CN104150607A - Device and method for degrading phenol and ammonia nitrogen simultaneously by virtue of microbial fuel cell - Google Patents

Device and method for degrading phenol and ammonia nitrogen simultaneously by virtue of microbial fuel cell Download PDF

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Publication number
CN104150607A
CN104150607A CN201410371379.7A CN201410371379A CN104150607A CN 104150607 A CN104150607 A CN 104150607A CN 201410371379 A CN201410371379 A CN 201410371379A CN 104150607 A CN104150607 A CN 104150607A
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phenol
ammonia nitrogen
fuel cell
degradation
cathode
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CN104150607B (en
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冯春华
杨晓双
黄丽巧
吕志盛
余辉
韦朝海
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South China University of Technology SCUT
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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

Abstract

The invention belongs to the technical field of wastewater treatment and discloses a device and method for degrading phenol and ammonia nitrogen simultaneously by virtue of a microbial fuel cell. The method comprises the following steps: by building a double-chamber microbial fuel cell system, inoculating domesticated electricity-producing mixed bacterial liquid and denitrifying bacteria to an anode chamber, adding sodium acetate as an electron donor, taking mixed liquid of a phosphate buffer solution of 0.1mol/L with pH value of 7.0 and culture liquid as nutritional substances, and meanwhile, providing a relatively strict anaerobic environment; adding phenol and ammonia nitrogen-containing wastewater and mixed sludge taking the nitrifying bacteria domesticated through ammonia nitrogen and phenol, and phenol degradation bacteria as main components into a cathode chamber, filling air through an aeration device, and connecting a closed circuit switch with an external circuit to start the microbial fuel cell so as to degrade ammonia nitrogen and phenol in the cathode chamber simultaneously. The device and the method are used for removing phenol and ammonia nitrogen in the wastewater, and have good economic and environment-friendly benefits.

Description

Utilize the device and method of microbiological fuel cell while degradation of phenol and ammonia nitrogen
Technical field
The invention belongs to technical field of sewage, be specifically related to a kind of device and method that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen.
Background technology
The problem of environmental pollution being on the rise is the two large fundamental issues that the mankind face on sustainable development path with seeking the new energy.Along with expanding economy, waste be treated as an important problem.Wherein trade effluent complicated component, strong toxicity, severe to environmental influence, deal with difficulty very big.In the trade effluents such as coking, petrochemical complex, synthetic ammonia and pharmacy waste water, contain a large amount of pollution substances such as phenol and ammonia nitrogen.Environmental Protection in America portion classifies phenol as the preferential excellent thing that dyes as, and phenol has corrodibility, the characteristic such as poisonous, when the phenol concentration in water reaches 5～25mg L -1can produce toxic action to fish, in tap water, the phenol of lower concentration also can produce detrimentally affect to human health; And nitrogenous effluent enters and can cause eutrophication in water body and cause water quality deterioration.The biological process dominate that the processing mode of nitrogenous effluent is low with energy consumption, processing efficiency is high, but the phenol material concentration in water body reaches 50mg L -1time can be to microorganisms restraining effect, how improving the adaptability that micropopulation drops on Pyrogentisinic Acid's concentration in denitrification process is effectively to process the key of phenolic comp ' ds pollution matter and nitrogen-containing pollutant.
The main method of processing at present phenolic waste water has adsorption photochemical catalysis, anaerobic degradation, aerobic degradation etc.And taking active sludge as main aerobic, anaerobism mode because cost is low, efficiency is high becomes the optimal selection of processing multiple mixed pollutants.The bacterial species of degradation of phenol and ammonia nitrogen is abundant according to reports, but because phenol has stronger restraining effect to methanogen, has limited the application of anaerobic process.And become with aerobic method Synergistic degradation phenol and ammonia nitrogen waste water the focus that people pay close attention to.The ability that microbiological fuel cell has the complicated organism of degraded electrogenesis with it has simultaneously obtained great concern.At present of common occurrence as the research of microbiological fuel cell electron donor electrogenesis using complicated organism, utilize microbiological fuel cell biological-cathode to carry out denitrification and nitration reaction has also obtained coverage.Therefore synchronize and degrade with ammonia nitrogen waste water for realizing phenol, reclaim electric energy simultaneously, realize effective utilization of resource, we must change the mode of traditional microbiological fuel cell processing waste water, invent a kind of method and apparatus that utilizes microbiological fuel cell technology to combine with water technology, realizing phenol synchronizes and degrades with ammonia nitrogen, recovered energy applies for expanding traditional microbiological fuel cell technology the thinking that provides new in water treatment simultaneously.
Summary of the invention
In order to solve the shortcoming and defect part of prior art, primary and foremost purpose of the present invention is to provide a kind of device that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen.
Another object of the present invention is to provide a kind of method of utilizing said apparatus while degradation of phenol and ammonia nitrogen.
The object of the invention is achieved through the following technical solutions:
A kind of device that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen, formed by anolyte compartment and cathode compartment, anolyte compartment and cathode compartment are separated by anion-exchange membrane, anolyte compartment arranges galvanic anode liquid adding hole and anode electrode, cathode compartment arranges negative electrode liquid adding hole, aerating apparatus and cathode electrode, aerating apparatus is arranged on cathode compartment bottom, and anode electrode is connected by external circuit with cathode electrode, and external circuit arranges pull-up resistor and contactor.
Described anode electrode and the preferred carbon paper of the material of cathode electrode, carbon cloth, graphite felt, stainless (steel) wire or nickel foam; More preferably pass through pretreated graphite felt, described pretreatment process is that graphite felt is placed in to massfraction is 10% hydrogen peroxide solution, be that 2h is boiled in 90 DEG C of Water Unders baths in temperature, then boil 2h with deionized water water-bath under same temperature, then use oven for drying.
The resistance value of described pull-up resistor is 1000 Ω preferably.
A method of utilizing said apparatus while degradation of phenol and ammonia nitrogen, comprises following operation steps:
The inoculation of anode chamber, through electrogenesis mixed bacteria liquid and the denitrifying bacteria of domestication, adds sodium acetate as electron donor, with 0.1mol L -1the phosphate buffer solution of pH 7.0 and the mixed solution of nutrient solution are nutritive substance, and relatively strict anaerobic environment is provided simultaneously; It is master's mixing sludge containing nitrobacteria and the Phenol-degrading Bacteria Strains of the sewage of phenol and ammonia nitrogen and process ammonia nitrogen and phenol domestication that cathode compartment adds containing different concns, and pass into air by aerating apparatus, then closed circuit switch is communicated with external circuit, microbiological fuel cell operation starts, and the ammonia nitrogen of cathode compartment and phenol are degraded simultaneously.
Described domestication refers to tames with sodium acetate.
Described 0.1mol L -1the composition of the phosphate buffer soln of pH 7.0 and the mixed solution of nutrient solution comprises 22.2g L -1na 2hPO 4, 5.92g L -1naH 2pO 4, 1.0g L -1naHCO 3, 0.10g L -1feSO 4, 0.10g L -1kCl, 0.015g L -1caCl 2, 0.25g L -1nH 4cl, 10mL L -1mineral solution and 10mL L -1vitamin b6 usp.
Described mineral solution composition comprises 1.5g L -1c 6h 6nO 63Na12H 2o, 0.13g L -1znCl 2, 3.0g L -1mgSO 4, 0.01g L -1cuSO 45H 2o, 0.5g L -1mnSO 4h 2o, 0.01g L -1alK (SO 4) 212H 2o, 1.0g L -1naCl, 0.01g L -1h 3bO 3, 0.1g L -1feSO 47H 2o, 0.025g L -1na 2moO 4, 0.1g L -1caCl 22H 2o, 0.024g L -1niCl 26H 2o, 0.1g L -1coCl 26H 2o and 0.025g L -1na 2wO 42H 2o.
Principle of the present invention is:
There is the microbiological fuel cell of anolyte compartment and cathode compartment by structure, electrogenesis bacterium in anolyte compartment utilizes sodium acetate to produce electronics, in cathode compartment, adding through nitrobacteria and the Phenol-degrading Bacteria Strains of ammonia nitrogen and phenol domestication is master's mixing sludge, pass into oxygen (being similar to the Aerobic Pond processing of traditional water treatment) simultaneously, the electronics acting in conjunction being produced by anolyte compartment on this basis, thereby reach the nitrated of the degraded of phenol and ammonia nitrogen, the NO that nitrification produces 3 -/ NO 2 -under the effect of concentration gradient, enter anode through anion-exchange membrane, what under the effect of anode denitrifying bacteria, occur that thereby denitrification realizes nitre nitrogen nitrite nitrogen is further degraded to nitrogen, make the ammonia nitrogen in cathode compartment constantly transform simultaneously, finally reach ammonia nitrogen and synchronize and degrade with phenol.
The material of electrode preferably passes through pretreated graphite felt, and graphite felt has higher specific surface area, good biocompatibility and reasonable price, graphite felt is carried out to pre-treatment and be conducive to improve its stability and electroconductibility.
Have the following advantages and beneficial effect by method of the present invention and device tool:
(1) invention adopts biological-cathode and anode electrogenesis to impel the degraded of pollutent, and microbiological fuel cell is combined with traditional aerobic water technology, can realize the phenol that is difficult to realize in traditional water treatment method and synchronize the object of degrading with ammonia nitrogen;
(2) mode of negative electrode employing aeration in invention, on the one hand for providing microbiological deterioration pollutent required oxygen, remaining O on the other hand 2can be used as electron acceptor(EA) and realize the electrogenesis of microbiological fuel cell.This method is applied to actual waste water Aerobic, can improve the utilization ratio of oxygen, thus save energy;
Brief description of the drawings
Fig. 1 is a kind of apparatus structure schematic diagram that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen of embodiment 1, in figure, mark is described as follows: 1-anolyte compartment, 2-cathode compartment, 3-anion-exchange membrane, 4-anode liquid adding hole, 5-anode electrode, 6-negative electrode liquid adding hole, 7-aerating apparatus, 8-cathode electrode, 9-external circuit, 10-pull-up resistor, 11-contactor.
Fig. 2 is the degraded figure of the apparatus and method of the embodiment of the present invention 1 ammonia nitrogen and phenol while processing different phenol concentration;
Fig. 3 is the degraded figure of the apparatus and method of the embodiment of the present invention 1 ammonia nitrogen and phenol under different dissolved oxygen (DO) condition;
Fig. 4 is the voltage-time diagram of apparatus and method battery under different dissolved oxygen (DO) condition of the embodiment of the present invention 1.
Embodiment
Below in conjunction with embodiment, the present invention is described in further detail, but embodiments of the present invention are not limited to this.
Embodiment 1
A kind of device that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen of the present embodiment, formed by anolyte compartment 1 and cathode compartment 2, anolyte compartment and cathode compartment are separated by anion-exchange membrane 3, anolyte compartment arranges galvanic anode liquid adding hole 4 and anode electrode 5, cathode compartment arranges negative electrode liquid adding hole 6, aerating apparatus 7 and cathode electrode 8, anode electrode is connected by external circuit 9 with cathode electrode, and external circuit arranges pull-up resistor 10 and contactor 11.
The device of the present embodiment is for removing and reclaim the method for ammonia nitrogen in sewage, and concrete steps are: the inoculation of anode chamber, through electrogenesis mixed bacteria liquid and the denitrifying bacteria of domestication, adds sodium acetate as electron donor, with 0.1molL -1the phosphate buffer solution of pH 7.0 and the mixed solution of nutrient solution are nutritive substance, and relatively strict anaerobic environment is provided simultaneously; Cathode compartment adds containing the sewage of different concns phenol and ammonia nitrogen and is master's mixing sludge through nitrobacteria and the Phenol-degrading Bacteria Strains of ammonia nitrogen and phenol domestication, and pass into air by aerating apparatus, then closed circuit switch is communicated with external circuit, microbiological fuel cell operation starts, the phenol of cathode compartment is degraded by Phenol-degrading Bacteria Strains, and ammonia nitrogen is converted into NO through nitrobacteria 3 -/ NO 2 -under the effect of concentration gradient, enter anode through anion-exchange membrane, thus under the effect of anode denitrifying bacteria, occur that denitrification realizes nitre nitrogen nitrite nitrogen be further degraded to nitrogen, make the ammonia nitrogen in cathode compartment constantly transform degraded simultaneously.
The cathode electrode of the present embodiment and the material of anode electrode are the electrode of pre-treatment graphite felt according to the following steps:
It is 10% hydrogen peroxide solution that graphite felt is placed in to massfraction, at 90 DEG C, 2h is boiled in water-bath, then boil 2h with deionized water water-bath under same temperature, then with being cut into long 7cm × wide 4cm size after oven for drying, put on and obtain pre-treatment graphite felt electrode with titanium silk.
Assembled battery: the anode of handling well is installed on anode casing, and concrete grammar is as follows:
The titanium silk of pre-treatment graphite felt anode electrode is passed by interior outward from anode casing aperture, electrode plane is parallel with anode casing board plane, titanium silk and anode casing aperture are glued with AB glue, place and within about 5 minutes, make it solidify, to pack in the same way cathode compartment into through pretreated graphite felt cathode electrode, again anion-exchange membrane is pressed on cathode compartment housing, then with anode casing, cathode shell, ion-exchange membrane is fixed to the screw nut of finally screwing on.
The device of the present embodiment is for removing and reclaim the method for ammonia nitrogen in sewage, and specific operation process is as follows: inoculation 10mL in anode chamber, through the electrogenesis mixed bacteria liquid of domestication, adds 20mmol L -1sodium acetate is as electron donor, the phosphate buffer soln and the nutrient solution that are 7.0 with pH are filled it up with reactor, it is 7.0 phosphate buffer soln that cathode compartment adds pH, and by aerating apparatus aeration, with gas meter control cathode aeration rate, external 1000 ohmic resistances, access the voltage collector of 32 passages, operation starts, and when loss of voltage is to 20mV, again changes liquid and cultivates, move at least one month, when after voltage stabilization, negative electrode adds the bacterium liquid of having tamed, and wherein the bacterium liquid acclimation method of negative electrode inoculation is as follows:
(1) taking nitrobacteria as main mud:
Take from Shaoguan, Guangzhou second phase Treatment of Coking Effluent two-stage Aerobic Pond mud, cultivate at the indigo plant lid bottle aeration of 1000mL.Mud adopts fresh NH 4cl nutrient solution replaces coking chemical waste water, and for enrichment culture nitrobacteria, nutrient solution composition also comprises: 0.1mol L -1phosphate buffer soln, 1.0g L -1naHCO 3, 0.10gL -1feSO 4, 0.10g L -1kCl, 0.015g L -1caCl 2, 10mL mineral solution and 10mL vitamin b6 usp, wherein every liter of mineral solution composition is by 1.5g C 6h 6nO 63Na12H 2o, 0.13g ZnCl 2, 3.0gMgSO4,0.01g CuSO 45H 2o, 0.5g MnSO 4h 2o, 0.01g AlK (SO 4) 212H 2o, 1.0gNaCl, 0.01g H 3bO 3, 0.1g FeSO 47H 2o, 0.025g Na 2moO 4, 0.1g CaCl 22H 2o, 0.024g NiCl 26H 2o, 0.1g CoCl 26H 2o and 0.025g Na 2wO 42H 2o composition.
(2) taking Phenol-degrading Bacteria Strains as main mud:
Phenol microbial culture mud is taken from Shaoguan second phase Treatment of Coking Effluent one-phase Aerobic Pond, and its acclimation method is compared with nitrobacteria sludge acclimatization method, and difference is NH 4cl nutrient solution changes phenol nutrient solution into, and rest part is identical.
The degraded situation of the apparatus and method of the present embodiment ammonia nitrogen and phenol in the time of different phenol concentration:
In the device cathode compartment after voltage stabilization, add 230mg L -1ammonia nitrogen, adding respectively concentration is 200mg L -1, 400mg L -1with 800mg L -1phenol solution, the different sampling times is set in operational process samples in negative electrode, after sampling, adopt respectively nessler reagent spectrophotometry and tetramino peace to measure the concentration of ammonia nitrogen and phenol for neighbour light-intensity method, until concentration will be 0, the degraded situation of concrete ammonia nitrogen and phenol as shown in Figure 2, under the condition of different concns phenol solution, the degraded of ammonia nitrogen is not suppressed as seen from Figure 2.
The degraded situation of the apparatus and method of the present embodiment ammonia nitrogen and phenol under different dissolved oxygen conditions:
In the device cathode compartment after voltage stabilization, pass into different flow (0.5mg L by aerating apparatus -1, 1～2mg L -1, 2～4mg L -1) air, form respectively the environment of anoxic, aerobic and oxygen enrichment, the initial phenol concentration wherein adding is 600mg L -1, ammonia nitrogen concentration is 230mg L -1sampling time is set equally in battery operation process samples, then measure the concentration of phenol and ammonia nitrogen, until concentration reduces to 0, the degraded of concrete phenol and ammonia nitrogen as shown in Figure 3, can find out in cathode compartment that, under the environmental change from anoxic to oxygen enrichment, the degradation rate of phenol and ammonia nitrogen improves gradually, illustrates that the growth metabolism of aerobic nitrification bacterium and Phenol-degrading Bacteria Strains shows stronger vigor in the high environment of dissolved oxygen concentration.
Record the voltage of battery under different dissolved oxygen conditions simultaneously by 32 Multichannel data acquisition devices in battery operation process, since weigh the electricity generation ability of battery, concrete outcome as shown in Figure 4, can be found out, under the condition of different aeration rates, the voltage of battery increases along with the raising of DO concentration.0～70h is mainly the nitrification of ammonia nitrogen and the degraded of phenol, is diffused into the NO of anode 3 -at the denitrifying electronics of competing anode simultaneously, make its voltage in this stage lower; To after 70h along with NO in denitrification 3 -the reduction of concentration, competition electronic capability weakens, and voltage improves gradually; Dissolved oxygen in negative electrode is meeting under condition nitrated and that phenol degrading is required, simultaneously as cathode electronics acceptor.
Above-described embodiment is preferably embodiment of the present invention; but embodiments of the present invention are not restricted to the described embodiments; other any do not deviate from change, the modification done under spirit of the present invention and principle, substitutes, combination, simplify; all should be equivalent substitute mode, within being included in protection scope of the present invention.

Claims (8)

1. one kind is utilized the device of microbiological fuel cell while degradation of phenol and ammonia nitrogen, it is characterized in that: described device is made up of anolyte compartment and cathode compartment, anolyte compartment and cathode compartment are separated by anion-exchange membrane, anolyte compartment arranges galvanic anode liquid adding hole and anode electrode, cathode compartment arranges negative electrode liquid adding hole, aerating apparatus and cathode electrode, aerating apparatus is arranged on cathode compartment bottom, and anode electrode is connected by external circuit with cathode electrode, and external circuit arranges pull-up resistor and contactor.
2. a kind of device that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen according to claim 1, is characterized in that: described anode electrode and the material of cathode electrode are carbon paper, carbon cloth, graphite felt, stainless (steel) wire or nickel foam.
3. a kind of device that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen according to claim 2, it is characterized in that: described graphite felt refers to through pretreated graphite felt, described pretreatment process is that graphite felt is placed in to massfraction is 10% hydrogen peroxide solution, be that 2h is boiled in 90 DEG C of Water Unders baths in temperature, then boil 2h with deionized water water-bath under same temperature, then use oven for drying.
4. a kind of device that utilizes microbiological fuel cell while degradation of phenol and ammonia nitrogen according to claim 1, is characterized in that: the resistance value of described pull-up resistor is 1000 Ω.
5. utilize device described in a claim 1～4 any one method for degradation of phenol and ammonia nitrogen simultaneously, it is characterized in that comprising following operation steps:
The inoculation of anode chamber, through electrogenesis mixed bacteria liquid and the denitrifying bacteria of domestication, adds sodium acetate as electron donor, with 0.1mol L -1the phosphate buffer solution of pH 7.0 and the mixed solution of nutrient solution are nutritive substance, and relatively strict anaerobic environment is provided simultaneously; Cathode compartment adds containing the sewage of phenol and ammonia nitrogen and is master's mixing sludge through nitrobacteria and the Phenol-degrading Bacteria Strains of ammonia nitrogen and phenol domestication, and pass into air by aerating apparatus, then closed circuit switch is communicated with external circuit, microbiological fuel cell operation starts, and the ammonia nitrogen of cathode compartment and phenol are degraded simultaneously.
6. the method for a kind of while degradation of phenol according to claim 5 and ammonia nitrogen, is characterized in that: described domestication refers to tames with sodium acetate.
7. the method for a kind of while degradation of phenol according to claim 5 and ammonia nitrogen, is characterized in that: described nutrient solution composition comprises 1.0g L -1naHCO 3, 0.10g L -1feSO 4, 0.10g L -1kCl, 0.015g L -1caCl 2, 0.25g/L NH 4cl, 10mL L -1mineral solution and 10mL L -1vitamin b6 usp.
8. the method for a kind of while degradation of phenol according to claim 7 and ammonia nitrogen, is characterized in that: described mineral solution composition comprises 1.5g L -1c 6h 6nO 63Na12H 2o, 0.13g L -1znCl 2, 3.0gL -1mgSO 4, 0.01g L -1cuSO 45H 2o, 0.5g L -1mnSO 4h 2o, 0.01g L -1alK (SO 4) 212H 2o, 1.0g L -1naCl, 0.01g L -1h 3bO 3, 0.1g L -1feSO 47H 2o, 0.025g L -1na 2moO 4, 0.1g L -1caCl 22H 2o, 0.024g L -1niCl 26H 2o, 0.1g L -1coCl 26H 2o and 0.025g L -1na 2wO 42H 2o.
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CN106229535A (en) * 2016-09-10 2016-12-14 华南理工大学 The device utilizing three electrode storage biological powers and the method storing biological power thereof
CN106229535B (en) * 2016-09-10 2019-04-09 华南理工大学 Utilize the method for the device and its storage biological power of three electrode storage biological powers
CN107010714A (en) * 2017-05-22 2017-08-04 东北大学 Waste Water Treatment and method that biological electro catalysis are coupled with photocatalytic contact oxidation
CN108675444A (en) * 2018-04-18 2018-10-19 厦门大学 A kind of apparatus and method rapidly promoting anthraquinone dye decoloration based on microbiological fuel cell technology
CN113754044A (en) * 2021-09-13 2021-12-07 清华大学 Device and method for improving ammoniation rate of membrane preparation wastewater and application

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