STOTEN-21364; No of Pages 20

Science of the Total Environment xxx (2016) xxx–xxx

Contents lists available at ScienceDirect

Science of the Total Environment

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

Review

Emerging usage of electrocoagulation technology for oil removal from

wastewater: A review
Chunjiang An a,b, Gordon Huang a,b,⁎, Yao Yao a, Shan Zhao b
a
Faculty of Engineering and Applied Science, University of Regina, Regina S4S 0A2, Canada
b
Institute for Energy, Environment and Sustainable Communities, University of Regina, Regina S4S 0A2, Canada

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Oil is one of the most important hydro-

carbon products in the modern world.
• There is a significant increase in the
amount of oil-containing wastewater.
• This review provides a deep insight into
the electrocoagulation for oil removal.
• It presents a full-scale review on the
most recent efforts in this emerging
field.

a r t i c l e i n f o a b s t r a c t

Article history: Electrocoagulation is a simple and efficient treatment method involving the electrodissolution of sacrificial an-
Received 3 October 2016 odes and formation of hydroxo-metal products as coagulants, while the simultaneous production of hydrogen
Received in revised form 8 November 2016 at the cathode facilitates the pollutant removal by flotation. Oil is one of the most important hydrocarbon prod-
Accepted 9 November 2016
ucts in the modern world. It can cause environmental pollution during various stages of production, transporta-
Available online xxxx
tion, refining and use. Electrocoagulation treatment is particularly effective for destabilization of oil-in-water
Editor: Jay Gan emulsions by neutralizing charges and bonding oil pollutants to generated flocs and hydrogen bubbles. The de-
velopment of electrocoagulation technologies provided a promising alternative for oil removal from wastewater.
Keywords: This paper presents a review of emerging electrochemical technologies used for treating oil-containing wastewa-
Electrocoagulation ter. It includes a brief description of the oily wastewater origin and characteristics. The treatment processes de-
Oil veloped so far for oily wastewater and the electrocoagulation mechanisms are also introduced. This paper
Wastewater treatment summarizes the current applications of electrocoagulation for oil removal from wastewater. The factors that in-
Removal mechanisms fluence the electrocoagulation treatment efficiencies as well as the process optimization and modeling studies
Design and process parameters
are discussed. The state-of-the-art and development trends of electrocoagulation process for oil removal are fur-
Physico-chemical processes
ther introduced.
© 2016 Elsevier B.V. All rights reserved.

⁎ Corresponding author at: Faculty of Engineering and Applied Science, University of Regina, Regina S4S 0A2, Canada.
E-mail address: gordon.huang@uregina.ca (G. Huang).

http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
0048-9697/© 2016 Elsevier B.V. All rights reserved.

Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
2 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2. Theoretical background of electrocoagulation treatment strategy. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.1. Characteristics of oily wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2. Available technologies for oil removal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.1. Gravity separation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.2. Hydrocyclones . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.3. Sorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.4. Chemical precipitation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.5. Flotation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.6. Membrane filtration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.7. Chemical oxidation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.2.8. Biodegradation. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.3. Basics of electrocoagulation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.3.1. Principles of electrocoagulation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
2.3.2. Destabilization and separation of oil-in-water emulsion by electrocoagulation . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3. Electrocoagulation applications for oil removal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.1. Oil removal from oilfield wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.2. Oil removal from petroleum refinery wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.3. Oil removal from metal processing and finishing wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.4. Oil removal from ship and vehicle cleaning wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.5. Oil removal from food processing wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.6. Oil removal from slaughterhouse wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.7. Oil removal from tannery wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
3.8. Oil removal from restaurant wastewater . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4. Optimization and modeling of electrocoagulation process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1. Influencing factors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1.1. Initial pH . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1.2. Current density . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1.3. Reaction time . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1.4. Electrode configuration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1.5. Wastewater conductivity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1.6. Initial oil concentration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.1.7. Other influencing parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.2. Optimization of electrocoagulation treatment process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
4.3. Modeling of electrocoagulation treatment process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
5. Technology advancement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
5.1. Advancements in reactor design and electrode selection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
5.2. Advancements in operation and control. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
6. Integration of electrocoagulation and other treatment techniques . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
7. Concluding remarks and recommendations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
Abbreviations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 0

1. Introduction
Oil is one of the most important hydrocarbon products in the mod-
ern world (Hildenbrand et al., 2016; Rengasamy et al., 2011). Oils may
be released into the environment at various stages of production, trans-
portation, refining and use. Major industrial sources of oily wastewater
include oil refineries, petrochemical, metal manufacture, machining and
finishing, food processing, textile and leather (Kajitvichyanukul et al.,
2011). Oily wastewater can also come from municipal sources such as
kitchen and human wastes (Hussein et al., 2008). Oils found in contam-
inated water can be fats, lubricants, cutting liquids, tars, grease, crude
oils, diesel oil, kerosene, jet fuel, gasoline, etc. (Srinivasan and
Viraraghavan, 2010). Oil concentrations in effluent also vary quite wide-
ly in different sources, from 1 to as high as 40,000 mg/L (Zouboulis and
Avranas, 2000). With the rapid industrial and urbanization develop-
ment during the past decades, a large amount of oily wastewater is gen-
erated from various sources (Suzuki and Maruyama, 2005). The global
amount of oily wastewater was 9–14 billion m3 in 2012 (Gitis and
Rothenberg, 2016). When discharged to the environment, oily waste-
water causes the formation of surface films and shoreline deposits,
which impact ecological resources and functions (Barrera-Díaz et al.,
2006; Noh et al., 2015). It can affect surface and groundwater resources,
endangering aquatic system and human health (Fox et al., 2016; Phillips
et al., 2015). The biodegradability of oil in natural ecosystem is low and
oily components can hinder biological functions in the environment for
a long time. Therefore, it is essential to remove oil from wastewater be-
fore discharge.
Oil removal from wastewater is regarded to be a main challenge in
treatment practices. Dispersed oil droplets usually have high surface
charges, resulting in the stability of oil-in-water system. This is especial-
ly true when emulsified oil exists. Emulsion generation and stabilization
are usually achieved by mechanical agitation and addition of emulsify-
ing agents. Although qualitative and quantitative compositions of oily
wastes are different in many effluent sources, significant part of oil is al-
ways present in the emulsified form (Bratskaya et al., 2006). Some avail-
able technologies such as gravity separation, cyclone separation,
chemical precipitation, sorption, membrane filtration and chemical ox-
idation have been used for oil removal (Adebajo et al., 2003; Andreozzi
et al., 2000; Ezzati et al., 2005; Husveg et al., 2007; Wilkinson et al.,
2000). Although many advantages of these technologies have been re-
ported, some specific disadvantages associated with these approaches
(i.e. low efficiency, long processing time, secondary pollution and high

Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
costs) exist in treatment applications. The efficiencies of many methods
for treatment of oily wastewater remain unsatisfactory. There is also an
increasing demand for clean water particularly in water-stressed areas
due to the rapid growth in population and economy (Rahmani and
Zarghami, 2015; Xiao et al., 2015). The development of advanced and
cost-effective treatment approaches is desired for better cleanup of
oil-containing wastewater and recovery of water resources.
An alternative to available oil removal technologies is
electrocoagulation. In this process, the electrodissolution of sacrificial
anodes, usually made of aluminum or iron, to the wastewater leads to
the formation of hydrolysis products (hydroxo-metal species) that are
effective in the destabilization of pollutants (Arsand et al., 2013;
Nguyen et al., 2016; Wang et al., 2016). The electrochemical reduction
of water in the cathode produces hydrogen bubbles that can promote
a soft turbulence in the system and bond with the pollutants, decreasing
their relative specific weight (Canizares et al., 2009; Tchamango et al.,
2010). In addition, the generated hydrogen can be collected and used
as fuel to produce energy (Ali and Yaakob, 2012). This treatment has
been successfully introduced in removing suspended solids (Den and
Huang, 2005; Solak et al., 2009), dyes (Cañizares et al., 2006), heavy
metals (Bhatti et al., 2009; Heidmann and Calmano, 2008), arsenic
(Wan et al., 2011), hardness (Malakootian et al., 2010), phosphate
(İrdemez et al., 2006), fluoride (Emamjomeh and Sivakumar, 2009),
pesticides (Behloul et al., 2012) and natural organic matter
(Vepsäläinen et al., 2009) from wastewater. Recently, there is an emerg-
ing trend in using electrocoagulation for the removal of oil from waste-
water. For the use of electrocoagulation, there are some advantages
such as requiring only simple equipment, ease of operation, less treat-
ment time, use of less or no chemicals, and smaller amount of sludge
(Un et al., 2009). Removal of oil from wastewater through
electrocoagulation is a complicated process involving various chemical
and physical phenomena, which are controlled by the lumped action
of electrochemical, physicochemical and hydrodynamic parameters
(Bensadok et al., 2011). As a promising treatment technology and
cost-effective solution for sustainable water management, it will be-
come increasingly important to provide a deeper insight into such
electrocoagulation treatment used in oil removal. The purpose of this ar-
ticle is therefore to present a full-scale review on the most recent efforts
in this emerging field. In detail, this review will focus on oily wastewater
origin and characteristics, available treatment technologies for oil re-
moval, fundamental mechanisms involved in the electrocoagulation
process, current applications of electrocoagulation for oil removal
from wastewater, optimization and modeling of electrocoagulation pro-
cess, advancements in electrocoagulation technology for oil removal,
combined methods to improve treatment performance and future de-
velopment needs.
2. Theoretical background of electrocoagulation treatment strategy
2.1. Characteristics of oily wastewater
Oily wastewater is generated from different sources such as oilfield
(Bande et al., 2008; Ben-Awuah et al., 2015; Fakhru'l-Razi et al., 2009),
petroleum refinery (El-Naas et al., 2009; El-Naas et al., 2014; Hladik et
al., 2014; Saeedi and Khalvati-Fahlyani, 2011), metal processing and
finishing (Aoudjehane et al., 2010; Bensadok et al., 2008; Kobya et al.,
2011), ship and vehicle cleaning (Ali et al., 2012; GilPavas et al., 2009),
food processing (Barrera-Díaz et al., 2006; Valta et al., 2014), slaughter-
house (Kazem et al., 2012; Kobya et al., 2006b), tannery (Maha Lakshmi
and Sivashanmugam, 2013; Şengil et al., 2009), and restaurant (Chen et
al., 2000a; Qin et al., 2013). Many countries have implemented stringent
standards for discharging oily wastewater due to environmental con-
cerns. For example, the permitted discharge limit of dispersed oil and
grease for treated produced water in Canada is 30 mg/L in daily average
(Veil et al., 2004). Based on the US EPA regulation, the daily maximum
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
3
and monthly average limit for oil and grease are 42 and 29 mg/L, respec-
tively (Fakhru'l-Razi et al., 2009).
The characteristics of oily wastewater depend on the nature of rele-
vant production, operation, and chemicals used in processing facilities.
The compositions of oily wastewater from different sources can vary
by order of magnitude. Constituents typically associated with oily
wastewater include: (i) Dispersed oil. Dispersed oil consists of small
droplets suspended in the aqueous phase. They may also reach the bot-
tom or rise to the surface of water body. (ii) Dissolved or soluble organic
components, such as organic acids, PAHs, phenols, and volatiles. These
hydrocarbons can often lead to additional toxicity of oily wastewater.
(iii) Processing chemicals, such as biocides, reverse emulsion breakers,
and corrosion inhibitors. Some of these chemicals are lethal at levels
as low as 0.1 mg/L (Glickman, 1998). Corrosion inhibitors can make
oil-water separation less efficient due to the formation of more stable
emulsions. (iv) Solids, such as precipitated solids, sand and silt, clays,
corrosion products, and other suspended solids derived from produc-
tion and operation. The fine-grained solids can reduce the efficiency of
oil-water separators, leading to the exceedance of oil and grease limit
in discharged wastewater (Cline, 1998). (v) Bacteria. Bacteria can clog
equipment and pipelines. They can also form difficult-to-break emul-
sions and hydrogen sulfides which are corrosive. (vi) Dissolved forma-
tion minerals, such as heavy metals, naturally occurring radioactive
materials, etc. Besides toxicity, these may cause production problems.
(vii) Salinity. Environmental impacts of salts in oily wastewater exist
in all regions where oil and gas are produced.
2.2. Available technologies for oil removal
Oil-containing wastewater can be treated through different physical,
chemical, and biological methods. Available individual treatment tech-
nologies that have been reported mainly include gravity separation,
hydrocyclone, sorption, chemical precipitation, flotation, membrane fil-
tration, chemical oxidation and biodegradation. Different treatment ap-
proaches are characterized by different application requirements and
treatment patterns. The advantages and disadvantages of these oily
water treatment technologies are summarized in Table 1.
2.2.1. Gravity separation
There are various oil-water separators, which are mainly dependent
on two types of design, gravity separation and coalescence separation.
Oil and water are not soluble in each other and gravity separation uti-
lizes the difference in specific gravity between oil and water. Traditional
gravity oil-water separation usually relies on the large water volume
and tank size. In order to achieve the high separation efficiency, oil-
water separation is expected to be facilitated by making the oil droplets
larger or making the flow slower. Based on different design configura-
tions, some improved gravity separators such as plate separator, tube
separator and lamella-type settler have been further developed
(Zeevalkink and Brunsmann, 1983). The principle used in these separa-
tors is classified into coalescence separation, which refers to the process
where small oil droplets contact with each other and then combine into
larger drops. Aspects of oil removal by gravity separator have been in-
vestigated both theoretically and experimentally (Deng et al., 2002;
Wilkinson et al., 2000; Zhang et al., 2007).
2.2.2. Hydrocyclones
Hydrocyclones have been widely used in various industries to sepa-
rate two components with different densities (Slack et al., 2000).
Hydrocyclones can separate target substance in a liquid suspension
based on centrifugal force. In the application for oil-water separation,
its tangential inlet creates a swirling motion and the vortex accelerates
as it moves down the cone. The heavier water phase tends to move out-
side of the vortex while the lighter oil phase moves to the centre. The
separated oil gets into an orifice located in the inlet end and the treated
water is discharged through the opposite end. The performance of
4 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx

Table 1 2006; Rajaković-Ognjanović et al., 2008; Wang et al., 2010). Recently,

Comparison of different methods for removal of oil from aqueous solution. attentions have also been paid to the use of natural organic sorbents
Methods Advantages Disadvantages such as corn cob, wood chip, sugarcane bagasse, rice husk, coconut
Gravity Simple design, low energy Large space requirement, slow
husk, saw dust, walnut shell media, kenaf, wool fiber, kapok fiber, cattail
separation consumption separation rate, ineffective for fiber, cotton fiber, milkweed floss and peat moss (Ali et al., 2012;
the removal of submicron-sized Rajaković-Ognjanović et al., 2008; Rajakovic et al., 2007; Srinivasan
oil droplets and Viraraghavan, 2010).
Hydrocyclones Large treatment capacity, small High energy requirement for
volume, simple operation and generating strong centrifugal
installation forces, low separation 2.2.4. Chemical precipitation
efficiency for fine oil droplets, Chemical precipitation has been used to destabilize the oil emulsion
high maintenance cost through aggregation, coalescence, and flocculation (Hempoonsert et al.,
Sorption Simple operation, good Low separation efficiency for 2010). The addition of electrolytes with opposite charge can lead to the
removal efficiency, low fine oil droplets, high costs for
reduction of net surface charge on oil droplet, resulting in the decrease
processing cost oil sorbents, less efficient at
high oil concentration of repulsive potential among oil droplets. The aggregation of oil droplets
Chemical Good oil removal efficiency Complex operation, high occur through attraction by van der Waals forces. Some other mecha-
precipitation operating cost for chemicals, nisms such as layer compression, inter-particle bridging and sweep co-
generation of secondary
agulation also contribute to the aggregation process. Oil droplets on
pollutants
Flotation High overflow rates, easy Generation of large amount of flocs are subsequently removed by sedimentation or flotation. Many co-
operation, robust and durable scums and sludge, long agulants are widely used in the oily wastewater treatment. These coag-
retention time for separation ulants are either inorganic (e.g., aluminum sulfate, poly-aluminum
Membrane Good oil removal efficiency, Requirement for pre-treatment, chloride, poly-zinc silicate) or synthetic organic polymers (e.g., poly-ac-
filtration absence of chemical addition decrease of membrane
rylamide derivatives) (Zeng et al., 2007; Zhao et al., 2014b). The selec-
and subsequent generation of performance caused by
oily sludge membrane fouling tion of coagulants depends on the chemical characteristics of oily
Chemical Good oil removal efficiency, High cost for oxidizer, wastewater. The use of corrosive coagulants may result in a large
oxidation rapid destruction, easy undesired by-product, safety amount of hazardous sludge. As an alternative, some natural coagulants
operation concerns associated with
have been also used for oily wastewater treatment due to their safe and
applying oxidants
Biodegradation Low operating cost, clean Long retention time, wide
environment-friendly features (Meyssami and Kasaeian, 2005).
technology space, sensitive to temperature
and pH variations, requirement 2.2.5. Flotation
for skilled operator Flotation is effective for the removal of emulsified-oil droplets
(Zouboulis and Avranas, 2000). During the flotation process, finely
suspended oil droplets can be separated by adhering to the surface of
hydrocyclones depends on appropriate design. The optimal operation rising air bubbles. When adhered to small air bubbles, the buoyancy dif-
parameters such as flow rate and flow split are also necessary for ference between oil and water is enhanced. The removal efficiency de-
obtaining adequate separation (Husveg et al., 2007). In order to enhance pends on both characteristics of oil droplet and air bubble. Increasing
the oil-water separation efficiency, some efforts have been made to im- droplet size and decreasing bubble size usually help achieve a higher
prove certain performance indices by introducing special structural oil removal efficiency (Medrzycka, 1993). Dissolved air flotation (DAF)
modifications or implementing optimal operations (Bai et al., 2011; is an effective technique to obtain fine air bubbles in flotation. Air is
Chu et al., 2000; Oropeza-Vazquez et al., 2003). Different mathematical injected into water under pressure to produce air-in-water solution,
models are theoretically developed for evaluation and improvement of which will be mixed with incoming wastewater. The dissolved air
the hydrocyclone performance (Amini et al., 2012). They have also comes out of solution in the form of micron-sized bubbles that attach
been used to predict fluid behaviour, velocity profile, flow split and effi- to the contaminants. Zouboulis and Avranas (2000) reported that DAF
ciency curve in hydrocyclones. The required input for these models usu- was successfully applied in the destabilization of oil-in-water emulsion.
ally include hydrocyclone geometry, fluid properties, inlet droplet size However, DAF requires a high-pressure condition to create a sufficient
distribution and operational conditions at the down hole (Amini et al., amount of dissolved-air water for the introduction of fine bubbles.
2012). High cost may be necessary to maintain the high-pressure equipment
for large-scale treatment system (Suzuki and Maruyama, 2005).
2.2.3. Sorption
The use of sorbents can induce separation of contaminants and 2.2.6. Membrane filtration
water (An et al., 2010c; Li et al., 2012; Wang et al., 2014; Zhao et al., The membrane with certain pore size can permit the passage of
2016). The sorbent used in oil-water separation is usually characterized water molecules and retain a wide range of particulates and
by high oleophilic and hydrophobic properties, which facilitate the re- dissolved compounds (Fu et al., 2015; Han et al., 2015). Membrane
tention of oil on sorbent surface (Deschamps et al., 2003). Other proper- filtration has gradually become a powerful technology for oil-water
ties of an ideal sorbent for oil-water separation include high uptake separation. The applications of microfiltration (MF), ultrafiltration
capacity and rate, buoyancy, retention over time, durability in aqueous (UF), nanofiltration (NF) and reverse osmosis (RO) were reported
media, reusability or biodegradability, and recoverability of oil (Ceylan in the separation of oil from water (Chakrabarty et al., 2010; Ezzati
et al., 2009). A wide range of materials have been applied in oil-water et al., 2005; Kasemset et al., 2013; Mondal and Wickramasinghe,
separation. Based on different criteria, they can be generally classified 2008; Yi et al., 2011). The filtration processes using these
into either organic and inorganic, natural and synthetic materials, or membranes are conceptually similar in mechanism, while the main
their combinations. Synthetic organic materials are usually the most difference is the pore size of membrane. A suitable membrane is usu-
commonly used commercial sorbents (Adebajo et al., 2003; Wei et al., ally featured by high permeability, good hydrophilicity and chemical
2003). These products include polypropylene, polyurethane, polyacry- resistance to the feed streams (Ahmad et al., 2011). Membranes for
lonitrile, butyl rubber, etc. (Ceylan et al., 2009; Ji et al., 2009; oil-water separation are made from several types of polymers such
Rengasamy et al., 2011). Natural inorganic sorbents mainly include min- as polysulfone (PSF), polyethersulfone (PES), polyacrylonitrile
eral products such as zeolites, silica, sepiolite, bentonite, perlite, exfoli- (PAN), polyamides (PA), and polyvinylidene difluoride (PVDF)
ated graphite, vermiculites, charcoal and diatomite (Bastani et al., (Chakrabarty et al., 2008; Padaki et al., 2015). There is also an

Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
increasing interest in exploring alternative membrane materials
with better performance. The composite membranes including
blended polymers and surface modification techniques are devel-
oped for oil and water separation (Asatekin and Mayes, 2009; Ju et
al., 2008; Sadeghi et al., 2013).
2.2.7. Chemical oxidation
Degradation of organic compounds present in water through
chemical oxidation has shown high efficiency even when they are
present at low concentrations (Wang et al., 2011b; Wang et al.,
2012). This approach offers some advantages such as no sludge for-
mation, near-complete conversion of pollutants to relatively harm-
less end products, and simultaneous removal of different organic
pollutants. Photocatalytic reactions have been used in the removal
of oil from water. Some semiconductor powders such as TiO2 were
used to treat oil-contained water with UV radiation (Emam and
Aboul-Gheit, 2014; Grzechulska et al., 2000). Recently, some re-
searchers investigated the application of advanced oxidation pro-
cesses as appropriate solutions for the treatment of oily effluents.
The generation of highly reactive intermediates (OH radicals) can
oxidize oil components. Vergara-Sanchez and Silva-Martinez
(2010) reported the degradation of used cooking oil solutions by
Fenton oxidation. Moreover, ozone oxidation has also been used in
the removal of oil from aqueous phase (Andreozzi et al., 2000;
Chang et al., 2001).
2.2.8. Biodegradation
Attention has also been paid to the application of biotechnology for
removing complex organic compounds from water (An et al., 2010a;
An et al., 2010b; An et al., 2012; Salam et al., 2016; Yu et al., 2011). Dur-
ing the biodegradation process, sufficient nutrients or other growth-
limiting co-substrates can be provided to improve the growth of indig-
enous oil degraders. If efficient microorganisms are not present natural-
ly in the system, extraneous microorganisms can be added as
supplements. Bacteria and fungi are the two major microbial groups
used in biological treatment of oily water. Pimda and Bunnag (2015) ex-
amined the biodegradation of waste motor oil by the strain TISTR 8405.
The results showed the strain TISTR 8405 grew well with waste motor
oil and satisfactory biodegradability was obtained. Wang et al. (2011a,
2011b) used the enriched bacteria from local produced water pond to
remove oil. The oil concentration in produced water was reduced from
689 to 3.51 mg/L through combined biodegradation and microfiltration.
Behnood et al. (2014) also reported the biodegradation of crude oil in
saline wastewater using white rot fungus Phanerochaete chrysosporium.
Biological treatment of oily water is generally regarded as a cost effec-
tive, versatile and environmentally friendly method. Since microorgan-
isms are sensitive to environmental changes, however, proper
maintenance and monitoring for treatment processes are necessary
for ensuring the system performance.
2.3. Basics of electrocoagulation
2.3.1. Principles of electrocoagulation
The basic principle of electrocoagulation was originated from “elec-
trolysis”. Michael Faraday first formulated the principle of electrolysis
(Chen et al., 2005). It occurs as direct electric current passing through
electrolyte, producing chemical reactions at electrodes. The electro-
chemical process in aqueous systems has been explained by Lin et al.
(1998). It is generally acknowledged that there are three major process-
es: electrocoagulation, electroflotation, and electrooxidation. The
electrocoagulation and electroflotation processes are particularly useful
for the treatment of oily wastewater.
During electrocoagulation, the most important chemical reactions
involve the dissolution of metal cations at the anode and formation of
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
5
hydroxyl ions and hydrogen gas at the cathode (Fig. 1):
M→M nþ þ ne−
2H 2 O ðlÞ þ 2e− →2OH − þ H 2 ðg Þ
The current passes through a metal electrode, oxidizing the metal
(M) to its cation (Mn+). Simultaneously, water is reduced to hydrogen
gas and the hydroxyl ion (OH−). Electrocoagulation thus introduces
metal cations in situ, using sacrificial anodes (typically iron or alumi-
num) that need to be periodically replaced (Carmona et al., 2006). The
cations (Al3+, Fe2+, etc.) destabilize colloidal particles by neutralizing
charges. They also produce monomeric and polymeric hydroxide com-
plex species as coagulants.
Mnþ ðaqÞ þ nOH − ðaqÞ→MðOH Þn ðsÞ
These coagulants form amorphous metal hydroxide precipitates
(Cañizares et al., 2006). Their high adsorption properties impart
strong affinity for dispersed particles and dissolved pollutants.
Thus the pollutants can be separated from aqueous phase by
coagulation. The hydrogen bubbles at cathode promote turbulence
in the system and bond with the pollutants, decreasing their relative
specific weight. Consequently, they enhance the separation process
by flotation.
2.3.2. Destabilization and separation of oil-in-water emulsion by
electrocoagulation
Electrocoagulation treatment is particularly effective for
destabilization of oil-in-water emulsions. Oil droplets in oil-in-
water emulsion exhibit net charge at the droplet surface. It is usually
a negative charge, and as described by the Helmholtz theory of the
electrical double layer, the negative charges are aligned or closely
bound to the interface. These charges attract counter ions from the
bulk solution which give rise to a zone of opposite sign, forming an
electrical double layer (Volkov et al., 1996). Moving away from the
oil surface into the water phase, the electrostatic potential drops,
as shown in Fig. 2. The potential produced by the double layer creates
a repulsive effect between the oil droplets and thus preventing
aggregation/coalescence of individual droplets. This repulsive
electrical potential can be indirectly represented by the zeta
potential (Liberman et al., 1989). The zeta potential is defined as
the difference in potential between the surface of the tightly bound
layer of ions on the particle surface and the electroneutral region of
the solution. It is a key indicator of the emulsion stability. Higher
zeta potential indicates higher stability. During electrocoagulation
process, the breaking of emulsions can be summarized as follows:
(i) compression of the diffuse double layer around the charged
species by ions generated from the sacrificial anode; (ii) charge neu-
tralization of the ionic species present in wastewater by counter ions
produced by the electrochemical dissolution of the sacrificial anode.
These counter ions reduce the electrostatic interparticle repulsion;
(iii) floc formation as the result of coagulation creates a sludge blan-
ket that entraps and bridges colloidal particles (Mollah et al., 2004).
Meanwhile, as fine hydrogen bubbles are introduced into wastewa-
ter, their adhesion to oil droplets or even to light solids in suspension
makes them more buoyant. Oil or solids can then rise more quickly to
the surface of the tank where it is skimmed off as aerated foam. The in-
teraction mechanism between air bubbles and oil droplets is shown in
Fig. 3 and follows these steps (Bennett and Peters, 1988; Vrablik,
1959): (i) collision and attachment of fine air bubbles to the surface of
oil droplets; (ii) collision between gas-attached droplets with the for-
mation of agglomerates; (iii) entrapment of more gas bubbles in the
flocculated structure of oil droplets as they rise; (iv) upward rise of
floc structures in a sweeping action called sweep flocculation.
6 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
Fig. 1. Mechanisms of electrocoagulation process.
The electrocoagulation has to be followed by a sludge removal pro-
cess. This process is often completed in the electrocoagulation cell in
batch operation, or in a subsequence sedimentation/flotation unit in
continuous operation. The sludge deposited at the bottom can be direct-
ly transferred. Flocs at the surface can be collected by scrubbing devices,
which shift flocs from the surface into a collecting pocket with a conic
bottom. The sludge and flocs are then transferred to a filter press for
de-watering via a branch pipe (Chen, 2004). It is generally acknowl-
edged that the electrocoagulation may produce less sludge than chem-
ical coagulation as less aluminum dosage is needed to get the same
removal efficiency. The sludge formed in electrocoagulation tends to
Fig. 2. Electrical double layer and electrical potential around negatively charged oil
droplet.
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
be readily settable and easy to de-water, because it is mainly composed
of metallic oxides/hydroxides (Ghernaout and Ghernaout, 2011).
3. Electrocoagulation applications for oil removal
3.1. Oil removal from oilfield wastewater
The oilfield wastewater is often characterized by complex compo-
nents, poor biodegradability and high salt level. Its direct discharge
may cause serious contamination. Electrocoagulation was proposed as
an effective technique for the treatment of oilfield wastewater.
Ighilahriz et al. (2014) studied electrocoagulation and electrooxidation
for the treatment of leachate and oil drilling muds. Electrocoagulation
was effective in removing fine colloids. Bande et al. (2008) studied the
separation of finely dispersed oil from oil-water emulsion in an
electrocoagulation cell with a set of perforated aluminum electrodes.
It was observed that the decrease in salinity and increase in oil content
of the effluent improved the oil removal efficiency. Panikulam et al.
(2015) employed electrocoagulation to treat effluent from oil-sand tail-
ings. The results showed that the electrocoagulation-assisted process
was characterized by not only enhanced pollutant removal rate but
also decreased energy consumption simultaneously. Younker et al.
(2011) investigated the chemical coagulation and electrocoagulation
for the treatment of synthetic oily wastewater. The highest COD remov-
al rates were 62 and 56% for chemical coagulation and
electrocoagulation, respectively. Electrocoagulation is also one of the
available technologies to treat oilfield wastewater for reuse, eliminating
not only the need to transport more water but also the costs of provid-
ing fresh water (Esmaeilirad et al., 2015).
3.2. Oil removal from petroleum refinery wastewater
Electrocoagulation has been used in the removal of oil from petro-
leum refinery wastewater. Dimoglo et al. (2004) studied the removal
of COD, turbidity, hydrocarbon and grease from petrochemical waste-
water using electrocoagulation. The effects of residence time, current
density, and electrode materials were evaluated. Martínez-Delgadillo
et al. (2010) reported the iron electrodes had better performance than
the aluminum ones in the treatment of petroleum refinery wastewater
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
Fig. 3. Interaction mechanism between gas bubbles and oil droplets during floatation.
through electrocoagulation. The COD removal was slower than the re-
moval of oil and sulfides. Yavuz et al. (2010) studied the direct and indi-
rect electrochemical oxidation using boron doped diamond anode,
direct electrochemical oxidation using ruthenium mixed metal oxide
electrode, and electrofenton-electrocoagulation using iron electrode
for the treatment of petroleum refinery wastewater. It was observed
that reaction time needed to be prolonged for achieving complete
COD removal through electrocoagulation. El-Naas et al. (2009) demon-
strated the technical feasibility of electrocoagulation as a possible and
reliable technique for the pre-treatment of heavily contaminated petro-
leum refinery wastewater. Although electrocoagulation was found to be
most effective at 25 °C and pH 8, the influence of these two parameters
on the removal rate was not significant. A novel three-step process con-
taining an electrocoagulation unit was further developed and evaluated
for the treatment of highly polluted refinery wastewater (El-Naas et al.,
2014). Saeedi and Khalvati-Fahlyani (2011) studied the treatment of
gas refinery oily wastewater using electrocoagulation with aluminum
electrodes. The effects of operating factors such as electrode distance,
initial pH, polyaluminum chloride (PAC) dosage as coagulant aid, sodi-
um sulfate as supporting electrolyte, and current density on the efficien-
cy of COD removal were studied. It was observed that nearly 99% of
normal hydrocarbons were removed in this process.
3.3. Oil removal from metal processing and finishing wastewater
The oily wastewater from metal processing and finishing is
usually produced by the consumption of cutting and washing fluids.
These fluids are widely used in metal industries, such as rolling mills,
forge and metal workshops, because of their cooling and lubrication
capabilities. The wastewater is characterized by containing stable
emulsions produced by mineral oils and surfactants, toxic additives
and metal particles (Soković and Mijanović, 2001). Due to the
effectiveness of electrocoagulation in demulsification, it has been
considered as a competitive alternative in the treatment of metal
processing wastewater. Studies have been focused on the operating
conditions such as pH, current density, electrode types, and reaction
time. In electrocoagulation of soluble cutting oil wastewater (Sangal
et al., 2013), it was reported a simple first order kinetics fit the
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
7
experimental data at a constant value of current density. It was re-
ported that with the optimum of initial pH around 7 and current den-
sity above 100 A/m 2, the removal efficiency of COD and turbidity
could reach above 90 and 99%, respectively (Bensadok et al., 2008;
Kobya et al., 2008). However, as the result of the high initial COD,
the COD of effluent from electrocoagulation usually fall for short of
discharge standards (Kobya et al., 2008). Therefore,
electrocoagulation process would be appropriate as a pre-treatment
step prior to other secondary process.
3.4. Oil removal from ship and vehicle cleaning wastewater
The ship and vehicle cleaning wastewater also features in free oil, oil
emulsified by surfactants, and heavy metals. The vehicle washing
wastewater ends up in municipal treatment plants, and the regulations
for reusing is becoming stringent. Panizza and Cerisola (2010) devel-
oped a combined two-step process consisting in electrocoagulation
with iron anodes and electrooxidation with boron-doped diamond
anodes for the treatment of car washing wastewater. A combined
electrocoagulation-ultrasound technique, was studied to treat the car
washing wastewater for reuse (Chu et al., 2012). The port and shipyard
wastewater, mostly the bilge water, goes to port waste reception plant
and then discharged to the ocean and river at a lower quality standard
(Sekman et al., 2011). The electrocoagulation treatment of oily bilge
water using two kinds of electrodes (iron and aluminum) arranged ei-
ther in bipolar or monopolar configuration was evaluated. The best per-
formance for oil removal was obtained using mild steel monopolar
electrode system operated at a current of 1.5 A (Asselin et al., 2008b).
Körbahti and Artut (2010) investigated the treatment of bilge water
using a batch electrocoagulation reactor with Platinum/Iridium
electrodes and high kinetics constant for COD removal was observed.
Another electrocoagulation treatment for bilge water, with a focus on
oily emulsions and heavy metals (copper, nickel and zinc), resulted in
satisfactory removal of oil, grease and zinc, but 70% removal rate for
copper and nickel (Rincón and La Motta, 2014). It also demonstrated
that oil removal by electrocoagulation followed a first-order reaction
(Rincón et al., 2013; Rincón and La Motta, 2014).
8 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
3.5. Oil removal from food processing wastewater
Water is used extensively in the food industry in preparing raw ma-
terials, generating vapor, cleaning packing materials, and washing
equipment and floors (Barrera-Díaz et al., 2006). Huge amount of oily
wastewater is generated every day in these processes. The manufac-
turers of oil-containing foods and dairy are seeking effective technolo-
gies to remove oil, fat, and grease from food processing wastewater at
acceptable cost. Phalakornkule et al. (2010) reported the treatment of
palm oil mill effluent using electrocoagulation. The oil removal efficien-
cy of 72% could be achieved at the optimal condition with a current den-
sity of 20 A/m2 for 5 min at 40 °C and pH 5. A combination of low current
density and low reaction time was preferable. The addition of NaNO3
could also improve the electrocoagulation efficiency. Nasution et al.
(2013) studied the effectiveness of electrocoagulation with aluminum
and iron as electrodes to treat palm oil mill effluent with oil and grease
concentration of 4000–6000 mg/L. The results showed that aluminum
electrodes exhibited a higher efficiency compared to iron electrodes.
COD in effluent pretreated by anaerobic pond dropped 62.35 and
59.41% using Al and Fe electrodes, respectively. The treatment cost can
be compensated to some extent by producing hydrogen gas. Bensadok
et al. (2011) reported the application of electrocoagulation for the treat-
ment of dairy wastewater. There was a high efficiency for the use of
both cathode and anode made of aluminum. The highest removal effi-
ciency was obtained when current density, reaction time, initial pH
and NaCl concentration, were 50 A/m2, 2 min, 6.6 and 1.5 g/L, respec-
tively. The efficiency for COD removal could reach 80% under optimal
conditions. Şengil (2006) studied the treatment of dairy wastewater
by electrocoagulation using mild steel electrodes. The results showed
that oil and grease were effectively removed at initial pH 6–7 when
the initial oil and grease concentration was 4570 mg/L. The removal ef-
ficiency of oil and grease was raised to 99%. The optimal current density
was 0.6 mA/cm2 for the operating time of 1 min.
The large amount of biodiesel wastewater containing residual oil
generated by the washing process creates a significant problem for the
industry and environment (Daud et al., 2015). Chavalparit and
Ongwandee (2009) investigated the efficiency of electrocoagulation
for treating the biodiesel wastewater containing 6020 mg/L oil and
grease. Aluminum anode and graphite cathode were effective in reduc-
ing oil and grease by N95% in biodiesel processing wastewater. The op-
timal conditions were pH of 6.06, applied voltage of 18.2 V, and reaction
time of 23.5 min. Ahmadi et al. (2013) studied the removal of oil and
grease from biodiesel wastewater using electrocoagulation with iron
electrodes. The effective removal of oil and grease was observed at ini-
tial pH 7 when the initial concentration of oil and grease was
6413 mg/L. The final concentration of oil and grease was 1098 mg/L at
optimal current density of 10 mA/cm2 and operating time of 25 min.
3.6. Oil removal from slaughterhouse wastewater
The slaughterhouse wastewater often contains high organic matter,
fat and oil. The highly polluted nature of such wastewater means that
the appropriate treatment is required before discharging (Ozyonar
and Karagozoglu, 2013). Asselin et al. (2008a) studied the effectiveness
of electrocoagulation in removing organic compounds from slaughter-
house wastewater using monopolar and bipolar electrolytic cells. The
best treatment performance was obtained using mild steel bipolar elec-
trode system operated at a current of 0.3 A, through 60 or 90 min of
treatment. Under these conditions, 99% oil and grease could be re-
moved. Kobya et al. (2006b) studied the treatment of poultry slaughter-
house wastewater by electrocoagulation. Low initial pH such as 2–3,
and current density of 150 A/m2 was preferable for having a high COD
removal efficiency in 25 min. The maximal oil and grease removal effi-
ciency of 98% was achieved with iron electrodes. Bayar et al. (2014) in-
vestigated the treatment of poultry slaughterhouse wastewater by
electrocoagulation method with aluminum plate electrodes. The
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
current density of 1 mA/cm2 of and the temperature of 20 °C were
used. The electrocoagulation was effective for the removal of oil and
grease and the highest removal efficiency was obtained when the initial
pH was 2. Bayramoglu et al. (2006) assessed the treatment of poultry
slaughterhouse wastewater using electrocoagulation. The higher effi-
ciency of 98% for removing oil and grease was obtained using iron elec-
trode rather than aluminum electrode, irrespective of the initial pH. The
operating cost with iron electrode was between 0.3 and 0.4 $/m3, which
was nearly half that with aluminum electrode. Compared with alumi-
num electrode, iron electrode was more successful in removing oil
and grease with the removal efficiency of 98%, irrespective of the initial
pH. From economic point of view, iron electrode is preferable. The total
operating cost was between 0.3 and 0.4 $/m3, which was nearly half that
of aluminum electrode. Ozyonar and Karagozoglu (2013) reported the
treatment of slaughterhouse wastewater by electrocoagulation in
batch reactor using aluminum and iron electrodes. The removal efficien-
cy for oil and grease in slaughterhouse was 94.7% with aluminum elec-
trode under the optimal conditions of pH 4, 100 A/m2 and 20 min; the
removal efficiency was 92.8% with iron electrode under the optimal
conditions of pH 6, 100 A/m2, and 20 min. Drogui et al. (2008) investi-
gated electrocoagulation for the treatment of wastewater from poultry
slaughtering. Iron and aluminum electrodes were used in either
monopolar or bipolar configuration. The COD removal efficiency of
85–86% was observed in electrocoagulation treatment process. Bipolar
configuration using mild steel electrodes was the optimal process
configuration.
3.7. Oil removal from tannery wastewater
Tanning industry is a water-intensive industry that produces large
quantities of wastewater and solid wastes. Tanning involves a complex
combination of mechanical and chemical processes. Effluents from tan-
ning industry contain oils, tissues, emulsifying agents, dyes etc. Maha
Lakshmi and Sivashanmugam (2013) evaluated the efficiencies of
electrocoagulation treatment for tannery effluent. The oil and grease
in raw wastewater was 4340 mg/L. The operating conditions for the
maximal COD removal of 90% were obtained at NaCl concentration of
1 g/L, current density of 20 mA/cm2 and reaction time of 15 min.
Under optimal conditions, operating cost was found to be 6.28 $/m3.
Thirugnanasambandham and Sivakumar (2014) investigated the appli-
cation of electrocoagulation for removing oil and grease from tannery
industry wastewater using stainless steel electrodes. At optimal operat-
ing conditions (pH of 9, reaction time of 40 min, current density of
20 mA/cm2 and sodium chloride dose of 1016 mg/L), 95% oil removal ef-
ficiency can be achieved. The electric energy consumption in optimal
condition was found to be 6 KWh/m3. Şengil et al. (2009) studied the ef-
fects of initial pH, reaction time and current density on the
electrocoagulation of tannery liming drum wastewater. The optimal
current density for removal of oil and grease was 3.5 mA/cm2 at
10 min reaction time and pH 3. Mean energy consumption was
0.00015 kWh/m3. The overall oil and grease removal efficiencies
reached 96%. Kongjao et al. (2008) used one-step electrocoagulation
process to simultaneously remove chromium and various pollutants
from tannery wastewater. Low-cost commercial iron plates were
employed as anodes and cathode materials. The optimal condition for
treating tannery wastewater was current density of 22.4 A/m2, circulat-
ing flow rate of wastewater in the reactor of 3.67 L/min, initial pH of 7–9,
and 20 min reaction time. Approximately 99% of oil and grease could be
removed under such condition. Low energy consumption was
0.13 kWh/m3 wastewater, leading to the low operating cost of approx-
imately 0.34 $/m3 wastewater.
3.8. Oil removal from restaurant wastewater
Restaurants generate a large volume of wastewater containing very
high concentrations of oil and grease, which can aggregate and foul the
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
sewer system and generate unpleasant odor. Appropriate treatment is
needed to ensure that the pollutants are within permissible limits be-
fore releasing them to drain. It is desired the appropriate treatment fa-
cilities can be efficient and small in size. The applications of
electrocoagulation in treatment of restaurant wastewater have been re-
ported. Chen et al. (2000b) applied electrocoagulation in the treatment
of restaurant wastewater with high oil and grease contents ranging
from 120 to 1500 mg/L. The results showed aluminum electrodes
were preferred compared with iron ones. The influent pH, conductivity
and electrical current density did not significantly affect the removal ef-
ficiency, while charge loading was the most important operating vari-
able. The removal efficiency of oil and grease was over 94% for all the
wastewater types tested. Daghrir et al. (2012) used electrocoagulation
in the treatment of restaurant wastewater consisting of organic and in-
organic matter, oil, grease, and suspensions solids. Electrocoagulation
treatment was carried out by using aluminum electrodes. The COD
and turbidity reduction rates were about 90 and 99%, respectively.
Cost analysis results showed the total operating cost for the
electrocoagulation process was 1.92 $/m3. Ji et al. (2014) reported the
electrocoagulation treatment for the effluent from the oil separation
tank of a university cafeteria. The oil and grease concentration ranged
from 180 to 280 mg/L, and the pH was between 5 and 6. The removal ef-
ficiency of oil and grease was above 95% under the optimal conditions
with the inter-electrode distance of 3.6 cm, reaction time of 34 min,
and current density of 43 A/m2. Xu and Zhu (2004) examined the effects
of different operational conditions on the performance of
electrocoagulation-assisted treatment of refectory wastewater with
high oil and grease contents. The removal efficiency of oil exceeded
95%. The optimal current density was 10–14 A/m2 within 30 min and
the optimal electrode distance was 10 mm. Conductivity had little effect
on the treatment efficiency. The addition of extra salts could reduce the
power consumption significantly. Considering the above-mentioned
facts, electrocoagulation applications for oil removal from wastewater
are summarized in Table 2.
4. Optimization and modeling of electrocoagulation process
4.1. Influencing factors
4.1.1. Initial pH
Initial pH is an essential factor for the electrocoagulation process and
plays an important role in oil removal from wastewater. Tir and Moulai-
Mostefa (2008) reported the use of electrocoagulation process with sac-
rificial aluminum anodes for separating oil from oily wastewater. The
maximal removal of turbidity and COD was observed at pH 5 and
remained unchanged between pH 6 and 7. Electrocoagulation was
used to treat refectory wastewater with high oil and grease content
(Xu and Zhu, 2004). Although the maximal removal of COD, oil and
grease was obtained at pH around 7, the pH effect was not so significant
in the range 3–10. Chavalparit and Ongwandee (2009) studied the
treatment of biodiesel wastewater through electrocoagulation process.
The pollutant removal efficiencies increased as the initial pH decreased
to the acidic level. As pH increased to 9, the decline of the removal effi-
ciency was observed due to less formation of the reactive flocs of alumi-
num hydroxide. Treatment of wastewater from potato chips
manufacturing by electrocoagulation was investigated (Kobya et al.,
2006a). As the pH increased from 2 to 6, the COD removal reached
53%, and it then sharply decreased at pH higher than 6. The treatment
performance depended on the nature of the pollutants with the highest
pollutant removal found near pH of 7. The effect of initial pH on the
treatment of poultry slaughterhouse wastewater by electrocoagulation
was studied (Bayar et al., 2014). When achieved the maximal oil and
grease removal, the initial pH was 2, while the suitable pH range was
3–5 for turbidity removal. At this pH level, either COD or turbidity
showed a steep decrease. The treatment of the synthetic oil-in-water
emulsion and actual effluent of a door-manufacturing factory were
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
9
investigated through coagulation and electrocoagulation process
(Canizares et al., 2009). The pH showed an important influence on the
coagulant species formed during coagulation processes. It also had ef-
fects on the superficial charge of the aluminum hydroxide precipitates.
The pH range from 3 to 11 was studied to determine the effects of
initial pH on the removal of COD, turbidity and hardness from oilfield
wastewater (Zhao et al., 2014a). Different pH conditions accounted for
different kinds of flocs. The green Fe(OH)2(s) flocs were generated at
acidic pH, while the green Fe(OH)2(s) and yellow Fe(OH)3(s) colloids
were produced at neutral pH, and the red-brown Fe(OH)3(s) flocs was
introduced at alkaline pH. Electrocoagulation treatment was more effec-
tive at alkaline conditions due to the fact that Fe(OH)2(s) was less effi-
cient than Fe(OH)3(s) in sweep flocculation or enmeshment
(Ghernaout et al., 2008). It indicated that there would be a more signif-
icant pH increase when the initial pH was lower in the
electrocoagulation process. These phenomena were stated previously
(Kobya et al., 2003; Malakootian et al., 2010), but were different from
those reported by Cañizares et al. (2007), where the final pH was
lower than the initial pH due to a series of complicated reactions of elec-
trodes at alkaline pH. However, all these results revealed that the
electrocoagulation process exhibited the pH buffering capacity, espe-
cially in the alkaline environment.
4.1.2. Current density
Current density is reported as another important parameter that in-
fluences the treatment efficiency. Treatment of wastewater from potato
chip manufacturing by electrocoagulation was studied (Kobya et al.,
2006a). The current density varying from 25 to 300 A/m2 showed a
great effect on COD and turbidity removal when the charge loading in-
creased from 10 to 118 Faradays/m3. The removal efficiencies increased
rapidly from 38 to 62% for COD and from 56 to 98% for turbidity, respec-
tively. When the initial pH was 3, the increase in current density caused
a decrease of the COD removal efficiency for the treatment of poultry
slaughterhouse wastewater (Bayar et al., 2011). The highest removal ef-
ficiency obtained for the current density of 0.5, 1.0, 1.5 and 2.0 mA/cm2
were 85, 85, 81 and 71%, respectively. The treatment of olive mill waste-
water was investigated, and the removal efficiency increased consider-
ably with the increase of current density for a given time (Adhoum and
Monser, 2004). 80.6% COD and 96% color reductions occurred at cur-
rents (75 and 120 mA/cm2) generated after 30 min. To study the effect
of current density on the electrocoagulation-electrooxidation process,
different current intensities were applied (Daghrir et al., 2012). To
achieve the maximal COD-turbidity-TSS removal and minimum energy
cost, the optimal current was 0.4 A for the treatment of restaurant
wastewater. The treatment of tannery wastewater was investigated
and the removal percentage of all pollutants increased as a function of
current density (Kongjao et al., 2008). The optimal current density
was found to be at 22.4 A/m2 and reaction time was longer than
20 min for the maximal removal of all pollutants. Considering the sludge
production and energy consumption, the effects of current density on
the treatment of oil tanning effluent was studied (Maha Lakshmi and
Sivashanmugam, 2013). As the current density increased from 10 to
20 and further to 40 mA/cm2, the COD removal efficiency increased
from 87 to 90% and then dropped from 90 to 81%.
According to Faraday's laws of electrolysis, the coagulant generated
from the anode was proportional to the total electric charge passing
through, that is, the current density. As the current density increased,
a large amount of Fe(OH)3 coagulant was produced to destabilize the
colloidal particles, together forming more precipitates which would
easily settle down (Tir and Moulai-Mostefa, 2008). On the other hand,
higher amount of H2 would be generated from the cathode due to the
higher current. Bubble size decreased with the increasing current densi-
ty, reported by Chen (2004), resulting in the increasing bubble densities
and the intense upward flux. Smaller bubbles also provided larger sur-
face area for particle attachment, ensuring high separation efficiency
10 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx

Table 2
Summary of reported studies on electrocoagulation for oil removal from water.

Oily water source Oil Electrode Current Reaction time Removal Energy and cost References
concentration density (A/m2) (min) efficiency (%) analysis
(mg/L) (kWh/m3)

Biodiesel wastewater 6412 Iron 100 25 82 0.43 kWh/g oil and (Ahmadi et al., 2013)
grease
Slaughterhouse 720–950 Iron 13.63 60 99 0.00015 kWh/m3 (Asselin et al., 2008a)
wastewater
Oilfield wastewater 50–100 Aluminum 18.5 40 N90 0.17–2.25 (Bande et al., 2008)
Slaughterhouse 1500–1800 Iron 100–150 25 98 0.015 $/kg COD (Bayramoglu et al., 2006)
wastewater removed
Slaughterhouse 143.1 Aluminum 10 20 85 (COD) 2.14 kWh/m3 (Bayar et al., 2014)
wastewater
Metal processing 60,282–116,128 Aluminum 100–200 60 60–90 / (Bensadok et al., 2008)
wastewater (COD)
Dairy wastewater 7560 (COD) Aluminum 50 2 80 (COD) 0.03 kWh/kg of COD (Bensadok et al., 2011)
Biodiesel wastewater 6020 Aluminum, 124.8 23.54 97.77 5.57 kWh/m3 (Chavalparit and Ongwandee,
graphite 2009)
Restaurant 120–1500 Aluminum 30–80 15 N94 b1.5 kWh/m3 (Chen et al., 2000b)
wastewater
Restaurant 1300 Aluminum, 12.12 90 98 3.35 kWh/m3 (Daghrir et al., 2012)
wastewater graphite
3
Petrochemical 1.96 Iron and 150 10 80 2.2 kWh/m (Dimoglo et al., 2004)
wastewater aluminum
3
Slaughterhouse 853 Aluminum 50 90 86.3 (COD) 11.3 kWh/m (Drogui et al., 2008)
wastewater
Petroleum refinery 596 (COD) Aluminum 130 60 63 / (El-Naas et al., 2009)
wastewater
Petroleum refinery 3600–5300 Aluminum 30 10 mL/min 46 / (El-Naas et al., 2014)
wastewater (COD)
Produced water N2400 Aluminum and 1343 6.8 L/min 0– 60% / (Esmaeilirad et al., 2015)
iron
Leachate of oil-drilling 303 (COD) Aluminum 286 60 95 / (Ighilahriz et al., 2014)
mud
Restaurant 180–280 Aluminum and 43 34 99 / (Ji et al., 2014)
wastewater iron
3
Slaughterhouse 1500–1800 Iron 150 25 98 N0.3 kWh/m (Kobya et al., 2006b)
wastewater
3
Metal processing 17,312 (COD) Iron 60 25 92 0.497 $/m (Kobya et al., 2008)
wastewater
Tannery wastewater 638–780 Iron 22.4 20 99 0.13 kWh/m3 (Kongjao et al., 2008)
Bilge water 2000 Pt/Ir 128 240 93.2 33.25 kWh/kg COD (Körbahti and Artut, 2010)
removed
Oil tanning 4340 Iron 200 15 90 (COD) 1.279 kWh/m3 and (Maha Lakshmi and
wastewater 6.28 $/m3 Sivashanmugam, 2013)
Oil petroleum refinery 700 (COD) Aluminum and 90 39 85 0.74 kWh/m3 (Martínez-Delgadillo et al.,
wastewater iron 2010)
Palm oil mill 50,000 (COD) Aluminum 35.8 480 57.66 (COD) 0.3 kWh/kg COD (Nasution et al., 2013)
wastewater removed
Slaughterhouse 275–376 Aluminum 100 20 94.7 25.02 kWh/m3 (Ozyonar and Karagozoglu,
wastewater 2013)
3
Vehicle cleaning 572 (COD) Iron, 20 6 75 0.14 kWh/m (Panizza and Cerisola, 2010)
wastewater boron-doped
diamond
Palm oil mill 3000 Aluminum 20 5 72 0.1 kWh/m3 (Phalakornkule et al., 2010)
wastewater
Bilge water 5000 Iron and 6 1 L/min N99 / (Rincón and La Motta, 2014)
aluminum
Gas refinery 4000 (COD) Aluminum 400 90 97 11.057 kWh/kg COD (Saeedi and Khalvati-Fahlyani,
wastewater removed 2011)
Metal processing 9600 Aluminum 60–180 120 N97 / (Sangal et al., 2013)
wastewater
Bilge water 39–736 Aluminum 120 20 81 / (Sekman et al., 2011)
Dairy wastewater 4750 Iron 6 1 99 0.003 kWh/kg COD (Şengil, 2006)
Tannery liming drum 185 Iron 35 10 96 0.00015 kWh/m3 of (Şengil et al., 2009)
wastewater oil and grease
Tannery wastewater 1574 Iron 200 40 95 6 KWh/m3 (Thirugnanasambandham and
Sivakumar, 2014)
Bilge water 338 Aluminum 30–150 12 82.8 / (Ulucan et al., 2014)
Restaurant 100–250 Iron 10–14 30 N95 0.60–0.84 kWh/m3 (Xu and Zhu, 2004)
wastewater
Petroleum refinery 590 (COD) Iron 10 36.3 × 10−3 L/min 6.27
wastewater
31.949 kWh/g (Yavuz et al.,
2010)

Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
(Chen et al., 2002). Oil was taken away through such flotation process
with flocs which were lifted by the large amount of tiny bubbles.
4.1.3. Reaction time
Reaction time has important influence on the treatment efficiency in
the electrochemical process. The effect of retention time on the treat-
ment of potato chips manufacturing wastewater was studied (Kobya
et al., 2006a). An increase in time from 5 to 40 min caused an increase
in energy consumption from 4.8 to 44.1 kWh/m3 and an increase in
electrode consumption from 0.2 to 2.1 kg Al/m3. Electrocoagulation
was used to treat refectory wastewater with high oil and grease content
and the influence of reaction time was studied (Xu and Zhu, 2004). Over
99% of oil and 77% of CODCr were removed within 60 min, and the main
removal occurred in the first 20–30 min. The effect of reaction time on
COD removal per unit of electrode consumption was investigated
when treating dairy wastewater (Şengil, 2006). Maximum COD re-
moved per unit of electrode consumed was obtained at the reaction
time of 60 s for the current density of 0.6 mA/cm2. The treatment of res-
taurant wastewater through electrocoagulation-electrooxidation pro-
cess was studied (Daghrir et al., 2012). The residual COD was stable
between 20 and 40 min and then reduced after 60 min to reach the
highest removal of COD (81.4%) at 90 min. The effect of reaction time
was explored based on COD removal from oil tanning effluent (Maha
Lakshmi and Sivashanmugam, 2013). The COD removal percentage de-
creased significantly after 10 min. Because most of the aggregates
formed were electro-floated from 10 to 15 min, the reaction time was
optimized as 15 min. The COD removal rate as a function of reaction
time was studied in the electrocoagulation treatment of ship effluent
(Drogui et al., 2009). The amount of COD reduced more quickly in the
initial stage of the treatment process and then decreased slightly from
20 to 90 min.
As the amount of dissolved coagulants at the iron electrode in-
creased, there was an increase in the removal efficiency. It might be ex-
plained by a sufficient quantity of coagulant dissolving from the iron
electrode to effectively reduce the double layer of the suspended metal-
lic hydroxides and to destabilize them (Chou et al., 2009). The released
ferric ions and hydroxyl from electrodes formed more hydroxide flocs,
which would adsorb more pollutant particles as the time extended
(Drouiche et al., 2009). Although further increasing time resulted in
slight increase in removal efficiency, this would not be applied due to
the high energy and electrode consumption. Considering the treatment
cost and efficiency, the optimal reaction time was 20–30 min normally
in literatures (Kobya et al., 2006a; Malakootian et al., 2010; Xu and
Zhu, 2004).
4.1.4. Electrode configuration
Electrode assembly is the heart of the electrocoagulation process.
Therefore, configurations such as the electrode materials and electrode
distance are greatly concerned. Because aluminum and iron electrodes
are cheap, readily available and proven effective, they are the most
widely used electrode materials in electrocoagulation applications.
Both sacrificial aluminum and iron electrodes were used to treat olive
mill wastewater using electrocoagulation (Adhoum and Monser,
2004). Aluminum electrode was found to be more effective in reducing
COD from the wastewater compared with iron electrode. The treatment
of liming drum wastewater using mild steel and aluminum electrodes
was studied (Şengil et al., 2009). There was no significant performance
difference between the two electrode materials for the removal of oil
and grease under the same condition. However, the rate for COD and
sulfide removal using mild steel electrodes was higher than that using
aluminum electrodes. Aluminum and titanium electrodes were selected
for the treatment of milk liquid fractions (Bensadok et al., 2011). The
highest COD removal was obtained when the anode and cathode were
both made of aluminum. Monopolar and bipolar cell arrangements
were studied to determine the optimal configuration for removing
organics and oil from sawmill and ship effluents through
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
11
electrocoagulation process (Drogui et al., 2009). An aluminum-bipolar
electrolytic cell operated at current of 0.3 A with reaction time of
60 min was found to be the optimal condition. The effect of electrode
distance on the electrocoagulation process was studied (Xu and Zhu,
2004). At the same voltage, the COD and oil removal efficiency and
power consumption went down as the iron electrode distance in-
creased. The optimal electrode distance was 10 mm for the studied
equipment in consideration of the treatment cost and efficiency. The ef-
fect of electrode configuration on simultaneous removal of organic and
inorganic pollutants in tannery wastewater using electrocoagulation
technique was studied (Kongjao et al., 2008). The electrode configura-
tion with parallel monopolar connection was more effective than the
other configurations because it required low applied voltage for driving
the same amount of current in the system. Maha Lakshmi and
Sivashanmugam (2013) studied the effect of electrode materials and
their combinations on the treatment of oil tanning effluent. 90, 86, 89
and 86% COD removals were obtained for the electrode combinations
of Fe/Fe, Al/Al, Al/Fe, and Fe/Al, respectively. Iron electrodes were pre-
ferred considering the sludge production rate, clarity of the treated ef-
fluent and cost of electrode material. To a certain degree, this might be
attributed to better bubble production at Fe electrode than Al electrode.
Due to the rough Al surface, bigger bubbles could be generated, provid-
ing less flocculation and disintegrating the formed flocs.
4.1.5. Wastewater conductivity
The conductivity of supporting electrolyte have important effects on
the current density in the electrocoagulation process. Therefore it may
influence the treatment efficiency significantly. The effect of salt on
the break-up of oil-in-water emulsions was investigated (Cañizares et
al., 2007). The lower the concentration of salt, the higher the COD re-
moval. For the same electrical charge passed, better removal of COD
was obtained in chloride medium compared to sulfate medium. Xu
and Zhu (2004) reported the effect of water conductivity on the treat-
ment of refectory oily wastewater. The NaCl concentration had little ef-
fect on removal of COD when it changed from 0.1 to 1.4 g/L. However,
adding salt to the wastewater could reduce power requirement signifi-
cantly. The effect of increasing water conductivity on the wastewater
treatment was studied (Chen, 2004). It was recommended that there
should be 20% Cl− to ensure a normal operation of electrocoagulation
in water treatment process. The addition of NaCl would lead to the de-
crease in power consumption with the increase in conductivity.
Trompette and Vergnes (2009) reported the effect of sulfate anions
on the treatment of the unskimmed milk and cutting oil emulsion.
Electrocoagulation in the presence of sulfate should be avoided when
operating with aluminum electrodes since sulfate anions had negative
influence on electric consumption and electrocoagulation efficiency.
Sulfate caused indirectly pH increase which reduced the separation effi-
ciency. The effect of NaCl concentration between 0.5 and 2 g/L on the
treatment of dairy effluent was studied (Bensadok et al., 2011). With
the increasing solution conductivity, the removal efficiency of COD,
phosphates and turbidity increased respectively from 24, 40 and 18%,
to 80, 59 and 96% after 2 min electrolysis at 50 A/m2. Şengil (2006) re-
ported the effect of solution conductivity on the treatment of dairy
wastewater. When the concentration of NaCl in solution increased, the
solution conductivity and the current density increased. When the
NaCl concentration approached 0.3 g/L, the removal efficiency of COD,
oil and grease increased to up to 100%. The study was consistent with
Hanafi et al.'s research (Hanafi et al., 2010) regarding the effect of
ionic strength on the treatment of olive mill wastewater.
When treating oil tanning effluent, the increase in NaCl concentra-
tion from 0.5 to 1.0 g/L resulted in the increasing COD removal from
85 to 90%. This might be attributed to more available chloride ions
that acted as better oxidizing agent. As chloride ion (Cl−) scavenged ox-
ygen to form oxychloride ion (OCl−) at the electrode, it reduced passiv-
ation effect and improved the current efficiency (Sridhar et al., 2011).
However, further increasing NaCl concentration from 1 to 2 g/L
12 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
decreased COD removal from 90 to 82%. This might be explained by
more coagulant production associated with increased conductivity. In
addition, at higher NaCl concentration, improper dissolution of iron
took place, causing undesired interaction between coagulants and par-
ticles. It was concluded that when NaCl was used as the supporting elec-
trolyte, the effluent was treated through two processes: (1)
electrocoagulation with the formation of coagulants and (2) electro-
chemical degradation as a result of indirect oxidation by hypochlorite
(Maha Lakshmi and Sivashanmugam, 2013).
4.1.6. Initial oil concentration
The initial contaminant concentration is another key parameter in
electrochemical treatment and the appropriate selection of concentra-
tion range is important. When treating the refectory oily wastewater,
the effect of initial contaminant concentration on the treatment efficien-
cy was investigated (Xu and Zhu, 2004). The COD removal efficiency
fluctuated between 44 and 79% when the influent COD changed from
150 to 3500 mg/L within 30 min. Removal of oil and grease was kept
at a high efficiency (N90%) when the influent oil and grease changed
from 45 to 450 mg/L within 30 min. Şengil (2006) reported the
influence of initial COD concentration on the treatment of dairy
wastewater. The COD removal increased from 88 to 98% when the initial
concentration of COD increased from 1550 to 19,800 mg/L. This was due
to the existence of excessive colloids for the adsorption at high COD
concentrations.
The relation between the oil amount in emulsion and a given
concentration of aluminum electrode dissolved was investigated
(Cañizares et al., 2007). The higher the concentration of oil, the
lower the removal of COD. For a given dose of aluminum there was
a concentration limit of oil in the emulsion for treatment. The
amount of aluminum for emulsion breakup was proportional to the
concentration of oil emulsified. The influence of initial effluent COD
was studied for the treatment of oil tanning effluent (Maha
Lakshmi and Sivashanmugam, 2013). Although the COD removal
increased with the increasing initial COD concentration, a significant
reduction in COD removal from 90 to 70% was observed. As per
Faraday's law, a constant amount of Fe 2 + was released into the
solution with the increasing initial effluent concentration at constant
current density and reaction time. Consequently, the same amount
of ferrous hydroxyl ions could be produced in the solution which
was insufficient to adsorb contaminants.
The relationship between initial oil concentration and correspond-
ing removal efficiency, was also described by the reaction order of the
electrocoagulation reaction. The removal of HEM from artificial bilge
water through electrocoagulation was conducted using a commercial
bench-scale reactor (Rincón and La Motta, 2014; Rincón et al., 2013).
A series of experiments were performed with the initial HEM concentra-
tion of approximately 700 mg/L. It was found that electrocoagulation of
HEM followed first order kinetics and kinetic constant of 0.0447 s−1 was
obtained. A parametric and kinetic study on the treatment of soluble oil
wastewater through electrocoagulation was investigated (Sangal et al.,
2013). At lower oil concentration, nearly 90% COD was removed;
while at higher oil concentration, the reduction of COD was ineffective.
The first order kinetics well fit the experimental data of residual oil. A
batch electrocoagulation study was conducted using aluminum elec-
trodes to investigate the treatability of synthetic bilge water (Aswathy
et al., 2016). The COD reduction kinetics was evaluated using second
order equations which were related to the soluble COD concentration.
The results showed that the second order model best fit the decrease
in COD concentration with time.
4.1.7. Other influencing parameters
Other operating parameters such as wastewater temperature,
stirring speed, and flow rate have also been investigated in previous
studies to explore their effects on oil removal in the
electrocoagulation process. The effect of temperature was
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
investigated for treating oil-containing wastewater through
electrocoagulation (Pazenko et al., 1986). The power consumption
reached a maximum at slightly lower temperature of 35 °C. Higher
temperature lead to a higher conductivity hence a lower energy con-
sumption. Körbahti and Artut (2010) investigated the effect of reac-
tion temperature on the electrochemical treatment of bilge water. It
was found that mass transport increased with the reaction tempera-
ture, which enhanced COD removal consequently. The effect of stir-
ring speed on COD removal from poultry slaughterhouse
wastewater was studied (Bayar et al., 2011). When stirring speed in-
creased from 100 to 150 rpm, Al(OH)3 flocks were attached together,
which was favorable for precipitation. When stirring speed increased
from 150 to 250 rpm, the flocks were degraded and adsorbed pollut-
ants were desorbed. This lead to a decrease of COD removal efficien-
cy. Stirring could efficiently transfer the coagulant matter which was
formed from electrode dissolution. It may also contribute to the ho-
mogenization of system variables such as temperature and pH. How-
ever, high speed stirring would destroy flocks formed in the reactor
and form small flocks which were hard to remove. The coagulation
process in some electrocoagulation reactors is a continuous process.
The influence of circulating flow rate in electrocoagulation reactor on
the treatment efficiency was investigated (Kongjao et al., 2008). The
removal efficiency for all pollutants including oil and grease in-
creased as a function of flow rate from 0 to 3.67 L/min. High flow
rate was corresponding with high removal efficiency for all pollut-
ants. This is because high circulating flow rate promoted either tur-
bulent flow or collision occasion between active species and
pollutant molecules.
4.2. Optimization of electrocoagulation treatment process
Optimization of process parameters has gained wide application in
environmental engineering practice (Han et al., 2015; Huang et al.,
1996; Li et al., 2015; Tan et al., 2015; Zhao et al., 2015). The combined
effects of variables can be predicted and the desired optimization can
be achieved with the help of the experimental design tool. Response
surface method (RSM) is a collection of mathematical and statistical
techniques useful for the modeling and analysis of problems. A response
of interest is influenced by several variables and the objective is to opti-
mize the response (Montgomery et al., 1984). RSM is suitable for inves-
tigating and optimizing the pertinent parameters in treatment process.
Zhao et al. (2014a) used RSM in the optimization of electrocoagulation
processes for the pre-treatment of produced water prior to RO. The op-
timized operating conditions were pH of 7.36, current density of
5.90 mA/cm2, and reaction time of 30.94 min with corresponding max-
imal hardness removal at 85.81%, COD at 66.64%, and turbidity at
93.80%. Tir and Moulai-Mostefa (2008) employed RSM in the optimiza-
tion of electrocoagulation process for separating oil from oily wastewa-
ter emulsion. The results indicated that electrocoagulation was very
efficient and able to achieve 99% turbidity and 90% COD removal in
b22 min and at current density of 25 mA/cm2. Ulucan et al. (2014) in-
vestigated the treatment of bilge water using electrocoagulation pro-
cess. The optimal removal of oil and grease through RSM analysis
were obtained under 9.87 mA/cm2 of current density in approximately
13 min and at approximately 29 °C of inlet temperature (Fig. 4).
Chavalparit and Ongwandee (2009) used Box-Behnken design, an ex-
perimental design for RSM, to optimize the operating conditions in
electrocoagulation for the treatment of biodiesel wastewater containing
high-level COD and oil and grease. Electrocoagulation could effectively
reduce COD, oil and grease, and SS by 55.43, 98.42, and 96.59%, respec-
tively, under the optimal conditions. Tir and Moulai-Mostefa (2009)
employed Box-Behnken design to investigate the effects of different op-
erating conditions on the removal of oil by electrocoagulation with alu-
minum electrodes. The electrocoagulation process was optimized and
the effects and interactions of variables including current density, initial
pH and reaction time on the turbidity removal were evaluated. RSM was
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
Fig. 4. Optimization of current density, reaction time and temperature for oil and grease removal using electrocoagulation (Ulucan et al., 2014).
also found to be efficient to model the treatment process of restaurant
wastewater by the combined electrocoagulation-electroflotation tech-
nique (Qin et al., 2013).
4.3. Modeling of electrocoagulation treatment process
Modeling of environmental process has been widely used in previ-
ous studies (Ahmadi et al., 2015; An and Huang, 2012; An et al., 2011;
Rege et al., 2015; Urquhart et al., 2015). The design of electrocoagulation
process and integration with other treatment technologies require
quantitative understanding of the process. Some efforts have been
made to model the performance of the electrocoagulation under various
settings. Carmona et al. (2006) developed a model to predict the remov-
al of hydrocarbon fractions from wastewater using sacrificial Al anodes.
This model features in the simulation of the adsorption of organic mat-
ter on aluminum hydroxide particles. It was applied to the interpreta-
tion of experimental data obtained in a laboratory electrochemical cell
operated in a batchwise manner. Khemis et al. (2006) developed a
model for prediction of the waste abatement in term of COD by com-
plexation of the matter suspended by Al (III), and taking into account
the “latency” period observed experimentally. While the above models
were based on a batch reactor, some preliminary works on plug-flow re-
actors have also been carried out. A series of electrocoagulation experi-
ments were performed using the synthetic emulsion with hexane
extractable materials at concentration of approximately 700 mg/L. It
was confirmed that electrocoagulation of hexane extractable materials
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
13
(HEM) follows first-order kinetics by applying both the dispersion and
tanks-in-series (TIS) models, respectively. TIS model indicated that
each cell of the electrocoagulation behaved as an independent continu-
ous-stirred batch reactor (Rincón et al., 2013).
5. Technology advancement
5.1. Advancements in reactor design and electrode selection
Among all the efforts in developing electrocoagulation techniques
for oily wastewater treatment, many has been made for the advance-
ment of reactor design and electrode materials. Fouad et al. (2009) com-
pared the performances of horizontally and vertically oriented
electrodes in electrocoagulation for oil separation. The cell anode was
an array of separated horizontal cylinders made of aluminum (Fig. 5).
It was suggested horizontal cell design was more efficient than the tra-
ditional vertical parallel plate cell. The performance of rotating cylinder
electrochemical reactor for the demulsification of crude oil emulsions
was also investigated (El-Ashtoukhy and Fouad, 2014). The advantage
of this design was demonstrated by the decrease in anode passivation
tendency as a result of the improved rate of mass transfer between
the anode and solution. In addition, the good mixing conditions in
bulk solution arose from the turbulence generated at the rotating cylin-
der anode. It would speed up the process of electrocoagulation.
A high-porosity fixed-bed sacrificial anode was developed for oil
separation through electrocoagulation (Hassan et al., 2015). It offers
14 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx

Fig. 5. (left) Electrocoagulation cell with horizontally oriented electrodes (Fouad et al., 2009); (right) electrocoagulation cell with rotating cylinder anode (El-Ashtoukhy and Fouad, 2014).

many advantages over conventional vertical or horizontal anodes in-
cluding higher removal rate of emulsions, longer operation time be-
tween electrode replacements, and lower space footprint. An
aluminum wire gauze anode was also studied in the separation of
crude oil from oil-in-water emulsions in a square batch
electrocoagulation cell (Fouad, 2012). The use of dimensionally stable
anodes represents another electrochemical treatment technique for
oily wastewater. The underlying mechanisms involve electrochemical
oxidation which does not occur in electrocoagulation. A combined
two-step process consisting in the electrochemical coagulation with
iron anodes and the electrochemical oxidation with boron-doped dia-
mond anode was developed for the treatment of a real carwash waste-
water (Panizza and Cerisola, 2010).
5.2. Advancements in operation and control
Another area of technology advancement is the operation and con-
trol of parameters taking into considerations of the dynamics of the
electrocoagulation process. In the direct current mode, the formation
of an impermeable oxide layer on the electrode leads to electrode pas-
sivation, causing the decline of treatment efficiency. To overcome such
impact, the development of pulsed or alternating current applications
has been explored in recent years. The effect of pulsed voltage applica-
tion on energy consumption during electrocoagulation of emulsified
oils was investigated by Genc and Bakirci (2015). It was found that
the pulsed voltages saved energy during the electrocoagulation process.
In continuous operation, energy saving was as high as 48%. A sono-
electrocoagulation technique was applied to the treatment of oil tan-
ning effluent (Maha Lakshmi and Sivashanmugam, 2013). It was
found that continuous sono-treatment adversely affected the
electrocoagulation process. Sonication can break bubbles or coalesced
them. It also inhibited the formation of flocs. However, intermittent ul-
trasonic impingement can be used to overcome passivation.
6. Integration of electrocoagulation and other treatment techniques
To better utilize the advantages of different treatment ap-
proaches, the integrated treatment processes are often employed in
engineering application. As a result, considerable efforts have been
devoted to using electrocoagulation combined with other technolo-
gies in oil removal. For example, the membrane technology showed
potential in oily wastewater treatment. Electrocoagulation can be ef-
fectively adopted in combination with membrane filtration to reduce
membrane fouling. Yang et al. (2015) examined the feasibility of
combined electrocoagulation and kaolin dynamic membrane for
improving the performance of oily wastewater treatment.
Electrocoagulation could effectively reduce the reversible resistance,
which was the primary cause of permeate flux decline. Compared
with aluminum anode, iron anode showed better performance in dy-
namic membrane-electrocoagulation process because aluminum
anode seemed more inclined to form a looser layer. The normalized
fluxes and oil removal rates increased with the rise of current density
and decline of initial pH. The maximal oil removal rates of effluent
and permeate at 65 and 98.5% have been observed, respectively.
Zhao et al. (2014a) investigated the treatment of produced water
by electrocoagulation prior to RO membrane. An
electrocoagulation–RO process for simultaneous removal of hard-
ness, COD, and turbidity was developed. The combined effectiveness

(1) EC equipment; (2) reaction/sedimentation

equipment; (3) UF membrane unit; (4) controller;
(5) RO unit; (6)trailer platform; (7) pressure filter.

Fig. 6. The integrated mobile system for oilfield produced water treatment (Huang et al., 2013).

Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
of electrocoagulation for the pre-treatment of produced water prior
to RO membranes was highlighted. The optimal operating conditions
were determined to be with the initial pH of 7.36, the current density
of 5.90 mA/cm2, and the reaction time of 30.94 min. N99.9% of oil can
be removed after the combined electrocoagulation-RO process. For
scale-up application, Huang et al. (2013) developed an integrated
mobile system for oilfield produced water treatment with the treat-
ment capacity of 15 m3/d. The combination of electrocoagulation and
membrane filtration approaches was used with integrated intelli-
gent automation and process optimization in the framework of a mo-
bile treatment platform (Fig. 6). More than 95% of oil, TOC, COD, TSS
and turbidity in produced water could be removed. The system could
also effectively remove about 90% of ions, including chloride, sulfate,
sodium, calcium, manganese, etc.
Electrocoagulation has also been used with other physiochemical
techniques to achieve a high oil removal efficiency. Gursoy-
Haksevenler and Arslan-Alaton (2014) reported the treatment of olive
oil mill wastewater through combined acid cracking and
electrocoagulation. Acid cracking was carried out by adjusting the pH
to 2 with 0.13 M H2SO4 and heating the wastewater samples to 70 °C.
Electrocoagulation experiments were performed with stainless steel
electrodes at pH 2 and current density of 50 mA/cm2 at 65 °C for
120 min. A removal efficiency of 96% could be achieved for oil and
grease using this combined acid cracking-electrocoagulation process.
Siles et al. (2010) studied the anaerobic co-digestion of wastewater de-
rived from biodiesel manufacturing using electrocoagulation as pre-
treatment. To reduce the content of oily organic matter, the wastewater
was acidified by adding H2SO4 at first. The wastewater was then neu-
tralized by adding NaOH and electrocoagulation reactor with eight alu-
minum electrodes was further used for pre-treatment. In the
electrocoagulation process, the total COD decreased by 6.25% and solu-
ble COD decreased by 13.60% after 30 min. The overall reduction of total
COD was found to be 45% with both the acidification-centrifugation and
electrocoagulation steps. The anaerobic co-digestion of glycerol and
wastewater was applied after electrocoagulation and the biodegradabil-
ity was found to be around 100%. Ngamlerdpokin et al. (2011) reported
the application of acidification and electrocoagulation for the remedia-
tion of biodiesel wastewater containing vegetable oil. Acid treatment
was used before electrocoagulation and 99.36% of oil and grease could
be removed.
Daghrir et al. (2012) investigated the electrocoagulation-
electrooxidation process for the treatment of restaurant wastewater
with oil, grease, and suspensions solids. The oxidant and coagulant
Fig. 7. Schematic representation of combined electro-Fenton, anaerobic and electrocoagulation treatment process (Khoufi et al., 2006).
Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
15
agents could be produced simultaneously in electrocoagulation-
electrooxidation process. More than 98% of oil and greases were re-
moved when using aluminum and graphite plates alternated in the
electrode pack and operated at current of 0.4 A during 90 min of treat-
ment with pH adjusted to approximately 7.0. Esfandyari et al. (2015) re-
ported the treatment of olive oil mill processing wastewater by peroxi-
electrocoagulation/electrooxidation-electroflotation process. In the
electrochemical unit, aluminum, stainless steel, and RuO2/Ti plates
were used. A removal efficiency of 97.1% for oil and grease could be
achieved under optimal conditions of pH 4, current density of
40 mA/m2, 1000 mg/L H2O2, 1 g/L NaCl, and 30 min reaction time. This
process could also help significantly improve the biodegradability of
olive mill wastewater.
Bazrafshan et al. (2012) investigated the feasibility of treating cattle-
slaughterhouse wastewater by combined chemical coagulation using
PAC and electrocoagulation using aluminum electrodes. Coagulation
process alone was not able to meet discharge standards. The removal ef-
ficiencies increased by increasing the coagulant dose and electrical po-
tential. At the highest applied voltage, the fastest treatment rate was
obtained. More than 99% removal of COD and BOD5 was obtained by
adding 100 mg/L PAC and applying 40 V voltage. Drogui et al. (2008) re-
ported the treatment of poultry slaughter wastewater using
electrocoagulation-flocculation process. To improve agglomeration of
flocs and facilitate sludge sedimentation, the polymer (LPM 9511) was
added as flocculants. This combined process can resulted in effective re-
moval of organics (98.5% total oil and grease removal and 81.6% total
COD removal), inorganics (with the exception of nitrogen), pathogen
destruction and solids and turbidity removal.
Ahmadi et al. (2013) observed that the presence of H2O2 and PAC
had significant influence on the treatment of biodiesel wastewater
using electrocoagulation. The assistance of oxidation using 2% H2O2
could lead to a low final concentration of oil and grease at 18 mg/L;
the assistance of coagulation using 0.5 g/L PAC could lead to a final con-
centration of oil and grease at 387 mg/L. A complete removal of oil and
grease could be achieved in the presence of both 2% H2O2 and 0.5 g/L
PAC. Ün et al. (2006) studied the treatment of olive mill wastewater
using electrocoagulation with either iron or aluminum as sacrificial
electrode. Differences between treatment efficiencies with and without
the aid of H2O2 and PAC were found to be significant. The best result for
oil and grease removal was obtained in electrocoagulation enhanced
with coagulation and oxidation using 2.3% H2O2 + 0.5 g/L PAC. Khoufi
et al. (2006) reported the use of integrated electro-Fenton, anaerobic di-
gestion and electrocoagulation processes for the treatment of olive mill
16 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx

wastewater containing 12 g/L COD (Fig. 7). The electro-Fenton method performance globally. Reduction in energy consumption can be achieved
was applied as pre-treatment to remove a large amount of recalcitrant through process optimization. A trade-off among various competing fac-
polyphenolic compounds. The anaerobic process was applied thereafter tors should be evaluated. In addition, it is also desired to find a better solu-
with a loading rate of 10 g COD/(L·d). Oil contents were all removed tion for disposal of generated sludge and utilization of generated hydrogen.
after anaerobic treatment. Electrocoagulation could help remove the re- This can make the technology a more effective, low-cost, eco-friendly, and
sidual polyphenols, COD and color. Maha Lakshmi and Sivashanmugam viable alternative process for the removal of oil from various wastewater
(2013) investigated the treatment of oil tanning effluent through sono- sources.
electrocoagulation. Indirect sonication was provided by means of bath Each oil removal approach has its own advantages and disadvan-
type sonicator (40 kHz, 350 W). Electrocoagulation showed better per- tages. This is also true for electrocoagulation. To meet ever-stricter envi-
formance than sono-electrocoagulation for the treatment, however it ronmental regulations, electrocoagulation can be used with other
was found that impingement of ultrasound can be used to overcome treatment techniques as either pre-treatment or post-treatment pro-
passivation. Some reported studies on integrated electrocoagulation cess. Choice of the best combination can be determined based on oily
and other techniques for oil removal from water are summarized in water characteristics, cost-effectiveness, space availability, and reuse
Table 3. and discharge plans. In such a way, the advantages of various methods
can be maximized to avoid their limitations. The higher percentages of
7. Concluding remarks and recommendations oil-containing water can be recovered and utilized for reducing operat-
ing costs and achieving environmental sustainability.
Oil is widely found in wastewater from various sources. This waste- Overall, electrocoagulation process is a promising technology for ap-
water, which poses a threat to the environment, needs to be treated ef- plication in oil removal from wastewater. Besides the application in in-
ficiently. Different physicochemical and biological treatment processes dustrial and municipal wastewater treatment, the technology has
have been used in bench or pilot scale to treat oily wastewater. Several potential for treating surface water and groundwater which are con-
issues such as economic and environmental factors have triggered the taminated by oil. This technique could be also applied to mitigate the
development of electrocoagulation technologies for oil removal from impact of environmental disaster with the massive oil spill. More math-
wastewater. Study on oil removal from wastewater through ematical, technical, and practical studies are required for the future ap-
electrocoagulation has received increased attention in the last decade. plication. It is expected that the full potential of the electrocoagulation
This approach has been successfully applied to remove oil from a wide process as an emerging wastewater treatment alternative for oil remov-
range of industrial wastewaters. The performance of electrocoagulation al from water can be realized.
process is related to many system characteristics and operation factors
such as the nature of electrodes, current density, exposed area of elec- Abbreviations
trodes, electrode configuration, spacing of electrodes, pH, initial concen-
tration of oil, and electrolyte concentration. Simple equipment, BOD biochemical oxygen demand
convenient operation, and non-requirement of chemical substances COD chemical oxygen demand
for sedimentation and floc generation are the main advantages of this DAF dissolved air flotation
technique. It can also achieve satisfied oil removal within short hydrau- EPA Environmental Protection Agency
lic retention time. HEM hexane extractable materials
The development of advanced electrode materials, application of MF microfiltration
different electrode configurations, and optimal design for reactors can be NF nanofiltration
promising for improving the treatment efficiency of electrocoagulation PA polyamides
process. Further research is needed for the application of PAC polyaluminum chloride
electrocoagulation using larger-scale and/or continuous systems. In- PAN polyacrylonitrile
depth study of oil removal mechanism under these conditions is also PES polyethersulfone
required to provide a solid theoretical foundation. Although many PSF polysulfone
individual case-related process optimization studies exist, a generalized PVDF polyvinylidene difluoride
approach is required to maximize removal efficiencies and predict reaction RO reverse osmosis

Table 3
Some reported studies on integrated electrocoagulation and other techniques for oil removal from water.

Oily water sources Oil concentration Electrocoagulation Combined technique Removal References
(mg/L) electrode efficiency

Biodiesel wastewater 6412 Iron Electro-Fenton process and chemical N99.9% Ahmadi et al. (2013B89)
coagulation
Slaughterhouse 34 Aluminum Chemical coagulation N99% Bazrafshan et al. (2012)
wastewater
Restaurant wastewater 1300 Aluminum/graphite Electrooxidation 98% Daghrir et al. (2012))
Slaughterhouse 853 Iron Flocculation 98.5% Drogui et al. (2008)
wastewater
Olive mill wastewater 5320 Aluminum, iron, Electrooxidation-electroflotation 97.1% Esfandyari et al. (2015)
RuO2/Ti
Olive oil mill 9000 Iron Acid cracking 96% Gursoy-Haksevenler and Arslan-Alaton
wastewater (2014)
Olive mill wastewater 12,000 Iron Electro-Fenton and anaerobic digestion N99.9% Khoufi et al. (2006)
Oil tanning wastewater 4340 Iron and aluminum Ultrasound 86% (COD) Maha Lakshmi and Sivashanmugam
(2013)
Biodiesel wastewater 18,000–22,000 Iron Acid protonation N99% Ngamlerdpokin et al. (2011)
Biodiesel wastewater 428 (COD) Aluminum Acidification-centrifugation 45% (COD) Siles et al. (2010)
Olive mill wastewater 45,000 (COD) Iron and aluminum Electro-Fenton and chemical coagulation 86% (COD) Ün et al. (2006)
Oilfield produced 3000 Iron/graphite Reverse osmosis N99.9% Zhao et al. (2014a)
water

Please cite this article as: An, C., et al., Emerging usage of electrocoagulation technology for oil removal from wastewater: A review, Sci Total En-
viron (2016), http://dx.doi.org/10.1016/j.scitotenv.2016.11.062
 C. An et al. / Science of the Total Environment xxx (2016) xxx–xxx
RSM response surface method
TIS tanks-in-series
TOC total organic carbon
TSS total suspended solids
UF ultrafiltration
UV ultraviolet
Acknowledgements
This research was supported by the Natural Science and Engineering
Research Council of Canada, the Canada Research Chairs Program (CRC),
the Canada Foundation for Innovation (CFI) and the Petroleum Technol-
ogy Research Centre. The authors are also grateful to the editors and the
reviewers for their insightful comments and suggestions.
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