CN112062271B - Bio-electrochemical reaction device and method for denitrifying anaerobic methane oxidation film - Google Patents
Bio-electrochemical reaction device and method for denitrifying anaerobic methane oxidation film Download PDFInfo
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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
- C02F3/2853—Anaerobic digestion processes using anaerobic membrane bioreactors
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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
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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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- 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
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
- C02F2101/163—Nitrates
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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
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/32—Hydrocarbons, e.g. oil
Abstract
The invention discloses a denitrification anaerobic methane oxidation film bioelectrochemical reaction device and a method thereof, wherein the device comprises a closed cylinder, and a cathode and an anode which are positioned in the inner cavity of the cylinder, wherein the cathode and the anode are respectively communicated with the cathode and the anode of an external power supply through leads; the anode comprises a titanium mesh, granular activated carbon and an MBR (membrane bioreactor) membrane component, and the titanium mesh wraps the granular activated carbon on the surface of the MBR membrane component; the surfaces of the granular activated carbon and the MBR membrane component are used for enriching denitrifying anaerobic methane oxidation microorganisms; the cathode is a carbon felt with the surface used for enriching autotrophic denitrifying microorganisms; the inner cavity of the cylinder body below the anode and the cathode is provided with water distribution pipes with uniform holes, and a gas distributor is arranged below the water distribution pipes. The invention realizes the cooperative removal of nitrate and methane in the wastewater treatment process by coupling the bioelectrochemical system, the membrane component and the denitrification anaerobic methane oxidation microorganism, and has the characteristics of high efficiency, low cost, low energy consumption and small space.
Description
Technical Field
The invention belongs to the field of biological treatment of wastewater, and particularly relates to a denitrification anaerobic methane oxidation film bioelectrochemical reaction device and a method thereof.
Background
The traditional nitrification-denitrification process for biological denitrification of wastewater has the condition of insufficient electron donor in a denitrification section, so that the denitrification efficiency is restricted, and simultaneously, a large amount of methane generated in an anaerobic digestion section is dissolved in water and finally discharged along with wastewater and released into the atmosphere, so that the nitrification-denitrification process is one of the main reasons of global greenhouse effect and is also a waste of resources.
Disclosure of Invention
The invention provides a denitrification anaerobic methane oxidation film bioelectrochemical reaction device and a method thereof, aiming at the problems that the denitrification process is not thorough and the generated methane is discharged out of order in the urban wastewater treatment.
The technical scheme adopted by the invention is as follows:
a denitrification anaerobic methane oxidation film bioelectrochemical reaction device comprises a closed cylinder, a cathode and an anode which are positioned in the inner cavity of the cylinder, wherein the cathode and the anode are respectively communicated with the cathode and the anode of an external power supply through leads;
the anode comprises a titanium mesh, granular activated carbon and an MBR (membrane bioreactor) membrane component, and the titanium mesh wraps the granular activated carbon on the surface of the MBR membrane component; the surfaces of the granular activated carbon and the MBR membrane component are used for enriching denitrifying anaerobic methane oxidation microorganisms, the titanium mesh is externally connected with titanium wires and communicated with the conducting wire, and the water outlet end of the MBR membrane component is communicated with the outside through a water outlet pipe provided with a water outlet pump; the cathode is a carbon felt with the surface used for enriching autotrophic denitrifying microorganisms;
water distribution pipes with uniform holes are arranged in the inner cavity of the cylinder body below the anode and the cathode, and a gas distributor is arranged below the water distribution pipes; the gas inlet end of the gas distributor is communicated with the outside and is used for blowing gas to the anode to ensure that the granular activated carbon realizes a fluidized state; the side wall of the upper part of the cylinder body is provided with a gas outlet which is communicated with the gas inlet end of the gas distributor through a gas pipeline provided with a circulating pump.
Preferably, the aperture ratio of the water distribution pipe is 10%, and a water inlet pump is arranged on the water distribution pipe positioned outside the barrel.
Preferably, the gas distributor is a disc distributor, and an aeration pump is arranged at the air inlet end of the gas distributor, which is positioned outside the cylinder body.
Preferably, a sampling opening is formed in the side wall of the cylinder body close to the anode.
Preferably, the mesh opening of the titanium mesh is a diamond mesh opening, and the length of the short diagonal line of the diamond mesh opening is 1 mm.
Preferably, the material of the MBR membrane module is polyvinylidene fluoride (PVDF).
Preferably, the wire is sequentially connected with a voltage sensor and an alarm in series and is connected with a resistor with the size of 500-1000 omega in parallel so as to monitor the voltage state of the reaction device in real time.
Preferably, the granular activated carbon is spherical granules with the average grain diameter of 2 mm; the filling degree of the granular activated carbon on the surface of the MBR membrane module is 20%.
Another object of the present invention is to provide a method for treating nitrate wastewater and methane waste gas according to any one of the above reaction devices, which comprises the following steps:
starting a water inlet pump, introducing the nitrate wastewater into the inner cavity of the barrel through the water distribution pipe and realizing uniform distribution; simultaneously starting an aeration pump, introducing the methane waste gas into the inner cavity of the cylinder through the gas distributor, and enabling the methane waste gas to be fully contacted with the wastewater, wherein the methane gas is dissolved in the wastewater;
turning off the aeration pump and turning on the circulating pump; methane gas which is not dissolved in the wastewater at the top of the inner cavity of the cylinder body is sucked to the gas inlet end of the gas distributor again under the action of the circulating pump, so that the methane gas is recycled; the flow rate of methane gas is adjusted by controlling a circulating pump, so that the granular activated carbon is fluidized;
nitrate in the wastewater and methane dissolved in the wastewater are enriched on the granular activated carbon and denitrifying anaerobic methane oxidizing microorganisms on the surface of the MBR membrane component and synchronously converted into nitrogen and carbon dioxide, and meanwhile, generated electrons are transferred to the granular activated carbon, so that the activity of the denitrifying anaerobic methane oxidizing microorganisms is improved by utilizing the promotion effect of bioelectrochemistry; the generated electrons are transmitted to the titanium net from the granular activated carbon through the mutual collision action of the granular activated carbon and the titanium net and then transmitted to the carbon felt through the external titanium wire through the lead; the autotrophic denitrification microorganisms enriched on the surface of the carbon felt further reduce the nitrate in the water into nitrogen by utilizing electrons;
monitoring the voltage state of the reaction device in real time through a voltage sensor arranged on a lead; an alarm in series with the voltage sensor sounds an alarm when the voltage deviates from a predetermined value.
Preferably, the waste water introduced into the cylinder occupies 3/4 of the volume of the inner cavity of the cylinder.
Compared with the prior art, the invention has the following beneficial effects:
1) in the reaction device, the cooperative removal of nitrate and methane in the wastewater treatment process is realized through the coupling of the bioelectrochemical system, the membrane component and the denitrification anaerobic methane oxidation microorganism;
2) the reaction device converts the nitrate type wastewater and redundant methane generated in the wastewater treatment into nitrogen and carbon dioxide, thereby realizing the effect of synchronous denitrification and carbon removal in the wastewater treatment;
3) the reaction device has the characteristics of high efficiency, low cost, low energy consumption and small space.
Drawings
FIG. 1 is a schematic view of the structure of a reaction apparatus according to the present invention;
in the figure: the device comprises a water outlet pump 1, a gas outlet 2, a sampling port 3, a circulating pump 4, a water inlet pump 5, a water inlet 6, a water distribution pipe 7, a gas distributor 8, a gas inlet 9, an aeration pump 10, granular activated carbon 11, an MBR (membrane bioreactor) membrane component 12, a titanium net 13, titanium wires 14, a voltage sensor 15, a resistor 16, an alarm 17, a lead 18, a carbon felt 19, an anode area 20 and a cathode area 21.
Detailed Description
The invention will be further elucidated and described with reference to the drawings and the detailed description. The technical features of the embodiments of the present invention can be combined correspondingly without mutual conflict.
As shown in figure 1, the invention relates to a denitrification anaerobic methane oxidation film bioelectrochemical reaction device, which comprises a closed cylindrical barrel, an anode area 20 and a cathode area 21 which are positioned in the inner cavity of the barrel. According to the invention, through process optimization, nitrate in the wastewater and methane generated in wastewater treatment can be cooperatively treated by the nitrification anaerobic methane oxidation microorganisms and the autotrophic denitrification microorganisms. The specific implementation of each structure is described in detail below:
the main body of the anode region 20 is an anode, the anode includes a titanium mesh 13, granular activated carbon 11 and an MBR membrane module 12, and the titanium mesh 13 wraps the granular activated carbon 11 on the surface of the MBR membrane module 12. It should be noted that the coating state is not to tightly coat the granular activated carbon 11 on the surface of the MBR membrane module 12, but only to perform a limiting function, that is, there is a certain space between the granular activated carbon 11 and the surface of the MBR membrane module 12, and the granular activated carbon 11 can move in the space to achieve a fluidized state. The filling degree of the granular activated carbon 11 on the surface of the MBR membrane module 12 is 20%.
The surfaces of the granular activated carbon 11 and the MBR membrane module 12 are used for enriching denitrifying anaerobic methane-oxidizing microorganisms, nitrate and methane are removed under the action of the denitrifying anaerobic methane-oxidizing microorganisms, and the granular activated carbon 11 is spherical granules with the average grain diameter of 2 mm. Since the growth rate of the microorganisms is slow and the activity is low, the MBR membrane module 12 is required to be arranged at the anode to intercept the microorganisms for improving the growth rate of the microorganisms, and the bioelectrochemical system is arranged to increase the activity of the microorganisms. The MBR membrane module 12 material adopted in the embodiment is polyvinylidene fluoride (PVDF). Since the MBR membrane modules 12 have a membrane fouling problem, the MBR membrane modules 12 are surrounded by granular activated carbon 11 for adsorbing the excessive microorganisms in the MBR membrane modules 12. The top of the MBR membrane module 12 in the anode is connected with the effluent pump 1. In order to make the promotion effect of the bioelectrochemical system more efficient, the titanium mesh 13 of the anode is in a shape of surrounding and open top, and the granular activated carbon 11 is completely wrapped in the titanium mesh. The titanium mesh 13 adopted in this embodiment is a diamond mesh, and the shortest diagonal distance is 1 mm. In practical application, the specific sizes of the MBR membrane modules 12 and the titanium mesh 13 can be determined according to the actual volume of the device.
The cathode is a carbon felt 19 with a surface for enriching autotrophic denitrifying microorganisms. The cathode and the anode are respectively communicated with the cathode and the anode of an external power supply through leads 18, and the nitrate and the methane in the wastewater are synchronously removed under the combined action.
The inner cavity of the cylinder body below the anode and the cathode is provided with water distribution pipes 7 with uniform holes, and a gas distributor 8 is arranged below the water distribution pipes 7. The water distribution pipe 7 positioned outside the barrel is provided with a water inlet pump 5 for providing power for wastewater to enter the inner cavity of the barrel, and the water inlet pump 5 adopts a peristaltic pump in the embodiment. The water inlet conduit 7 traverses the whole reaction device and is uniformly designed with pores, and the opening rate of the water distribution pipe 7 is preferably 10% so as to facilitate more uniform water inlet.
The gas distributor 8 is a disc distributor so as to facilitate the methane to enter more uniformly, and an aeration pump 10 is arranged at the gas inlet end of the gas distributor 8 positioned outside the cylinder. The gas inlet end of the gas distributor 8 passes through a gas inlet 9 arranged at the bottom of the cylinder body to be communicated with the outside and is used for blowing gas to the anode to ensure that the granular activated carbon 11 realizes a fluidized state. The gas outlet 2 is formed in the side wall of the upper portion of the barrel, the gas outlet 2 is communicated with the gas inlet end of the gas distributor 8 through a gas pipeline provided with a circulating pump 4, and methane gas which is not dissolved in water at the top of the barrel is sucked to the gas inlet end of the gas distributor 8, so that cyclic utilization of the methane gas is achieved. Methane in the initial reaction stage is pumped to the air inlet 9 through the aeration pump 10, and then is uniformly conveyed to the inner cavity of the cylinder through the air distributor 8, so that the subsequent water-gas cooperative treatment is facilitated. After the aeration is completed, the aeration pump 10 is turned off and the circulation pump 4 is turned on. Because the solubility of methane in aqueous is lower, consequently with unnecessary methane that is in the overhead device through circulating pump 4 from air inlet 2 circulation to barrel inner chamber, improve methane's availability, this process is through adjusting the velocity of flow of circulating pump 4 control methane gas simultaneously for anodal granule active carbon 11 is in fluidization state.
In addition, the outer circuit area 22 is provided with a voltage sensor 15 and an alarm 17, the voltage sensor 15 monitors the condition of generated voltage in real time, and when the voltage deviates from a preset value, the alarm 17 gives an alarm to indicate that the device is not operated normally. The voltage sensor 15 is connected in series with the alarm 17, both of which are connected in parallel with a resistor 16 of 500-1000 Ω. Meanwhile, a sampling port 3 is arranged on the wall of the middle part of the device close to the anode side, and various parameters of the discharged water are monitored at any time.
In the invention, the coupling of the bioelectrochemical system, the membrane component and the denitrification anaerobic methane oxidation microorganism realizes the cooperative removal of nitrate and methane in the wastewater treatment process. Through double optimization of the process and the treatment method, the nitrate type wastewater and redundant methane generated during wastewater treatment are converted into nitrogen and carbon dioxide, so that the effect of synchronous denitrification and carbon removal in wastewater treatment is realized.
Therefore, based on the reaction device, the invention also provides a method for treating nitrate wastewater and methane waste gas, which comprises the following steps:
firstly, the water inlet pump 5 is started, and nitrate wastewater is introduced into the inner cavity of the barrel through the water distribution pipe 7 and is uniformly distributed. The wastewater introduced into the cylinder occupies 3/4 of the volume of the cylinder cavity calculated according to chemometrics and henry's law of gas dissolution. And simultaneously, the aeration pump 10 is started, methane waste gas is introduced into the inner cavity of the cylinder through the gas distributor 8 and is fully contacted with the wastewater, and the methane gas is dissolved in the wastewater.
Then the aeration pump 10 is turned off and the circulation pump 4 is turned on. Methane gas which is not dissolved in the wastewater at the top of the inner cavity of the cylinder body is pumped to the gas inlet end of the gas distributor 8 again under the action of the circulating pump 4, so that the methane gas is recycled. The flow rate of the methane gas is adjusted by controlling the circulation pump 4 so that the granular activated carbon 11 is fluidized.
During this period, nitrate in the wastewater and methane dissolved in the wastewater are simultaneously converted into nitrogen and carbon dioxide by the denitrification anaerobic methane oxidation microorganisms enriched on the granular activated carbon 11 and the surface of the MBR membrane module 12. Meanwhile, the generated electrons are transferred to the granular activated carbon 11, and the activity of the denitrifying anaerobic methane-oxidizing microorganisms is improved by utilizing the promotion effect of bioelectrochemistry. The generated electrons are transferred from the granular activated carbon 11 to the titanium mesh 13 through the mutual collision action of the granular activated carbon 11 and the titanium mesh 13, and then transferred to the carbon felt 19 through the externally connected titanium wire 14 via the lead wire 18. The autotrophic denitrifying microorganisms enriched on the surface of the carbon felt 19 utilize the electrons in the portion to further reduce the nitrate in the water into nitrogen.
During the operation of the device for treating nitrate wastewater and methane waste gas, the voltage state of the reaction device is monitored in real time by the voltage sensor 15 arranged on the lead 18. When the voltage deviates from the predetermined value, an alarm 17 connected in series with the voltage sensor 15 gives an alarm to indicate that the reactor is operating abnormally.
The above-described embodiments are merely preferred embodiments of the present invention, which should not be construed as limiting the invention. Various changes and modifications may be made by one of ordinary skill in the pertinent art without departing from the spirit and scope of the present invention. Therefore, the technical scheme obtained by adopting the mode of equivalent replacement or equivalent transformation is within the protection scope of the invention.
Claims (9)
1. A method for treating nitrate wastewater and methane waste gas by using a denitrification anaerobic methane oxidation film bioelectrochemical reaction device is characterized in that the denitrification anaerobic methane oxidation film bioelectrochemical reaction device comprises a closed cylinder, and a cathode and an anode which are positioned in the inner cavity of the cylinder, wherein the cathode and the anode are respectively communicated with the cathode and the anode of an external power supply through leads (18); the anode comprises a titanium mesh (13), granular activated carbon (11) and an MBR (membrane bioreactor) membrane module (12), wherein the titanium mesh (13) wraps the granular activated carbon (11) on the surface of the MBR membrane module (12); the surfaces of the granular activated carbon (11) and the MBR membrane component (12) are used for enriching denitrifying anaerobic methane oxidation microorganisms, the titanium mesh (13) is externally connected with titanium wires (14) and communicated with the lead (18), and the water outlet end of the MBR membrane component (12) is communicated with the outside through a water outlet pipe provided with a water outlet pump (1); the cathode is a carbon felt (19) with the surface used for enriching autotrophic denitrifying microorganisms; water distribution pipes (7) with uniform holes are arranged in the inner cavity of the cylinder body below the anode and the cathode, and a gas distributor (8) is arranged below the water distribution pipes (7); the gas inlet end of the gas distributor (8) is communicated with the outside and is used for blowing gas to the anode to ensure that the granular activated carbon (11) achieves a fluidized state; the side wall of the upper part of the cylinder body is provided with a gas outlet (2), and the gas outlet (2) is communicated with the gas inlet end of the gas distributor (8) through a gas pipeline provided with a circulating pump (4);
the method specifically comprises the following steps: starting a water inlet pump (5), and introducing the nitrate wastewater into the inner cavity of the barrel through a water distribution pipe (7) to realize uniform distribution; simultaneously, starting an aeration pump (10), introducing the methane waste gas into the inner cavity of the cylinder through a gas distributor (8) and enabling the methane waste gas to be fully contacted with the wastewater, and dissolving the methane gas in the wastewater; turning off the aeration pump (10) and turning on the circulating pump (4); methane gas which is not dissolved in the wastewater at the top of the inner cavity of the cylinder body is pumped to the gas inlet end of the gas distributor (8) again under the action of the circulating pump (4), so that the cyclic utilization of the methane gas is realized; the flow rate of the methane gas is adjusted by controlling the circulating pump (4), so that the granular activated carbon (11) is fluidized; nitrate in the wastewater and methane dissolved in the wastewater are enriched on the granular activated carbon (11) and denitrifying anaerobic methane oxidizing microorganisms on the surface of the MBR membrane component (12) and synchronously converted into nitrogen and carbon dioxide, and meanwhile, generated electrons are transferred to the granular activated carbon (11), and the activity of the denitrifying anaerobic methane oxidizing microorganisms is improved by the aid of the bioelectrochemistry promotion; the generated electrons are transmitted to the titanium net (13) from the granular activated carbon (11) through the mutual collision action of the granular activated carbon (11) and the titanium net (13), and then are transmitted to the carbon felt (19) through the external titanium wire (14) through the lead (18); autotrophic denitrification microorganisms enriched on the surface of the carbon felt (19) further reduce the nitrate in the water into nitrogen by utilizing electrons; monitoring the voltage state of the reaction device in real time through a voltage sensor (15) arranged on a lead (18); an alarm (17) in series with the voltage sensor (15) issues an alarm when the voltage deviates from a predetermined value.
2. The method for treating nitrate containing waste water and methane waste gas according to claim 1, wherein the water distribution pipe (7) has an opening rate of 10%, and a water feed pump (5) is provided on the water distribution pipe (7) located outside the drum.
3. The method for treating nitrate containing wastewater and methane off-gas according to claim 1, wherein the gas distributor (8) is a disc distributor provided with an aeration pump (10) at the inlet end located outside the cylinder.
4. The method for treating nitrate wastewater and methane off-gas according to claim 1, wherein a sampling port (3) is opened on the side wall of the cylinder body near the anode.
5. The method for treating nitrate wastewater and methane off-gas according to claim 1, wherein the mesh opening of the titanium mesh (13) is a diamond mesh opening with a short diagonal length of 1 mm.
6. The method of treating nitrate-containing wastewater and methane offgas according to claim 1, wherein the material of the MBR membrane modules (12) is polyvinylidene fluoride, PVDF.
7. The method for treating nitrate wastewater and methane off-gas according to claim 1, wherein the conducting wire (18) is connected in series with a voltage sensor (15) and an alarm (17) in turn and is connected in parallel with a resistor (16) with the size of 500- "1000 Ω for monitoring the voltage state of the reaction device in real time.
8. The method for treating nitrate waste water and methane off-gas according to claim 1, wherein the granular activated carbon (11) is spherical granules having an average particle diameter of 2 mm; the filling degree of the granular activated carbon (11) on the surface of the MBR membrane module (12) is 20%.
9. The method of treating nitrate containing wastewater and methane offgas as claimed in claim 1, wherein the wastewater introduced into the cylinder occupies 3/4 of the volume of the cylinder cavity.
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| CN113336327A (en) * | 2021-04-13 | 2021-09-03 | 西安建筑科技大学 | Synergism method of anaerobic membrane bioreactor based on biochar addition |
| CN116040796A (en) * | 2022-12-29 | 2023-05-02 | 大连理工大学 | Device and process for oxidizing treatment of nitrogen-containing wastewater by electric field coupling magnetite-enhanced anaerobic methane |
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