CN111087071A - Microbial electrochemical device and method for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater - Google Patents

Microbial electrochemical device and method for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater Download PDF

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CN111087071A
CN111087071A CN201911357427.6A CN201911357427A CN111087071A CN 111087071 A CN111087071 A CN 111087071A CN 201911357427 A CN201911357427 A CN 201911357427A CN 111087071 A CN111087071 A CN 111087071A
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electrolysis cell
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孙德智
聂含冰
党岩
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Beijing Forestry University
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    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00Biological treatment of water, waste water, or sewage
    • C02F3/30Aerobic and anaerobic processes
    • C02F3/302Nitrification and denitrification treatment
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F3/00Biological treatment of water, waste water, or sewage
    • C02F3/005Combined electrochemical biological processes
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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Abstract

The invention discloses a microbial electrochemical device and a method for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater. The device comprises a shortcut nitrification tank, a cathode chamber of a microbial electrolysis tank and an anode chamber of the microbial electrolysis tank which are connected in sequence; the short-cut nitrification tank is provided with a water inlet and a water outlet a, and the water outlet a is connected with an inlet of the cathode chamber of the microbial electrolysis tank through a connecting pipeline; a cathode electrode is arranged in the cathode chamber of the microbial electrolysis cell and is connected with the cathode of the electrochemical workstation through a lead; the top of the anode chamber of the microbial electrolysis cell is provided with a gas collecting hood, the lower part of the anode chamber is provided with a medicine inlet, and the inside of the anode chamber is provided with an anode electrode; the gas collecting hood is connected with a collecting pipe to be connected with a collecting device; the anode electrode is connected with the anode of the electrochemical workstation through a lead; microbial electrolysis cell cathodeThe polar chamber is communicated with the anode chamber of the microbial electrolysis cell, and an anion exchange membrane is arranged at the joint. The invention solves the problem of the biological sewage treatment process N2Low conversion of O and N2O is a problem of practical application of functional strains of the final product.

Description

Microbial electrochemical device and method for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater
Technical Field
The invention relates to a microbial electrochemical device and a method for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater, belonging to the technical field of biological sewage treatment.
Background
Nitrous oxide (N)2O) is a greenhouseGas, N in biological denitrification of waste water2O is mainly formed by nitrate → nitrite → NO → N2And generating a denitrification link of O. However, N is2O is also a highly efficient clean energy gas which decomposes into N during combustion2And O2Does not generate secondary pollutants and is compared with O2The combustion process as oxidant can release more heat, so it can be used as combustion improver and oxygen-making agent. Thus, in the biological denitrification of waste water, for example, the formation of N can be controlled2At this stage of O, N can be recovered2O energy gas, the purpose of converting nitrogen-containing organic matters in the wastewater into clean energy gas is realized.
Currently, N is produced and recovered from wastewater treatment processes2The O method utilizes high-concentration nitrite to inhibit the activity of the nitrous oxide reductase, and utilizes the simultaneous nitrification and denitrification without the AOB of the nitrous oxide reductase and a batch type aerobic-anoxic coupled denitrification process (CANDO) process. Among them, the invention patent (CN201310357185.7) provides a reinforced N2The device and the control method for O generation utilize high-concentration nitrite to inhibit the activity of nitrous oxide reductase so as to convert more nitrite nitrogen into N in the denitrification process2O, followed by aeration of N2O headspace Collection, Final N2The accumulation rate of O is between 15 and 60 percent. However, N of this method2The O accumulation rate is unstable, and N is added by aeration2O headspace will result in recovered N2The concentration of O is lower, and the embodiment aims at the sewage of the septic tank in the residential area, the concentration of ammonia nitrogen is lower, and the sewage is not suitable for N2And (4) recovering O in a large amount. The invention patent (CN201310743142.2) provides N in the process of realizing short-cut nitrification of sludge digestive fluid2A method for generating and utilizing O comprises the steps of treating sludge digestive juice by using shortcut nitrification granular sludge, under the condition of high dissolved oxygen concentration, using AOB to consume a large amount of dissolved oxygen on the surface of the shortcut nitrification granular sludge as an electron acceptor to oxidize high-concentration ammonia nitrogen into nitrite, using the high-concentration nitrite to inhibit the activity of denitrifying bacteria nitrous oxide reductase, forming a microscopic anaerobic environment in the granular sludge, and using AOB without nitrous oxide reductase to treat sludge digestive juiceDenitrifying nitrite nitrogen to N2O, realization of N2Accumulation of O, finally N2The release amount of O accounts for 15-30% of the oxidation amount of ammonia nitrogen. N achieved by the method2Low conversion of O, aeration due to dissolved oxygen control, N2The actual concentration of O recovery will be lower. The invention patent (CN201710127743.9) discloses a reinforced N2The invention relates to a sewage biological denitrification method and a sewage biological denitrification device for O generation and recycling, which mainly adopt an intermittent aerobic-anoxic coupling denitrification process to slowly provide a denitrification carbon source in a PHB form by adjusting operation process parameters so as to realize N2And (4) accumulating O. The method has complex operation and harsh control conditions in the actual operation process, and is not suitable for efficiently producing N from actual wastewater2O。
In the process of biological sewage treatment, nitrate nitrogen or nitrite nitrogen is completely converted into N2O, requires cleaving N2Conversion of O to N2The pathway of (1). The invention patent (CN201711100403.3) discloses a method for synthesizing N2O is the denitrifying bacteria of the final product, the denitrifying bacteria are obtained by domestication in the SBR reactor according to specific operation process parameters (such as nitrogen exposure and low C/N ratio), but whether the denitrifying bacteria can become dominant bacteria under the process condition of treating actual wastewater is not clear, once the bacteria cannot become dominant bacteria, the N produced by denitrification of the bacteria is2O is continuously utilized and reduced into N by common denitrifying bacteria2
Disclosure of Invention
The invention aims to provide a microbial electrochemical device and a method for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater, and the invention solves the problem of N in the biological sewage treatment process2Low conversion of O and N2O is a problem of practical application of functional strains of the final product.
The invention provides a microbial electrochemical device for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater, which comprises a shortcut nitrification tank, a microbial electrolysis tank cathode chamber and a microbial electrolysis tank anode chamber which are sequentially connected;
the short-cut nitrification tank is provided with a water inlet and a water outlet a, and the water outlet a is connected with an inlet of the cathode chamber of the microbial electrolysis tank through a connecting pipeline;
a cathode electrode is arranged in the cathode chamber of the microbial electrolysis cell and is connected with the cathode of the electrochemical workstation through a lead;
the top of the anode chamber of the microbial electrolysis cell is provided with a gas collecting hood, the lower part of the anode chamber is provided with a medicine inlet, and the inside of the anode chamber is provided with an anode electrode; the gas collecting hood is connected with a collecting pipe to be connected with a collecting device; the anode electrode is connected with the anode of the electrochemical workstation through a lead;
the cathode chamber of the microbial electrolysis cell is communicated with the anode chamber of the microbial electrolysis cell, and an anion exchange membrane is arranged at the joint of the cathode chamber and the anode chamber.
In the microbial electrochemical device, the short-cut nitrification tank is inoculated with activated sludge in an aerobic tank of a sewage treatment plant;
the anode chamber of the microbial electrolytic cell is inoculated with a Pseudomonas aeruginosa PAO1 denitrifying strain with a deletion of the nosZ gene.
In the microbial electrochemical device, an aeration device is arranged in the short-cut nitrification tank.
In the above microbial electrochemical device, the shortcut nitrification tank is provided with at least one of a temperature control device for monitoring the internal temperature thereof, a dissolved oxygen on-line monitoring system for monitoring the dissolved oxygen therein, and a pH on-line monitoring system for monitoring the pH value therein.
In the microbial electrochemical device, the stirring device a is arranged in the short-cut nitrification tank and used for ensuring the uniform distribution of substances in the tank.
In the above microbial electrochemical device, the stirring device b is arranged in the cathode chamber of the microbial electrolytic cell, and is used for ensuring the uniform distribution of substances in the cathode chamber.
In the above-mentioned microbial electrochemical device, a stirring device c is disposed inside the anode chamber of the microbial electrolytic cell, so as to ensure uniform distribution of substances therein.
In the microbial electrochemical device, the upper part of the cathode chamber of the microbial electrolytic cell is provided with a water outlet b for overflowing.
And a water outlet c is arranged at the upper part of the anode chamber of the microbial electrolysis cell and plays a role in overflowing.
In the invention, the anode chamber of the microbial electrolysis cell is provided with a gas collecting hood and a collecting pipe for collecting gaseous N generated in the biological treatment process2O。
The invention also provides a microbial electrochemical method for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater by adopting the microbial electrochemical device, which comprises the following steps: 1) nitrogen-containing wastewater enters from a water inlet of the short-cut nitrification tank, and is subjected to nitrification reaction in the short-cut nitrification tank to obtain short-cut nitrification effluent;
2) the short-range nitrified effluent enters a cathode chamber of the microbial electrolysis cell through the connecting pipeline, a Pseudomonas aeruginosa PAO1 denitrifying strain with a nonsZ gene deletion is inoculated into the anode chamber of the microbial electrolysis cell, a carbon source is introduced into the drug inlet, an electrolytic reaction is carried out under the control of the electrochemical workstation, and a gas-state N is collected and generated through a gas collecting hood of the anode chamber of the microbial electrolysis cell and a collecting pipe connected with the gas collecting hood2O, i.e. effecting the collection of gaseous N produced during the biological treatment2O。
In the microbial electrochemical method, the short-cut nitrification tank is inoculated with the activated sludge in the aerobic tank of the sewage treatment plant for carrying out the denitrification reaction;
the denitrification reaction time can be 44-52 h, specifically 48h, 44-48 h, 48-52 h or 46-50 h, and the temperature is 30-31 ℃;
the time of the electrolytic reaction can be 44-52 h, specifically 48h, 44-48 h, 48-52 h or 46-50 h;
the C/N of the anode chamber of the microbial electrolysis cell is 4.5-5; the carbon source is sodium acetate, and specifically sterile sodium acetate is used.
In the microbial electrochemical method, the concentration of dissolved oxygen in the shortcut nitrification tank is 0.1-0.5 mg/L;
the stirring speed in the short-cut nitrification tank can be 150-250 r/min, and specifically can be 200 r/min; the pH value is 8.5-8.7; specifically, 0.1mol/L sodium hydroxide solution is used as a regulator to control the pH value in the pool as the data;
the stirring speed of the cathode chamber of the microbial electrolysis cell and the stirring speed of the anode chamber of the microbial electrolysis cell can be 50-100 r/min, and particularly can be 50 r/min;
in the microbial electrochemical method, the step 2) is followed by a step of purifying the wastewater discharged from the water outlet c of the anode chamber of the microbial electrolytic cell.
The invention has the following advantages:
1. compared with the traditional short-cut denitrification method for recovering N2The invention can reduce the risk that the inoculated Pseudomonas aeruginosa PAO1 functional strain with the deletion of the nosZ gene is occupied with the dominant position by other denitrifying bacteria, and can obtain the recovered N with higher efficiency and more stability2And (4) O effect.
2. The functional strain of the invention has high abundance in the reaction system, thereby increasing the utilization rate of the carbon source, reducing the carbon source adding amount in the actual engineering and reducing the cost.
3. The external potential of the microbial electrolytic cell is utilized to accelerate the mass transfer rate of nitrite ions, and the mass transfer rate is cooperated with the denitrification of the Pseudomonas aeruginosa PAO1 denitrifying strain with the loss of the nosZ gene, so that the denitrification efficiency is improved, and the N is further improved2The yield of O.
Drawings
FIG. 1 is a schematic diagram showing the efficient production and recovery of N from nitrogen-containing wastewater in the present invention2And O, structural schematic diagram of the microbial electrochemical device.
The individual labels in the figure are as follows:
1, a water inlet; 2 connecting a pipeline; 3, a water outlet of a cathode chamber of the microbial electrolysis cell; 4, continuously feeding medicine; 5, a water outlet of the anode chamber of the microbial electrolysis cell; 6 an aeration device; 7, a stirring device of the short-cut nitrification tank; 8, temperature control equipment of the shortcut nitrification tank; 9DO online monitoring equipment; 10pH on-line monitoring equipment; 11 temperature control equipment of a cathode chamber of the microbial electrolysis cell; 12 a stirring device of a cathode chamber of the microbial electrolysis cell; 13 cathode electrode of microbial electrolysis cell; 14 cathode lead of microbial electrolysis cell; 15 stirring device for anode chamber of microbial electrolysis cell; 16 microbial cell anode electrode; 17 gas-collecting channel; 18 microbial cell anode lead; 19 temperature control equipment for the anode chamber of the microbial electrolysis cell; 20 collecting pipes; 21 an anion exchange membrane; 22 short-cut nitrification tank; 23 microbial cell cathode chamber; 24 anode chamber of microbial electrolysis cell.
FIG. 2 is a graph comparing experimental data of example 2 of the present invention with comparative example.
Detailed Description
The experimental procedures used in the following examples are all conventional procedures unless otherwise specified.
Materials, reagents and the like used in the following examples are commercially available unless otherwise specified.
In the examples described below, the Pseudomonas aeruginosa PAO1 denitrifying strain (nonsZ-deletion mutant of Pseudomonas aeruginosa PAO1) with the deletion of the nosZ gene was derived from the document Significan mutation of nitrogen oxide genes from water step extracted from fermented by bioautomation with a recombinant strain of Pseudomonas aeruginosa, (2018)8: 11916.
Example 1 efficient production and recovery of N from Nitrogen-containing wastewater2Microbial electrochemical device of O
As shown in figure 1, the method is used for efficiently producing and recovering N from the nitrogen-containing wastewater2The O microbial electrochemical device is sequentially provided with a short-cut nitrification tank 22, a microbial electrolytic tank cathode chamber 23 and a microbial electrolytic tank anode chamber 24 along the conversion direction of nitrogenous substances, wherein wastewater containing ammonia nitrogen enters the short-cut nitrification tank 22 through a water inlet 1, ammonia nitrogen in the wastewater is converted into nitrite nitrogen after staying for 48 hours, then the nitrite nitrogen overflows into the microbial electrolytic tank cathode chamber 23 through a pipeline 2, the nitrite nitrogen overflows and is discharged from a water outlet 3 of the microbial electrolytic tank cathode chamber after staying for 24 hours, and the nitrite nitrogen enters the microbial electrolytic tank anode chamber 24 under the action of a cathode electrode 13 (connected with the cathode of an electrochemical workstation through a microbial electrolytic tank cathode lead 14) and an anode electrode 16 (connected with the cathode of the electrochemical workstation through a microbial electrolytic tank anode lead 18) and is converted into N through the denitrification of the knock-out bacteria of the nosZ genes2And O is collected and recovered through the gas collecting hood 17 and the collecting pipe 20. In addition, microorganisms are generated in the short-cut nitrification tank 22The cathode chamber 23 of the animal electrolytic cell and the anode chamber 24 of the microbial electrolytic cell are respectively provided with stirring devices 7, 12 and 15 and temperature control devices 8, 11 and 19, the short-cut nitrification tank is also provided with a DO online monitoring device 9, a pH online monitoring device 10 and an aeration device 6, the cathode chamber 23 of the microbial electrolytic cell is provided with a continuous medicine inlet 4 for continuously providing a carbon source, effluent flows through a water outlet 5 of the anode chamber 24 of the microbial electrolytic cell along with overflow and is discharged, and the cathode chamber 23 of the microbial electrolytic cell and the anode chamber 24 of the microbial electrolytic cell are separated 21 by an anion exchange membrane.
Ammonia nitrogen-containing wastewater enters a short-cut nitrification tank 22 from a water inlet 1 at the lower part of the short-cut nitrification tank 22, the retention time is 48 hours, an aeration device 6 and a DO online monitoring device 9 are arranged in the short-cut nitrification tank 22 and used for controlling the concentration of dissolved oxygen in the wastewater to be 0.1-0.5mg/L, a short-cut nitrification tank stirring device 7 is arranged in the short-cut nitrification tank 22 and used for keeping sludge and wastewater in uniform contact, the stirring speed is controlled to be 200r/min, a pH online monitoring device is arranged in the short-cut nitrification tank 22, 0.1mol/L sodium hydroxide solution is used for adjusting the pH to be 8.5-8.7, a temperature control device is arranged in the short-cut nitrification tank 22 and is controlled to be 30-31 ℃, the setting conditions are the optimal nitrification conditions of nitrifying bacteria (AOB) and are not beneficial to the growth of Nitrosobacteria (NOB), and4 +more oxidation to NO2 -But not NO3 -Thereby reducing unnecessary energy consumption of aeration. The wastewater of the short-cut nitrification tank 22 overflows into a cathode chamber 23 of the microbial electrolysis tank through a connecting pipe 2, the retention time is 48 hours, the cathode chamber 23 of the microbial electrolysis tank and an anode chamber 24 of the microbial electrolysis tank are respectively provided with a stirring device 12 of the cathode chamber of the microbial electrolysis tank and a stirring device 15 of the anode chamber of the microbial electrolysis tank, the stirring speed is set to be 50r/min to ensure the uniform concentration distribution of water ions in the tank and the stable mass transfer speed, the cathode chamber of the microbial electrolysis tank and the anode chamber of the microbial electrolysis tank are respectively provided with a temperature control device 11 of the cathode chamber of the microbial electrolysis tank and a temperature control device 19 of the anode chamber of the microbial electrolysis tank, the temperature is controlled to be about 30 ℃ to ensure the most efficient denitrification rate of bacteria2 -Enters through an anion exchange membrane 21 under the potential of the cathode 14 electrode 13 of the microbial electrolysis cell and the anode 18 electrode 16 of the microbial electrolysis cellAnode chamber, reduced to N by NosZ gene knock-out bacteria denitrification2And O. The anode chamber 24 of the microbial electrolysis cell is enriched with a large amount of nosZ gene knocking bacteria, and can be purified and cultured without being influenced by external bacteria under the isolation action of the anion exchange membrane 21, so that NO transferred from the cathode chamber can be purified2 -Conversion to N in large amounts2And O, the gas-collecting hood 17 and the collecting pipe 20 are recycled, sodium acetate is continuously provided through the continuous medicine inlet 4 to maintain C/N and 4.5-5 to ensure that bacteria in the microbial anode chamber 24 can be efficiently denitrified, and excessive bacteria liquid is discharged through the water outlet 5 of the microbial electrolytic cell anode chamber to maintain the balance of the system.
Examples 2,
Taking the waste incineration leachate of a certain waste incineration plant for anaerobic treatment of effluent as an example, the quality of the inlet water is as follows: COD concentration 2500mg/L, BOD5Concentration 1200mg/L, NH4 +The concentration of-N is 1000-1200 mg/L, and the pH is about 8.3. 2L of selected shortcut nitrification tank, 1L of cathode chamber and anode chamber of microbial electrolysis tank, inoculating activated sludge in aerobic tank of certain sewage treatment plant, maintaining sludge concentration at 3000mg/L, sludge age at 15 days, and maintaining dissolved oxygen in shortcut nitrification tank at 0.1-0.5 mg/L. The positive pole of the microbial electrolytic cell is inoculated with the nonsZ gene deletion strain Pseudomonas aeruginosa PAO 150 mL, and the temperature of the two chambers of the electrolytic cell is controlled at 30 ℃.
The specific operation steps are as follows:
(1) inoculating in a reactor: inoculating activated sludge in an aerobic tank of a sewage treatment plant in a shortcut nitrification tank, keeping the sludge concentration at 3000mg/L, inoculating a nonsZ gene deletion strain Pseudomonas aeruginosa PAO1 (OD) subjected to activation culture in an anode chamber of a microbial electrolysis tank600About 0.8) 50 mL;
(2) and (3) controlling reactor parameters: controlling the dissolved oxygen in the shortcut nitrification tank to be between 0.1 and 0.5mg/L, controlling the pH to be between 8.5 and 8.7, and controlling the operation temperature to be between 30 and 31 ℃; the operating temperature of the cathode chamber and the anode chamber of the microbial electrolysis cell is controlled at 30 ℃;
(3) the operation of the reactor: the microorganisms in each reaction tank are domesticated by feeding water with gradient concentration, and the anode chamber of the microorganisms continuously feeds sodium acetate as electrons for denitrificationDonor, ensuring NO2 -Complete conversion to N2O。
Test results show that after microorganisms in each reaction tank are acclimatized in a gradient concentration water inlet mode, the reaction device runs stably, and more than 95% of NH in the shortcut nitrification tank4 +Conversion of-N to NO2 --N, over 90% NO in the cathode compartment of the microbial electrolysis cell2 -The N is transferred into an anode chamber of the microbial electrolytic cell, the denitrification load reaches 500 mgN/(L.d), 99 percent of the NO2 -N was transformed by the nonsZ gene-deleted strain Pseudomonas aeruginosa PAO1 to obtain N2O, wherein gaseous N2The content of O is more than 85 percent. Realizes high-efficiency denitrification and simultaneously carries out N treatment2O is also recovered with great efficiency.
Examples 3,
From a sewage treatment plant2The anaerobic effluent of the O process is taken as an example, and the water inlet quality is as follows: COD concentration 500mg/L, BOD5Concentration 200mg/L, NH4 +The concentration of N is 120mg/L, and the pH value is about 8.3. 4L of selected shortcut nitrification tank, 2L of cathode chamber and anode chamber of microbial electrolysis tank, inoculating activated sludge in aerobic tank of certain sewage treatment plant, maintaining sludge concentration in tank at 2500mg/L, sludge age at 25d, and maintaining dissolved oxygen in shortcut nitrification tank at 0.1-0.5 mg/L. The positive pole of the microbial electrolytic cell is inoculated with the nonsZ gene deletion strain Pseudomonas aeruginosa PAO1100mL, and the temperature of the two chambers of the electrolytic cell is controlled at 30 ℃.
The specific operation steps are as follows:
(1) inoculating in a reactor: inoculating activated sludge in an aerobic tank of a sewage treatment plant in a shortcut nitrification tank, maintaining the sludge concentration at 2500mg/L, inoculating a nonsZ gene deletion strain Pseudomonas aeruginosa PAO1 (OD) subjected to activation culture in an anode chamber of a microbial electrolysis tank600About 0.8) 100 mL;
(2) and (3) controlling reactor parameters: controlling the dissolved oxygen in the shortcut nitrification tank to be between 0.1 and 0.5mg/L, controlling the pH to be between 8.5 and 8.7, and controlling the operation temperature to be between 30 and 31 ℃; the operating temperature of the cathode chamber and the anode chamber of the microbial electrolysis cell is controlled at 30 ℃;
(3) the operation of the reactor: in gradient concentrationFeeding water to domesticate microorganisms in each reaction tank, continuously feeding sodium acetate into a microorganism anode chamber to serve as an electron donor for denitrification, and ensuring NO2 -Complete conversion to N2O。
Test results show that after microorganisms in each reaction tank are acclimatized in a gradient concentration water inlet mode, the reaction device runs stably, and more than 98% of NH in the shortcut nitrification tank4 +Conversion of-N to NO2 --N, more than 95% NO in the cathode chamber of the microbial electrolysis cell2 -The N is transferred into an anode chamber of the microbial electrolytic cell, the denitrification load reaches 111 mgN/(L.d), 99 percent of the NO2 --N Pseudomonas aeruginosa PAO1 denitrifying Strain deleted by the nosZ Gene was transformed into N2O, wherein gaseous N2O accounts for more than 82 percent. Realizes high-efficiency denitrification and simultaneously carries out N treatment2O is also recovered with great efficiency.
Comparative examples 1,
The garbage incineration leachate is treated by adopting the traditional AO denitrification process to recover N2O is taken as a comparison example, the quality of inlet water is the same as that of the inlet water in the embodiment 2 of the invention, the operation condition of the short-cut nitrification tank is 2L and is the same as that of the inlet water in the embodiment 2 of the invention, 50mL of Pseudomonas aeruginosa PAO1 denitrifying strain with nonsZ gene deletion is inoculated in the short-cut denitrification tank 2L, and the operation temperature is 30 ℃.
Comparative examples 2,
Separately adopting electrolysis experiment to treat garbage incineration leachate and recover N2O, without inoculation of Pseudomonas aeruginosa PAO1 denitrifying strain with deletion of the nosZ gene, the result was that N was hardly reached2Effect of O recovery.
Inventive example 2 was compared to comparative example 1: 1. the nitrogen load is increased: traditionally 300 mgN/(L.d), the embodiment 2 of the invention achieves 500 mgN/(L.d); 2. n is a radical of2Conversion rate of O: the traditional rate is 82%, and the invention reaches 95%; 3. the abundance of functional flora (Pseudomonas aeruginosa PAO1 denitrified strain with deletion of the nosZ gene, marked as Pseudomonas in fig. 2) is shown in fig. 2: traditional 40% and the invention 81%.
As can be seen from the above experimental data,the denitrifying strain of the invention performs denitrification and electrode electrolysis in coordination, and has the advantages of high-efficiency denitrification and extremely high N2And (4) O conversion rate.
The foregoing embodiments are illustrative of the principles, implementations and practices of the present invention, and it will be understood by those skilled in the art that the invention is not limited thereto, and that the foregoing embodiments and descriptions are illustrative of the principles of the invention, and are intended to cover various modifications, equivalents, improvements, etc. within the spirit and scope of the invention.

Claims (10)

1. A microbial electrochemical device for efficiently generating and recovering nitrous oxide from nitrogen-containing wastewater comprises a shortcut nitrification tank, a microbial electrolysis tank cathode chamber and a microbial electrolysis tank anode chamber which are sequentially connected;
the short-cut nitrification tank is provided with a water inlet and a water outlet a, and the water outlet a is connected with an inlet of the cathode chamber of the microbial electrolysis tank through a connecting pipeline;
a cathode electrode is arranged in the cathode chamber of the microbial electrolysis cell and is connected with the cathode of the electrochemical workstation through a lead;
the top of the anode chamber of the microbial electrolysis cell is provided with a gas collecting hood, the lower part of the anode chamber is provided with a medicine inlet, and the inside of the anode chamber is provided with an anode electrode; the gas collecting hood is connected with a collecting pipe to be connected with a collecting device; the anode electrode is connected with the anode of the electrochemical workstation through a lead;
the cathode chamber of the microbial electrolysis cell is communicated with the anode chamber of the microbial electrolysis cell, and an anion exchange membrane is arranged at the joint of the cathode chamber and the anode chamber.
2. The microbial electrochemical device according to claim 1, wherein: the short-cut nitrification tank is inoculated with activated sludge in an aerobic tank of a sewage treatment plant;
the anode chamber of the microbial electrolytic cell is inoculated with a Pseudomonas aeruginosa PAO1 denitrifying strain with a deletion of the nosZ gene.
3. The microbial electrochemical device according to claim 1 or 2, wherein: an aeration device is arranged in the short-cut nitrification tank.
4. The microbial electrochemical device according to any one of claims 1 to 3, wherein: the shortcut nitrification tank is provided with at least one of a temperature control device for monitoring the internal temperature thereof, a dissolved oxygen on-line monitoring system for monitoring the dissolved oxygen therein and a pH on-line monitoring system for monitoring the pH value therein.
5. The microbial electrochemical device according to any one of claims 1 to 4, wherein: a stirring device a is arranged in the short-cut nitrification tank;
a stirring device b is arranged in the cathode chamber of the microbial electrolysis cell;
and a stirring device c is arranged inside the anode chamber of the microbial electrolysis cell.
6. The microbial electrochemical device according to any one of claims 1 to 5, wherein: a water outlet b is formed in the upper part of the cathode chamber of the microbial electrolysis cell;
and a water outlet c is formed in the upper part of the anode chamber of the microbial electrolysis cell.
7. A microbial electrochemical process for efficiently producing and recovering nitrous oxide from nitrogen-containing wastewater using the microbial electrochemical device according to any one of claims 1 to 6, comprising the steps of: 1) nitrogen-containing wastewater enters from a water inlet of the short-cut nitrification tank, and is subjected to nitrification reaction in the short-cut nitrification tank to obtain wastewater;
2) the short-range nitrified effluent enters a cathode chamber of the microbial electrolysis cell through the connecting pipeline, a Pseudomonas aeruginosa PAO1 denitrifying strain with a nonsZ gene deletion is inoculated into the anode chamber of the microbial electrolysis cell, a carbon source is introduced into the drug inlet, an electrolytic reaction is carried out under the control of the electrochemical workstation, and a gas-state N is collected and generated through a gas collecting hood of the anode chamber of the microbial electrolysis cell and a collecting pipe connected with the gas collecting hood2O, i.e. effecting the collection of gaseous N produced during the biological treatment2O。
8. The microbial electrochemical process of claim 7, wherein: the short-cut nitrification tank is inoculated with activated sludge in an aerobic tank of a sewage treatment plant to carry out denitrification reaction;
the denitrification reaction time is 44-52 h, and the temperature is 30-31 ℃;
the time of the electrolytic reaction is 44-52 h;
the C/N of the anode chamber of the microbial electrolysis cell is 4.5-5; the carbon source is sodium acetate.
9. The microbial electrochemical process of claim 7 or 8, wherein: the concentration of dissolved oxygen in the shortcut nitrification tank is 0.1-0.5 mg/L;
the stirring speed in the short-cut nitrification tank is 150-250 r/min; the pH value is 8.5-8.7;
the stirring speed of the cathode chamber of the microbial electrolysis cell and the stirring speed of the anode chamber of the microbial electrolysis cell are both 50-100 r/min.
10. Microbial electrochemical process according to any one of claims 7 to 9, characterized in that: the step 2) is followed by a step of purifying the wastewater discharged from the water outlet c of the anode chamber of the microbial electrolysis cell.
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112320940A (en) * 2020-10-21 2021-02-05 西安建筑科技大学 N production by enrichment of membrane contactor2Device and method for O denitrifying bacteria
CN112320942A (en) * 2020-10-21 2021-02-05 西安建筑科技大学 Method for realizing short-cut denitrification directional conversion N by utilizing modified flat membrane2O device and method

Citations (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH0839095A (en) * 1994-08-03 1996-02-13 Japan Organo Co Ltd Water treatment apparatus
CN101497862A (en) * 2009-02-27 2009-08-05 哈尔滨工业大学 Orienting enriching method for function strengthened microflora
CN101570731A (en) * 2009-03-25 2009-11-04 新奥科技发展有限公司 Method for domesticating and separating electricigens by electrochemistry
JP2012034576A (en) * 2010-08-03 2012-02-23 Kajima Corp Nitrous oxide decomposition apparatus
CN103043776A (en) * 2012-12-04 2013-04-17 哈尔滨工业大学 Sleeve-type microorganism catalysis electrolysis device and method for degrading waste water by using sleeve-type microorganism catalysis electrolysis device
CN104330455A (en) * 2014-07-16 2015-02-04 内蒙古科技大学 Method and device of on-line monitoring nitrate nitrogen through microbial electrolytic tank technology
EP2925679A1 (en) * 2012-11-28 2015-10-07 Universitat de Girona Bioelectrochemical water treatment and apparatus
CN105217796A (en) * 2015-11-04 2016-01-06 中国科学院水生生物研究所 A kind of method of downward vertical artificial wetland coupling microorganism electrolysis cell strengthened denitrification and device
CN106430870A (en) * 2016-10-17 2017-02-22 尚川(北京)水务有限公司 System and method for reinforcing excess sludge recycling
CN108946941A (en) * 2018-06-22 2018-12-07 南京大学 A kind of microorganism of low energy consumption-electrochemistry sewage disposal system
US20190119821A1 (en) * 2017-10-05 2019-04-25 Indian Oil Corporation Limited Treatment and recovery of caustic from spent caustic through bioelectrochemical process
WO2019079908A1 (en) * 2017-10-29 2019-05-02 Michael Siegert Bioelectrochemical method and apparatus for energy reclamation from nitrogen compounds

Patent Citations (12)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH0839095A (en) * 1994-08-03 1996-02-13 Japan Organo Co Ltd Water treatment apparatus
CN101497862A (en) * 2009-02-27 2009-08-05 哈尔滨工业大学 Orienting enriching method for function strengthened microflora
CN101570731A (en) * 2009-03-25 2009-11-04 新奥科技发展有限公司 Method for domesticating and separating electricigens by electrochemistry
JP2012034576A (en) * 2010-08-03 2012-02-23 Kajima Corp Nitrous oxide decomposition apparatus
EP2925679A1 (en) * 2012-11-28 2015-10-07 Universitat de Girona Bioelectrochemical water treatment and apparatus
CN103043776A (en) * 2012-12-04 2013-04-17 哈尔滨工业大学 Sleeve-type microorganism catalysis electrolysis device and method for degrading waste water by using sleeve-type microorganism catalysis electrolysis device
CN104330455A (en) * 2014-07-16 2015-02-04 内蒙古科技大学 Method and device of on-line monitoring nitrate nitrogen through microbial electrolytic tank technology
CN105217796A (en) * 2015-11-04 2016-01-06 中国科学院水生生物研究所 A kind of method of downward vertical artificial wetland coupling microorganism electrolysis cell strengthened denitrification and device
CN106430870A (en) * 2016-10-17 2017-02-22 尚川(北京)水务有限公司 System and method for reinforcing excess sludge recycling
US20190119821A1 (en) * 2017-10-05 2019-04-25 Indian Oil Corporation Limited Treatment and recovery of caustic from spent caustic through bioelectrochemical process
WO2019079908A1 (en) * 2017-10-29 2019-05-02 Michael Siegert Bioelectrochemical method and apparatus for energy reclamation from nitrogen compounds
CN108946941A (en) * 2018-06-22 2018-12-07 南京大学 A kind of microorganism of low energy consumption-electrochemistry sewage disposal system

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
ZIYU LIN等: "Significant enhancement of nitrous oxide energy yields from wastewater achieved by bioaugmentation with a recombinant strain of Pseudomonas aeruginosa", 《SCIENTIFIC REPORTS》 *
徐功娣等: "《微生物燃料电池原理与应用》", 30 November 2012, 哈尔滨工业大学出版社 *

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112320940A (en) * 2020-10-21 2021-02-05 西安建筑科技大学 N production by enrichment of membrane contactor2Device and method for O denitrifying bacteria
CN112320942A (en) * 2020-10-21 2021-02-05 西安建筑科技大学 Method for realizing short-cut denitrification directional conversion N by utilizing modified flat membrane2O device and method
CN112320942B (en) * 2020-10-21 2022-09-27 西安建筑科技大学 Method for realizing short-cut denitrification directional conversion N by utilizing modified flat membrane 2 O device and method
CN112320940B (en) * 2020-10-21 2023-03-14 西安建筑科技大学 N production by enrichment of membrane contactor 2 Device and method for O denitrifying bacteria

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