CN113735248A - Integrated sectional reactor for coupling anaerobic ammonia oxidation and three-dimensional electrode membrane biological process - Google Patents
Integrated sectional reactor for coupling anaerobic ammonia oxidation and three-dimensional electrode membrane biological process Download PDFInfo
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/005—Combined electrochemical biological processes
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- 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
- C02F3/28—Anaerobic digestion processes
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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
- C02F3/28—Anaerobic digestion processes
- C02F3/2866—Particular arrangements for anaerobic reactors
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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
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
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- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
Abstract
The invention relates to an integrated sectional reactor for coupling anaerobic ammonia oxidation and a three-dimensional electrode membrane biological process. The anaerobic ammonia oxidation reaction zone at the lower part of the shell comprises a porous water distributor, a temperature/dissolved oxygen/oxidation-reduction potential measuring instrument, a three-phase separator, an external reflux system and a gas collecting bag; the three-dimensional electrode membrane biological reaction area at the upper part of the shell comprises a sieve plate flange, a porous water distributor, a cathode, an anode, sponge iron, an activated carbon filling layer and a direct current power supply; sponge iron and an active carbon filling layer are filled between the cathode and the anode to form a three-dimensional electrode structure under the medium of sewage and wastewater. The high-concentration ammonia nitrogen is used as an electron donor for denitrification to form nitrogen and nitrate nitrogen, the nitrogen is discharged out of the reactor through the three-phase separator, the nitrate nitrogen enters the three-dimensional electrode membrane biological reaction area and generates hydrogen by utilizing electrode electrolysis wastewater, an intermediate water inlet denitrification effect of the electron donor and strong oxidizing property is provided, and the nitrate nitrogen in the water body is further removed.
Description
Technical Field
The invention belongs to the field of water pollution control, mainly relates to the field of low-carbon-nitrogen-ratio high-concentration ammonia nitrogen wastewater treatment, and particularly relates to an integrated sectional reactor coupling anaerobic ammonia oxidation and a three-dimensional electrode membrane biological process.
Background
With the continuous development of society, the content of nitrogen in industrial and agricultural wastewater and urban domestic sewage is higher and higher. The discharge of large amounts of nitrogen-containing sewage causes a series of serious environmental problems. For example, serious eutrophication of water body caused by excessive nitrogen and phosphorus causes mass propagation of algae, death of fishes and shrimps and further water ecology pollution. The utilization of a large amount of nitrogen fertilizer in agriculture also seriously pollutes underground water. In the industrial field, urea of printing and dyeing wastewater, ammonia water of electroplating wastewater, nitric acid in the steel industry and the like have certain toxicity, are not beneficial to the growth and development of microorganisms, further threaten the health of human beings through food chain enrichment, and also severely restrict the sustainable development of the society. Various sewages have high nitrogen content and imbalance of C/N ratio under most conditions, and bring about a plurality of difficulties for harmless treatment of the sewages.
In sewage plants, the conventional biological denitrification process uses an activated sludge process or a membrane biological process as a reaction main body, and provides a treatment effect by controlling dissolved oxygen, organic matter concentration, hydraulic retention time and the like. A common process comprises A2O activated sludge process, membrane biological process, oxidation ditch, biological rotating disk and biological fluidized bed, etc. The traditional treatment process needs to have sufficient carbon source in the denitrification section to ensure the integral denitrification effect. Therefore, the wastewater with low carbon-nitrogen ratio brings certain challenges to the traditional biological denitrification process.
The anaerobic ammonia oxidation process completes the denitrification process without an external carbon source, and the reaction principle is shown in the following formula.
It is known that the process is carried out under anaerobic conditions with NH4 +N is an electron donor, NO2 --N is an electron acceptor, NH4 +-N and NO2 --N to N2. Compared with the traditional denitrification process, the process does not need an external carbon source, does not need aeration, has low sludge production and has higher denitrification efficiency. But each 1mol of NH consumed4 +-N and 1.32NO2 -N except for 1.02mol/L N2At the same time, 0.26mol/L NO will remain3 —N。
The three-dimensional electrode biomembrane process is characterized in that a particle or flake-shaped filler is added between an anode and a cathode in the traditional two-dimensional electrode equipment to serve as a third electrode, and under the action of an electric field, the surface of the loaded filler is charged and generates polarization. Meanwhile, a large number of microorganisms are adsorbed on the surfaces of the fillers to form the three-dimensional electrode biofilm reactor. The principle is as follows:
the reaction mainly occurs on the surface of the anode during electrolysis:
C+2H2O→CO2+4H+the
H2O→1/2O2+2H++2e- … … … … … … … … … type (1-3)
The reaction mainly occurs on the cathode surface during electrolysis:
1/2O2+H2o +2e- → 2OH- … … … … … … … … … formula (1-4)
2H2O+2e-→2H2+2OH- … … … … … … … … formula (1-5)
The hydrogen autotrophic denitrification process:
8NO3 -+5CH3COO-→10HCO3-+H2O+4N2+3OH-… … … … type (1-6)
2.5H2+10NO3 -→0.5N2+2H2O + OH- … … … … … … formula (1-7)
From the above, the three-dimensional electrode can generate H by the action of electrolyzed water2And O2In which H is produced at the cathode2Providing an electron donor for the denitrification process of growing the hydrogenotrophic microorganisms attached to the electrode surface and the filler, and adding NO3 -Reduction of-N to N2. Meanwhile, when a carbon rod is used as an anode, the anode generates CO under the action of electrolysis2Can be used as inorganic carbon source for providing energy source for autotrophic microorganisms and producing CO2Dissolving in water to produce CO3 2-And HCO3 -. Can also improve the activity of microorganisms under the action of current and promote the denitrification process.
However, anammox bacteria are environmentally critical, such as: temperature, dissolved oxygen and the like are easily affected by toxic and harmful substances, the sludge form is difficult to maintain granulation, and complete denitrification cannot be realized because nitrate nitrogen is generated by denitrification. The three-dimensional electrode membrane biological process utilizes three-dimensional electrodes under micro-current and hydrogen autotrophic microorganisms to purify sewage, has the advantages of cleanness and no secondary pollution, but is not suitable for treating high-concentration ammonia nitrogen wastewater because the system cannot bear the impact of high-concentration sewage wastewater and can cause the collapse of the system.
Disclosure of Invention
Aiming at the process principle, the invention aims to design a bioreactor which can couple the advantages of an anaerobic ammonia oxidation process and a three-dimensional electrode membrane biological process, reasonably utilizes the advantages and the disadvantages of the anaerobic ammonia oxidation process and the three-dimensional electrode membrane biological process, develops a treatment device which can be used for low-carbon ratio high ammonia nitrogen wastewater, and is an integrated sectional reactor which couples the anaerobic ammonia oxidation process and the three-dimensional electrode membrane biological process. The anaerobic ammonia oxidation reaction zone at the lower part of the shell comprises a porous water distributor, a temperature/dissolved oxygen/oxidation-reduction potential measuring instrument, a three-phase separator, an external reflux system and a gas collecting bag; the three-dimensional electrode membrane biological reaction area at the upper part of the shell comprises a sieve plate flange, a porous water distributor, a cathode, an anode, sponge iron, an activated carbon filling layer and a direct current power supply; sponge iron and an active carbon filling layer are filled between the cathode and the anode to form a three-dimensional electrode structure under the medium of sewage and wastewater. High-concentration ammonia nitrogen is used as an electron donor for denitrification to form nitrogen and nitrate nitrogen, the nitrogen is discharged out of the reactor through the three-phase separator, the nitrate nitrogen enters the three-dimensional electrode membrane biological reaction area and generates hydrogen by using electrode electrolysis wastewater, and the electron donor and a strong-oxidizing intermediate are provided for water inlet denitrification, so that the nitrate nitrogen in the water body is further removed, and the method has the advantages of low energy consumption, high efficiency and simple structure; lays a foundation for the development of a novel high-efficiency denitrification reactor.
The technical scheme of the invention is as follows:
an integrated sectional reactor for coupling anaerobic ammonia oxidation and three-dimensional electrode membrane biological processes is characterized in that an anaerobic ammonia oxidation reaction area at the bottom and a three-dimensional electrode membrane biological reaction area at the top are divided by a sieve plate flange (16) in a reactor shell (41); the anaerobic ammonia oxidation reaction zone multipoint water distributor (20) is arranged at the bottom of the reactor; the bottom side is provided with an opening to connect a digital display screen (17) and a high-sensitivity temperature/dissolved oxygen/oxidation-reduction potential probe (19), and a three-phase separator (5) is arranged at the upper end of the anaerobic ammonia oxidation reaction zone at the bottom and is fixed on the top cover of a shell (41) through a closed rubber plug (8); a three-dimensional electrode membrane biological reaction zone multipoint water distributor (15) and a cathode (14) are arranged at the upper end of a sieve plate flange (16), a sponge iron and activated carbon packing layer (13) is arranged on the cathode (14), and an anode (12) is arranged on the packing layer; the anode (12) and the cathode (14) are connected with a direct current power supply (11) through wires to form a three-dimensional electrode; the water bath water inlet (2) is located the casing (41) lower extreme, and water bath delivery port (10) are located casing (41) upper end, and casing (41) lateral wall sets up the sample connection, is anaerobic ammonia oxidation reaction zone bottom sample connection (31), anaerobic ammonia oxidation reaction zone top sample connection (32), three-dimensional electrode membrane biological reaction zone bottom sample connection (33), three-dimensional electrode membrane biological reaction zone top sample connection (34) respectively.
The reflux water outlet (6) and the reflux water inlet (23) of the reactor are respectively arranged at the upper end and the lower end of the reactor, and an integral peristaltic pump (1-1) is arranged between the reflux water outlet (6) and the reflux water inlet (23); an anaerobic ammonia oxidation reaction zone peristaltic pump (1-2) is arranged between an anaerobic ammonia oxidation reaction zone bottom sampling port (31) and an anaerobic ammonia oxidation reaction zone top sampling port (32); a peristaltic pump (1-3) of the three-dimensional electrode membrane biological reaction area is arranged between a sampling port (33) at the bottom of the three-dimensional electrode membrane biological reaction area and a sampling port (34) at the top of the three-dimensional electrode membrane biological reaction area; a water distribution pipe and four same three-way valves (24) are used for connecting a bottom sampling port (31) of an anaerobic ammonia oxidation reaction zone, a top sampling port (32) of the anaerobic ammonia oxidation reaction zone, a bottom sampling port (33) of a three-dimensional electrode membrane biological reaction zone, a top sampling port (34) of the three-dimensional electrode membrane biological reaction zone, a return water outlet (6) and a return water inlet (23); the water inlet pump (21) of the water inlet barrel (18) is connected with the water inlet (22) at the bottom of the shell (41) by the water distribution pipe; a water bath heat-insulating layer (42) is arranged outside the shell (41).
The circulating systems of the reactor are respectively an integral external circulating system, an anaerobic ammonia-oxygen reaction section external circulating system and a three-dimensional electrode membrane biological reaction section external circulating system; the integral external circulation system enables the integral peristaltic pump (1-1), the backflow water outlet (6) and the backflow water inlet (23) to form a circulation by adjusting the four three-way valves (24); the anaerobic ammonia oxygen section external circulation system enables the anaerobic ammonia oxidation reaction zone peristaltic pump (1-2), the anaerobic ammonia oxidation reaction zone top sampling port (32) and the anaerobic ammonia oxidation reaction zone bottom sampling port (31) to form a circulation by adjusting four three-way valves; the external circulation system of the three-dimensional electrode film biological reaction section enables a peristaltic pump (1-3) of a three-dimensional electrode film biological reaction area, a top sampling port (34) of the three-dimensional electrode film biological reaction area and a bottom sampling port (33) of the three-dimensional electrode film biological reaction area to form a circulation by adjusting four three-way valves.
The reactor three-phase separator (5) forms a solid-liquid-gas separation system, and the three-phase separator (5) is positioned at the top of the anaerobic ammonia oxidation reaction zone; the air duct extends through the three-dimensional electrode membrane biological reaction area and is fixed through a sealed rubber plug (8) positioned at the top of the shell (41), gas is collected through a gas collecting bag (7), liquid is discharged through a return water outlet (6) and a water outlet (9), and sludge is retained and stored in the anaerobic ammonia oxidation reaction area by a three-phase separator (5).
The reactor comprises a heating and heat-insulating system consisting of a shell (41), a water bath heat-insulating layer (42), a water bath water inlet (2) and a water bath water outlet (10), and the temperature of the system is maintained in a water bath circulation heating mode.
Preferably, the volume ratio of the anaerobic ammonia oxidation reaction zone at the bottom of the reactor to the three-dimensional electrode membrane biological reaction zone at the top of the reactor is 1:1.
Preferably, the aperture of the reactor sieve plate flange (16) is set to intercept the microorganism of the three-dimensional electrode membrane biological reaction zone falling from the surface of the packed layer into the anaerobic ammonia oxidation reaction zone at the bottom.
Preferably, the reactor height to diameter ratio is 30.
Compared with the prior art, the invention has the following beneficial effects:
the invention effectively utilizes the three-dimensional electrode membrane biological reaction area to treat the nitrate nitrogen generated by denitrification of the anaerobic ammonia oxidation reaction section, and improves the integral denitrification efficiency of the wastewater with low carbon-nitrogen ratio through the interaction of anaerobic ammonia oxidation bacteria, hydrogen autotrophic microorganisms and the three-dimensional electrode.
The invention can monitor the temperature, dissolved oxygen and oxidation-reduction potential of the anaerobic ammonia oxidation reaction zone in real time and adjust the operation parameters in time.
The invention is provided with the integral external circulation system, which can reduce pollution load, improve hydraulic shearing force, is beneficial to the formation of anaerobic ammonia oxidation granular sludge, and can independently select the circulation system of the anaerobic ammonia oxidation reaction section and the circulation system of the three-dimensional electrode membrane biological reaction section according to the water quality condition of effluent, thereby further improving the denitrification capability of the reactor.
The invention selects a high-purity mesoporous graphite carbon plate as an anode material, and CO can be generated by electrolysis2Inorganic carbon sources can be provided for the autotrophic microorganisms, and water solubility also contributes to the pH of the system.
The invention selects a high-purity mesoporous graphite carbon plate as a cathode material, and H can be generated by electrolysis2NO can be supplied to the hydrogen autotrophic microorganisms as an electron donor3 -Reduction of-N to N2。
The invention fills active carbon and graphite filler between the cathode and the anode, the filler is electrified and polarized to form a third dimension electrode, and the third dimension electrode can also be used as a carrier of autotrophic microorganisms.
Drawings
FIG. 1 is a block diagram of the present invention
FIG. 2 is a diagram showing the change of inlet and outlet water quality and stoichiometric ratio during the start-up process
FIG. 3 is a graph comparing the denitrification rates of the UASB reactor of the present invention and a conventional UASB reactor
Wherein: the device comprises an integral peristaltic pump (1-1), an anaerobic ammonia oxidation reaction zone peristaltic pump (1-2), a three-dimensional electrode membrane biological reaction zone peristaltic pump (1-3), a water bath water inlet (2), an anaerobic ammonia oxidation reaction zone bottom sampling port (31), an anaerobic ammonia oxidation reaction zone top sampling port (32), a three-dimensional electrode membrane biological reaction zone bottom sampling port (33), a three-dimensional electrode membrane biological reaction zone top sampling port (34), a shell (41), a water bath heat preservation layer (42), a three-phase separator (5), a backflow water outlet (6), a gas collection bag (7), a closed rubber plug (8), a water outlet (9), a water bath water outlet (10), a direct current power supply (11), an anode (12), iron carbon and active carbon fillers (13), a cathode (14), a three-dimensional electrode membrane biological reaction zone multi-point water distributor (15), a sieve plate (16), The device comprises a digital display screen (17), a water inlet barrel (18), a high-sensitivity temperature/dissolved oxygen/oxidation-reduction potential probe (19), an anaerobic ammonia oxidation reaction zone multipoint water distributor (20), a water inlet pump (21), a water inlet (22), a backflow water inlet (23) and four three-way valves (24).
Detailed Description
The schematic diagram of the test device is shown in FIG. 1, and the embodiment of the invention is explained by combining FIG. 1:
the invention provides an integrated sectional reactor for coupling anaerobic ammonia oxidation and three-dimensional electrode membrane biological processes, which comprises an integral peristaltic pump (1-1), an anaerobic ammonia oxidation reaction region peristaltic pump (1-2), a three-dimensional electrode membrane biological reaction region peristaltic pump (1-3), a water bath water inlet (2), an anaerobic ammonia oxidation reaction region bottom sampling port (31), an anaerobic ammonia oxidation reaction region top sampling port (32), a three-dimensional electrode membrane biological reaction region bottom sampling port (33), a three-dimensional electrode membrane biological reaction region top sampling port (34), a shell (41), a water bath heat-insulating layer (42), a three-phase separator (5), a backflow water outlet (6), a gas collection bag (7), a closed rubber plug (8), a water outlet (9), a water bath water outlet (10), a direct current power supply (11), an anode (12), iron carbon and activated carbon fillers (13), The device comprises a cathode (14), a three-dimensional electrode membrane biological reaction zone multipoint water distributor (15), a sieve plate flange (16), a digital display screen (17), a water inlet barrel (18), a high-sensitivity temperature/dissolved oxygen/oxidation-reduction potential probe (19), an anaerobic ammonia oxidation reaction zone multipoint water distributor (20), a water inlet pump (21), a water inlet (22), a backflow water inlet (23) and four three-way valves (24); the reactor is divided into an anaerobic ammonia oxidation reaction zone at the bottom and a three-dimensional electrode membrane biological reaction zone at the top by a sieve plate flange (16); a bottom anaerobic ammonia oxidation reaction zone: the water inlet pump (21) of the water inlet barrel (18) is connected with the water inlet (22) at the bottom of the shell (41) through a water distribution pipe, and the multipoint water distributor (20) of the anaerobic ammonia oxidation reaction zone is adhered to the bottom of the reactor. The bottom side is provided with an opening to connect a digital display screen (17) and a high-sensitivity temperature/dissolved oxygen/oxidation-reduction potential probe (19), and a three-phase separator (5) is arranged at the upper end of the anaerobic ammonia oxidation reaction zone at the bottom and is fixed on the top cover of a shell (41) through a closed rubber plug (8); top three-dimensional electrode membrane bioreaction zone: a three-dimensional electrode membrane biological reaction zone multipoint water distributor (15) and a cathode (14) are arranged at the upper end of a sieve plate flange (16), sponge iron and activated carbon (13) filler are added above the cathode (14), and an anode (12) is arranged at the upper end of the filler; the anode (12) and the cathode (14) are connected with a direct current power supply (11) through wires to form a three-dimensional electrode; the effluent water flows out through the water outlet (9) under the action of gravity. The surface of the shell (41) is covered with a water bath heat preservation layer (42), a water bath water inlet (2) is positioned at the lower end of the shell (41), a water bath water outlet (10) is positioned at the upper end of the shell (41), and the side wall of the shell (41) is provided with sampling ports which are respectively an anaerobic ammonia oxidation reaction zone bottom sampling port (31), an anaerobic ammonia oxidation reaction zone top sampling port (32), a three-dimensional electrode membrane biological reaction zone bottom sampling port (33) and a three-dimensional electrode membrane biological reaction zone top sampling port (34); the anaerobic ammonia oxidation reaction zone bottom sampling port (31) is positioned at the bottom end of the anaerobic ammonia oxidation zone, the anaerobic ammonia oxidation reaction zone top sampling port (32) is positioned at the upper end of the anaerobic ammonia oxidation zone, the third sampling port (33) is positioned at the bottom end of the three-dimensional electrode membrane biological reaction zone, and the three-dimensional electrode membrane biological reaction zone top sampling port (34) is positioned at the upper end of the three-dimensional electrode membrane biological reaction zone; the return water outlet (6) and the return water inlet (23) are respectively arranged at the upper end and the lower end of the right side of the reactor. A water distribution pipe and four same three-way valves (24) are used for connecting a bottom sampling port (31) of an anaerobic ammonia oxidation reaction zone, a top sampling port (32) of the anaerobic ammonia oxidation reaction zone, a bottom sampling port (33) of a three-dimensional electrode membrane biological reaction zone, a top sampling port (34) of the three-dimensional electrode membrane biological reaction zone, a return water outlet (6) and a return water inlet (23); the integral peristaltic pump (1-1) is connected between the backflow water outlet (6) and the backflow water inlet (23); the anaerobic ammonia oxidation reaction zone peristaltic pump (1-2) is connected between a sampling port (31) at the bottom of the anaerobic ammonia oxidation reaction zone and a sampling port (32) at the top of the anaerobic ammonia oxidation reaction zone; the peristaltic pump (1-3) of the three-dimensional electrode film biological reaction area is connected between a sampling port (33) at the bottom of the three-dimensional electrode film biological reaction area and a sampling port (34) at the top of the three-dimensional electrode film biological reaction area.
The reactor circulating system comprises an integral external circulating system, an anaerobic ammonia-oxygen reaction section external circulating system and a three-dimensional electrode membrane biological reaction section external circulating system; the integral external circulation system enables the integral peristaltic pump (1-1), the backflow water outlet (6) and the backflow water inlet (23) to form a circulation by adjusting the four three-way valves; the anaerobic ammonia oxygen section external circulation system enables the anaerobic ammonia oxidation reaction zone peristaltic pump (1-2), the anaerobic ammonia oxidation reaction zone top sampling port (32) and the anaerobic ammonia oxidation reaction zone bottom sampling port (31) to form a circulation by adjusting four three-way valves; the external circulation system of the three-dimensional electrode membrane biological reaction section enables a peristaltic pump (1-3) of a three-dimensional electrode membrane biological reaction area, a top sampling port (34) of the three-dimensional electrode membrane biological reaction area and a bottom sampling port (33) of the three-dimensional electrode membrane biological reaction area to form a circulation by adjusting four three-way valves;
the solid-liquid-gas separation system consists of a three-phase separator (5) which is positioned at the top of the anaerobic ammonia oxidation reaction zone; the air duct extends through the three-dimensional electrode membrane biological reaction area and is fixed through a sealed rubber plug (8) positioned at the top of the shell (41), gas is collected through a gas collecting bag (7), liquid is discharged through a return water outlet (6) and a water outlet (9), and sludge is retained and stored in the anaerobic ammonia oxidation reaction area by a three-phase separator (5).
The online monitoring system consists of a digital display screen (17) and a high-sensitivity temperature/dissolved oxygen/oxidation-reduction potential probe (19), wherein the probe is arranged in the bottom area of the anaerobic ammonia oxidation reaction zone of the shell (41);
the three-dimensional electrode membrane biological reaction area consists of a direct-current power supply (11), an anode (12), iron carbon and activated carbon fillers (13), a cathode (14), a three-dimensional electrode membrane biological reaction area multipoint water distributor (15) and a sieve plate flange (16); the sieve plate flange (16) is positioned in the middle of the reactor; a multipoint water distributor (15) of the three-dimensional electrode membrane biological reaction area is arranged at the upper end of a sieve plate flange (16); a cathode (14) is arranged at the upper end of the multi-point water distributor (15) of the three-dimensional electrode membrane biological reaction area; filling iron carbon and activated carbon (13) in the cathode (14) and inoculating anaerobic microorganisms; placing an anode (12) on the upper end of the filler; the anode (12) and the cathode (14) are connected with a direct current power supply (11) through wires to form a three-dimensional electrode.
The heating and heat-insulating system consists of a shell (41), a water bath heat-insulating layer (42), a water bath water inlet (2) and a water bath water outlet (10). The temperature of the system is maintained at about 35 ℃ by circularly heating the water bath.
The sewage and wastewater is stored in a water inlet barrel (17), pumped into the reactor through a water inlet pump (20) and a water inlet (21), and discharged out of the reactor through the action of gravity at a water outlet (9);
the volume ratio of the anaerobic ammonia oxidation reaction zone at the bottom of the reactor to the three-dimensional electrode membrane biological reaction zone at the top of the reactor is maintained at 1: 1; the aperture of the sieve plate flange (16) is 2mm, and the sieve plate flange is used for intercepting microorganisms in the three-dimensional electrode membrane biological reaction area, and the microorganisms fall off from the surface of the filling layer and enter the anaerobic ammonia oxidation reaction area at the bottom. According to the following steps of 1:1, inoculating anaerobic ammonium oxidation microorganisms and anaerobic granular sludge, and domesticating to form an anaerobic ammonium oxidation reaction area; activated carbon (with the particle size of 4-6 mm) and sponge iron (with the particle size of 6-8 mm) are selected as particle fillers according to the proportion of 8:1, and the particle fillers are attached to the growth biological membrane.
The total effective volume of the reactor is 10L, and the height-diameter ratio is 30; the effective volume of the anaerobic ammonia oxidation reaction section is 5L; the effective volume of the three-dimensional electrode membrane biological reaction area is 5L.
The three-dimensional electrode membrane biological reaction area selects a cylindrical middle-hole-shaped high-purity graphite plate as a cathode material and an anode material.
The following example operations were carried out using the preferred conditions described above:
firstly, a water inlet pump (21) and a water inlet (22) are opened to pump the sewage and wastewater in a water bucket (18) into a reactor, the rotating speed of the water inlet pump (21) is adjusted to set the water inlet flow, and the sewage and wastewater uniformly enter an anaerobic ammonia oxidation reaction zone through a multipoint water distributor (20) of the anaerobic ammonia oxidation reaction zone;
secondly, starting a digital display screen (17) and a high-sensitivity temperature/dissolved oxygen/oxidation reduction potential probe (19) to monitor the physical and chemical indexes of the anaerobic ammonia oxidation reaction area on line, and regulating and controlling the operation parameters of the reactor through monitoring feedback;
and thirdly, collecting effluent of the anaerobic ammonia oxidation reaction section at a sampling port (32) at the top of the anaerobic ammonia oxidation reaction zone, and monitoring the quality of the effluent. Gas generated in the anaerobic ammonia oxidation reaction zone is separated by a three-phase separator (5), is collected by a gas collecting bag (7), and is detected by gas chromatography;
fourthly, the effluent of the anaerobic ammonia oxidation reaction zone uniformly enters a three-dimensional electrode membrane biological reaction section through a multi-point water distributor (15) of the three-dimensional electrode membrane biological reaction zone;
(V) the anode (12) and the cathode (14) are connected with a direct current power supply (11) through wires and form a three-dimensional electrode with the packing layer under the action of water to realize the hydrogen autotrophic denitrification reaction;
and (VI) collecting effluent of the three-dimensional electrode membrane biological reaction section at a sampling port (34) at the top of the three-dimensional electrode membrane biological reaction area, and monitoring the quality of the effluent. (ii) a
Collecting the effluent of the integral reactor at a water outlet (10), and monitoring the quality of the effluent;
(eighth) refluxing operation: the anaerobic ammonia oxidation reaction section and the three-dimensional electrode membrane biological reaction section are both provided with independent reflux systems, and reflux regulation and control are respectively carried out according to the conditions of the two sections of effluent water quality:
and (3) cyclic operation of an anaerobic ammonia oxidation reaction section: under the condition that the content of ammonia nitrogen and nitrite nitrogen in the effluent of the anaerobic ammonia oxidation reaction section exceeds 5mg/L, adjusting a three-way valve (24), and connecting a peristaltic pump (1-2) of the anaerobic ammonia oxidation reaction section, a top sampling port (32) of the anaerobic ammonia oxidation reaction section and a bottom sampling port (31) of the anaerobic ammonia oxidation reaction section through a water distribution pipe to form a circulation system, so that the content of ammonia nitrogen and nitrite nitrogen in the effluent of the anaerobic ammonia oxidation reaction section is kept to be not more than 5 mg/L.
And (3) cyclic operation of the three-dimensional electrode membrane biological reaction section: under the condition that the nitrate nitrogen content of the effluent of the three-dimensional electrode membrane biological reaction section exceeds 5mg/L, a three-way valve (24) is adjusted, and a peristaltic pump (1-3) of the three-dimensional electrode membrane biological reaction region, a top sampling port (34) of the three-dimensional electrode membrane biological reaction region and a bottom sampling port (33) of the three-dimensional electrode membrane biological reaction region are connected through a water distribution pipe to form a circulation system, so that the nitrate nitrogen content of the effluent of the three-dimensional electrode membrane biological reaction section is kept to be not more than 5 mg/L.
Integral external circulation operation: under the condition that the total nitrogen content of the effluent of the reactor exceeds 15mg/L, adjusting a three-way valve (24), and connecting an integral peristaltic pump (1-1), a backflow water outlet (6) and a backflow water inlet (23) through a water distribution pipe to form a cycle, so that the total nitrogen content of the effluent of the reactor is kept not to exceed 15 mg/L;
example 1:
the sludge at the bottom of the early reactor is taken from the acclimatized anaerobic ammonia oxidation sludge in a laboratory and the anaerobic section sludge taken from a sewage plant, and the sludge and the anaerobic section sludge are mixed by the weight ratio of 1:1 by volume. The mixed sludge MLSS is 12.57g/L, the MLVSS is 4.75g/L, the MLVSS/MLSS is 37.78%, the inoculation volume is 2.5L, and the inoculation volume occupies 25% of the effective volume. The upper inoculation sewage plant obtains sludge in an anaerobic section, and the basic indexes are as follows: MLSS was 26.5g/L, MLVSS 17.69 g/L. In order to successfully activate an anaerobic ammonia oxidation system and an autotrophic denitrification system in a reactor, a starting culture method with low matrix and high flow rate is adopted at the early stage. Feed water NH4 +N load, increasing through five concentration gradients of 50, 60, 70, 80, 90, 100mg/L, NO2 -N, HRT was gradually reduced over five stages of 24, 20, 16, 12, 6h via five increases in concentration gradients 66, 79.2, 92.4, 105.6, 118.8, 132 mg/L. The other components are as follows: other components include NaHCO3 1250mg/L，MgSO4·7H2O 300mg/L，KH2PO4 10mg/L，CaCl25.6 mg/L. 1mL/L of trace element I and 1mL/L of trace element II. And trace elements I: EDTA 5000mg/L, FeSO4·7H2O5000 mg/L. And (4) trace element II: EDTA 5000mg/L, MnCl2·4H2O 990mg/L，CuSO4·5H2O 250mg/L，ZnSO4·7H2O 430mg/L，CoCl2·6H2O 240mg/L，Na2MoO4·2H2O 220mg/L，NiCl2·6H2O 190mg/L，H3BO4 14mg/L。
In the starting phase, the whole external circulation system is started: the peristaltic pump (1), the return water outlet (6) and the return water inlet (23) are opened and connected through the water distribution pipe to form a circulation. And adjusting the operation parameters in time according to the data fed back by the online monitoring system. During the 60 day start-up phase, the substrate concentration was increased from stage one to stage five, the ammonia nitrogen removal was reduced from 99.53% to 92.1%, and the nitrous nitrogen removal was reduced from 99.64% to 94.01%, achieving a steady nitrogen removal (fig. 2). And Rs is higher than 1.32 and Rp is lower than 0.26 during the whole starting period, so that an anaerobic ammonia oxidation system and autotrophic denitrification effect can be proved to occur in the system (figure 2).
Example 2
After the start is finished, the mass concentration ratio of the ammonia nitrogen to the nitrite nitrogen is maintained at 1:1.32, the inlet water concentration is 100mg/L ammonia nitrogen, 132mg/L nitrite nitrogen and other nutrient elements are maintained unchanged. While another conventional UASB reactor is operated. The two reactors have the same operating conditions except for the difference in configuration. The difference of the total nitrogen of the effluent is shown in fig. 3, which shows that the two-stage bioreactor coupling the anaerobic ammonia oxidation and the three-dimensional electrode is more stable, the total nitrogen removal rate is 88% higher than the maximum nitrogen removal rate of the anaerobic ammonia oxidation theory, and the existence of the autotrophic denitrification process can be assisted and confirmed (fig. 3).
Example 3
After the start is finished, the mass concentration ratio of the ammonia nitrogen to the nitrite nitrogen is maintained at 1:1.32, the inlet water concentration is 100mg/L ammonia nitrogen, 132mg/L nitrite nitrogen and other nutrient elements are maintained unchanged, 30mg/L nitrate nitrogen is added into the inlet water, an external circulation system of the three-dimensional electrode membrane biological reaction zone is opened, a peristaltic pump of the three-dimensional electrode membrane biological reaction zone is set at 1rpm/min, and the nitrate nitrogen content of the outlet water of the three-dimensional electrode membrane biological reaction zone is successfully reduced to 5 mg/L. And then increasing the ammonia nitrogen concentration of the inlet water to 120mg/L, and opening an external circulation system of the anaerobic ammonia oxidation section to successfully realize that the ammonia nitrogen content of the outlet water of the anaerobic ammonia oxidation reaction zone is lower than 5 mg/L. And then continuously increasing the concentration of nitrite nitrogen to 159mg/L (the concentration of inlet ammonia nitrogen is 120mg/L, the concentration of nitrite nitrogen is 159mg/L and the concentration of nitrate nitrogen is 30mg/L), closing an external circulation system of the three-dimensional electrode membrane biological reaction area and an external circulation system of the anaerobic ammonia oxidation section, opening the whole external circulation system, and successfully realizing that the total nitrogen of outlet water of the reactor is lower than 15 mg/L.
While the methods and techniques of the present invention have been described in terms of preferred embodiments, it will be apparent to those of ordinary skill in the art that variations and/or modifications of the methods and techniques described herein may be made without departing from the spirit and scope of the invention. It is expressly intended that all such similar substitutes and modifications apparent to those skilled in the art are deemed to be within the spirit, scope and content of the invention. The invention belongs to the known technology.
Claims (8)
1. An integrated sectional reactor for coupling anaerobic ammonia oxidation and three-dimensional electrode membrane biological processes is characterized in that a reactor shell (41) is divided into an anaerobic ammonia oxidation reaction area at the bottom and a three-dimensional electrode membrane biological reaction area at the top by a sieve plate flange (16); the anaerobic ammonia oxidation reaction zone multipoint water distributor (20) is arranged at the bottom of the reactor; the bottom side is provided with an opening to connect a digital display screen (17) and a high-sensitivity temperature/dissolved oxygen/oxidation-reduction potential probe (19), and a three-phase separator (5) is arranged at the upper end of the anaerobic ammonia oxidation reaction zone at the bottom and is fixed on the top cover of a shell (41) through a closed rubber plug (8); a three-dimensional electrode membrane biological reaction zone multipoint water distributor (15) and a cathode (14) are arranged at the upper end of a sieve plate flange (16), a sponge iron and activated carbon packing layer (13) is arranged on the cathode (14), and an anode (12) is arranged on the packing layer; the anode (12) and the cathode (14) are connected with a direct current power supply (11) through wires to form a three-dimensional electrode; the water bath water inlet (2) is located the casing (41) lower extreme, and water bath delivery port (10) are located casing (41) upper end, and casing (41) lateral wall sets up the sample connection, is anaerobic ammonia oxidation reaction zone bottom sample connection (31), anaerobic ammonia oxidation reaction zone top sample connection (32), three-dimensional electrode membrane biological reaction zone bottom sample connection (33), three-dimensional electrode membrane biological reaction zone top sample connection (34) respectively.
2. A reactor according to claim 1, characterized in that the return water outlet (6) and the return water inlet (23) are arranged at the upper end and the lower end of the reactor, respectively, and an integral peristaltic pump (1-1) is arranged between the return water outlet (6) and the return water inlet (23); an anaerobic ammonia oxidation reaction zone peristaltic pump (1-2) is arranged between an anaerobic ammonia oxidation reaction zone bottom sampling port (31) and an anaerobic ammonia oxidation reaction zone top sampling port (32); a peristaltic pump (1-3) of the three-dimensional electrode membrane biological reaction area is arranged between a sampling port (33) at the bottom of the three-dimensional electrode membrane biological reaction area and a sampling port (34) at the top of the three-dimensional electrode membrane biological reaction area; a water distribution pipe and four same three-way valves (24) are used for connecting a bottom sampling port (31) of an anaerobic ammonia oxidation reaction zone, a top sampling port (32) of the anaerobic ammonia oxidation reaction zone, a bottom sampling port (33) of a three-dimensional electrode membrane biological reaction zone, a top sampling port (34) of the three-dimensional electrode membrane biological reaction zone, a return water outlet (6) and a return water inlet (23); the water inlet pump (21) of the water inlet barrel (18) is connected with the water inlet (22) at the bottom of the shell (41) by the water distribution pipe; a water bath heat-insulating layer (42) is arranged outside the shell (41).
3. The reactor as set forth in claim 1 or 2, wherein the circulating systems of the reactor are an integral external circulating system, an anaerobic ammonia-oxygen reaction section external circulating system, and a three-dimensional electrode membrane biological reaction section external circulating system, respectively; the integral external circulation system enables the integral peristaltic pump (1-1), the backflow water outlet (6) and the backflow water inlet (23) to form a circulation by adjusting the four three-way valves (24); the anaerobic ammonia oxygen section external circulation system enables the anaerobic ammonia oxidation reaction zone peristaltic pump (1-2), the anaerobic ammonia oxidation reaction zone top sampling port (32) and the anaerobic ammonia oxidation reaction zone bottom sampling port (31) to form a circulation by adjusting four three-way valves; the external circulation system of the three-dimensional electrode film biological reaction section enables a peristaltic pump (1-3) of a three-dimensional electrode film biological reaction area, a top sampling port (34) of the three-dimensional electrode film biological reaction area and a bottom sampling port (33) of the three-dimensional electrode film biological reaction area to form a circulation by adjusting four three-way valves.
4. A reactor according to claim 1, characterized in that the three-phase separator (5) constitutes a solid-liquid-gas separation system, the three-phase separator (5) being located at the top of the anammox reaction zone; the air duct extends through the three-dimensional electrode membrane biological reaction area and is fixed through a sealed rubber plug (8) positioned at the top of the shell (41), gas is collected through a gas collecting bag (7), liquid is discharged through a return water outlet (6) and a water outlet (9), and sludge is retained and stored in the anaerobic ammonia oxidation reaction area by a three-phase separator (5).
5. The reactor of claim 1, wherein the heating and heat-insulating system is composed of a shell (41), a water bath heat-insulating layer (42), a water bath water inlet (2) and a water bath water outlet (10), and the temperature of the system is maintained by circularly heating the water bath.
6. The reactor of claim 1, wherein the volume ratio of the bottom anammox reaction zone to the top three-dimensional electrode membrane bioreactor zone is 1:1.
7. A reactor according to claim 1, wherein the screen flange (16) is apertured to retain microorganisms in the three-dimensional electrode membrane bioreactor zone from shedding from the surface of the packed bed into the bottom anammox reactor zone.
8. The reactor of claim 1 wherein the reactor height to diameter ratio is 30.
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