**Removal of COD by Two-Chamber Microbial Fuel Cells**

Katalin Belafi-Bako, Balazs Vajda, Peter Bakonyi and Nandor Nemestothy

Additional information is available at the end of the chapter

http://dx.doi.org/10.5772/58373

## **1. Introduction**

Microbial fuel cells (MFC) are regarded as special bio-electrochemical systems which seem to have a high potential in the future technology for energy production in the section of renewable green energy sources [1-5].

A classical MFC in general [4-8] consist of an anodic and cathodic chamber divided by a proton (cation) selective membrane (Figure 1). Microbes in the anodic cell – mostly attached to the electrode surface forming a biofilm – oxidize the substrates and generate electrons and protons in the process. Then electrons are transported from the anode to the cathode through an external circuit (wire) resulting measurable electric current. Meanwhile protons are passing through the membrane and enter the cathode cell where they combine with oxygen to form water.

MFC-s can be operated by either monoculture (e.g. *Geobacter sulfurreducens* [5], *Shewanella oneidensis, Lactococcus lactis* [9], *Lysinibacillus sphaericus* [10]) – where the electrogenic species release electron to the anode electrode directly or with the use of electroactive metabolites –, or multiculture (microbe consortia) system, which can be found in e.g. anaerobic sewage sludge acting in a similar way. The substrates of the MFCs operated by sewage sludge can be provided from various wastewaters, thus electricity generation in the MFCs can be coupled with the degradation of organic matters even e.g. wastewater treatment processes [11-20].

Many types of wastewaters were investigated (e.g. beer brewery wastewater [22], food industrial wastewaters [22, 23]) where the degradation can be followed by COD removal determination [14]. In MFCs applied for treatment of organic matters, the feed can be enriched with various substrates. It has been noted that non-fermentable substrates are superior to fermentable substrate as the electron donor for power output and electron recovery. E.g. it was reported that an acetate enriched MFC produced higher power output than a glucose enriched

© 2014 The Author(s). Licensee InTech. This chapter is distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

**Figure 2.** The main process streams in the factory

**2. Materials and methods**

was 50 cm2

cell by using wastewater from the sugar beet factory.

adapt the actual conditions and colonise locally.

K2Cr2O7+ 4H2SO4= K2SO4+ Cr2(SO4)3

In this project the aim was to find out how to work and operate a two chamber microbial fuel

A two-chamber MFC was used in the experiments (Figure 3). Both cells have a 240 cm3 volume, the membrane between them was a Nafion N115 proton selective membrane, its surface area

cell distilled water was used. Both electrodes were carbon cloth, their surface area was 50 cm2

The electrodes were connected via a resistor and the voltage data were continuously quantified by a parallel measuring system. It contained a 100 MΩ resistor and the voltage data were directly collected by a data acquisition device (National Instruments USB-6008/6009). The data were recorded by the LabVIEW program. Based on the voltage and resistance data the current values were calculated, thus the electric power (in mW units) was possible to provide. The cumulated electricity data were summarized (in mWh) taken into account the operating time.

The anaerobic sludge applied in the anodic cell was pretreated prior to usage, as it was reported [26]. The MFC was placed in a thermostated container, where the liquids in both cells were possible to circulate and stir. In the cathodic cell air was entered continuously by a pump to ensure aerobic environment, while N2 was sparged through the anodic cell to assure the anaerobic conditions. The MFC reactor was initially inoculated with the pretreated anaerobic sludge. Then the microbial consortia started to operate in the cell and they were allowed to

To follow the processes various analytical methods: pH, total solid substance (TSS), COD were applied. COD values of the samples taken from the cells were determined by the potassium dichromate method, which is based on the following oxidation reaction in acidic environment:

+ 4H2O + 3O

(from a local working biogas plant, initial COD value was 70 000 mg/dm3

and thickness was 125 µm. In the anodic cell a complex mesophilic anaerobic sludge

), while in the cathodic

Removal of COD by Two-Chamber Microbial Fuel Cells

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79

.

**Figure 1.** The scheme of a two-chamber microbial fuel cell

MFC [24, 25]. In contrast we found that certain carbohydrate substrates resulted in higher electricity generation [26]. Wastewaters from a sugar beet factory obviously consists of carbohydrates (mono-and/or disaccharides), which are probably suitable enrichments compounds for MFCs.

One of the application segments where extremely promising possibilities are visualised is the integration of the MFCs into wastewater treatment, since these systems are capable to consume organic material even from waste streams to produce power.

In Kaposvar (a city in Southern Hungary) there is a sugar factory, where saccharose (crystal‐ lized sugar) is produced from sugar beet [27]. It is an energy intensive process, thus the company has to make great efforts to optimise energy and resource usage, trying to apply environmentally sound, sustainable and waste minimising technologies, which cover water and air quality management as well as usage of by-products. Regarding air quality, the factory has taken extensive measure to decrease dust, smell and sound emissions in recent years, modern biofilters were installed. As to the water issue, special attention is payed to clean the wastewater streams generated during the manufacturing process. The by-products of the processes: the green leaves of sugar beet, the pressed slices (pulp) and other substances are used as components of fertilizers, soil conditioners and for other purposes.

In this factory the processing of all the by-product and waste streams is carefully designed and performed. The leadership of the factory felt responsibility to operate the plant according to environmental safe conditions, therefore they completed the sugar technology with compost‐ ing – to handle the green parts of the plant –, with a wastewater treatment plant and recently even a biogas fermenter was installed (Figure 2). Inserting microbial fuel cells into this system direct electric power could be produced by reduction of the COD from the waste streams.

**Figure 2.** The main process streams in the factory

In this project the aim was to find out how to work and operate a two chamber microbial fuel cell by using wastewater from the sugar beet factory.

## **2. Materials and methods**

MFC [24, 25]. In contrast we found that certain carbohydrate substrates resulted in higher electricity generation [26]. Wastewaters from a sugar beet factory obviously consists of carbohydrates (mono-and/or disaccharides), which are probably suitable enrichments

One of the application segments where extremely promising possibilities are visualised is the integration of the MFCs into wastewater treatment, since these systems are capable to consume

In Kaposvar (a city in Southern Hungary) there is a sugar factory, where saccharose (crystal‐ lized sugar) is produced from sugar beet [27]. It is an energy intensive process, thus the company has to make great efforts to optimise energy and resource usage, trying to apply environmentally sound, sustainable and waste minimising technologies, which cover water and air quality management as well as usage of by-products. Regarding air quality, the factory has taken extensive measure to decrease dust, smell and sound emissions in recent years, modern biofilters were installed. As to the water issue, special attention is payed to clean the wastewater streams generated during the manufacturing process. The by-products of the processes: the green leaves of sugar beet, the pressed slices (pulp) and other substances are

In this factory the processing of all the by-product and waste streams is carefully designed and performed. The leadership of the factory felt responsibility to operate the plant according to environmental safe conditions, therefore they completed the sugar technology with compost‐ ing – to handle the green parts of the plant –, with a wastewater treatment plant and recently even a biogas fermenter was installed (Figure 2). Inserting microbial fuel cells into this system direct electric power could be produced by reduction of the COD from the waste streams.

organic material even from waste streams to produce power.

**Figure 1.** The scheme of a two-chamber microbial fuel cell

78 Technology and Application of Microbial Fuel Cells

used as components of fertilizers, soil conditioners and for other purposes.

compounds for MFCs.

A two-chamber MFC was used in the experiments (Figure 3). Both cells have a 240 cm3 volume, the membrane between them was a Nafion N115 proton selective membrane, its surface area was 50 cm2 and thickness was 125 µm. In the anodic cell a complex mesophilic anaerobic sludge (from a local working biogas plant, initial COD value was 70 000 mg/dm3 ), while in the cathodic cell distilled water was used. Both electrodes were carbon cloth, their surface area was 50 cm2 . The electrodes were connected via a resistor and the voltage data were continuously quantified by a parallel measuring system. It contained a 100 MΩ resistor and the voltage data were directly collected by a data acquisition device (National Instruments USB-6008/6009). The data were recorded by the LabVIEW program. Based on the voltage and resistance data the current values were calculated, thus the electric power (in mW units) was possible to provide. The cumulated electricity data were summarized (in mWh) taken into account the operating time.

The anaerobic sludge applied in the anodic cell was pretreated prior to usage, as it was reported [26]. The MFC was placed in a thermostated container, where the liquids in both cells were possible to circulate and stir. In the cathodic cell air was entered continuously by a pump to ensure aerobic environment, while N2 was sparged through the anodic cell to assure the anaerobic conditions. The MFC reactor was initially inoculated with the pretreated anaerobic sludge. Then the microbial consortia started to operate in the cell and they were allowed to adapt the actual conditions and colonise locally.

To follow the processes various analytical methods: pH, total solid substance (TSS), COD were applied. COD values of the samples taken from the cells were determined by the potassium dichromate method, which is based on the following oxidation reaction in acidic environment:

K2Cr2O7+ 4H2SO4= K2SO4+ Cr2(SO4)3 + 4H2O + 3O

**Figure 3.** The picture of MFC used

The organic substances in the samples were ravaged in the presence of potassium dichromate and catalysts (AgSO4, HgSO4) in sulphuric acid solution at 145 o C. The absorbance of the chromium (III) ions from the reduction of K2CrO7 during the oxidation process was determined by a spectrophotometer (Hach LANGE DR 3900) at 600 nm. The COD values of the samples were calculated using a calibration curve taken in the range of 750 – 4000 KOI mg/cm3 .

**Figure 4.** Power generation using model waste water

**Table 1.** Changes of COD values using model waste stream

**Table 2.** TSS and pH values using model waste stream

are summarised in Tables 1 and 2.

Samples were taken regularly and the COD values, pH and TSS were determined. The data

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81

**Time (h) COD (mg/dm3) COD decrease (%)** Adding substrate End of period 1-192 19800 4900 75 192-336 7150 2775 61 336-480 5025 3075 39 480-650 5325 1810 66 650-880 4060 1250 69

**Time (h) pH TSS (g/dm3)** 1 6.70 35.9 192 8.25 3.9 336 7.65 1.9 480 7.55 1.6 650 7.05 1.1 880 4.45 0.9

## **3. Results**

#### **3.1. Experiments with model wastewater**

To test the behaviour of the MFC, model substrates were used for the experiments. The composition of the model mixture – similar to the waste stream of the sugar beet factory – was carbohydrates (0.6 %) and inorganic substances (ash, 3 %).

The MFC operation was started by inoculation with the pretreated anaerobic sludge, then the processes were followed by recording the voltage data continuously (Figure 4). A 10 Ω resistor was used in the circuit. After certain intervals 100 cm3 fresh substrate was added (marked by the arrows) to the system to maintain the carbohydrate concentration. These additions mean 9000 mg/cm3 COD input each.

The voltage data have shown that the substrate addition enhanced the power generation and quite high voltage (current density) values were achieved (in the range of 10 and 24 mV).

**Figure 4.** Power generation using model waste water

The organic substances in the samples were ravaged in the presence of potassium dichromate

chromium (III) ions from the reduction of K2CrO7 during the oxidation process was determined by a spectrophotometer (Hach LANGE DR 3900) at 600 nm. The COD values of the samples were calculated using a calibration curve taken in the range of 750 – 4000 KOI mg/cm3

To test the behaviour of the MFC, model substrates were used for the experiments. The composition of the model mixture – similar to the waste stream of the sugar beet factory – was

The MFC operation was started by inoculation with the pretreated anaerobic sludge, then the processes were followed by recording the voltage data continuously (Figure 4). A 10 Ω resistor

the arrows) to the system to maintain the carbohydrate concentration. These additions mean

The voltage data have shown that the substrate addition enhanced the power generation and quite high voltage (current density) values were achieved (in the range of 10 and 24 mV).

C. The absorbance of the

fresh substrate was added (marked by

.

and catalysts (AgSO4, HgSO4) in sulphuric acid solution at 145 o

**3. Results**

**Figure 3.** The picture of MFC used

80 Technology and Application of Microbial Fuel Cells

9000 mg/cm3

**3.1. Experiments with model wastewater**

carbohydrates (0.6 %) and inorganic substances (ash, 3 %).

was used in the circuit. After certain intervals 100 cm3

COD input each.

Samples were taken regularly and the COD values, pH and TSS were determined. The data are summarised in Tables 1 and 2.


**Table 1.** Changes of COD values using model waste stream


**Table 2.** TSS and pH values using model waste stream

As it can be seen remarkable TSS and COD decrease could be observed during the processes, while electric power was generated continuously. The drop in the pH at 880 h has shown that the operation of the MFC should be ceased due to the unfavourable biochemical processes. The values of current density, J (normalized to the 50 cm2 carbon cloth electrode) and power density (calculated from the current density and voltage data; Pa and Pm, normalized to the surface of the carbon cloth electrode and the membrane surface area, respectively), moreover the cumulated energy data ∑P (taken into account the time period of the experiment) are summarized in Table 3.


**Table 3.** Results obtained using model waste stream

The values have shown that notable power density was achieved during the operation and finally altogether more than 10 thousands mWh/m2 energy was generated by consuming the organic substances from the model waste water in the MFC.

Now the MFC was operated by a 330 Ω resistance built in the circuit, which was considered as a more effective operation condition point according to the polarization curve. The adapted microbial consortium was used to inoculate the cell. After certain intervals 100 cm3 fresh substrate (wastewater) was added (marked by the arrows) to the system. In Figure 6 the voltage data obtained in the MFC by the waste water from the sugar beet factory are presented.

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83

**Figure 5.** The variance of the voltage and power density in different resistances

**Figure 6.** Power generation using industrial waste water from Kaposvar

#### **3.2. Polarization curve**

Our next purpose was to determine the polarization curve using the adapted microbe consortia (grown up in the experiments by the model wastewater). Therefore a serial of experiments were carried out applying various resistances (in the range of 5 and 500 Ω) built in the system and the voltage/current data were measured (Figure 5). Moreover the power density values were calculated.

It can be seen from the figure that voltage data decreased gradually as higher resistances were installed into the system up to 12 mA current, thus the MFC was in a stationer state in the given range from electrochemical point of view. With the growing resistance values, however, increasing power density values were possible to achieve, which mean that it is advisable to use higher resistances for the further measurements. The results shown in the Figure are similar as reported in literature [22].

#### **3.3. Experiments with industrial wastewater**

Wastewater from the sugar factory in Kaposvar was used in the next experiments of our work. It consisted of carbohydrates (others than saccharose: mainly glucose and fructose; altogether 0.6 %) and ash 3 %. The other features of the waste water were: pH 5.4, TSS 34.8 g/dm3 and COD value 12 075 mg/dm3 .

**Figure 5.** The variance of the voltage and power density in different resistances

As it can be seen remarkable TSS and COD decrease could be observed during the processes, while electric power was generated continuously. The drop in the pH at 880 h has shown that the operation of the MFC should be ceased due to the unfavourable biochemical processes. The values of current density, J (normalized to the 50 cm2 carbon cloth electrode) and power density (calculated from the current density and voltage data; Pa and Pm, normalized to the surface of the carbon cloth electrode and the membrane surface area, respectively), moreover the cumulated energy data ∑P (taken into account the time period of the experiment) are

**Time (h) J (mA/m2) Pa (mW/m2) Pm (mW/m2)** ∑**P (mWh/m2)** 1-192 260 3.380 4.023 649.0 192-336 416 8.652 10.300 1245.9 336-480 220 2.420 2.880 4114.0 480-650 240 2.880 3.428 4896.0 650-880 300 4.500 5.357 1035.0

The values have shown that notable power density was achieved during the operation and finally altogether more than 10 thousands mWh/m2 energy was generated by consuming the

Our next purpose was to determine the polarization curve using the adapted microbe consortia (grown up in the experiments by the model wastewater). Therefore a serial of experiments were carried out applying various resistances (in the range of 5 and 500 Ω) built in the system and the voltage/current data were measured (Figure 5). Moreover the power density values

It can be seen from the figure that voltage data decreased gradually as higher resistances were installed into the system up to 12 mA current, thus the MFC was in a stationer state in the given range from electrochemical point of view. With the growing resistance values, however, increasing power density values were possible to achieve, which mean that it is advisable to use higher resistances for the further measurements. The results shown in the Figure are similar

Wastewater from the sugar factory in Kaposvar was used in the next experiments of our work. It consisted of carbohydrates (others than saccharose: mainly glucose and fructose; altogether 0.6 %) and ash 3 %. The other features of the waste water were: pH 5.4, TSS 34.8 g/dm3 and

summarized in Table 3.

82 Technology and Application of Microbial Fuel Cells

**3.2. Polarization curve**

were calculated.

as reported in literature [22].

COD value 12 075 mg/dm3

**3.3. Experiments with industrial wastewater**

.

**Table 3.** Results obtained using model waste stream

organic substances from the model waste water in the MFC.

Now the MFC was operated by a 330 Ω resistance built in the circuit, which was considered as a more effective operation condition point according to the polarization curve. The adapted microbial consortium was used to inoculate the cell. After certain intervals 100 cm3 fresh substrate (wastewater) was added (marked by the arrows) to the system. In Figure 6 the voltage data obtained in the MFC by the waste water from the sugar beet factory are presented.

**Figure 6.** Power generation using industrial waste water from Kaposvar

The changes of COD values of the samples were determined and summarized in Table 4, while the TSS and pH data are shown in Table 5.

decreased sharply, showing that the biochemical processes in the MFC have not been working

Removal of COD by Two-Chamber Microbial Fuel Cells

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85

A two-chamber MFC was designed and built in our laboratory where carbon cloth (fibres) were used as electrodes and Nafion 0125 protonselective membrane was placed between the two cells. Pretreated anaerobic sludge from a local biogas plant was applied in the anode chamber. Experiments with model and industrial wastewaters from a sugar beet factory were carried out to study the efficiency and stability of the system and to measure the electric power generated. It has turned out that it was possible to generate bioelectricity from the particular wastewater and the power data obtained were found similar or higher to the data published in literature, i.e. comparable performance was achieved in our MFC system. Our next purpose is to study the MFC for longer term operation, even in continuous mode of operation, so that

This work was supported by the European Union and co-financed by the European Social Fund in the frame of the TAMOP-4.2.2.A-11/1/KONV-2012-0071 and TÁMOP-4.2.2.A-11/1/ KONV-2012-0038 projects; and the János Bolyai Research Scholarship of the Hungarian

, Balazs Vajda, Peter Bakonyi and Nandor Nemestothy

[3] Y. Mohan, S.N. Muthu Kumar, D. Das: Electricity generation using microbial fuel

\*Address all correspondence to: bako@almos.uni-pannon.hu

cells, Int. J. Hydrogen En. 33 (2008) 423-426

[1] B.E. Logan: Microbial fuel cells, Wiley & Sons, New York, 2008

University of Pannonia, Veszprem, Hungary

[2] www.microbialfuelcell.org

we can insert the MFC into the processing scheme of the sugar beet factory [28].

properly any longer, thus the operation was ended.

**4. Conclusion**

**Acknowledgements**

Academy of Sciences.

**Author details**

Katalin Belafi-Bako\*

**References**


**Table 4.** Changes of COD values using waste water from the factory


**Table 5.** TSS and pH values using industrial wastewater

The values of current density, power density – which are higher here than in case of model waste water due to the higher resistance – and the cumulated energy data ∑P are listed in Table 6.


**Table 6.** Results obtained using industrial waste stream

The current and power density values were outstanding compared to literature data [20-22] or the values obtained with the model wastewater. Altogether more than 60 thousands mWh/ m2 energy was generated during the over 800 hour operation. In the last interval (after 840 hour) the substrate addition did not result in any increase of voltage data, moreover the pH decreased sharply, showing that the biochemical processes in the MFC have not been working properly any longer, thus the operation was ended.

## **4. Conclusion**

The changes of COD values of the samples were determined and summarized in Table 4, while

**Time (h) COD (mg/dm3) decrease of COD (%)**

**Time (h) pH TSS (g/dm3)** 1 8.1 34.8 330 8.0 10.8 600 7.6 3.2 840 7.1 2.5 1000 4.1 4.2

The values of current density, power density – which are higher here than in case of model waste water due to the higher resistance – and the cumulated energy data ∑P are listed in

**Time (h) J (mA/m2) Pa (mW/m2) Pm (mW/m2)** ∑**P (mWh/m2)** 1-330 181 52 59.5 17 160 330-600 242 95 113 25 650 600-840 245 99.2 118.2 23 808 840-1000 51 4.2 5.0 642

The current and power density values were outstanding compared to literature data [20-22] or the values obtained with the model wastewater. Altogether more than 60 thousands mWh/

 energy was generated during the over 800 hour operation. In the last interval (after 840 hour) the substrate addition did not result in any increase of voltage data, moreover the pH

Adding substrate End of period 1-330 21850 13850 37 330-600 13673 5225 62 600-840 7795 3875 50 840-1000 7975 5900 26

the TSS and pH data are shown in Table 5.

84 Technology and Application of Microbial Fuel Cells

**Table 4.** Changes of COD values using waste water from the factory

**Table 5.** TSS and pH values using industrial wastewater

**Table 6.** Results obtained using industrial waste stream

Table 6.

m2

A two-chamber MFC was designed and built in our laboratory where carbon cloth (fibres) were used as electrodes and Nafion 0125 protonselective membrane was placed between the two cells. Pretreated anaerobic sludge from a local biogas plant was applied in the anode chamber. Experiments with model and industrial wastewaters from a sugar beet factory were carried out to study the efficiency and stability of the system and to measure the electric power generated. It has turned out that it was possible to generate bioelectricity from the particular wastewater and the power data obtained were found similar or higher to the data published in literature, i.e. comparable performance was achieved in our MFC system. Our next purpose is to study the MFC for longer term operation, even in continuous mode of operation, so that we can insert the MFC into the processing scheme of the sugar beet factory [28].

## **Acknowledgements**

This work was supported by the European Union and co-financed by the European Social Fund in the frame of the TAMOP-4.2.2.A-11/1/KONV-2012-0071 and TÁMOP-4.2.2.A-11/1/ KONV-2012-0038 projects; and the János Bolyai Research Scholarship of the Hungarian Academy of Sciences.

## **Author details**

Katalin Belafi-Bako\* , Balazs Vajda, Peter Bakonyi and Nandor Nemestothy

\*Address all correspondence to: bako@almos.uni-pannon.hu

University of Pannonia, Veszprem, Hungary

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## *Edited by Chin-Tsan Wang*

Faced with the upcoming serious deficiency of energy, food and water, along with inevitable environmental pollution, much related research has been on the upsurge because Microbial Fuel Cells (MFCs) seem to be one of the solutions to these concerns in the future. The aim of this book is to describe and consider some concepts regarding MFC application designs for interested colleagues. Five topics regarding the technology of flow control, biocatalysts, biofilms, removal of chemical oxygen demand and biochemical fields are addressed in the book. Considering the low power density and short life span of MFCs, there has been a dramatic increase in funding and research that has led to a greater understanding of the fundamental science behind MFC study. This is driving significant improvements in both the reliability and efficiency of MFCs and hence their future use.

Photo by wongwean / Shutterstock

Technology and Application of Microbial Fuel Cells

Technology and Application

of Microbial Fuel Cells