CN117398966A - Carbon dioxide adsorbent and preparation method and application thereof - Google Patents
Carbon dioxide adsorbent and preparation method and application thereof Download PDFInfo
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- CN117398966A CN117398966A CN202311428074.0A CN202311428074A CN117398966A CN 117398966 A CN117398966 A CN 117398966A CN 202311428074 A CN202311428074 A CN 202311428074A CN 117398966 A CN117398966 A CN 117398966A
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- carbon dioxide
- dioxide adsorbent
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 107
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 53
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 53
- 239000003463 adsorbent Substances 0.000 title claims abstract description 45
- 238000002360 preparation method Methods 0.000 title claims abstract description 15
- 229920001661 Chitosan Polymers 0.000 claims abstract description 37
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims abstract description 36
- 239000012153 distilled water Substances 0.000 claims abstract description 26
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 26
- 238000003756 stirring Methods 0.000 claims abstract description 24
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 22
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims abstract description 20
- 239000002114 nanocomposite Substances 0.000 claims abstract description 20
- 238000001179 sorption measurement Methods 0.000 claims abstract description 19
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 16
- 238000010000 carbonizing Methods 0.000 claims abstract description 16
- 238000001035 drying Methods 0.000 claims abstract description 16
- 238000010438 heat treatment Methods 0.000 claims abstract description 16
- 239000011259 mixed solution Substances 0.000 claims abstract description 16
- 238000005406 washing Methods 0.000 claims abstract description 16
- 238000010335 hydrothermal treatment Methods 0.000 claims abstract description 12
- 230000003213 activating effect Effects 0.000 claims abstract description 10
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 10
- 239000005543 nano-size silicon particle Substances 0.000 claims abstract description 10
- 235000012239 silicon dioxide Nutrition 0.000 claims abstract description 10
- 238000000227 grinding Methods 0.000 claims abstract description 8
- 238000002156 mixing Methods 0.000 claims abstract description 8
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 8
- 238000000967 suction filtration Methods 0.000 claims abstract description 8
- 238000000034 method Methods 0.000 claims description 12
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 claims description 6
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 6
- 239000012190 activator Substances 0.000 claims description 4
- 239000000377 silicon dioxide Substances 0.000 claims 1
- 230000000694 effects Effects 0.000 abstract description 5
- 238000004134 energy conservation Methods 0.000 abstract description 2
- 230000007613 environmental effect Effects 0.000 abstract description 2
- 230000000052 comparative effect Effects 0.000 description 7
- 230000007935 neutral effect Effects 0.000 description 5
- 239000002244 precipitate Substances 0.000 description 5
- 230000009286 beneficial effect Effects 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 239000003575 carbonaceous material Substances 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000001514 detection method Methods 0.000 description 2
- 238000005265 energy consumption Methods 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 1
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonium chloride Substances [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 1
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 235000011114 ammonium hydroxide Nutrition 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 229910002090 carbon oxide Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 239000013310 covalent-organic framework Substances 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 239000012621 metal-organic framework Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 230000009972 noncorrosive effect Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/10—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate
- B01J20/103—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising silica or silicate comprising silica
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
- B01J20/26—Synthetic macromolecular compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/504—Carbon dioxide
-
- 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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- Chemical & Material Sciences (AREA)
- Analytical Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
The invention belongs to the technical field of carbon dioxide adsorption, and particularly relates to a carbon dioxide adsorbent, and a preparation method and application thereof. The preparation method comprises the following steps: 1) Adding chitosan and nano silicon dioxide into distilled water, uniformly stirring, then adding acetic acid under the condition of stirring, and continuously stirring to obtain uniform mixed solution; 2) Carrying out hydrothermal treatment on the mixed solution obtained in the step 1), then carrying out suction filtration, washing with distilled water, and drying to obtain the protonated chitosan nanocomposite; 3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) with an activating agent, heating and carbonizing under the nitrogen condition, alternately washing with hydrochloric acid and distilled water, and drying to obtain the carbon dioxide adsorbent. The prepared carbon dioxide adsorbent has a porous structure, a relatively high specific surface area, excellent carbon dioxide adsorption capacity and remarkable effects in the fields of environmental protection, energy conservation, emission reduction and the like.
Description
Technical Field
The invention belongs to the technical field of carbon dioxide adsorption, and particularly relates to a carbon dioxide adsorbent, and a preparation method and application thereof.
Background
During the fuel combustion process, a large amount of greenhouse gases are generated, of which more than nine are carbon dioxide. The elevated concentration of carbon dioxide in the atmosphere is a major cause of global warming and climate change. At present, the technology of absorbing carbon dioxide by liquid ammonia solution is widely applied in industry, but the defects of high energy consumption for desorption, solvent degradation, secondary pollution, equipment rust and the like exist. Membrane separation technology has advantages of low energy consumption and non-corrosive compound use, however, the problems of membrane regeneration and purity of separated compounds remain to be solved, which limits its application in the field of carbon dioxide capture and removal.
In order to solve the problems faced by the adsorption separation technology, adsorbents have been widely used in the field of carbon oxide adsorption technology, including porous adsorbents such as metal organic frameworks, covalent organic frameworks, silicate-based materials, metal oxide-based adsorbents, porous carbonaceous materials, and the like. Among these adsorbents, highly porous carbonaceous adsorbents exhibit unique advantages such as low cost, chemical inertness, high stability, high porosity, and easy recovery. Researchers have developed various methods to improve the morphology, composition and structural characteristics of porous carbonaceous materials to enhance their carbon dioxide adsorption properties.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide the carbon dioxide adsorbent which is of a porous structure, has higher specific surface area and excellent carbon dioxide adsorption capacity, and has remarkable effects in the fields of environmental protection, energy conservation, emission reduction and the like;
another object of the present invention is to provide a method for preparing a carbon dioxide adsorbent and use thereof.
The technical scheme adopted by the invention is as follows:
the preparation method of the carbon dioxide adsorbent is characterized by comprising the following steps:
1) Adding chitosan and nano silicon dioxide into distilled water, uniformly stirring, then adding acetic acid under the condition of stirring, and continuously stirring to obtain uniform mixed solution;
2) Carrying out hydrothermal treatment on the mixed solution obtained in the step 1), then carrying out suction filtration, washing with distilled water, and drying to obtain the protonated chitosan nanocomposite;
3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) with an activating agent, heating and carbonizing under the nitrogen condition, alternately washing with hydrochloric acid and distilled water, and drying to obtain the carbon dioxide adsorbent.
The mass ratio of the chitosan to the nano silicon dioxide in the step 1) is (1-3) 1.
The mass volume ratio of the chitosan to the distilled water in the step 1) is 1 (25-30), and the mass volume ratio of the chitosan to the acetic acid is 1 (6-8).
The temperature of the hydrothermal treatment in the step 2) is 100-120 ℃ and the time is 2-3h.
The mass ratio of the protonated chitosan nanocomposite to the activator in the step 3) is 1 (1-3).
The heating and carbonizing temperature in the step 3) is 150-180 ℃ and the time is 2-4h.
The activating agent in the step 3) is one of potassium hydroxide or sodium hydroxide; the concentration of the hydrochloric acid is 0.1-1mol/L.
The carbon dioxide adsorbent is prepared by the preparation method of the carbon dioxide adsorbent.
The application of the carbon dioxide adsorbent is used for adsorbing carbon dioxide.
Acetic acid in the invention acts as an additive in the hydrothermal treatment process, the accessibility of the activating agent is increased by protonating chitosan, and the existence of the acetic acid is beneficial to the dissolution of the chitosan, so that more net-shaped porous structures are generated in the hydrothermal treatment process. The existence of the nano silicon dioxide is beneficial to improving the specific surface area and the surface activity, so that the stability and the dispersity of the adsorbent are improved, the nano silicon dioxide and the chitosan form the protonated chitosan nanocomposite together, and the protonated chitosan nanocomposite has a good carbon dioxide adsorption effect.
Compared with the prior art, the invention has the following beneficial effects:
(1) The carbon dioxide adsorbent disclosed by the invention is of a porous structure, has a relatively high specific surface area, can provide more adsorption sites, and is beneficial to improving the adsorption rate and adsorption capacity of carbon dioxide; and good channel transmission performance is ensured, so that carbon dioxide can rapidly enter and diffuse into the adsorbent in the adsorption process, and the adsorption effect is further improved;
(2) The preparation method of the carbon dioxide adsorbent is simple in preparation process and easy to control; in addition, the used raw materials and the activator have wide sources and low cost, and the production cost of the adsorbent is further reduced.
Detailed Description
The invention is further illustrated below with reference to examples, which are not intended to limit the practice of the invention.
The raw materials used in examples and comparative examples, unless otherwise specified, were conventional commercially available products.
Example 1
The preparation method of the carbon dioxide adsorbent comprises the following steps:
1) Respectively adding 10g of chitosan and nano silicon dioxide into 300mL of distilled water, stirring for 3h, slowly adding 80mL of acetic acid under the stirring condition, and continuously stirring for 3h to obtain a uniform mixed solution;
2) And (3) carrying out hydrothermal treatment on the mixed solution obtained in the step (1) at the temperature of 120 ℃ for 3 hours, and then carrying out suction filtration to obtain brown precipitate. Washing with distilled water until the pH is 7, and drying to obtain the protonated chitosan nanocomposite;
3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) and an activating agent according to the mass ratio of 1:3, heating and carbonizing under the condition of nitrogen, wherein the heating and carbonizing temperature is 180 ℃, the heating and carbonizing time is 3 hours, alternately washing with 1mol/L hydrochloric acid and distilled water until neutral pH is obtained, and drying to obtain the carbon dioxide adsorbent.
Example 2
The preparation method of the carbon dioxide adsorbent comprises the following steps:
1) Respectively adding 10g of chitosan and 7g of nano silicon dioxide into 280mL of distilled water, stirring for 3h, slowly adding 70mL of acetic acid under the stirring condition, and continuously stirring for 3h to obtain a uniform mixed solution;
2) And 2) carrying out hydrothermal treatment on the mixed solution obtained in the step 1) at the temperature of 110 ℃ for 2 hours, and then carrying out suction filtration to obtain brown precipitate. Washing with distilled water until the pH is 7, and drying to obtain the protonated chitosan nanocomposite;
3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) and an activating agent according to the mass ratio of 1:2, heating and carbonizing under the condition of nitrogen at 170 ℃ for 3 hours, alternately washing with 0.5mol/L hydrochloric acid and distilled water until neutral pH is obtained, and drying to obtain the carbon dioxide adsorbent.
Example 3
The preparation method of the carbon dioxide adsorbent comprises the following steps:
1) Respectively adding 10g of chitosan and 5g of nano silicon dioxide into 250mL of distilled water, stirring for 3h, slowly adding 60mL of acetic acid under the stirring condition, and continuously stirring for 3h to obtain a uniform mixed solution;
2) And (3) carrying out hydrothermal treatment on the mixed solution obtained in the step (1) at the temperature of 100 ℃ for 3 hours, and then carrying out suction filtration to obtain brown precipitate. Washing with distilled water until the pH is 7, and drying to obtain the protonated chitosan nanocomposite;
3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) and an activating agent according to the mass ratio of 1:1, heating and carbonizing under the condition of nitrogen at 150 ℃ for 4 hours, alternately washing with 0.1mol/L hydrochloric acid and distilled water until neutral pH is obtained, and drying to obtain the carbon dioxide adsorbent.
Comparative example 1
The preparation method of the carbon dioxide adsorbent comprises the following steps:
1) Adding 10g of chitosan into 300mL of distilled water, stirring for 3h, slowly adding 80mL of acetic acid under the stirring condition, and continuously stirring for 3h to obtain a uniform mixed solution;
2) And (3) carrying out hydrothermal treatment on the mixed solution obtained in the step (1) at the temperature of 120 ℃ for 3 hours, and then carrying out suction filtration to obtain brown precipitate. Washing with distilled water until the pH is 7, and drying to obtain the protonated chitosan nanocomposite;
3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) and an activating agent according to the mass ratio of 1:3, heating and carbonizing under the condition of nitrogen, wherein the heating and carbonizing temperature is 180 ℃, the heating and carbonizing time is 3 hours, alternately washing with 1mol/L hydrochloric acid and distilled water until neutral pH is obtained, and drying to obtain the carbon dioxide adsorbent.
Comparative example 2
The preparation method of the carbon dioxide adsorbent comprises the following steps:
1) Respectively adding 10g of chitosan and nano silicon dioxide into 300mL of distilled water, stirring for 3h, slowly adding 80mL of acetic acid under the stirring condition, and continuously stirring for 3h to obtain a uniform mixed solution;
2) And (3) carrying out hydrothermal treatment on the mixed solution obtained in the step (1) at the temperature of 120 ℃ for 3 hours, and then carrying out suction filtration to obtain brown precipitate. Washing with distilled water until the pH is 7, and drying to obtain the protonated chitosan nanocomposite;
3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) and an activating agent according to the mass ratio of 1:0.3, heating and carbonizing under the condition of nitrogen, wherein the heating and carbonizing temperature is 180 ℃, the heating and carbonizing time is 3 hours, alternately washing with 1mol/L hydrochloric acid and distilled water until neutral pH is obtained, and drying to obtain the carbon dioxide adsorbent.
The detection method comprises the following steps:
specific surface area (m) of carbon dioxide adsorbent using BET test 2 /g) and an adsorption amount (mg/g), wherein the adsorption amount is carried out under a pressure of 0.1MPa at 25 ℃.
The results of the tests of the examples and comparative examples are shown in Table 1.
Table 1 results of the tests of examples and comparative examples
Project | Example 1 | Example 2 | Example 3 | Comparative example 1 | Comparative example 2 |
Specific surface area | 3732 | 3594 | 3347 | 3084 | 3517 |
Adsorption quantity | 418 | 397 | 381 | 327 | 325 |
From the detection data, it can be seen that the carbon dioxide adsorbent prepared by the invention has higher specific surface area and excellent carbon dioxide adsorption capacity, and is suitable for being applied to the field of carbon dioxide adsorption.
Claims (9)
1. The preparation method of the carbon dioxide adsorbent is characterized by comprising the following steps:
1) Adding chitosan and nano silicon dioxide into distilled water, uniformly stirring, then adding acetic acid under the condition of stirring, and continuously stirring to obtain uniform mixed solution;
2) Carrying out hydrothermal treatment on the mixed solution obtained in the step 1), then carrying out suction filtration, washing with distilled water, and drying to obtain the protonated chitosan nanocomposite;
3) Mixing and grinding the protonated chitosan nanocomposite obtained in the step 2) with an activating agent, heating and carbonizing under the nitrogen condition, alternately washing with hydrochloric acid and distilled water, and drying to obtain the carbon dioxide adsorbent.
2. The method for preparing carbon dioxide adsorbent according to claim 1, wherein the mass ratio of chitosan to nano silica in the step 1) is (1-3): 1.
3. The method for preparing carbon dioxide adsorbent according to claim 1, wherein the mass-to-volume ratio of chitosan to distilled water in the step 1) is 1 (25-30), and the mass-to-volume ratio of chitosan to acetic acid is 1 (6-8).
4. The method for preparing carbon dioxide adsorbent according to claim 1, wherein the hydrothermal treatment in step 2) is carried out at a temperature of 100-120 ℃ for a time of 2-3 hours.
5. The method for preparing carbon dioxide adsorbent according to claim 1, wherein the mass ratio of the protonated chitosan nanocomposite to the activator in the step 3) is 1 (1-3).
6. The method for preparing carbon dioxide adsorbent according to claim 1, wherein the heating and carbonizing temperature in step 3) is 150-180 ℃ for 2-4h.
7. The method for preparing carbon dioxide adsorbent according to claim 1, wherein the activator in the step 3) is one of potassium hydroxide or sodium hydroxide; the concentration of the hydrochloric acid is 0.1-1mol/L.
8. A carbon dioxide adsorbent prepared by the method of any one of claims 1 to 7.
9. Use of a carbon dioxide adsorbent according to claim 8 for carbon dioxide adsorption.
Priority Applications (1)
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CN202311428074.0A CN117398966A (en) | 2023-10-31 | 2023-10-31 | Carbon dioxide adsorbent and preparation method and application thereof |
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