Journal of Environmental Management 272 (2020) 111057

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Journal of Environmental Management

journal homepage: http://www.elsevier.com/locate/jenvman

Review

A review on treatment of petroleum refinery and petrochemical plant

wastewater: A special emphasis on constructed wetlands
Mahak Jain a, Abhradeep Majumder b, Partha Sarathi Ghosal a, Ashok Kumar Gupta c, *
a
School of Water Resources, Indian Institute of Technology Kharagpur, Kharagpur, 721302, India
b
School of Environmental Science and Engineering, Indian Institute of Technology Kharagpur, Kharagpur, 721302, India
c
Environmental Engineering Division, Department of Civil Engineering, Indian Institute of Technology Kharagpur, Kharagpur, 721302, India

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

Keywords: Petroleum refinery and petrochemical plants (PRPP) are one of the major contributors to toxic and recalcitrant
PRPP wastewater organic polluted water, which has become a significant concern in the field of environmental engineering.
Constructed wetlands Several contaminants of PRPP wastewater are genotoxic, phytotoxic, and carcinogenic, thereby imposing
Environmental impacts
detrimental effects on the environment. Many biological processes were able to achieve chemical oxygen demand
Phytoremediation
(COD) removal ranging from 60% to 90%, and their retention time usually ranged from 10 to 100 days. These
Biological treatment
Persistent organic pollutants methods were not efficient in removing the petroleum hydrocarbons present in PRPP wastewater and produced a
significant amount of oily sludge. Advanced oxidation processes achieved the same COD removal efficiency in a
few hours and were able to break down recalcitrant organic compounds. However, the associated high cost is a
significant drawback concerning PRPP wastewater treatment. In this context, constructed wetlands (CWs) could
effectively remove the recalcitrant organic fraction of the wastewater because of the various inherent mecha­
nisms involved, such as phytodegradation, rhizofiltration, microbial degradation, sorption, etc. In this review, we
found that CWs were efficient in handling large quantities of high strength PRPP wastewater exhibiting average
COD removal of around 80%. Horizontal subsurface flow CWs exhibited better performance than the free surface
and floating CWs. These systems could also effectively remove heavy oil and recalcitrant organic compounds,
with an average removal efficiency exceeding 80% and 90%, respectively. Furthermore, modifications by
varying the aeration system, purposeful hybridization, and identifying the suitable substrate led to the enhanced
performance of the systems.

Administration, 2020). Furthermore, the world oil demand is expected

1. Introduction
Petroleum refinery and petrochemical plants (PRPP) are a group of
industries that deal with the production of fuels, lubricants, petro­
chemicals, and their intermediates. The global economic development
and increase in population have created a considerable demand for
PRPP products. The steps involved in crude-oil extraction and process­
ing involve large quantities of water, resulting in the generation of a
significant volume of wastewater. The amount of wastewater generated
by PRPP is almost around 0.4 to 1.6 times the amount of crude oil
produced (Coelho et al., 2006). As per Energy Information Administra­
tion (EIA), 2019 report world oil consumption was 99.93 million barrels
per day (mBPD) in 2018, indicating generation of about 6500 million
liters of PRPP wastewater per day (U.S. Energy Information
to rise to 102.22 mBPD and 107 mBPD in 2020 and 2030, respectively
(Diya’Uddeen et al., 2011; U.S. Energy Information Administration,
2020). This surge in the demand for PRPP products is making the sci­
entists apprehensive about the safety of the environment. The PRPP
wastewater is composed of various toxic organic compounds, which
impose a significant threat to the aquatic environment. As a result, the
development of advanced strategies for PRPP wastewater remediation is
of utmost priority.
Large quantities of aromatic and aliphatic hydrocarbon compounds
are present in PRPP wastewater, which can significantly affect the
aquatic ecosystem. Furthermore, oil being an immiscible liquid forms a
layer on the surface of water bodies and inhibits the entry of sunlight
and oxygen, leading to less dissolved oxygen (DO) and increased mor­
tality rate of the aquatic species. Onwumere and Oladimeji (1990)

* Corresponding author.
E-mail addresses: mahakjain140@iitkgp.ac.in (M. Jain), abhradeep.majumder@iitkgp.ac.in (A. Majumder), psghosal@swr.iitkgp.ac.in (P.S. Ghosal), agupta@
civil.iitkgp.ac.in (A.K. Gupta).

https://doi.org/10.1016/j.jenvman.2020.111057
Received 2 May 2020; Received in revised form 29 June 2020; Accepted 3 July 2020
Available online 21 July 2020
0301-4797/© 2020 Elsevier Ltd. All rights reserved.
M. Jain et al. Journal of Environmental Management 272 (2020) 111057

List of abbreviations MFC Microbial fuel cell

MHA Microaerobic hydrolysis–acidification
A/O-BR Anaerobic-aerobic-biofilm reactor MSBR Membrane sequencing batch reactors
AASP Aerobic activated sludge process MTBE Methyl tertiary butyl ether
ABR Anaerobic baffled reactor NP Nonylphenols
AMBR Anaerobic membrane bioreactors O&G Oil and grease
AOP Advanced oxidation processes OCP Organochlorine pesticides
API American petroleum institute PACT Packed activated carbon treatment
ASP Activated sludge process PAH Polycyclic aromatic hydrocarbons
BOD Biochemical oxygen demand PBR Photo-bioreactors
BTEX Benzene, toluene, ethylbenzene, xylene PCB Polychlorinated biphenyls
BPA Bisphenol A POP Persistent organic pollutant
COD Chemical oxygen demand PRPP Petroleum refinery and petrochemical plants
CW Constructed wetlands SBBR Spouted bed bioreactor
DO Dissolved oxygen SBR Sequential bioreactor
EF Electro-Fenton SFCW Surface flow constructed wetlands
EGSB-BR Expanded granular sludge bed bioreactor SSF-CW Subsurface flow constructed wetlands
EIA Energy information administration TDS Total dissolved solids
EU European Union TN Total nitrogen
FSF-CW Free surface flow constructed wetlands TOC Total organic carbon
FW Floating wetland TPH Total petroleum hydrocarbon
HAR Hybrid anaerobic reactor TSS Total suspended solids
HF Horizontal flow UAFB Up-flow anaerobic fixed bed
HF-MBR Hollow fiber membrane bioreactor UASB Up-flow anaerobic sludge blanket
HLR Hydraulic loading rate USEPA United States Environmental Protection Agency
HRT Hydraulic retention time VF Vertical flow
HSSF-CW Horizontal subsurface flow constructed wetlands VSSF-CW Vertical subsurface flow constructed wetlands
KH Henry’s constant WAO Wet air oxidation
mBPD Million barrel per day WBG World bank group
MBR Membrane bio-reactor WWTP Wastewater treatment plant
MBBR Moving bed bio-reactor

showed that there was an accumulation of metals in Oreochromis nilo­
ticus when the fish was exposed to treated petroleum refinery effluent
from the Nigerian National Petroleum Corporation, Kaduna. Uzoekwe
and Oghosanine (2011) studied the effect of petrochemical effluent on
the water quality of Ubeji Creek in the Niger Delta of Nigeria and sug­
gested that the mixing of petrochemical effluent with brackish waters at
the lower reaches of the river was detrimental to aquatic life. Also, it has
been reported that exposure to these toxic hydrocarbons over a pro­
longed period can also severely affect human beings (Zhang et al.,
2016). Furthermore, they are highly soluble and persistent and may
migrate into groundwater. As a result, PRPP wastewater should be
treated to meet the effluent standards before it can become detrimental
to the environment.
Numerous processes, such as membrane bio-reactor (MBR), moving
bed bio-reactor (MBBR), activated sludge process (ASP), up-flow
anaerobic sludge blanket (UASB), anaerobic membrane bioreactors
(AMBR), hybrid anaerobic reactor (HAR), up-flow anaerobic fixed bed
(UAFB) reactor, anaerobic-aerobic-biofilm reactor (A/O-BR), micro­
aerobic hydrolysis acidification (MHA), membrane sequencing batch
reactors (MSBR) photocatalysis, electro-Fenton (EF), catalytic ozona­
tion, membrane filtration, etc. have been generally used for the treat­
ment of PRPP wastewater (Jafarinejad and Jiang, 2019; Tian et al.,
2019). However, such established technologies are characterized by
inherent limitations, such as high capital and operation/maintenance
cost, technical complexity, etc. These limitations reduce the technical
feasibility and economic viability of the treatment processes, especially
for developing countries (Ahmad et al., 2019). Also, the disposal of a
considerable amount of oily sludge generated after the conventional
treatment processes is a significant concern. PRPP wastewater comprises
of non-biodegradable, refractory, recalcitrant organic matters, which
are resistant to the existing technologies. Hence eco-friendly,
cost-efficient, easy-to-operate treatment technologies are required,
which can efficiently treat the various components of PRPP wastewater
and also not produce any harmful metabolites and sludge. Constructed
wetlands (CWs) have shown considerable viability for the treatment of
such contaminants due to the presence of multiple removal mechanisms,
such as phytoremediation, microbial degradation, substrate intercep­
tion, etc. They do not require skilled labor, regular monitoring, high
initial, and operation cost, which add on to the numerous advantages of
these systems. Additionally, since PRPP wastewater comprises of
various organic hydrocarbons, it may act as a source of nutrients for the
plants and microbes (Martin et al., 2014).
Over the past few decades, numerous studies have been carried out
involving constructed wetlands and PRPP wastewater separately. Fig. 1
depicts that research involving PRPP wastewater treatment started back
in the late 1970s, and substantial work on constructed wetlands started
from the early 1990s. However, only a handful of studies have been
carried out involving the treatment of PRPP wastewater using CWs. Tian
et al. (2019) and Jafarinejad and Jiang (2019) reviewed the efficiency of
various biological methods and advanced oxidation methods in terms of
PRPP wastewater. However, constructed wetlands were not considered
in their study. On the other hand, various researchers reviewed the
performance of constructed wetlands in terms of removal of nitrogen,
phosphorous, COD and other nutrients from various types of wastewater
but did not focus on PRPP wastewater (Healy and O’ Flynn, 2011;
Lakatos et al., 2014; Valipour and Ahn, 2016; Vymazal, 2014, 2013,
2007). Mustapha and Lens (2018) addressed the role of various oper­
ating conditions and performance of CWs in treating PRPP wastewater
but comparison of the performance of CWs with other treatment
methods was not addressed. Moreover, there is a lack of compiled
literature addressing optimum operating conditions, plants, and mi­
croorganisms capable of degrading phenolic compounds, etc.

2
M. Jain et al.
Fig. 1. Frequency of publications on petroleum refinery and petrochemical
plants wastewater treatment and constructed wetlands with selected keywords
(Details are given in Section A of supplementary materials).
This paper presents a qualitative and quantitative analysis of the
major components of PRPP wastewater. It also highlights the various
environmental impacts concerning the harmful contaminants of this
wastewater. This article not only focuses on CWs in treating PRPP
wastewater, but also compares its treatment efficiency with other
established wastewater treatment technologies in this field. Due to the
lack of compiled literature on CWs in treating PRPP wastewater, a
special emphasis has been given on this technology. Various types of
CWs have been addressed along with the role of operational parameters
(macrophytes, flow rate, microorganisms, substrate, and aeration) on
contaminant removal. An insight has been provided on the various
mechanisms involved in PRPP wastewater treatment by CWs. Modifi­
cation of conventional CWs by varying operating conditions to attain
Fig. 2. Discharge of different contaminants resulting from various processes in petroleum refinery and petrochemical plants.
3
Journal of Environmental Management 272 (2020) 111057
enhanced performance have also been discussed.
2. Sources of water pollution from PRPPs
PRPPs produce several valuable and useful products, such as poly­
mers, fertilizers, synthetic rubber, pharmaceuticals, additives, adhe­
sives, etc. They involve various processes, such as drilling, exploration,
cracking, crude desalting, fractional distillation, polymerization, isom­
erization, catalytic reforming, hydro-treating, alkylation, trans­
portation, etc. (Cholakov, 2009). At each step, a wide range of
contaminants is discharged into the environment (Fig. 2). A large
quantum of water is required in the production process, which makes
the petroleum industry as one of the most water demanding establish­
ment. Consequently, a large volume of wastewater is also generated in
the production stages. Exploration and production of crude oil deterio­
rate the quality of the water and land. Exploration is carried out to
outline the reservoirs of oil and gas (Cholakov, 2009; Jafarinejad and
Jiang, 2019). This process involves geological surveys using methods,
such as magnetic and seismic geophysical methods. Improper applica­
tion of seismic methods can severely affect the aquatic ecosystem and
harm marine species. Drilling requires gel-like water or oil-based
emulsions, which include various polymers, ionic and nonionic emul­
sifiers, etc. (Cholakov, 2009). These chemicals come in contact with the
ground creating soil and water pollution. Enhanced oil recovery
methods and on-site processing of crude oil and natural gas may release
hydrocarbons and sulfur into the atmosphere. Processes, such as
cracking, distillation, catalytic reforming, alkylation, are aimed at pro­
ducing high-quality end-products, such as petrol (or gasoline), kerosene,
diesel, lubricating oil, fuel oil, grease, wax, etc. However, large quan­
tities of sulfides, ammonia, cyanide, hydrocarbons, etc. are released with
effluent (Cholakov, 2009; Tian et al., 2019). Propylene and benzene are
also discharged into the water after thermal or catalytic cracking.
Transport networks, such as pipelines, tankers, rail-tracks, suffer from
oil spills resulting in further contamination of the environment
(Alva-Arga �ez et al., 2007; Cholakov, 2009). The contaminants contrib­
uting to PRPP effluents from various production processes are given in
Fig. 2.
M. Jain et al. Journal of Environmental Management 272 (2020) 111057

2.1. PRPP wastewater characteristics and disposal standards
The components of PRPP effluent varies widely depending on their
origin. The quality and quantity of wastewater produced depend on the
type of crude oil used, the final product generated, and the operation
processes involved. Several aliphatic and aromatic hydrocarbons of
toxic nature are found in PRPP effluent, such as benzene, toluene, eth­
ylbenzene,t, xylene (BTEX), methyl tertiary butyl ether (MTBE), poly­
cyclic aromatic hydrocarbons (PAHs), phenols, naphthalenic acid,
sulfides, metals derivatives, etc. (Liu et al., 2014; Yavari et al., 2015).
The characteristics of major PRPP compounds have been mentioned in
Table 1. These components are persistent in nature and are responsible
for the high Chemical oxygen demand (COD) and toxicity of the PRPP
wastewater. PAHs are a group of polycyclic aromatic hydrocarbons with
two or more benzene rings. These compounds are nearly colorless, hy­
drophobic, and has less vapor pressure, with high melting and boiling
points (Haritash and Kaushik, 2009). Furthermore, they have very high
toxicity levels and can undergo bio-accumulation leading to subsequent
bio-magnification. Oil and grease (O&G) or heavy oil, is another primary
component of PRPP effluent, which comes in contact with water bodies
through oil spills and discharge. Heavy oils are large hydrocarbons
having a higher number of carbon atoms, having high viscosity, heat
resistance, and chemical stability along with low biodegradability and
water solubility (Kuo et al., 2014). The treated effluents from various
conventional treatment systems of PRPP wastewater have a consider­
able amount of COD, Biochemical Oxygen Demand (BOD), Total
Organic Carbon (TOC), turbidity, phenolic compounds, etc., which
highlight the incompetence of these treatment systems (Banerjee and
Ghoshal, 2017; Majone et al., 2010). The variation of concentration of
these contaminants in PRPP effluent has been presented in Fig. 3. The
concentration of contaminants varies with the location and the type of
petrochemical plant. A maximum COD concentration of 266,000 mg/L
in the petrochemical wastewater of Taiwan was reported by Chang et al.
(2005). Bayat et al. (2015) reported a BOD concentration of 1266 mg/L
in petrochemical wastewater in Iran. High levels of phenol, BTEX, Total
Suspended Solids (TSS), Total Dissolved Solids (TDS), O&G were also
reported by various authors in petrochemical wastewater (Al Zarooni
and Elshorbagy, 2006; Jafarinejad and Jiang, 2019; Mustapha and Lens,
2018; Rehman et al., 2019). Due to the high concentrations of the
various contaminants in PRPP wastewater and their subsequent toxi­
cological impacts, various environmental agencies have set standard
limits for disposal of treated PRPP effluent to surface water, marine
water, and reuse in agricultural fields. Table S2 shows the standards set
by United States Environmental Protection Agency (USEPA) and the
World Bank Group (WBG) for different contaminants in oil refinery
effluent. However, conventional treatment systems are often unable to
meet these standards. These circumstances pave the way for a new
domain of proficient technologies.
2.2. Impacts of PPRP wastewater on environmental health
The PRPP contaminants are not only toxic to microorganisms
and aquatic life but also pose a severe health hazard to human beings.
Prolonged exposure to these PRPP contaminants is associated with
several kinds of anomalies among all kinds of lifeforms. Various
environmental impacts of some major components of PRPP wastewater
have been mentioned in Table 1. O&G form a layer on the water surface
and create an anoxic condition for the aquatic organisms. Researchers
observed a delay in the development process, late head formation, and
abnormal neural development in the embryo of a fish (Verasper
variegatus) due to the presence of heavy oil on the seawater surface
(Murakami et al., 2008). It also increased larval mortality and showed a

Table 1
PRPP wastewater major components and their environmental impacts.
Wastewater Characteristics Environmental Impact References
components

Heavy oil Large no. of C- atoms, viscous, heat resistant, stable chemical Growth retardation, Toxic Murakami et al. (2008)
structure, less biodegradable
PAH Colorless, hydrophobic, volatile, high melting, high boiling points. Genotoxic, Carcinogenic, Haritash and Kaushik (2009), Xiu et al. (2014)
Most common PAHs in PRPP wastewater are naphthalene, mutagenic in nature
phenanthrene, anthracene, fluorine, pyrene, benzo(e)pyrene and
benzo(k)fluoranthene
Phenolic Colorless to pale color liquid or crystals, volatile in nature. Phytotoxic, ecotoxic, carcinogenic Khairy (2013), Kottuparambil et al. (2014),
compounds Common phenolic compounds in PRPP wastewater are phenol, 2- in nature MacCrehan and Brown-Thomas (1987);
methylphenol, 1-napthol, 2-napthol Pugazhendi et al. (2017); Vosoughi et al. (2017)
Benzene Colorless liquid with distinct gasoline like smell Carcinogenic in nature Carvajal et al. (2018), Dehghani et al. (2018),
Flash point: 11.07 � F Reduces the production of both Pubchem (2020), Rahul et al. (2013)
Density: 876 kg/m3 red and white blood cells
Affects the lymphatic system and
central nervous system
Toluene Clear colorless liquid with aromatic odor Affects the central nervous system, Carvajal et al. (2018), Pubchem (2020), Rahul et al.
Flash point: 40� F eyes, respiratory system, liver and (2013), Tham et al. (2011)
Density: 867 kg/m3 kidney.
Non-carcinogenic
Causes drowsiness, fatigue, ataxia,
tremors, cerebral atrophy,
nystagmus
Xylene Colorless liquid with sweet color Non- carcinogenic Carvajal et al. (2018), Pubchem (2020), Rahul et al.
Flash point: 86 � F Alters enzymatic activity, causes (2013)
Density: 864 kg/m3 skin inflammation and can affect
the kidney
Ethylbenzene Colorless, volatile and highly inflammable liquid with gasoline like Affects the respiratory system and Carvajal et al. (2018), Pubchem (2020), Rahul et al.
odor nervous system (2013)
Flash Point: 59 � F
Density: 866 kg/m3
MTBE High water solubility, small molecular size and relatively low Carcinogenic, Allergic, affects the Pubchem (2020); Yu and Gu (2006), Zadaka-Amir
Henry’s law constant, non- degradable central nervous system et al. (2012)
Flash point: 27.4 � F Causes mucous membrane
Density: 740 kg/m3 irritation, labored breathing and
ataxia

4
M. Jain et al.
Fig. 3. Box-and-whisker plots (along with data points) showing variation in the
concentration of selected contaminants in petroleum refinery and petrochem­
ical plants wastewater as obtained from various literature. Data from: Table S1.
detrimental impact on the embryo stage of the fish due to its highly toxic
nature (Murakami et al., 2008). The adverse effects of BTEX include
genotoxicity, carcinogenicity, nervous system, and respiratory system
disorders (Carvajal et al., 2018; Thullner et al., 2018). Moreover,
toluene, ethylbenzene, and xylene may act as a mutagen. USEPA
recognized benzene as a class-A carcinogenic pollutant because of its
highly carcinogenic nature (Carvajal et al., 2018; Rahul et al., 2013).
BTEX is readily absorbed through the gastrointestinal tract and easily
reach the nervous tissues just after ingestion, which causes subsequent
damage to the nervous system (Bustillo-Lecompte et al., 2018). MTBE is
a highly volatile compound, which may lead to irritation, nausea, or
headache. It not only affects the respiratory, nervous, and cardiac
systems but also exhibits carcinogenic properties (Yu and Gu, 2006).
Apart from that, these compounds show toxic effects on soil
invertebrates, namely earthworms, springtail, etc., and many strains of
bacteria and yeast (Hentati et al., 2013; Roslev et al., 2015). However,
microorganisms are more sensitive towards MTBE as compared to
invertebrates in the water, exhibiting a negative impact on ecological
processes, such as biodegradation and nutrient cycles (Roslev et al.,
2015; Werner et al., 2001). Phenolic compounds generally occur in
the PRPP wastewater and can affect the metabolic and enzymatic
mechanisms of aquatic microorganisms even at low doses. Since the
degradation of phenolic compounds is a prolonged process, these
persistent compounds accumulate in the tissues of aquatic organisms
and subsequently cause bio-magnification. Phenols have been known to
be immunotoxic, genotoxic, carcinogenic, teratotoxic, as well as hae­
matologically and physiologically toxic (Mustapha and Lens, 2018).
Therefore, USEPA has designated phenolic compounds as priority
pollutant (Saleem et al., 2018). Kottuparambil et al. (2014) experi­
mentally confirmed the phytotoxicity of phenols on Eucyclops agilis,
where phenol reduced photosynthetic activity and motility of euglena.
Apart from that, phenol can infiltrate into the cell and rupture the in­
ternal membranous structure. Exposure to PAH compounds present in
the PRPP wastewater may also cause genotoxicity among the aquatic
organisms. Xiu et al. (2014) reported that the exposure to some of PAHs,
such as benzo[a]pyrene (BaP), benzo[b]fluoranthene (BbF) and
chrysene (CHR) compounds in juvenile scallop Chlamys farreri resulted
in lipid peroxidation, protein oxidation, DNA damage, etc. and
their toxicity sequence was reported as BaP > BbF > CHR. If PAH con­
centrations increase in the different exposure routes, such as drinking,
5
Journal of Environmental Management 272 (2020) 111057
inhalation, etc., then its overall concentration may exceed Excess
Lifetime Cancer Risk standards set by USEPA for carcinogenic chemicals,
thereby adversely affecting human life (Li and Li, 2017).
3. Treatment technologies
Treatment of PRPP wastewater targets a multifaceted approach for
the removal of oil, hydrocarbons, sulfates, and trace metals simulta­
neously. Over the past few decades, numerous treatment techniques
have been employed to treat PRPP wastewater (Fig. 4). Firstly, oil is
separated from water in the primary stage of treatment by several in­
terceptors, floatation chambers, and equalization tanks. Gravity sepa­
ration, such as the American petroleum institute (API) separator, can
also be used with less energy consumption (Jafarinejad and Jiang,
2019). The dissolved air flotation method was found to remove oil in the
range of 70%–90% from oily wastewater (Al-Shamrani et al., 2002;
Hanafy and Nabih, 2007). The primary system reduces the suspended
solids, O&G, and turbidity, which may otherwise influence the func­
tioning of microbes used in the secondary treatment (Aljuboury et al.,
2017).
Biological treatment aims at the decomposition of any remaining oil,
degradable organic compounds, a fraction of recalcitrant organic pol­
lutants, trace metals, nutrients, etc. (Gümüş and Akbal, 2016; Jafar­
inejad and Jiang, 2019; Khatri et al., 2018). Many biological treatment
processes have been efficient in the treatment of PRPP wastewater. The
salient features of the biological treatment systems have been depicted
in Fig. S1. Amongst, the ASP is the most commonly used treatment
process Ahmadi et al. (2017a). Ma et al. (2009) and Ebrahimi et al.
(2016) observed a COD removal efficiency in the range of 70%–80%
while treating PRPP wastewater using ASP. A relatively higher COD
removal efficiency of 96% was obtained by Mirbagheri et al. (2014),
which may be accounted for the high artificial aeration induced in the
process. The combination of two or more biological processes or the
combination of the biological process with membrane-based technolo­
gies has been effective in the treatment of wastewater. Liang et al.
(2019) combined an expanded granular sludge bed bioreactor
(EGSB-BR) with ASP to treat petroleum wastewater, having a COD of
4600–5300 mg/L and obtained a COD reduction of 85% after 62.8 h
retention time. Razavi and Miri (2015) used hollow fiber membrane
bioreactors (HF-MBR) to treat refinery effluent and achieved a COD
removal of 82% after providing 36 h retention time. Huo et al. (2018a)
combined photo-bioreactors (PBR) with traditional oxic/anoxic process
to treat low concentration petrochemical wastewater (COD: 312.8
mg/L) and achieved a removal efficiency of 71%. El-Naas et al. (2014)
augmented a spouted bed bioreactor (SBBR) with packed activated
carbon treatment (PACT) and electrocoagulation cell (EC) to treat high
concentration petrochemical water (COD: 3600–5300 mg/L) and ach­
ieved a removal efficiency of 97%. Ji et al. (2009) used the anaerobic
baffled reactor (ABR) to treat heavy oil produced water and achieved a
removal efficiency of 65% and O&G removal of 88%. Ruwais refinery
wastewater treatment plant (WWTP) successfully used a corrugated
plate interceptor for the separation of immiscible oil and water
(Benyahia et al., 2006). However, most of these processes produce a
tremendous amount of sludge, requires skilled labor and regular main­
tenance. Some of the processes also require very high hydraulic reten­
tion time (HRT), which is an inherent disadvantage to these methods.
Various biological treatment processes employed to treat petrochemical
wastewater have been given in Table 2. Fig. 5 depicts the HRT and
performance of various biological processes in terms of treating petro­
chemical wastewater. The operating conditions and performance level
of these processes have been listed in Table 2.
Tertiary treatment is provided to bring down the concentration of the
contaminant in secondary effluent to meet the reuse or discharge stan­
dards set by environmental agencies (USEPA, WHO, etc.). Various
advanced oxidation processes (AOPs), such as photocatalysis, wet air
oxidation (WAO), Fenton process, EF oxidation, etc. have been
M. Jain et al.
Fig. 4. Various treatment processes and their target contaminants during the treatment of petroleum refinery and petrochemical plants wastewater.
employed for tertiary treatment of PRPP wastewater. AOPs generate
various oxidizing radicals that react with the complex organics to form
simpler compounds (Majumder et al., 2019). AOPs may be considered as
a better option than adsorption as they can breakdown the parent
compound into their non-toxic forms, whereas the organics are only
transferred from aqueous medium to a solid medium by adsorption
(Majumder et al., 2019; Raza et al., 2019). Zhao et al. (2018) used a
two-stage WAO method to treat oily sludge from petrochemical waste­
water and achieved a removal efficiency of 85.4%. Mohanakrishna et al.
(2018) used a bioelectrochemical treatment system to treat refinery
wastewater and reduced COD by 75%. Several photocatalysts were used
for degradation of petrochemical wastewater, and a COD removal effi­
ciency ranging from 65% to 85% was achieved (Bustillo-Lecompte et al.,
2018; Meng et al., 2018; Shokri et al., 2016). Keramati and Ayati (2019)
combined photocatalysis with electrocoagulation to treat oil refinery
wastewater and achieved a COD removal of 95%. The EF process has
also been used to treat petroleum wastewater, and their COD removal
efficiency has varied from 54% to 84% (Davarnejad et al., 2014; Gümüş
and Akbal, 2016; Khatri et al., 2018). The catalytic ozonation process
exhibited more efficiency compared to photocatalysis and the EF process
in the treatment of petrochemical wastewater, showing a COD reduction
of up to 96% (Ahmadi et al., 2017b; Huang et al., 2019). Studies
reporting different AOPs and other tertiary treatment methods used in
the treatment of petrochemical wastewater are listed in Table 3, and
their effectiveness and reaction time have been provided in Fig. 5.
However, AOPs and other processes involved in tertiary treatment
require very expensive reactants, which limit their application at
full-scale levels. Furthermore, the efficiency of these AOPs decrease with
the increasing COD concentration (Levchuk et al., 2014). Hence, various
combinations of mechanical, physiochemical, and biological treatments
have been used in PRPPs for achieving higher removal efficiency. High
cost, low operating pH, and a large volume of sludge production are the
major drawbacks of PRPP wastewater treatment, which demands
extensive research and development of advanced and cost-effective
treatment systems.
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Journal of Environmental Management 272 (2020) 111057
4. Constructed wetlands as a plausible solution to remediate
PRPP wastewater
CWs have been recognized as an efficient water treatment technol­
ogy for the last five decades. These artificial wetlands have been used to
treat sewage, greywater, effluent from dairy, pulp, glass, petrochemical,
pharmaceutical, paper mill, and other industries (Aalam and Khalil,
2019; Avery et al., 2007; Chen et al., 2019; Gholipour et al., 2020;
Newman et al., 1999; Rühmland et al., 2015; Yusoff et al., 2019). CWs
are environment-friendly and economically sustainable systems having
multiple social advantages, such as habitat enrichment, raising the
aesthetic value of a wastewater treatment site, etc. (Bedessem et al.,
2007; Thullner et al., 2018). Furthermore, they are easy to operate, do
not require skilled labor and daily maintenance. Hence, it can be a better
treatment option for both developing and developed countries. Studies
have shown that this robust process can deal with varying contaminants
in wastewater, and its performance is not significantly affected by the
type and strength of the wastewater (Stefanakis et al., 2016). Moreover,
the substrate and macrophytes used in wetlands are not strictly specific,
very cheap, and are conveniently available. Plants used in wetlands can
be selected depending upon the environmental conditions and avail­
ability in close vicinity. Low sludge production is a fascinating feature of
CWs, which makes it a more desirable option over conventional treat­
ment systems associated with the production of a large amount of bulky
sludge (Jafarinejad and Jiang, 2019). Flores et al. (2019) carried out the
life cycle assessment of CW and ASP, and concluded that engineered
wetlands provide a natural way of treating contaminated wastewater
with minimum harm to the surrounding.
4.1. Conventional types of constructed wetlands
The efficiency of CW depends on its size, flow rates, retention time,
substrate, and macrophytes used (Aalam and Khalil, 2019; Al-Baldawi
et al., 2017; Ji et al., 2002, 2007; Stefanakis et al., 2016; Sudarsan et al.,
2016). The different types of conventional CWs have been depicted in
Fig. 6. Based on the macrophytes, CWs can be classified into three major
categories. The plants can be free-floating, floating-leaved, emerged, or
completely submerged. In floating wetlands (FW), the plants are not
 Table 2
Performance of biological treatment methods in treating PRPP wastewater.
Treatment method Wastewater type Wastewater characteristics HRT Operating conditions Removal Efficiency References
M. Jain et al.

HF-MBR Refinery effluent TSS ¼ 110 mg/l, BOD ¼ 203 mg/l, 25–36 h mixed liquor suspended solids (MLSS)- 3–6.6 g/ COD-82%, BOD-89%, TSS-98%, VSS-99%, Razavi and Miri
COD ¼ 580 mg/l, Turbidity-40 NTU L, temperature- 20 � C Turbidity-98% (2015)
ASP Petrochemical COD-300–600 mg/l, NHþ4 -N- 10–30 30 h Temperature- 27–32 � C, pH- 7–9 COD-74.4%, NHþ4 -N-19.6% Ma et al. (2009a)
wastewater mg/l
MSBR Refining wastewater COD – 310 mg/l 24 h MLSS-8.5 mg/l, temperature- 21 � 2 � C, DO- 2.5 COD- 97% Ahmadi et al. (2019)
� 0.2 mg/l
EGSB-BR and AAS Petrochemical COD- 4600–5300 mg/l, EGSB- 62.8 h, Annual treated Volume ¼ 657,000 m3, COD - 85.6 � 2.5%, petrochemicals - 81.5 � Liang et al. (2019)
wastewater petrochemicals- 50–80 mg/l AAS- 133.3 h temperature- 35 � C 4.8%
ABR heavy oil produced water heavy oil ¼ 1.01 g/cm 3, loading rate 60.0–144 h Low nutrient ratio COD:TN:TP ratio ¼ COD- 65% and oil- 88% Ji et al. (2009)
0.070–0.5 kg COD/m3/d 1200:15:1
ASP Petrochemical COD- 1000–1500 mg/l, OLR- 24–96 h MLSS- 3000 mg/l, flow rate- 3–12 l/h, SRT- COD- 78.7-61.5% Ahmadi et al. (2017a)
wastewater 0.33–1.21 kg COD/m3/d 13.5–5 d
UASB Synthetic phenolic COD- 530–2240 mg/l, phenolics- 226 18–7.92 h Temperature-27-35 � C, working volume-13.3 L, COD- 82.8%–91% Ramakrishnan and
wastewater to 752 mg/l SRT- 32–68 d Phenolics- 68%–95% Surampalli (2012)
ARH Synthetic phenolic COD- 530–2240 mg/l, phenolics- 226 18–7.92 h Temperature-27-35 � C, filter media- PVC rings, COD- 84%–90% Ramakrishnan and
wastewater to 752 mg/l SRT- 32–68 d Phenolics- 77%–99% Surampalli (2012)
UASB and biological Heavy oil wastewater COD- 129.8–1238 mg/l, NHþ 4 -N- 12 h Temperature- 25–35 � C, carrier-FPU (Function COD- 74%, NHþ 4 -N- 94% SS- 98% (Liu et al. (2013a))
aerated filter 38.21–83.64 mg/l, SS- 23.80–777.0 Polycin Urepan)
mg/l
AMBR synthetic wastewater OLR- 0.5–0.57 kg COD/m3/d and 144–216 h Temperature- 37 � 1 � C, flow rate- 2.25 l/day, NB-100%, COD- 85–94% Kuscu and Sponza
nitrobenzene (NB)- 20–400 mg/l (2009a)
ASP Refinery wastewater COD- 377–422 mg/l, MLSS- 4.19 h DO- 3.7 mg/l, flow rate- 700 l/h, contact COD- 78.65% Ebrahimi et al. (2016)
1865–2389 mg/l stabilization method
ABR synthetic wastewater NB- 30–700 mg/l, OLR- 0.29–3 kg 24–250 h Flow rate- 2.77–28.8 l/day NB- 100%, COD- 79–92% Kuscu and Sponza
COD/m3/d, (2009b)
�
HAR synthetic TA wastewater Terephthalate (TA) 600 mg/L,1000 18.9–24 h Temperature- 33-52 C COD- 66.1–91.9%, TA- 60.8–94.0% (Li et al. (2014b))

7
mg/L, OLR ¼ 1.6–4.5 kg COD m3/d
UASB synthetic petroleum OLR ¼ 0 - 11 kg-COD/m3/d 240–480 h Temperature- 36 � 2 � C COD- 93% at OLR- 11 kg-COD/m3/d Chen et al. (2017)
wastewater
ABR synthetic wastewater OLR- 2.67–5.4 kg COD m3/d 40–60 h Temperature- 40 � 1 � C, COD: N:P – COD- 88.2- 84.9% Zhang et al. (2011)
200–300:5:1
Packed-bed biofilm synthetic wastewater COD- 14–28 g/L, OLR- 3.4–20 g COD/ 33–100 h Temperature- 35 � C, COD- 78–97% Majone et al. (2010)
reactor (PBBR) from fisher tropsch L/d
process
UAFB FT wastewater COD- 32.855–38.461 g/L 40–144 h Temperature- 34 � 1 � C COD- 43–72% Wang et al. (2017)
hydrolytic Petrochemical COD- 856 � 11 mg/l, NHþ 4 -N- 40 � 1 – pH 6.47–7.45, ORP-110 � 25.0 mV and NHþ4 -N- 100.0%, Huo et al. (2018b)
�
acidification with wastewater mg/l, TP- 1.83 � 0.03 mg/l temperature- 35.0 C TP- 89.0%, COD- 83%
algal microcosms
MFC Petrochemical COD- 5000 mg/l 264 h Electrode- Carbon felt, biocatalyst -anaerobic COD- 82% Sarmin et al. (2019)
wastewater from acrylic sludge
acid plants
ASP Refinery wastewater COD- 1060 mg/l F/M- 0.38, Aeration- 120 L/min, F/M ratio- COD- 96% Mirbagheri et al.
0.38, Return sludge- 110%, (2014)
MSBR Refinery wastewater O&G- 21.5 mg/l, TOC- 123.4 mg/l, SRT- 480 h, total cycle time- 4 h and volume exchange ratio COD-80%, TOC-81.5%, O&G-82% Pajoumshariati et al.
COD- 191.8 mg/l, Turbidity- 42 NTU HRT- 8 h (VER) 0.5, temperature- 27 � 1 � C Turbidity- 99.3% (2017)
UASB and CSTR synthetic wastewater 2,4 dichlorophenol (DCP)- 5–120 mg/ 20 h flow rate – 3–3.48 l/d, temperature – 20 � C 2,4 DCP- 91.08–99.90%, COD- Sponza and Uluk€ oy
l, COD- 3000–3193 mg/l 86.67–95.14% (2006)
UASB Synthetic wastewater phenol-0-840 mg/l 48–72 h Temperature- 35 � 1 � C Phenol- 90% Guo et al. (2015)
UASB phenolic wastewater OLR of 1–2.5 kg-COD/m3/day – Temperature- 36 � 2 � C, Turf soil- 1.12 mg/g, COD and phenols- 97% Chen et al. (2018)
pH- 6.5- 8
MHA - A/O process petrochemical COD- 348 � 59 mg/l - 529 � 30 mg/l, 20.0 h Dominant bacteria- Proteobacteria, DO- 4–6 mg/ Ammonium ->94.0%, COD-72–79% Yang et al. (2015)
wastewater Ammonium-N- 25.8 � 5.8 mg/L - L, air flow rate- 0.3 L/h, temperature- 22–28 � C,
28.5 � 5.4 mg/L SRT- 30 dli
A/O-BR Heavy oil refinery COD- 650–1150 mg/L, Petroleum- 36.0–50.0 h Temperature- 30–35 � C, flow rate- 6.9 mL/h and COD- 93.2% and TN - 82.8% Li et al. (2017)
wastewater 70.5–95.8 mg/L, TN- 35–70 mg/L 184.7 mL/h
(continued on next page)
Journal of Environmental Management 272 (2020) 111057
 M. Jain et al. Journal of Environmental Management 272 (2020) 111057

Mahmoudkhani et al.
Cao and Zhao (2012)
El-Naas et al. (2014)

Yeruva et al. (2015)

Huo et al. (2018a)
References

(2012)
4 -N- >99%, P- >99%

COD- 97%, Phenol-100%, m, p-cresol-

100%, while the activated carbon was
saturated after only 8 h of operation
COD removal was 54.45%
COD- 71%–97.8%, NHþ
Removal Efficiency

Phenol- 55 to 90%
COD- 62 to 63%
COD-70 to 80%
Electrodes type: aluminum, current density of 3

operated in suspended growth configuration at

Volume ¼ 550 L, 85% of the reactor was filled

mA/cm2, air flow rate- 3 L/min, temperature-

ambient room temperature, DO- 0.75 � 0.25

Used filamentous microalgae Tribonema sp.,

Fig. 5. Box-and-whisker plots showing variation in the performance of various

with Polyurethane elements and MLSS ¼

treatment processes in terms of COD removal and time taken to achieve the
removal efficiency as obtained from diverse literature. Data from: Tables 2
30 � C, Liquid flow rate-10 mL/min

and 3.
Air flow rate ¼ 1.25 L/min

rooted in the soil media; rather, they are entangled with each other in
the form of a mat, facilitating the plant to float on the water surface
Operating conditions

freely and promoting the hydroponic growth of emergent macrophytes

1400–1700 mg/L

(Healy and O’ Flynn, 2011; Vymazal, 2007; Zhang et al., 2014). FWs
allow nutrient removal directly via root uptake, although the filtering
action of the media is absent (McAndrew and Ahn, 2017). CWs having
mg/l

emergent macrophytes can be further classified based on the flow

pattern of wastewater. In free surface flow CW (FSF-CW), water flows
over the surface of the soil, having direct contact with atmospheric ox­
ygen, while in subsurface flow (SSF) treatment systems, the flow path of
water is beneath the media surface. This flow path may be horizontal
216 h

(HF) or vertical (VF), depending upon the availability of land and media
24 h

48 h
HRT

8h

4h

(Vymazal, 2013). Furthermore, the VF can be upward with the help of a

pump or can be downward under the influence of gravity. Often, a
COD- 3600 to 5300 mg/l and Phenol-
4 -N-
18.1 mg/L- 7.9 mg/L, P-0.87 mg/L-

combination of two or more CWs, is used to achieve better removal ef­

11 to 14 mg/l, m, p-Cresol - 72–75
COD-80.8 mg/l- 312.8 mg/l, NHþ

OLR- 1.0 – 2.0 kg COD/m3- day

ficiencies. Such combinations of VF-CW and HF-CW, multistage CWs are

classified as hybrid CWs. Many studies compare the performance of
OLR- 9.68 kg COD/m3- day
Wastewater characteristics

wetlands depending on their flow patterns. Substrate selection is one of

the essential criteria for better working of a CW. Flow pattern, hydraulic
Phenol- 0.66 mg/L
COD- 1568 mg/L

loading rate (HLR), and HRT are some of the significant parameters,
which are critically considered while designing the CWs.
0.12 mg/L

mg/l

4.2. Use of constructed wetlands for PRPP treatment

In the past two decades, various pilot-scale and full-scale CWs have
Petroleum contaminated

been used for the treatment of PRPP wastewater. Full-scale CW treat­

Refinery wastewater

ment systems were adopted in Hungary for the treatment of Tisza Oil
Low concentration
Wastewater type

Refinery Plant (TIFO) and Nyirbogd� any Petrochemical Plant (NYKV)

Petrochemical

Petrochemical
petrochemical

wastewater (Lakatos et al., 2014). The pre-treatment system in TIFO

wastewater

wastewater

wastewater

wastewater

consisted of interceptors, flotation chambers, and an aeration basin,

while in NYKV, the wastewater was subjected to ASP after mechanical
and chemical treatment. This pre-treated effluent was transferred to a
CW system. NYKC consisted of a pre-settling pond unit, an oxidation
Table 2 (continued )

EC, SBBR and PACT

pond unit, and a post-settling reed pond, while TIFO consisted of algal
Treatment method

pond, fish pond, and reed pond units. Lakatos et al. (2014) found that
SBR and BET

the TIFO wetland pond system contributed around 40% TP and 35% TN
removal to the system over a period of 13 years. Likewise, the NYKV CW
MBBR

MBBR

system removed around 30% oil, and the whole composite treatment
PBR

system could remove up to 90% COD and 72–100% oil from wastewater.

8
 Table 3
Performance of tertiary treatment methods in treating PRPP wastewater.
Treatment method Wastewater type Wastewater characteristics Reaction time Operating Conditions Removal Efficiency References
M. Jain et al.

Adsorption Super heavy oil Oil- 0.754 mg/l and COD- Temperature-293, 303, 313 and 323 � 0.2 K, pH- 8.483, COD- 50.3%, Oil- 25.83% Tong et al. (2014)
wastewater 74.84 mg/l adsorbent- Lignite activated coke
Electrochemical catalytic Synthetic wastewater Phenol-520 mg/L, COD 1214 40 min Catalyst- ferric sulfate and potassium permanganate, adsorbent- COD- up to 99% Ma et al., (2009b)
treatment mg/L active bentonite, electrode- graphite
Two stage WAO Oily sludge from Oil content- 15% (mass 150 min Emulsion splitter- Sodium carbonate, oxidant- H2O2, Overall oil content- 93.1% Zhao et al. (2018)
petrochemical plant percentage), COD-419.9 mg/l Temperature- 240 � C. and oil sludge volume-
First stage- reaction time- 90 min, oxidant dose- 80 ml 85.4%
Second stage- reaction time- 60 min, oxidant dose- 40 ml
Bioelectrochemical Refinery wastewater COD- 2150 mg/L, TPH- 15 mg/ 96 h Electrode- Graphite, current density- 278 mA/m2, power density- COD- 75%, diesel range Mohanakrishna et al.
treatment L, pH- 7.45 222 mW/m2, potential- 800 mV organics- 90% (2018)
Electrocoagulation cell and Oil refinery effluent COD- 1000 mg/l EC- 8.7 min, Electrode- Stainless steel plates, Power- UV-C lamps of 8 W COD-95.8% Keramati and Ayati
Photo-catalysis Photo-catalysis- (2019)
180 min
Photochemical treatment BTEX wastewater TOC ¼ 65–135 mg/l 4h UV-254nm/H2O2 and UV-185nm/H2O2, pH- 3 (acidic condition) UV-254/H2O2-TOC-62%, Bustillo-Lecompte
UV-185/H2O2- TOC-80% et al. (2018)
Fenton process Petroleum refinery COD- 1259 mg/l, TOC-186 mg/ 10 h pH ¼ 3.0, molar ratio-[H2O2]:[COD]0- 6, [H2O2]:[Fe0]- 10 COD- 76.5%, TOC- 45% Diya’uddeen et al.
effluent l, phenol-14.7 mg/l, O&G- 233 and phenol- 96%, O&G- (2015)
mg/l 100%
Photocatalysis Petrochemical COD ¼ 300 mg/l, 4 Nitro phenol 180 min Catalyst (dose- 1 g/l, 100 W tungsten lamp visible light) 4-NP: Shokri et al. (2016)
wastewater (4-NP) ¼ 25 mg/l B–GO–TiO2-100%,
B–TiO2- 85%,
GO–TiO2- 80%
COD:
B–GO–TiO2-85%,
B–TiO2-70%,
GO–TiO2- 65%

9
Photocatalysis Phenolic water – 80 min Catalysts- Bi4O5BrxI2-x, Phenols- 92%, TOC- 79% Meng et al. (2018)
Catalyst dosage- 1.00 mg/ml, light intensity- 500 W halogen lamp
visible light
Catalytic ozonation Petrochemical nitrobenzene-300 mg/L, pH- 30 min Temperature- 25.0–50.0 � C, catalyst- Spent fluid catalytic cracking COD- 55.6–87.2 Chen et al. (2015)
wastewater 6.53, and COD- 538.4 mg/L catalysts (dose ¼ 0.250–1.00 g), Oxygen dose ¼ 0.62–2.25 mg/
min
Catalytic ozonation Petrochemical COD- 144 mg/L 120 min Temperature-20.0–25.0 � C, catalyst- Fe–Ni foam (dose-110 g/L), COD- 96%, DOC- 61% Huang et al. (2019)
wastewater Ozone dose ¼ 10.2 mg/L O3
Catalytic ozonation Petrochemical COD- 362 � 36.0 mg/L 120 min Temperature-20.0–25.0 � C, catalyst- PAC@Fe3O4 (dose- COD- 75.3%, TOC- 50.3% Ahmadi et al. (2017a)
wastewater 0.150–0.750 g/L), Ozone dose ¼ 0.050–0.300 g/h O3, pH-
3.00–11.0
EF Synthetic wastewater Phenol ¼ 250 mg/L 30 min Electrode- iron, electrolyte- NaCl, H2O2- 37.2 mM, pH- 5.20, EC- COD- 84%, TOC- 52%, Khatri et al. (2018)
125 μS/cm, stirring speed-100 rpm, inter-electrode gap 4.00 cm, phenol- 100%
current density- 0.800 mA/cm2
EF Synthetic wastewater Phenol- 250 mg/L, COD- 800 5 min Electrode- iron, electrolyte- raw effluent, pH- 3.00, H2O2-500 mg/ COD- 87.5%, Phenol- Gümüş and Akbal
mg/L L, current density- 1.00 mA/cm2, EC- 1000 μS/cm 93.3% (2016)
Electrocoagulation cell Petrochemical COD- 2,746 mg/L 480 min Electrode- Ti/Pt, boron-doped diamond (BDD), electrolyte- raw COD- 98.7% (dos Santos et al.,
industry effluent, pH- 3.00, electrode gap- 10 mm, current density- 40.00 2014)
mA/cm2, temperature- 60�
EF Petrochemical COD- 1400–1700 mg/l, BOD/ 78.97 min Electrode- Aluminum, electrolyte-Feþ2 solution, Inter-electrode COD- 51.23% Davarnejad et al.
wastewater (PW) COD- 0.4–0.6 gap- 3.00 cm, current density 68.7 mA/m2, pH- 3.06, H2O2/PW - (2014)
2.14 ml/l, and H2O2/Feþ2–4.99 M ratio.
EF Petrochemical COD- 1400–1700 mg/l, BOD/ 73.19 min Electrode- Iron, electrolyte-Feþ2 solution, Inter-electrode gap 3.00 COD- 66.85% Davarnejad et al.
wastewater (PW) COD- 0.4–0.6 cm, current density 59.7 mA/m2, pH- 2.67, H2O2/PW - 1.23 ml/l, (2014)
and H2O2/Feþ2–3.65 M ratio.
Journal of Environmental Management 272 (2020) 111057
M. Jain et al.
Fig. 6. Classification of constructed wetlands for wastewater treatment and their features.
It was observed that the presence of phytoplankton and zooplankton in
both CW systems did not allow oxygen deficiency or toxic conditions to
prevail.
Wallace et al. (2011) carried out the study of two full-scale CWs and
demonstrated a very high potential of SSF-CW for organic compounds
removal from oil refinery wastewater in cold climates. In order to free
the wastewater from iron, a cascade aerator was used before the CW.
The first CW system located in Casper, Wyoming, was operated at
temperatures as low as 35 � C and showed a 100% removal efficiency
for BTEX and gasoline-range organics. The second CW located in
Wellsville, New York, was operated at temperatures below 20 � C, and
it was found to remove 94% of the aniline and 93% of the nitrobenzene
with a high percentage of BTEX removal. This system also included
artificial aeration to prevent the freezing of water in VSSF-CW.
Stefanakis et al. (2016) used horizontal subsurface flow CWs
(HSSF-CWs) having a surface area of 6.5 m2 and a bed depth of 1 m filled
with gravel (grain size 2–3.2 mm) to treat groundwater contaminated
with phenols, benzene, m-cresol, etc. The flow rate was maintained
around 11 L/h, and Phragmites australis was planted to enhance the
performance of the CW. High removal efficiency of 99.8% and 97.7%
were observed for phenol and m-cresol, respectively, after ten days of
HRT. The removal of phenolic compounds did not affect the removal
efficiency of MTBE and benzene, which ascertained the versatility of
CWs. It was also found that the presence of phenolic compounds did not
have any toxic effects on the plants. Aerobic conditions in the top layer
of the bed facilitated the growth of microorganisms leading to biodeg­
radation, which was found to be the primary mechanism for the treat­
ment system.
Pardue et al. (2014) developed a pilot-scale CW system comprising of
three series, out of which two series consisted of four vertical subsurface
flow CWs (VSSF-CWs) and the other one consisted of four free water
surface CW. An oil-water separator was also attached as a preliminary
treatment. Pea gravel of size 5–10 mm and granitic gravel of size 20–30
mm was used as the substrate while Phragmites australis was the plant
used. Pardue et al. (2014) observed an O&G reduction ranging from
10
Journal of Environmental Management 272 (2020) 111057
69.3% to 98.4% after a retention time of 2–4 days. Additionally, a high
average removal efficiency (>85%) of metals, such as Zn, Ni, Fe, and
Mn, was also observed.
Seeger et al. (2011) used Phragmites australis planted HSSF-CWs (L �
B � H ¼ 5 m � 1.1 m � 0.6 m) with gravel substrate to treat benzene,
MTBE contaminated water. Temperature above 15 � C was found to be
favorable for the performance of the CWs. Maximum removal efficiency
for benzene, MTBE, and ammonia was found to be 99%, 82%, and 41%,
respectively. Microbial degradation was found to be the primary driving
force in contaminant removal.
Ranieri et al. (2013) used CWs (L � B � H ¼ 7.5 m � 4.8 m � 0.6 m)
having a surface area of 35 m2 and planted area of 15 m2 (Phragmites
australis and Typha latifolia) for BTEX (0.5 mg/L) removal at a flow rate
of 1 m3/day. The substrate comprised 0.1 m of clay soil (0.05 mm), 0.2
m of stones (5 mm), and 0.30–0.35 m of gravel (1.5 mm). The volume of
voids was calculated to be 1.56 m3, and the porosity of the overall
substrate was found to be 0.17. After 100 h of HRT, the overall BTEX
removal in the unplanted CW was found to be 46%, while the removal
efficiency increased up to 57% in the presence of Phragmites australis.
Al-Baldawi et al. (2013a) used Scirpus grossus planted HSSF-CWs (L
� B � H ¼ 1.8 m � 0.9 m � 0.9 m) to treat diesel contaminated
wastewater. Gravels of sizes ranging from 1 to 2 mm, 10–20 mm, and
20–50 mm were used as the substrate. The TPH removal efficiencies
obtained after 72 days was found to vary from 67% to 82%. Further­
more, a high removal efficiency of 100% and 75% were obtained for TSS
and COD, respectively. In another study, Al-Baldawi et al. (2014)
attained a removal efficiency of 72.5% after 63 days of HRT. Al-Baldawi
et al. (2013c) used Scirpus grossus planted SSF-CWs (L � B � H ¼ 0.3 m
� 0.3 m � 0.3 m) for treating synthetic diesel contaminated wastewater
and attained a TPH removal efficiency of 91.5%.
A detailed list of studies regarding the treatment of PRPP wastewater
using CW and their contaminant removal efficacy, including the
wastewater characteristics, operation conditions, flow types, and mac­
rophytes used, have been presented in Table 4. Based on various liter­
ature, the performance of CWs in terms of removal of BOD, COD, O&G,
 Table 4
Performance of constructed wetlands in treating PRPP wastewater.
Wastewater type Wastewater characteristics CW type CW Scale & Size HRT Flow rate Plant Removal efficiency References
M. Jain et al.

Refinery effluent – SSF Full scale – – Common reed Phragmites australis, COD-90%, O&G-72-100%, TN- Lakatos et al.
cattail (Typha angustifolia L.) 35%, TP- 40% (2014)
Refinery wastewater Turbidity- 18.3 NTU, BOD-20.4 mg/L, VSSF Lab scale-50 L Batch 10 d Batch Eichhornia crassipes (water hyacinth) Turbidity-91.5%, BOD5-94.6%, Agarry et al.
COD- 86 mg/L, O&G- 18.4 mg/L, TPH- fill COD-80.2%, O&G- 90.4%, TPH- (2018)
16.6 mg/L 92.6%
Petrochemical HSSF Lab scale-70x40 � 30 90 d 6 L/day a-Typha latifolia (Cattail) b-Pragmites BOD, COD, TSS-90-95% Sudarsan et al.
effluent cm and a slight slope of australis(Reed) Phenolic compounds- 65–90% (2016)
<1%
Oil produced water COD- 401 mg/L/BOD- 31.9 mg/L/ SSF Pilot scale- 60x15 � 3d 30,000 L/day Common reed Reed1 (30,000 L/day): BOD- Ji et al. (2002)
O&G- 24.7 mg/L, TKN- 11.7 mg/L. 0.6 m slope ¼ 2% and 18,000 L/ 80%, COD- 67%, O&G: 78%,
day TKN: 75%
Reed2 (18,000 L/day): BOD-
89%, COD- 81%, O&G: 89%,
TKN: 81%
Refinery wastewater TN-15.6 mg/l,TP-0.6 mg/l,COD-142.8 FW Lab scale-75 L 35 d Batch fill Perennial grasses [Geophila herbacea COD-52-67%, TPH-40-55%, TP- Li et al. (2012)
mg/l,TPH-1720 mg/l container D ¼ 80 cm, O Kumtze (GHK), Lolium perenne CV. up to 56%, TN-up to 60%
H ¼ 100 cm Caddieshack (LCC), Lolium perenne
Topone (LPT) and Lolium perenne L.
(LPL)]
Secondary refinery Phenol- 0.053 μg/L, O&G- 6.78 mg/L, VSSF Lab scale H ¼ 0.88m, 180 d 11,520 L/day Typha latifolia and unplanted Unplanted: COD- 66%, TPH- Mustapha
wastewater TPH- 6.2 mg/L, COD- 200–600 mg/L, D ¼ 0.22m microcosm CW 58%, O&G- 44%, Phenol- 91%, et al. (2018b)
TSS- 70–110 mg/L TSS- 55%
Planted: COD- 91%, TPH- 99%,
O&G- 80%, Phenol- 100%, TSS-
88%
Petroleum Refinery TSS-60.8 mg/L, BOD- 95.2 mg/L, COD- VSSF þ Lab scale VSSF- VSSF-48 h, 19.92 L/day Typha latifolia (HSSF þ VSSF) Turbidity-97%, Mustapha and

11
Wastewater 164 mg/L, NHþ4 -N - 1.8 mg/L, NO3 N- HSSF circular D ¼ 47 cm, H and HSSF- BOD5-94%, COD-88%, TP-78%, Bruggen
1.6 mg/L, TP-4 mg/L ¼ 55 cm HSSF- LxBxH 148 h TN-85%, NHþ 4 -N-84%, NO3 N- (2018)
¼ 110 cm � 70 cm � 89%
40 cm
Phenol and Phenol- 6.39 mg/L, m-cresol-0.895 mg/ HSSF Pilot-scale 3 units 10 d 264 L/day 2 common reeds (Phragmites Phenol- 99.8%, m-cresol- 97.7% Stefanakis
petroleum L LxBxH ¼ 5.9 m � 1.1 australis) þ unplanted et al. (2016)
derivatives in m � 1.2 m
groundwater
TPH effluents 0.25% diesel HSSF Pilot scale LxBxH ¼ 63 d Batch Scirpus grossus three rhizobacteria Without rhizobacteria- TPH-72%, Al-Baldawi
1.8 m � 0.9 m x0.9m strains (Bacillus aquimaris, Bacillus With rhizobacteria- TPH-84% et al. (2017)
vol. ¼ 500 L anthracis, and Bacillus cereus)
Synthetic diesel oil COD-31.7 mg/L, Diesel range organics- VSSF þ Lab Scale- VSSF- VSSF-4.85 VSSF- Phragmites australis HSSF- COD- >32%, Diesel range Mustapha
refinery 246.4 mg/L, benzene- 0.2 mg/L, HSSF LxBxH ¼ 0.6 m � 0.4 d HSSF- unplanted organics->97%, Benzene->96%, et al. (2018a)
wastewater toluene- 0.06 mg/L, ethyl benzene- m x0.8m, HSSF- 2.1 d Toluene->93%, Ethyl benzene-
0.09 mg/L, m/p- xylene-0.06 mg/L, o- LxBxH ¼ 0.6 m � 0.4 >96%, m/p-xylene->86%, 0-
xylene- 0.06 mg/L m x 0.35m xylene->98%
Synthetic Diesel concentration 17400 mg/L SSF Lab scale-L ¼ 72 d Batch Scirpus grossus TPH-91.5% Al-Baldawi
wastewater with B–
–H¼30 cm 7 L et al. (2013b)
diesel
Synthetic Diesel concentration of 0.25%. HSSF Pilot-scale LxBxH ¼ 63 d Scirpus grossus After 63 days-TPH from water- Al-Baldawi
wastewater 180 cm � 90 cm x 90 72.5%, TPH from sand- 59% et al. (2014)
cm
Synthetic Diesel conc. 0.1%(a), 0.2%(b), 0.25% HSSF Pilot scale LxBxH ¼ 72 d Scirpus grossus a-82%, b-71%, c-67% Al-Baldawi
wastewater (c) 180 cm � 90 cm �90 et al. (2013a)
cm
Synthetic water Diesel concentrations (1%, 2%, and 3%) SSF, FSF Pilot scale L ¼ 72 d Scirpus grossus Avg TPH removal- SSF-91.5%, Al-Baldawi
B–
–H¼30 cm FSF-80.2% et al. (2013c)
Crude oil Cd- 3.21 mg/L, Cr- 11.48 mg/L, Pb, FW Lab Scale-LxBxH ¼ 50 60 d Duckweeds (L. paucicostata) After 60 days- Cd-32.45%, Cr- Ekperusi et al.
0.39 mg/L, V- 3.64 mg/L. cm � 50 cm x 10 cm 13.76%, Pb-41.03%, V-26.37% (2019)
(continued on next page)
Journal of Environmental Management 272 (2020) 111057
 Table 4 (continued )
Wastewater type Wastewater characteristics CW type CW Scale & Size HRT Flow rate Plant Removal efficiency References

Crude oil- COD- 1324 mg/L, BOD- 475 mg/L, FW Lab Scale- 20 L tank 42 d Batch Plant-T.domingensis, Leptochloa T. domingensis þ bacteria- Total Rehman et al.
M. Jain et al.

contaminated Total hydrocarbon- 304 mg/L fusca, bacteria- Bacillus subtilis, hydrocarbon (95%), COD (90%), (2019)
wastewater Klebsiella sp., Acinetobacter Junii, and BOD (93%)
Acinetobacter sp.
Groundwater Benzene- 13 mg/L, MTBE- 2.2 mg/L HSSF Pilot-scale LxBxH ¼ 6d 144 L/day Common reed (Phragmites australis) Unplanted (HSSF): Benzene-33%, (Z. Chen et al.,
contaminated with combined 5.0 m � 1.1 m � 0.6 þ Unplanted MTBE: 33% 2012)
benzene and with FW Reed (HSSF): Benzene- 24%–
MTBE 100%, MTBE- 16%–93%
Reed (FW): Benzene- 22%–100%,
MTBE- 8%–93%
Municipal Bisphenol A (8.8 μg/L) (BPA) and HSSF Pilot scale L ¼ 9 m, B 1.8 d 3500 L/day Phragmites australis(a); Heliconia Plant a: BPA- 70.2%, NP- 52.1% Toro-V� elez
wastewater nonylphenols (1671 μg/L) (NP) ¼ 3 m, H ¼ 0.25m psitacorum(b); unplanted(c). Plant b: BPA- 73.3%, NP- 62.8% et al. (2016)
Plant c: BPA- 62.2%, NP- 25.3%
Heavy oil-produced COD- 390 mg/L, BOD- 32 mg/L, O&G- FSF Pilot scale L ¼ 75m, B Bed 1–15 Bed 1–18,750 Common reed (Phragmites australis) Reed 1: BOD5- 88%, COD- 80%, Ji et al. (2007)
water 20 mg/L, TKN- 11.6 mg/L ¼ 7.5m, H ¼ 0.25m d Bed L/day, Bed O&G- 93%, TKN:86%
2–7.5 d 2–37,500 L/ Reed 2: BOD5- 77%, COD- 71%,
day O&G- 92%, TKN- 81%
Benzene, MTBE, Benzene- 20 mg/L, MTBE- 3.7 mg/L, HSSF and Pilot scale- 5 m (L) � 3d 287 L/day Phragmites australis HSSF: Benzene- 53%, MTBE- Seeger et al.
NHþ4 -N NHþ4 -N- 57 mg/L FW 1.1 m (W) � 0.6 m (H) 33%, NHþ 4 - N-39% (2013)
contaminated FW: Benzene- 98%, MTBE- 78%,
water NHþ4 - N-74%
Benzene, MTBE, Benzene- 20 mg/L, MTBE- 3.7 mg/L, HSSF and Pilot scale- 5 m (L) � 144 L/day Phragmites australis HSSF: Benzene-81%, MTBE -17%, Seeger et al.
NHþ4 -N NHþ4 -N- 45 mg/L FW 1.1 m (W) � 0.6 m (H) NHþ4 -N 54% (2011)
contaminated FW: Benzene-99%, MTBE -82%,
water BTEX-41%
Synthetic BTEX- 0.5 mg/L HSSF Pilot Scale- 3 m (L) � 5 100 h Phragmites australis, Typha latifolia, 46% (unplanted field) - 57% Ranieri et al.
wastewater m (W) � 0.6 m (H) unplanted (Phragmites field) (2015)

12
Petroleum- HSSF and Pilot scale 5472 L/day willows (Salix), reed (Phragmites), Benzene-80%, total BTEX- 88% Bedessem
Contaminated VSSF bulrush (Scirpus), rush (Juncus), and et al. (2007)
Groundwater dogwood (Corn
Synthetic diesel- total petroleum hydrocarbons TPH- HSSF Pilot Scale- 1.8 m (L) 72 d Scirpus grossus TPH- 81.5%–66.6% Al-Baldawi
contaminated 0.4–1.18 mg/L � 0.9 m (W) � 0.9 m et al. (2015)
water (H)
Journal of Environmental Management 272 (2020) 111057
M. Jain et al.
Fig. 7. Plots showing variation in removal efficiency of a) CWs in removing various contaminants, b) different types of CWs in removing COD, the effect of c) flow
rate on COD removal, and d) plants on organics removal from petroleum refinery and petrochemical plants wastewater. Data from Table 4.
total phosphorus (TP), total nitrogen (TN), and other organic com­
pounds (MTBE, BTEX, Phenol, etc.) have been depicted in Fig. 7a.
4.2.1. Role of flow pattern and type of CW
The flow pattern of wastewater is one of the determining factors for
the performance of wetlands. Among the various single CW systems used
for the treatment of PRPP wastewater, it was found that HSSF-CWs
exhibited higher removal efficiency (Fig. 7b). HSSF-CWs have shown a
slightly better removal efficiency when compared to VSSF-CWs because
of the large surface area and more exposure to atmospheric oxygen.
Furthermore, a continuous flow with a low gradient can efficiently
remove BOD, COD, and TSS (Vymazal, 2013). Also, the intermittent
supply of wastewater, which is better suited for the proper functioning
of VSSFs, accounted for the slightly less COD removal. VSSF-CWs are
more efficient than HSSF-CWs, in terms of nitrogen removal because
conditions favoring nitrification prevail in this system. However, these
systems are subjected to clogging and are inefficient in the removal of
solids. It was observed that when HSSF-CWs were combined with
VSSF-CWs, the performance of the hybrid system was better as
compared to the single system CWs (Fig. 7b). Such enhancement in
performance of the hybrid CWs may be because the advantages of both
HSSF-CWs and VSSF-CWs nullify their individual drawbacks. Vymazal
(2013) reported an increased COD removal efficiency ranging from 10 to
30% when the two systems were combined. The COD reduction ach­
ieved was greater than 90%, which indicated the higher efficiency of
13
Journal of Environmental Management 272 (2020) 111057
these processes over other CWs (Fig. 7b). FSF-CWs provide an average
removal efficiency of 80% (Al-Baldawi et al., 2013c; Ji et al., 2007). Li
et al. (2012) reported lower COD removal efficiency for FWs, which can
be attributed to the lack of substrate. The flow rate in CWs also played a
significant role in the removal of COD, as observed in Fig. 7c. It is
evident that the performance of the CW deteriorates with an increased
flow rate. When the flow rate was kept below 20 L/day, COD removal
efficiency of around 90% was achieved. However, when the flow rate
was increased, the COD removal kept on decreasing (Ji et al., 2002,
2007; Mustapha et al., 2018b; Mustapha and Bruggen, 2018; Sudarsan
et al., 2016). It may be attributed to the less contact time available to
wastewater at higher flow rates.
4.2.2. Types and role of substrate
Apart from microbes and plants, the substrate of the wetland is also
an integral factor for the removal of contaminants from wastewater. The
most commonly used natural substrates used in CWs are gravel, sand,
zeolite, minerals, limestone, and volcanic rocks (Wang et al., 2020). The
substrates act as the base for all biotic (phytoremediation, biodegrada­
tion) and abiotic (sorption, volatilization, hydrolysis, redox reactions)
functions of the wetlands. The substrate is decided according to its
capability to support the natural growth conditions required for the
biological species (bacteria, plants, fungi, etc.) and also its ability for
adsorption and retention of pollutants in the small pores (filter media).
The sand was found to be more efficient in the removal of TP and TN as
M. Jain et al.
compared to gravel (Wang et al., 2020). Sandy soil exhibited better
performance as compared to sandy clay. Zeolite has shown excellent
efficiency in terms of the removal of TP and ammonia. It is also rich in
micro-pores and macro-pores, which facilitates the adsorption of various
pollutants (Wang et al., 2020). Sometimes an upper layer of soil is also
provided for plant root stabilization. Various substrates have different
interactions with the wastewater due to their diverse chemical compo­
sitions, surface/charge ratio, porosity, hydraulic properties, mineral­
ogical compositions, and sorptive properties. Large pore spaces provide
more surface area for microbial growth, and higher hydraulic conduc­
tivity, while the pH of media affects the plant and biofilm growth
(Dordio and Carvalho, 2013). Ranieri et al. (2013) used an HSSF-CW
with a substrate layer of clay soil, stones, and gravels for the treat­
ment of BTEX solution and obtained a removal efficiency of around 46%
in the absence of macrophytes. The use of medium size gravel (10–20
mm), fine gravel (1–5 mm), and fine sand (1–2 mm) in a CW planted
with Scirpus grossus resulted in 66.6%–81.5% removal of total petroleum
hydrocarbon (TPH) from water contaminated with different concen­
tration of diesel (Al-Baldawi et al., 2015).
4.2.3. Role of various species of macrophytes and microorganisms
The removal of nutrients and organic contaminants in wetlands de­
pends mostly on the type of plant and microbial species. Many re­
searchers studied the effect of different plant and microbial species on
treatment efficiencies of CWs. The efficiency of CW in the presence and
absence of plants was compared by Mustapha et al. (2018b). At the same
time, Mustapha and Bruggen (2018) observed the alteration of the
performance of the CW using different plant species. The presence of
plants facilitated the phytoremediation process and enhanced the
removal efficiencies of various contaminants (Fig. 7d). Sudarsan et al.
(2016) performed multiple trials for the treatment of petrochemical
industry wastewater using Typha latifolia and Phragmites australis and
achieved removal efficiencies in the range of 90–95% for BOD, COD, and
TSS, while the removal efficiency of phenolic compounds was found to
be in the range of 65–90%. It was found that Typha latifolia performed
better than Phragmites australis for the removal of phenolic compounds.
Additionaly, Sudarsan et al. (2018) had also reported that the CW
containing Typha latifolia exhibited better removal of BOD and COD as
compared to a CW containing Phragmites australis The CW containing
Phragmites australis exhibited around 85% BOD removal and 89% COD
removal, whereas the CW containing Typha latifolia exhibited around
90% BOD removal and 93% COD removal after 24 h of the study
(Sudarsan et al., 2018). Ranieri et al. (2013) observed BTEX removal
from HSSF-CWs planted with Typha latifolia, Phragmites australis, and
one unplanted CW at a flow rate of 1 m3/d. Phragmites australis planted
CW field removal was 5% higher than the Typha latifolia planted field
and 23% higher than the unplanted field. Phytoremediation is not only
confined to the use of grasses or weeds, but different kinds of cereals are
also capable of removing contaminants from wastewater. Baoune et al.
(2019) used Zea mays inoculated with Streptomyces sp. for removing
petroleum hydrocarbons, i.e., phenanthrene, pyrene, and anthracene
from petroleum crude contaminated soil, and achieved the removal ef­
ficiency of 61%, 59%, and 46%, respectively. Hairy tomato roots can
also be used for phytoremediation of phenols by exploiting their basic
peroxidase isoenzymes (Gonza �lez et al., 2006). However, the tolerance
capacity of the plant for different contaminants should be explored for
selecting the appropriate species (Zhang et al., 2010). Guittonny-Phi­
lippe et al. (2015) assessed the tolerance of five helophyte species in
water containing a mixture of metals and organic pollutants and sug­
gested the use of species growing at close vicinity of the industrial dis­
charges for phytoremediation. In the case of the submerged
macrophytes, the biofilms present on their roots also affect the perfor­
mance of wetlands. Biofilms attached to the submerged macrophytes are
positively correlated to PAH (pyrene & phenanthrene) and TN removal,
and also help to regulate the nitrogen cycle, thereby reducing their risk
of contamination in other organisms and environment (Qin et al., 2019).
14
Journal of Environmental Management 272 (2020) 111057
Recently, FWs have gained importance in the PRPP wastewater treat­
ment due to their low complexity. Free-floating plants, such as Lemna
paucicostata (duckweeds), Eichhornia crassipes, Typha domingensis,
perennial grass species, such as Geophila herbacea, Lolium perenne, etc.
are commonly used for removal of contaminants from oily wastewater.
Ekperusi et al. (2019) used duckweed for simulating crude oil spill sites
for the remediation of heavy metal by using an artificial FW and
observed an increase in the heavy metal removal potential of plants.
Plant configuration can be decided based on the local climate, nutri­
tional level of the wastewater, etc. The various plants used for treating
petrochemical wastewater in CWs have been shown in Table 4.
Microorganisms also play a vital role in the removal of organics as
they degrade the complex compounds into simpler non-toxic forms.
Different types of bacteria and fungi are present in the rhizosphere of the
plant root system in CWs. Fester (2013) observed substantial arbuscular
mycorrhizal fungi colonization in plant roots of Phragmites australis
treating groundwater contaminated with benzene, MTBE, and ammonia.
Bioaugmentation can assist wetlands in improving their removal effi­
ciency by aiding the synergistic effect on plants. Bioaugmentation using
Typha domingensis with three phenol-degrading bacterial strains, Aci­
netobacter lwofii, Bacillus cereus, and Pseudomonas sp., can provide
enhanced phenol removal varying from 0.146 g/m2/day to 0.166
g/m2/day (Saleem et al., 2018). Wang et al. (2019) reported the increase
in the population of oil-degrading bacteria and soil respiration with the
rise in oil dosage in soil. Furthermore, PAH degrading bacteria were
found to be more effective for oil degradation than alkane degrading
bacteria (Wang et al., 2019). El-Naas et al. (2014) and Fahid et al. (2020)
investigated the activity of bacteria, such as Acinetobacter sp. BRRH61,
Bacillus megaterium RGR14, Acinetobacter iwoffii AKR1, and Pseudony­
mous putida in CWs to treat diesel contaminated wastewater and pe­
troleum refinery wastewater. The presence of bacteria not only
improved the efficiency of the system but also enhanced plant growth.
Supplementing the CWs with dephosphorization and nitrogen removing
bacteria can further enhance the removal of TN and TP from the
wastewater (Ji et al., 2020).
4.2.4. Role of dissolved oxygen
DO in the wastewater plays a pivotal role in the performance of the
CWs. The DO primarily influences the microbial degradation of organic
contaminants in the CW. Although microbial degradation can be both
aerobic and anaerobic, aerobic degradation is preferred in the treatment
of PRPP wastewater (Al-Baldawi et al., 2013d). It has been reported that
higher oxygen content facilitates the degradation of organic compounds
(Liu et al., 2016). Since the organic compounds tend to use up most of
the available DO, there is little DO left for removal of ammonia and TN.
Establishing aerobic condition can significantly improve the COD,
ammonia, and TN removal (Li et al., 2014a). However, denitrification is
also essential for complete nitrogen removal, and denitrification re­
quires anaerobic conditions. As a result, proper distribution of DO is
required so that aerobic and anaerobic zones are created, which can
facilitate the growth of different bacteria (Li et al., 2014a). In order to
induce both aerobic and anaerobic conditions and achieve a proper
distribution of DO, artificial aeration is carried out in the CWs. It en­
hances both nitrification and denitrification, leading to the improved
overall performance of the system. Artificial aeration is usually achieved
by air pumps and air blowers. In VSSF-CWs and HSSF-CWs increased
removal of organic matter, TN and ammonia were obtained when arti­
ficial aeration was provided (Al-Baldawi et al., 2013d; Dong et al.,
2012).
4.3. Removal of contaminants present in PRPP wastewater and their
mechanism
The main concern associated with the effluent coming out of the
PRPPs is the complex organic compounds that need to be removed for
preventing toxicity of wastewater. CWs are believed to be an effective
M. Jain et al.
Fig. 8. Mechanism of contaminant removal from petroleum refinery and petrochemical plants wastewater using constructed wetlands.
technique to get rid of these recalcitrant components. They are efficient
in transforming complex organic compounds into simple non-toxic
products. The main feature of the CW system is that the pollutants are
removed via multiple pathways/mechanisms. Physical removal, such as
adsorption, sedimentation, volatilization, and chemical processes, such
as oxidation, reduction, photolysis (in FWS), etc. are essential pathways.
Biological processes, namely nitrification, denitrification, microbial
degradation, rhizofiltration, and also phytoremediation, lead to com­
plete bioremediation of contaminants (Fig. 8). Rhizofiltration involves
the filtration of toxic components through the roots (Rahman and
Hasegawa, 2011). Phytoremediation consists of processes, such as
phytoextraction, phytostabilization, phytovolatilization, phytode­
gradation, and phytodesalination (Ali et al., 2013). In phytoextraction,
pollutants are absorbed by roots, transported, and stored in the upper
parts of the plants. Pollutants are stabilized into the rhizosphere by
reducing its mobility through phytostabilization. The organic hydro­
carbons are absorbed from the soil and converted to a less toxic, volatile
form in plants and are subsequently released into the atmosphere
through phytovolatilization. However, during phytovolatilization, con­
taminants are transferred from the wastewater to the atmosphere
instead of degrading them. Hence, it should be avoided in highly
populated areas (Padmavathiamma and Li, 2007). Phytodegradation
reduces the toxic pollutants into less toxic components by using the
plant enzymes.
Literature suggests that aerobic microbial degradation is a useful
technique for MTBE removal (Thullner et al., 2018). Studies have shown
that MTBE is primarily volatilized from the plant with a minimal amount
detected in plant tissues (Yu and Gu, 2006). Furthermore, MTBE is
sensitive to photo-oxidation in the atmosphere (Reiche et al., 2010).
Stefanakis et al. (2016) compared two planted HSSF-CW (both with reed
grass) and one unplanted HSSF-CW and found higher removal rates for
MTBE and Benzene in planted CW and around complete removal of
phenols in all CWs. Seeger et al. (2013) investigated the efficiency of two
CWs and one plant root mat (FW) and observed that the FW achieved the
highest removal for benzene, MTBE, and ammonium-nitrogen. The
removal of MTBE was found to be lower than that of BTEX in
petroleum-contaminated groundwater, which may be due to lower
biodegradability of MTBE as compared to BTEX constituents (Bedessem
15
Journal of Environmental Management 272 (2020) 111057
et al., 2007). In another study, similar results were obtained for BTEX
removal, and also around 5–10% higher removal of toluene was
observed compared to other BTEX compounds, which may be due to the
higher volatile nature of toluene (Ranieri et al., 2015).
For most of the hydrocarbons, degradation is the main pathway that
predominantly occurs inside the plant or in the rhizosphere (Yin et al.,
2011). Additionally, for volatile organic compounds, such as BTEX,
trichloroethene, vinyl chloride, and carbon tetrachloride, having Hen­
ry’s constant (KH) > 10 atm m3 water m 3 air, phytovolatilization also
acts as a vital reduction pathway (Rozaimah et al., 2020). Phenols and
PAH can also be removed by sorption through plant roots (Poerschmann
and Schultze-Nobre, 2014). Al-Baldawi et al. (2015) showed that plants
S. grossus could uptake TPH (Phytoextraction), and the rhizobacteria
degraded it in sub-surface batch CW (biodegradation). Salmon et al.
(1998) found that hydrocarbon removal in the artificial wetland was
about 90%, in which biodegradation accounted for 60%, phytovolatili­
zation accounted for more than 25%, while the remaining 10% was
removed by sorption. Ranieri et al. (2013) found that the BTEX removal
in pilot-scale HSSF-CW was primarily through volatilization and
biodegradation played a secondary role. TPH, phenol, O&G, and TN
have good translocation ability in plants and were removed mainly by
phytoextraction (Mustapha et al., 2018b). Other organic matters, which
are represented in terms of COD and BOD in the PRPP wastewater, are
removed by a combination of physical, chemical, and biological pro­
cesses. In FSF-CWs, photochemical reactions, sorption, reduction,
oxidation reactions, and biodegradation are the main pathways for
organic matter decomposition. Mishra and Maiti (2017) found that
water hyacinth (Eichhornia crassipes) can be instrumental in the phy­
toextraction of organics and heavy metals from wastewater.
Metals removal from PRPP wastewater is also a major concern in
conventional treatment systems. However, the removal of metals is
easily attained in CWs due to the presence of multiple mechanisms. The
media adsorbs and filters the pollutants from the wastewater stream and
plants help in the translocation of contaminants from the media leading
to subsequent contaminant removal from the treatment system.
Furthermore, the elemental composition of the media, such as Ca, Al, Si
oxides, etc. may act as a catalyst for the removal processes. Additionally,
processes, such as reduction, oxidation, sedimentation, flocculation,
M. Jain et al.
precipitation, and ion exchange, also occur simultaneously in CWs
(Batool and Saleh, 2019). Mustapha et al. (2018b) used VSSF-CW for
removing heavy metals from secondary treated refinery wastewater and
found that Cu, Cr, Zn, Pb, Cd, and Fe were accumulated in the stem,
leaves, and roots of the plants with maximum accumulation in roots.
Additionally, the substrate helps to reduce the mobility of metals in the
rhizosphere (Lesage, 2007). The floating aquatic plants uptake metals
through their roots, while the whole plant body acts as the uptake
pathway for submerged plants (Rahman and Hasegawa, 2011).
TSS is primarily removed by interception and sedimentation in the
wetland media. In HSSF-CW, its maximum removal is achieved near the
inlet zone, and gradually the removal rate decreases. In FSF-CWs,
interception plays a minor role, while the major part of the TSS is
adsorbed on the macrophyte surface. Ammonia can be removed by
physical processes, such as filtration, adsorption, and also by microbes
involving aerobic degradation. Since the removal of TP primarily de­
pends on the adsorption by the media, a media with higher sorption
capacity is preferred (Zhaia et al., 2011). Furthermore, phosphorus can
be retained in the roots of the macrophyte population (Mustapha et al.,
2018b).
4.4. Modification of CW systems for enhanced performance
The salient features in the modification of single wetland systems
include modification of flow, implementation of artificial aeration, and
use of substrate supplements (Ji et al., 2020; Valipour and Ahn, 2016).
Tidal flow works on the batch principle, where the CW is flooded peri­
odically multiple times. The primary attribute for this process in the high
oxygen transfer efficiency. In order to increase the flow path and to
create sequential aerobic, anoxic, and anaerobic conditions, vertical
baffles along the width of the CW are provided. Step feeding of waste­
water in a CW is carried out by providing multiple inlet points to give the
entire area of the CW a uniform loading (Valipour and Ahn, 2016).
Artificial aeration is predominately carried out to induce aerobic
conditions. The position of the aerators has been reported to influence
the performance of the system. Researchers achieved better removal of
COD and TN when they employed middle aeration to achieve uniform
oxygen distribution (Dong et al., 2012; Liu et al., 2013b). Wang et al.
(2015) observed better performance in the case of middle aeration as
compared to surface aeration and bottom aeration in a VSSF-CW. Re­
searchers reported that intermittent aeration facilitated better removal
of TN in HSSF-CW and VSSF-CW because it provides both aerobic and
anaerobic conditions for efficient nitrification and denitrification.
Continuous aeration facilitated better removal of ammonia, but the
oversaturation of the CW with DO inhibited the removal of nitrate and
TN (Ji et al., 2020). Artificial aeration stimulates the activity of het­
erotrophic bacteria even in a cold climate to enhance the performance of
the CWs. Fan et al. (2013) found that a combination of intermittent
aeration combined with step feeding resulted in the best removal of both
nitrate and ammonia. Artificial aeration has also been instrumental in
treating PRPP wastewater in cold climates, where the low temperature
severely affects the working of the CWs. Wallace et al. (2011) incorpo­
rated artificial aeration in CWs and achieved a removal efficiency of
100%, 94%, and 93% for BTEX, aniline, and nitrobenzene at tempera­
tures below 20 � C. It can be observed that if proper aeration is sup­
plied, then the performance of the single system CWs can be significantly
enhanced.
Apart from the regular substrates that are used in CWs, as mentioned
in Sect. 4.2.4, various agricultural or industrial wastes, such as oyster
shells, alum sludge, woodchip, plant waste, fly ash, slag, etc. can also be
used as substrates. Among the plant wastes, various plant by-products
generated during plant processing, such as coconut dust, rice husk,
reed leaves, etc. were used. Artificial materials, such as ceramics, acti­
vated carbon, cement clicker, synthetic fibers, modified clays, and
recycled concrete, have also been used in CWs to evaluate the perfor­
mance of the system (Wang et al., 2020). Activated carbon showed
16
Journal of Environmental Management 272 (2020) 111057
promising removal efficiency when it comes to the removal of TP, TN,
and ammonia (Fu et al., 2017). However, synthetic fibers showed poor
removal efficiency of ammonia (Y. Chen et al., 2012). The effectiveness
of these systems primarily depends on the adsorption capacity of these
substrates. Adequate research needs to be done to identify the best
substrate for the treatment of petrochemical wastewater in CWs.
Hybrid CWs are improvised in many places by using the combination
of different CWs for an enhanced level of performance. Different
multistage CW, such as VF-VF-HF-CWs, VF-HF-VF-CWs, HF-VF-FH-CWs,
and HF-HF-VF-CWs, have been used to improve the efficiency of the
process. Often two VSSF-CWs are placed atop each other to create
anaerobic conditions. These systems usually employ one down-flow
VSSF and one up-flow VSSF connected at the bottom. Since the final
outflow of the water is from the top of the second bed, both the beds are
saturated, leading to anoxic conditions. The FSF-CW has also been
augmented with HSSF-CWs and VSSF-CWs. This process may not be as
efficient as a combination of VSSF-CWs and HSSF-CWs or multistage
CWs, but it increases the overall performance of the single wetland
system (Vymazal, 2013). These modifications were not only instru­
mental in the removal of COD, but also enhanced the removal efficiency
of ammonia, TN, and TP. However, most of the applications of these
CWs have been limited to the treatment of municipal sewage, waste­
water from food industries, aquaculture, and tannery. Their perfor­
mance in the remediation of petrochemical wastewater has not been
thoroughly studied.
5. Issues and concerns
Most of the studies in this field involving CWs have been carried out
for a selected number of organic contaminants or with synthetic
wastewater, while real-life PRPP wastewater contains numerous organic
contaminants with pronounced toxicity. Furthermore, there exist many
ambiguities regarding the shock loading capacity of wetlands concern­
ing the variability of the PRPP wastewater. In order to be implemented
at an industrial level, CWs must be able to bear continuous variations in
influent. As a result, proper designing and planning are required to cater
to the influent water quality and quantity from various industries.
Denitrification and nitrification are essential steps for TN removal, and it
is greatly influenced by the presence of DO. Proper TN removal is not
achieved due to the poor control of DO. This drawback can be addressed
by providing proper aeration or distribution of DO in the system (Jiz­
heng et al., 2019). The performance of CWs in a cold climate is another
concern because of the freezing of water, and the low temperature may
not be suitable for the proper growth and performance of the microor­
ganisms. Concerning these problems, various aeration techniques have
been used. However, further research is needed in this area to
completely eradicate this drawback (Rozema et al., 2016). Additionally,
media porosity and clogging are other factors influencing the perfor­
mance of the CW for a long-term period. Porosity is affected by the
solids, root elongation, and attached biofilm growth. Zidan et al. (2015)
studied the effect of different types of media for CW and found that after
218 days of operation of CW, porosity decreased by 16.94% for gravel
media, 12.33% for rubber media, and by 9.01% for plastic media. It was
found that plastic media performed better than the other two media in
the removal of COD, BOD, and TSS and also showed more resistance to
clogging. However, Al-Isawi et al. (2015) observed that clogging of
media due to diesel spills did not severely affect the contaminant
removal. As a result, a long term assessment of porosity of the soil and
contaminant removal is required.
Phytotoxicity is a matter of concern, that is required for examining
the tolerance levels of plant species for different concentrations of
contaminants. Al-Baldawi et al. (2013a) used an HSSF-CW planted with
Scirpus grossus species for the treatment of diesel in water and found that
this plant can remove diesel, only up to a certain concentration level,
above which the removal efficiency of wetlands decreases. In a similar
study, Wang et al. (2014) found that Polygonum orientale was intolerant
M. Jain et al.
for phenol above a concentration of 100 mg/L. These issues have a
negative impact on the performance of CWs and need to be addressed
while designing. Generally, a single bacterial strain is not sufficient for
the complete remediation of petrochemical contaminants (Singh and
Borthakur, 2018). As a result, a microbial consortium or coupling of
bacteria and fungi is required for treatment (Singh and Borthakur,
2018). Microbial processes are affected by root exudation of oxygen and
organics, which may be affected by photosynthesis (Lünsmann et al.,
2016). The diurnal variations in photosynthesis and the release of oxy­
gen in CWs need to be explored more to bring out the maximum effi­
ciency of CWs. Furthermore, the reuse of CW effluent for irrigation is
still a topic of research, and analysis of contamination in the soil
resulting from the reuse of CW effluent needs to be carried out carefully.
However, the most challenging attribute about the CWs is the require­
ment of a vast area for their establishment. Many developing countries
do not have large spaces available for the accommodation of these
wetlands, which is a significant challenge for this efficient technique.
6. Summary of findings
In the present review, we have demonstrated the global challenges
concerning the management of PRPP wastewater, in emphasizing
environmental impact and its remediation technologies. It was found
that various components of PRPP wastewater exceeded the permissible
limits set by USEPA and the WBG. The PRPP wastewater of multiple
regions was found to be characterized by high concentrations of BTEX,
Phenol, MTBE, etc. which may pose a threat to all kinds of living or­
ganisms. Subsequently, tremendous stress on research concerning the
remediation of PRPP wastewater is prioritized in the arena of environ­
mental engineering. Various studies of remediation of PRPP wastewater
by conventional treatment technologies focused on the reduction of
COD; however, the remediation of toxic organic compounds have not
been provided significant attention. Furthermore, a considerable
amount of oily sludge is produced, which is an added drawback to many
conventional biological treatment processes. Among the established
advanced treatment techniques, AOPs were efficient in terms of the
removal of recalcitrant organic compounds, but they are not as
economical as that of the CWs. CWs were found to overcome the limi­
tations of other processes in terms of treating PRPP wastewater, since
they were not only able to remove COD, ammonia, phosphate, nitrate
but also were quite efficient in the removal of PAHs, BTEX, phenols, and
other recalcitrant organic compounds without producing any significant
amount of sludge. Such efficiency of CWs is attributed to the various
mechanisms, such as phytodegradation, phytovolatilization, phytosta­
bilization, microbial degradation, rhizofiltration, sorption, substrate
filtration, etc., which occur simultaneously. The type of flow was found
to vary the performance of the constructed wetlands. HSSF-CWs pro­
vided better performance when compared to other single system CWs.
Often the CW systems were provided with aeration or arranged in a way
to provide both aerobic and anaerobic conditions for efficient removal of
nutrients. Middle aeration was found to be the most effective in VSSF-
CWs. Planted CW systems showed considerable improvement in treat­
ment when compared to unplanted CW systems. Typha latifolia and
Phragmites australis were found to be the most efficient in terms of
treating PRPP wastewater. The performance of the single CW systems
can be further enhanced by providing different flow patterns, artificial
aeration, and modification of the substrate. Hybrid CWs further negate
few drawbacks of single CW systems and provide excellent treatment.
This paper opens various avenues for the use of CWs for the treatment of
PRPP wastewater by providing insights into various modifications of the
existing CWs and the role of operating parameters. This review can also
catalyze the research involving proper modifications of CW and opti­
mization of the operating conditions, thereby providing a breakthrough
in the field of PRPP wastewater treatment.
17
Journal of Environmental Management 272 (2020) 111057
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
M.Jain and A. Majumder are grateful to the Indian Institute of
Technology Kharagpur, India, for financial support.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jenvman.2020.111057.
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