Environ Monit Assess (2022) 194:875

https://doi.org/10.1007/s10661-022-10569-9

Partially hydrolyzed polyacrylamide: enhanced oil

recovery applications, oil‑field produced water pollution,
and possible solutions
Shatha Al‑Kindi · Saif Al‑Bahry ·
Yahya Al‑Wahaibi · Usman Taura · Sanket Joshi

Received: 31 October 2021 / Accepted: 19 March 2022 / Published online: 13 October 2022
© The Author(s), under exclusive licence to Springer Nature Switzerland AG 2022

Abstract Polymers, such as partially hydrolyzed an environmentally safe manner from the produced
polyacrylamide (HPAM), are widely used in oil fields water before proper disposal. Several chemical and
to enhance or improve the recovery of crude oil from thermal techniques are employed for the removal of
the reservoirs. It works by increasing the viscos- HPAM, but they are not so environmentally friendly
ity of the injected water, thus improving its mobility and somewhat expensive. Among different types
and oil recovery. However, during such enhanced oil of treatments, biodegradation with the aid of indi-
recovery (EOR) operations, it also produces a huge vidual or mixed microbes (as biofilms) is touted to
quantity of water alongside oil. Depending on the be an efficient and environmentally friendly way to
age and the stage of the oil reserve, the oil field pro- solve the problem without harmful side effects. Many
duces ~ 7–10 times more water than oil. Such water researchers have explored and reported the potential
contains various types of toxic components, such as of such bioremediation technology with a variable
traces of crude oil, heavy metals, and different types removal efficiency of HPAM from the oil field pro-
of chemicals (used during EOR operations such as duced water, both in lab scale and field scale studies.
HPAM). Thus, a huge quantity of HPAM contain- The current review is in line with United Nations Sus-
ing produced water generated worldwide requires tainability Goals, related to water security–UNSDG
proper treatment and usage. The possible toxicity of 6. It highlights the scale of such HPAM-based EOR
HPAM is still ambiguous, but its natural decomposi- applications, the challenge of produced water treat-
tion product, acrylamide, threatens humans’ health ment, current possible solutions, and future possi-
and ecological environments. Therefore, the main bilities to reuse such treated water sources for other
challenge is the removal or degradation of HPAM in applications.

Keywords Partially hydrolyzed polyacrylamide ·

S. Al‑Kindi · S. Al‑Bahry
Department of Biology, College of Science, Sultan Qaboos Enhanced oil recovery · Produced water ·
University, Muscat, Oman Acrylamide · Toxicity · Bioremediation

S. Al‑Bahry · U. Taura · S. Joshi (*)

Oil & Gas Research Center, Sultan Qaboos University,
Muscat, Oman Introduction
e-mail: [email protected]
The majority of crude oil-producing countries (mainly
Y. Al‑Wahaibi
Middle Eastern countries) belong to arid regions, hav-
A’Sharqiyah University, Postal Code: 400, P.O. Box 42,
Ibra, Oman ing a scarcity of freshwater sources, potable water, and

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almost no rain throughout the year. Reverse osmosis of reservoirs, the depletion of crude oil in old reservoirs,
seawater, and other technologies, provides majority of and pandemic like COVID-19 has led to fluctuations in
water requirements in such countries, which are either crude oil prices (Abidin et al., 2012; Braun et al., 2022;
inefficient or highly energy-intensive. Apart from oil- Quadri et al., 2015). Extraction of oil as the upstream
producing countries, access to potable and clean water process of the petroleum industry occurs in three
is one of the major challenges, which has been included phases (Fig. 1). At the primary stage, the natural inter-
in the United Nations Sustainable Goals (UNSDG 6). nal pressure of the reservoir from aquifer water and
It states that “Ensure availability and sustainable man- gas helps to extract about 5–10% of total oil reserves.
agement of water and sanitation for all” (https://​sdgs.​ At the second stage, 30–40% of oil is recovered (Al-
un.​org/​goals/​goal6). It may come as a surprise that the Sulaimani et al., 2011; Lucas et al., 2009; Geetha et al.,
petroleum industries are one of the largest consum- 2018; Al-Ghailani et al., 2021; Braun et al., 2022).
ers of fresh or saline water. Daily basis and enhanced At this stage, injected water extracts additional oil by
oil recovery operations require substantial volumes of increasing reservoir pressure. However, researchers
water. Thus, oil industries are suffering from two major reported that approximately 50% of oil remaining in
issues: the requirement of huge volumes of fresh (or place needs to be retrieved by enhanced oil recovery
normal) water for EOR operations, and the treatment (EOR) means (Abidin et al., 2012; Braun et al., 2022;
and safe disposal of huge volumes of oil field produced Gao, 2016; Joshi et al., 2022). A tertiary oil recovery
water. As such, this produced water cannot be used for includes the injection of different materials normally
any other applications (such as irrigation, livestock not present in oil wells. Various EOR methods such as
water supply, wildlife watering), or direct disposal, as thermal, chemical, microbial, and gas injection meth-
it is quite a toxic wastewater source. Besides, this jeop- ods were reported to extract ~ 5–30% of the remaining
ardizes UNSDG 6 as well. The current review paper oil (Al-Ghailani et al., 2021; Braun et al., 2022; Geetha
focuses on one of the possible toxic chemicals, gener- et al., 2018; Lehmköster et al., 2014).
ally used in EOR applications: HPAM and its deriva- Chemical EOR includes flooding of polymers, sur-
tives, and its possible degradation, for better and safe factants, and alkaline to improve the recovery of crude
disposal of produced water. oil (Al-Sulaimani et al., 2011; Al-Ghailani et al., 2021;
At present, fossil fuels are the main source of greater Joshi et al., 2022; Braun et al., 2022; Xue et al., 2022).
than 85% of the energy consumption worldwide, and Polymers, surfactants, and solvents work via chang-
especially crude oil will still play a major role in trans- ing reservoir characteristics to improve the recovery
portation and other industrial sectors for years to come process (Bai et al., 2015; Xue et al., 2022). Among
(Joshi et al., 2022). The difficulty in discovering new them, polymers (synthetic and biopolymers) showed

Fig. 1  The three phases of

crude oil recovery from oil
reservoirs

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efficient oil recovery when combined with water flood- viscosity has direct relation to its chemical structure,
ing, because of their viscosity (Braun et al., 2022; Choi which has negative charges on the chains’ backbone
et al., 2014; Elshafie et al., 2017; Quadri et al., 2015). It causing repulsion between the polymer chains. The
increases the water viscosity (as viscosifying agent) and chain’s repulsion leads to its extension, making the pol-
decreases the reservoir permeability, which helps to dis- ymer more viscous yielding the wanted viscosity even
place the oil uniformly from the porous rocks (Abidin with a low concentration (Lee et al., 2009).
et al., 2012; Braun et al., 2022; Elshafie et al., 2017;
Stokka, 2018; Xue et al., 2022). The main types of pol-
ymers frequently used for EOR are, microbial xanthan Uses of PAM and HPAM
gum and synthetic chemicals — polyacrylamide (PAM)
and partially hydrolyzed polyacrylamide (HPAM) (Al- PAM and HPAM performance depends on their molecu-
Sabahi et al., 2018; Braun et al., 2022; Martin et al., 1983; lar weight and degree of hydrolysis (Abidin et al., 2012).
Xue et al., 2022). HPAM is a water-soluble, commonly They are often used in many industrial applications,
injected polymer into oil reservoirs to improve the water mainly as friction reducers and viscosity modifiers for
flooding process (Xue et al., 2022; Zhao et al., 2008). oil extraction, water purification, soil conditioning, ero-
sion control, and mining (Berdugo-Clavijo et al., 2019;
Braun et al., 2022; Liu et al., 2016; Nyyssölä & Ahlgren,
Polyacrylamide and partially hydrolyzed 2019; Xiong et al., 2018; Yu et al., 2015). In the paper-
polyacrylamide making, PAM works as a strengthener for pulp fiber,
so we have to be careful about wastepaper discharges
Polyacrylamide (PAM) is a synthetic polymer of long- into the environment (Lu & Wu, 2002; Matsuoka et al.,
chain acrylamide subunits, high molecular weight (1000 2002). Usually, PAM is used in sewage treatment, where
to 20 × ­106 g/mol), and a wide range degree of hydrolysis it helps to improve sedimentation and for purification
(Abidin et al., 2012; Joshi & Abed, 2017). It is extremely of drinking water (Filippini, 1986; Yu et al., 2015). In
soluble in water, but not soluble in organic solvents, such addition, it plays a big role in the agricultural field in the
as methanol and hydrocarbons (Lu & Wu, 2002; Braun case of herbicide application, which helps to increase
et al., 2022). PAM is used to produce partially hydro- the viscosity of the sprayed solution. Moreover, it is also
lyzed polyacrylamide (HPAM), which is linear, anionic, used in capillary electrophoresis for DNA sequencing
water-soluble, stable, polymeric, and high molecular (Caulfield et al., 2002).
weight chain of acrylamide ­(C3H5NO) monomers (Bao On the other hand, the application of PAM in bio-
et al., 2010; Braun et al., 2022; Liu et al., 2016; Xiong medical fields is associated with some concerns, since
et al., 2018). In addition, it is highly prone to degradation it contains the neurotoxic acrylamide monomer. The
in high temperature and saline reservoirs (Al-Moqbali usage reluctance is mainly where the polymer encoun-
et al., 2018). The general chemical structure of PAM and ters the patient’s blood for filtration or renal dialysis.
HPAM is shown in Fig. 2. Although both polymers con- Similarly, it is not as safe as a component of therapeutic
tain acrylamide, they are chemically and biologically dif- products. The main issue is about the risk of residual
ferent from that monomer (Caulfield et al., 2002). acrylamide monomer presence with PAM polymeric
In comparison with other polymers, HPAM showed material and the dangers of its degradation (Caulfield
the highest viscosity, highlighting its applications in et al., 2002). According to the Environmental Health
the EOR sector (Choi et al., 2014; Xue et al., 2022). Its Criteria (EHC) number 49 of acrylamide, published

Fig. 2  The chemical struc-

ture of PAM and HPAM

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in 1985 by the World Health Organization (WHO), also cause peripheral neuropathy (Al-Azkawi et al., 2013;
the source of acrylamide in the environment is mainly Liu et al., 2016; Raju et al., 2015). Acrylamide monomer
released from polyacrylamide usage (Filippini, 1986). then discharges into terrestrial and aquatic ecosystems,
Polymers like PAM, HPAM, and xanthan gum inducing abnormalities in animal and plant cells (Yu
work by improving water mobility in the reservoir, et al., 2015). In addition, acrylamide can decompose non-
aiding oil extraction (Abidin et al., 2012). Among thermally to ammonia, and thermally to carbon monox-
them, HPAM’s long-term stability increases its suc- ide, carbon dioxide, and nitrogen oxides (Charoenpanich,
cess in field application and improves oil recovery 2013).
by up to 45% (Al-Sabahi et al., 2018; Braun et al., Another challenge is the difficulty of reinjecting
2022; Choi et al., 2014). HPAM flooding as a ter- HPAM-containing produced water because of its vis-
tiary EOR method functions to increase the injected cosity. Likewise, it is hard to separate the extracted oil
water viscosity and reduce its mobility, which accel- from the produced water and consequential drop in oil
erates the oil extraction rate (Al-Sabahi et al., 2018; yield (Al-Sabahi et al., 2018). Increasing the HPAM
Liu et al., 2016). HPAM viscosity of 150–1000 cP concentration in the produced water makes the sepa-
showed improvement in oil recovery, when compared ration and treatment process quite challenging. This is
with water injection (Seright, 2010), but its usage has due to the anionic charge of HPAM, which increases
temperature and salinity restrictions. So, reservoir the viscosity of oily produced water and decreases the
permeability, rock composition, and oil viscosity are rising tendency (Zhao et al., 2008). Subsequently, oil
important in the selection of the applied polymer in seeps into the sewage, which means that wastewa-
the field (Abidin et al., 2012). ter will exceed the local discharge limit (Bao et al.,
2010). Besides, the contaminated produced water
can leak into groundwater aquifers, which can endan-
Problems associated with PAM and HPAM ger plants, animals, and human health (Sang et al.,
2015). Thus, there is a need to treat produced water
As a byproduct from oilfields using the polymer flood- from acrylamide, but water treatment and disposal are
ing method, produced water is contaminated with HPAM costly (Bai et al., 2015; Warmt-Murray, 2015).
even after conventional treatment (Al-Sabahi et al., 2018). One of the main obstacles in the oil and gas indus-
The potential toxicity of HPAM is neglected, but after try is microbial-induced corrosion (MIC) and reser-
natural or chemical degradation, it can be converted into voir souring because of microbial growth in the pipe-
acrylamide ­(CH2 = ­CHCONH2, Fig. 3). Acrylamide is line system (Hasrizal & Yaakob, 2019). The injection
a toxic chemical that endangers the local ecosystem and of HPAM polymer promotes this effect since the oil-
human health (Bao et al., 2010; Elshafie et al., 2017; Liu field biofilm consortium (mainly sulfate-reducing bac-
et al., 2016). The International Agency for Research on teria) use it as a secondary nutrient (Jia et al., 2018).
Cancer has classified acrylamide as a group “group 2A” Sulfate-reducing bacteria (SRB) work by utilizing
carcinogenic agent. It is known to be a carcinogenic, neu- sulfate as an electron acceptor to produce hydrogen
rotoxic, mutagenic, and teratogenic monomer, and could sulfide ­(H2S). This product reacts with the metal (Fe),
corroding it by forming iron sulfide (FeS) and hydro-
gen (Fig. 4) (Chen et al., 2013; Makhlouf et al., 2018).

Oilfield produced water

Throughout the oil production phase, water produced

along with oil (produced water) is the largest liquid
waste (Ebrahimi et al., 2010; Li et al., 2010; Tellez
et al., 2002). During the oil extraction process, the
injected water flows through the organic phases of the
reservoir because of rock permeability, developed pres-
Fig. 3  The chemical structure of acrylamide sure, and temperature changes. In addition, water is an

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Fig. 4  Microbial induced

corrosion (MIC) in the oil
and gas pipeline system
(Modified from Chen et al.,
2013)

excellent extraction solvent, which means to dissolve Liu et al., 2021). Around 250 million barrels of pro-
a variety of chemical compounds used to enhance the duced water are generated globally, along with 80 mil-
recovery of oil. All these aspects make the composition lion barrels per day of crude oil (Fakhru’l-Razi et al.,
of produced water complex and difficult to manage 2009). It is the main source of oily water, as it reached
(Klemz et al., 2021). The volumes of produced water 90% in the final stage of oil production in many Chi-
in different countries depend on the fields’ location nese oilfields (Lu et al., 2009). Thus, the water-to oil
and the methods of oil extraction. Table 1 highlights ratio is around 3:1, and the ratio is increasing as the
produced water volumes reported from oil and gas oil wells age (Al-Ghouti et al., 2019; Hirayama et al.,
fields of different parts of the world (Al-Ghouti et al., 2002; Liu et al., 2021). Nowadays, there is a big effort
2019; Alsarayreh et al., 2022; Echchelh et al., 2018; worldwide to utilize and treat a significant quantity of
produced water properly.
Different countries have many regulatory standards
Table 1  Volumes of oil and gas fields produced water in dif- and restrictive regulations for oil and gas discharges. The
ferent countries (Al-Ghouti et al., 2019; Alsarayreh et al., United States Environmental Protection Agency (USEPA)
2022; Echchelh et al., 2018; Liu et al., 2021) allows a daily maximum limit of 42 mg/L, and a monthly
Country Produced water (bbl/year) limit of 29 mg/L of treated produced water discharge,
while the People’s Republic of China (PRC) established
USA 21,000,000,000 a monthly limit of less than 10 mg/L, ~ 30 mg/L daily
Australia 207,570,000 discharge in Australia, and a monthly limit of 30 mg/L in
China 45,917,000 Canada. In the UK, following the Oil Pollution Preven-
Colorado 92,274,300 tion Control (OPPC) of the Energy and Climate Change
Iraq 105,853,190 Departments (DECC), the limit is set at 30 mg/L monthly.
Oman 900,000* Moreover, the annually produced water discharge into the
Qatar 50,508,816 sea is 40 mg/L, according to (OSPAR Convention) the
Australia 3.02 × ­1010 Convention of the Protection of the Marine Environment
New Mexico 1.25 × ­109 of the North-East Atlantic. Also, the National Environ-
*
m3/day mental Council (CONAMA) in Brazil stated a monthly

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limit of 29 mg/L, and daily values of 42 mg/L (Fakhru’l- depth and age of the well, and chemical composition of
Razi et al., 2009; Klemz et al., 2021; Tellez et al., 2002). the reservoir (Al-Ghouti et al., 2019). Oilfield produced
The European Union Water Framework Directive (WFD) water contains soluble and insoluble petroleum frac-
in 2000 adopted a decision of “zero discharge” of the tions with different concentrations. The major hydro-
harmful produced water after 20 years (by 2020) to pro- carbons are alkanes, alkenes, alkynes, and aromatics.
tect the marine ecosystem from sequel pollution. Cur- Produced water pH, salinity, temperature, and dissolved
rently, the majority of oil and gas companies in different chemicals affect the amount of oil present in it. In addi-
countries are trying to fulfill this agreement (Klemz et al., tion, dissolved salt concentration as inorganic com-
2021). pounds exceed the seawater levels. Sodium chloride
salt is the main salinity contributor (between 1000 and
40,000 mg/L), but phosphate is present as the lowest
Components of produced water concentration, while water-soluble organic compounds
involve different types of organic acids (such as formic,
A large quantity of produced water with distinctive acetic, and propionic acids), where the pH, temperature,
characteristics is generated from oil fields, but its vol- and pressure influence the solubility of such organic
ume and characteristics are mainly dependent on the acids, but not salinity. Regarding the ionic composi-
lifetime of a reservoir and the method of recovery tion, cations include calcium ­(Ca2+), barium ­(Ba2+),
(Ebrahimi et al., 2010; Li et al., 2021; Tellez et al., potassium ­(K+), sodium (­ Na+), iron (­ Fe2+), magnesium
2002). Produced water contains different combina- ­(Mg2+), and strontium ­(Sr2+), while anions include sul-
tions of organic and inorganic materials (Klemz et al., fate ­(SO42−), carbonate (­CO32−), bicarbonate (­HCO3−),
2021) (Table 2). Its physical and chemical properties and chloride ­(Cl−). These ions can react to form C­ aCO2,
are mainly affected by the field’s geological location, ­CaSO4, and F­ eS2, which cause corrosion in the pipeline

Table 2  General produced water parameters from different oil fields in the world (Klemz et al., 2021; Rahman et al, 2020; and some
of our results from oilfields in Oman)
Oilfield produced water parameters Typical value Metal concentration Value (mg/L)

Density (kg/m3) 1000–1140 Calcium 13–30800

Conductivity (μS/cm) < 1000–600.000 + Sodium 50–297000 +
Surface tension (mN/m)* 38–78 Potassium 24–5500
Turbidity (NTU) > 100 Magnesium < 8–10000 +
Total organic carbon (TOC) (mg/L) 0–1500 Iron < 0.1–100
Chemical oxygen demand (COD) (mg/L) 177–1300 Aluminum 310–410
Total suspended solids (TSS) (mg/L) 1–1000 Boron < 5–95
pH 4.0–10 Barium < 1.3–650
Total Dissolved Solids (TDS) (mg/L) 2650–138,500 Nickel 0.06–0.2
Total oil (IR, mg/L) ~ 0.0–565 Cadmium 0–0.2
Volatile (BTEX; mg/L) < 0.20–55 Chromium 0–10
Total petroleum hydrocarbon (TPH) < 0.5–350 Copper 0–50
Oil and grease (mg/L) ~ 0–540 Lithium 0.1–500
Chloride (mg/L) 80–300,000 + Manganese < 0.004–175
Bicarbonate (mg/L) 71–3990 Lead 0–8.8
Sulfate (mg/L) < 2–3000 Strontium 0.02–1000
Ammoniacal nitrogen (mg/L) 10–300 Titanium < 0.01–0.7
Sulfite (mg/L) 0–50 Zinc 0–55
Phenols (mg/L) 0–23 Arsenic 0–0.3
Volatile fatty acids (VFAs) (mg/L) ~ 0–6000 Mercury 0–10
*
Depending on the type of surfactants used for EOR operations

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system. Another type of heavy metals could also be pre- above the air quality standards is associated with many
sent, but their concentration depends on the wells’ age respiratory problems in humans (Wang et al., 2012).
and geology. Heavy metals in produced water are usu- Various organic and inorganic components of pro-
ally in trace quantities, such as nickel (Ni), chromium duced water, including salts, are dangerous for surface
(Cr), lead (Pb), copper (Cu), cadmium (Cd), zinc (Zn), and underground water (tend to precipitate and accu-
mercury (Hg), and silver (Ag). Besides that, the inor- mulate in aquatic sediments), plants, atmosphere, soil,
ganic salts and organic compounds in produced water and human health. Irrigation of the soil with produced
create an enriched environment for microbial growth, water with high salts and oil content affects the soil
such as algae, bacteria, and fungi. The bacteria are usu- negatively. It blocks the soil pores and weakens the
ally saprophytic bacteria and sulfate-reducing bacte- soil ecosystem. In addition, the presence of hydrocar-
ria, which enhance the pipelines’ corrosion issue (Al- bons in the produced water discharged in the streams
Ghouti et al., 2019; Fakhru’l-Razi et al., 2009; Li et al., has a great effect on the species diversity of the marine
2021; Tellez et al., 2002). communities (Fakhru’l-Razi et al., 2009; Li et al.,
2021; Tellez et al., 2002). Researchers have reported
that some petroleum hydrocarbons are carcinogenic,
and can cause embryo distortion, organ (heart, kidney,
Characteristics of produced water and brain) damage, and gene mutations in organisms
(Lahiri et al., 2021). In addition, produced water dis-
Produced water is a mixture of organic and inorganic charges in surface water tend to form an oil layer at the
chemicals varying from simple to complex nature, mak- top that reduces the oxygen transmission into the water
ing the produced water different from other type of liq- ecosystem (Ossai et al., 2020).
uid wastes. Some contain high polymer content, such
as PAM and HPAM, which ranges between 200 and
500 mg/L. The presence of a huge quantity of polymers Management of produced water
raises the water viscosity. In addition, the oil in the pro-
duced water is with a smaller diameter droplet (approxi- To mitigate and control pollution, it requires proper
mately 3–5 μm) than the conventional size (about 35 μm) produced water management techniques. Several fac-
that makes it difficult to remove. The residual oil-in- tors determine the selection of produced water man-
water forms a stable emulsion, which increases the com- agement options, such as the county laws and regu-
plexity of the produced water. As well, the existence of lations, cost, technical potentials, and geographical
different organic compounds (such as benzene, toluene, situation with the available infrastructure. The first
and xylene) raises the biological toxicity of produced step in that direction is to minimize its production
water. Their concentration is significantly elevated, from the oil fields by different technologies, which
exceeding the allowed standards. For example, benzene showed not-so convincing results. Produced water
concentration in produced water is > 35,000 μg/L which reuse in oil and gas operation is a second possibility,
is considered 7000 times higher than the limit for drink- after the suitable accurate treatment, such as utilizing
ing water in the USA (Al-Ghouti et al., 2019; Li et al., to prepare a polymer solution or in other beneficial
2021). uses such as livestock consumption, irrigation, fire
control, industrial power generation, and drinking
water. The most common reuse of produced water
Environmental risk of produced water is re-injection into oil reservoirs for EOR. The final
management option is disposal, but after extensive
Recently, the influence of untreated produced water dis- treatment because of the complex nature of produced
charge has become a significant environmental issue (Lu water components. Produced water discharged should
et al., 2009; Tellez et al., 2002). In the past, the produced meet the national standards which differ between dif-
water from oil fields was disposed of in large evapora- ferent countries and even between regions of the same
tion ponds. This leads to the emission of volatile organic country (Al-Ghouti et al., 2019; Arthur et al., 2005;
compounds (VOCs) in the atmosphere, which contains Fakhru’l-Razi et al., 2009; Li et al., 2021). The most
ozone precursor compounds. Increasing ozone to levels effective handling option for the produced water is by

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applying a suitable method of treatment to convert it water and find alternative treatment methods. These
to a harmless product. There are many treatment tech- researches involved the produced water characterization,
niques but all focus on de-oiling, disinfection, desali- compositional analysis, environmental impacts, treatment
nation, and suspended particle removal (Ebrahimi technologies, and cost. Klemz et al. (2021) reported that
et al., 2010; Echchelh et al., 2018; Fakhru’l-Razi et al., around 2000 publications were published between 1999
2009). The degree of treatment depends mainly on the and 2019, related to this field.
produced water application afterward. Minimal treat-
ment is required to use the treated water in industrial
applications, but a high level of treatment is needed to The degradation of PAM and HPAM
use the treated water for drinking or agriculture (Al-
Ghouti et al., 2019; Echchelh et al., 2018). Polymers are susceptible to various degradation pro-
cesses, depending on polymers’ nature and conditions.
Most degradation processes are irreversible reactions
Produced water treatment methods that change the polymers’ physical and chemical char-
acteristics (Caulfield et al., 2002). HPAM persists for
The produced water as a byproduct after EOR opera- a long time in the water with a slow degradation rate
tions requires special-effective treatment to reduce the contaminating ground and surface water affecting the
viscosity, the content of free oil, and break the emul- environment, animal, plant, and leading to serious pub-
sion without any environmental issues (Li et al., 2021; lic health problems if not treated efficiently (Al-Moqbali
Nicolaisen, 2003). Such treatment is a challenging task et al., 2018; Al-Sabahi et al., 2018). The degraded
since it is produced in large amounts (~ 90% of the total hydrophilic PAM increases the mobility of environmen-
extracted fluids) with complex compositions and dif- tal molecules because of its carboxylic group content,
ferent contaminants (Al-Ghouti et al., 2019; Li et al., after hydrolysis by many environmental factors (Xiong
2021). Thus, the easily available handling options are et al., 2018). In nature, HPAM and PAM degradation
either disposal after following environmental regula- may occur thermally, mechanically, chemically, or pho-
tions, or re-injection after skillful planning to avoid tolytically. Thermal degradation depends on polymer
damage (Ebrahimi et al., 2010; Lu et al., 2009). molecular weight, impurities, and the mode of synthe-
For produced water treatment, different types of physi- sis, while mechanical degradation occurs because of
cal, chemical, and biological treatment methods are avail- polymer plumbing with a high flow rate and high shear,
able. In the case of physical methods, the pollutants are elongational flow, or elevated agitation, depending on
not destroyed, but are destroyed with chemical and biolog- the application of the polymer. In the EOR process,
ical methods. Physical treatments include the adsorption the polymer is injected with high viscosity through the
on activated carbon (achieving better quality, low con- porous reservoir rock, which results in the polymer’s
tamination water), sand filtration, gravity separation, and exposure to high mechanical stress. This subsequently
evaporation. In the case of chemical treatment, it involves affects the polymer’s properties and causes a reduction
chemical precipitation (through coagulation and floccula- in its viscosity and performance. The chemical degrada-
tion), chemical oxidation, demulsifier (oil–water separa- tion of the polymer chain is related to the amide group
tion), electrochemical, and photocatalytic processes, while reactivity, which results in the release of free hydroxyl
biological treatment (via aerobic and anaerobic microor- radicals. Similarly, oxygen-free radicals are released
ganisms) is more effective that supports the economic fea- photolytically by sunlight, which is extremely unsta-
sibility with lower cost. The biological treatment includes ble reactive species. In both cases, oxygen radicals will
using activated sludge (the usual biological method), have negative effects on the environment and public
sequencing batch reactors (SBRs), and biological aerated health. Al-Sabahi et al. (2018) reported photocatalytic
filters (BAF). This was accomplished after understand- degradation of ~ 74% of HPAM in produced water using
ing the mechanisms of the used microbes (Adewumi supported zinc oxide nanorods. The photo-degradation
et al., 1992; Al-Ghouti et al., 2019; Fakhru’l-Razi et al., reaction is a photon’s energy absorption mechanism,
2009; Li et al., 2010, 2021; Lu et al., 2009; Wang et al., which results in backbone cleavage of the polymer and
2012). In the past 20 years, many researchers have per- free radical formation. (Caulfield et al., 2002; Reddy
formed projects aiming to study the oilfield-produced et al., 1994; Xiong et al., 2018). Khan et al. (2019)

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reported innovative combination of ultrasonic waves

and chemical agents for HPAM degradation and deplug-
ging of the core sample. It has been reported that acryla-
mide is formed upon polyacrylamide exposure to UV
radiation (Al-Moqbali et al., 2018; Smith et al., 1997).
Thus, the byproducts of these reactions are important
since they can raise the toxicity of the degradation pro-
cesses, especially radical formation. Feng et al (2022)
reported ~ 97.63% HPAM removal (as measured by vis-
cosity reduction), by an electrochemical method using a
novel La-In co-doped PbO2 electrode. Although vari-
ous kinds of chemical agents are reported handle PAM/
HPAM degradation, it still needs a huge financial invest-
ment, and also suffers from environmental and other
associated issues such as corrosion, which motivates
researchers to look for other efficient and environmental
friendly techniques (Khan et al., 2019).
Fig. 5  Extracellular amidase induce the bacterial degradation
of PAM (Caulfield et al., 2002; Nyyssölä & Ahlgren, 2019)

Biodegradation of PAM and HPAM

To degrade the main carbon backbone of PAM and to
Although environments like oil fields, produced water, utilize it as a carbon source for bacterial growth, other
and soils surrounding oil fields are considered as quite enzymes are required. Several reports showed poten-
harsh, microbes beneficial for biodegradation of such tial role of mixed microbial biofilms in the treatment of
pollutants are reported (Abed et al., 2021; Al-Sayegh PAM or HPAM containing wastewater (Li et al., 2016;
et al., 2021; Wei et al., 2022; Zhang et al., 2021). Song et al., 2019a, b; Zhang et al., 2020, 2021). Zhang
Among different types of toxic and recalcitrant chemi- et al. (2019) reported efficient degradation of PAM and
cals present in produced water, polymers such as PAM acrylamide in a multistage contact reactor, using anam-
and HPAM are somewhat difficult for biodegradation, mox and ammonia-oxidizing bacteria-enriched biofilms.
as both PAM and HPAM cannot pass through most Song et al. (2021) reported ~ 85% HPAM removal using
bacterial membranes due to their higher molecular mixed microbial-ozonic-anaerobic–aerobic biofilm mul-
weight (Berdugo-Clavijo et al., 2019; Joshi & Abed, tistage bioreactor treatment process.
2017; Ma et al., 2021). PAM and HPAM biodegrada- Two polyacrylamide-degrading bacterial strains were
tion occur when microbes utilize the amide group of the isolated from soil, Bacillus sphaericus and Acinetobac-
polymer as a nitrogen source and/or the polymer carbon ter sp., utilizing 16–19% polyacrylamide after 14 days
backbone as a carbon source. Microbial biodegrada- of cultivation (Matsuoka et al., 2002). Al-Moqbali et al.
tion is favored since it yields higher removal efficiency (2018), on the other hand, isolated Bacillus sp. and Che-
without additional environmental pollution (Liu et al., latococcus sp., from polymer flooded produced water,
2016; Nyyssölä & Ahlgren, 2019). Bao et al. (2010) which degraded HPAM efficiently after 9 days of treat-
reported that some microorganisms from produced ment. Azomonas macrocytogenes and Enterobacter
water could utilize HPAM either as carbon or nitrogen agglomerans, PAM-degrading bacteria, were isolated
sources. Caulfield et al. (2002) explained that bacte- from the soil, which consumed PAM as the sole source
ria can grow in the presence of PAM, by utilizing it as of carbon and nitrogen (Nakamiya & Kinoshita, 1995).
a nitrogen source by hydrolyzing the amide to acid and Pseudomonas putida showed 45% PAM degradation
­NH3 by extracellular amidase. The resulting byproducts efficiency in 7 days as its sole nutrient source (Yu et al.,
were of a lower molecular weight than the polymer, 2015). Several reports highlight bacterial degradation of
with several ­COO− groups and without acrylamide for- PAM and HPAM polymers, using different isolates from
mation (Fig. 5). Many types of amidase differ in their diverse sources. However, it varies in its removal effi-
activity depending on the bacterial genera it is isolated. ciency under anaerobic or aerobic conditions (Table 3).

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Table 3  Different published reports for removal and biodegradation of PAM and HPAM
Microorganism Source of isolation Conditions HPAM/PAM removal Reference
%

Mixed microbes Wastewater from Aerobic–anoxic– 11–16.79% Wei et al. (2022)

“alkaline-surfactant- anaerobic/20–33 °C
polymer” flooding
water treatment station
Mixed microbial mats Constructed wetland Aerobic–anoxic /30 °C 7–34% Abed et al. (2021)
treating oilfield
produced water
Mixed microbes/ Biological contact Aerobic 64% Zhang et al. (2021)
microalgae oxidation reactor
used for the treatment
of PAM containing
wastewater
Mixed microbes Simulated synthetic Ozonic-anaerobic– 85.06% Song et al. (2021)
wastewater and aerobic/25–35 °C
activated wastewater
sludge
Klebsiella sp. PCX- The laboratory of Aerobic/38 °C 69.1% Ma et al. (2021)
biochar composite and Southwest
other mixed microbes Petroleum University
(China)
Mixed microbes Domestic sewage Aerobic–anoxic– 43.6% Zhang et al. (2020)
treatment plant anaerobic/30 °C
Acinetobacter sp. and Wastewater samples Aerobic/35 °C 45.82% Dong et al. (2020)
Pseudomonas from coking plant and
sp. shale gas field
Mixed microbes Sludge from wastewater Aerobic/25 °C ~ 75% (as viscosity Zhang et al. (2019)
treatment plant reduction)
Mixed microbes Oilfield produced Aerobic/50 °C Partial Berdugo-Clavijo et al.
water and activated (2019)
wastewater sludge
Mixed microbes Activated sludge from a Anaerobic/33 °C 40.5% Zhao et al. (2019a, b)
wastewater treatment
plant
Mixed microbes HPAM containing Aerobic and 38–65% Zhao et al. (2019a, b)
samples from anoxic/35 °C
Wastewater treatment
stations
Mixed microbes Oilfield wastewater Aerobic-Ozone- 90.79% Song et al. (2019a)
treatment station and aerobic/25–35 °C
aerobic activated
sludge from a domestic
wastewater treatment
plant
Bacillus megaterium Oilfield soil Aerobic/24 °C 55.93% Song et al. (2019b)
SZK-5 contaminated with
produced water
Mixed microbes Production water Anaerobic/36–37 °C Partial/not specified Hu et al. (2018)
samples
Mixed microbes Wastewater from Aerobic–anoxic– 7% Liu et al. (2018)
“alkaline-surfactant- anaerobic/30 °C
polymer” flooded
oilfield

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Table 3  (continued)
Microorganism Source of isolation Conditions HPAM/PAM removal Reference
%
Bacillus sp. Polymer flooded Aerobic/40 °C 59.9% Al-Moqbali et al. (2018)
Chelatococcus sp. produced water 58.4%
Paenibacillus sp. Activated sludge Anaerobic/36 °C 68.27% Li (2017)
Mixed microbes Water injection pipeline Not specified Partial/not specified Li et al. (2016)
from oilfield
Pseudomonas HPAM-containing Aerobic/35 °C 41.6% Liu et al. (2016)
aeruginosa wastewater
Bacillus cereus, Bacillus Polymer flooded Anaerobic and Partial/not specified Zhao et al. (2016)
sp., Rhodococcus sp. produced water aerobic/37 °C
Bacillus cereus and Polymer flooded Anaerobic and aerobic 75.8% Sang et al. (2015)
Rhodococcus sp. produced water
Pseudomonas putida Dewatered sludge Aerobic/39 °C 45% Yu et al. (2015)
Mixed bacteria HPAM-containing Aerobic/35 °C 62.1% Liu et al. (2013)
sewage
Bacillus cereus and Polymer flooded Aerobic/ 40 °C 42.1% Bao et al. (2010)
Bacillus sp. produced water
Bacillus cereus and Activated sludge and oil- Aerobic/30 °C 70% Wen et al. (2010)
Bacillus flexus contaminated soil
Clostridium Curing pot in the HPAM Anaerobic 30.8% Ma et al. (2008)
bifermentans H1 distribution station
Anaerofilum Oilfield Anaerobic 61.2% Li and Fang (2007)
pentosovorans A9
Enterobacter sp. Curing pot in the HPAM Anaerobic/38 °C 63.17% Wei et al. (2007)
distribution station
Bacillus sphaericus Soil Aerobic/30 °C 16% Matsuoka et al. (2002)
Acinetobacter sp. 19%
Enterobacter Soil Aerobic/30 °C 20% Nakamiya and Kinoshita
agglomerans 15% (1995)
Azomonas
macrocytogenes

NA not available

Bacterial degradation metabolic pathway carbon backbone via monooxygenases oxidation into
smaller molecules, such as acrylamide and/or acrylic
The complete metabolic pathway of PAM and HPAM acid, which could be further degraded (Joshi & Abed,
degradation is still not clear. The enzyme amidase is 2017). In general, PAM degradation by bacteria cause
known to initiate the biodegradation of PAM and changes in the polymer structure (Caulfield et al.,
HPAM under aerobic or anaerobic conditions, fol- 2002). The degradation pathway of PAM and HPAM
lowed by different enzymes involved yielding partial or to a smaller molecular weight product like acrylamide
complete degradation (Joshi & Abed, 2017). Extracel- has been proposed (Fig. 6) (Bao et al., 2010; Joshi &
lular amidases work on PAM amide group hydrolyza- Abed, 2017). The amidase action on the amide group
tion, as reported by Pseudomonas putida after incuba- of PAM and HPAM results in the release of ­NH3 and
tion at 39 °C for 7 days (Yu et al., 2015). The Fourier COOH addition. Subsequent monooxygenase oxida-
transform infrared (FTIR) spectrograms of Bacillus tion leads to cleaving the main carbon backbone of
cereus and B. flexus cultures after PAM degrada- PAM and HPAM. After many cycles, smaller organic
tion showed the removal of the amide group from the molecules are formed including acrylamide (Eubeler
polymer (Wen et al., 2010). While catalyzing PAM’s et al., 2009, 2010).

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Fig. 6  The proposed biodegradation pathway of PAM and HPAM to acrylamide (Modified from Joshi & Abed, 2017)

Characterization of biodegraded PAM and HPAM (GPC) and Fourier transform infrared (FTIR) methods.
The concentration of HPAM can also be measured by
After the biodegradation process of PAM and HPAM, it the starch-cadmium iodide method (Yongrui et al., 2015).
is necessary to measure its concentration and determine After the measurement of HPAM at 585 nm, the differ-
its fate, via various methods, depending on its sensitiv- ence between control and biodegraded sample readings
ity and detection limits. The initial method used was a are used for HPAM removal ratio calculation. Using this
photometric titration procedure which involved the reac- method, the quantity of PAM is presented as a concentra-
tion of crystal violet (CV) dye with PAM in the sample tion by spectrophotometry after a series of reactions with
and was followed by an absorbance reading at 590 nm amide groups in PAM (Lu & Wu, 2002). In addition to
(Masadome, 2003). The C18 and ion-exchange columns HPAM concentration measurements, the viscosity pre-
were developed in high-performance liquid chromatog- and post-biodegradation can be determined by a rheom-
raphy (HPLC) to measure acrylamide in polymers (Vers eter to acquire the viscosity reduction rate (VRR) which is
& Leonard, 1999). This method works successfully for the difference between control and biodegraded samples’
all types of polymers and matrices with a parts-per-billion shear viscosity (Zhao et al., 2016). HPAM removal effi-
(ppb) ranges of detection. Yu et al. (2015) reported change ciency can be determined based on total organic carbon
in PAM molecular weight and functional groups after bac- (TOC) that helps in evaluating PAM and HPAM biodeg-
terial biodegradation by gel transmission chromatography radation using a TOC analyzer (Sang et al., 2015). 13C

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Nuclear magnetic resonance (NMR) studies confirmed oil considerably to overcome the current energy crisis,
PAM degradation by the action of microbes (Wampler it is adverse environmental and health issues suggested
& Ensign, 2005). Other methods include ­NH3 selective searching for other eco-friendly alternative polymers.
electrode (Zi-jun & Lang, 2008), a sodium hypochlorite Extracellular polysaccharides formed by different bacte-
oxidation method (Neng et al., 2005), film drying method rial species give light to work as environmental-friendly,
(You et al., 2007), quantitative turbidimetry (Qing-Xiang chemical stability, and biodegradable polymers can be
et al., 2009), biochemical methane potential (BMP) test used in EOR applications. Xanthan gum produced by
(Dai et al., 2014), and size exclusion chromatography Xanthomonas campestris (Abidin et al., 2012), pullulan
(SEC) (Asano et al., 1982). Furthermore, liquid chro- produced by Aureobasidium pullulans (Al-Araimi et al.,
matography-mass spectrometry (LC–MS) can verify the 2021; Elshafie et al., 2017), and schizophyllan pro-
biodegradation of HPAM to acrylamide and measure its duced by Schizophyllum commune (Joshi et al., 2016),
concentration in the samples (Al-Moqbali et al., 2018). are well-known polysaccharide biopolymers showed an
outstanding performance in tertiary oil recovery (Fig. 7).
Such microbial metabolites helps in the oil recovery pro-
Biopolymers as an alternative for PAM cess by reducing mobility and modifying permeability
and HPAM during water flooding (Shabani Afrapoli et al., 2012).
Another reported advantage for the biopolymers are
One of the important ways to recover more oil from stability at high salinity and temperature, unlike chemi-
exhausted oil reservoirs after water flooding is poly- cal polymers (Gao, 2016; Quadri et al., 2015). This is
mer flooding (Pu et al., 2018). PAM and HPAM are the due to its helical structure (triple or double), rigidity,
most extensively used polymers in enhancing oil recov- and charge-free chains which increase its stability and
ery due to their customized properties and wide avail- thickening potential in harsh elevated temperature and
ability. Although the usage of PAM and HPAM as an saline oil reservoirs (Pu et al., 2018). However, its draw-
EOR method resulted in increasing the production of back is related to its poor filterability, which can lead to

Fig. 7  The chemical

structure of polysaccharide
biopolymers (A pullulan, B
schizophyllan, C Xanthan
gum) (Ferreira et al., 2015;
Lochhead, 2017; Sutivisedsak
et al., 2013)

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cell debris plugging during the injection which requires been reported, it still needs additional-extensive studies to
a pretreatment to eliminate it (Kulawardana et al. 2012; better understand the exact mechanisms and optimized-
Rivenq et al., 1992). Additionally, biopolymer’s proper- economic scaled-up processes for field-scale applications,
ties have to be tested before using it in polymer flooding and to make it economically attractive option. Advances
for EOR application. The properties include molecular in “omics” and synthetic biology-based technologies
and chemical stability, temperature and salt tolerance, could play an important role in the future applications of
thickening capability, rheology, and adsorption (Pu biodegradation of HPAM from produced water, and a safe
et al., 2018). disposal or other applications using such treated water, to
support UNSDG 6.

Conclusion and future prospects Acknowledgements SK and SJ would like to kindly acknowl-
edge research fellowship and research funding, respectively, by
The Research Council (TRC) Oman, and Sultan Qaboos Uni-
Renewed interests and improved economy of the non- versity (RC/RG-DVC/OGRC/18/01). Authors would also like
fossil-based energy sources, awareness about a role in to acknowledge kind support provided by local oil companies
environmental pollution, international policies governing (for providing produced water samples, polymers, and analysis
data), and Central Analytical and Applied Research Unit, Sul-
the supply, and demand of crude oil (and other types of tan Qaboos University, Oman.
fossil-based energy sources), are some challenges faced
by petroleum industries. Apart from those current chal- Declarations
lenges, the petroleum industry was already facing two
Conflict of interest The authors declare no competing inter-
major issues: the requirement of water for enhancing/ ests.
increasing oil recovery, and the treatment and disposal of
such a huge quantity of oilfield produced water. To make
matters worse, the majority of oil-producing countries References
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