CN101710625A - Fuel cell system and method of generating electricity and reducing heavy metal through sewage treatment - Google Patents

Fuel cell system and method of generating electricity and reducing heavy metal through sewage treatment Download PDF

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CN101710625A
CN101710625A CN200910110425A CN200910110425A CN101710625A CN 101710625 A CN101710625 A CN 101710625A CN 200910110425 A CN200910110425 A CN 200910110425A CN 200910110425 A CN200910110425 A CN 200910110425A CN 101710625 A CN101710625 A CN 101710625A
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heavy metal
chamber
cathode chamber
sewage
metal ion
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CN101710625B (en
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陶虎春
梁敏
倪晋仁
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Huizhou Dayawan Julian Information Technology Co ltd
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Peking University Shenzhen Graduate School
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    • 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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Abstract

The invention provides a fuel cell system and a method of generating electricity and reducing heavy metal through sewage treatment. The system comprises a bioreactor, wherein the bioreactor comprises a negative chamber and a positive chamber, a negative electrode and a positive electrode are separately arranged in the negative chamber and the positive chamber, the two chambers are provided with microbial active material and are separated by a proton exchange membrane, the sewage is introduced to the positive chamber of which microbial active material is used to treat the sewage, the negative chamber contains heavy metal ion solution and reduces heavy metal ions, the inside of the positive chamber generates electrons and electrons, and the electrons migrate to the negative chamber through the proton exchange membrane so that current is generated between the two chambers in the reactor and the bioreactor can treat the sewage while generating electrical energy. In the system and method, the heavy metal ion solution is used as electron acceptor so that oxygen is not needed to be filled; and the whole system has simple structure, low cost and easy operation and heavy metal can be recycled from the negative solution.

Description

The method of fuel cell system and sewage disposal electrogenesis and reducing heavy metal
Technical field
The present invention relates to water treatment technology, relate in particular to and a kind ofly adopt microbial reaction to dispose of sewage and produce the method for fuel cell system and the sewage disposal electrogenesis and the reducing heavy metal of electric energy.
Background technology
Along with country or enterprise to environmental protection and the demand that economizes on resources etc., dirty (or useless) water treatment becomes and more and more is subjected to popular attention.Bioremediation is adopted in comparatively effective and feasible sewage disposal at present usually.For example, traditional biological treatment uses secondary sedimentation tank to come sewage is handled.Yet when carrying out sewage disposal, sewage also needs just can discharge through the secondary sedimentation tank post precipitation through behind the biochemical reaction, causes the process of sewage disposal longer.In addition, adopt the treatment process floor space of secondary sedimentation tank big, the cost of investment height.Especially when operation mud age was higher, this can cause bad sludge settling.Therefore, this treatment system and technology are not suitable for densely populated region.
Along with the development of suitability for industrialized production, heavy metal more and more causes people's attention.Along with the increasingly stringent of environmental requirement, also more and more higher to the requirement of heavy metal-containing wastewater treatment, be not confined to end treatment merely, but transformed to cleaner production, realize the recovery of heavy metal when requiring to realize the purification of waste water reuse.The heavy metal-containing wastewater treatment method of Application and Development mainly contains chemical method, physical-chemical process and bioanalysis at present, comprises methods such as chemical precipitation, electrolysis, ion-exchange, film separation, activated carbon and silica gel absorption, bioflocculation, biological absorption, plant regulation.During general chemical Treatment heavy metal-containing waste water, owing to contain a large amount of organic complexs in many heavy metal wastewater therebies, limited the chemical settling process, the waste water content of beary metal after causing handling exceeds standard; Processing procedure adds the soda acid medicament, and complicated operation, cost are difficult to control, and sedimentation sludge components complexity is difficult to handle, and brings secondary pollution easily.Though it is low that biological treatment has a cost, handles advantage easily, owing to be subjected to the influence of wastewater toxicity, be difficult to extensive the realization, and the efficient of handling is low, effect is relatively poor.The Applied Electrochemistry method reclaims the processing method of heavy metal, in electrolytic process, solution contacts with the both positive and negative polarity of power supply and redox reaction takes place, when heavy metal wastewater thereby is carried out electrolysis, heavy metal ion in the waste water obtains electronics and is reduced at negative electrode, these heavy metals or be deposited on electrode surface or be deposited to reaction tank bottom, thus content of beary metal in the waste water reduced.
China is faced with conspicuous contradiction fast-developing and environmental constraints, has organic substance and the serious situation of heavy metal pollution in some regional water environment.For example, the Delta of the Pearl River is important printed circuit board (PCB) (PrintedCircuit Board, PCB) production and export base, only just there is family surplus the PCB manufacturing enterprise 150 in Shenzhen, yearly productive capacity is more than 1,100 ten thousand square metres, also produces to contain high concentration heavy metal and organic waste liquid and waste water in a large number when creating hundred million yuan of output values of hundreds of.Because processing method falls behind, and causes the waste water of discharging to contain heavy metal ion such as copper, nickel, lead, serious environment pollution.Therefore, how effectively to remove the current problem that presses for solution that becomes of heavy metal ion such as copper, nickel, lead.
Summary of the invention
In view of this, be necessary to provide a kind of simple in structure, cost is low, can make full use of the fuel cell system of cathodic reduction power.
And provide a kind of method that adopts above-mentioned fuel cell system to carry out sewage disposal electrogenesis and reducing heavy metal.
A kind of fuel cell system, it comprises bioreactor, described bioreactor comprises cathode chamber and anode chamber, be respectively equipped with negative electrode and positive electrode in described cathode chamber and the anode chamber, has the microbial activity thing in described cathode chamber and the anode chamber respectively, pass through proton exchange membrane separately between described cathode chamber and the anode chamber, circulation sewage and sewage is handled in the described anode chamber by the microbial activity thing in it, comprise heavy metal ion solution in the described cathode chamber and make the heavy metal ion reduction within it, produce proton and electronics in the described anode chamber, described proton migrates to described cathode chamber by described proton exchange membrane, make chamber, the two poles of the earth in the inside reactor electrical communication, and produce electric energy when making bioreactor sewage treatment.
And, the method for a kind of sewage disposal electrogenesis and reducing heavy metal, it adopts above-mentioned fuel cell system to carry out sewage disposal, electrogenesis and reducing heavy metal, and this method may further comprise the steps:
Sewage is imported in the described anode chamber;
Heavy metal ion solution is imported in the described cathode chamber;
By the microbial activity thing in the described anode chamber sewage of the described anode chamber that flows through is handled, produced proton and electronics simultaneously, described proton migrates to described cathode chamber by described proton exchange membrane;
Described heavy metal ion solution is accepted electronics and is reduced in described cathode chamber, the proton that produces in the described anode chamber migrates to described cathode chamber by described proton exchange membrane, makes chamber, the two poles of the earth in the inside reactor electrical communication, produces electric energy.
In technique scheme, comprise heavy metal ion solution in the described cathode chamber, and with it as electron acceptor, thereby need not blast oxygen in sewage disposal and electricity generation process, whole fuel cell system can be save the required aerator of tradition, thereby, make whole system simple in structure, cost is low, when carrying out sewage disposal and electrogenesis, operates also comparatively easy.And, because cathode chamber can adopt the solution that comprises heavy metal ion as cathode solution, so said system and method not only can realize sewage purification and electrogenesis simultaneously, heavy metal ion can also be reduced, make full use of cathodic reduction power, from cathode solution, reclaim heavy metal.
Description of drawings
Fig. 1 is the fuel cell system schematic diagram of the embodiment of the invention.
Fig. 2 is the sewage disposal electrogenesis of the embodiment of the invention and the method flow diagram of reducing heavy metal.
Fig. 3 be embodiments of the invention 1 and 2 and Comparative Examples in microbiological fuel cell (MFC) start back voltage change curve in time.
Fig. 4 be embodiments of the invention 1 and 2 and Comparative Examples in the output voltage in MFC when operation and power with the change curve of current strength.
Fig. 5 be embodiments of the invention 1 and 2 and Comparative Examples in the anodic dissolution in MFC when operation and cathode solution in the change curve of concentration of heavy metal ion.
Fig. 6 be embodiments of the invention 1 and 2 and Comparative Examples in the MFC end of run after the XRD figure spectrum of graphite cathode.
Embodiment
In order to make purpose of the present invention, technical scheme and advantage clearer,, the present invention is further elaborated below in conjunction with drawings and Examples.Should be appreciated that specific embodiment described herein only in order to explanation the present invention, and be not used in qualification the present invention.
See also Fig. 1, the fuel cell system 10 that shows the embodiment of the invention, this fuel cell system 10 is a microbial fuel cells system, comprise a biological reactor 12, this bioreactor 12 comprises the proton exchange membrane (PEM) 16 of cathode chamber 13 and anode chamber 14 and separation cathode chamber 13 and anode chamber 14. Cathode chamber 13 and 14 inside, anode chamber are respectively equipped with negative electrode 131 and positive electrode 141.Have the microbial activity thing respectively in cathode chamber 13 and the anode chamber 14, be used for current are handled.Proton exchange membrane 16 constitutes the passage 17 of conducting cathode chamber 13 and anode chamber 14.Circulation sewage and sewage is handled by the microbial activity thing in it in the anode chamber 14 for example, carry out oxidation processes to the organic substance in the sewage, produce proton and electronics in the anode chamber 14.Comprise heavy metal ion solution in the cathode chamber 13 and make the heavy metal ion reduction within it, the proton that produces in the anode chamber 14 migrates to cathode chamber 13 by proton exchange membrane 16, make chamber, the two poles of the earth in the inside reactor electrical communication, and produce electric energy when making bioreactor sewage treatment.
Reactor 12 can adopt transparent material such as organic glass to become, so that the water level in the observing response device 12, but be not limited thereto.Cathode chamber 13 has cathode chamber inlet 132 and cathode chamber outlet 133, and anode chamber 14 has anode chamber's inlet 142 and anode chamber's outlet 143.Wherein, each enters the mouth and 132 and 142 is opened in each chamber near the position at top, each exports 133 and 143 and is opened in the position of each chamber near the bottom respectively, thereby makes that the water (flow) direction in cathode chamber 13 and the anode chamber 14 is to flow to streaming down, and the indoor separately electrode of flowing through respectively.
Negative electrode 131 and positive electrode 141 in the chamber, the two poles of the earth 13 and 14 can adopt graphite electrode, each graphite electrode all is that to be inserted into correspondence in the inclination mode extremely indoor, inclination can be that relative proton exchange membrane or flow direction are angled, for example, the angle of inclination of the relative horizontal direction of graphite electrode is roughly at the 30-75 degree, be preferably the 45-65 degree, more preferably 60 degree.Wherein, be provided with two graphite electrodes in anode chamber 14, their interconnections are provided with, and electrically connect mutually, and negative electrode 13 comprises the graphite electrode that a slice at least is obliquely installed.Rectangular vessel can be adopted in chamber, the two poles of the earth 13 and 14, and at this moment, each graphite electrode can be to be obliquely installed by the diagonal angle that is connected to container, promptly is arranged on the diagonal of container.When using, the graphite electrode outer end in the chamber, the two poles of the earth 13 and 14 further is connected a load 15.
Adopt heavy metal ion solution as cathode solution in the present embodiment, accept electronics, do not need to blast oxygen or air, thereby, aerator can not adopted.Heavy metal ion solution can comprise at least a in copper ion, zinc ion, nickel ion, lead ion, cadmium ion or the chromium ion, but is not limited to above-mentioned ionic species.In a specific embodiment, further be added with cushioning liquid, for example phosphate solution in the cathode chamber 13.This cushioning liquid is to join in the cathode chamber 13 before importing heavy metal ion solution, promptly postpones to add heavy metal ion solution.At this moment, owing to temporarily a large amount of electron acceptors is not arranged, can utilize an aerator (figure does not show) in cathode chamber 13, to blast oxygen or air earlier, so that aerobic environment temporarily to be provided.Behind the operation certain hour, in cathode chamber 13, import heavy metal ion solution more like this.
In another specific embodiment, even in cathode chamber 13, be added with the cushioning liquid that is neutral, also can not adopt aerator to carry out air-blowing, directly utilize cushioning liquid to move water treatment and electricity generation process in advance, make microbe tentatively be cultivated.Behind the operation certain hour, in cathode chamber 13, import heavy metal ion solution more like this.
See also Fig. 1 and Fig. 2, illustrate that the microbial fuel cells system 10 that utilizes present embodiment carries out the method for sewage disposal electrogenesis and reducing heavy metal, this method may further comprise the steps:
S01: sewage is imported in the anode chamber 14;
S02: heavy metal ion solution is imported in the cathode chamber 13;
S03: by the microbial activity thing in the anode chamber 14 sewage of the anode chamber 14 that flows through is handled, produced proton and electronics simultaneously, proton migrates to cathode chamber 13 by proton exchange membrane 16;
S04: heavy metal ion solution is accepted electronics and is reduced in cathode chamber 13, and the proton that produces in the anode chamber 14 migrates to cathode chamber 14 by proton exchange membrane 16, makes chamber, the two poles of the earth in reactor 12 inner electrical communication, produces electric energy.
In step S01 and S02, the sewage of present embodiment is taken from the anaerobic sludge of Shenzhen Luo Fang sewage treatment plant, it is added tame the scheduled time (24 hours according to appointment) back in the sewage as seed sludge.As test, the substrate of supplying with in the reactor 12 is the organic sewage/wastewater of glucose of autogamy in the present embodiment.Sewage can utilize a peristaltic pump to import in the anode chamber 14, and reaction temperature is constant in 35 ± 2 ℃.In the present embodiment, heavy metal ion solution in the cathode chamber 13 adopts the sulfate liquor of heavy metal as example, the concentration of sulfate liquor is 0.1mol/L, can adopt other heavy metal ion solution as required during practical application, and be made into required concentration, perhaps directly get the sewage/waste water that contains heavy metal ion, be not limited to this.
In step S03, down to flowing water flow through the anode chamber 14, the microbial activity thing in it is handled current, produces proton and electronics simultaneously.Electronics then moves out through anode 141, enters external circuit.Proton then penetrates proton exchange membrane 16 and migrates to cathode chamber 13.
In step S04, heavy metal ion solution is accepted electronics and is reduced in cathode chamber 13, and this electronics comes from external circuit, for example by having the external path of load 15.The proton that produces in the anode chamber 14 migrates to cathode chamber 14 by proton exchange membrane 16, makes chamber, the two poles of the earth in reactor 12 inner electrical communication, and externally circuit and internal circuit all form and electrically conduct, thereby produces electric energy.
Be example below with the test, adopt simulated wastewater, for example can take from the anaerobic sludge of Shenzhen Luo Fang sewage treatment plant, with its add in sewage domestication after 24 hours as seed sludge, heavy metal ion solution is example with the copper-bath that comprises copper ion.Substrate is a G/W, and its main component has (mg/L): C 6H 12O 65000; CaCl 2275; NaCl 1000; NH 4 Cl 400; NaHCO 33000; Also add the required trace element of growth of microorganism simultaneously.In addition, as shown in Figure 1, variable resistance box 15 (the resistance value scope is at 0～9999 Ω) is adopted in load, and resistance is adjusted into 1000 Ω.Utilize a data collecting card 152 image data again,, deposit computer in every 30 seconds record primary voltage data.
During operation, the activated sludge 100ml that inoculation was tamed in above-mentioned swash plate MFC, and add the 900ml simulated wastewater, and utilize peristaltic pump that simulated wastewater is pumped in the anode chamber 14, same, cathode solution is imported in the cathode chamber 13.Under the external resistance load of 1000 Ω, measure output voltage curve over time.
Wherein, every 30 seconds output voltages (U), obtain electric current by I=U/R by data acquisition system record reactor.Take the steady-state discharge method of polarization curve to measure apparent extrernal resistance.TOC adopts TOC analyzer (multiN/C3100) to measure; The cathode solution concentration of heavy metal ion adopts atomic absorption spectrophotometry to measure.Enclosed pasture efficient E calculates according to formula (1).
E = Σ i = 1 n U i T i RF i b i ΔSV M × 100 % - - - ( 1 )
In the formula, U iBe t iMoment MFC output voltage; R is an external resistance; F iBe Faraday constant, 9645Cmol -1B is the molal quantity that microbe is decomposed the electronics that 1mol TOC produced, and equals 4e -1Molmol -1Δ S is the removal concentration (gL of TOC -1), V is the volume (L) of anodic dissolution, M is the molecular weight of carbon, equals 12gL -1
The cathodic reduction material composition is analyzed: Japan is of science, and D/max 2500PC type high-resolution X-ray diffractometer changes target, 18KW.
In specific embodiment, cathode chamber 13 has two kinds of feeding manners at least, and is specific as follows.
Embodiment 1 (M2)
After anode chamber 14 li addings 900ml glucose simulated wastewater and bacterial classification mixed liquor, add 900ml phosphate buffer (pH=6.8) toward 13 li of cathode chambers earlier and also exposes to the sun into oxygen, behind the operation 24h, again cushioning liquid is changed into the copper-bath of 0.1mol/L.Then, operate according to above-mentioned steps S03-S04 again.In operating process, measure the MFC output voltage and change in time, obtain circular icon curve as shown in Figure 3, arrow represents to add the time point of copper-bath in cathode chamber.
Embodiment 2 (M3)
After 14 li of anode chambers add 900ml glucose simulated wastewater and bacterial classification mixed liquor, add 900ml phosphate buffer (pH=6.8) but aeration not toward 13 li of cathode chambers earlier, again cushioning liquid is changed into the copper-bath of 0.1mol/L behind the operation 48h.Then, operate according to above-mentioned steps S03-S04 again.In operating process, measure the MFC output voltage and change in time, obtain square icon curve as shown in Figure 3, arrow represents to add the time point of copper-bath in cathode chamber.
Comparative Examples (M1)
As with the contrast of above-mentioned two embodiment, carry out following feeding manner.Elder generation anode chamber adds 900ml glucose simulated wastewater and bacterial classification mixed liquor for 14 li, adds the 900ml copper-bath then simultaneously in cathode chamber, operates according to above-mentioned steps S03-S04 again.In operating process, measure the MFC output voltage and change in time, obtain triangle icon curve as shown in Figure 3, arrow represents to add the time point of copper-bath in cathode chamber.
In the foregoing description and Comparative Examples, as shown in Figure 3, the starting stage that Comparative Examples starts, output voltage only increased about 50mv and slowly basically always because cathode chamber does not have aeration, but found behind the 5h that its output voltage begins to continue to drop to 0V.Probe into its reason, the existing a considerable amount of copper ions that make discovery from observation are moved to anode chamber 13 through PEM makes anode mixture liquid be light blue, and copper ion causes the anode microbial death, and Comparative Examples starts failure.In embodiment 1, electrogenesis rises very fast behind the negative electrode aeration, after during operation 24h, after changing the cushioning liquid of cathode chamber 13 copper-bath of 0.1mol/L into, output voltage sharply drops to about 0.2V from 0.35V, operation during 48h after, go up after dropping to 0.15V, be stabilized between the 0.2V-0.25V at last.In embodiment 2, behind the operation 48h, change the cushioning liquid of cathode chamber 13 copper-bath of 0.1mol/L into after, electrogenesis sharply rises to 0.22V, slowly growth is stabilized in about 0.46V at last afterwards.
This shows, copper sulphate is made the problem that there is the infiltration of copper ion ion anode chamber in the MFC cathode solution, postpone to add the infiltration that copper sulphate helps to reduce the copper ion ion, main cause is, the a large amount of electronics that accumulate on the biomembrane of anode microbe through forming after the cultivation after a while make anode form higher initial potential, and the tow sides that circuit is connected back PEM will form certain electrical potential difference and impel H in the anodic dissolution +And other cations anode chamber migration under the pressure of copper ion in concentration difference of cathode chamber migration and obstruction cathode solution the inside.
Two embodiment 1 that start for success and 2, carry out the steady-state discharge test after the MFC electrogenesis of copper sulphate cathode solution is basicly stable, measure gained polarization curve and output power density (power density and current density all calculate by anode chamber's effective volume) as shown in Figure 4.The result shows that the open circuit voltage of embodiment 1 only is 0.4958V, and can obtain apparent internal resistance to its polarization curve match is 454.4 Ω, and maximum electrogenesis power density is 115.26mw/m 3And the open circuit voltage of embodiment 2 can reach 0.7477V, and it is 339.39 Ω that its polarization curve match is obtained apparent internal resistance, and maximum power density reaches 355.5mw/m 3As seen, the startup method (or feed way) of the MFC of copper sulphate cathode solution not only influences output voltage, but also influences the apparent internal resistance and the power output of battery.Try to achieve accumulative total electrogenesis amount according to the change in voltage curvilinear integral
Figure G2009101104257D0000091
By TOC accumulative total removal amount and accumulative total electrogenesis amount, the enclosed pasture efficient of trying to achieve embodiment 1 and 2 according to formula (1) is respectively 1.93% and 1.85% again.
Present embodiment is further tested removal efficient and the migration rule of MFC to copper, gets anodic dissolution and cathode solution copper ion concentration in the atomic absorption spectroscopy determination solution of embodiment 1 and 2 respectively every 24h, and the result as shown in Figure 5.In embodiment 1, the copper ion concentration in its anodic dissolution of initial operating stage continues to rise and is up to 10.28mg/L, the inhibitory action that the antianode microorganisms is bigger; Battery enters stable discharging may be because the effect of film two sides electrical potential difference stops copper ion in the cathode solution after period + Further anode chamber 13 infiltrations, the copper ion that has been penetrated into anode chamber 13 generates Cu (OH) under the 13 li higher pH environment in anode chamber 2Precipitation, thus the copper ion concentration in the anodic dissolution is dropped to below the 1mg/L gradually.In embodiment 2, copper ion concentration in the anodic dissolution has also experienced similar variation, but its initial operating stage copper ion concentration peak only is 5.22mg/L, and is reduced to below the 1mg/L in the short period of time, so the antianode microbe is not caused the obvious suppression effect.In embodiment 2, the copper ion in the cathode solution has tangible minimizing trend, and its concentration is reduced to 5437.25mg.L behind the 360h, and the clearance of copper ion reaches 18.59%; Though and copper ion concentration also has and significantly to reduce but have a rebound in the cathode solution of embodiment 1 midway, the clearance of copper ion only 8.58% behind the 360h.
In addition, all deposited the thicker blue material of one deck at embodiment 1 with after 2 operation a period of times on its proton exchange membrane, the copper ion that reduces in the visible MFC solution is not all moved to send out on the negative electrode and is gone up reduction reaction.Therefore, not only the copper ion in the copper ion solution is reduced into copper simple substance and is deposited on the described negative electrode 131, also on described negative electrode 131 and/or described proton exchange membrane 16, form the precipitation compound of copper simultaneously, thereby can collect the copper simple substance that is deposited on the negative electrode 131 and the precipitation compound of copper respectively.The precipitation compound of copper comprises Cu (OH) 2, Cu 4(OH) 6SO 4And Cu 2O.Therefore, in actual applications, can remove reactor 12, take out anode 141, negative electrode 131 and proton exchange membrane 16, collect the copper simple substance that is deposited on the negative electrode 131 and the precipitation compound of copper in MFCs operation back.For testing the concrete content of these materials, after embodiment 1 and 2 operations, with purified rinse water anode 141, negative electrode 131 and proton exchange membrane 16, put into the rare nitric acid dousing of 100ml beaker after rinsing well with 1mol/L, measure the copper ion concentration of nitric acid dousing liquid, thereby the copper content of trying to achieve separately is as shown in table 1.The result shows that the copper ion in the cathode solution also moves deposition on a large scale when negative electrode is moved on proton exchange membrane.
Copper content (mg) on table 1 MFCs end of run rear electrode and the proton exchange membrane
Figure G2009101104257D0000101
For proving the existence of above-mentioned copper species, behind embodiment 1 and 2 end of runs, scraping negative electrode 131 top layer precipitates step pitch with 0.02 degree on Japan's D/MAX 2500 type X-ray diffractometers of science spends to such an extent that its XRD figure is composed from 10 degree continuous sweeps to 80, as shown in Figure 6, lowermost lines are the XRD standard diagram of four kinds of matter of matching among the figure.The diffract spectral line of observing negative electrode 131 precipitates among the embodiment 1 in 2 θ=13.9 °, 16.5 °, 22.8 ° and 35.6 ° locate all to occur sharp-pointed diffraction maximum, the Cu of PDF 01-085-1316 in machine examination rope and the standard card as calculated 4(OH) 6SO 4Unanimity can determine to exist a large amount of Cu 4(OH) 6SO 4Spectral line in 2 θ=43.9 °, 50.4 ° and 74.1 ° locate to occur characteristic peak, the machine examination rope is consistent with the Cu of PDF01-071-4610 in the standard card as calculated, proving has portion C u in the cathode solution among the embodiment 1 2+On negative electrode, be reduced into copper simple substance.Observe the diffract spectral line of negative electrode 131 precipitates among the embodiment 2 and also find stronger Cu 4(OH) 6SO 4Characteristic peak; In 2 θ=36.4 °, 43.2 °, 61.4 ° and 73.6 ° locate to occur stronger sharp peak, the Cu of PDF 01-078-2076 in machine examination rope and the standard card as calculated 2The O unanimity proves and contains more Cu among the embodiment 2 in the negative electrode precipitate 2O; ° 50.4 ° and 74.1 ° of diffraction maximums of locating also to find Cu in 2 θ=43.9.The relative intensity of each material diffraction maximum on the negative electrode 131 from embodiment 1 and 2 generates a large amount of Cu on the negative electrode 131 among the embodiment 1 4(OH) 6SO 4With a spot of Cu simple substance, and on the negative electrode 131 among the embodiment 2 Cu is arranged 4(OH) 6SO 4More Cu is also arranged 2O and Cu.
According to the product of XRD spectrum analysis MFC cathodic reduction Cu (II), can roughly obtain following reduction process: at first discharge electronics in the process of anode microbial degradation glucose and be delivered on the negative electrode graphite cake by external circuit; Positively charged Cu in the cathode solution 2+Ion is moved to the negative electrode near surface by mass transfer in liquid phase, electronegative SO 4 2-To the negative electrode migration velocity since negative electrode on negative electrical charge the repulsion effect and much smaller than Cu 2+On the MFC negative electrode in the electron amount deficiency, on the negative electrode surface near a large amount of Cu of accumulation 2+Just be hydrolyzed into Cu (OH) 2And be adsorbed onto on the negative electrode, and then with solution in CuSO 4Reaction generates 3Cu (OH) 2CuSO 4Its reducing power was stronger when electron amount was more on the negative electrode, the Cu of negative electrode surface accumulation 2+The Cu (OH) that partial hydrolysis generates 2, and then and Cu 2+Be reduced into Cu together 2O separates out on negative electrode; When electron amount is sufficient on the negative electrode, move near the Cu of electrode surface in the cathode solution 2+Be not reduced into the Cu particle soon and be adsorbed on electrode plate surface, be transformed into crystalline state from ADSORPTION STATE then and separate out at electrode plate surface.
Add the glucose simulated wastewater in the anode chamber of clean MFC reactor and do not inoculate bacterial classification, add copper-bath in the cathode chamber and make up the check experiment discovery, all does not have the deposition copper-containing compound on the battery lead plate of blank MFC and the proton exchange membrane, but it is equal to exist concentration difference to infiltrate in the two Room solution copper ion concentration.Therefore as can be known, embodiment 1 that success starts and 2 MFC closed circuit can stop the copper ion anode chamber infiltration in the cathode solution, separate out but the copper ion that migration path is blocked can be deposited on the proton exchange membrane form with crystal.
In the above-described embodiments, MFC is to be cathode solution with the copper-bath directly, for the anode substrate makes up two chambers film MFC is arranged with waste water, under the condition that is applied to 1000 Ω external resistances, continuous discharge 400h, maximum output voltage reaches 488.8mV, and maximum power density is 355.5mw/m 3The battery apparent internal resistance is 339 Ω, and open circuit voltage can reach 747.7mV, and enclosed pasture efficient is 1.93%.In running, the Cu in the MFC cathode solution 2+Under the pressure of concentration difference, can be penetrated into the anode chamber,, postpone to add copper-bath and can effectively suppress Cu because of face by proton exchange membrane 2+Infiltration, make the MFC function smoothly.In embodiment 2, MFC is to Cu in the 0.1mol/L copper-bath 2+Clearance higher, can reach 18.59%; XRD analysis proof Cu (II) can form a large amount of Cu in negative electrode surface reduction process 4(OH) 6SO 4, reduzate comprises Cu and Cu 2O, and be deposited on respectively on electrode and the proton exchange membrane.
For the heavy metal outside the copper removal, the method flow of its sewage disposal electrogenesis and reducing heavy metal and the operation of the foregoing description and data and result are similar, after treatment, other heavy metal also has multiple as precipitation of hydroxide, simple substance and other similar product, does not repeat them here.
As from the foregoing, in the method for the fuel cell system 10 of present embodiment and sewage disposal electrogenesis and reducing heavy metal, comprise the heavy metal ion solion in the cathode chamber 14, and with it as electron acceptor, thereby in sewage disposal and electricity generation process, need not blast oxygen, whole fuel cell system can be save the required aerator of tradition, thereby, make whole system simple in structure, cost is low, when carrying out sewage disposal and electrogenesis, operate also comparatively easy.And, because cathode chamber can adopt and comprises the heavy metal ion ion solution as cathode solution, so said system and method not only can realize sewage purification and electrogenesis simultaneously, heavy metal ion can also be reduced, make full use of cathodic reduction power, from cathode solution, reclaim heavy metal.
The above only is preferred embodiment of the present invention, not in order to restriction the present invention, all any modifications of being done within the spirit and principles in the present invention, is equal to and replaces and improvement etc., all should be included within protection scope of the present invention.

Claims (10)

1. fuel cell system, it comprises bioreactor, described bioreactor comprises cathode chamber and anode chamber, be respectively equipped with negative electrode and positive electrode in described cathode chamber and the anode chamber, has the microbial activity thing in described cathode chamber and the anode chamber respectively, pass through proton exchange membrane separately between described cathode chamber and the anode chamber, it is characterized in that, circulation sewage and sewage is handled in the described anode chamber by the microbial activity thing in it, comprise heavy metal ion solution in the described cathode chamber and make the heavy metal ion reduction within it, produce proton and electronics in the described anode chamber, described proton migrates to described cathode chamber by described proton exchange membrane, make chamber, the two poles of the earth in the inside reactor electrical communication, and produce electric energy when making bioreactor sewage treatment.
2. fuel cell system as claimed in claim 1 is characterized in that, described positive electrode comprises two cross-coupled graphite electrodes, and described negative electrode comprises the graphite electrode that a slice at least is obliquely installed.
3. fuel cell system as claimed in claim 1 is characterized in that, described heavy metal ion solution comprises at least a in copper ion, zinc ion, nickel ion, lead ion, cadmium ion or the chromium ion.
4. fuel cell system as claimed in claim 1 is characterized in that, further is added with cushioning liquid before adding heavy metal ion solution in the described cathode chamber.
5. the method for sewage disposal electrogenesis and reducing heavy metal, it adopts as each described fuel cell system of claim 1 to 4 and carries out sewage disposal, electrogenesis and reducing heavy metal, and this method may further comprise the steps:
Sewage is imported in the described anode chamber;
Heavy metal ion solution is imported in the described cathode chamber;
By the microbial activity thing in the described anode chamber sewage of the described anode chamber that flows through is handled, produced proton and electronics simultaneously, described proton migrates to described cathode chamber by described proton exchange membrane;
Described heavy metal ion solution is accepted electronics and is reduced in described cathode chamber, the proton that produces in the described anode chamber migrates to described cathode chamber by described proton exchange membrane, makes chamber, the two poles of the earth in the inside reactor electrical communication, produces electric energy.
6. the method for sewage disposal electrogenesis as claimed in claim 5 and reducing heavy metal is characterized in that, the inherent heavy metal ion solution that imports of described cathode chamber adds cushioning liquid before, and postpones to add heavy metal ion solution.
7. the method for sewage disposal electrogenesis as claimed in claim 5 and reducing heavy metal is characterized in that, adds cushioning liquid in the described cathode chamber earlier, carries out aeration simultaneously, imports heavy metal ion solution again after the operation scheduled time.
8. the method for sewage disposal electrogenesis as claimed in claim 5 and reducing heavy metal is characterized in that, adds cushioning liquid in the described cathode chamber earlier, moves the scheduled time under the state that does not carry out aeration, imports heavy metal ion solution again.
9. as the method for claim 7 or 8 described sewage disposal electrogenesis and reducing heavy metal, it is characterized in that the described scheduled time is 24 hours to 72 hours.
10. the method for sewage disposal electrogenesis as claimed in claim 5 and reducing heavy metal, it is characterized in that, heavy metal ion in the described heavy metal ion solution is reduced into heavy metal simple substance and is deposited on the described negative electrode, also on described negative electrode and/or described proton exchange membrane, form the precipitation compound of heavy metal simultaneously, collect the heavy metal simple substance that is deposited on described negative electrode and/or the described proton exchange membrane and the precipitation compound of heavy metal respectively.
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