CN113546509A - Packed tower type microbial electrolysis cell system and application thereof in degrading organic pollutants - Google Patents
Packed tower type microbial electrolysis cell system and application thereof in degrading organic pollutants Download PDFInfo
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
- B01D53/326—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00 in electrochemical cells
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/38—Removing components of undefined structure
- B01D53/44—Organic components
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/72—Organic compounds not provided for in groups B01D53/48 - B01D53/70, e.g. hydrocarbons
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/84—Biological processes
- B01D53/85—Biological processes with gas-solid contact
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/95—Specific microorganisms
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/702—Hydrocarbons
- B01D2257/7027—Aromatic hydrocarbons
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/704—Solvents not covered by groups B01D2257/702 - B01D2257/7027
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/708—Volatile organic compounds V.O.C.'s
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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
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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Abstract
The invention discloses a packed tower type microbial electrolysis cell system and application thereof in degrading organic pollutants. The packed tower type microbial electrolytic tank greatly improves the removal efficiency of VOCs such as toluene and the like, and is 1.21-1.44 times of that of a common packed tower. The invention does not use proton or cation exchange membranes with high price, short service life and high installation difficulty, reduces the cost and difficulty of the device, can better adsorb volatile organic compounds, reduces gas-liquid mass transfer resistance, and can strengthen the adhesion growth of electroactive functional bacteria, the formation of biological membranes and the conduction of electrons.
Description
(I) technical field
The invention relates to a packed tower type microbial electrolytic cell system and application thereof in degrading organic pollutants.
(II) background of the invention
Volatile Organic Compounds (VOCs) as important precursors for ozone and Secondary Organic Aerosols (SOA) in ambient air, emission control for O3、 PM2.5The composite pollution treatment is of great importance and is one of the key pollutants for winning the blue sky guard war. According to the measurement and calculation of the discharge list of human-source VOCs in China, the VOCs discharged by the industrial coating related industries accounts for more than 20% of the discharge amount of the VOCs of the whole industrial source. The coating waste gas has complex components and contains lipids, benzene series, alcohols and other substances; wherein, the detection rate of benzene VOCs such as toluene, dimethylbenzene, trimethylbenzene and the like is high, and the O of the benzene VOCs is3And the SOA generation potential is higher than that of other VOCs components in the coating waste gas. Therefore, along with the highlighting of the problem of composite atmospheric pollution in China, the development of a high-efficiency and economic deep treatment technology aiming at benzene-series VOCs (volatile organic compounds) such as toluene, xylene and the like in industrial coating waste gas has important significance for atmospheric quality control and social development.
Microbial Electrolysis Cells (MECs) are an emerging technology for recycling environmental resources and have recently been used by many researchers to study the treatment of sewage and exhaust gases. In the MEC, under the action of an applied electric potential, the electron transfer of the process of degrading organic matters by microorganisms on the electrode is accelerated, so that the enhancement of biological reaction is realized. Zhang et al developed a study of toluene waste gas treatment by constructing BES based on carbon brush electrodes, and the inlet gas concentration was 300mg m-3Then, the toluene degradation efficiency and the mineralization rate respectively reach 88 percent (about 1.7 times under the open circuit condition) and 55 percent, and the feasibility of a microbial electrochemical system on the purification of VOCs waste gas (https:// doi. org/10.101) is proved6/j.cej.2018.06.027). However, similar to many reports of the microbial electrochemical system exhaust gas purification, most of the devices in the working microbial electrochemical system are of a bubbling structure, and the shortage of the gas-liquid mass transfer rate severely limits the benzene-based VOCs removal load of the whole system. And the packed tower is one of the most common absorption tower configurations, and has a higher gas-liquid contact area and a higher gas-liquid mass transfer rate compared with a bubble tower. The biological film is attached to the surface of the filler, so that waste gas absorption and biodegradation can be synchronously performed in a single biological film packed tower (BPT), and the aim of simplifying the process flow is fulfilled. At present, the reactor configurations of a biological filter bed, a biological trickling filter and the like are widely applied in the engineering fields of biological deodorization and the like. If the biomembrane packed tower can be coupled with a microbial electrochemical system, the process of gas-liquid mass transfer and biodegradation of VOCs waste gas purification can be synchronously strengthened.
Therefore, it is necessary to research and develop a packed tower type microbial electrolytic cell device which has a simple structure, low construction cost and easy scale-up, can improve the mass transfer area, the microbial attachment amount and the electron transfer rate, and can strengthen the gas-liquid mass transfer and biodegradation processes of the benzene-series VOCs.
Disclosure of the invention
The invention aims to provide a packed tower type microbial electrolysis cell system for removing volatile organic pollutants and application thereof in degrading organic pollutants, wherein a biological membrane packed tower is combined with a biological electrolysis cell, the process of VOCs gas-liquid mass transfer and biodegradation is enhanced by improving the mass transfer area, the microbial attachment amount and the electron transfer rate, a new thought is provided for the rapid and effective treatment of VOCs, and the method is used for providing a new idea for the rapid and effective treatment of volatile organic matters in industrial waste gas, such as: the high-efficiency purification of butyl acetate, benzene, toluene, xylene and other benzene series has important significance.
The technical scheme adopted by the invention is as follows:
the invention provides a packed tower type microbial electrolysis cell system for removing volatile organic pollutants, which comprises a packed tower, a gas tank 17 and an electrochemical workstation 4; the packed tower consists of a tower body 1, a tower base 2 and a tower top 3, wherein the tower body is mutually communicated with the tower bottom and the tower top to form a reaction cavity for gas and liquid to flow; the bottom of the tower body 1 is provided with a gas distributor 7 connected with the bottom of the tower, and the inside of the tower body is provided with a porous organic glass sleeve 8 with the same height as the tower body; the periphery of the porous organic glass sleeve 8 surrounds a cathode carbon cloth 9, a conductive filler 10 is arranged inside the porous organic glass sleeve, and an anode graphite rod 11 is arranged in the conductive filler 10; the tower top 3 is provided with a liquid inlet 6, a gas outlet 5 and a sampling port 12, and the liquid inlet 6 is communicated with a spray ring 13; the tower bottom 2 is a liquid collecting tank for collecting and storing liquid flowing through the tower body, and is provided with a liquid outlet 14, a gas inlet 15 and a sampling port 18; liquid at the bottom of the tower is conveyed to a liquid inlet 6 at the top of the tower through a liquid outlet 14, a peristaltic pump 16 and a pipeline, and is sprayed to the tower body through a spraying ring to form a liquid path ii; gas in a gas tank 17 is introduced into the tower body through a gas inlet 15 at the bottom of the tower through a gas distributor 7 to form a gas path i; the cathode carbon cloth is connected with the electrochemical workstation through a conducting wire (namely a cathode wiring iv); the anode graphite rod is connected with the electrochemical workstation through a lead (namely an anode wiring iii).
The tower body is in a cylindrical shape, and the height-diameter ratio is 2-6:1 (preferably 2: 1); the diameter of the porous organic glass sleeve is smaller than that of the tower body, the open area accounts for 30-50% (preferably 40%) of the surface area of the sleeve, and the diameter of the hole is 1/10-1/50 (preferably 1/20) of the diameter of the sleeve; the gas distributor is a cylinder with holes on the top surface and the bottom surface; the gas distributor hole diameter is 1/10-1/50 (preferably 1/33) of the sleeve diameter.
The conductive filler is coke filler, iron carbon filler, graphite carbon black and sponge iron filler (preferably coke filler, the size is 1.5-2.5cm, the porosity is 45-55%, and the specific surface area is 40-65 m)2/m3The bulk density is 450-600kg/m3) The filling height is 3/5-4/5 (preferably 2/3) of the height of the porous plexiglass sleeve. The number of the anode graphite rods is 4, the anode graphite rods are respectively inserted into the conductive filler and do not contact with each other, and the anode graphite rods are preferably 3/5-4/5 (preferably 2/3) in height and 1/30-1/15 (preferably 1/20) in diameter.
The invention also provides an application of the packed tower type microbial electrolysis cell system in degrading organic pollutants, and the application method comprises the following steps: (1) a packed tower type microbial electrolytic cell system is adopted, firstly, sludge and inorganic salt solution are used as spraying liquid, the spraying liquid at the bottom of the tower is conveyed to a liquid inlet at the top of the tower through a peristaltic pump, and the spraying liquid is sprayed to a tower body through a spraying ring; simultaneously, organic waste gas is introduced from a gas inlet, the anode potential is controlled to be 0.3-0.7V (preferably 0.5V) (relative to Ag/AgCl) through an electrochemical workstation, and the microbial biofilm formation is successful when the degradation rate of the organic waste gas reaches 80-90 percent through an electrolytic reaction; (2) then inorganic salt solution is used as spraying liquid, organic waste gas is introduced, the potential of the anode is controlled to be 0.3-0.7V (preferably 0.5V) through an electrochemical work station, the organic waste gas is dispersed from a gas distributor and enters a tower body, the gas entering the tower body is contacted with microorganisms (liquid) adhered to the conductive filler and the anode graphite, and partial VOCs adsorbed on the conductive filler and the anode graphite are subjected to in-situ degradation, so that the degradation of organic pollutants is realized.
The volume ratio of the sludge to the inorganic salt solution in the step (1) is 1:4-1:3 (preferably 1: 4). The sludge is anaerobic sludge (Hangzhou city seven grids sewage treatment plant, pH 6.8, BOD)55400. Carbohydrates (as COD) 1500).
The liquid-gas ratio of the spraying liquid to the organic waste gas in the step (1) and the step (2) is 8-50L/m3Preferably 33L/m3。
And (3) mixing each 1L of the inorganic salt solution obtained in the step (1) and the step (2) with 982.5mL of phosphate buffer solution, 12.5mL of trace element solution and 5mL of vitamin solution. The phosphate buffer solution comprises the following components: NH (NH)4Cl 0.31g/L、NaH2PO4·H2O 2.452g/L、Na2HPO44.576g/L, KCl 0.13.13 g/L, deionized water as solvent; the composition of the trace element solution is as follows: MgSO (MgSO)4 3g/L、MnSO4·H2O 0.5g/L、NaCl 1g/L、 FeSO4·7H2O 0.1g/L、CaCl2·2H2O 0.1g/L、CoCl2·6H2O 0.1g/L、ZnCl2 0.13g/L、CuSO4 5H2O 0.01g/L、AlK(SO4)2·12H2O 0.01g/L、H3BO3 0.01g/L、Na2MoO4 0.025g/L、 Na2WO4·2H2O0.025 g/L and deionized water as solvent; the vitamin solution comprises the following components: 0.002g/L of biotin, 0.002g/L of folic acid, 0.01g/L of pyridoxine, 0.005g/L of riboflavin, 0.005g/L of thiamine, 0.005g/L of nicotinic acid, 0.005g/L, B-120.0001 g/L of pantothenic acid, 0.005g/L of p-aminobenzoic acid and 0.005g/L of lipoic acid, and the solvent is deionized water.
The organic waste gas in the step (1) and the step (2) is common industrial waste gas containing volatile organic compounds, such as ethyl acetate, butyl acetate, toluene, chlorobenzene or xylene, and the like, the organic waste gas is added in the form of organic waste gas air mixed gas, and the concentration of the organic waste gas is 100-3。
The adding speed of the spray liquid in the step (1) and the step (2) is 50-150mL/min, preferably 100 mL/min; the feeding speed of the organic waste gas is 2-6L/min, preferably 3L/min.
Compared with the prior art, the invention has the following beneficial effects:
in the invention, the anode graphite rods and the cathode carbon cloth are separated by the porous organic glass sleeve in the packed tower type microbial electrolysis cell device, the cathode carbon cloth is closely attached to the periphery of the sleeve and is arranged in a surrounding way, and the four anode graphite rods are inserted in the conductive filler, so that the microbial electrolysis cell and the packed tower are integrated into a whole, and the construction cost of the reactor is reduced. The packed tower type microbial electrolytic tank greatly improves the removal effect of VOCs such as toluene and the like, and the removal effect is 1.21-1.44 times that of a common packed tower.
The invention does not use proton or cation exchange membranes with high price, short service life and large installation difficulty, thereby reducing the cost and difficulty of the device.
The three-dimensional structure and the excellent conductivity of the conductive filler are fully utilized, the volatile organic compounds can be better adsorbed, the gas-liquid mass transfer resistance is reduced, and the adhesion growth of electroactive functional bacteria, the formation of a biological film and the conduction of electrons can be strengthened.
The invention can be used for treating wastewater besides degrading volatile organic gases.
The invention can realize the high-efficiency purification of VOCs in industrial waste gas, does not generate any secondary pollution, is easy to popularize and has low purification cost.
(IV) description of the drawings
FIG. 1 is a schematic diagram of a packed tower microbial electrolyzer system according to the invention; the device comprises a tower body 1, a tower base 2, a tower top 3, an electrochemical workstation 4, a gas outlet 5, a liquid inlet 6, a gas distributor 7, a porous organic glass sleeve 8, cathode carbon cloth 9, a conductive material 10, an anode graphite rod 11, a sampling port 12, a spray ring 13, a liquid outlet 14, a gas inlet 15, a peristaltic pump 16, a gas tank 17 and a sampling port 18.
FIG. 2 is a graph showing the toluene removal rate during the start-up period of the packed tower type microbial electrolysis cell system of example 2.
FIG. 3 is a scanning electron microscope photograph of a biofilm on the anode packing of a packed tower type microbial electrolysis cell system.
FIG. 4 is a graph showing the removal of toluene at different concentrations in a packed tower microbial cell system.
FIG. 5 shows the toluene removal rate of the packed tower type microbial cell system of example 2 at different anode potentials.
FIG. 6 is a graph showing the chlorobenzene and o-xylene removal rates of the packed tower microbial cell system of example 2.
FIG. 7 shows the toluene removal efficiency of the packed tower type microbial cell system and the general packed tower in example 3.
(V) detailed description of the preferred embodiments
The invention will be further described with reference to specific examples, but the scope of the invention is not limited thereto:
materials, reagents and the like used in the following examples are commercially available unless otherwise specified.
Example 1: packing tower type microbial electrolysis cell system
Referring to fig. 1, the packed tower type microbial electrolysis cell system for removing volatile organic pollutants comprises a packed tower, a gas tank 17 and an electrochemical workstation 4, wherein the packed tower consists of a tower body 1, a tower base 2 and a tower top 3, and the tower body is communicated with the tower bottom and the tower top to form a reaction cavity for gas and liquid to flow through; the bottom of the tower body 1 is provided with a gas distributor 7 connected with the bottom of the tower, and the inside of the tower body is provided with a porous organic glass sleeve 8 with the same height as the tower body; the periphery of the porous organic glass sleeve 8 surrounds a cathode carbon cloth 9, a conductive filler 10 is arranged inside the porous organic glass sleeve, and four anode graphite rods 11 are arranged in the conductive filler 10; the tower top 3 is provided with a liquid inlet 6, a gas outlet 5 and a sampling port 12, and the liquid inlet 6 is communicated with a spray ring 13; the tower bottom 2 is a liquid collecting tank for collecting and storing liquid flowing through the tower body, and is provided with a liquid outlet 14, a gas inlet 15 and a sampling port 18; liquid at the bottom of the tower is conveyed to a liquid inlet 6 at the top of the tower through a peristaltic pump 16 and a pipeline ii through a liquid outlet 14 and is sprayed to the tower body through a spraying ring 13; the gas of the gas tank 17 is introduced into the tower body through a gas inlet 15 at the bottom of the tower and a gas distributor 7; the cathode carbon cloth 9 is connected with the electrochemical workstation 4 through a cathode connection iv, and the anode graphite rod is connected with the electrochemical workstation 4 through an anode connection iii.
The packed tower is a normal pressure device, the tower body is in a cylindrical shape, and the height-diameter ratio is 2:1 (the height is 20cm, and the diameter is 10 cm); the height of the porous organic glass sleeve is 20cm, the diameter is 9cm (the diameter of the hole is 0.45cm, and the area of the hole accounts for 40 percent of the surface area of the sleeve); the gas distributor is cylindrical, the diameter is 10cm, the height is 0.4cm (the plate surface is full of small holes, and the diameter of the holes is 0.3 cm). The conductive filler is coke filler (purchased from Xin Source Water treatment plant, the size is 1.5-2.5cm, the porosity is 45-55 percent, and the specific surface area is 40-65m2/m3The bulk density is 450-600kg/m3) The fill height is 2/3 for the porous plexiglass sleeve height. The anode graphite rods are provided with 4 (the diameter is 0.5cm, the height is 13.3cm) and are respectively inserted into the conductive filler without contacting with each other.
Liquid (mixture of sludge and inorganic salt solution or inorganic salt solution) at the bottom of the tower is conveyed to a liquid inlet 6 at the top of the tower by a peristaltic pump 16 and is sprayed on the conductive filler by a spray ring 13; meanwhile, organic waste gas is introduced into the gas inlet 15, the gas is dispersed from the gas distributor 7 and enters the tower body, the gas entering the tower body is in contact with microorganisms (liquid) adhered to the conductive filler and the anode graphite rod, part of the gas is adsorbed to the conductive filler, in-situ degradation occurs to VOCs on the anode graphite, the microorganisms adhered to the graphite anode and the surface of the conductive filler rapidly degrade organic matters in the liquid to generate electrons and carbon dioxide, the carbon dioxide is discharged along with the gas, the electrons are transmitted to the carbon cloth cathode through the connected electrochemical workstation, and the degradation and electricity generation capabilities of the VOCs are improved.
Example 2: application of packed tower type microbial electrolytic cell system
1. Inoculation and start-up of packed tower microbial electrolysis cell systems
Using the packed tower type microbial cell system of example 1, 0.3L of anaerobic sludge (pH 6.8, BOD, from seven-grid sewage treatment plant in Hangzhou City) obtained by treating wastewater was treated under optimum environmental factor conditions (culture temperature 30 ℃ C., culture solution pH 7)55400. Carbohydrate (calculated by COD) 1500) and 1.2L of inorganic salt solution (phosphate buffer solution + trace elements + vitamin solution) as spraying liquid are sprayed to the tower body by a peristaltic pump at the flow rate of 100 mL/min. In addition, the liquid-gas ratio of the spraying liquid to the organic waste gas is 33L/m3Directly introducing mixed gas of toluene and air at a flow rate of 3L/min as a carbon source (the concentration of toluene after mixing is 100 mg/m)3The air provided by the steel cylinder is divided into two air flows of large flow and small flow by two flowmeters, the air of small flow is introduced into a liquid benzene series storage tank, so that part of concentration toluene pollutants are brought out along with the flow of the air, then the toluene pollutants are mixed with the air flow of large flow in a mixing bottle, the concentration of the toluene pollutants in the waste gas is controlled by adjusting the two flows, and the anode potential is controlled to be 0.5V (relative to Ag/AgCl) by an electrochemical workstation. Sampling is respectively carried out at the sampling ports 12 and 18 every 30min, and the degradation and mineralization of the toluene are detected by using gas chromatography, wherein the toluene removal efficiency is (inlet concentration-outlet concentration)/inlet concentration multiplied by 100%. When the toluene removal rate is stable, the active functional flora on the anode of the packed tower type microbial electrolysis cell system is considered to be successfully biofilm-forming.
Gas chromatography detection conditions: 6890N GC (Agilent, USA) using an HP Innowax capillary column (30 m.times.320 μm.times.0.5 μm). At 40mLmin-1Supply carrier gas N at a flow rate2Air flow rate of 450mL min-1. Temperature of column box and detectorSet at 200 and 180 deg.c, respectively.
Each 1L of the inorganic salt solution is prepared by mixing 982.5mL of phosphate buffer solution, 12.5mL of trace element solution and 5mL of vitamin solution.
The phosphate buffer solution comprises the following components: NH (NH)4Cl 0.31g/L、NaH2PO4·H2O 2.452g/L、 Na2HPO44.576g/L, KCl 0.13.13 g/L, deionized water as solvent;
the composition of the trace element solution is as follows: MgSO (MgSO)4 3g/L、MnSO4·H2O 0.5g/L、NaCl 1g/L、 FeSO4·7H2O 0.1g/L、CaCl2·2H2O 0.1g/L、CoCl2·6H2O 0.1g/L、ZnCl2 0.13g/L、CuSO45H2O 0.01g/L、AlK(SO4)2·12H2O 0.01g/L、H3BO3 0.01g/L、Na2MoO4 0.025g/L、 Na2WO4·2H2O0.025 g/L and deionized water as solvent;
the vitamin solution comprises the following components: 0.002g/L of biotin, 0.002g/L of folic acid, 0.01g/L of pyridoxine, 0.005g/L of riboflavin, 0.005g/L of thiamine, 0.005g/L of nicotinic acid, 0.005g/L, B-120.0001 g/L of pantothenic acid, 0.005g/L of p-aminobenzoic acid and 0.005g/L of lipoic acid, and the solvent is deionized water.
Fig. 2 is a graph showing the toluene removal rate during the start-up of the packed tower type microbial electrolysis cell system. With a large amount of microorganisms adhered to the surface of the conductive filler, the removal rate gradually stabilizes to about 90% at the beginning of the third day, which indicates that the packed tower type microorganism electrolytic cell system is successfully and rapidly started. The system showed weak toluene removal capacity in the first few days because the microorganisms were not adapted to the packed tower type microbial electrolysis cell system, and after three days of adaptation, the number of toluene-degrading bacteria rapidly increased, showing high toluene-degrading capacity.
Fig. 3 shows the growth of organisms on the surface of the conductive filler after the packed tower type microbial electrolytic cell system is successfully started, and a large number of rod-shaped microorganisms are adhered to the surface of the conductive particles after the system is started, so that the microorganisms grow well, and the microorganisms are better adapted to the environment of the reactor.
2. Mineralization and removal performance of typical VOCs toluene by packed tower type microbial electrolytic cell
FIG. 4 reflects the degradation and mineralization of toluene at different concentrations in the packed tower microbial electrolyzer system. With toluene concentration from 100mg/m3Increased to 1500mg/m3The removal rate of the toluene is reduced from 95% to 83%, and the mineralization rate is maintained at 60-65%.
3. Removal performance of typical VOCs toluene by using packed tower type microbial electrolysis cell system with different anode potentials
FIG. 5 reflects the degradation of toluene in the packed tower microbial electrolysis cell at different anode potentials. 1000mg/m3Toluene was best at an anodic potential of 0.5V with 87.9% removal. At 0.3V and 0.7V only 74.5% and 79.4%.
4. Removal performance of packed tower type microbial electrolytic cell system on typical VOCs chlorobenzene and o-xylene
The toluene gas in step 1 was replaced by chlorobenzene, initially at 500mg/m3The mixed gas of chlorobenzene and air is used as a carbon source, the flow rate is 3L/min, the inorganic salt solution is used as a spraying liquid, the flow rate is 100mL/min, the spraying liquid and the organic waste gas have the liquid-gas ratio of 33L/m3And operating for one month until the packed tower type microbial electrolysis cell system is successfully and quickly started. Then introducing mixed gas of chlorobenzene and air as carbon source (chlorobenzene concentration after mixing is 100, 200, 300, 500, 800, 1000, 1200 and 1500 mg/m)3) The flow rate is 3L/min, the system takes inorganic salt solution as spraying liquid and sprays the inorganic salt solution to the tower body at the flow rate of 100mL/min, and the liquid-gas ratio of the spraying liquid to the organic waste gas is 33L/m3The anode potential (0.5V vs Ag/AgCl) was controlled by an electrochemical workstation and the degradation rate of chlorobenzene was determined by gas chromatography.
The same conditions were used to replace toluene with o-xylene and the other operations were the same.
FIG. 6 reflects the degradation of chlorobenzene and o-xylene removal at anode potential (0.5V vs Ag/AgCl) for this packed tower microbial electrolyzer system. The system can also better degrade chlorobenzene and o-xylene, and the removal rate is higher than 75%.
Example 3: comparison of Performance of packed column microbial Electrolysis cell System and packed column reactor
Example 2 step 1 after successful start-up of a packed tower type microbial electrolysis cell system, inorganic salt solution was used as a spray solution, the inorganic salt solution was sprayed into a tower body at a flow rate of 100mL/min, and a mixed gas of toluene and air was introduced as a carbon source (the toluene concentration after mixing was 100, 200, 300, 500, 800, 1000, 1200, and 1500 mg/m)3) The flow rate is 3L/min, and the liquid-gas ratio of the spraying liquid to the organic waste gas is 33L/m3. The anodic potential (0.5V vs Ag/AgCl) was controlled by an electrochemical workstation, the reaction was carried out for 20 days, samples were taken as in example 2, and degradation and mineralization of toluene were detected by gas chromatography.
When the anode potential is not applied to the packed tower type microbial electrolysis cell system, the packed tower type microbial electrolysis cell system is regarded as a common packed tower reactor, and other operations are the same.
FIG. 6 reflects the degradation of toluene at different concentrations in the two reactors. At 100-3The degradation effect of the packed tower type microbial electrolytic tank under the toluene concentration is far higher than that of a common packed tower, and the removal rate of the material tower type microbial electrolytic tank is 1.21-1.44 times that of the packed tower.
Although the present invention has been described with reference to the above embodiments, it should be understood that the scope of the present invention is not limited thereto, and any changes and modifications made by those skilled in the art without departing from the spirit and scope of the present invention should be construed as being limited thereto.
Claims (10)
1. A packed tower microbial electrolysis cell system, characterized in that the system comprises a packed tower, a gas tank and an electrochemical workstation; the packed tower consists of a tower body, a tower base and a tower top, wherein the tower body is communicated with the tower bottom and the tower top to form a reaction cavity for gas and liquid to flow; the bottom of the tower body is provided with a gas distributor connected with the bottom of the tower, and the inside of the tower body is provided with a porous organic glass sleeve which has the same height as the tower body; the periphery of the porous organic glass sleeve is surrounded by cathode carbon cloth, conductive filler is arranged inside the porous organic glass sleeve, and an anode graphite rod is arranged in the filler; the tower top is provided with a liquid inlet, a gas outlet and a sampling port, and the liquid inlet is communicated with the spray ring; the tower bottom is provided with a liquid collecting tank for collecting and storing liquid flowing through the tower body, and a liquid outlet, a gas inlet and a sampling port; liquid at the bottom of the tower is conveyed to a liquid inlet at the top of the tower through a peristaltic pump and a pipeline through a liquid outlet, and is sprayed to the tower body through a spraying ring; the gas of the gas tank is introduced into the tower body through a gas inlet at the bottom of the tower through a gas distributor; the cathode carbon cloth is connected with the electrochemical workstation through a lead; the anode graphite rod is connected with the electrochemical workstation through a lead.
2. The packed tower type microbial electrolysis cell system according to claim 1, wherein the tower body is in a cylindrical shape, and the height-diameter ratio is 2-6: 1; the diameter of the porous organic glass sleeve is smaller than the diameter of the tower body, the area of an opening hole accounts for 30-50% of the surface area of the sleeve, and the diameter of the opening hole is 1/10-1/50 of the diameter of the sleeve; the gas distributor hole diameter is 1/10-1/50 of the sleeve diameter.
3. The packed tower microbial electrolysis cell system of claim 1, wherein the conductive filler is a coke filler, an iron carbon filler, graphite carbon black, or a sponge iron filler.
4. The packed tower microbial electrolyzer system of claim 1 wherein the conductive packing fill height is 3/5-4/5 of the porous plexiglas sleeve height.
5. Use of the packed tower microbial electrolyzer system of claim 1 for the degradation of organic pollutants.
6. The application according to claim 5, characterized in that the method of application is: (1) a packed tower type microbial electrolysis cell system is adopted, firstly, sludge and inorganic salt solution are used as spraying liquid, the spraying liquid is conveyed to a liquid inlet at the top of a tower through a peristaltic pump and is sprayed to a tower body through a spraying ring; simultaneously, organic waste gas is introduced from a gas inlet, the anode potential is controlled to be 0.3-0.7V by an electrochemical workstation, and the microbial biofilm formation is successful when the degradation rate of the organic waste gas reaches 80-90 percent through an electrolytic reaction; (2) then inorganic salt solution is used as spraying liquid, organic waste gas is introduced, and the potential of the anode is controlled to be 0.3-0.7V by an electrochemical workstation, so that the degradation of organic pollutants is realized.
7. The use according to claim 6, characterized in that the volume ratio of the sludge to the inorganic salt solution in step (1) is 1:4 to 1: 3; the sludge is anaerobic sludge with pH of 6.8 and BOD55400. The carbohydrates were counted as COD 1500.
8. The method as claimed in claim 6, wherein the liquid-gas ratio of the spraying liquid to the organic waste gas in step (1) and step (2) is 8-75L/m3(ii) a The adding speed of the spray liquid is 50-150mL/min, and the introducing speed of the organic waste gas is 2-6L/min.
9. The use according to claim 6, wherein each 1L of the inorganic salt solution obtained in step (1) and step (2) is prepared by mixing 982.5mL of phosphate buffer solution, 12.5mL of trace element solution and 5mL of vitamin solution; the phosphate buffer solution comprises the following components: NH (NH)4Cl 0.31g/L、NaH2PO4·H2O 2.452g/L、Na2HPO44.576g/L, KCl 0.13.13 g/L, deionized water as solvent; the composition of the trace element solution is as follows: MgSO (MgSO)4 3g/L、MnSO4·H2O 0.5g/L、NaCl 1g/L、FeSO4·7H2O 0.1g/L、CaCl2·2H2O 0.1g/L、CoCl2·6H2O 0.1g/L、ZnCl2 0.13g/L、CuSO45H2O 0.01g/L、AlK(SO4)2·12H2O 0.01g/L、H3BO3 0.01g/L、Na2MoO4 0.025g/L、Na2WO4·2H2O0.025 g/L and deionized water as solvent; the vitamin solution comprises the following components: 0.002g/L of biotin, 0.002g/L of folic acid, 0.01g/L of pyridoxine, 0.005g/L of riboflavin, 0.005g/L of thiamine, 0.005g/L of nicotinic acid, 0.005g/L, B-120.0001 g/L of pantothenic acid, 0.005g/L of p-aminobenzoic acid and 0.005g/L of lipoic acid, and the solvent is deionized water.
10. The method as claimed in claim 6, wherein the organic waste gas in step (1) and step (2) comprises ethyl acetate, butyl acetate, toluene, chlorobenzene or xylene, and the organic waste gas is added in the form of a mixed gas of organic waste gas and air, and the concentration of the organic waste gas is 100-1500mg/m3。
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| CN115475503A (en) * | 2022-10-20 | 2022-12-16 | 延边大学 | Three-dimensional electrode biomembrane reaction device and method for removing chlorobenzene waste gas by using same |
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