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Water Resources and Industry 31 (2024) 100243

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Water Resources and Industry


journal homepage: www.elsevier.com/locate/wri

Electrocoagulation as a pretreatment for reverse osmosis for


potable water from brackish groundwater
Mahmood Jebur a, b, Yu-Hsuan Chiao a, c, **, Hideto Matsuyama c, S.
Ranil Wickramasinghe a, *
a
Ralph E Martin Department of Chemical Engineering, University of Arkansas, Fayetteville, AR, 72701, United States
b
Department of Chemical Engineering, Tikrit University, Tikrit, Salah Al-din, Iraq
c
Research Center for Membrane and Film Technology, Kobe University, Nada-ku, Kobe, 657-8501, Japan

A R T I C L E I N F O A B S T R A C T

Keywords: Reverse osmosis (RO) is a widely utilized method for water treatment and desalination. Our study
Desalination examined the application of an electrocoagulation (EC) and RO hybrid system for treating actual
Brackish groundwater brackish groundwater (BGW), focusing on reducing RO scaling by EC pretreatment. A series of EC
Reverse osmosis
operating conditions were investigated, such as applied voltage, pH, EC reaction time, and type of
Pretreatment
Electrocoagulation
electrode. The commercial software WAVE was utilized to analyze the water quality to assess the
scaling potential of the EC pretreated feed stream for the San Antonio Water System (SAWS) BGW
desalination plant. The SAWS BGW desalination process involves a three-stage RO process. Our
findings indicate that pretreatment with EC effectively prevents membrane scaling when
compared to feed without EC. We conducted continuous EC experiments which showed stable
performance and the potential for future commercialization.

1. Introduction

There is an ever increasing world demand for potable water [1]. The development of low cost, robust, integrated water treatment
technologies is essential. More than 50 % of the total available groundwater is brackish groundwater (BGW). BGW is defined as
groundwater with a concentration of total dissolved solids (TDS) in the range from 1000 to 10,000 mg/L. With appropriate treatment,
the BGW could be a source of potable water [2]. There are several desalination processes used to treat BGW such as electrodialysis
reversal, multistage flash evaporation, and reverse osmosis (RO) [3,4]. RO is considered an essential technology that has been used
widely for BGW desalination [5,6]. Approximately, 15,500 desalination plants have been installed in the world using RO technology
which constitutes about 74 % of all desalination plants. Today RO for sea water desalination is routine with over 52.8 % of sea water
desalination conducted by RO. However, in the case of BGW only 28.7 % is desalinated by RO. Though RO is a promising low-cost
alternative, scaling of the RO membrane is a major concern [7–9].
BGW contains significant concentrations of sulfates, silica, bicarbonates, and other inorganic species which can lead to increased
membrane scaling [10]. When using RO to treat BGW, pretreatment is essential to prevent membrane fouling. Using an RO system to
desalinate BGW can increase the concentration of dissolved salts from 4 to 10 times, which may exceed the solubility limit at the

* Corresponding author.
** Corresponding author. Ralph E Martin Department of Chemical Engineering, University of Arkansas, Fayetteville, AR, 72701, United States.
E-mail addresses: msdonaldc@hotmail.com (Y.-H. Chiao), swickram@uark.edu (S.R. Wickramasinghe).

https://doi.org/10.1016/j.wri.2024.100243
Received 28 August 2023; Received in revised form 5 January 2024; Accepted 15 January 2024
Available online 26 January 2024
2212-3717/© 2024 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
M. Jebur et al. Water Resources and Industry 31 (2024) 100243

membrane surface [11]. Crystallization/precipitation of inorganic species on the membrane surface fouls the membrane and limits
long-term operation [12,13]. Thus, choosing an appropriate feed pretreatment process is essential to improve RO productivity and
alleviate mineral precipitation. There have been various RO pretreatment technologies used to minimize the scaling and fouling risk on
the RO membrane surface [14]. Conventional pretreatments including chlorination, clarification/dissolved air floatation (DAF),
ozonation, coagulation–flocculation, and addition of antiscalants are reported to enable maintenance of stable RO membrane per­
formance. Moreover, membrane-based pretreatments, such as microfiltration and ultrafiltration (UF), even nanofiltration, have been
considered promising candidates for reducing the chemical doses and large footprint caused by conventional pretreatments. However,
the capital cost is much higher than conventional pretreatments. Organics smaller than the membrane pore size for these
membrane-based pretreatment operations are still a problem and can lead to fouling of the RO membrane.
Pretreatment by electrocoagulation (EC) could be an effective solution to reduce both inorganic and bio -foulants. Briefly, EC is an
electrolysis process involving the in-situ production of metal cations and OH− ions under the influence of an applied electric field. As a
result, hydrolysis occurs in the solution, leading to the formation of hydroxide flocs. These flocs have a high specific surface area and
abundant surface hydroxyl groups, which enable them to effectively adsorb substances in water through complexation, netting, or
bridging [15]. Moreover, EC has the capability to operate continuously, resulting in a significant decrease in both capital investment
and chemical consumption. Previous studies indicated good removal of turbidity, total suspended solids (TSS), and total organic
carbon (TOC) [16–19].
The BGW used in this study was obtained from the San Antonio Water System (SAWS). The main foulants found in the RO process at
SAWS are sand, silt, silica, iron, and sulfates, which could form iron silicate, iron sulfide, or iron sulfate, which will precipitate and
deposit on the membrane surface [10]. The SAWS BGW desalination system consists of pretreatment, RO, and posttreatment systems.
The RO concentrate is then discharged into two injection wells, while the desalinated water is sent for distribution. The pretreatment
step consists of both chemical addition (93 % sulfuric acid solution and a proprietary antiscalant) and a physical barrier (a nominally
rated 5 μm cartridge filter system) to protect the RO membranes from scaling and plugging by suspended solids. A three-stage RO
process is then used for desalination. Four primary RO skids are applied in the 1st and 2nd stages, while two concentrator RO skids are
used in the 3rd stage. A calcite contactor system, a degasifier system, a chlorination chamber, and a source water bypass system are
used as a part of the posttreatment setup. Fig. 1 is a schematic diagram of the SAWS BGW desalination plant [10]. Currently, the
antiscalant dosage used at the SAWS BGW desalination plant is 11.66 ml/min. The metal consumption for EC is about 0.20 lbs/1000
gallons based on Powell Water Systems Inc (Centennial, CO). Even with the addition of antiscalant in the pretreatment step, membrane
fouling is more severe in the 3rd stage RO units due to the increase in TDS concentration.
In this study, we aim to evaluate the feasibility of using EC to replace the use of an antiscalant. Several mechanisms are involved in
the removal of contaminants by EC, such as oxidation, reduction, coagulation, adsorption, precipitation, and flotation. We used a
Design of Experiments (DOE) approach. Batch EC experiments were conducted to determine the effect of EC system parameters on the
removal of the main foulants found in the RO system. Both raw water (collected directly from 12 supply wells in the lower Wilcox
aquifer in Texas) and feed water to the 3rd-stage RO unit were treated using the batch EC unit. It is the 3rd-stage RO unit that has the
major scaling issue in the desalination plant. The EC system parameters investigated in this work are voltage from 5 to 20 V, initial pH
from 4 to 8, reaction time from 1 to 5 min using Fe, Al or a combination of Fe and Al electrodes. The optimized EC parameters were
determined and utilized. The Water Application Value Engine (WAVE) software was utilized to simulate the membrane performance
based on the water quality analysis results. The untreated water samples were also included in the comparison. Finally, a small-scale
continuous EC unit was operated at optimized operating conditions that were determined by batch experimentation. The removal
efficiency of the main foulants, including silica, iron, calcium, and magnesium, was monitored during the continuous experiment. The

Fig. 1. Schematic diagram of the SAWS BGW desalination plant, which is a reproduction from [10].

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results collected from the small-scale continuous EC unit provide insights into the performance of an industrial process. The results
generated in this study will be used to evaluate the integrated EC-RO system in terms of reducing the number of cleaning cycles and the
operating feed pressure.

2. Theoretical background

The EC process involves a number of sequential steps. EC is an electrolysis process. Release of metal ions, e.g., iron or aluminum,
depending on the electrode material, occurs at the anode, while the reduction of water leading to the release of hydrogen gas occurs at
the cathode. Unlike coagulation using alum and ferric salts, the metal ions are generated in situ. Table 1 displays the standard state
reduction potentials for potential reactions. These reactions could take place during EC of the BGW samples tested in this study at a
temperature of 25 ◦ C. In reality, this is only a guide to possible reactions, as EC is not conducted under standard conditions.
During EC, water is reduced at the cathode, resulting in the formation of hydroxide ions (2H2 O + 2e → H2 + 2OH− ), while metal
ions are continuously generated at the anode (M →Mz+ + ze− ). A variety of metal hydroxides are produced in the solution when
coagulating ions (metal and/or hydroxide ions) undergo hydrolysis in water. Introducing metal hydroxides can help destabilize
suspended, emulsified, and dissolved contaminants, which can further aggregate and precipitate as sludge or lift up to the surface as
flocs. A number of processes occur during EC such as oxidation and reduction, coagulation, adsorption, precipitation, and flotation.
Here the importance of oxidation and reduction, coagulation and adsorption are investigated.

3. Method

3.1. Water samples characterization

Water samples were analyzed at the Arkansas Water Resources Center, University of Arkansas (Fayetteville, AR, USA). TOC,
turbidity, TSS, and TDS were measured using the following EPA standard methods 180.1, 415.1, 160.2, and 160.1, respectively. In
addition, cations and anions were measured using the EPA methods 200.7 and 300.0, respectively. Conductivity was measured using
conductivity meter (VWR, Radnor, PA).

3.2. EC pretreatment

A custom polycarbonate reactor was built with a volume of 1078 cm3 (dimensions 7 cm × 11 cm x 14 cm) to conduct all batch and
continuous EC experiments. The EC reactor contained five vertically oriented aluminum or/and iron electrodes with inter-electrode
spacing of 10 mm. Raw BGW and feed to the 3rd stage RO unit were used in the EC experiments. A DC power supply from Hewlett
Packard in Palo Alto, CA, USA was connected to a reverse polarity switch. This can alternate the direction of current every 30 s to
prevent the formation of a passivation layer on the electrode surface that could hinder further reactions [19,20].
Here, a bipolar series (BPS) configuration (only the first and last electrodes are connected to the power supply) was used to simplify
the electrical connections. Further, the BPS configuration was used in previous studies, which show an enhancement in the removal of
contaminant compared to other configurations [17].
A DOE was established using JMP software in order to determine the effect of EC on the removal of Mg, Si, K, and Ca as well as to
optimize the number of batch experiments that needed to be conducted. Applied voltage, reaction time, electrode material, and initial
pH are the main parameters used here to optimize the EC operating conditions. These factors were tested using three levels in the
following range: voltage 5–20 V, reaction time 1–5 min, initial pH 4 to 8, and using Fe, Al or a combination of Fe & Al electrodes. The
effects of oxidation and reduction can be determined by varying the reaction conditions (applied voltage and reaction time).
Firstly, a set of batch EC experiments was conducted to optimize the operating conditions based on achieving a high removal of
contaminants. After each batch EC, the feed was held in the reactor in order to sediment the floc. After optimizing the operating
conditions, the EC reactor was run in continuous mode (for 9 h). Fig. 2 shows the proposed process flow diagram of the continuous EC

Table 1
Standard reduction potentials at 25 ◦ C.
Half-reaction Eo (V)

H2 O2 (aq) + 2H (aq) + 2e →2H2 O (3)


+ − +1.77
Cl2 (g) + 2e− →2Cl− (aq) (4) +1.36
O2 (g) + 4H+ (aq) + 2e− →2H2 O (5) +1.23
Fe3+ (aq) + e− →Fe2+ (aq) (6) +0.77
O2 (g) + 2H+ (aq) + 2e− →H2 O2 (aq) (7) +0.68
O2 (g) + 2H2 O + 4e− →4OH− (aq) (8) +0.40
2H+ (aq) + 2e− →H2 (g) (9) 0.00
Fe2+ (aq) + 2e− →Fe(s) (10) − 0.44
2H2 O + 2e− →H2 (g) + 2OH− (aq) (11) − 0.83
Al3+ (aq) + 3e− →Al(s) (12) − 1.66
Mg2+ (aq) + 2e− →Mg(s) (13) − 2.37
Ca2+ (aq) + 2e− →Ca(s) (14) − 2.87

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reactor integrated with RO process.


Mixing experiments were conducted to determine the importance of adsorption on foulant removal. A synthetic brackish water
having the same TDS as the feed to the 3rd stage RO unit (10,628 mg/L as NaCl) was prepared. Then, the EC experiment was conducted
using synthetic water at 20 V for 5 min using 3 Fe and 2 Al electrodes (DOE # 1). After that, the generated sludge from the synthetic
water after EC was separated and mixed with real feed to the 3rd stage RO unit at four different speeds (800 rpm for 5 min, 500 rpm for
5 min, 300 rpm for 10 min, and 200 rpm for 10 min). The water sample after mixing with sludge was collected and analyzed using
Inductive Couple Plasma (ICP).
The effects of adding a chemical coagulant (coagulation) during EC were evaluated to obtain any changes in the removal efficiency
of Si, Ca, Mg, and K. Aluminum sulfate-18-hydrate (500 mg/L) was added as a chemical coagulant to the feed to the 3rd stage RO unit
prior to EC. Then EC experiment was conducted at 5 V for 3 min using 3 Fe and 2 Al electrodes (DOE # 7), which indicates a low
removal efficiency. If adding chemical coagulants during EC did not improve the removal efficiency of EC, this means the oxidation and
reduction reactions occurred in EC at optimized conditions are the dominant mechanism to obtain high RO foulants removal.

3.3. Scaling analysis

WAVE software to evaluate how the RO membrane is affected by fouling and scaling after EC. WAVE is a software developed by
DuPont Water Solution, Hayward, CA, USA, that can simulate the performance of water treatment processes like UF and RO [21]. The
software can model unit operations and provide a digital representation of industrial processes. This innovation has the potential to
eliminate the need for pilot plants to conduct commercial trials. By using WAVE software, we were able to simulate how fouling affects
the RO membrane due to RO foulants in the feed water.

3.4. Sludge characterization

To understand the adsorption mechanism, sludge produced after EC was characterized using Scanning Electron Microscopy (SEM),
Energy-Dispersive X-Ray (EDX) Spectroscopy, and X-Ray Diffraction (XRD) analysis to determine the foulants adsorbed in sludge.
Several sludge samples produced after EC at specific operating conditions were characterized, using SEM and EDX, spectroscopy to
determine the foulants adsorbed in the sludge. Both SEM and EDX were applied using Nova Nanolab 200 Duo-Beam Workstation (FEI,
Hillsboro, OR, USA).

4. Results and discussion

4.1. BGW characterization

The water quality parameters of the raw BGW samples and feed to the 3rd stage RO unit are shown in Table 2. The TDS increased
from 1268 to 10,628 after pre-treatment and 1st and 2nd stage RO. Chlorine, sulfate, calcium, magnesium, potassium, and sodium are
the majority of the inorganic ions present in BGW. Membrane scaling can be caused by a high concentration of inorganic ions, which
will precipitate and deposit on the membrane surface.

Fig. 2. The proposed EC pretreatment integrated with the RO process at SAWS.

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Table 2
Water quality analysis for raw BGW and the feed to the 3rd stage RO.
Parameter Unit Raw BGW Feed to 3rd Stage RO

TDS mg/L 1268 10,628


TSS mg/L 1.1 3.1
TOC 14 94.9
Hardness mg/L 400 1600
pH – 7.8 7.9
Chloride mg/L 250 2183
Nitrate mg/L 1.088 0.809
Sulfate mg/L 492 5096
Aluminum mg/L 0.0 0.0
Boron mg/L 0.73 2.26
Silica 11.5 74
Calcium mg/L 26.5 232
Magnesium mg/L 13.3 112
Potassium mg/L 10.6 96.4
Sodium mg/L 445 3747
Total Nitrogen mg/L as N 1.18 17.3
Conductivity μS/cm 2246 17,240
Iron mg/L 0.0 0.83
Barium mg/L 0.04 0.26
Turbidity NTU’s 0.22 0.29

4.2. Batch EC performance

The DOE and batch EC experiments conducted during this study are summarized in Table 3 and Table 4. The selection of the
parameter ranges was guided by a combination of experience in the field of EC and a comprehensive review of relevant literature [22].
Two sources of BGW from SAWS were tested, raw BGW and the feed to the 3rd stage RO unit. A total of 30 experiments were conducted
(15 each for BGW and feed water), which determined the effects of applied voltage, EC reaction time, initial pH, and electrode
material.
Table 5 and Table 6 depict the experimental conditions and water quality results (turbidity and total hardness) for both raw BGW
and feed to the 3rd stage RO unit, respectively, treated by EC using the DOE. It is clear that using a combination of Fe and Al electrodes
minimizes the turbidity of the treated water at pH 8 or higher. Decreasing the initial pH increases the turbidity of treated water due to
late oxidation of Fe2+ ions resulting ultimately in an orange/yellow precipitate that can cause an increase in the turbidity. The
reduction in total hardness was almost the same (50 % for raw water and 25 % for feed water) for most of the EC experiments.
However, a significant decrease in the total hardness was observed (up to 75 % removal for raw BGW and 69 % removal for feed to the
3rd stage RO unit) when increasing the voltage to 20 V, reaction time to 5 min, and pH to 8 as shown in Table 5.
In general, the removal efficiency of RO foulants increased with increasing applied voltage and reaction time for both BGW and the
feed to the 3rd stage RO unit as given in Figs. 3 and 4, respectively. Increasing the applied voltage leads to an increase in the removal
efficiency of Mg, Si, and Ca. A significant increase in the removal efficiency of Mg, Si, and Ca was obtained at 20 V, 5 min reaction time,
and pH 8 using a combination of Fe & Al electrodes.
Our results indicate that the efficiency of the EC process depends on a number of variables. For example, using the highest voltage
by itself does not guarantee maximum pollutant removal. Over addition of metal ions will lead to higher operating costs and most
likely higher Al and Fe concentrations in the treated water.
Fig. 5 gives ICP analysis results for 4 experiments. Experiments 1 and 2 involved conducting EC on the feed to the 3rd RO stage.
They were conducted using 5 V for a duration of 3 min. However, in the first experiment, 500 mg/L dose of a chemical coagulant
(aluminum sulfate-18-hydrate) was added. As can be seen, coagulation has only a minor positive effect on performance. Experiment 3
involved adding the sludge after EC at 20 V for 5 min produced from synthetic stage 3 RO feed water to additional untreated stage 3 RO
feed water. As can be seen, there is significant Si removal. Finally, experiment 4, which involved running EC at 20 V for 5 min, gave a
similar Si removal to experiment 3. However, Mg and Ca removal are superior. The results indicate the importance of water quality in
determining the effectiveness of EC and the optimum EC operating conditions.

Table 3
Factors and levels for design of experiments.
Factors Levels Reaction Time (min) Voltage (volts) Fe/Al electrodes pH

Levels

1 1 5 5 Fe/0 Al 4
2 3 10 4 Fe/1 Al 6
3 5 20 3 Fe/2 Al 8

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Table 4
Design of Experiments conducted for raw BGW and the feed to the 3rd stage RO.
Run Voltage (volts) Reaction Time (min) Fe/Al electrodes pH

1 20 5 3 Fe/2 Al 8
2 20 1 3 Fe/2 Al 4
3 10 1 5 Fe/0 Al 4
4 10 1 4 Fe/1 Al 8
5 5 1 4 Fe/1 Al 6
6 20 1 5 Fe/0 Al 6
7 5 3 3 Fe/2 Al 8
8 5 3 5 Fe/0 Al 6
9 5 3 4 Fe/1 Al 4
10 10 3 3 Fe/2 Al 8
11 10 3 5 Fe/0 Al 6
12 20 5 4 Fe/1 Al 6
13 10 5 4 Fe/1 Al 4
14 5 5 5 Fe/0 Al 8
15 10 5 3 Fe/2 Al 6

Table 5
Experimental conditions and results from DOE for raw BGW.
Run Total Hardness (mg/L) Turbidity (NTU) Electrode Material Current Density (mA/cm2) pH EEC (KW h/m3)

400 0.22 N/A N/A 8 N/A


1 100 0.16 3Fe & 2Al 7.7 8 1.73
2 180 14 3Fe & 2Al 9.2 4 0.411
3 190 176 5Fe & 0Al 3.6 4 0.080
4 200 0.30 4Fe &1Al 3.1 8 0.069
5 200 0.23 4Fe & 1Al 0.6 6 0.006
6 200 137 5Fe & 0Al 7.7 6 0.346
7 200 0.29 3Fe & 2Al 0.7 8 0.024
8 200 0.31 5Fe & 0Al 0.9 6 0.030
9 200 8.74 4Fe & 1Al 0.7 4 0.024
10 200 0.12 3Fe & 2Al 3.2 8 0.196
11 200 19 5Fe & 0Al 3.3 6 0.225
12 200 3.59 4Fe & 1Al 8.3 6 1.86
13 200 17.5 4Fe & 1Al 3.0 4 0.33
14 200 1.03 5Fe & 0Al 0.99 8 0.056
15 200 35.2 3Fe & 2Al 2.8 6 0.32

Table 6
Experimental conditions and results from DOE for feed to the 3rd stage RO unit.
Run Total Hardness (mg/L) Turbidity (NTU) Electrode Material Current Density (mA/cm2) pH EEC (KW h/m3)

1600 0.29 N/A N/A 8 N/A


1 500 2.49 3Fe & 2Al 53.5 8 13.6
2 1400 >1000 3Fe & 2Al 47.6 4 2.3
3 1200 >1000 5Fe & 0Al 18.4 4 0.38
4 1200 21.6 4Fe &1Al 15.1 8 0.34
5 1200 77.4 4Fe & 1Al 3 6 0.03
6 1200 >1000 5Fe & 0Al 44.6 6 2
7 1200 0.75 3Fe & 2Al 2.1 8 0.07
8 1200 397 5Fe & 0Al 3.8 6 0.13
9 1200 462 4Fe & 1Al 3.9 4 0.17
10 1200 18 3Fe & 2Al 15.2 8 1.03
11 1200 >1000 5Fe & 0Al 17.5 6 1.18
12 1200 654 4Fe & 1Al 52.4 6 11.8
13 1200 >1000 4Fe & 1Al 15.7 4 1.95
14 1200 0.56 5Fe & 0Al 3.6 8 0.2
15 1200 846 3Fe & 2Al 15.8 6 1.77

4.3. Sludge characterization

The sludge produced from different operating conditions during EC was characterized using SEM and EDX spectroscopy. The SEM
images shown in Fig. 6 illustrate that using a combination of Fe and Al electrodes gives an amorphous and poorly crystalline structure
of the sludge. In our earlier work [23], we showed that flocs produced by different metal ions have very different properties. By using

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Fig. 3. Removal efficiency of RO foulants for raw BGW treated under different conditions as part of the DOE.

Fig. 4. Removal efficiency of RO foulants for the feed to the 3rd stage RO unit treated under different conditions as part of the DOE.

electrodes consisting of different metals, EC performance may be enhanced.


From the EDX results, we can see that most of the elements removed by EC were captured in the sludge, such as Mg, Si, and Ca as
shown in Table 7. A slight increase in the amount of Ca and Mg was observed in the EDX analysis when increasing the applied voltage
and reaction time from 5 V to 10 V and 1 min–3 min, for both raw BGW (run 1 and 3) and feed to the 3rd RO unit (run 2 and 4). Thus,
using EC as a pretreatment step prior to RO successfully removes RO scalants.

4.4. WAVE software analysis

WAVE software was used to model the performance of the RO membrane based on the feed water quality by comparing the raw
BGW without any pretreatment, BGW with antiscalant pretreatment, and BGW with EC, treated by the 1st and 2nd stage RO units. As we
mentioned earlier, the most severe scaling occurred at the 3rd stage RO unit. At the SAWS BGW desalination plant, the amount of
antiscalant dosage used is 11.66 ml per minute. BW30-400/34 elements from Dupont Water were used in the desalination plant. There
were 40 vessels in each 1st stage skid and 20 vessels in each 2nd stage skid of the RO unit. The 3rd stage RO skid has 16 vessels. Each
vessel was equipped with 7 elements.
The results shown in Table 8 indicate that the antiscalant did not efficiently reduce the scaling potential at the 3rd stage RO units.
Instead, the RO solubility warning occurred (CaSO₄, BaSO₄, and CaF₂ % saturation >100). Although the silica saturation % was
dramatically reduced from 51.1 to 6.2, the added antiscalant obviously did not work very well in this case. On the other hand, the EC-

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Fig. 5. Results of ICP analysis for four different experiments. 1. EC 5 V, 3 min using feed to 3rd stage RO with addition of coagulants; 2. EC 5 V, 3
min using feed to 3rd stage RO; 3. sludge from EC 20 V, 5 min of synthetic feed to 3rd stage RO added untreated feed to 3rd stage RO; 4. EC 20 V, 5
min using feed to 3rd stage RO.

Fig. 6. SEM images of sludge generated after EC at different operating conditions: (a) Raw BGW DOE run 5 (5 V, 1 min, 4 Fe & 1 Al electrodes, pH
6), (b) the Feed to the 3rd stage RO unit DOE run 5 (5 V, 1 min, 4 Fe & 1 Al electrodes, pH 6), (c) Raw BGW DOE run 10 (10 V, 3 min, 3 Fe & 2 Al
electrodes, pH 8), (d) The feed to the 3rd stage RO unit DOE run 10 (10 V, 3 min, 3 Fe & 2 Al electrodes, pH 8). Insert scale bar is 3 μm.

treated water sample (***) showed a high enhancement in reducing the saturation % to CaSO₄, BaSO₄, and CaF₂ even though the silica
saturation % was decreased to 0.08. From the results shown in Table 8, we can see that no RO solubility warnings were found after
applying EC (***), which indicates that EC can be used effectively to reduce the RO scaling. The WAVE program result showed the EC
has more efficient lower RO scaling than no pretreatment water sample, even better than adding antiscalant in this case. We believe
that in the future, EC pretreatment will be a strong competitor to conventional antiscalants.

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Table 7
EDX results were obtained for sludge generated under different operating conditions. Samples a-d were associated with the SEM images in Fig. 6.
Samplesa

Element (%) a b c d

C 15.12 2.76 5.19 2.66


N 4.79 2.71 5.23 1.86
O 63.13 57.71 66.49 44.52
P 0.94 2.36 2.25 0.81
Fe 3.48 12.46 1.31 19.2
Ca 0.35 1.42 0.39 2.88
Mg 0.7 0.62 1.17 1.06
Na 1.75 3.33 2.09 4.85
Si 3.28 9.31 2.67 8.47
Cl 0.2 0.69 0 2.29
Al 3.71 2.33 6.73 8.28
S 0.46 0.71 0.12 1.08
a
(a) Raw BGW DOE run 5 (5 V, 1 min, 4 Fe & 1 Al electrodes, pH 6), (b) the Feed to the 3rd stage RO unit DOE run 5 (5 V, 1 min, 4 Fe & 1 Al
electrodes, pH 6), (c) Raw BGW DOE run 10 (10 V, 3 min, 3 Fe & 2 Al electrodes, pH 8), (d) The Feed to the 3rd stage RO unit DOE run 10 (10 V, 3
min, 3 Fe & 2 Al electrodes, pH 8).

Table 8
The RO Solubility Warnings using the WAVE software comparing the water samples from the San Antonio Water System (SAWS). (*) raw BGW
without any pretreatment, (**) the feed to the 3rd stage RO water, and (***) the feed to the 3rd stage RO water with EC to the 3rd RO unit. Feed
samples were treated by the 1st and 2nd stage RO units.
RO Chemical Adjustments * Feed *Conc **Feed **Conc ***Feed ***Conc

pH 7.8 7.8 7.0 7.1 7.0 7.1


Langelier Saturation Index 0.00 0.00 0.00 0.00 0.00 0.00
Stiff & Davis Stability Index 0.00 0.00 0.00 0.00 0.00 0.00
TDSᵃ (mg/L) 6405 12,762 11,676 23,201 11,264 19,410
Ionic Strength (molal) 0.13 0.26 0.25 0.49 0.23 0.40
HCO₃⁻ (mg/L) 0.00 0.00 0.00 0.00 0.00 0.00
CO₂ (mg/l) 0.00 0.00 0.00 0.00 0.00 0.00
CO₃2⁻ (mg/L) 0.00 0.00 0.00 0.00 0.00 0.00
CaSO₄ (% saturation) 24.2 56.8 55.0 123.9 22.1 42.2
BaSO₄ (% saturation) 3072 6599 4728 10,008 120 259
SrSO₄ (% saturation) 0.00 0.00 0.00 0.00 0.00 0.00
CaF₂ (% saturation) 0.00 12.4 27.3 169.8 10.2 43.3
SiO₂ (% saturation) 51.1 102.0 6.2 12.4 0.08 0.13
Mg(OH)₂ (% saturation) 0.02 0.08 0.00 0.00 0.00 0.00

Fig. 7. The removal efficiency of Mg, Si, Ca, and Ba at different operating times during the continuous EC experiment of raw BGW for 540 min.

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M. Jebur et al. Water Resources and Industry 31 (2024) 100243

4.5. Continuous EC performance

Batch EC demonstrated effective reduction of the scaling potential for the RO process section 4.2. To upscale and commercialize EC,
continuous EC development and evaluation is necessary. A continuous EC experiment was conducted in the laboratory to evaluate the
performance of long-term EC. Several samples were collected during the continuous EC experiment at different times to evaluate the
removal efficiency of Mg, Si, Ca, and Ba. In general, the removal efficiency of RO foulants decreased slightly with time, as given in
Fig. 7. The slight decrease in the removal efficiency was mainly caused by the formation of a passivation layer on the electrodes, which
indicates the need for cleaning as well as switching of the electrode polarity of the electrodes as done here. However, we can reliably
conclude that continuous-EC has potential for future development in terms of removal efficiency.

4.6. Implications

Membrane technology plays a vital role in treating industrial water, but it faces challenges such as fouling and scaling, which can
reduce membrane effectiveness and lifespan. This can lead to high energy consumption and operational costs. EC is an eco-friendly
alternative to using chemical dosing and has the potential to address these challenges. According to our result, EC can be a suitable
and highly efficient pretreatment step for producing potable water from brackish groundwater. EC is also expected to be beneficial for
treating boiler water and surface water. It can help increase water recovery and prevent the wastage of water resources.

5. Conclusions

Here we investigated the use of EC as a pretreatment to a 3rd stage RO system for BGW desalination to produce potable water. The
efficacy of the EC process was tested on feed streams sourced from a municipal BGW treatment plant. The study showed that EC has the
potential to be an effective pretreatment process for removing the primary RO membrane scalants such as Si, Mg, Ca, and Ba. However,
since EC is a complicated process involving the removal of foulants through various mechanisms, it is essential to optimize the EC
process for the specific water quality of the feed water. Si and Ca for the water either raw or feed for 3rd RO can be removed up to 98 %
and 60 %, respectively, using an EC process with 3 Fe and 2 Al electrodes at 20 V for 5 min. The WAVE software results indicate that the
EC process can effectively reduce the concentration of foulants below their saturation limit in the 3rd RO stage. Moreover, the
continuous EC process showed stable performance, making it a promising solution for future commercial use. However, electrode
passivation must be prevented to ensure long-term efficient operation. This can be achieved by regularly switching the polarity of the
electrodes and cleaning them frequently. In addition it will be necessary to measure residual Fe and Al concentrations in the treated
water when developing a practical process.

CRediT authorship contribution statement

Mahmood Jebur: Investigation, Methodology, Writing – original draft. Yu-Hsuan Chiao: Formal analysis, Methodology, Writing –
review & editing. Hideto Matsuyama: Writing – review & editing. S. Ranil Wickramasinghe: Funding acquisition, Supervision,
Writing – review & editing.

Declaration of competing interest

The authors declare the following financial interests/personal relationships which may be considered as potential competing in­
terests: S. Ranil Wickramasinghe reports financial support was provided by National Science Foundation. Yu-Hsuan Chiao reports
financial support was provided by Japan Society for the Promotion of Science. S. Ranil Wickramasinghe reports financial support was
provided by Japan Society for the Promotion of Science.

Data availability

Data will be made available on request.

Acknowledgements

This work was supported by the Arkansas Research Alliance, National Science Foundation through (a) Industry/University
Cooperative Research Center for Membrane Science, Engineering and Technology, (IIP 1822101, 1913839, 1930079), (b) Research
Experiences for Undergraduates REU Site: From Bench to Market: Engineering Systems for High Efficiency Separations (EEC 1659653)
and the University of Arkansas. The author Y.-H.C. and R.W., acknowledges the JSPS International Research Fellow (Graduate School
of Science, Kobe University) and the Kobe University Strategic International Collaborative Research Grant (Type B Fostering Joint
Research). M. J. and S. R. W. acknowledge SAWS for provideing water samples and gor information on their current water treatment
system.

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M. Jebur et al. Water Resources and Industry 31 (2024) 100243

Abbreviations

BPS Bipolar Series


BGW Brackish Groundwater
DOE Design of Experiments
EC Electrocoagulation
EDX Energy-dispersive X-ray
ICP Inductive Couple Plasma
RO Reverse Osmosis
SAWS San Antonio Water System
SEM Scanning Electron Microscopy
TDS Total Dissolved Solids
TOC Total Organic Carbon
TSS Total Suspended Solids
UF Ultrafiltration
WAVE Water Application Value Engine
XRD X-ray Diffraction

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