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Transcript of Electricity Generation in a Membrane-less
Accepted Manuscript
Electricity generation in a membrane-less microbial fuel cell with down-flow
feeding onto the cathode
Feng Zhu, Wancheng Wang, Xiaoyan Zhang, Guanhong Tao
PII: S0960-8524(11)00576-1
DOI: 10.1016/j.biortech.2011.04.062
Reference: BITE 8408
To appear in: Bioresource Technology
Received Date: 20 February 2011
Revised Date: 18 April 2011
Accepted Date: 19 April 2011
Please cite this article as: Zhu, F., Wang, W., Zhang, X., Tao, G., Electricity generation in a membrane-less microbial
fuel cell with down-flow feeding onto the cathode, Bioresource Technology (2011), doi: 10.1016/j.biortech.
2011.04.062
This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers
we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and
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1
Electricity generation in a membrane-less microbial fuel cell
with down-flow feeding onto the cathode
Feng Zhu, Wancheng Wang, Xiaoyan Zhang, Guanhong Tao*
College of Chemistry, Chemical Engineering and Materials Science, Soochow
University, Suzhou, Jiangsu 215123, China
* Corresponding author. Tel: +86 512 65226517; fax: +86 512 65223409; E-mail
address: [email protected] (G. Tao)
2
Abstract
A novel membrane-less microbial fuel cell (MFC) with down-flow feeding was
constructed to generate electricity. Wastewater was fed directly onto the cathode
which was horizontally installed in the upper part of the MFC. Oxygen could be
utilized readily from the air. The concentration of dissolved oxygen in the influent
wastewater had little effect on the power generation. A saturation-type relationship
was observed between the initial COD and the power generation. The influent flow
rate could affect greatly the power density. Fed by the synthetic glucose wastewater
with a COD value of 3500 mg/L at a flow rate of 4.0 mL/min, the developed MFC
could produce a maximum power density of 37.4 mW/m2. Its applicability was further
evaluated by the treatment of brewery wastewater. The system could be scaled up
readily due to its simple configuration, easy operation and relatively high power
density.
Keywords: microbial fuel cell; membrane-less; down-flow; air cathode; oxygen
diffusion
3
1. Introduction
A microbial fuel cell (MFC) is a device that uses microorganisms to convert
chemical energy from biodegradable substrates to electrical energy via
microbial-catalyzed redox reactions (Logan et al., 2006; Du et al., 2007; Oh et al.,
2010). Electrons and protons are generated during the oxidization of substrates by
microorganisms. The generated electrons flow from the anode via an external circuit
to the cathode, where they typically combine with protons and oxygen to form water.
Electricity is thus produced and harnessed by inserting a load between the two
electrodes. This provides MFCs promising potentials to generate renewable electricity
while accomplishing the biodegradation of organic matters or wastes when they are
assembled and integrated in wastewater treatment process. Therefore, MFCs have
attracted great attentions in recent years.
It has been reported that the construction of the microbial reactor in MFCs is an
important factor that affects the performance and further application of MFC (He et
al., 2006; Li et al., 2009; Liu and Logan, 2004). The most commonly reported MFCs
consist of an anode chamber and a cathode chamber separated by a proton exchange
membrane (PEM) (Oh et al., 2004; You et al., 2006; Fornero et al., 2008). However,
the so-called dual-chamber MFCs possess some inherent disadvantages, such as the
high cost of PEM, the potential for bio-fouling and associated high internal resistance
(Liu and Logan, 2004; Liu et al., 2008). In order to overcome these disadvantages,
single–chamber MFCs without PEM have been developed (Min et al., 2005; Jang et
al., 2004). The omission of PEM significantly simplifies the configuration and
4
reduces the cost and the internal resistance. In the membrane-less MFCs, oxygen is
often used as the terminal electron acceptor. Compared to the other electron acceptors
such as potassium ferricyanide and potassium permanganate (You et al., 2006; Oh et
al., 2004), oxygen can be freely available in the air and readily reduced on the cathode.
Therefore, the so-called air-cathode MFCs can reduce the cost and improve
sustainability.
In the air-cathode MFCs, the power density is often constrained by the oxygen
reduction rate on the cathode. It is caused by the low solubility of oxygen in the
aqueous cathodic solution and its subsequent availability at the cathode. To enhance
the efficiency of oxygen utilization, cathodes are often treated by coating a catalyst
(Yang et al., 2009; Lefebvre et al., 2009; Zhang et al., 2009). Air aeration in the
cathodic area is also used to increase the oxygen concentration (Ghangrekar et al.,
2007; Aldrovandi et al., 2009; Luo et al., 2009). Fornero et al. (2008) constructed a
MFC with pressurized cathodic chamber to increase the solubility of oxygen. Li et al.
(2009) reported an overflow-type wetted-wall MFC with a tubular cathode chamber to
improve the oxygen utilization.
However, in the membrane-less air-cathode MFCs, oxygen can diffuse from the
cathode area to the anode chamber as removing PEM. Oxygen diffusion into the
anode chamber can result in a loss of electron donor and thus lowering overall
Coulombic efficiency (CE) (Liu and Logan, 2004). In order to restrain the oxygen
diffusion, some modifications have been made on the configuration of the
membrane-less air-cathode MFCs. Fan et al. (2007) used a cloth between the anode
5
and cathode to reduce the oxygen diffusion rate. You et al. (2007) developed a MFC
with graphite-granule anode and tubular air-cathode. Aldrovandi et al. (2009) and Hu
(2008) designed a baffle-chamber reactor to improve the CE. Li et al. (2009)
combined a tubular anode chamber reactor and a baffle-chamber reactor together. Yet,
particularly due to their reactor and electrode designs, these systems are still somehow
complicated, making it difficult to be scaled up.
In the present study, a new single-chamber membrane-less air-cathode MFC was
constructed. The top of the single-chamber MFC was open to air. Inexpensive
graphite plates were used as the electrodes without catalyst-coating treatment.
Wastewater was fed directly onto the graphite cathode which was horizontally placed
just above the water surface, and flowed out from the bottom of the MFC. It is the
most significant difference from the previously reported MFCs, in which wastewater
was fed from the bottom of the MFCs (Jang et al., 2004; Rabaey et al., 2005). The
MFC developed in this study was referred as down-flow MFC. The goal of the
present study was to develop a MFC with simple and inexpensive configuration which
could be easily scaled-up. The feasibility of continuous electricity generation using
this down-flow MFC and factors affecting its performance were investigated.
2. Materials and Methods
2.1. MFC construction
The scheme of the down-flow single-chamber MFC is shown in Fig. 1. A
6
cylindrical glass tube was used to construct the MFC. The inner diameter of the tube
was 6 cm and the height was 30 cm, with a working volume of about 850 mL. The top
of the MFC was open to air. A rectangle anode (10×4×0.5 cm) was vertically inserted
into the anaerobic activated sludge at the bottom of the MFC and a circular cathode
with a diameter of 5.6 cm and a thickness of 0.5 cm was horizontally placed on the
support in the upper part of the MFC. About half of the cathode was kept above the
liquid level. Both anode and cathode were made from graphite plates (Wangnian
Graphite Factory, Jiangsu, China) without catalyst-coating treatment. The effect of the
distance between the cathode and anode on the power production was investigated.
The graphite electrodes were connected with copper wire coming out of the glass tube
to provide the connection points for the external circuit. All the connection points
were sealed with epoxy resin. The anode and cathode were connected via an external
variable resistor. A plastic tube was connected to the conical bottom of the MFC so
that the liquid level in the chamber could be adjusted by raising or lowering the outlet
of the plastic tube. An overflow port was opened on the wall of glass chamber about
2.5 cm down from the top.
2.2. Inoculation and operation
The MFC was inoculated with anaerobic activated sludge collected from the
up-flow anaerobic sludge bed reactor in our laboratory, which has been run for over
one year to treat synthetic glucose wastewater. It was filled with 200 mL of the
anaerobic sludge, reaching a concentration of ca. 10.0 g/L for volatile suspended
7
solids. After the MFC was inoculated with synthetic wastewater for half a month in a
batch operating mode, the down-flow feeding was used. Wastewater was introduced
continuously onto the air cathode and flowed out from the bottom of the MFC at a
fixed flow-rate of 4.0 mL/min using a peristaltic pump (BT100-100M, Longer
Precision Pump, China). A water bath was used to maintain the temperature of the
MFCs at 30±1oC. The system was considered to be operating under stable conditions
when the power production reached stable for at least 10 hrs.
The anode and the cathode were connected via an external resistor. The voltage
(V) on the external resistor was monitored with a data acquisition system and
converted to the power density, P (W/m2) according to P=V2/(RA), where R is the
external load and A is the submerged area of the cathode, which is 26.0 cm2 in this
study. The current density (Id) was calculated as Id=I/A, where I is the current and A is
the submerged area of the cathode.
In order to compare the present system with the previously reported MFC system
with up-flow feeding (Ghangrekar et al., 2007; Jang et al., 2004; Rabaey et al., 2005),
another MFC with the same configuration was operated in parallel using the same
conditions except that the wastewater was introduced from the bottom of the MFC
and flowed out from the top.
Synthetic glucose wastewater was used to investigate the effect of affecting
factors on the performance of the developed MFC because of its simple and constant
composition. It contained (per liter of tap water) 3.95 g glucose, 0.38 g NH4Cl, 0.015g
FeSO4•7H2O, 0.026g MgSO4, 0.019 g CaCl2, 0.76 mg NiSO4•6H2O and 9.36 g NaCl.
8
A phosphate buffer solution (50 mM) was used to adjust its pH to 7.0. Wastewater
collected from a local brewery was used to evaluate the applicability of the developed
system. The characteristics of the brewery wastewater were: pH, 4.65; COD, 2850
mg/L; NH3-N, 45.3 mg/L; TN, 67.2 mg/L; TP, 22.7 mg/L; SS, 725 mg/L. Its pH was
adjusted to 7.0 with sodium carbonate powder and phosphate buffer. Same amounts of
trace elements required by microorganism growth and NaCl were added as did in the
synthetic wastewater. During the application test, the MFC was first fed with brewery
wastewater diluted with the synthetic glucose wastewater (1:1) and run for 7 days.
Then the brewery wastewater was introduced until the MFC reached stable.
3. Results and discussion
3.1. Electrical power production and polarization
As shown in Fig. 2, the down-flow MFC could successfully produce a stable
power density of 30.0 mW/m2, i.e. an output voltage of 153 mV at a fixed external
load of 300 �, 11 hrs after its operation. The power density was twice higher than that
achieved by the MFC using up-flow feeding, which was 14.6 mW/m2. This
comparison was made under the same conditions that the DO concentration in the
feeding wastewater was about 3.0 mg/L and air aeration was not used in the cathode
area for both feeding modes.
For the down-flow MFC, the DO concentration in the feeding wastewater had
little effect on power output, which will be discussed later in Section 3.2. However,
9
for the up-flow feeding, as shown in Fig. 2, the power density was increased from
14.6 to 18.7 mW/m2 after the feed was deoxygenated with nitrogen purging. This was
because that the DO in the feed could lead to the non-productive redox reaction of
organic carbon oxidation coupled with oxygen reduction in the anode biofilm (Liu et
al., 2004). The reaction was minimized when the feed was deoxygenated, resulting
higher power output.
In the air cathode MFCs, DO concentration in the cathode area played a
significant role in power production (Fornero et al., 2008; An et al., 2009). When the
up-flow feeding was used, the DO concentration in the cathode area became very low
(0 to 1.2 mg/L) after it passed through the MFC from the bottom. The low DO
concentration restrained the oxygen reduction rate on the cathode, resulting in low
power density (An et al., 2009). Several measures were reported to improve the
efficiency of oxygen utilization (Li et al., 2009; Ghangrekar et al., 2007; Aldrovandi
et al., 2009). Air aeration in the cathode area that was commonly used in the previous
studies (Aldrovandi et al., 2009; Luo et al., 2009) was adopted in the present study
with up-flow feeding. As shown in Fig. 2, the power density was increased to 33.2
and 24.0 mW/m2 when aeration was used in the up-flow MFC with and without
deoxygenation, respectively.
As shown in Fig. 2, the down-flow MFC could achieve higher power output than
the up-flow MFC without the deoxygenation of the feed or aeration in the cathode
area, and almost the same power output as the up-flow MFC with deoxygenation and
aeration. It showed the superiority of the down-flow MFC to its up-flow counterpart
10
thanks to its simple configuration and easy operation.
In order to investigate the performance of the down-flow MFC, the output
voltages under various external loads from 0 to 15000 � were recorded and the
polarization curve was obtained. As shown in Fig. 3, the power density increased with
the decrease of external resistance and a maximum power density of 30.0 mW/m2 was
reached with the external resistance of 300 �, corresponding to a current density of
196 mA/m2. The maximum power density was higher than that obtained by using
up-flow feeding mode in this study (14.6 mW/m2) and that achieved in a similar MFC
configuration reported by Ghangrekar et al (2007) (10.13 mW/m2). It is also shown in
Fig. 3 that the power density was declined with the decrease of external resistance
lower than 300 �. The results suggested that the electron transfer through the external
circuit to the cathode be the limiting factor for power production at higher external
loads.
3.2. Effect of dissolved oxygen concentration on power production
It was reported that DO concentration in the cathode area played a great role in
power density in the air cathode MFCs (Fornero et al., 2008). In the present study
with down-flow feeding, the effect of DO concentration in wastewater on power
production was investigated and the results are shown Fig. 4. Yet, the initial DO
concentration in wastewater did not affect the power production significantly in the
present study. It was revealed in Fig. 4 that the DO concentration in the cathode area
had become almost the same after the wastewater was fed dropwise onto the cathode.
11
Oxygen in air could be dissolved readily into the wastewater while it was fed
dropwise onto the cathode. The DO concentration reached to 6.0 to 6.3 mg/L at room
temperature of 25 oC. The oxygen-saturated wastewater (8.25 mg/L) also reached to
that DO level by releasing oxygen to air when it entered the MFC. Therefore the
initial DO concentration in wastewater had little effect on the power production in the
present study. It made the present system simpler than the previous systems due to the
omission of air-aeration while high power density could still be achieved.
3.3. Effect of distance between anode and cathode on power generation
The position of cathode was adjusted to investigate the effect of the distance
between the cathode and the top of the anode on power generation. Three different
distances, i.e. 5, 10 and 15 cm were evaluated. The highest power density of 37.4
mW/m2 was obtained with the distance of 10 cm. The maximum power densities were
22.3 and 30.0 mW/m2 for the distances of 5 and 15 cm. The internal resistances were
135, 210 and 300 � for the distances of 5, 10 and 15 cm, respectively. For the
distance of 15 cm, the internal resistance was increased, resulting in a lower power
output. Although shorter electrode distance reduced the internal resistance, the
diffusion of oxygen to the anode area increased. It was observed that the DO
concentration of effluent was 2.5±0.3 mg/L for the distance of 5 cm, which was
higher than those (1.5±0.2 and 1.2±0.2 mg/L) for the distances of 10 and 15 cm. The
decline of power generation for the distance of 5 cm would be attributed to the
diffusion of oxygen to the anode. Therefore the spacing of 10 cm was used for the
12
further study.
3.4. Effect of influent flow rate on power production
To examine the effect of wastewater feeding rate on power production, the flow
rate was increased from 0.8 to 8.0 mL/min. An external resistor of 210 � was used for
the investigation. As shown in Fig. 5, when the flow rate was increased from 0.8 to
4.0 mL/min, the power density increased from 19.4 to 37.4 mW/m2 and the internal
resistance decreased from 395 to 210 �. With the increase in flow rate, the boundary
layer over the electrode surface became thinner and thus the mass transfer to the
electrodes was enhanced, resulting in lower internal resistance and therefore higher
power output. Another possible explanation for this increase might be the
enhancement of electrochemical activity of the bacteria by an increase in the rate of
mass transport. (Di Lorenzo et al., 2009). Yet, further increasing the flow rate to 8.0
mL/min resulted in the decrease of the maximum power density to 25.9 mW/min. The
possible explanation might be that oxygen diffusion to the anode area at higher flow
rates became more straightforwardly, causing the loss of electron donor and thus
lowering the power density.
3.5. Effect of COD on power generation
The effect of COD value in wastewater on power generation was investigated in
the range of 875 to 4000 mg/L. As shown in Fig. 6, power density increased with the
increase in COD concentration. The power generation as a function of initial COD
13
concentration showed a saturation-type relationship in the investigated range. The
power density was modeled as a function of COD concentration using the
Monod-type equation (Kovar and Egli, 1998). The maximum power density in the
equation for this hyperbola was 45.9 mW/m2 with a half-saturation constant of 1638
mg/L. The observation was consistent with the results reported in previous studies
regardless of the cell configuration and substrates (Min et al., 2005; Li et al., 2009; Li
et al., 2008).
3.6. Effect of ionic strength on power generation
Ohmic loss was one of the main causes for the decrease of power generation in a
MFC system (Liu et al., 2008; Liu et al., 2005). It could be reduced by increasing the
electrical conductivity in the cell. In this study, NaCl was added to adjust the ionic
strength, and thus the electrical conductivity. With the increase of NaCl concentration
from 0 to 0.16 M, the power density increased rapidly. Further increase of ionic
strength from 0.16 to 0.32 M had a negligible effect on the power density, indicating
that the ionic strength was not a limiting factor beyond 0.16 M. Therefore 0.16 M of
NaCl was added in the synthetic wastewater in the present study.
3.7. Application of the developed system
The developed MFC system was applied to the treatment of the wastewater from
a local brewery. A maximum power density of 19.8 mV/m2, i.e. 104 mV was achieved
after it was run for three weeks. It showed the feasibility for the application of the
14
system to real wastewater treatment. The study on the scaling up of the system was
currently conducting on a reactor with a volume of 25 L. in which wastewater was fed
onto the cathode with a shower nozzle-like distributor.
4. Conclusions
The feasibility of the down-flow MFC with air cathode in electricity generation
was demonstrated. Oxygen could be utilized directly from the air with the downward
feeding of wastewater onto the cathode. Factors such as electrode spacing, influent
flow rate and COD concentration affected significantly the power production while
DO concentration didn’t. A maximum power density of 37.4 mW/m2 was produced
from the MFC fed by synthetic wastewater with a COD value of 3500 mg/L. The
system was characterized by simple configuration, easy operation and relatively high
power density. It was successfully applied to the treatment of brewery wastewater.
Acknowledgements
This research is partially supported by National Natural Science Foundation of
China (Project Nos. 20345006 and 20575043).
15
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19
Figure Captions
Fig. 1. Schematic diagram of the down-flow MFC used in the study.
Fig. 2. MFC performance using different feeding mode. The distance between the two
electrodes was 15 cm. The external load was 300 �. Other conditions are specified in
Section 2.
Fig. 3. Power density and voltage as function of current density. Same operating
conditions were used as shown in Fig. 2.
Fig. 4. Effect of DO in influent wastewater on power density. Same operating
conditions were used as shown in Fig. 2.
Fig. 5. Effect of feeding rate on power production and internal resistance. The
distance between the two electrodes was 10 cm. Other conditions are specified in
Section 2.
Fig. 6. Effect of influent COD concentration on power density. Same operating
conditions were used as shown in Fig. 5.
Oxygen was utilized readily from air while wastewater feeding onto the cathode.
DO did not affect power generation while COD, flow rate and electrode spacing
did.
Maximum power density was twice as high as that obtained by up-flow feeding.
Readily to be scaled up due to its simple configuration and easy operation.