Discharge of wastewater containing traces of cow dung from a dairy farm poses significant threat to the environment, which necessitates the effluent treatment. Microbes present in organic rich dairy effluent containing traces of cow dung produced electricity. The performance of Microbial Fuel Cell(MFC) was analyzed by drawing I-V curves and performing electrochemical impedance spectroscopy (EIS). The MFC produced maximum power density of 203 mWm-2 at a current density of 1191 mAm-2. The Chemical Oxygen Demand (COD) removal efficiency was found to be 81% after 10 days of MFC operation. Decrease in anode polarization resistance confirmed the formation of biofilm at anode surface.
Research
Simultaneous Power Generation and Dairy Effluent treatment Using Microbial Fuel Cell
https://doi.org/10.21203/rs.3.rs-285485/v2
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published 15 Mar, 2023
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Nation`s development and prosperity are largely based on energy [1]. Electricity production from renewable energy resources such as solar, biomass, hydel and wind is insufficient to meet the present industrial, agricultural or transportation demand, thereby utilization of conventional energy resources coal, gas, oil is allowed to meet the new technological applications [2]. The utilization of fossil fuels has increased the presence of harmful gases (CO2, NOx, and SOx) and other volatile organic matter in the atmosphere which contributes towards global warming, eutrophication, and acid rain causing severe environmental and health issues for man and aquatic life [3]. Rising energy demand in Pakistan due to industrial growth and population has increased the utilization of fossil fuels posing significant threats to the environment [4]. World is moving towards low carbon energy resources to mitigate the effects of climate change [5]. An Increase in the carbon emission level in 2017, despite the decline in coal consumption per year, shows that the current renewable energy may be an addition to the global energy mix. A sustainable decrease in the utilization of conventional energy resources requires innovation in renewable energy technologies [6], [7]. Rapid depletion of fossil fuels and the environmental damage caused by them have stimulated the exploration of new energy sources [8]. Researchers are well focused on sustainable energy production from low carbon energy technologies. Currently, The largest contributor to the renewable energy sector in the USA is bioenergy, which constitutes 44.4% of renewable energy consumption [9], [10].
Wastewater from industries and sewage is the main source of water pollution, which causes water-borne diseases such as hepatitis, diarrhea, giardiasis, and cholera [11]. Water pollution has negative impacts on human health and aquatic life being the major cause of morbidity and mortality around the globe. Improved health outcomes have observed by the treatment of wastewater [12]. The dissolved organics present in wastewater requires its treatment before it is discharged to the environment. Wastewater is considered as a renewable source for the production of electricity, chemicals, and fuels.
MFC is a bioreactor that converts chemical energy, present between chemical bonds of an organic compound, into electrical energy [13] through microorganisms under anaerobic conditions [14]. This MFC operation differs bioremediation, which is the conversion of chemical and simple organic compounds to H2O and CO2 under aerobic conditions [15]. The history of MFC dates back to 1911 when potter generated electricity through microbes using platinum as electrodes [16]. The energy crisis shifted focus towards renewable energy generation [17] and it was found that use of mediators, proper design, and suitable electrode material can significantly increase power density and wastewater treatment efficiency [18]. Microbial fuel cell gives lower power density as compared to the well- established fuel cell technology. The later uses methanol and hydrogen as fuel [19] but its application in wastewater treatment is promising in saving energy [20]. Industrial Revolution has largely increased the complexity of wastewater [21] which necessitates the use of versatile technology like MFC for its treatment. MFC technology can treat the wastewater ranging from a simple or defined substrate (sucrose, glucose protein) to complex or undefined substrate such as domestic and municipal, pharmaceutical, brewery, dairy, food processing, agro-processing livestock, petroleum, paper recycling industry, and the list is no more exhaustive. Another advantage of MFCs over other treatment technologies is that it can also treat diluted wastewater [22], [23]. Integration of anaerobic digestion with MFCs can establish synergy between the two processes resulting in enhanced energy recovery, pollutant removal and resource recovery from high strength waste water [24]. Recently MFC technology is emerging for the treatment of wastewater other than waste treatment technologies such as anaerobic digestions and aerated lagoon that require energy input for their operations. Some MFC designs do not require external energy or pump for aeration, resulting in the net output of energy. Removal rates achieved with the help of MFC technology are comparable to those achieved in industrial wastewater management systems notably without large energy consumptions. Microbial fuel cells remove COD and BOD up to 90% and release lesser sludge in comparison with other bioprocesses, thus, resulting in ultimate cost reduction for sludge disposal [25], [26].
Components and configuration of MFC:
MFCs face limitations such as high capital cost, low power densities, and a lack of larger-scale applications [27], [28]. In recent years, various anode, cathode, membrane materials and MFC configurations have been developed to overcome the shortcomings of the MFC technology [29]. The performance of MFCs is greatly influenced by the metabolism, electron transfer mechanism, and type of separator such as salt bridge and Proton exchange membrane used [30]. There is three vital components in an MFC namely, cathode, anode, and separator [31]. A single chamber MFC does not require any separator [32], [33]. The purpose of a separator in a double chamber MFC is to separate the cathode and anode chambers, transfer protons from anode towards the cathode compartment, block air leakage that is provided for oxygen reduction reaction (ORR) reaction at cathode[34]. Salt bridge made from KCL and agar solution has been reported [35], [36]. Different proton exchange membranes such as Nafion is reported, but a problem like high cost, leakage of oxygen, bio-fouling, and accumulation of charges affect the performance of MFC[37]. The choice of anode and cathode materials depends on characteristics like chemical stability, biological compatibility, low resistance, and mechanical strength. Surface morphology, material types, and anode area are factors that determine the biofilm formation, rate of electron transfer, power density, as well as COD removal efficiency [38].
Working of MFC:
Oxidation of substrate in wastewater generates electrons and protons. Electrons from the external circuit reach at the cathode where they combine with oxygen and proton to complete the circuit and electricity is generated in this way [39]. Three types of electron transfer mechanism have been reported:
a) Direct electron transfer at the anode surface through outer membrane cytochromes to carry out respiration [40].
b) Electron transfer by shuttling of electrons between anode surface and mediators [41]and
c) Electron transfer through solid or semi-solid conductive material, known as nanowires [42].
MFC materials:
In MFCs practical applications, electrodes account for lager share in MFC capital cost. Therefore, the identification of less expensive and catalytically effective electrodes can improve the cost-effectiveness and performance of MFC at the site [43]. Carbon based anodes being less expensive and biologically compatible are widely used in different configurations like mesh, granules, brush, sheets or rods. Carbon clothe[44], graphite fiber brush[45], carbon foam[46], carbon-nano tubes [47], and graphene-based electrodes [48] has been reported in MFC to give good results. Use of metal anodes has also been studied. Stainless steel has been reported suitable for larger-sale application and longer operation due to good conductance and mechanical stability [49]. Platinum being an expensive metal is far from an appropriate material in scale up applications [49]. Anode modifications with polymers and metal oxides have been employed to enhance performance of MFC [50][51]. Cathode is also an important part of MFC. The main reaction that occurs at cathode is oxygen reduction reactions, which can be increased using platinum and platinum-based catalyst [52]. Bio cathodes due to low cost and better conductivity has extensively been employed in MFCs [53].
MFC being a bio-electrochemical device activation and concentration resistances predominate due to microbial activities [54] Internal resistance as well contribution of different components can individually be determined but the earlier method largely based on ohm law or current interruption method can`t evaluate the kinetics involved in microbial fuel cell[55]. Formation of biofilm lowers the activation resistance in carbon-based electrodes as compared to metal electrodes which require a coating of a layer of catalyst to perform better [56]. The low power density of MFC is due to ohmic and polarization losses [57]. The electrochemical impedance spectroscopy (EIS) can be employed to understand and quantify various aspects of MFC operation such as [58]
- Formation of biofilm on the anode surface.
- Ohmic resistance, charge transfer or polarization resistance, the kinetics of electron transfer
- Impedance due to diffusion
- Identification of the type of bacteria
- Properties of electrode material
Fitting EIS spectra with an electrical equivalent circuit give the value of resistances, capacitances and impedance due to diffusion and reactions [59].
Mediator and mediator-less MFCs
Non-conductive lipid layers present at the outer portion of the majority of microbial species inhibit direct electron transfer to the anode surface. Therefore, an electron mediator is used to accelerate the electron transfer rate. The best mediator can be identified for achieving high-performance MFC, based on redox potential difference [60]. Oxygen reduction reaction (ORR), which requires high reduction potential, can affect the performance of MFC. To overcome this problem mediators can be used which not only helps in the electron transfer mechanism but also reduces reduction potential at cathode [61][62]. Toxicity, diffusion towards anode compartment and increased cost limits its use in MFC [63], [64]. In mediator free MFCs electrochemically active bacteria transfer electrons directly to electrodes [65]–[67]. Shewanella Putrefactions, Aeromonas hydrophilia, Geobacter and others are among the electrochemically active bacteria [68][69]–[72]. To increase the ORR reaction and proton conductivity different electrolytes such as phosphate buffer saline solution, potassium ferricyanide, potassium phosphate, and potassium permanganate phosphate buffer solution has been employed [73]–[75].
Rapid development of livestock in developing countries has increased the share of 45.5% of dairy manure and it is increasing every passing year. Cow dung contains nutrients (nitrogen, phosphorous, protein, organic matters), if not disposed properly can cause water eutrophication and environment pollution. Pathogens and protozoa present in dairy manure can cause diseases, if discharged untreated in to fresh water bodies[76], [77]. The present study demonstrated the dual application: treatment of dairy effluent and electric power generation. Moreover, EIS gave an insight view of the various components of the resistance involved and their contribution to overall impedance of MFC. MFC performance in terms of power generation can improve by minimizing the internal resistance component.
2.1 Materials and Construction:
Two containers made of plastic with volume capacity 300 mL each was separated by the heterogeneous anionic AMI-7001 (US international) ion exchange membrane as shown in Figure 1 . Anode chamber was filled with 250 mL cow dung and sugar solution. Anodic solution was prepared in the lab by mixing 10 g cow dung and 10 g sugar in 1000 ml of distilled water; to get initial COD value of 4520 mgL-1 distilled water was added to dilute anolyte. Anode in the form of disc having surface area 12 cm2 was made with carbon paste in Lab. Carbon paste was prepared by mixing 45 g of graphite, 25 g of activated carbon, and 30 g of paraffin oil(used as binder) in mortar and castle. Electrodes were washed with the ethanol solution to remove any impurities present. The anode was placed in anodic chamber provided with inlet and outlet port and container was sealed to create anaerobic conditions. Both electrodes were connected with copper wire through an external resistor. Cathode was filled with 250 mL of phosphate buffer Saline solution (PBS). PBS was prepared by adding 0.2 g of KCL, 0.8 g of NaCl, 1.44 g of Na2HPO4 , and 0.24 g of KH2PO4 in 800 mL of distilled water and to make a total solution volume of 1000 mL more distilled water was added [78]. PH of PBS solution was adjusted at 7.4 with HCL. Buffer solutions are widely used in MFCs due to their property to maintain constant PH. Cathode, slightly larger than anode area (15 cm2), was placed in cathode chamber. The larger area of cathode favors oxygen reduction reaction (ORR) at cathode chamber. Aeration was provided in cathode chamber by a fish pump. MFC cycle was run in batch mode for 10 days at room temperature.
2.2. Analysis and Calculations:
Electrochemical impedance spectroscopy (EIS) was performed using Gamry 1000 Interface. Present study characterizes the MFC with two-electrode mode system in which the cathode acts as both counter as well as reference electrode. A sinusoidal potential of magnitude 10 mV between a frequency range of 0.05 Hz to 100 kHz was applied using Gamry Potentiostat. The dynamic response of the cell was obtained in the form of Nyquist and Bode plots. The results of EIS were fitted to an electrical equivalent circuit using Gamry Echem Analyst.
The internal losses were calculated using 
Where
Rap= Anode polarization resistance and Rcp = cathode polarization resistance
I-V curves were drawn using Gamry Potentiostat. I-V curves were obtained with an applied current range of 0 to 0.002 ampere at a scan rate of 0.005 As-1. The system was given sometime to restore equilibrium after drawing current. Power density was calculated by dividing product of current and potential with total area of anode.
PH of the electrolyte was calculated electrometrically using Hanna instrument.
Microbial fuel cell finds its best application in wastewater treatment, a method proposed for wastewater treatment. Treatment performance of a microbial fuel cell can be evaluated in terms of COD removal rates. COD is an index of water quality and for wastewater; it measures how much fuel has been converted into electrical energy. Chemical oxygen demand of electrolyte was measured using high range COD vials (HI-937540). 0.2 mL of waste water solution was put into COD vial and placed in COD test tube heater for 120 minutes at 150 0C. After this COD was measured using Hanna photometer instrument.
COD removal efficiency was measured using the formula:
CODi = Chemical oxygen demand of influent
CODf = Chemical oxygen demand of effluent.
3.1. Chemical analysis of the dairy effluent
The cell was operated for a period of 10 days. Chemical properties like chemical oxygen demand (COD) and pH of the anolyte solution were measured before and after the cell operation. The initial COD value was found to be 4520 mg L-1 which on utilization by microorganisms decreased to 850 mg L-1 after 10 days, thereby giving percentage removal of 81% which is in reasonable agreement with the performance of MFC operated with domestic and sewage waste water [80] [81]. The pH of the anolyte decreased from 7.62 to 5.8 which indicates a strong shift from near neutral to the acidic behavior. Such behavior was expected as electrochemical oxidation creates an acidic environment inside the solution.
3.2. OCV and polarization study
Figure 1 shows the change in cell voltage for sample with initial COD value of 4520 mg/L. It is found that the cell voltage gradually increases at the start to a maximum value of 0.396 V on the third day and then drops. The gradual increase in the voltage at the start is attributed to ……………………… and decline may be due to the utilization of organic matter present in the sample. The OCV of 0.396 V is comparable with the reported value and indicates the metabolism of organic matter by microorganisms and formation of biofilm on the carbon-based electrode.
Figure 2 shows the polarization curve. A linear decrease in the cell voltage is observed which suggests a strong influence of the ohmic resistance on the cell performance. The maximum power density is found to be 140 mWm-2 which is higher than the value as reported for domestic waste water [80], however lower than that of distillery waste water [82]. A comparison of the results found in this study with the reported literature is provided in Table 1.
Table 1: Comparison of results of current study with the literature
|
Substrate |
Anode/Cathode |
OCVmax (V) |
COD removal Efficiency (%) |
Power Density (mWm-2) |
Reference |
|
Dairy effluent |
Carbon Paste/Carbon Paste |
0.396 |
82 |
140 |
Present |
|
Soak liquor |
Graphite/Graphite |
0.76 |
94 |
44 |
[79] |
|
Domestic waste water |
Carbon fiber brush/carbon fiber brush |
0.2 |
78 |
92 |
[80] |
|
Sewage waste water |
Graphite Rod/Graphite Rod |
0.18 |
82.7 |
6.73 |
[81] |
|
Distillery waste water |
Graphite Plate/Graphite Rod |
0.68 |
71.8 |
202 |
[82] |
|
Brewery waste water |
Carbon brush fibers / Activated carbon and PTFE with Pt catalyst |
0.51 |
20.7 |
669 |
[83] |
|
Cheese whey |
Carbon paper/carbon cloth |
N.A |
94 |
46 |
[84] |
3.3. Electrochemical impedance Spectroscopy (EIS):
Impedance spectroscopy was performed to study the dynamic response of the electrodes. Figure 4 shows Nyquist plots for three selected days (Day 3, Day 7, and Day 10). The corresponding Bode plot for day 3 is shown in Figure 5. Two clearly distinct curves can be identified; first at higher frequency (between 1 MHz and 100 Hz) and second at lower frequency (between 100 Hz and 0.05 Hz). The higher frequency curve is attributed to the charge transfer process whereas lower frequency curve is attributed to the diffusional process[ANT1] . The curve at lower frequency in Figure 4 corresponds to nearly 45 degree angle which is clear indication of the diffusional process. Such process is expected from the highly porous structure of the electrodes made of carbon paste.
3.4. Equivalent circuit model fitting
In order to deconvolute the impedance spectra, an equivalent circuit model of the form Rs(R1CPE2) (R2CPE3W) is developed as shown in Figure 4. Owing to the distributed capacitance response, the constant phase element is used in the model instead of pure capacitor. Rs refers to the ohmic resistance, R1CPE2 to the higher frequency charge transfer process, and R2CPE3W refers to the low frequency diffusional process.
The results of Electrical Equivalent circuit Fitting are as follow:
1. The solution resistance remains in the range 280.8 ohms to 316 ohms obtained from Nyquist plot. The solution resistance did not show any significant trend from day 1-10 as shown in Figure 6. The total bulk resistance i.e. sum of the solution as well as polarization resistances is 687.8 ohms. The solution resistance measured is less than or comparable with already measured values reported in literature.
2. Anode polarization showed a continuous decreasing trend from day 3 to day 10. The resistance at day 3 was 76 ohm and 46 ohm at day 10 as shown in Figure 7 . It is due to the formation of biofilm at anode surface, which helped in electron transfer mechanism between anode-electrolyte interfaces. Anode polarization resistance dominates the solution resistance dominates with time. The increase in Y02 parameter to 6.94E-4 and a2 of .543 at day 10 confirms the formation of biofilm at anodic surface and CPE element is moving towards ideal capacitor with time. Anodic capacitance is correlated with the anodic resistance. The value of anode capacitance at day 3, calculated from CPE elements, is 1.5386 µF, which has increased to 35.02 µF at day 10. The increase in capacitance and decrease in anode polarization resistance with time shows the formation of biofilm[85], which effectively utilized the organic matter present in the anolyte and generated electricity.
3. No significant trend is observed from day 3 to day 7 of cathode polarization resistance, but value drastically increased to 537 ohm at day 10 Figure 8. During this period, no aeration was provided and increase in cathode polarization resistance is due to accumulation of charges and slow oxygen reduction reaction at anode due to limited supply of oxygen[86], resulting in increase in resistance. No significant trend is observed for cathode capacitance.
4. The Warburg resistance is gives an increasing trend with time in Figure 9. The resistance is due to the accumulation of the hydronium ions at cathode. When hydrogen are transferred from anode to cathode, they get hydrated because cathode is much diluted solution resulting in the formation of hydronium ions, which gets reduced to give hydrogen at cathode and decreased performance of MFC[87].
The results of the electrical equivalent circuit fitting are shown in the Table 2.
Table 2: Results of Electrochemical impedance spectroscopy
|
Day |
R1 |
R2 |
R3 |
Y02 |
a2 |
Y03 |
a3 |
W3 |
|
3 |
280.8 |
76.5 |
330.8 |
3.06E-4 |
.415 |
2.13E-6 |
0.5 |
5.43E-3 |
|
7 |
316 |
54 |
345.7 |
4.06E-4 |
.54 |
3.69E-6 |
.404 |
6.49E-3 |
|
10 |
280.8 |
48 |
537.8 |
6.49E-4 |
.543 |
1.71E-7 |
.44 |
7.94E-3 |
The discharge of untreated dairy effluent containing traces of cow dung pollutes the environment. The present study dealt with remediation of cow dung and sugar solution and simultaneous power generation. The designed MFC produced a maximum power density of 203mWm-2 at a current density of 1191 mAm-2.In addition to this 81 % COD removal efficiency and 23%, change in PH is observed. Thereby this study demonstrated the dual application i.e. treatment of wastewater and electricity generation. Moreover electrochemical impedance spectroscopy gave an insight view of individual resistances and their contributions to overall impedance of MFC.
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Graphical Abstract
