FRMST 03 1361433
FRMST 03 1361433
FRMST 03 1361433
Recent advances of
OPEN ACCESS membrane-based hybrid
EDITED BY
Mohammad Mahdi A. Shirazi,
Aalborg University, Denmark
membrane bioreactors for
REVIEWED BY
Hang Liu,
wastewater reclamation
Chinese Academy of Sciences (CAS), China
Nuwan Asanka Weerasekara,
University of Sri Jayewardenepura, Sri Lanka
Jeonghwan Kim 1*, Bing Wu 2, Sanghyun Jeong 3,
S. Saeid Hosseini, Seongpil Jeong 4,5 and Minseok Kim 1
University of South Africa, South Africa
1
Department of Environmental Engineering, Program of Environmental and Polymer Engineering, Inha
*CORRESPONDENCE
University, Incheon, Republic of Korea, 2Faculty of Civil and Environmental Engineering, University of
Jeonghwan Kim,
Iceland, Reykjavík, Iceland, 3Department of Environmental Engineering, Pusan National University,
jeonghwankim@inha.ac.kr
Busan, Republic of Korea, 4Center for Water Cycle Research, Korea Institute of Science and Technology,
RECEIVED 26 December 2023 Seoul, Republic of Korea, 5Division of Energy & Environmental Technology, KIST School, University of
ACCEPTED 15 February 2024 Science and Technology (UST), Seoul, Republic of Korea
PUBLISHED 29 February 2024
CITATION
Kim J, Wu B, Jeong S, Jeong S and Kim M
(2024), Recent advances of membrane-based
Membrane bioreactor (MBR) is an advanced wastewater treatment technology,
hybrid membrane bioreactors for
wastewater reclamation. which has been established for more than 3 decades. In MBRs, membrane
Front. Membr. Sci. Technol. 3:1361433. separation allows not only rejecting microorganisms/greater-sized molecules
doi: 10.3389/frmst.2024.1361433
but decoupling hydraulic retention time (HRT) and solid retention time (SRT).
COPYRIGHT Low-pressure driven, porous membranes have been widely used in MBRs, but
© 2024 Kim, Wu, Jeong, Jeong and Kim. This is
their performances are mainly limited for wastewater reuse applications.
an open-access article distributed under the
terms of the Creative Commons Attribution Recently, many attempts have been made to combine desalination
License (CC BY). The use, distribution or technologies to advance hybrid MBR processes for wastewater reclamation.
reproduction in other forums is permitted,
Nanofiltration (NF) and reverse osmosis (RO) have been applied with the MBRs
provided the original author(s) and the
copyright owner(s) are credited and that the to improve effluent quality, and their advantages and challenges have been well
original publication in this journal is cited, in reported in terms of rejection efficiency, operational energy, fouling control and
accordance with accepted academic practice.
recovery of retentate stream. Alternatively, the direct introduction of non-
No use, distribution or reproduction is
permitted which does not comply with these pressurized desalination technologies such as forward osmosis (FO) and
terms. membrane distillation (MD) into MBR processes for wastewater reclamation or
probably for microbial activity have been considered substantially due to their low
energy consumption and excellent rejection efficiency of solid materials.
However, several technical limitations still need to be resolved to
commercialize hybrid FO- or MD-MBR processes. This paper reviews recent
advances of MBR technology integrated with desalination technologies for
wastewater reclamation and suggests perspectives to optimize membrane-
based hybrid MBR process.
KEYWORDS
1 Introduction
Membrane bioreactor (MBR) is a well-developed membrane-based wastewater
process by combining biodegradation and separation to remove organic/inorganic
contaminants from wastewater (Xue et al., 2010). The MBR has great advantages in
terms of separating hydraulic retention time (HRT) and solid retention time (SRT) while
producing excellent effluent (permeate) quality for discharge (Skouteris et al., 2012; Smith
et al., 2012). Needs to incorporate reuse of wastewater effluents by consequences of
population growth, rapid urbanization and water shortage are 2 Conventional MBR combined with
growing rapidly for sustainable wastewater management NF/RO membrane system
planning (Van de Walle et al., 2023). However, due to strict
wastewater reuse standards, the MBR permeate may not meet 2.1 Overview
such requirements, thus requiring additional treatments (Tibi
et al., 2019; Kwon et al., 2021). Generally, MBRs displayed excellent removal efficiency for
Value of reclaimed water can be enhanced further by organics and nutrients via biodegradation and membrane
developing membrane based hybrid MBR processes (Liu et al., rejection, but showed limited rejection of smaller-sized, dissolved
2010; Krzeminski et al., 2012). Desalination technologies such as substances (such as humic-like substances, low molecule weight
reverse osmosis (RO), nanofiltration (NF), forward osmosis (FO) organics, heavy metals, micropollutants, etc.) that readily pass
and membrane distillation (MD) have been established mostly in through the porous membranes (Judd, 2010). Towards achieving
seawater desalination (Aliyu et al., 2018; Ray et al., 2018; Qasim wastewater reclamation, further membrane separation processes,
et al., 2019; Wafi et al., 2019). Here, membrane-based hybrid MBR such as NF or RO, have been employed to further purify the MBR
is classified into conventional MBR integrated with desalination permeate. Many research studies listed in Table 1 have proven that
membrane such as NF or RO as post-treatment and a novel hybrid the MBR + NF/RO hybrid processes could achieve high efficiency
MBR where NF, FO or MD membrane is introduced directly into and stable performance, which allows them as the most promising
bioreactor. However, there are many attempts how to combine technologies for wastewater reclamation.
and tailor desalination technologies with MBRs to provide Compared to RO processes, the NF processes are capable to
synergistic impacts for wastewater reuse purposes. Membrane- provide a higher permeate flux or higher recovery ratio with lower
based hybrid MBR processes offer great benefits because they can operating pressure and cost (Sert et al., 2016). The NF membrane
produce superior water quality criteria at small footprint and may be suitable to remove low salinity wastewater where high ion
excellent rejection efficiency (Rodríguez-Hernández et al., 2014; selectivity is not required, inducing monovalent-divalent ion
Tang et al., 2022). Additionally, combining the MBRs with selectivity (Nativ et al., 2021). The NF membranes can provide
desalination membranes can intensify the MBR centered very high removal of macromolecules that include those associated
process for wastewater reclamation (Krzeminski et al., 2012; with EPS, SMP and NOM. However, the RO membrane can remove
Wang et al., 2015b; Burman and Sinha, 2020; Zhu et al., 2022). all inorganic chemicals and low-molecular weight organic chemicals
Nevertheless, the effluent produced by MBR still contains variety that would pass through the NF membrane. Thus, the MF/UF-MBR
of pollutants mostly caused by microbial activities, inorganic + NF process is considered as an alternative approach for wastewater
species and non-biodegradable fractions (Stoquart et al., 2012; reclamation that can compromise between permeability and
Yan et al., 2018). Therefore, additional treatments for fit-for- selectivity. As indicated in Table 1, the MF/UF-MBR + NF
purpose should be required to reuse secondary effluent for various process has been successfully applied to treat municipal
reuse purposes. For indirect potable reuse, the existence of wastewater (Jacob et al., 2010; Chon et al., 2011; Chon et al.,
refractory (or non-biodegradable) natural organic matter 2013; Kappel et al., 2014; Chon et al., 2015; Woo et al., 2016;
(NOM) which would not be rejected effectively by MF or Arola et al., 2017; Hacıfazlıoğlu et al., 2019; Arola et al., 2021;
ultrafiltration (UF) in the MBR needs post-treatment or direct Yacouba et al., 2021) and various types of industrial wastewater
usage of the membranes having much high rejection capability in (Wintgens et al., 2002; Dialynas and Diamadopoulos, 2009; Andrade
bioreactor. Organics of potential concern, particularly for indirect et al., 2014; Wang et al., 2015a; Hosseini et al., 2016; Li et al., 2016;
potable reuse applications, include pesticides, pharmaceutically- Reis et al., 2017; Sert et al., 2017; Lan et al., 2018; Moser et al., 2018;
active chemicals and endocrine-disrupting chemicals. For Cinperi et al., 2019; Li et al., 2020a; Reis et al., 2020). In most of the
anaerobic MBR (AnMBR), anaerobic effluent (permeate) studies, the treated water quality could meet the standards of
contains high load of nutrients such as nitrogen and dissolved reclaimed water quality for different uses, such as for urban uses,
methane. Depending upon qualities in MBR permeate, for industrial uses, for groundwater recharge, and for farmland
desalination technologies are reliable options and thus needs to irrigation (WHO, 2006).
be tailored to improve not only effluent qualities but also Towards further improving the treated water quality (e.g.,
microbial activities (Pearce, 2008; Falizi et al., 2018; Liu producing ultrapure water as fresh water source), a combination
et al., 2023). of MBR and RO was adopted, which could exhibit superior organic
The MBR requires additional treatment although there is removals compared to MBR + NF systems. The total nitrogen (TN)
currently no agreement on the best among the current options; in the permeates of MBR + RO and MBR + NF were different,
NF, RO, FO and MD technology. Mostly, the MBR uses MF or UF possibly due to different rejection efficiencies of nitrogen species, for
membranes for removal of particles, macromolecules and larger example, 71.7% for NF90% and 86.2% for BW30 membrane by both
microbes. However, there are existences of non-biodegradable NF and RO membranes (Cinperi et al., 2019; Hacıfazlıoğlu et al.,
organics, effluent organic matter or colloidal fraction consisting 2019). It was also reported that the MBR + RO rejected TN about
of microbial by-products. Macromolecules associated with 10% higher than MBR + NF (Cinperi et al., 2019). Also, there was
microbial product such as extracellular polymeric substance only 3% higher in TN removal efficiency by MBR + RO than MBR +
(EPS), soluble microbial product (SMP) or NOM, low- NF process operated at same transmembrane pressure (TMP)
molecular weight organic chemicals and inorganic chemicals (Hacıfazlıoğlu et al., 2019). Thus, the conventional biological
present in the MBR should also be multiple barriers to indirect processes such as anaerobic and/or anoxic reactors are generally
potable reuse. implemented with an aerobic MBR for elimination of both organics
Municipal Aerobic MBR Submerged MF COD: 22 mg/L; TP: Two-stage NF (220- COD: 2.6 mg/L; TP: Arola et al. (2021)
wastewater (PVDF, 0.2 μm) 4.4 mg/L; TN: 250 Da, recovery 0.7 mg/L; TN: 22 mg/L
23 mg/L ratio at 83% and
98% for first- and
second-stage,
respectively)
Municipal Aerobic MBR Submerged hollow DOC: 6.01 mg/L NF (350 and DOC: 0.4-0.7 mg/L Chon et al. (2015)
wastewater fibre MF (PVDF, 210 Da)
0.1 μm)
Municipal Aerobic MBR Submerged hollow DOC: 6.07 mg/L; TN: NF (350 and DOC: 0.4-0.7 mg/L; TN: Chon et al. (2013)
wastewater fibre MF (PVDF, 32.99 mg/L 210 Da) 9.7-31.1 mg/L
0.1 μm)
Municipal Aerobic MBR Submerged hollow DOC: 8.16 mg/L; TN: NF (210 Da) DOC: 2.8 mg/L; TN: Chon et al. (2011)
wastewater fibre MF (PVDF, 48.06 mg/L 11.4 mg/L
0.1 μm)
Municipal Aerobic MBR Submerged hollow NF (~150 Da) or MBR + NF: TOC: Hacıfazlıoğlu et al.
wastewater fiber MF (PVDF, RO (recovery ratio 1.46 mg/L; TN: 1.44 mg/ (2019)
0.1 μm) at 50%) L MBR + RO: TOC:
0.91 mg/L; TN:
1.25 mg/L
Municipal Aerobic MBR Submerged hollow TOC: 6.0-8.0 mg/L NF (~150 Da) or MBR + NF: TOC: 0.54- Jacob et al. (2010)
wastewater fibre UF (PVDF, RO (recovery ratio 0.72 mg/L; MBR + RO:
200 kDa) at 10%-70%) TOC: 0.24-0.3 mg/L
Municipal Aerobic MBR Submerged flat sheet TOC: 17 mg/L NF (recovery ratio TOC: 0.5 mg/L Kappel et al. (2014)
wastewater MF (PVDF, 0.4 μm) at 85%)
Municipal Aerobic MBR (with and Submerged flat sheet MBR: COD: NF (300-400 Da, MBR + NF: COD: Woo et al. (2016)
wastewater without PAC) MF (PVDF, 0.08 μm) 158.83 mg/L; TN: recovery ratio 15 mg/L; TN: 2.68 mg/L
(Synthetic) 24.50 mg/L PAC- at 82.5%) PAC-MBR + NF: COD:
MBR: COD: 9.88 mg/L; TN:
133.49 mg/L; TN: 1.89 mg/L
24.47 mg/L
Municipal Aerobic MBR Submerged hollow DOC: 2.12-10.21 mg/ RO (recovery ratio DOC: 1.04–4.1 mg/L; Dialynas and
wastewater fibre MF (0.04 μm) L; TN: 47-83 mg/L at 50%) TN: 17-21 mg/L Diamadopoulos
(2009)
Municipal Aerobic MBR Submerged hollow DOC: 3.6-5.9 mg/L RO (recovery ratio DOC: 0.1–0.39 mg/L Farias et al. (2014)
wastewater fibre MF (0.05 μm) at 62%-70%)
Municipal Aerobic MBR Submerged flat sheet COD: 21 mg/L; RO (recovery ratio COD: <4 mg/L; Malamis et al.
wastewater MF (PVDF, 0.04 μm) Ammonium-N: <0.5- at 40%) Ammonium-N: 0.5- (2012)
24.0 mg/L; Nitrate-N: 1.1 mg/L; Nitrate-N:
17-48 mg/L 2.2-3.8 mg/L
Municipal Aerobic moving bed External hollow fibre RO (recovery ratio - Tay et al. (2018)
wastewater biofilm MBR NF (200-300 Da) at 0% and 90%)
Municipal Aerobic moving bed Submerged tubular COD: 7.2-7.4 mg/L; RO COD: 0.24-0.44 mg/L Wang et al. (2019)
wastewater biofilm MBR MF (Ceramic, TN: 19.6-25.94 mg/L TN: 0.98-1.15 mg/L
(Synthetic) 0.02 μm)
Municipal Aerobic moving bed Submerged tubular TOC: 3.1 mg/L; RO TOC: 0.093 mg/L; Sun et al. (2021)
wastewater biofilm MBR MF (Ceramic, 0.2 μm) Nitrate-N: 1.83 mg/L Ammonium-N: N.D.
(Synthetic) Nitrate-N: 0.110 mg/L
Municipal Anaerobic MBR Submerged hollow TOC: 3.60 mg/L; RO + ion exchange MBR + RO: TOC: Gu et al. (2019)
wastewater fibre MF (PVDF, Ammonium-N: 0.13 mg/L; Ammonium-
(Synthetic) 0.02 μm) 41.9 mg/L N: 2.1 mg/L; MBR + RO
+ ion exchange: TOC:
0.13 mg/L; Ammonium-
N: <1 mg/L
Antibiotic processing Aerobic MBR Submerged flat sheet TOC: 126.24 mg/L NF (150-300 Da, TOC: 2 mg/L Li et al. (2016)
wastewater MF (PVDF, 0.1 μm) recovery ratio at
40%-90%)
Antibiotic processing Aerobic MBR Submerged flat sheet TOC: 79 mg/L; NF (~150 Da, TOC: 5.52 mg/L; Wang et al. (2015a)
wastewater MF (PVDF, 0.1 μm) Ammonium-N: recovery ratio Ammonium-N:
9.4 mg/L at 92%) 0.68 mg/L
Dairy wastewater Aerobic MBR Submerged hollow COD: 57.3 mg/L; TS: NF (~150 Da, COD: 4 mg/L; TS: Andrade et al.
fibre MF (PEI,0.5 μm) 1.647 mg/L recovery ratio 233 mg/L (2014)
at 45%)
Fruit processing Aerobic MBR Submerged flat sheet RO Pesticides >95.4% de Almeida Lopes
wastewater UF (PES) et al. (2020)
Hospital wastewater Aerobic MBR Submerged hollow NF (250 Da, - Lan et al. (2017)
fibre MF (PS, 0.2 μm) recovery ratio
at 80%)
Hospital wastewater Aerobic MBR Submerged hollow TOC: 8.40-31.40 mg/L NF (250 Da, TOC: 0.5-15.5 mg/L Lan et al. (2018)
fibre MF (PS, 0.2 μm) recovery ratio
at 80%)
Industrial wastewater - - COD: 21.5 mg/L; RO (recovery ratio MBR + RO: COD: 5 mg/ Parlar et al. (2019)
TN: 45.5 at 68.6%) or NF + L; TN: 3.8 mg/L MBR +
RO (recovery ratio NF + RO: COD: 5 mg/L;
at 67.7% and 69.1% TN: 2.8 mg/L
respectively)
Industrial wastewater - - NF (~200 Da, MBR + NF: TOC: Sert et al. (2016)
recovery ratio at 2.15 mg/L; Ammonium-
35%-52.5%) or RO N: 0.14 mg/L; Nitrate-N:
(recovery ratio at 6.21 mg/L MBR + RO:
35%-44.5%) TOC: 1.95 mg/L;
Ammonium-N:
0.10 mg/L; Nitrate-N:
3.56 mg/L
Leachate wastewater Aerobic MBR Submerged hollow COD: 1,445-3374 mg/ NF (200-400 Da, COD: 77-457 mg/L; TN: Reis et al. (2017)
fibre MF (PEI, 0.5 μm) L; TN: 888-1,508 mg/L recovery ratio 230-699 mg/L
at 60%)
Leachate wastewater Aerobic MBR Submerged hollow COD: 3374 mg/L; TN: NF (200-400 Da) COD: 457 mg/L; TN: Reis et al. (2020)
fibre MF (PEI, 1750 mg/L 699 mg/L
0.45 μm)
Petroleum refinery Aerobic MBR Submerged hollow TOC: 12.70 mg/L; NF (100 Da) or MBR + NF: TOC: Moser et al. (2018)
wastewater fibre MF (PVDF, Ammonium-N: UV/H2O2 +NF 0.58 mg/L Ammonium-
0.04 μm) 1.6 mg/L; Nitrate-N: (100 Da) N: 0.4 mg/L; Nitrate-N:
169 mg/L 6.52 mg/L MBR + UV/
H2O2 +NF: TOC:
0.96 mg/L; Ammonium-
N: 0.3 mg/L; Nitrate-N:
5.82 mg/L
Textile wastewater Aerobic MBR Submerged hollow COD: 132.8 mg/L; TN: NF (220-250 Da) MBR + NF: COD: 3- Cinperi et al. (2019)
fibre MF (0.02 μm) 34.2 mg/L or RO 5 mg/L; TN: 17.7-
18.4 mg/L MBR + RO:
COD: <1 mg/L; TN:
14.4-16.5 mg/L
Textile wastewater Aerobic MBR Submerged flat sheet NF (200-400 Da, COD: 13.94 mg/L; Li et al. (2020a)
UF (PVDF, ≤100 Da) recovery ratio at Ammonium-N:
39%-90%) 3.54 mg/L; Nitrate-N:
75.79 mg/L
COD, chemical oxygen demand; PE, polyethylene; PEI, polyetherimide; PS, polysulfone; PVDF, polyvinylidene fluoride; TOC, total organic carbon; TN, total nitrogen.
and nutrients (nitrogen and phosphorus) before the MBR permeate approach via integrating a bioreactor with an external porous NF
is fed into the RO system (Li et al., 2020b). Alternatively, a biofilm membrane (i.e., NF-MBR) has been attempted as pretreatment of
MBR is adopted for simultaneous removals of organic and nitrogen wastewater for the RO process (Tay et al., 2018; Tay et al., 2020).
and its permeate is further purified by a RO membrane, which shows Apparently, compared to MF/UF-MBR, the NF-MBR produced the
several advantages such as low energy consumption, small footprint, permeate with lower organic/inorganic substances, accordingly, the
and limited sludge production (Wang et al., 2019). Whether the RO subsequent RO membrane receiving the NF-MBR permeate
membranes would experience more fouling potential than the NF displayed better performance. Importantly, under the comparable
membranes in the MBR + NF/RO systems are still under debate. energy consumption scenario, the NF-MBR-RO system could
Some research work highlighted that the RO membrane displayed achieve a water recovery ratio up to 90%, higher than that of the
excellent rejection of both cations and anions, which could be MF/UF-MBR-RO system (recovery ratio of 75%).
responsible for more inorganic fouling of RO membranes In this decade, AnMBRs have received great attention due to
(Hacıfazlıoğlu et al., 2019). While other studies pointed out the their high-quality effluent, limited sludge production, and energy
low molecular weight organic molecules in the MBR permeate could production (i.e., methane) (Wu and Kim, 2020). A combination of
potentially contribute to internal pore blocking of NF membranes, anaerobic MBR with RO process have been explored to produce
which led to more serious NF membrane fouling, especially at lower high-grade reclaimed water for both non-potable and potable use
water recovery ratios and for more tight NF membranes (Jacob (Gu et al., 2019; Li et al., 2020b). As stand-alone AnMBRs are
et al., 2010). ineffective for removing nutrients (e.g., ammonium and phosphate)
Effluent quality from the MBR is critical in biofouling on NF/RO and RO membranes have limited ammonium rejection efficiency,
membranes (Al-Amoudi and Lovitt, 2007; Jiang et al., 2017; Matin integration of an additional polishing process with AnMBR + RO for
et al., 2021). Nevertheless, studies to make direct comparison of ammonium removal is suggested. For example, an ion exchange
fouling behaviors between NF and RO membrane are still very process was supplemented to purify AnMBR + RO permeate (Gu
limited. Effect of surface roughness on biofouling was more et al., 2019); a zeolite adsorption process was employed to treat an
pronounced than operational conditions for both NF and RO AnMBR permeate water before its feeding to a RO process (Li
membrane (Alturki et al., 2010). Given its relatively high et al., 2020b).
rejection efficiency, biofouling would be formed more
preferentially by RO than NF membrane from MBR permeate
(Kimura et al., 2009). Moreover, when RO and NF membranes 2.2 The factors that influencing MBR + NF/
were exposed to the same biofouling condition with Pseudomonas RO performance
aeruginosa, final cell concentration on RO membrane was lower
than NF membrane in the presence of pharmaceutically active 2.2.1 Effect of NF/RO membrane property
compounds (Yang et al., 2018). Although NF/RO membranes show great rejection of organics/
Nevertheless, improving the quality of MBR permeate (i.e., RO inorganics derived from the MBR permeate due to their dense
feed water) is crucial in alleviating RO membrane fouling. A feasible membrane natures, the MBR + NF/RO permeate quality could be
impacted by the NF/RO membrane property (such as pore size of such effects could be accelerated when the recovery ratio is above
NF membrane, surface charge, hydrophobicity, etc.). It has been well certain threshold level which is about 45% (Andrade et al., 2014).
illustrated that size-exclusion performed a crucial role in rejection of Towards superior NF/RO permeate quality, the NF recovery ratio at
organic substances by NF membranes, i.e., with decreasing NF 50%-85% and RO recovery ratio at 50%-75% were generally adopted
membrane pore size, more organic substances (such as humic- in the reported studies (Table 1). Thus, high volume of NF/RO
like substances) could be retained by NF membranes, improving concentrate with diluted nature is produced. Further post-treatment
MBR + NF permeate quality (Chon et al., 2013; Chon et al., 2015). of NF/RO brines that contain great amounts of nutrients, refractory
While, in terms of micropollutants, size exclusion, hydrophobic/ organic compounds, and inorganic salts is necessary as an efficient
hydrophilic interactions, and electrostatic interactions performed membrane concentrate management strategy. To increase water
major roles in rejection of micropollutants in NF/RO processes, and recovery ratio in the MBR + NF system, one solution was to employ
the dominance of these mechanisms is associated with the second-stage rotational NF process with high turbulent force by
characteristics of NF/RO membranes and micropollutants. For rotating blade on membrane surface to concentrate the first-stage
example, the molecular weight cut-off of NF membranes NF brine, which allowed simultaneously improving water
governed the removal efficiencies of N-nitrosamines, heavy production, allowing 300 times NF brine volume reduction, and
metals, and metalloids compared to adsorption and formation of recovering phosphorus to 86% via spontaneous crystallization of
membrane fouling on the NF membranes (Chon et al., 2013; Chon calcium phosphate (Arola et al., 2021).
et al., 2015). In a study on MBR + NF for leachate wastewater In the real operation of MBR + NF, the NF concentrate is
treatment (Wintgens et al., 2002), it was found that the generally recycled back to the preceding MBR in order to enhance
hydrophobicity of the NF membrane could influence the wastewater recycling efficiency and reduced the discharge of NF
retention of nonylphenol (NP), but did not determine the brine wastewater. While, the recirculation of RO concentrate to the
retention of bisphenol A. With solution-diffusion transport of NP MBR is not practical due to their relatively higher salinity, which
through NF membrane, the transport of NP is constant through the generally requires post-treatment before discharge. It is noted that
membrane while the water flux increases in more hydrophilic recirculating NF brine back to the bioreactor caused the
conditions, so that the NP retention increases (Wintgens et al., accumulation of organics, nitrogen, phosphorus and divalent ions
2004). In contrast, the MBR + RO displayed excellent mitigation of in the MBRs, which could potentially affect the system performance
organics (Jacob et al., 2010; Hacıfazlıoğlu et al., 2019), and pollutant mitigation (Kappel et al., 2014; Wang et al., 2015a).
micropollutants, such as pesticides (de Almeida Lopes et al., First, increasing NF brine recirculation ratio could lead to a
2020), heavy metals (Dialynas and Diamadopoulos, 2009). It decreased of biomass amount, which was attributed to the negative
should be realized that in certain conditions, the micropollutant effects of accumulated toxic and refractory organics/inorganics
removal ratios in the MBR + RO still slightly lower than that in the (especially causing increased salinity) on the sludge production in
MBR + activated carbon system (e.g., >95.4% of 2,4-D, atrazine, the MBR. Nevertheless, no significant change of microbial
carbendazim, and diuron removal in MBR + RO vs >98.6% in MBR community in the MBR was noticed with the recycling of the NF
+ activated carbon), implying the importance of RO membrane concentrate. Meanwhile, once the microbial community adopted to
property in micropollutant mitigation (de Almeida Lopes such operation conditions, the sludge was able to maintain at a
et al., 2020). relatively constant level (Kappel et al., 2014; Wang et al., 2015a; Li
Furthermore, the NF/RO membrane characteristics also et al., 2020a).
influence NF/RO fouling potential. Compared to the NF Second, recirculating NF brine back to the MBR may influence
membrane with relatively larger pore size, the NF membrane the permeate quality of both MBR and MBR + NF. In several
with fine pore size had more significant flux decline when they documented studies, it was observed that the presence of the
received the same MBR permeate (Jacob et al., 2010; Chon et al., recirculation of NF retentate could cause decreasing removal
2013). Similarly, the permeability decline of the RO membrane ratios of organics and ammonia in the MBR. Generally, the
decreased more significantly than the NF membrane, especially at a predominant organics in the MBR permeate are proteins,
higher recovery ratio (Jacob et al., 2010; Hacıfazlıoğlu et al., 2019). polysaccharides, and humic-like substances, which can be almost
However, at a lower recovery ratio, the flux decline of the RO completely rejected by NF membranes (Li et al., 2016). Accordingly,
membrane was slower than that of the NF membrane because the the organic contents in the MBR + NF permeate was negligibly
low molecular weight molecules in the MBR permeate could cause impacted by the NF brine recirculation ratio, showing steady
serious pore blocking of the NF membrane (Jacob et al., 2010). performance of NF membranes. However, it was noticed that
recirculating NF brine back to the MBR significantly aggregated
2.2.2 Effect of recovery ratio and brine the accumulation of nitrate in both the MBR and NF units, leading
recirculation ratio to more nitrate present in the MBR + NF permeate (Wang et al.,
In the MBR + NF/RO processes, water recovery ratio of NF/RO 2015a; Li et al., 2016; Li et al., 2020a). Furthermore, recirculating NF
process is an important parameter in determining productivity of retentate increases concentration-polarization layer on membrane
reclaimed water. Increasing recovery ratio in the NF/RO process due to the concentration of organics in MBR effluent, and this can
benefits improving water production, but more hydraulic driving reduce rejection efficiency by NF membrane. In terms of inorganics,
force is needed due to increased osmotic pressure and fouling (cause especially monovalent ions that are not readily completely rejected
by gel layer or adsorption) (Andrade et al., 2014; Arola et al., 2021). by the NF membranes, their levels in the MBR + NF permeate could
As a result, increased driving force could facilitate the retained significantly increase with elevating the recirculation ratio of the NF
molecules passing through the NF/RO membranes. In particular, retentate back to the MBR (Kappel et al., 2014; Li et al., 2016).
Third, the presence of NF brine recirculation back to the MBR permeate could be strongly dependent upon the feed wastewater
aggregated both MBR and NF membrane fouling. Several studies conditions and operation conditions of MBRs, which potentially
have highlighted that divalent ions and SMPs brought by NF influence the subsequent NF/RO performance (Wu et al., 2013;
concentrate are the dominant factors causing the severe Farias et al., 2014).
membrane fouling in MBRs. In addition, the organic fouling and For example, Farias et al. (2014) found that increasing the
inorganic scaling on the NF membrane appeared to increase due to SRT from 2 to 20 days facilitated alleviating membrane fouling
relatively high levels of organics/inorganics in the MBR permeate and enhanced organic removal in the MF-MBRs, but increased
(Kappel et al., 2014; Li et al., 2016; Li et al., 2020a). However, the fouling potential of the subsequent RO membranes. While, Wu
dominant NF membrane fouling mechanisms in the reported MBR et al. (2013) noticed that the MF-MBR operated at a high F/M
+ NF systems were dissimilar, possibly relating to the different ratio (0.50 g/g day−1, i.e., SRT at 7 days) had a more serious MF
operation conditions and wastewater properties. For example, in the membrane fouling and produced the MBR permeate with greater
MBR + NF system for municipal wastewater reclamation, the amounts of organic substances, accordingly, causing a higher RO
predominance of NF membrane fouling was inorganic scaling, fouling rate compared to the low F/M ratio (0.17 g/g day−1,
which could be alleviated by regulating the pH level of NF feed i.e., SRT at 45 days). In a recent study on NF-MBR + RO
water (Kappel et al., 2014). While, in another study focusing on process (Tay et al., 2020), the NF-MBR at a longer SRT
MBR + NF for antibiotic processing wastewater treatment, the (60 days) had greater accumulation of divalent salts in the
soluble organic substances (especially fulvic acid-like and humic bioreactors compared to that at a shorter SRT (30 days),
acid-like compounds) accumulated on the NF membrane leading to more severe inorganic fouling on the NF
determined the NF fouling potential (Li et al., 2016). Under these membrane. As both NF-MBRs displayed similar microbial
scenarios, more frequent membrane cleaning was therefore adopted viability and biodegradation efficiency in terms of organic
in order to maintain constant permeate productivity, which led to carbon and ammonia, comparable permeate qualities were
increased operation cost and capital cost (due to shortening NF achieved in both NF-MBRs. However, a higher RO fouling
membrane lifespan). However, the high recovery of reclaimed water rate was observed when the RO membrane was fed with the
brought considerable potential economic benefits, thus, the permeate produced by NF-MBR at a higher SRT, implying the
applicability and feasibility of various MBR + NF operation effect of organic composites (such as assimilable organic carbon)
configurations should be optimized with regards to both in the NF-MBR permeate on the RO performance. Notably, the
operation performance and overall economic benefits (Li conclusions relating to the influence of SRT on the consequent
et al., 2020a). NF/RO performance were not always in a consistent pattern in
these reported studies, possibly due to dissimilar wastewater and
2.2.3 Effect of MBR operation conditions membrane nature, reactor configuration, and operating
It has been well illustrated that (1) variable feed wastewater philosophy. Nevertheless, operational parameters of HRT and
characteristics and operation conditions in the MBRs could SRT should influence membrane fouling because they should be
influence on the membrane performance and permeate quality of involved critically for substrate utilization and cell growth.
MBRs (such as organics, nutrients, inorganics) (Wu and Fane, 2012; Additionally, the dissolved oxygen (DO) level in the MBRs has
Meng et al., 2017; Wu and Kim, 2020); (2) The feed water quality of also been reported to impact the subsequent NF/RO membrane
MBRs is a critical factor in determining organic fouling, scaling and performance. It was found that decreasing the DO level in a moving
biofouling of NF/RO membranes (Al-Amoudi and Lovitt, 2007; bed biofilm MBR from 4.0, to 2.5, and to 1.0 mg/L, the fouling rate of
Jiang et al., 2017; Matin et al., 2021). Not surprisingly, the MBR the RO membrane fed with the MBR permeate increased from 0.015,
operation conditions could have potential impact on the overall to 0.023, and to 0.055 bar/d (Wang et al., 2019). The biopolymers in
MBR + NF/RO performance. the MBR permeate was further identified to be correspondent with
As expected, several studies have revealed that a higher level the RO fouling potential, i.e., the MBR at a higher DO level produced
of organic substances in the MBR permeate reduced NF/RO the permeate with less amounts of biopolymers. Similarly, although
performance. For example, Reis et al. (2017) pointed out that a the aerobic MBR and AnMBR-zeolite column produced the
yeast-based MBR treating landfill leachate wastewater could permeate with comparable organic and nitrogen concentrations,
benefit producing the permeate with less organics compared the performance of the RO membrane fed with the aerobic MBR
to a conventional MBR. As a result, the permeate of the yeast- permeate was better than that with the AnMBR-zeolite column
based MBR + NF was superior than the conventional MBR + NF. effluent. It appears that the divalent ions released from the zeolite
Woo et al. (2016) found that the presence of activated carbon column could interact with phosphate to accelerate inorganic
(1 g/L) in the MBR could produce the permeate with less colloidal fouling on the RO membranes (Li et al., 2020b).
organics, allowing the subsequent NF membrane operated at Such observations highlighted that (1) besides organic amounts,
a higher flux compared to that without powdered activated the organic/inorganic compositions in the MBR permeate could
carbon (PAC). Meanwhile, better permeate quality was have a significant influence on the performance of following NF/RO
achieved in the PAC-MBR + NF. processes, which should be given more attention in future research;
Despite of this fact, the MBRs generally show excellent organic (2) during optimization of MBR + NF/RO for wastewater
removals from wastewater and produced superior permeate reclamation, the combined effects of the operation conditions of
quality. However, the detailed organic compositions (such as MBRs on both MBR and NF/RO performance need be carefully
hydrophobicity, aromaticity, biopolymer fraction, or evaluated in terms of membrane fouling control and
carboxylate/acid/base nature of the organics) in the MBR economic benefits.
osmotic pressure caused by concentration gradient through also water quality as well as microbial activities. Especially, the
membrane materials, an energy demand required for TMP to reverse salt transport may increase the amount of salt in bulk
operate the system is very low. As filtration progresses with time, suspension of MBRs, which would provide adverse effects on
however, the draw solution becomes diluted, so that both feed and microbial community and bacterial growth (Nawaz et al., 2013;
bulk solution in the MBR should be concentrated subsequently. The Nawaz et al., 2016). Subsequently, the salt concentration in the MBR
waste product concentrated by FO membrane is easy to be disposed increased by the FO membrane varies depending upon the growth
or reused downstream as useful energy and resource source. Since rate of biomass, particle size distribution and sludge filterability
the wastewater is transported from a feed side toward draw solution, (Nguyen et al., 2015; Adnan et al., 2019). Therefore, more studies are
it can be recovered for the production of high quality of permeate needed to understand effect of draw solution concentrated by FO
given that draw solution regeneration step is integrated, for example, membrane in bioreactor performance, such as microbial activities.
a double-barrier membrane (Holloway et al., 2014; Lutchmiah et al., Also, proper selection of draw solution should be suggested to
2014; Im et al., 2020). Nevertheless, the purity of the permeate confirm operational energy.
depends on the rejection features of FO membranes and the Like other membrane processes, the membrane fouling
separation effectiveness of permeate water from draw solution observed with FO membrane is a necessary phenomenon
strongly. Depending upon the characteristics of the effluent because biofouling can be formed particularly on the surface of
stream and the effectiveness of the entire treatment train, the FO membrane (Qin et al., 2010; Bao et al., 2019). In fact, the FO
extracted permeate can also be reused for various purposes such membrane can be fouled more easily than other types of high
as cooling, rinsing or even irrigation and drinking water. In pressure-driven membrane due to relatively lower crossflow
particular, this unique characteristics in FO membrane process is velocity on membrane surface. Furthermore, the fouling rate on
also beneficial for Zero Liquid Discharge (ZLD) waste disposal FO membrane can be severe as it is combined with bioreactor
system because it leaves much less water to be removed by because both organic/inorganic loadings increase gradually by FO
evaporators, so that energy demand can be further reduced filtration (Parida and Ng, 2013; Aftab et al., 2017). High organic
significantly. Here, the product water extracted by a FO loading can increase microbial by-products such as EPS while
membrane can be reused for other purposes such as process reducing sludge dewaterability (Aftab et al., 2015). A recent study
water for industrial manufactures (Im et al., 2018). The FO-MBR (Olives et al., 2023) on granular sludge based AnMBR proved that
shows acceptable permeate flux and superior removal efficiency of fouling occurred less frequently than MF. It was also confirmed
organic contaminants as well as other emerging contaminants that the change in salinity within the MBR caused the draw
without applying external pressure (Zhu and Li, 2013; Jang et al., solution’s reverse salt flux. The use of FO resulted in complete
2018; Sivodia and Sinha, 2023). Therefore, the FO-MBR should have and very high purity in effluent, but the presence of MF was
a great potential to replace the conventional MBR processes for necessary for the removal of salts. A method combining thermal
wastewater reclamation conditioning that sources suitable for draw osmotic backwashing and air scouring and osmotic backwashing
solution, i.e., seawater can be obtained easily nearby the MBR plants were evaluated as non-chemical methods to remove biological
(Arnaldos et al., 2023). contamination of FO-MBR (Satterfield et al., 2021). Considering
For the FO-MBR process, there are two functions designated by energy efficiency, optimization of backwashing period and
FO membranes such as wastewater concentration and water frequency was found to be the most economically efficient way
recovery or extraction (Wu et al., 2021). The wastewater to remove FO-MBR fouling.
concentrated by the FO process should be particularly helpful in
anaerobic MBR systems because it can retain anaerobes completely
in anaerobic bioreactor (Chen et al., 2014; Anjum et al., 2021). 3.3 Hybrid MD-MBR
Additionally, the FO membrane process has been employed for the
treatment of AnMBR effluents containing high nutrient loadings MD is the thermally driven hybrid membrane process. The
such as ammonia nitrogen as they are applied as post-treatment MD process could concentrate the non-volatile impurities in the
(Kwon et al., 2020). Although biodegradation and/or feed solution and transport volatile matters to the permeate
biotransformation is the main mechanism for trace organic solution though the hydrophobic pores of membranes. The
contaminants removal by both aerobic MBR (AeMBR) and schematic diagram of the MD process for wastewater treatment
AnMBR, the removal of some specific materials can be different is presented in Figure 1. Due to the relatively lower fouling
since the microbial community differs between the two (Liu et al., potential than that of pressurized-driven membrane process, the
2020). While there is no significant difference in permeate qualities MD process is combined with a bioreactor has been applied as
produced by desalination technologies with AnMBR, some portion main or side streams for various wastewater treatment and water
of methane produced can be dissolved in permeate particularly reuse (Julian et al., 2022; Kharraz et al., 2022), treatment of
AnMBR treats domestic sewage. In terms of water extraction, the FO industrial wastewaters (petrochemical (Santos et al., 2020), flue
membranes can be applied to separate the water from MBR effluents gas (Li et al., 2021), desulfurization (Zheng et al., 2022), coking
or directly from bioreactor. Nevertheless, the regeneration step for (Guo et al., 2022), textile (Elcik et al., 2021), seawater brine (Kim
the recovery of draw solution should be required, and this will be the et al., 2019) and radioactive (Jia et al., 2021)) as well as resource
bottleneck to be overcome for FO-MBR processes (Qiu et al., 2016; recovery (Julian et al., 2022; Kharraz et al., 2022). In the MD-MBR,
Song et al., 2020). the MD process could be used as final barrier in the water
The selection of draw solution acts as an important role in FO- treatment process because it allows the transports for the
MBR processes because it can determine not only permeate flux but volatile matters such as water. However, feed solution
FIGURE 1
Schematic diagram of the membrane distillation process during the wastewater treatment.
containing volatile impurities such as nitrogen (ammonia) fabricate a flat-sheet or hollow fiber type MD membranes,
sometimes required a pH control to regulate ammonia which have been used in various MD module configurations
transport through membrane (Tun et al., 2016; Lee et al., 2021b). such as direct contact membrane distillation (DCMD), air-gap
As mentioned, the main purpose of MBR process is to separate membrane distillation (AGMD), solar driven membrane
biomass and improve permeate quality by controlling HRT and distillation (SGMD), and vacuum membrane distillation (VMD)
SRT independently. When the MD process is combined with MBR (Tibi et al., 2020; Julian et al., 2022; Kharraz et al., 2022).
in municipal wastewater treatment, the deionized water could be Specifically, the aramid layer was suggested to be coated on the
produced by municipal wastewater (Tun et al., 2016; Song et al., PVDF membrane to enhance chemical resistances (e.g., harsh
2018; Lee et al., 2021a; Simoni et al., 2021; Dow et al., 2022). Like pH conditions) (Ji et al., 2021). Moreover, the MD membrane
pressure-driven membrane process, the MD membrane can be modified for anti-wetting (Madalosso et al., 2022), self-
experiences severe fouling caused by particulates (Choudhury cleaning efficiency (Yan et al., 2022), and photothermal property
et al., 2019), organic compounds (Guo et al., 2019; Elcik et al., (Lee et al., 2022) to achieve its high sustainability for hybrid MD-
2021; Jeong et al., 2021), inorganic compounds (Kim et al., 2019; MBR processes. Nevertheless, the techno-economic analysis
Kim et al., 2022), and microorganisms (Zheng et al., 2022). should be conducted for hybrid MD-MBRs to accelerate
Additionally, the fouling rate can be accelerated by the commercialization. Operational energy required for MD
membrane wetting (Choudhury et al., 2019; Kim et al., 2019; processes may be still high due to maintaining required
Madalosso et al., 2022) during long-term operation of MD temperature driving force, but if the renewable energy or waste
membrane. To improve the membrane permeability of MD heat is available from anaerobic bioreactor, for example, the energy
membrane or antifouling capability, the modified MD demand to operate the MD-MBRs can decrease significantly. As
membrane materials have been adopted (Günay et al., 2023). reported in a recent study of pilot-scale MD-MBR (treating 10 m3/
The performance of MD membrane could be enhanced by day wastewater) using single-solar power panel without and with
fabricating the membranes with proper membrane pore size the heat pump, the costs were expected to be 56.5 and 87.3 $/m3
and thickness to prevent membrane wetting or heat loss across produced water respectively, considering the gain output ratio
the membrane (Tibi et al., 2020; Julian et al., 2022; Kharraz et al., (GOR) of 0.5–0.8 (Choi et al., 2022). It has been well documented,
2022). It is reported that higher hydrophobicity and porosity of the for the multi-staged MD system, the water production cost was
MD membrane results in higher rejection with organic and from 6.1 to 7.4 $/m3 with reduction of GOR from 4.6 to 4.4 as the
inorganic species (Tibi et al., 2020; Julian et al., 2022; Kharraz number of stages increased from 8 to 16 (Dudchenko et al., 2021).
et al., 2022). The PVDF, polypropylene (PP), and Both evaporation efficiencies (48%-69%) and the GOR (2.0-3.4) of
polytetrafluoroethylene (PTFE) polymers have been used to the multi-stage MD system could be increased with increasing
wind speed (8-11 m/s). Moreover, waste heat can be produced by Author contributions
the wind turbine, which is available for energy source to operate
MD system (Memon et al., 2022). As a result, it is worthwhile to JK: Conceptualization, Funding acquisition, Writing–original
develop MD-MBR processes to simultaneously capture renewable draft, Writing–review and editing. BW: Writing–original draft,
energy and perform wastewater reclamation. Writing–review and editing. SaJ: Writing–original draft. SeJ:
Writing–original draft. MK: Resources, Writing–review and editing.
4 Conclusion
Funding
This review describes the state-of-art of the MBR integrated
with desalination technologies to improve effluent quality and The author(s) declare financial support was received for the
membrane performance as well as optimize it for wastewater reuse research, authorship, and/or publication of this article. This study
applications. Applications of RO, NF, FO and MD to improve was supported by National Research Foundation of Korea (NRF)
MBR based process for wastewater reclamation were reviewed grant funded by the Korean Government (Ministry of Science and
critically. Although NF/RO can provide high permeate quality, this ICT) (2022R1A4A3029607, 2022R1A2C2010993).
should be impacted by membrane materials strongly. Increasing
the ratio of water recovery in NF/RO process enhances
productivity of reclaimed water. However, membrane fouling is Conflict of interest
necessary phenomena and thus it needs to be controlled.
Recirculating NF/RO residual to bioreactor may provide adverse The authors declare that the research was conducted in the
effect on both MBR permeability and NF or RO permeability, so absence of any commercial or financial relationships that could be
that recovery ratio needs to be optimized. Both HRT and SRT are construed as a potential conflict of interest.
important operational parameters to determine both MBR The author(s) declared that they were an editorial board
performance and desalination performance. Nevertheless, the member of Frontiers, at the time of submission. This had no
effectiveness to desalination membrane varies strongly impact on the peer review process and the final decision.
depending upon wastewater characteristics, membrane materials
and reactor configurations. The FO membrane has a great
potential because it can reduce energy demand in hybrid MBR Publisher’s note
process significantly. However, increasing salt content in bulk
solution of MBR due to dilution of draw solution may reduce All claims expressed in this article are solely those of the authors
microbial activity. The use of MD membrane has great potential to and do not necessarily represent those of their affiliated
enhance the value of reclaimed water in hybrid MBR because it can organizations, or those of the publisher, the editors and the
use any potential waste heat source available. Nevertheless, the reviewers. Any product that may be evaluated in this article, or
long-term performance of MD membrane in bioreactor needs to claim that may be made by its manufacturer, is not guaranteed or
be evaluated. endorsed by the publisher.
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