CN110563158B - Coil spring type synchronous nitrogen and phosphorus removal microbial fuel cell based on zero-valent iron and working method thereof - Google Patents
Coil spring type synchronous nitrogen and phosphorus removal microbial fuel cell based on zero-valent iron and working method thereof Download PDFInfo
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- CN110563158B CN110563158B CN201910926511.9A CN201910926511A CN110563158B CN 110563158 B CN110563158 B CN 110563158B CN 201910926511 A CN201910926511 A CN 201910926511A CN 110563158 B CN110563158 B CN 110563158B
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 46
- 239000000446 fuel Substances 0.000 title claims abstract description 33
- 230000000813 microbial effect Effects 0.000 title claims abstract description 29
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 25
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 title claims abstract description 24
- 229910052698 phosphorus Inorganic materials 0.000 title claims abstract description 23
- 239000011574 phosphorus Substances 0.000 title claims abstract description 23
- 230000001360 synchronised effect Effects 0.000 title claims abstract description 19
- 238000000034 method Methods 0.000 title claims abstract description 15
- 229910052757 nitrogen Inorganic materials 0.000 title claims abstract description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 78
- 238000007789 sealing Methods 0.000 claims abstract description 57
- 239000002351 wastewater Substances 0.000 claims abstract description 25
- 239000012528 membrane Substances 0.000 claims abstract description 24
- 238000006243 chemical reaction Methods 0.000 claims description 44
- 239000003792 electrolyte Substances 0.000 claims description 20
- 229910002651 NO3 Inorganic materials 0.000 claims description 18
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 18
- CWYNVVGOOAEACU-UHFFFAOYSA-N Fe2+ Chemical compound [Fe+2] CWYNVVGOOAEACU-UHFFFAOYSA-N 0.000 claims description 15
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 15
- XKMRRTOUMJRJIA-UHFFFAOYSA-N ammonia nh3 Chemical compound N.N XKMRRTOUMJRJIA-UHFFFAOYSA-N 0.000 claims description 12
- 229910001448 ferrous ion Inorganic materials 0.000 claims description 11
- 239000011159 matrix material Substances 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
- 239000000126 substance Substances 0.000 claims description 9
- 229910052742 iron Inorganic materials 0.000 claims description 8
- 230000000630 rising effect Effects 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
- 239000000741 silica gel Substances 0.000 claims description 6
- 229910002027 silica gel Inorganic materials 0.000 claims description 6
- 230000005611 electricity Effects 0.000 claims description 5
- 239000011521 glass Substances 0.000 claims description 5
- 244000005700 microbiome Species 0.000 claims description 5
- 238000001556 precipitation Methods 0.000 claims description 5
- 239000013049 sediment Substances 0.000 claims description 5
- 229910052984 zinc sulfide Inorganic materials 0.000 claims description 5
- 239000010865 sewage Substances 0.000 abstract description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 4
- 229910052799 carbon Inorganic materials 0.000 abstract description 4
- 238000011084 recovery Methods 0.000 abstract description 4
- 230000007613 environmental effect Effects 0.000 abstract description 3
- 239000007787 solid Substances 0.000 description 8
- 238000005202 decontamination Methods 0.000 description 5
- 230000003588 decontaminative effect Effects 0.000 description 5
- 239000007788 liquid Substances 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 230000000694 effects Effects 0.000 description 4
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
- 238000000926 separation method Methods 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 2
- VVQNEPGJFQJSBK-UHFFFAOYSA-N Methyl methacrylate Chemical compound COC(=O)C(C)=C VVQNEPGJFQJSBK-UHFFFAOYSA-N 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
- 229920005372 Plexiglas® Polymers 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
- 238000009825 accumulation Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000012851 eutrophication Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 230000005484 gravity Effects 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000004064 recycling Methods 0.000 description 2
- 230000027756 respiratory electron transport chain Effects 0.000 description 2
- 241000195493 Cryptophyta Species 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 230000001174 ascending effect Effects 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
- 238000011021 bench scale process Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000002551 biofuel Substances 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 239000000975 dye Substances 0.000 description 1
- 159000000014 iron salts Chemical class 0.000 description 1
- 239000008239 natural water Substances 0.000 description 1
- 235000015097 nutrients Nutrition 0.000 description 1
- 239000005416 organic matter Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 238000004065 wastewater treatment 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
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- Life Sciences & Earth Sciences (AREA)
- Chemical & Material Sciences (AREA)
- Microbiology (AREA)
- General Chemical & Material Sciences (AREA)
- Electrochemistry (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Water Supply & Treatment (AREA)
- Environmental & Geological Engineering (AREA)
- Hydrology & Water Resources (AREA)
- Biodiversity & Conservation Biology (AREA)
- Biochemistry (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Health & Medical Sciences (AREA)
- Molecular Biology (AREA)
- Water Treatment By Electricity Or Magnetism (AREA)
Abstract
The invention discloses a coil spring type microbial fuel cell based on zero-valent iron for synchronous denitrification and dephosphorization and a working method thereof, wherein a cathode electrode and an anode reactor are in coil spring shapes; the cathode biomembrane is arranged on the surface of the cathode electrode; the upper ends of the cathode electrode and the anode reactor are 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 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 connected with external leads which extend to the outside of the shell. The invention can solve the difficult problems of denitrification and dephosphorization of sewage with insufficient carbon source in China, realizes the recovery of nitrogen and phosphorus resources of the wastewater, and has the advantages of economy, environmental protection, resource reutilization 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 capable of synchronously removing nitrogen and phosphorus 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 admitting capability, so that the receiving water body is eutrophicated, aquatic organisms in the water body, particularly algae and some aquatic plants, overgrow and propagate, and the ecological system of the water body is destroyed, thereby losing the proper functions of the water body. Water eutrophication is a prominent global environmental problem, and increasingly serious water eutrophication causes 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 of China, reducing the environmental load of water bodies and improving the quantity and quality of water for human production and living. 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 CNP ratio wastewater, conventional denitrification processes have failed to meet emission standards because the conventional denitrification process requires organics as electron donors. Likewise, conventional biological phosphorus removal processes also typically require organic matter to provide energy materials during biological phosphorus uptake. The shortage of carbon source has become the bottleneck factor for biological denitrification and dephosphorization of town sewage.
In recent years, iron and ferric salts have been widely used in sewage treatment processes, including zero-valent iron, divalent ferric salt, trivalent ferric salt, and the like. Ferrous autotrophic denitrification technology has been successfully implemented in laboratory bench scale equipment, which utilizes ferrous iron salts instead of organics as electron donors for denitrification, but iron salts are consumed in huge amounts.
Disclosure of Invention
The invention aims to solve the difficult problem of nitrogen and phosphorus removal of low C: N: P ratio sewage in China, improves the electricity generation and decontamination capacity by changing the reaction configuration of a Microbial Fuel Cell (MFC), and provides a zero-valent iron-based coil spring type microbial fuel cell for synchronous nitrogen and phosphorus removal and a working method thereof.
The technical scheme adopted by the invention is as follows:
a coil spring type synchronous denitrification and dephosphorization microbial fuel cell based on zero-valent iron comprises a shell, and a sealing plate, a cathode electrode, an anode reactor and a cathode biomembrane which are arranged in the shell, wherein the cathode electrode and the anode reactor are arranged in close proximity, and the cathode electrode and the anode reactor are in coil spring shapes; the cathode biomembrane 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 connected with the sealing plate, and the upper end of the anode reactor is connected with the sealing plate in a sealing way; the inner cavity of the anode reactor is an anode reaction zone, an anode electrode is arranged in the anode reactor, zero-valent iron is adopted as the anode electrode, a proton exchange membrane is arranged on the outer wall of the anode reactor, and the proton exchange membrane is used for carrying out substance exchange 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 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 connected with external leads which extend to the outside of the shell.
The lower end of the anode reactor is in a spiral structure with spiral descending, the anode water outlet pipe is arranged at the lower end of the edge of the anode spiral structure, and the 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 the cathode biomembrane falling hopper is provided with a cathode biomembrane falling outlet.
When the lower end of the anode reactor is in a spiral structure of spiral descending, the lower end of the anode reactor stretches into the cathode biomembrane falling hopper, and the anode product discharge pipe stretches out from 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 coil spring-shaped which is the same as that of the anode reactor.
The upper end and the lower end of the anode reactor are respectively provided with an end face, the upper end of the anode reactor is in sealing connection with the sealing plate, the anode electrode is suspended and fixed 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.
The outer wall of the anode reactor is provided with a plurality of longitudinal openings at intervals, and the proton exchange membrane is arranged at the longitudinal openings.
The cathode electrode is wrapped outside the anode reactor and is closely adjacent to the outer wall of the anode, and both sides of the cathode electrode are provided with cathode biomembranes.
The anode reactor is filled with an electrogenesis matrix containing phosphate, the inner cavity of the shell is filled with an electricity consumption matrix containing nitrate, and DNRA bacteria are attached to the surface of the cathode biomembrane.
The shell and the sealing plate are made of PVC, and the outer wall of the anode reactor is made of organic glass.
A working method of a zero-valent iron-based coil spring type synchronous denitrification and dephosphorization microbial fuel cell comprises the following steps:
the anode reactor adopts sequencing batch operation, and the waste water containing phosphate enters an anode reaction zone from an anode water inlet pipe to form anode electrolyte; the anode electrode loses electrons to become soluble ferrous ions, and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate blue iron ore sediment; the wustite is discharged from the anode product discharge outlet through precipitation; the treated wastewater without phosphorus is discharged from an anode water outlet pipe;
adopting sequencing batch operation, enabling the wastewater containing nitrate to enter a cathode reaction zone of the inner cavity of the shell by adopting a rising mass transfer mode from a cathode water inlet pipe to form a cathode electrolyte;
when the cathode electrode and the anode electrode are connected to form a loop, microorganisms on the cathode biological film convert nitrate in the cathode electrolyte into ammonia nitrogen by utilizing electrons lost from the anode electrode, and the generated wastewater containing the ammonia nitrogen is discharged from a cathode water outlet pipe;
the anolyte and catholyte maintain charge balance through the proton exchange membrane of the anode reactor outer wall.
The invention has the following beneficial effects:
the microbial fuel cell adopts low-cost and easily-obtained zero-valent iron to replace the organic matters in the prior art as the electron donor for biological denitrification of the wastewater, so the cost is saved; the anode electrode adopts zero-valent iron, and after the anode electrode is connected with the cathode electrode, current can be generated through electron transfer, so that the recycling recovery of electric energy is realized; the cathode electrode and the anode reactor are closely arranged, and are in coil spring shape, 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 the higher volume energy density is obtained. The lower end of the anode reactor is provided with an anode product discharge pipe and an anode water outlet pipe, so that the anode reactor can separate and discharge liquid and solid in the anode reactor, is convenient to recycle and utilize respectively, and can avoid using special separation equipment to separate and treat wastes generated in the anode reactor. 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 a rising mass transfer mode, and has better mass transfer effect compared with the traditional mass transfer mode.
Further, the lower end of the anode reactor is in a spiral structure with spiral descending, the anode water outlet pipe is arranged at the lower end of the edge of the anode spiral structure, and the anode product discharge pipe is arranged at the lower end of the center of the spiral structure. The structure enables the substances generated in the anode reactor to be subjected to solid-liquid separation, and as the lower end of the anode reactor is in a spiral structure with spiral descending, after the heavier solid substances are generated, the solid substances descend to the bottom along the spiral structure and can be discharged through an anode product discharge pipe, and the lighter liquid substances are discharged through an anode water outlet pipe with a higher position, so that the solid-liquid separation is directly realized in the oxygen reactor.
Furthermore, the lower part of the shell is provided with a cathode biomembrane falling hopper which is funnel-shaped, so that solid matters generated by the cathode can be gathered in the cathode biomembrane falling hopper, and the generated solid matters can be easily discharged through a cathode biomembrane falling outlet by utilizing the gravity of the solid matters and the gravity action of upper liquid matters.
Furthermore, when the lower end of the anode reactor is in a spiral structure with spiral descending, the lower end of the anode reactor stretches 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 from the cathode biomembrane falling-off outlet, firstly, the anode product discharge pipe can be directly upwards and downwards prevented from turning, solid matters generated by the anode can be discharged, secondly, the solid matters generated by the cathode can be prevented from being deposited on the anode product discharge pipe and the connection part of the anode product discharge pipe and the shell or the cathode biomembrane falling-off hopper, and the pollution discharge is incomplete.
Further, 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 coil spring-shaped which is the same as that of the anode reactor, 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 the refueling period can be increased.
Furthermore, DNRA bacteria are attached to the surface of the cathode biological film, and can directly convert nitrate nitrogen into ammonia nitrogen, so that the microbial fuel cell has no accumulation of nitrite nitrogen.
When the microbial fuel cell works, the anode reactor adopts sequencing batch operation, and the waste water containing phosphate enters an anode reaction zone from an anode water inlet pipe to form anode electrolyte; the anode electrode loses electrons to become soluble ferrous ions, and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate blue iron ore sediment; the wustite is discharged from the anode product discharge outlet through precipitation; the treated wastewater without phosphorus is discharged from an anode water outlet pipe; adopting sequencing batch operation, enabling the wastewater containing nitrate to enter a cathode reaction zone of the inner cavity of the shell by adopting a rising mass transfer mode from a cathode water inlet pipe to form a cathode electrolyte; when the cathode electrode and the anode electrode are connected to form a loop, microorganisms on the cathode biological film convert nitrate in the cathode electrolyte into ammonia nitrogen by utilizing electrons lost from the anode electrode, and the generated wastewater containing the ammonia nitrogen is discharged from a cathode water outlet pipe; the anolyte and catholyte maintain charge balance through the proton exchange membrane of the anode reactor outer wall. Therefore, the working method of the microbial fuel cell is simple to operate, and ferrous iron and phosphorus form wustite while phosphorus is removed in the anode reactor, phosphorus is removed and recovered at the same time, and the cathode part adopts an ascending mass transfer mode, so that the mass transfer effect is better compared with the traditional mass transfer mode.
Drawings
FIG. 1 is a front cross-sectional view of a zero-valent iron-based coil spring type microbial fuel cell for synchronous denitrification and dephosphorization of the invention;
FIG. 2 is a cross-sectional view taken along line A-A of FIG. 1.
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 denitrification and dephosphorization.
Fig. 4 is an enlarged schematic view of the portion B in fig. 1.
Fig. 5 is an enlarged schematic view of the portion C in fig. 1.
In the figure, a 1-electric signal acquisition system, a 2-external load, a 3-anode water inlet pipe, a 4-external lead, a 5-shell, a 6-cathode water outlet pipe, a 7-cathode external lead port, an 8-sealing plate, a 9-cathode electrode, a 10-anode electrode, an 11-anode reactor outer wall, a 12-cathode biomembrane, a 13-anode silica gel sealing strip, a 14-cathode water inlet pipe, a 15-anode water outlet pipe, a 16-water stop valve, a 17-anode product discharge pipe, a 18-anode external lead port, a 19-anode reaction zone, a 20-cathode reaction zone, a 21-cathode biomembrane dropping hopper, a 22-cathode biomembrane dropping outlet, a 23-proton exchange membrane, 24-organic glass and a 24-1-opening.
Detailed Description
The invention will be further described with reference to the following drawings and detailed description.
Referring to fig. 1 and 2, the zero-valent iron-based coil spring type synchronous denitrification and dephosphorization microbial fuel cell of the invention comprises a shell 5, and a sealing plate 8, a cathode electrode 9, an anode reactor and a cathode biomembrane 12 which are arranged in the shell 5, wherein the cathode electrode 9 and the anode reactor are arranged in close proximity, and the cathode electrode 9 and the anode reactor are in coil spring shapes; the cathode biological film 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 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, zero-valent iron is adopted as the anode electrode 10, 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 substance exchange between the anode reaction zone 19 and a 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 connected with an external lead 4, and the external lead 4 extends to the outside of the housing 5.
As a preferred embodiment of the present invention, referring to fig. 1, the anode reactor has a spiral structure in which the lower end is spirally lowered, an anode outlet pipe 15 is provided at the lower end of the edge of the anode spiral structure, and an anode product discharge pipe 17 is provided at the lower end of the center of the spiral structure.
As a preferred embodiment of the present invention, referring to fig. 1, a cathode biofilm removal hopper 21 is provided at a lower portion of the housing 5, the cathode biofilm removal hopper 21 is funnel-shaped, and the cathode biofilm removal hopper 21 is provided with a cathode biofilm removal outlet 22.
As a preferred embodiment of the present invention, referring to fig. 1, when the lower end of the anode reactor has a spiral structure of spirally descending, the lower end of the anode reactor is projected into the cathode biofilm removal hopper 21, and the anode product discharge pipe 17 is projected from the cathode biofilm removal discharge port 22.
As a preferred embodiment of the present invention, referring to fig. 1, 2 and 5, 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.
As a preferred embodiment of the present invention, referring to fig. 1, 4 and 5, the anode reactor has no end surfaces at both upper and lower ends, the upper end of the anode reactor is hermetically connected with the sealing plate 8, the anode electrode 10 is suspended and fixed to 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.
As a preferred embodiment of the present invention, referring to fig. 5, the anode reactor outer wall 11 is provided with a plurality of longitudinal openings 24-1 at intervals, and the proton exchange membrane 23 is provided at the longitudinal openings.
As a preferred embodiment of the present invention, referring to fig. 1, 2, 4 and 5, the cathode electrode 9 is wrapped around the outside of the anode reactor and is adjacent to the anode outer wall 11, and the cathode biofilm 12 is provided on both sides of the cathode electrode 9.
As a preferred embodiment of the invention, the anode reactor is filled with an electrogenesis matrix containing phosphate, the inner cavity of the shell 5 is filled with an electricity consumption matrix containing nitrate, and DNRA bacteria are attached to the surface of the cathode biological film 12.
In a preferred embodiment of the present invention, the material of the casing 5 and the sealing plate 8 is PVC, and the material of the anode reactor outer wall 11 is plexiglass.
Referring to fig. 1 and 2, the working method of the zero-valent iron-based coil spring type synchronous denitrification and dephosphorization microbial fuel cell of the invention comprises the following steps:
the anode reactor adopts sequencing batch operation, and the waste water 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 which enter an anode reaction zone 19, and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate blue iron ore sediment; the wurtzite is discharged through the anode product discharge outlet 17 through precipitation; the treated wastewater without phosphorus is discharged from an anode water outlet pipe 15;
adopting sequencing batch operation, enabling the wastewater containing nitrate to enter a cathode reaction zone 20 in the inner cavity of the shell 5 by adopting a rising mass transfer mode from a cathode water inlet pipe 14 to form a cathode electrolyte;
when the cathode electrode 9 and the anode electrode 10 are connected to form a loop, microorganisms on the cathode biological film 12 convert nitrate in the cathode electrolyte into ammonia nitrogen by utilizing 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 maintain charge balance through the proton exchange membrane 23 of the anode reactor outer wall 11.
Examples
As shown in fig. 1 and 2, the coiled spring type synchronous denitrification and dephosphorization microbial fuel cell based on zero-valent iron in the embodiment comprises a shell 5, a sealing plate 8, a cathode electrode 9, an anode reactor and a cathode biological film 12, wherein the sealing plate 8, the cathode electrode 9 and the anode reactor are arranged in close proximity, and the cathode electrode 9 and the anode reactor are in coiled spring shapes; the cathode biological film 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 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, zero-valent iron is adopted as the anode electrode 10, 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 substance exchange between the anode reaction zone 19 and a 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, water stop valves 16 are respectively arranged on the anode product discharge pipe 17 and the 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, 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 through which the external lead 4 passes are arranged on the sealing plate 8. The lower part of the shell 5 is provided with a cathode biological film falling-off hopper 21, the cathode biological film falling-off hopper 21 is funnel-shaped, and the cathode biological film falling-off hopper 21 is provided with a cathode biological film falling-off outlet 22. The lower end of the anode reactor is in a spiral structure with spiral descending, 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 biofilm removal hopper 21, and an anode product discharge pipe 17 extends from a cathode biofilm removal discharge outlet 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 identical to the shape of the anode reactor. The upper end and the lower end of the anode reactor are respectively provided with an end face, the upper end of the anode reactor is in sealing connection with the sealing plate 8, the anode electrode 10 is suspended and fixed 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 outer wall 11 of the anode reactor is made of organic glass, a plurality of longitudinal openings 24-1 are arranged on the outer wall 11 of the anode reactor at intervals, and the 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 both sides of the cathode electrode 9 are provided with cathode biomembranes 12. The anode reactor is filled with an electrogenesis matrix containing phosphate, the inner cavity of the shell 5 is filled with an electricity consumption matrix containing nitrate, DNRA bacteria (high-efficiency nitrate is reduced into ammonium bacteria (Dissimilatory Nitrate Reduction to Ammonium)) are attached to the surface of the cathode biomembrane 12. The shell 5 and the sealing plate 8 are made of PVC. Wherein the inner cavity of the anode reactor is an anode reaction zone 19; in the inner cavity of the shell, the area outside the anode reactor is taken as a cathode reaction zone 20, and a cathode water inlet pipe 14 is arranged at the lower end of the cathode reaction zone 20, so that mass transfer can be carried out in a rising mass transfer mode. The external lead 4 connected to the anode electrode 10 extends into the cathode reaction zone 20 through the anode external lead interface 18 to be connected with the cathode electrode 9, and the anode water inlet pipe 3 is arranged above the center of the coil spring-shaped structure. The external lead 4 connected to the cathode electrode 9 is connected to the anode electrode 10 via the cathode external lead interface 7 and then extends into the anode reaction zone 19. The cathode electrode 9 is suspended and fixed to the sealing plate 8. 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 to an electric signal acquisition system 1, and an anode chamber matrix and a cathode chamber matrix exchange substances through a proton exchange membrane of an outer wall 11 of an anode reactor.
Specifically, the dimensions and proportions of the above-described components may be set as appropriate. In the scheme of the embodiment, the ratio of the minimum inner diameter to the maximum outer diameter of the coil spring-like structure in which the anode reaction region 19 and the cathode electrode 9 are wound is 1:48, the coil spring-shaped structure has 3 turns, and the height-to-diameter ratio of the coil spring-shaped structure is 25:6. the distance from the anode 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 the height of the anode reaction zone 19.The anode electrode 10 had a height to length ratio of 1:9 and a surface area to total volume of the anode reaction zone 19 of 1cm 2 :50cm 3 The anode electrode 10 is fixedly suspended from the lower end of the upper end and penetrates the entire anode reaction zone 19. The bottom of the anode reaction zone 19 is spirally lowered 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-to-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 top duty ratio is 12.5%. The cathode electrode 9 is made of carbon felt with the thickness of 2mm, and the height of the cathode electrode 9 extends downwards from the sealing plate to the cathode biomembrane falling hopper 21. The cathode electrode 9 has a height-to-length ratio of 1:9 and a ratio of a surface area to a total volume of the cathode portion of 1cm 2 :50cm 3 . The included angle between the biofilm falling-off collecting hopper 21 and the horizontal direction is 30 degrees, and the ratio of the inner diameter of the cathode biofilm falling-off discharge outlet 22 to the inner diameter of the biofilm falling-off collecting hopper is 1:64.
As shown in FIG. 3, the anode reactor outer wall 11 is formed by alternately arranging a proton exchange membrane 23 and a plexiglass 24, and the ratio of the area of the proton exchange membrane to the surface area of the anode reactor outer wall 11 is 1cm 2 :1.5cm 2 . The anode silica gel sealing strip 13 at the bottom end of the anode reaction zone is wrapped by organic glass and is connected with the anode water outlet pipe 15. The anolyte (containing phosphate) and catholyte (containing nitrate) are isolated by a proton exchange membrane 23 of the outer wall 11 of the anode reactor, the ratio of the area of the proton exchange membrane 23 to the surface area of the anode electrode 10 being 1cm 2 :1.5cm 2 . Through experiments, the sizes and the proportions can well fulfill the aim of the experiment.
The microbial fuel cell of this example works as follows: the anode part adopts sequencing batch operation, and the 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 which enter an anode reaction zone 19, and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate blue iron ore sediment; the wurtzite is discharged through the anode product discharge outlet 17 through precipitation; the treated wastewater without phosphorus is discharged from the anode water outlet pipe 15. The electrons lost by 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 simulated wastewater containing nitrate enters the cathode reaction zone 20 by adopting a rising mass transfer mode from the cathode water inlet pipe 14 to form a cathode electrolyte; microorganisms on a cathode biological film 12 on a cathode electrode 9 utilize electrons from an anode part to dissimilarly reduce nitrate in a power consumption matrix, nitrate in a cathode electrolyte is converted into ammonia nitrogen, and the generated wastewater containing the ammonia nitrogen is discharged from a cathode water outlet pipe 6 and can be subjected to the next treatment; as the reaction proceeds, the outer layer of the cathode biofilm 12 gradually ages and falls off, and the falling-off biofilm is collected by the falling-off biofilm collecting hopper 21 and discharged from the falling-off biofilm discharge outlet 22. The anolyte and catholyte maintain charge balance in 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) the low-cost and easily-obtained zero-valent iron is adopted to replace organic matters to be used as an electron donor for biological denitrification of wastewater, so that the cost is saved; 2) The anode part removes phosphorus and simultaneously ferrous iron and phosphorus form wurtzite, and the removal and recovery of the phosphorus are realized, and the wurtzite can be used for processing ornaments or making drawing dyes after being collected; 3) The DNRA bacteria in the cathode part can directly convert nitrate nitrogen into ammonia nitrogen, so that no accumulation of nitrite nitrogen exists; 4) The anode electrode adopts zero-valent iron, the cathode electrode adopts carbon felt, and current is generated between the electrodes through electron transfer, so that the recycling recovery of electric energy is realized; 5) The cathode part adopts a rising mass transfer mode, and compared with the traditional mass transfer mode, the mass transfer effect is better; 6) The coil spring type structure is adopted, 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 the higher volume energy density is obtained.
Claims (8)
1. The coil spring type synchronous nitrogen and phosphorus removal microbial fuel cell based on zero-valent iron is characterized by comprising a shell (5), a sealing plate (8), a cathode electrode (9), an anode reactor and a cathode biomembrane (12), wherein the sealing plate (8), the cathode electrode (9), the anode reactor and the cathode biomembrane (12) are arranged in the shell (5), the cathode electrode (9) and the anode reactor are arranged in close proximity, and the cathode electrode (9) and the anode reactor are in a coil spring shape; the cathode biomembrane (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 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, zero-valent iron is adopted for the anode electrode (10), 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 substance exchange between the anode reaction zone (19) and a cathode reaction zone (20); an anode water inlet pipe (3) is arranged at the upper end of the anode reactor, an anode product discharge pipe (17) and an anode water outlet pipe (15) are arranged at the lower end of the anode reactor, 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 connected with an external lead (4), and the external lead (4) extends to the outside of the shell (5);
the lower end of the anode reactor is in a spiral structure with spiral descending, 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 anode reactor is filled with an electrogenesis matrix containing phosphate, the inner cavity of the shell (5) is filled with an electricity consumption matrix containing nitrate, and DNRA bacteria are attached to the surface of the cathode biomembrane (12).
2. The zero-valent iron-based coil spring type synchronous nitrogen and phosphorus removal microbial fuel cell according to claim 1, wherein a cathode biofilm removal hopper (21) is arranged at the lower part of the shell (5), the cathode biofilm removal hopper (21) is funnel-shaped, and the cathode biofilm removal hopper (21) is provided with a cathode biofilm removal outlet (22).
3. A zero-valent iron-based coil spring type synchronous denitrification and dephosphorization microbial fuel cell according to claim 2, characterized in that when the lower end of the anode reactor is in a spiral structure of spiral descending, the lower end of the anode reactor extends into the cathode biofilm removal hopper (21), and the anode product discharge pipe (17) extends out from the cathode biofilm removal discharge port (22).
4. The zero-valent iron-based coil spring type synchronous nitrogen and phosphorus removal microbial fuel cell according to claim 1, wherein 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 like a coil spring with the same shape as the anode reactor.
5. The zero-valent iron-based coil spring type synchronous denitrification and dephosphorization microbial fuel cell is characterized in that the upper end and the lower end of an anode reactor are not provided with end surfaces, the upper end of the anode reactor is in sealing connection 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); 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.
6. A zero-valent iron-based coil spring type synchronous denitrification and dephosphorization microbial fuel cell according to claim 1, characterized in that the cathode electrode (9) is wrapped outside the anode reactor and is close to the anode outer wall (11), and the cathode biomembrane (12) is arranged on both sides of the cathode electrode (9).
7. The zero-valent iron-based coil spring type synchronous denitrification and dephosphorization microbial fuel cell according to claim 1, wherein the shell (5) and the sealing plate (8) are made of PVC, and the outer wall (11) of the anode reactor is made of organic glass.
8. A method of operating a zero-valent iron-based coiled spring synchronous nitrogen and phosphorus removal microbial fuel cell according to any one of claims 1 to 7, comprising the steps of:
the anode reactor adopts sequencing batch operation, and the waste water 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, the soluble ferrous ions enter an anode reaction zone (19), and the soluble ferrous ions react with phosphate ions of the anode electrolyte to generate blue iron ore sediment; the wurtzite is discharged from the anode product discharge outlet (17) through precipitation; the treated wastewater without phosphorus is discharged from an anode water outlet pipe (15);
adopting sequencing batch operation, enabling the wastewater containing nitrate to enter a cathode reaction zone (20) in the inner cavity of the shell (5) by adopting a rising mass transfer mode from a cathode water inlet pipe (14) to form a cathode electrolyte;
when the cathode electrode (9) and the anode electrode (10) are connected to form a loop, microorganisms on the cathode biological film (12) convert nitrate in the cathode electrolyte into ammonia nitrogen by utilizing 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 maintain charge balance through the proton exchange membrane (23) of the anode reactor outer wall (11).
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