Accepted Manuscript

Title: Membrane bioreactors and electrochemical processes

for treatment of wastewaters containing heavy metal ions,
organics, micropollutants and dyes: Recent developments

Authors: Adewale Giwa, Abdallah Dindi, Joanna Kujawa

PII: S0304-3894(18)30465-5
DOI: https://doi.org/10.1016/j.jhazmat.2018.06.025
Reference: HAZMAT 19462

To appear in: Journal of Hazardous Materials

Received date: 3-1-2018

Revised date: 10-6-2018
Accepted date: 11-6-2018

Please cite this article as: Giwa A, Dindi A, Kujawa J, Membrane bioreactors and
electrochemical processes for treatment of wastewaters containing heavy metal ions,
organics, micropollutants and dyes: Recent developments, Journal of Hazardous
Materials (2018), https://doi.org/10.1016/j.jhazmat.2018.06.025

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 Membrane bioreactors and electrochemical processes for treatment of wastewaters

containing heavy metal ions, organics, micropollutants and dyes: recent developments

Adewale Giwaa,*, Abdallah Dindib, Joanna Kujawac

a,b
Department of Chemical Engineering, Khalifa University of Science and Technology, Masdar

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Institute, P.O. Box 54224, Abu Dhabi, United Arab Emirates.

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c
Faculty of Chemistry, Nicolaus Copernicus University in Toruń, 7, Gagarina Street, 87-100

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Torun, Poland.

*agiwa@masdar.ac.ae.

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Highlights
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 Recent challenges in MBR and electrochemical processes are discussed.

 New configurations of MBR and electrochemical reactors are examined.
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 Removal of organics, heavy metal ions, micropollutants, and dyes are analyzed.
 Low-voltage electrically-enhanced MBRs address the drawbacks of standalone units.
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 Future prospects are discussed.

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Abstract
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Research and development activities on standalone systems of membrane bioreactors and

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electrochemical reactors for wastewater treatment have been intensified recently. However,

several challenges are still being faced during the operation of these reactors. The current

challenges associated with the operation of standalone MBR and electrochemical reactors

include: membrane fouling in MBR, set-backs from operational errors and conditions, energy

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consumption in electrochemical systems, high cost requirement, and the need for simplified

models. The advantage of this review is to present the most critical challenges and opportunities.

These challenges have necessitated the design of MBR derivatives such as anaerobic MBR

(AnMBR), osmotic MBR (OMBR), biofilm MBR (BF-MBR), membrane aerated biofilm reactor

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(MABR), and magnetically-enhanced systems. Likewise, electrochemical reactors with different

configurations such as parallel, cylindrical, rotating impeller-electrode, packed bed, and moving

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particle configurations have emerged. One of the most effective approaches towards reducing

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energy consumption and membrane fouling rate is the integration of MBR with low-voltage

electrochemical processes in an electrically-enhanced membrane bioreactor (eMBR).

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Meanwhile, research on eMBR modeling and sludge reuse is limited. Future trends should focus

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on novel/fresh concepts such as electrically-enhanced AnMBRs, electrically-enhanced OMBRs,
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and coupled systems with microbial fuel cells to further improve energy efficiency and effluent
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quality.
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Keywords: Membrane bioreactor; Electrochemical processes; Electrically-enhanced membrane

bioreactor; Membrane fouling; Energy consumption.

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1. Introduction
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Research on membrane bioreactors (MBRs) and electrochemical processes has surged recently

because these are two techniques that can be used to remove several pollutants from different

types of wastewater. However, both techniques still face some drawbacks and some of the recent

studies have been directed towards these drawbacks. MBRs are faced with high cost

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requirements resulting from membrane fouling, aeration, excess sludge management, and

removal of phosphorus and heavy metals. Firstly, membrane fouling in MBRs contributes to the

cost of membrane cleaning and replacement [1]. Critical compounds that contribute immensely

to membrane fouling in MBRs are soluble microbial products (SMP) or soluble extracellular

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polymeric substances (EPS) that are produced during the metabolism and lysis of the microbes in

the bioreactor [2]. One of the ways to mitigate this problem is a coupling with additional

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techniques e.g. multi-stage processes. Secondly, considerable levels of coarse aeration are

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required for membrane scouring in MBRs which affect the overall operating costs. Aeration

might contribute up to 35-50% of the overall operating cost in MBRs [3].

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Thirdly, huge amounts of sludge are ejected from some MBR systems as wastes [4]. The excess
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sludge production arising from biomass retention in MBRs leads to high costs of sludge handling
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and management. Sometimes, the cost of sludge management is even higher than the cost of
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aeration. Fourthly, adequate phosphorus removal in MBRs is not achieved by phosphorus

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accumulating organisms; hence there is need to incorporate enhanced phosphorus removal

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systems with MBRs [5]. Furthermore, process biokinetics can be inhibited by the presence or

accumulation of heavy metal ions [6].

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Electrochemical processes can be implemented for the efficient removal of hazardous

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compounds, such as soluble products and metal ions, from the wastewater. In addition, these

processes have significant influence on the destruction of microorganisms in treated effluents.

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Electrolysis gases that can be used to provide aeration for enhanced reaction kinetics are

generated from these processes [7]. Many electrochemical systems produce coalesced and dense

waste sludge that is more convenient to handle. However, the electrical energy consumption per

mass of pollutant removed during the process is a drawback, as electrochemical systems

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designed to remove medium to high strength wastewaters might consume a lot of electrical

energy [4]. Passivation and electrode corrosion over time also pose some constraints to

electrochemical processes. To mitigate the aforementioned drawbacks, the integration of

electrochemical reactors with MBR has been proposed in recent studies [4,8,9]. The coupled

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technologies have been demonstrated to facilitate the removal of SMP, curtail membrane fouling,

improve the physicochemical characteristics of sludge, and enhance the removal of phosphorus

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and heavy metal ions.

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In this paper, the recent advances in standalone systems of MBRs and electrochemical processes

are first discussed. From google scholar and ScienceDirect search results (Fig. 1), research and

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development activities on these technologies for wastewater treatment have been intensified
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recently. From the 17-year trends shown in Fig. 1, the annual number of research publications on
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MBRs and electrochemical processes has continued to increase.
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Fig. 1. Annual number of publications on wastewater treatment through MBR and

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electrochemical processes from 2000 to 2017.

The recent advances in wastewater treatment by MBR are aimed at: addressing the problem of

membrane fouling and operational error; evaluating the influence of operating conditions on

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MBR performance; assessing the influence of system design on energy consumption and cost;

and formulating models for process control and optimization. These advances are illustrated in

Fig. 2.

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Fig. 2 Recent focus areas in MBR research, based on current challenges.

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Membrane fouling remains a critical challenge in standalone MBR operations. Operating

conditions and membrane properties still determine the extent of membrane fouling to a large

extent. On the other hand, the recent studies on standalone electrochemical processes have been

directed towards energy requirement and electrode scaling; the impact of operating conditions;

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and modeling and simulations (Fig. 3). Electrical energy consumption remains a crucial factor

that influences the competitiveness of standalone electrochemical systems for wastewater

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treatment. Therefore, the recent studies aimed at evaluating the impact of operating conditions

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and electrode materials on the energy requirements of electrochemical processes are mainly

discussed in this review. The relevance of models for the prediction of standalone MBR and

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electrochemical system performance is also discussed in detail.

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The integration of MBR with electrochemical processes has shown comparative benefits. These
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benefits that are incorporated in the integrated technology, known as electrically enhanced
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membrane bioreactor (eMBR), are discussed. eMBR technology is fairly recent; therefore,
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eMBR appraisal is an important aspect of this review. Extensive information is shown in order to
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provide a comprehensive background on eMBR systems.

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2. Recent advances in standalone membrane bioreactors

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2.1 Fouling in standalone membrane bioreactors

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Recently, it has been shown that considerable adverse effects are contributed by operational error

and system failure to membrane performance in standalone MBRs [10]. These effects arise from

unwarranted loss of mixed liquor suspended solids (MLSS), unmonitored aeration decrease,

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membrane permeability loss arising from erratic cleaning, toxic components in unscreened

wastewater fed into MBR, and other operational deficiencies. However, in the absence of human

and equipment error, fouling has been considered as a major contributor to loss of performance

efficiency in MBRs [11]. Fouling increases the overall resistance of the filtration process. This

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increase in filtration resistance will ultimately lead to decline in the flow of permeate, increase in

transmembrane pressure (TMP), increase in the filtration energy required, and decrease in

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membrane life. Conventionally, membrane fouling in MBR systems can be classified into:

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biofouling, organic, colloidal and inorganic fouling. Biofouling is one of the most critical forms

of membrane fouling. Tsuneda et al. [12] described biofouling as the formation of gel layer on

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the membrane surface and the reduction of effective membrane pore diameter resulting from

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extracellular polymeric substances (EPS) secreted by microbial flocs. EPS are insoluble
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macromolecules consisting of carbohydrates, proteins, nucleic acids, and humic compounds
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polymerized by microorganisms [13]. The EPS (or bound EPS) matrix releases colloids into the

bulk solution, and these colloids have a major effect on fouling. These macromolecules prevent
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water recovery from the flocs.

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Fig. 3. Recent research areas on electrochemical processes for wastewater treatment, based on

current challenges.

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Meanwhile, the explanations from Liao et al. [14] indicated that soluble microbial products

(SMP), also secreted by microbial flocs, rather than insoluble macromolecules are the major

biofoulants. SMPs were illustrated by Tarnacki et al. [13] as consisting of large soluble

molecules produced by cell metabolism. Wisniewski and Grasmick [15] stated that the

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contributions of the soluble and particulate portions of mixed liquor to membrane fouling are

52% and 23%, respectively. Therefore, the biopolymers in SMPs (or soluble EPS) deposit more

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freely on the surface of the membrane than the larger-sized microbial flocs or suspended solids.

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Wisniewski et al. [16] also observed that the soluble fractions in the bulk solution enhance the

build-up of deposits on the membrane surface because they cause highly intensive physico-

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chemical interactions with the material of the membrane. These solutes enhance membrane pore

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clogging [17]. Other studies from Lesjean et al. [18] and Ng and Hermanowicz [19] also
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concluded that SMPs are the major contributors to membrane fouling in the MBRs. There is a
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positive correlation between soluble COD or in particular, the protein fraction in sludge

supernatant, and filtration resistance. Rojas et al. observed that there is no correlation between
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the particulate portion of sludge and filtration resistance, and concluded that sludge supernatant
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contributes more to membrane fouling [20]. This conclusion is also supported by the findings in
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a related study which confirmed that fouling is caused more by particles smaller than 5 μm [21].

Other critical types of fouling in MBR are inorganic and colloidal fouling [22]. In general, the
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tendency of a membrane to foul rapidly during MBR operation is dependent on the operating

conditions including sludge and feed water characteristics, and membrane properties.
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2.1.1 Influence of operating conditions

Operating conditions such as hydraulic retention time (HRT), sludge retention time (SRT), and

aeration intensity influence the propensity of MBR to undergo membrane fouling. A decrease in

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HRT for the same reactor volume might lead to an increase in volumetric loading and TMP. This

decrease in HRT will increase the MLSS and worsen membrane fouling [23]. MLSS

concentration, however, increases when SRT is increased for the same reactor volume, thereby

leading to high sludge viscosity and increased fouling [23]. Another operating condition that

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influences the possibility of early fouling of a membrane during MBR operation is the specific

aeration demand (SAD). SAD is a very important parameter because the scouring of the

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membrane reduces fouling and the air transfer to microorganisms ensures growth. Fan and Zhou

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[24] explored the interconnected influence of mixed liquor fractions and aeration intensity on

membrane fouling and concluded that membrane fouling was strongly related to aeration

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intensity. However, air requirement results in a high energy demand in the MBR operation. Four-

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fifth of the total energy cost in a submerged MBR could be due to aeration; thus, the selection of
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energy-efficient aeration intensity is necessary [25]. A dramatic drop in the overall fouling rates
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can result from an increase in aeration intensity but the breaking of flocs might arise if the air

flow into the MBR system is more than the required amount and this will lead to more fouling
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[26]. Therefore, the use of the optimum aeration rates, beyond which any further increase would
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have no impact on the suppression of membrane fouling, is crucial for process performance.
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Hwang et al. [27] recommended a range from 2 to 4 L/min for 5.6 g/L of sludge at 50 kPa of

pressure.
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The sludge characteristics which influence membrane fouling are: SMP, EPS, MLSS, sludge
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viscosity, floc size, dewaterability, and filterability. EPS can be categorized as bound EPS and

soluble EPS which could settle on the membrane surface. Laspidou and Rittman [28] reported

that soluble EPS are identical to SMP and are formed from the hydrolysis of bound EPS. Other

researchers such as Ramesh et al. [29] and Barker and Stuckey [30], however, concluded that

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SMP contains protein in the form of amides whereas soluble EPS do not. It was observed that

there are differences in the overall chemical compositions of soluble EPS and SMP.

Nevertheless, Cho et al. [31] observed that SMP could be assumed to be soluble EPS in the

quantification of microbial products. Many membranes for MBR process were produced as a

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hydrophilic material. Nevertheless, the hydrophilicity of the membranes is changed by the

adsorption of hydrophobic organics on the membranes. In the long run, the membranes might

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possess the same level of hydrophobicity as the organics present in the sludge suspension [32].

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Therefore, as the bound EPS and SMP concentrations in the mixed liquor increase, the fouling

tendency of the membrane increases.

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The total suspended solids (MLSS) have also been known to influence membrane fouling by
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increasing the thickness of the sludge dynamic layer around the membrane and sludge viscosity
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[23]. The hydrodynamic stress needed to propel sludge circulation increases as sludge viscosity
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increases, thereby resulting in more attachment of the sludge cake on the dynamic film than
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detachment. However, this pattern was discountenanced by another study [33], which indicated
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that the specific cake resistance of filtration might vary inversely with total suspended solids.

Chang and Kim [33] examined the influence of biosolids concentration (3700, 2900, 250 and 90
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mg/L) on cake resistance and observed that cake resistance reduced with MLSS concentration.

An opposite relationship between cake resistance and specific cake resistance was shown.
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Floc size represents the average size of sludge particles. Smaller particles have greater tendency
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to aggravate filtration resistance and reduce the flux of permeate. Small flocs have the ultimate

impact on cake resistance, as they blind the sludge cake during filtration. Cake moisture content

also increases as the mean size of flocs particles decreases. Larger particles deposition would, on

the other hand, result in the formation of more porous cake layers and less sludge volume. Larger

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floc sizes have a higher back transport velocity and drag forces, and as a result, these particles

migrate less to the membrane surface [34]. Sludge viscosity is the resistance of sludge to motion,

and it is an important factor for assessing the tendency of membranes in MBR to undergo

fouling. Sludge viscosity is related to sludge concentration, surface charge, degree of hydration,

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particle size, and flocs cohesion of agglomerated particles in suspension. Sludge viscosity is also

proportionally related to EPS and filamentous microorganisms in the sludge. The viscosity of

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sludge is increased as EPS are produced, leading to increased membrane fouling [35]. Sewage

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sludge shows non-Newtonian flow and has usually been demonstrated in the scientific literature

through the pseudoplastic rheological model. The pseudo-plastic characteristics mean that the

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system would behave like a solid whose viscosity decreases with the shear rate and varies with

sludge structural changes during the flow [8]. N

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Another sludge property which influences membrane fouling is sludge dewaterability. This
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property offers a quantitative degree of how sludge repels water, i.e. rate of water release from
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sludge. Sludge dewaterability is important to check the filterability and settling properties of
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sludge. Sludge settling tendency or settleability is commonly measured through the sludge

volume index (SVI). SVI values less than 120 mL/g are satisfactory; those over 150 mL/g can
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result in bulking. An increase in SVI due to the proliferation of filamentous bacteria can be

interpreted as a decrease in settleability leading to TMP increase and filtration instability [36].
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Filterability can be expressed in terms of indices such as membrane fouling index (MFI),
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combined fouling index, modified fouling index, or unified fouling index. MFI is estimated

according to the cake filtration mechanism that considers the association between filtration time

and flow volume at a constant TMP. However, MFI is no longer applicable to real operating

conditions because the pressure is never constant during these conditions due to cake

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compression. In addition, most real operating plants operate under constant flux and not under

constant TMP. The total resistance in real operations includes cake and fouling resistances, apart

from the intrinsic membrane resistance. Thus the modified and unified fouling indices are

preferred nowadays.

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The composition of influent wastewater and influent organic loading profile also influence

fouling in MBR. Gao et al. [37] examined the effects of wastewater characteristics on membrane

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fouling in a MBR by using four types of industrial wastewaters having different pollutant

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concentrations. The differences in wastewater were then correlated to the differences in the rate

of membrane filtration. It was observed that the colloidal and protein contents in the feed play a

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dominant role in controlling membrane fouling and are more important than the quantity of total
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suspended solids. A complete description of feed may be a viable tool for membrane fouling
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predictions in MBR.
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2.1.2 Impact of membrane characteristics and configurations

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Organic materials are used for the fabrication of most membranes in MBRs nowadays. The
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prominence of organic membranes is due to their relatively easy fabrication techniques [38].
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These materials consist of polymers such as polysulfone (PSF), polyethersulfone (PES),

polyvinylidene fluoride (PVDF), polyethylene (PE), polyamide (PA), among others. Inorganic
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membranes, on the other hand, are made from inorganic materials such as ceramics, glass zeolite,

metal oxides, among others [39]. High stabilities are associated with inorganic membranes, but

these membranes suffer from rapid surface poisoning and cracking. Membranes are also in

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different shapes and configurations, in accordance with conditions under which they will be

applied.

Research focus has also been directed towards other MBR derivatives such as anaerobic

membrane bioreactor (AnMBR), membrane aerated biofilm reactor (MABR), biofilm membrane

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bioreactor (BF-MBR), forward osmosis membrane bioreactor (FO-MBR), and magnetically-

enhanced MBR. Aerobic MBR is compared with its derivatives in Fig. 4, in terms of

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environmental impacts due to energy-related emissions and eutrophication. AnMBR combines

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anaerobic process with membrane technology and offers desirable advantages such as low sludge

production and energy production in the form of biogas, when compared with aerobic MBRs

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[40]. However, as in aerobic MBRs, a critical challenge faced in the operation of AnMBRs is
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membrane fouling. Biofilm-based and biofilm-assisted reactors such as BF-MBR, MABR, and
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the moving bed biofilm reactor (MBBR) have been shown to provide high volumetric reaction
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rate due to the high specific biomass concentration of biofilms (rather than activated sludge)
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exploited in these reactors [41,42]. The biofilms used in BF-MBR, such as granular media, are
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thick biofilms that might cause membrane clogging. In addition, the energy requirement of BF-

MBR is relatively high due to the aerobic conditions in the reactor. MABR is based on passive
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aeration, whereby air or oxygen is made to diffuse through the membrane to ensure energy-

efficient aeration and reduce membrane clogging [43]. However, like AnMBRs that offer low
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nutrient removal efficiencies, eutrophication of fresh water is one of the drawbacks of this
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technology. Osmotic membrane bioreactor (OMBR) or FO-MBR makes use of the osmotic

power of a high-salinity draw solution to recover fresh water from the mixed liquor. This

technology is capable of reducing energy consumption and cost at the draw dilution stage;

however, draw regeneration in a large scale is still a challenge [44].

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Fig. 4 Comparative analysis of MBR and its derivatives, in terms of emissions from energy
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consumption, eutrophication of fresh water resources, and eutrophication of marine environment.
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(adapted from [45]).

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Research activities on magnetically enhanced MBRs are limited. The use of these MBRs has

only been shown lately. Magnetically enhanced MBR can be configured either by incorporating
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magnetic nanoparticles in the membrane polymer dope during membrane synthesis or by adding
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these nanoparticles directly into the MBR mixed liquor. A nanocomposite ultrafiltration

membrane formed by blending up to 0.11 wt% Fe3O4 nanoparticles with PSf has been shown to
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reduce MBR filtration resistance by 27% and increase water flux by 30% due to the presence of

magnetic field around the MBR, when compared with a commercial membrane [46]. In another

study on magnetically enhanced MBR [47], the direct addition of Fe3O4 magnetic powder to the

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activated sludge in a MBR has been shown to reduce membrane fouling. Membrane cleaning

period was extended by 3 days due to the magnetic activation of the sludge.

Meanwhile, recent studies on OMBR surpass the studies on other MBR configurations. Recent

OMBR systems exist in the form of: submerged OMBR for aerobic wastewater treatment;

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submerged OMBR for aerobic wastewater concentration and seawater dilution; submerged

OMBR for biogas recovery under anaerobic condition; and side-stream and combined OMBRs

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under aerobic condition [48]. The integration of MBR or OMBR with reverse osmosis (RO) has

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been used to achieve high quality-effluent. Less membrane fouling is observed in OMBR-RO

because the osmotic process reduces the migration of foulants towards the membrane [49]. The

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RO stage is used to re-concentrate the draw solution diluted in the OMBR stage or post-treat the
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MBR permeate. Seawater desalination, seawater or brine dilution, and energy recovery can be
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achieved by MBR configurations integrated with RO. Recent MBR-RO and OMBR-RO systems
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for potable water production and energy recovery are shown in Fig. 5. Meanwhile, salinity build-
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up in the feed solution remains a problem in OMBR operations. This problem is caused by
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reverse salt diffusion from the draw side of the OMBR to the feed side, depending on the

membrane and the size of the particles in the draw solution. The integration of OMBR with MF
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and electrodialysis (ED) has been used recently to address the problem of salinity build-up [50].

The use of halophilic bacteria that can withstand high salinity in high-retention MBR (HR-MBR)
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has also been suggested for process optimization [51]. Some of the recent studies on OMBR and
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their findings are summarized in Table 1.

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 A (a)
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(e)
(c)

(d)
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(b)

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 Fig. 5 MBR-RO potable water production systems involving: draw solute re-concentration via

RO in OMBR-RO (a, b) [52]; post-treatment of MBR permeate via RO (c) [53] and then UV (d)

[54]; enhanced water recovery and reuse in seawater desalination via RO (e, left) or water

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desalination and energy recovery (e, right) [52].

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Table 1. Recent studies on OMBR and their findings.

Wastewater Pollutants System design Operating conditions Pollutant Other notable findings Ref.

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type removed and removal

configuration
N efficiency
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Activated Membrane OMBR-RO Lab and bench scale FO N/A A minimum flux of 15 [55]
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Sludge fouling study module LMH at 0.5M NaCl for

OMBR-RO is cost-
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effective, depending on
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the FO membrane price

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Domestic COD, UF-OMBR, 120 days operation, DS- COD-96%, TN FO water flux was [56]

wastewater TN, plate, and 32g/L NaCl -82%, P-99%, maintained constant for
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P frame FO more than four months

module, with the UF-OMBR

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Hollow fiber

UF module

Glucose- Organic MFC-OMBR DS-0.5 NaCl OM-95%, P - MFC coupled with [57]

based matter, 99% OMBR increased power

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synthetic Phosphorus production from 3 to 11

W/m3

Granular COD, N Anaerobic– SRT- 10, 30, 90 days, COD- >95%, SRT of 30 days gave [58]

sludge oxic 37 C NH3+-N-94%, better filtration

from a membrane TN-70.6% performance than SRTs

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Pilot-scale bioreactor of 10 and 90 days.

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aerobic (AOMBR)

MBR with HFM

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microporous

module

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Municipal Trace Pilot-scale SRT-63 to 68 days, DS- COD- 99%, Low nitrate rejection by [59]

wastewater Organic hybrid UF- 0.7M NaCl,

N TN-82%, P- FO CTA membrane
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Chemicals OMBR, UF 99%
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hollow-fiber

PVDF
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membrane
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module, FO

plate-and-
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frame cassette
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Pharmaceut Pharmaceutic OMBR 73 days operation, DS- >96% The major portion of total [60]

ical als 0.5 NaCl, SRT- 20 days, organic carbon (TOC)

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wastewater HRT- 33h that permeated the FO

membrane was low-

molecular weight neutral

compounds

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Synthetic – sCOD, VFA, Anaerobic 120 days operation, DS- sCOD-100%, Methane production of [61]

sCOD NH3-N, P OMBR- 0.5M NaCl, SRT of 90 P- 100% 0.25 - 0.3 L CH4/g sCOD

Membrane day; 35°C. digested was

area-250 cm2 obtained.

Synthetic EPS OMBR, DS-0.5M NaCl N/A Without air scouring at [62]

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municipal Reactor Vol – the feed side of the

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wastewater 4L membrane, flux at

22.4 atm osmotic pressure

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declined by 30%

Synthetic Membrane FOMBR - DS – 0.5M NaCl N/A 45% permeate flux [63]

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municipal fouling study submerged SRT - 10 days. decrease was observed in

wastewater hollow fiber HRT - 7 h

N the FOMBR
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FO membrane
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module

Synthetic Trace organic Lab scale DS-0.5 NaCl 99% for Both physical separation [64]
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Wastewater contaminants OMBR compounds and biodegradation

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>266 g/mol influenced removal of

compounds >266 g/mol

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MBR and its hybrid forms such as MBR-MBBR have also been shown to be viable for the

removal of micropollutants and dyes in recent investigations. The micropollutants were removed
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from raw and synthetic municipal wastewater, hospital wastewater or effluent, synthetic trace

organic wastewater, and leachate. High removal efficiencies (up to 80% or more) of hydrophobic

micropollutants such as nonylphenol, 17α-ethynylestradiol, 17β-estradiol, estrone, bisphenol A,

and triclosan were reported due to the tendency of these micropollutants to undergo hydrophobic
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interaction (or adsorption) with the activated sludge in MBR. Adsorption of hydrophobic

micropollutants to activated sludge improves the biodegradability of these pollutants. However,

some hydrophobic micropollutants containing electron withdrawing functional groups such as

chlorine atom (e.g. diclofenac) or amide group (e.g. carbamazepine) might show low removal

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efficiencies because these functional groups compete with bacteria for electrons, thus hindering

biodegradation. Low removal efficiencies of hydrophilic micropollutants such as diclofenac and

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sulfamethoxazole were reported. However, some hydrophilic compounds containing an electron

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donating functional groups such as amine group (e.g. atenolol) exhibited high removal

efficiencies. Some hydrophilic compounds such as ibuprofen and sulfamethoxazole might also

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be removed significantly from wastewater if MBR is operated under acidic conditions rather than

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neutral conditions. The conversion of these compounds from hydrophilic ionic forms to more
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hydrophobic forms can occur at pH lower than the pKa of these compounds. MBR-MBBR has
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been used to remove ketoprofen, carbamazepine, primidone, bisphenol A and estriol from

wastewater, with MBBR as the pretreatment technique to reduce SMP levels and membrane
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fouling tendency [65]. Dyes from textile wastewater have also been removed using MBR
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configurations. 30-100% dye removal in the form of COD and color have been reported in recent
EP

studies [66–77]. The performance of MBR for micropollutant and dye removal in terms of

removal percentages is shown in Fig. 6.

CC
A

22
(a)

100

80

PT
% removal

60

RI
40

SC
20

U
0

17β-estradiol

17α-ethynylestradiol
Ibuprofen

Sulfamethoxazole

Trimethoprim

Estriol

BisphenolA

Atrazine
Carbamazepine

Estrone

Atenolol
Diclofenac

Nonylphenol

Triclosan
N
A
M
D
TE

Synthetic bisphenol wastewater Hospital effluent

Synthetic trace organic wastewater Hospital wastewater
EP

Raw wastewater Synthetic municipal wastewater

Synthetic medium strength wastewater Municipal solid waste leachate
Raw sewage Landfill leachate
CC
A

23
 (b)
100 Feng et al. (2010)
Qin et al. (2012)
80
Removal efficiency

PT
Deowan et al. (2013)

60 Baêta et al. (2013)

RI
Keerthi et al. (2013)
40 Friha et al. (2015)

SC
Yurtsever et al. (2016)
20
Deveci et al. (2016)

U
0
COD N Color
A
M
Fig. 6 Removal efficiencies of micropollutants and dyes from recent MBR studies aimed at

removing (a) micropollutants from synthetic bisphenol wastewater [78], hospital effluent [79],
D

synthetic trace organic wastewater [80], hospital wastewater [81], raw wastewater [82] or sewage
TE

[83], synthetic municipal wastewater [84], synthetic medium strength wastewater [85], municipal

solid waste leachate [86] or landfill leachate [87]; (b) COD and color from textile dye
EP

wastewater, as reported in recent studies [66–77].

CC
A

2.2 Modeling Approaches for standalone membrane bioreactors

Various factors relating to model performance such as model definition, model selection and

objective, influent and biomass characterization, model parameter calibration, and model

validation are crucial components of a MBR model for wastewater treatment [88]. After

24
 modeling, computer simulation is important to explain some of the complex interactions of the

processes in MBR because the overall number of reactions and microbial species which are

involved in each treatment process may be huge. Specifically, the integrated models of biological

degradation and membrane filtration in the MBR are useful for the prediction of the influent

PT
load; estimation of biomass activities, effluent water quality, and membrane fouling parameters;

and prediction of operating constraints in hybrid systems such as salt accumulation in OMBR.

RI
The Activated Sludge Models (ASMs) developed by International Water Association (IWA) task

SC
group are still being used. Recent MBR modeling studies have been directed towards MBR

performance, salt accumulation in OMBR, fouling mechanisms and biocake layer morphology,

U
interfacial interactions and bioreactor geometry, as shown in Table 2. Gao et al. [89] attempted to

N
predict the effects of dissolved oxygen (DO) on the behavior of biological nutrient removal
A
organisms using ASM2d model. Unsteady state predictions of COD, nitrogen and phosphorus
M

concentrations were carried out using a dynamic model. It was observed that biological

phosphorus and nitrogen removal took place only when DO was above 1.5 mg/l. The calibration
D

of process parameters using experimental data was also carried out.

TE
EP

Table 2 Findings in recent models for the prediction of MBR performance.

CC

Model Model design Model

Model focus Other notable findings Ref.
approach parameters accuracy
A

Biocake Fractal Fractal Fractal dimension is found as the

layer Geometry dimension, <5% error predominant factor governing the [90]

morphology Weierstrass- particle size surface roughness biocake.

25
 Mandelbrot distribution

function

Tank width; Use of baffles in the MBR increased

Bioreactor Volumes of the

CFD 1.4% error [91]

PT
geometry riser and down average membrane surface shear by

comer 74% compared to an unbaffled one,

RI
Cake filtration,
The combined models usually

SC
Classical pore blocking,
Fouling achieved better fits of the
fouling and pore size N/A [92]

U
mechanism experimental data
models reduction

parameters N than the basic fouling models

A
Electron donor surface tension
M
XDLVO,
Interfacial Surface tension parameter was found to be a reliable
Simpsons N/A [93]
interactions parameters indicator for membrane fouling
D

method
prediction
TE

Surface Acid-base
EP

element (AB), Vander

integration Waals (LW)

CC

The interfacial interactions between

Interfacial (SEI), and
< 3% the modeled rough floc surface and [94]
Interactions differential electrostatic
A

membrane surface can be quantified

geometry, double layer

composite (EL)

Simpson’s interactions

26
 rule, XDLVO

PT
The ANN had

two layers

RI
The ANN model can easily be used
including 17
MBR to predict COD concentration and

SC
ANN and 2 neurons 99.99% [95]
performance TMP in the effluent.
in the hidden

U
layer and output

layer
N
A
Classical
M

Temperature was the variable

fouling Temperature,
Membrane having the main positive effect on
D

models, pressure, cross 65-99% [96]

fouling flux stability by decreasing the
TE

2k factorial flow velocity

solution viscosity
design
EP

Fractal Fractal

Membrane geometry and dimension, cut The reconstructed membrane

CC

10.8%
surface Weierstrass- off frequency, surface can be potentially used for [97]
error
morphology Mandelbrot fractal interaction energy evaluation
A

function roughness

27
OMBR Internal Membrane 68–77% Modeled FO water flux and RO

performance concentration properties, energy consumption ranges from

polarization draw solution 3.03 to 13.76 LMH and 0.35 to 1.39 [98]

theory, mass conc., kWh/m3

PT
balances HRT and SRT

Flow rate, ratio

RI
of membrane
The results showed that, increase in

SC
porosity to
flow rate, membrane length, the
tortuosity,

U
ratio ofmembrane porosity to the
Phenol membrane 9 - 15%

removal
CFD
length, initial error N tortuosity, and inner radius of the [99]
A
membrane resulted in the
phenol
M
improvement in phenol removal
concentration,
efficiency
number of
D

fibers
TE

Salt Internal Membrane 80–92% Tremendous water flux decline (10

EP

accumulatio concentration properties, to 0.82 LMH) and SRT (5 days) due

n polarization draw solution to salt accumulation and DS dilution [100]

CC

theory, mass conc., when OMBR is scaled up

balances HRT, and SRT

A

Weierstrass- Higher fractal dimension induced a

Sludge floc Fractal
Mandelbrot N/A more compact and smoother surface [101]
morphology dimension
(WM) morphology

28
 function, and

Fractal

geometry

*N/A means not available.

PT
RI
3. Recent advances in standalone electrochemical reactors

SC
3.1 Electric energy requirement of standalone electrochemical systems

U
Electrochemical processes provide a nexus between electric current and the chemical energy in
N
wastewater. These processes are accompanied by electron transfer ensured by the passage of
A
electric current between electrodes and wastewater. The electrochemical processes that have
M

been employed in wastewater treatment include electrochemical oxidation, electrochemical

D

reduction, electrodeposition, electrocoagulation, electroflotation, electrodialysis, electroosmosis

TE

and electrochemical advanced oxidation processes such as electro-Fenton, photoelectron-Fenton,

sonoelectrocatalysis, etc [102,103]. Two or more of these processes can also occur
EP

simultaneously in an electrochemical reactor. Recently, electrochemical processes have been

used for the treatment of groundwater, municipal, domestic, textile, tannery and leather industry,
CC

metal plating, chrome tanning, paper mill, restaurant, abattoir, semiconductor, shale gas,

hydraulic fracturing, lubricant, coal acid drainage and biodiesel production wastewaters [104–
A

115].

Of all electrochemical processes, the electrocoagulation process is one of the most frequently

studied electrochemical methods. It has been used effectively over the years for the treatment of

29
all kinds of wastewater. Electrocoagulation of contaminants in wastewater involves the use of a

direct current (DC) voltage applied to electrodes, usually made of iron or aluminum to produce

coagulants [116]. Recently, alternating current has also been employed for electrocoagulation

[117]. The current passes through a metal anode and oxidizes the metal (M) to its cation (M+). In

PT
the case of aluminum anode, Al3+ cation is released from the oxidation of the sacrificial

aluminum anode into the wastewater. The dissolved aluminum ions form hydrated ions within

RI
the wastewater suspension. These hydroxides form compounds with phosphates and other

SC
impurities. The compounds formed can then be easily removed by coagulation. A part of the

aluminum ions released by the anode also moves to the cathode with other hydrated cations in

U
the wastewater and are deposited on the cathode.

N
Electrocoagulation occurs when the positively charged hydroxide flocs become attracted to the
A
negatively charged pollutant species in the wastewater (and vice versa for the negatively charged
M

hydrated flocs), resulting in a decrease in the electrostatic forces of repulsion between these
D

species in the wastewater. The van der Waal’s force of attraction that occurs between the
TE

hydrated flocs and pollutants leads to the compression of the diffuse double layer nearby the

charged ions [118]. The passage of current through the anode might also lead to the electrolysis
EP

of water; hydrogen gas is generated at the cathode due to the movement of hydrogen ions

towards it.
CC

A critical application of electrocoagulation in wastewater treatment is colloids removal. Colloids

A

are solids that could not be totally dissolved or could not be settled due to their Brownian

motion. As a result, they cause high water turbidity and contribute adversely to membrane

filtration. In recent studies, colloids have been removed from the bulk suspension by

destabilization through electrocoagulation [107,119]. Colloids have like electrical charge that

30
yields a repulsion force between colloidal particles. If the charge was high, the particles would

remain discrete and in suspension. Therefore, the reduction of the repulsion force would help

those colloids to agglomerate and settle out of suspension [120]. The electro-coagulants have

high adsorption properties that enable them to form aggregates with colloids. The aggregates can

PT
then be further oxidized to less toxic compounds. Once the highly charged aluminum hydroxide

coagulants are formed in the suspension, the complexes of polyvalent oxyhydroxides that are

RI
produced would lead to the destabilization of the colloidal particles in the suspension. The

SC
quantity of cations released into the mixed liquor from the anode is determined by the current

density (CD). CD is the current per unit area of the electrode.

U
To comprehend the performance of colloids in suspensions during electrocoagulation, an
N
overview of Stern layer, double layer, diffuse layer, and zeta potential is crucial. Positive ions
A
(counterions) in the suspension would attract the negative colloids, forming an attached layer
M

around the surface of the colloid known as Stern layer. Additional positive ions that are attracted
D

by the negative colloids would, however, be repelled by the Stern layer and other positive ions in
TE

the vicinity of the Stern layer. Similarly, repulsive force occurs between the negative colloidal

particles (co-ions) near the surface of the Stern layer but their concentration increases with time
EP

until equilibrium is accomplished. A dynamic equilibrium would occur, resulting in the

formation of a diffuse layer of counterions. The diffuse layer could be defined as a charged
CC

environment around the colloid. These counterions would have a high concentration near the
A

Stern layer, but the concentration decreases with time until equilibrium is attained with the

concentration of the counterions in the solution [121]. The Stern layer and the charged

atmosphere in the diffuse layer form the double layer. The thickness of this layer can change,

depending on the nature of ions in the suspension and their concentration.

31
An indicator of this thickness is the surface potential, which is the potential between any point in

the mass of the suspension and surface of the colloid, indicating the strength of the electrical

force between the particles in the suspension. Surface potential drops linearly in the Stern layer

and then exponentially in the diffuse layer, approaching zero at the boundary of the double layer

PT
[122]. Although zeta potential is often used to represent surface potential in electrocoagulation

studies, both are not the same; zeta potential is the potential difference between the shear or

RI
slipping plane and bulk solution where relative motion occurs between them. Zeta potential can

SC
only be used to quantify the size of the electric charges at the double layer and it does not give

the same measurement as the surface or stern potential. However, the extent of coagulation of

U
colloids can be evaluated using the zeta potential. A high zeta potential denotes that colloids

N
would stabilize and resist aggregation. The attraction would exceed repulsion and the dispersion
A
would break and flocculate when the zeta potential is low. Colloids with high magnitude of zeta
M

potential are electrically stabilized while colloids with the low magnitude of zeta potentials tend

to coagulate or flocculate. So, zeta potential depends on the concentration and charge of colloidal
D

particles in the wastewater.

TE

Electrocoagulation has also been proved to be more efficient than chemical coagulation for the
EP

removal of several pollutants from municipal and industrial wastewaters [123,124]. However,

chemical coagulation has been reported as cheaper than electrocoagulation in recent studies
CC

[125]. Impressive removal rates of heavy metal ions, colloids, soluble organic and inorganic
A

pollutants by electrocoagulation were reported in these studies. Al-Shannag et al. [107] used

carbon steel electrodes to remove Cu2+, Ni2+, Zn2+, and Cr3+ via electrocoagulation from metal

plating wastewater. More than 97% of these heavy metal ions were removed at electrical energy

consumption of about 6.25 kWh/m3. Electrocoagulation has been employed by Guvenc et al.

32
[105] for the removal of COD, phenol, and Ca2+ from paper mill industry wastewater. Economic

and statistical tools were used to evaluate the operating costs and interaction between the

operating variables. An operating cost of 6.44 €/m3 was reported for the electrocoagulation

treatment, depending on the nature of the electrodes. Bazrafshan et al. [109] employed

PT
electrocoagulation to remove 93.1% COD and 98.6% dye from real textile wastewater. The

influence of operating factors such as applied electrical potential and reaction time on the

RI
performance of treatment system was studied. In another study on pollutants removal from

SC
textile wastewater [110], electrocoagulation was used as the first stage of an integrated system to

partially remove dissolved organic carbon (DOC) and COD. The optimal operating conditions

U
were also assessed. Gerek et al. [111] used electrocoagulation with aluminum electrodes to

N
reduce the COD concentration of leather industry wastewater from 1,024 to 180.7 mg/L at
A
specific energy consumption of 8.3 kWh/m3. The possibility of utilizing renewable energy was
M

also analyzed.
D

Electroflotation is another electrochemical process that has been employed in many recent
TE

studies for wastewater treatment. Electrofloation is a process that floats ions or solid particles,

suspended or dissolved in an electrochemical reactor by gas injection or via the gas bubbles
EP

formed by the electrolysis of water in the reactor [4]. Meanwhile, if electrocoagulation process is

desired in an electrochemical reactor, the hydrogen gas produced at the cathode would prevent
CC

floc settling due to the buoyancy force of the gas. Therefore, a combined electrocoagulation-
A

electroflotation process has also been devised recently. This combined process involves an

electrocoagulation process followed by electroflotation, such that the flocs displaced at the

surface of the treated effluent during electrocoagulation can be removed further via flotation

[126]. Aluminum anode and stainless steel cathode were used by Aoudj et al. [108] to remove

33
 fluoride and turbidity from synthetic semiconductor wastewater via electrocoagulation–flotation

process. Up to 90% and 85% removal of fluoride and turbidity, respectively was reported. These

removal efficiencies correspond to effluent concentrations of 4.61 mg/L fluoride and turbidity of

3.09 NTU.

PT
Electroosmosis process has also been studied recently to improve water recovery. This process is

enhanced by the formation of an electric double layer and ensures dewaterability [116,122].

RI
Water molecules are repelled by the ions released from the anode due to the migration of these

SC
ions, leading to the transport of water out of the particles in the reactor. Notable findings reported

in recent studies on the treatment of wastewater by electrochemical processes are summarized in

U
Table 3.
N
A
M

Table 3 Notable findings reported in recent studies on the treatment of wastewater by

electrochemical processes.
D
TE

Electrochemic Wastewater System design and Operating Pollutant removal Electrode Ref.

al Process type configuration conditions efficiency materials

EP

Gentamicin

Anodic and Cylindrical flow 2–5 A/dm2, 85.5% COD at Ti/RuO2

CC

[127]
oxidation dexamethason reactor 10–40 L/h control conditions anode

e wastewater
A

100-450 mA, Up to complete Boron-

Anodic Paracetamol Cylindrical cell with
25-45 ⁰C, 3 removal of doped [128]
oxidation wastewater electrode sheets
cm2 electrode paracetamol diamond

34
 area (BDD) and

graphite

AC-powered Parallel electrodes , 1.2 V, 0-5 A,

Oil and gas 99% suspended
electrocoagula AC power, electrode 3.33 mH, Al [117]
wastewater solids
tion area 56.32 cm2

PT
Anodic Integrated anodic
20 V, 10 A,

RI
oxidation and Textile oxidation/Electrocoag 48.6% COD,
CD: 79 A/m2, Fe [129]
electrocoagula wastewater ulation; cylindrical 80% dye

SC
pH 6, 700 cm2
tion anode and cathode

0.31 V/cm

U
electric field
N
intensity, 7.5
A
Anodic Carbon membrane
Oily r/min pump 92% oil and 70 % Carbon/titan
oxidation and anode and cylindrical [130]
M

wastewater rotate speed, COD ium

electroosmosis titanium cathode
and 5 g/L
D

electrolyte
TE

concentration

Coupled
EP

Bioelectroche Oil Refinery electrocoagulation 6.5 V, 0.1 M 98% COD,

Al [131]
CC

mical process wastewater fixed film biological NaCl 95% Petroleum HC

processes
A

Turbidity 3.3%,
Electrocoagul Textile Parallel plate 50 mA/cm2,
COD 99.7% and Cr Al and Fe [132]
ation wastewater electrodes pH 7, 25 mins
82%

Electrocoagul Metalworking Parallel plate Al (pH: 5, 80 Al (93% COD 80% Al and Fe [125]

35
 ation fluid electrodes A/m2, TOC)

wastewater 25 min) Fe (93% COD and

Fe (pH: 7, 80 82% TOC)

A/m2, 25 min),

143 cm2

PT
EC - COD: 34%,

RI
Phenol: 92.32%,
Paper mill Parallel electrodes, pH: 2 or 9; 96
Electrocoagul Ca2+: 32.6%

SC
2
industry 1000 ppm NaOH mA/cm , 184 Fe [105]
ation EF - COD:74.31%,
wastewater Solution cm2,
phenol: 99.99%

U
Ca2+: 61.18%
N Fe/Al
A
Electrocoagul Synthetic dye Fe/Al gel anode, 20 mA/ cm2, 85% COD, 99%
composite [133]
ation wastewater Titanium cathode 15 V ARS
M

hydrogel

Rushton type impeller 20 mA/cm2,

D

Electrocoagul Chromium (RT) pH: 2.4,

TE

100% Cr Fe [134]
ation wastewater electrocoagulation 0.05 M NaCl

reactor electrolyte
EP

Electrocoagul Plastic factory Parallel plate 15 mA/cm, 70% DBP, 90%

Al [135]
CC

ation wastewater electrodes pH 8-9 COD

Electrocoagul 37.5 mA/cm2,

Perfluorooctan 99% of
A

ation- Parallel plate pH: 3.77,

oic acid perfluorooctanoic Al or Fe [126]
electroflotatio electrodes mixing speed:
wastewater acid
n 180 rpm

36
Over the years, electrochemical processes have also been found to be useful for the removal of

various types of dyes and emerging pollutants from wastewater. Acid dyes, basic dyes, reactive

dyes, disperse dyes, azo dyes, and sulfur dyes have all been removed via electrochemical

processes. Meanwhile, pollutant removal efficiencies depend on operating conditions. Therefore,

PT
electrochemical techniques have been combined with other advanced oxidation processes

(AOPs) in many recent studies in order to achieve efficient treatment. Electrochemical AOP

RI
techniques such as anodic oxidation, electro-Fenton, photoelectro-Fenton, solar photoelectro-

SC
Fenton, peroxi-electrocoagulation, and sono-electrochemical oxidation have been employed

[136].

U
Anodic oxidation is one of the most popular electrochemical AOP, whereby the anode ensures
N
the direct or indirect oxidation of organic pollutants on its surface [136]. Direct oxidation is
A
ensured by direct electron transfer to the surface of the anode while indirect oxidation is ensured
M

by reactive oxygen species including •OH radical generated from the oxidation of water.
D

Oxidizing agents such as O3, H2O2, active chlorine species, and persulfates that are
TE

electrochemically generated from the bulk suspension might also enhance the advanced

oxidation of pollutants at the anode [137]. H2O2 can be generated from the reduction of oxygen
EP

gas at the cathode through electroperoxidation [138]. Since pollutants need to migrate to the

anode for anodic oxidation to take place, the efficiency of this method is highly dependent on the
CC

anode material and kinetics of pollutant mass transfer to the anode. Active electrodes such as
A

platinum, RuO2, IrO2, and carbon-based electrodes exhibit low potentials for O2 evolution (< 1.8

V/standard hydrogen electrode) whereas non-active anode materials such as BDD, SnO2, and

PbO2 exhibit higher O2 overpotentials [137].

37
The most recent studies on this method involve the application of anodic oxidation for the

removal of organic and emerging contaminants such as aspirin, salicylic acid, caffeine, p-

chlorobenzoic acid, chlorate and perchlorate species from water. He et al. [139] carried out the

anodic oxidation of aspirin by testing the efficiency of PbO2, flat BDD, and porous Ti/BDD as

PT
anodes. Ti/BDD anode ensured the complete mineralization of aspirin and provided the highest

pseudo first-order rate constant of 0.367/h. The rate constants provided by other anodes are 0.051

RI
and 0.185/h for PbO2 and flat BDD, respectively. BDD anodes ensured direct and indirect anodic

SC
oxidation of aspirin whereas PbO2 anode ensured indirect oxidation only. The degradation of

salicylic acid and caffeine have been reported in a recent study by Arfanis et al. [140] using

U
electrochemically-prepared titania nanotubes. Open porous anatase titanium nanotube films were

N
prepared by the electrochemical anodization of titanium metal. To prepare the nanotube films,
A
titanium foils were employed as the anode in a Teflon cell while platinum mesh was used as the
M

counter electrode. The nanotubular films were applicable under both acidic and alkaline

conditions, unlike the reference P25 film that showed deterioration. Garcia-Segura et al. [141]
D

employed anodic oxidation to remove 29 target pharmaceuticals and pesticides from the
TE

secondary effluent of a municipal wastewater treatment plant. This effluent was spiked with the
EP

pharmaceuticals and pesticides, including acetaminophen, enrofloxacin, gemfibrozil,

hydrochlorothiazide, ibuprofen, ranitidine hydrochloride, sulfadiazine, tramadol hydrochloride,

CC

venlafaxine, caffeine, carbamazepine, N,N-diethyl-meta-toluamide, diclofenac, trimethoprim,

etc. to a final concentration of 100 µg/L. BDD anode was employed to achieve complete
A

mineralization of these contaminants. Complete removal of DOC was achieved at 196 A/m2 and

pH 3.0 after 6 h of anodic oxidation. The specific energy consumption of the anodic

38
compartment was 1.92 kWh/m3. BDD anode has also been used in another recent study for the

anodic oxidation of p-chlorobenzoic acid [142].

Since H2O2 is a moderately strong oxidant, it requires the presence of Fe2+ in order to sufficiently

generate •OH through the electro-Fenton process. This process involves: the generation of H2O2

PT
in the presence of O2 gas at the cathode, the electrodissolution of Fe2+ from the anode, the

cathodic reduction of H2O2 to •OH radical by Fe2+, and then the attack of organic pollutants by

RI
the •OH radical. Fe3+ hydroxyl complexes that aid coagulation might be formed in the bulk

SC
suspension and Fe2+ is regenerated at the cathode, depending on the amount of H2O2

electrogenerated. Recent advances in electro-Fenton process for wastewater treatment include

U
the degradation of ionic liquids, fungicide, sweeteners, and 5-fluorouracil drug. Poza-Nogueiras
N
et al. [143] carried out the degradation of complex imidazolinium-based (1,3-Bis(2,4,6-
A
trimethylphenyl) imidazolinium chloride) ionic liquids family by using iron alginate spheres as
M

catalyst in an electro-Fenton process. 77% removal of TOC was achieved after 2 h of treatment.
D

Electro-Fenton process was also employed by Zazou et al. [144] to remove imazalil fungicide, a
TE

persistent organic pollutant, from water. Almost complete (97%) mineralization of aqueous

solutions having initial imazalil concentration of 0.1 mM (or 17 mg/L TOC) was achieved after 4
EP

h using BDD anode. BDD anode ensured the generation of •OH radical that degraded the

carboxylic acids formed during the mineralization of the imazalil. Lin et al. [145] employed the
CC

electro-Fenton process to quickly degrade artificial sweeteners (aspartame, saccharin, and

A

sucralose) in aqueous solutions. Using BDD as the anode, carbon-felt as the cathode, applied

current of 200 mA, initial pH of 3.0, and initial total concentration of 0.2 mM, all artificial

sweeteners were completely mineralized after 6 h. Short-chain carboxylic acids and inorganic

acids, which were generated during the mineralization of the artificial sweeteners, could be

39
completely removed at longer electrochemical treatment time. The electro-Fenton process was

also used recently by Ganzenko et al. [146] to remove a cytotoxic drug, 5-fluorouracil, from

water using BDD anode and carbon felt cathode. Almost complete mineralization (>94% TOC

removal) was achieved at 1,500 mA after 6 h of operation. Short-chain carboxylic acids were

PT
formed and destroyed during the mineralization process.

In order to accelerate the reduction of the Fe3+ hydroxyl complexes formed during electro-Fenton

RI
process to Fe2+ and consequent production of •OH, the photoelectro-Fenton process incorporates

SC
UV or visible light irradiation with the electro-Fenton process under acidic pH conditions. Direct

photolysis of pollutants can occur when the radiation is emitted at the range of wavelength

U
necessary for efficient absorption by the pollutants. Recent applications of the photoelectro-
N
Fenton process include the removal of Nafcillin, diatrizoic acid, and chloramphenicol. Almost
A
complete removal of Nafcillin from aqueous suspensions with initial concentration up to 100
M

mg/L has been achieved after 90 min of electrolysis using the photoelectro-Fenton process [147].
D

BDD anode and carbon-PTFE air diffusion were used. With a current density of 2 mA/cm2 and
TE

pH 2.8, organic intermediates such as inorganic ions and carboxylic acids were formed in the

suspensions. These intermediates were completely destroyed after 24 h by integrating the process
EP

with an anaerobic biological process. In another recent study that employed BDD anode for

photoelectro-Fenton degradation, complete mineralization of diatrizoic acid from 0.1 mM

CC

aqueous solutions was achieved within only 2 h [148].

A

However, a major drawback of the photoelectro-Fenton process is that high cost is required for

irradiation. The cost requirement can be reduced by the application of the solar photoelectro-

Fenton process, whereby natural sunlight is employed to provide free irradiation. This irradiation

can also produce other radicals such as SO4•− and Cl•, if their precursors are present in the

40
suspension. With a BDD and an air-diffusion cathode, complete mineralization of the antibiotic

chloramphenicol has been reported in a recent study that employed the solar photoelectro-Fenton

process [149]. The decay of chloramphenicol followed pseudo first-order kinetics. Solar

photoelectro-Fenton process has also been employed by Garza-Campos et al. [150] to degrade

PT
salicylic acid using a platinum anode. Up to 87% mineralization was achieved.

RI
3.2 Influence of operating conditions on electrochemical processes

SC
The efficiency of an electrochemical process for a specific application would still depend on

U
certain operating factors such as time of exposure of the treatment system to electric current,
N
applied CD, wastewater conductivity, anode material, and pH. Exposure time is the wastewater
A
residence time, which is the ratio of the reactor volume to the influent flow rate. For intermittent
M

current supply, exposure time also depends on the fraction of the total process time during which

electric current is supplied to the process. The distance between the electrodes in the reactor also
D

determines the exposure time. CD is the applied current per effective surface area of the anode.
TE

CD determines how much anodic ions are released into the solution. The larger the CD is, the
EP

smaller the reactor that can be designed for the same current. Short exposure times and CD might

reduce the removal efficiency of an electrochemical process.

CC

On the other hand, excessive exposure times and CD beyond the required levels might increase
A

sludge production and cost, without corresponding increase in removal efficiency [151].

Excessive CD worsens the possibility of wasting energy in heating up the water. A decrease in

phosphorus removal, in particular, will occur at excessive CD because the size of the gas bubbles

released during electrocoagulation would increase at high CD, allowing more phosphorus to be

41
attached to the gas bubbles. This would reduce the collisions between phosphorus compounds

and the discharged anodic ions. Lower rates of removal could also be due to the decrease in

microbial activity at high electrical pulse because some microorganisms might die in the sludge

suspension. Moreover, an unnecessary increase in the fixed suspended solids fraction and

PT
viscosity of the mixed liquor could occur at unwarranted CD. CD also affects the rates of

electrode scaling and cleaning, by influencing the charge potential in the mixed liquor around the

RI
electrodes.

SC
Water conductivity or ionic strength of wastewater is still of crucial concern to the performance

of electrochemical systems. The applicable electric potential at a particular CD decreases with

U
increasing wastewater conductivity. Therefore, wastewater conductivity influences the electric
N
power requirements of an electrochemical system. Sodium chloride (NaCl) has been used to
A
enhance the conductivity of the wastewater and improve the transport of electric charge in the
M

mixed liquor [152]. Anode material also determines the rate of the release of anodic ions into the
D

suspension. Several studies have been carried out recently to investigate the dependence of
TE

electrochemical processes on the anode material. The efficiency of an anode material depends on

the wastewater type and operating conditions. Ndjomgoue-Yossa et al. [153] observed that
EP

electrocoagulation was highly enhanced at ordinary steel electrode surfaces in comparison to

aluminum and carbon graphite for the removal of bacteria from wastewater. For the removal of
CC

COD and turbidity from car wash wastewater, it has been observed that aluminum provides
A

higher removal efficiencies than iron [154]. However, iron has been presented a better anode

material for the removal of Cr(VI), when it is compared with aluminum [155]. Iron has also been

shown to exhibit better performance than aluminum for the removal of turbidity from urban

wastewater. Other electrode materials that have been used in recent studies include monopolar

42
and bipolar forms of stainless steel, boron doped diamond, aluminum/copper/magnesium alloy,

granular and powdered activated carbon, stainless steel coated with single-walled carbon

nanotubes, Al/Fe-impregnated granular activated carbon, air, etc. in parallel/rectangular,

cylindrical, rotating impeller, and moving particle configurations. Some of these configurations

PT
are shown in Fig. 7.

RI
SC
U
N
A
M
D
TE
EP
CC
A

43
 PT
RI
SC
(f)

U
(d) (e)

N
A
M
D
TE

(h) (i)
(g)
EP
CC
A

44
 Fig. 7 Configurations of electrochemical reactors including (a) monopolar electrodes in parallel

connection, (b) monopolar electrodes in series connection, (c) bipolar electrodes in series connection, (d)

cylindrical concentric electrodes, (e) flow type system with rotating-screw type electrodes [156], (f)

horizontal rotating screw-type anode and U-shaped cathode [157], vertical rotating impeller anode and

cylindrical vessel cathode [4], (g) vertical rotating impeller cathode and cylindrical vessel anode [158], (i)

PT
cylindrical cathode and packed bed of wire netting wrapped cylindrically as anode [159].

RI
SC
However, electrode passivation is still a major concern in the operation of electrochemical

reactors. Passivation refers to the spontaneous creation of a hard non-reactive surface film,

U
usually an oxide or hydroxide, which inhibits the electrochemical activity of an electrode.
N
Meanwhile, passivation has been curtailed in recent studies by changing the polarity of the
A
electrodes, implementing periodic mechanical cleaning, applying alternating current, and
M

employing operating conditions that inhibits passivation [114,160].

D

pH also plays a vital role in electrochemical processes. It influences the solubility or otherwise of
TE

the targeted pollutants. For example, in an attempt to remove trace levels of five heavy metals -

arsenic, cadmium, chromium, lead, and nickel – from synthetic contaminated drinking water,
EP

Heffron et al. [161] observed that cadmium and nickel removal was significantly affected by pH.
CC

At pH 6.5, greater removal of cadmium and nickel was observed with aluminum electrodes; at

pH 8.5, greater removal was seen with iron electrodes.

A

45
 3.3 Modeling approaches for electrochemical processes

Nowadays, the modeling of standalone electrochemical systems is used for the optimization of

cost and electrical energy requirement. Many authors have attempted to model electrochemical

mechanisms for wastewater treatment. However, only a few have modeled the removal of

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wastewater pollutants from real medium-strength and high-strength municipal wastewater. Most

of the modelers in this field have only attempted to model composite constituents of wastewater

RI
and not fractions of wastewater constituents in detail. Most of the models were focused on

SC
electrocoagulation. Since electrocoagulation is a physicochemical process rather than a

biological process, previous models have been formulated by using physicochemical rate

U
equations, statistical analysis, and adsorption isotherms in order to determine the parameters

influencing the process.

N
A
M

Some of these rate equations employed recently to meet specific objectives are discussed here.

Electrostatic adsorption of pollutants on the surface of the coagulants has been identified as the
D

critical step in the process rate modeling [23]. Although equilibrium is unlikely to occur in
TE

continuous variable-feed wastewater treatment systems, the adsorption mechanism can still be

adapted for pollutant removal by electrocoagulation because of the formation of aggregates by

EP

this process. In general, pseudo-first and pseudo-second order rate equations have been primarily
CC

used to predict the adsorption kinetics during electrochemical processes. Adsorption isotherms

are also crucial for the modeling of electrocoagulation process because the adsorption capacity of
A

coagulant and driving force of adsorption can be estimated via adsorption isotherms. Freundlich

and Langmuir adsorption isotherms have been mainly used in recent studies but for process

intermediate products such as nitrates, Freundlich isotherm could provide the best fit for

experimental results [162].

46
 Statistical and empirical models have also been used successfully to model electrochemical

processes for wastewater treatment. Zaroual et al. [163] developed a model to obtain the

treatment efficiency of Cr3+ with aluminum anode using central composite design. 91% removal

efficiency of Cr3+ was obtained. Artificial neural network approach was used by Aber et al. [164]

PT
to model the removal of Cr6+ from polluted solutions by electrocoagulation and R2 value of 0.976

was obtained. The recent approaches used for the modeling of electrochemical systems and the

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notable findings from these approaches are summarized in Table 4.

SC
U
Table 4 Findings reported in recent studies on the modeling of electrochemical processes

N
for wastewater treatment.
A
M

Pollutant
Electrochemical Model Other
D

Wastewater type Model removal Ref.

process approach notable findings
TE

accuracy efficiency

Optimum conditions: pH 7.78,

EP

inter-electrode distance: 1 cm,

reaction time: 20 min, CD: 12.5

CC

Electrocoagulati Pharmaceutical 88.75%

RSM 90% mA/cm2, and electrolyte dose: [165]
on wastewater ciprofloxacin
0.07 M NaCl, initial
A

ciprofloxacin concentration:

32.5 mg/L.

Ozone-advanced Industrial RSM – 91.10% 100% color, CD: 3 A/cm2, COD [166]

47
electrochemical effluent CCD 97.5% COD concentration: 3000 ppm, pH:

process 7, inter-electrode: 1.8 cm, time:

5h

Electrocoagulati Synthetic RSM – 86.60% pH: 4, Co: 5 mg/L, CD: 4.325

79% [167]
2
on wastewater BBD ciprofloxacin mA/cm , time: 10 min

PT
UV-based

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sulfate radical
Pulp and paper RSM – Natural pH, time: 33.7 min,
electrochemical 97% 61% COD [168]

SC
wastewater BBD CD: 5.55 mA/cm2
oxidation

processes

U
RSM:

96.5%;
N Optimum conditions for min.
A
Electrocoagulati Synthetic RSM and energy consumption and max.
ANN- 82% Cr6+ [169]
on wastewater ANN-GA Cr(VI) removal >
M

GA:
20–40 A/m2, time: 10 min
98.7%
D

Sludge recycling
TE

in photo-Fenton The optimum conditions were

Synthetic dye RSM – 96.27% color,
process with 96.30% pH 8, 150 mA, and 20 min [170]
EP

wastewater CCD 67.5% TOC

electrocoagulati electrolysis time.
CC

on

Wastewater Al: (PA- pH: 5–13, CD: 49.5–

Central
A

containing 56.21%, BA- 255.5 A/m2, supporting

Electrocoagulati composite
terephthalic acid 59.52%, electrolyte concentration NaCl: [171]
on design
(TA), p-TA-45.71%, 0.25–2.25 g/L, electrolysis
(CCD)
Benzoicacid COD- time: 15–95 min

48
 (BA), Para- 49.91%);

toluicacid (p- Fe: (PA-

TA), COD 54.10%, BA-

53.84%, p-

TA-39.91%,

PT
COD-42.95%)

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Combined

Photocatalytic RSM, electrocoagulation/photocatalyti

SC
Lithographic
electrocoagulati Kinetic 99.20% >74% TOC c system was successful in [172]
wastewater
on modelling removing TOC content of the

U
wastewater

2,4-
N
A
dihydroxybenzo First order Cavitation phenomena increase
Sonoelectroche
M

ic acid (2,4- kinetic N/A 47% TOC the active electrode surface by [173]
mical cavitation
DHBA) model cleaning the electrode surface.
D

wastewater
TE

Optimum conditions: Stainless

Electrocoagulati
steel - (pH 7.80, CD 2.68
Hospital RSM – 94 - 99.11% -
mA/cm2), Al - (pH 5.45, [174]
EP

on wastewater CCD 99.8% 99.91% TOC

CD 4.46 mA/cm2), Fe - (pH
7.56, CD 4.87 mA/cm2)
CC

4. Integrated systems of MBR and electrochemical processes

A

The integration of MBR with electrochemical processes has been shown to enhance effluent

quality and reduce membrane fouling in many recent studies [175–179]. The electrodes can be

submerged in MBR or placed externally as a pre- or post-treatment unit. Meanwhile, a hybrid

wastewater treatment technique whereby MBR and electrochemical processes can be carried out

49
concurrently further reduces the environmental footprint of wastewater treatment. Such

integration provides the opportunity to achieve a one-stage treatment, or two-stage treatment if

further treatment to potable water levels is desired. An integrated system of MBR with

electrochemical processes can allow the use of low voltage, as compared to standalone

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electrochemical systems, because the integrated system is supported by other processes such as

biological treatment and membrane filtration. This integrated system is now commonly known as

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electrically-enhanced MBR (eMBR). Reduction in overall power consumption can be achieved

SC
with eMBR due to lower pumping energy required for membrane filtration (because TMP can be

kept at sub-fouling levels) and the lower voltages required for electrochemical processes. For

U
example, a pilot eMBR plant has been shown to consume specific electric power of 1.1–1.6

N
kWh/m3, compared to conventional MBR systems with power requirements above 2 kWh/m3, as
A
reported in some studies [116,180]. Most of the recent studies on eMBR have focused on the
M

impact of electrochemical processes on MBR. Due to the aforementioned reasons, the advances

on the integration of electrochemical processes with MBR have been directed towards the
D

application of minute electric field for minimization of electric power requirements, self-
TE

generation of electricity, and fouling suppression leading to improved performance.

EP
CC

4.1 Application of minute electric field and low voltage in eMBR

The possibility of attaining low energy consumption in eMBRs has encouraged researchers to
A

apply minute electric fields to eMBRs to further increase energy efficiency in these systems

[181,182]. Some of the recent configurations of eMBR are shown in Fig. 8. Liu et al. [181] tested

a new eMBR configuration to minimize energy consumption by placing many copper wires

50
inside a flat sheet membrane module. Two stainless mesh anodes were placed outside the

module. Microporous non-woven PP sheet (or polyester (PE) fabric filter cloth) was used as the

filtration membrane matrix. A minute electric field (0.036 V/cm or 0.073 V/cm) was then

applied to reduce the energy consumption and anodic corrosion. Although the applied electric

PT
field was low, sludge activity was significantly enhanced, compared to the control system that

was operated without the influence of external electric field. The minute electric field ensured

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electrophoresis and electrostatic repulsion between the EPS in the sludge and the membrane.

SC
Potential negative effects of excess electric field on microbes such as lysis and endogenous

respiration were also avoided through the application of the minute electric field. Therefore,

U
stable operation of the eMBR was achieved through the application of minute field.

N
Zhang et al. [182] also studied low voltage fouling mitigation using two eMBRs - one fixed with
A
stainless steel anode (Fe-MBR) and, the other, a titanium anode (Ti-MBR). The Fe-MBR showed
M

lower transmembrane pressure (TMP), less irreversible fouling and higher pollutant removals
D

under a low intermittent voltage of 2.72 V and current of 0.1 A. Under the influence of the low
TE

electric field, iron was released from the anode. The released iron reacted with soluble microbial

products (SMPs) to decrease TOC and polysaccharide in the reactor, thereby reducing the
EP

specific resistance to filtration (SRF) of the mixed liquor. The TMPs of Fe-MBR and Ti-MBR

were lower than those of the control MBR by up to 40.4 and 28.9%, respectively, indicating the
CC

effectiveness of low-voltage eMBR for overall fouling suppression. The fouling rates in both
A

eMBRs were lower than that of the control one, among which the Fe-MBR had the lowest (30%

lower than control MBR).

51
 (a) (b)

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SC
U
(c) (d)
N
A
M
D
TE
EP
CC

Fig. 8 Recent configurations of eMBR including (a) parallel external electrodes [183]; (b)
A

parallel submerged electrodes and flat sheet membrane [184]; (c) submerged membrane electro

bioreactor [116]; (d) parallel submerged electrodes and hollow fiber membrane [179].

52
Giwa et al. [8] used a low voltage gradient of 1.18 V/cm in an eMBR containing an aluminum

anode and stainless steel cathode to remove heavy metal ions and nutrients from medium-

strength raw wastewater. From the analysis of the chemical distribution pathways, the eMBR

also exhibited a viable potential for the recovery of the heavy metal ions and nutrients. The

PT
heavy metal ions removed from the wastewater were Si, Mn, V, Ti, etc. The application of low

electric field enhanced sludge settleability and filterability by significantly reducing the sludge

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volume index (SVI) and time-to-filter (TTF). Over 120 days of operation, low SVI and TTF of

SC
21.7 mL/g and 7 min, respectively, were achieved. The low electric field also caused pH

alterations in the mixed liquor such that the spatial distribution of heavy metal ions in the reactor

U
was influenced by electrophoresis, electro-deposition on electrodes, and electrocoagulation

N
leading to precipitation. The electrodes received less Si (bounded silicates) and more Mg than
A
the residual bottom sludge, as shown in eq. (4)–(6). The pH-induced effects of the low-voltage
M

electrokinetics ensured that Mg was kept in the mobile phase and adsorbed on the charged flocs

attracted to the electrodes. The influence of mobility gradient on Si was less (compared to Mg),
D

and Si was present in an excess amount in the sludge sediment than in the electrodes’ deposits.
TE

The amphoteric nature of silicates (and aluminates) facilitated the electrocoagulation of silicates
EP

under pH variations. Mn formed a large variety of oxy-manganates with net positive charge

collected predominantly on cathode instead of the anode. Fe appeared in both sludge sediment
CC

and electrode deposits due to its capacity to coagulate fellow heavy metal ions. V and Ti, which

are essential parts of cosmetics discarded into water, were also deposited in all pathways as
A

complex metal hydrates such as Mn.V2O6.6H2O in monoclinic form.

On sludge sediment:

Al > Si > Mg > Cr > Zn > Fe > Cu > Ti > V (4)

53
On cathode deposit:

Al > Mg > Si > Fe > Mn > Cr > V > Ti (5)

On anode deposit:

PT
Al > Mg > Si > Fe > Cr > V >Ti (6)

In general, it can be summarized that eMBR and its variants offer reduction in membrane fouling

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rate and energy consumption.

SC
U
4.2 Conductive membranes and self-generation of electricity in eMBR
N
A
The application of low voltages in eMBR would reduce cost. Likewise, other approaches such as
M
the use of conductive membranes and self-generation of electricity in eMBR systems have been

adopted in recent studies to further achieve cost-competitiveness. The use of conductive

D

membranes ensures that the electric field is directly applied to the membranes rather than the
TE

electrodes, thus minimizing material requirements. In some cases, conductive materials such as

porous carbon structures having low electrical resistance and good mechanical stability are
EP

embedded with the membranes. Akamatsu et al. [185] developed a membrane–carbon cloth
CC

assembly for submerged eMBRs. The assembly consisted of a flat sheet PVDF membrane

embedded with plain woven carbon cloth electrode and the porous support. This membrane
A

assembly has a porous structure, good conductive property, and low cost relative to alternative

materials. It was found that the assembly improved the capacity of the system to resist membrane

fouling. Membrane fouling was suppressed by applying an electric field continuously, and even

54
intermittently. The flux obtained while using the system to treat silica suspension was up to 2.4

times higher than the flux without applying any electric field.

Liu et al. [186] also fabricated electrically conductive membrane via the deposition of

polypyrrole. This electrically conductive polypyrrole was used to coat a base filter of terylene

PT
cloth membrane. The membrane developed was also employed as a cathode to induce an electric

field in an eMBR, thereby eliminating the need for an external cathode. Lower electric field

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strengths were facilitated by the conductive membrane for fouling control. A very small electric

SC
field (∼0.2 V/cm) applied to the stainless steel mesh anode was found to be sufficient to reduce

fouling. Polypyrrole modified membrane prepared via vapor phase exhibited smoother surface

U
and stronger attachment of polypyrrole particles, and hence showed better antifouling
N
performance than that prepared via liquid phase polymerization. Using the vapor-phase
A
polypyrrole modified membrane to treat simulated wastewater with an initial MLSS
M

concentration of 5770 mg/L for 10 days, about 50% reduction in membrane filtration resistance
D

was observed.
TE

eMBR can be made to generate its own power by combining it with a microbial fuel cell (MFC)

unit. MFC converts organic matter directly to electricity through bacteria in an anaerobic anodic
EP

chamber. The electrons flow from the bacteria to the anode, from where the electrons move to
CC

the aerobic cathodic chamber and electric current is generated in the circuit. A membrane is

placed between the chambers to maintain charge balance and ensure that the hydrogen ions
A

displaced from the anodic chamber are reduced in the cathodic chamber. Membrane fouling

reduction is also achieved in eMBR-MFC systems through the repulsive electrostatic force

between the sludge particles on the membrane surface, which would consequently enhance

sludge detachment from the surface [187]. H2O2 might also be generated to clean the foulants in-

55
situ [188]. Liu et al. [189] developed a bio-electrochemical membrane reactor (BEMR) system

with independent flat sheet stainless steel mesh membrane for electricity generation and

wastewater treatment. The flat membrane module functioned as the cathode of MFC as well. A

filter cloth was used to separate the aerobic cathode and anaerobic anode chambers. About 0.2 V

PT
cell potential was maintained under the stable situation to ensure energy efficiency. Significant

membrane fouling mitigation on the cathodic stainless steel membrane was achieved by the bio-

RI
generated electricity. The maximum power density of 1.43 W/m3 and a current density of 18.49

SC
A/m3 have been achieved in an eMBR-MFC system, indicating that eMBR can be used to

produce considerable power when coupled with MFC [188]. Current generation by eMBR-MFC

U
could reach a plateau of 16.9 mA when the organic loading rate is 11.4 kgCOD/m3day [190].

N
Liu et al. [187] developed a MBR system in which electricity from a MFC was used to power the
A
MBR. A bio electrochemical cell consisting of iron anodes, microbes and conductive membrane
M

cathodes modified by polypyrrole was integrated with the MBR. This configuration permitted
D

the use of an internally generated electric potential for the reduction of membrane fouling as
TE

opposed to using externally supplied electrical energy, thereby further reducing the high energy

requirement typical of conventional MBRs. About 0.2 V cell potential was obtained under
EP

different conditions. The benefits of integrating MFCs with eMBR such as better effluent

quality, longer operational time, and partially self-supplied energy were demonstrated. The
CC

electric potential caused accumulation of negative charges on the membrane cathode, leading to
A

the rejection of foulants via electrostatic repulsion.

eMBR-MFC systems without ion exchange membranes have also been devised recently. Zhou et

al. [191] has integrated an overflow eMBR with MFC, in such a way that ion exchange

membranes were eliminated due to their high costs and the need to remove internal resistance

56
that might be introduced by these membranes. The integrated system was able to mitigate

membrane fouling because of the effect of the MFC on sludge properties such as a decrease in

sludge particle zeta potential; an alteration of particle size distribution; and reduction of EPS and

SMP. Ma et al. [178] studied the long-term performance of an eMBR-MFC system in which the

PT
ion exchange membrane was replaced with a perforated plate to separate the anode and cathode

chambers. The maximum power density of the eMBR reached 98.4 mW/m2 after 250 days. An

RI
efficient degradation of organic matter was achieved in the anode chamber of the eMBR, which

SC
subsequently resulted in sludge reduction and membrane fouling mitigation (27.3% lower than

that of the control MBR).

U
N
A
4.3 Enhanced performance and treatment efficiency in eMBR
M

The quality of treated effluent from eMBR has been shown to meet the standards for water reuse

applications in recent studies. High-quality effluents from eMBR is related to the tendency of the
D

system to suppress membrane fouling by modifying the properties of the mixed liquor and
TE

fouling layers on the membrane, as earlier discussed. Many of the recent studies on eMBR have
EP

reported high removal efficiencies of organics, nutrients, and heavy metal ions. In a pilot-scale

submerged membrane electro bioreactor (SMEBR) system used to treat municipal wastewater,
CC

removal efficiencies of 92% COD, 99% PO43--P, and 99% NH4+-N, respectively have been

achieved [116]. These high removal efficiencies could be attributed to the effect of electrokinetic
A

phenomena which improved sludge properties, leading to 81% reduction in fouling index of the

sludge. The inclusion of the electrical field in eMBR leads to changes in the physical, chemical,

and biological properties of the MLSS [122]. Borea et al. [192] indicated that the electrochemical

57
 processes in eMBR might increase the sludge hydrophobicity to about 72 %, thereby improving

sludge dewaterability and reducing membrane cleaning frequency. Another eMBR pilot plant

operated for 6 months at a harsh temperature of 10 ⁰C in Northern Canada has been shown to be

able to achieve high removal efficiencies of >99% NH4+-N, >95% dissolved COD, and >90%

PT
PO43--P from real municipal sewage [193].

Giwa et al. [184] obtained high removal efficiencies of 98%, 99%, and 98%, for COD, PO43--P,

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and NH4+-N respectively from medium-strength municipal wastewater with eMBR. The effluent

SC
contaminant concentrations were below the water reuse quality standards for irrigation in Abu

Dhabi (UAE). Giwa et al. [88] also developed a numerical model of an eMBR in which the

U
electrodes were assembled in a new configuration of anode-cathode-membrane-module-cathode-
N
anode (A-C-M-C-A) to predict the quality of the treated wastewater. High removal rates of COD,
A
TP, TN, Ni, Fe, and Cr were obtained as 99%, 99%, 91%, 80%, 89%, and 80% respectively.
M

These results were correlated with the experimental data obtained from the system. The treated
D

effluent was useful for agricultural and forestry irrigation. The efficiencies of eMBR systems for
TE

the removal of wastewater pollutants, as reported in recent studies, are summarized in Table 5.
EP

Table 5 Removal efficiencies reported in studies on integrated systems of MBR and

CC

electrochemical processes.
A

Electrochemical Operating Pollutant removal

System design and configuration Ref.
processes conditions* efficiency

Electrocatalytic Electro-microbial membrane system Voltage: 1.6V Phenol: 99.6% COD:

[194]
membrane system (EMSS) with cylindrical titanium plate Influent/air ratio: 95.4%

58
 anode and Pd/carbon tubular membrane 1:15

SSA: 418 cm2

COD: 90.68%

NH4+-N: 72.10%
2
Electrocoagulation, CD: 0.5 mA/cm

PT
eMBR with Al cylindrical anode and PO43—P: 100%
electrophoresis, and HRT: 19 h [9]
stainless steel cathode DCF: 75.25% CBZ:
electrooxidation SSA: 0.047 m2

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73.84% AMX:

72.12%

SC
CD: 10-40 A/m2

U
HRT: 25 h Average fouling rate
Electrocoagulation eMBR with Al electrode [195]
SRT: 60 days reduced by 7.8 fold
N
SSA: 18 cm2
A
eMBR with bare copper wire cathode 20-25% permeate
M

Electrophoresis, and inside the membrane module and EF: 0.036 V/cm or flux and 20 times
[181]
D

electrocoagulation stainless steel mesh anode outside the 0.073 V/cm reduction of filtration
TE

module resistance

HRT: 15.3 h
eMBR with carbon felt anode and
EP

Exoelectrogenesis SRT: 220 days TN: 78.2% [178]

carbon fiber cathode
SSA: 0.0019m2
CC

CD: 15 A/m2,
COD: 99% PO43--P:
5 min ON and 15
Electrophoresis, 99% NH4+-N: 91%
A

eMBR with parallel plate Al electrode min OFF.

electrocoagulation, and Ni: 79% [88]
configuration HRT: 13.5 h SRT:
electrodeposition Fe: 89%
10 days
Cr: 80%
2
SSA: 0.11 m

59
Electroflotation, CD: 60 A/m2 Time:
eMBR with parallel plate Al electrode Cu: 63.6%
electrocoagulation, and 16 h [4]
configuration Zn: 93.7%
electrodeposition SSA: 88 cm2

EF: 0.1 V/cm COD: 84.8%

PT
Electrocatalytic eMBR with stainless steel anode and HRT: 12 h Phenol: 97.9%
[176]
degradation cathode SRT: 20 days Pyridine: 94.7%

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Spacing: 1.5 cm Quinolone: 94.1%

Membrane bioelectrochemical reactors

SC
HRT: 10 h
(MBER)-MFC with external membrane
anolyte flow:
Bioelectrogenesis module, carbon brush anodic chamber, COD: 98.5% [190]

U
20–90 mL/min
and carbon cloth cathode
N
A
Membrane fouling
M

12 or 32 V/cm
Membrane–carbon cloth SMEBR with was suppressed by
Electrocoagulation 4 min ON/4 min [185]
carbon cloth anode and cathode continuous and
D

OFF
intermittent EF
TE

MFC volume: 110

EP

MFC-OMBR system with anaerobic and 120 mL OMBR

PO43--P: 75% COD:
Exoelectrogenesis graphite filled chamber and stainless volume: 1.5 L [189]
95%
CC

steel cathode chambers OMBR membrane

area: 81 cm2
A

Electrophoresis and Moving bed eMBR with Al anode and EF: 3 V/cm PO43--P: 55% NH4+-
[196]
electrocoagulation SS cathode SSA: 0.047 m2 N: 98.7%

60
 Submerged membrane bioreactor
Electroosmosis and HRT: 12 h
(SMBR) with platinum plated titanium COD: >90% [175]
electrophoresis SRT: 20 days
anode and stainless steel cathode

SMBR with titanium cathode and Carbamazepine,

HRT: 18 h
several anodic materials such as ibuprofen, estradiol,

PT
Anodic oxidation SRT: 140 d [197]
Ti/IrO2, Nb/BDD, Ti/Pt, and venlafaxine: up to
Current: 2 A
∼97%

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Ti/IrO2/RuO2

HRT: 2 h

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Coal gasification
SMBR with Ti/SnO2 anode and active Inter-electrode
Electro-Fenton wastewater TOC: [198]
carbon fiber cathode distance: 5 cm

U
75%
TOC: 110–125 mg/L
N UV power: 8 W
A
Photoelectro-Fenton with cast iron H2O2 dosage: 57.6 % Landfill leachate
M
Photoelectro-Fenton [199]
electrodes followed by MBR pH: 2.9 SO42-: 82.7%

CD: 140.5 A/m2

D
TE

*CD is CD; HRT is hydraulic retention time; SRT is sludge retention time; Temp is
EP

temperature; EF is electric field; SSA is effective area.

CC

eMBR has also been employed for the enhanced removal of micropollutants and persistent
A

organic compounds such as pharmaceuticals and phenol from wastewater. Ensano et al. [9]

achieved enhanced removal of diclofenac (DCF), carbamazepine (CBZ), and amoxicillin (AMX)

of 75.25%, 73.84%, and 72.12%, respectively due to the different electrochemical mechanisms

inside the bioreactor. Jiang et al. [176] applied a novel eMBR configuration to remove phenol,
61
pyridine, and quinolone from coking wastewater. In this configuration, two pieces of stainless

steel mesh were placed inside a flat sheet membrane module as the cathode. Two stainless steel

mesh anodes were placed outside the module. It was found that phenol, pyridine, and quinoline

degradation rates in the eMBR were significantly higher, compared with the control reactor

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without an electric field. The electric field also resulted in a richer and more diverse bacterial

community in the eMBR.

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Cao et al. [194] achieved 99.6% phenol via an integrated electro microbial membrane system

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(EMMS) containing a Pd/C conductive membrane as a cathode. This removal efficiency was

higher than that of standalone microbial membrane system (MMS) and standalone

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electrocatalytic membrane system (EMS). Membrane fouling was also significantly reduced in
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the EMMS as shown by the membrane flux, which was 2.64 times that in MMS and 1.25 times
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that in EMS. In another attempt aimed at mitigating membrane fouling through eMBR by Hua et
M

al. [195], the average fouling rate was substantially reduced by 7.8 fold; therefore no chemical
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cleaning was required during the entire operation of the eMBR. This reduction was attributed to
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the additive benefits of electrocoagulation processes in eMBR such as charge neutralization by

electrostatic attraction, adsorption, and electro-chemical oxidation. The eMBR was also found to
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enhance sludge compressibility and control the growth of filamentous bacteria in the system.

Recently, the hybridization of eMBR systems with post-treatment or pretreatment units has also
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been shown to provide added benefits. An electro moving bed membrane bioreactor (eMB-
A

MBR) - a system that combines eMBR with a moving bed membrane bioreactor – has been

devised by Borea et al. [196]. A 60% reduction of membrane fouling was observed while using

the eMB-MBR, as compared to the MB-MBR.

62
In general, although considerable membrane performance has been reported in some studies on

individual electrochemical reactor and MBR units [200–202], improvements in membrane

performance offered by eMBR have resulted in higher permeate productivity and less membrane

backwashing. Bayar et al. [175] observed that the application of an electric field in SMEBR

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enhanced the permeate flux substantially, up to 54 L/m2/h, as compared to lower flux values in

conventional MBRs. This increase is observed in systems fed with both continuous and pulsed

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voltages. The use of alternating current (AC) dielectrophoretic (DEP) force in an inhomogeneous

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electrical field has also been shown to provide high permeate flux [203]. The permeate flux in

the test without DEP reduced to 50% of its initial value after only 20 min of operation whereas

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the flux obtained with electric field was above 50% of its original value even after 60 min. The

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applied DEP was also able to recover up to 85% of the initial flux after backwashing compared
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to the 50% for the system without DEP. Bani-Melhem et al. [204] reported membrane fouling
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reduction by an average of 16.3% in SMEBR without any backwashing of the membrane

module, compared with traditional submerged MBR.

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However, potential negative effects have also been highlighted in some studies. Timmes et al.

[205] compared the effectiveness of an ultrafiltration setup after a pilot-scale electrocoagulation

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pretreatment step. It was observed that the TMP in the set-up increased due to the pre-treatment.

It was suggested that problem might be attributed to the existence of soluble Fe(II) in the pre-
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treated effluent [206]. However, such a problem would not come up if aluminum was used as the
A

anode. Yu et al. [207] studied the influence of alum and FeCl3 on ultrafiltration (UF) membrane

fouling. FeCl3–UF exhibited significantly higher membrane fouling rate than the alum–UF

system. Fe-induced coagulation produced smaller particles, and denser and thicker cake layer,

which was considered to be responsible for the inferior membrane performance. Furthermore,

63
eMBR systems have also been shown to be susceptible to electrode fouling but this drawback

has been addressed through periodic manual or mechanical cleaning and polarity switching

[8,184].

Meanwhile, eMBR can be further tuned to produce optimized results by carefully selecting the

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operating conditions such as current density (CD), hydraulic retention time (HRT), sludge

retention time (SRT), and pore diameter of anode (dp) [23]. A mathematical model used to study

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the effect of operating conditions on eMBR performance revealed that an increase in CD or HRT

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and a decrease in anode porosity might lead to enhanced removal efficiencies of COD, TN, TP

and Fe due to higher amounts of hydrated coagulants that could be obtained under these

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conditions [23,184]. Increase in the SRT could favor nitrogen removal due to the delayed growth
N
of denitrifying organisms but influence COD and phosphorus removal negatively. However,
A
excessive CD and exposure time to current might adversely influence microbial activity. It is
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therefore important to adjust the electrical supply in the system to such a level that facilitates
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electrochemical treatment and permits the growth of microbial communities. Microbial

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communities have been found to thrive at continuous low CD of about 5 A/m2 [151]. This low

CD is desirable because it permits low consumption of electrical energy.

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5. Concluding remarks and future trends

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An extensive and detailed review of the current status, opportunities, and challenges of

wastewater treatment through MBR and electrochemical processes has been carried out. From

the broad literature survey, the most important features of standalone and hybrid processes

implemented for wastewater treatment are highlighted. These features include membrane

64
fouling, operating conditions as well as membrane characteristics, energy consumption, and cost.

Meanwhile, several recent studies on eMBRs have shown that eMBRs are able to address the

challenges of membrane fouling in MBRs and electricity consumption required for

electrochemical processes. Improved removal of organics, heavy metal ions, dyes and

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micropollutants via eMBRs have also been reported. However, studies on eMBRs are currently

focused on aerobic conditions. Furthermore, research on eMBR modeling that takes real feed

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solutions into account is currently limited and should be enriched. Future trends should focus on

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novel ideas such as electrically-enhanced anaerobic membrane bioreactors and electrically-

enhanced osmotic membrane bioreactors to further reduce energy consumption and ensure

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energy efficiency. The incorporation of low-voltage electric field with AnMBRs and OMBRs

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could improve the performance of these systems in terms of effluent quality, membrane
A
performance, and energy consumption. Meanwhile, to avoid being pre-emptive, such novel ideas
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should first be modeled and assessed experimentally. Other fresh concepts such as the coupling

of electrically enhanced OMBRs with MFC for improvement in self-electricity generation should
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be tested in the future. Although submerged eMBRs have been shown to offer lower
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environmental footprints, such footprints can be further reduced by using dual-purpose

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membranes, i.e. membranes that integrate the functionalities of membranes and electrodes.
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Acknowledgment
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Khalifa University of Science and Technology, Masdar City campus, is appreciated for providing

the platform and resources used for the preparation of this review paper.

65
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