Journal of Cleaner Production 378 (2022) 134532

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Journal of Cleaner Production

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Treatment of oil-field produced wastewater by electron beam technology:

Demulsification, disinfection and oil removal
Libing Chu a, b, Jianlong Wang a, b, *
a
Laboratory of Environmental Technology, INET, Tsinghua University, Beijing, 100084, PR China
b
Beijing Key Laboratory of Radioactive Waste Treatment, INET, Tsinghua University, Beijing, 100084, PR China

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

Handling Editor: Zhen Leng The treatment of polymer-containing produced wastewater with high viscosity and emulsification is a chal­
lenging issue in the oilfield. In this paper, electron beam (EB) radiation technology was firstly applied to treat the
Keywords: real oilfield produced wastewater. The results showed that the viscosity of the produced wastewater decreased
Produced water rapidly from initial 3.7 mPa s to 1.5 mPa s after EB radiation at absorbed dose of 1.0 kGy, then it gradually
Electron beam
reached the level of pure water at 5.0 kGy. The produced wastewater was negatively charged and the absolute
Radiation
value of zeta potential diminished stepwise during EB radiation process, indicating that the stability of oil/water
Wastewater treatment
emulsion decreased. Radiation pretreatment contributed to the oil removal by coagulation. The efficiency of oil
removal increased remarkably from 47% by coagulation alone to 85% with EB pretreatment at 1.0 kGy. Radi­
ation is also effective to disinfect the three typical bacteria in oilfield wastewater, saprophytic bacteria (TGB),
sulfate-reducing bacteria (SRB) and iron bacteria (IB). More than 99.8% of TGB, SRB and IB were killed at 1.0
kGy, and a complete inactivation was obtained at 2.5 kGy. Oxidation by ⋅OH radicals formed in water radiolysis
is the major pathway to decrease the viscosity and kill the bacteria, while the direct action of EB radiation also
plays a role. The members belonging to genera Thauera, Defluviimonas and Comamonadaceae were predominant
in the produced wastewater, with a relative abundance of 40%, 19% and 16%. Based on PICRUSt analysis, the
function genes related to metabolism exhibit the highest abundance (25%), which increased at 1.0 kGy, and then
decreased at 10 kGy, suggesting that EB radiation at low dose might stimulate the bacterial activity.

1. Introduction
Petroleum is an important and nonrenewable energy source. With
increasing energy demand worldwide, many techniques have been
developed for enhanced oil recovery (EOR), such as chemical flooding,
miscible flooding and thermal flooding (Bierman et al., 2014; Jia et al.,
2019; Bealessio et al., 2021). Among them, polymer flooding is the most
often used and efficient EOR method (Pogaku et al., 2018). Polymers,
such as polyacrylamide (PAM) and partly hydrolyzed PAM (HPAM) are
added into the floodwater, to increase the viscosity and reduce the
relative permeability mobility in the reservoir, leading to the improve­
ment in exploiting crude oil trapped in the porous stratum. Polymer
flooding could increase the oil recovery rate up to 30% (Pogaku et al.,
2018), which is currently implemented in the major oilfields of China,
such as Daqing and Shengli oilfields. However, the wastewater produced
during polymer flooding with huge amount has become a challenging
issue in the oilfield (Olajire, 2014).
The composition of the produced wastewater from crude oil exploi­
tation is complex (Li et al., 2021). The residue oil is the major pollutant,
which occurs in four forms, including free oil, dispersed oil, emulsified
oil and soluble oil. The other constitutes of produced wastewater include
chemical additives, such as oil displacement agents, anti-corrosion and
anti-sludging agent, solids such as clay particles, silt and fine sands,
bacteria usually involve saprophytic bacteria (TGB), sulfate-reducing
bacteria (SRB) and iron bacteria (IB), and inorganic ions such as Fe2+,
Ca2+, Mg2+, Cl− , CO2− 2−
3 , SO4 , etc. Especially, the produced wastewater
generated from polymer flooding contains residue polymer with high
concentration of 200–600 mg/L (Li et al., 2021).
The oilfield produced wastewater is mostly reused as injection water
into the reservoir after being treated properly, which is an economic and
environmental friendly option to save fresh water consumption and
abate pollution from wastewater discharging (Su et al., 2007, 2009;
Jiménez et al., 2018). It is noticeable that the standard of wastewater for
reinjection is different from that for discharging, thus the treatment

* Corresponding author. INET, Tsinghua University, Energy Science Building, China.

E-mail address: wangjl@tsinghua.edu.cn (J. Wang).

https://doi.org/10.1016/j.jclepro.2022.134532
Received 23 July 2022; Received in revised form 5 September 2022; Accepted 2 October 2022
Available online 7 October 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
L. Chu and J. Wang Journal of Cleaner Production 378 (2022) 134532

methods are different. Based on the Water Quality Standard of Oil and Table 1
Gas Trade Standard of China (SY/T 5329-2012), the control parameters Characteristics of oil-field produced wastewater.
for oilfield injection water in clastic reservoir include the content of oil Parameters Values Parameters Values
and suspended solids (SS), the median of particle size and the bacterial
pH 7.92–7.99 SS (mg/L) 85.0 ± 5.0
number of TGB, SRB and IB. The conventional and popularly used COD (mg/L) 629 ± 12 CH3COOH (mg/L) 37.3 ± 0.6
treatment processes in oilfield produced wastewater for reinjection TOC (mg/L) 311 ± 1.5 C3H7COOH (mg/L) 60.0 ± 0.3
include gravitation setting, coagulation/floatation, filtration and disin­ Oil (mg/L) 295 ± 36 C5H11COOH (mg/L) 18.3 ± 1.0
fection, to remove oil, SS and three bacteria (Li et al., 2021). However, HPAM (mg/L) 334 ± 17 Cl− (mg/L) 887 ± 15
Viscosity (mg/L) 3.7 ± 0.1 SO2−
4 (mg/L) 9.0 ± 0.9
these systems are not efficient to treat the produced wastewater gener­ Salinity (mg/L) 4226 ± 20 S2− (mg/L) 2.84 ± 0.1
ated from polymer flooding with increasing ageing well.
PAM/HPAM with extreme high molecular weight of several million
Daltons can raise the viscosity of produced wastewater significantly. In simultaneously.
the produced wastewater with high viscosity, the rising viscosity of oil
H2 O → [0.27] ⋅ OH + [0.26]e−aq + [0.06] ⋅ H + [0.26]H + + [0.07]H2 O2
droplets is reduced and the droplets coalescence is blocked. As a result,
the oil droplets stabilize in the produced wastewater to form stable oil in + [0.045]H2 (1)
water emulsion, making the poor separation of oil by the conventional
treatment processes (Umar et al., 2018). The effluent quality, especially where the values (μmol/J) in square bracket mean the radiation chem­
the oil content, is difficult to meet the standard for reinjection water. It is ical yields of each species.
critical to develop new technology to reduce the viscosity and destroy In present work, electron beam radiation was applied to treat the real
the emulsification of polymer-containing produced wastewater. oilfield produced wastewater from polymer flooding in north China. The
The advanced oxidation processes (AOPs), such as photocatalytic, effect of radiation on viscosity reduction and demulsification was
Fenton oxidation, ozonation and electrochemical oxidation are devel­ determined. The changes in wastewater characteristics, such as organic
oped to decompose the recalcitrant organic pollutants and reduce vis­ content, particle size distribution, bacterial community and function
cosity (Al-Sabahi et al., 2018; Maryam and Saeid, 2019; Han et al., 2020; were evaluated. The efficacy of radiation on inactivation of three typical
Ma et al., 2020; Chen et al., 2021a,b; Wang and Xu, 2012; Chen and bacteria in produced wastewater was assessed. Furthermore, the
Wang, 2021; Liu et al., 2020, 2021; Wang and Wang, 2021). Wang et al. enhancement of ionizing radiation as pretreatment to flocculation for oil
(2006) investigated the photocatalytical treatment of produced waste­ removal was investigated. This research could provide a new strategy for
water, and found that under TiO2-photocatalysis, the viscosity of treating the oilfield produced wastewater from polymer flooding with
PAM-containing produced wastewater could decline to the similar level high viscosity and emulsification by ionizing radiation.
of pure water with reaction time of 5–10 min, and around 80% of PAM
was decomposed with 90 min of illumination reaction. Song et al. (2021) 2. Materials and methods
found that ozonation was able to remove 85% of HPAM in the modified
produced wastewater with ozone dose of 25 g/g total organic carbon 2.1. Source and characteristics of produced wastewater
and HPAM concentration of 500 mg/L, which facilitated the subsequent
biological treatment. Al-Sabahi et al. (2018) found that the viscosity of The produced wastewater was taken from an oilfield wastewater
HPAM-containing wastewater with concentration of 250–1000 mg/L treatment plant in north China. The influent is derived from HPAM-
decreased by 30–60% after 6 h of visible photocatalytic reaction using flooding crude oil extraction processes. The plant adopts conventional
ZnO as catalyst. It appeared that during photolysis processes the cata­ treatment processes involving gravitation, flocculation and nuts filtra­
lytic agents are necessary, which are hard to be recovered and ozone is tion with the capacity of 5000 m3/d. The effluent of the plant is rein­
decomposed easily. It is imperative to develop new AOPs without use of jected into the reservoir after adding chemicals such as germicide, scale
chemicals. and corrosion inhibitor, etc.
Ionizing radiation is a novel advanced oxidation technology for Table 1 shows the characteristics of the produced wastewater. pH is
wastewater treatment, which applies gamma ray (γ-ray) radiation or slightly alkaline. The content of COD, residue oil and HPAM is high. The
electron beam (EB) radiation to treat wastewater. Under both the direct high salinity and chloride are common for produced wastewater. The
adsorption of high-energy ray/EB and the oxidation and reduction by short-chain volatile fatty acids (VFA) including acetate, butyrate and
active species involving ⋅OH, e−aq and ⋅H formed in water radiolysis (as hexanoic acid were found. The number of the three bacteria of TGB, SRB
shown in Eq. (1)) (Spinks and Woods, 1990), a variety of recalcitrant and IB per milliliter is in the 3.4–4.4 log order of magnitude.
pollutants are able to be degraded effectively, such as chloride phenols,
pesticides, antibiotics and dyes (Wojnarovits and Takacs, 2008; Csay 2.2. Experimental methods
et al., 2012; Liu and Wang, 2013, 2020; Liu et al., 2014; Wang and Chu,
2016; Tegze et al., 2018, 2019; Wojnarovits et al., 2018; Wang and The experiments of EB radiation were conducted using an electron
Wang, 2018, 2022a; Wang et al., 2019). accelerator (IBA, Belgium, 10 MeV, 10 mA) with the dose rate of around
EB radiation by electron accelerator was reported to be more eco­ 14.2 kGy/s. Around 50 mL of wastewater were put into the trays and
nomic than other AOPs for practical wastewater treatment, which is safe delivered for radiation at ambient temperature of around 25 ◦ C. The
without the use of radioisotopes and chemicals, and characterized with a different absorbed doses were obtained by controlling the beam current
small footprint and very short processing time in a second (Homlok (mA) and the transportation velocity (m/min). After irradiation, the
et al., 2011, 2021; He et al., 2014; Szabo et al., 2017; Rozsa et al., 2019; wastewater samples with different absorbed doses were analyzed
Zhuan and Wang, 2019; Capodaglio, 2020). A full-scale advanced directly for the parameters involving COD, oil, HPAM, particle size, zeta
treatment of dyestuff wastewater (30, 000 m3/d) by EB technology has potential, number of TGB, SRB and IB, the bacterial community and
been operated successfully in a knitting factory in southern China (Wang function, etc. The wastewater was filtered by 0.22 μm filter and the
and Wang, 2022b; Wang et al., 2022b). In addition, ionizing radiation filtrate was collected to analyze TOC and dissolved organic matters
with high energy and penetration is an efficient disinfection method to (DOM).
damage DNA or disintegrate bacteria (Wang and Wang, 2007; Yin and To study the enhancement of radiation pretreatment to coagulation
Wang, 2019; Wang et al., 2022a). Ionizing radiation might be a prom­ for oil removal, the produced wastewater was firstly irradiated with the
ising option to treat the polymer-containing produced wastewater to absorbed dose of 1.0 kGy prior to coagulation. The coagulation with the
decompose polymers, reduce viscosity, break emulsion and kill bacteria raw produced wastewater was conducted in parallel for comparison. The

2
L. Chu and J. Wang
Fig. 1. Changes in viscosity, HPAM content and zeta potential in produced
wastewater during radiation.
coagulation experiments were performed using electric agitator (GUO­
HUA Electric Appliances Company, China) with 500 mL of each bottle.
The coagulant was poly-ferric aluminum sulfate (PFAS) with two dos­
ages of 50 mg/L and 100 mg/L. After the coagulant was added into the
wastewater, agitator was operated by rapid mixing (170 rpm for 5 min)
and slow mixing (50 rpm for 10 min). Then the wastewater was settled
for 30 min and the oil content in the supernatant was detected. The
temperature was kept at 30 ◦ C.
2.3. Analytic methods
COD, SS and salinity were detected by the standard method for water
and wastewater (SEPA, 2002). Total organic carbon (TOC) was deter­
mined by a TOC/TN analytic instrument (Jena Multi N/C 2100, Ger­
many). The composition of DOM was identified using three-dimensional
excitation emission matrix (3D-EEM) spectrum (Hitachi F-7000, Japan).
The wavelength of excitation (Ex) and emission (Em) ranged 200–400
nm and 200–500 nm. The scan interval of Em and Ex was 10 nm and 5.0
nm and the scan speed of 1200 nm/min was applied.
Oil was detected by spectrophotometric method using petroleum
ether (60–90 ◦ C) as the extract (SY/T 5329-2012). HPAM was evaluated
by starch cadmium iodide method (Lu and Wu, 2002). Briefly, the
quantity of HPAM was converted to starch− triiodide complex content
by adding the starch–cadmium iodide reagent, which was then
measured at 590 nm using pure water as reference.
Viscosity was detected by a NDJ-79 rotary viscometer (Bangxi In­
strument, China) with water bath circulation at 20 ◦ C. Zeta potential was
measured by a Zeta Potential Analyzer (Brookhaven ZetaPALS, USA). pH
was monitored by a pH meter (Thermo Orion, USA). The anions were
determined by an Ion Chromatograph (Thermo Dionex ICS 2100, USA)
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Journal of Cleaner Production 378 (2022) 134532
with an ASRS-4mm suppressor and a DS6 conductive detector at a flow
rate of 1.0 mL/min. The suppressor current is 45 mA and the cell tem­
perature was 35 ◦ C. VFAs were evaluated by a Gas Chromatograph
(Agilent 7697A, USA).
The number of TGB, SRB and IB was determined by the disappearing
dilution method (SY/T 5329-2012). Briefly, the wastewater samples
were injected into a series of test bottles for different bacteria which are
purchased from Zhengzhou Water Testing Technology Company of
China and diluted stepwise. Then the test bottles were cultivated at
30 ◦ C for 1d (TGB) or 7 d (SRB and IB). The number of bacteria was
calculated based on the number of test bottles with positive reaction and
dilution ratio.
The bacterial community and function of the raw produced waste­
water and irradiated at 1.0 kGy and 10 kGy were analyzed. About 500
mL of wastewater samples were filtrated and the membrane with the
solids were used for extraction of the genetic DNA by a Fast DNA
extraction kit following the manufacture’s protocol. The bacterial
community of DNA extracted was analyzed by Illumina Miseq pyrose­
quencing in Majorbio Biopharm Technol Company (Shanghai, China)
following the procedure described in previous study (Shen et al., 2019).
The relative abundance and diversity of bacteria at the level of phylum
to genus were identified. Besides, based on 16S rRNA data, the func­
tional profile prediction of bacterial sequences was determined using
Phylogenetic Investigation of Communities by Reconstruction of Un­
observed States (PICRUSt) using Kyoto Encyclipedia of Genes and Ge­
nomes (KEGG) (Chu et al., 2021a; Yin and Wang, 2021).
3. Results and discussion
3.1. Viscosity reduction and demulsification
Fig. 1 depicts the changes in viscosity and HPAM content during EB
radiation. It is obvious that radiation is effective to reduce the viscosity
of the produced wastewater. The viscosity declined sharply from initial
3.7 mPa s to 1.5 mPa s with the absorbed dose of 1.0 kGy and then
gradually with rising the absorbed doses, reaching to the level of pure
water under the same temperature at 5.0 kGy. The HPAM decomposition
rate is lower than viscosity reduction rate. The efficiency of HPAM
removal was around 22% at 2.0 kGy and increased to 35% at 10 kGy.
The results were comparable to the literatures. Ren et al. (2006) studied
the treatment of PAM-containing oilfield produced wastewater by
UV/H2O2/O3 combined processes. With the ozone dosage of 230 mg/L,
H2O2 dosage of 660 mg/L and UV lamp of 20 W, the removal efficiency
of PAM was around 30% after reaction of 30 min, and it increased to
60% as prolonging the reaction time to 90 min. It is noticeable that the
amount of ozone and H2O2 applied is high.
HPAM is characterized with an extreme high molecular weight of
several million Da. In HPAM-containing wastewater, the monomer
molecules of HPAM exhibit a network structure owing to the intermo­
lecular and intramolecular interaction of hydrogen bonds, resulting in
the high viscosity (Du et al., 2020). Electron beam with high energy and
the active species such as ⋅OH with high oxidation might destroy the
hydrogen bonding easily, leading to the destruction of the network
structure. However, much high energy is required to decompose HPAM
molecules. This could explain the sharp reduction of viscosity and low
HPAM removal during radiation within 0–10 kGy.
Following the viscosity reduction, the stability of oil/water emulsion
was abated. Zeta potential is a main tool to represent the stability of
colloidal solution (Kumar and Dixit, 2017). The lower the absolute value
of zeta potential, the higher the stability of the solution. As shown in
Fig. 1, the produced wastewater was negatively charged and the abso­
lute value of zeta potential declined stepwise during radiation. This
implies that radiation is efficient to decrease the stability of emulsion of
the produced wastewater. It is worthwhile to note that the rapid vis­
cosity reduction and demulsification by radiation are favorable for the
oil-water separation, leading to the improvement in oil removal.
L. Chu and J. Wang Journal of Cleaner Production 378 (2022) 134532

The changes in DOM composition during radiation were further

evaluated by 3-D EEM spectrum (Fig. 3). According to the contour plots,
the DOM in the produced wastewater is characterized with three com­
ponents: tyrosine-like (Peak A, Ex/Em of 200–250/200–230 nm),
tryptophan-like (Peak B, Ex/Em of 200–250/330–380 nm) and soluble
microbial products (Peak C, Ex/Em of 250–300/<380 nm). As exposed
the produced wastewater to radiation, the fluorescence intensity of peak
C decreased rapidly and disappeared with the absorbed dose of 5.0 kGy.
The intensity of peak B decreased gradually and the intensity of peak A
exhibited a slight increase at the low dose of 1.0 kGy and then declined
with increasing the absorbed dose. This suggests that ionizing radiation
is more efficient to remove the soluble microbial products than the
protein-like substances.

3.3. Variation in particle size distribution

Fig. 4 presents the changes in particle size distribution in the

Fig. 2. Removal of COD, TOC and oil during radiation of the pro­
duced wastewater.

3.2. Removal of organics and oil

Fig. 2 presents the changes in COD, TOC and oil content in the
produced wastewater during radiation. The concentration of COD and
TOC decreased slowly with increasing the adsorbed doses. The removal
percentage of COD and TOC was 5.5%–10.7% at 1.0 kGy and reached
11.0%–22.7% at 10 kGy. The reduction of oil content is higher than
COD/TOC removal. Oil removal reached 24.6% with the absorbed dose
of 1.0 kGy and rose to 40.3% at 10 kGy. Crude oil is a mixture of volatile
liquid hydrocarbons mainly involving paraffins, naphthene, and aro­
matics. During the AOPs such as ionizing radiation and Fenton, the
macro-molecular organic substances especially with benzene rings and
double bonds could be degraded into to biodegradable intermediates,
while a much high demand in energy or chemicals is required to
mineralize the intermediates into CO2 and water (Yu et al., 2010a, Fig. 4. Particle size distribution, mean and medium (insert graph) with
2010b; Wang and Wang, 2019; Chu et al., 2021b). different absorbed doses.

Fig. 3. 3D-EEM spectrum of DOM in produced wastewater during radiation.

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L. Chu and J. Wang
Fig. 5. Changes in the number of three typical bacteria in produced wastewater
during radiation.
produced wastewater during radiation. The particle size of the raw
produced wastewater varied in the range of 0.4–75 μm. EB radiation
could cause the breakage of large particles by direct electron beam
Fig. 6. Variation in bacterial genera with the relative abundance of higher than 1% (A) and the function genes related metabolism (B) predicted by PICRUSt during
radiation of produced wastewater, the inset graph shows the changes in relative abundance of function genes at pathway 1 during radiation.
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Journal of Cleaner Production 378 (2022) 134532
radiation and indirect ⋅OH oxidation, leading to the distinct decrease in
the particle size, involving the range, the mean and medium. Our pre­
vious studies (Chu et al., 2011) demonstrated that gamma irradiation
was able to disintegrate the sludge flocs and break the bacterial cells.
The particle medium declined from initial 5.1 μm to less than 1.0 μm at
5.0 kGy which meets the strictest standard (≤1.0 μm) for oilfield rein­
jection water (SY/T 5329-2012).
3.4. Inactivation of TGB, SRB and IB
Ionizing radiation was efficient to kill the three typical bacteria in the
HPAM-containing produced wastewater. As exposed to radiation, the
number of the three bacteria declined rapidly (Fig. 5). With the absorbed
dose of 1.0 kGy, more than 99.8% of TGB, SRB and IB were killed and a
complete inactivation was observed as increasing the dose to 2.5 kGy.
This is beneficial for treating the produced wastewater for reinjection
because the consumption for germicidal agent is going to be saved (see
Fig. 6).
The good performance in sterilization was in agreement with our
previous studies about treating the pharmaceutical wastewater by ra­
diation (Chu et al., 2021b) and comparable to the literature. The
removal efficiency of colony-forming units (CFU) in pharmaceutical
wastewater reached 99.9% at 1.0 kGy and 100% at 5.0 kGy. Qiao et al.
(2008) found that the number of SRB, TGB and IB in the oilfield
L. Chu and J. Wang
produced wastewater decreased from initial 2.5 × 103, 2.5 × 101, 5.0 ×
101 to 2.5 × 100, 1.2 × 101 and 1.3 × 100 by UF filtration. Wei et al.
(2013) investigated the sterilization effect of a quaternary ammonium
salt, 1,12-dodecylidene triphenyl double phosphonium bromide. With
the concentration of 20 mg/L and contact time of 30 min, SRB, TGB and
IB were killed by 84%, 96% and 99%, respectively.
3.5. Changes in bacterial community and predictive function
Based on Illumina pyrosequencing, the sequence number for the
three wastewater samples was 50879 (0 kGy), 58798 (1.0 kGy) and
40919 (10 kGy). The sequence length ranged from 201 bp to 531 bp with
the mean value of 376 bp. The high Good’s coverage of more than 0.998
for each sample implies that the library could reflect the real profile of
bacterial community.
The bacterial diversity of the oilfield produced wastewater was
found to be relatively low. At the phylum level, Proteobacteria was
predominant remarkable with the relative abundance of 94.5%, fol­
lowed by Campilobacterota (2.0%), Firmicutes (0.8%) and Desulfobacter­
ota (0.4%). Proteobacteria is a large group of bacteria with a broad
variety of aerobic and anaerobic bacteria, which is often identified in the
wastewater treatment system to degrade the organic pollutants (Snaidr
et al., 1997). Campylobacterota are gram-negative, mainly spiral-shaped
motile bacteria and some members are reported to be found in the oil
filed or oil-contaminated groundwater (van der Stel and Wösten, 2019).
The members belonging to Firmicutes could excrete extracellular en­
zymes to degrade the macro-molecular organics such as protein (Hasan
et al., 2006). The sulfur-cycling bacteria in the phylum Desulfobacterota
were identified in a groundwater from deep terrestrial bedrock (Bell
et al., 2022).
Fig. 6A depicts the changes in the abundance of the top genera
identified in the HPAM-containing produced wastewater. The members
of Thauera, Defluviimonas and Comamonadaceae were dominant with the
relative abundance of 40%, 19% and 16%. Rochman et al. (2017) found
that some strains identified in an oil sand in Canada belonged to genus
Thauera which are the major naphthalene degraders. Pan et al. (2015)
isolated two strains of genus Defluviimonas from an oilfield produced
wastewater. A species in genus Defluviimonas isolated from a river
sediment was reported to be capable of degrading pyrene, a polycyclic
aromatic hydrocarbon (Zhang et al., 2018). The bacteria of genus
Comamonadaceae were enriched highly in an oil-polluted groundwater
in the area of a petrochemical plant in northeast China (Sun et al., 2017).
After radiation, the relative abundance of genera Thauera and Coma­
monadaceae decreased, while the members in the genera Pseudarco­
bacter, Aquabacterium, Sphingomonas and Thiofaba exhibited a great
increase in the relative abundance.
Based on PICRUSt analysis (Fig. 6B), the function gene related
metabolism exhibits the highest abundance (25%), followed by envi­
ronmental and genetic information processing (8.4% and 6.8%). The
relative abundance of genes coding for cellular processes, human dis­
eases and organismal systems was lower than 2.4%. The genes in
charges of metabolism mainly include carbohydrate, energy, xenobi­
otics biodegradation, lipid, nucleotide and glycan biosynthesis meta­
bolism. It is interesting to note that the abundance of almost all the genes
coding for metabolism increased with the low absorbed dose of 1.0 kGy
and then declined with increasing the dose to 10 kGy. This suggests that
ionizing radiation at low dose might be able to stimulate the bacterial
activity for metabolism which abated by a high dose of radiation.
3.6. Enhancement of radiation pretreatment to coagulation for oil
removal
Ionizing radiation combined with the conventional coagulation was
performed to enhance oil removal, because coagulation is usually used
to remove the particulates and high weigh molecular compounds (Liu
et al., 2022). As shown in Fig. 7, radiation pretreatment with the low
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Journal of Cleaner Production 378 (2022) 134532
Fig. 7. Oil removal by coagulation and radiation pretreatment (1.0 kGy) with
two PFAS dosages of 50 mg/L and 100 mg/L, the pictures of coagulation
without (beaker 2) and with radiation pretreatment (beaker 4) were present.
Table 2
Changes in viscosity and number of TGB and IB. during radiation in presence of
t-BuOH.
Doses (kGy) Viscosity (mPa s) Number per mL
TGB IB
1.0 3.5 ± 0.01 2.5 × 103 ± 6.0 × 102 6.0 × 102 ± 2.5 × 101
5.0 3.4 ± 0.02 6.0 × 102 ± 6.0 × 101 2.5 × 102 ± 6.0 × 101
10.0 3.3 ± 0.01 2.5 × 102 ± 2.5 × 101 6.0 × 102 ± 0.6 × 100
absorbed dose of 1.0 kGy improved oil removal by coagulation
remarkably. The efficiency of oil removal was 39–47% by coagulation
alone and reached 73–85% with radiation pretreatment at PFAC dosages
of 50 mg/L and 100 mg/L. For the HPAM-containing produced waste­
water with initial oil content of around 300 mg/L, the oil content could
decrease to 45 mg/L by combining radiation pretreatment (1.0 kGy) and
coagulation (100 mg/L PFAC), which meets the standard (≤50 mg/L) of
oilfield reinjection water in China as the permeability of reservoir rock
was higher than 1.5 μm2 (SY/T 5329-2012). Since radiation pretreat­
ment reduced the viscosity and broke the oil-water emulsification, the
oil particles are able to be settled easily by coagulation. It was observed
(Fig. 7, the picture of flocculation) that the flocs formed during coagu­
lation alone are loose and suspended in the liquid, while the flocs formed
by radiation/coagulation treatment have compact structure and settled
in the bottom of the reactor.
3.7. Mechanism of viscosity reduction and sterilization
To illustrate the major mechanism responsible for viscosity reduction
and sterilization during EB radiation of the produced wastewater, t-
BuOH (100 mM) was added into the wastewater and mixed before ra­
diation. Table 2 reveals the changes in the viscosity and the numbers of
TGB and IB in the presence of t-BuOH. It is well-known that t-BuOH
reacts fast with ⋅OH radical with the rate constant of (3.8–7.6) × 1010
Lmol− 1 s− 1 (Buxton et al., 1988; Wang and Wang, 2020) and can scav­
enge the generation of ⋅OH radical during radiation. It should be
mentioned that the initial viscosity and bacterial numbers detected in
the produced wastewater did not change with t-BuOH addition.
It is clear that the efficacy of both viscosity reduction and steriliza­
tion diminished greatly with t-BuOH addition. During radiation with t-
BuOH addition, the viscosity and bacterial numbers in the produced
wastewater decreased slowly. With the high absorbed dose of 10 kGy,
L. Chu and J. Wang
Fig. 8. The schematic graph showing the application of ionizing radiation by electron accelerator for treating polymer-containing oil-field produced wastewater
through combining with the conventional oilfield wastewater treatment processes for reinjection.
the viscosity maintained at around 3.3 mPa s and there are still 60–250
TGB and IB per mL detected in the produced wastewater. This suggests
that ⋅OH oxidation is the major mechanism to reduce viscosity and kill
bacteria, while the direct energy absorption of radiation also play a role.
3.8. Primary cost analysis
The above results demonstrated that ionizing radiation with a low
dose of 1.0 kGy was enough to decrease the viscosity and sterilize the
produced wastewater (see Supporting Information, Table S1) and
enhance the oil removal by coagulation. In practical application, EB
radiation by electron accelerator could be added before coagulation in
the conventional produced wastewater treatment processes for reinjec­
tion (Fig. 8). The increased operation cost is the electricity consumption
of accelerator, while the consumption for sterilizing agent can be
diminished (see Supporting Information, Table S2).
Based on our previous studies (Chu et al., 2021a), the electricity
consumption of 1.0 kGy is equal to around 1 kw⋅h/m3 that costs 0.7
CNY/m3 (around 0.10 USD/m3) in most area of China. The expense of
sterilizing agent for the polymer-containing produced wastewater
treatment plant is around 1.1 CNY/m3 (around 0.16 USD/m3). In
addition to the improved oil removal, ionizing radiation-coupled pro­
cesses are capable of decreasing the operation cost of 0.4 CNY/m3
(around 0.06 USD/m3). Ganiyu et al. (2022) reported that the opera­
tional cost was in the range of 0.4–1.5 USD/m3 by the AOPs involving
photocatalysis, ozonation and UV/H2O2 for treating produced waste­
water. EB irradiation was competitive for practical application. How­
ever, the industrial application of EB technology for wastewater
treatment is limited by the public concerns about radiation safety, na­
tional policy about nuclear technology and the relatively high cost of
investment.
4. Conclusions
Electron beam radiation was effective to reduce the viscosity, break
the emulsion stability and disinfect the three typical bacteria of the
HPAM-containing oilfield produced wastewater. With the absorbed dose
of 1.0 kGy, the viscosity decreased rapidly from initial 3.7 mPa s to 1.5
mPa s and more than 99.8% of TGB, SRB and IB were deactivated. The
content of COD, HPAM and particle size decreased gradually following
radiation. DOM in the produced wastewater is composed of tyrosine-like
substances, tryptophan-like substances and soluble microbial products.
During radiation, the fluorescence intensity of soluble microbial prod­
ucts decreased rapidly and disappeared with the absorbed dose of 5.0
kGy. Radiation pretreatment with the low absorbed dose of 1.0 kGy
improved oil removal by coagulation remarkably. The oil removal
increased from 47% by coagulation alone to 85% with radiation pre­
treatment of 1.0 kGy with the similar PFAC dosages of 100 mg/L.
Ionizing radiation by electron accelerator combined with the conven­
tional produced wastewater treatment processes could provide a
promising technology to treat the polymer-containing oilfield produced
wastewater for reinjection.
7
Journal of Cleaner Production 378 (2022) 134532
CRediT authorship contribution statement
Libing Chu: Investigation, Formal analysis, Funding acquisition,
Writing – original draft. Jianlong Wang: Conceptualization, Funding
acquisition, Methodology, Writing – review & editing, Supervision.
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.
Data availability
Data will be made available on request.
Acknowledgements
This research was supported by the National Natural Science Foun­
dation of China (No 21777083) and the Huaneng Group Science and
Technology Research Project (HNKJ22-HXX).
Appendix ASupplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.jclepro.2022.134532.
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