Bioresource Technology 100 (2009) 41714175

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Bioresource Technology
journal homepage: www.elsevier.com/locate/biortech

Electricity generation and modeling of microbial fuel cell from continuous

beer brewery wastewater
Qing Wen a,*, Ying Wu a, Dianxue Cao a, Lixin Zhao b, Qian Sun a
a
College of Material Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China
b
Mechanical Science and Engineering College, Daqing Petroleum Institute, Daqing, Heilongjiang, China

a r t i c l e i n f o a b s t r a c t

Article history: Electricity production and modeling of microbial fuel cell (MFC) from continuous beer brewery wastewa-
Received 16 December 2008 ter was studied in this paper. A single air-cathode MFC was constructed, carbon ber was used as anode
Received in revised form 24 February 2009 and diluted brewery wastewater (COD = 626.58 mg/L) as substrate. The MFC displayed an open-circuit
Accepted 27 February 2009
voltage of 0.578 V and a maximum power density of 9.52 W/m3 (264 mW/m2). Using the model based
Available online 29 April 2009
on polarization curve, various voltage losses were quantied. At current density of 1.79 A/m2, reaction
kinetic loss and mass transport loss both achieved to 0.248 V; while ohmic loss was 0.046 V. Results dem-
Keywords:
onstrated that it was feasible and stable for producing bioelectricity from brewery wastewater; while the
Beer brewery wastewater
Microbial fuel cell
most important factors which inuenced the performance of the MFC are reaction kinetic loss and mass
Continuous operation transport loss.
Model 2009 Elsevier Ltd. All rights reserved.

1. Introduction hand by biological parameters such as the substrate (COD) removal

Energy need has been increasing worldwide exponentially. At
present, global energy requirements are mostly dependent on the
fossil fuels, which eventually lead to foreseeable depletion of lim-
ited fossil energy sources. Combustion of fossil fuels also has seri-
ous negative effect on the environment due to CO2 emission.
Climate changes, increased global demand for the nite oil, natural
gas reserves and energy security have intensied the search for
alternatives to fossil fuels.
MFC is promising as a device to treat urban wastewater and
produce electricity at the same time, which can directly convert
chemical energy of organic matter into electrical energy under
anaerobic condition (Larminie and Dicks, 2000). The principle re-
lies on the fact that the generation of current is in the nature of
microorganisms, as they transfer electrons from a reduced electron
donor to an electron acceptor at a higher electrochemical potential.
The anodic process uses bacteria to catalyze the electron transfer
from organic electron donors to the anodic electrode. The electrons
are then transferred through an external circuit to the cathode
chamber where they reduce the nal electron acceptor, typically
oxygen. MFC has characteristics similar to traditional power
sources as well as to anaerobic reactors, which can be described
on the one hand by electrochemical parameters such as power
density, electrical current output and cell voltage; on the other
* Corresponding author. Tel.: +86 13351403636.
E-mail address: wenqing_hrbeu@yahoo.com.cn (Q. Wen).
efciency (Rabaey et al., 2003).
The study of MFC is gaining importance recently (Rozendal
et al., 2006; Kargi and Eker, 2007; Liu and Li, 2007; Min and Angel-
idaki, 2008; Venkata-Mohan et al., 2008a,b; You et al., 2008), but
most studies were based on articial wastewater, for example, glu-
cose, acetate, sucrose (Menicucci et al., 2006; Freguia et al., 2007;
Kargi and Eker, 2007; Liu and Li, 2007; Venkata-Mohan et al.,
2008b; You et al., 2008), etc. There were only a few researches
on actual wastewaters. Domestic wastewater were reported to be
available for electricity generation in several MFC congurations
(Liu and Logan, 2004; You et al., 2006; Min and Angelidaki, 2008;
Zhan et al., 2008), the maximum power density of 204 mW/m2
was documented. Huang and Logan (2008) reported the effective-
ness of electricity production with paper recycling plant wastewa-
ter using MFC, the maximum power density reached 672 27
mW/m2. According to Venkata-Mohan et al. (2008a), specic
power density of 0.73 W/kg COD (67.48 mW/m2) with chemical
wastewater was recorded. Beer brewery wastewater treatment
using air-cathode microbial fuel cell (MFC) was investigated by
Feng and Wang (Feng et al., 2008; Wang et al., 2008), a maximum
power density of 528 mW/m2 was achieved. All these papers
mainly studied the effects of operational parameters and solution
chemistry on MFC performance, such as substrate concentration,
substrate loading rates, temperature, etc.
Up to now, there are a few mathematical models for MFC (Picio-
reanua et al., 2007, 2008; Torres et al., 2008), such as electrochem-
ical model, biochemical model, biolm model, bulk liquid model,
etc. Most of these models are based on Nernst equation; frames

0960-8524/$ - see front matter 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.biortech.2009.02.058
4172 Q. Wen et al. / Bioresource Technology 100 (2009) 41714175

and parameters of the models are complicated, the process of mod-
eling is also complex. A basic simple model, which can provide
important predictions and optimization about inuence of activa-
tion loss, charge transport and mass transport on the performance
of MFC, is more applicable. Therefore, establishing of simple model
for MFC should be given attention.
In this paper, the feasibility of electricity production from con-
tinuous brewery wastewater using air-cathode MFC was demon-
strated. The inuences of external resistance on voltage, power
density, COD removal efciency and Coulombic efciency (CE) on
performance of MFC were investigated. A basic electrochemical
model of MFC was established based on polarization curve; a de-
tailed analysis of various voltage losses was carried out to obtain
the net fuel cell jV behavior.
2. Methods
2.1. Microbial fuel cell conguration
on the unit change; 0.1 denotes the volume of anolyte (L). To mea-
sure electrode potentials, a digital voltmeter was used against a
saturated Ag/AgCl reference electrode. The Coulombic efciency
(CE) was calculated using the ratio of total Coulombs obtained in
the experiment (CP) to the theoretical amount (CT) available from
complete substrate oxidation (Liu et al., 2004):
CP It
CE  100% M 1
CT F  n  DS  V
where I represents the current (A); t is the time interval (s); F is the
Faraday constant = 96,485 C/mol; n is the number of moles of elec-
trons produced per mol of substrate (n = 4 for oxygen reduction on
cathode); DS is the absolute removal amount of COD (mg/L); V is
the volume of anolyte (L); M is molecular weight of the substrate
(32 g/mol for oxygen).
Polarization curves were obtained by plotting potential and
power density against current density. Potential were measured
at variable resistance points (900020 X) during stabilized fuel cell
operation. COD was determined by standard method (Wei, 2002).

Single-chambered MFC was constructed by a Plexiglas vessel

3. Results and discussion
with internal dimensions of 6  5  6 cm (180 mL in volume). A
water inlet and an outlet port were set up on each side of the ves-
3.1. Startup of MFC
sel; six electrode tip jacks with diameter of 9 mm were installed on
the top of the vessel. Anode was made of three parallel groups of
Voltage was produced over time when brewery wastewater was
carbon bers, which were winded on two graphite rods forming
pumped into anode chamber. When voltage reached to 0.263 V, the
a window blind-like structure. The net volume of this reactor
cell voltage and current density were recorded using a data acqui-
was reduced to 100 mL. Air-cathode and proton exchange mem-
sition board controlled by a computer (Fig. 1). With the increase of
brane (PEM, Naon 117, Dupont Co., USA) were pressed together
the time, a steady increase in open-circuit voltage was observed
tightly. The air-cathode was manufactured by pressing catalyst
and registered a maximum of 0.578 V after 55.6 h. Along with
layer (88 wt.% activated carbon powder and 12% polytetrauoro-
the voltage increase, biolm growth on the anode was observed.
ethylene (PTFE), containing 0.8 mg/cm2 Pt catalyst), stainless steel
Thereafter, external resistance (R = 9000 X) was connected to the
net and wet-proof gas diffusion layers (50% Na2SO4 and 50% PTFE).
circuit, after a short time decrease, a relatively steady voltage of
The projected surface area of cathode was 36 cm2. PEM was pre-
0.534 V and current density of 0.059 A/m2 were achieved, which
treated according to the procedure reported by Yoshitake et al.
indicated that the startup of MFC had nished. The experimental
(1996) to increase the porosity and stored in deionized water prior
data demonstrated the feasibility of bioelectricity from brewery
to use. Sealing was assured by rubber sheet. Connections between
wastewater using MFC.
two electrodes were made with copper wires through a rheostat
(0.19999 X).
3.2. Polarization curves of MFC

2.2. Culture and operation Polarization curves are useful for determining dependence on
resistance of fuel cell performance. To obtain the polarization
Anaerobic mixed consortia from Harbin beer brewery (China) curve, the current density was calculated and plotted against volt-
was used as inoculums in the anode chamber of MFC for electricity
generation. Diluted beer brewery wastewater, supplemented with
phosphate buffer solution (PBS) and other trace elements required
by microorganism growth (Lovley and Phillips, 1988), was used as 1.0
0.07
substrate. The characteristics of raw brewery wastewater are: pH,
-2
current density / A m

0.06
0.9
6.6 0.2; COD, 1680 400 mg/L; NH3-N, 19 10 mg/L; TN,
0.05 current density
27 12 mg/L; SS, 600700 mg/L.
0.8 0.04
Fuel cell was operated in continuous ow at room temperature
(24 4 C). Brewery wastewater, which was diluted by PBS (4.97 g/ 0.03

0.7
voltage / V

L NaH2PO4, 2.75 g/L Na2HPO4) at a COD range of 600660 mg/L, 0.02

80 100 120 140

was feed continuously by a peristaltic pump (Longer BT100-1 J, time / h

0.6 open-circuited-operation external resistance=9000
China) from the water inlet. The upow rate was controlled at
47 mL h1, corresponding to a hydraulic residence time (HRT) of 0.5
2.13 h. Efuent was collected with a beaker from the outlet.
0.4
2.3. Analytical methods
0.3
Voltage (U) yielded from MFC for long time operation was re-
corded automatically by a computer at an interval of three minutes 0.2
0 20 40 60 80 100 120 140
and converted to power density, according to P (W/
time / h
m3) = 1000U  j  A/0.1 or P (W/m2) = U  j, where j is current den-
sity (A/m2), which is calculated by j = U/(R  A) based on external Fig. 1. MFC performance during startup period [insert is the current density as a
resistance R (X) and projected surface area A (m2); 1000 is based function of time when 9000 X external resistance was applied].
 Q. Wen et al. / Bioresource Technology 100 (2009) 41714175 4173

0.6 12 Table 1
voltage(V) Substrate degradation at different external resistance.
activation -3
0.5 polarization power density(W m ) External resistance (X) 9000 500 100 70 60 20
10
Inuent COD (mg/L) 604 636 652 657 626 654
0.4 Efuent COD (mg/L) 344 372 387 391 358 380

power density / W m
8
COD removal amount (mg/L) 260 264 265 266 268 273
COD removal efciency (%) 43.0 41.5 40.6 40.5 42.8 41.7
voltage / V

0.3
6

ohmic loss that the reactor has a well ability and stability in wastewater treat-
0.2
4 ment in various conditions.
Coulombic efciency (CE) is shown in Fig. 3. As current density

0.1
0.0 concentation polarization
0.0 0.5 1.0 1.5
current density / A m
-2
Fig. 2. Voltage and power density generation as a function of current density.
age and power density at different external resistances (20
9000 X) (Fig. 2). Results showed a maximum power density of
9.52 W/m3 (264 mW/m2) at external resistance of 60 10 X. Cur-
rent decreased consistently with the increase in the resistance,
which is accordance with literatures reported earlier (Liu and Lo-
gan, 2004; You et al., 2006; Venkata-Mohan et al., 2008b).
It is evident from the experimental data that the voltagecur-
rent density curve can be roughly divided into three stages: activa-
tion polarization, ohmic loss and concentration polarization. At the
rst stage, current was relatively low, activation resistance caused
by reaction kinetics played a dominant role, which caused a rapid
voltage decrease. As current increased, polarization curve showed
a linear relationship between voltage and current, which is called
ohmic polarization, resulted from ionic resistance and electronic
resistance. In this phase, there was also non-ohmic polarization;
when external resistance was equal to internal resistance
(60 10 X), power density reached the maximum of 9.52 W/m3
(264 mW/m2). With continued increase of current density, concen-
tration diffusion became obvious.
3.3. The inuence of external resistance on MFC
3.3.1. Voltages at different external resistance
The voltages at different external resistance (1000, 500, 100, 70,
60 and 20 X) were recorded when MFC was controlled under sta-
ble phase for 6.05 h at each resistance (data not show). It was con-
cluded that voltage showed a consistent decreasing trend with
decrease in the external resistance. But the cell voltage is relatively
-3
2 increased, CE increased linearly. According to formula (1)
CE CC PT  100% FnItDSV  M (Liu et al., 2004) and data in Table
1, it can be seen that DS is nearly independent of R, thus the theo-
0
2.0 retical electricity production (CT) had a little change. But as current
increased, total electrons obtained (CP) in the experiment in-
creased, which resulted in an increasing CE. According to linear
t of this curve, it was found that the relationship between CE
and j is CE = 0.1298 + 8.3624  j, with a correlation coefcient of
0.9998.
A maximum CE of 19.75% was obtained at external resistance of
20 X, which is quite lower than CE of synthetic wastewater (Liu
and Logan, 2004; Venkata-Mohan et al., 2008b). There are many
possible reasons for such a low Coulombic efciency, such as the
complicated component of brewery wastewater (probably includ-
ing some other electron donors), oxygen diffusion to the wastewa-
ter, etc.
3.4. MFC modeling
3.4.1. Establishment of a model of MFC
For a fuel cell, the real voltage output could be written by start-
ing with the thermodynamically predicted voltage and then sub-
tracting the various overvoltage losses (Ryan et al., 2007):
V Ethermo  gact  gohmic  gconc 2
where V is operating voltage of fuel cell; Ethermo is thermody-
namically predicted voltage of fuel cell; gact, gohmic and gconc are
voltage losses due to reaction kinetics, ohmic polarization and
mass transport, respectively. Mathematically, the net fuel cell jV
behavior can be written as:
V Ethermo  aA bA  ln j  aC bC  ln j
  
jL
 j  S  Rohmic  c  ln 3
jL  j
20

stable at each external resistance, which showed that the reactor

had a well stability and can obtain sustainable electricity from
coulombic efficiency / %

brewery wastewater. Therefore, it can be concluded that MFC with 15

brewery wastewater can be operated in a long time period, thus
has a widely application prospect in practical projects. y=0.1298+8.3624x
r=0.9998
10
3.3.2. COD removal efciency and Coulombic efciency
MFC used for wastewater treatment, which resembles anaero-
bic suspended growth contact reactor, documented its capacity
in treating wastewater in association with power generation. Table 5
1 shows the results of wastewater degradation. In the experiment,
the hydraulic resistance time (HRT) was kept at 2.13 h and inuent
COD was controlled between 600 and 660 mg/L. Data showed that
0
as external resistance decreased, effective electron discharge was 0.0 0.5 1.0 1.5 2.0 2.5
obtained, hence COD absolute removal amount increased, but only current density / A m
-2

slightly, from 260.07 to 273.69 mg/L, COD removal efciency at dif-

ferent external resistance remained 4043%. This result indicated Fig. 3. Coulombic efciency as a linear function of current density.
4174 Q. Wen et al. / Bioresource Technology 100 (2009) 41714175
where gact = (aA + bA  lnj) + (aC + bC  lnj), represents activation
losses from both anode (A) and the cathode (C) based on natural
logarithm form of Tafel equation; gohmic = j  S  Rohmic is ohmic
resistance loss based on current density j, cross-sectional area S
and resistance Rohmic; gconc = c  ln[jL/(jL  j)] is combined fuel cell
concentration loss, where c is a empirical constant and jL is limiting
current density.
Formula (3) shows the theoretical equation of fuel cell, but in
reality, it is found that one additional term is usually needed to re-
ect the true behavior of most fuel cell systems. This additional
term, jleak, is associated with the parasitic loss due to current leak-
age, gas crossover and unwanted side reaction. jgross is used to ex-
press gross current density produced at the fuel cell electrodes; j is
the measured current density of the fuel cell. The relationship of
jgross, jleak and j can be expressed as:
J gross j jleak
In the fuel cell model, gact and gconc should be based on jgross since
the reaction kinetics and species concentrations are affected by the
leakage current. However, gohmic should be based on j, since only
the operating current of the fuel cell is actually conducted through
the cell. Thus, the model can be rewritten as follows:
V Ethermo  aA bA  lnj jleak   aC bC  lnj jleak 
 
jL
 j  S  Rohmic  c  ln
jL  jL jleak
In this experiment, because of the complicated composition of
brewery wastewater, Ethermo and jleak cannot be obtained. In order
to make it convenient for the establishment of model, the equation
is rewritten as follows:
V U  aA bA  ln j  aC bC  ln j  j  S  Rohmic
  
jL
 c  ln
jL  j
where U is the open-circuit voltage of MFC, which can be re-
garded as the voltage that without the loss of this system itself
and the effect of jleak. Hence, formula (6) is the nal model that
established for the MFC with brewery wastewater.
3.4.2. Non-linear t and analysis of polarization curve
According to the measurement, the open-circuit voltage U was
0.578 V, the cross-sectional area of electrode S was 0.0036 m2. So
the nal model became to:
V 0:578  aA bA  ln j  aC bC  ln j
  
jL
 0:0036  j  Rohmic  c  ln
jL  j
Formula (7) was used to make a non-linear curve t of the
polarization curve by Origin 7.5. The nal values of parameters
are given by the software directly: aA, 0.1090; bA, 0.0229; aC,
0.1148; bC, 0.0232; Rohmic (X), 7.3049; c (V), 0.1271; jL (A/m2),
2.0805.
In order to validate the creditability of the model and these
parameters, a test of electrochemical impedance spectroscopy
(EIS) of the MFC was carried out. Result showed that the ohmic
resistance was 7.160 X, which is close to that from the model, sug-
gesting that the model established for the MFC is reasonable.
Fig. 4 shows the results of the tting and analysis of various
voltage losses. The line down most is the tted curve; the one on
the top is the open-circuit voltage. The activation loss (including
anodic activation and cathodic activation), ohmic loss and concen-
0.6 open-circuit voltage
anodic active loss
0.5
0.4 cathodic active loss
voltage / V
0.3 ohmic loss
0.2 concentration loss
0.1
0.0 -2
j=1.79A m
0.0 0.4 0.8 1.2 1.6 2.0
4 -2
current density / A m
Fig. 4. Non-linear t of polarization curve and voltage losses analysis.
tration loss were calculated separately by those parameters ob-
tained from the t. It was found that all of the three losses were
increased as current density. Moreover, at low current density,
activation polarization was the most important limitation; as cur-
rent increased, concentration loss was observed gradually. At
5 j = 1.79 A/m2, concentration loss came up to activation loss, both
reached 0.248 V, while activation loss of anode and cathode were
0.119 and 0.129 V, respectively, indicated that the activation polar-
ization of anode and cathode differs a little. In the whole process,
ohmic loss, which was 0.046 V at current density of 1.79 A/m2,
was low; it was accordance with the low ohmic resistance
Rohmic = 7.3049 X from the model.
Thus, the primary factors which inuenced the performance of
MFC with brewery wastewater are kinetics loss and concentration
6
loss, how to reduce these two losses is the primary research focus.
There are four major ways to improve kinetic performance:
a. Increase the reactant concentration. For anode, increasing the
concentration of brewery wastewater is effective; while for
cathode, making MFC worked at a high pressure can increase
the gas concentration. But in real fuel cells, kinetic reactant
concentration effects generally work against this rule for
several reasons, which need deep research.
b. Decrease the activation barrier. A catalytic electrode can sig-
nicantly lower the activation barrier for the reaction.
Because activation barrier appears as an exponent, even
small decreases in it can cause large effects. Using a highly
catalytic electrode therefore provides a way to quite signi-
cant increase of kinetic performance.
7
c. Increase the temperature. By increasing the reaction temper-
ature, the thermal energy available in the system is
increased, which makes reactants obtain enough energy to
reach activated state. Temperature increase is also propi-
tious to anaerobic organisms, which has a better electricity
production environment.
d. Increase the number of possible reaction sites (i.e., increase the
reaction interface roughness). A rough electrode has quite lar-
ger surface area than smooth surface; it provides more sites
for reaction. Therefore, a rough electrode surface will be
more effective than a smooth one.
Besides reaction kinetics, concentration loss also is an impor-
tant issue of the MFC. The reactant depletion (and product accu-
mulation) affects fuel cell performance in two ways: Nerstian
losses and reaction losses. Increasing limiting current density jL
 Q. Wen et al. / Bioresource Technology 100 (2009) 41714175
can greatly extend a fuel cells potential operating range. jL can be
improved by two ways: one is increasing reactant concentration,
especially the pressure of oxygen; the other is to improve the ow
structure of MFC, scilicet, it is possible to improve MFC congura-
tion to decrease mass transport losses. In real fuel cells, mass trans-
port losses are minimized by employing intricate ow structures
containing many small ow channels, which mean corridor struc-
ture, can be applied in MFC. The ow structure often provides the
best opportunities for mass transport optimization, which need
deep research.
4. Conclusions
The feasibility of MFC in bioelectricity generation from brewery
wastewater was demonstrated. The open-circuit voltage and the
maximum power density reached 0.578 V and 9.52 W/m3
(264 mW/m2). COD removal efciency was always kept at 40
43% with a hydraulic residence time (HRT) of 2.13 h, which indi-
cated the stability of wastewater treatment in different conditions
of the MFC. The maximum Coulombic efciency of 19.75% was doc-
umented at external resistance of 20 X. Moreover, using the model
established based on polarization curve for the MFC, it was found
that the most important factors which inuenced the performance
of the MFC were reaction kinetic loss and mass transport loss (both
were 0.248 V when current density was 1.79 A/m2). There are
many effective methods to decrease these losses, for example,
increasing reactant concentration; employing more effective and
cheaper electrode catalysts; increasing reaction temperature;
employing rough electrode and improving the ow structure, etc.
Acknowledgements
The authors would like to thank Group of Heilongjiang Science
and Technology, Heilongjiang, China for funding the research and
Harbin Beer Brewery, Harbin, China for providing the sludge.
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