CN110563158A - Zero-valent iron-based coil spring type microbial fuel cell capable of synchronously removing nitrogen and phosphorus and working method thereof - Google Patents
Zero-valent iron-based coil spring type microbial fuel cell capable of synchronously removing nitrogen and phosphorus and working method thereof Download PDFInfo
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- CN110563158A CN110563158A CN201910926511.9A CN201910926511A CN110563158A CN 110563158 A CN110563158 A CN 110563158A CN 201910926511 A CN201910926511 A CN 201910926511A CN 110563158 A CN110563158 A CN 110563158A
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 56
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 title claims abstract description 54
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 38
- 229910052698 phosphorus Inorganic materials 0.000 title claims abstract description 36
- 239000011574 phosphorus Substances 0.000 title claims abstract description 36
- 239000000446 fuel Substances 0.000 title claims abstract description 35
- 230000000813 microbial effect Effects 0.000 title claims abstract description 31
- 229910052757 nitrogen Inorganic materials 0.000 title claims abstract description 27
- 238000000034 method Methods 0.000 title abstract description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 78
- 238000007789 sealing Methods 0.000 claims abstract description 49
- 239000012528 membrane Substances 0.000 claims abstract description 37
- 239000002351 wastewater Substances 0.000 claims abstract description 25
- 230000001360 synchronised effect Effects 0.000 claims abstract description 16
- 238000006243 chemical reaction Methods 0.000 claims description 46
- 239000000047 product Substances 0.000 claims description 32
- 239000003792 electrolyte Substances 0.000 claims description 22
- 229910002651 NO3 Inorganic materials 0.000 claims description 17
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 17
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 15
- 229910052742 iron Inorganic materials 0.000 claims description 13
- XKMRRTOUMJRJIA-UHFFFAOYSA-N ammonia nh3 Chemical compound N.N XKMRRTOUMJRJIA-UHFFFAOYSA-N 0.000 claims description 12
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims description 11
- 229910019142 PO4 Inorganic materials 0.000 claims description 10
- 239000010452 phosphate Substances 0.000 claims description 10
- 238000012163 sequencing technique Methods 0.000 claims description 10
- 230000001174 ascending effect Effects 0.000 claims description 9
- 239000000758 substrate Substances 0.000 claims description 9
- 229910001448 ferrous ion Inorganic materials 0.000 claims description 8
- 239000000463 material Substances 0.000 claims description 8
- 241000894006 Bacteria Species 0.000 claims description 7
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 6
- 239000011521 glass Substances 0.000 claims description 6
- 239000000741 silica gel Substances 0.000 claims description 6
- 229910002027 silica gel Inorganic materials 0.000 claims description 6
- 244000005700 microbiome Species 0.000 claims description 5
- 239000002244 precipitate Substances 0.000 claims description 5
- 238000001556 precipitation Methods 0.000 claims description 5
- 229910052683 pyrite Inorganic materials 0.000 claims description 4
- NIFIFKQPDTWWGU-UHFFFAOYSA-N pyrite Chemical compound [Fe+2].[S-][S-] NIFIFKQPDTWWGU-UHFFFAOYSA-N 0.000 claims description 3
- 239000011028 pyrite Substances 0.000 claims description 3
- 230000005611 electricity Effects 0.000 claims 2
- 238000011017 operating method Methods 0.000 claims 1
- 239000010865 sewage Substances 0.000 abstract description 7
- 238000011084 recovery Methods 0.000 abstract description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 4
- 229910052799 carbon Inorganic materials 0.000 abstract description 4
- 230000007613 environmental effect Effects 0.000 abstract description 3
- 238000004064 recycling Methods 0.000 abstract 1
- 239000000126 substance Substances 0.000 description 11
- 239000007787 solid Substances 0.000 description 8
- 230000008569 process Effects 0.000 description 7
- 238000005202 decontamination Methods 0.000 description 5
- 230000003588 decontaminative effect Effects 0.000 description 5
- 239000007788 liquid Substances 0.000 description 5
- 230000000694 effects Effects 0.000 description 4
- 238000007599 discharging Methods 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 241000282414 Homo sapiens Species 0.000 description 2
- JVMRPSJZNHXORP-UHFFFAOYSA-N ON=O.ON=O.ON=O.N Chemical compound ON=O.ON=O.ON=O.N JVMRPSJZNHXORP-UHFFFAOYSA-N 0.000 description 2
- MMDJDBSEMBIJBB-UHFFFAOYSA-N [O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[NH6+3] Chemical compound [O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[NH6+3] MMDJDBSEMBIJBB-UHFFFAOYSA-N 0.000 description 2
- 238000012851 eutrophication Methods 0.000 description 2
- 230000005484 gravity Effects 0.000 description 2
- -1 iron ions Chemical class 0.000 description 2
- 239000011159 matrix material Substances 0.000 description 2
- 239000005416 organic matter Substances 0.000 description 2
- 230000027756 respiratory electron transport chain Effects 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- 241000195493 Cryptophyta Species 0.000 description 1
- VVQNEPGJFQJSBK-UHFFFAOYSA-N Methyl methacrylate Chemical group COC(=O)C(C)=C VVQNEPGJFQJSBK-UHFFFAOYSA-N 0.000 description 1
- 229920005372 Plexiglas® Polymers 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000001651 autotrophic effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000002551 biofuel Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 230000004069 differentiation Effects 0.000 description 1
- 239000000975 dye Substances 0.000 description 1
- 159000000014 iron salts Chemical class 0.000 description 1
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 description 1
- 239000008239 natural water Substances 0.000 description 1
- 235000015097 nutrients Nutrition 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000004065 wastewater treatment Methods 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
Classifications
-
- 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
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- 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
-
- 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
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/105—Phosphorus compounds
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/46115—Electrolytic cell with membranes or diaphragms
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/4618—Supplying or removing reactants or electrolyte
-
- 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
Abstract
the invention discloses a zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal and a working method thereof.A cathode electrode and an anode reactor are both in coil spring shapes; the cathode biological membrane is arranged on the surface of the cathode electrode; the upper ends of the cathode electrode and the anode reactor are both connected with a sealing plate; an anode electrode of zero-valent iron is arranged in the anode reactor, and a proton exchange membrane is arranged on the outer wall of the anode reactor; the upper end of the anode reactor is provided with an anode water inlet pipe, the lower end of the anode reactor is provided with an anode product discharge pipe and an anode water outlet pipe, and the anode water inlet pipe, the anode water outlet pipe and the anode product discharge pipe all extend to the outside of the shell; the lower end of the shell is provided with a cathode water inlet pipe, and the upper part of the shell is provided with a cathode water outlet pipe; the cathode electrode and the anode electrode are both connected with external leads which extend to the outside of the shell. The invention can solve the problem of nitrogen and phosphorus removal of sewage with insufficient carbon source in China, realizes the recovery of nitrogen and phosphorus resources in the wastewater, and has a plurality of advantages of economy, environmental protection, resource recycling and the like.
Description
Technical Field
The invention belongs to the technical field of microbial fuel cells, and particularly relates to a zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal and a working method thereof.
Background
The amount of nutrients such as nitrogen, phosphorus and the like discharged into the natural water body exceeds the water body accepting capacity, so that the accepting water body is eutrophicated, aquatic organisms, particularly algae and some aquatic plants in the water body excessively grow and propagate, and the water body ecological system is damaged, so that the water body loses due functions. The eutrophication of water is a prominent global environmental problem, and the increasingly serious eutrophication of water brings great negative effects on human life, production and the whole ecological system.
The construction of sewage treatment plants is an effective method for reducing the sewage discharge amount in China, reducing the environmental load of water bodies and improving the quantity and quality of water for production and living of human beings. The biological wastewater treatment technology is the mainstream technology of modern town sewage treatment. The concentration of the organic matters in the wastewater after biological treatment basically reaches the standard, but the concentration of nitrogen and phosphorus still exceeds the standard. For such low C: N: P ratio wastewater, conventional denitrification processes have failed to meet emission standards because conventional denitrification processes require organic matter as an electron donor. Similarly, conventional biological phosphorus removal processes typically require organic matter to provide an energy source during biological phosphorus uptake. The shortage of carbon source has become a bottleneck factor for biological nitrogen and phosphorus removal of town sewage.
In recent years, iron and iron salts have been widely used in sewage treatment processes, including zero-valent iron, ferrous salts, and ferric salts. The ferrous autotrophic denitrification technology has been successfully realized in laboratory devices, and the technology utilizes ferrous salt to replace organic matters as an electron donor for denitrification, but the consumption of the ferric salt is huge.
Disclosure of Invention
The invention aims to solve the problem of nitrogen and phosphorus removal of sewage with low C: N: P ratio in China, improve the power generation and decontamination capability by changing the reaction configuration of a Microbial Fuel Cell (MFC), and provide a coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal based on zero-valent iron and a working method thereof.
The technical scheme adopted by the invention is as follows:
A zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal comprises a shell, and a sealing plate, a cathode electrode, an anode reactor and a cathode biological membrane which are arranged in the shell, wherein the cathode electrode and the anode reactor are arranged closely, and both the cathode electrode and the anode reactor are in a coil spring shape; the cathode biological membrane is arranged on the surface of the cathode electrode; the sealing plate is arranged at the upper part of the inner cavity of the shell, and the cathode electrode and the anode reactor are positioned at the lower part of the sealing plate; the upper ends of the cathode electrode and the anode reactor are both connected with the sealing plate, and the upper end of the anode reactor is hermetically connected with the sealing plate; the inner cavity of the anode reactor is an anode reaction zone, an anode electrode is arranged in the anode reactor, the anode electrode adopts zero-valent iron, the outer wall of the anode reactor is provided with a proton exchange membrane, and the proton exchange membrane is used for exchanging substances between the anode reaction zone and the cathode reaction zone; the upper end of the anode reactor is provided with an anode water inlet pipe, the lower end of the anode reactor is provided with an anode product discharge pipe and an anode water outlet pipe, and the anode water inlet pipe, the anode water outlet pipe and the anode product discharge pipe all extend to the outside of the shell; the lower end of the shell is provided with a cathode water inlet pipe, and the upper part of the shell is provided with a cathode water outlet pipe; the cathode electrode and the anode electrode are both connected with external leads which extend to the outside of the shell.
The lower end of the anode reactor is of a spiral descending structure, an anode water outlet pipe is arranged at the lower end of the edge of the anode spiral structure, and an anode product discharge pipe is arranged at the lower end of the center of the spiral structure.
The lower part of the shell is provided with a cathode biomembrane falling hopper which is funnel-shaped and is provided with a cathode biomembrane falling outlet.
When the lower end of the anode reactor is in a spiral descending structure, the lower end of the anode reactor extends into the cathode biomembrane falling hopper, and the anode product discharge pipe extends out of the cathode biomembrane falling discharge port.
The upper end of the anode electrode extends to the sealing plate, the lower end of the anode electrode extends to the bottom of the anode reactor, and the shape of the anode electrode is a coil spring shape which is the same as that of the anode reactor.
the upper end and the lower end of the anode reactor are not provided with end faces, the upper end of the anode reactor is hermetically connected with the sealing plate, the anode electrode is fixedly suspended on the sealing plate, and the upper end of the anode electrode is connected with an external lead; the lower end of the anode reactor is sealed by an anode silica gel sealing strip.
a plurality of longitudinal openings are arranged on the outer wall of the anode reactor at intervals, and the proton exchange membrane is arranged at the longitudinal openings.
The cathode electrode is wrapped outside the anode reactor and is close to the outer wall of the anode, and cathode biological films are arranged on two sides of the cathode electrode.
An electrogenesis substrate containing phosphate is filled in the anode reactor, an electrogenesis substrate containing nitrate is filled in the inner cavity of the shell, and DNRA bacteria are attached to the surface of the cathode biomembrane.
The material of shell and closing plate is PVC, and the material of anode reactor outer wall is organic glass.
a working method of a zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal comprises the following steps:
The anode reactor adopts sequencing batch operation, and wastewater containing phosphate enters an anode reaction area from an anode water inlet pipe to form anode electrolyte; the anode electrode loses electrons to become soluble ferrous ions which enter an anode reaction zone, and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate blue iron ore precipitates; the pyrite is discharged from an anode product discharge port through precipitation; discharging the treated phosphorus-free wastewater through an anode water outlet pipe;
Adopting sequencing batch operation, and enabling the nitrate-containing wastewater to enter a cathode reaction zone in an inner cavity of the shell through a cathode water inlet pipe in an ascending mass transfer mode to form cathode electrolyte;
when a loop is formed by connecting the cathode electrode and the anode electrode, the nitrate in the cathode electrolyte is converted into ammonia nitrogen by the microorganisms on the cathode biomembrane by using electrons lost from the anode electrode, and the generated waste water containing the ammonia nitrogen is discharged from the cathode water outlet pipe;
the anolyte and catholyte maintain charge balance through the proton exchange membrane on the outer wall of the anode reactor.
The invention has the following beneficial effects:
The microbial fuel cell of the invention adopts cheap and easily available zero-valent iron to replace organic matters as an electron donor for biological denitrification of wastewater in the prior art, thereby saving the cost; the anode electrode adopts zero-valent iron, and after the anode electrode and the cathode electrode are communicated, current can be generated through electron transfer, so that the resource recovery of electric energy is realized; the cathode electrode and the anode reactor are arranged closely and are both in coil spring shapes, so that the area of the opposite electrode is greatly increased, the mass transfer area is increased, and the decontamination capability of the fuel cell is enhanced while higher volume energy density is obtained. The anode reactor lower extreme is equipped with positive pole product discharge pipe and positive pole outlet pipe, therefore the anode reactor can separately discharge liquid and solid wherein, is convenient for retrieve respectively and utilizes, can avoid using special splitter to separate the processing to the discarded object that produces in the anode reactor simultaneously. The lower end of the shell is provided with a cathode water inlet pipe, and the upper part of the shell is provided with a cathode water outlet pipe, so that the microbial fuel cell can adopt an ascending mass transfer mode, and has better mass transfer effect compared with the traditional mass transfer mode.
Furthermore, the lower end of the anode reactor is of a spiral descending structure, an anode water outlet pipe is arranged at the lower end of the edge of the anode spiral structure, and an anode product discharge pipe is arranged at the lower end of the center of the spiral structure. The structure enables substances generated in the anode reactor to be subjected to solid-liquid separation, and the lower end of the anode reactor is of a spiral descending spiral structure, so that after heavier solid substances are generated, the solid substances descend to the bottom along the spiral structure and can be discharged through the anode product discharge pipe, the lighter liquid substances are discharged through the anode water outlet pipe with a higher position, and then the solid-liquid separation is directly realized in the oxygen reactor.
Furthermore, the lower part of the shell is provided with a cathode biological film falling hopper which is funnel-shaped, so that solid substances generated by the cathode can be gathered in the cathode biological film falling hopper, and the generated solid substances can be easily discharged through the cathode biological film falling discharge port by utilizing the gravity of the solid substances and the gravity of liquid substances on the upper part.
Furthermore, when the lower end of the anode reactor is in a spiral descending structure, the lower end of the anode reactor extends into the cathode biomembrane falling hopper, so that the effective reaction area of the anode electrode and the cathode electrode can be further increased, the volume energy density of the microbial fuel cell is increased, and the decontamination capability of the fuel cell is enhanced; the anode product discharge pipe extends out of the falling discharge outlet of the cathode biomembrane, so that the anode product discharge pipe can be straight up and down to avoid turning, solid matters generated by the anode can be discharged, and the solid matters generated by the cathode can be prevented from being deposited on the anode product discharge pipe and at the joint of the anode product discharge pipe and the shell or the falling bucket of the cathode biomembrane, so that incomplete pollution discharge is caused.
Furthermore, the upper end of the anode electrode extends to the sealing plate, the lower end of the anode electrode extends to the bottom of the anode reactor, and the anode electrode is in a coil spring shape which is the same as the anode reactor in shape, so that the surface area of the anode electrode is larger, the area of the opposite electrode is increased, the mass transfer area is increased, higher volume energy density can be obtained, the decontamination capability of the fuel cell is enhanced, and meanwhile, the material change period can be increased.
Furthermore, DNRA bacteria are attached to the surface of the cathode biological membrane, and can directly convert nitrate nitrogen into ammonia nitrogen, so that no nitrite nitrogen is accumulated in the microbial fuel cell.
When the microbial fuel cell works, the anode reactor adopts sequencing batch operation, and phosphate-containing wastewater enters an anode reaction area from an anode water inlet pipe to form anode electrolyte; the anode electrode loses electrons to become soluble ferrous ions which enter an anode reaction zone, and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate blue iron ore precipitates; the pyrite is discharged from an anode product discharge port through precipitation; discharging the treated phosphorus-free wastewater through an anode water outlet pipe; adopting sequencing batch operation, and enabling the nitrate-containing wastewater to enter a cathode reaction zone in the inner cavity of the shell through a cathode water inlet pipe in an ascending mass transfer mode to form cathode electrolyte; when a loop is formed by connecting the cathode electrode and the anode electrode, the nitrate in the cathode electrolyte is converted into ammonia nitrogen by the microorganisms on the cathode biomembrane by using electrons lost from the anode electrode, and the generated waste water containing the ammonia nitrogen is discharged from the cathode water outlet pipe; the anolyte and catholyte maintain charge balance through the proton exchange membrane on the outer wall of the anode reactor. Therefore, the working method of the microbial fuel cell is simple to operate, divalent iron and phosphorus form iron cyanite while phosphorus is removed in the anode reactor, the removal and recovery of phosphorus are realized, and the mass transfer effect is better when the cathode part adopts an ascending mass transfer mode compared with the traditional mass transfer mode.
Drawings
FIG. 1 is a front sectional view of a zero-valent iron-based coiled spring type microbial fuel cell for synchronous nitrogen and phosphorus removal;
3 fig. 3 2 3 is 3 a 3 cross 3- 3 sectional 3 view 3 taken 3 along 3 line 3 a 3- 3 a 3 of 3 fig. 3 1 3. 3
FIG. 3 is a partial view of the outer wall of the microbial fuel cell anode reactor based on zero-valent iron coil spring type synchronous nitrogen and phosphorus removal.
Fig. 4 is an enlarged schematic view of a portion B in fig. 1.
Fig. 5 is an enlarged schematic view of the portion C in fig. 1.
In the figure, 1-an electric signal acquisition system, 2-an external load, 3-an anode water inlet pipe, 4-an external lead, 5 shells, 6-a cathode water outlet pipe, 7-a cathode external lead port, 8-a sealing plate, 9-a cathode electrode, 10-an anode electrode and 11-an anode reactor outer wall, 12-cathode biomembrane, 13-anode silica gel sealing strip, 14-cathode water inlet pipe, 15-anode water outlet pipe, 16-water stop valve, 17-anode product discharge pipe, 18-anode external lead port, 19-anode reaction zone, 20-cathode reaction zone, 21-cathode biomembrane falling bucket, 22-cathode biomembrane falling discharge port, 23-proton exchange membrane, 24-organic glass, and 24-1-opening.
Detailed Description
the invention is further described with reference to the following detailed description of the invention and the accompanying drawings.
referring to fig. 1 and 2, the zero-valent iron-based coil spring type synchronous nitrogen and phosphorus removal microbial fuel cell of the invention comprises a housing 5, a sealing plate 8 arranged in the housing 5, a cathode electrode 9, an anode reactor and a cathode biological membrane 12, wherein the cathode electrode 9 and the anode reactor are arranged closely, and both the cathode electrode 9 and the anode reactor are in a coil spring shape; the cathode biological membrane 12 is arranged on the surface of the cathode electrode 9; the sealing plate 8 is arranged at the upper part of the inner cavity of the shell 5, and the cathode electrode 9 and the anode reactor are positioned at the lower part of the sealing plate 8; the upper ends of the cathode electrode 9 and the anode reactor are both connected with the sealing plate 8, and the upper end of the anode reactor is connected with the sealing plate 8 in a sealing way; the inner cavity of the anode reactor is an anode reaction zone 19, an anode electrode 10 is arranged in the anode reactor, the anode electrode 10 adopts zero-valent iron, a proton exchange membrane 23 is arranged on the outer wall 11 of the anode reactor, and the proton exchange membrane 23 is used for exchanging substances between the anode reaction zone 19 and the cathode reaction zone 20; the upper end of the anode reactor is provided with an anode water inlet pipe 3, the lower end of the anode reactor is provided with an anode product discharge pipe 17 and an anode water outlet pipe 15, and the anode water inlet pipe 3, the anode water outlet pipe 15 and the anode product discharge pipe 17 extend to the outside of the shell 5; the lower end of the shell 5 is provided with a cathode water inlet pipe 14, and the upper part of the shell 5 is provided with a cathode water outlet pipe 6; the cathode electrode 9 and the anode electrode 10 are both connected with an external lead 4, and the external lead 4 extends to the outside of the shell 5.
Referring to fig. 1, as a preferred embodiment of the present invention, the lower end of the anode reactor has a spiral structure spirally descending, an anode outlet pipe 15 is provided at the lower end of the edge of the spiral structure of the anode, and an anode product outlet pipe 17 is provided at the lower end of the center of the spiral structure.
referring to fig. 1, a cathode biofilm detachment funnel 21 is provided at a lower portion of the housing 5, the cathode biofilm detachment funnel 21 is funnel-shaped, and the cathode biofilm detachment funnel 21 is provided with a cathode biofilm detachment outlet 22.
referring to fig. 1, in a preferred embodiment of the present invention, when the lower end of the anode reactor has a spiral structure that spirally descends, the lower end of the anode reactor extends into a cathode biofilm falling hopper 21, and an anode product discharge pipe 17 extends from a cathode biofilm falling outlet 22.
Referring to fig. 1, 2 and 5, as a preferred embodiment of the present invention, the upper end of the anode electrode 10 extends to the sealing plate 8, the lower end of the anode electrode 10 extends to the bottom of the anode reactor, and the shape of the anode electrode 10 is a coil spring shape identical to the shape of the anode reactor.
Referring to fig. 1, 4 and 5, as a preferred embodiment of the present invention, both the upper and lower ends of the anode reactor have no end surface, the upper end of the anode reactor is hermetically connected with a sealing plate 8, an anode electrode 10 is suspended and fixed on the sealing plate 8, and the upper end of the anode electrode 10 is connected with an external lead 4; the lower end of the anode reactor is sealed by an anode silica gel sealing strip 13.
Referring to fig. 5, as a preferred embodiment of the present invention, a plurality of longitudinal openings 24-1 are spaced apart from each other on the outer wall 11 of the anode reactor, and a proton exchange membrane 23 is disposed at the longitudinal openings.
Referring to fig. 1, 2, 4 and 5, as a preferred embodiment of the present invention, a cathode electrode 9 is wrapped outside the anode reactor and is adjacent to an anode outer wall 11, and cathode biofilms 12 are disposed on both sides of the cathode electrode 9.
As a preferred embodiment of the invention, the anode reactor is filled with an electrogenesis substrate containing phosphate, the inner cavity of the shell 5 is filled with an electrogenesis substrate containing nitrate, and DNRA bacteria are attached to the surface of the cathode biological membrane 12.
In a preferred embodiment of the present invention, the material of the outer shell 5 and the sealing plate 8 is PVC, and the material of the outer wall 11 of the anode reactor is plexiglass.
Referring to fig. 1 and 2, the working method of the zero-valent iron-based coil spring type synchronous nitrogen and phosphorus removal microbial fuel cell of the invention comprises the following processes:
The anode reactor adopts sequencing batch operation, and wastewater containing phosphate enters an anode reaction zone 19 from an anode water inlet pipe 3 to form anode electrolyte; the anode electrode 10 loses electrons to become soluble divalent iron ions which enter the anode reaction zone 19, and the soluble divalent iron ions react with phosphate ions of the anode electrolyte to generate blue iron ore precipitates; the vivianite is discharged through the anode product discharge port 17 via precipitation; the treated wastewater without phosphorus is discharged from the anode water outlet pipe 15;
Adopting sequencing batch operation, leading the nitrate-containing wastewater to enter a cathode reaction zone 20 in the inner cavity of the shell 5 from a cathode water inlet pipe 14 in an ascending mass transfer mode to form cathode electrolyte;
when a loop is formed by connecting the cathode electrode 9 and the anode electrode 10, the microorganisms on the cathode biological membrane 12 convert nitrate in the cathode electrolyte into ammonia nitrogen by using electrons lost from the anode electrode 10, and the generated wastewater containing the ammonia nitrogen is discharged from the cathode water outlet pipe 6;
the anolyte and catholyte are maintained in charge balance by the proton exchange membrane 23 of the anode reactor outer wall 11.
Examples
As shown in fig. 1 and fig. 2, the zero-valent iron-based coiled spring type microbial fuel cell for simultaneous denitrification and dephosphorization comprises a housing 5, and a sealing plate 8, a cathode electrode 9, an anode reactor and a cathode biofilm 12 which are arranged in the housing 5, wherein the cathode electrode 9 and the anode reactor are arranged closely, and both the cathode electrode 9 and the anode reactor are in a coiled spring shape; the cathode biological membrane 12 is arranged on the surface of the cathode electrode 9; the sealing plate 8 is arranged at the upper part of the inner cavity of the shell 5, and the cathode electrode 9 and the anode reactor are positioned at the lower part of the sealing plate 8; the upper ends of the cathode electrode 9 and the anode reactor are both connected with the sealing plate 8, and the upper end of the anode reactor is connected with the sealing plate 8 in a sealing way; the inner cavity of the anode reactor is an anode reaction zone 19, an anode electrode 10 is arranged in the anode reactor, the anode electrode 10 adopts zero-valent iron, a proton exchange membrane 23 is arranged on the outer wall 11 of the anode reactor, and the proton exchange membrane 23 is used for exchanging substances between the anode reaction zone 19 and the cathode reaction zone 20; the upper end of the anode reactor is provided with an anode water inlet pipe 3, the lower end of the anode reactor is provided with an anode product discharge pipe 17 and an anode water outlet pipe 15, the anode product discharge pipe 17 and the anode water outlet pipe 15 are both provided with a water stop valve 16, and the anode water inlet pipe 3, the anode water outlet pipe 15 and the anode product discharge pipe 17 all extend to the outside of the shell 5; the lower end of the shell 5 is provided with a cathode water inlet pipe 14, and the upper part of the shell 5 is provided with a cathode water outlet pipe 6; the cathode electrode 9 and the anode electrode 10 are both connected with an external lead 4, the external lead 4 extends to the outside of the shell 5, and a cathode external lead port 7 and an anode external lead port 18 for the external lead 4 to penetrate out are arranged on the sealing plate 8. The lower part of the shell 5 is provided with a cathode biomembrane falling hopper 21, the cathode biomembrane falling hopper 21 is funnel-shaped, and the cathode biomembrane falling hopper 21 is provided with a cathode biomembrane falling outlet 22. The lower end of the anode reactor is of a spiral descending structure, an anode water outlet pipe 15 is arranged at the lower end of the edge of the anode spiral structure, and an anode product discharge pipe 17 is arranged at the lower end of the center of the spiral structure. The lower end of the anode reactor extends into a cathode biomembrane falling hopper 21, and an anode product discharge pipe 17 extends out from a cathode biomembrane falling discharge port 22. The upper end of the anode electrode 10 extends to the sealing plate 8, the lower end of the anode electrode 10 extends to the bottom of the anode reactor, and the shape of the anode electrode 10 is a coil spring shape which is the same as the shape of the anode reactor. The upper end and the lower end of the anode reactor are both provided with no end surface, the upper end of the anode reactor is hermetically connected with the sealing plate 8, the anode electrode 10 is fixedly suspended on the sealing plate 8, and the upper end of the anode electrode 10 is connected with the external lead 4; the lower end of the anode reactor is sealed by an anode silica gel sealing strip 13. The material of the outer wall 11 of the anode reactor is organic glass, a plurality of longitudinal openings 24-1 are arranged on the outer wall 11 of the anode reactor at intervals, and a proton exchange membrane 23 is arranged at the longitudinal openings. The cathode electrode 9 is wrapped outside the anode reactor and is close to the anode outer wall 11, and cathode biological films 12 are arranged on two sides of the cathode electrode 9. An anode reactor is filled with an electrogenesis substrate containing phosphate, an inner cavity of a shell 5 is filled with an electrogenesis substrate containing Nitrate, and DNRA bacteria (highly efficient Nitrate differentiation to Ammonium bacteria) are attached to the surface of a cathode biomembrane 12. The housing 5 and the sealing plate 8 are made of PVC. Wherein, the inner cavity of the anode reactor is an anode reaction area 19; the area outside the anode reactor in the inner cavity of the shell is used as a cathode reaction area 20, and the cathode water inlet pipe 14 is arranged at the lower end of the cathode reaction area 20, so that mass transfer can be carried out in an ascending mass transfer mode. The external lead 4 connected to the anode electrode 10 is connected to the cathode electrode 9 by extending into the cathode reaction region 20 via the anode external lead interface 18, and the anode water inlet pipe 3 is disposed above the center of the coil spring-like structure. The external lead 4 connected with the cathode electrode 9 extends into the anode reaction area 19 through the cathode external lead interface 7 to be connected with the anode electrode 10. The cathode electrode 9 is fixed to the sealing plate 8 in a suspended manner. The housing 5 is a sealed housing.
When the biofuel cell is detected, as shown in fig. 1, a load 2 is arranged on an external lead 4, two ends of the load are connected in parallel with an electric signal acquisition system 1, and the anode chamber matrix and the cathode chamber matrix are subjected to material exchange through a proton exchange membrane on the outer wall 11 of an anode reactor.
Specifically, the size and the proportion of the above components can be set according to actual conditions. In the solution of this embodiment, the ratio of the minimum inner diameter to the maximum outer diameter of the coil spring structure formed by winding the anode reaction zone 19 and the cathode electrode 9 is 1: 48, the number of turns of the coil spring-shaped structure is 3, and the height-diameter ratio of the coil spring-shaped structure is 25: 6. the distance from the anode water inlet pipe 3 to the top of the anode reaction zone 19 is 1/10 of the height of the anode reaction zone 19. The anode electrode 10 is a pure iron sheet with the thickness of 2mm, and the height of the anode electrode 10 is consistent with that of the anode reaction zone 19. The height-to-length ratio of the anode electrode 10 is 1:9, and the ratio of the surface area to the total volume of the anode reaction zone 19 is 1cm2:50cm3The anode electrode 10 is fixedly suspended from the upper end and the lower end and penetrates through the whole anode reaction area 19. The bottom of the anode reaction zone 19 spirally descends from the edge to the center to form a slope, so that anode products can be conveniently collected. The bottom of the anode reaction zone 19 is provided with an anode product discharge pipe 17.
The height-diameter ratio of the shell 5 is 14: 5, the distance from the cathode water outlet pipe 6 to the top of the shell 5 is 1/8 of the total height of the shell 5, and the headspace ratio is 12.5%. The cathode electrode 9 is made of carbon felt and has a thickness of 2mm, and the height of the cathode electrode 9 extends downwards from the sealing plate to the cathode biomembrane falling bucket 21. The cathode electrode 9 has a height-to-length ratio of 1:9, and a ratio of the surface area to the total volume of the cathode portion of 1cm2:50cm3. The included angle between the biomembrane falling collecting hopper 21 and the horizontal direction is 30 degrees, and the ratio of the inner diameter of the cathode biomembrane falling discharge port 22 to the inner diameter of the biomembrane falling collecting hopper is 1: 64.
As shown in FIG. 3, the outer wall 11 of the anode reactor is formed by alternately arranging a proton exchange membrane 23 and organic glass 24, and the ratio of the area of the proton exchange membrane to the surface area of the outer wall 11 of the anode reactor is 1cm2:1.5cm2. Anode reaction zoneThe anode silica gel sealing strip 13 at the bottom end is wrapped by organic glass and is connected with the anode water outlet pipe 15. The anode electrolyte (containing phosphate) and the cathode electrolyte (containing nitrate) are separated by a proton exchange membrane 23 on the outer wall 11 of the anode reactor, and the ratio of the area of the proton exchange membrane 23 to the surface area of the anode electrode 10 is 1cm2:1.5cm2. Through tests, the sizes and the proportions can well fulfill the test aim of the invention.
The working process of the microbial fuel cell of the embodiment is as follows: the anode part adopts sequencing batch operation, and simulated wastewater containing phosphate enters an anode reaction zone 19 from an anode water inlet pipe 3 to form anode electrolyte; the iron sheet of the anode electrode 10 loses electrons to become soluble ferrous ions and enters an anode reaction zone 19, and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate iron pyrite precipitate; the vivianite is discharged through the anode product discharge port 17 via precipitation; the treated wastewater without phosphorus is discharged from the anode water outlet pipe 15. The lost electrons of the anode electrode 10 are transmitted to the cathode electrode 9 through the external lead 4, and the electric signals generated in the process are detected by the electric signal acquisition system 1. The cathode part adopts sequencing batch operation, and the nitrate-containing simulated wastewater enters a cathode reaction zone 20 from a cathode water inlet pipe 14 in an ascending mass transfer mode to form cathode electrolyte; the microorganisms on the cathode biomembrane 12 on the cathode electrode 9 utilize electrons from the anode part to dissimilarly reduce nitrate in the power consumption substrate, so that the nitrate in the cathode electrolyte is converted into ammonia nitrogen, and the generated wastewater containing the ammonia nitrogen is discharged from the cathode water outlet pipe 6 and can be treated in the next step; along with the reaction, the outer layer of the cathode biological film 12 is gradually aged and falls off, and the fallen biological film is collected by the fallen biological film collecting hopper 21 and then is discharged by the fallen biological film discharging port 22. The anolyte and catholyte maintain charge balance of the anode and cathode portions through the proton exchange membrane of the anode reactor outer wall 11.
In conclusion, the invention has the advantages that 1) cheap and easily available zero-valent iron is adopted to replace organic matters to be used as an electron donor for biological denitrification of wastewater, thereby saving the cost; 2) the ferrous iron and the phosphorus form iron cyanite when the phosphorus is removed from the anode part, and the removal and recovery of the phosphorus are realized at the same time, and the iron cyanite can be used for processing ornaments or manufacturing drawing dyes after being collected; 3) the DNRA bacteria at the cathode part can directly convert nitrate nitrogen into ammonia nitrogen without accumulation of nitrite nitrogen; 4) zero-valent iron is adopted as an anode electrode, carbon felt is adopted as a cathode electrode, and current is generated between the electrodes through electron transfer, so that the resource recovery of electric energy is realized; 5) the cathode part adopts an ascending mass transfer mode, and compared with the traditional mass transfer mode, the mass transfer effect is better; 6) by adopting the coil spring type configuration, the area of the opposite electrode is greatly increased, the mass transfer area is increased, and the decontamination capability of the fuel cell is enhanced while higher volume energy density is obtained.
Claims (10)
1. A zero-valent iron-based coil spring type microbial fuel cell capable of synchronously removing nitrogen and phosphorus is characterized by comprising a shell (5), and a sealing plate (8), a cathode electrode (9), an anode reactor and a cathode biological membrane (12) which are arranged in the shell (5), wherein the cathode electrode (9) and the anode reactor are arranged closely, and the cathode electrode (9) and the anode reactor are both in a coil spring shape; the cathode biological membrane (12) is arranged on the surface of the cathode electrode (9); the sealing plate (8) is arranged at the upper part of the inner cavity of the shell (5), and the cathode electrode (9) and the anode reactor are positioned at the lower part of the sealing plate (8); the upper ends of the cathode electrode (9) and the anode reactor are both connected with the sealing plate (8), and the upper end of the anode reactor is hermetically connected with the sealing plate (8); the inner cavity of the anode reactor is an anode reaction zone (19), an anode electrode (10) is arranged in the anode reactor, the anode electrode (10) adopts zero-valent iron, a proton exchange membrane (23) is arranged on the outer wall (11) of the anode reactor, and the proton exchange membrane (23) is used for carrying out material exchange between the anode reaction zone (19) and the cathode reaction zone (20); the upper end of the anode reactor is provided with an anode water inlet pipe (3), the lower end of the anode reactor is provided with an anode product discharge pipe (17) and an anode water outlet pipe (15), and the anode water inlet pipe (3), the anode water outlet pipe (15) and the anode product discharge pipe (17) all extend to the outside of the shell (5); the lower end of the shell (5) is provided with a cathode water inlet pipe (14), and the upper part of the shell (5) is provided with a cathode water outlet pipe (6); the cathode electrode (9) and the anode electrode (10) are both connected with an external lead (4), and the external lead (4) extends to the outside of the shell (5).
2. the zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal is characterized in that the lower end of the anode reactor is of a spiral structure which descends spirally, an anode water outlet pipe (15) is arranged at the lower end of the edge of the spiral structure of the anode, and an anode product discharge pipe (17) is arranged at the lower end of the center of the spiral structure.
3. The zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal is characterized in that a cathode biofilm falling hopper (21) is arranged at the lower part of the shell (5), the cathode biofilm falling hopper (21) is funnel-shaped, and the cathode biofilm falling hopper (21) is provided with a cathode biofilm falling outlet (22).
4. The zero-valent iron based coil spring type microbial fuel cell for simultaneous nitrogen and phosphorus removal is characterized in that when the lower end of the anode reactor is in a spiral structure with spiral descending, the lower end of the anode reactor extends into a cathode biofilm falling hopper (21), and an anode product discharge pipe (17) extends out of a cathode biofilm falling discharge outlet (22).
5. the zero-valent iron-based coiled spring type simultaneous nitrogen and phosphorus removal microbial fuel cell is characterized in that the upper end of the anode electrode (10) extends to the sealing plate (8), the lower end of the anode electrode (10) extends to the bottom of the anode reactor, and the shape of the anode electrode (10) is a coiled spring shape which is the same as the shape of the anode reactor.
6. The zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal is characterized in that the upper end and the lower end of the anode reactor are not provided with end faces, the upper end of the anode reactor is hermetically connected with a sealing plate (8), an anode electrode (10) is fixedly suspended on the sealing plate (8), and the upper end of the anode electrode (10) is connected with an external lead (4); the lower end of the anode reactor is sealed by an anode silica gel sealing strip (13); a plurality of longitudinal openings are arranged on the outer wall (11) of the anode reactor at intervals, and a proton exchange membrane (23) is arranged at the longitudinal openings.
7. The zero-valent iron-based coiled spring type microbial fuel cell for synchronous nitrogen and phosphorus removal is characterized in that a cathode electrode (9) is wrapped outside an anode reactor and is close to an anode outer wall (11), and cathode biological membranes (12) are arranged on two sides of the cathode electrode (9).
8. The zero-valent iron-based coiled spring type microbial fuel cell for synchronous nitrogen and phosphorus removal is characterized in that an anode reactor is filled with an electricity generating substrate containing phosphate, an inner cavity of a shell (5) is filled with an electricity consuming substrate containing nitrate, and DNRA bacteria are attached to the surface of a cathode biological membrane (12).
9. The zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal, according to claim 1, characterized in that the outer casing (5) and the sealing plate (8) are made of PVC, and the outer wall (11) of the anode reactor is made of organic glass.
10. The operating method of the zero-valent iron-based coiled spring type synchronous nitrogen and phosphorus removal microbial fuel cell is characterized by comprising the following steps of:
The anode reactor adopts sequencing batch operation, and wastewater containing phosphate enters an anode reaction zone (19) from an anode water inlet pipe (3) to form anode electrolyte; the anode electrode (10) loses electrons to become soluble ferrous ions and enters an anode reaction zone (19), and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate a blue iron ore precipitate; the pyrite is discharged from an anode product discharge port (17) through precipitation; the treated wastewater without phosphorus is discharged from an anode water outlet pipe (15);
Adopting sequencing batch operation, and enabling the nitrate-containing wastewater to enter a cathode reaction zone (20) in the inner cavity of the shell (5) from a cathode water inlet pipe (14) in an ascending mass transfer mode to form cathode electrolyte;
When a loop is formed by connecting the cathode electrode (9) and the anode electrode (10), the nitrate in the cathode electrolyte is converted into ammonia nitrogen by the microorganisms on the cathode biomembrane (12) by using electrons lost from the anode electrode (10), and the generated wastewater containing the ammonia nitrogen is discharged from the cathode water outlet pipe (6);
the anolyte and catholyte are maintained in charge balance by a proton exchange membrane (23) in the outer wall (11) of the anode reactor.
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