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Ceramic-based microbial fuel cells (MFCs): A review

Vajihe Yousefi a, Davod Mohebbi-Kalhori a,b,*, Abdolreza Samimi a

a
Chemical Engineering Department, Faculty of Engineering, University of Sistan and Baluchestan, Zahedan, Iran
b
University of Sistan and Baluchestan Central Laboratory, Zahedan, Iran

article info abstract

Article history: Recently, porous ceramic and clayware membranes have been widely used in microbial
Received 25 February 2016 fuel cells (MFCs) as separators. Chemical, thermal and mechanical stability, low-cost and
Received in revised form many other advantages of ceramic membranes make them an appropriate substitute for
1 June 2016 expensive polymeric ion exchange membranes. Moreover, good power performances in
Accepted 3 June 2016 short and long-term periods were observed using ceramic membranes. In this review, we
Available online xxx attempted to gather and assort all the experiments which applied ceramic or other
earthenware membranes as the separator of MFCs. The effects of physical and chemical
Keywords: properties of ceramic membranes on the power efficiency of MFCs as well as scale-up
Microbial fuel cell (MFC) challenges and future aspects were also studied.
Low-cost separator 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
Ceramic membranes
Earthenware
Clayware
Proton exchange membrane (PEM)

done to bring this technology even closer to real world appli-

Introduction
Providing sufficient clean water and introducing new neat and
economic sources of energy instead of fossil fuel-based energy
are the most important challenges at present. Microbial fuel
cell (MFC) technology offers a solution to these problems by
simultaneously removing the organic pollutants in the
wastewater and providing clean electrical energy through a
catalytic reaction of microorganisms [1,2]. However, despite
the considerable developments in the past decades, the
commercialization of MFCs technology is delayed as a result
of several barriers such as low power performance [3,4], the
high cost of materials including high-priced proton exchange
membranes (PEM) and expensive metallic catalysts used in
the electrodes [5]. Until today, several researches have been
cations by engineering or technical approaches. Among them,
finding appropriate and economic separators attracted great
attentions [6,7].
In addition to high price, ion exchange membranes, i.e.
cation exchange membranes (CEM) and anion exchange
membranes (AEM), caused other problems including pH
splitting [8], biofouling [9], high oxygen and substrate diffu-
sion. Therefore, the cheaper and more effective alternatives
such as porous cloths, J-cloth, glass fiber, composite/polymer
membranes and etc were examined as separators in MFCs
[7,10].
Recently, ceramic membranes were introduced as a viable
option for scaling-up and the practical application of MFC
technology due to their low production cost, availability, very
good stability and high structural strength compared to other

* Corresponding author. Chemical Engineering Department, Faculty of Engineering, University of Sistan and Baluchestan, PO Box 98164-
161, Zahedan, Iran. Tel.: 98 54 31136459; fax: 98 54 2447092.
E-mail addresses: davoodmk@egn.usb.ac.ir, davod.mohebbi@gmail.com (D. Mohebbi-Kalhori).
http://dx.doi.org/10.1016/j.ijhydene.2016.06.054
0360-3199/ 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

Please cite this article in press as: Yousefi V, et al., Ceramic-based microbial fuel cells (MFCs): A review, International Journal of
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2 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9
separator materials. In this review, we focused exclusively on
the ceramic or other earthenware membranes used in MFCs
as the ion exchange medium. The effects of physical and
chemical properties of ceramic membranes on the perfor-
mance of ceramic-based MFCs were also investigated. Finally,
scale-up and stacking challenges, as well as future opportu-
nities, were discussed.
Parameters affecting the performance of
ceramic-based MFCs
The various methods of synthesis, unique thermal, chemical
and mechanical stability of ceramic membranes make them
an attractive option for many applications including fluid or
gas separations [11,12], solid oxide fuel cells (SOFC) [13], and
recently, MFCs. Fig. 1 briefly presents some important ad-
vantages of porous ceramic membranes.
Several factors like physical and chemical specifications of
the ceramic separator, type of electrodes and reactor config-
uration could affect the performance of ceramic-based MFCs.
In this regard, direct comparison of published performance
data of ceramic-based MFCs is not possible due to the signif-
icant differences in the systems and operating conditions
used. Therefore, a general and complete overview can yield
useful information. Table 1 summarizes the performance data
of applied ceramic and earthenware separators in MFCs up
until now.
MFC configurations
Designing the scalable MFC reactor with the lowest space
between the electrodes can significantly improve the MFC
performance especially when real domestic wastewater with
low conductivity is applied as a feedstock [28]. Many different
configurations were studied for ceramic-based MFC con-
struction including cylindrical or flat plate, single chambered
Fig. 1 e Some important advantages of ceramic
membranes.
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air-cathode as well as conventional dual chambered design.
Fig. 2 schematically illustrates the mechanism of electricity
generation in the conventional dual-chambered and single-
chambered air-cathode designs of MFCs. Typically, organic
substrates are degraded to protons, electrons and carbon di-
oxide by exoelectrogenic bacteria in the anode chamber
[29,30]. Then, the produced protons are transferred through
the membrane to be combined with oxygen (or other electron
acceptors) in the cathode chamber or on the cathode surface
for air-cathode MFCs. On the other hand, the generated elec-
trons are conveyed to the cathode via an external circuit,
leading to electricity power production. In air-cathode MFCs,
oxygen diffuses, directly, from the air to the cathode surface,
whereas in the aqueous-cathode of dual-chambered MFCs,
aeration or addition of other electron acceptors (like ferricy-
anide) is needed due to the limited solubility of oxygen in the
water [31]. For the first time, clayware separator was
employed by Park and Zeikus in one chambered air-cathode
MFC. Their clayware separator that was made of 100%
Kaolinite produced the nearly equivalent amount of electricity
as the conventional polymeric PEM containing dual-
chambered MFC [14].
Tamakloe and Singh compared the performance of one
and two chambered configurations of ceramic MFCs, both for
flat plate and cylindrical designs. Higher power performance
was obtained with the aqueous cathode as compared to the air
cathode ceramic-based MFCs when hydrogen peroxide solu-
tion was added to the cathode chambers [32]. However, it was
shown that air cathode design could outperform the aqueous
cathode when no additional electron acceptors were added to
the aqueous cathode. Chatterjee and Ghangrekar compared
different configurations of MFCs as well as different
separator-electrode assemblies. The air-cathode MFC with
carbon coating on the both sides of clayware separator and
proper current collector outperformed the other designs. This
air-cathode MFC produced 5.2 times higher power density
(4.38 W/m3) than the dual-chambered MFC with aqueous
cathode [33].
Simple and applicable air-cathode ceramic-based MFC was
also constructed by Ajayi and Weigele using off-the-shelf
terracotta flower pot painted by conductive graphite paint
[18]. They obtained relatively high current (22 mA) and voltage
(0.56 0.02 V) using 50 mM acetate solution as substrate.
The air-cathode MFCs are very favorable and advantageous
due to their simplicity and cost saving. Nevertheless, they
usually had anolyte leakage problem when porous ceramic
separators were used as ion exchange membrane of MFC and
thereby continuous hydration of cathode surface was needed
especially when those were operated in the batch mode
[19,33]. Winfield et al. proposed that pre-treatment of the
cathode or applying one hydrophobic gas diffusion layer (GDL)
like polyurethane or PTFE [34] on the cathode surface might
help to counter this problem when working in batch fed sys-
tem. In continues feeding of anolyte, moisture movement
through the ceramic could even contribute to a more efficient
wastewater treatment, due to electro-osmotic drag force [19].
However, hydrophobic polymeric layers like PTFE generally
have a low conductivity which hinders the efficient electron
transfer. Applying conductive gas diffusion layer on the air-
side surface of cathode may also improve the MFC
 Table 1 e Overview of ceramic-based MFC's performance.
MFC Separator Thickness Anode/ Anolyte Catholyte COD Rint (U) PD VPD CE (%) OCV Current CD Ref.
configure (mm) Cathode removal (mW/m2) (W/m3) (V) (mA) (mA/m2)
Hydrogen Energy (2016), http://dx.doi.org/10.1016/j.ijhydene.2016.06.054
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-ation (%)
One porcelain 2 Mn4 -graphite/ Sewage Air-cathode 787.5 0.45 14 1750 [14]
chamber septum Fe3-graphite sludge
(100% Kaolinite)
Dual Earthen pot 4 SS mesh/graphite plate Rice mill Aerated 96.5 171 48.64 2.31 21.2 0.772 3.04 [15]
chamber wastewater water
(PH 8.0)
Dual Earthen pot 5 SS mesh/ Sucrose Aerated 92e95.5 69 48.30 3.58 0.715 12.25 [16]
chambered graphite plate medium water
Dual Earthenware 3 SS mesh/ Sucrose Aerated 81.4 1.68 175 1.042 7.7 0.191 [17]

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chamber graphite plate medium water
5 SS mesh/ Sucrose Aerated 79.3 2.96 184 0.905 7.1
graphite plate medium water
7 SS mesh/ Sucrose Aerated 81.5 1.61 196 0.896 6.8
graphite plate medium water
8.5 SS mesh/ Sucrose Aerated 80.9 1.61 231 0.780 6.0
graphite plate medium water
One Terracotta nd Carbon felt/ Acetate Air-cathode 33.13 21 5 0.56 0.02 22 [18]
chambered graphite paint
One Ceramic 4 Both Carbon veil Tryptone Air-cathode 1.12  102 [19]
chambered Ceramic 8 Both Carbon veil Tryptone Air-cathode 7.22  103
Ceramic 18 Both Carbon veil Tryptone Air-cathode 8.02  103
Terracotta 4 Both Carbon veil Tryptone Air-cathode 1.08  102
Terracotta 8 Both Carbon veil Tryptone Air-cathode 8.06  103
Terracotta 18 Both Carbon veil Tryptone Air-cathode 6.62  103
Dual Red soil 5 mm/11.6% SS mesh/carbon Acetate Aerated 78.9 3.9 36 51.65 1.49 7.69 1.52 0.610 [20]
chamber clayware porosity felt medium water
Black soil 5 mm/17.6% SS mesh/carbon Acetate Aerated 89.6 3.2 56.5 31.20 1.12 6.39 1.40 0.580
clayware porosity felt medium water
Dual Red soil 4 Both carbon felt Acetate Aerated 74.4 3.76 136 3.95 18.3 1.57 0.507 0.0069 [21]
chamber control medium water
clayware
Dual Clayware 4 Both carbon felt Acetate Aerated 75.2 3.46 118 5.28 23.9 1.98 0.493 0.007
chamber 10% MMT medium water
Dual Clayware 4 Both carbon felt Acetate Aerated 78.5 3.85 96 6.87 27.3 1.04 0.501 0.009
chamber 15% MMT medium water
Dual Clayware 4 Both carbon felt Acetate Aerated 85.4 3.88 78 7.55 30.4 1.77 0.507 0.009
chamber 20% MMT medium water
Dual Clayware 4 Both carbon felt Acetate Aerated 75.1 5.92 104 5.51 23.1 1.15 0.498 0.0103
chamber 20% kaolinite medium water
Dual Ceramic 5 Both carbon felt WAS Aerated 65.4 8.2 251 nd 4.22 3.52 0.748 0.015 11.5 [22]
chamber water (A/m3)
NaOCl 81.7 7.8 90 nd 8.72 13.83 0.965 0.023 31.4
(A/m3)
(continued on next page)

3
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Table 1 e (continued )
MFC Separator Thickness Anode/ Anolyte Catholyte COD Rint (U) PD VPD CE (%) OCV Current CD Ref.
configure (mm) Cathode removal (mW/m2) (W/m3) (V) (mA) (mA/m2)
-ation (%)
Single mullite 4 mm/27% Carbon veil/ urine Air-cathode 41.5 5.9 500 3.94 4.98 0.550 [23]
chamber porosity conductive paint
Single earthenware 3.5 mm/14% Carbon veil/ urine Air-cathode 46.5 4.5 304 5.43 6.85 0.532
chamber porosity conductive paint
Single pyrophyllite 2 mm/2% Carbon veil/ urine Air-cathode 50.2 3.7 905 6.16 6.93 0.634
chamber porosity conductive paint

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Single alumina 3 mm/<1% Carbon veil/ urine Air-cathode 49.4 7.3 2000 2.06 2.06 0.499
chamber porosity conductive paint
Single earthenware 5 Both Carbon veil TYE Air-cathode Ca. 4.6 60 [4]
chamber solutiona (A/m3)
Dual Terracotta 3 Carbon veil/ Activated Internal 92 216 80.21 5.9 1.3 [24]
chamber activated carbon sludge cathode
sodium
acetate
Dual Mfensi 10 mm/14.3% Zinc/ wastewater 40% H2O2 86.98 69 0.863 100 [25]
chamber clayware porosity Aluminum solution
(1.7L anode)
Dual Mfensi 10 mm/14.3% Zn/Al wastewater 40% H2O2 88.10 55 0.844 89
chamber clayware porosity solution
(1L anode)
Dual Mfensi 10 mm/14.3% Zn/Cu wastewater 40% H2O2 solution 86.98 200 403 0.800 403 [26]
chamber clayware porosity
Dual Mfensi 10 mm/14.3% Graphite/ wastewater 40% H2O2 88.10 556 19 0.250 19
chamber clayware porosity graphite solution
Dual clayware 6 mm SS mesh/ Acetate NaOCl 90 3.2 15 148 6.57 25.6 Ca. 1.0 10.714 [27]
chamber carbon felt medium 2.9 (A/m3)

PD: power density, VPD: volumetric power density, CD: current density.
a
TYE solution is a mixture of tryptone, yeast extract and deionized water.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9 5

Fig. 2 e (A) schematic presentation of electricity generation mechanism in dual-chambered ceramic-based MFCs; (B) typical
picture of dual-chambered ceramic-based [32]; (C) schematic presentation of electricity generation mechanism in air-
cathode ceramic-based MFCs; (D) typical picture of air-cathode single chambered ceramic-based MFC [32] (open access,
Journal of the Ghana Science Association).

performance. Ortiz-Martinez et al., added ionic liquid mixture
to the PTFE to improve the conductivity of GDL and, subse-
quently, obtaining around 37% higher power [35].
Nevertheless, the dual-chambered design was equally
used in the ceramic-based MFCs same as the air-cathode
approach. Table 1 summarizes different configuration of
MFCs applied ceramic or clayware separators yet.
In addition to common single and dual-chambered designs
of MFCs, some innovative designs were also proposed to
improve the MFC performance in terms of power production
or wastewater treatment efficiencies. In order to improve the
quality of wastewater treatment, Jana et al. introduced a novel
up-flow cylindrical design of MFC with the concentric inner
earthen cylinder as both the anodic chamber and the sepa-
rator of MFC. In this novel design, high COD removal
(92e95.5%) was achieved since the anode effluent was entered
to the cathode chamber as catholyte for further aerobic
treatment (Fig. 3A) [16]. Similarly, Jadhav et al. entered the
anode effluent to the cathode chamber in order to improve the
treatment quality and disinfect the anode effluent in the
presence of sodium hypochlorite (NaOCl). Application of hy-
pochlorite as an electron acceptor in the cathode chamber
notably improved the MFC power performance too (Fig. 3B)
[27].
On the other hand, Gajda et al. presented a novel func-
tional cylindrical configuration with internal cathode cham-
ber (Fig. 4B), instead of typical internal anode design (Fig. 4A).
Interestingly, this simple and applicable MFC could be directly
immersed in the wastewater tank, meanwhile, the caustic
solution could be recovered as catholyte solution in the in-
ternal cathode chamber, at the same time. They found that
more volume of catholyte with higher pH level and conduc-
tivity was produced when MFC was under load as compared to
the open-circuit condition, due to electro-osmotic drag force.
Moreover, catholyte accumulation in the cathode chamber
provided a moisture bridge and sufficient hydration for the
oxygen reduction reaction (ORR). Therefore, the power pro-
duction performance was significantly improved [36]. In order
to achieve the more scalable design, Ghadge and Ghangrekar
constructed liter-scale cylindrical clayware MFC with multiple
electrodes. This larger scale MFC acted as three hydraulically
connected MFCs because of three embedded pairs of anode
and cathode in the cylindrical clayware anode chamber
(Fig. 4C).
Dan Thanh and Nitisoravut applied one cylindrical PVC
reactor consisted of one tube as anode chamber and V-shaped
earthen membrane as ion exchange membrane on the top of
it. However, this strange designed MFC only utilized to study
the effect of the anode to the cathode electrode ratio on the
performance of MFC (Fig. 4D) [37].
Cathodic reaction
Not efficient oxygen reduction reaction (ORR) on the cathode
is one of the most important problems of MFC technology in
practical implementation. Several factors affect the cathodic

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6 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9

Fig. 3 e Innovative ceramic-based MFC designs which were proposed to improve the wastewater treatment quality: (A)
novel up-flow design of ceramic-based MFC [16], reproduced with permission from Elsevier (license number 3885480253021)
(B) dual-chambered ceramic-based MFC designed for disinfection of anode effluent [27] reproduced with permission from
Elsevier (license number 3887520071556).

Fig. 4 e (A) typical cylindrical MFC with internal anode chamber [19], with permission from Elsevier (license number
3885920996106), (B) cylindrical MFC with internal cathode design [24], reproduced with permission from Elsevier (license
number 3885930188571), (C) multi-electrode large-scale MFC and representation of different electrical configurations [38],
reproduced with permission from Elsevier (license number 3887530383262), (D) V-shaped clayware MFC [37]).

reaction including cathode configuration (air-cathode or collector, catholyte and etc. As discussed in Section MFC
aqueous cathode), biotic or abiotic cathode, electrode and configurations, the air-cathode design of MFC has much
catalyst materials, electrode dimension, cathode current more superiority over the aqueous cathode if appropriate gas

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 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9
diffusion layer prevents the water leakage through the
ceramic separator.
Utilization of biotic cathodes, which used microorganisms
as a biocatalyst for ORR, can improve the power performance
and simultaneously can eliminate many toxic pollutants. Jana
et al. used aerobic cathode to improve the treatment quality
by entering the anodic effluent to the cathode chamber as
described in the previous section [16].
Cathode electrode type and material
Cathode electrode materials have a great impact on the power
performance of MFC. In addition to conductivity and the high
surface area, it should have a high redox potential to facilitate
the oxygen reduction on the cathode surface. Carbon based
materials like carbon cloth, carbon paper, carbon veil,
graphite and metallic electrodes were utilized as cathode
materials in the ceramic-based MFCs, thus far (Table 1).
Behera et al. compared the performance of stainless steel
(SS) mesh and graphite plate as cathodes in different condi-
tions (Table 2). More power output and current efficiency were
observed with graphite plate cathode as compared to SS mesh
under the most experimental conditions, excluding the ex-
periments carried out with the permanganate as catholyte.
The fourfold higher maximum power of 70.48 W/m3 at twofold
higher CE of 64.5% was obtained using SS mesh cathode as
compared to graphite plate with permanganate containing
catholyte. They suggested that the higher surface area of SS
and its short distance from the anode might be the reason for
the higher power production. In other experiments, particu-
larly when operating with the catholyte consisting organic
compounds, thicker biofilm layer, produced on the surface of
SS mesh, limited the oxygen diffusion towards the cathode
surface and diminished the power output [39].
Santoro et al. surveyed the performance of ceramic-based
MFCs with three different carbonaceous-based materials
including carbon cloth (CC), carbon mesh (CM) and carbon veil
(CV) as electrodes and current collectors. They found that the
current production performance of MFC was linearly correlated
with the nano-scale roughness of cathode electrode materials.
In fact, the higher roughness of the cathode material resulted in
better contact between the cathode and the ceramic mem-
brane. However, cost analysis showed that the CM was the
most cost effective electrode material among the others [40].
Chatterjee and Ghangrekar studied various electrode as-
semblies by different cathode materials and found that
although both the carbon powder and graphite plate electrodes
had relatively low conductivity, the MFC performance could be
improved considerably by utilizing SS mesh as a current col-
lector. Therefore, application of SS sock net current collector,
which thoroughly attached to the cathode surface, ensured
appropriate electron distribution and complete ORR occur-
rence; thereby less ohmic losses and higher power performance
were obtained. Furthermore, the MFC with SS sock net current
collector gained significantly more power performance than
the same MFC with SS wires as a current collector, probably due
to the higher surface area of SS sock net and its better attach-
ment to the cathode surface as compared to the SS wires [33].
Therefore, in addition to the selection of appropriate
electrode materials, through attachment of the electrode to
the ceramic membrane and application of effective current
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7
collector are the other important factors that assure the effi-
cient electron and proton transfer in the cathode.
Cathode catalysts or modifications
The addition of catalyst to the cathode is another method of
improving the cathode performance and lowering the over-
potential of ORR. Several materials were examined as cathode
catalyst in the MFCs yet, including conventional Pt catalyst
[41], carbon-based materials [42], metal oxide catalysts such
as iron, cobalt and manganese oxide, activated carbon [43] and
recently hybrid metal oxide/carbon nanotubes (CNTs) com-
posites [44,45].
In this regard, Park and Zeikus studied the effect of
different modification of electrodes on the performance of air-
cathode clayware-MFC. They applied Fe(III)-graphite as cath-
ode and Mn(IV)-graphite as anode electrodes and obtained the
best current production compared to the other electrode
combinations (Table 2) [14]. Seo et al. also applied modified Fe
(III)-carbon plate as cathode and Mn(IV)-carbon plate as anode
electrodes of single-chambered air-cathode ceramic-based
MFC. Their modified cathode was composed of three layers,
including semi-permeable cellulose acetate film (35 mm
thickness), a porous ceramic membrane (2 mm thickness),
and a modified porous carbon plate (20 mm thickness) with
Fe(III) ion [46]. Application of Fe(III) modified electrode for the
cathode purpose might be acted as ferricyanide addition in the
cathode chamber. This would be for the reason that Fe(III)/
Fe(II) (0.78 V) and O2/H2O (0.82 V) had a rather similar redox
potential differences, and therefore considerably boosted the
power performance of MFC [47].
Midyurova et al. also examined the effect of MnO2 addition
to the ceramic separator of one chambered air-cathode MFC.
They applied one modified ceramic membrane that was made
of Trojan clay impregnated with MnO2 and carbon fibers as
air-cathode. They observed 66% higher OCV (508 mV) in MFC
with this modified air-cathode compared to simple Trojan
clayware membrane with no MnO2 content [48].
Likewise, Santoro et al. utilized the inorganic Fe-
Aminoantipyrine (Fe-AAPyr) on the surface of three different
carbonaceous-based supports (CC, CM and CV) and almost
doubled current obtained by the addition of this catalyst layer
for all the support materials. They also studied the effect of
surface cathode modification by the addition of conductive
paint (PA) and microporous layer (MPL) on the surface of these
support materials [40]. The MPL is usually a mixture of carbon
black, PTFE dispersion, surfactant and solvent (e.g. iso-
propanol) which has small pore sizes of 0.1e1 mm [34]. These
modifications improved the performance of ceramic-based
MFCs considerably, since the addition of these layers
increased the conductivity of cathode materials, by filling
their pores. Furthermore, the above modifications increased
their roughness at nano-scale (60e500 nm), simultaneously,
and hence helped to better contact of the cathode materials
with the ceramic separator [40]. It was shown that the appli-
cation of MPL on the cathode surface could also prevent the
condensation of produced water on the cathode and thereby
could maintain appropriate surface cathode hydration for air-
cathode MFCs [49].
To improve the cathode conductivity, Ortiz-Martinez et al.
examined the modification of cathode by the addition of ionic
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Table 2 e The effect of electrode and electrolyte types on the performance of ceramic-based MFCs.
Anode Cathode Anolyte Catholyte Rint (U) PD (mW/m2) VPD (W/m3) CE (%) Voltage (V) Current (mA) Ref
SS mesh SS mesh Anaerobic Biotic- aerated 94 3.8 0.085 0.85 [39],a
sludge synthetic wastewater in
wastewater oxidation pond
(9days)
SS mesh SS mesh Anaerobic Biotic- aerated 90 19.6 5 12.5 0.193 (0.457 OCV) 1.93
sludge synthetic water with nitrate (4.38 short
wastewater (5days) circuit current)
SS mesh SS mesh Anaerobic Biotic- aerated 124 18.2 0.186 1.86
sludge synthetic

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distilled water
wastewater (3days)
SS mesh SS mesh Anaerobic Abiotic- aerated 215 16.0 0.174 1.74
sludge synthetic distilled water
wastewater (3days)
SS mesh SS mesh Anaerobic Abiotic- aerated 104 16.9 0.179 1.79
sludge synthetic water with nitrate
wastewater (6days)
SS mesh SS mesh Anaerobic Biotic- aerated 178 7.6 0.120 1.20
sludge synthetic wastewater in
wastewater oxidation pond
(14days)
SS mesh SS mesh Anaerobic permanganate 70.4 64.5 0.976 28.16
sludge synthetic
wastewater
SS mesh graphite Anaerobic Biotic- aerated 75 20.2 0.195 1.95
plate sludge synthetic wastewater in
wastewater oxidation pond
(9days)
SS mesh graphite Anaerobic Biotic- aerated 50 36.7 16.8 31.3 0.265 2.65
plate sludge synthetic water with nitrate (0.512 OCV) (13.11 short
wastewater (5days) circuit current)
SS mesh graphite Anaerobic Biotic- aerated 145 26.8 0.225 2.25
plate sludge synthetic distilled water
wastewater (3days)
SS mesh graphite Anaerobic Abiotic- aerated 150 24.9 0.217 2.17
plate sludge synthetic distilled water
wastewater (3days)
SS mesh graphite Anaerobic Abiotic- aerated 62 36.5 0.263 2.63
plate sludge synthetic water with nitrate
wastewater (6days)
SS mesh graphite Anaerobic Biotic- aerated 121 21.5 0.202 2.02
plate sludge synthetic wastewater in
wastewater oxidation pond
(14days)
SS mesh graphite Anaerobic permanganate 42.2 37.6 1.07 16.86
plate sludge synthetic
wastewater
Hydrogen Energy (2016), http://dx.doi.org/10.1016/j.ijhydene.2016.06.054
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SS mesh graphite Rice mill wastewater Dissolved oxygen 171 48.64 2.31 21.2 0.772 3.04 [15]
plate (PH 8.0)
Woven Woven Sewage sludge Dissolved oxygen 0.17 0.6 0.34 [14]
graphite graphiteb ferricyanide
Woven Fe3-graphite Sewage sludge Air-cathode 0.65 0.6 1.30
graphite lactate medium
NR- Woven Fe3-graphite Sewage sludge Air-cathode 5.32 (844.6) 0.58 11.0
graphitec lactate medium
Mn4-graphite Fe3-graphite Sewage sludge Air-cathode 787.5 0.45 14.0
lactate medium
Woven Woven E. coli lactate medium Dissolved oxygen 0.30 0.6 0.6
graphite graphite ferricyanide

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9
Woven Fe3-graphite E. coli lactate medium Air-cathode 0.44 0.35 1.5
graphite
NR- Woven Fe3-graphite E. coli lactate medium Air-cathode 1.20 (152.4) 0.35 3.3
graphite
Mn4-graphite Fe3-graphite E. coli lactate medium Air-cathode 91.0 0.28 2.6
Woven Fe3-graphite S. putrefaciens Lactate Air-cathode 0.18 [50]
graphite
NR- Woven Fe3-graphite S. putrefaciens Lactate Air-cathode 1.062
graphite
Mn4-graphite Fe3-graphite S. putrefaciens Lactate Air-cathode 1.238
Woven Fe3-graphite S. putrefaciens Pyrovate Air-cathode 0.196
graphite
NR- Woven Fe3-graphite S. putrefaciens Pyrovate Air-cathode 0.969
graphite
Mn4-graphite Fe3-graphite S. putrefaciens Pyrovate Air-cathode 1.089
Woven Fe3-graphite S. putrefaciens Acetate Air-cathode 0.134
graphite
NR- Woven Fe3-graphite S. putrefaciens Acetate Air-cathode 0.098
graphite
Mn4-graphite Fe3-graphite S. putrefaciens Acetate Air-cathode 0.071
Woven Fe3-graphite S. putrefaciens Air-cathode 0.102
graphite Glucose
NR- Woven Fe3-graphite S. putrefaciens Glucose Air-cathode 0.081
graphite
Mn4-graphite Fe3-graphite S. putrefaciens Glucose Air-cathode 0.056
CL GP Acetate heat-treated Dissolved oxygen 76 21 0.8384 0.798 [33],d
anaerobic sludge
CC CP Acetate heat-treated Air-cathode 239 17.24 0.5157 0.619
anaerobic sludge
CP&CL CP(SS sock net) Acetate heat-treated Air-cathode 62 45.89 1.373 0.649
anaerobic sludge
CP&CL CP(SS wires) Acetate heat-treated Air-cathode 23 146.42 4.381 0.595
anaerobic sludge
CC CP Acetate heat-treated Dissolved oxygen 308 12.6 0.3771 0.605
anaerobic sludge
CP&CL CP Acetate heat-treated Dissolved oxygen 109 21.4 0.6404 0.419
anaerobic sludge

9
10 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9

liquid (IL) on the cathode surface and also on the cathode-side

The two-compartment system (with PEM separator) was used only for the graphiteegraphite electrode combinations, the single-compartment air-cathode system (with kaolin ceramic separator)

Modified graphite woven electrode with covalently linked natural red (NR). First value represents theoretical outside plus inside surface area (1.27 m2). Parentheses indicate value for outside surface
surface of the terracotta separator. More than 86% improve-
ment in the power performance was observed by pressing the
The mentioned voltages and currents for this reference were obtained under a100 U load. The OCV and short circuit current values only determined for nitrated water experiments (Run2).

mixture of carbon active, PTFE and IL on the cathode surface.

On the other hand, the addition of IL layer on the ceramic wall
inhibited the proper ion transport through the porous ceramic
separator as a result of hydrophobic properties of IL, thereby
the MFC performance was significantly deteriorated [35].

Cathode electrolyte
Behera et al. investigated the effect of different catholytes
including aerated wastewater in the oxidation pond, nitrated
water and aerated distilled water for biotic and abiotic cath-
ode conditions. Abiotic cathode condition was studied by
removing the biofilm layer formed on the cathode surface
using 0.1 N HCl. They observed that the current and voltage
were reduced gradually during the operation in the oxidation
CL: carbon loth, CC: carbon cloth, CP: carbon powder, GP: graphite plate, SS: stainless steel; the voltage values for this reference were OCVs.

pond, due to the growth of thick biofilm on the cathode sur-

face and therewith the oxidation of organic matters in the
biocathode. Higher power production than the other cath-
olytes was observed by using nitrated water. The latter per-
formance was observed probably because of higher
electrochemical activity and conductivity of cathode in the
presence of nitrate or elimination of aerobic oxidation of
organic materials existed in the oxidation pond [39]. Indeed,
higher conductivity of electrolytes can help better trans-
portation of electrons and ions, thereby the ohmic resistance
and internal resistance of MFC is lowered.

Anodic reaction

The efficient anodic reactions of MFC are mainly contributed

by providing an appropriate environment for electro-active
bacteria, especially when mixed bacterial communities like
wastewater are used as the substrate. Many factors like MFC
configuration, inoculum type, anode electrode type and
dimension [42], temperature, conductivity, oxygen concen-
tration and pH level of anolyte as well as the membrane type
could affect the anodic reaction.
Type of biocatalyst used for inoculation of the anode is one
of the most critical components that directly affect the sub-
was used for all other experiments of this reference [14].

strate metabolism and extracellular electron transfer (EET)

mechanisms [51].
For example, comparison of different biocatalysts showed
that the ceramic-MFCs inoculated with sewage sludge bacte-
rial consortium outperformed both the Escherichia coli and
Shewanella putrefaciens-MFCs. It would probably be due to the
existence of electrophiles/anodophiles such as metal-
reducing bacteria in the sewage sludge which could better
transfer the electrons than the E. coli and S. putrefaciens. On the
other hand, organic materials were completely oxidized using
the sewage sludge consortium whereas E. coli and S. putrefa-
(80 cm2) alone [14].

ciens could only oxidize the lactate to acetate, thereby lower

electrons were produced [14,50]. Moreover, systems with
mixed culture biocatalysts are open systems which are suit-
able more for industrial applications. However, the variety of
the microbial community of mixed cultures might depend
widely on the origin of inoculum, substrate availability, MFC
d
b
a

configuration and operational conditions [52].

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Anode electrode
It is well known that an efficient anode electrode must be
conductive, biocompatible, non-corrosive, chemically and
mechanically stable and must have a high available surface
area for the efficient electron transfer from the bacteria to the
external electrical circuit [53].
To date, different anode electrode materials were
employed for ceramic based MFCs including metallic or
carbon-based materials as summarized in Table 1. In addition,
various electrode modifications, which have been so far
examined for the ceramic-based MFCs, have been particularly
presented and compared in Table 2.
Tamakloe et al. compared the performance of dual-
chambered Mfensi clayware-based MFCs with different elec-
trode pairs including Zn/Cu and graphite/graphite electrodes.
The MFC with Zn/Cu electrode pairs notably outperformed the
graphite/graphite electrode pairs so that 40% higher power
density and more than 300% higher current density were ob-
tained by the Zn/Cu electrode pairs as compared to the
graphite electrodes [26]. These great differences in the elec-
trical performance may contribute to the lower resistance of
metallic materials compared to graphite or carbon powder.
For instance, Rozendal et al. estimated the electrical resis-
tance of 1375 mU cm for graphite compared to 42 mU cm for the
metal titanium [54]. However, practical implementation of
metallic materials are limited due to their relatively high cost,
corrosion problem, and toxicity to bacteria [55]. On the other
hand, cheaper carbonaceous materials with high surface area,
good bacterial adhesion, and non-corrosive properties are the
best alternative for electrode materials [42]. However, their
relatively lower conductivity problem could be alleviated by
the application of metallic current collector along with them.
Different modifications and catalyst additions to the anode
could also be applied to improve the anode performance. In
this way, Park and Zeikus examined immobilization of one
electron mediator (natural red) on the surface of the graphite
electrode. They also added Mn4 as a catalyst to the anode and
compared the electrical performance of these modified elec-
trodes with the plane graphite felt electrode. Both of these
modifications improved the electricity generation perfor-
mance notably (Table 2) [14].
Seo et al. proved that Mn-oxidizing bacteria and Burkholderia
sp. constituted more than 99% of anodic bacteria after 90 days
of operation when Mn(IV) modified electrode was used as
anode [46]. Moreover, it was previously demonstrated that
exoelectrogenic bacteria, and in particular Mn(IV)-reducing
bacteria, can directly transfer electrons to the electrode,
without the addition of any electron mediator agent [56].
Operational conditions
It is well known that the operational conditions could signif-
icantly affect the power performance and in the particular
anodic reaction of MFC. However, the time that the anodic
microbial communities need to adapt the new conditions are
dissimilar for different membrane types.
The effect of influent wastewater pH on the performance of
both the earthenware and the Nafion-based MFCs was evaluated.
The lower power output and COD removal efficiency were
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obtained in rather acidic influent pH (6.0 and 7.0), as compared to
the pH level of 8.0. The lower conductivity of anolyte in the more
acidic pH levels resulted to the higher ohmic resistance and
thereby the higher internal resistance of MFC. Besides, the
slightly alkaline anodic pH might help better establishment and
activity of electrogenic bacteria as well as the other essential
bacteria which participating in the complete conversion of
complex substrates in the anode chamber. However, this power
deterioration at acidic pH was more pronounced for Nafion-
based MFC compared to earthenware-based MFC, probably
because of pH splitting phenomena occurred in PEM containing
MFCs or better proton conductivity of earthenware separator [15].
Application of ion-selective membranes as a separator in
the MFCs led to pH splitting and acidification of anode
chamber, which could inhibit the activity and development of
electro-active bacteria in the anode chamber and hence
deteriorated the power performance of MFCs. In contrast, the
size selective separators like ceramic membranes, which
transferred the protons based on their porosity, did not exhibit
any pH drop in the anolyte [7].
In this regard, Winfield et al. monitored the anodic pH of
MFCs under distinct loads with three different separators
including; CEM, biodegradable Bio-Bag, and ceramic mem-
branes. They observed that the anolyte pH level of all MFCs
dropped immediately when those were operated under the
critical loads (i.e. the load that caused the most instability
during the polarization sweep). However, for the CEM-based
MFC pH reduction was almost up to double the levels that
porous ceramic and Bio-Bag membranes reached after 4 h. On
the other hand, the MFCs with porous membranes were
recovered to near neutral pH after 18 h, but CEM-based MFC
still remained rather acidic after 48 h. Under the non-critical
loads, the CEM-based MFC pH was dropped to around 0.6
after 4 h, but for the ceramic and Bio-Bag membranes it did not
change at all. Therefore, the membrane materials could
remarkably affect the internal electrochemistry of MFC [4].
Finally, the ceramic porous membranes can provide an
appropriate stable environment for the development of bacteria
in the anode chamber, and upon to proper tuning of the physical
and chemical properties of ceramic membrane its good perfor-
mance is assured too. Pasternak et al. affirmed that the porosity
and the chemical composition of ceramic membranes applied in
the MFCs could notably affect the dynamic behavior of the bio-
film development and therefore determines the dominant mi-
crobial consortia in the anode chamber. For example, applying
mullite ceramic with high porosity (27%) as separator promoted
the facultative aerobic bacteria instead of electro-active bacte-
ria, due to more oxygen diffusion to the anode chamber [23]. A
comprehensive discussion about the effect of physical and
chemical properties of the ceramic membranes on the perfor-
mance of ceramic-based MFCs followed in the next section.
Physical and chemical properties of ceramic
separators
Ceramic separator composition
Type of minerals, their degree of dispersion and particle size
distribution of clay used for ceramic production can certainly
12 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9

affect the technological properties of ceramic such as density,
porosity, and proton conductivity, thereupon MFC perfor-
mance. In this regard, one of the most important specifica-
tions in the ceramic separator is the cation exchange capacity
(CEC) of its soil. CEC was defined as the sum of exchangeable
cations of the soil which could reversibly replace with cations
of salt solutions and acids [57]. On the other word, CEC is the
capacity of clay to hold on the positively charged exchange-
able cations and it is measured as milliequivalents per 100
grams of clay (meq/100 g) [58].
The effects of cation exchange capacity (CEC), pH, electrical
conductivity and porosity of the soil, used for ceramic pro-
duction, on the performance of MFC was explored using two
different clayware separators. The red soil (rich in aluminum
and silica) had higher CEC and electrical conductivity, but
lower pH and porosity as compared to the black soil (con-
taining more calcium, iron, and magnesium). The MFC with
red soil clayware generated higher volumetric power density
(1.49 W/m3) than the MFC made with black soil clayware
(1.12 W/m3) [20].
Pasternak et al. also compared the performance of MFCs
constructed with four different ceramic types including;
mullite, earthenware, pyrophyllite, and alumina. Earthenware
and pyrophyllite ceramics, with the higher silica concentra-
tions, obtained the higher power performance than the other
two ceramics [23]. However, the rate of proton transport
through the clayware membranes was restricted by the
number of exchangeable sites of minerals and by the strength
of the bonding of exchangeable cations to the mineral surface.
Some special minerals, called cation exchangers, have more
available exchange sites such as vermiculite, montmoril-
lonite, illite, kaolinite and etc. [59]. Moreover, the layered
silicate minerals like montmorillonite have good hygroscopic
properties that authenticating their application in proton ex-
change membranes of conventional fuel cells [60,61].
In a commercial point of view, application of locally
available and inexpensive materials is one of the notable
features of ceramic separators for scale up purpose. Never-
theless, some studies were carried out on the optimization
and improvement of physical and chemical specifications of
ceramics by the addition of some materials such as the cation
exchanger minerals to the ceramic clays.
In this regards, Ghadge and Ghangrekar blended different
proportion of montmorillonite and kaolinite with the ceramic
separators that were employed in MFCs. They systematically
compared the properties of those ceramic separators in terms
of conductivity, ion transport number, as well as oxygen and
acetate transfer coefficients. They found that the addition of
cation exchangers to the ceramic separator of MFC signifi-
cantly improved the power production and coulombic effi-
ciency. The MFCs with the highest percent of Montmorillonite
(20% w/w) generated 48% higher power density (7.55 W/m3)
than the control MFC (3.95 W/m3 without exchangers). In fact,
the addition of more montmorillonite acted as conductive
filler which reduced the oxygen and acetate diffusion co-
efficients and therewith improved the proton transfer rate
and membrane conductivity due to its great CEC (80e150 meq/
100 g). Higher proton conductivity decreased the internal
resistance and hence improved the power output of MFC. In
comparison, adding the same amount of kaolinite (20% w/w),
which have less CEC (15e20 meq/100 g), resulted in lower
membrane conductivity and cation transport number and
thereby lower power production (5.51 W/m3) as compared to
montmorillonite [21].

Fig. 5 e Comparison of the chemical structures and SEM cross sections of (A): montmorillonite [62], reproduced with
permission from Elsevier (license number 3887660698269) and (B): kaolinite minerals [63], reproduced with permission from
Elsevier (license number 3887661365389).

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Therefore, the addition of cation exchangers not only
reduced the porosity of separator by occupying the void space
of ceramic separator but also facilitated the proton transfer
through the separator by increasing the conductivity and
cationic exchangeable sites. However different clay minerals
have a different range of exchange capacities due to their
distinct structures and chemical compositions [59]. Fig. 5
compares the chemical structure of montmorillonite and
kaolinite minerals, as an example. Each layer of montmoril-
lonite clay contains one aluminum octahedral sheet sand-
wiched between two silicon tetrahedral sheets. Exchangeable
cations like Ca2, Mg2, Na, K and water molecules could
attract and hold between the layer of montmorillonite due to
the negative charge of the aluminum octahedron and silicon-
oxygen tetrahedron structures. Whereas, each layer of
kaolinite mineral contains one silicon tetrahedral sheet
attached with aluminum octahedral sheet [58]. Hence, these
clay minerals have so different cation exchange capacities.
Thickness and porosity of ceramic separator
The effect of earthenware separator thickness on the perfor-
mance of MFC firstly studied by Behera and Ghangrekar using
dual chambered earthen pot MFC. They observed that the
thinnest separator (3 mm thickness) significantly out-
performed the performance of MFC as compared to the
thickest separator (8.5 mm thickness). They suggested that
the increased electrode spacing may lead to the higher inter-
nal resistance of thicker separator compared to that of thinner
separator [17].
In this respect, Winfield et al., simultaneously, investigated
the effect of wall thickness, porosity, and water absorption
capacity of the separator on the MFC performance by
comparing terracotta and earthenware separators. They
found that the more porous earthenware was unstable be-
tween feeding due to anolyte leakage, but after three weeks it
was acclimated to MFC operations, perhaps because of biofilm
growth in the pores. Then, they proved that the more porous
terracotta separator was more efficient in power production
than the denser one. Insofar as, after 6 weeks of operation
insignificant distinction between power output and a wall
thickness of each separator was observed. For instance, the
MFCs with 8 mm terracotta and earthenware separators pro-
duced almost the same power levels as their respective 4 mm
separator containing MFCs. Meanwhile, the thickest earth-
enware separator (18 mm) produced 15% higher power than
the thinnest terracotta separator (4 mm). They explained that
higher water absorption capacity of earthenware separator
(16.6%), compared to the terracotta material (9.1%) signifi-
cantly assisted its proton conductivity. Therefore, the higher
power was obtained despite its higher porosity and increased
electrode spacing compared to terracotta [19].
In contrast, Ghadge et al., found that the higher porosity of
clayware separator resulted in the higher oxygen and sub-
strate crossovers between the MFC chambers and thereby the
lowered coulombic efficiency and volumetric power density.
More diffusion of oxygen also promoted the aerobic oxidation
of the substrate in the anodic chamber and resulted in the
higher COD removal of more porous clayware MFC. However,
they demonstrated that the higher volumetric power density
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of less porous clayware MFC was related to the higher CEC and
electrical conductivity of its constructing soil (red soil), and
not to its lower porosity.
On the other hand, Pasternak et al. observed the worse
power performance for the MFC with alumina membrane
which had the lowest porosity (<1%) among the four ceramic
membranes. They found that in addition to low silica content
and proton conductivity of alumina, the very low porosity of
alumina hindered the water diffusion from the anode to the
air-side surface of air-cathode. This limited the water hydra-
tion of air-cathode for the batch-fed system, and delayed the
efficient power production of alumina-based MFC. This was
the case until the time that, sufficient water molecules were
produced on the cathode and conveyed via electro-osmotic
drag mechanism to the cathode surface. Moreover, the
alumina-based MFC obtained the highest COD removal among
the other ceramic containing MFCs, probably due to the
occurrence of competitive reactions like fermentation or hy-
drolysis of urine by ureases [23].
In total, the compromises between the porosity and
thickness of ceramic separator must be considered for the
efficient MFC performance. Nevertheless, it should be noted
that the acceptable proton conductivity of ceramic separator
is a more determinative factor as compared to the other
physical specifications of the ceramic separator.
Short-term and long-term stability of ceramic
membranes
Winfield et al. compared the performance of ceramic mem-
brane with one plain compostable biodegradable bag (Bio-Bag)
and commercial CEM membranes, both in short and long-
term periods of operations. Long-term analysis showed that
the power generation of all MFCs was increased continuously
until the month six of operation. Then, the power output of
ceramic and CEM-MFCs stayed stable at the constant power
level by the month eight. Therefore, the ceramic separator
exhibited good performance in long-term operation as
compared to the commercial CEM membrane. However, the
bio-bag-MFC was deteriorated significantly after the month
six of operation and the power output declined to such an
extent that the MFC was completely depleted by the month
eight (Fig. 6A). In order to analyze the performance of each
separator in short time period, the bi-directional analysis was
performed (Fig. 6B, C, and D). The performance of CEM-MFC
declined significantly during the reverse sweep compared to
the forward polarization sweep, and obvious power overshoot
was observed for this MFC. The ceramic-based MFC produced
the highest maximum power density and almost two times
current density than the both CEM and Bio-Bag MFCs, without
any power overshoot problem. These results showed notable
short and long-term stability of ceramic membrane,
compared to the expensive commercial CEM, despite its high
power and current production [4].
Pasternak et al. also studied the short and long-term
performance of MFCs with four different ceramic mem-
branes. Inconsistent with Winfield et al., the power over-
shoot was observed for all ceramic-based MFCs at high
current densities during the polarization sweep, after 10
14 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9

Fig. 6 e Short and long-term analysis of different MFCs: (A) long-term variation of power density of three different type
membrane; (B) Bi-directional the power density curves for MFCs using CEM, (C) compostable BioBag and (D) ceramic as a
membrane. Square symbols indicate the forward curve (OCV to short circuit) and closed circles represent the reverse sweep
(short circuit to OCV). Asterisk show the point where power overshoot occurs [4], reproduced with permission from Elsevier
(license number 3887520162790).

days of operation [23]. The overshoot phenomenon
occurred when the demand for electrons overcame the
metabolic abilities of microorganisms due to the immatu-
rity of bio-film or mass transfer limitations [62]. However,
the anodic bacteria could overcome the electron demand
over time as far as only a negligible power overshoot was
observed after 18 days of operation for earthenware and
pyrophyllite. The bio-film adaptation time was not similar
for different types of ceramic membranes, since, for mullite
and alumina membranes, symmetric polarization curves
were recorded after 32 days of operation. Finally, analyzing
the polarization experiment after 32 days of operation
showed that both earthenware and pyrophyllite mem-
branes outperformed the other two ceramic types [23].
Ghadge and Ghangrekar studied the long-term perfor-
mance of large-scale MFC for 14 months. Obvious fouling was
observed on the surface of cathode after 360 days of operation
which resulted in increasing the internal resistance and
diminishing the power production by 41% (from 0.74 to
0.43 W/m3). In addition to bio-fouling, significant chemical
fouling also occurred as a result of synthetic wastewater
feeding [38]. Similarly, Behera et al. reported that the forma-
tion of thick bio-film on the cathode surface bounded the
oxygen diffusion towards the electrode surface. As a result,
then, the power output declined due to limited oxygen
reduction reaction on the cathode [39]. The thickness of bio-
film also affected on its conductivity and electron transfer
capability [63].
Pasternak et al. noticed 72%, 23%, 30% and 33% power drop
for earthenware, pyrophyllite, mullite, and alumina, respec-
tively, after 88 days of operation. They suggested that these
notable decreases of the power density of ceramic-based
MFCs occurred as a result of combined biological, physico-
chemical and electrochemical phenomena. Those included of
increasing the thickness and aging of the bio-film, precipita-
tion and accumulation of uric salts on the cathode which may
deteriorate the cathode activity as well as microorganisms
growing on the membrane pores [23]. Chatterjee and Ghan-
grekar also observed the biological and chemical fouling
layers on the surface of cathode after 3e4 weeks of operation
which gradually limited the oxygen diffusion and decreased
the operating voltage. However, they reported that installa-
tion of SS sock net current collector on the outer surface of air-
cathode could significantly prevent the MFC fouling. The
proper electron distribution by the SS net resulted in imme-
diate utilization of protons and uniform pH on the cathode
surface. Whereas in the MFCs without the efficient current
collector non-uniform consumption of proton caused to
localized pH and thereby deposition of inorganic salts on the
cathode surface [33].
The ceramic membranes have superior physical integrity,
chemical resistance and thermal stability which render them

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suitable for extreme cleaning conditions including acid or
alkaline washing as well as physical cleaning methods. Se-
lection of the best method for the cleaning of fouled mem-
brane and degrees of membrane regeneration depends on the
type of fouling. Zhong et al. reported that particle cleaning
combined with acid cleaning methods completely restored
the fouled ceramic membrane for the filtration application
[64], whereas the physical washing of biofouled CEM did not
improve the MFC performance at all [65].
MFC stacking and scale-up challenges
In spite of viable properties of ceramic separators for large-
scale application, in this regard, little efforts have been done
yet. Tamakloe et al. compared the performance of two Mfensi
clayware-based MFCs with 1 L and 1.7 L anodic volumes. No
significant distinction between the electrical performances of
these MFCs was observed, so that only 14% higher power
density and 11% higher current density were obtained for the
bigger MFC [25]. Previously, similar results were observed for
MFC scale-up [66], and it was proved that by increasing the
volume of MFC, internal resistance increased, accordingly [67].
However, by introducing innovative designs so that mini-
mizing the electrode distance and ensuring the optimal con-
tact of the electrodes to the ceramic separator, acceptable
power efficiencies could be achieved using even large-scale
MFCs [68]. Ghadge and Ghangrekar presented novel scalable
26 litter air-cathode clayware-MFC with multiple electrodes.
Three embedded pairs of anode and cathode electrodes in this
large-scale MFC acted as three hydraulically connected small
MFCs (Fig. 4C). Different electrical connections of these MFCs
were examined, in which parallel configuration presented the
best performance. The power of 11.46 mW, coulombic effi-
ciency of 5.10 0.13% and very low internal resistance of 5.2 U
were obtained when MFCs were connected in parallel [38].
On the other hand, stacking of small-scale MFCs is another
promising approach for MFC scale-up which could provide
acceptable power output level for practical implementation of
MFC technology [69]. In this context, Ieropoulos et al. could
directly charge one mobile phone by a stack of 24 small-scale
(6.25 ml) ceramic MFCs feeding on urine. The produced power
was still low for realistic application since 24 h charging by
this MFC stack was sufficient to power the phone for only
25 min [70].
Gajda et al. directly connected three novel-designed
tubular MFCs with the internal cathode in parallel to power
one motorized model windmill and the excess energy stored
in one 300 F supercapacitor. Then, they proved that even one
single MFC could charge the mobile phone, using an energy
harvesting system [36]. Wang et al. reviewed various energy
harvesting systems, which can capture and store energy, and

Fig. 7 e Stacking the ceramic-based MFCs applied for indoor lighting; (A) 288-MFC stack trial in the UWE campus, (B) 3-D
representation of 288-MFC stack with the inlet and outlet tanks underneath the urinal, (C) 432-MFC stack trial in
Glastonbury Music Festival, (D) 432-MFC stack arranged in 12 modules [74], reproduced with permission from Elsevier
(license number 3885950988011).

Please cite this article in press as: Yousefi V, et al., Ceramic-based microbial fuel cells (MFCs): A review, International Journal of
Hydrogen Energy (2016), http://dx.doi.org/10.1016/j.ijhydene.2016.06.054
16 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9
also existing challenges and barriers of this technology for
practical application of MFCs or other bioelectrochemical
systems (BESs) [3].
Different electrical configurations of MFC-stacks were
investigated previously. Nearly two-fold power and 10-fold
current were produced when MFCs were electrically con-
nected in parallel compared to serial configuration [71].
Nonlinearity of MFCs resulted in cell reversal and instability
especially when MFCs were connected in series and thereby
the power performance decreased significantly [23,72]. More-
over, faster COD removal observed in parallel connection due
to the generation of higher current densities [73]. Seo et al.
connected four ceramic-based MFCs serially with one solar
cell. The electrical generation efficiency increased from 1.57%
to 29.4% as a result of electron driving force generated by the
solar cell [46].
More practical implementation of ceramic-based MFCs has
been done by stacking 288 MFC reactors feeding with urine to
directly power the indoor lighting [74]. These MFCs were
similarly built using low-cost cylindrical terracotta as a
separator and an internal cathode. The latter MFCs could
directly immerse into the wastewater chamber, and in addi-
tion to electricity generation, those could produce an alkaline
solution as catholyte [24]. Their 288-MFC stack consisted of
eight serially connected modules and each module contained
thirty-six MFCs which electrically connected in parallel
(Fig. 7A, B). This 288-MFC stack produced 400 mW power when
directly connected to the lights and maximum 160 mW power
was generated when connected via supercapacitor. Despite
underperformance of one module, compared to the other
seven modules, no voltage reversal was observed for this MFC
stack. Then, even larger urinal MFC stack was set up, during
the music festival, for more than 1000 audiences per day, by
stacking 432 MFCs together (12 modules). This system could
produce 800 mW directly and maximum 400 mW by applying
the capacitor (Fig. 7C, D). Although the significant higher
power performance of the second MFC stack was obtained,
the urine treatment performance decreased notably due to
very high flow rate and low hydraulic retention time (HRT) of
urine in the MFCs. In this case, the COD removal efficiency
decreased from more than 95% in the first 228-MFC stack to
the 30% for the 432-MFC stack trial [74].
Future aspects
Outstanding specifications of ceramic membranes in MFC
applications proposed them as a viable candidate including
treatment of large-scale massive wastewaters or strong acidic
and alkaline solutions, thermal shock separations as well as
wastewater treatment. However, their usage was limited to
the scientific communities instead of industrial applications
as a result of some drawbacks on the development of com-
mercial ceramics. There are a number of questions to be
addressed through more research on ceramic-based MFCs.
Finding the technology, which could provide the ceramic
membrane with high permeability, good selectivity, and low
cost is the most challenging aspect in the development of
ceramic membranes. Wu et al. reviewed the common
Please cite this article in press as: Yousefi V, et al., Ceramic-based microbial fuel cells (MFCs): A review, International Journal of
Hydrogen Energy (2016), http://dx.doi.org/10.1016/j.ijhydene.2016.06.054
techniques for preparation of porous ceramic membranes as
well as their challenges for industrialization [75].
Moreover, finding new materials or novel surface modifi-
cation techniques might be the future trends for ceramic
membrane development technology, particularly for MFC
applications. The materials and techniques such as grafting
hydrophilic polymers [76] on the surface of ceramic mem-
branes, which could eliminate the bio-fouling problems and
concurrently provide acceptable short and long-term MFC
performance.
One of the drawbacks accompanied by employing ceramic
membrane as a separator in MCFs can be its low ion conduc-
tivity. One method of avoiding this is the using of a hydro-
phobic gas diffusion layer.
In addition ceramic-based MFC performance has been
negatively affected by oxygen diffusion into the anode
chamber. The oxygen consumption by the existing bacteria in
the anode chamber as the terminal electron acceptor instead
of the current collector, decrease the coulombic efficiency
(CE). In this situation the anode potential will become more
positive, resulting decrease of the current density of the MFC.
In this regard, coating of the ceramic membrane on the
cathode side by the suitable nanocomposite materials can be
useful in ceramic-based MFC designs. Development of nano-
composite material coatings that facilitate proton transfer to
the cathode but limit oxygen diffusion into the electrolyte and
along with providing an electrically insulating surface can be
considered as an alternative method.
Power densities of ceramic-based MFCs when scaled-up
are still not enough high to be competitive with fuel cells or
waste-to-energy technologies. Therefore, a greater focus on
scaling-up of these cells needs to be conducted to obtain sig-
nificant advances in the technology of MFCs from lab-scale to
the pilot-scale and beyond.
Conclusions
MFC technologies, which can provide valuable green en-
ergies like hydrogen or electricity by treating the waste ma-
terials, can actually introduce one of the best solutions for
environmental problems of modern communities. Applica-
tion of porous ceramic membranes in the biological systems
showed their future opportunities for further development
and industrial applications. In this review, the most impor-
tant parameters on the performance of ceramic-based MFCs
were investigated comprehensively, including the MFC
configurations, the cathode and anode performances as well
as chemical and physical specifications of ceramic
separators.
Although air-cathode MFCs have many benefits over the
conventional dual-chambered MFCs, their power perfor-
mance was disrupted significantly as a result of anolyte
leakage through the porous ceramic separator, especially at
the batch fed operations. This problem could be alleviated by
applying one hydrophobic gas diffusion layer on the air side of
the cathode surface. In the review, the other innovative de-
signs of ceramic-based MFCs were discussed as well. The
different anode and cathode electrode materials and their
modifications also affected the MFC power performance.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y x x x ( 2 0 1 6 ) 1 e1 9
Selection of more conductive materials and proper attach-
ment of electrodes to the ceramic separator using efficient
current collector decreased the internal resistance of MFC. On
the other hand, the chemical composition of ceramic sepa-
rators, as well as acidity and cation exchange capacity (CEC) of
constructive clay of ceramics could significantly affect the ion
conductivity and thereby ohmic resistance of ceramic
separators.
Physical specifications of ceramic separators such as their
porosity, thickness and surface morphology could also influ-
ence the power performance and stability of ceramic-based
MFCs. However, the proton conductivity of ceramic is the
most critical factor among the physical and chemical specifi-
cations of ceramic separators which could fade the impor-
tance of other influencing factors. In addition, due to the
complexity of biological systems, many other factors can
affect the performance of MFCs, and further researches need
to be done to take this technology a step ahead toward
commercialization.
Acknowledgments
This research was supported by the University of Sistan and
Baluchestan (Grant No. G1393/1).
The authors acknowledge Mr. Sepehr Mohebbi Kalhori
from John Abbott College, Montreal, Canada for proof editing
of English language of the manuscript.
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