Separation and Purification Technology 291 (2022) 120920

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Separation and Purification Technology

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

Oxidation-biotreatment-membrane combined process for external reuse of

shale gas wastewater
Peng Tang a, b, Wancen Xie a, b, Lun Tian a, b, Bin Tan c, Yongli Zhang a, Zhishan Yang a, b, *,
Chen Chen d, Weiming Zhang e, Baicang Liu a, b, *
a
Key Laboratory of Deep Earth Science and Engineering (Ministry of Education), Institute for Disaster Management and Reconstruction, College of Architecture and
Environment, Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu, Sichuan 610207, PR China
b
Yibin Institute of Industrial Technology, Sichuan University, Yibin Park, Section 2, Lingang Ave., Cuiping District, Yibin, Sichuan 644000, PR China
c
Hangzhou Shangtuo Environmental Technology Co., Ltd., Hangzhou, Zhejiang 310000, PR China
d
Litree Purifying Technology Co., Ltd., Haikou, Hainan 571126, PR China
e
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, PR China

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

Keywords: The external reuse of shale gas wastewater (SGW) is inevitable and challenging from the long-term perspective of
Shale gas wastewater the shale gas industry. Among the numerous reuse methods of SGW, pretreatment-membrane combined pro­
Pre-oxidation cesses are regarded as a suitable and effective method. In this work, an integrated oxidation-biologically active
Biologically active filtration
filtration (BAF)-ultrafiltration (UF)-reverse osmosis (RO) process is firstly proposed for the external reuse of
Membrane fouling
External water reuse
SGW. The results indicated that pre-oxidation, especially O3 pre-oxidation, can effectively improve the efficiency
of removing organic matter in the subsequent BAF process, despite the variable feed chemistry and salinity
(1.2%-2.3%). Herein, after ozonation, the removal rate of dissolved organic carbon in the BAF system was
increased by 1.1–1.3 times. Meanwhile, oxidation-BAF, especially O3-BAF, can also significantly reduce UF
membrane fouling (7%-60%) in the subsequent UF system compared with that of the alone BAF system. The
principal mechanism of UF membrane fouling mitigation was that oxidation-BAF increased the cohesion energy
between foulants and foulants and the adhesion energy between foulants and the UF membrane, making it more
difficult for foulants to adsorb on or deposit on the membrane pores and membrane surface. In addition, the
effluent of the integrated process can meet the water quality standards for SGW external reuse. Therefore, the O3-
BAF-UF-RO process proposed here has broad engineering application potential for desalination, removal of
organic pollutants, and realization of safe reuse of SGW.

1. Introduction
In the past decade, the development of hydraulic fracturing and
horizontal drilling techniques has unlocked vast shale gas resources
[1,2]. With the continuous use of hydraulic fracturing in shale gas
extraction, the problems of water resource consumption and water
environment pollution have become increasingly serious. This is
because the operation of hydraulic fracturing not only requires a large
volume of fracturing fluid composed primarily of freshwater but also
generates a large amount of shale gas wastewater (SGW, ~
5200–25,870 m3 per well) [3]. SGW contains many toxic substances and
salts, which can seriously threaten the aquatic ecological environment if
not reused effectively [4]. In addition, the increased need for fresh water
in the shale gas industry and resulting continuous production of SGW
also warrants the reuse of SGW [1].
At present, the combination of pretreatment technology and mem­
brane technology has become a suitable and recommended method to
reuse SGW [5–9]. In the pretreatment-membrane separation combined
system, pretreatment plays a role in removing suspended solids, espe­
cially organic matter. These organic components can cause serious
membrane fouling in subsequent membrane processes [10,11], while
their removal in pretreatment will reduce operation costs, prolong
membrane service life, and improve the treatment effect of subsequent
membrane processes [11–13]. The membrane process further removes
salts, organic matter, microorganisms, and other components in SGW so
that the effluent can meet reuse standards [6,14].

* Corresponding authors.
E-mail addresses: yangzs@scu.edu.cn (Z. Yang), bcliu@scu.edu.cn (B. Liu).

https://doi.org/10.1016/j.seppur.2022.120920
Received 21 December 2021; Received in revised form 18 March 2022; Accepted 22 March 2022
Available online 23 March 2022
1383-5866/© 2022 Elsevier B.V. All rights reserved.
P. Tang et al.
Numerous pretreatment processes, including coagulation [15],
adsorption [16], advanced oxidation processes [12,13], walnut shell
filtration [17], and biotreatment [14,18], are currently being applied in
combination with membrane technology for the effective reuse of SGW.
Among current pretreatments, biological treatment technology is
regarded as a promising potential pretreatment of membrane technol­
ogy due to its cost-effectiveness. Furthermore, the potential of biological
treatment technology in SGW treatment has been emphasized in recent
years because studies have found that much of the organic matter in
SGW is biodegradable and that microorganisms in SGW have a robust
capability for degrading organic matter [18–22]. Riley et al. [14] re­
ported that biologically active filtration (BAF) could efficiently control
membrane fouling in ultrafiltration (UF) and nanofiltration processes by
effectively removing organic compounds. In our previous study [23], we
proved that pre-oxidation alone, using ozone (O3) or ferrate (Fe(VI))
could improve the efficiency of organics removal in BAF systems by
increasing the biodegradability of organics, which has also been re­
ported in other studies [24,25]. Whether the oxidation-BAF process can
remove membrane fouling has been debated. While some have found
that the oxidation-BAF process can mitigate membrane fouling by
improving water quality and removing suspended solids [26], others
have reported that the oxidation-BAF process can accelerate membrane
fouling by promoting biofouling [27,28]. Therefore, the effect of the
oxidation-BAF process on membrane fouling needed further assessment
and discussion. Additionally, oxidation-BAF had not been combined
with membrane technology for reusing SGW, and the effect on mem­
brane fouling had not been investigated. Furthermore, given the com­
plex compositions of SGW, the understanding of membrane fouling
mechanisms is critical for fouling control, which was still deficient in
treating SGW by membrane technology.
In this study, for the first time, oxidation-BAF was combined with a
membrane separation process specifically to reuse SGW conducted by
using four kinds of SGW samples with varied water quality. In addition,
the effect of pre-oxidation on the removal of organic matter in BAF
systems under different empty-bed contact times (EBCT) was further
evaluated. Notably the mechanism of mitigating membrane fouling by
oxidation-BAF was analyzed using the extended Derjaguin-Landau-
Verwey-Overbeek (XDLVO) analysis, the classic pore blocking model,
and statistical analysis.
2. Experimental section
2.1. Geochemical characterizations of SGW samples
Four kinds of SGW samples, labeled SGW1-4 for this research, were
obtained from separate shale gas wells in the Changning area of China.
The geochemical characterizations of SGW samples are presented in
Table S1 of the Supplementary Information. The corresponding analyt­
ical methods of geochemical characterizations are summarized in
Table S2.
2.2. Experimental protocol
The hybrid treatment train consisted of pre-oxidation (O3 or Fe(VI)),
BAF, UF, and RO, as depicted in Fig. S1. The treatment scheme and
operating parameters of pre-oxidation and BAF were described in our
previous study [23]. The dosage of O3 and Fe(VI) was 80 mg/L and 40
mg/L, respectively. The BAF system was first subjected to microbial
acclimation prior to continuous operation of the system. After 42 days of
acclimation, the system gradually formed a stable microbial community
structure. In our past work [23], we evaluated the performance of
oxidation-BAF in removing organic contaminants. The BAF system was
running for approximately 100 days under the condition that the EBCT
was 5 h. In this work, we further explored the treatment efficiency of
oxidation-BAF for four kinds of SGW samples with different EBCT by
using the previous device and varying process parameters. The EBCT
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Separation and Purification Technology 291 (2022) 120920
changed from 5 h to 1 h to reduce the operating cost of the BAF system.
The effluent of the oxidation-BAF reactors was collected for 48 h for
each SGW sample (Table S3), which underwent subsequent membrane
filtration.
The detailed steps of the membrane process are similar with our
previous works [11,29]. For UF experiment, 10 cm2 poly(vinylidene
fluoride) (PVDF) hollow fiber UF membrane (Litree Purifying Technol­
ogy Co., Ltd., China) were employed. The filtration contained a 2 h
filtration and 8 min hydraulic backwash under a constant flux of 50 L/
(m2⋅h) (LMH). The filtration was automatically stopped when the
transmembrane pressure (TMP) reached 55 kPa. For RO experiment,
14.6 cm2 aromatic polyamide composite membrane (Vontron Mem­
brane Technology Co., Ltd., China) were employed. Water recovery of
50% was assessed in the RO process with a 5.5 MPa operation pressure.
2.3. Membrane fouling evaluation and XDLVO theory
The fouling index was used to evaluate the extent of UF membrane
fouling under constant flux. The total fouling index (TFI) represents the
extent of membrane fouling after the whole filtration [30]. In contrast,
the hydraulically irreversible fouling index (HIFI) stands for membrane
fouling that cannot be removed through hydraulic backwash [30]. The
type of membrane fouling was identified by fitting the UF system data
with the classical pore blocking model [29]. The four kinds of membrane
pore blocking models are listed in Table S4. The interaction energy of
cohesion between foulants and foulants (ΔGTOT fwf ) and the adhesion be­
tween foulants and the UF membrane (ΔGTOT fwm ) were correlated with the
surface tension parameters of foulants and the membrane based on the
XDLVO theory. The total interaction energy was the sum of the Lifshitz-
Van der Waals components, the Lewis acid-base components, and the
electrostatic force component. Thereinto, the value of electrostatic force
component was small which can be neglected [31–33]. The foulants in
SGW were deposited onto a PVDF UF membrane with the molecular
weight cut-off of 100 kDa, using a dead-end membrane filtration system
for a 24 h to obtain a dense fouling layer. And the fouling layer deposited
on the membrane was allowed to dry for 24 h at 40 ℃ prior to taking the
contact angle measurements. The measurement was performed on the
fouling layer using the above sessile-drop method, in which a 2 µL liquid
droplet of the probe liquid was utilized. At least six measurements were
taken for each sample. The calculation steps of XDLVO theory are pre­
sented in Text S2 and can be found in our previous study [29].
2.4. Membrane fouling layer characterization
Scanning electron microscopy (SEM) (Regulus 8230, Hitachi, Japan)
and energy dispersive spectroscopy (EDS) were used to acquire the
morphology and elemental ratio of the membrane fouling layers. The
chemical bonds on membrane fouling layers were measured using a
Fourier transform infrared spectrometer attenuated total reflectance
(ATR-FTIR) (Nicolet IS20, Thermo Fisher Scientific Inc., USA). ATR-
FTIR can detect the depth over 300 nm when wavenumbers are below
2000 cm− 1 [34].
3. Results and discussion
3.1. Oxidation behavior of two oxidants (O3 and Fe(VI))
The effects of pre-oxidation on the water quality characteristics of
the four kinds of SGW samples are shown in Table S5 and Fig. S2. The
data showed that two oxidants (O3 and Fe(VI)) had a limited ability to
mineralize organic compounds in treating SGW (DOC removal rate <
6%), and that they principally altered the properties of organic com­
pounds [11,23,29]. Meanwhile, we observed that the oxidation
behavior of Fe(VI) was different from that of O3. For example, the
removal of fluorescent organics using Fe(VI) pre-oxidation was
P. Tang et al.
significantly lower than that using pre-ozonation, but the removal rate
of DOC by Fe(VI) was slightly higher than that of O3.
3.2. Oxidation-BAF performance under different EBCT in treating four
kinds of SGW samples
Fig. 1 shows that a decrease in EBCT slightly reduces the removal
rate of organic matter in all BAF systems. When the EBCT was 5 h, the
alone BAF system and oxidation-BAF systems could significantly remove
75.8% DOC and 80.0%-81.2% DOC, respectively. When the EBCT
changed to 1 h, the alone BAF system and oxidation-BAF systems could
remove 70.6% DOC and 72.7%-77.7% DOC, respectively. Similarly, the
reduction of EBCT slightly reduced the removal rate of UV254 by the BAF
systems. Thus, under the comprehensive consideration of economy and
process performance, 1 h was the optimal EBCT compared with 5 h. In
addition, the DOC removal efficiency decreased in the order O3-BAF >
Fe(VI)-BAF > BAF.
It is well known that the geochemical characteristics of SGW vary
with well location and operation time. Therefore, we measured the
removal efficiency of organic matter from the three BAF systems in
treating four kinds of SGW samples to assess its application potential, as
shown in Fig. 2. As expected, the efficiency of removing organic matter
by all BAF systems fluctuated greatly. The alone BAF system could
remove 45.3%-70.6% DOC. The DOC removal rate of the O3-BAF system
was 1.1–1.35 times higher than that of the alone BAF system, and the
DOC removal rate of the Fe(VI)-BAF system was 1.03–1.22 times higher
than that of the alone BAF system. These results indicated that pre-
oxidation could improve the efficiency of removing organic matter of
the subsequent BAF system, which may be attributed to the improve­
ment of the biodegradability of organic matter [23] and, in addition, the
enhancement influence of O3 was stronger than that of Fe(VI). The
UV254 removal rate of the alone BAF system was higher than that of the
oxidation-BAF systems. In our previous study [23], we found that pre-
oxidation decreased the adsorption rate and capacity of activated car­
bon for UV254-like organic compounds, and the Mesorhizobium genus in
Fig. 1. Removal of DOC and UV254 from SGW1 by BAF systems with or without pre-oxidation under different EBCT.
3
Separation and Purification Technology 291 (2022) 120920
the alone BAF reactor was significantly correlated with the UV254
removal rate, which might be the reason for the high UV254 removal rate
in the alone BAF reactor.
Furthermore, we performed linear fitting for the removal rate of
organic matter (DOC and UV254) with the influent concentration of
organic matter, as well as for the removal rate of organic matter with
influent salinity (TDS), as presented in Fig. 3. Notably, there was a
certain positive correlation (R2 = 0.53–0.87) between the removal rate
of organic matter and the influent content of organic matter. This result
suggested that the higher the concentration of organic matter in the
influent is, the higher the removal rate of organic matter in BAF systems.
This seemed an obvious result since, in general, the higher the concen­
tration of organic matter is, the higher the concentration of degradable
components of organic matter. Interestingly, there was no correlation
(R2 = 0.03–0.45) between the removal rate of organic matter and the
TDS content. This demonstrated that salinity had almost no effect on the
removal rate of organic matter in BAF systems when the TDS content
was 10–24 g/L, as with other published research [14].
3.3. Oxidation-BAF-UF performance: the primary mechanism of
membrane fouling mitigation
Fig. 4 presents the performance of UF systems with different pre-
treatments (BAF, O3-BAF or Fe(VI)-BAF) in treating four kinds of SGW
samples. This result demonstrated that pre-oxidation could not only
improve the removal efficiency of organic matter in the BAF system
(Fig. 2) but also effectively reduce UF membrane fouling in the UF
system (Fig. 4), especially using O3 pre-oxidation. Compared with BAF
pretreatment, O3-BAF could reduce TFI by 37%-60% and HIFI by 50%-
80%, and Fe(VI)-BAF could reduce TFI by 7%-24% and HIFI by 24%-
48% HIFI. Besides, it can be seen that the oxidation-BAF systems
reduced the DOC interception of the UF system compared with the alone
BAF system. This meant that the content of organic compounds that
could not pass through the UF membrane was reduced after oxidation-
BAF [29].
P. Tang et al.
Fig. 2. Removal of DOC and UV254 from four kinds of SGW samples by BAF systems with or without pre-oxidation. The EBCT is 1 h.
As shown in Fig. S4, there is little difference in the FTIR spectra of the
fouling layers of all UF systems. Some typical spectral peaks (600–1500
cm− 1) of the virgin PVDF membrane were only slightly weakened in the
FTIR spectra of all fouled membranes, which proved that the thickness
of all fouling layers was thin [35,36]. Meanwhile, three new peaks were
mainly discovered for the fouled membranes rather than the virgin
membranes. These peaks, which were located at 3200–3550 cm− 1, 1650
cm− 1, and 1540 cm− 1, originated from O-H stretching, amide I bands,
and amide II bands, respectively [37]. The results indicated that some
types of organic matter, such as proteins and humic substances, which
were common components of SGW [37,38], existed in the fouling layers.
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Separation and Purification Technology 291 (2022) 120920
From the surface topographies of fouling layers (Fig. S5), it was observed
that the fouling layer of the BAF-UF system was the densest compared
with oxidation-BAF-UF systems. Ca, Si, Na, Cl, K, C, and O were the
major constituents of the fouling layers (Fig. S5).
The fouling mitigation behavior of UF systems at the first filtration
cycle without or with pretreatment was further analyzed using four
classic membrane fouling models, namely, complete blocking, standard
blocking, intermediate blocking, and cake filtration [39–42]. The cor­
relation coefficient values (R2) of the regression analysis are shown in
Table S6. For the BAF-UF system, the R2 values of the four models are
almost all greater than 0.86, indicating that all four fouling types were
P. Tang et al.
Fig. 3. The relationship of DOC removal rate with influent DOC content, DOC removal rate with influent TDS content, UV254 removal rate with influent UV254
content, and UV254 removal rate with influent TDS content. The EBCT of BAF systems is 1 h.
present. Meanwhile, those results showed that all four membrane
fouling types existed in oxidation-BAF-UF systems (R2 greater than
0.87), which confirmed that pre-oxidation has little effect on the type of
membrane fouling. Therefore, we hypothesized that oxidation-BAF
mainly changed the rate of membrane fouling formation compared
with that of the alone BAF.
The pure water contact angles of the fouled UF membranes are
presented in Table S7. Compared to the fouled membrane of the BAF-UF
system, the contact angle of the fouled membrane of the oxidation-BAF-
UF system was lower, especially for the O3-BAF-UF system. This result
indicated that the organic matter in the effluent of the BAF was more
hydrophilic after pre-oxidation [29]. The variation in the hydrophilicity
of foulants would affect the physicochemical interactions between
membrane and foulants, and between foulants and foulants [43].
XDLVO theory has been widely used to quantitatively calculate inter­
facial energy between membrane and foulants, and between foulants
and foulants, in evaluating the potential of membrane fouling [43,44].
By calculation, the values of ΔGTOT TOT
fwf and ΔGfwm are obtained, as shown in
Table S8. In general, a positive value of interaction energy indicates
repulsion, and a negative value means attraction [45]. Table S8 shows
that the values of ΔGTOT TOT
fwf and ΔGfwm in the BAF-UF system are negative,
suggesting an attractive function between foulants and foulants and
between membrane and foulants that would aggravate membrane
fouling. However, the values of ΔGTOT TOT
fwf and ΔGfwm of oxidation-BAF-UF
systems increased to positive values, indicating that oxidation-BAF can
reduce the hydrophobic adsorption of foulants-foulants and decrease the
attraction between the membrane and foulants compared with the alone
BAF [46]. Furthermore, we performed linear fitting for the membrane
fouling index (TFI and HIFI) with ΔGTOT TOT
fwf or ΔGfwm , as presented in Fig. 5.
Notably, there was a significant positive correlation (R2 = 0.77–0.88)
5
Separation and Purification Technology 291 (2022) 120920
between TFI and ΔGTOT
fwf , and there was a significant positive correlation
(R2 = 0.59–0.83) between HIFI and ΔGTOT fwm . These results suggested that
oxidation-BAF decreased the TFI value of the UF process by mainly
decreasing the hydrophobic adsorption of foulant-foulants and reduced
the HIFI value of the UF process by mainly increasing the repulsion
between the membrane and foulants compared with the alone BAF. This
was the main mechanism of membrane fouling mitigation in the
oxidation-BAF-UF system.
3.4. Oxidation-BAF-UF-RO performance
Fig. 6 illustrates the variation of RO fluxes in treating effluents of the
BAF-UF system or oxidation-BAF-UF systems. In general, the flux dif­
ference between oxidation-BAF-UF-RO systems and the BAF-UF-RO
system was small, and the flux of oxidation-BAF-UF-RO systems was
slightly larger than that of BAF-UF-RO system which may be attributed
to the low content of organics in effluents of oxidation-BAF-UF process.
Images of the RO membrane fouling layers were obtained by using SEM,
as presented in Fig. S8. Some contaminants, such as crystals, were
deposited on the surface, and the dominant proportions of contaminants
were Na, Cl, K, Mg, and Si, which was similar to past research [11]. As
expected, there was no significant difference in the effluent quality of all
systems (Table S9). In short, the combined process displayed good
performance in removing cations and organics, and the water quality of
the effluent met the standard for external reuse (Table S10 and
Table S11).
4. Conclusion
A combined system of pre-oxidation, BAF, UF, and RO was demon
P. Tang et al.
Fig. 4. The variation of TMP, FI index, and DOC interception of UF systems with different pre-treatments (BAF, O3-BAF or Fe(VI)-BAF) in treating SGW1 (A), SGW2
(B), SGW3 (C), and SGW4 (D). The EBCT of BAF system is 1 h.
strated for treating four varied SGW samples. This work showed that
pre-oxidation could effectively improve the efficiency of removing
organic substances in the subsequent BAF process, despite the variable
geochemical characterizations of the four sourced SGW samples
(ranging from 11.71 to 22.54 g/L TDS). Thereinto, O3 pre-oxidation
significantly improved the removal rate of DOC (110%-135%) in the
BAF system. Under the comprehensive consideration of economy and
6
Separation and Purification Technology 291 (2022) 120920
process performance, 1 h was the optimal EBCT of the BAF system
compared with 5 h previously. Moreover, it was found that oxidation-
BAF can also significantly reduce UF membrane fouling in subsequent
membrane processes. Compared with BAF pretreatment, O3-BAF
reduced TFI by 37%-60% and HIFI by 50%-80%. The fitting result of the
membrane pore blocking model and the result of XDLVO theory
demonstrated that the principal mechanism of UF membrane fouling
P. Tang et al. Separation and Purification Technology 291 (2022) 120920

Fig. 5. The relationship of ΔGTOT TOT TOT TOT

fwf with TFI, ΔGfwf with HIFI, ΔGfwm with TFI, and ΔGfwm with HIFI.

Fig. 6. The variation of flux in RO systems with different pre-treatments (BAF-UF, O3-BAF-UF or Fe(VI)-BAF-UF) in treating four kinds of SGW samples. The EBCT of
BAF system is 1 h.

mitigation was the increased values of ΔGTOT TOT

fwf and ΔGfwm by oxidation-
BAF letting it more difficult for foulants to absorb or deposit on the
membrane pores and membrane surface, thus delaying the formation
rate of membrane fouling. The influence of pre-oxidation on mitigating
membrane fouling should be further verified in long-term operation, and
biological fouling should be considered in the analysis of the membrane
fouling mitigation mechanism. Overall, the effluent of the oxidation-
BAF-UF-RO process can meet the standard for external reuse. In

7
P. Tang et al.
addition, the O3-BAF-UF-RO process has exciting potential to be
employed onsite on a large scale.
CRediT authorship contribution statement
Peng Tang: Investigation, Validation, Writing – original draft.
Wancen Xie: . Lun Tian: . Bin Tan: Resources. Yongli Zhang: Re­
sources, Writing – review & editing. Zhishan Yang: Writing – review &
editing. Chen Chen: Resources. Weiming Zhang: Writing – review &
editing. Baicang Liu: Conceptualization, Supervision, Writing – review
& editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
This work was supported by the National Natural Science Foundation
of China (52070134), State Key Laboratory of Pollution Control and
Resource Reuse (PCRRF20016), and Sichuan University and Yibin City
People’s Government strategic cooperation project (2020CDYB-2).
Appendix A. Supplementary material
The Supporting Information is available open-access on the website.
Supplementary data to this article can be found online at https://doi.org
/10.1016/j.seppur.2022.120920.
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