CN107010714B - Wastewater treatment system and method with coupling of bioelectrocatalysis and photocatalytic contact oxidation - Google Patents
Wastewater treatment system and method with coupling of bioelectrocatalysis and photocatalytic contact oxidation Download PDFInfo
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- CN107010714B CN107010714B CN201710363732.0A CN201710363732A CN107010714B CN 107010714 B CN107010714 B CN 107010714B CN 201710363732 A CN201710363732 A CN 201710363732A CN 107010714 B CN107010714 B CN 107010714B
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Images
Classifications
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/005—Combined electrochemical biological processes
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
- C02F1/32—Treatment of water, waste water, or sewage by irradiation with ultraviolet light
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/30—Aerobic and anaerobic processes
- C02F3/301—Aerobic and anaerobic treatment in the same reactor
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/308—Dyes; Colorants; Fluorescent agents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
Abstract
The invention relates to the technical field of wastewater treatment, and particularly discloses a wastewater treatment system with coupling of bioelectrocatalysis and photocatalytic contact oxidation, which comprises: the device comprises a first tube body, a second tube body and a third tube body which are sequentially connected, wherein a liquid inlet is formed in the tube wall of the first tube body, a liquid outlet is formed in the third tube body, a biological cathode is arranged in the first tube body and is connected with an external circuit, a biological anode is arranged in the second tube body and is connected with the external circuit, and microorganisms are attached to the surfaces of the biological anode and the biological cathode; the third pipe body is internally provided with a mixed filler and an ultraviolet lamp, the center of the mixed filler is a cavity, and the ultraviolet lamp is arranged in the cavity. The wastewater treatment system utilizes dissolved oxygen in a gradient way through reasonable arrangement of the structure and the space application of the biological film inside the mixed filler, so that the problem that the dissolved oxygen is difficult to control accurately in the past through a micro-oxygen technology is avoided, and the removal of residual COD (chemical oxygen demand) in the contact oxidation part biological film on the azo dye, the intermediate product and the wastewater is improved.
Description
Technical Field
The invention relates to the technical field of wastewater treatment, in particular to a wastewater treatment system and method with coupling of bioelectrocatalysis and photocatalytic contact oxidation.
Background
The printing and dyeing industry in China is developed, a large amount of printing and dyeing wastewater is generated every year, and azo dyes are taken as one of typical pollutants in the printing and dyeing wastewater, and due to extremely high chromaticity, the environment is influenced and photosynthesis of aquatic organisms is influenced, so that the ecological environment of a water body is destroyed.
The prior biological treatment as a main technology of a wastewater treatment plant can be used for mineralizing azo dyes, and the technical process mainly comprises a anaerobic bioreactor in a decoloring stage and an aerobic bioreactor for secondary treatment which are connected in series. The anaerobic and aerobic series process can achieve better decoloring effect, but has some defects, such as large occupied area, low decoloring rate, high cost of early-stage investment and later-stage management maintenance, unstable treatment effect, difficulty in reaching standards, and the like.
An integrated reactor which combines an anaerobic process and an aerobic process has been developed nowadays, as in the patent with publication number CN 205838677U, and an integrated wastewater treatment device is proposed, which can effectively treat azo dye wastewater with low Chemical Oxygen Demand (COD) concentration by precisely controlling aeration amount and creating micro-aerobic condition. However, the system has the problems that the treatment speed is slower, the precise aeration is difficult to control, toxic products in the middle of azo decomposition are easy to remain, and the oxygen supply of the contact oxidation aerobic biomembrane is insufficient under the micro-oxygen environment, so that the COD removal of the high-concentration COD azo dye wastewater is limited.
Disclosure of Invention
First, the technical problem to be solved
In order to solve the problems in the prior art, the invention provides a bioelectrocatalysis and photocatalysis contact oxidation coupling wastewater treatment system which is high in decoloring rate, more complete in mineralization of toxic decoloring intermediate products, and capable of effectively degrading high-concentration COD in dye wastewater without secondary treatment. The invention also provides a method for treating wastewater by coupling bioelectrocatalysis and photocatalysis contact oxidation.
(II) technical scheme
In order to achieve the above purpose, the main technical scheme adopted by the invention comprises the following steps:
a wastewater treatment system coupled with biocatalysis and photocatalytic contact oxidation, comprising: the first pipe body, the second pipe body and the third pipe body are connected in sequence, wherein the pipe wall of the first pipe body is provided with a liquid inlet, the third pipe body is provided with a liquid outlet,
a biological cathode is arranged in the first tube body and is connected with an external circuit,
a biological anode is arranged in the second pipe body and is connected with an external circuit, and microorganisms are attached to the surfaces of the biological anode and the biological cathode;
the third tube body is internally provided with a mixed filler and an ultraviolet lamp, the mixed filler consists of an outer layer of barrel-shaped filler and an inner layer of plate-shaped filler, the center of the mixed filler is a cavity, an aerobic biomembrane and an anaerobic biomembrane are attached to the barrel-shaped filler, the outer surface of the plate-shaped filler is plated with a photocatalytic material, and the ultraviolet lamp is arranged in the cavity.
The wastewater treatment system as described above, preferably, the plate-type packing is a polyurethane material; the inner side of the cylinder-shaped filler is attached with an aerobic biomembrane, and the outer side of the cylinder-shaped filler is attached with an anaerobic biomembrane;
and an aeration head is further arranged in the third pipe body, and the aeration head is arranged close to the inside of the cylindrical filler.
In the wastewater treatment system, preferably, the biocathode and the bioanode are annular carbon brush electrodes, and the biocathode is provided with two groups, three groups or more than three groups;
the microorganism is an anaerobic microorganism, the anaerobic microorganism is a mixed bacterium or a single extracellular electrogenerator, or the microorganism is an osneshop bacterium;
the photocatalytic material is TiO 2 A photocatalyst.
In the wastewater treatment system as described above, preferably, the first tube body is provided with a first reference electrode.
In the above wastewater treatment system, preferably, the first pipe body, the second pipe body and the third pipe body are sequentially connected from bottom to top, a lower end cover is arranged at the lower end of the first pipe body, and an upper end cover is arranged at the upper end of the third pipe body; a first water distribution plate is arranged between the first pipe body and the second pipe body, and a plurality of small holes are formed in the first water distribution plate; a second water distribution plate is arranged between the second pipe body and the third pipe body, and the second water distribution plate is provided with a water inlet hole.
In the above wastewater treatment system, preferably, a fourth pipe body is further disposed between the third pipe body and the upper end cover, the fourth pipe body is provided with the wastewater outflow hole, and the through hole on the third pipe body is used as a sampling hole; preferably, the fourth tube body is provided with a second reference electrode.
In the wastewater treatment system as described above, preferably, the first pipe body is provided with a first sampling hole, and/or the second pipe body is provided with a second sampling hole.
A method for treating wastewater by coupling bioelectrocatalysis and photocatalytic contact oxidation comprises the following steps:
1) The wastewater is contacted with a biological cathode, and under the combined action of microorganisms and electrochemical catalytic reduction on the biological cathode, the azo double bond of a chromophoric group in the azo dye is broken and decomposed into toxic micromolecular aromatic hydrocarbon substances;
2) The wastewater containing the micromolecular aromatic hydrocarbon substances is contacted with a biological anode, microorganisms are attached to the biological anode, more electrons are transmitted to an electrode while the micromolecular organic substances are degraded, and then the extra electrons are provided for the biological cathode through an external circuit, so that COD (chemical oxygen demand) removal is realized, the biological cathode reaction is promoted, the fracture of azo bonds is accelerated, and further decolorization is realized;
3) The wastewater treated in the step 2) is contacted with mixed filler, the mixed filler consists of inner filler hung with photocatalytic material and outer filler hung with mixed biological film, the mixed biological film comprises an aerobic biological film and an anaerobic biological film, the photocatalytic material promotes the decoloration of residual azo dye under the irradiation of ultraviolet lamp, the aerobic biological film opens a chain to benzene rings in micromolecular aromatic hydrocarbon substances, the anaerobic biological film further degrades the azo dye with residual azo bond not broken, and the residual azo dye is further degraded and the degraded product is completely mineralized under the combined action of the mixed biological film and the photocatalytic material.
In the above method, preferably, in the step 3), an aeration head is provided near the aerobic microbial membrane to provide oxygen source for the aerobic microorganisms, so that the near aerobic microbial membrane effectively removes high concentration COD in the wastewater.
Preferably, the anaerobic microorganism is a mixed bacterium or a single extracellular electrogenic bacterium, as described above. Still further, the single extracellular electrogenerator is Shewanella oneidensis MR-1.
(III) beneficial effects
The beneficial effects of the invention are as follows: the wastewater treatment method combines the enhanced biological membrane bioelectrocatalysis technology, the contact oxidation technology and the photocatalysis technology together, plays the advantages of the technologies, breaks and reduces azo bonds of azo dye chromophores under the combined action of the photocathode electrocatalysis, degrades the azo bonds into aromatic hydrocarbon toxic intermediate products which are difficult to degrade under anaerobic conditions, effectively improves the extracellular electricity production performance of the anode biological membrane through the bioanode, accelerates the decoloring rate of the biocathode while removing COD, and enhances the high-efficiency decoloring process of the azo dye by using the photocatalysis technology. The wastewater treatment system utilizes dissolved oxygen in a gradient way through reasonable arrangement of the structure and the space application of the biological film inside the mixed filler, so that the problem that the dissolved oxygen is difficult to control accurately in the past through a micro-oxygen technology is avoided, and the removal of residual COD (chemical oxygen demand) in the contact oxidation part biological film on the azo dye, the intermediate product and the wastewater is improved.
The wastewater treatment system is integrated equipment, so that the occupied area of a treatment device is greatly reduced, the treatment speed and the treatment effect of dye wastewater are improved, the dye wastewater with high COD concentration is effectively degraded, no secondary pollution is caused, and the early equipment investment and the operation cost are reduced.
Drawings
FIG. 1 is a schematic view of a preferred embodiment of the present invention;
FIG. 2 is a partial schematic view of a cartridge packing in accordance with a preferred embodiment of the present invention;
fig. 3 is a schematic structural view of another preferred embodiment of the present invention.
[ reference numerals description ]
1: a lower end cap;
2: a first tube body;
3: a second tube body;
4: a third tube body;
5: an upper end cap;
6: an external circuit;
7: the first water distribution plate;
8: the second water distribution plate;
9: a fourth pipe body;
10: an aerobic layer;
11: an anaerobic layer;
101: an outer layer of biofilm;
102: an inner layer biofilm;
201: a liquid inlet hole;
202: a biological cathode;
203: a first reference electrode;
204: a first sampling hole;
301: a biological anode;
302: a second sampling hole;
401: a through hole;
402: an aeration head;
403: an ultraviolet lamp;
404: a cylindrical filler;
405: plate-type packing;
901: a waste water outflow hole;
902: and a second reference electrode.
Detailed Description
The invention aims at solving the problems that the existing integrated wastewater treatment device is low in treatment speed, accurate aeration is difficult to control, toxic products in the middle of azo decomposition are easy to remain, and the oxygen supply of a contact oxidation aerobic biomembrane is insufficient in a micro-oxygen environment, so that the COD (chemical oxygen demand) removal of high-concentration COD azo dye wastewater is limited. Meanwhile, the photocatalyst can degrade azo dyes, but has the disadvantages that the pollutant concentration of the azo dyes has direct influence on the degradation process, the high-concentration azo dyes deepen the color of a reaction system, influence the light transmittance of the system, reduce the removal efficiency of the azo dyes, indirectly increase the energy consumption of the degradation reaction process, develop an integrated wastewater treatment system and process capable of solving the defects of the prior art, enable the dye wastewater treatment process to be more energy-saving and efficient, and particularly provide a biocatalysis and photocatalytic contact oxidation coupling wastewater treatment system.
The invention will be better explained by the following detailed description of the embodiments with reference to the drawings.
Example 1
A wastewater treatment system coupled with biocatalysis and photocatalytic contact oxidation, as shown in fig. 1, comprising: the lower end cover 1, the first pipe body 2, the second pipe body 3, the third pipe body 4 and the upper end cover 5 are sequentially connected from bottom to top; a liquid inlet 201 is formed on one side of the pipe wall of the first pipe body 1 and is used as a waste water inlet hole, a through hole 401 is formed on one side of the pipe wall of the third pipe body 4 and is used as a liquid outlet, and waste water flows from the first pipe body 2 to the third pipe body 3; a biological cathode 202 is arranged in the first tube body 2 and is connected with an external circuit 6; a biological anode 301 is arranged in the second pipe body 3, and the biological anode 301 is connected with an external circuit 6; microorganisms are attached to the surfaces of the biocathode 202 and the bioanode 301, and the microorganisms can break the azo double bonds of the chromophores in the azo dye and decompose the azo double bonds into toxic small-molecule aromatic hydrocarbon substances. The microorganism is an anaerobic biological film, and the anaerobic biological film can be mixed bacteria or single extracellular electrogenesis bacteria; the third pipe body 4 is internally provided with a mixed filler and an ultraviolet lamp 403, the mixed filler consists of an outer layer of barrel-shaped filler 404 and an inner layer of plate-shaped filler 405, the center of the mixed filler is a cavity, the barrel-shaped filler 404 is attached with a mixed biological film of an aerobic biological film and an anaerobic biological film, the outer surface of the plate-shaped filler 405 is plated with a photocatalytic material, the barrel-shaped filler 404 is cylindrical, the plate-shaped filler 405 is just clamped and embedded on the barrel-shaped filler 404, a gap is reserved between the barrel-shaped filler 404 and the plate-shaped filler 405, the contact area between the waste water and the mixed biological film on the barrel-shaped filler and the photocatalytic material is increased, the waste water can be fully reacted with the mixed biological film and the photocatalytic material, and the ultraviolet lamp 403 is arranged in the middle of the cavity of the plate-shaped filler 405.
The plate-type filler 405 can be made of polyurethane material, and the photocatalytic material is TiO 2 A photocatalyst; the cylinder type filler is attached with a mixed biological film, wherein the cylinder type filler can be made of polyethylene fiber material and is cylindrical, and the inner side of the cylinder type filler is attached with an aerobic biological film and the outer side of the cylinder type filler is attached with an anaerobic biological film; specifically, when the treated wastewater is nitrogen dye, the aerobic biomembrane can open the benzene ring in the micromolecular aromatic hydrocarbon substances, and the treated wastewater is nitrogen dyeAnaerobic biofilms can degrade azo dyes. In order to enable the aerobic biomembrane to exert the optimal effect, an aeration head is further arranged in the third pipe body, and the aeration head is arranged close to the inside of the cylindrical filler. Aerobic microorganisms are attached to the outer layer biological film close to the aeration zone, and facultative microorganisms are attached to the inner layer biological film far away from the aeration zone; anaerobic microorganisms and partial facultative microorganisms are attached to the anaerobic biofilm. The photocatalytic material can promote the decolorization of azo dyes.
Specifically, anaerobic biomembrane is arranged on one side of the outer wall of the cylindrical filler 404, which is close to the inner wall of the third pipe body 4, aerobic biomembrane is arranged on one side of the cylindrical filler 404, which is far away from the inner wall of the third pipe body 4, an aeration head 402 and an ultraviolet lamp 403 are arranged in the cylindrical filler 404, a plate-shaped filler 405 is arranged in the cylindrical filler 404, a photocatalytic material is plated on the outer surface of the plate-shaped filler 405, and an ultraviolet lamp 403 is arranged in the plate-shaped filler.
The specific preparation of the mixed microorganism attached to the cylindrical filler can adopt the following method that the biofilm formation of the cylindrical filler is started: the inoculated sludge is taken from secondary sedimentation tank activated sludge (taking secondary sedimentation tank activated sludge of a sewage treatment plant of a Shenshui bay as an example), cylindrical mixed filler is put into a barrel, quantitative PBS buffer solution and glucose are added for 48 hours of stuffy exposure, then continuous water inflow is started, the hydraulic retention time is 24 hours, and the aeration quantity is controlled to control the concentration of dissolved oxygen to be about 2-3 mg/L. 2-naphthylamine-4, 8-disulfonic acid and 1-naphthylamine are added according to the mass concentration of the substances, the total concentration gradient of the two substances is gradually increased from 10mg/L, 30mg/L, 50mg/L and 70mg/L to 100mg/L, meanwhile, the COD concentration of the entering water is controlled to be 5000mg/L, the COD concentration of the water is detected, when the concentration of the aromatic amine substances reaches 100mg/L and the COD removal rate is stabilized to be more than 90%, the film hanging is successfully started, and as the Dissolved Oxygen (DO) concentration in the mixed filler gradually decreases from inside to outside, as shown in figure 2, the cylindrical filler consists of an inner aerobic layer 10 and an outer anaerobic layer 11, aerobic microorganisms are attached to an outer layer biological film 101 of the aerobic layer 10, which is close to an aeration zone, facultative microorganisms are attached to an inner layer biological film 102 of the aerobic layer, and partial facultative microorganisms are attached to the biological film on the anaerobic layer 11.
At the same time utilize TiO 2 And carrying out load coating on the plate type filler by using the photocatalyst. After two kinds of fillers with different load types are fixed on the inner side and the outer side of a cylindrical filler frame, the mixed filler is obtained and is placed into a biological contact oxidation-photocatalysis composite zone of the system, namely a third pipe body.
Wherein, the quantitative PBS buffer solution and glucose are 2L, and the preparation method of the PBS buffer solution is that sodium dihydrogen phosphate is 2g/L disodium hydrogen phosphate, 11.5g/L potassium chloride is 0.2g/L ammonium chloride is 0.5g/L; the glucose addition amount is 1000mg/L.
The manufacturing method of the biocathode and the biocathode can be as follows: the manufactured annular carbon brush electrode is put into a muffle furnace to be pretreated by calcining at the high temperature of 450 ℃ for 30min, one group of carbon brushes are installed in the second tube body to serve as anodes, and three groups of carbon brushes are installed in the first tube body to serve as cathodes. Pure Ornida Shewanella (Shewanella oneidensis MR-1) is used as an inoculum, electrode liquid with common matrix sodium lactate (with the concentration of 2000 mg/L) is replaced in an ultra-clean bench, the cultured MR-1 bacterial liquid is poured into a sterilized centrifuge tube, the supernatant is centrifuged in the centrifuge, the bacterial liquid reserved in the centrifuge tube is flushed by a prepared and sterilized catholyte (PBS buffer) by a sterile syringe, and the reactor electrode is connected, and then the reactor is connected to an external voltage for operation. The voltage of the direct current stabilized power supply is fixed to be 0.7V, data of the microbial electrolytic cell are sampled periodically, after the potential of the two poles of the microbial electrolytic cell is stabilized, electrogenic microorganisms (namely, onedawatt bacteria) are considered to be fully attached to the surface of the electrode, and at the moment, the manufacturing of the biological cathode 202 serving as the MR-1 reinforced biological cathode and the biological anode 301 serving as the MR-1 reinforced biological anode is completed.
Film formation starting of MR-1 reinforced biocathode and MR-1 reinforced bioanode: after the MR-1 reinforced biological cathode and the MR-1 reinforced biological anode are manufactured, adding azo dye to enable the gradient of the biological electrode to adapt to the toxicity of the azo dye, and enabling the concentration gradient of the azo dye to be sequentially increased to 10mg/L, 30mg/L, 50mg/L, 70mg/L and 100mg/L; the hydraulic retention time under each dye gradient is determined according to the change of the potential of the MR-1 reinforced biological cathode and the MR-1 reinforced biological anode after liquid exchange.
In order to monitor the treatment condition of the wastewater at any time, as shown in fig. 1, a first sampling hole 204 is provided in the pipe wall of the first pipe body 2. A second sampling hole 302 may be formed in the wall of the second tube 3. In order to facilitate measuring the potential of the bioanode and the biocathode, a first reference electrode 203 is provided at the upper portion of the first tube body near the second tube body.
In order to make the water flow in the whole reaction system more uniform, a first water distribution plate 7 is further arranged between the first pipe body 2 and the second pipe body 3, and a plurality of small holes are formed in the middle of the first water distribution plate 7 for allowing wastewater to flow into the second pipe body 3. In order to reduce the influence of the dissolved oxygen in the third pipe body 3 on the biological anode 301, a second water distribution plate 8 is further arranged between the first pipe body 2 and the second pipe body 3. A water inlet hole is arranged in the middle of the second water distribution plate 8 for wastewater to flow into the third pipe body 4, and only one water inlet hole is arranged for avoiding the influence of the oxygen content on the biological anode 301 after aeration.
The technical process for treating the wastewater by adopting the bioelectrocatalysis and photocatalytic contact oxidation coupling wastewater treatment system comprises the following steps:
a. passing dye wastewater through a wastewater inlet aperture into a wastewater treatment system as described above;
b. the wastewater is firstly contacted with a biological cathode at the lower section of the reactor, the biological cathode can be an anaerobic microorganism Shewanella oneidensis MR-1 reinforced biological cathode, the material is a carbon brush, and under the combined action of the strain MR-1 vat azo dye and electrochemical catalytic reduction, the azo double bond of the chromophoric group in the azo dye is broken, so that the primary decolorization effect is achieved, and the azo dye is decomposed into toxic micromolecular aromatic hydrocarbon substances.
c. The waste water passing through the biological cathode contacts with the biological anode at the middle section of the reactor, the biological anode is an enhanced biological anode of anaerobic microorganism Shewanella oneidensis MR-1, the anode material is a carbon brush, and due to the extracellular electron transfer characteristic of the strain Shewanella oneidensisMR-1, compared with a mixed bacterial biological membrane, more electrons can be transferred to the electrode while small molecular organic matters are degraded, and then the additional electrons are provided for the enhanced biological cathode through an external circuit, so that COD (chemical oxygen demand) removal and the degradation process of the cathode are realized, and the fracture of azo bonds and further decolorization are accelerated.
d. The waste water passing through the biological anode and the mixed dimension filler at the upper section of the reactor are divided into an inner layer and an outer layer, a photocatalytic material is hung on the inner layer plate-type filler, and the photocatalytic material promotes the decoloration of residual azo dye under the irradiation of an ultraviolet lamp; the outer cylindrical filler is hung with a mixed biological film, and residual azo dye is further degraded under the combined action of the aerobic biological film and the anaerobic biological film, and the degraded product is completely mineralized. Because of sufficient aeration, the contact oxidation of the aerobic biomembrane can effectively remove the high-concentration COD in the wastewater.
f. And finally discharging the treated liquid through the wastewater outflow hole.
Compared with the prior integrated reactor, the invention moves the biological anode at the last section to the middle section of the reactor, so that the internal resistance between the biological anode and the biological cathode is effectively reduced, the coulomb efficiency of the biological electrolytic cell is improved, the whole biological electro-catalysis stage has more pertinence to the decoloring process of azo dyes, the carrier consisting of the contact oxidation system and the photocatalysis system is arranged at the last section of the reactor, the pertinence of mixed filler to aromatic hydrocarbon substances of azo decomposition products is enhanced, the influence on the bioelectrocatalysis process is reduced, and the reactor can maintain stable COD removal rate even under the condition of high COD content of inflow water, thereby ensuring the effect of realizing final mineralization of wastewater.
Example 2
The bio-electro-catalytic and photo-catalytic contact oxidation coupling wastewater treatment system of this embodiment is based on embodiment 1, as shown in fig. 3, a fourth pipe body 9 is disposed between the third pipe body 4 and the upper end cover 5, so that the water outlet of the third pipe body 4 is an opening communicated with the fourth pipe body, after the wastewater fully contacts and reacts in the third pipe body 4, the wastewater flows to the fourth pipe body 9, flows out from a wastewater outflow hole 901 disposed on the pipe wall of the fourth pipe body, and a through hole 401 originally used as a water outlet on the original third pipe body 4 can be used as a third sampling hole for detecting the decolorization effect of the wastewater after treatment. In order to detect the activity of the strain, a second reference electrode 902 is also provided on the wall of the fourth tube 9.
Taking dye direct blue 71 wastewater treatment as an example, the direct blue 71 is decolorized and deeply mineralized by adopting the bioelectrocatalysis and photocatalytic contact oxidation coupling wastewater treatment system of the embodiment, and the method specifically comprises the following steps:
A. the concentration of direct blue 71 is 100mg/L, COD is 5000mg/L, and wastewater with pH value of 6-8 enters through the liquid inlet hole 201;
B. the wastewater flows into the first tube body 2 to be contacted with the carbon brush MR-1 reinforced biological cathode attached with anaerobic organisms, the MR-1 reinforced biological cathode is connected with an external circuit, the applied voltage is 0.7V, the tube wall of the first tube body 2 is provided with a first sampling hole 204, and the first sampling hole 204 is arranged at the cross section where the MR-1 reinforced biological cathode is positioned or at the position far away from the cross section of the MR-1 reinforced biological cathode along the water flow for sampling and detecting the wastewater treatment condition. Under the electrochemical reduction action of MR-1 intensified biological cathode, the azo double bond of chromophoric group in azo dye is broken to generate small molecular aromatic hydrocarbon substance, in particular, the azo bond between benzene rings in direct blue 71 is broken, one molecule of direct blue 71 substance is degraded into one molecule of 2-naphthylamine-4, 8-disulfonic acid, one molecule of 1-naphthylamine-7-sulfonic acid and one molecule of 2-amino-5-naphthol-7-sulfonic acid substance, and the waste water removes its own deep blue.
C. The wastewater passing through the MR-1 reinforced biological cathode flows into the second pipe body 3 through a plurality of small holes of the first water distribution plate 7, a single biological anode 301 is arranged in the second pipe body 3, and a graphite carbon brush attached with anaerobic organisms is used as the MR-1 reinforced biological anode. The wastewater is contacted with the MR-1 reinforced bioanode 301 in the second pipe body 3, and the anaerobic biomembrane (Shewanella oneidensis MR-1) attached to the surface of the MR-1 reinforced bioanode 301 decomposes the micromolecular degradable organic matters and generates extra electrons, and the extra electrons are provided for the MR-1 reinforced bioanode through an external circuit to promote the progress of the biocathode reaction, so that the rupture of azo bonds is further accelerated, and the effect of further decoloring is achieved.
D. The waste water passing through the MR-1 reinforced bioanode flows into the third pipe body 4 from the through hole in the middle of the second water distribution plate 8 through up-flow, the waste water is subjected to contact oxidation reaction and photocatalysis reaction in the third pipe body 4, the third pipe body 4 is filled with mixed filler, the mixed filler consists of middle plate-type filler 405 (polyurethane) and outer cylindrical filler 404 (polyethylene fiber) 3, oxygen enters the third pipe body 4 through the aeration head 402, oxygen source is provided for aerobic microorganisms attached to the cylindrical filler, meanwhile, the flow of liquid in the pipe body is promoted through aeration (aeration amount is 900 mL/min), the rest azo dye is promoted to decolorize under the irradiation of an ultraviolet lamp 403, the anaerobic microorganisms on the inner ring of the mixed filler open chains on benzene rings in small molecular aromatic hydrocarbon substances, the anaerobic biological film (the anaerobic biological film can also be a system consisting of highly dense aerobic bacteria, anaerobic bacteria, facultative bacteria, fungi, protozoa and algae) on the outer ring of the mixed filler, the anaerobic biological film occupies the anaerobic bacteria to occupy the large scale, azo bonds in the anaerobic biological film can further degrade azo dye residues in the cylindrical filler, and the azo dye residues in the pipe body can be further detected, the COD (COD) can be further reduced, the concentration of the azo dye can be further detected, and the sample concentration of the waste water can be further reduced, and the sample 4 can be further combined with the through hole is further arranged.
E. The third pipe body 4 is communicated with the fourth pipe body 9, and finished water obtained through the fourth pipe body 9 is discharged through the waste water outflow holes 901. A second reference electrode 902 for monitoring the activity of the bioelectrode electrogenesis bacteria is installed on the pipe wall in the fourth pipe body 9. Under the condition of hydraulic retention time of 12h, sampling is carried out for multiple times at the second sampling hole 302, the decoloring rate of the direct blue 71 waste water can reach 85%, and sampling is carried out for multiple times at the through hole 401, so that the decoloring rate of the direct blue 71 dye waste water can reach 96% +/-2%. Through detection, the COD of the water is lower than 200mg/L, and the concentration of the direct blue 71 is lower than 5mg/L, so that the COD removal rate of the water at the position of the wastewater outflow hole 901 can reach 96%. Therefore, the wastewater treatment system can effectively remove dye macromolecular substances in wastewater, and has obvious effect on wastewater treatment with high COD content.
The above description is only a preferred embodiment of the present invention, and is not intended to limit the invention in any way, and any person skilled in the art may make modifications or alterations to the disclosed technical content to the equivalent embodiments. However, any simple modification, equivalent variation and variation of the above embodiments according to the technical substance of the present invention still fall within the protection scope of the technical solution of the present invention.
Claims (9)
1. A wastewater treatment system coupled with biocatalysis and photocatalytic contact oxidation, comprising:
the device comprises a first pipe body, a second pipe body and a third pipe body which are connected in sequence, wherein a liquid inlet is formed in the pipe wall of the first pipe body, and a liquid outlet is formed in the third pipe body; it is characterized in that the method comprises the steps of,
a biological cathode is arranged in the first tube body and is connected with an external circuit;
a biological anode is arranged in the second pipe body and is connected with an external circuit, and microorganisms are attached to the surfaces of the biological anode and the biological cathode;
the third pipe body is internally provided with a mixed filler and an ultraviolet lamp, the mixed filler consists of an outer layer of barrel-shaped filler and an inner layer of plate-shaped filler, the center of the mixed filler is a cavity, an aerobic biomembrane and an anaerobic biomembrane are attached to the barrel-shaped filler, the outer surface of the plate-shaped filler is plated with a photocatalytic material, and the ultraviolet lamp is arranged in the cavity;
the plate-type filler is made of polyurethane material; the inner side of the cylinder-shaped filler is attached with an aerobic biomembrane, and the outer side of the cylinder-shaped filler is attached with an anaerobic biomembrane;
and an aeration head is further arranged in the third pipe body, and the aeration head is arranged close to the inside of the cylindrical filler.
2. The wastewater treatment system of claim 1, wherein,
the biological cathode and the biological anode are annular carbon brush electrodes, and the biological cathode is provided with two or more than three groups;
the microorganism is an anaerobic microorganism which is a mixed bacterium or a single extracellular electrogenesis bacterium, or
The microorganism is osnescen Shewanella;
the photocatalytic material is TiO 2 A photocatalyst.
3. The wastewater treatment system of claim 1, wherein,
the first tube body is provided with a first reference electrode.
4. The wastewater treatment system of claim 1, wherein,
the first pipe body, the second pipe body and the third pipe body are sequentially connected from bottom to top, the lower end of the first pipe body is provided with a lower end cover, and the upper end of the third pipe body is provided with an upper end cover; a first water distribution plate is arranged between the first pipe body and the second pipe body, and a plurality of small holes are formed in the first water distribution plate; a second water distribution plate is arranged between the second pipe body and the third pipe body, and the second water distribution plate is provided with a water inlet hole.
5. The wastewater treatment system of claim 1, wherein,
a fourth pipe body is arranged between the third pipe body and the upper end cover, and a wastewater outflow hole is formed in the fourth pipe body; and a second reference electrode is arranged on the fourth tube body.
6. The wastewater treatment system of any one of claim 1 to 5,
the first pipe body is provided with a first sampling hole, and/or the second pipe body is provided with a second sampling hole.
7. A method for treating wastewater by coupling bioelectrocatalysis and photocatalysis contact oxidation is characterized in that,
the method comprises the following steps:
1) The wastewater is contacted with a biological cathode, and under the combined action of microorganisms and electrochemical catalytic reduction on the biological cathode, the azo double bond of a chromophoric group in the azo dye is broken and decomposed into toxic micromolecular aromatic hydrocarbon substances;
2) The wastewater containing the micromolecular aromatic hydrocarbon substances is contacted with a biological anode, microorganisms are attached to the biological anode, more electrons are transmitted to an electrode while the micromolecular organic substances are degraded, and then the extra electrons are provided for the biological cathode through an external circuit, so that COD (chemical oxygen demand) removal is realized, the biological cathode reaction is promoted, the fracture of azo bonds is accelerated, and further decolorization is realized;
3) The wastewater treated in the step 2) is contacted with mixed filler, the mixed filler consists of inner filler hung with photocatalytic material and outer filler hung with mixed biological film, the mixed biological film comprises an aerobic biological film and an anaerobic biological film, the photocatalytic material promotes the decoloration of residual azo dye under the irradiation of ultraviolet lamp, the aerobic biological film opens a chain to benzene rings in micromolecular aromatic hydrocarbon substances, the anaerobic biological film further degrades the azo dye with residual azo bond not broken, and the residual azo dye is further degraded and the degraded product is completely mineralized under the combined action of the mixed biological film and the photocatalytic material.
8. The method of claim 7, wherein,
in the step 3), an aeration head is arranged close to the aerobic microbial film to provide an oxygen source for the aerobic microorganisms, so that the close aerobic microbial film can effectively remove high-concentration COD in the wastewater.
9. The method of claim 7, wherein,
the anaerobic microorganisms in the anaerobic microbial membrane are mixed bacteria or single extracellular electrogenerated bacteria.
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