CN108565483B - Synchronous nitrogen and phosphorus removal microbial fuel cell based on zero-valent iron and nitrogen and phosphorus removal method - Google Patents
Synchronous nitrogen and phosphorus removal microbial fuel cell based on zero-valent iron and nitrogen and phosphorus removal method Download PDFInfo
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 title claims abstract description 62
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 48
- 229910052698 phosphorus Inorganic materials 0.000 title claims abstract description 35
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 34
- 239000011574 phosphorus Substances 0.000 title claims abstract description 34
- 229910052757 nitrogen Inorganic materials 0.000 title claims abstract description 31
- 239000000446 fuel Substances 0.000 title claims abstract description 25
- 230000000813 microbial effect Effects 0.000 title claims abstract description 18
- 230000001360 synchronised effect Effects 0.000 title claims abstract description 17
- 238000000034 method Methods 0.000 title claims abstract description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 73
- 238000006243 chemical reaction Methods 0.000 claims abstract description 58
- 239000011159 matrix material Substances 0.000 claims abstract description 26
- 230000005611 electricity Effects 0.000 claims abstract description 22
- 239000012528 membrane Substances 0.000 claims abstract description 15
- 239000002351 wastewater Substances 0.000 claims description 54
- 239000000047 product Substances 0.000 claims description 32
- NHNBFGGVMKEFGY-UHFFFAOYSA-N nitrate group Chemical group [N+](=O)([O-])[O-] NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 25
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 25
- 238000007789 sealing Methods 0.000 claims description 25
- 229910002651 NO3 Inorganic materials 0.000 claims description 24
- 229910019142 PO4 Inorganic materials 0.000 claims description 21
- 239000010452 phosphate Substances 0.000 claims description 21
- 239000007788 liquid Substances 0.000 claims description 13
- 229910052742 iron Inorganic materials 0.000 claims description 12
- 239000002244 precipitate Substances 0.000 claims description 10
- 239000000758 substrate Substances 0.000 claims description 9
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 6
- 229910052799 carbon Inorganic materials 0.000 claims description 6
- 150000002500 ions Chemical class 0.000 claims description 6
- 238000001556 precipitation Methods 0.000 claims description 5
- 241000894006 Bacteria Species 0.000 claims description 4
- 125000002467 phosphate group Chemical group [H]OP(=O)(O[H])O[*] 0.000 claims description 3
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 description 14
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 238000011084 recovery Methods 0.000 description 4
- 229910052984 zinc sulfide Inorganic materials 0.000 description 4
- 238000007599 discharging Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 229910001448 ferrous ion Inorganic materials 0.000 description 2
- 239000005431 greenhouse gas Substances 0.000 description 2
- 244000005700 microbiome Species 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- VTLYFUHAOXGGBS-UHFFFAOYSA-N Fe3+ Chemical compound [Fe+3] VTLYFUHAOXGGBS-UHFFFAOYSA-N 0.000 description 1
- IRERQBUNZFJFGC-UHFFFAOYSA-L azure blue Chemical compound [Na+].[Na+].[Na+].[Na+].[Na+].[Na+].[Na+].[Na+].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[S-]S[S-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-] IRERQBUNZFJFGC-UHFFFAOYSA-L 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- 229910052667 lazurite Inorganic materials 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- QMQXDJATSGGYDR-UHFFFAOYSA-N methylidyneiron Chemical compound [C].[Fe] QMQXDJATSGGYDR-UHFFFAOYSA-N 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 239000013049 sediment Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
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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
- C02F3/28—Anaerobic digestion processes
- C02F3/2806—Anaerobic processes using solid supports for microorganisms
-
- 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- 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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- Life Sciences & Earth Sciences (AREA)
- Chemical & Material Sciences (AREA)
- Microbiology (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Biodiversity & Conservation Biology (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Biochemistry (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Organic Chemistry (AREA)
- Water Treatment By Electricity Or Magnetism (AREA)
- Fuel Cell (AREA)
Abstract
The invention discloses a synchronous nitrogen and phosphorus removal microbial fuel cell based on zero-valent iron and a nitrogen and phosphorus removal method, wherein an anode chamber and a cathode chamber of the cell are respectively filled with an electricity generating matrix and a power consumption matrix, an anode chamber water inlet, an anode chamber water outlet and an anode product outlet are sequentially arranged on the anode chamber from top to bottom, and the part between the anode chamber water inlet and the anode chamber water outlet is an anode chamber reaction zone; the cathode chamber is sequentially provided with an exhaust port, a cathode chamber water inlet, a cathode chamber water outlet and a cathode biomembrane discharge port from top to bottom, the part between the cathode chamber water inlet and the cathode chamber water outlet is a cathode chamber reaction zone, and a cathode biomembrane is attached to the cathode electrode; the anode chamber reaction zone is communicated with the cathode chamber reaction zone through a pipeline, and a proton exchange membrane is arranged in the pipeline.
Description
Technical Field
The invention relates to the technical field of fuel cells, in particular to a zero-valent iron-based synchronous nitrogen and phosphorus removal microbial fuel cell and a nitrogen and phosphorus removal method.
Background
The traditional denitrification technology mostly adopts organic matters as electron donors, and the traditional biological dephosphorization technology also needs the organic matters as biological phosphorus-uptake energy materials. For the treatment of wastewater with low ratio of C to N to P, the additional addition of organic matters not only increases investment cost and is easy to cause secondary pollution, but also increases the emission of greenhouse gases. The novel denitrification and dephosphorization technology aiming at low CN and P ratio wastewater is searched and has great significance.
Iron and ferric salts are widely used agents in water treatment processes, including zero-valent iron, ferrous and ferric salts, and the like. Zero-valent iron is low in price, rich in source and has stronger potential for supplying electricity. The zero-valent iron is used as a denitrification electron donor, and the generated ferrous iron is used for dephosphorizing wastewater and generating wustite, so that synchronous denitrification and dephosphorization of the water body can be realized, and the recovery and reutilization of phosphorus resources in the water body can be realized.
However, the zero-valent iron is used as a denitrification electron donor, the generated ferrous iron is unstable and is easily oxidized into ferric iron or accumulated on the surface of microorganism cells in the form of iron oxide, so that the dephosphorization function is lost; even if a small amount of soluble ferrous iron reacts with phosphate to form wurtzite, the wurtzite is adsorbed to the surface of microorganisms, and separation of the wurtzite is difficult to achieve. How to extract ferrous iron which is a denitrification product of zero-valent iron and independently apply the ferrous iron to dephosphorization is a key point of synchronous denitrification and dephosphorization technology based on zero-valent iron.
Disclosure of Invention
Aiming at the current situation of low C: N: P ratio of wastewater in China, the invention provides a zero-valent iron-based synchronous denitrification and dephosphorization microbial fuel cell and a denitrification and dephosphorization method, and the invention utilizes an iron-carbon electrode to realize the transfer of electrons from an anode to a cathode, and generates electric energy for recycling; the iron anode loses electrons, and the generated soluble ferrous iron reacts with phosphate to generate wustite, so that phosphorus resources in the wastewater are removed and recycled; electrons are obtained from the carbon cathode, and the denitrification biomembrane on the surface of the carbon cathode reduces nitrate into nitrogen by utilizing the electrons, so that wastewater denitrification is realized.
In order to achieve the above purpose, the specific technical scheme adopted by the invention is as follows:
The synchronous denitrification and dephosphorization microbial fuel cell based on zero-valent iron comprises an anode chamber and a cathode chamber, wherein the anode chamber and the cathode chamber are respectively filled with an electricity-generating substrate and an electricity-consuming substrate, an anode chamber water inlet, an anode chamber water outlet and an anode product outlet are sequentially arranged on the anode chamber from top to bottom, an anode chamber reaction zone is arranged between the anode chamber water inlet and the anode chamber water outlet, an anode electrode is arranged in the anode chamber reaction zone, the anode electrode is made of zero-valent iron and is positioned below the liquid level of the electricity-generating substrate;
The cathode chamber is sequentially provided with an exhaust port, a cathode chamber water inlet, a cathode chamber water outlet and a cathode biological film exhaust port from top to bottom, wherein a cathode chamber reaction area is arranged between the cathode chamber water inlet and the cathode chamber water outlet, a cathode electrode is arranged in the cathode chamber reaction area, a cathode biological film with a denitrification function is attached to the cathode electrode, and the cathode electrode is below the liquid level of the power consumption matrix;
the anode chamber reaction zone is communicated with the cathode chamber reaction zone through a pipeline, and a proton exchange membrane is arranged in the pipeline.
The anode chamber and the cathode chamber are hollow structures, the upper ends of the anode chamber and the cathode chamber are provided with sealing flanges, sealing covers are detachably connected to the sealing flanges, an anode electrode is suspended on the sealing covers of the anode chamber and is positioned in the middle of a reaction zone of the anode chamber, an external lead is connected to the anode electrode, and one end of the external lead extends to the outside of the anode chamber;
the cathode electrode is hung on the sealing cover of the cathode chamber and is positioned in the middle of the reaction zone of the cathode chamber, an external lead is connected to the cathode electrode, and one end of the external lead extends to the outside of the anode chamber.
The exhaust port is arranged on the sealing cover of the cathode chamber, the sealing covers of the anode chamber and the cathode chamber are respectively provided with an external lead port, and the external lead connected to the anode electrode and the external lead connected to the cathode electrode respectively extend to the outside of the anode chamber and the outside of the cathode chamber from the external lead ports.
The lower ends of the anode chamber and the cathode chamber are respectively provided with an anode product collecting bucket and a falling biological film collecting bucket at the lower parts of the water outlet of the anode chamber and the lower part of the water outlet of the cathode chamber, and an anode product outlet and a cathode biological film outlet are respectively arranged at the lower parts of the anode product collecting bucket and the falling biological film collecting bucket.
The anode product collecting hopper and the falling biological film collecting hopper are of inverted cone structures, the inclination angle of the anode product collecting hopper is 60+/-2 degrees, and the inclination angle of the falling biological film collecting hopper is 55+/-2 degrees.
The anode chamber and the cathode chamber are respectively and vertically connected with a communicating pipe at the middle part of the anode chamber reaction zone and the middle part of the cathode chamber reaction zone, the anode chamber reaction zone and the cathode chamber reaction zone are respectively communicated with the communicating pipe, the free ends of the communicating pipes are respectively provided with a connecting flange for connecting the anode chamber and the cathode chamber into a whole, and the proton exchange membrane is arranged at the connecting flange.
The anode electrode is a rectangular iron sheet, the height-width ratio is (2.5:1) - (3.5:1), the ratio of the surface area of the anode electrode to the total volume of the anode chamber is (1 cm 2:8 cm3）~（1 cm2:12 cm3), and the distance between the top of the anode electrode and the liquid level of the electricity generating matrix is at least 30mm;
The cathode electrode is a rectangular carbon felt piece, the height-width ratio is (2.5:1) - (3.5:1), the cathode biological film is a denitrifying bacteria biological film, and the ratio of the surface area of the cathode electrode to the total volume of the cathode chamber is (1 cm 2:8 cm3）~（1 cm2:12 cm3);
The height-diameter ratio of the anode chamber to the cathode chamber is (3.5:1) - (4.5:1), and the top space ratio is 10% -15%;
The ratio of the area of the proton exchange membrane to the sum of the volumes of the anode and cathode compartments was (1 cm 2:50 cm3）~（1 cm2:70 cm3).
The electricity generating matrix is phosphate-containing electricity generating matrix, and the electricity consuming matrix is nitrate-containing electricity consuming matrix.
The denitrification and dephosphorization method is carried out by the microbial fuel cell and comprises the following steps:
step 1, an anode chamber adopts batch operation, and phosphate-containing wastewater is introduced into the anode chamber from a water inlet of the anode chamber, so that the liquid level of the phosphate-containing wastewater is higher than the top end of an anode electrode;
The cathode chamber adopts batch operation, and the wastewater containing nitrate is introduced into the cathode chamber from a water inlet of the cathode chamber, so that the liquid level of the wastewater containing nitrate is higher than the top end of the cathode electrode;
step 2, the anode electrode and the cathode electrode are respectively and electrically connected with a load, so that in the anode chamber, the anode electrode loses electrons to become soluble ions and enters an anode chamber reaction zone, and the soluble ions react with phosphate ions in phosphate-containing wastewater to generate a precipitate, thereby realizing dephosphorization; the generated precipitate is discharged through an anode product discharge outlet, and the wastewater which is subjected to precipitation reaction and does not contain phosphorus is discharged through an anode chamber water outlet;
In the cathode chamber, the cathode electrode obtains electrons lost by the anode electrode, and the cathode biomembrane reduces nitrate in the nitrate-containing wastewater into nitrogen by utilizing the electrons so as to realize denitrification; the generated nitrogen is discharged from the exhaust port; the nitrogen-free wastewater after denitrification is discharged from a water outlet of the cathode chamber;
In the process of dephosphorization in the anode chamber and denitrification in the cathode chamber, proton exchange is carried out between the anode chamber and the cathode chamber through a proton exchange membrane, so that charge balance is maintained between the anode chamber and the cathode chamber.
In the step 2, in the cathode chamber, the outer layer of the cathode biological film is gradually aged and falls off along with the denitrification reaction, the fallen cathode biological film is discharged from the cathode biological film discharge port, and the cathode biological film is replaced after the falling-off amount of the cathode biological film reaches a set amount.
The beneficial effects of the invention are as follows:
The anode electrode of the microbial fuel cell is made of zero-valent iron, a cathode biomembrane with a denitrification function is attached to the cathode electrode, an upper anode chamber water inlet and an anode chamber water outlet are arranged on the anode chamber, a cathode chamber water inlet and a cathode chamber water outlet are arranged on the cathode chamber, when the microbial fuel cell is used, phosphate-containing wastewater is introduced into the anode chamber from the anode chamber water inlet, nitrate-containing wastewater is introduced into the cathode chamber from the cathode chamber water inlet, after the anode electrode and the cathode electrode are respectively electrically connected with a load, the anode electrode loses electrons to become ferrous ions and enters an anode chamber reaction zone, and the ferrous ions react with phosphate ions in the phosphate-containing wastewater to generate wurtzite precipitates, so that dephosphorization is realized; the generated blue iron ore precipitate is discharged through an anode product discharge outlet, and phosphorus-free wastewater after the precipitation reaction is discharged through an anode chamber water outlet; the cathode electrode obtains electrons lost by the anode electrode, and the cathode biomembrane reduces nitrate in the nitrate-containing wastewater into nitrogen by utilizing the electrons so as to realize denitrification; the generated nitrogen is discharged from the exhaust port; the nitrogen-free wastewater after denitrification is discharged from a water outlet of the cathode chamber; in the process of dephosphorizing in the anode chamber and denitrifying in the cathode chamber, proton exchange is carried out between the anode chamber and the cathode chamber through a proton exchange membrane, so that charge balance is maintained between the anode chamber and the cathode chamber; through the above, the fuel cell provided by the invention can utilize phosphorus in phosphate wastewater and nitrogen in nitrate-containing wastewater to generate electricity, and can realize synchronous and continuous treatment of the phosphorus in the phosphate-containing wastewater and the nitrogen in the nitrate-containing wastewater, and the fuel cell provided by the invention uses the zero-valent iron sheet as an electron donor for biological denitrification of wastewater, so that the additional addition of organic matters can be avoided, the cost is saved, the emission of greenhouse gases is reduced, the phosphorus can be recovered in a delafossite form, the phosphorus removal and the phosphorus recovery can be synchronously realized, the purposes of both the two purposes and the waste are changed into valuables, and because the fuel cell provided by the invention has the above performances, the low-C-N-P wastewater can be utilized to generate electricity, and the low-C-N-P wastewater can be removed, so that the fuel cell has the characteristics of economy and environmental protection.
According to the effect of the fuel cell, the nitrogen and phosphorus removal method can remove phosphorus and nitrogen in the low-C-N-P wastewater, the phosphorus is converted into the lafuite precipitation to realize the removal of the phosphorus and the recovery of the phosphorus, the phosphorus removal and the phosphorus recovery are synchronously realized, the waste is changed into valuables, the nitrogen in the wastewater is converted into nitrogen to be discharged, the air is not polluted, and the removal is thorough; the invention can synchronously remove the phosphorus in the phosphate-containing wastewater and the nitrogen in the nitrate-containing wastewater, and can also generate electricity in the removal process, and the generated electric energy can be exported and utilized, so the invention has the characteristics of economy and environmental protection.
Drawings
FIG. 1 is a schematic diagram of the structure of a zero-valent iron-based synchronous denitrification and dephosphorization microbial fuel cell of the invention;
FIG. 2 is a top view of a zero-valent iron-based synchronous nitrogen and phosphorus removal microbial fuel cell of the present invention;
FIG. 3 is a schematic view in section A-A of FIG. 1;
FIG. 4 is a sectional view B-B of FIG. 1;
In the figure: the device comprises a 1-anode product discharge port, a 2-anode product collection bucket, a 3-anode chamber water outlet, a 4-anode chamber reaction zone, a 5-anode electrode, a 6-anode chamber water inlet, a 7-sealing cover, an 8-sealing flange, a 9-external lead port, a 10-cathode biological film discharge port, a 11-falling biological film collection bucket, a 12-cathode chamber water outlet, a 13-cathode chamber reaction zone, a 14-cathode biological film, a 15-cathode electrode, a 16-cathode chamber water inlet, a 17-exhaust port, a 18-proton exchange film, a 19-lead, a 20-load, a 21-electric signal collection system and a 22-communicating pipe.
Detailed Description
The invention will be further described with reference to the following drawings and detailed description. The preferred embodiments may be combined in any desired manner unless specifically stated or conflicting.
Referring to fig. 1, the zero-valent iron-based synchronous denitrification and dephosphorization microbial fuel cell of the invention comprises an anode chamber and a cathode chamber, wherein the anode chamber and the cathode chamber are respectively filled with an electricity generating matrix and an electricity consuming matrix, the electricity generating matrix is an electricity generating matrix containing phosphate, and the electricity consuming matrix is an electricity consuming matrix containing nitrate; the anode chamber and the cathode chamber are hollow structures, the upper ends of the anode chamber and the cathode chamber are respectively provided with a sealing flange 8, the sealing flanges 8 are detachably connected with sealing covers 7, and the sealing covers 7 of the anode chamber and the cathode chamber are respectively provided with an external lead port 9;
An anode chamber water inlet 6, an anode chamber water outlet 3 and an anode product outlet 1 are sequentially arranged on the anode chamber from top to bottom, wherein an anode chamber reaction zone 4 is arranged between the anode chamber water inlet 6 and the anode chamber water outlet 3 in the anode chamber, an anode electrode 5 is arranged in the anode chamber reaction zone 4, and the anode electrode 5 is below the liquid level of the electricity generating matrix; the anode electrode 5 is hung on the sealing cover 7 of the anode chamber and is positioned in the middle of the reaction zone 4 of the anode chamber, the anode electrode 5 is connected with an external lead 19, and the external lead 19 connected to the anode electrode 5 extends to the outside of the anode chamber from the external lead port 9;
The cathode chamber is sequentially provided with an exhaust port 17, a cathode chamber water inlet 16, a cathode chamber water outlet 12 and a cathode biological film exhaust port 10 from top to bottom, the exhaust port 17 is arranged on a sealing cover 7 of the cathode chamber, a cathode chamber reaction zone 13 is arranged between the cathode chamber water inlet 16 and the cathode chamber water outlet 12, a cathode electrode 15 is arranged in the cathode chamber reaction zone 13, a cathode biological film 14 with a denitrification function is attached to the cathode electrode 15, and the cathode electrode 15 is below the liquid level of the power consumption matrix; the cathode electrode 15 is hung on the sealing cover 7 of the cathode chamber and is positioned in the middle of the reaction zone 13 of the cathode chamber, the cathode electrode 15 is connected with an external lead 19, and the external lead 19 connected with the cathode electrode 15 extends to the outside of the cathode chamber from the external lead port 9;
The anode chamber and the cathode chamber are respectively and vertically connected with a communicating pipe 22 at the middle part of the anode chamber reaction zone 4 and the middle part of the cathode chamber reaction zone 13, the anode chamber reaction zone 4 and the cathode chamber reaction zone 13 are respectively communicated with the communicating pipe 22, the free ends of the communicating pipes 22 are respectively provided with a connecting flange for connecting the anode chamber and the cathode chamber into a whole, the connecting flange is provided with a proton exchange membrane 18, and the anode chamber substrate and the cathode chamber substrate exchange substances through the proton exchange membrane 18.
Referring to fig. 1, 3 and 4, the anode electrode 5 and the cathode electrode 15 of the present invention are both plate-like structures having the same shape, wherein the anode electrode 5 is an iron sheet, and the top of the anode electrode 5 is at least 30mm from the surface of the electrogenerated matrix. The cathode electrode 15 is a carbon mat and the cathode biofilm 14 is a denitrifying bacteria biofilm. The height-diameter ratio of the anode chamber to the cathode chamber is (3.5:1) - (4.5:1), the top duty ratio is 10% -15%, and the top duty ratio is the ratio of the top space of the anode chamber (or the cathode chamber) to the volume of the anode chamber (or the volume of the cathode chamber).
The lower ends of an anode chamber and a cathode chamber of the invention are respectively provided with an anode product collecting bucket 2 and a falling biological film collecting bucket 11 at the lower parts of an anode chamber water outlet 3 and a cathode chamber water outlet 12, and an anode product discharge port 1 and a cathode biological film discharge port 10 are respectively arranged at the lower parts of the anode product collecting bucket 2 and the falling biological film collecting bucket 11.
The anode product collecting hopper 2 and the falling biological film collecting hopper 11 are of inverted cone structures, the inclination angle of the anode product collecting hopper 2 is 60+/-2 degrees, and the inclination angle of the falling biological film collecting hopper 11 is 55+/-2 degrees.
The denitrification and dephosphorization method is carried out by the microbial fuel cell, and comprises the following steps:
step 1, the anode chamber adopts batch operation, and phosphate-containing wastewater is introduced into the anode chamber from the water inlet 6 of the anode chamber, so that the liquid level of the phosphate-containing wastewater is higher than the top end of the anode electrode 5;
the cathode chamber adopts batch operation, and nitrate-containing wastewater is introduced into the cathode chamber from a cathode chamber water inlet 16, so that the liquid level of the nitrate-containing wastewater is higher than the top end of a cathode electrode 15;
Step 2, the anode electrode 5 and the cathode electrode 15 are respectively and electrically connected with the load 20, so that in the anode chamber, the anode electrode 5 loses electrons to become soluble ions and enters the anode chamber reaction zone 4, and the soluble ions react with phosphate ions in the phosphate-containing wastewater to generate a precipitate, thereby realizing dephosphorization; the generated precipitate is collected by an anode product collecting hopper 2 and is discharged by an anode product discharge port 1, and phosphorus-free wastewater after precipitation reaction is discharged by an anode chamber water outlet 3;
In the cathode chamber, the cathode electrode 15 obtains electrons lost by the anode electrode 5, and the cathode biomembrane 14 reduces nitrate in the nitrate-containing wastewater into nitrogen by utilizing the electrons to realize denitrification; the generated nitrogen is discharged from the exhaust port 17; the nitrogen-free wastewater after denitrification is discharged from the water outlet 12 of the cathode chamber;
in the process of dephosphorizing in the anode chamber and denitrifying in the cathode chamber, proton exchange is carried out between the anode chamber and the cathode chamber through the proton exchange membrane 18, so that charge balance is maintained between the anode chamber and the cathode chamber;
In the cathode chamber, as the denitrification reaction proceeds, the outer layer of the cathode biofilm 14 gradually ages and falls off, and the falling-off cathode biofilm 14 is collected by the falling-off biofilm collecting hopper 11 and then discharged from the cathode biofilm discharge port 10, and when the falling-off amount of the cathode biofilm 14 reaches a set amount, the cathode biofilm 14 or the cathode electrode and the cathode biofilm 14 as a whole are replaced.
Preferably, when iron pieces are used as the anode electrode, the iron pieces lose electrons to soluble ferrous iron, which reacts with phosphate ions in the phosphate-containing wastewater to form a blue iron ore precipitate, and the soluble ferrous iron enters the anode chamber reaction zone 4.
Examples
As shown in fig. 1 to 4, the anode electrode 5 of the anode chamber and the cathode electrode 15 of the cathode chamber are connected through an external lead 19, a load 20 is arranged on the external lead 19, and two ends of the load 20 are connected in parallel to an electric signal acquisition system 21.
In the fuel cell of the present invention, the dimensions and proportions of the respective components may be set as appropriate. In the embodiment, the height-diameter ratio of the anode chamber to the cathode chamber is 4:1, the distance from the water outlet 3 of the anode chamber to the top of the anode product collecting hopper 2 is 1/12 of the total height of the anode chamber, the distance from the water inlet 6 of the anode chamber to the lower end face of the sealing flange 8 is 1/8 of the total height of the anode chamber, and the top space ratio of the anode chamber is 12.5%; the distance from the water outlet 12 of the cathode chamber to the top of the falling biological film collecting hopper 11 is 1/12 of the total height of the cathode chamber, the distance from the water inlet 16 of the cathode chamber to the lower end face of the sealing flange 8 is 1/8 of the total height of the cathode chamber, and the top duty ratio of the cathode chamber is 12.5%. The anode electrode material is an iron sheet, the anode electrode 5 is rectangular, the height-width ratio is 3:1, and the ratio of the surface area of the anode electrode 5 to the total volume of the anode chamber is 1cm 2：10cm3. The inclination angle of the phosphorus removal product collection hopper 2 is 60 degrees, and the inner diameter ratio of the phosphorus removal product discharge outlet 1 to the phosphorus removal product collection hopper 2 is 1:3. The cathode electrode 15 is a rectangular carbon felt sheet, and a denitrifying bacteria biological film 14 is attached to the surface of the cathode electrode 15; the aspect ratio of the cathode electrode 15 was 3:1 and the ratio of the surface area to the total volume of the cathode chamber was 1cm 2：10cm3. The inclination angle of the falling biological film collecting hopper 11 is 55 degrees, and the inner diameter ratio of the cathode biological film discharging outlet 10 to the falling biological film collecting hopper 11 is 1:6. The ratio of the membrane area of the proton exchange membrane 18 to the sum of the volumes of the cathode chamber and the anode chamber was 1cm 2：60cm3. Through experiments, the sizes and the proportions can well fulfill the aim of the experiment.
In the embodiment, the zero-valent iron-based synchronous denitrification and dephosphorization microbial fuel cell is manufactured by adopting organic glass, and the working process is as follows:
The anode chamber adopts batch operation, the simulated wastewater containing phosphate enters the anode chamber reaction zone 4 from the anode chamber water inlet 6, and the anode chamber reaction zone 4 of the simulated wastewater containing phosphate forms an electricity generating matrix; the iron sheet of the anode electrode 5 loses electrons to become soluble ferrous iron, and the soluble ferrous iron enters an anode chamber reaction zone 4, and the ferrous iron reacts with phosphate ions in an electrogenerated matrix to generate a blue iron ore precipitate; the lazurite sediment is collected by a dephosphorization product collecting hopper 2 and is discharged from a dephosphorization product discharging port 1; the treated wastewater without phosphorus is discharged from the water outlet 3 of the anode chamber. Electrons lost from the anode electrode 5 are transmitted to the cathode electrode 15 via the external lead 19, and the generated electrical signal can be monitored by the electrical signal acquisition system 21. The cathode chamber adopts batch operation, the simulated wastewater containing nitrate enters the cathode chamber reaction zone 13 from the cathode chamber water inlet 16, and the simulated wastewater containing nitrate forms a power consumption matrix in the cathode chamber reaction zone 13; the cathode electrode 15 obtains electrons from the anode electrode 5 of the anode chamber, and the cathode biological film 14 attached to the cathode electrode 15 reduces nitrate in the power consumption matrix into nitrogen by utilizing the electrons to realize denitrification; the generated nitrogen is discharged from the exhaust port 17; the treated nitrogen-free wastewater is discharged from the cathode chamber water outlet 12; as the reaction proceeds, the outer layer of the cathode biofilm 14 gradually ages and falls off, and the falling-off biofilm is collected by the falling-off biofilm collecting hopper 11 and discharged from the cathode biofilm discharge outlet 10. To maintain the charge balance of the anode and cathode compartments, the electrogenic and dissipative substrates are proton exchanged through the proton exchange membrane 18.
Claims (4)
1. The synchronous denitrification and dephosphorization microbial fuel cell based on zero-valent iron is characterized by comprising an anode chamber and a cathode chamber, wherein an electricity-generating substrate and a power-consuming substrate are respectively filled in the anode chamber and the cathode chamber, an anode chamber water inlet (6), an anode chamber water outlet (3) and an anode product outlet (1) are sequentially arranged on the anode chamber from top to bottom, an anode chamber reaction zone (4) is arranged at a part between the anode chamber water inlet (6) and the anode chamber water outlet (3) in the anode chamber, an anode electrode (5) is arranged in the anode chamber reaction zone (4), and the anode electrode (5) is made of zero-valent iron and is positioned below the liquid level of the electricity-generating substrate;
an exhaust port (17), a cathode chamber water inlet (16), a cathode chamber water outlet (12) and a cathode biological film discharge port (10) are sequentially arranged on the cathode chamber from top to bottom, a cathode chamber reaction zone (13) is arranged between the cathode chamber water inlet (16) and the cathode chamber water outlet (12), a cathode electrode (15) is arranged in the cathode chamber reaction zone (13), a cathode biological film (14) with a denitrification function is attached to the cathode electrode (15), and the cathode electrode (15) is below the liquid level of the power consumption matrix;
The anode chamber reaction zone (4) is communicated with the cathode chamber reaction zone (13) through a pipeline, and a proton exchange membrane (18) is arranged in the pipeline;
The anode chamber and the cathode chamber are of hollow structures, the upper ends of the anode chamber and the cathode chamber are provided with sealing flanges (8), sealing covers (7) are detachably connected to the sealing flanges (8), the anode electrode (5) is suspended on the sealing covers (7) of the anode chamber and is positioned in the middle of the anode chamber reaction zone (4), the anode electrode (5) is connected with an external lead (19), and one end of the external lead (19) extends to the outside of the anode chamber;
The cathode electrode (15) is hung on the sealing cover (7) of the cathode chamber and is positioned in the middle of the reaction zone (13) of the cathode chamber, an external lead (19) is connected to the cathode electrode (15), and one end of the external lead (19) extends to the outside of the anode chamber;
The lower ends of the anode chamber and the cathode chamber are respectively provided with an anode product collecting hopper (2) and a falling biological film collecting hopper (11) at the lower parts of the water outlet (3) of the anode chamber and the water outlet (12) of the cathode chamber, and an anode product outlet (1) and a cathode biological film outlet (10) are respectively arranged at the lower parts of the anode product collecting hopper (2) and the falling biological film collecting hopper (11);
The anode product collecting hopper (2) and the falling biological film collecting hopper (11) are of inverted cone structures, the inclination angle of the anode product collecting hopper (2) is 60+/-2 degrees, and the inclination angle of the falling biological film collecting hopper (11) is 55+/-2 degrees;
The anode electrode (5) is an iron sheet, the cathode electrode (15) is a carbon felt sheet, and the cathode biological film (14) is a denitrifying bacteria biological film;
the electricity generating matrix is phosphate-containing electricity generating matrix, and the electricity consuming matrix is nitrate-containing electricity consuming matrix.
2. The synchronous nitrogen and phosphorus removal microbial fuel cell based on zero-valent iron according to claim 1, wherein the exhaust port (17) is arranged on the sealing cover (7) of the cathode chamber, the sealing covers (7) of the anode chamber and the cathode chamber are both provided with external lead ports (9), and the external lead (19) connected on the anode electrode (5) and the external lead (19) connected on the cathode electrode (15) respectively extend to the outside of the anode chamber and the outside of the cathode chamber from the external lead ports (9).
3. The zero-valent iron-based synchronous nitrogen and phosphorus removal microbial fuel cell according to claim 1, wherein the anode chamber and the cathode chamber are vertically connected with a communicating pipe (22) respectively at the middle part of the anode chamber reaction zone (4) and the middle part of the cathode chamber reaction zone (13), the anode chamber reaction zone (4) and the cathode chamber reaction zone (13) are respectively communicated with the communicating pipe (22), the free ends of the communicating pipes (22) are respectively provided with a connecting flange for connecting the anode chamber and the cathode chamber into a whole, and the proton exchange membrane (18) is arranged at the connecting flange.
4. A nitrogen and phosphorus removal method based on the zero-valent iron-based synchronous nitrogen and phosphorus removal microbial fuel cell as claimed in any one of claims 1 to 3, characterized by comprising the following steps:
step 1, an anode chamber adopts batch operation, and phosphate-containing wastewater is introduced into the anode chamber from a water inlet (6) of the anode chamber, so that the liquid level of the phosphate-containing wastewater is higher than the top end of an anode electrode (5);
the cathode chamber adopts batch operation, and nitrate-containing wastewater is introduced into the cathode chamber from a cathode chamber water inlet (16) so that the liquid level of the nitrate-containing wastewater is higher than the top end of a cathode electrode (15);
Step 2, the anode electrode (5) and the cathode electrode (15) are respectively and electrically connected with a load (20), so that in an anode chamber, the anode electrode (5) loses electrons to become soluble ions and enters an anode chamber reaction zone (4), and the soluble ions react with phosphate ions in phosphate-containing wastewater to generate a precipitate, thereby realizing dephosphorization; the generated precipitate is discharged through an anode product discharge port (1), and the wastewater which is not phosphorus after the precipitation reaction is discharged through an anode chamber water outlet (3);
In the cathode chamber, a cathode electrode (15) obtains electrons lost by an anode electrode (5), and a cathode biological film (14) reduces nitrate in nitrate-containing wastewater into nitrogen by utilizing the electrons so as to realize denitrification; the generated nitrogen is discharged from an exhaust port (17); the nitrogen-free wastewater after denitrification is discharged from a water outlet (12) of the cathode chamber;
In the process of dephosphorizing in the anode chamber and denitrifying in the cathode chamber, proton exchange is carried out between the anode chamber and the cathode chamber through a proton exchange membrane (18), so that charge balance is maintained between the anode chamber and the cathode chamber;
In the step 2, the outer layer of the cathode biological film (14) is gradually aged and falls off as the denitrification reaction proceeds in the cathode chamber, the fallen cathode biological film (14) is discharged from the cathode biological film discharge port (10), and when the falling-off amount of the cathode biological film (14) reaches a set amount, the cathode biological film (14) is replaced.
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