CN113980781A - Tidal carbon dioxide biological methanation device and method - Google Patents
Tidal carbon dioxide biological methanation device and method Download PDFInfo
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- CN113980781A CN113980781A CN202111230594.1A CN202111230594A CN113980781A CN 113980781 A CN113980781 A CN 113980781A CN 202111230594 A CN202111230594 A CN 202111230594A CN 113980781 A CN113980781 A CN 113980781A
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 70
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 42
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 35
- 238000000034 method Methods 0.000 title claims abstract description 15
- 235000015097 nutrients Nutrition 0.000 claims abstract description 61
- 238000006243 chemical reaction Methods 0.000 claims abstract description 53
- 239000007791 liquid phase Substances 0.000 claims abstract description 43
- 239000007789 gas Substances 0.000 claims abstract description 41
- 238000010574 gas phase reaction Methods 0.000 claims abstract description 38
- 238000009792 diffusion process Methods 0.000 claims abstract description 25
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000007788 liquid Substances 0.000 claims abstract description 15
- 238000005276 aerator Methods 0.000 claims abstract description 9
- 230000000694 effects Effects 0.000 claims abstract description 8
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 7
- 239000001257 hydrogen Substances 0.000 claims abstract description 7
- 230000003068 static effect Effects 0.000 claims abstract description 4
- 239000000969 carrier Substances 0.000 claims description 15
- 238000005086 pumping Methods 0.000 claims description 12
- 239000012528 membrane Substances 0.000 claims description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 9
- 244000005700 microbiome Species 0.000 claims description 8
- 238000002791 soaking Methods 0.000 claims description 4
- 239000010802 sludge Substances 0.000 claims description 3
- 238000005243 fluidization Methods 0.000 claims description 2
- 230000008569 process Effects 0.000 claims description 2
- 239000002028 Biomass Substances 0.000 abstract description 2
- 230000005540 biological transmission Effects 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 40
- 230000036983 biotransformation Effects 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 102000004190 Enzymes Human genes 0.000 description 1
- 108090000790 Enzymes Proteins 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000007865 diluting Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 239000002737 fuel gas Substances 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 229910017053 inorganic salt Inorganic materials 0.000 description 1
- 239000002207 metabolite Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000012452 mother liquor Substances 0.000 description 1
- 239000010413 mother solution Substances 0.000 description 1
- 235000016709 nutrition Nutrition 0.000 description 1
- 230000035764 nutrition Effects 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000007711 solidification Methods 0.000 description 1
- 239000011573 trace mineral Substances 0.000 description 1
- 235000013619 trace mineral Nutrition 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 235000013343 vitamin Nutrition 0.000 description 1
- 239000011782 vitamin Substances 0.000 description 1
- 229940088594 vitamin Drugs 0.000 description 1
- 229930003231 vitamin Natural products 0.000 description 1
- 150000003722 vitamin derivatives Chemical class 0.000 description 1
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- C12M—APPARATUS FOR ENZYMOLOGY OR MICROBIOLOGY; APPARATUS FOR CULTURING MICROORGANISMS FOR PRODUCING BIOMASS, FOR GROWING CELLS OR FOR OBTAINING FERMENTATION OR METABOLIC PRODUCTS, i.e. BIOREACTORS OR FERMENTERS
- C12M21/00—Bioreactors or fermenters specially adapted for specific uses
- C12M21/04—Bioreactors or fermenters specially adapted for specific uses for producing gas, e.g. biogas
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- C12M25/00—Means for supporting, enclosing or fixing the microorganisms, e.g. immunocoatings
- C12M25/02—Membranes; Filters
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- C12M25/00—Means for supporting, enclosing or fixing the microorganisms, e.g. immunocoatings
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- C12M27/00—Means for mixing, agitating or circulating fluids in the vessel
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- C12M29/00—Means for introduction, extraction or recirculation of materials, e.g. pumps
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Abstract
A tidal type carbon dioxide high-efficiency biological methanation device and a method thereof mainly comprise a gas diffusion zone, a liquid phase reaction zone and a gas phase reaction zone; a microporous aerator is arranged between the gas diffusion zone and the liquid phase reaction zone, and a porous plate is arranged between the liquid phase reaction zone and the gas phase reaction zone. The liquid phase reaction zone and the gas phase reaction zone are respectively filled with a granular anaerobic biomembrane and a biomembrane carrier with good carbon dioxide methanation activity. In the tidal mode of operation, the granular anaerobic biofilm is always immersed in the nutrient solution and is in an expanded or fluidized state, while the biofilm carrier is in an alternate environment of static state and dry-wet state. Carbon dioxide and hydrogen are sequentially converted by the granular anaerobic biomembrane and the biomembrane carrier to finally generate high-grade methane. The invention can improve the active biomass and gas-liquid transmission under the condition of low costMass efficiency, realization of CO2Efficient biological methanation to CO2Provides an effective way for resource utilization.
Description
Technical Field
The invention belongs to the technical field of environmental protection, relates to resource application of carbon dioxide, and particularly relates to a tidal carbon dioxide biological methanation device and method.
Background
CO2The conversion method mainly comprises hydrogenation conversion, electrochemical conversion, photochemical conversion, biotransformation and the like. The first three belong to pure chemical catalytic processes, the conversion rate is high, but the requirements on the catalyst are high, and the problems of poor selectivity, high operation cost and the like are faced at present. The biotransformation takes enzyme in the microorganism as a catalyst, and can realize CO at high selectivity under mild conditions2And (4) transformation. CO 22The products of biotransformation mainly comprise energy substances or chemicals such as methane, acids, alcohols and the like, wherein the methane is taken as a target product, and the method has the advantages of easy product separation, high applicability and the like.
The most studied CO is currently2The biomethanation apparatus has a CSTR, a fixed bed, a trickle bed and a membrane reactor. However, these devices are faced with CO due to gas-liquid mass transfer limitations2Low conversion efficiency.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide a tidal carbon dioxide biological methanation device and method, which can improve the gas-liquid mass transfer efficiency and realize CO by further increasing the gas-liquid contact area2High-efficiency biological methanation.
In order to achieve the purpose, the invention adopts the technical scheme that:
a tidal carbon dioxide biological methanation device comprises a gas diffusion zone, a liquid phase reaction zone and a gas phase reaction zone which are sequentially distributed from bottom to top, wherein a microporous aerator is arranged between the gas diffusion zone and the liquid phase reaction zone, a porous plate is arranged between the liquid phase reaction zone and the gas phase reaction zone, and the gas diffusion zone is communicated with a gas inlet valve; the liquid phase reaction zone is filled with nutrient solution and is filled with a granular anaerobic biomembrane, and during the working period of the device, the granular anaerobic biomembrane is always immersed in the nutrient solution and is in an expansion or fluidization state; the gas phase reaction zone is filled with a biofilm carrier, the biofilm carrier is soaked in nutrient solution at the working interval of the device so that microorganisms in the biofilm can obtain nutrient elements and promote the growth and the propagation of the microorganisms, and the biofilm carrier is not immersed in the nutrient solution and is in a static state during the working period of the device.
Preferably, the upper part of the liquid phase reaction zone is connected with the bottom of the nutrient solution tank through a first pipeline with a water pump; the top of the gas phase reaction zone is connected with the top of the nutrient solution tank through a second pipeline; the top of the nutrient solution tank is provided with an air outlet; and the air outlet is provided with an air outlet valve.
Preferably, the gas diffusion zone accounts for 5% -10% of the total volume of the apparatus, the liquid phase reaction zone accounts for 20% -40% of the total volume of the apparatus, and the gas phase reaction zone accounts for 50% -75% of the total volume of the apparatus.
Preferably, the effective volume of the nutrient solution tank is 1.2 to 1.5 times of the volume of the gas phase reaction zone.
Preferably, the filling rate of the nutrient solution in the liquid phase reaction zone is 70-90%.
Preferably, the granular anaerobic biofilm is anaerobic granular sludge formed by self-immobilization or anaerobic biofilm growing on a granular carrier.
Preferably, the filling rate of the biofilm carriers in the gas phase reaction zone is 80-100%.
The invention also provides a tidal carbon dioxide biomethanation method based on the tidal carbon dioxide biomethanation device, which comprises the following steps:
step one, filling a granular anaerobic biomembrane and a biomembrane carrier with carbon dioxide methanation activity into a liquid phase reaction zone and a gas phase reaction zone respectively in an anaerobic environment, and pumping nutrient solution into the liquid phase reaction zone until the liquid level rises to a porous plate;
step two, carbon dioxide and hydrogen enter a gas diffusion zone from a gas inlet according to the volume ratio of 0.2-0.3, enter a liquid phase reaction zone and a gas phase reaction zone sequentially through a microporous aerator, and are treated by a particle type anaerobic biological membrane and a biological membrane carrier to CO2And H2Carrying out conversion to generate methane;
step three, after the device continuously operates for 5-30 days, closing the air inlet valve, pumping the nutrient solution into the liquid phase reaction zone again until the nutrient solution in the gas phase reaction zone submerges all the biomembrane carriers, and continuously soaking the biomembrane carriers in the nutrient solution for 5-30 minutes;
pumping out the nutrient solution until the liquid level in the device drops to the position of the porous plate, and opening the air inlet valve after waiting for 30-60 minutes;
and step five, repeating the step two to the step four.
Compared with the prior art, the invention has the beneficial effects that:
1. the invention adopts a tidal operation mode to make the device have CO2The biomembrane carrier with methanation activity is in a dry-wet alternative state, on one hand, the gas-liquid contact area is increased, the gas-liquid mass transfer efficiency is improved, on the other hand, the microorganism nutrition supply is fully ensured, and the CO can be greatly improved2Biological methanation efficiency.
2. The invention synchronously realizes CO by utilizing the high biomass characteristic of the granular anaerobic biomembrane2And efficient biotransformation of intermediate metabolites such as acetic acid.
3. The device and the method can realize CO under the condition of low cost2Efficient biological methanation to CO2Provides an effective way for resource utilization.
Drawings
FIG. 1 is a schematic diagram of the present invention.
Detailed Description
The embodiments of the present invention will be described in detail below with reference to the drawings and examples.
As shown in figure 1, the invention relates to a tidal carbon dioxide biological methanation device, which comprises a gas diffusion zone 1, a liquid phase reaction zone 2 and a gas phase reaction zone 3 which are sequentially distributed from bottom to top. The gas diffusion zone 1, the liquid phase reaction zone 2 and the gas phase reaction zone 3 may be arranged in a cylindrical, square or the like vessel. Illustratively, the gas diffusion zone 1 accounts for 5 to 10% of the total volume of the apparatus, the liquid-phase reaction zone 2 accounts for 20 to 40% of the total volume of the apparatus, and the gas-phase reaction zone 3 accounts for 50 to 75% of the total volume of the apparatus. In one embodiment of the present invention, the total volume of the device is 60L, and the gas diffusion zone 1 occupies 5% of the total volume of the device, i.e. 3L; the liquid phase reaction zone 2 accounts for 5 percent of the total volume of the device, namely 15L; the gas-phase reaction zone 3 accounted for 70% of the total volume of the apparatus, i.e., 42L.
The gas diffusion zone 1 is communicated with a gas inlet 4 with a gas inlet valve 13, a microporous aerator 5 is arranged between the gas diffusion zone 1 and the liquid phase reaction zone 2, and a porous plate 7 is arranged between the liquid phase reaction zone 2 and the gas phase reaction zone 3.
The gas inlet 4 may be provided at a side wall of the gas diffusion area 1 for feeding the mixed gas of carbon dioxide and hydrogen to the gas diffusion area 1, where the mixed gas can be sufficiently diffused at the gas diffusion area 1.
The shape of the micropore aerator 5 can be round or square, the average diameter of micropores is 2-5 microns, and the function is to enable gas entering the liquid phase reaction zone 2 to form tiny bubbles and increase the gas-liquid mass transfer area.
The perforated plate 7 may have a circular or square shape and a hole diameter of 10 mm, and functions to intercept the biofilm carriers 8 filled in the gas phase reaction zone 3.
The liquid phase reaction zone 2 is filled with nutrient solution and is filled with a granular anaerobic biofilm 6. The nutrient solution is filled with various nutrient elements required by the growth of anaerobic microorganisms, the filling rate is 70% -90%, 80% is selected in the embodiment, and the volume of the corresponding nutrient solution is 12L. As an example, one possible specific formulation of the nutrient solution is as follows:
each liter of nutrient solution is formed by diluting five nutrient mother solutions of A (10mL), B (2mL), C (1mL), D (1mL) and E (5 mL). The components of 5 kinds of nutrient mother liquor of A (main inorganic salt), B (phosphate), C (sulfate), D (trace elements) and E (vitamin) are shown in the following table:
during the operation of the device, the granular anaerobic biofilm 6 should be always immersed in the nutrient solution and in an expanded or fluidized state. The granular anaerobic biofilm 6 has good carbon dioxide methanation activity, and can be, for example, anaerobic granular sludge formed by self-solidification or an anaerobic biofilm grown on a granular carrier.
The gas phase reaction zone 3 is filled with biofilm carriers 8, illustratively, at a filling rate of 80% to 100%, preferably 100% in this embodiment. During the working period of the device, the biomembrane carrier 8 is not immersed in the nutrient solution and is in a static state, and in the working interval of the device, the biomembrane carrier 8 is soaked in the nutrient solution to ensure that microorganisms in the biomembrane obtain nutrient elements and promote the growth and the propagation of the microorganisms.
Carbon dioxide and hydrogen are sequentially converted by the granular anaerobic biomembrane 6 and the biomembrane carrier 8, and finally high-grade methane is generated. The biofilm carrier 8 has good carbon dioxide methanation activity, which can be a carbon-loaded sponge particle of 2-4 cm size.
Based on the device, the tidal carbon dioxide biological methanation method comprises the following steps:
step one, filling a granular anaerobic biomembrane 6 with carbon dioxide methanation activity and a biomembrane carrier 8 into a liquid phase reaction zone 2 and a gas phase reaction zone 3 respectively in an anaerobic environment, and pumping nutrient solution into the liquid phase reaction zone 2 until the liquid level rises to a porous plate 7;
step two, carbon dioxide and hydrogen enter a gas diffusion zone 1 from a gas inlet 4 according to the volume ratio of 0.2-0.3, enter a liquid phase reaction zone 2 and a gas phase reaction zone 3 in sequence through a microporous aerator 5, and CO is treated by a granular anaerobic biological membrane 6 and a biological membrane carrier 82And H2Carrying out conversion to generate methane;
step three, after the device continuously operates for 5 to 30 days, closing the air inlet valve 13, pumping the nutrient solution into the liquid phase reaction zone 2 again until the nutrient solution in the gas phase reaction zone 3 submerges all the biomembrane carriers 8, and continuously soaking the biomembrane carriers 8 in the nutrient solution for 5 to 30 minutes;
pumping out the nutrient solution until the liquid level in the device drops to the position of the porous plate 7, and opening the air inlet valve 13 after waiting for 30-60 minutes;
and step five, repeating the step two to the step four.
In one embodiment of the invention, the upper part of the liquid phase reaction zone 2 is connected with the bottom of a nutrient solution tank 10 through a first pipeline 9 with a water pump 11; the top of the gas-phase reaction zone 3 is connected with the top of a nutrient solution tank 10 through a second pipeline 9; the top of the nutrient solution tank 10 is provided with an air outlet 12; the air outlet 12 is provided with an air outlet valve 14. Illustratively, the effective volume of the nutrient solution tank 10 is 1.2-1.5 times of the volume of the gas phase reaction zone 3, and in this embodiment, 1.25 times is selected, and the corresponding volume is 52.5L.
At the moment, the tidal carbon dioxide efficient biological methanation method comprises the following steps:
step one, respectively filling a granular anaerobic biomembrane 6 and a biomembrane carrier 8 with good carbon dioxide methanation activity into a liquid phase reaction zone 2 and a gas phase reaction zone 3 under an anaerobic environment, starting a water pump 11, pumping nutrient solution into the liquid phase reaction zone 2 from a nutrient solution tank 10 until the liquid level in the device rises to a porous plate 7, and closing the water pump 11;
step two, carbon dioxide and hydrogen enter a gas diffusion zone 1 from a gas inlet 4 according to the proportion of 0.25, enter a liquid phase reaction zone 2 and a gas phase reaction zone 3 in turn through a microporous aerator 5, and CO is treated by a granular anaerobic biological membrane 6 and a biological membrane carrier 82And H2The methane is converted to generate methane, the methane enters a nutrient solution tank 10 through a first pipeline 9, and finally the methane is discharged from a gas outlet 12 and collected by a gas bag;
step three, after the device continuously operates for 15 days, closing the air inlet valve 13 and the air outlet valve 14, starting the water pump, pumping nutrient solution into the liquid phase reaction zone 2 from the nutrient solution tank 10 until all the biomembrane carriers 8 are submerged by the nutrient solution in the gas phase reaction zone 3, closing the water pump 11, and continuously soaking the biomembrane carriers 8 in the nutrient solution for 5 minutes;
and step four, starting the water pump 11 reversely, pumping the nutrient solution from the liquid phase reaction zone 2 to the nutrient solution tank 10 until the liquid level in the device is reduced to the position of the porous plate 7, closing the water pump 11, and opening the air inlet valve 13 and the air outlet valve 14 after waiting for 30 minutes.
And step five, repeating the step two to the step four.
The device and the method of the invention are adopted to treat CO2The result of the biological methanation experiment carried out for 3 months shows that the treatment flow is 1m3Under the condition of/d, the methane content in the product gas is kept above 95%, and the purity meets the utilization requirement of fuel gas.
It will be apparent to those skilled in the art that, based on the above principle, the method of the present invention may be subject to several changes and modifications, which are also included in the scope of the present invention.
Claims (8)
1. A tidal carbon dioxide biological methanation device is characterized by comprising a gas diffusion zone (1), a liquid phase reaction zone (2) and a gas phase reaction zone (3) which are sequentially distributed from bottom to top, wherein a microporous aerator (5) is arranged between the gas diffusion zone (1) and the liquid phase reaction zone (2), a porous plate (7) is arranged between the liquid phase reaction zone (2) and the gas phase reaction zone (3), and the gas diffusion zone (1) is communicated with a gas inlet (4) with a gas inlet valve (13); the liquid phase reaction zone (2) is filled with nutrient solution and is filled with a granular anaerobic biological membrane (6), and during the working period of the device, the granular anaerobic biological membrane (6) is always immersed in the nutrient solution and is in an expansion or fluidization state; the gas phase reaction zone (3) is filled with biofilm carriers (8), the biofilm carriers (8) are soaked in nutrient solution in the working interval of the device so that microorganisms in the biofilm can obtain nutrient elements, and the biofilm carriers (8) are not immersed in the nutrient solution and are in a static state during the working of the device.
2. The tidal carbon dioxide biomethanation plant according to claim 1, wherein the upper part of the liquid phase reaction zone (2) is connected with the bottom of the nutrient solution tank (10) through a first pipeline (9) with a water pump (11); the top of the gas phase reaction zone (3) is connected with the top of a nutrient solution tank (10) through a second pipeline (9); the top of the nutrient solution tank (10) is provided with an air outlet (12); the air outlet (12) is provided with an air outlet valve (14).
3. The tidal carbon dioxide biomethanation plant according to claim 1, wherein the gas diffusion zone (1) accounts for 5-10% of the total volume of the plant, the liquid phase reaction zone (2) accounts for 20-40% of the total volume of the plant, and the gas phase reaction zone (3) accounts for 50-75% of the total volume of the plant.
4. The tidal carbon dioxide biomethanation plant according to claim 1, wherein the effective volume of the nutrient solution tank (10) is 1.2-1.5 times of the volume of the gas phase reaction zone (3).
5. The tidal carbon dioxide biomethanation plant according to claim 1, wherein the liquid phase reaction zone (2) has a nutrient solution filling rate of 70-90%.
6. The tidal carbon dioxide biomethanation plant according to claim 1, wherein the granular anaerobic biofilm (6) is a self-solidified anaerobic granular sludge or an anaerobic biofilm attached to a granular carrier.
7. The tidal carbon dioxide biomethanation plant according to claim 1, wherein the filling rate of the biofilm carriers (8) in the gas phase reaction zone (3) is 80-100%.
8. The tidal carbon dioxide biomethanation process based on the tidal carbon dioxide biomethanation plant of claim 1, comprising the steps of:
step one, filling a granular anaerobic biomembrane (6) and a biomembrane carrier (8) with carbon dioxide methanation activity into a liquid phase reaction zone (2) and a gas phase reaction zone (3) respectively in an anaerobic environment, and pumping nutrient solution into the liquid phase reaction zone (2) until the liquid level rises to a porous plate (7);
secondly, carbon dioxide and hydrogen enter the gas diffusion area (1) from the gas inlet (4) according to the volume ratio of 0.2-0.3, and sequentially enter the gas diffusion area through the microporous aerator (5) and then enter the gas diffusion areaA reaction zone (2) and a gas phase reaction zone (3), and CO is treated by a granular anaerobic biomembrane (6) and a biomembrane carrier (8)2And H2Carrying out conversion to generate methane;
step three, after the device continuously operates for 5-30 days, closing the air inlet valve (13), pumping the nutrient solution into the liquid phase reaction zone (2) again until all the biomembrane carriers (8) are submerged by the nutrient solution in the gas phase reaction zone (3), and continuously soaking the biomembrane carriers (8) in the nutrient solution for 5-30 minutes;
pumping out the nutrient solution until the liquid level in the device drops to the position of the porous plate (7), and opening the air inlet valve (13) after waiting for 30-60 minutes;
and step five, repeating the step two to the step four.
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