CN120242698A - A method for carbon sequestration using alkalinity source - Google Patents
A method for carbon sequestration using alkalinity source Download PDFInfo
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- CN120242698A CN120242698A CN202510409398.2A CN202510409398A CN120242698A CN 120242698 A CN120242698 A CN 120242698A CN 202510409398 A CN202510409398 A CN 202510409398A CN 120242698 A CN120242698 A CN 120242698A
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Abstract
The invention provides a method for realizing carbon sequestration by utilizing an alkalinity source, which comprises the following steps of (1) grinding and crushing the alkalinity source and screening to obtain alkalinity source powder, wherein the alkalinity source comprises olivine, basalt, wollastonite and anorthite, (2) carrying out acid leaching on the alkalinity source powder to obtain a mineral leaching suspension, then reacting the mineral leaching suspension with a pretreatment agent under the conditions of 150 ℃ and 5MPa and a liquid-solid ratio of 20:1 to obtain a pretreated alkalinity source, (3) mixing the pretreated alkalinity source with water, then introducing carbon dioxide gas for carbonation reaction, closing a gas channel after the reaction is finished, and obtaining carbonate mineral after cooling and solid-liquid separation, thereby realizing the sequestration of carbon and realizing the permanent, stable and large-scale sequestration of carbon dioxide.
Description
Technical Field
The invention relates to the technical field of carbon dioxide sealing and storage, in particular to a method for realizing carbon sealing and storage by utilizing an alkalinity source.
Background
As the greenhouse gas content in the atmosphere gradually increases, the global climate changes significantly and the atmospheric concentration of carbon dioxide increases significantly.
At present, the internationally common carbon dioxide control technology mainly comprises three steps of (1) reducing the use of non-renewable energy sources such as fossil fuel (coal, petroleum and natural gas), developing and utilizing renewable energy sources such as geothermal energy, wind energy and biomass energy, reducing the occupation ratio of primary energy consumption by changing an energy structure, (2) improving the energy conversion efficiency, advocating green and energy-saving life, and (3) adopting a carbon dioxide capturing and sealing technology (CCS). Among them, CCS technology is considered as one of the most promising technologies for solving the greenhouse effect, and has a certain feasibility in the treatment of large-scale carbon dioxide sources.
The carbon dioxide sealing mode mainly comprises geological sealing, mineral sealing and marine sealing, wherein the geological sealing is to pour carbon dioxide into a proper stratum under pressure, the carbon dioxide is stored in the pore space of the stratum, the mineral sealing is to enable the carbon dioxide to chemically react with metal oxide to form carbonate and other byproducts in solid forms, and the marine sealing is to pour liquid carbon dioxide into a deep sea water area to form a stable lake-shaped structure under high-pressure conditions.
The mineral sealing and storage method utilizes the chemical reaction of carbon dioxide and certain minerals (such as olivine) to generate stable carbonate minerals, and the sealing and storage method is stable and has no leakage risk. And most of carbon on the earth exists in the form of carbonate minerals, and carbon sequestration in the crystal structure of the minerals is a long-lasting and reliable method, so carbon dioxide mineral sequestration is acknowledged as the safest and reliable sequestration method.
Based on this, when carbon dioxide is sequestered, if dry carbonation is adopted, that is, carbonate is obtained directly by using a gas-solid one-step reaction mode, but the method needs to be carried out at high temperature and high pressure to isolate carbon dioxide from the atmosphere, however, one major disadvantage of the method is that the reaction kinetics of calcium silicate and magnesium silicate are often too slow, and the acceleration of the reaction kinetics by increasing the temperature is often thermodynamically limited. It is therefore important to find a suitable and stable wet carbonation for carbon dioxide sequestration.
Disclosure of Invention
Based on the above problems, it is an object of the present invention to provide a method for carbon sequestration using an alkalinity source which allows permanent, stable and large scale sequestration of carbon dioxide.
The inventor seeks to sequester carbon dioxide in a wet carbonation manner, however, in research and practice the inventor has found that calcium and magnesium ions migrate to the surface of the mineral during the reaction to form carbonate minerals, which encapsulate the mineral and hinder the carbonation reaction and thus affect the sequestering effect. Therefore, the method comprises the steps of firstly carrying out acid leaching pretreatment on an alkalinity source before reaction, firstly dissolving out partial calcium and magnesium ions preferentially, then carbonating the pretreated alkalinity source with carbon dioxide, dissolving the carbon dioxide in a liquid phase to generate carbonic acid, decomposing the carbonic acid into carbonate ions or bicarbonate ions, dissolving out metal ions by the alkalinity source under the proton exchange effect, and carrying out chemical precipitation with the carbonic acid decomposed carbonate ions or bicarbonate ions to form stable carbonate rock mineral, thereby realizing the carbon sequestration.
The implementation mode of the invention is realized by the following technical scheme:
a method for carbon sequestration using an alkalinity source comprising the steps of:
(1) Grinding and crushing an alkalinity source and screening the alkalinity source to the particle size of 30-50 mu m to obtain alkalinity source powder, wherein the alkalinity source comprises olivine, basalt, wollastonite, anorthite and the like;
(2) Acid leaching is carried out on the alkalinity source powder, the liquid-solid ratio during acid leaching is 10-20:1mL/g, thus obtaining an ore leaching suspension, and then the ore leaching suspension and a pretreatment agent are mixed according to the mass ratio of 10-20:1 for reaction, thus obtaining a pretreatment alkalinity source;
(3) Mixing a pretreated alkalinity source and water according to a mass ratio of 1:10-20, adding the mixture into a reaction kettle, stirring the mixture for 5-20min at a stirring speed of 200-300r/min, then introducing carbon dioxide gas, wherein the carbon dioxide gas can be sourced from a carbon dioxide discharge tower or other carbon dioxide discharge towers of a thermal power plant, and carrying out carbonation reaction for 0.5-1.5h at a stirring speed of 200-300r/min under the conditions of 100-200 ℃ and 5-10MPa, closing a gas channel after the reaction is finished, and cooling and carrying out solid-liquid separation to obtain carbonate minerals so as to realize carbon sequestration.
The elevation of the temperature within a certain range can improve the dissolution reaction activity of an alkalinity source in the mineral leaching suspension, accelerate the dissolution of calcium and magnesium ions, increase the concentration of the calcium and magnesium ions in the solution, thereby being beneficial to separating out calcium carbonate and magnesium carbonate and improving the carbonation conversion rate, however, excessive elevation of the temperature also can lead to the reduction of the solubility of carbon dioxide, and lead to the reduction of carbonate radical or bicarbonate radical ions in the solution, thereby being unfavorable for the forward progress of the precipitation reaction, therefore, the inventor controls the reaction temperature within 100-200 ℃ to ensure that the carbonation conversion rate of the carbonation reaction is maximum, and simultaneously has better carbon fixation effect, and better temperature control is 15-180 ℃ and is optimal. The pressure is also controlled within the carbonation conversion range, so that the dissolution of calcium and magnesium ions is accelerated, and more carbonate or bicarbonate ions are generated, so that the carbonation reaction is more efficient.
The acid liquor used in the acid leaching pretreatment is different according to the difference of alkalinity sources, and concretely comprises the following steps of pretreatment of olivine by sulfuric acid, pretreatment of basalt by hydrochloric acid, pretreatment of wollastonite by hydrochloric acid and pretreatment of anorthite by acetic acid.
Wherein, the pretreatment agent is different according to the difference of alkalinity sources, and the specific following steps are adopted:
The pretreatment agent added into the olivine and anorthite mineral leaching suspension under the condition of pH value of 10-11 is 0.50mol/L NaHCO 3 and 1.00mol/L NaCl;
under the condition of pH value of 10, adding a pretreatment agent which is 0.50mol/L NaHCO 3 into the basalt mineral leaching suspension;
The pretreatment agent added into the wollastonite mineral leaching suspension at the pH of 10 is 0.50mol/L NaHCO 3 and 0.25mol/L NaCl.
The NaHCO 3 is used for keeping the concentration of bicarbonate ions in the solution to be higher, and can well regulate pH change caused by dissolution of carbon dioxide while promoting the reaction, reduce the resistance in the formation process of calcium carbonate and magnesium carbonate, and the addition of NaCl can improve the solubility of silicate minerals, thereby promoting the leaching of calcium and magnesium ions and promoting the reaction. When NaHCO 3 and NaCl are mixed for use, the synergistic effect of the two components can further improve the carbonation conversion rate, mainly because NaCl is completely ionized in suspension, the salt ion effect is fully exerted, and the solubility of calcium carbonate is improved while the dissolution of wollastonite is promoted.
In addition, the mass ratio of the mineral leaching suspension to the pretreatment agent is controlled to be 10-20:1, and the increase of the liquid-solid ratio is not only beneficial to the dispersion of an alkalinity source, but also reduces the wrapping of the surface of the mineral by the generated carbonate mineral, so that the carbonation reaction efficiency is improved, and more carbonate minerals can be generated within a certain time.
Finally, it should be noted that the carbon dioxide gas of the present invention may originate from a carbon dioxide emission tower or other carbon dioxide emission points of a thermal power plant, such as a power plant, a metallurgical plant, an oil refinery, etc., where the carbon emission points preferably themselves generate alkalinity sources, especially mines, and surrounding rocks of many mining areas are such as olivine rocks and basalt rocks, while the downstream beneficiation metallurgical process has a large amount of carbon emission, and the two areas are generally very close together, so that the carbon emission of each process can be reduced, and the coal mine is also similar. The carbon emission is carried out, and meanwhile, the permanent sealing and storage of carbon dioxide are realized, so that the development goal of green low carbon is realized.
The technical scheme of the embodiment of the invention has at least the following advantages and beneficial effects:
1. the method comprises the steps of sealing and storing carbon dioxide in a wet carbonation mode, carrying out acid leaching pretreatment on an alkalinity source before reaction, firstly dissolving out partial calcium and magnesium ions preferentially, avoiding that the calcium and magnesium ions migrate to the surface of the alkalinity source mineral in the reaction process to generate carbonate minerals so as to prevent the subsequent carbonation reaction from being carried out and affecting the sealing and storing effect, and carrying out carbonation reaction on the pretreated alkalinity source and the carbon dioxide to form stable carbonate minerals, thereby realizing the sealing and storing of the carbon.
2. In the invention, different alkalinity sources are treated by different acids and then mixed with different pretreatment agents to obtain the pretreated alkalinity sources, so that the carbonation conversion rate is improved and the carbon sealing quantity is also improved in the carbonation reaction process, thereby realizing the permanent, stable and large-scale sealing of carbon dioxide.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention more clear, the technical solutions of the embodiments of the present invention will be clearly and completely described below. The specific conditions are not noted in the examples and are carried out according to conventional conditions or conditions recommended by the manufacturer. The reagents or apparatus used were conventional products commercially available without the manufacturer's attention.
Example 1
A method for carbon sequestration using an alkalinity source comprising the steps of:
(1) Grinding and crushing an alkalinity source and screening the alkalinity source to obtain alkalinity source powder with the particle size of 38 mu m, wherein the alkalinity source comprises olivine, basalt, wollastonite and anorthite;
(2) Acid leaching is carried out on the alkalinity source powder, the liquid-solid ratio during acid leaching is 10:1mL/g, thus obtaining an ore leaching suspension, and then the ore leaching suspension and a pretreatment agent are mixed according to the mass ratio of 20:1 for reaction, thus obtaining a pretreatment alkalinity source;
wherein, during acid leaching, sulfuric acid is utilized to pretreat olivine, hydrochloric acid is utilized to pretreat basalt, hydrochloric acid is utilized to pretreat wollastonite, and acetic acid is utilized to pretreat anorthite;
the pretreatment agent is different according to the alkalinity sources, and the pretreatment agent is concretely as follows:
The pretreatment agent added into the olivine and anorthite mineral leaching suspension at pH 11 is NaHCO 3 with the concentration of 0.50mol/L and NaCl with the concentration of 1.00 mol/L;
Under the condition of pH value of 10, adding a pretreatment agent of 0.50mol/L NaHCO 3 into the basalt mineral leaching suspension;
The pretreatment agent added into wollastonite mineral leaching suspension liquid under the condition of pH 10 is NaHCO 3 with the concentration of 0.50mol/L and NaCl with the concentration of 0.25 mol/L;
(3) Mixing the pretreated alkalinity source and water according to the mass ratio of 1:20, adding into a reaction kettle, stirring for 10min at the stirring speed of 260r/min, then introducing carbon dioxide gas of a carbon dioxide discharge tower of a thermal power plant, performing carbonation reaction for 1h at the stirring speed of 240r/min under the conditions of 180 ℃ and 8MPa, closing a gas channel after the reaction is finished, and cooling and separating solid from liquid to obtain carbonate minerals, thereby realizing the carbon sequestration.
Example 2
A method for carbon sequestration using an alkalinity source comprising the steps of:
(1) Grinding and crushing an alkalinity source and screening the alkalinity source to obtain alkalinity source powder with the particle size of 33 mu m, wherein the alkalinity source comprises olivine, basalt, wollastonite and anorthite;
(2) Acid leaching is carried out on the alkalinity source powder, the liquid-solid ratio during acid leaching is 15:1mL/g, thus obtaining an ore leaching suspension, and then the ore leaching suspension and a pretreatment agent are mixed according to the mass ratio of 20:1 for reaction, thus obtaining a pretreatment alkalinity source;
wherein, during the acid leaching pretreatment, sulfuric acid is utilized to pretreat olivine, hydrochloric acid is utilized to pretreat basalt, hydrochloric acid is utilized to pretreat wollastonite, and acetic acid is utilized to pretreat anorthite;
the pretreatment agent is different according to the alkalinity sources, and the pretreatment agent is concretely as follows:
The pretreatment agent added into the olivine and anorthite mineral leaching suspension at pH of 10 is NaHCO 3 with the concentration of 0.50mol/L and NaCl with the concentration of 1.00 mol/L;
Under the condition of pH value of 10, adding a pretreatment agent of 0.50mol/L NaHCO 3 into the basalt mineral leaching suspension;
The pretreatment agent added into wollastonite mineral leaching suspension liquid under the condition of pH 10 is NaHCO 3 with the concentration of 0.50mol/L and NaCl with the concentration of 0.25 mol/L;
(3) Mixing the pretreated alkalinity source and water according to the mass ratio of 1:20, adding into a reaction kettle, stirring for 20min at the stirring speed of 200r/min, then introducing carbon dioxide gas of a carbon dioxide discharge tower of a thermal power plant, performing carbonation reaction for 1h at the stirring speed of 280r/min under the conditions of 120 ℃ and 6MPa, closing a gas channel after the reaction is finished, and cooling and separating solid from liquid to obtain carbonate minerals, thereby realizing the carbon sequestration.
Example 3
A method for carbon sequestration using an alkalinity source comprising the steps of:
(1) Grinding and crushing an alkalinity source and screening the alkalinity source to obtain alkalinity source powder with the particle size of 42 mu m, wherein the alkalinity source comprises olivine, basalt, wollastonite and anorthite;
(2) Acid leaching is carried out on the alkalinity source powder, the liquid-solid ratio during acid leaching is 10:1mL/g, thus obtaining an ore leaching suspension, and then the ore leaching suspension and a pretreatment agent are mixed according to the mass ratio of 20:1 for reaction, thus obtaining a pretreatment alkalinity source;
wherein, during the acid leaching pretreatment, sulfuric acid is utilized to pretreat olivine, hydrochloric acid is utilized to pretreat basalt, hydrochloric acid is utilized to pretreat wollastonite, and acetic acid is utilized to pretreat anorthite;
the pretreatment agent is different according to the alkalinity sources, and the pretreatment agent is concretely as follows:
The pretreatment agent added into the olivine and anorthite mineral leaching suspension at pH of 10.5 is NaHCO 3 with the concentration of 0.50mol/L and NaCl with the concentration of 1.00 mol/L;
Under the condition of pH value of 10, adding a pretreatment agent of 0.50mol/L NaHCO 3 into the basalt mineral leaching suspension;
The pretreatment agent added into wollastonite mineral leaching suspension liquid under the condition of pH 10 is NaHCO 3 with the concentration of 0.50mol/L and NaCl with the concentration of 0.25 mol/L;
(3) Mixing the pretreated alkalinity source and water according to the mass ratio of 1:20, adding into a reaction kettle, stirring for 5min at the stirring speed of 300r/min, then introducing carbon dioxide gas of a carbon dioxide discharge tower of a thermal power plant, performing carbonation reaction for 1h at the stirring speed of 200r/min and under the conditions of 160 ℃ and 7MPa, closing a gas channel after the reaction is finished, and cooling and separating solid from liquid to obtain carbonate minerals, thereby realizing the carbon sequestration.
Comparative example 1
The comparative example differs from example 1 in that step (2) was not included.
Comparative example 2
This comparative example differs from example 1 in that in step (2), the alkalinity source powder is not subjected to acid leaching treatment.
Comparative example 3
This comparative example differs from example 1 in that in step (2) the mineral leaching suspension is not reacted with the pretreatment agent.
Experimental example
1. The carbonation conversion and carbon sequestration amount in each example and comparative example were separately tested and the test results are shown in Table 1, wherein the carbonation conversion was measured by measuring the initial amount of CO 2 before the reaction (gas chromatography), filtering the solid product after the reaction, measuring the amount of CO 2 released after acidolysis (hydrochloric acid titration), the conversion = (reaction consumed CO 2 amount/initial CO 2 amount) ×100%, and the carbon sequestration amount was measured by measuring the total amount of carbonate in the product by chemical analysis, converting to CO 2 sequestration amount in combination with molar mass, specifically by extracting and purifying the carbonate product, and calculating the corresponding amount of CO 2 by stoichiometric relation.
Table 1-test results for each example and comparative example
| Carbonation conversion (%) | Carbon inventory (mol/kg) | |
| Example 1 | 91.5 | 9.23 |
| Example 2 | 90.8 | 9.20 |
| Example 3 | 91.2 | 9.21 |
| Comparative example 1 | 58.6 | 5.2 |
| Comparative example 2 | 36.2 | 3.1 |
| Comparative example 3 | 25.7 | 2.4 |
The results in table 1 show that the method comprises the steps of firstly carrying out acid leaching pretreatment on the alkalinity source before reaction, firstly dissolving out part of calcium and magnesium ions preferentially, and then carbonating the pretreated alkalinity source with carbon dioxide, so that the carbon is stored, more importantly, the carbonation conversion rate and the carbon storage quantity are improved, carbonate minerals are prevented from being generated by migration of the calcium and magnesium ions to the surfaces of the minerals in the carbonation reaction process of the alkalinity source and the carbon dioxide, and the part of carbonate minerals can wrap the minerals to hinder the carbonation reaction, so that the storage effect is affected.
The above is only a preferred embodiment of the present invention, and is not intended to limit the present invention, but various modifications and variations can be made to the present invention by those skilled in the art. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1.A method for achieving carbon sequestration using an alkalinity source, comprising the steps of:
(1) Grinding and crushing the alkalinity source and screening to obtain alkalinity source powder with the particle size of 30-50 mu m;
(2) Acid leaching is carried out on the alkalinity source powder to obtain an ore leaching suspension, and then the ore leaching suspension reacts with a pretreatment agent under the conditions of 150 ℃ and 5MPa and a liquid-solid ratio of 20:1 to obtain a pretreatment alkalinity source;
(3) And after the reaction is finished, closing a gas channel, cooling and carrying out solid-liquid separation to obtain carbonate minerals, thereby realizing the carbon sealing.
2. The method for carbon sequestration using an alkalinity source according to claim 1, wherein in step (1), the alkalinity source is ground and crushed and sieved to a particle size of 30-50 μm.
3. The method for carbon sequestration using an alkalinity source according to claim 1, wherein in step (1), the alkalinity source comprises olivine, basalt, wollastonite, anorthite.
4. The method for carbon sequestration using an alkalinity source according to claim 1, wherein in step (2), when the alkalinity source powder is subjected to acid leaching, the acid liquor used is different according to the alkalinity source, concretely comprising the steps of pretreatment of olivine with sulfuric acid, pretreatment of basalt with hydrochloric acid, pretreatment of wollastonite with hydrochloric acid, and pretreatment of anorthite with acetic acid.
5. The method for carbon sequestration using an alkalinity source according to claim 4, wherein in step (2), the pretreatment agents used are different depending on the alkalinity source, and specifically, the pretreatment agents added to the olivine and anorthite mineral leaching suspensions are 0.50mol/L NaHCO 3 and 1.00mol/L NaCl, the pretreatment agents added to the basalt mineral leaching suspensions are 0.50mol/L NaHCO 3, and the pretreatment agents added to the wollastonite mineral leaching suspensions are 0.50mol/L NaHCO 3 and 0.25mol/L NaCl.
6. The method for carbon sequestration using an alkalinity source according to claim 1, wherein in step (2), the liquid-solid ratio at the time of pickling is 10-20:1ml/g.
7. The method for carbon sequestration using an alkalinity source according to claim 1, wherein in step (2), the mass ratio of the mineral leaching suspension to the pretreatment agent is 10-20:1.
8. The method for carbon sequestration using an alkalinity source according to claim 1, wherein the reaction conditions for the carbonation reaction in step (3) are 100 to 200 ℃ and 5 to 10MPa.
9. The method for carbon sequestration using an alkalinity source according to claim 1, wherein in step (3), the reaction is carried out for 0.5 to 1.5 hours under stirring speed of 200 to 300 r/min.
10. The method for carbon sequestration using an alkalinity source according to claim 1, wherein in step (3), the carbon dioxide gas is derived from a carbon dioxide discharge tower.
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