CN104150607B - Utilize the device and method of microbiological fuel cell simultaneously degradation of phenol and ammonia nitrogen - Google Patents

Utilize the device and method of microbiological fuel cell simultaneously degradation of phenol and ammonia nitrogen Download PDF

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CN104150607B
CN104150607B CN201410371379.7A CN201410371379A CN104150607B CN 104150607 B CN104150607 B CN 104150607B CN 201410371379 A CN201410371379 A CN 201410371379A CN 104150607 B CN104150607 B CN 104150607B
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phenol
ammonia nitrogen
fuel cell
anode
degradation
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CN104150607A (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 technical field of sewage, disclose a kind of device and method utilizing microbiological fuel cell simultaneously degradation of phenol and ammonia nitrogen.By building double-chamber microbiological fuel cell system, electrogenesis mixed bacteria liquid and the denitrifying bacterium of domestication are passed through in the inoculation of anode room, add sodium acetate as electron donor, with 0.1mol? L -1pH? the phosphate buffer solution of 7.0 and the mixed liquor of nutrient solution are nutriment, provide relatively strict anaerobic environment simultaneously; It is main mixing sludge that cathode chamber adds containing the sewage of phenol and ammonia nitrogen and the nitrobacteria tamed through ammonia nitrogen and phenol and Phenol-degrading Bacteria Strains, and pass into air by aerator, then closed circuit switch is communicated with external circuit, microbiological fuel cell runs and starts, and the ammonia nitrogen of cathode chamber and phenol are degraded simultaneously.Be used for the removal of phenol and ammonia nitrogen in sewage by device and method of the present invention, there is good economic benefit and environmental benefit.

Description

Utilize the device and method of microbiological fuel cell simultaneously 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 utilizing microbiological fuel cell simultaneously degradation of phenol and ammonia nitrogen.
Background technology
The problem of environmental pollution be 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, discarded object be treated as an important problem.Wherein industrial wastewater complicated component, strong toxicity, severe to environmental impact, deal with difficulty very big.Containing the polluter such as a large amount of phenol and ammonia nitrogen in the industrial wastewaters such as coking, petrochemical industry, synthetic ammonia and pharmacy waste water.Environmental Protection in America portion is classified as phenol as preferential excellent dye thing, and phenol has corrosivity, the characteristic such as poisonous, when the phenol concentration in water reaches 5 ~ 25mgL -1can produce toxic action to fish, in drinking water, the phenol of low concentration also can produce harmful effect to human health; And nitrogenous effluent enters in water body and can cause eutrophication and cause water quality deterioration.The bioanalysis dominate that the processing mode of nitrogenous effluent is low with energy consumption, treatment effeciency is high, but the phenol material concentration in water body reaches 50mgL -1time can produce inhibitory action to microbe, how improving the adaptability that micropopulation drops on Pyrogentisinic Acid's concentration in denitrification process is the key effectively processing phenolic comp ' ds pollution matter and nitrogen-containing pollutant.
The main method of current process phenolic waste water has adsorption photochemical catalysis, anaerobic degradation, aerobic degradation etc.And aerobic, the anaerobism mode based on activated sludge becomes because cost is low, efficiency is high the optimal selection processing multiple mixed pollutants.The bacterial species of degradation of phenol and ammonia nitrogen enriches according to reports, but has stronger inhibitory action to methanogen because of phenol, limits 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.Microbiological fuel cell has the complicated organic substance of degraded with it simultaneously and the ability of electrogenesis obtains great concern.At present of common occurrence as the research of microbiological fuel cell electron donor electrogenesis using complicated organic substance, utilize microbiological fuel cell biological-cathode to carry out denitrification and nitration reaction have also been obtained coverage.Therefore for realizing phenol and ammonia nitrogen waste water synchronous degradation, reclaim electric energy simultaneously, realize effective utilization of resource, we must change the mode of traditional microbiological fuel cell process waste water, invent a kind of method and apparatus utilizing microbiological fuel cell technology to combine with water technology, realize phenol and ammonia nitrogen synchronous degradation, recuperated energy simultaneously, applies for expansion traditional microbiological fuel cell technology and provides new thinking in water treatment.
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 utilizing microbiological fuel cell degradation of phenol and ammonia nitrogen simultaneously.
Another object of the present invention is to provide a kind of method utilizing said apparatus degradation of phenol and ammonia nitrogen simultaneously.
The object of the invention is achieved through the following technical solutions:
A kind of device utilizing microbiological fuel cell simultaneously degradation of phenol and ammonia nitrogen, be made up of anode chamber and cathode chamber, anode chamber and cathode chamber are separated by anion-exchange membrane, anode chamber arranges galvanic anode filling opening and anode electrode, cathode chamber arranges negative electrode filling opening, aerator and cathode electrode, aerator is arranged on bottom cathode chamber, and anode electrode is connected by external circuit with cathode electrode, and external circuit arranges load resistance 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 through pretreated graphite felt, described preprocess method is graphite felt is placed in the hydrogen peroxide solution that mass fraction is 10%, be that 2h is boiled in the bath of 90 DEG C of Water Unders in temperature, then with deionized water at the same temperature water-bath boil 2h, then use oven for drying.
Resistance value preferably 1000 Ω of described load resistance.
Utilize a method for said apparatus simultaneously degradation of phenol and ammonia nitrogen, comprise following operating procedure:
Electrogenesis mixed bacteria liquid and the denitrifying bacterium of domestication are passed through in the inoculation of anode room, add sodium acetate as electron donor, with 0.1molL -1the phosphate buffer solution of pH7.0 and the mixed liquor of nutrient solution are nutriment, provide relatively strict anaerobic environment simultaneously; It is the mixing sludge led that cathode chamber to add containing variable concentrations containing the sewage of phenol and ammonia nitrogen and the nitrobacteria tamed through ammonia nitrogen and phenol and Phenol-degrading Bacteria Strains, and pass into air by aerator, then closed circuit switch is communicated with external circuit, microbiological fuel cell runs and starts, and the ammonia nitrogen of cathode chamber and phenol are degraded simultaneously.
Described domestication refers to tames with sodium acetate.
Described 0.1molL -1the composition of the PBS of pH7.0 and the mixed liquor of nutrient solution comprises 22.2gL -1na 2hPO 4, 5.92gL -1naH 2pO 4, 1.0gL -1naHCO 3, 0.10gL -1feSO 4, 0.10gL -1kCl, 0.015gL -1caCl 2, 0.25gL -1nH 4cl, 10mLL -1mineral solution and 10mLL -1vitamin.
Described mineral solution composition comprises 1.5gL -1c 6h 6nO 63NaH 2o, 0.13gL -1znCl 2, 3.0gL -1mgSO 4, 0.01gL -1cuSO 45H 2o, 0.5gL -1mnSO 4h 2o, 0.01gL -1alK (SO 4) 212H 2o, 1.0gL -1naCl, 0.01gL -1h 3bO 3, 0.1gL -1feSO 47H 2o, 0.025gL -1na 2moO 4, 0.1gL -1caCl 22H 2o, 0.024gL -1niCl 26H 2o, 0.1gL -1coCl 26H 2o and 0.025gL -1na 2wO 42H 2o.
Principle of the present invention is:
By building the microbiological fuel cell with anode chamber and cathode chamber, electrogenesis bacterium in anode chamber utilizes sodium acetate to produce electronics, the nitrobacteria tamed through ammonia nitrogen and phenol is added and Phenol-degrading Bacteria Strains is main mixing sludge in cathode chamber, pass into oxygen (being similar to the Aerobic Pond process of traditional water treatment) simultaneously, the electronics acting in conjunction produced by anode chamber on this basis, thus reach the degraded of phenol and the nitrated of ammonia nitrogen, the NO that nitrification produces 3 -/ NO 2 -anode is entered through anion-exchange membrane under the effect of concentration gradient, under the effect of anode denitrifying bacterium, there is denitrification thus realize nitre nitrogen nitrite nitrogen be degraded to nitrogen further, make the ammonia nitrogen in cathode chamber constantly transform simultaneously, finally reach ammonia nitrogen and phenol synchronous degradation.
The material of electrode is preferably through pretreated graphite felt, and graphite felt has higher specific area, good biocompatibility and reasonable prices, graphite felt is carried out preliminary treatment and is conducive to improving its stability and conductivity.
Had 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 pollutant, is combined by aerobic to microbiological fuel cell and tradition water technology, can be implemented in traditional method for treating water the object being difficult to phenol and the ammonia nitrogen synchronous degradation realized;
(2) in invention, negative electrode adopts the mode of aeration, on the one hand for providing the oxygen needed for microbial degradation pollutant, and remaining O on the other hand 2the electrogenesis of microbiological fuel cell can be realized as electron acceptor.This method is applied to actual waste water Aerobic, can improve the utilance of oxygen, thus energy savings;
Accompanying drawing explanation
Fig. 1 is the apparatus structure schematic diagram that embodiment 1 a kind of utilizes microbiological fuel cell degradation of phenol and ammonia nitrogen simultaneously, in figure, mark is described as follows: 1-anode chamber, 2-cathode chamber, 3-anion-exchange membrane, 4-anode filling opening, 5-anode electrode, 6-negative electrode filling opening, 7-aerator, 8-cathode electrode, 9-external circuit, 10-load resistance, 11-contactor.
The degraded figure of ammonia nitrogen and phenol when Fig. 2 is the apparatus and method process difference phenol concentration of the embodiment of the present invention 1;
Fig. 3 is the degraded figure of apparatus and method ammonia nitrogen and phenol under different dissolved oxygen (DO) condition of the embodiment of the present invention 1;
Fig. 4 is the voltage-time graph 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 thereto.
Embodiment 1
The present embodiment a kind of utilizes the device of microbiological fuel cell degradation of phenol and ammonia nitrogen simultaneously, be made up of anode chamber 1 and cathode chamber 2, anode chamber and cathode chamber are separated by anion-exchange membrane 3, anode chamber arranges galvanic anode filling opening 4 and anode electrode 5, cathode chamber arranges negative electrode filling opening 6, aerator 7 and cathode electrode 8, anode electrode is connected by external circuit 9 with cathode electrode, and external circuit arranges load resistance 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: electrogenesis mixed bacteria liquid and the denitrifying bacterium of domestication are passed through in the inoculation of anode room, add sodium acetate as electron donor, with 0.1molL -1the phosphate buffer solution of pH7.0 and the mixed liquor of nutrient solution are nutriment, provide relatively strict anaerobic environment simultaneously; It is main mixing sludge that cathode chamber adds containing the sewage of variable concentrations phenol and ammonia nitrogen and the nitrobacteria tamed through ammonia nitrogen and phenol and Phenol-degrading Bacteria Strains, and pass into air by aerator, then closed circuit switch is communicated with external circuit, microbiological fuel cell runs and starts, the phenol of cathode chamber 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, under the effect of anode denitrifying bacterium, there is denitrification thus realize nitre nitrogen nitrite nitrogen be degraded to nitrogen further, make the ammonia nitrogen in cathode chamber constantly transform degraded simultaneously.
The cathode electrode of the present embodiment and the material of anode electrode are pretreating graphite felt electrode according to the following steps:
Graphite felt is placed in the hydrogen peroxide solution that mass fraction is 10%, at 90 DEG C, 2h is boiled in water-bath, then with deionized water at the same temperature water-bath boil 2h, then with being cut into long 7cm × wide 4cm size after oven for drying, putting on titanium silk and obtaining pretreating graphite felt electrode.
Assembled battery: install on anode casing by the anode handled well, concrete grammar is as follows:
The titanium silk of pretreating graphite felt anode electrode is passed from anode casing aperture outward by interior, electrode plane is parallel with anode casing board plane, with AB glue, titanium silk and anode casing aperture are glued, place and make it solidify in about 5 minutes, cathode chamber will be loaded in the same way through pretreated graphite felt cathode electrode, again anion-exchange membrane is pressed on cathode chamber housing, then with anode casing, cathode shell, amberplex is fixed, 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: anode room inoculation 10mL, through the electrogenesis mixed bacteria liquid of domestication, adds 20mmolL -1sodium acetate is as electron donor, with pH be 7.0 PBS and nutrient solution fill it up with reactor, cathode chamber adds the PBS that pH is 7.0, and by aerator aeration, with gas flowmeter control cathode aeration rate, external 1000 Ohmic resistances, access the voltage collector of 32 passages, run and start, when voltage drop is low to moderate below 20mV, again change liquid and cultivate, run at least one moon, 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) mud based on nitrobacteria:
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: 0.1molL -1pBS, 1.0gL -1naHCO 3, 0.10gL -1feSO 4, 0.10gL -1kCl, 0.015gL -1caCl 2, 10mL mineral solution and 10mL vitamin, wherein often liter of mineral solution composition is by 1.5gC 6h 6nO 63NaH 2o, 0.13gZnCl 2, 3.0gMgSO4,0.01gCuSO 45H 2o, 0.5gMnSO 4h 2o, 0.01gAlK (SO 4) 212H 2o, 1.0gNaCl, 0.01gH 3bO 3, 0.1gFeSO 47H 2o, 0.025gNa 2moO 4, 0.1gCaCl 22H 2o, 0.024gNiCl 26H 2o, 0.1gCoCl 26H 2o and 0.025gNa 2wO 42H 2o forms.
(2) mud based on Phenol-degrading Bacteria Strains:
Phenol Bacteria Culture mud takes 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 remainder is identical.
The degraded situation of apparatus and method ammonia nitrogen and phenol when different phenol concentration of the present embodiment:
230mgL is added in the device cathode chamber after voltage stabilization -1ammonia nitrogen, adding concentration is respectively 200mgL -1, 400mgL -1and 800mgL -1phenol solution, arranging the different sampling times in running samples in the cathode, Berthelot spectrophotometry and tetramino peace is adopted respectively for neighbour photometry to measure the concentration of ammonia nitrogen and phenol after sampling, until concentration will be 0, the degraded situation of concrete ammonia nitrogen and phenol as shown in Figure 2, as seen from Figure 2 under the condition of variable concentrations phenol solution, the degraded of ammonia nitrogen is not suppressed.
The degraded situation of apparatus and method ammonia nitrogen and phenol under different dissolved oxygen conditions of the present embodiment:
Different flow (0.5mgL is passed into by aerator in the device cathode chamber after voltage stabilization -1, 1 ~ 2mgL -1, 2 ~ 4mgL -1) air, form the environment of anoxic, aerobic and oxygen enrichment respectively, the initial phenol concentration wherein added is 600mgL -1, ammonia nitrogen concentration is 230mgL -1same the sampling time is set in cell operation samples, then the concentration of phenol and ammonia nitrogen is measured, until concentration reduces to 0, the degraded of concrete phenol and ammonia nitrogen as shown in Figure 3, under can finding out the environmental change in cathode chamber 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 environment that dissolved oxygen concentration is high.
The simultaneously voltage of battery under cell operation records different dissolved oxygen conditions by 32 Multichannel data acquisition devices, 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 rate, 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 competing anode simultaneously, make it lower at the voltage in this stage; Along with NO in denitrification after 70h 3 -the reduction of concentration, competition electronic capability weakens, and voltage improves gradually; Dissolved oxygen in negative electrode meet nitrated with under the condition needed for phenol degrading, simultaneously as cathode electronics acceptor.
Above-described embodiment is the present invention's preferably execution mode; but embodiments of the present invention are not restricted to the described embodiments; change, the modification done under other any does not deviate from Spirit Essence of the present invention and principle, substitute, combine, simplify; all should be the substitute mode of equivalence, be included within protection scope of the present invention.

Claims (7)

1. one kind utilizes the method for microbial fuel cell unit simultaneously degradation of phenol and ammonia nitrogen, it is characterized in that: described microbial fuel cell unit is made up of anode chamber and cathode chamber, anode chamber and cathode chamber are separated by anion-exchange membrane, anode chamber arranges galvanic anode filling opening and anode electrode, cathode chamber arranges negative electrode filling opening, aerator and cathode electrode, aerator is arranged on bottom cathode chamber, anode electrode is connected by external circuit with cathode electrode, and external circuit arranges load resistance and contactor; Said method comprises following operating procedure: electrogenesis mixed bacteria liquid and the denitrifying bacterium of domestication are passed through in the inoculation of anode room, add sodium acetate as electron donor, with the mixed liquor of the phosphate buffer solution of 0.1mol/LpH7.0 and nutrient solution for nutriment, provide relatively strict anaerobic environment simultaneously; It is main mixing sludge that cathode chamber adds containing the sewage of phenol and ammonia nitrogen and the nitrobacteria tamed through ammonia nitrogen and phenol and Phenol-degrading Bacteria Strains, and pass into air by aerator, then closed circuit switch is communicated with external circuit, microbiological fuel cell runs and starts, and the ammonia nitrogen of cathode chamber and phenol are degraded simultaneously.
2. a kind of method utilizing microbial fuel cell unit simultaneously 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 method utilizing microbial fuel cell unit simultaneously 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 preprocess method is graphite felt is placed in the hydrogen peroxide solution that mass fraction is 10%, be that 2h is boiled in the bath of 90 DEG C of Water Unders in temperature, then with deionized water at the same temperature water-bath boil 2h, then use oven for drying.
4. a kind of method utilizing microbial fuel cell unit simultaneously degradation of phenol and ammonia nitrogen according to claim 1, is characterized in that: the resistance value of described load resistance is 1000 Ω.
5. a kind of method utilizing microbial fuel cell unit simultaneously degradation of phenol and ammonia nitrogen according to claim 1, is characterized in that: described domestication refers to tames with sodium acetate.
6. a kind of method utilizing microbial fuel cell unit simultaneously degradation of phenol and ammonia nitrogen according to claim 1, is characterized in that: the composition of described nutrient solution comprises 1.0g/LNaHCO 3, 0.10g/LFeSO 4, 0.10g/LKCl, 0.015g/LCaCl 2, 0.25g/LNH 4cl, 10mL/L mineral solution and 10mL/L vitamin.
7. a kind of method utilizing microbial fuel cell unit simultaneously degradation of phenol and ammonia nitrogen according to claim 6, is characterized in that: the composition of described mineral solution comprises 1.5g/LC 6h 6nO 63NaH 2o, 0.13g/LZnCl 2, 3.0g/LMgSO 4, 0.01g/LCuSO 45H 2o, 0.5g/LMnSO 4h 2o, 0.01g/LAlK (SO 4) 212H 2o, 1.0g/LNaCl, 0.01g/LH 3bO 3, 0.1g/LFeSO 47H 2o, 0.025g/LNa 2moO 4, 0.1g/LCaCl 22H 2o, 0.024g/LNiCl 26H 2o, 0.1g/LCoCl 26H 2o and 0.025g/LNa 2wO 42H 2o.
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