Bioresource Technology 355 (2022) 127263

Contents lists available at ScienceDirect

Bioresource Technology
journal homepage: www.elsevier.com/locate/biortech

Review

Current technologies and future perspectives for the treatment of complex

petroleum refinery wastewater: A review
Bhaskar Narayan Thorat a, Ravi Kumar Sonwani a, b, *
a
Department of Chemical Engineering, Institute of Chemical Technology, Mumbai–Indian Oil Odisha Campus, Bhubaneswar, Odisha 751013, India
b
Department of Chemical Engineering, Indian Institute of Petroleum and Energy (IIPE), Visakhapatnam, Andhra Pradesh 530003, India

H I G H L I G H T S

• Petroleum refinery wastewater adversely affects human beings, animals, and ecosystems.
• A segregated approach has been proposed to treat the petroleum refinery wastewater.
• Combined treatment system can provide better outcomes than the individual process.
• Toxicity and biodegradability test are vital indicators to develop combined system.

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

Keywords: Petroleum refinery wastewater (PRW) is a complex mixture of hydrocarbons, sulphides, ammonia, oils, sus­
Petroleum refinery wastewater pended and dissolved solids, and heavy metals. As these pollutants are toxic and recalcitrant, it is essential to
Biodegradation address the above issue with efficient, economical, and eco-friendly technologies. In this review, initially, an
Combined treatment system
overview of the characteristics of wastewater discharged from different petroleum refinery units is discussed.
Toxicity test
Segregated approach
Further, various pre-treatment and post-treatment strategies for complex PRW are introduced. A segregated
approach has been proposed to treat the crude desalting, sour, spent caustic, and oily wastewater of petroleum
refineries. The combined systems (e.g., ozonation + moving bed biofilm reactor and photocatalysis + packed bed
biofilm reactor) for the treatment of low biodegradability index wastewater (BOD5/COD < 0.2) were discussed to
construct a perspective map and implement the proposed system efficiently. The economic, toxicity, and
biodegradability aspects are also introduced, along with research gaps and future scope.

1. Introduction pollutants (e.g., aromatic hydrocarbons, hydrogen sulphides, heavy

Clean water is one of the most valuable and essential natural re­
sources on Earth. It is crucial for our survival and is also required for
various domestic, agriculture, and industrial activities. In the last few
decades, the water demand is significantly increased due to rapid
industrialization and population growth, which subsequently leads to
the issue of water pollution and depletion of scarce water resources
(Cinperi et al., 2019; Singh et al., 2022). Industries that use a significant
amount of water, such as petroleum refineries, pulp and papers, textiles,
leather tannings, etc., cause a considerable burden on natural water
resources (Sonwani et al., 2021a; Swain et al., 2021). Among these in­
dustries, petroleum refineries have been reported as the most polluting
industry because it discharges a wide range of toxic and recalcitrant
metals, etc.) into the environment. These pollutants exert adverse im­
pacts on human beings, animals, and aquatic plants (Jafarinejad and
Jiang, 2019). In petroleum refinery, the crude petroleum oil is processed
to produce various useful products (such as gasoline, petroleum
naphtha, diesel, lubricating oil, kerosene, etc.) using various unit op­
erations and processes (e.g., crude desalting, atmospheric and vacuum
distillation, hydrotreating, etc.) (Varjani et al., 2017). These unit oper­
ations and processes require a large amount of water (or steam),
resulting in generation of million gallons of petroleum refinery waste­
water (PRW) (Jain et al., 2020).
As a general rule, petroleum refineries produced about 0.4–1.5 times
of wastewater per unit volume of petroleum oil refined (Jafarinejad and
Jiang, 2019). According to Jain et al. (2020), the world crude oil

* Corresponding author.
E-mail address: raviks.rs.che16@itbhu.ac.in (R. Kumar Sonwani).

https://doi.org/10.1016/j.biortech.2022.127263
Received 19 February 2022; Received in revised form 28 April 2022; Accepted 1 May 2022
Available online 5 May 2022
0960-8524/© 2022 Elsevier Ltd. All rights reserved.
B. Narayan Thorat and R. Kumar Sonwani Bioresource Technology 355 (2022) 127263

demand was approximately 99.93 × 106 barrels per day (BPD) in 2018, summarized in Table 1. A wide range of pollutants such as phenols,
signifying generation of around 6500–24000 × 106 l/d of PRW. Further, hydrogen sulphides, mercaptans, ammonia, aromatic hydrocarbons, oil
the world crude oil demand is expected to reach approximately 121.5 × and grease, heavy metals, and other complex contaminants are generally
106 BPD in 2050 (U.S. EPA, 2019). Accordingly, around 7800–29000 × found in PRW (Varjani et al., 2017; Yuan et al., 2020). Hariz et al. (2013)
106 l/d of PRW will get produced. Additionally, it is reported that about informed that the wastewater obtained from a caustic tower of a local
80–90% of the water supplied or used in petroleum refineries is ulti­ refinery treatment has high BOD (15000 mg/L). Similarly, a high
mately released as wastewater (Jafarinejad and Jiang, 2019). However, amount of total dissolved solids (TDS) (6200 mg/L) (El-Naas et al.,
the configuration of petroleum refinery, nature of crude oil, plant size, 2014), total suspended solids (TSS) (5000 mg/L) (Sun et al., 2021),
and location can significantly affect the quality and quantity of PRW. hydrogen sulphides (12000 mg/L) (Addington et al., 2011), total
According to Younis et al. (2020), around 3.0–3.5 m3 of PRW is pro­ organic carbons (TOC) (24552 mg/L) (Rita et al., 2020), oil and grease
duced per ton of petroleum oil. In the last few decades, petroleum re­ (10000 mg/L) (Sun et al., 2021), and phenol (2900 mg/L) (Rita et al.,
fineries have been amongst the fastest-growing industries and are 2020), have been reported by previous researchers in PRW. However,
considered the backbone for developing nations like India’s economic the characteristics of PRW can significantly vary from plant to plant. The
growth and development (Varjani et al., 2020). As of June 01, 2021, the characteristics of PRW mainly depend on the quality of petroleum oil,
crude refining capacity of India was about 248.9 million metric tons per refinery configuration, preferred products, and process used in petro­
annum (MMTPA) (https://www.ibef.org/industry/oil-gas-india.aspx). leum refinery.
Also, India is the second-largest refiner in Asia and fourth in the world. The complex pollutants pose a significant threat to human beings,
Consequently, a significant amount of wastewater is generated from animals, and aquatic plants due to their highly toxic and carcinogenic
Indian petroleum refineries that are further needed to treat properly properties (Sonwani et al., 2021b; Srikanth et al., 2018). The pollutants
before being discharged into water bodies. The list of oil refineries in such as phenols and aromatic hydrocarbons (e.g., benzene, toluene,
India with their capacity and location is summarized in E-supplementary benzo[a]pyrene, phenanthrene, etc.) have been stated as persistent
Data. organic pollutants (POPs) (Swain et al., 2020). Human beings and ani­
Wastewater released from various unit operations and processes of mals are exposed to the pollutants through (a) dermal contact or skin
petroleum can roughly be divided into four-streams: 1) Desalter penetration, (b) Inhalation-through respiration, (c) food ingestion
wastewater (from Desalter), 2) sour wastewater (from atmospheric and (Varjani et al., 2017). Due to the toxic and recalcitrant nature, envi­
vacuum distillation, fluidized catalytic cracking, stripper, hydrotreater, ronmental organizations such as United State Environmental Protection
etc.), 3) spent caustic wastewater (from Merox process, alkylation, Agency (USEPA), World Bank Group (WBG), Central Pollution Control
ethylene, visbraker, etc.), and 4) oily wastewater (from Crude and slop Board, India (CPCB, India), have released standard guidelines for the
tanks) (Bastos et al., 2020; Soares et al., 2021; Yuan et al., 2020; IPIECA, safe disposal of PRW. The standard guidelines for the disposal of PRW
2010). A classification of PRW stream and its characteristics have been are summarized in Table 2. Therefore, an efficient, cost-effective, eco-
friendly, and sustainable treatment system is highly desirable to address
this global concern.
Table 1
A myriad of conventional technologies based on primary, secondary,
A classification of petroleum refinery wastewater (PRW) stream and it general
and tertiary treatment have been developed and employed to treat the
characteristics.
PRWs. In general, conventional technologies are consist of (a) physical
Stream Unit Characteristics Reference (e.g., skimmer tank, dissolved air floatation (DAF), filtration, etc.), (b)
type
chemical (e.g., coagulation-flocculation, ozonation, electrochemical
Desalter Desalter Oil and grease, (El-Naas et al., oxidation, etc.), and (c) biological processes (e.g., tricking biofilter
water surfactants, emulsifiers, 2014;Ye et al.,
(TBF), activated sludge process (ASP), rotating biological contactor,
ammonia, sulphides, 2021)
suspended solids, heavy
metals, dissolved
organic compounds (e.
Table 2
g., PAHs and Standard discharge limits for petrochemical and refinery effluents.
naphthenic acids) Guideline by CPCBa, India Guideline by WBGb
Sour water Atmospheric Hydrogen sulphide, (Addington
c
distillation ammonia, mercaptans, et al., 2011; S.N. Parameter Unit (mg/L) Unit (mg/L)c
Vacuum distillation phenols, hydrocarbons, Soares et al., 1 pH 6.0–8.0 6.0–9.0
Fluidized catalytic and suspended solids 2021; IPIECA 2 Oil and Grease 5 10
cracking 2010) 3 BOD3 (at 27 ◦ C) 15 30
Stripper 4 COD 125 125
Sulphur plant 5 Suspended solids 20 30
Hydrodesulphurizer 6 Phenols 0.35 0.2
Hydrocrackers 7 Sulphides 0.5 0.2
Visbraker 8 CN 0.2 –
Naphtha 9 Ammonia as N 15 –
hydrotreater 10 TKN 40 –
Diesel hydrotreater 11 P 3 2
Amine regeneration 12 Cr (VI) 0.1 0.05
Spent Kerosene Merox Odorous, highly (Yuan et al., 13 Cr (Total) 2 0.5
caustic LPG unit coloured, contain 2020; Rita et al., 14 Pb 0.1 0.1
Gasoline unit sodium sulphides, 2020) 15 Hg 0.01 0.003
Fluidized catalytic mercaptans, Sodium 16 Zn 5 –
cracking hydroxide, phenols, 17 Ni 1 0.5
Alkylation thiol, amine, and 18 Cu 1 0.5
Visbraker emulsified 19 V 0.2 1
Ethylene unit hydrocarbons 20 Benzene 0.1 0.05
Isomerization 21 Benzo (a)-pyrene 0.2 0.05
Oily Water Crude tanks Oil and greases, waste Younis et al., 22 As – 0.1
from Gasoline tanks solid sludge, oil sands, 2020 23 Fe – 3
storage Slop tanks heavy metals, and resin. a
Central Pollution Control Board, bWord Bank Group, cAll parameters in mg/
tanks
L except pH.

2
B. Narayan Thorat and R. Kumar Sonwani
etc.) (Chan et al., 2022; IPIECA, 2010; Leyva-Díaz et al., 2020; Mahto
and Das, 2022; Sonwani et al., 2021c; Tian et al., 2020). The application
of these conventional technologies often results in low performance for
the treatment of PRW due to the presence of complex pollutants (e.g.,
benzene, hydrogen sulphides, ammonia, phenanthrene, heavy metals,
etc.) (Younis et al., 2020). However, the pre-treatment of segregated
wastewater stream followed by post-treatment using advanced treat­
ment system can significantly improve the efficiency and overcome the
limitations of the conventional treatment system.
In this review, the current technologies and future perspectives have
been discussed to treat the PRW effectively. A brief overview of PRW
released from different units (e.g., crude desalter, atmospheric and
vacuum distillation, sulphur recovery unit, alkylation, ethylene, etc.) is
introduced. Further discussion is extended to cover various pre-
treatment and post-treatment technologies to treat the complex PRW
(i.e., crude desalting, sour, spent caustic, and oily wastewater). The
challenges of conventional technologies and opportunities of advanced
proposed treatment systems are also discussed. In addition, the per­
spectives for selecting suitable combined treatment systems are dis­
cussed to efficiently treat the low biodegradability index (BOD5/COD <
0.2) PRW along with techno-economic and life cycle assessment aspects.
2. Source of wastewater in different units of petroleum refinery
2.1. Crude desalting unit
Crude desalting is the first step in petroleum refining to remove
objectionable contaminants (e.g., inorganic salts, suspended solids, etc.)
from crude oil before it is processed to atmospheric distillation. It pre­
vents plugging and fouling of equipment due to the deposition of salts
and avoids corrosion (Dadari et al., 2016; Wu et al., 2021). The crude oil
received in the refinery from upstream process generally contains
around 0.1–2.0% of water (IPIECA, 2010). As a result, a significant
amount of wastewater is generated from the crude desalting unit. The
wastewater is generally contaminated with pollutants such as free oil,
ammonia, sulphides, suspended solids, dissolved organic compounds,
metals, etc. (El-Naas et al., 2014; Ye et al., 2021). Wu et al. (2021) have
characterized the electric desalting wastewater (EDW) obtained from a
local petroleum refinery. They found that the EDW has a high concen­
tration of oil (400–2500 mg/L) and COD (2500–13000 mg/L) with
higher temperature (70–80 ◦ C). In another study, a high level of COD
(2254 mg/L), petroleum hydrocarbons (288 mg/L), TDS (4262 mg/0L),
and TSS (1020 mg/L) was reported in EDW collected from Liaohe
Petrochemical Company, China (Ye et al., 2021).
2.2. Atmospheric and vacuum distillation
Atmospheric and vacuum distillation units are used to separate
volatile products (e.g., naphtha, motor spirit, kerosene, diesel, gas oil,
etc.) from desalted crude oil. Atmospheric distillation is employed to
separate the lighter hydrocarbons from the crude oil. In contrast, vac­
uum distillation is used to get relatively low volatile products from the
atmospheric residue under reduced pressure (Heinemann, 2017). A
significant amount of steam is used in the distillation unit; resulting
vapours get condensed that contain hydrocarbons products, hydrogen
sulphide, ammonia, etc. (EI-Nass et al., 2014). Distillation unit produces
sour water, usually contaminated with ammonia, chlorides, phenol,
hydrogen sulphide, mercaptans, and suspended solids (Singh, 2019).
2.3. Hydrotreating units
Hydrotreating units are used to remove the impurities, such as
sulphur (e.g., mercaptans, sulphides, disulphides, and thiophenes) and
nitrogen compounds from distillate products (e.g., naphtha, diesel, etc.)
(Novaes et al., 2021). The distillate products are treated with hydrogen
gas under high pressure and temperature. In hydrotreating, sulphur and
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Bioresource Technology 355 (2022) 127263
nitrogen compounds are generally transformed into hydrogen sulphide
and ammonia. The products, namely kerosene, naphtha, and vacuum
gas oil are treated in kerosene/ATF hydrotreating unit (KHTU), naphtha
hydrotreating unit (NHTU), diesel hydrotreating unit (DHDT), and
vacuum gas oil hydrotreating unit (VGO HDT), respectively. Hydro­
treating units produce sour water that contains suspended solids,
hydrogen sulphide and phenol (Fasihi et al., 2020; Singh, 2019).
2.4. Catalytic cracking unit
Fluidized catalytic cracking (FCC) unit is employed to convert heavy
complex hydrocarbons (i.e., heavy gas oils) into lighter and valuable
products (e.g., gasoline, distillate fuel oil, and liquefied petroleum gas)
(IPIECA, 2014). It also reduces the amount of heavy residuals. It is
carried out in the presence of catalyst at high temperature. The catalytic
processes, namely, FCC, moving-bed catalytic cracking, and Thermo­
for® catalytic cracking, are employed in petroleum refineries. FCC unit
generates sour water containing hydrogen sulphide, ammonia, oil, and a
large amount of spent catalyst (EI-Naas et al., 2014).
2.5. Thermal cracking unit
Thermal cracking unit is subjected to breaks down the higher-boiling
hydrocarbons into lower-boiling hydrocarbons to yield products such as
gasoil, ethylene, propane, and propylene. This operation is carried out
under high temperature (455–540 ◦ C) and pressure (100–1000 psi)
(Heinemann, 2017). High-pressure steam is mixed with the hydrocar­
bons to break them down into shorter chain hydrocarbons, and resulting
hydrocarbons and other pollutants contaminated steam are cause of
environmental concern (Pinheiro et al., 2017). The wastewater released
from the thermal cracking unit generally contains dissolved solids,
hydrogen sulphide, ammonia, phenol, dissolved organic carbon (DOC),
and COD (Guimaraes et al., 2012). It is broadly classified as sour water.
2.6. Alkylation
Alkylation is used to combine olefins with paraffins to produce high
molecular weight iso-paraffins (i.e., alkylate). Strong acids (e.g., sul­
phuric acid and hydrofluoric acid) are generally employed as catalysts
under low temperature. According to Heinemann (2017), olefins are
reactive and unstable compounds. These compounds are responsible for
environmental pollution. WBG has reported that the alkylation unit
generates acid spent, which generally contains either sulphuric acid or
hydrofluoric acid along with some amount of oil and sulphide (WBG,
2016). These acid vents should be collected and regenerated to recover
the acid for further use, which may subsequently reduce the disposal
issue of highly acidic pollutants.
2.7. Polymerization
It is used to convert the light olefin gases (e.g., ethylene, propylene,
etc.) into higher molecular weight hydrocarbons with high octane
numbers that can further be used as gasoline (polymer gasoline) or other
liquid fuels blending stocks. Acid catalysts, namely sulphuric acid,
copper pyrophosphate, phosphoric acid are commonly used in the
polymerization of light olefin gases. Water scrubbing is carried out to
remove dissolved impurities from the products, resulting wastewater is
generated (EI-Naas et al., 2014). The wastewater released from poly­
merization unit is generally contain sulphides, mercaptans, and
ammonia. Acid spent may also be generated because sulphuric acid,
copper pyrophosphate, phosphoric acid are used as catalysts.
2.8. Isomerization
Isomerization unit is used to upgrades the light naphtha fractions
(C5/C6) streams into high-octane motor gasoline (Valavarasu and
B. Narayan Thorat and R. Kumar Sonwani Bioresource Technology 355 (2022) 127263

Sairam, 2013). The process is conducted in the presence of hydrogen Table 3

using metal catalyst (e.g., aluminium chloride activated with hydro­ A summary of traditional technologies for treatment of petroleum refinery
chloric acid) at low temperature. This process generates caustic wash wastewater.
water (contain calcium chloride) and sour water (contain ammonia and Sr. Treatment Process Remarks Reference
hydrogen sulphide) (Singh, 2019). No. stage

1 Primary (i) Screening,(ii) Used to reduces the Aljuboury

stage API separator large floating and et al. (2017)
2.9. Amine regeneration unit (gravity settleable materials,
separation) total suspended solids
,(iii) (TSS), oil and grease,
In petroleum refinery, the concentrated solution of alkanolamine, Dissolved air turbidity, etc., which
namely diethanolamine (DEA) and methyl diethanolamine (MDEA) are flotation (DAF) or may otherwise effect
commercially employed to remove the acid gases such as H2S and CO2 induced air the efficacy of
from process streams (or sour gas) (Ibrahim et al., 2021). This step refers flotation (IAF), microorganisms
(iv) employed in the
to the gas sweetening process, as it prevents environmental pollution.
Coagulation- secondary treatment
Amine regeneration unit generally consists of an absorber (contactor) flocculation,(v)
and generator (stripper). In absorber, sour gases are contacted with lean Equalization tank
amine solution, whereas a regenerator is employed to reactivate the rich 2 Secondary (i) Activated Used to degrade the Khatri et al.
amine solution (Ahmad et al., 2021). During these operations, amine- stage sludge process(ii) remaining oil, (2018);
Sequential batch degradable organic Sonwani
rich wastewater is commonly discharged, leading to environmental is­ reactor(iii) compounds, a fraction et al. (2021a)
sues such as disruption of aquatic life and bio-concentration potential Membrane of recalcitrant organic
(Salim, 2021). bioreactor(iv) pollutants, trace
Up-flow metals, nutrients, etc.
anaerobic sludge
blanket reactor(v)
2.10. Sulphur recovery and tail gas treating unit Moving bed
biofilm reactor
The sour gas derived from various units (e.g., catalytic cracking, (vi) Fluidized bed
hydrotreating, and hydro-processing) contains a high concentration of bioreactor
3 Tertiary (i) Photocatalysis A polishing step to Jain et al.
hazardous hydrogen sulphide. The stripping of sour gas in lean solvent
stage (ii) meet treated water to (2020);
(e.g., alkanolamine) simply transforms air pollution into water pollu­ Ozonation(ii) reuse or discharge as Singh and
tion. Therefore, sulphur recovery units are generally employed in pe­ Fenton process standards set by Kumar
troleum refineries to recover elemental sulphur from hydrogen sulphide (iv) environmental (2020)
to avoid acidic gas emissions (Ibrahim et al., 2021). Claus process is Catalytic organizations.
oxidation(v)
commonly used to recover the sulphur (95 to 97%) from sour gas. The Electro-chemical
tail gas is subject to the tail gas treating unit (TGT) for further sulphur oxidation(vi)
recovery (Mokhatab and Poe, 2012). The effluent generated from these Membrane
units may contain a significant amount sulphur compounds that are separation
(vi) Adsorption
highly toxic and exert foul odour in the environment.

3. Strategy for the treatment of complex petroleum refinery
wastewater
A wastewater treatment plant is generally installed within the pe­
troleum refinery to collect and treat the wastewater streams generated
during crude oil processing (Younis et al., 2020). Over the last few de­
cades, various physiochemical (e.g., adsorption, coagulation-
flocculation, membrane separation, dissolved air flotation, photo­
catalysis, ozonation, etc.) and biological (e.g., bioremediation, con­
structed wetlands, etc.) methods have been employed to treat the PRW
(Varjani et al., 2020). The literature study suggests that every treatment
technology has its own advantages and disadvantages based on the
following benchmarks: process efficiency under various conditions,
applicability, environmental impact, and techno-economic aspects
(Routoula and Patwardhan, 2020). The overall wastewater treatment
processes are categorized as treatment of specific stream source, pre-
treatment, primary treatment, secondary treatment, and tertiary treat­
ment (Englande et al., 2015). A typical refinery wastewater treatment
plant consists of three stages as follows; (1) primary treatment (e.g.,
screening, DAF, induced air floatation (IAF), coagulation-flocculation,
equalization tank, and gravity separation (GS)), (2) secondary treat­
ment (e.g., ASP, TBF, sequential batch reactor (SBR), etc.), and (3) ter­
tiary treatment (e.g., photocatalysis, ozonation, catalytic oxidation,
membrane separation, adsorption, etc.) (Table 3). A summary of tradi­
tional technologies (primary, secondary, and tertiary) for the treatment
of PRW is represented in E-Supplementary data. The present section
describes an overview of primary, secondary, and tertiary technologies
for the treatment of PRW.
3.1. Primary treatment
Primary treatment is used to reduce the large floating and settleable
materials, TSS, turbidity, oil, and grease of PRW (Aljuboury et al., 2017).
It consists of physical operations (e.g., API separator, corrugated plate
interceptor (CPI) separator, DAF, IAF, equalization tanks) to remove the
floating and settleable pollutants from PRW. It allows wastewater for
further treatment (secondary treatment stage). According to Englande
et al. (2015), primary treatment generally removes 35–40% of the BOD
and 60–65% of the settleable solids. The key primary treatment steps are
described below.
3.1.1. API separator (gravity separation)
American petroleum institute (API) separator (or gravity separator)
is the first treatment step and generally used to remove the free oil and
suspended solids from PRW. PRW generally contains oil-bearing sludge
and oil in three forms (i.e., free oil, emulsified oil, and dissolved oil). API
separator works on the principle of difference in specific gravity (or
density). It allows high molecular weight solids to settle underneath the
lighter liquids and separate the oil, water, and solids (Varjani et al.,
2020). The oils that float on the surface of wastewater are removed by
skimming, whereas sludge that settles down to the bottom of the API
separator is removed periodically (IPIECA, 2010). It is widely employed
to remove the free oil because of its high efficacy and low cost (Varjani
et al., 2020). However, it is ineffective in removing the emulsified and
soluble oil (Abdulredha et al. 2020). Also, high pH can stabilize the
emulsion, which may reduce the performance of the API separator.

4
B. Narayan Thorat and R. Kumar Sonwani
Therefore, the spent caustic stream can be neutralized with acids or
directed to an equalization tank to reduce the pH before being subjected
to primary treatment (IPIECA, 2010).
3.1.2. Dissolved air flotation (DAF)
DAF uses air to remove small oil droplets, suspended matter, and
other insoluble impurities from wastewater. In this process, the air is
continuously sparged through wastewater to produce millions of tiny air
bubbles in a floatation tank at atmospheric pressure (Varjani et al.,
2020). The dissolved tiny air bubbles interact with the surface of oil/
solids matters and subsequently float them to the surface of the waste­
water. The skimmer removes the floated oil/solids which is further
subjected to refinery slops for additional treatment (IPIECA, 2010).
Generally, the dispersed particles (oil/solids) repels each other due to
the negative electric charge on their surface, which resists them to form
larger size particle (or floc) and avoid them to settle. Therefore, DAF
process is often assisted by adding chemical coagulant and flocculent to
enhance the aggregation of suspended oil/solids into large size
(Abdulredha et al., 2020). The small foot-print and high efficiency are
the merits of DAF. Whereas, the high operating cost to produce tiny air
bubbles and emission of harmful compounds such as H2S and NH3 (leads
to odour issues) are the major demerit associated with this process (An
et al., 2017; Radzuan et al., 2016).
3.1.3. Induced air flotation (IAF)
Induced air floatation (IAF) is a clarification process used in in­
dustries, including petroleum refineries to remove the emulsified oil and
suspended solids from wastewater. In IAF, a rotor-disperser injects the
air, forces them to flow through the disperser and generates vacuum in
stand pipe to force air (IPIECA, 2010). Consequently, the wastewater
flows through a series of cells and floats over the surface wastewater.
The compact size, low-cost, less sludge production, and high efficiency
are the merits of IAF, whereas high operating cost is the limitation of this
process (Varjani et al., 2020).
3.1.4. Equalization tank
Equalization tank is used to reduce the fluctuations in the wastewater
stream (IPIECA, 2010). In industries, the wastewater streams fluctuate
considerably in both flow rates and composition (COD, pH, colour,
turbidity, oil, TSS, etc.) during the working cycle (Manderso, 2018). The
high fluctuation of wastewater streams could adversely affect the per­
formance of individual treatment units, especially biological processes.
Therefore, it is necessary to equalize and maintain the constant influent
flow rate of wastewater streams before being sent to the downstream
treatment units. Equalization tank stores the fluctuating wastewater
streams and lets it out at consistent influent flow to downstream units
(Raji et al., 2018). However, aeration and continuous mixing are
essential in the equalization tank to avoid septic conditions and keep
solids in suspension (Jasim and Aziz, 2020). Equalization tank can
reduce the expenditures associated with pH neutralization and
coagulation-flocculation. Equalization is generally achieved by either
flow equalization or concentration equalization. It can be placed upstream
of the API separator, upstream of the DAF/IAF, and downstream of the
DAF/IAF, and mainly depends on the inlet loading rates and composi­
tion of PRW.
3.1.5. Coagulation-flocculation
Coagulation-flocculation is a pre-treatment step in which chemicals
such as ferric chloride, aluminium chloride, aluminium sulphate, poly­
mers, etc., are added in wastewater to destabilize the colloidal particles
(Fernandez-Gonzalez et al., 2018). The small particles are agglomerated
into larger size settleable flocs. Mechanisms, namely inter-particle
bridging, charge neutralization, and sweep coagulation that reduces
the zeta potential and consequently decrease the repulsive forces be­
tween particles to agglomerate (Almojjly et al., 2019). Similarly, in
flocculation, high molecular weight polymers (e.g., alginates, poly
5
Bioresource Technology 355 (2022) 127263
aluminium chloride, sodium aluminate, chitosan, etc.) are employed to
promote the agglomeration of colloidal and suspended materials (Verma
et al., 2012). It is an economical and straight forward method to reduce
the turbidity, COD, TDS, and colour of PRW (Singh and Kumar, 2020;
Verma et al., 2012). However, in some cases, a considerable amount of
coagulant and flocculent is required to attain the desired separation,
resulting generation of a large quantity of toxic sludge, which is often
more difficult to handle. Recently, coagulation-flocculation was used as
a pre-treatment step to treat the real PRW collected from a local pe­
troleum refinery situated in Northern India (Singh and Kumar, 2020).
They evaluated the efficacy of three coagulants (i.e., CuSO4, FeCl3, and
CuSO4 + FeCl3) and found that the mixed coagulant (CuSO4 + FeCl3)
exert higher removal efficiency (turbidity: 89.47 %, TDS: 94.16 %, and
colour: 95.29 %) than CuSO4 and FeCl3 individually.
3.2. Secondary treatment
The wastewater discharge from the primary stage is treated further
to reduce/remove the residual oil, biodegradable and refractory organic
pollutants, trace metals, and nutrients (e.g., nitrogen and phosphorous)
(Khatri et al., 2018). This is generally achieved through biological
treatment where microorganisms break down or mineralized the dis­
solved and colloidal organic pollutants into innocuous compounds such
as CO2, H2O, and CH4 (El-Naas et al., 2014; Nagarajan et al., 2019). The
mineralization of pollutants is accomplished by respiration (catabolism)
and synthesis (anabolism), and resulting end products are gas, liquid,
and microbial biomass (cell tissue) (Metcalf and Eddy, 2014). The mi­
crobial biomass has high specific gravity than water and can be easily
separated out in clarifiers (sedimentation tank). Therefore, secondary
treatment generally comprises of a biological reactor followed by a
clarifier to separate the biomass called sludge. Along with organic
substrates, microorganisms also require inorganic nutrients (such as N,
P, K, Mg, Ca, Fe, Na, Zn, Mn, Co, Ni, Cu, etc.) for their respiration and
synthesis (Kalantary et al., 2014). It is reported that the nutrient
requirement is higher for the aerobic process (minimum COD:N:P ratio
of 100:10:5) due to higher microbial growth than anaerobic process
(minimum COD:N:P ratio of 350:5:1) (Ghangrekar and Behera, 2014).
Based on the application, the biological treatment can broadly be clas­
sified as: (1) suspended growth (i.e., free cell) and (b) attached growth
(i.e., attached biofilm) processes (Sonwani et al., 2019).
3.2.1. Suspended growth processes
In this process, microorganisms (i.e., bacteria, algae, and fungi) are
retained in liquid suspension by thoroughly mixing (aeration and stir­
rer). The suspended growth processes may be aerobic or anaerobic and
generally used for low and high-strength organic wastewater, respec­
tively (Ghangrekar and Behera, 2014). Aerated lagoon, ASP, MBR, SBR,
anaerobic digestion, and UASBR have come under suspended growth
processes (Swain et al., 2021). Perfect fluid mixing, high oxygen transfer
rate, and easy to scale-up are the main benefits associated with the
suspended growth processes (Pugazhendi et al., 2017). However, high
shear to bacterial culture, membrane fouling, and low efficiency are
major limitations associated with the suspended growth processes
(Mohan and Nagalakshmi, 2020; Vikrant et al., 2018).
A conventional ASP (30 L) was employed to treat the oilfield-
produced wastewater (Lusinier et al., 2021). ASP achieved a COD
removal efficiency. Mirbagheri et al. (2014) have estimated the effi­
ciency of ASP to treat the PRW having COD of 1060 mg/L. The COD
removal efficiency of 96% was achieved using activated sludge. Alsalhy
et al. (2016) studied the biological treatment of PRW (COD 500 mg/L) in
a membrane bioreactor. They reported that more than 70% of COD and
100% phenol were removed at 20 ± 1.0 ◦ C. In another study, a hollow
fibre membrane bioreactor was employed to treat the real petroleum
wastewater (COD = 580 mg/L, BOD5 = 203 mg/L, TSS = 110 mg/L,
TDS = 2100 mg/L, and turbidity = 40 NTU) obtained from Arak Pe­
troleum Refining Co., Iran (Razavi and Miri, 2015). They reported that
B. Narayan Thorat and R. Kumar Sonwani
the hollow fibre membrane bioreactor successfully removed 82 %, 89 %,
98 %, 99 %, and 98 % of COD, BOD5, TSS, VSS, and turbidity, respec­
tively after 36 h of retention time under the following conditions (pH =
7.6, Temp. = 20 ◦ C, COD = 580 mg/L (COD). Chen et al. (2018) used a
UASBR to treat the phenolic wastewater. They achieved more than 96%
of COD and phenol removal under a high organic loading rate (COD of
3000 mg/L and phenol of 1200 mg/L). SBR was employed to treat PRW
with COD of 350 mg/L and TOC of 70 mg/L, and they reported that COD
and TOC removal efficiencies of 80% and 84%, respectively were ob­
tained (Thakur et al., 2014).
3.2.2. Attached growth processes
In the attached growth processes, microorganisms are attached to the
surface and pores of support media (e.g., polyvinyl chloride, activated
carbons, biochars, etc.). A thin microbial biofilm (generally 10 µm to 1
mm) is grown onto an inert packing medium through which substrates
and nutrients are diffused and finally mineralized into end products
(Sonwani et al., 2021a). The bioreactors, namely TBF, PBBR (packed bed
bioreactor), RBC (rotating biological contactor), IFAS (integrated fixed-
film activated sludge), MBBR (moving bed biofilm reactor), and FBBR
(fluidized bed bioreactor), are well known attached growth processes
(EI-Nass et al., 2014; Novotný et al., 2012; Mudliar et al., 2010; Swain
et al., 2021). The inert packing medium such as polyvinyl chloride,
polyurethane foam, polypropylene, rocks, and gravels offer a very high
surface area per unit volume, are extensively applied as packing media
in bioreactors (Shen et al., 2015; Sonwani et al., 2020; Swain et al.,
2020). The packing media can be stationary in the bioreactor (e.g., TBF,
PBBR) and such systems are referred to as fixed-film reactors or it can be
moving media (e.g., FBBR, MBBR) and such systems referred to as
submerged moving bed reactors (Metcalf and Eddy, 2014). These pro­
cesses are more efficient for the treatment of wastewater due to high
biomass concentration, small foot-print, and low hydraulic retention
time (HRT) compared to the suspended growth processes (Shen et al.,
2015). However, clogging of packing media, mass transfer resistance,
high pressure drop, and design complexity are the major disadvantages
of the attached growth processes (Sonwani et al., 2021b).
In the last few decades, the attached growth processes have received
significant attention from scientific communities and are extensively
used to treat wastewater, including PRW (Bharti et al., 2019; Goswami
et al., 2020; Sonwani et al., 2019). Recently, Swain et al. (2020) used a
MBBR (2.0 L) to treat the phenol (100 mg/L) and ammonia (100 mg/L)
from simulated petroleum wastewater. They reported the phenol and
ammonia removal efficiency of 92.6% and 91.8%, respectively. In
another study, a MBBR (2 L) removed more than 95% of phenol and COD
from phenolic wastewater at HRT of 48 h and pH of 7.5 (Zhou et al.,
2018). PBBR was employed to treat real petroleum wastewater (COD of
9200 mg/L, TOC of 4548 mg/L, phenolic compounds of 3561 mg/L, and
ammonia of 121 mg/L) collected from the oil refinery, Guwahati, India
(Banerjee and Ghoshal, 2017). PBBR packed with immobilized Ca −
alginate-Bacillus species was effectively removed 99.2 % of COD, 95.9 %
of TOC, 99.7 % of phenolic compounds, and 49.3 % of ammonia,
respectively. Similarly, the PBBR packed with immobilized PUF-Bacillus
species was effectively removed 90.9 % of COD, 88 % of TOC, 91.5 % of
phenolic compounds, and 42.7 % of ammonia, respectively. A four-stage
RBC (total volume of 16 L) was operated in continuous mode to treat the
PRW (Ghalehkhondabi et al., 2021). They reported that four-stage RBC
successfully removed 99.07% of ammonia and 85.76 % of COD, under
optimum conditions. In another work, polyacrylate containing waste­
water was successfully treated in combined anaerobic–aerobic FBBR
(Song et al., 2021).
The parameters such as inlet loading rate of wastewater and its
characteristics, aeration rate, food/microorganism (F/M) ratio, sludge
volume index, sludge retention time (SRT), HRT, nutrients, and oper­
ating parameters (e.g., pH, temperature, DO, etc.), adversely affects the
performance of bioreactors (Jafarinejad and Jiang, 2019). Bioreactors
are generally run at decline growth or endogenous growth phase with
6
Bioresource Technology 355 (2022) 127263
enough F/M ratio to keep the concentration of the microorganisms
constant and avoid depletion of active microorganisms in bioreactors
(Ghangrekar and Behera, 2014). Also, sludge formed during the
endogenous growth phase poses higher settling characteristics.
3.2.3. Nitrification and denitrification
The condensates from the fractional distillation column, catalytic
cracking, reflux column, and spent amine consist of a large amount of
nitrogen compounds (Kenari et al., 2010). Nitrogen is an essential
nutrient for the growth and survival of living organisms. However, a
high concentration of nitrogen compounds in PRW could lead to
eutrophication (i.e., excess algal growth) in water resources, resulting
destruction of aquatic life (Wang et al., 2021). Therefore, nitrification
and denitrification steps should be added in biological treatment to meet
regulatory limits. Nitrification and denitrification is a two-step process
of bio-elimination of nitrogenous compounds (i.e., ammonia (NH3) and
ammonium ion (NH+ 4 )) from wastewater (Manu et al., 2021; Xiang et al.,
2020). Nitrification is carried out under strict aerobic conditions.
Whereas, denitrification is performed under anoxic conditions. In
nitrification, initially, ammonia is converted to nitrite (NO–2) by
ammonia-oxidizing bacteria (e.g., Nitrosomonas, Nitrosopira, etc.), which
is further converted to nitrate (NO–3) by nitrite-oxidizing bacteria (e.g.,
Nitrobacter. Nitrospina, Nitrocystis, etc.) (Eq. (1), 2, 3) (Thakur and
Medhi, 2019). In denitrification, nitrite (NO–2) and nitrate (NO–3) are
reduced in gaseous nitrogen either as molecular N2 or as an oxide of N by
anoxic bacteria (Eq. (4), 5, 6).
Nitrification.
(1)
Nitroso− bacteria
2NH4+ + 3O2 ̅̅̅̅̅̅̅→ 2NO−2 + 4H + + 2H2 O
(2)
Nitro− bacteria
2NO−2 + O2 ̅̅̅̅̅̅→ 2NO−3
Nitrifiers
2NH4+ + 2O2 ̅̅̅̅̅→ NO−3 + 2H + + H2 O (3)
Denitrification.
(4)
Axonix− bacteria
6NO−3 + 2CH3 OH ̅̅̅̅̅̅
̅→ 6NO−2 + 2CO2 + 4H2 O
(5)
Nitro− bacteria
2NO−2 + 3CH3 OH ̅̅̅̅̅̅→ 3N2 + 3CO2 + 3H2 O + 6OH −
(6)
Axonix− bacteria
6NO−3 + 5CH3 OH ̅̅̅̅̅̅
̅→ 3N2 + 5CO2 + 7H2 O + 6OH −
In this direction, various bioreactors such as SBR, biofilters, bio­
scrubbers, airlift bioreactors, and membrane biofilm reactors have been
extensively employed (Thakur and Medhi, 2019). The microorganisms,
namely Acinetobacter sp. YY1, Sphingomonas sp. YY2 and Pseudomonas
sp. YY3, were obtained from caprolactam treatment unit to remove the
total nitrogen from petroleum wastewater (Lang et al., 2019). These
microorganisms effectively removed total nitrogen of 94.22% and
90.10% by nitrification and denitrification process, respectively in 48 h.
A partial nitrification–denitrification coupled with simultaneous
anammox and denitrification (PND-SAD) system was employed to ni­
trogen compounds from domestic wastewater (Zhao et al., 2022). They
reported that PND-SAD successfully removed 97.3% of ammonia from
domestic wastewater. Lan et al. (2011) have developed a simultaneous
nitrification, anammox, and denitrification (SNAD) process in a SBR.
They found that SBR removed about 96% of NH+ 4 -N and 87% of COD at
9 days of HRT.
3.2.4. Biodegradation of various pollutants
Biological processes (i.e., biodegradation) have been extensively
used to treat the various pollutants, such as phenols, hydrogen sul­
phides, mercaptans, ammonia, aromatic hydrocarbons, oil and grease,
and heavy metals (EI-Naas et al., 2014; Sonwani et al., 2021c). A large
number of microorganisms such as Enterobacter cloacae SG208, Bacillus
flexus GS1 IIT (BHU), Bordetella avium, Acinetobacter tandoiii, Ralstonia
B. Narayan Thorat and R. Kumar Sonwani Bioresource Technology 355 (2022) 127263

eutroph, Acinetobacter baumannii AL-6, Pseudomonas sp. HXF, etc., has
been employed for the biodegradation of various pollutants (Abo-state
et al., 2018; Dexter and Boopathy, 2019; Hu et al., 2021; Sedighi et al.,
2016; Swain et al., 2021). A summary of the biological degradation of
various pollutants and their metabolites is reported in Table 4. Kureel
et al. (2017) have isolated Bacillus sp. M3 from the petroleum-
contaminated site and employed in the biodegradation of aromatic hy­
drocarbon (i.e., benzene). According to them, more than 90% of benzene
removal was attained under optimum conditions. Phenol, 1,2-benzene­
diol, hydroquinone, and benzoate were the major intermediates of
benzene biodegradation. Bordetella avium obtained from PRW was
employed to degrade the naphthalene (Abo-state et al., 2018). Bordetella
avium was effective to degrade the 95% of naphthalene with an initial
concentration 7 mM. According to them, the intermediate metabolites,
namely 1,2-Benzene dicarboxylic acid, Butyl-2,4-dimethyl-2-nitro-4-
pentenoate were formed during naphthalene biodegradation. In
another study, Hu et al. (2021) have employed Pseudomonas sp. HXF1
for the simultaneous degradation of ammonia nitrogen and fluoride.
They reported that 99.2% of NH4+-N and 87.3% of F− removals were
obtained. Li et al. (2021a); Li et al. (2021b) have evaluated the
biodegradation potential of Stenotrophomonas acidaminiphila 4–1 to treat
the hexavalent chromium and found that 75.69% removal of hexavalent
chromium was achieved with an initial concentration of 15 mg/L. Ac­
cording to Dexter and Boopathy (2019), Acinetobacter tandoii success­
fully mineralized phenol into Catechol, cis cis-muconic acid, succinic
acid, oxaloacetic acid, and acetic acid via the ortho and β-ketoadipase
pathway.
The biological degradation of pollutants (such as phenols, aromatic
hydrocarbons, etc.) involves a series of steps using different microbes/
enzymes (Ghosal et al. 2016). Also, the degradation pathway is gener­
ally varied with the type of pollutants and microorganisms employed in
the processes. The enzymes, namely monooxygenases, dioxygenases,
peroxidases, reductases, laccases, hydroxylases, and dehydrogenases
play a key role in the biodegradation of petroleum hydrocarbon pol­
lutants under aerobic and anaerobic conditions (Ghosal et al. 2016;
Varjani and Upasani, 2017; Sonwani et al., 2021a). For example, mon­
ohydroxylation and dihydroxylation of aromatic hydrocarbons (e.g.,
toluene, naphthalene, etc.) occur due to the activation of mono­
oxygenases and dioxygenases, respectively (Abbasian et al., 2015). The
metabolic pathway of aromatic hydrocarbons biodegradation using
microorganisms (i.e., bacterial, algae, and fungi) is described in detail
earlier (Sonwani et al., 2021a). The metabolic pathway of cyclohexane
biodegradation is represented in E-supplementary Data. Initially,
cyclohexane monooxygenase attacks the cyclohexane ring to break it
down into cyclohexanol, which is then converted into cyclohexanone
and caprolactone by cyclohexanol dehydrogenase and cyclohexanone
monooxygenase, respectively. Further, caprolactone is broken down
into 6-Hydroxy hexanoic acid and 6-oxohexanoic acid by caprolactone
hydrolase and 6-Hydroxyhexanote dehydrogenase, respectively. Suc­
cessive cleavage of 6-oxohexanoic acid leads to the formation of Acetyl
CoA and other intermediates. According to Varjani and Upasani, (2017),
the genes such as alkA, alkM, alkB, LadA, assA1, assA2, nahA-M, napA,
amoA, dsrAB and mcrA, are important to study the biodegradation of
aromatic hydrocarbon. The details of mechanisms and degradation
pathways of pollutants have been well described elsewhere (Ghosal
et al., 2016; Varjani and Upasani, 2017; Varjani, 2017; Sonwani et al.,
2021a).
3.3. Tertiary treatment
In tertiary treatment, effluent received from the secondary treatment
unit is further treated to reduce the concentration of the pollutants (i.e.,
trace organics, suspended solids, dissolved solids, metals, and patho­
gens). It is generally referred to as a polishing step to meet treated water
to reuse or discharge as standards set by environmental organizations
(Jain et al., 2020; Singh and Kumar, 2020). Conventionally, tertiary
treatment is accomplished by sand filtration, activated carbon filtration,
and chemical oxidation (e.g., hydrogen peroxide (H2O2), chlorination)
(Varjani et al., 2020). However, PRW contains recalcitrant pollutants
such as benzene, toluene, xylene, naphthalene, fluorene, and pyrene,
phenols, etc., and conventional tertiary treatment methods could not
effectively treat these pollutants. In this contest, currently, membrane
separation processes (e.g., ultrafiltration, reverse osmosis, etc.) and
advanced oxidation processes (AOPs) (e.g., photo-Fenton, photo­
catalysis, hydrogen peroxide/ultraviolet, ozonation, wet air oxidation,
and electrochemical oxidation) are extensively employed to treat such
complex pollutants (Tian et al., 2020). In AOPs, reactive hydroxyl rad­
icals are produced to degrade a wide range of pollutants, resulting in
generation of less toxic intermediate products. AOPs are associated with
merits such as very short reaction times (usually few minutes), high
efficiency, and mineralization of pollutants (Routoula and Patwardhan,
2020). However, high cost, unsafe by-products, and toxic sludge gen­
eration are the major demerits of AOPs (Al-Mamun et al., 2019). The
photocatalytic degradation of monocyclic aromatic hydrocarbons (i.e.,
benzene, toluene, ethylbenzene, and xylenes (BTEX)) was studied by
AOP (UV/H2O2) (Bustillo-Lecompte et al., 2018). They reported that
more than 90% of BTEX removal was obtained under acidic conditions
(pH 3). The previous researchers have well described the details of AOPs
for the treatment of PRW (Olajire, 2020; Tian et al., 2020). An integrated
system consists of electrocoagulation, biodegradation, and adsorption in
series was used to treat the real petroleum wastewater (Naas et al.,
2014). The wastewater has average COD of 4450 mg/L, TDS of 5000
mg/L, and total phenol of 172.5 mg/L. They found that the integrated
system removed overall 97% of COD and 100% of phenol.

Table 4
A summary of biological degradation of various pollutants and their metabolites.
S. N. Pollutant Microbe(s) Metabolites/intermediates Reference

1 Benzene
2 Naphthalene
3 O-Xylene
4 4-Chlorophenol
5 Phenol
6 Phenol
7 Naphthalene
Bacillus sp. Phenol, 1,2-benzenediol, hydroquinone and benzoate (Kureel et al., 2017)
Consortium Catechol and 2-naphthol (Sonwani et al., 2019)
Rhodococcussp. ZJUT312 2-methylbenzylalcohol, (You et al., 2018)
2-methylbenzoic acid, and 3-methylcatechol
Bacillus flexus GS1 IIT (BHU) 4-Chlorocatechol, 5-chloro-2-hydroxymuconicsemialdehyde (Swain et al., 2021)
Acinetobacter tandoii Catechol, cis cis-muconic acid, succinic acid, oxaloacetic acid, and acetic acid (Dexter and Boopathy, 2019)
Acinetobacter Catechol, cis,cis-muconic acid (Paisio et al., 2016)
sp. RTE1.4
Bordetella avium 1,2-Benzene dicarboxylic acid, Butyl-2,4-dimethyl-2-nitro-4-pentenoate (Abo-state et al., 2018)

8 Xylene Bacillus sp. – (Singh et al., 2017)

9 Ethyl mercaptan Ralstonia eutroph – (Sedighi et al., 2016)
10 O-Xylene Rhodococcussp. ZJUT312 2-methylbenzylalcohol, (You et al., 2018)
2-methylbenzoic acid, and 3-methylcatechol
11 Ammonia nitrogen Pseudomonas sp. HXF1 – (Hu et al., 2021)
12 Ammonia nitrogen Acinetobacter baumannii strain AL-6 Nitrate/nitrite (An et al., 2020)

7
B. Narayan Thorat and R. Kumar Sonwani
A typical PRW treatment system consists of equalization, primary
and secondary oil/water separation, biological treatment, clarification,
tertiary treatment, and solids handling (Fig. 1) (Jafarinejad and Jiang,
2019).
4. Segregated approach for the treatment of complex petroleum
refinery wastewater
A segregated strategy for the treatment of PRW can improve the
overall treatment efficiency, enhance treated effluent quality, and reuse
treated wastewater in internal routines like fire-water makeup, cooling
tower, and green belt development. Such segregated strategy is partic­
ularly important in water-scarce regions. The segregation of wastewater
streams based on characteristics (COD, BOD, TSS, TDS, recalcitrant
pollutants, etc.) is general practice in several industries. Wastewater
generated from unit operations and processes of petroleum refinery can
broadly be segregated into four streams: 1) Desalter wastewater, 2) sour
wastewater, 3) spent caustic wastewater, and 4) Oily wastewater
(Addington et al., 2011; Bastos et al., 2020; IPIECA, 2010). The char­
acteristics of the various stream of petroleum refinery wastewater re­
ported by previous researchers have been summarized in Table 5. The
strategy for the treatment of above segregated wastewater streams is
discussed in the next section.
4.1. Crude desalting wastewater and its treatment method
Desalter wastewater generally contains oil, grease, surfactants,
emulsifiers, ammonia, sulphides, suspended solids, heavy metals, and
dissolved organic compounds (Ye et al., 2021). The characteristics of
desalter wastewater, treatment methods, and their process efficiency
reported by the previous researcher are summarized in Table 6. Previ­
ously, methods such as gravity settling, coagulation-flocculation, cen­
trifugal contactor, membrane separation, adsorption,
biodegradation have been employed to treat desalter wastewater
(Dadari et al., 2016). However, most of the researchers focused on
treating individual contaminants and simulated wastewater. In reality,
desalter wastewater shows high pollutants contents (such as oil and
grease (400–2500 mg/L), TDS (400–2500 mg/L), TSS (50–5000 mg/L),
COD (100–13000)), complicated compositions, strong stability, and
acute bio-toxicity (Sun et al., 2021; Wu et al., 2021). It also contains
toxic and recalcitrant compounds (e.g., BTEX, naphthalene, ammonia,
hydrogen sulphide, etc.), and an individual approach is not appropriate
to produce high-quality treated wastewater that can be further reused in
refinery (Ye et al., 2021). If it is directly sent to the wastewater treatment
plant without pre-treatment, it may adversely affect the overall perfor­
mance of physicochemical and biological processes. Therefore, pre-
treatment or primary treatment followed secondary treatment and
Fig. 1. Schematic diagram of a typical petroleum refinery wastewater treatment system (Modified from Schultz, 2006).
Bioresource Technology 355 (2022) 127263
tertiary treatment is suggested as a better solution to manage the
desalter wastewater effectively. The pre-treatment or primary treatment
methods such as coagulation (Ye et al., 2021), swirling flotation (Wu
et al., 2021), API separator, air flotation tank (Sun et al., 2021),
Hydrocyclone-intensified filtration, and centrifugal contactors (Hao
et al., 2013), have been broadly employed to reduce the pollutants load.
The pre-treatment improves the biodegradability of desalter wastewater
for further treatment. In this direction, a swirling flotation was
employed as a pre-treatment stage to treat the desalter wastewater and
found that 98.4% of the oil was removed with an initial oil content of
2500 mg/L (Wu et al., 2021). Also, oil, suspended solids, and COD were
reduced below 30 mg/L, 15 mg/L, and 700 mg/L, respectively. In
another work, a Hydrocyclone-intensified filter removed more than 85%
of oil and suspended solids from desalter wastewater which was then
further subjected to secondary and tertiary treatment (Sun et al., 2021).
According to Hao et al. (2013), a centrifugal contactor was employed as
a pre-treatment step to treat the oil concentrations ranging from 60,000
mg/L to below 200 mg/L. The pre-treatment reduced oil contents and
toxicity as well as improved the biodegradability of pollutants. A typical
segregated approach for the treatment of desalter wastewater is illus­
trated in Fig. 2.
In refinery, desalter wastewater is generally subjected to an oil/
water separation unit before sending it to the main treatment units.
According to IPIECA (2010), installing a separate oil/water separation
unit is economical to handle the highly contaminated desalter waste­
water instead of upgrading the existing wastewater treatment plant
configuration. A schematic diagram of a typical desalter effluent pre-
treatment is represented in Fig. 3a.
Initially, desalter wastewater is fed to a floating roof tank (reduce
VOC emissions) for equalization and upset buffering. The oil float on the
top of wastewater is skimmed off and sent to refinery slops. Whereas,
wastewater (middle phase) is subjected to the wastewater treatment
and plant. The heavier solids (or sludge) are allowed to settle (generally one
day of residence time) at the bottom of the tank and sent to the sludge
disposal site for further treatment. In many reports, it has been found
that desalter effluent contains a significant amount of volatile organic
compounds, which may be emitted to the environment and cause air
pollution. Such compounds can be controlled using strippers, as illus­
trated in Fig. 3b.
4.2. Spent caustic wastewater and its treatment method
In petroleum refinery, an aqueous solution of concentrated sodium
hydroxide (NaOH) is widely used to remove the impurities, namely
hydrogen sulphides and carbon dioxide from various hydrocarbons
streams (e.g., gasoline, kerosene/jet fuel, natural gas, ethylene, etc.)
(Sabri et al., 2018). The resulting effluent stream is referred as spent
8
B. Narayan Thorat and R. Kumar Sonwani Bioresource Technology 355 (2022) 127263

Table 5
Characteristics of various stream of petroleum refinery wastewater reported by previous researchers.
S. Stream type Characteristics Reference
N.

pH COD BOD TOC TDS TSS Sulphide Phenol Ammonia Oil and
grease
1 Desalter 8.61 2254 120 4262 0.12 16 22.5 346 Ye et al. (2021)
2 7 7750a 40.7 1450a Wu et al. (2021)
3 6.0–9.0 300a 2525a 6a 15 5025a Sun et al. (2021)
4 Spent caustic 12 38,500 9500 Yuan et al. (2020)
5 13.7 96,980 24,552 63.2 2900 16,544 Rita et al. (2020)
13.7 1420 664 298 6820 400 100a Devarnejad and Bakhshandeh
(2018)
7 31000a 10000a 13000a 25000a 2000 Hariz et al. (2013)
8 Sour water 8.1a 935a 570 23 92–128 21.1 12.7 Coelho et al. (2006)
9 Oily 8.2a 900a 86a 2 44a Li et al. (2017)
wastewater
10 7.6 3150 323 1550 85 Wei et al. (2010)
11 637 214.9 15.8 15.5 Li et al. (2006)

All parameters are in mg/L except pH; aMean value.

caustic wastewater. Spent caustic wastewater is corrosive and toxic due
to its alkaline nature and presence of a significant amount of contami­
nants such as sulphides, disulphides, mercaptans, phenols, hydroxides,
etc. (Rita et al., 2020). According to the United States Resource Con­
servation and Recovery Act, sour water is highly hazardous due to the
presence of high amount sulphide (1–4 wt%), salinity (sodium 5–12 wt
%), COD (20000–40000 mg/L) and pH (pH greater than 12) (Hariz et al.,
2013; Li et al., 2021a; Li et al., 2021b). Therefore it must be treated
before it is discharged into the water bodies. Spent caustics wastewater
streams are broadly classified as; sulfidic (produced during ethylene and
LPG scrubbing and contains sulphides and mercaptans), cresylic (pro­
duced during gasoline scrubbing and contains phenolic, cresol, and
sulphur compounds), and naphthenic (produced during kerosene,
diesel, jet fuel, and petroleum scrubbing and contains sulphur com­
pounds) (Alipour and Azar, 2020). The segregation of each kind of spent
caustic stream is not economic. These streams are mixed together in
petroleum refinery and sent for further purification and treatment. The
methods such as thermal processes (Incineration and wet air oxidation),
chemical oxidation (neutralization, neutralization combined with AOP),
biological degradation, and electrochemical oxidation (Electro­
coagulation, and Electro-Fenton) have been used to treat spent caustic
wastewater (Dadari et al., 2016; Ye et al., 2021). Every method has its
own merits and demerits. An electrocoagulation method was employed
for the treatment of caustic wastewater collected from a local refinery
(initial sulphide concentration of 34,517 mg/L and COD of 72,450 mg/
L) (Hariz et al., 2013). More than 90% of sulphide and COD removal was
found under optimum conditions (time of 30 min and pH of 9.0). Sabri
et al. (2018) used hydrophobic ionic liquid for the treatment of spent
caustic wastewater; accordingly, the COD of spent caustic was reduced
from 64166 mg/L to 63.0 mg/L. An isolated fungi (i.e., Aspergillus sp.
SMHS-3) was used to treat low-diluted spent caustic wastewater. It was
found that Aspergillus sp. SMHS-3 removed 16% of COD, 10% of TDS,
and 55% of sulphite within 10 days (Gholipour et al., 2018). However,
biological treatment is not recommended as a pre-treatment option for
spent caustic wastewater due to its highly alkaline nature (induces
swelling of cells and inhibits enzymatic activity) and presence of a high
concentration of phenols and sulphides (Heidarinasab and Hashemi,
2011; Li et al., 2021a; Li et al., 2021b). Wet air oxidation removed about
80% of COD from spent caustic wastewater (Alipour and Azari., 2020).
However, it is energy-intensive and associated with high operating cost
(Rita et al., 2020).
In refinery, spent caustic wastewater is usually generated as batch
dumps which are further neutralized with the acidic stream of refining
processes or equalized before being treated or discharged to the general
wastewater treatment plant. Sulphuric acid (98%) and hydrochloric acid
are suitable to neutralize the spent caustic wastewater (Samadiafshar,
2012). According to Alipour and Azari (2020), acid neutralization of
spent caustic wastewater converts compounds into their basic elements.
Neutralization is the most suitable technique for the treatment of spent
caustic wastewater due to its extremely alkaline nature (Rita et al.,
2020). Further, neutralization combined with advanced oxidation pro­
cesses could be a good choice for the pre-treatment of spent caustic
wastewater. However, this approach is associated with high cost. Spent
caustic wastewater can also be treated by neutralization with flue gas,
where hydroxides are converted to carbonates. A typical segregated
approach for the treatment of spent caustic wastewater is represented in
Fig. 4.
One more option for the management and cut off the waste disposal
cost of spent caustic wastewater is to use it in the pulp and paper mill’s
Kraft process. Heidarinasab and Hashemi (2011) reported that Shell
Puget Sound Refinery in the United States sent their spent caustic
effluent to nearby pulp and paper mill, which subsequently reduced the
disposal cost of spent caustic of about $ 400,000 per year.
4.3. Sour wastewater and its treatment method
Steam is widely used as a stripping medium in unit processes (e.g.,
atmospheric distillation, vacuum distillation, naphtha hydrotreater,
fluidized catalytic cracking, etc.). It is further condensed as an aqueous
phase. The produced wastewater contains a high concentration of
hydrogen sulphide and ammonia, called “sour wastewater” (Fasihi et al.,
2020; Sahraeian et al., 2021). In general, sour wastewater is classified as
phenolic (contains hydrogen sulphide, ammonia, mercaptans, phenols,
hydrocarbons, suspended solids, and a small amount of carbon dioxide)
and non-phenolic compounds (contains hydrogen sulphide, ammonia,
and carbon dioxide) (Soares et al., 2021). Sour wastewater is extremely
toxic due to the presence of hydrogen sulphide. Also, a high concen­
tration of hydrogen sulphide and ammonia causes corrosion of pipes and
combustion engines (Fasihi et al., 2020). The units namely, atmospheric
and vacuum distillation, hydro-desulfurizers, amine regeneration, FCC,
delayed cokers, Claus process, and visbreaker release sour wastewater
(Bastos et al., 2020; Zahid et al., 2019). According to Zahid et al. (2019),
sour water strippers are the “toilets” of petroleum refineries. In order to
comply with environmental legislation, sour wastewater should be
treated before discharge to the environment. After the refining stage, the
produced sour wastewater is subjected to the sour water treatment unit
to remove the contaminants.
Initially, sour water is sent to the stripper (one or two columns) to
remove H2S and NH3. Sour water strippers are an essential part of the
petroleum refinery and are extensively employed to treat H2S and NH3
from sour water (Soares et al., 2021). The ideal pH for hydrogen sul­
phide stripping is below 5; since above 5, it appears in ions (HS- or S-2).

9
 B. Narayan Thorat and R. Kumar Sonwani
Table 6
Characteristics of PRW, treatment methods, and process efficacy.
Type of Process unit Main pollutants Target pollutant and Treatment methods Applied method Efficiency Reference
wastewater its conc.

Desalting Crude desalting Free oil, ammonia, sulfides, Oil (4000–60,000 Gravity settling, Flocculation, Centrifugal contactor 98.70% Hao et al. (2013)
wastewater suspended solids, dissolved mg/L) Hydrocyclone separation, Coarse graining,
organic compounds (e.g., Centrifugal contactor
PAHs and naphthenic COD (417–1241 mg/ Demulsification, Coagulation, Adsorption, Coagulation (aluminum sulfate) Ye et al. (2021)
acids) L) Biodegradation, Electrochemistry,
Oxidation
Oil (400–2500 mg/L), Gravity separators, Hydrocyclones, Media Swirling flotation coupled with 98.4% Oil, COD Wu et al. (2021)
COD (2500–13000 filtration, Centrifugal seperator, medium coalescence 94.5%, Suspended
mg/L) Membrane filtration solid 97.6%
Oil (1078.9 mg/L), Gravity separator, Flotation, Electro- Hydrocyclone-intensified filter Oil 99.1%, Suspended Sun et al. (2021)
Suspended solids flotation, Adsorption, Coalescence, solids 85.4%
(214.2 mg/L) Membrane
COD (1000–5000 Nanofiltration membrane greater than75% Dadari et al.
mg/L) (2016)
Atmospheric distillation Hydrogen sulfide, H2S (98.4 mg/L) Membrane contactors followed greater than95% Minier-Matar
columns ammonia, mercaptans, striping in NaOH solution et al. (2017)
Sour water Vacuum distillation towers phenols, hydrocarbons, H2S (1300 mg/L) Catalysis (V2O5) 100% Sahraeian et al.
stream and suspended solids (2021)
Delayed cokers H2S (10–60 mg/L) Catalysis, Amine-Claus process (stripping), Trickling biofilter and biofilter 251.93 g S m3/h Fasihi et al.
Biodegradation (Elimination capacity) (2020)
Hydro-desulfurizers (HDS) H2S (100 mg/L) Chemical scavenger (monoethanolamine Coupling system: membrane Dardor et al.
(MEA) and N-methyldiethanolamine contactor + NaoH + UV light + Air (2020)
(MDEA), NaOH, triazine-based
watersoluble chemicals)
10

Fluidized catalytic cracking
(FCC) units
Amine regeneration units
Claus process
Visbreaker fractionators
Naphtha hydrotreater
Diesel hydrotreater
Spent caustic Ethylene unit, kerosene
wastewater Merox spent caustic
(Used NaOH (Refining keresene/jet
solution) unit), LPG unit, Gasoline
unit, FCC, Visbraker,
Odorous, highly colored,
contain sodium sulfides,
mercaptans, phenols, thiol,
amine, and emulsifed
hydrocarbon
Dissolved organic H2O2, H2O2/UV, UV, photocatalysis, Fenton and photo-Fenton greater than90% Coelho et al.
carbon (300–440 mg/ ozonation, Fenton and photo-Fenton (2006)
L)
electrocoagulation
Sulphide (9500 mg/ Wet air oxidation (WAO), biological Suspension crystallization 89.40% Yuan et al.
L) treatmenr, Incineration (2020)
TOC (20417 mg/L), Incineration, Neutralization, Fenton Neutralization + Fenton oxidation 70% TOC, 80% COD, Rita et al. (2020)
COD (84570 mg/L), oxidation (N + FO) & Neutralization + 95% O&G by N + FO &
O&G (15255 mg/L) liquid–liquid extraction (N + LLE) 97% TOC, 96% COD,
99% O&G by N + LLE
Thermal processes (Inceneration, WAO), Alipour and
chemical oxidation (Chem, AOP), Azari (2020)
biological methods, membrane separation,

Bioresource Technology 355 (2022) 127263

and electrochemical (Electrocoagulation,
and Electro-Fenton
COD (64166 mg/L) Incineration, chemical oxidation, AOPs Ionic liquid (tetrahexylammonium greater than90% COD Sabri et al.
dihexyl-sulfosuccinate and (2018)
trioctylmethylammonium
salicylate)
Sulphide (720 mg/L) Extractive desulfurization and oxidative Aspergillus sp. SMHS-3 55% Gholipour et al.
desulfurization (2018)
COD (400 mg/L), Chemical oxidation process and wet air Microbial fuel cell 89.1% COD, 97.9% Fazli et al.
Sulphide (0.1 mg/L) oxidation Sulphide (2018)
COD (1420 mg/L), Acid neutralization + steam stripping, Electro-Fenton 81.2% COD, 99.9%
Sulphide (6820 mg/ WAO, AOPs Sulphide
(continued on next page)
B. Narayan Thorat and R. Kumar Sonwani Bioresource Technology 355 (2022) 127263

Whereas, suitable pH for ammonia stripping is above 10 to avoid the

ammonium (NH4+) formation that cannot be stripped. Therefore,

Davarnejad and

Li et al. (2017)
Bakhshandeh
two-stage strippers (one for hydrogen sulphide and other for ammonia

Salahi et al.
Hariz et al.
Reference
stripping) are generally recommended. Two-stage stripper is expensive.

(2018)

(2013)

(2013)
Therefore, single stage stripper is usually employed with a moderate pH
range of around 8.0 to allow adequate removal of both gases. Sour
wastewater received after stripping is sent it to the pre-treatment stage

greater than80% COD,

grease, COD 80.3, and

to reduce the phenolic compounds and finally sent to a main wastewater

95% COD, 99% total

TDS, 99.9 % Oil and
100 % TSS, 44.4%
treatment plant for further treatment. Steam is commonly used as a
greater than95% striping medium that may be directly injected to stripper or reboiler to
stripper. Fig. 5 demonstrates a typical segregated approach for the
Efficiency

Sulphide

nitrogen
treatment of sour wastewater. Initially, sour water received from com­

76.9
plex refinery processes is flushed in a tank. The vapours formed in the
tank are sent to the flare. Whereas, separated oil is subjected to oil slops
for further treatment. Sour water is then sent to a storage tank followed
by stripper. The vapours generated in stripper is sent to the sulphur
recovery unit. Whereas, the stripped water is routed to the wastewater
Nano-porous membrane

treatment plant. After that, the striped water is subjected to a secondary

Anaerobic and aerobic

oil/water separator, equalization tank, biological treatment, clarifica­

Electrocoagulation

tion, and tertiary treatment (or polishing). The details of these units are
Applied method

biodegradation

described in section 3. Sour water generated in petroleum refineries is

considered the low TDS stream compared to the desalter and spent
caustic wastewater (Jafarinejad and Jiang, 2019). Therefore, an API
separator is generally not recommended for the low total dissolved
stream (IPIECA, 2010).
Gravity separation, dissolved air flotation,

Various treatment methods, namely chemical scavenger (mono­

Oil separation, air floatation, anaerobic
Acid neutralization + steam stripping,

ethanolamine (MEA) and N-methyldiethanolamine (MDEA), PETRO­

SWEET, SULFIXTM) (Dader et al., 2020), membrane contactor (Bastos
adsorption, biological treatment,

et al., 2020), steam strippers (Soares et al., 2021), biofilters, and AOPs
sedimentation, hydrocyclone

and aerobic biodegradation

have been used for the treatment of sour wastewater. Each technique has
its own merits and demerits. For example, steam strippers are more
Treatment methods

suitable for treating large scale of hydrogen sulphide (1 ton/day) from

sour water; however, large energy requirements, corrosion, foaming,
WAO, AOPs

and weeping are the major issues associated with steam stripping.
Similarly, the regenerative chemical scavenger is another better option
to treat the sour wastewater but the high cost resists its application.
Bastos et al. (2020) employed a reverse osmosis process to treat the
phenolic sour water collected from the cracking complex at the Sines
Sulphide (34517 mg/

TSS (250 mg/L), TDS

L), phenols (420 mg/

COD (650–1150 mg/

Target pollutant and

COD (72450 mg/L),

(8200 mg/L), COD

refinery. Reverse osmosis removed 98% of phenols, 99% of COD, and

L), Total nitrogen
(456 mg/L), BOD

99% of TOC from phenolic sour water. They also compared the sour
(35–70 mg/L)
(321 mg/L)

wastewater treatment circuit of Sines Refinery with proposed membrane

its conc.

treatment (E-Supplementary data) and suggested that the effluent

received after membrane treatment could be employed in cooling tower.
L)

L)

aromatic, asphaltenes, and

4.4. Oily wastewater and its treatment method

Oil and grease, aliphatic,

nitrogen Sulphur oxygen

A significant amount of oils and greases are released during pro­

(NSO) compounds
Main pollutants

duction, transportation, refining processes, and leakage (e.g., crude

tanks, slop tanks, etc.), which contaminates the process water and is
referred to as oily wastewater (An et al., 2017). According to Varjani
et al. (2020), generally, four types of hydrocarbons, namely aliphatic,
aromatic, asphaltenes, and nitrogen sulphur oxygen (NSO) associated
compounds, are present in oily wastewater. It is sticky, clogs drainpipes,
Production, transportation,

leakage (e.g., crude tanks,

and produces an unpleasant odour under anaerobic conditions (Xu and

refining processes, and

Zhu, 2004). The technologies, namely API separation, hydrocyclone,

adsorption, coagulation-flocculation, biodegradation, dissolved air
slop tanks, etc.)

flotation, reverse osmosis, membrane filtration, and AOPs are widely

Process unit

employed for the treatment of oily wastewater (An et al., 2017). A nano-
porous membrane was used treat the oily wastewater of petroleum re­
finery (Salahi et al., 2013). They reported that the nano-porous mem­
Table 6 (continued )

brane removed suspended solids, oil, and grease, COD of 100%, 99.9%,
Oily wastewater

and 80.3%, respectively. An anaerobic–aerobic biological system

removed 95% of chemical oxygen demand and 99% of total nitrogen
wastewater

from heavy oil refinery wastewater without pre-treatment (Li et al.,

Type of

2017). Every technology has its specific scope and individual processes
may not achieve the desired level of treatment as per environmental

11
B. Narayan Thorat and R. Kumar Sonwani Bioresource Technology 355 (2022) 127263

Fig. 2. Schematic diagram of a typical desalter wastewater treatment system (Modified from Jafarinejad and Jiang, 2019).

Fig. 3. Pre-treatment of desalter wastewater in (a) floating roof tank and (b) floating roof tank followed by Hydrocyclone and stripper (modified and redraw from
IPIECA, 2010).

Fig. 4. Schematic diagram of a typical spent caustic wastewater treatment system (Modified from IPIECA, 2010).

regulation due to the complexity of oily wastewater. Therefore, the
combination of physical, chemical, and biological treatment is suggested
to achieve satisfactory results. A typical segregated system recom­
mended for the treatment of desalter wastewater can be used for the
treatment of oily wastewater (Fig. 2) (Jafarinejad and Jiang).
5. Combined treatment system and its selection strategy
5.1. Overview of combined treatment system
Currently, the main routes for the treatment of complex petroleum
wastewater are biodegradation (i.e., bioreactors) and advanced oxida­
tion processes (e.g., photocatalysis, ozonation, wet air oxidation, etc.).
Biodegradation refers to the degradation of pollutants by the metabolic
activity of microorganisms. It is considered one of the better options due

12
B. Narayan Thorat and R. Kumar Sonwani
Fig. 5. Schematic diagram of a typical sour wastewater treatment system
(Modified from Jafarinejad and Jiang, 2019).
to its eco-friendly and cost-effectiveness than the other treatment tech­
niques (Sonwani et al., 2020). However, conventional biological treat­
ments do not always offer acceptable outcomes due to the presence of
toxic or recalcitrant pollutants in PRW (Goswami et al., 2018). In
addition, it is ineffective when wastewater has a low biodegradability
index (BOD5/COD < 0.2) (Malik et al., 2020). The literature indicates
that the wastewater released from many petroleum refineries has a low
biodegradability index (Karray et al., 2020; Mirbagheri et al., 2014;
Razavi and Miri, 2015). For example, Karray et al. (2020) reported that
refinery wastewater has a low biodegradability index (BOD/COD of 0.2)
with the BOD and COD of 1310 mg/L and 6444 mg/L, respectively.
Previous studies suggested that AOPs are the most feasible and highly
efficient route for the treatment of such biologically persistent waste­
water (Lofrano et al., 2013; Rostam and Taghizadeh, 2020). AOPs are
associated with the applications of hydrogen peroxide (H2O2), ozone
(O3), and photocatalyst to produce free hydroxyl radicals (OH•), which
are highly reactive and non-selective with the organic compounds
(Malik et al., 2020). However, high energy requirements (e.g., UV-
radiation and ozone), large chemical consumption (e.g., catalysts and
oxidizers), controlled operating conditions, and possibilities of hazard­
ous intermediates generation are major drawbacks associated with AOPs
(Rostam and Taghizadeh, 2020; Oller et al., 2011). Along these lines,
one potential alternative is to use AOPs as a pre-treatment step to
initially mineralize the recalcitrant organic compounds (i.e., biologi­
cally persistent pollutants) into more biodegradable intermediates that
can be treated further by biological processes (Oller et al., 2011). A
combined treatment system can provide a better solution for the treat­
ment of complex PRW (Rostam and Taghizadeh, 2020). The integration
of two treatment techniques, namely AOPs and biodegradation, is
referred to combined treatment system (e.g., ozonation followed by
MBBR, photocatalysis followed by PBBR, etc.). However, the selection of
a suitable combined system for the treatment of specific industrial
wastewater is a highly complex job. In the next section, an overview of
the combined treatment system is described.
5.2. Strategy for the selection best combined treatment system
The selection of one or more processes to develop a combined
treatment system depends on the quality of effluent discharge guidelines
to be met and the most effective management with the economical route.
It should also be considered whether the AOPs are integrated as pre-
treatment or post-treatment with the biological process to develop an
appropriate combined treatment system. For example, it is well
informed that the pre-treatment of wastewater by AOPs is beneficial to
initially convert recalcitrant organic pollutants into more biodegradable
intermediates (Malik et al., 2020). However, at the same time, there are
some possibilities that the oxidation step could adversely affect the
performance of the overall treatment system. These possibilities are: (1)
produced intermediates may be more complex and less biodegradable
than the parent state of the pollutant, (2) too much pre-oxidation may
13
Bioresource Technology 355 (2022) 127263
lead to the formation of wastewater with very less metabolic value (i.e.,
low organic and nutrients) for the microorganisms, and (3) application
of a large amount of chemical in AOPs generates excessive oxidants (e.g.,
hydroxyl radicals, ozone molecules) and metal salts (e.g., catalyst)
which may be toxic and biocides to microorganisms (Malik et al., 2020;
Oller et al., 2011). Therefore, benchmarks namely wastewater charac­
teristics (e.g., BOD, COD, TOC, TDS, TSS, ions, non-volatile compounds,
etc.), biodegradation mechanisms, metabolic pathway and kinetics, ef­
fects of pre- and -post treatment of AOPs on toxicity and biodegrad­
ability, etc. must be considered to establish a combined research
methodology (Oller et al., 2011; Sonwani et al., 2021b). Also, the pa­
rameters (e.g., pH, temperature, pollutant concentration, microorgan­
isms, catalyst amount, etc.) affecting the performance of individual
treatment units. These parameters should be optimized to enhance the
performance of the combined treatment system. A strategy to estimate
the practicability of the combined system to treat complex PRW is
summarized in Fig. 6.
5.2.1. Toxicity test
PRW contains a wide range of toxic pollutants (e.g., benzene,
toluene, xylene, benzo[a]pyrene, phenanthrene, hydrogen sulphides,
heavy metals, etc. (Yonis et al., 2020; Varjani and Upasani, 2017). The
wastewater may exert a great threat to the terrestrial as well as the
aquatic environment if released directly into the environment. There­
fore, it is essential to evaluate the biodegradability and toxicity of AOPs
treated effluent before it is sent to a biological unit for further degra­
dation (Sonwani et al., 2021c). It is also imperative to estimate the
toxicity of the wastewaters which are being discharged into the open
water bodies. Toxicity is a measure of the degree to which single or
multiple constituents present in PRW can cause adverse impacts on
human beings, aquatic animals, and ecosystems (Metcalf and Eddy,
2014). Toxicity test (also known as a safety assessment test) uses or­
ganisms (e.g., fish, plants, bacteria, etc.) to evaluate the toxic effects of
recalcitrant substances present in wastewater. Various organisms such
as bacteria (e.g., Vibrio fischeri and Bacillus subtilis), invertebrates (e.g.,
Paracentrotus lividius and Daphnia magna), algal species (e.g., Pseudo­
kirchneriella subcapitata and Selenastrum capricornutum), plants (Avena
sativa, Vigna radiata, and Cicer arietinum), and fish species (e.g., Poecilia
vivipara) have been employed to evaluate the adverse impacts of toxic
compounds in the aquatic ecosystem (Babu et al., 2019). Based on
duration, the toxicity tests can broadly be classified as; (a) acute toxicity
(typically a lethal response is observed within 48 or 96 h) and chronic
toxicity (lethal response observed over long-term, often 1/10 of life
span) (Metcalf and Eddy, 2014). In the last few decades, acute toxicity
testing.
(i.e., bacterial toxicity and phytotoxicity) have gained significant
attention to evaluate the toxicity of substances.
5.2.1.1. Bacterial toxicity. This methods utilize the metabolic activity of
bacteria species (as inhibition tests or bioluminescence) to estimate the
toxicity of pollutants (Babu et al., 2019). It is based on the inhibition of
the bioluminescence of luminescent bacteria (e.g., Vibrio fischeri, Pseu­
domonas fluorescens, etc.) as a result of the alteration of the metabolic
activity in the presence of toxic pollutants (Bharagava et al., 2018; Iqbal
et al., 2017). These luminescent bacteria naturally emit light at 490 nm
due to luciferase enzyme, which is a flavin-dependent monooxygenase
and transform chemical energy into photons of visible light (Tinikul
et al., 2020). The basic mechanism can be elucidated by the following
biochemical reactions (Eq.7 and Eq. (8)) (Girotti et al., 2008):
(7)
NAD(P)H:FMNoxidoreductase
NAD(P)H + FMN + H + ̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅→ NAD(P)+ + FMNH2
Luciferase
FMNH2 + O2 + R − CHO ̅̅̅̅̅→ FMN + R − COOH + H2 O + Light (8)
Initially, flavin mononucleotide (FMN) is converted into reduced
flavin mononucleotide (FMNH2) via the action of oxidoreductase
B. Narayan Thorat and R. Kumar Sonwani
Fig. 6. A strategy to evaluate the feasibility of combined system for the treatment of complex petroleum refinery wastewater ().
Reproduced from Oller et al. 2011
enzyme. This reduced FMN and a long-chain aliphatic aldehyde (R-
CHO) are further oxidized in the presence of molecular oxygen via the
action of the luciferase enzyme. The light produced by the luminescent
bacterial species (Eq. (2)) is directly proportional to the metabolic ac­
tivity of the bacterial cell. Any inhibition to the metabolic activity (due
to chemical inhibition) of the cell is revealed in decrease in the amount
of light emitted (bioluminescence). The bacterial toxicity is generally
expressed as effective concentration (EC50). EC represents the 50%
reduction in bioluminescence in a specified period (usually, 96 h) on the
exposure to the effective concentration of the toxic substance (Babu
et al., 2019). The following equation determines the percentage inhi­
bition (I %) of bioluminescence:
[ ( )]
Intensityofsample
%Inhibition = 1 − × 100 (9)
Intensityofcontrol
5.2.1.2. Phytotoxicity test. The reuse of petroleum refinery-treated
wastewater in irrigation can offer two essential resources: nutrients
and water. However, it may change the physicochemical and biological
characteristics of soil such as pH, salinity, nutrient, and organic content
(Haq et al., 2021; Leiva et al., 2019). In addition, excessive concentra­
tion of compounds may lead to the accretion of possibly harmful pol­
lutants into soil. In this context, the phytotoxicity text can provide a
quick overview of the suitability of treated wastewater in irrigation.
Phytotoxicity test includes the study of the seed germination rate,
leaf number, root and shoot length measurement, and enzyme activity in
the presence of toxic pollutants (phytotoxins) (Sonwani et al., 2021c). In
this test, plant species such as Vigna radiata, Cicer arietinum, Lepidium
sativum, Chlorella vulgaris, etc., have been tested (Bankole et al., 2018;
Leiva et al., 2019). The previous researchers have described the details
of the phytotoxicity procedure (Bankole et al., 2018; Sonwani et al.,
2021c). The following equation can be applied to estimate the per­
centage of seeds germination:
No.ofseedsgerminated
%Seedsgemination = × 100 (10)
No.seedssowed
As the concentration of toxic substances in water increases, the
germination, shoot length, and root length of seeds decrease due to toxic
substances and ultimately inhibit plant growth. Recently, Haq et al.
(2018) investigated the toxicity of PRW by plant bioassay (i.e., Vigna
radiata seeds). They found that the Vigna radiata seeds irrigated in un­
treated PRW significantly reduced seeds germination, root length, and
14
Bioresource Technology 355 (2022) 127263
shoot length by 50%, 85.1%, and 69.3%, respectively, after 5 days of
treatment than to control.
5.2.2. Biodegradability test
The biodegradability test refers to the fraction of the organic matter
in wastewater that can be easily degraded by microorganisms (i.e.,
bacteria, fungi, and algae). The biodegradability assessment of waste­
water is not only necessary during biological treatment, but it is also
required in a combined system to treat recalcitrant contaminants. The
biodegradability of the wastewater can be estimated by the following
benchmarks; (i) Biodegradability index (BOD5/COD), (ii) Long
activated-sludge biodegradability test (e.g., Zahn–Wellens test), and (iii)
Oxygen uptake rate (OUR) by respirometric measurements (Oller et al.,
2011). The above tests are based on the analysis of common parameters,
namely BOD, COD, and DOC.
BOD5/COD is a conventional and most widely employed parameter
to evaluate the biodegradability of organic matters in wastewater. It
offers a most accurate approach to find out whether the pollutants are
biodegradable or not under aerobic conditions. It can be evaluated by
estimating the BOD (generally 5 days) and COD ratio of wastewater. It is
well reported that if the wastewater has low BOD5/COD (<0.2) then it
represents poor biodegradability, whereas high BOD5/COD (greater
than0.4) represents wastewater that can easily be biodegraded (Lofrano
et al., 2013; Malik et al., 2020). The ratio of BOD5/COD between 0.2 and
0.4 denotes wastewater is partially biodegradable (Malik et al., 2017).
Zahn–Wellens test is employed to estimate the biodegradability of
various kind of pollutants. A large amount of activated sludge (i.e.,
biomass containing a high concentration of microorganisms) is added to
wastewater containing organic contaminants and mineral nutrients. The
whole mixture is agitated at 20–25 ◦ C under dark for 28 days. The
biodegradability of wastewater is estimated by measuring the DOC (or
COD) at regular time intervals. The ratio of reduced DOC to the original
DOC gives an approximate estimation of the biodegradability index. If
the ratio of reduced DOC to the original DOC is more than 70%,
wastewater is suitable for biological treatment (Oller et al., 2011). The
measurement of OUR is another method to estimate the biodegradability
of wastewater by respirometric measurements (short analysis). In this
test, OUR of microorganisms during the break down of organic sub­
stances is evaluated after 20 min, which is further correlated to the
reduction in BOD or COD (Drewnowski, 2014). The ratio of readily
biodegradable COD to COD (CODrb/COD) is used as the
B. Narayan Thorat and R. Kumar Sonwani
biodegradability index. A ratio of more than 0.1 indicates the waste­
water is biodegradable, whereas below 0.05 represents it is not biode­
gradable. The ratio between 0.05 and 0.10 is indicates the wastewater
being partially biodegradable (Oller et al., 2011).
Both methods (i.e., toxicity and biodegradability) can be employed
to develop a combined treatment system. The conventional biodegrad­
ability test (i.e., BODx/COD rate) is most widely used to estimate the
improved biodegradation rate. Malik et al. (2017) have evaluated the
feasibility of ozone oxidation as a pre-treatment option to enhance the
biodegradability index (BOD5/COD) of distillery wastewater. They re­
ported that the biodegradability index of distillery wastewater was
significantly improved from 0.17 to 0.6 by ozone pre-treatment. In
another study, the biodegradability index of complex petrochemical
wastewater was improved (0.3 to 0.6) through pre-treatment by photo-
Fenton method (Derakhshan and Fazeli, 2018).
6. Economic and life cycle assessment
Petroleum refineries have been reported among the most polluting
industries and exert adverse impacts on both water and carbon cycles.
The sustainable development goals, zero liquid discharge (ZLD), water
conservation, and water reclamation are vital for minimizing the wastes
and their adverse impacts (Hashemi et al., 2022). In this regard, the
economic and life cycle assessment are important subjects for consid­
eration. Generally, two important cost components, i.e., capital expen­
ditures (CAPEX) and operating expenditures (OPEX) are involved to
estimate the economic viability of the wastewater treatment plant,
including petroleum refineries. CAPEX includes direct and indirect
costs. Direct CAPEX includes the capital costs associated with land,
construction facilities, equipment installation, auxiliary equipment, and
tanks (Ghaffour et al., 2013). Indirect CAPEX involves transportation
and insurance costs, project management costs, and working capital
(Hashemi et al., 2022). Similarly, OPEX embraces the costs for the
chemical supply, process utilities, maintenance, electricity, labour,
depreciation disposal costs, property taxes and insurance, and general
expenses (Tian et al., 2020). According to Sonwani et al. (2021a), the net
present value (NPV) method can be employed as a quantitative measure
to evaluate the capital required for competing products and processes in
current terms. The higher NPV than the reference design indicates the
economic viability of the proposed project. The OPEX and NPV of the
wastewater treatment plant can be evaluated by the following eqs. (11)
and (12).
∑
T
OPEXt
OPEX = (11)
t=1 (1 + r)t
∑ effluent can further be used in fire water make up, cooling tower, and
T
Ct
NPV = − CAPEX (12)
t=1 (1 + r)t
∑
T
It
I = (13)
(1 + r)t
t=1
where OPEX is total operational expenses; OPEXt is operational ex­
penses at time t; It signifies incomes at time t; Ct represents net cash flow
at time t; r is the discount rate of 5%, and T is the time horizon of the
project, 30 years. An economic assessment was carried out for the
treatment of petroleum refinery wastewater using a membrane system
(Hashemi et al., 2022). They reported that the initial investment for the
launch of this treatment system was estimated at $255,750. Also, the
regeneration cost for the treated wastewater was $0.24/m3. In another
study, the economic evaluation of wastewater treatment plants was
estimated (Garrido-Baserba et al., 2018). They found that the cost of
pipeline distribution and operation varied from 60% to 70% of the
overall costs.
Life cycle assessment is an effective tool to assess the environmental
15
Bioresource Technology 355 (2022) 127263
impacts of a product or process from its origin to its final disposal (Igos
et al., 2014). This approach has also been widely employed to evaluate
the environmental loads from the wastewater treatment systems;
(including petroleum refineries) and reclamation processes (Sonwani
et al., 2021a; Yenkie, 2019). The load imposed on the environment from
wastewater treatment plants of petroleum refineries may be ascertained
by accounting for the resources and energy (inputs) consumed at each
stage (i.e., unit operations and unit processes) in the life cycle of a
product and the resulting emission of pollutants (e.g., hydrogen sul­
phides, ammonia, hydrocarbons, etc.) (Output) (Hashemi et al., 2022;
Sonwani et al., 2021a). The adverse impacts of inputs and outputs on
environmental sustainability, human health, aquatic life, etc., are
studied. Generally, the life cycle assessment study consist of four stages,
namely (i) goal and scope definition, (ii) inventory analysis, (iii) impact
assessment, and (iv) interpretation of the outcomes (Muralikrishna and
Manickam, 2017; Tian et al., 2020). Recently, the life cycle assessment
of petroleum refineries wastewater was studied to evaluate the envi­
ronmental impacts (Hashemi et al., 2022). In their study, eight envi­
ronmental indicators, namely ozone-depleting potential, global
warming, greenhouse gases, acidification potential, eutrophication po­
tential, health effects, environmental toxicity potential, and photo­
chemical oxidation potential were included. They reported that global
warming, greenhouse gases, health effects, and photochemical oxidation
potential had shown the maximum environmental impact among eight
indicators.
7. Research gap and future perspectives
Over the last few decades, the effective treatment of PRWs has
received notable attention due to the significant growth of the petro­
leum industry and environmental legislation imposed by government
agencies (such as USEPA, WBG, CPCB, etc.). In this context, various
physical (e.g., skimmer tank, DAF, etc.), chemical (e.g., coagulation-
flocculation, ozonation, AOPs, etc.), and biological (e.g., tricking fil­
ter, ASP, etc.) treatment processes have been extensively employed.
However, most of the published experimental studies focused on bench-
scale laboratory studies, which is mainly based on simulated wastewater
and ignore real case experimental studies. In addition, each of the above
methods has its specific scope, and individual process may not provide
the desired level of treatment as per environmental guidelines due to the
complex nature of PRW. Therefore, the combination of physical,
chemical, and biological treatment is suggested to attain acceptable
results. Further, the segregation of complex PRW into four streams (i.e.,
desalter wastewater, sour wastewater, spent caustic wastewater, and
oily wastewater), followed by separate treatment according to their
characteristics, can improve the overall treatment efficacy. The treated
green belt development. Such approach can be more useful in water-
scarce regions. Biological treatment (i.e., biodegradation) of PRW is
considered a most promising option due to its eco-friendly and cost-
effective nature than other treatment techniques. However, conven­
tional biological treatment is ineffective, especially when wastewater
has a low biodegradability index (BOD5/COD < 0.2) and contains a
significant amount of POPs. Along these lines, a combined treatment
system (i.e., combination of AOPs (as pre- or post- treatment) with
biological treatment) can provide better outcomes than the individual
process. The selection of the best-combined system for the treatment of
specific wastewater is a highly complex job. In this context, toxicity and
biodegradability test during and after treatment are the most important
indicators and must be evaluated before applying to real wastewater. In
the last few years, many researchers have developed combined treat­
ment systems (i.e., AOPs and biological systems) to treat various kinds of
pollutants. However, combined treatment technologies are under-
explored area, and most of the studies are mainly concentrated on
bench-scale laboratory experiments, yet these are not practically applied
in industries. The combined technologies are associated with higher
B. Narayan Thorat and R. Kumar Sonwani
cost, extensive technical knowledge, and regular monitoring of toxicity
and biodegradability parameters. Although the combined treatment
system offered higher removal efficiency of recalcitrant pollutants, the
removal mechanisms of most of the pollutants have not yet been found
out. Therefore, future investigations should focus on the identification of
intermediates, reaction mechanisms, and scale-up the cutting-edge
combined treatment system with real industrial wastewater. From the
real application point of view, knowledge of reaction kinetics, mass
transfer mechanisms, modelling aspects, and techno-economic aspects
should be assessed accurately. The life cycle assessment and techno-
economic aspect of wastewater treatment should also be considered.
8. Conclusions
To date, various physicochemical and biological technologies have
been employed to treat the PRW. Each of the above technologies has its
specific scope. The individual process may not provide the desired level
of treatment due to the complex nature of PRW, especially when
wastewater has a low biodegradability index (BOD5/COD < 0.2) and
contains persistent pollutants. This review highlighted the current
technologies and future perspectives to treat such complex PRW. A
combined treatment system (i.e., combination of AOPs (as pre- or post-
treatment) with biological treatment) has been discussed to construct a
perspective map and implement the proposed system efficiently.
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.
Acknowledgment
The authors thankfully acknowledge the Institute of Chemical
Technology, Mumbai–Indian Oil Odisha Campus, Bhubaneswar, India,
for providing financial support and laboratory facilities to execute the
work. This work acknowledges the Indian Institute of Petroleum and
Energy (IIPE), Visakhapatnam, India, for providing laboratory facilities
to execute the work.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.biortech.2022.127263.
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