CN105060619A - Apparatus for treating degradation-resistant organic wastewater and use thereof - Google Patents
Apparatus for treating degradation-resistant organic wastewater and use thereof Download PDFInfo
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Abstract
The present invention provides an apparatus for treating degradation-resistant organic wastewater. The apparatus comprises a photoelectrocatalytic oxidation unit and a microbial fuel cell (MFC) coupling system, wherein the photoelectrocatalytic oxidation unit and the MFCs are simultaneously connected and matched with each other in an electric circuit and a water circuit respectively, and the MFCs comprise a first-level MFC and a second-level MFC. Water body is firstly subjected to photoelectrocatalytic oxidation, and then enters into the two-level MFCs which are connected with the water circuit in series ; and in the electric circuit, each MFC of the two-level MFCs is independent, and provides bias voltages to the photoelectrocatalytic oxidation device. The present invention further provides a method for treating wastewater by utilizing the photoelectrocatalytic oxidation unit and the microbial fuel cell (MFC) coupling system, and a use of the apparatus in organic sewage treatment.
Description
Technical field
The present invention relates to the process of organic wastewater with difficult degradation thereby, specifically, relate to conbined usage photoelectrocatalysioxidization oxidization unit and microbiological fuel cell (MFC) coupled system to process the apparatus and method of organic waste water, and the purposes of described device in organic wastewater with difficult degradation thereby process.
Background technology
Along with the raising of industrial expansion and human living standard, kind and the quantity discharged of industrial organic waste water and sanitary sewage are increasing, and composition is also more complicated.At present, the research of administering about Persistent organic pollutants in water is more, and the technology adopted mainly comprises Physical (absorption, ultrafiltration etc.), chemical method (advanced oxidation), biochemical process (active sludge etc.) method.But large multi-method needs external energy, and energy consumption is higher, and this will certainly increase cost of water treatment, aggravation energy dilemma; Meanwhile, monotechnics processing efficiency is lower.Therefore, foundation has synergistic integrated approach and realizes Persistent organic pollutants in high-efficiency low energy consumption removal water, is the focus of water treatment field research.
Photoelectrocatalysioxidization oxidization is a kind of method of the synergistic oxidation organic pollutants that photochemical catalysis combined with electrocatalysis.Relative to independent photochemical catalysis, photo-electrocatalytic technology can stop light induced electron and hole compound occurs thus improves the organic efficiency of catalyzed oxidation effectively; Relative to independent electrocatalysis, the current carrier that photochemical catalysis produces can overcome the large energy barrier of electrocatalysis oxidation reaction, and then reduces required electric energy, and namely photoelectrocatalysis only needs to provide a lower bias voltage to realize efficient oxidation.Relative to other method, due to photoelectrocatalysis method be easy to control to safeguard, equipment is simple, non-secondary pollution etc., so have huge application potential in organic pollutants catalyzed degradation.In Sewage treatment systems, utilize photoelectrocatalysis to significantly improve the biological degradability of organic pollutants, not only increase subsequent disposal efficiency, decrease energy consumption simultaneously.But utilize photoelectrocatalysis method to be difficult to direct for the organism in sewage permineralization, and need additional electric energy.Therefore photo-electrocatalytic technology combines with other techniques by Many researchers, as combined with biological process, to realize advanced treatment.Other direction, the input of sustainability cheap electric energy, can significantly reduce photo-electrocatalytic technology cost.
Microbiological fuel cell (Microbialfuelcell, MFC) is a kind of energy conversion device participated in by microorganism, can be electric energy by the chemical energy in sewage, synchronously realize sewage purification and electrogenesis.MFC development prospect more and more receives publicity.But compare with normal power supplies, to produce electric power quality all lower for MFC electrogenesis power and institute, be difficult to be directly incorporated into electrical network use.The low-quality electric energy of MFC output how is effectively utilized to be the large technical barrier that current MFC studies.Other direction, single-stage MFC is more difficult realizes organic advanced treatment (permineralization).
Although someone proposes MFC and other technologies coupling (Sun Zhe etc., 2014; Xie Qing etc., 2010) however described coupling all just mention general, be only that circuit connects or water route connects individually at the most, and fail to realize effectively being connected respectively on circuit with water route simultaneously, and then the height cooperation in realizing circuit water route.Not by theoretical restriction, applicant proposes, and the key that photoelectrocatalysis preoxidation coordinates with the height in MFC circuit water route is whether effectively to control the running balance between electronics and material.Utilize photoelectrocatalysis preoxidation organic waste water, after preoxidation, intermediate product is usually extremely complicated, and preoxidation degree is different, and product composition and toxicity difference are comparatively large, and it often brings disadvantageous effect in the electricity generation performance of follow-up MFC and deep purifying degree; On the other hand, the quality of follow-up MFC institute electrogenesis energy also has a significant effect to the stability tool that photoelectrocatalysis runs conversely.As high in photoelectrocatalysis preoxidation degree, the carbon source of supply MFC is not enough, and the electron deficiency of its Gong photoelectrocatalysis preoxidation produced, causes photoelectrocatalysis preoxidation degree to reduce conversely; As low in photoelectrocatalysis preoxidation degree, water outlet structure of matter composition is too complicated, and single-stage MFC is difficult to effectively utilize electrogenesis, and is difficult to the degree of depth mineralising realizing water body.Therefore, how effectively controlling electronics is the difficult point that realizing circuit and water route effectively coordinate simultaneously with the running balance between material, is also the technical barrier that prior art is thirsted for solving.
Patent publication No. CN103265149A reports a kind of electro-adsorption process waste water plant without the need to additional power source and method, and MFC utilizes and is easy to biodegradable material electrogenesis, and the electric energy of generation is used for electro-adsorption; Electro-adsorption is used for absorption and is difficult to biodegradable material, although the electric energy original position that this patent achieves MFC utilizes, is inspissated, can not removes from environment for recalcitrant substance.Patent publication No. CN103266331A reports the method that the self-driven microorganism electrolysis cell coupled system of a kind of microbiological fuel cell reclaims simple substance cobalt from cobalt acid lithium, for the recovery of heavy metal, but its be also only achieve MFC institute electrogenesis can original position utilize, and fail the coupling that realizes on water route.LiuXianwei (Liuetal., 2012) two-chamber-type air cathode MFC is coupled with anode Fenton, also the two room air cathode MFC of research and utilization H type is had to be coupled with cathode electro-Fenton (FernandezdeDiosetal., 2013), such report is all only that the original position achieving MFCs institute electrogenesis energy utilizes, and fails to realize water route coupling.LiJun (Lietal., 2013) single chamber is overlapped photosynthetic organism hydrogen generation reactor (PBR) without barrier film air cathode MFC and two to be coupled on water route, MFC anode can change the composition of voltaile fatty acid in the water outlet of photosynthetic organism hydrogen generation reactor, and negative electrode can remove extra proton, substrate solution is made more to be applicable to the carrying out of follow-up product H-H reaction, it achieves the coupling in water route, but does not have the original position of MFC electric energy to utilize.
Therefore, in prior art still in the urgent need to having the organic wastewater with difficult degradation thereby treatment technology of good treatment effect and less energy-consumption simultaneously.
Summary of the invention
The present inventor is through test of many times, find unexpectedly, by photoelectrocatalysioxidization oxidization and MFC combine with technique, be effectively connected respectively on circuit with water route and coordinate simultaneously, running balance between effective control electronics and material, can realize gratifying water treatment effect.The present inventor finds under study for action, if effectively coordinated with two-stage MFC by photoelectrocatalysioxidization oxidization and be connected, likely overcomes the problems referred to above and shortcoming.Specifically, the present inventor finds, described photoelectrocatalysis unit is connected respectively with MFC and coordinates simultaneously on circuit and water route, and adopt two-stage MFC to connect on water route simultaneously, but it is independent on circuit both keeping, effectively can control the running balance between electronics and material, and then desired technique effect is provided.
Therefore, in first, the invention provides a kind of device for the treatment of organic wastewater with difficult degradation thereby, comprise photoelectrocatalysis unit and microbiological fuel cell (MFC) coupled system, wherein said photoelectrocatalysis unit is connected respectively with MFC and coordinates simultaneously on circuit and water route, and wherein said microbiological fuel cell comprises one-level MFC and secondary MFC connects on water route, described one-level MFC is connected by water route with photoelectrocatalysioxidization oxidization unit, and water body is first through photoelectrocatalysioxidization oxidization, and water outlet enters one-level MFC; On circuit, described two-stage MFC is independent separately, provides bias voltage respectively to photocatalysis apparatus.
Result of study according to us finds, in circuit arrangement, make two-stage MFC independent separately, provide bias voltage to respectively photoelectrocatalysioxidization oxidization device, there is reverse electrode phenomena when can effectively prevent front and back stages MFC voltage phase difference larger, and the stability of power supply can be ensured.
In preferred at one, MFC of the present invention has two-chamber-type structure, it comprises by the separated cathode compartment of cationic exchange membrane and anolyte compartment, described anolyte compartment and cathode compartment are filled with activated carbon granule, and described cathode compartment and anolyte compartment are respectively arranged with circulation line and at outer setting circulation vessel, described circulation line two ends are connection electrode cavity and circulation vessel respectively.Like this, effectively can improve waste water treatment efficiency, ensure the stability of effluent quality; Two-stage MFC series connection simultaneously, the Complex water body produced in various degree for photoelectrocatalysis preoxidation has certain buffering usefulness, effectively control the running balance between electronics and material, improve the electrogenesis stability of MFC, ensured that effluent quality obtains deep purifying simultaneously.
MFC in the present invention can also adopt three grades of even more senior MFC to connect according to actual needs.But when adopting three or more level MFC series connection, internal mass transfer resistance significantly improves usually, correspondingly need the quantity increasing peristaltic pump, this can increase running cost; What is more important, during three or more level MFC series connection, the third stage or the fourth stage and above MFC are difficult to obtain carbon source from anolyte, show corresponding MFC output voltage and remain unchanged or slowly slightly decline.
In another aspect of this invention, provide a kind of method processing organic wastewater with difficult degradation thereby, comprise and use photoelectrocatalysioxidization oxidization unit and microbiological fuel cell (MFC) coupled system, wherein said photoelectrocatalysioxidization oxidization unit is connected respectively with MFC and coordinates simultaneously on circuit and water route, and wherein said microbiological fuel cell comprises one-level MFC and secondary MFC connects on water route, described one-level MFC is connected by water route with photoelectrocatalysioxidization oxidization unit; On circuit, described two-stage MFC is independent separately, provides bias voltage to respectively photoelectrocatalysioxidization oxidization device; Described method comprises makes organic waste water first carry out pre-treatment by photocatalysis unit, then after shock-absorbing capacity regulates as MFC electrogenesis substrate once via one-level MFC and secondary MFC process.
In preferred at one, in the method for the invention, described MFC has two-chamber-type structure, it comprises by the separated cathode compartment of cationic exchange membrane and anolyte compartment, described anolyte compartment and cathode compartment are filled with activated carbon granule, and described cathode compartment and anolyte compartment are respectively arranged with circulation line and at outer setting circulation vessel, described circulation line two ends are connection electrode cavity and circulation vessel respectively, the described waste water through two-stage MFC process circulates, to be further processed between anode circulation container and two-stage MFC anolyte compartment.
Particularly preferred, in the method for the invention, described organic waste water is wastewater containing phenol.
In another, the purposes of device according to the present invention for the treatment of organic wastewater with difficult degradation thereby is additionally provided of the present invention.Particularly preferred, described organic waste water is wastewater containing phenol.
Accompanying drawing explanation
Fig. 1 is the present invention's a kind of two-chamber-type MFC device schematic diagram used;
Fig. 2 is the schematic diagram of a kind of photoelectrocatalysis testing apparatus adopted in the present invention;
Fig. 3 is secondary MFC-photoelectrocatalysioxidization oxidization coupling process organic waste water device schematic diagram of the present invention;
Fig. 4 shows the effect adopting device of the present invention to carry out wastewater containing phenol process.
Embodiment
The present invention is illustrated below in conjunction with accompanying drawing and further detailed description in detail.It is pointed out that following explanation is only illustrating the technical scheme that application claims is protected, any restriction not to these technical schemes.The content that protection scope of the present invention is recorded with appended claims is as the criterion.
In the present invention, microbiological fuel cell (MicrobialFuelCell, MFC) is a kind of technology well known in the art, and it utilizes microorganism that the chemical energy in organism is directly changed into electric energy.Its basic functional principle is: under anolyte compartment's anaerobic environment, organism decomposes and discharges electronics and proton under microbial process, electronics relies on suitable electron transfer mediator effectively to transmit between biological components and anode, and be delivered to negative electrode formation electric current by external circuit, and proton is delivered to negative electrode by proton exchange membrane, oxygenant (being generally oxygen) obtains electronics at negative electrode and is reduced and is combined into water with proton.
By device of the present invention or method, with industrial organic waste water or sanitary sewage for object, photoelectrocatalysioxidization oxidization is organically combined with MFC, form the method that a kind of photoelectrocatalysis-microbiological fuel cell coupling processing organic waste water realizes less energy-consumption, the method utilizes photo-electro chemical oxidation organism activity high but the feature that selectivity is not high, lower bias voltage is utilized to be oxidized by organic pollutant, improve the biodegradability of sewage thus, reduce water quality toxicity simultaneously, or macromolecular substance is converted into the biological small-molecule substance more easily utilized, and then improve efficiency of fuel cell generation and the operation stability of MFC, the electric energy that organism in MFC degradation of sewage produces is directly used in photoelectrocatalysis reaction member simultaneously, achieves electric energy original position and utilize, further increase the practical application potentiality of MFC.
By method of the present invention, make MFC technology carry out being coupled and mating with on photoelectro-catalytic oxidation technology water route He on circuit simultaneously, effectively can realize two kinds of technology whereby to the effect of sewage disposal, not only range of application can be opened up, and efficiency of fuel cell generation and the detergent power of MFC can be improved, make MFC institute electrogenesis be fully used simultaneously.
In order to verify effect of the present invention, adopt wastewater containing phenol as organic waste water, adopt two cavity two-chamber-type MFC reactor (see Fig. 1), full column type active carbon particles is all filled by anolyte compartment and anolyte compartment, cathode compartment and anolyte compartment's cationic exchange membrane separate, and cavity body volume is 115mL.Anolyte, namely anode electrogenesis substrate solution is made up of organic carbon source and inorganic salt, is specially: 50mM phosphate buffer (potassium primary phosphate KH
2pO
4h
2o4.4g/L, dipotassium hydrogen phosphate K
2hPO
43.4g/L), ammonium chloride NH
4cl0.31g/L, MgCl
26H
2o0.1g/L, CaCl
22H
2o0.1g/L and on a small quantity VITAMIN and trace element, organic carbon source is: anhydrous sodium acetate NaAc1.64g/L (degraded product of phenol or phenol).Cathode substrate consists of 50mM phosphate buffer, sodium bicarbonate NaHCO
31.92g/L, NH
4cl0.31g/L, MgCl
26H
2o0.1g/L, CaCl
22H
2o0.1g/L.For ensureing there is sufficient dissolved oxygen in catholyte, carry out continuous aeration with the solution in miniature aeration pump anticathode circulation bottle.
Photoelectrocatalysioxidization oxidization device: as shown in Figure 2, photoelectrocatalysioxidization oxidization reaction is carried out in a homemade cuboid quartz glass reactor, and whole pilot system is made up of titanium dioxide nanotube electrode (working electrode), titanium plate (to electrode), ultraviolet source (visible light source), magnetic stirring apparatus, electrochemical workstation etc.Photoelectrocatalysioxidization oxidization device is coupled with MFC, during reaction, the external resistance at MFC two ends is disconnected, and by the cathode and anode of MFC respectively with the working electrode in photoelectrocatalysidevice device and to Electrode connection, the voltage in reaction process and curent change situation are recorded by System of voltage acquisition and reometer respectively.
Embodiment
When 1 single-stage MFC and two-stage MFC connects on water route, organic matter removal situation compares
Electricity generation performance and organic matter removal effect during series operation on single-stage MFC and two-stage MFC water route under the identical water quality and quantity of Test and Comparison Study.Anolyte compartment intakes as the initial phenol concentration through photoelectrocatalysioxidization oxidization pre-treatment 4h is the degraded product of 400mg/L, and volume is 200mL.As can be seen from result, during single-stage MFC treatment of simulated phenolic wastewater degraded product, after more fresh fuel, voltage raises fast, and rise to maximum value after about 3h, then start slow decline, maximum voltage increasing degree is 97mV.Connect in water route two-stage MFC, the voltage change situation difference of front and back stages MFC is comparatively large, and the maximum voltage increasing degree of 1#MFC and 2#MFC is respectively 135mV and 101mV, and difference is the relatively high pressure time length of 34mV, 1#MFC be longer than 2#MFC.When connecting in water route, the carbon source in anolyte is mainly absorbed by the MFC of front end and utilizes, and seldom, therefore the output voltage that MFC is overlapped in front and back two differs larger to carbon source remaining when anolyte flows through 2#MFC.
During single-stage MFC process waste water, after more fresh fuel, phenol concentration is reduced to about 4mg/L in 3h after water inlet, and examined in water outlet after 4h and do not measured phenol, corresponding phenol clearance can reach more than 99%; COD concentration can be reduced to about 40mg/L in 4h, and after 4h, COD concentration also keeps stable all the time between 26 ~ 30mg/L, and corresponding COD clearance can reach 96% ~ 97%.When two-stage MFC connects, more after fresh fuel, namely phenol concentration is reduced to 4mg/L after 1h, has examined and do not measure phenol after 2h in water outlet; COD concentration is reduced to about 40mg/L rapidly after 1h, continues to be reduced to also to keep stable between 25 ~ 30mg/L after 2h.It can thus be appreciated that can significantly improve sewage treating efficiency during the series connection of water route, for reaching identical effluent quality, the time needed during single MFC and two cover MFC series connection process is respectively 4h and 2h.
2 two-stage series connection MFC-photoelectrocatalysioxidization oxidizations are coupled with on water route at circuit simultaneously
Photoelectrocatalysioxidization oxidization-MFCs coupled system is coupled on circuit and water route simultaneously.Coupled system as shown in Figure 3.On water route, simulation phenolic wastewater first carries out pre-treatment 4h by photoelectrocatalysis unit, and as MFC anolyte compartment electrogenesis substrate, wastewater treatment is carried out in two-stage MFC series connection, and waste water, at circulation bottle and the inner constantly circulation of MFC 3 ~ 4h, completes wastewater treatment process; On circuit, for there is reverse electrode phenomena when preventing two cover MFC voltage phase difference larger, electrocatalysis unit is powered by the higher more stable a set of MFC of voltage.
Simulation phenolic wastewater is through photoelectrocatalysis pre-treatment 4h, again after MFC process 2h, and phenol clearance also keeps stable close to 100%, COD clearance higher than 97%, COD content between 26 ~ 30mg/L.
Fig. 4 is the treatment effect of this coupled system to simulation phenolic waste water.In simulation phenolic waste water, initial phenol concentration is about 400mg/L, first through photoelectrocatalysioxidization oxidization pre-treatment 4h, after use after 50mM phosphate buffered saline buffer adjust ph as MFC electrogenesis substrate, discharge after two-stage MFC anolyte compartment internal recycle 2h, as complete cycle of operation, two cycles are run continuously altogether.As can be seen from the figure, within two cycles run continuously, initial phenol concentration is that the simulation phenolic wastewater of 410mg/L is through photoelectrocatalysis pre-treatment 4h, again after MFC process 2h, phenol clearance is close to 100%, COD clearance is 97% ~ 98%, examined in water outlet and do not measured phenol, COD content is between 26 ~ 30mg/L and maintenance is stable.Above result absolutely proves, the coupled system that the present invention sets up is respond well for combination treatment simulation phenolic wastewater, synchronously achieves sewage purification and electrogenesis, improves the comprehensive utilization ratio of phenolic wastewater.
Reference:
1. Sun Zhe, Huang Manhong, Chen Liang, Chen Donghui. photocatalyst-type Development of Microbiol Fuel Cells. Treatment of Industrial Water, 2014,34 (3): 11-14.
2. thank fine, Yang Jiawei, Wang Bin, cold heptan, but moral is loyal. for the microbiological fuel cell research latest developments of sewage disposal. water technology, 2010,36 (3): 10-14.
3.FernandezdeDios，M.A.，delCampo，A.G.，Fernandez，F.J.，Rodrigo，M.，Pazos，M.，Sanroman，M.A.，2013.Bacterial-fungalinteractionsenhancepowergenerationinmicrobialfuelcellsanddrivedyedecolourisationbyanexsituandinsituelectro-Fentonprocess.Bioresourcetechnology148，39-46.
4.Li，J.，Zou，W.，Xu，Z.，Ye，D.，Zhu，X.，Liao，Q.，2013.Improvedhydrogenproductionofthedownstreambioreactorbycouplingsinglechambermicrobialfuelcellsbetweenseries-connectedphotosyntheticbiohydrogenreactors.InternationalJournalofHydrogenEnergy38，15613-15619.
5.Liu，X.W.，Sun，X.F.，Li，D.B.，Li，W.W.，Huang，Y.X.，Sheng，G.P.，Yu，H.Q.，2012.AnodicFentonprocessassistedbyamicrobialfuelcellforenhanceddegradationoforganicpollutants.Waterresearch46，4371-4378.
Claims (5)
1. the device for the treatment of organic wastewater with difficult degradation thereby, comprise photoelectrocatalysioxidization oxidization unit and microbiological fuel cell (MFC) coupled system, wherein said photoelectrocatalysioxidization oxidization unit is connected respectively with MFC and coordinates simultaneously on circuit and water route, and wherein said microbiological fuel cell comprises one-level MFC and secondary MFC connects on water route, described one-level MFC is connected by water route with photoelectrocatalysioxidization oxidization unit, and water body is first through photoelectrocatalysioxidization oxidization, and water outlet enters one-level MFC; On circuit, described two-stage MFC is independent separately, provides bias voltage to respectively photoelectrocatalysioxidization oxidization device.
2. device according to claim 1, wherein said MFC has two-chamber-type structure, it comprises by the separated cathode compartment of cationic exchange membrane and anolyte compartment, described anolyte compartment and cathode compartment are filled with activated carbon granule, and described cathode compartment and anolyte compartment are respectively arranged with circulation line and at outer setting circulation vessel, described circulation line two ends are connection electrode cavity and circulation vessel respectively.
3., according to the device of claim 1 or 2, wherein said device has structure as shown in Figure 1.
4. device as claimed in one of claims 1-3 is for the treatment of the purposes of organic wastewater with difficult degradation thereby.
5. purposes according to claim 4, wherein said organic wastewater with difficult degradation thereby is wastewater containing phenol.
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