CN115888648B - Multi-element modified porous carbon adsorption CO removal based on free radical induction 2 Method and system of (2) - Google Patents
Multi-element modified porous carbon adsorption CO removal based on free radical induction 2 Method and system of (2) Download PDFInfo
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
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Abstract
The invention provides a method for removing CO based on free radical induced multielement modified porous carbon adsorption 2 The method and the system belong to the CO 2 The technical field of trapping; in the invention, the high-activity free radical modified biochar is utilized, and CO in the flue gas is removed through the adsorption of the modified biochar 2 The biochar after saturation is heated to desorb CO 2 And realize CO 2 Recycling; the method has the outstanding comprehensive advantages of low raw material cost, low energy consumption of the modification method, environmental protection, real-time online activation and regeneration of the adsorbent, and the like, has quite obvious comprehensive advantages of technology, economy and environmental protection, and is CO with wide industrial application prospect 2 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 based on free radical induced multielement modified porous carbon adsorption 2 Is a method and system of (a).
Background
Among various "greenhouse gases", CO 2 Is more than 55% and the energy power and fossil fuel combustion emissions in industrial processesCO 2 About all of the CO 2 More than 50% of the sources. Therefore, active research and development of CO in combustion flue gas 2 Has important strategic significance in emission reduction technology.
Currently, 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 looping combustion method, an optical/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 Is absorbed and trapped, and then the regeneration of the absorbent and CO are realized by methods such as heating desorption 2 Is recovered. The method can realize the recycling of the absorbent theoretically, but the practical application finds that the defects of serious reagent loss, large regeneration energy consumption and the like exist, and part of the reagents also have the problems of equipment corrosion and the like. 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 the membrane material, 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 But will affect the existing combustion device and working condition, and is not suitable for treating the existing and huge-keeping boiler/kiln and other traditional combustion devices. The emerging carbon emission reduction technologies such as photo/electrochemical methods are still in the laboratory exploration stage and are still a distance from industrial applications. The adsorption and removal method has been widely focused by academia and engineering world at home and abroad because the adsorbent can be recycled and no waste liquid is produced in the removal process, and has become the CO with the most development prospect at present 2 One of the trapping techniques. Adsorption separation of CO 2 The technology is most applied to the adsorption of CO in the flue gas by adopting activated carbon as an adsorbent 2 Regeneration of the adsorbent and CO is then achieved by thermal desorption 2 Is recovered. However, the technology has the defects of huge consumption of active carbon, high application cost and the like, and cannot realize large-scale industrial application. Development of low cost adsorbents is a key point for the implementation of the technologyA ring.
Biochar (Biochar) is a pyrolysis product from agricultural and forestry waste, and has the advantages of wide raw material source, low cost, environmental protection and the like, thus being used in CO 2 The adsorption field has received a great deal of attention. However, the raw biomass charcoal which is not activated and modified generally has the defects of small specific surface area, poor active site and the like, and is difficult to obtain satisfactory CO 2 Adsorption capacity. To improve CO of biochar 2 The adsorption performance can be improved by scholars at home and abroad through various physicochemical activation/modification means, or active sites are induced on the surface of the biochar, so that the biochar has a special high-activity surface. Although the pore structure and specific surface area of biochar can be improved by activating biochar at high temperature or under a special atmosphere, the improvement of critical active sites is very limited. Most research work is currently focused on improving the surface active sites of biochar by various chemical means, and the most studied ideas mainly include: (1) Modifying by adopting reagents such as organic alcohol ammonium or ionic liquid; (2) Doping modification is carried out by adopting various metal or nonmetal elements; and (3) adopting strong acid and strong oxidant to carry out oxidation modification. Although the activated modification method can effectively increase the specific surface area or the surface active site of the biochar, the activated modification method still has the problems of high cost, poor effect, secondary pollution and the like. Therefore, the development of a novel efficient green biochar modification method is actively explored, and the method has important scientific significance and practical significance.
Disclosure of Invention
Aiming at the problems of high cost, poor effect, secondary pollution and the like in the conventional adsorbent modification, the invention provides a porous carbon adsorption method for removing CO based on free radical-induced multielement modification 2 In the method and the system, the high-activity free radical modified biochar is utilized, and CO in the flue gas is removed through adsorption of the modified biochar 2 The biochar after saturation is heated to desorb CO 2 And realize CO 2 Recycling; the method has the advantages of low raw material cost, low energy consumption of the modification method, environment friendliness, real-time online activation and regeneration of the adsorbent and the likeHas very obvious comprehensive advantages of technology, economy and environmental protection, and is CO with wide industrial application prospect 2 Trapping method and system.
The invention firstly provides a method for removing CO based on free radical induced multielement modified porous carbon adsorption 2 Comprises a photochemical rotating bed modifying device for modifying biochar and a rotating bed adsorbing device for adsorbing and removing;
the photochemical rotating bed modification device is internally provided with a plurality of first stirring paddles and a plurality of ultraviolet lamp tubes, a modification gas inlet connected with a modification gas source is arranged on the photochemical rotating bed modification device, and a modified biochar outlet communicated with the rotating bed adsorption device is arranged on the bottom surface of the photochemical rotating bed modification device; the top of the photochemical rotating bed modification device is provided with a plurality of biochar inlets, the biochar inlets are connected with a biochar storage tank through a pipeline, and a microwave activator, a biochar feeder and a first material conveying pump are sequentially arranged on the pipeline from the biochar storage tank; the microwave activator is also connected with a humidifier;
a plurality of second stirring paddles are arranged in the rotating bed adsorption device, and a flue gas distributor is arranged on the bottom surface of the rotating bed adsorption device; the bottom of the rotating bed adsorption device is provided with an adsorbed biochar outlet communicated with a biochar reserve tank, and a pipeline communicated with the adsorbed biochar outlet is provided with a second material conveying pump; the top of the rotating bed adsorption device is provided with a plurality of modified biochar inlets communicated with modified biochar outlets in the photochemical rotating bed modification device and a plurality of clean smoke outlets connected with a chimney through an exhaust pipeline, and the exhaust pipeline is provided with a fan; the rotating 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 rotating 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 30-50 degrees with the horizontal plane; the ultraviolet lamp tubes in the photochemical rotating bed modification device are arranged at equal intervals and in parallel, the interval range of the adjacent ultraviolet lamp tubes is 10-60 cm, and the length of the ultraviolet lamp tubes is 30-200 cm; the first stirring paddles are screw stirring paddles with lifting force, the first stirring paddles are arranged at equal intervals and in a parallel row, and the length of the first stirring paddles is not more than 20cm shorter than that of the 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 center line of two adjacent ultraviolet lamp tubes.
Further, the cross section of the rotating bed adsorption device is rectangular, the height of the rotating bed adsorption device is 40-500 cm, and the inner side of the lower part of the rotating 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 at equal intervals and in a fork row, the interval between every two adjacent second stirring paddles is 30-160 cm, and the height of each second stirring paddle is not more than 30cm smaller than that of the rotating bed adsorption device; the flue gas distributor at the bottom surface of the rotating bed adsorption device comprises a plurality of pipelines and gas nozzles, wherein the pipelines are connected with the gas nozzles, and the distances between the adjacent pipelines and between the adjacent gas nozzles are 5-60 cm.
The invention also provides the method for removing CO based on the free radical-induced multielement modified porous carbon adsorption 2 The system 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 S, calculating the input amount of modified gas and biochar according to the volume of the photochemical rotating bed modification device;
the input of biochar=photochemical rotating bed modification apparatus volume (m 3 ) X (0.2-20 kg); the concentration of the modifying gas is 50ppm-5000ppm, and the mass ratio of carbon to gas components between the biochar and the modifying gas is 300:1-20000:1.
(2) Modifying biochar:
introducing modified gas and biochar into photochemical rotating bed for modificationBuilt-in, utilizing ultraviolet lamp tube to induce modified gas H 2 O 2 、NH 3 ﹑H 2 One or more of S generates one or more of OH, HS and HN free radicals to attack the surface of the biochar, so that the surface of the biochar generates active sites, and the body process can be represented by the following chemical reaction equations (1) - (4):
n·OH+nHN·+nHS·+Biochar——→Biochar-active sites (4)
(3) Adsorption removal:
introducing the modified biochar and the flue gas in the boiler/kiln into a rotating bed adsorption device, and removing CO in the flue gas by utilizing the active site adsorption on the biochar 2 The biochar after saturation is heated to desorb CO 2 And realize CO 2 And (3) recycling, namely 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 obtained by cracking one or more agricultural straws in cornstalks, rice husks, rice stalks, wheat straws, cotton stalks and corncobs, or biochar obtained by cracking 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), photochemistryThe ultraviolet radiation intensity of the ultraviolet lamp tube in the rotating bed modification device is 10-220 mu W/cm 2 The effective wavelength of ultraviolet light is 100nm-360nm; the stirring speed of the first stirring paddle is 300-3000 r/min; the modification temperature in the photochemical rotating bed modification device ranges from 20 ℃ to 120 ℃.
Further, in the step (3), the addition amount of the modified biochar=the 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 rpm, and the temperature of the adsorption reaction is 10-150 ℃; when the modified biochar saturated in adsorption is separated, the stirring speed is 150-1500 rpm.
CO in the present invention 2 Is a trapping process and basic principle:
(1) Modification:
decomposition of the 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 be utilized to rapidly attack the Biochar (Biochar), so that various high-activity sites (active sites) are generated on the surface of the Biochar, and the modified Biochar synergistically modified by multiple elements is obtained, and the specific process can be represented by the following chemical reaction equations (1) - (4):
n·OH+n HN·+n HS·+Biochar→Biochar-active sites (4)。
(2) And (3) removing:
by the generation on the carbon surface of the modified biocharAbundant high active sites (active sites) efficiently adsorb CO in flue gas 2 The specific process can be expressed by the following equation (5):
Biochar-active sites+CO 2 →Biochar-CO 2 (5)。
the modified biochar after saturation is heated to desorb CO 2 And realize CO 2 Recovery, in which the biochar has lost active sites, can be regenerated by activating modification through equations (1) - (4) to recover CO 2 Adsorption capacity, thereby achieving recycling.
Compared with the prior art, the invention has the beneficial effects that:
the invention relates to a method for removing CO based on free radical induced multielement modified porous carbon adsorption 2 The distance and the radiation intensity of the ultraviolet lamp tubes in the photochemical rotating bed modification device are adjusted, the use quantity of the ultraviolet lamp tubes and the investment cost of the light sources are reduced on the premise of improving the radiation coverage rate of ultraviolet light and ensuring that the magnetic catalyst particles have enough fluidization reflux mixing space, and the activation modification effect is ensured while the initial investment and the operation energy consumption are controlled.
The invention also adjusts the inclination angles of the photochemical rotating bed modifying device and the rotating bed adsorbing device, ensures that the falling collecting speed of the modified biochar is kept at a proper speed, and the biochar after saturated adsorption slips off as soon as possible to collect, re-modify and regenerate.
The invention adopts the low-cost agricultural straw to prepare the biochar, and adopts the technical route of real-time on-line modification, thereby realizing the repeated reuse of the adsorbent and having extremely low material cost. The separation, recovery and reutilization 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 biochar, and adopts a rotating bed adsorption device with low energy consumption to adsorb CO 2 Because the intensity of the adopted ultraviolet radiation is very low, the energy consumption is 3 orders of magnitude lower than that of the low-temperature separation technology, and the method has very low operation energy consumption and low cost. The invention adopts thatAdsorption CO removal by dry radical advanced oxidation technology 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, in the present invention, CO 2 The adsorption efficiency of the catalyst can reach 92.5%, and the catalyst has wide industrial application prospect.
Drawings
FIG. 1 is a schematic illustration of CO removal based on free radical induced multi-element modified porous carbon adsorption 2 Is a schematic of the system.
FIG. 2 is a front view and a size diagram of a photochemical rotating bed modification apparatus.
FIG. 3 is a front view and size diagram of a rotating bed adsorbent device.
FIG. 4 is a diagram showing the arrangement of a first stirring paddle and an ultraviolet lamp tube inside a photochemical rotating bed modification device.
FIG. 5 is a diagram of a second agitator paddle arrangement inside a rotating bed adsorption unit.
FIG. 6 is a diagram of a flue gas distributor arrangement inside a rotating bed adsorption apparatus.
In the figure, a 1-photochemistry rotating bed modifying device; 2-a rotating bed adsorption unit; 3-a first stirring paddle; 3-1-a first paddle cross-sectional view; 4-ultraviolet lamp tube; 4-1-ultraviolet lamp tube section view; 5-modifying gas inlet; 6-modified biochar outlet; 7-biochar inlet; 8-a source of modifying gas; 9-a biochar reserve tank; 10-a microwave activator; 11-biochar feeder; 12-a first material conveying pump; 13-a humidifier; 14-a second stirring paddle; 14-1-a second paddle cross-sectional view; 15-a flue gas distributor; 15-1-gas nozzle cross-section; 15-2-a flue gas duct cross-sectional view; 16-a biochar outlet after adsorption; 17-a second material conveying pump; 18-modified biochar inlet; 19-chimney; 20-cleaning a flue gas outlet; 21-a fan; 22-boiler/kiln; 23-flue gas inlet; 24-flue gas attemperator; 25-bracket
Detailed Description
The invention will be further described with reference to the drawings and the specific embodiments, but the scope of the invention is not limited thereto.
FIG. 1 is a schematic illustration of CO removal based on free radical induced multi-element modified porous carbon adsorption 2 Is a structural schematic diagram of the system of (1), comprising the biological systemA photochemical rotating bed modification device 1 for carbon modification and a rotating bed adsorption device 2 for adsorption removal;
the photochemical rotating bed modification device is internally provided with a plurality of first stirring paddles 3 for improving the suspending capacity and the mixing mass transfer rate of the raw biochar, and a plurality of ultraviolet lamp tubes 4 for decomposing and modifying gas components (mainly comprising H) by ultraviolet radiation 2 O 2 ﹑NH 3 ﹑H 2 S, etc.) generates a plurality of high-activity free radicals (OH, HS, HN, etc.). The photochemical rotating bed modification device 1 is provided with a modification gas inlet 5 connected with a modification gas source 8, and the bottom 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 biochar inlets 7, the biochar inlets 7 are connected with a biochar reserve tank 9 after being converged through a pipeline, and a microwave activator 10, a biochar feeder 11 and a first material conveying pump 12 are sequentially arranged on the pipeline from the biochar reserve 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 after microwave steam activation enters the biochar feeder 11 for quantitative distribution.
The rotating bed adsorption device 2 internally mounted has a plurality of second stirring paddles 14, the bottom surface is equipped with flue gas distributor 15, flue gas distributor 15 comprises 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 adsorb back biochar and fall into rotating bed adsorption device 2 bottom and retrieve the recycle. The bottom of the rotating bed adsorption device 2 is provided with an adsorbed biochar outlet connected with a biochar reserve 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 modified biochar outlets 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 a fan 21 is arranged on the exhaust pipeline; the rotating 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 the boiler/kiln 22 through a gas supply pipeline, and the gas supply pipeline is provided with a flue gas temperature regulator 24; the bottom of the rotating bed adsorption device 2 is also provided with a bracket 25.
Fig. 2 and 4 are front view and size view of the photochemical rotating bed modification apparatus 1, and an arrangement of the inner 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 is inclined at 30-50 degrees; the ultraviolet lamp tubes 4 in the photochemical rotating bed modification device 1 are arranged at equal intervals and in parallel, the interval range of the adjacent ultraviolet lamp tubes 4 is 10-60 cm, and the length of the ultraviolet lamp tubes 4 is 30-200 cm; the first stirring paddles 3 are screw stirring paddles with lifting force, the first stirring paddles 3 are arranged at equal intervals and in a parallel manner, and the length of the first stirring paddles 3 is not shorter than 20cm than that of the ultraviolet lamp tube 4; 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 center line of two adjacent ultraviolet lamp tubes 4.
Fig. 3 is a front view of the rotating bed adsorption device 2 and its size, and fig. 5 and 6 are layout views of the second stirring paddles 14 and the flue gas distributor 15 inside the rotating bed adsorption device 2. Wherein the cross section of the rotating bed adsorption device 2 is rectangular, the height of the rotating bed adsorption device 2 is 40-500 cm, and the lower part of the rotating bed adsorption device 2 is inclined at 50-80 degrees; the second stirring paddles 14 in the rotating bed adsorption device 2 are arranged at equal intervals and in a fork row, the interval between every two adjacent second stirring paddles 14 is 30-160 cm, and the height of each second stirring paddle 14 is not more than 30cm smaller than that of the rotating bed adsorption device 2; the flue gas distributor 15 on the bottom surface of the rotating bed adsorption device 2 comprises a plurality of pipelines and gas nozzles, the pipelines are connected with the gas nozzles, and the distances between the adjacent pipelines and between the adjacent gas nozzles are 5-60 cm.
The invention also provides the method for removing CO based on the free radical-induced multielement modified porous carbon adsorption 2 The system 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 S, calculating the input amount of modifying gas and biochar according to the volume of the photochemical rotating bed modifying device 1; the saidThe biochar comprises biochar obtained by cracking one or more agricultural straws in cornstalks, rice hulls, rice stems, wheat straws, cotton stalks and corncobs, or biochar obtained by cracking 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 biochar=2 volumes (m 3 ) X (0.2-20 kg); the concentration of the modifying gas is 50ppm-5000ppm, and the mass ratio of carbon to gas components between the biochar and the modifying gas is 300:1-20000:1.
(2) Modifying biochar:
the ultraviolet radiation intensity, the ultraviolet effective wavelength, the modification temperature in the photochemical rotating bed modification device 1 and the stirring speed of the first stirring paddle 3 of the ultraviolet lamp tube 4 are preset: the ultraviolet radiation intensity of the ultraviolet lamp tube 4 in the photochemical rotating bed modification device 1 is 10-220 mu W/cm 2 The effective wavelength of ultraviolet light is 100nm-360nm; the stirring speed of the first stirring paddle 3 is 300-3000 r/min; the modification temperature in the photochemical rotating bed modification device 1 ranges from 20 ℃ to 120 ℃.
Then introducing the modified gas and biochar into the photochemistry rotating bed modification device 1, and inducing the modified gas H by using the ultraviolet lamp tube 4 2 O 2 、NH 3 ﹑H 2 One or more of S generates one or more of OH, HS and HN free radicals to attack the surface of the biochar, so that the surface of the biochar generates active sites, and the body process can be represented by the following chemical reaction equations (1) - (4):
n·OH+nHN·+nHS·+Biochar——→Biochar-active sites (4)
(3) Adsorption removal:
the addition amount of the modified biochar in the rotating bed adsorption apparatus 2, the particle diameter of the modified biochar, the stirring speed of the second stirring paddle 14, and the temperature of the adsorption reaction in the rotating bed adsorption apparatus 2 are preset. Addition amount of modified biochar=2 volumes of rotating bed adsorption apparatus (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 rpm, and the temperature of the adsorption reaction is 10-150 ℃; when the modified biochar saturated in adsorption is separated, the stirring speed is 150-1500 rpm.
Subsequently, the modified biochar and the flue gas in the boiler/kiln 22 are introduced into the rotating bed adsorption device 2, and CO in the flue gas is removed by utilizing the active site adsorption on the biochar 2 The biochar after saturation is heated to desorb CO 2 And realize CO 2 And (3) recycling, wherein the treated clean flue gas is discharged into the atmosphere through a chimney 19, and activated modified regeneration of the activated carbon with lost active sites can be realized 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 device for CO in the flue gas under different test conditions 2 Examples of removal efficiency experiments:
example 1:
the modification temperature in the photochemical rotating bed modification device is 25 ℃, and the radiation intensity and 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 catalyst is 500ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 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 wavelength of ultraviolet light are 30 mu W/cm respectively 2 And 254nm, modified gas component H 2 O 2 The adding concentration of the catalyst is 700ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 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 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 catalyst is 1000ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 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 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 is 3 The adding concentration of the catalyst is 100ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 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 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 is 3 The adding concentration of the catalyst is 300ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 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 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 is 3 The adding concentration of the catalyst is 600ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 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 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 is 3 The addition concentration of (C) is 600ppm, and the modified gas component H 2 The adding concentration of S is 300ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 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 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 is 3 The addition concentration of (C) is 600ppm, and the modified gas component H 2 The adding concentration of S is 600ppm, the biochar is microwave activated rice straw carbon, and the adsorption temperature of the rotating bed adsorption device is 25 ℃. The mass concentration of the modified biochar is 2.0 kg/cubic meter of rotating bed adsorption device, and CO in the flue gas 2 The concentration was 10%. The test results are: CO 2 The removal efficiency was 92.5%.
In conclusion, the invention relates to a method for preparing CO based on free radical induced multielement 2 The method for removing the porous carbon adsorbent has the comprehensive advantages of low initial investment and operation cost, high removal efficiency, high gas-solid mass transfer rate, green and environment-friendly process, real-time online activation and regeneration of the adsorbent and the like, and has wide industrial application prospect.
The examples are preferred embodiments of the present invention, but the present invention is not limited to the above-described embodiments, and any obvious modifications, substitutions or variations that can be made by one skilled in the art without departing from the spirit of the present invention are within the scope of the present invention.
Claims (10)
1. Multi-element modified porous carbon adsorption CO removal based on free radical induction 2 Is characterized in that the system comprises a photochemical rotating bed modification device (1) for modifying biochar and a rotating bed adsorption device (2) for adsorbing and removing;
the photochemical rotating bed modification device (1) is internally provided with a plurality of first stirring paddles (3) and a plurality of ultraviolet lamp tubes (4), the photochemical rotating bed modification device (1) is provided with a modification gas inlet (5) connected with a modification gas source (8), and the bottom surface of the photochemical rotating bed modification device (1) 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 biochar inlets (7), the biochar inlets (7) are communicated with a biochar reserve tank (9) through a pipeline, and a microwave activator (10), a biochar feeder (11) and a first material conveying pump (12) are sequentially arranged on the pipeline from the biochar reserve tank (9); the microwave activator (10) is also connected with a humidifier (13);
a plurality of second stirring paddles (14) are arranged in the rotating bed adsorption device (2), and a smoke distributor (15) is arranged on the bottom surface of the rotating bed adsorption device (2); the bottom of the rotating bed adsorption device (2) is provided with an adsorbed biochar outlet (16) communicated with the biochar reserve tank (9), and a second material conveying pump (17) is arranged between the biochar reserve tank (9) and the adsorbed biochar outlet (16); the top of the rotating 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 smoke outlets (20) connected with a chimney (19) through an exhaust pipeline, and the exhaust pipeline is provided with a fan (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 temperature regulator (24) is arranged on the gas supply pipeline; the bottom of the rotating bed adsorption device (2) is also provided with a bracket (25).
2. The method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 1 2 The system is characterized in that the cross section of the photochemical rotating bed modification device (1) is rectangular, the height of the photochemical rotating bed modification device is 50-220 cm, and the inner side of the lower part of the photochemical rotating bed modification device (1) is inclined at 30-50 degrees with the horizontal plane; the ultraviolet lamp tubes (4) in the photochemical rotating bed modification device (1) are arranged at equal intervals and in parallel, the interval range of the adjacent ultraviolet lamp tubes (4) is 10-60 cm, and the length of the ultraviolet lamp tubes (4) is 30-200 cm; the first stirring paddles (3) are screw stirring paddles with lifting force, the first stirring paddles (3) are arranged at equal intervals and in a parallel row, and the length of the first stirring paddles (3) is shorter than that of the ultraviolet lamp tube (4) by not 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 center line of two adjacent ultraviolet lamp tubes (4).
3. The method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 1 2 The system is characterized in that the cross section of the rotating bed adsorption device (2) is rectangular, the height of the rotating bed adsorption device (2) is 40-500 cm, and the inner side of the lower part of the rotating bed adsorption device (2) is inclined at 50-80 degrees with the horizontal plane; the second stirring paddles (14) in the rotating bed adsorption device (2) are arranged at equal intervals and in a fork row, the interval between every two adjacent second stirring paddles (14) is 30-160 cm, and the second stirring paddles (14)The height of the bed is not more than 30cm smaller than the height of the rotating bed adsorption device (2); the flue gas distributor (15) on the bottom surface of the rotating bed adsorption device (2) comprises a plurality of pipelines and gas nozzles, wherein the pipelines are communicated with the gas nozzles, and the distances between the adjacent pipelines and between the adjacent gas nozzles are 5-60 cm.
4. Multi-element modified porous carbon adsorption CO removal based on free radical induction 2 The method is characterized in that the removal method is based on the free radical-induced multi-element modified porous carbon adsorption-based CO removal method according to 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 S, calculating the input amount of modified gas and biochar according to the volume of the photochemical rotating bed modification device;
(2) Modifying biochar:
introducing the modified gas and biochar into a photochemical rotating bed modification device, and inducing the modified gas H by using an ultraviolet lamp tube 2 O 2 、NH 3 ﹑H 2 One or more of S generates one or more of OH, HS and HN free radicals to attack the surface of the biochar, so that active sites are generated on the surface of the biochar;
(3) Adsorption removal:
introducing the modified biochar and the flue gas in the boiler/kiln into a rotating bed adsorption device, and removing CO in the flue gas by utilizing the active site adsorption on the biochar 2 The biochar after saturation is heated to desorb CO 2 And realize CO 2 And (3) recycling, namely 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).
5. The method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 4 2 Is characterized by the steps ofIn the step (1), the biochar comprises biochar obtained by cracking one or more agricultural straws in cornstalks, rice hulls, rice stems, wheat straws, cotton stalks and corncobs, or biochar obtained by cracking municipal sludge, fruit shells and industrial organic wastes; the particle size of the biochar is 0.001-0.5 mu m.
6. The method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 4 2 In the step (1), the amount of the biochar added=the volume (m 3 ) X (0.2-20 kg); the concentration of the modifying gas is 50ppm-5000ppm, and the mass ratio of carbon to gas components between the biochar and the modifying gas is 300:1-20000:1.
7. The method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 4 2 In the step (2), the ultraviolet radiation intensity of the ultraviolet lamp tube (4) in the photochemical rotating bed modification device (1) is 10-220 mu W/cm 2 The effective wavelength of 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 method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 4 2 In the step (3), the addition amount of the modified biochar=the volume (m 3 ) X (0.5-50 kg), the particle size of the modified biochar is 0.002-0.8 μm.
9. The method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 4 2 In the step (3), the stirring speed of the second stirring paddle (14) in the rotating bed adsorption device (2) is 200-2500 rpm, and the temperature of the adsorption reaction is 10-150 ℃.
10. The method for removing CO based on free radical induced multi-element modified porous carbon adsorption according to claim 4 2 In the step (3), when the modified biochar saturated in adsorption is separated, the stirring speed of the second stirring paddle (14) in the rotating bed adsorption device (2) is 150-1500 rpm.
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