CN115888648A - CO adsorption and removal based on free radical induction multi-element modified porous carbon 2 Method and system for generating a response to a user - Google Patents
CO adsorption and removal based on free radical induction multi-element modified porous carbon 2 Method and system for generating a response to a user Download PDFInfo
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
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Abstract
The invention provides a method for removing CO through adsorption of multi-element modified porous carbon based on free radical induction 2 Method and system of (1), belonging to CO 2 The technical field of trapping; in the invention, high-activity free radicals are used for modifying the biochar, and CO in the flue gas is removed by the modified biochar in an adsorption manner 2 Desorbing CO from the saturated biochar by heating 2 And realize CO 2 Recovering; the method has the outstanding comprehensive advantages of cheap raw materials, low energy consumption and environmental protection of the modification method, real-time online activation and regeneration of the adsorbent and the like, has very obvious technical, economic and environmental protection comprehensive advantages, and is CO with wide industrial application prospect 2 A trapping method and system.
Description
Technical Field
The invention belongs to CO 2 The technical field of trapping, in particular to a method for removing CO through adsorption of multi-element modified porous carbon based on free radical induction 2 Methods and systems of (1).
Background
Among the various "greenhouse gases", CO 2 Over 55%, and energy power and CO emitted from fossil fuel combustion in industrial processes 2 About total CO 2 The source is more than 50%. Therefore, active research and development of CO in combustion flue gas 2 The emission reduction technology has important strategic significance.
At present, the mainstream CO developed at home and abroad 2 The trapping technology can be mainly classified into a liquid phase absorption method, an adsorption method, a membrane separation method, a low temperature separation method, an oxygen-enriched combustion method, a chemical chain combustion method, a photo/electrochemical method, and the like. The liquid phase absorption method mainly utilizes various alcohol amine organic solvents/ammonia water/ionic liquid and the like to realize CO 2 Absorption and capture, then regeneration of the absorbent and CO are realized by heating desorption and other methods 2 And (4) recovering. The method can theoretically realize the recycling of the absorbent, but in practical application, the defects of serious reagent loss, large regeneration energy consumption and the like are found, and the problems of equipment corrosion and the like exist in part of reagents. The membrane separation method has the advantages of simple process, no waste generation and the like, and is CO with good development prospect 2 The separation technology has the defects of short service life of membrane materials, low separation purity and the like at present. The low-temperature separation method has the advantages of simple and environment-friendly process, suitability for large-scale treatment and the like, but has the defects of high energy consumption, high-pressure operation and the like. The oxygen-enriched combustion method and the chemical-looping combustion method mainly realize CO by constructing novel combustion conditions and combustion modes 2 The trapping and separating of the gas can affect the existing combustion device and working conditions, and is not suitable for treating the existing traditional combustion devices such as boilers/kilns and the like with huge reserves. Emerging carbon emission reduction technologies such as optical/electrochemical methods are still in the laboratory exploration stage, and are far away from industrial application. The adsorption and desorption method has been widely concerned by the academic and engineering circles at home and abroad due to the advantages of the regenerable utilization of the adsorbent, no waste liquid generation in the desorption process and the like, and has become the CO with the most development prospect at present 2 One of the trapping techniques. Adsorptive separation of CO 2 The most widely used technology is to use active carbon as adsorbent to adsorb CO in flue gas 2 Then byHeating desorption for regeneration of adsorbent and CO 2 And (4) recovering. However, the technology has the defects of very large consumption of the active carbon, high application cost and the like, and cannot realize large-scale industrial application. The development of low cost adsorbents is a key part of the application of this technology.
Biochar (Biochar) is a pyrolysis product from agricultural and forestry wastes, has the advantages of wide raw material source, low cost, environmental friendliness and the like, and is used for producing carbon dioxide (CO) 2 The field of adsorption has received much attention. However, the raw biochar without activation modification generally has the disadvantages of small specific surface area, poor active sites and the like, and satisfactory CO is difficult to obtain 2 Adsorption capacity. To increase CO of biochar 2 The adsorption performance is that scholars at home and abroad improve the pore structure of the biochar by various physical and chemical activation/modification means or induce active sites on the surface of the biochar to generate a special high-activity surface. Although the pore structure and the specific surface area of the biochar can be improved by activating the biochar under a special atmosphere by adopting high temperature or microwaves, the promotion of vital active sites is very limited. Most research works at present mainly focus on improving the surface active sites of the biochar by various chemical means, and the most studied ideas mainly comprise: (1) Modifying by using organic alcohol ammonium or ionic liquid and other reagents; (2) Various metal or nonmetal elements are adopted for doping modification; and (3) carrying out oxidation modification by adopting strong acid and strong oxidant. Although the modification of the biochar by the activation modification method can effectively increase the specific surface area or surface active sites of the biochar, the problems of high cost, poor effect or secondary pollution and the like still exist. Therefore, the active exploration and development of a novel efficient green biochar modification method has important scientific significance and practical significance.
Disclosure of Invention
Aiming at the problems of high cost, poor effect or secondary pollution and the like existing in the modification of the existing adsorbent, the invention provides a method for removing CO through adsorption based on free radical induction multi-element modified porous carbon 2 In the method and the system, the biochar is modified by utilizing high-activity free radicals, and the modified biochar is absorbedRemoving CO in flue gas 2 Desorbing CO from the saturated biochar by heating 2 And realize CO 2 Recovering; the method has the outstanding comprehensive advantages of cheap raw materials, low energy consumption and environmental protection of the modification method, real-time online activation and regeneration of the adsorbent and the like, has very obvious technical, economic and environmental protection comprehensive advantages, and is CO with wide industrial application prospect 2 A trapping method and system.
The invention firstly provides a method for removing CO through adsorption of multi-element modified porous carbon based on free radical induction 2 The system comprises a photochemical rotating bed modification device for modifying the biochar and a rotating bed adsorption device for adsorption and desorption;
the photochemical rotating bed modification device is internally provided with a plurality of first stirring paddles and a plurality of ultraviolet lamp tubes, the photochemical rotating bed modification device is provided with a modified gas inlet connected with a modified gas source, and the bottom surface of the photochemical rotating bed modification device is provided with a modified biochar outlet communicated with the rotating bed adsorption device; the top of the photochemical rotating bed modification device is provided with a plurality of biological carbon inlets, the plurality of biological carbon inlets are connected with a biological carbon storage tank through a pipeline, and a microwave activator, a biological carbon feeder and a first material conveying pump are sequentially arranged on the pipeline from the biological carbon storage tank; the microwave activator is also connected with a humidifier;
a plurality of second stirring paddles are arranged in the rotary bed adsorption device, and a flue gas distributor is arranged on the bottom surface of the rotary bed adsorption device; the bottom of the rotary bed adsorption device is provided with an adsorbed biochar outlet communicated with a biochar storage tank, and a pipeline for communicating the biochar storage tank with the adsorbed biochar outlet is provided with a second material conveying pump; the top of the rotary bed adsorption device is provided with a plurality of modified biochar inlets communicated with the modified biochar outlets in the photochemical rotary bed modification device and a plurality of clean flue gas outlets connected with a chimney through an exhaust pipeline, and the exhaust pipeline is provided with a fan; the rotary bed adsorption device is provided with a flue gas inlet, the flue gas inlet is connected with a flue gas distributor and a flue gas outlet of a boiler/kiln through a gas supply pipeline, and a flue gas temperature regulator is arranged on the gas supply pipeline; the bottom of the rotary bed adsorption device is also provided with a bracket.
Further, the cross section of the photochemical rotating bed modification device is rectangular, the height is 50-220 cm, and the inner side of the lower part of the photochemical rotating bed modification device is inclined at an angle of 30-50 degrees with the horizontal plane; ultraviolet lamp tubes in the photochemical rotating bed modification device are arranged in an equal distance and in a row, the distance between every two adjacent ultraviolet lamp tubes is 10-60 cm, and the length of each ultraviolet lamp tube is 30-200 cm; the first stirring paddles are spiral stirring paddles with lifting force, the first stirring paddles are arranged in an equal interval and in a row, and the length of each first stirring paddle is less than or equal to 20cm shorter than that of each ultraviolet lamp tube; the ultraviolet lamp tubes and the first stirring paddles are arranged in a staggered mode, and each first stirring paddle is arranged at the middle line of two adjacent ultraviolet lamp tubes.
Furthermore, the cross section of the rotary bed adsorption device is rectangular, the height of the rotary bed adsorption device is 40-500 cm, and the inner side of the lower part of the rotary bed adsorption device is inclined at 50-80 degrees with the horizontal plane; the second stirring paddles in the rotating bed adsorption device are arranged in a staggered manner at equal intervals, the interval between every two adjacent stirring paddles is 30-160 cm, and the height of each second stirring paddle is less than that of the rotating bed adsorption device by no more than 30cm; the flue gas distributor on the bottom surface of the rotary bed adsorption device comprises a plurality of pipelines and gas nozzles, the pipelines are connected with the gas nozzles, and the distance between every two adjacent pipelines and the distance between every two adjacent gas nozzles are both 5-60 cm.
The invention also provides a method for removing CO through adsorption of the multi-element modified porous carbon based on the free radical induction 2 The removal method of the system comprises the following steps:
(1) Selecting materials:
selecting modified gas and biochar, wherein the modified gas comprises H 2 O 2 ﹑NH 3 ﹑H 2 S, calculating the input amount of the modified gas and the biochar according to the volume of the photochemical swirling bed modification device;
the input amount of the biochar = volume of the photochemical rotating bed modification device (m) 3 ) X (0.2 to 20 kg); the concentration of the modifying gas is 50ppm-5000ppm, the mass ratio of carbon/gas components between the biochar and the modifying gas is 300.
(2) Modifying the biochar:
introducing modified gas and biochar into photochemical rotating bed modifying device, and inducing modified gas H by ultraviolet lamp tube 2 O 2 、NH 3 ﹑H 2 One or more of S generates one or more of OH, HS and HN to attack the biochar surface, so that the biochar surface generates active sites, and the process can be represented by the following chemical reaction equations (1) - (4):
n·OH+nHN·+nHS·+Biochar——→Biochar-active sites (4)
(3) Adsorption and desorption:
introducing the modified biochar and the flue gas in the boiler/kiln into a rotating bed adsorption device, and adsorbing and removing CO in the flue gas by using active sites on the biochar 2 Desorbing CO from the saturated charcoal by heating 2 And realize CO 2 And (3) recovering, discharging the treated clean flue gas into the atmosphere through a chimney, and activating, modifying and regenerating the biochar without active sites through the step (2).
The specific process can be expressed by the following equation (5):
Biochar-active sites+CO 2 ——→Biochar-CO 2 (5)。
further, in the step (1), the biochar comprises biochar cracked by one or more agricultural straws of cornstalks, rice husks, rice straws, wheat straws, cotton straws and corncobs, or biochar cracked by municipal sludge, fruit shells and industrial organic wastes; the particle size of the biochar is 0.001-0.5 mu m.
Further, in the step (2), the ultraviolet radiation intensity of the ultraviolet lamp tube in the photochemical rotating bed modification device is 10-220 muW/cm 2 The effective wavelength of the ultraviolet light is 100nm-360nm; the stirring speed of the first stirring paddle is 300-3000 r/min; the modification temperature range in the photochemical rotating bed modification device is 20-120 ℃.
Further, in step (3), the addition amount of the modified biochar = volume of the rotating bed adsorption device (m) 3 ) X (0.5-50 kg), the particle size of the modified biochar is 0.002-0.8 mu m, the stirring speed of the second stirring paddle is 200-2500 r/min, and the temperature of the adsorption reaction is 10-150 ℃; when the saturated modified biochar is adsorbed for separation, the stirring speed is 150-1500 revolutions per minute.
CO in the invention 2 Capture process and rationale of (c):
(1) Modification:
decomposition of modified gas component (mainly comprising H) by ultraviolet radiation 2 O 2 ﹑NH 3 ﹑H 2 S, etc.) to generate various high-activity free radicals (OH, HS, HN, etc.), the generated high-activity free radicals can rapidly attack Biochar (Biochar), so that various high-activity sites (active sites) are generated on the surface of the Biochar, and modified Biochar cooperatively modified by multiple elements is obtained, and the specific process can be expressed by the following chemical reaction equations (1) - (4):
n·OH+n HN·+n HS·+Biochar→Biochar-active sites (4)。
(2) Removing:
CO in the flue gas is efficiently adsorbed by utilizing abundant high-activity sites (active sites) generated on the carbon surface of the modified charcoal 2 The specific process can be expressed by the following equation (5):
Biochar-active sites+CO 2 →Biochar-CO 2 (5)。
desorbing CO by heating the saturated modified biochar 2 And realize CO 2 Recovering, namely the biochar loses active sites (active sites), and realizing activation modification regeneration through equations (1) - (4) to recover CO 2 Adsorption capacity, thereby obtaining recycling.
Compared with the prior art, the invention has the beneficial effects that:
in the invention, the free radical-induced multi-element modified porous carbon is used for adsorbing and removing CO 2 The system adjusts the distance and the radiation intensity of ultraviolet lamp tubes in the photochemical rotating bed modification device, reduces the using quantity of the ultraviolet lamp tubes and the investment cost of a light source on the premise of improving the radiation coverage rate of ultraviolet light and ensuring that magnetic catalyst particles have enough fluidized reflux mixing space, and ensures the activation modification effect while controlling initial investment and operation energy consumption.
The invention also adjusts the inclination angles of the photochemical rotating bed modification device and the rotating bed adsorption device, ensures that the falling collection speed of the modified biochar is kept at a proper speed, and the biochar after adsorption saturation slides down as soon as possible to be collected, modified and regenerated again.
The invention adopts cheap agricultural straws to prepare the biochar, and adopts a technical route of real-time online modification, so that the repeated reuse of the adsorbent can be realized, and the material cost is extremely low. The separation, recovery and reuse of the adsorbent greatly reduces the solid waste post-treatment cost of the deactivated adsorbent.
The invention adopts ultraviolet radiation to induce high-activity free radical modified organismsCharcoal and CO adsorption by low energy consumption rotary bed adsorption apparatus 2 Because the ultraviolet radiation intensity is very low, the energy consumption is 3 orders of magnitude lower than that of the low-temperature separation technology, and the low-temperature separation technology has very low operation energy consumption and low cost. The invention adopts dry free radical advanced oxidation technology to adsorb and remove CO 2 The method has the advantages of green and environment-friendly process, no secondary pollution and the like, and has good technical and economic advantages. And, CO in the present invention 2 The adsorption efficiency can reach 92.5%, and the method has wide industrial application prospect.
Drawings
FIG. 1 shows the CO adsorption and removal of multi-element modified porous carbon based on free radical induction 2 Schematic structural diagram of the system of (1).
FIG. 2 is a front view of the photochemical swirling bed modification apparatus and a dimension view thereof.
FIG. 3 is a front view of a rotating bed adsorption apparatus and its dimensional diagrams.
FIG. 4 is a layout diagram of the first stirring paddle and the ultraviolet lamp inside the photochemical revolving bed modification device.
FIG. 5 is a diagram of the arrangement of a second stirring blade inside the spin-bed adsorption apparatus.
FIG. 6 is a diagram of the arrangement of the flue gas distributor inside the rotating bed adsorption unit.
In the figure, 1-photochemical rotating bed modifying device; 2-a rotating bed adsorption unit; 3-a first stirring paddle; 3-1-first stirring paddle section view; 4-ultraviolet lamp tube; 4-1-ultraviolet lamp tube cross-sectional view; 5-a modified gas inlet; 6-modified biochar outlet; 7-biochar inlet; 8-a source of modifying gas; 9-a biochar storage tank; 10-a microwave activator; 11-biochar feeders; 12-a first delivery pump; 13-a humidifier; 14-a second stirring paddle; 14-1-second stirring paddle section view; 15-a flue gas distributor; 15-1-gas nozzle cross-sectional view; 15-2-flue gas duct cross-section; 16-a biochar outlet after adsorption; 17-a second delivery pump; 18-modified charcoal inlet; 19-a chimney; 20-cleaning the flue gas outlet; 21-a fan; 22-boiler/kiln; 23-a flue gas inlet; 24-a flue gas attemperator; 25-Stent
Detailed Description
The invention will be further described with reference to the following figures and specific examples, but the scope of the invention is not limited thereto.
FIG. 1 shows the CO adsorption and removal of multi-element modified porous carbon based on free radical induction 2 The system comprises a photochemical rotating bed modification device 1 for modifying the biochar and a rotating bed adsorption device 2 for adsorption and removal;
the photochemical rotating bed modification device is internally provided with a plurality of first stirring paddles 3 for improving the suspension capacity and the mixed mass transfer rate of original biochar, and a plurality of ultraviolet lamp tubes 4 for decomposing modified gas components (mainly comprising H) by ultraviolet radiation 2 O 2 ﹑NH 3 ﹑H 2 S, etc.) to generate various high-activity free radicals (OH, HS, HN, etc.). The photochemical rotating bed modification device 1 is provided with a modified gas inlet 5 connected with a modified gas source 8, and the bottom of the photochemical rotating bed modification device is provided with a modified biochar outlet 6 communicated with the rotating bed adsorption device 2; the top of the photochemical rotating bed modification device 1 is provided with a plurality of biological carbon inlets 7, the plurality of biological carbon inlets 7 are connected with a biological carbon storage tank 9 after being converged by a pipeline, and a microwave activator 10, a biological carbon feeder 11 and a first material conveying pump 12 are sequentially arranged on the pipeline from the biological carbon storage tank 9; the microwave activator 10 is also connected with a humidifier 13. The microwave activator 10 performs microwave steam activation reaming on the biochar, and the biochar activated by the microwave steam enters the biochar feeder 11 for quantitative distribution.
Rotating bed adsorption equipment 2 internally mounted has a plurality of second stirring rakes 14, and the bottom surface is equipped with flue gas distributor 15, flue gas distributor 15 is constituteed by many equidistant pipelines and equidistant gas nozzle and guarantees that the flue gas can distribute evenly, can leave enough interval again and be convenient for after the absorption charcoal fall into rotating bed adsorption equipment 2 bottoms and retrieve and recycle. The bottom of the rotary bed adsorption device 2 is provided with an adsorbed biochar outlet which is connected with the biochar storage tank 9 through a pipeline, and the pipeline is also provided with a second material conveying pump 17; the top of the rotating bed adsorption device 2 is provided with a plurality of modified biochar inlets 18 connected with the modified biochar outlet 6 in the photochemical rotating bed modification device 1 and a plurality of clean flue gas outlets 20 connected with a chimney 19 through an exhaust pipeline, and the exhaust pipeline is provided with a fan 21; the rotary bed adsorption device 2 is provided with a flue gas inlet 23, the flue gas inlet 23 is connected with a flue gas distributor 24 and a flue gas outlet of a boiler/kiln 22 through a gas supply pipeline, and a flue gas temperature regulator 24 is arranged on the gas supply pipeline; the bottom of the rotary bed adsorption device 2 is also provided with a bracket 25.
Fig. 2 and 4 are front views and size diagrams of the photochemical rotating bed modification device 1, and layout diagrams of the internal first stirring paddle 3 and the ultraviolet lamp tube 4. Wherein the cross section of the photochemical rotating bed modification device 1 is rectangular, the height is 50-220 cm, and the lower part of the photochemical rotating bed modification device is inclined at an angle of 30-50 degrees; ultraviolet lamp tubes 4 in the photochemical swirling bed modification device 1 are arranged in an equal distance and in a row, the distance between every two adjacent ultraviolet lamp tubes 4 ranges from 10 cm to 60cm, and the length of each ultraviolet lamp tube 4 ranges from 30cm to 200cm; the first stirring paddles 3 are spiral stirring paddles with lifting force, the first stirring paddles 3 are arranged in a row at equal intervals, and the length of each first stirring paddle 3 is less than that of the ultraviolet lamp tube 4 by no more than 20cm; the ultraviolet lamp tubes 4 and the first stirring paddles 3 are arranged in a staggered mode, and each first stirring paddle 3 is arranged at the middle line of two adjacent ultraviolet lamp tubes 4.
Fig. 3 is a front view of the rotating bed adsorption device 2 and a size diagram thereof, and fig. 5 and 6 are layout diagrams of the second stirring paddle 14 and the flue gas distributor 15 inside the rotating bed adsorption device 2. Wherein, the cross section of the rotary bed adsorption device 2 is rectangular, the height of the rotary bed adsorption device 2 is 40-500 cm, and the lower part of the rotary bed adsorption device 2 is inclined at an angle of 50-80 degrees; the second stirring paddles 14 in the rotating bed adsorption device 2 are arranged in a staggered manner at equal intervals, the interval between every two adjacent stirring paddles 14 is 30-160 cm, and the height of each second stirring paddle 14 is less than that of the rotating bed adsorption device 2 by no more than 30cm; the flue gas distributor 15 on the bottom surface of the rotary bed adsorption device 2 comprises a plurality of pipelines and gas nozzles, the pipelines are connected with the gas nozzles, and the distance between every two adjacent pipelines and the distance between every two adjacent gas nozzles are 5-60 cm.
The invention also provides a method for removing CO through adsorption of the multi-element modified porous carbon based on the free radical induction 2 The removal method of the system comprises the following steps: (1) selecting materials:
selection changeSex gas and biochar, the modifying gas including H 2 O 2 ﹑NH 3 ﹑H 2 S, calculating the input amount of the modified gas and the biochar according to the volume of the photochemical swirling bed modification device 1; the biochar comprises biochar cracked by one or more agricultural straws of corn stalks, rice husks, rice straws, wheat straws, cotton stalks and corn cobs, or biochar cracked by municipal sludge, fruit shells and industrial organic wastes; the particle size of the biochar is 0.001-0.5 mu m.
The input amount of the biochar = 2 volume (m) of the photochemical rotating bed modification device 3 ) X (0.2 to 20 kg); the concentration of the modified gas is 50ppm-5000ppm, and the mass ratio of carbon/gas components between the biochar and the modified gas is 300.
(2) Modifying the biochar:
presetting ultraviolet radiation intensity and ultraviolet effective wavelength of an ultraviolet lamp tube 4, modification temperature in a photochemical rotating bed modification device 1 and stirring speed of a first stirring paddle 3: the ultraviolet radiation intensity of the ultraviolet lamp tube 4 in the photochemical rotating bed modification device 1 is 10 to 220 mu W/cm 2 The effective wavelength of the ultraviolet light is 100nm-360nm; the stirring speed of the first stirring paddle 3 is 300-3000 r/min; the modification temperature range in the photochemical rotating bed modification device 1 is 20-120 ℃.
Then introducing the modified gas and the biochar into a photochemical rotating bed modification device 1, and inducing the modified gas H by using an ultraviolet lamp tube 4 2 O 2 、NH 3 ﹑H 2 One or more of S generates one or more of OH, HS, HN free radicals to attack the biochar surface, so that the biochar surface generates active sites, and the bulk process can be represented by the following chemical reaction equations (1) - (4):
n·OH+nHN·+nHS·+Biochar——→Biochar-active sites (4)
(3) Adsorption and desorption:
the amount of the modified biochar added to the rotary bed adsorption apparatus 2, the particle size of the modified biochar, the stirring speed of the second stirring paddle 14, and the temperature of the adsorption reaction in the rotary bed adsorption apparatus 2 are preset. Addition amount of modified biochar = volume of rotating bed adsorption device 2 (m) 3 ) X (0.5-50 kg), the particle size of the modified biochar is 0.002-0.8 mu m, the stirring speed of the second stirring paddle 14 is 200-2500 r/min, and the temperature of the adsorption reaction is 10-150 ℃; when the saturated modified biochar is adsorbed for separation, the stirring speed is 150-1500 revolutions per minute.
Then the modified biological carbon and the flue gas in the boiler/kiln 22 are introduced into a rotating bed adsorption device 2, and CO in the flue gas is adsorbed and removed by utilizing active sites on the biological carbon 2 Desorbing CO from the saturated biochar by heating 2 And realize CO 2 And (3) recovering, discharging the treated clean flue gas into the atmosphere through a chimney 19, and realizing activation modification regeneration of the biochar without active sites (active sites) through the step (2).
The specific process can be expressed by the following equation (5):
Biochar-active sites+CO 2 ——→Biochar-CO 2 (5)。
the following is the test for CO in flue gas under different conditions 2 Example of the removal efficiency experiment:
example 1:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are respectively 20 mu W/cm 2 And 254nm, modified gas component H 2 O 2 The adding concentration of the activated carbon is 500ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of a rotary bed adsorption device is 25 ℃. Modified organismsThe mass concentration of the carbon is 2.0 kg/per cubic meter of the rotary bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 2 The removal efficiency was 20.2%.
Example 2:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are respectively 30 mu W/cm 2 And 254nm, modified gas component H 2 O 2 The adding concentration of the activated carbon is 700ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of a rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/per cubic meter of the rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 2 The removal efficiency was 29.7%.
Example 3:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are 40 mu W/cm respectively 2 And 254nm, modified gas component H 2 O 2 The adding concentration of the activated carbon is 1000ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of a rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/per cubic meter of the rotary bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are as follows: CO 2 2 The removal efficiency was 36.5%.
Example 4:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are respectively 50 mu W/cm 2 And 254nm, modified gas component H 2 O 2 The addition concentration of (2) is 1000ppm, and the modified gas component NH 3 The adding concentration of the activated carbon is 100ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of a rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/per cubic meter of the rotary bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 2 The removal efficiency was 49.8%.
Example 5:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are respectively50μW/cm 2 And 254nm, modified gas component H 2 O 2 The addition concentration of (2) is 1000ppm, and the modified gas component NH 3 The adding concentration of the activated carbon is 300ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of a rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/per cubic meter of the rotary bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 2 The removal efficiency was 63.9%.
Example 6:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are respectively 50 mu W/cm 2 And 254nm, modified gas component H 2 O 2 The addition concentration of (2) is 1000ppm, and the modified gas component NH 3 The adding concentration of the activated carbon is 600ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of a rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/per cubic meter of the rotary bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 2 The removal efficiency was 77.2%.
Example 7:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are respectively 50 mu W/cm 2 And 254nm, modified gas component H 2 O 2 Is added at a concentration of 1000ppm, and a modified gas component NH 3 Has an addition concentration of 600ppm and a modified gas component H 2 The adding concentration of S is 300ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of the rotary bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/per cubic meter of the rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 2 The removal efficiency was 88.6%.
Example 8:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and the wavelength of ultraviolet light are respectively 50 mu W/cm 2 And 254nm, modified gas component H 2 O 2 The addition concentration of (2) is 1000ppm, and the modified gas component NH 3 The adding concentration of the modified gas is 600ppmBody component H 2 The adding concentration of S is 600ppm, the biochar is microwave activated straw carbon, and the adsorption temperature of the rotary bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/per cubic meter of the rotary bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 2 The removal efficiency was 92.5%.
In summary, the invention relates to the preparation of CO based on free radical induction of multiple elements 2 The method for removing the porous carbon adsorbent system has the advantages of low initial investment and operation cost, high removal efficiency, high gas-solid mass transfer rate, green and environment-friendly process, capability of real-time online activation and regeneration of the adsorbent and the like, and has wide industrial application prospects.
The present invention is not limited to the above-described embodiments, and any obvious improvements, substitutions or modifications can be made by those skilled in the art without departing from the spirit of the present invention.
Claims (10)
1. CO removal through adsorption of multi-element modified porous carbon based on free radical induction 2 The system is characterized by comprising a photochemical rotating bed modification device (1) for modifying the biochar and a rotating bed adsorption device (2) for adsorption removal;
a plurality of first stirring paddles (3) and a plurality of ultraviolet lamp tubes (4) are arranged in the photochemical rotating bed modification device (1), a modified gas inlet (5) connected with a modified gas source (8) is formed in the photochemical rotating bed modification device (1), and a modified biochar outlet (6) communicated with the rotating bed adsorption device (2) is formed in the bottom surface of the photochemical rotating bed modification device (1); the top of the photochemical rotating bed modification device (1) is provided with a plurality of biological carbon inlets (7), the plurality of biological carbon inlets (7) are communicated with a biological carbon storage tank (9) through a pipeline, and a microwave activator (10), a biological carbon feeder (11) and a first material conveying pump (12) are sequentially arranged on the pipeline from the biological carbon storage tank (9); the microwave activator (10) is also connected with a humidifier (13);
a plurality of second stirring paddles (14) are arranged in the rotary bed adsorption device (2), and a flue gas distributor (15) is arranged on the bottom surface of the rotary bed adsorption device (2); the bottom of the rotary bed adsorption device (2) is provided with an adsorbed biochar outlet (16) communicated with the biochar storage tank (9), and a second material conveying pump (17) is arranged between the biochar storage tank (9) and the adsorbed biochar outlet (16); the top of the rotary bed adsorption device (2) is provided with a plurality of modified biochar inlets (18) communicated with the modified biochar outlets (6) and a plurality of clean flue gas outlets (20) connected with a chimney (19) through exhaust pipelines, and the exhaust pipelines are provided with fans (21); a flue gas inlet (23) is formed in the rotating bed adsorption device (2), the flue gas inlet (23) is connected with a flue gas distributor (15) and a flue gas outlet of a boiler/kiln (22) through a gas supply pipeline, and a flue gas thermoregulator (24) is mounted on the gas supply pipeline; the bottom of the rotary bed adsorption device (2) is also provided with a bracket (25).
2. The free radical-induced multi-element-based modified porous carbon adsorption CO removal based on claim 1 2 The system is characterized in that the cross section of the photochemical rotating bed modification device (1) is rectangular, the height is 50-220 cm, and the inner side of the lower part of the photochemical rotating bed modification device (1) is inclined at an angle of 30-50 degrees with the horizontal plane; ultraviolet lamp tubes (4) in the photochemical rotating bed modification device (1) are arranged in an equal distance and in a row, the distance between every two adjacent ultraviolet lamp tubes (4) ranges from 10 cm to 60cm, and the length of each ultraviolet lamp tube (4) ranges from 30cm to 200cm; the first stirring paddles (3) are spiral stirring paddles with lifting force, the first stirring paddles (3) are arranged in a row at equal intervals, and the length of each first stirring paddle (3) is less than that of each ultraviolet lamp tube (4) by no more than 20cm; the ultraviolet lamp tubes (4) and the first stirring paddles (3) are arranged in a staggered mode, namely each first stirring paddle (3) is arranged at the middle line of two adjacent ultraviolet lamp tubes (4).
3. The free radical-induced multi-element-based modified porous carbon adsorption CO removal based on claim 1 2 The system is characterized in that the cross section of the rotary bed adsorption device (2) is rectangular, the height of the rotary bed adsorption device (2) is 40-500 cm, and the rotary bed adsorption device (2) is rotatedThe inner side of the lower part of the bed adsorption device (2) is inclined at an angle of 50-80 degrees with the horizontal plane; the second stirring paddles (14) in the rotary bed adsorption device (2) are arranged in a staggered manner at equal intervals, the interval between every two adjacent second stirring paddles (14) is 30-160 cm, and the height of each second stirring paddle (14) is less than that of the rotary bed adsorption device (2) and is not more than 30cm; the flue gas distributor (15) on the bottom surface of the rotary bed adsorption device (2) comprises a plurality of pipelines and gas nozzles, wherein the pipelines are communicated with the gas nozzles, and the distance between every two adjacent pipelines and the distance between every two adjacent gas nozzles are both 5-60 cm.
4. CO adsorption and removal based on free radical induction multi-element modified porous carbon 2 The method is characterized in that the removal method is based on the CO adsorption removal method based on the free radical induction multi-element modified porous carbon of any one of claims 1 to 3 2 The removal method comprises the following steps:
(1) Selecting materials:
selecting modified gas and biochar, wherein the modified gas comprises H 2 O 2 ﹑NH 3 ﹑H 2 Calculating the input amount of the modified gas and the biochar according to the volume of the photochemical swirling bed modifying device for any one or mixture of S;
(2) Modifying the biochar:
introducing modified gas and biochar into photochemical rotating bed modifying device, and inducing modified gas H by ultraviolet lamp tube 2 O 2 、NH 3 ﹑H 2 One or more of the S generates one or more of OH, HS, HN and free radicals to attack the surface of the biochar, so that the surface of the biochar generates active sites;
(3) Adsorption and desorption:
introducing the modified biochar and the flue gas in the boiler/kiln into a rotary bed adsorption device, and adsorbing and removing CO in the flue gas by using active sites on the biochar 2 Desorbing CO from the saturated biochar by heating 2 And realize CO 2 The recovered and treated clean flue gas is discharged into the atmosphere through a chimney, and the biochar without active sites can be activated and modified through the step (2)Sexual regeneration.
5. The free radical-induced multi-element-based modified porous carbon adsorption removal of CO according to claim 4 2 The method is characterized in that in the step (1), the biochar comprises biochar cracked by one or more agricultural straws of cornstalks, rice husks, rice straws, wheat straws, cotton straws and corncobs, or biochar cracked by municipal sludge, fruit hulls and industrial organic wastes; the particle size of the biochar is 0.001-0.5 mu m.
6. The free radical-induced multi-element-based modified porous carbon adsorption removal of CO according to claim 4 2 The method of (1), wherein the amount of the biochar charged in the step (1) is = the volume (m) of the photochemical revolving bed modification apparatus (1) 3 ) X (0.2 to 20 kg); the concentration of the modified gas is 50ppm-5000ppm, and the mass ratio of carbon/gas components between the biochar and the modified gas is 300.
7. The free radical-induced multi-element-based modified porous carbon adsorption CO removal method according to claim 4 2 The method is characterized in that in the step (2), the ultraviolet radiation intensity of an ultraviolet lamp tube (4) in the photochemical rotating bed modification device (1) is 10-220 mu W/cm 2 The effective wavelength of the ultraviolet light is 100nm-360nm; the stirring speed of the first stirring paddle (3) is 300-3000 r/min; the modification temperature range in the photochemical rotating bed modification device (1) is 20-120 ℃.
8. The removal of CO by adsorption based on free radical induced multi-element modified porous carbon according to claim 4 2 Characterized in that, in the step (3), the adding amount of the modified biochar = the volume (m) of the rotary bed adsorption device (2) 3 ) X (0.5-50 kg), and the particle diameter of the modified biochar is between 0.002 and 0.8 mu m.
9. The removal of CO by adsorption based on free radical induced multi-element modified porous carbon according to claim 4 2 Method of (1), which is characterized inCharacterized in that in the step (3), the stirring speed of the second stirring paddle (14) in the rotary bed adsorption device (2) is 200-2500 r/min, and the temperature of the adsorption reaction is 10-150 ℃.
10. The free radical-induced multi-element-based modified porous carbon adsorption CO removal method according to claim 4 2 The method is characterized in that in the step (3), when the modified biochar saturated in adsorption is separated, the stirring speed of a second stirring paddle (14) in the rotary bed adsorption device (2) is 150-1500 revolutions per minute.
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