CN110729487A - Microbial fuel cell based on molybdenum disulfide composite material as anode - Google Patents
Microbial fuel cell based on molybdenum disulfide composite material as anode Download PDFInfo
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
A high-performance microbial fuel cell based on a molybdenum disulfide composite material as an anode comprises an anode chamber and a cathode chamber, the maximum liquid filling volume of which is 20mL, and a double-chamber microbial fuel cell adopting a sandwich structure, wherein the two chambers are separated by a cation exchange membrane. The invention passes through MoS2The electrochemical performance of the carbon material is obviously improved by the modification of the nano material, and the MoS is shown by a test of a double-chamber microbial fuel cell2The modification of the nano material enables the internal resistance of the MFCs taking the carbon cloth as the anode to be reduced by 43 percent, the power to be improved by 60 percent, and the average coulombic efficiency to be 2.86 times that of the blank carbon cloth as the anode MFCs; the MoS can be further improved by compounding the conductive polymer2The conductivity of the/carbon cloth electrode material, the reduction of charge transfer resistance and the improvement of electrocatalytic activity, and the whole invention is based on the molybdenum disulfide composite materialThe material anode has low price, simple preparation and easy batch production, and can greatly reduce the operation cost of the microbial fuel cell.
Description
Technical Field
The invention relates to a microbial fuel cell, in particular to a high-performance microbial fuel cell based on a molybdenum disulfide composite material as an anode.
Background
Microbial Fuel Cell (MFCs) technology is a new type of device that can both treat wastewater containing organic pollutants and recover energy simultaneously. The basic principle is that in the anode chamber, microbe is used as catalyst to decompose organic matter under anaerobic condition, the produced electrons are transferred via external circuit, the produced protons are transferred to the cathode chamber via ion exchange membrane, and in the cathode, oxidant (electron acceptor) reacts with the arriving electrons and protons to produce reduction product. Because of good social and economic benefits, the method becomes a research hotspot in recent years.
However, the current battery has low output power density, which limits the wide application. The anode is a carrier attached to microorganisms and a current collector responsible for transferring electrons out, and the anode material plays an important role in the performance of power output of the MFCs and the like. The development of an anode material with good electrocatalytic performance, large specific surface area, high conductivity and good biocompatibility is one of the main strategies for improving the output power density of the MFCs.
Carbon materials are common anode materials because of the advantages of good conductivity, wide sources, low cost and the like, however, carbon elements have higher surface energy states and are easy to lose electronic reducibility, electrons need higher energy if the electrons directly jump to the surface of the carbon materials, so that the activation overpotential of an anode is larger, and the biocompatibility of the pure carbon materials is often poor. Therefore, the surface of the carbon material is subjected to various treatments and different nano materials are modified to increase the specific surface area of the anode and reduce the energy state, so that the activation overpotential and the like can be reduced, and the positive effect on the improvement of the power is achieved.
Disclosure of Invention
The invention aims to provide a high-performance microbial fuel cell based on a molybdenum disulfide composite material as an anode, wherein a molybdenum disulfide nano material modified carbon material is adopted as the composite anode of the microbial fuel cell to improve the output power density of the microbial fuel cell.
In order to achieve the purpose, the invention provides the following technical scheme:
a high-performance microbial fuel cell based on a molybdenum disulfide composite material as an anode adopts a sandwich type double-chamber structure comprising an anode chamber and a cathode chamber, and the anode chamber and the cathode chamber are separated by a cation exchange membrane;
the cathode chamber is used for storing cathode liquid, and the cathode immersed in the cathode liquid is carbon paper or carbon cloth;
the anode chamber is used for storing anolyte, and an anode immersed in the anolyte is molybdenum disulfide/carbon cloth or conductive polymer/molybdenum disulfide/carbon cloth (here, "/" refers to an interface existing between two different substances in a composite material, such as molybdenum disulfide/carbon cloth, and indicates that molybdenum disulfide grows on the carbon cloth, and "conductive polymer/molybdenum disulfide/carbon cloth, indicates that molybdenum disulfide grows on the carbon cloth, and conductive polymer is loaded on molybdenum disulfide.)
The catholyte stored in the cathode chamber was a pH-neutral PBS buffer solution (10.0 g/L sodium bicarbonate, 11.2g/L disodium hydrogen phosphate) containing 50mmol/L K3[Fe(CN)6]。
The anode is molybdenum disulfide/carbon cloth or conductive polymer/molybdenum disulfide/carbon cloth, and anolyte is stored in the anode chamber. The anolyte is PBS buffer solution (10.0 g/L sodium bicarbonate, 11.2g/L disodium hydrogen phosphate) with neutral pH, and contains 10.0g/L anhydrous glucose, 5 g/L yeast extract and 0.8707 g/L2-hydroxy-1, 4-naphthoquinone (HNQ). The conductive polymer is molybdenum disulfide/carbon cloth which is also compounded with polyaniline, polypyrrole or polythiophene. In general, the maximum liquid-holding volumes of the anode chamber and the cathode chamber are both 20 mL.
Further, the preparation method of the molybdenum disulfide composite anode comprises the following steps: :
s1: ultrasonically cleaning a carbon cloth sold in the market for half an hour by using acetone, ethanol and deionized water in sequence, and then drying for later use;
s2: putting the cleaned carbon material into a solution containing 0.5-1.5 g of thiourea, 1.0-1g of sodium molybdate, 0.2-0.6 g of P123 and 30-70 mL of deionized water, carrying out hydrothermal reaction for 4-6 hours at the temperature of 200 ℃ in a high-pressure reaction kettle, naturally cooling, then washing with the deionized water, and drying to obtain the grown MoS2Carbon material of nanomaterial.
Further, the preparation method of the composite polyaniline conductive polymer comprises the following steps:
s1: in the presence of 0.1mol L-1And 1mol L of aniline-1In the sulfuric acid solution, an electrode with hydrothermally grown molybdenum disulfide/carbon cloth is used as a working electrode;
s2: using Pt electrode as counter electrode and calomel electrode as reference, electroplating by cyclic voltammetry with scanning potential range of-0.2V-0.9V and scanning speed of 10mV s-1The number of scanning turns is 6-20.
Compared with the prior art, the invention has the beneficial effects that:
1. the invention passes through MoS2The electrochemical performance of the carbon material is obviously improved by the modification of the nano material, a certain direct catalytic performance to substrate glucose is shown, and the maximum catalytic oxidation peak current of the carbon material in a solution containing the substrate glucose and an electron transfer mediator is 2.7 mA/cm2Far higher than that of blank carbon cloth by 0.37 mA/cm2。
2. The invention shows that MoS is prepared by testing the double-chamber microbial fuel cell2The modification of the nano material enables the internal resistance of the MFCs taking the carbon cloth as the anode to be reduced by 43 percent, the power to be improved by 60 percent, and the average coulombic efficiency to be 2.86 times that of the blank carbon cloth as the anode MFCs.
3. The invention can further improve MoS by the polymerization of polyaniline PANI2The conductivity of the carbon cloth electrode material reduces the charge transfer resistance and improves the electrocatalytic activity.
4. PANI/MoS of the invention2/carbon cloth asThe maximum power density and internal resistance of the battery of the anode MFCs are 42.13 Wm-3(135 omega) is far superior to 22.12W m of PANI/carbon cloth-MFC single material-3(180. OMEGA.), and MoS227.97W m for/carbon cloth-MFC-3(210 omega), therefore, the anode based on the molybdenum disulfide composite material is low in price, easy to produce in batches, capable of greatly reducing the running cost of the microbial fuel cell, simple to prepare and good in application prospect.
Drawings
FIG. 1 shows a blank carbon cloth and a MoS-loaded carbon cloth according to the present invention2A cyclic voltammetry curve of carbon cloth of a nano valve in anolyte;
FIG. 2 is a plot of a polarization for various anode microbial fuel cells of the present invention; b power density graph;
FIG. 3 shows the PANI/carbon cloth, MoS, of the present invention2Carbon cloth and PANI/MoS2A cyclic voltammogram of carbon cloth in anolyte;
FIG. 4 shows the PANI/carbon cloth, MoS, of the present invention2Carbon cloth and PANI/MoS2A polarization curve of the carbon cloth anode microbial fuel cell; b power density plot.
Detailed Description
The technical solution of the present invention will be clearly and completely described below with reference to the embodiments of the present invention and the accompanying drawings. It is to be understood that the described embodiments are merely exemplary of the invention, and not restrictive of the full scope of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
In the embodiment of the invention: a high-performance microbial fuel cell based on a molybdenum disulfide composite material as an anode is provided, wherein the preparation method of the molybdenum disulfide composite anode comprises the following steps: ultrasonically cleaning commercially available carbon cloth (not limited to carbon cloth, carbon paper, carbon felt and other carbon materials) by acetone, ethanol and deionized water for half an hour, and drying for later use; washing carbon material, and placing the carbon material in a container containing 0.5-1.5 g of thiourea, 1.0-1g of sodium molybdate, 0.2-0.6 g of P123 and30-70 mL of deionized water, performing hydrothermal reaction in a high-pressure reaction kettle at the temperature of 150-2Carbon material of nanomaterial.
In order to further increase the conductivity of the material, another embodiment of the present invention further includes compounding a conductive polymer such as polyaniline, polypyrrole, or polythiophene on the molybdenum disulfide/carbon material prepared above.
The preparation method of the composite Polyaniline (PANI) conductive polymer comprises the following steps: in the presence of 0.1mol L-1And 1mol L of aniline-1In the sulfuric acid solution, an electrode in which molybdenum disulfide/carbon cloth grows hydrothermally is used as a working electrode, a Pt electrode is used as a counter electrode, a calomel electrode is used as a reference, cyclic voltammetry is used for electroplating, the scanning potential range is-0.2V-0.9V, and the scanning speed is 10mV s-1The number of scanning turns is 6-20.
In conclusion, the high-performance microbial fuel cell based on the molybdenum disulfide composite material as the anode is a double-chamber microbial fuel cell, a sandwich structure is adopted, the maximum liquid filling volumes of an anode chamber and a cathode chamber are both 20mL, and the anode chamber and the cathode chamber are separated by a cation exchange membrane; wherein the cathode is carbon paper or carbon cloth, and the catholyte is pH neutral PBS buffer solution (10.0 g/L sodium bicarbonate, 11.2g/L disodium hydrogen phosphate) containing 50mmol/L K3[Fe(CN)6](ii) a The anode is molybdenum disulfide/carbon cloth or conductive polymer/molybdenum disulfide/carbon cloth, and the anolyte is PBS buffer solution (10.0 g/L sodium bicarbonate, 11.2g/L disodium hydrogen phosphate) with neutral pH and contains 10.0g/L anhydrous glucose, 5 g/L yeast extract and 0.8707 g/L2-hydroxy-1, 4-naphthoquinone (HNQ).
Referring to fig. 4, based on the above cell structure, the start-up and power density polarization curves of the cell were determined: putting 18 mL of anolyte into a reactor, introducing high-purity nitrogen for 15 minutes, putting 2 mL of escherichia coli bacterial liquid into the reactor after the gas is introduced, and plugging an opening at the upper end of the reactor by using a rubber plug to enable the reactor to be in a sealed state; after the open-circuit voltage of the battery is stable, different resistors are sequentially loaded on the battery, and the system automatically records the voltage value, the power density and the current density output when the resistors are loaded at different loads.
The tests show that: (1) MoS2The modification of the nano material enables the internal resistance of MFCs based on carbon cloth as the anode to be reduced by 43 percent and the power to be improved by 60 percent; the average coulombic efficiency is 2.86 times that of the blank carbon cloth which is used as the anode MFCs; (2) polymerization of Polyaniline (PANI) may further enhance MoS2The conductivity of the carbon cloth electrode material reduces the charge transfer resistance and improves the electrocatalytic activity; (3) PANI/MoS2The maximum power density and the internal resistance of the battery with/carbon cloth as the anode MFCs are 42.13W m-3(135 omega) far superior to 22.12W m of PANI/carbon cloth-MFC single material-3(180. OMEGA.), and MoS227.97W m for/carbon cloth-MFC-3（210 Ω）。
Therefore, the anode based on the molybdenum disulfide composite material is low in price and easy to produce in batches, and therefore the operation cost of the microbial fuel cell can be greatly reduced.
In order to further and better verify the invention, the following specific embodiments are also provided:
example 1:
MoS2study of electrocatalytic performance of/carbon cloth:
the first step is as follows: MoS2Preparation of carbon cloth: ultrasonically cleaning commercial carbon cloth with acetone, ethanol and deionized water for half an hour in sequence, and then drying for later use; MoS2The synthesis of the nano valve on the carbon cloth is carried out by putting the carbon cloth (2.5 cm multiplied by 5 cm) into the solution containing 0.9 g thiourea, 0.450 g sodium molybdate, 0.4 g P123 and 60 mL deionized water, hydrothermal reacting at 200 deg.C for 3-6 h in high pressure reactor, naturally cooling, washing with deionized water, drying to obtain the product2A carbon cloth of a nano material;
the second step is that: and testing the electrocatalytic performance.
MoS prepared as above2And measuring a cyclic voltammogram in anolyte by using carbon cloth as a working electrode, Ag/AgCl as a reference electrode and a platinum wire as a counter electrode.
Example 2:
MoS2research on microbial fuel cells with carbon cloth as the anode:
in MoS2The carbon cloth is taken as an anode, and the blank carbon paper is taken as a cathode; MoS2The carbon cloth anode was prepared as in example 1.
The cell adopts a sandwich structure, the maximum liquid filling volumes of an anode chamber and a cathode chamber are both 20mL, and the anode chamber and the cathode chamber are separated by a cation exchange membrane; the anolyte is PBS buffer solution (10.0 g/L sodium bicarbonate, 11.2g/L disodium hydrogen phosphate) with neutral pH, and contains 10.0g/L anhydrous glucose, 5 g/L yeast extract and 0.8707 g/L2-hydroxy-1, 4-naphthoquinone (HNQ); the catholyte was a pH-neutral PBS buffer solution (10.0 g/L sodium bicarbonate, 11.2g/L disodium hydrogen phosphate) containing 50mmol/L K3[Fe(CN)6]。
Starting of the cell and determination of the power density polarization curve: putting 18 mL of anolyte into a reactor, introducing high-purity nitrogen for 15 minutes, putting 2 mL of escherichia coli bacterial liquid into the reactor after the gas is introduced, and plugging an opening at the upper end of the reactor by using a rubber plug to enable the reactor to be in a sealed state; after the open-circuit voltage of the battery is stable, different resistors are sequentially loaded on the battery, and the system automatically records the voltage value, the power density and the current density output when the resistors are loaded at different loads.
Example 3:
PANI/MoS2study of a microbial fuel cell with carbon cloth as anode:
the synthesis method of PANI/MoS 2/carbon cloth is as follows: with PANI/MoS2The carbon cloth is taken as an anode, and the blank carbon paper is taken as a cathode; in the presence of 0.1mol L-1And 1mol L of aniline-1In the sulfuric acid solution, carbon cloth with hydrothermally grown molybdenum disulfide is used as a working electrode, a Pt electrode is used as a counter electrode, a calomel electrode is used as a reference electrode, cyclic voltammetry is used for electroplating, the scanning potential range is-0.2V-0.9V, and the scanning speed is 10mV s-1。
The assembly of the microbial fuel cell, the power density and the polarization curve were measured as in example 2.
Example 4:
preparing and measuring a blank carbon cloth anode microbial fuel cell of a comparison system:
the assembly, power density and polarization curve of the microbial fuel cell were measured as in example 2, using a blank carbon cloth as the anode and a blank carbon paper as the cathode.
And (4) conclusion: referring to FIG. 1, a blank carbon cloth and grown MoS are shown2The cyclic voltammogram of the carbon cloth of the nanomaterial in the anolyte shows that for MoS2The carbon cloth electrode has obvious oxidation-reduction peak current for catalyzing glucose/HNQ in a range of-0.2V to-0.4V; shows the MoS2The carbon cloth electrode shows excellent electrocatalytic performance in a microbial fuel cell anode system, and the maximum catalytic oxidation peak current of the carbon cloth electrode is 2.7 mA/cm2Far higher than that of blank carbon cloth by 0.37 mA/cm2。
Referring to FIG. 2, MoS is shown from a test of a two-compartment microbial fuel cell2The modification of the nano material enables the internal resistance of the MFCs based on the carbon cloth as the anode to be reduced by 43 percent, the power to be improved by 60 percent, and the result of periodic operation shows that the average coulombic efficiency of the MFCs is 2.86 times that of the MFCs of the blank carbon cloth.
Referring to FIG. 3, it can be seen from the cyclic voltammetry and impedance tests that polymerization of PANI can greatly improve MoS2The conductivity of the carbon cloth electrode material reduces the charge transfer resistance and improves the electrocatalytic activity; PANI/MoS2The maximum power density and the internal resistance of the battery with/carbon cloth as the anode MFCs are 42.13W m-3(135 omega) is far superior to 22.12W m of PANI/carbon cloth-MFC single material-3(180. OMEGA.), and MoS227.97W m for/carbon cloth-MFC-3（210 Ω）。
Therefore, the anode based on the molybdenum disulfide composite material is low in price and easy to produce in batches, and the operation cost of the microbial fuel cell can be greatly reduced.
In summary, the following steps: the invention provides a high-performance microbial fuel cell based on a molybdenum disulfide composite material as an anode, which is prepared by MoS2The modification of the nano material obviously improves the electrochemical performance of the carbon material, shows certain direct catalytic performance to substrate glucose, and is 2.7 percent in solution containing the substrate glucose and an electron transfer mediator mA/cm2Far higher than that of blank carbon cloth by 0.37 mA/cm2(ii) a Second, testing of a two-compartment microbial fuel cell showed that MoS2The modification of the nano material enables the internal resistance of the MFCs taking the carbon cloth as the anode to be reduced by 43 percent, the power to be improved by 60 percent, the average coulombic efficiency is 2.86 times that of the blank carbon cloth as the anode MFCs, and meanwhile, the polymerization of PANI can further improve MoS2The conductivity of the carbon cloth electrode material reduces the charge transfer resistance and improves the electrocatalytic activity; in addition, PANI/MoS2The maximum power density and the internal resistance of the battery with/carbon cloth as the anode MFCs are 42.13W m-3(135 omega) is far superior to 22.12W m of PANI/carbon cloth-MFC single material-3(180. OMEGA.), and MoS227.97W m for/carbon cloth-MFC-3(210 omega), therefore, the anode based on the molybdenum disulfide composite material is low in price and easy to produce in batches, and the running cost of the microbial fuel cell can be greatly reduced.
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art should be able to cover the technical solutions and the inventive concepts of the present invention within the technical scope of the present invention.
Claims (6)
1. A microbial fuel cell based on a molybdenum disulfide composite material as an anode is characterized in that a sandwich type double-chamber structure comprising an anode chamber and a cathode chamber is adopted, and the anode chamber and the cathode chamber are separated by a cation exchange membrane;
the cathode chamber is used for storing cathode liquid, and the cathode immersed in the cathode liquid is carbon paper or carbon cloth;
the anode chamber is internally stored with anolyte, and the anode immersed in the anolyte is molybdenum disulfide/carbon cloth or conductive polymer/molybdenum disulfide/carbon cloth.
2. A microbial fuel cell based on a molybdenum disulfide composite as an anode in accordance with claim 1, wherein: the catholyte is a PBS buffer solution with neutral pH and consists of10.0g/L sodium bicarbonate and 11.2g/L disodium hydrogen phosphate, and contains 50mmol/L K3[Fe(CN)6]。
3. A microbial fuel cell based on a molybdenum disulfide composite as an anode in accordance with claim 1, wherein: the anolyte is PBS buffer solution with neutral pH, is formed by mixing 10.0g/L sodium bicarbonate and 11.2g/L disodium hydrogen phosphate, and contains 10.0g/L anhydrous glucose, 5 g/L yeast extract and 0.8707 g/L2-hydroxy-1, 4-naphthoquinone HNQ.
4. A microbial fuel cell based on a molybdenum disulfide composite as an anode in accordance with claim 1, wherein: the conductive polymer is formed by compounding polyaniline, polypyrrole or polythiophene conductive polymer on molybdenum disulfide/carbon cloth.
5. The microbial fuel cell based on the molybdenum disulfide composite material as the anode according to any one of claims 1 to 4, wherein the molybdenum disulfide composite anode is prepared by the following method:
s1: ultrasonically cleaning a carbon cloth sold in the market for half an hour by using acetone, ethanol and deionized water in sequence, and then drying for later use;
s2: putting the cleaned carbon material into a solution containing 0.5-1.5 g of thiourea, 1.0-1g of sodium molybdate, 0.2-0.6 g of P123 and 30-70 mL of deionized water, putting the solution into a high-pressure reaction kettle, carrying out hydrothermal reaction for 4-6 hours at the temperature of 150 ℃ plus 200 ℃, naturally cooling, washing the solution clean with the deionized water, and drying the solution to obtain the MoS grown on the carbon material2Carbon material of nanomaterial.
6. The microbial fuel cell based on a molybdenum disulfide composite as an anode according to claim 4, wherein the preparation method of the composite polyaniline conductive polymer is as follows:
s1: in the presence of 0.1mol L-1And 1mol L of aniline-1In the sulfuric acid solution, an electrode with hydrothermally grown molybdenum disulfide/carbon cloth is used as a working electrode;
s2: using Pt electrode as counter electrode and calomel electrode as reference, electroplating by cyclic voltammetry with scanning potential range of-0.2V-0.9V and scanning speed of 10mV s-1The number of scanning turns is 6-20.
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| CN113571716A (en) * | 2021-07-12 | 2021-10-29 | 新乡医学院 | Anode for microbial fuel cell, preparation method of anode and microbial fuel cell |
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