Evaluation and optimization of electrocoagulation process

parameters for the treatment of oil drill site wastewater

Pramod Kumara, Tabish Nawaz*a, Swatantra P. Singha,b,c*
a
Environmental Science and Engineering Department (ESED), Indian Institute of Technology
Bombay, Mumbai 400076, India.
b
Centre for Research in Nanotechnology & Science (CRNTS), Indian Institute of Technology
Bombay, Mumbai 400076, India
c
Interdisciplinary Program in Climate Studies, Indian Institute of Technology Bombay,
Mumbai 400076, India

* Corresponding author. Email address: swatantra@iitb.ac.in, tnawaz@iitb.ac.in

Graphical Abstract:

1
Abstract: The effluent from the oil drilling site is a complex mixture of harmful chemicals
that causes environmental impacts on its disposal. The treatment of oil drilling site wastewater
has not been explored in-depth in the available literature and requires understanding about its
characteristics and optimization of the treatment process. In the present study, we have
optimized the electrocoagulation process with aluminum electrodes for the drill site wastewater
treatment. A multi-level factorial center composite design using response surface methodology
(RSM) is applied to quantify the individual and combined effect of the current density, pH and
inter-electrode distance (IED) on the COD removal from the drill site wastewater and the
energy consumption of the electrocoagulation process. The increasing current density shows
significant increase in COD removal. A similar trend was observed with decrease in pH on
COD removal. The model obtained from RSM study predicted the optimum current density,
pH, and IED within the experimental range of the study. It was found that the optimum
condition for DSW-1 samples for 78% COD removal is at 4.76 mA/cm2 and 4 pH, and for
DSW-2, we get the COD removal of 64% at 19.04 mA/cm2 and 1.2 cm IED. The study shows
that the current density is the dominant factor for the process's energy consumption and
operating cost as compared to the pH and IED. The study demonstrated optimization of the
electrocoagulation process in drill site wastewater treatment and could be effectively used for
large-scale treatment through the electrocoagulation process.

Keywords: drill site wastewater, electrocoagulation response surface methodology, current

density.

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1. Introduction

In recent times, the freshwater availability for consumption has been severely affected due to
population growth, unsustainable industrialization, and climate change (Jing et al., 2021;
Yavuz & Ogütveren, 2018). Wastewater streams generated from various industries cause a
two-fold impact on this issue – first, they pollute the available water resources, and second, the
'contaminants' load in these streams limits the chances of their reusability at the source end.
(Babu et al., 2020; Shahedi et al., 2020; Yavuz & Ogütveren, 2018). Furthermore, the
contaminants in different industrial wastewater pose a severe threat to living organisms as
many of them are carcinogenic in nature (Elnenay et al., 2017; Ighilahriz et al., 2014; Pichtel,
2016). To combat these issues, strict regulations, on-site treatment, and enhancing reusability
of the wastewater should be the prime focus (Babu et al., 2020; Fang et al., 2013; Yavuz &
Ogütveren, 2018). One of the industries on the list is the oil and gas industry which generates
wastewater at different extraction stages with high contamination levels due to the use of
different chemicals (Coday et al., 2014b; Hickenbottom et al., 2013a; Ighilahriz et al., 2014).
The wastewater generated during the construction of well to extract oil is termed as drilling
wastewater and the wastewater generated after well construction for oil and natural gas
recovery is termed as produced water (Coday et al., 2014b; Ighilahriz et al., 2014; Sardari et
al., 2018; Zhao et al., 2014). The drilling process consumes up to 3800 m3 of water that
generates wastewater streams comprising drilling additives and contains high concentrations
of chemical oxygen demand (COD), total suspended and dissolved solids (Coday et al., 2014a;
Elnenay et al., 2017; Hickenbottom et al., 2013a; Ighilahriz et al., 2014). The typical range of
of the mentioned parameters was found as COD 600-5600 mg l-1, total suspended solids, 0.5-
2.5 g l-1 mg, and toal dissolved solids 1.0-8.2 g l-1 ((Ighilahriz et al., 2014; Ma et al., 2016;
Mohamed et al., 2017; Mu et al., 2021; Zhang et al., 2021). Generally, the wastewater is
collected in the pit near the dilling site, and in most of operations, it is discharged off-site into
deep wells after the settlement of solids (Coday et al., 2014a; Hickenbottom et al., 2013a). This
kind of practice degrades the groundwater quality and could cause health issues upon further
use.

The drilling mud is used to drill the well and generates significant waste (Codey et al., 2014;
Changmai et al., 2019). The drilling mud consists of a mixture of chemicals like emulsifiers,
viscosifier, lubricants, proppants, gallants, crosslinkers, foamers, and stabilizers (Coday et al.,
2014a; Hickenbottom et al., 2013b; Ighilahriz et al., 2014; Pichtel, 2016). These chemicals in
drill mud threaten the ecosystem and public health, and many are carcinogenic in nature or

3
endocrine disruptors (Ighilahriz et al., 2014; Liu et al., 2020; Pichtel, 2016; Zhu et al., 2021).
The toxic and complex nature of the wastewater thus create the need for appropriate treatment
due to its high volume generations and disposal scenario (Hickenbottom et al., 2013).
(Changmai et al., 2019; Elnenay et al., 2017; Hickenbottom et al., 2013b; Ighilahriz et al., 2014;
Liu et al., 2020). Among the various treatment process available, electrocoagulation (EC) is
one of the processes that could be applied to treat the drill site wastewater effectively.

The EC process uses electricity and sacrificial metal as an electrode for the coagulation
process. It consists of an electrode arrangement in contact with the target wastewater. The
electric current passes through electrodes and causes the dissolution of the metal ions from the
anode and hydroxyl ions from the cathode (Hakizimana et al., 2017; Mollah et al., 2004a;
Mousazadeh et al., 2021; Sivaranjani et al., 2021). These metals ions generated in-situ cause
the formation of the floc by combining with hydroxyl ions within the wastewater (An et al.,
2017; Garcia-Segura et al., 2017; Ghernaout et al., 2012; Hakizimana et al., 2017; Kabdaşlı et
al., 2012; Mollah et al., 2004a). The complete process of treatment consists of three major
steps, i.e., the generation of ions at anode and cathode due to electrolytic reaction, formation
of coagulants in the wastewater, and lastly, the removal of the pollutant by adsorption that gets
settles down or floats to form the scum layer (Garcia-Segura et al., 2017; Hakizimana et al.,
2017; Islam, 2019; Mollah et al., 2004; Sahu et al., 2014; Kumar et al., 2021). In EC, multiple
factors affect the process, such as current density (CD), pH, electrode arrangement,
conductivity, reactor design, electrode arrangement, and concentration of other ions. The
researchers have considered many factors and their combinations to get the maximum possible
removal. The studies found that the removal also increases with an increase in electrolysis time
and CD (Elnenay et al., 2017; Khorram & Fallah, 2018; Wagle et al., 2020). The maximum
removal of 99 % was also achieved by combining CD and salt composition to treat produced
water (Manilal et al., 2020). The studies were also conducted using the combination of CD,
pH, reaction time for COD, hardness, and turbidity removal from produced water(Zhao et al.,
2014). Some studies have also used a combination of EC, forward osmosis, and microfiltration
for produced water and drilling wastewater treatment (Changmai et al., 2019; Sardari et al.,
2018). With these many factors, optimization of the process and mathematical modeling
become quite difficult (Amani-Ghadim et al., 2013). The mentioned limitations can overcome
this issue by applying experimental optimization methodologies such as response surface
methodology (RSM) (Khorram & Fallah, 2018; Ponselvan et al., 2009). This technique used
the statistical and mathematical equations/methods for developing a model and evaluating the

4
individual and combined effect of the number of parameters on the designed response. The
technique also provides the results in graphical forms that make it easier to visualize and
comprehend the results (Amani-Ghadim et al., 2013; Khorram & Fallah, 2018; Pi et al., 2014;
Wagle et al., 2020). In addition to these advantages, RSM dramatically decreases the total
number of experiments required for optimization, saving time and experimental costs.

The study focuses on drill-site wastewater treatment to optimize the EC process using the
response surface methodology. The study's objective is to evaluate the performance of the EC
process for the treatment of drilling site wastewater and optimize the process to remove
pollutants effectively. The optimization process is applied with two factors and three levels of
factorial design using a center composite design by using Design Expert software (version 13
year 2022). The two factors used for the optimization process are different for each wastewater.
The objective is to quantify the individual and interactive effects of the process parameters.
This will help in finding out the optimized value of process parameters. The energy and cost
estimation is also calculated to understand the energy and economic aspects of the process
parameters.

2. Material and methods

Wastewater characteristics

The wastewater was collected from the drill-site location at two depths of the wells owned
by Oil and Natural Gas Corporation (ONGC), Mehsana, Gujarat, India. The samples were taken
from the drill site at Mahesana from two depths, 1311 m, and 2300 m. The wastewater
characteristics are given in Table 1. The characteristic depicts the presence of high TDS in both
samples and a moderate level of suspended solids.

Table 1 Characteristics of the wastewater studied drill site wastewater

S. No Parameter Unit Concentration (μ± σ) n = 3
DSW-1 DSW-2
1 Total solids g l-1 11.61 ± 0.32 9.26 ± 0.33
2 Total dissolved solids g l-1 10.53 ± 0.22 6.99 ± 0.27
3 Total suspended solids g l -1 1.08 ± 0.18 2.27 ± 0.23
4 pH - 8.44 ± 0.02 7.61 ± 0.02
-1
5 Conductivity mS cm 21.04 ± 0.30 13.99 ± 0.30
6 COD mg l-1 560 ± 3.2 1488 ± 4.8

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 Experimental setup

The EC reactor of 400 ml capacity is fabricated with plexiglass. The aluminum electrodes of
dimensions 70×40×4 mm were taken for the experiments (Fig 1). All the experiments were
conducted in galvanostatic mode. The electrodes were connected to the external DC power
supply (make: HTC, 2021). The electrode was cleaned with carbide paper (C-220), washed
with deionized water, and put in 0.1 M hydrochloric acid and 0.1 M acetone solution. for x
hours. The EC process is carried out in batch mode and is continuously stirred to maintain the
uniformity of the sample during the process. The sample was taken and kept for 2 hours for
settlement of solids, and then the supernatant is used for analysis. Preliminary runs were carried
out to observe the behavior of the sample on COD removal by applying variables like CD,
reaction time, and pH. The runs were also carried out to set up the variables for optimization
study using the Design Expert software . The preliminary study's objective was to develop a
pair of variables for the optimization study.

2.2 Analytical methods

The sample measured the chemical oxygen demand (COD) values before and after the run.
For each run, the change in cell voltage (CCV) was recorded; CCV is the difference in voltage
value before and after the experiment by applying constant current value to the
electrocagulation experiement. The COD of the sample was measured by APHA standard
potassium dichromate titrimetric method. The COD removal efficiency was calculated using
Equation 1 below

(𝐶𝑖 − 𝐶𝑓 ) (1)
𝐶𝑂𝐷 𝑟𝑒𝑚𝑜𝑣𝑎𝑙 (%) = 𝑥 100
𝐶𝑖
Where Ci and Cf are the sample's initial and final COD in mg l-1.

The EC process is optimized using Response Surface Methodology (RSM) using Design-
Expert software version 13. The two factors three-point design by face-centered central
composite design (CCD) was applied to evaluate the effects of CD, inter-electrode distance
(IED), and pH individually and in combination on COD removal performance of the EC
process. The set of experiments obtained from the software is then carried out, and the data
obtained was then used to optimize the process and predict the optimum conditions for the
process. Based on preliminary results, the levels of variables was entered in the software for
each sample and the EC runs was generated by the software. A total of 13 experiments for each
sample were performed, 9 were based on a 3-level factorial design, and 4 additional

6
experiments replicated central points to predict the curvature and region of the optimum
condition. The experimental data obtained was utilized to fit a full quadratic model as follows:

2 2
𝑌 = 𝛽𝑜 + 𝛽1 𝑋1 + 𝛽2 𝑋2 + 𝛽11 𝑋11 + 𝛽22 𝑋22 + 𝛽12 𝑋1 𝑋2 + 𝜀 (2)

where, Y is the response (COD removal); β0, is the coefficient of model intercept, i(β1,β2),are
the linear coefficient of the the independent variables, (β11,β22), are the quadratic coefficient of
the independent variables and β12 is the interaction coefficient of the independent variables; X1
and X2 are the independent variables, and ε is error term in the evaluation. All of the coefficients
the variables impact on the dependent variable either in positive or negative manner, their
value suggest the impact they put on the dependent variable.

The data from a series of EC runs were fitted in the model, and coefficients were obtained for
the model. The model's quality and prediction power were analyzed by the value of the
coefficient of determination, R2. Fisher F-test was used to check the significance of the
parameters. The model coefficients obtained were selected based on their calculated probability
(p) value at a 95% confidence interval. The contour plots based on the experiment runs show
the effect of independent variables on the response variable. The predicted versus observed
plots also depict the performance of the model. The variables used in the optimization process
for each type of wastewater are shown in Table 2. The parameters for the DSW-1 are CD and
pH, and DSW-2 are CD and IED. The runs were designed based on three-level of the
independent variables. The experiment was designed to observe the individual and combined
effect of the independent variable on the response variable.

Table 2: The table depicts the coded value of the independent variables and levels of
variables used for the optimization study with the help of the software.
Level of variables
Wastewater Variables Code used
-1 0 +1
CD (mA cm-2) A 4.76 11.90 19.04
DSW-1
pH B 4 6 8
CD (mA cm-2) A 4.76 11.90 19.04
DSW-2
IED (cm) B 1.2 2.6 4

Cost and energy calculation

7
 Every treatment method bears a cost for its setup and operation. Consumption of energy is
a primary factor in the EC process operating cost. The energy consumption per kg of the
pollutant removed is calculated using Equation 3 (Wagle et al., 2020)

𝑉×𝑖×𝑡 (3)
𝐸𝐸 (kWh/kg) =
(60 × 10−3 )∆𝐶 × 𝑉𝑟

where, V is the cell voltage (V), I is the applied current (A), t is the reaction time (min), ΔC is
the difference in pollutant concentration (mg/L) before and after the EC treatment, and Vr is
the volume (L) of the EC reactor.

Other operating costs include electrode material consumption, labor, timely maintenance,
sludge and scum management, and other fixed costs. The operating cost chiefly includes the
cost of electrical energy required and electrodes consumed during the process. The equation
(3) below is used for the energy consumption, electrode consumption calculations, and
operating cost analysis of the EC process (Wagle et al., 2020)

Operating Cost = 𝑎𝐶𝑒𝑛𝑒𝑟𝑔𝑦 + 𝑏𝐶𝑒𝑙𝑒𝑐𝑡𝑟𝑜𝑑𝑒 (3)

where, Cenergy (kWh m-3) and Celectrode (Kg-Al m-3) are the electrical energy consumption and
amount of electrode dissolved for treating 1 m3 of wastewater. "a" and "b" are the unit cost of
electrical energy and electrode material. The value for "a" is Rs 6.09 unit-1 , and "b" is Rs 350
kg-1.
𝑉∗𝐼∗𝑡 (4)
Cenergy (kWhm-3) =
𝑉𝑟 ∗1000∗60
𝑀𝑤 ∗𝐼∗𝑡 (5)
Celectrode (Kg of Alm-3) =
𝑧∗𝐹∗𝑉𝑟 ∗1000∗60

where V, I, t, Vr, Mw, z, and F are voltage (V), current (A), reaction time (min), reactor volume
(m3), the molecular mass of aluminum (26.98 g mol-1), number of electrons transferred (3), and
Faraday's constant (96487 C mol-1), respectively.

3. Result and discussion

Preliminary results of the study

The sample was preliminary treated at different CD, pH, and reaction time values.. In the
preliminary studies, the IED was kept constant at 2 cm in all the runs, and the mixing speed
was maintained at 300 rpm. The result obtained from the preliminary studies is shown in figure
1. The results show that the COD removal increases in both samples with increased reaction
time and CD. There is a significant increase in COD removal on increasing the CD, as shown

8
in fig 1b. In the case of DSW-1 at 11.90 mA cm-2 CD, the removal efficiency increases from
13.33% to 41.11% percent by increasing the run-time from 15 to 45 minutes. The effect of pH
was observed by treating the sample at their natural pH as given in table 1and an acidic pH
value of 4, and was shown in figure 1c. On varying the pH to 4, the increase in COD was
observed in both the samples. Similarly, from fig 1d, on increasing the CD from 4.76 mA to
19.04 mA cm-2, the COD removal increases from 35.56% to 61.25 %.

Figure 1: Illustration of the experimental work. A) Electrocoagulation setup; b) Effect of time on

COD removal; c) effect of pH on COD removal. d) effect of pH on COD removal

A similar trend was observed in the case of DSW-2; on increasing the reaction time from
15 to 45 minutes, the removal increases from 19.23 to 57.69%, and on increasing CD from 4.76
to 19.04 mA cm-2, the removal increases from 42.31 to 65.21%. Similar results were observed
in other studies; researchers depict that increasing the CD causes an increase in bubble density
and decreases bubble size, enhancing the removal process (Khosla & Venkatachalam, 1991).
Researchers also depict the COD removal increase with the reaction time due to an increase in
flocs formation and settlement(Huda et al., 2017). Therefore, increasing the COD removal by
increasing the reaction time is a predicted point followed in studies.

9
 Based on the results observed from preliminary studies, the reaction time was kept constant
at 45 minutes as the maximum COD removal was observed between 30 to 45 minutes in both
the samples. Furthermore, the other parameter that affects the process is CD, as it directly
influences the coagulant generation, so it was kept as a variable for both the samples. The other
parameter for the optimization process, in the case of DSW-1, was selected as pH. The effect
of initial pH plays a crucial role in determining the performance of the EC process. Various
studies have used a range of pH values to maximize COD removal. Researchers varied the
initial pH from 5-to 11 to analyze its effect on COD removal (Tir & Moulai-Mostefa, 2008). It
was observed that dominant aluminum species play a critical role in pollutant removal at a pH
range of 5-6 (Ponselvan et al., 2009). A similar trend was observed on varying pH from 4-10
for COD removal (Faheem et al., 2021). In the case of DSW-1, the effect of change in pH was
observed to be more dominating in DSW-1 than DSW-2. On changing the pH value to 4, the
increase in COD removal was more than doubled from 42 to 88 % in the case of DSW-1, while
for DSW-2, the change in COD removal was only marginal, form 53% to 67%. .

The results depict pH as an impactful variable for DSW-1. Therefore, the other parameter
selected for optimizations analysis for DSW-1 was pH. For DSW-2, the other parameter
selected was IED, as it also plays a significant role in removing pollutants. The IED affects
drop in the ohmic resistance of the cell,it increases by increasing the IED. The IED also affects
the electric energy; for a low conductivity solution, the energy consumption increases with the
IED and vice versa (Mollah et al., 2004a; Yoosefian et al., 2017). The decrease in IED value
also causes more bubbles generation and leads to high mass transfer and reaction rate between
the pollutant and coagulant (Mollah et al., 2001; Sahu et al., 2017; Hakizamana et al., 2017).
The two variables are paired with CD to observe COD removal's individual and combined
effect.

Effect of variables on treatment performance

RSM is commonly used for optimization purposes in industry and academic research areas
when a number of variables influence the system's performance (Khorram & Fallah, 2018).
This technique provides a relationship between the independent variables and response or
dependent variables. The software generated experimental runs, and the COD removal results
and CCVs are presented in Table 3. All the parameters have significantly affected COD
removal except the IED, the p-value of IED was 0.40, which is more than the significant p-
value of 0.05. In the case of DSW-1, the synergistic effect of the two variablesi.e., pH and CD,
was observed. In the case of DSW-2, the CD is the major factor leading the removal process.

10
The CCV also reaches its maximum value of 0.4 V in case of wastewater with low
conductivity, i.e., DSW-2. There is a synergistic effect of both variables, CD, and pH, on the
CCV in the case of DSW-1; the increase in CD increases the COD remaoval and CCV, and
the decrease in pH increases the COD removal. Whereas, in the case of DSW-2, CD plays a
major role in COD removal compared to IED. It means that the pH and CD play a significant
role in the COD removal process and contributes to the system performance; specifically, CD
contributes majorly to the treatment performance for both the wastewater samples within the
experimental range of this study
Table 3: Experimental results obtained from the factorial runs of COD removal and the CCV
between the two samples.
DSW-1 DSW-2
Run CD pH COD CCV (V) CD IED COD removal CCV (V)
(mA removal (% (mA (cm) (% ±SD)
-2
cm ) ±SD) cm-2)
1 11.90 4 81.88 ± 0.46 0.12 11.9 2.6 43.32 ± 1.07 0.13
2 19.04 6 90.5 ± 1.03 0.18 11.9 1.2 44.00 ± 0.91 0.3
3 19.04 4 80.86 ± 0.54 0.2 11.9 4 47.06 ± 0.62 0.18
4 4.76 8 22.64 ± 2.25 0.01 19.04 4 64.76 ± 0.59 0.52
5 11.90 6 70.52 ± 0.64 0.07 19.04 1.2 60.78 ± 0.33 0.18
6 4.76 4 77.03 ± 1.75 0.16 19.04 2.6 70.59 ± 1.35 0.2
7 11.90 6 71.5 ± 0.64 0.07 4.76 2.6 32.14 ± 1.15 0.1
8 11.90 6 70.52 ± 0.64 0.07 11.9 2.6 42.26 ± 1.07 0.13
9 11.90 6 71.43 ± 0.64 0.07 11.9 2.6 42.86 ± 1.07 0.13
10 11.90 8 57.14 ± 0.52 0.1 4.76 1.2 42.00 ± 8.03 0.2
11 19.04 8 67.46 ± 1.25 0.3 4.76 4 44.00 ± 6.65 0.21
12 11.90 6 70.52 ± 0.64 0.07 11.9 2.6 42.04 ± 1.07 0.13
13 4.76 6 66.67 ± 0.27 0.1 11.9 2.6 41.05 ± 1.07 0.13

The quadratic model stated in equation 2 was developed by the experimental data to
replicate the effect of variables during the EC process. The model terms developed by the data
were tested for their significance statistically using a t-test. The significant level of all the
variables was tested at the 95% confidence limit, the significant variables were included, and
nominal terms were excluded from the model. The model's significance can also be tested by
calculating the coefficient of variance, it depicts the spread of the data around the mean and its
acceptbale values should be less than 10 % (Asfaha et al., 2022; Nasrullah et al., 2022) In the

11
current study, the coefficient of variance was calculated, in the case of DSW-1 the value is
7.56; for DSW-2, it was 8.76. The model developed for the COD removal, and the CCV is
shown in table 4 with the respective R2 and adjusted R2 value. The scatter plots of predicted
versus actual values for COD removal and the CCV are shown in fig 2 and fig 3. The R2 value
for COD removal suggests that the models explain 92- 94% of the process and 80-97% in case
of the CCV. The high value of the adjusted R2 value also shows the significance of the model.
The difference between R2 and adjusted R2 also advocated the high significance of the model
(Acharya et al., 2020). Similar trends were also observed in other studies with dye, palm oil,
and textile wastewaters, where observed and adjusted R2 values were ~99% and ~98%,
respectively (Amani-Ghadim et al., 2013; Khorram & Fallah, 2018; Nasrullah et al., 2022).
The trend of R2 value of more than 95% was observed in the case of COD removal in studies
done with other kinds of wastewater and is considered a reliable and effective model for
optimizing the process (Manilal et al., 2020; Nasrullah et al., 2022; Ponselvan et al., 2009; Tir
& Moulai-Mostefa, 2008). The results from all the studies show the closeness of the of R2, and
the adjusted R2 value depicts that the model and the independent variable are significant
statistically and can predict the response (Acharya et al., 2020; Khorram & Fallah, 2018;
Nasrullah et al., 2022).

Figure 2: Illustration of the predicted versus actual COD removal of the model obtained from RSM.
a) DSW-1; b) DSW-2

12
 Figure 3: Illustration of the predicted versus the actual CCV of the model obtained from RSM. a)
DSW-1; b) DSW-2

Table 4: Statistical parameters obtained from response surface model

Sample Response R2 Adjusted Significant Quadratic model of response

2
R terms
DSW-1 COD removal (%) 0.94 0.8974 A, B, AB, B2 72.99+12.08A -15.42B +10.25AB -8.72B²

CCV (V) 0.97 0.9375 A, AB, A2, B2 0.0717-0.0117B + 0.0625AB + 0.0640A²

+ 0.0340B²
2
DSW-2 COD removal (%) 0.92 0.8552 A, A 42.54+ 13.00A +8.24 A2

CCV (V) 0.80 0.6526 A, AB, B2 0.1276 +0.065A+ 0.0825AB + 0.1184B2

Response surface Modelling(RSM)

RSM helps in estimating the significant operating parameters of the process and their
synergistic and antagonistic effects (Ponselvan et al., 2009). Based on the result obtained from
the factorial design, response surface modeling was performed to visualize the effect of the
independent variable on the response variable. Although the result table and model developed
by the RSM significantly illustrate the effects of the variables, the visualization of the effects
provides a more intuitive representation of the data. The individual and combined effect of CD,
pH, and IED on the COD removal and CCV was presented in the graphical form by the
software. The contour plots and 3d surface plots for COD removal are shown in fig 4. The

13
contour plots are the 2D representation of the response variable where each line shows the
individual removal efficiency and its curvature with the independent parameter. The 3D plot
shows the effect of individual parameters on the response and 3D repsentaion. Both the tools
help in understanding the synergestic or antagonistic reffect of the independent paraemters on
the response variable. The contour plot provides thw values of the independent variables to
achieve a certain value of efficiency and the 3d plot depicts the curvature and the point of
inflexion for each parameter i.e., the value at which the parameters change its direction.

Other studies carried out also used the above parameters to evaluate the effect on
different responses like COD removal, turbidity removal, decolorization, and TOC removal
(Khorram & Fallah, 2018; Maha Lakshmi & Sivashanmugam, 2013; Ponselvan et al., 2009;
Tir & Moulai-Mostefa, 2008). The most common parameters used in all studies in CD and
reaction time, and apart from these, pH, electrolyte, inter-electrode concentration, and initial
pollutant concentration were used for optimization. The individual and combined effect of
parameters on the response helps to understand the EC process and manage the desired point
of pollutant removal by optimizing the process parameters.

3.3.1 Impact of CD, pH, and IED

Among all the parameters in the EC process, CD plays a vital role in the removal
process. It controls the reaction rate and determines the metal dissolution rate in the reactor
(Khorram and Fallah, 2018). The CD causes the generation of metal ions that form flocs that
either settle or float up to form a scum layer (Sahu et al., 2014; Hakizimana et al., 2017). In the
case of both samples, an increase in CD increases the removal and reaches the maximum at
19.04 mA cm-2 value. The maximum removal of 90.5 % and 70.59% was achieved with DSW-
1 and DSW-2, respectively, at the maximum CD of 19.04 mA cm-2 (fig 4). The contour lines
and the 3D plot shows that COD removal increases with the increase in CD in both samples.
In the EC process, oxidation occurs at the anode due to the current flow and causes the
generation of Al3+ ions and OH- at the cathode due to water reduction. Those two metal ions
react and form monomeric and polymeric hydroxyl of aluminum that act as coagulants and
form the flocs (Mollah et al., 2001). A large polymeric chain formation leads to contaminant
removal by attachment to the chain and precipitation. The formation of Al3+ also causes
destabilization of the colloidal particles and leads to either settling or collapsing to form flocs
with aluminum flocs (Hakizimana et al., 2017; Moussa et al., 2017). The CD increases the

14
number of metal ions and the formation of flocs and the amount of Al ions formed during the
process was explained by Faraday's law (equation. 6) (Wagle et al., 2020).
𝑖𝑡𝑀 (6)
𝑊=
𝑧𝐹

where, W is the aluminum dissolved in grams, i is the current in Ampere, t is the run time in
seconds, M is the atomic weight of aluminum, Z is the number of electrons (3 for Al), and F is
the Faraday constant. The relationship shows that current is directly proportional to the amount
of aluminum generated in the solution, and increasing the value leads to pollutant removal.

The effect of variation in pH was also investigated by varying the pH from 4 to 8 and the result
is illustrated in fig 4a. The region of maximum removal was observed between the pH range
of 4-6 at all CD values, and the removal was more than 70 %. The maximum removal of 90.5%
percent was observed at 6 pH and 81.88% at 4 pH, at the maximum CD of 19.04 mA cm-2.
These results agree with previous studies, and it was observed that the maximum COD removal
was obtained for pH< 6.0 (Ponsevlan et al., 2009). In another study, the maximum COD
removal of more than 80 % was also observed at pH 4 (Genec et al., 2012). At a low pH value,
metal species like Al3+ generated at the anode cause destabilization of the colloidal particles.
This causes agglomeration of the particles that precipitate or float up by the bubbles to form a
scum layer At a pH of around 6 and more, amorphous aluminum monomeric and polymeric
species cause adsorption, and many such species cause sweep coagulation (Canizares et al.,
2007). The results confirm the impacts of pH on the removal process and critical parameters
for EC for drill-site wastewater treatment.

15
 Figure 4: Graphical reprsentaiton of the Contour and 3d surface plots of COD removal for
the two samples. a) DSW-1; b) DSW-2.

The combined effect of pH and CD can be visualized from the 3D plot in fig 4a, it was observed
that with increased CD, the removal process enhances while maintaining a constant pH. On the
other hand, by increasing the CD and pH simultaneously, we can observe a reduction in COD
removal from 4 to 8. In the case of pH 4, the removal of 77% was obtained at the CD of 4.76
mA cm-2. On increasing the pH, it reduces to 22% removal, while on increasing the current, it
reaches 80%. As seen in fig 4a, in the region of 5-6 pH, there is a small increase and drop in
COD removal, signifying the optimum pH range for COD removal. Similar kinds of trends
were reported in other studies too; the optimum condition of pH for COD removal was in the
range of 4-7 (Faheem et al., 2021; Gengec et al., 2012; Khorram & Fallah, 2018; Tak et al.,
2015; Tir & Moulai-Mostefa, 2008). It was observed that the maximum COD removal at 5 pH

16
remains constant till 6 pH and starts decreasing after that value (Tir & Moulai-Mostefa, 2008).
Similar result was observed in other studies, the maximum removal was reported in the n the
pH range of 4-6 (Gengec et al., 2012; Khorram & Fallah, 2018). All the studies showed that
the effective pollutant removal region was observed in acidic pH. The reason behind this
phenomenon is that in a acidic medium formation of Al3+ ions and hydrolysis of the ions lead
to the formation of monomeric Al(OH)2+ and Al(OH)2+. These monomeric cations further react
to form hydroxypolymeric chains such as Al2(OH)24+ and Al6(OH)153+ (Faheem et al., 2021).
The polymeric chains formed have a large surface area and cause adsorption of entrapment of
soluble organic and inorganic compounds and colloidal particles. The particles' adsorption and
entrapment will separate from the solution by settlement or floating by bubbles.

Figure 5: Contour and 3d surface plots of COD removal. a) DSW-1; b) DSW-2

17
 In the case of DSW-2, the combined effect of CD and IED can be seen in fig 4b. The
contour and 3d plot depict the COD removal effect of varying the independent variables. It can
be observed from the contour plot that the effect of IED on COD removal is insignificant as
compared to the CD. Although, it can be observed that at 2.6 cm IED, we get maximum
removal of 70.59% for a CD of 19.04 mA cm-2. Also, at the CD of 11.9 mA cm-2, we get the
removal in the 43-47% range in all the IED values. The only effect of IED was observed in the
case of maximum CD, at maximum CD value, the COD removal first increases and then
decreases by varying the IED form 1.2 to 4 cm, although the difference was insignificant. The
possible reason for these results could be the high conductivity of the wastewater that nullifies
the resistance caused by varying the IED. The IED variation affects the electrode resistance;
therefore, for a constant current value more voltage is required to overcome that resistance.
Therefore we require an optimum IED value for the process, which provides maximum
pollutant removal (Huda et al., 2017; Ponselvan et al., 2009). In the samples DSW-1 and DSW-
2, due to the high conductivity of the wastewater the effect of IED gets diminished and the
voltage developed by varying the IED did not impact the COD removal process; hence, the
effect was seen in the results.

The effect of varying the independent parameters (CD, pH, IED) on the CCV during the process
was also observed and shown as contour and 3d plots in fig 5. The voltage applied during the
process was the sum of the equilibrium overpotential anode and cathode overpotential and
ohmic resistance drop of the solution (Chen et al., 2002). It directly influence the energy
consumption and as its value increases so is the energy consumption of the process. In the case
of DSW-1, the maximum CCV of 0.25 V was observed at the maximum CD value of 19.04
mA cm-2 and at pH 8. It was also observed from fig 4 a, that at a constant pH 8 value, increasing
the CD from 4.76 mA cm-2 to 19,04 mA cm-2 increases the CCV from 0.05 to 0.25 V.
Furthermore, it was observed that at a low CD value of 4.76 mA cm-2, the CCV increases from
0.01 to 0.16 V and at high CD value of 19.04 mA cm-2 it decreases from 0.3 to 0.2 of by varying
the pH from 8 to 4. The two results signify that high CD and low pH or acidic pH cause the
major CCV. Due to high current input, more voltage is required to be pushed to manage the
power requirements as power is directly proportional to the current and voltage; however, the
high conductivity value can compensate for the power requirement. It was reported that current,
voltage, and conductivity are correlated to each other and hence the parameter associated with
them, like CD and power requirement (Chen et al., 2002). Although the change in the CCV
due to change in CD is not major, it still signifies that the CD impacts the change in voltage

18
and plays a dominant role in the process. Additionally, it was observed that in the case of
aluminum electrodes less CCV was observed as compared to other metals used in EC
(Izquierdo et al., 2010). In the case of DSW-2, a similar trend was observed with an increase
in CD.

The CCV change was maximum at high CD and at high IED values. The minimum change
was observed in the IED value of 2.6 cm. At a low IED value, due to less resistance, flow of
current is smooth and hence causes less CCV (Ponsevlan et al., 2021). At a high IED of 4 cm,
the resistance is higher than low IED value of 2.6 cm ; hence, the voltage needs to increase to
maintain the flow of constant current, which adds to the CCV value (Huda et al., 2017). It was
observed that change in voltage also impacts the removal process as it also directly affects the
bubble generation (Khatibikamal et al., 2010). In the case of aluminum, it was reported that the
CCV also causes significant COD removal up to a certain optimum value and has a low impact
on COD removal after the optimum conditons. after that point (which point?) (Moosavirad,
2017). From results obtained by treating both the samples, it can be concluded that CD, pH,
and IED play a role in the CCV initially and during the process any changes in above mentioned
parameters also reflects the impact on CCV .

3.3.2 Optimization of Cost and energy consumption

The energy consumption with respect to COD removal and electrode was calculated and
shown in Table 5. The operating cost associated with energy is shown in Table 5. In the case
of DSW-1, the energy consumption value ranges from 0.81 to 10.38 Kwh kg-1COD-1 with COD
removal of 67-77%. The maximum removal of 90% was observed with an energy consumption
of 7.22 Kwh kg-1COD-1. The minimum energy consumption was observed at acidic pH and at
4.76 mA cm-2. In contrast, the maximum value of ? was at pH 8 and a CD of 19.04 mA cm-2.
A similar trend was observed in the process' operating cost and was in agreement with earlier
studies on other kinds of wastewaters (Elabbas et al., 2016; Kobya et al., 2003; Tezcan et al.,
2009). It was reported that the increase in CD value contributes directly to energy consumption
(Faheem et al., 2021). It can be evident that energy consumption is directly affected by the
current supply. The energy consumption increases from 0.53 to 3 Kwh m-3 on increasing the
CD from 10 to 40 mA cm-2 (Lakshmi et al., 2013). Furthermore, it was observed that a pH
change does not significantly affect operating costs. In DSW-1, the change in pH from 4 to 8
increases the operating cost from 0.041 to 0.42 USD m-3. A similar result was reported that
changing pH from 4 to 10 does not significantly affect energy consumption and operating cost

19
Faheem et al. (2021). Thus it can be concluded that CD contributes majorly to energy
consumption and operating cost, followed by IED and pH. However, the impact of CD is way
more than the other two parameters.

Table 5: Energy consumption and cost analysis at different values of variables of the two samples.

DSW-1
CD (mA pH EE (Kwh kg- Cenergy Celectrode Operational
cm-2) 1
COD-1) (Kwhm-3) (kg of Alm-3) Cost (USD m-3)

4.76 4 0.81 0.53 2.80E-05 0.04

19.04 4 6.83 4.68 1.12E-04 0.36
4.76 8 2.81 0.54 2.80E-05 0.04
19.04 8 10.38 5.94 1.12E-04 0.46
4.76 6 0.93 0.53 2.80E-05 0.04
19.04 6 7.22 5.54 1.12E-04 0.43
11.9 4 3.23 2.24 6.99E-05 0.17
11.9 8 4.95 2.40 6.99E-05 0.18
11.9 6 3.70 2.24 6.99E-05 0.17
DSW-2
CD (mA IED EE(Kwh kg-1 Cenergy Celectrode (kg Operational
cm-2) (cm) COD-1) (Kwh m-3) of Al m-3) Cost (USD m-3)
4.76 1.2 2.50 0.42 2.80E-05 0.03
19.04 1.2 12.24 3.168 1.12E-04 0.24
4.76 4 2.86 0.594 2.80E-05 0.05
19.04 4 23.28 6.072 1.12E-04 0.47
4.76 2.6 4.08 0.525 2.80E-05 0.04
19.04 2.6 15.64 4.416 1.12E-04 0.34
11.9 1.2 7.42 1.425 6.99E-05 0.11
11.9 4 11.71 2.6475 6.99E-05 0.20
11.9 2.6 11.46 1.965 6.99E-05 0.15
CD: CD.

Whereas, in the case of DSW-2, the energy consumption varied from 2.5 to 23.28 Kwh kg-
1
COD-1 with COD removal of 43-65 %. The maximum removal was also observed at the energy
consumption of 15.64 Kwh kg-1COD-1. In both samples, the CD is the dominating factor in
energy consumption; however, changes in the IED value significantly affect operating costs.

20
While increasing the IED from 1.2 to 4 cm increased the operating cost from 0.05 to 0.03 USD
m-3 at 4.76 mA cm-2 and, a similar trend was observed on increasing the CD value, the cost
increased from 0.03 to 0.24 USD m-3; from 4.76 to 19.04 mA cm-2. Increasing the IED causes
an increase in resistance, leading to an increase in the CCV that causes more energy to be
required to overcome the resistance.

Table 6: Optimization value of independent variables based on optimum criteria

Optimum criteria DSW-1 DSW-2

CD (mA cm-2) pH CD (mA cm-2) IED
(cm)
Max COD removal (%) 19.04 5.4 19.04 4
Min Cost 4.83 6.2 4.76 4
Min cost and max COD removal (%) 4.76 4 19.04 1.2

The optimization of the process for the two wastewater was shown in table 6. The
optimization was carried by the help of the software and is based on the criteria required at the
end. In each case, all other parameters were kept in range, and the parameter was either
maximized or minimized. In both the samples, the minimum cost criteria have the highest
desirability of 1 and 0.951 in DSW-1 and DSW-2. Although in both cases, it gives the
maximum COD removal of 39.84% and 41.208. The maximum COD removal criteria give out
86.19 % and 68.19% COD removal in both wastewaters. The minimum cost and maximum
COD removal criteria give the best combination and a significant COD removal of 78.21% and
64.19%. It should be noted that earlier studies show optimized conditions based on maximum
pollutant removal. The reason could be to meet the desired discharge standard. However, this
study demonstrated that treatment costs could be optimized simultaneously with maximum
COD removal based on wastewater management objectives.

Energy consumption per percent COD removal

The validation of the results was carried out by calculating the results of energy
consumption per percent COD removal versus the process parameters for both the samples; the
results obtained are shown in fig 6. In the case of DSW-1, the energy consumption per percent
COD removal versus pH depicts a similar pattern in all CD values, as shown in fig 6a. However,
the difference in energy consumption between 11.9 and 19.04 mA cm-1 CD value is 1.5 times
more than the CD value of 11.9 and 4.76 mA cm-. Furthermore, it can be observed that this

21
difference keeps increasing at higher pH values of 6 and 8. This indicates the impact of pH
with CD; at low pH of 4-6, the Al metal ions flocs formation rate is higher than at 8 pH, and
hence there is more COD removal in less energy consumption. The energy consumption per
COD percent removal versus CD was also calculated and plotted for varying CD in fig 6b. The
fig shows that at pH values of 4 and 6, the difference in energy consumption is negligible at all
CD values. Although the case is opposite with 8 pH, the energy consumption is twice more
than the pH 4 and 6 at CD value of 4.76 mA cm-1, and the difference decreases at 11.90 mA
cm-1 CD and then increases for 19.04 mA cm-1 CD value. The results depict that the optimum
condition for energy consumption per percent COD removal is 11.90 mA cm-1 and 6 pH value.

Figure 6: Illustration of the energy consumption per COD removal versus the process parameters in the
analysis; a)DSW-1 pH; b) DSW-1 Current Density; c) DSW-2 Inter-Electrode Distance; d) DSW-2
Current Density.

In the case of DSW-2 the energy consumption per percent COD removal versus IED and
CD was shown in figs 6c and 6d respectively. The difference in energy consumption at the IED
value of 1.2 cm is the same for all CD values, but for 2.6 cm IED, the difference is more
between the CD value of 4.76 and 11.90 mA cm-1 than between 11.90 and 19.04 mA cm-1.
Although the difference in energy consumption between 4.76 and 11.90 mA cm-1 becomes
constant at IED above 2.6 cm, it keeps on increasing for 11.90 and 19.04 mA cm-1 CD value.
The results indicate that increasing the IED value increases the energy consumption as the

22
resistance increases, impacts the current flow, and hence requires more voltage to pass current
through the medium, resulting in energy consumption. However, the difference in energy
consumption at different IED values is not that high due to the high conductivity of water that
compensates for the resistance. But the difference in consumption depicts the impact of IED in
the low conductivity water system. The energy consumption per percent COD removal versus
CD shows that the difference in energy consumption at the CD value of 4.76 mA cm-1 is almost
the same for all IED values. While increasing the CD value to 11.90 mA cm-1, the energy
consumption was almost the same for the IED value of 2.6 and 4 cm, and at the CD value of
19.04 mA cm-1, the difference in energy consumption rapidly increased for the IED value of 4
and CD value of 19.04 mA cm-1. This also depicts that at a high CD value, the energy
consumption is less at a low IED value and more at a high IED due to an increase in resistance.
The results show that the optimum energy consumption condition is 1.2 cm and 11.90 mA cm-
1
.

4. Conclusion

In this study, the performance of EC with aluminum electrodes was investigated with two
different drill site wastewater. The process was optimized with the help of response surface
methodology using design expert software. The result of the factorial experiments showed that
the CD has a major effect on COD removal, followed by pH and inter-electrode distance has
the least effect on COD removal. The model generated for COD removal for both samples has
an R2 value of more than 90%. It was also demonstrated that significant COD removal was
obtained at low pH and low CD. Furthermore, it was observed that the effective pH range of
COD removal is 4-6. In the case of a CCV, high current and low pH contribute more to the
CCV than inter-electrode distance. Increasing the inter-electrode distance increases the CCV.
The effect of these parameters on cost and energy consumption is also evaluated. The
maximum cost was obtained at high CD and low pH in the case of DSW-1 and high CD and
maximum value of inter-electrode distance in the case of DSW-2. The optimum range for
DSW-1 was obtained at 4.76 mA cm-2 and 4 pH, and for DSW-2, 19.04 mA cm-2 and 1.2
inter-electrode distance. The energy consumption and cost analysis indicate that current plays
a significant role in optimizing the EC process, followed by pH and IED, and has a major
impact on them. The present study first presents the optimization process for drill site
wastewater treatment using RSM and further focuses on energy and cost evaluation. The study

23
demonstrated the effectiveness of EC in treating oil drill site wastewater and depicts the
significance of optimization for both process and energy and cost optimization. This study
could open the path for on-site drill site treatment and bring a holistic study on energy and cost
optimization of the treatment process.

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