CN111146484A - Microbial fuel cell and method for promoting wastewater denitrification of microbial fuel cell - Google Patents

Microbial fuel cell and method for promoting wastewater denitrification of microbial fuel cell Download PDF

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CN111146484A
CN111146484A CN202010068553.6A CN202010068553A CN111146484A CN 111146484 A CN111146484 A CN 111146484A CN 202010068553 A CN202010068553 A CN 202010068553A CN 111146484 A CN111146484 A CN 111146484A
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CN111146484B (en
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李超
骆苗苗
操家顺
许明
冯骞
方芳
郭文
薛朝霞
罗景阳
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Hohai University HHU
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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
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/005—Combined electrochemical biological processes
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00—Biological treatment of water, waste water, or sewage
    • C02F3/28—Anaerobic digestion processes
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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    • C02F2101/10—Inorganic compounds
    • C02F2101/16—Nitrogen compounds, e.g. ammonia
    • C02F2101/163—Nitrates
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Abstract

The invention belongs to the technical field of microbial fuel cells and water treatment, and provides a microbial fuel cell and a method for promoting wastewater denitrification of the microbial fuel cell. The anode chamber is sealed by a sealing cover, and the anode sludge anaerobic digestion liquid flows back to the cathode chamber through a peristaltic pump; the anode chamber and the cathode chamber are separated by a proton exchange membrane in a communicating side pipe, the cathode and the anode are connected by a lead, and an external resistor is arranged on the lead; carbon dioxide is introduced to the cathode through a microporous aeration disc at the bottom of the cathode chamber, and the carbon dioxide is used as a carbon source of the cathode. The anode chamber sludge of the microbial fuel cell can generate substances such as VFA, water and the like in an anaerobic state, and the returned anode sludge anaerobic digestion liquid and the introduced carbon dioxide are simultaneously used as a cathode carbon source, so that the sludge of the anode can be reduced, the pH of the cathode can be adjusted, the denitrification efficiency of the cathode is improved, and the performance of the microbial fuel cell in treating nitrogen-containing wastewater is improved.

Description

Microbial fuel cell and method for promoting wastewater denitrification of microbial fuel cell
Technical Field
The invention belongs to the technical field of microbial fuel cells and water treatment, and particularly relates to a microbial fuel cell and a method for promoting wastewater denitrification of the microbial fuel cell.
Background
Under the anaerobic state of an MFC (microbial fuel cell) anode, microorganisms degrade organic matters to generate electrons, protons, carbon dioxide, VFA and other substances, the protons are introduced into a cathode chamber through a proton exchange membrane, the electrons are introduced into a cathode through a lead, and sludge in the anode chamber can be reduced under the anaerobic state.
The electron donors required for the MFC cathode denitrification process are mainly derived from the carbon source and the cathode electrons. Different electron donors can have an effect on the denitrification performance of the cathode, and there is some competition and contradiction between the two electron donors in the MFC cathode system: when a carbon source electron donor exists, heterotrophic denitrifying bacteria can be used as the electron donor for denitrification, so that a large number of cathode heterotrophic bacteria are bred to be unfavorable for the growth of autotrophic denitrifying bacteria, and the efficiency of the battery is low; however, if the carbon source is too little, the microorganisms are stressed to use only the cathode electrons for denitrification (autotrophic denitrifying bacteria), and the comprehensive denitrification rate of the system is greatly reduced.
Production of VFA and CO from anaerobic digestion of MFC anode sludge2Simultaneously, the carbon source is used as a cathode carbon source, so that microorganisms can be converted from single electrode denitrification into combination with non-electrode denitrification, the non-electrode denitrification process has high speed, and the carbon source canSo as to effectively improve the denitrification efficiency of the cathode.
At present, factors influencing the denitrification of the MFC comprise the shape and configuration of a battery, pH, external resistance, a carrier electrode and the like, wherein the addition of different types of carbon sources causes the denitrification effect of the MFC to be greatly different, common carbon sources comprise organic carbon sources such as sodium acetate, methanol, glucose and the like, inorganic carbon sources such as carbon dioxide and the like are less researched as nutrient substances of microorganisms, and the sludge in an anode chamber is anaerobically hydrolyzed to generate VFA, water, CO2Iso-substance, VFA and CO produced2Can be used as a carbon source of a cathode by microorganisms, so that the resources are utilized to the maximum extent, the denitrification effect is improved, and the reduction of sludge is realized at the same time.
Disclosure of Invention
The purpose of the invention is as follows: the invention provides a method for promoting microbial fuel cell wastewater denitrification by utilizing carbon dioxide, which takes the carbon dioxide as a main carbon source of a cathode and then leads VFA generated by anode sludge anaerobic digestion to flow back to a cathode chamber, so that on one hand, cathode microorganisms can be utilized to generate electrons for denitrifying bacteria to realize the aim of denitrification, on the other hand, the pH value of the cathode can be adjusted, and simultaneously, sludge reduction can be realized in an anode chamber.
In order to solve the problems, the technical scheme adopted by the invention is as follows:
a microbial fuel cell comprises an anode chamber, a cathode chamber and a carbon dioxide ventilation device, wherein a sealing cover is arranged on the anode chamber for sealing and keeping an anaerobic state; the anode chamber and the cathode chamber are separated by a proton exchange membrane, and the sludge anaerobic digestion solution in the anode chamber flows back to the cathode chamber; the anode and the cathode are connected through a lead, and an external resistor is arranged on the lead; the carbon dioxide ventilation device comprises a carbon dioxide gas cylinder, a flow valve and a carbon dioxide ventilation hose which are sequentially connected, and the carbon dioxide ventilation device is used for introducing carbon dioxide in the gas cylinder into the cathode chamber.
Wherein a communicating side pipe is arranged between the anode chamber and the cathode chamber, and the proton exchange membrane is arranged in the communicating side pipe.
Preferably, the anode and cathode are both carbon felt.
Specifically, the range of the external resistance is 100-1000 omega.
The carbon dioxide gas bottle is connected with the glass rotameter, and carbon dioxide is introduced into the cathode through the microporous aeration disc at the bottom of the cathode chamber.
The anode chamber is inoculated with sludge for anaerobic digestion, and the inoculation volume is that of the anode chamber
Figure BDA0002376672110000021
And adding organic culture solution in the volume of anode chamber
Figure BDA0002376672110000022
The anode chamber is provided with a reflux port which is arranged at the height of the anode chamber
Figure BDA0002376672110000023
And a control valve is arranged on the backflow port, the anode sludge anaerobic digestion liquid is controlled to flow back to the cathode chamber through a peristaltic pump, and the backflow volume is 100-300 mL.
The culture solution containing nitrate and nitrogen is added into the cathode chamber, in some embodiments, nitrate and nitrogen-containing wastewater can be added, so that the ratio of C to N of the cathode is 1-3.
The invention further provides a method for promoting the wastewater denitrification of the device, which realizes the high-efficiency denitrification of the wastewater by controlling the anaerobic digestion reflux of the anode sludge and the aeration rate of the cathode carbon dioxide and jointly regulating and controlling the cathode denitrification carbon source.
Besides the realization of electric energy recovery, the anode chamber unit can realize sludge reduction and control the function of anode sludge anaerobic digestion liquid reflux to supply cathode organic carbon source; the carbon dioxide aeration of the cathode chamber unit can realize the functions of stirring, cathode pH adjustment and inorganic carbon source supplement.
Furthermore, the microbial fuel cell can jointly regulate and control a cathode denitrification carbon source by controlling the anaerobic digestion reflux of anode sludge and the aeration rate of cathode carbon dioxide, so that the efficient denitrification of wastewater is realized.
In the microbial fuel cell, the anode sludge can generate VFA and CO in an anaerobic state2And water, etc., thereby realizing the reduction of the sludge.
The cathode chamber microorganisms utilize carbon dioxide and the reflowed VFA as carbon sources, so that electrons are generated for denitrifying bacteria to utilize, and the denitrification performance can be improved; and CO2The pH and alkalinity of the cathode can be adjusted by dissolving in water to make the solution acidic, together with the refluxing VFA.
The electron donors required for the MFC cathode denitrification process are mainly derived from the carbon source and the cathode electrons. Different electron donors can have an effect on the denitrification performance of the cathode, and there is some competition and contradiction between the two electron donors in the MFC cathode system: when a carbon source electron donor exists, heterotrophic denitrifying bacteria can be used as the electron donor for denitrification, so that a large number of cathode heterotrophic bacteria are bred to be unfavorable for the growth of autotrophic denitrifying bacteria, and the efficiency of the battery is low; however, if the carbon source is too little, the microorganisms are stressed to use only the cathode electrons for denitrification (autotrophic denitrifying bacteria), and the comprehensive denitrification rate of the system is greatly reduced. Feeding CO to the cathode2And VFA is used as a carbon source, so that microorganisms can be converted from single electrode denitrification into combination with non-electrode denitrification, the speed of the non-electrode denitrification process is high, and the denitrification efficiency of the cathode can be effectively improved.
Has the advantages that: compared with the prior art, the microbial fuel cell adopts carbon dioxide as a main carbon source of the cathode, and then the VFA generated by anaerobic digestion of anode sludge flows back to the cathode chamber, so that on one hand, cathode microorganisms can be utilized to generate electrons for denitrifying bacteria to realize the aim of denitrification, on the other hand, the pH of the cathode can be adjusted, and meanwhile, sludge reduction can be realized in the anode chamber.
Drawings
FIG. 1 is a schematic view of the structure of a microbial fuel cell of the present invention;
in the drawings, the components represented by the respective reference numerals are listed below:
1. anode chamber 2, cathode chamber 3, connecting side4, a proton exchange membrane, 5, an anode sludge anaerobic digestion liquid reflux port, 6, an anode chamber water inlet, 7, an anode chamber sealing cover, 8, a wire guide port, 9, an external resistor, 10, anaerobic sludge, 11, a carbon felt, 12, a cathode chamber water inlet, 13, a cathode chamber reflux water inlet, 14, a micropore aeration disc, 15, CO, 152Gas cylinder, 16, glass rotameter, 17, peristaltic pump, 18, reflux hose, 19, carbon dioxide vent hose.
Detailed Description
The technical solution of the present invention will be further described in detail with reference to the accompanying drawings and examples.
As shown in FIG. 1, the present invention proposes a microbial fuel cell comprising an anode chamber 1, a cathode chamber 2 and a carbon dioxide aeration device, all of which have a volume of 900 mL. The anode chamber 1 is sealed by a sealing cover 7 to keep an anaerobic state, the anode chamber 1 is also provided with a water inlet 6, a return port 5 and a wire port 8, and the return port is arranged at the height of the anode chamber
Figure BDA0002376672110000041
The control valve is arranged on the reflux port, the anode sludge anaerobic digestion liquid flows back to the cathode chamber 2 through a reflux liquid hose 18 through a peristaltic pump 17, the anode chamber 1 and the cathode chamber 2 are separated by a proton exchange membrane 4 in a communication side pipe 3, the cathode and the anode are connected through a lead, an external resistor 9 is arranged on the lead, the carbon dioxide aeration device comprises a carbon dioxide gas cylinder 15, a flow valve and a carbon dioxide aeration hose 19 which are sequentially connected, the carbon dioxide gas cylinder 15 is connected with a glass rotameter 16, and carbon dioxide is introduced into the cathode 2 through a micropore aeration disc 14 at the bottom of the cathode chamber; the cathode and the anode adopt carbon felts 11 with the size of 6cm multiplied by 4cm multiplied by 0.3 cm; the range of the external resistor 9 is 100-1000 omega.
The operation process of the microbial fuel cell comprises the following steps: directly inoculating anaerobic sludge and organic culture solution into the anode chamber, wherein the inoculation volume of the anaerobic sludge is that of the anode chamber
Figure BDA0002376672110000042
The volume of the organic culture solution being that of the anode chamber
Figure BDA0002376672110000043
The method comprises the steps that an electrogenesis microorganism oxidizes organic matters to generate electrons, protons and carbon dioxide, the electrons are transferred to a cathode of a cathode chamber through an external circuit lead, the protons diffuse into the cathode chamber through a proton exchange membrane, oxygen is reduced at a cathode active site, water is generated by combining with the protons, nitrate nitrogen-containing wastewater is directly added into the cathode chamber, a carbon dioxide aeration device introduces the carbon dioxide in a gas cylinder into the cathode chamber to serve as an inorganic carbon source, an anode sludge anaerobic digestion reflux liquid can be introduced into the cathode chamber by 100-300 mL through a peristaltic pump control, the carbon source and the carbon dioxide are simultaneously used as a carbon source of the cathode, nutrient solutions of the cathode and the anode are replaced every three days, sludge in the anode chamber is added, and meanwhile.
The cathode and anode culture solution formula comprises: the anode organic culture solution comprises the following components: 6g/L Na2HPO4，3g/L KH2PO4，0.5g/LNaCl，0.1g/L MgSO4·7H2O，0.015CaCl2And 1mL/L of trace elements, and simultaneously adding sodium acetate to ensure that the COD content of the anode is 1000mg/L, so that the anode microorganisms utilize organic matters to generate electrons; the cathode nitrate nitrogen wastewater comprises the following components: 0.364g/L NaNO3(C: N of catholyte is 1-3 when carbon dioxide is introduced), 6g/L Na2HPO4，3g/L KH2PO4，0.5g/L NaCl，0.1g/L MgSO4·7H2O，0.015CaCl2And 1mL/L trace elements.
The device can realize the electric energy recovery, the anode chamber unit can realize the sludge reduction, and the function of controlling the anode sludge anaerobic digestion liquid to flow back to supply the cathode organic carbon source is realized; the carbon dioxide aeration of the cathode chamber unit can realize the functions of stirring, cathode pH adjustment and inorganic carbon source supplement. The high-efficiency denitrification of the wastewater can be realized by controlling the anaerobic digestion reflux of the anode sludge and the aeration rate of the cathode carbon dioxide and jointly regulating and controlling the cathode denitrification carbon source.
The table 1 is a comparison table of the ratio of carbon to nitrogen (C: N is 1-3) of catholyte when different volumes of carbon dioxide are introduced and the cathode denitrification effect of refluxing different volumes of the anode sludge anaerobic digestion solution, when the anolyte does not flow back and carbon dioxide is not introduced, the microorganisms perform autotrophic denitrification, the denitrification efficiency is only 60.9%, the microorganisms can perform heterotrophic denitrification by the anolyte backflow and the carbon dioxide introduction, so that the denitrification efficiency is improved, and the denitrification effect is more obvious when carbon dioxide is introduced, so that the carbon dioxide and the refluxing anolyte are effectively feasible for denitrification by taking the carbon dioxide as a cathode carbon source.
TABLE 1
Figure BDA0002376672110000051
In summary, the microbial fuel cell of the present invention uses carbon dioxide as a main carbon source of the cathode, and then the VFA generated by anaerobic digestion of the anode sludge is returned to the cathode chamber, so that on one hand, the VFA can be utilized by the cathode microorganisms to generate electrons for denitrifying bacteria to achieve the purpose of denitrification, and on the other hand, the pH of the cathode can be adjusted, and at the same time, the sludge reduction in the anode chamber can be achieved.

Claims (9)

1. A microbial fuel cell is characterized by comprising an anode chamber, a cathode chamber and a carbon dioxide ventilation device, wherein a sealing cover is arranged on the anode chamber for sealing and keeping an anaerobic state; the anode chamber and the cathode chamber are separated by a proton exchange membrane, and the sludge anaerobic digestion solution in the anode chamber flows back to the cathode chamber; the anode and the cathode are connected through a lead, and an external resistor is arranged on the lead; the carbon dioxide aeration device is used for introducing carbon dioxide in the gas cylinder into the cathode chamber.
2. The microbial fuel cell according to claim 1, wherein a communication side pipe is provided between the anode chamber and the cathode chamber, and the proton exchange membrane is provided in the communication side pipe.
3. The microbial fuel cell of claim 1, wherein the anode and cathode are both carbon felt.
4. The microbial fuel cell according to claim 1, wherein the external resistance is in a range of 100 to 1000 Ω.
5. The microbial fuel cell of claim 1, wherein the carbon dioxide cylinder is connected with a glass rotameter, and carbon dioxide is introduced into the cathode through a microporous aeration disc at the bottom of the cathode chamber.
6. The microbial fuel cell of claim 1, wherein the anode compartment is inoculated with sludge for anaerobic digestion and the inoculation volume is that of the anode compartment
Figure FDA0002376672100000011
And adding organic culture solution in the volume of anode chamber
Figure FDA0002376672100000012
7. The microbial fuel cell of claim 1, wherein the anode chamber is provided with a return port, and the return port is arranged at a higher position of the anode chamber
Figure FDA0002376672100000013
And a control valve is arranged on the backflow port, the anode sludge anaerobic digestion liquid is controlled to flow back to the cathode chamber through a peristaltic pump, and the backflow volume is 100-300 mL.
8. The microbial fuel cell according to claim 1, wherein a nitrate nitrogen-containing culture solution is added to the entire cathode chamber, and the cathode has a ratio of C to N of 1-3.
9. A method for promoting denitrification of wastewater of a microbial fuel cell according to any one of claims 1 to 8, wherein efficient denitrification of wastewater is realized by controlling anode sludge anaerobic digestion liquid reflux and cathode carbon dioxide aeration amount and jointly adjusting and controlling a cathode denitrification carbon source.
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CN111646635A (en) * 2020-05-19 2020-09-11 河海大学 Method for strengthening performance of constructed wetland-microbial fuel cell coupling system
CN112047456A (en) * 2020-07-28 2020-12-08 国河环境研究院(南京)有限公司 Microbial fuel cell wastewater denitrification device and method
CN113371818A (en) * 2021-06-24 2021-09-10 广东石油化工学院 Method for strengthening nitrogen/sulfur-containing wastewater autotrophic treatment of MEC (methanol-organic carbon) biological cathode
CN116395801A (en) * 2023-03-16 2023-07-07 中国矿业大学 Organic anodic oxidation CO 2 Cathode reduction energy device and method

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CN113371818A (en) * 2021-06-24 2021-09-10 广东石油化工学院 Method for strengthening nitrogen/sulfur-containing wastewater autotrophic treatment of MEC (methanol-organic carbon) biological cathode
CN116395801A (en) * 2023-03-16 2023-07-07 中国矿业大学 Organic anodic oxidation CO 2 Cathode reduction energy device and method

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