. NF 3.3. Electrodialysis (ED)
essentially uses a coarse form of a RO membrane. Because NF uses less
fine membranes, the feed pressure of the NF system is generally lower Electrodialysis consists of a large number of cells alternately
than that of RO systems. In addition, NF has a lower fouling rate than contained within anion-exchange and cation-exchange membranes
RO. NF is a special process selected when RO and Ultrafiltration (UF) and arranged between an anode and a cathode. Under the influence of
are not the ideal choice for separation. NF can perform separation the applied electric field, the ions migrate towards the electrodes.
applications that are not otherwise economically feasible, such as Because alternate membranes are permeable only to cations or
demineralization, color removal, and desalination. During the con- anions, the water cells between the membranes are alternately
centration of organic solutes, suspended solids, and polyvalent ions, depleted and enriched with salt ions. The cation membranes allow
the permeate contains monovalent ions and low-molecular-weight only positively charged ions to diffuse through them.
organic solutions such as alcohol. Electrodialysis has been used to desalt surface and ground water since
This method not only removes organic substances, but also the 1950s [43]. This technique has been investigated for its feasibility and
inorganic content from wastewater. Based on the disposal of heavily performance in the desalination of brackish water [44–50], effluent
loaded industrial wastewater, recovery of substances from wastewa- treatment and recycling of industrial process streams [51–53], salt
ter, reduction in the load on treatment plants and the wastewater production [29], [54–57], and recovery of organic acids from waste salt
quantity produced, RO is a very economical and safe process that solutions [58]. Electrodialysis can be used as a pre-treatment or a pre-
has already been shown to be successful for practical use [32]. concentration method before the brine is supplied to an evaporative
Membranes employed in RO are usually made of cellulose acetate, crystallizer [29,56,57]. This method can reduce the concentration of
aromatic polyamide, polyimide, polysulfones, or thin film composites. calcium or sulfate ions to avoid gypsum crystallization during further
Membranes can be designed to remove specific inorganic and organic evaporation [29]. During the process, fouling by colloidal material,
contaminants, such as trihalomethanes. The efficiency of RO opera- organics, and biogrowth should be considered and treated to help sustain
tions will increase and costs will decrease as membranes are the equipment. These problems must be overcome for electrodialysis to
improved. Such improvements may include increased rejection of be used more widely.
salt, increased membrane resistance to compaction, chlorine, and
microorganisms, and large-scale production of standardized RO 3.4. Ion exchange
elements. There are many commercial RO membranes available,
including cellulose acetate and polyamide membranes, which are In this process, feed water is passed through a column containing
suitable for water treatment on a technical scale. These membranes the active form of a solid cation exchanger, which is an organic resin
have salt rejection rates of cellulose acetate and polyamide of 94–97% that contains hydrogen ions and is capable of exchanging them
and 94%, respectively [32]. There are also a wide variety of membrane against the positive ions contained in the feed water.
systems available for the treatment of wastewater. Pretreatment The ion exchange process has been studied, investigated, and applied
processes are essential to all systems to ensure a long service life of for desalting brackish water and recovering salts over several decades
membranes and trouble-free operation. Adequate pretreatment is [59–66]. This technique is only competitive with other desalination
critical for the successful use of RO membranes for desalination. methods for water containing relatively low concentrations of salts due
Water separation processes were demonstrated in the 1960s, and to the rising costs of resins and of treating regeneration solutions.
combined processes were then proposed in which RO units and
crystallizers were used to recover salts from the solutions [33]. Karelin 3.5. Eutectic freezing crystallization (EFC)
et al. (1996) [34] investigated the capacities of NF and RO high-
pressure membrane systems to separate a high-concentration In this process, the feed is frozen continuously until the eutectic
solution. The RO membranes were able to retain NaCl, even if its temperature is reached. Further heat removal then generates both ice
concentration in aqueous solutions was near the saturation level. and salt crystals. Specifically, ice is formed when the unsaturated
Membrane separation techniques have also been applied for the re- solution is cooled to its freezing point, after which, the removal of
use of salts and water from dyeing effluent [35,36], water recovery additional heat induces the system to follow its freezing curve and the
from brackish water [37,38], separation of salt from wastewater proportion of brine to ice decreases. At the eutectic point, ice and salt
4 D.H. Kim / Desalination 270 (2011) 1–8
crystallize simultaneously. When compared to conventional techni- Therefore, the multiple effect evaporation method has been used to
ques of evaporative and cooling crystallization, the advantages of EFC reduce the volume of the wastewater, and Na2SO4 was obtained by
are that it has a low energy requirement and the theoretical possibility calcinating the concentrated wastewater in a muffle furnace at a
of complete conversion of feed into water and solidified solutes. temperature range of 300 and 800 °C [35].
A continuous EFC system based on direct cooling in a mixed
crystallizer followed by salt–ice separation has been developed at the 3.7. Combination of techniques
bench scale [67]. Specifically, EFC was used to recover magnesium
sulfate heptahydrate (MgSO4·7H2O) from a magnesium sulfate Several techniques have been combined to increase system
industrial stream emitted from flue gas desulphurization [12]. performance efficiency and reduce final rejected brine, or even achieve
MgSO4·12H2O was formed in the crystallizer and recrystallization zero-discharge. The combined techniques were ultrafiltration as a
into MgSO4·7H2O occurred spontaneously during the subsequent pretreatment, nanofiltration for concentrating brine, multi-stage flash
filtration and drying above 0.4 °C. The produced salt crystals were for desalting water, and crystallization for recovering salts [27].
reasonably pure. Additionally, a cooled disk column crystallizer Alternatively, electrodialysis for concentrating brine, multi-stage flash
(CDCC) that employed the EFC technique was developed to recover for desalting water, and crystallization for recovering salts were
CuSO4 crystals from copper sulfate solution [68,69]. Crystallization employed [29,56], or the same process with RO instead of the multi-
was achieved by indirect cooling with wiped disks and separation by stage flash [25]. Discharged brine from RO was supplied to an ion-
means of gravity. In this system, the liquid feed stream enters the exchange membrane electrodialyzer, and the concentrated brine from
column at the center, while ice leaves the column at the top and salt is the electrodialyzer was then sent to a multi-effect vacuum evaporator to
discharged from the bottom. When compared to conventional crystallize the salts [57]. Sequential extraction of a variety of salts from
evaporative crystallization, the energy required for EFC can be rejected brine with high levels of dissolved sulfate, potassium, and
reduced by up to 70% and the 100% conversion into water and salt magnesium salts has also been conducted using multiple evaporation
is an advantage [68]. EFC system analysis and modeling have been and cooling of saline wastewater, chemical reactions, crystallization,
conducted to simulate its transient behavior [70–72]. washing, and dewatering [15,28]. The combined process was also
applied to recover salts and water from dye house effluents [36]. Pre-
3.6. Chemical processes filtration has been employed to remove cotton fibers and other large size
components from dye effluents, after which neutralization, and
Generally, retentate contains calcium, magnesium, sodium, sulfate, nanofiltration was applied to separate the mineral salts and the
chloride, and bicarbonate. Gypsum (CaSO4) precipitation occurs first as hydrolyzed dye and dyeing auxiliaries. RO can be conducted as a final
the concentration of the retentate increases due to its solubility step, if necessary, to increase the concentration of mineral salts and
characteristics (0.2 g of gypsum is dissolved in 100 g of water, which produce water that can be reused for the dyeing process.
results in minor deviations in temperature). To prevent the loss of SO2−4
via gypsum precipitation and to recover more Na2SO4 and MgSO4, the 4. Economic analysis of concentrate utilization
precipitation of gypsum can be limited by adding NaHCO3/Na2CO3 so that
Ca2+ ions are precipitated as carbonates. Calcination is a thermal Economic analysis of concentrate utilization in comparison with
treatment process applied to ores and other solid materials to induce disposal was performed. Specifically, a literature review was con-
thermal decomposition, phase transition, or removal of a volatile fraction. ducted to evaluate salt recovery techniques, such as MSF and
The calcination process normally occurs at temperatures below the electrodialysis [24], nanofiltration and membrane crystallization
melting point of the product materials. The process of calcination derives [73], the Dow chemical process [74], VC and electrodialysis [25], and
its name from its most common application, the decomposition of RO and ion-exchange [75]. These techniques have previously been
calcium carbonate (limestone) to calcium oxide (lime). The product of analyzed and compared with each other and with brine disposal by
calcination is usually referred to as calcine, regardless of the actual deep well injection and evaporation basin methods in the US [76].
minerals undergoing thermal treatment. Calcination is conducted in Simplified flow sheet for each treatment processes for cost compar-
furnaces or reactors (sometimes referred to as kilns) of various designs, ison is given in Fig. 1, and feed analysis to each process in Table 1. The
including shaft furnaces, rotary kilns, multiple hearth furnaces, and levelized cash flow approach was used for this analysis.
fluidized bed reactors.
−n
Recovery of CaCO3 from nanofiltration retentate has been Present Worth = ðP = F; i; nÞ = F ð1 + iÞ ð1Þ
conducted using reactive precipitation by adding NaHCO3/Na2CO3
aqueous solutions to the retentate [7]. Specifically, to recover The revenue requirements method was used to determine the salt
MgSO4·7H2O from the retentate produced by seawater nanofiltration, price required to yield the desired rate of return. The revenue
Ca2+ ions were precipitated as carbonates by reaction with NaHCO3/ requirements, Ig, are the sum of the four items as shown below:
Na2CO3 solutions so that calcium sulfate precipitation, which causes
the reduction of SO2− 4 content in the solution following limitation of Ig = C r + Ir + T + E ð2Þ
the recovery of magnesium sulfate, was limited. Sodium (bi)
carbonate solutions were produced by reactive transfer of carbon where,
dioxide into sodium hydroxide solutions. This technique has been
used to recover magnesium sulfate from high sulfate brine, rock- Cr capital repayment ($)
forming minerals, and salty lake water [1,2,4]. Ir return on investment ($)
Sequential extraction of a variety of salts from rejected brine with E expenses ($)
high levels of dissolved sulfate, potassium, and magnesium salts has
been conducted using multiple evaporation and cooling of saline t i r
T = tax paymentð DÞ = T = Cr −Dt + Ir 1− D D ð3Þ
wastewater, chemical reaction, crystallization, washing, and dewater- 1−t i
ing [15,28]. In this process, magnesium hydroxide is produced by the
addition of lime to the brine and the recovery of Na2SO4 from where,
wastewater is accomplished using calcinations of waste sodium
sulfate following evaporation [11]. In the dye industry, wastewater t tax rate
produced from dyeing processes contains a large amount of Na2SO4. Dt depreciation for tax purposes ($)
D.H. Kim / Desalination 270 (2011) 1–8 5
Fig. 1. Flow sheet for each treatment processes for cost comparison given in Table 1. (a) Nanofiltration and membrane crystallization [73] (b) Dow chemical process [74] (c) MSF and
electrodialysis [24] (d) VC and electrodialysis [25] (e) RO and ion-exchange [75].
Table 1
Feed analysis to each process (unit: mg/L).
Constituents MSF and electrodialysis [24] Nanofiltration and membrane Dow chemical process [74] VC and electrodialysis [25] RO and ion-exchange [75]
crystallization [73]
Thus, the cost per unit production for each plant is: each process with the cost when disposing of such feed streams by the
conventional methods of deep well injection and evaporation ponds.
LARR
Cost per unit production Dt
−1
= ð7Þ Disposal costs of the suggested techniques are relatively high compared
Q with deep well injection and evaporation ponds except RO and ion-
exchange (Table 4), however, the plants of [24,25,73,74] and [75] can
where, profit by commercializing salts or water produced indicating that these
alternative treatment methods for saline effluent disposal are viable
Q the quantity of salts produced per year. based on economic aspects. The production of salt (NaOH, Cl2) using
MSF and electrodialysis [24] costs $166 t− 1, the use of nanofiltration
And the cost paid to dispose per feed flow for each plant is: and membrane crystallization [73] costs $18 t− 1 to produce CaCO3,
NaCl, and MgSO4·7 H2O, while the Dow chemical process [74] costs
LARR
Cost to dispose per feed flow Dm
−3
= : ð8Þ $14,146 t− 1 to produce magnesium which is very expensive. When VC
FF and electrodialysis are employed to produce salt [25], the cost is $90 t− 1,
while RO and ion-exchange [75] costs $0.16 t− 1 (Table 4). Overall,
Where,
increasing performance efficiency can reduce the brine disposal cost.
FF feed flow rate (m3 y− 1)
5. Conclusions
The comparative cost evaluation for each plant is shown in Table 2.
The first three techniques have generated commercialized-possible Here, techniques for salt recovery from retentate were reviewed.
salts, but the last three focused on zero discharge and the removal of Literature survey revealed that evaporation and cooling are the most
boron and salt so that costs for treating feed water or desalted water common methods used for salt recovery, but that membrane
were compared with others for economic aspects. The cost calculation separation techniques have gained popularity worldwide as cheaper
of annual revenue requirements for the MSF and electrodialysis [24] is membranes with better performance have developed. Ion-exchange,
given in Table 3. electrodialysis, eutectic freezing, and chemical reaction are also
It is difficult to compare salt removal techniques due to the different increasingly being used. For better system performance, hybrid
times and purposes (e.g., producing salt, water, or removing salts) of systems that employ combined nanofiltration, reverse osmosis, and
each plant, but it is possible to observe tendencies among techniques thermal processes have been developed and applied. To select suitable
when they are compared. For better understanding, the capital cost and techniques for salt recovery, several parameters, such as geological,
the operating and maintenance expenses for each plant were estimated hydrological, climatic, and economic conditions, should be considered
based on equal feed flow rates (1000 m3 h− 1) and the comparison was for each site in advance. Economic analysis of concentrate utilization
performed based on the cost paid to dispose of the saline effluent fed to in comparison with disposal was also performed, and MSF and
Table 2
Comparative cost evaluation for each plant.
Plants MSF and electrodialysis Nanofiltration and membrane Dow chemical process VC and electrodialysis RO and ion-exchange
[24] crystallization [73] [74] [25] [75]
Products NaOH, Cl2 CaCO3, NaCl, MgSO4·7 H2O Magnesium Zero liquid discharge Boron removal
a
Capital cost ($) 12,748,000 7,108,000 100,000,000 8,719,000 776,000
Plant life (y) 10 30 10 10 10
a
Annual O&M expense ($/y) $1.18/h 859,000 $1237/t of Mg 30,800 110,900
Equal feed flow rate(m3/h) 1000
Interest rate on debt (%/y) 5
Cost of equity (%/y) 15
Debt ratio (%) 50
Effective income-tax rate (%) 50
Book depreciation method Straight line
Tax depreciation method Straight line
Average annual inflation rate (%) 2
a
Estimated based on equal feed flow rate.
D.H. Kim / Desalination 270 (2011) 1–8 7
Table 3
Annual revenue requirements of MSF and electrodialysis [24].
a b c d e f g h
Year Unrecovered Book Tax Debt Equity Income Annual Revenue requirement
investment ($) depreciation ($) depreciation ($) return ($) return ($) tax ($) expenses ($) in year ($)
Table 4
Levelized annual cost for each salt recovery plants and disposal costs using deep well injection and evaporation.
Plants MSF and Nanofiltration and Dow chemical VC and RO and Deep well injection
electrodialysis membrane process [74] electrodialysis ion-exchange and evaporation
[24] crystallization [73] [25] [75] basin [76]
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