CN101118973A - Microbiological fuel cell device and battery and use and water treatment system - Google Patents
Microbiological fuel cell device and battery and use and water treatment system Download PDFInfo
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- CN101118973A CN101118973A CNA2006101040815A CN200610104081A CN101118973A CN 101118973 A CN101118973 A CN 101118973A CN A2006101040815 A CNA2006101040815 A CN A2006101040815A CN 200610104081 A CN200610104081 A CN 200610104081A CN 101118973 A CN101118973 A CN 101118973A
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
A microorganism fuel cell device comprises an outer cover(1) of the fuel cell, an anode chamber(3), an anode(13), a cathode chamber(4), a cathode(16) and a septum(17). Wherein, the anode(13) is positioned inside the anode chamber(3); the septum(17) is positioned between the anode chamber(30) and the cathode chamber(4). The cathode(16) is a slice-shaped cathode, one surface of the slice-shaped cathode and one surface of septum(17) are jointed to form a septum cathode component(10); the surface of slice-shaped cathode not jointing with the septum(17) is positioned at one side of the cathode chamber(4). As the disclosed microorganism fuel cell device forms the septum cathode component by jointing the slice-shaped cathode with the septum, the invention further improves the moving efficiency of the media and also speeds up the cathode reaction, so that the overall reacting speed of the microorganism fuel cell for the device is greatly improved. Therefore, the invention can realize the large scaled successive disposal of the waste water.
Description
Technical field
The invention relates to a kind of fuel-cell device and battery with this device, and the using method of this battery and the sewage disposal system that comprises this battery, especially about a kind of microbial fuel cell unit with have the microbiological fuel cell of this device, and the using method of this battery and comprise the sewage disposal system of this battery.
Background technology
Pollution of waterhead is harm the widest maximum pollution, and for the purpose of protection environment, pollutant especially sewage must reach national pollutant emission standard, therefore must handle sewage.The method of sewage disposal comprises physical treatment process, method of chemical treatment, physicochemical treatment method, biological treatment and their combination.At present, being rich in organic high chemical oxygen demand (COD) value sewage mainly utilizes biological treatment to focus on by sewage treatment plant.The most frequently used biological treatment mainly comprises two kinds in the sewage disposal: a kind of is to make good use of oxygen animalcule to carry out the aeration processing in cesspool, but aeration belongs to the high energy consumption process, makes the cost of sewage disposal very high, is unfavorable for the popularization of this method; Another kind is to utilize anaerobe the oxidation operation in the cesspool to be decomposed into small-molecule substances such as carbon dioxide and methane, but the Anaerobic Treatment process can not with whole organic substances all exhaustive oxidation become carbon dioxide, therefore micro-molecular gas such as methane, the carbon monoxide etc. of this process generation are comprehended surrounding air generation secondary pollution in case can not get appropriate location.Therefore need better to handle the method for organic wastewater, neither need the aeration process of high energy consumption, simultaneously again can be with the organic substance exhaustive oxidation.
Chaudhuri and Lovley are at Electricity generation by direct oxidation of glucosein mediator-less microbial fuel cells.Nature Biotechnology 2003, propose to adopt alienation reduction bacterium among the 21:1229-1232, make up microbiological fuel cell with special metabolic characteristic.Such alienation reduction bacterium extensively is present in the mud of bottom sediment, river bottom, irrigation canals and ditches, can be with multiple organic substance as metabolism substrate, and for example can be with the electron donor in the respiration (as glucose, acetate, Sodium Benzoate etc.) complete oxidation; Be that metal oxide (as the oxide of iron, manganese, cobalt) with solid is as electron acceptor simultaneously.Solid metal oxide is reduced in its metabolic process, and organic substrates is oxidized to carbon dioxide.It is fuel that the microbiological fuel cell that makes up with above-mentioned alienation bacterium can utilize the organic substance in the sewage, is carbon dioxide with its exhaustive oxidation, produces electric energy simultaneously.
CN1164509C discloses a kind of biological fuel cell, and as shown in Figure 4, this battery comprises anode chamber that contains conducting medium respectively 3 and the cathode chamber 4 that is positioned at biological fuel cell inside; Be placed in the anode 13 in the anode chamber 3; Be placed in the negative electrode 16 in the cathode chamber 4; And the barrier film 17 between anode chamber 3 and cathode chamber 4 (being amberplex); Wherein anode chamber 3 contains organic wastewater and activated sludge and keep anaerobic condition in the operating process of biological fuel cell.This biological fuel cell can use the organic substance in the electro-chemical activity microbiological oxidation waste water in waste water and the activated sludge, and the electronics that oxidation produced flows out the extracellular, directly transfers on the electrode, thereby handle waste water when producing electric current.But the solution in this cell cathode chamber 4 need continue to feed the oxygen that reaches capacity and could work, and the solubility of oxygen in water is low, and can cause the concentration polarization of cathode chamber 4, so not only consumes energy but also can not effectively utilize the effective electromotive force of oxygen, also can increase the internal resistance of battery simultaneously, finally cause protolysis efficient low; In addition, this biological fuel cell can only be criticized the formula batch process to sewage, and promptly a collection of sewage disposal finishes, and needs to discharge anode chamber solution by valve 2 earlier, and the next group sewage that reinjects can not be disposed of sewage continuous large-scale; Need large-area expensive proton exchange membrane because of this battery simultaneously, so cost is very high.
A kind of microbiological fuel cell is disclosed among the CN 2745229Y, this battery mainly is made of anode cavity, negative electrode cavity and the dividing plate between them, utilize saccharomyces cerevisiae metabolism organic substrates glucose, with the potassium ferricyanide and Ferrous Fumarate as electron acceptor, with graphite rod as anode and negative electrode, thereby utilize the energy that microbial consumption glucose emits to produce electric energy.But equally also need big proton exchange membrane on this battery separator, cost is higher; The electro-chemical activity of the selected saccharomyces cerevisiae of this battery is low simultaneously, be not easy to lose the electronics of its cell membrane outer surface, make that the electromotive force of this battery is on the low side, must utilize materials such as the potassium ferricyanide and Ferrous Fumarate to come replace oxygen, improve the oxidation-reduction potential of cathode chamber, just have tangible electric current, protolysis efficient is low; And the potassium ferricyanide has very strong toxicity, is not suitable for being applied in the actual microbiological fuel cell.And because brewer's yeast is very strict to the requirement of condition of culture, so this utility model can not be used for treatment of Organic Wastewater.
In sum, there is the inefficient defective of protolysis in existing microbiological fuel cell, can not be used for disposing of sewage continuously on a large scale and the cost height, therefore, need a kind of microbiological fuel cell that can overcome the prior art aforementioned disadvantages, protolysis efficient height can be disposed of sewage on a large scale continuously non-secondary pollution, can produce electric energy by low-cost high-efficiency again simultaneously.
Summary of the invention
The objective of the invention is to overcome the prior art microbiological fuel cell and have the inefficient shortcoming of protolysis, a kind of microbial fuel cell unit that can make the protolysis efficient raising of microbiological fuel cell is provided.
Second purpose of the present invention provides the microbiological fuel cell that comprises this microbial fuel cell unit.
The 3rd purpose of the present invention provides the using method of microorganism fuel cell.
The 4th purpose of the present invention provides a kind of sewage disposal system that comprises microorganism fuel cell.
The invention provides a kind of microbial fuel cell unit, this device comprises battery case 1, anode chamber 3, anode 13, cathode chamber 4, negative electrode 16 and barrier film 17; Described anode 13 is arranged in anode chamber 3, barrier film 17 is between anode chamber 3 and cathode chamber 4, wherein, described negative electrode 16 is a plate-like cathode, fit and form film cathode assembly 10 in a surface of surface of plate-like cathode and barrier film 17, plate-like cathode is not positioned at cathode chamber 4 one sides with the one side that barrier film 17 is fitted.
The present invention also provides a kind of microbiological fuel cell, this battery comprises microbial fuel cell unit, is arranged in the electro-chemical activity microbe of this device, and working solution and/or working gas, wherein, described microbial fuel cell unit is a microbial fuel cell unit provided by the invention.
The invention provides the using method of microorganism fuel cell, this method comprises:
1) external circuit and the negative electrode 16 of microbiological fuel cell are connected with anode 13 to constitute the loop;
2) add working solution in the anode chamber 3, and to make working solution be 20-30 hour in the time of staying of anode chamber 3; In cathode chamber 4, add working solution or feed working gas.
The present invention also provides a kind of sewage disposal system that comprises microbiological fuel cell, and wherein, described microbiological fuel cell is a microbiological fuel cell provided by the invention.
According to the present invention, because fitting by plate-like cathode and barrier film, described microbial fuel cell unit constitutes the film cathode assembly, thereby can improve the efficient of protolysis, then accelerate cathode reaction speed, use the W-response speed of the microbiological fuel cell of this device to increase substantially, therefore can realize the extensive processing continuously of sewage.
Description of drawings
Fig. 1 is the embodiment of the invention 1 an inner core barrel structural representation;
Fig. 2 is the structural profile schematic diagram of the embodiment of the invention 1 microbial fuel cell unit;
Fig. 3 is the structural profile schematic diagram of the embodiment of the invention 2 microbial fuel cell units;
Fig. 4 is the structural profile schematic diagram of prior art microbial fuel cell unit;
Fig. 5 is the process schematic representation of sewage disposal system of the present invention;
Fig. 6 is the graph of a relation that chemical oxygen demand (COD) value of the embodiment of the invention 1 organic wastewater changed with the microbiological fuel cell decomposition time.
Among the figure:
1---battery case 2---valve
3---anode chamber 4---cathode chamber
5---anode inlet 6---anode export
7---cathode inlet 8---cathode outlet
9---wire netting 10---film cathode assembly
11---interior tube stent 12---mesh
13---anode 14---plunger water pump
15---air blast 16---negative electrode
17---barrier film
Embodiment
Microbial fuel cell unit provided by the invention comprises battery case 1, anode chamber 3, anode 13, cathode chamber 4, negative electrode 16 and barrier film 17; Described anode 13 is arranged in anode chamber 3, barrier film 17 is between anode chamber 3 and cathode chamber 4, wherein, described negative electrode 16 is a plate-like cathode, fit and form film cathode assembly 10 in a surface of surface of plate-like cathode and barrier film 17, plate-like cathode is not positioned at cathode chamber 4 one sides with the one side that barrier film 17 is fitted.
Fitting and form film cathode assembly 10 in a surface of surface of described plate-like cathode and barrier film 17, can be by pressing (as hot pressing) or method realization well known in the art such as bonding.The negative electrode of the microbial fuel cell unit of prior art is generally selected bar-shaped graphite cathode for use, usually finish by intermediate medium and barrier film between protolysis; And microbial fuel cell unit of the present invention adopts a surface of surface of plate-like cathode and plate-like cathode and barrier film to fit to form the film cathode assembly, proton is once producing on the barrier film and need not directly just can moving on the negative electrode by intermediate medium like this, thereby can improve the efficient of protolysis, then accelerate cathode reaction speed, finally can improve the W-response speed of the microbiological fuel cell that uses this device.Therefore, the area on described plate-like cathode surface is at least 75% of barrier film 17 surface areas, and the area on preferred plate-like cathode surface is the 90-100% of barrier film 17 surface areas.Plate-like cathode of the present invention is selected from the material that this area plate-like cathode commonly used such as charcoal cloth, carbon paper etc. can be made plate-like cathode, the charcoal cloth of preferred good toughness.
It is plate-like cathode that microbial fuel cell unit of the present invention removes described negative electrode 16, fit and form film cathode assembly 10 in a surface of surface of plate-like cathode and barrier film 17, plate-like cathode is not positioned at outside cathode chamber 4 one sides with the one side that barrier film 17 is fitted, structure to other parts of microbial fuel cell unit has no particular limits, can adopt structure of the prior art, for example disclosed structure among CN 2745229Y or the CN 1164509C.Microbiological cell device of the present invention can be as shown in Figure 3, described negative electrode 16 is a plate-like cathode, fit and form film cathode assembly 10 in a surface of surface of plate-like cathode and barrier film 17, battery case 1 is formed anode chamber 3 and cathode chamber 4 with film cathode assembly 10; Other structures are identical with as shown in Figure 4 prior art microbiological cell device, all are arranged in anode chamber 3 such as the two anode 13.
More preferably, microbial fuel cell unit of the present invention has following structure (as shown in Figure 2): described microbial fuel cell unit comprises urceolus and the inner core that is enclosed within the urceolus, and the barrel of described battery urceolus is a battery case 1; Anode 13 is positioned at described anode chamber 3 (being the space between the barrel of the barrel of inner core and urceolus); Space between the barrel of described inner core and the barrel of urceolus is an anode chamber 3; The barrel of described inner core comprises a surface of plate-like cathode and a film cathode assembly 10 of fitting and form in the surface of barrier film 17, and plate-like cathode is not positioned at inner core with the one side that barrier film 17 is fitted; Space in the described inner core is a cathode chamber 4.The barrel of described urceolus is a battery case 1, can select for use this area material that is used as battery case commonly used such as glass, thermoplastics, heat fixing character plastics, metal etc. to make.
The urceolus of described sleeve and the shape of inner core also have no particular limits, as long as inner core can be included in the urceolus, just can realize making full use of the purpose in space; Because material of the same area surrounds the spatial volume maximum that columniform tube can surround, and the cylindrical dead angle problem that do not exist, therefore the cross section of the urceolus of preferred described sleeve and inner core is circular.The volume ratio of described anode chamber 3 and cathode chamber 4 has no particular limits, and the volume ratio of preferred described anode chamber 3 and cathode chamber 4 was greater than 1: 1, and promptly the volume of anode chamber is greater than cathode chamber.The volume ratio of more preferably described anode chamber 3 and cathode chamber 4 is 2: 1 to 100: 1.The volume of anode chamber is big more, and the anode that can hold is many more, and then the total surface area of anode is big more, thereby can adhere to more relatively microbe on the anode, helps improving the ability to work of microbiological fuel cell.The volume of cathode chamber is little, and it is low more to surround the more little cost of the used barrier film of cathode chamber (being proton exchange membrane) area.Described barrier film is that proton exchange membrane can be the proton exchange membrane that this area is usually used in microbiological cell device, and its kind has been conventionally known to one of skill in the art.Proton exchange membrane can be commercially available, and for example the Nafion film of being produced by E.I.Du Pont Company comprises Nafion112 film, Nafion115 film, Nafion117 film, Nafion1035 film etc.
As shown in Figure 2, described anode chamber 3 also comprises anode inlet 5 and anode export 6, there is no particular limitation for the relative position of antianode inlet 5 of the present invention and anode export 6, preferred described anode inlet 5 is lower than anode export 6, closes 6 described anode chamber 3 of sealing of described anode inlet 5 and anode export.Described cathode chamber 4 also comprises cathode inlet 7 and cathode outlet 8, and there is no particular limitation to the two relative position in the present invention.
As shown in Figure 1, the barrel of described inner core also comprises the wire netting 9 between film cathode assembly 10 and anode chamber 3, and described wire netting 9 is fitted with the barrier film face of film cathode assembly 10.Described wire netting 9 plays and prevents that barrier film from peeling off the effect that comes off, and the wire netting that can function as described above may be used to the present invention such as stainless steel fine-structure mesh, aluminium alloy net, titanium alloy reticulated etc.In addition, the barrel of described inner core also comprises the interior tube stent 11 between film cathode assembly 10 and cathode chamber 4, and described interior tube stent 11 is fitted with the cathode plane of film cathode assembly 10.Tube stent 11 plays the reinforced membrane cathode assembly in described, and keep the effect of film cathode assembly and whole inner core shape, therefore, tube stent 11 preferably can play the inorganic material of mechanical support effect such as glass, thermoplastics, heat fixing character plastics, metal etc. and makes in described.This support is mesh 12 structures (as shown in Figure 1), can guarantee that gas or the liquid in the cathode chamber 4 arrives film cathode assembly 10 easily.Described mesh 12 plays ventilative effect, and the big more air permeable effect of mesh is good more, but mesh is crossed the mechanical strength of the whole interior tube stent 11 of conference influence, and therefore the diameter of preferred described mesh 12 is the 0.5-5 millimeter.
Preferred described anode 13 is a graphite rod.Described graphite rod is the microorganism carrier of microbiological fuel cell normally, and the graphite rod that has a microbe contacts to finish the electrode reaction of microbiological fuel cell with the working solution of anode chamber usually.The number of described graphite rod is many more, graphite rod with microbe also many more, total contact area of working solution is big more in graphite rod and the anode chamber, the efficient of the anode that obtains thus is high more, but graphite rod is too much, can make the total amount of anode chamber working solution very few or influence it and flow, therefore the number of preferred described graphite rod is 3-10, and more preferably number is 4-8; The cumulative volume of described graphite rod accounts for the 10-70% of the total measurement (volume) of described anode chamber 3 (being the space between the barrel of the barrel of inner core and urceolus), more preferably 10-40%.The diameter of described graphite rod should be less than the width of anode chamber 3.Preferred described graphite rod evenly distributes in described anode chamber 3 (being the space between the barrel of the barrel of inner core and urceolus), can make distributing in anode chamber or flowing more evenly of working solution.Described even distribution is preferably graphite rod and is spacedly distributed on circle, and this circle is the center of circle with the inner core center of circle, and this diameter of a circle is the mean value of inner diameter of steel flue and urceolus diameter.
Microbiological fuel cell provided by the invention comprises microbial fuel cell unit, is arranged in the electro-chemical activity microbe of this device, and working solution and/or working gas, wherein, described microbial fuel cell unit is a microbial fuel cell unit provided by the invention.
The present invention has no particular limits described electro-chemical activity microbe, and every microbe that utilizes organic substance to make substrate, generation electric energy can both be realized goal of the invention of the present invention.Preferred described electro-chemical activity microbe is oxidation of organic compounds and produces electron discharge to the extracellular, is transferred to electronics produces electric current to electrode microbe.When cultivating anaerobe, need not power consumption processes such as aeration, therefore preferred anaerobe.Described anaerobe can be the anaerobe that separates from sewage, also can (bacterial concentration is 10 for high nectar degree
5More than the bacteria/milliliters) the activation bacterium liquid of alienation reduction bacterium bacterial classification.Described alienation reduction bacterium bacterial classification can be for need not the organic various alienation reduction bacterium of power consumption process exhaustive oxidation such as aeration, for example the microbe of Geobacter Pseudomonas etc.In addition, the anaerobe that separates from sewage can survive in the environment of 10-80 ℃ of pH5-9 temperature, but its growth optimum condition is 30 ℃, pH neutrality, be more suitable in therefrom separating the sewage environment of this bacterium, carrying out various physiological metabolism activities, therefore microbiological fuel cell of the present invention can be used for handling at normal temperatures neutral sewage, and effect is best, most economical.Graphite anode rod need have described electro-chemical activity microbe usually, and preferred described electro-chemical activity microbe is inlayed or attached on the graphite rod.Make graphite rod have the electro-chemical activity microbe and can adopt method well known in the art, such as there being structures such as groove, coarse decorative pattern, hole on set effect that utilizes electro-chemical activity microbe itself or the graphite rod, described microbe can be inlayed wherein.
Also comprise anode working liquid in the anode chamber 3 of microbiological fuel cell of the present invention, described anode working liquid can be sewage, especially is rich in the organic sewage of organic high COD value, also can be the special prepared culture that microbe can utilize.The preferred sewage of the present invention, microbe in the microbiological fuel cell of the present invention can be carbon dioxide with the organic substance exhaustive oxidation in the sewage by the metabolism decomposition on the one hand, the energy that produces in this process can be converted into electric energy, can also reach the effect of disposing of sewage on the other hand.
Also comprise negative electrode working solution or working gas in the cathode chamber 4 of described microbiological fuel cell, feed the negative electrode working solution in cathode chamber 4 after, the negative electrode working solution provides electron acceptor, and the reaction of assurance battery electrode is finished.Described negative electrode working solution can be oxygen saturation water, also can be lower than the solution of the anode working liquid that feeds anode chamber for this area oxidation-reduction potential commonly used.Described working gas is oxygen or air.Preferably feed above-mentioned gas to cathode chamber, resistance is little, less energy consumption, and sufficient electron acceptor can be provided.Negative electrode working solution or working gas feed from cathode inlet 7, discharge from cathode outlet 8.
When preparing microbiological fuel cell of the present invention, can adopt this area method commonly used is to add nutrient medium in the anode chamber, and inoculation has the microbe of electro-chemical activity then.Preferred sealing anode chamber forms anaerobic environment, leaves standstill and cultivates the anaerobe with electro-chemical activity.Simultaneously can in cathode chamber, feed working solution or working gas, preferably in cathode chamber, feed working gas, help to accelerate the metabolic process of microbe, promote to have microbe on the graphite anode rod.
Described inoculum concentration with microbe of electro-chemical activity is the 5-15% that kind of daughter bacteria solution accounts for total liquor capacity in the anode chamber, preferred 10%; Wherein, planting the microbe density of daughter bacteria solution and the microbe density in the anode nutrient solution of inoculation back can measure by total protein determination method in this area method commonly used such as viable count method, the nutrient solution etc.For example, the bacterial concentration of planting daughter bacteria solution according to the viable count method as can be known 10
5More than the bacteria/milliliters.The degree that graphite anode rod has a microbe can record that the total protein content result determines indirectly in the anodic dissolution according to the specification of BCA (bicinchoninic acid) protein detection reagent kit.According to the present invention, when the total protein content in the anode nutrient solution after the inoculated and cultured reaches the 5-20 mg/litre, when preferably reaching the 8-10 mg/litre, promptly can think to have had enough microbes on the graphite rod, can form microbiological fuel cell.In addition, can also detect graphite anode rod by this area method commonly used and whether as often as possible have the microbe that is inoculated, for example on the battery external circuit, connect resistance, and the variation of writing down its voltage, through 10-15 days, above-mentioned voltage slowly rises to stationary value, proves that microbial cell forms fine and close network structure on the graphite anode rod surface.
Even without enrichment process, also can realize the present invention, but because to have the concentration of microbe of electro-chemical activity low, the kind daughter bacteria solution with electro-chemical activity microbe, microbe inoculation in the anode chamber are then cultivated in therefore preferred first enrichment.The method of microorganism that described enrichment culture has electro-chemical activity is conventionally known to one of skill in the art, generally comprise from the anaerobic sludge of river bottom or irrigation canals and ditches deep layer and take a sample, the preferred river bed layer mud that will flow through as the organic sewage of working solution, cultivate at anaerobic condition (as nutrient solution) lower seal with selective medium with the nitrogen deoxygenation, the lowering of concentration of the oxidizing substance (as Fe (III)) that quantitatively adds in the monitoring culture medium during 60-80%, (volume with initial selective medium is a benchmark to get the nutrient solution that part growth has microbe, get the nutrient solution of 10-30%) going down to posterity is transferred in the fresh selective medium, go down to posterity repeatedly to get the microbe with electro-chemical activity of enrichment culture for three times.Gained comprises the nutrient solution of the microbe with electro-chemical activity, can be used as the kind daughter bacteria solution of preparation microbiological fuel cell.Since in the microbe of enrichment from mud except that great majority for the anaerobism alienation reduction bacterium, also comprise a small amount of facultative aerobic microbe, can consume the dissolved oxygen in the nutrient medium, therefore the nutrient medium of anode chamber can not carry out deoxygenation, but preferred deoxygenation, more preferably two step deoxygenations before inoculation and after the inoculation.Deoxygenation can be carried out with the method that this area is known altogether, such as feed the nitrogen deoxygenation in fluid nutrient medium.
The using method of microbiological fuel cell provided by the invention comprises:
1) external circuit and the negative electrode 16 of microbiological fuel cell are connected with anode 13 to constitute the loop;
2) add working solution in the anode chamber 3, and to make working solution be 20-30 hour in the time of staying of anode chamber 3; In cathode chamber 4, add working solution or feed working gas.
Step 1) adopts this area method commonly used that the external circuit and the negative electrode 16 of microbiological fuel cell are connected with anode 13 to constitute the loop.Wherein, the circuit of being made up of electric elements such as the electrical appliance beyond the power supply, telegraph key, leads is an external circuit, and external circuit of the present invention can comprise electric elements such as electrical appliance, telegraph key, lead.
Step 2) adds working solution in the described anode chamber 3, can intermittently add also and can add continuously.Adding working solution in the preferred described anode chamber 3 is to add working solution in the anode chamber 3 continuously, and the working solution after the electro-chemical activity microbe is decomposed is discharged anode chamber 3 continuously.Simultaneously can in cathode chamber 4, feed working solution or working gas, preferably in cathode chamber 4, feed working gas.When adding anode working liquid continuously, the graphite anode rod that has microbe is static, in the case, because the metabolic activity of microbe carries out always, therefore redox reaction is able to carry out continuously on anode 13, the refuse of microbial metabolism is taken away by the working solution that flows, free electron that metabolic response produces and hydrogen ion constantly see through barrier film 17 (being proton exchange membrane) and are delivered to plate-like cathode chamber 4, working solution or the working gas reaction that feeds with cathode chamber 4 and being consumed, the Conversion of energy that is discharged simultaneously is an electric energy.If when feeding working gas, keep its flow be the 50-60 liter/minute.Formula is followed in the metering of the described anode working liquid time of staying: the time of staying=the anode chamber volume/rate.The described time of staying of anode working liquid in anode chamber is under the situation of organic wastewater at anode working liquid, i.e. the time of the processing organic wastewater of microbiological fuel cell of the present invention.The chemical oxygen demand of organic wastewater (COD) value constantly descends with the prolongation of microbial decomposition time in the microbiological fuel cell of the present invention, but overstand, then can reduce the discharging efficiency of microbiological fuel cell, if but the anode working liquid time of staying is too short, the abundant organic substance in the disintegration liquid of microbe then, the therefore preferred time of staying is 20-30 hour.
The present invention also provides a kind of sewage disposal system that comprises microbiological fuel cell, and wherein, described microbiological fuel cell is a microbiological fuel cell provided by the invention.As shown in Figure 5, microbiological fuel cell can be used as the core part of sewage disposal system, finishes sewage disposal.Sewage is purified in the anode chamber 3 of microorganism battery, and the COD value reduces, and meanwhile microorganism battery produces electric energy.
The present invention is described further below in conjunction with embodiment.
Embodiment 1
Present embodiment illustrates microbial fuel cell unit provided by the invention and has the microbiological fuel cell of this device, and the using method of this battery and the sewage disposal system that comprises this battery.
(1) preparation of microbial fuel cell unit
As shown in Figure 1, in cylindrical polymethyl methacrylate the barrel outer surface of tube stent 11 successively in the pressing with should in identical charcoal cloth, Nafion117 film and the stainless (steel) wire of barrel exterior surface area of tube stent 11, make the inner core barrel.The area on plate-like cathode (charcoal cloth) surface is 100% of barrier film (being a Nafion117 proton exchange membrane) surface area, and the two is fitted and forms film cathode assembly 10.Tube stent 11 interior diameters are 4 centimetres in described, and long 50 centimetres, 2 millimeters of wall thickness, and be evenly distributed with 2 millimeters mesh 12 of diameter.Inner core one end and annular polymethyl methacrylate sheet end face are bondd with glass cement, and the center of circle, inner core cross section is overlapped with the center of circle of annular polymethyl methacrylate sheet end face; Polymethyl methacrylate urceolus one end and above-mentioned annular polymethyl methacrylate sheet end face are bondd with glass cement, and the center of circle, urceolus cross section is also overlapped with the center of circle of annular polymethyl methacrylate sheet end face, use joint seal of flanges between this end face and inner core, the urceolus.15 centimetres of described urceolus interior diameters, long 50 centimetres, 2 millimeters of wall thickness have anode inlet 5 and anode export 6.2 centimetres of described annular end face inner edge diameters, 18 centimetres of external profile diameters, thick 2 millimeters.Make 6 long 50 centimetres, diameter is that 2 centimetres graphite rod is uniformly distributed in the anode chamber 3 (being the space between the barrel of the barrel of inner core and urceolus), promptly this graphite rod is spacedly distributed on the circle that with the inner core center of circle is 9.5 centimetres in the center of circle, diameter, then, make the end face bonding of inner core urceolus opening one end and another annular polymethyl methacrylate sheet, the center of circle of urceolus cross section, inner core cross section and annular polymethyl methacrylate sheet end face is overlapped, and use joint seal of flanges.The volume ratio of gained microbial fuel cell unit anode chamber and cathode chamber is 209: 16.The cumulative volume of described graphite rod accounts for 11.5% of anode chamber total measurement (volume).Cathode chamber has cathode inlet 7 and cathode outlet 8.
(2) enrichment of microbe
Get Sewage Disposal sewage inlet bottom anaerobic sludge 20 and restrain in the anaerobism blake bottle that is sealed to 250 milliliters, fill 150 milliliters of anaerobic bacteria culture liquid in this container in advance.The prescription of described anaerobic bacteria culture liquid is that per 1 liter of nutrient solution contains 0.8 grams per liter NH
4Cl, 1.0 grams per liter KCl, 1.5 grams per liter Na
2HPO4,1.0 grams per liter yeast extracts, 10mM glucose, 10mM sodium lactate, 50mM ironic citrate, all the other are water, and transfer pH to neutral with sodium carbonate and sodium bicarbonate buffer solution.Feed nitrogen remove dissolved oxygen in the solution after sealing cultivated 15 days, obtain kind of a daughter bacteria solution, kind of the daughter bacteria solution that takes a morsel is with chemical method analysis Fe (III) concentration wherein, the result has shown Fe (III) lowering of concentration 70%, and plants in the daughter bacteria solution and contain Fe (II).By the inoculum concentration of 10 volume %, the kind daughter bacteria solution of above-mentioned gained is inoculated in the same anaerobic bacteria culture liquid in the same way, continue to cultivate.Enrichment is three times so repeatedly, obtains the anaerobic bacteria bacterium liquid that is mainly alienation reduction bacterium of enrichment.
(3) microbe adheres to
External circuit is connected 10 ohm resistance, and with lead external circuit is linked to each other with negative electrode 16 with the anode 13 of microbiological fuel cell respectively.Add nutrient medium in the anode chamber 3 of microbiological fuel cell, make nutrient medium be full of whole anode chamber 3, the prescription of this nutrient medium is that per 1 liter of nutrient solution contains 0.8 grams per liter NH
4Cl, 1.0KCl grams per liter, 1.5 grams per liter Na
2HPO
4, 1 grams per liter yeast extract, 2mM glucose, 2mM sodium lactate, all the other are water.By the inoculum concentration of 10 volume %, insert the bacterium liquid of step (2) gained, airtightly leave standstill cultivation.Leave standstill and cultivate the while to cathode chamber 4 bubbling airs, keeping the flow of air is 55 liters/minute.Write down ohmically voltage, the initial voltage of resistance is zero after rigidly connecting kind, and along with incubation time is passed, voltage rises gradually.Maintenance is stablized after observing voltage to rise to 0.6 volt in the 12nd day that cultivates, and proves that microbial cell has formed fine and close network structure at anode surface, obtains microbiological fuel cell.
4) the continuous processing of organic wastewater
As shown in Figure 5, from anode inlet anode chamber 3, inject continuously the pH value 8, the COD value is the organic wastewater of 460 mg/litre, guarantee that with plunger water pump 14 time of staying of organic wastewater in anode chamber is 20 hours, cathode chamber 4 is 60 liters/minute by air blast 15 positive air outputs.
Under the constant situation of other condition, adjust the time of staying of organic wastewater in anode chamber 3 with plunger water pump 14 and be respectively 5,10,15,25,30,35,40 hours, detect the COD value of the organic wastewater after processed then with standard GB 11914-89 water quality-COD determination-potassium dichromate method respectively.The result as shown in Figure 6, the time of staying of organic wastewater is long more, its COD value reduces many more, but after the time of staying surpassed 20 hours, COD of sewage value decline scope was obviously slowed down.Therefore in 20-30 hour time range, the microbe that has on anode working liquid and the graphite anode rod can fully be reacted, and is electric energy with the Conversion of energy that discharges in the course of reaction simultaneously.
Embodiment 2
Present embodiment illustrates microbial fuel cell unit provided by the invention and has the microbiological fuel cell of this device, and the using method of this battery and the sewage disposal system that comprises this battery.
1) preparation of microbial fuel cell unit
At first pressing Nafion117 film and negative electrode carbon paper obtain film cathode assembly 10, and the size of this film cathode assembly is 20 centimetres of 20 cm x, and wherein, the area on plate-like cathode (carbon paper) surface is 90% of barrier film (being a Nafion117 proton exchange membrane) surface area.As shown in Figure 3, use the battery case 1 of 30.75 centimetres of bonding organic glass preparation 20 cm x 20 cm x of glass cement, and be 2: 1 cuboid anode chamber 3 and cathode chamber 4 with cathode assembly 10 and battery case formation volume ratio.The anode chamber volume of gained microbial fuel cell unit is identical with embodiment 1 anode chamber volume.The film cathode assembly 10 that pressing obtains is between anode chamber 3 and cathode chamber 4.As shown in Figure 3, fix anode 13 graphite rods in the anode chamber 3, the cumulative volume of this stone mill rod accounts for 30% of anode chamber total measurement (volume).Cathode chamber has cathode inlet 7 and cathode outlet 8.
2) microbe adheres to
Get in the anaerobism blake bottle that anaerobic sludge 20 grams in Sewage Disposal sewage inlet bottom are sealed to 250 milliliters standbyly, fill 150 milliliters of anaerobic bacteria culture liquid in this container in advance.External circuit is connected 10 ohm resistance, and with lead external circuit is linked to each other with negative electrode with the anode of microbiological fuel cell respectively.Add nutrient medium in the anode chamber 3 of microbiological fuel cell, make nutrient medium be full of whole anode chamber, the prescription of this nutrient solution is that per 1 liter of nutrient solution contains 0.8 grams per liter NH
4Cl, 1.0 grams per liter KCl, 1.5 grams per liter Na
2HPO
4, 1 grams per liter yeast extract, 2mM glucose, 2mM sodium lactate, all the other are water.By the inoculum concentration of 10 volume %, insert the bacterium liquid that above-mentioned Sewage Disposal is gathered, airtightly leave standstill cultivation.Leave standstill to cultivate simultaneously to cathode chamber and feed oxygen-saturated water by plunger water pump with 4.8 liters/minute flow, described oxygen saturation water is full of cathode chamber 4.Described cathode chamber has cathode inlet 7 and cathode outlet 8.Postvaccinal initial voltage is zero, and along with incubation time is passed, voltage rises gradually.Maintenance is stablized after observing voltage to rise to 0.5 volt in the 17th day that cultivates, and proves that microbial cell has formed fine and close network structure at electrode surface, obtains microbiological fuel cell.
3) the continuous processing of organic wastewater
From anode inlet 5 anode chambers 3, inject continuously the pH value 9, the COD value is the organic wastewater of 600 mg/litre, guarantee that with plunger water pump 14 time of staying of organic wastewater in anode chamber is 30 hours, cathode chamber 4 is by 4.8 liters/minute of water pump delivery of oxygen saturated waters, and described oxygen saturation water is full of cathode chamber 4.
Comparative example 1
This comparative example illustrates the microbial fuel cell unit of prior art and has the microbiological fuel cell of this device, and the using method of this battery and the sewage disposal system that comprises this battery.
Prepare microbial fuel cell unit according to structure shown in Figure 4 with reference to the method for embodiment 2, different is that negative electrode 16 is the stick electrode of graphite, and separate with barrier film 17 (being the Nafion117 proton exchange membrane), the size of this barrier film is 20 centimetres of 20 cm x, negative electrode 16 is positioned at cathode chamber 4 centers, be immersed in the oxygen saturation water of cathode chamber 4, the surface area that negative electrode 16 is immersed in the oxygen saturation water equates with area of plate-like cathode of embodiment 2; The microbiological cell device of this comparative example comprises the anode chamber 3 and the cathode chamber 4 of the cuboid that is made of barrier film 17 and polymethyl methacrylate battery case 1, the volume of anode chamber 3 is identical with the volume of embodiment 1 anode chamber, anode chamber 3 is 1: 1 with the volume ratio of cathode chamber 4, and the cumulative volume of anode 13 stone mill rods accounts for 15% of anode chamber total measurement (volume).Method according to embodiment 1 connects external circuit, microbe inoculation constitutes microbiological fuel cell, oxygen saturation water in sewage in the anode chamber 3 and the cathode chamber 4 all intermittently adds in batches and discharges, be that sewage in the anode chamber 3 is by anode inlet 5 with have the anode export 6 of valve 2, oxygen saturation water in the cathode chamber 4 was changed once by cathode inlet 7 and the cathode outlet 8 that has valve 2 in per 30 hours.
Test result analysis
The decline degree of sewage COD value before and after microbiological fuel cell is handled can reflect the microbiological fuel cell sewage treatment capacity.Detect the These parameters of embodiment 1-2 and comparative example 1 respectively with standard GB 11914-89 water quality-COD determination-potassium dichromate method, the result is as shown in table 1.
Table 1
| Processing time (hour) | The rate of descent of COD of sewage value (%) | |
| Embodiment 1 | 20 | 65 |
| Embodiment 2 | 30 | 57 |
| Comparative example 1 | 30 | 20 |
As can be seen from Table 1, because fitting by plate-like cathode and barrier film, the microbial fuel cell unit of embodiment constitutes the film cathode assembly, improved the efficient of protolysis, then accelerate cathode reaction speed, use the W-response speed of the microbiological fuel cell of this device to increase substantially, therefore microbiological fuel cell of the present invention is compared with the comparative example microbiological fuel cell, and the ability of disposing of sewage is strengthened greatly, and efficient is higher.
Claims (18)
1. microbial fuel cell unit, this device comprises battery case (1), anode chamber (3), anode (13), cathode chamber (4), negative electrode (16) and barrier film (17); Described anode (13) is arranged in anode chamber (3), barrier film (17) is positioned between anode chamber (3) and the cathode chamber (4), it is characterized in that, described negative electrode (16) is a plate-like cathode, fit and form film cathode assembly (10) in a surface of surface of plate-like cathode and barrier film (17), plate-like cathode is not positioned at cathode chamber (4) one sides with the one side that barrier film (17) is fitted.
2. microbial fuel cell unit according to claim 1, wherein, the area on plate-like cathode surface is at least 75% of barrier film (a 17) surface area.
3. microbial fuel cell unit according to claim 2, wherein, the area on plate-like cathode surface is the 90-100% of barrier film (17) surface area.
4. microbial fuel cell unit according to claim 1, wherein, described plate-like cathode is selected from charcoal cloth or carbon paper.
5. microbial fuel cell unit according to claim 1, wherein, described microbial fuel cell unit comprises urceolus and the inner core that is enclosed within the urceolus, the barrel of described battery urceolus is battery case (1); In the space of anode (13) between the barrel of the barrel of described inner core and urceolus; Space between the barrel of described inner core and the barrel of urceolus is anode chamber (3); The barrel of described inner core comprises a surface of plate-like cathode and a film cathode assembly (10) of fitting and form in the surface of barrier film (17), and plate-like cathode is not positioned at inner core with the one side that barrier film (17) is fitted; Space in the described inner core is cathode chamber (4).
6. microbial fuel cell unit according to claim 5, wherein, the urceolus of described sleeve and the cross section of inner core are circular; The volume ratio of described anode chamber (3) and cathode chamber (4) was greater than 1: 1.
7. microbial fuel cell unit according to claim 6, wherein, the volume ratio of anode chamber (3) and cathode chamber (4) is 2: 1 to 100: 1.
8. microbial fuel cell unit according to claim 5, wherein, described anode chamber (3) also comprises anode inlet (5) and anode export (6), described anode inlet (5) is lower than anode export (6); Described cathode chamber (4) also comprises cathode inlet (7) and cathode outlet (8).
9. microbial fuel cell unit according to claim 5, wherein, the barrel of described inner core also comprises the wire netting (9) that is positioned between film cathode assembly (10) and the anode chamber (3); Described wire netting (9) is fitted with the barrier film face of film cathode assembly (10).
10. microbial fuel cell unit according to claim 5, wherein, the barrel of described inner core also comprises the tube stent (11) that is positioned between film cathode assembly (10) and the cathode chamber (4); Tube stent (11) is fitted with the cathode plane of film cathode assembly (10) in described; This support is mesh (a 12) structure.
11. microbial fuel cell unit according to claim 5, wherein, described anode (13) is a graphite rod; The number of described graphite rod is 3-10; The cumulative volume of described graphite rod accounts for the 10-70% of the total measurement (volume) of described anode chamber (3).
12. microbial fuel cell unit according to claim 11, wherein, described graphite rod evenly distributes in described anode chamber (3).
13. microbiological fuel cell, this battery comprises microbial fuel cell unit, is arranged in the electro-chemical activity microbe of this device, and working solution and/or working gas, it is characterized in that described microbial fuel cell unit is any described microbial fuel cell unit among the claim 1-12.
14. microbiological fuel cell according to claim 13, wherein, described electro-chemical activity microbe is an anaerobe.
15. microbiological fuel cell according to claim 13, wherein, the anode chamber of described microbiological fuel cell also comprises anode working liquid in (3); Described anode working liquid is the nutrient solution of sewage or described electro-chemical activity microbe; The cathode chamber of described microbiological fuel cell also comprises negative electrode working solution or working gas in (4); Described negative electrode working solution is the solution that oxygen saturation water or oxidation-reduction potential are lower than the anode chamber working solution; Described working gas is oxygen or air.
16. the using method of the described microbiological fuel cell of claim 13, this method comprises:
1) external circuit and the negative electrode (16) of microbiological fuel cell are connected with anode (13) to constitute the loop;
2) add working solution in the anode chamber (3), and to make working solution be 20-30 hour in the time of staying of anode chamber (3); In cathode chamber (4), add working solution or feed working gas.
17. method according to claim 16, wherein, adding working solution in the described anode chamber (3) is to add working solution in the anode chamber (3) continuously, and the working solution after the electro-chemical activity microbe is decomposed is discharged anode chamber (3) continuously.
18. a sewage disposal system that comprises microbiological fuel cell, wherein, described microbiological fuel cell is any described microbiological fuel cell among the claim 13-15.
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