Method for capturing and mineralizing CO2 by metal-based desulfurization product and coupling regeneration and recycling of sulfur resource
By reducing the metal-based desulfurization product with sulfur, a slurry captures CO2 and using iron (III) chelate solution to recover elemental sulfur, the problems of desulfurization product emissions and carbon sequestration in the prior art are solved, and resource recycling and efficient carbon emission reduction are achieved.
Patent Information
- Application Number
- CN202411448336.4
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- Filing Date
- 2024-10-17
- Publication Date
- 2025-04-15
AI Technical Summary
The existing carbon sequestration methods have defects, calcium/magnesium/sodium-based desulfurization products are severely emitted, and related technologies cannot effectively solve the problem of carbon sequestration, and there is a risk of environmental pollution and resource waste.
By mixing the metal-based desulfurization product with sulfur for reduction reaction, metal sulfide is obtained and mixed with water to form a slurry, mineralized CO2 is captured to form carbonate and H2S gas. The H2S gas was treated with iron (III) chelate solution, the elemental sulfur was recovered and returned to the reduction reaction.
The combination of low-cost treatment of metal-based desulfurization products and carbon emission reduction has been achieved, sulfur resources have been recovered, carbonate products with economic value have been generated, and environmental, economic and social benefits have been improved.
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Figure CN119822393A_ABST
Abstract
Description
Technical Field
[0001] The present invention relates to the technical field of resource utilization, and in particular to a method for metal-based desulfurization product capture and mineralization of CO2 coupled with sulfur resource regeneration and recycling. Background Art
[0002] Carbon dioxide is a common compound in the air. It is a colorless and odorless gas at room temperature. Its density is slightly greater than that of air. It can dissolve in water and generate carbonic acid. Due to the influence of human activities, the current carbon dioxide content on the earth has soared, leading to the greenhouse effect, global warming, glacier melting, and sea level rise. Carbon capture is the collection of carbon dioxide produced in the industrial production process to prevent it from entering the atmosphere, thereby helping to reduce carbon emissions; carbon sequestration is the storage of captured carbon dioxide. The existing carbon storage technologies mainly include deep sea storage, alkaline soil storage, and coal seam, natural gas, and oil layer storage. However, the related technology concentrates and liquefies the collected carbon dioxide, solidifies it, and then buries it deep underground and in the deep sea. First, in the long run, it cannot solve the carbon sequestration problem well; second, the amount of carbon stored is limited and the cost is huge; third, it will leave serious ecological crisis risks.
[0003] A large amount of SO2 is generated during the combustion of coal. In order to meet the flue gas SO2 emission standards, about 92% of the flue gas desulfurization units of coal-fired power plants use the limestone-gypsum method for flue gas desulfurization. Desulfurization gypsum is a solid byproduct of the reaction of limestone slurry absorbing sulfur dioxide. Its main component is CaSO4·2H2O. The unused desulfurization gypsum storage occupies a large amount of land and is prone to secondary pollution. The magnesium oxide desulfurization process is a desulfurization process second only to the calcium method in maturity. It has been widely used and has the characteristics of no blockage, easy control and management, simple operation, high desulfurization efficiency and low operating cost. However, the magnesium oxide desulfurization process will produce a large amount of desulfurization waste liquid, the main substance of which is MgSO4. Most of the desulfurization waste liquid is directly discharged into the environment, causing environmental pollution. The sodium-alkali desulfurization method uses alkaline substances such as NaOH or NaHCO3 as absorbents to absorb SO2 in flue gas, and the removal rate can reach more than 99%. Its main characteristics are high desulfurization agent utilization rate, high desulfurization efficiency, low system failure rate and high equipment availability. However, if the by-product desulfurization liquid with Na2SO4 as the main component is not properly handled, it will pollute the environment and waste resources.
[0004] It can be seen that the existing carbon fixation methods still have defects, and the emission of calcium / magnesium / sodium-based desulfurization products is an increasingly serious problem, all of which need to be improved. Summary of the invention
[0005] In view of this, the purpose of the present invention is to provide a method for metal-based desulfurization product capture and mineralization of CO2 coupled with sulfur resource regeneration and recycling. The present invention can combine the treatment and disposal of solid waste with CO2 emission reduction, while realizing the resource recycling of sulfur elements, and can obtain carbonate products, creating higher environmental, economic and social benefits.
[0006] In order to achieve the above-mentioned object of the invention, the present invention provides the following technical solutions:
[0007] The present invention provides a method for capturing mineralized CO2 with metal-based desulfurization products and coupling sulfur resource regeneration and recycling, comprising the following steps:
[0008] The metal-based desulfurization product and sulfur are mixed and subjected to a reduction reaction to obtain a metal sulfide;
[0009] mixing the metal sulfide and water to obtain a slurry;
[0010] A gas containing CO2 is introduced into the slurry to capture the mineralized CO2 and obtain a gas containing H2S and carbonate;
[0011] The H2S-containing gas is introduced into an iron (III) chelate solution to undergo an oxidation-reduction reaction to obtain elemental sulfur; and the elemental sulfur is reused in the reduction reaction.
[0012] Preferably, the metal-based desulfurization product includes one or more of calcium sulfate, magnesium sulfate and sodium sulfate.
[0013] Preferably, the mixing of the metal-based desulfurization product and sulfur comprises: drying the metal-based desulfurization product to obtain a pretreated metal-based desulfurization product; and mixing the pretreated metal-based desulfurization product and sulfur.
[0014] Preferably, the drying temperature is 100-200° C., and the drying time is 0.5-1.5 hours.
[0015] Preferably, the metal-based desulfurization product is SO4 2- The sulfur is calculated as S, and the molar ratio of the metal-based desulfurization product to sulfur is 1:1-5.
[0016] Preferably, the temperature of the reduction reaction is 500-1150° C., and the insulation time is 0.5-4 h.
[0017] Preferably, the mass ratio of the metal sulfide to water is 1:10-200.
[0018] Preferably, the temperature of capturing mineralized CO2 is 25-60°C.
[0019] Preferably, the raw materials for preparing the iron (III) chelate solution include trivalent iron salt, organic acid, NaHCO3, Na2CO3 and water.
[0020] Preferably, the iron (III) chelate solution contains Fe 3+ The concentration is 0.05~3mol / L.
[0021] The present invention provides a method for metal-based desulfurization product to capture mineralized CO2 coupled with sulfur resource regeneration and recycling. After calcium / magnesium / sodium-based desulfurizer removes SO2 by dry method or semi-dry method, a large amount of metal-based desulfurization products that are difficult to dispose of will be generated. The present invention uses sulfur as a reducing agent to reduce these metal-based desulfurization products to metal sulfides; further, the metal sulfides are prepared into slurry for CO2 capture, and carbonate products with certain economic value can be generated when capturing CO2. At the same time, the generated H2S gas can be obtained by oxidation and reduction to obtain elemental sulfur; the elemental sulfur can be recovered and returned as a reducing agent to the reduction step of the metal-based desulfurization product. The present invention combines the treatment and disposal of solid waste with CO2 emission reduction, realizes the resource recycling of sulfur element at the same time, and can obtain carbonate products, creating higher environmental benefits, economic benefits and social benefits.
[0022] Beneficial effects of the present invention:
[0023] (1) The present invention provides a process method that can realize low-cost treatment of metal-based desulfurization products combined with carbon emission reduction and simultaneously recover sulfur resources. The process is safe and reliable, and realizes the recycling and reuse of sulfur resources while achieving "waste treatment with waste";
[0024] (2) The process of the present invention is simple and easy to operate, with low operating costs. The obtained carbonate products can be used in the pharmaceutical, construction, papermaking and other industries, achieving environmental benefits while also having certain economic benefits;
[0025] (3) Using sulfur as a reducing agent to reduce the metal-based desulfurization product makes the process simpler and can also improve the reduction rate of the metal-based desulfurization product and reduce the decomposition temperature to a certain extent;
[0026] (4) The present invention can achieve a carbon fixation capacity of ≥1000 mg CO2 / g for metal-based desulfurization products. After the slurry method is completed to capture the mineralized CO2 reaction, the metal sulfide can be completely converted into a carbonate product. At the same time, the concentration of H2S generated is ≥3%. After absorption treatment with an iron (III) chelate solution, elemental sulfur with a diameter of 0.5 to 5 μm can be obtained. BRIEF DESCRIPTION OF THE DRAWINGS
[0027] Figure 1 It is a process flow chart of the metal-based desulfurization product capturing mineralized CO2 coupled with sulfur resource regeneration and recycling in an embodiment of the present invention;
[0028] Figure 2 This is a graph of the carbon fixation capacity of the reduction product obtained by reducing the metal-based desulfurization product in Examples 1 to 3 of the present invention. DETAILED DESCRIPTION
[0029] The present invention provides a method for capturing mineralized CO2 with metal-based desulfurization products and coupling sulfur resource regeneration and recycling, comprising the following steps:
[0030] The metal-based desulfurization product and sulfur are mixed and subjected to a reduction reaction to obtain a metal sulfide;
[0031] mixing the metal sulfide and water to obtain a slurry;
[0032] A gas containing CO2 is introduced into the slurry to capture the mineralized CO2 and obtain a gas containing H2S and carbonate;
[0033] The H2S-containing gas is introduced into an iron (III) chelate solution to undergo an oxidation-reduction reaction to obtain elemental sulfur; and the elemental sulfur is reused in the reduction reaction.
[0034] Unless otherwise specified, the materials and equipment used in the present invention are all commercially available products in the art.
[0035] The present invention mixes a metal-based desulfurization product and sulfur, performs a reduction reaction, and obtains a metal sulfide. In the present invention, the metal-based desulfurization product preferably includes one or more of calcium sulfate, magnesium sulfate, and sodium sulfate. In a specific embodiment of the present invention, the metal-based desulfurization product also includes iron and / or silicon impurities. In the present invention, the purity of the metal-based desulfurization product is preferably 70% to 98%, more preferably 90% to 98%. In the present invention, the source of the metal-based desulfurization product includes: one or more of a calcium-based desulfurizer, a magnesium-based desulfurizer, and a sodium-based desulfurizer, and the metal-based desulfurization product produced after SO2 removal by a dry method or a semi-dry method.
[0036] In the present invention, the mixing of the metal-based desulfurization product and sulfur preferably includes: drying the metal-based desulfurization product to obtain a pretreated metal-based desulfurization product; mixing the pretreated metal-based desulfurization product and sulfur. In the present invention, the drying temperature is preferably 100 to 200°C, more preferably 150 to 180°C; the drying time is preferably 0.5 to 1.5 hours, more preferably 1 to 1.2 hours; the drying is preferably carried out in an oven. In the present invention, the purpose of the drying is to remove moisture from the metal-based desulfurization product.
[0037] In the present invention, the metal-based desulfurization product is SO4 2-The sulfur is calculated as S, and the molar ratio of the metal-based desulfurization product to sulfur is preferably 1:1-5, more preferably 1:2.5-3.
[0038] In the present invention, the temperature of the reduction reaction is preferably 500-1150°C, more preferably 900-1100°C, and further preferably 950-1000°C; the holding time is preferably 0.5-4h, more preferably 2-3h. In the present invention, the heating rate from room temperature to the temperature of the reduction reaction is preferably 5-10°C / min, more preferably 6-8°C / min. In the present invention, the atmosphere of the reduction reaction is preferably a protective atmosphere, more preferably a N2 atmosphere. In the present invention, the reduction reaction is preferably carried out in a tubular furnace. The present invention uses sulfur as a reducing agent to reduce the metal-based desulfurization product to metal sulfide.
[0039] In a specific embodiment of the present invention, the metal sulfide includes one or more of calcium sulfide, magnesium sulfide and sodium sulfide.
[0040] After obtaining the metal sulfide, the present invention mixes the metal sulfide and water to obtain a slurry. In the present invention, the mass ratio of the metal sulfide to water is preferably 1:10 to 200, and more preferably 1:50 to 100. In the present invention, the water is preferably deionized water. In the present invention, the mixing is preferably carried out in a closed stirring reactor. In the present invention, the mixing is preferably carried out under stirring conditions; the stirring speed is preferably 100 to 1000 r / min, and more preferably 500 to 700 r / min; the stirring time is preferably 10 to 90 min, and more preferably 30 to 60 min. The present invention disperses the metal sulfide uniformly in water by stirring.
[0041] After obtaining the slurry, the present invention introduces a gas containing CO2 into the slurry, captures mineralized CO2, and obtains H2S-containing gas and carbonate. In the present invention, the introduction rate of the gas containing CO2 is preferably 100-500mL / min, more preferably 300-400mL / min. In the present invention, the volume content of CO2 in the CO2-containing gas is preferably 10-15%, more preferably 12-14%. In a specific embodiment of the present invention, the CO2-containing gas is a mixed gas of nitrogen and carbon dioxide. In the present invention, the temperature for capturing the mineralized CO2 is preferably 25-60°C, more preferably 40-50°C.
[0042] In a specific embodiment of the present invention, the H2S-containing gas is a mixed gas containing H2S, CO2 and nitrogen, and the obtained mixed gas containing H2S, CO2 and nitrogen is directly introduced into an iron (III) chelate solution to perform an oxidation-reduction reaction to obtain elemental sulfur. The present invention does not require purification of the mixed gas containing H2S, CO2 and nitrogen.
[0043] After obtaining the H2S-containing gas, the present invention passes the H2S-containing gas into an iron (III) chelate solution to perform an oxidation-reduction reaction to obtain elemental sulfur; and the elemental sulfur is reused in the reduction reaction. In the present invention, the raw materials for preparing the iron (III) chelate solution preferably include trivalent iron salt, organic acid, NaHCO3, Na2CO3 and water. In the present invention, the trivalent iron salt preferably includes Fe2(SO4)3; the organic acid preferably includes C6H8O7, and C6H8O7 provides an organic ligand L n- In the present invention, the L n- In the present invention, the Fe(III) chelate solution contains 3+ The concentration of L is preferably 0.05 mol to 3 mol / L, more preferably 0.05 mol / L. n- with Fe 3+ The concentration ratio of Na in the iron (III) chelate solution is preferably 1 to 5:1, more preferably 1.4:1. + The concentration is preferably 0.1-1 mol / L, more preferably 0.4 mol / L. In the present invention, NaHCO3 and Na2CO3 are used as buffers. In the present invention, the pH of the iron (III) chelate solution is preferably 8-11, more preferably 9.0.
[0044] In the present invention, the flow rate of the H2S-containing gas into the iron (III) chelate solution is preferably 200-1000 mL / min, more preferably 300 mL / min.
[0045] In the present invention, the redox reaction is preferably carried out under normal temperature and pressure. In the present invention, after the redox reaction, the obtained elemental sulfur precipitate is preferably washed and dried in sequence to obtain elemental sulfur. In a specific embodiment of the present invention, the obtained system is filtered after the redox reaction to obtain elemental sulfur precipitate. In the present invention, the washing liquid used for the washing is preferably water, more preferably distilled water. In the present invention, the drying temperature is preferably 100°C, and the drying time is preferably 24 hours.
[0046] In the present invention, the elemental sulfur is used as a reducing agent for the metal-based desulfurization product and is recycled in the above reduction reaction.
[0047] Figure 1 The process flow chart of the metal-based desulfurization product capturing and mineralizing CO2 coupled with sulfur resource regeneration and recycling in the embodiment of the present invention is as follows:
[0048] Step 1: Reduce the metal-based desulfurization products to obtain metal sulfides within the range of 500-1150°C:
[0049] MSO4+2S=MS+2SO2(g)
[0050] Among them, MSO4 represents CaSO4, MgSO4, Na2SO4, and MS represents CaS, MgS, Na2S;
[0051] Step 2: Use metal sulfide to prepare slurry to capture mineralized CO2:
[0052] MS+H2O+CO2(g)=MCO3+H2S(g)
[0053] Among them, MS represents CaS, MgS, and Na2S, and MCO3 represents CaCO3, MgCO3, and Na2CO3;
[0054] Step 3: Recover sulfur resources using iron (III) chelate solution:
[0055] H2S+2Fe 3+ L n- →S 0 +2Fe 2+ L n- +2H + .
[0056] The present invention can realize the combination of low-cost reduction of metal-based desulfurization products and carbon emission reduction and the recovery of sulfur resources at the same time. The process is safe and reliable, and the metal-based desulfurization products and CO2 are recovered simultaneously, while the recycling of sulfur resources is realized.
[0057] The technical solutions in the present invention will be described clearly and completely below in conjunction with the embodiments of the present invention. Obviously, the described embodiments are only a part of the embodiments of the present invention, not all of them. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.
[0058] Example 1
[0059] A method for metal-based desulfurization product CaSO4 to capture mineralized CO2 coupled with sulfur resource regeneration and recycling, the specific steps are as follows:
[0060] (1) CaSO4 reduction: CaSO4 is placed in an oven at 100°C for drying pretreatment for 1.5 hours to obtain pretreated CaSO4; the pretreated CaSO4 is mixed evenly with sulfur at a CaSO4 / S molar ratio of 1 / 3, and then placed in a tubular furnace for reduction reaction under a N2 atmosphere, the heating rate of the tubular furnace is controlled at 5°C / min, the temperature of the reduction reaction is 1000°C, and the insulation time is 2 hours to obtain a reduction product mainly composed of CaS;
[0061] (2) placing the reduction product obtained in step (1) and deionized water (liquid-to-solid mass ratio of 10:1) in a closed stirred reactor, setting the stirring speed of the electric stirrer to 700 r / min, stirring for 90 min to obtain a slurry; introducing a mixed gas of nitrogen and carbon dioxide (the volume fraction of CO2 is 15%) into the slurry at a constant flow rate of 300 mL / min, capturing and mineralizing CO2 at 25° C., allowing CO2 to react with calcium ions in the slurry to produce CaCO3, and generating a gas containing H2S, thereby achieving CO2 capture and mineralization;
[0062] (3) Recovery of sulfur resources: Fe2(SO4)3, C6H8O7 (providing organic ligand L n- ), NaHCO3, Na2CO3 and water were mixed to obtain an iron (III) chelate solution with a pH value of 9.0, wherein [Fe 3+ ]=0.05mol / L,[L n- ] / [Fe 3+ ]=1.4:1,[Na + ]=0.4mol / L, NaHCO3 and Na2CO3 are used as buffers;
[0063] The H2S-containing gas produced in step (2) is introduced into the iron (III) chelate solution at a flow rate of 300 mL / min to carry out a redox reaction, and an elemental sulfur precipitate is obtained by filtration; the elemental sulfur precipitate is washed with distilled water and dried at 100°C for 24 hours. The obtained elemental sulfur can be returned to step (1) as a reducing agent for CaSO4.
[0064] By using the formula: Carbon fixation capacity = carbon dioxide absorbed by slurry (mg) / reduction product mainly composed of CaS (g), the carbon fixation capacity of the reduction product obtained by CaSO4 reduction when the carbon fixation time is 85 minutes is calculated to be 951 mg CO2 / g, and a gas with an H2S concentration of 3.12% (v%) is produced. After treatment, elemental sulfur is obtained, which can be used as a reducing agent.
[0065] Example 2
[0066] A method for metal-based desulfurization product MgSO4 to capture mineralized CO2 coupled with sulfur resource regeneration and recycling, the specific steps are as follows:
[0067] (1) MgSO4 reduction: MgSO4 is placed in an oven at 100°C for drying pretreatment for 1.5 hours to obtain pretreated MgSO4; the pretreated MgSO4 is mixed evenly with sulfur at a MgSO4 / S molar ratio of 1 / 2.5, and then placed in a tubular furnace for reduction reaction under a N2 atmosphere, the heating rate of the tubular furnace is controlled at 8°C / min, the reduction reaction temperature is 900°C, and the insulation time is 2 hours to obtain a reduction product mainly composed of MgS;
[0068] (2) placing the reduction product obtained in step (1) and deionized water (liquid-to-solid mass ratio of 10:1) in a closed stirred reactor, setting the stirring speed of the electric stirrer to 700 r / min, stirring for 90 min to obtain a slurry; introducing a mixed gas of nitrogen and carbon dioxide (the volume fraction of CO2 is 15%) into the slurry at a constant flow rate of 300 mL / min, capturing and mineralizing CO2 at 25° C., allowing CO2 to react with magnesium ions in the slurry to produce MgCO3, and generating a gas containing H2S, thereby achieving CO2 capture and mineralization;
[0069] (3) Recovery of sulfur resources: Fe2(SO4)3, C6H8O7 (providing organic ligand L n- ), NaHCO3, Na2CO3 and water were mixed to obtain an iron (III) chelate solution with a pH value of 9.0, wherein [Fe 3+ ]=0.05mol / L,[L n- ] / [Fe 3+ ]=1.4:1,[Na + ]=0.4mol / L, NaHCO3 and Na2CO3 are used as buffers;
[0070] The H2S-containing gas produced in step (2) is introduced into the iron (III) chelate solution at a flow rate of 300 mL / min to carry out a redox reaction, and an elemental sulfur precipitate is obtained by filtration; the elemental sulfur precipitate is washed with distilled water and dried at 100°C for 24 hours. The obtained elemental sulfur can be returned to step (1) as a reducing agent for MgSO4.
[0071] According to the formula: Carbon fixation capacity = carbon dioxide absorbed by slurry (mg) / reduction product mainly composed of MgS (g), the carbon fixation capacity of the reduction product obtained by MgSO4 reduction when the carbon fixation time is 85 minutes is calculated to be 1276 mg CO2 / g, and the gas with H2S concentration of 0.38% (v%) is produced. After treatment, elemental sulfur is obtained, which can be used as a reducing agent.
[0072] Example 3
[0073] A method for metal-based desulfurization product Na2SO4 to capture mineralized CO2 coupled with sulfur resource regeneration and recycling, the specific steps are as follows:
[0074] (1) Na2SO4 reduction: Na2SO4 is placed in an oven at 100°C for drying pretreatment for 1.5 hours to obtain pretreated Na2SO4; the pretreated Na2SO4 is mixed with sulfur at a Na2SO4 / S molar ratio of 1 / 3, and then placed in a tubular furnace for reduction reaction under N2 atmosphere, the heating rate of the tubular furnace is controlled at 8°C / min, the temperature of the reduction reaction is 1150°C, and the insulation time is 2 hours to obtain a reduction product mainly composed of Na2S;
[0075] (2) placing the reduction product obtained in step (1) and deionized water (liquid-to-solid mass ratio of 10:1) in a closed stirred reactor, setting the stirring speed of the electric stirrer to 700 r / min, stirring for 90 min to obtain a slurry; introducing a mixed gas of nitrogen and carbon dioxide (the volume fraction of CO2 is 15%) into the slurry at a constant flow rate of 300 mL / min, capturing and mineralizing CO2 at 40° C., allowing CO2 to react with sodium ions in the slurry to produce Na2CO3, and simultaneously generating a gas containing H2S, thereby achieving CO2 capture and mineralization;
[0076] (3) Recovery of sulfur resources: Fe2(SO4)3, C6H8O7 (providing organic ligand L n- ), NaHCO3, Na2CO3 and water were mixed to obtain an iron (III) chelate solution with a pH value of 9.0, wherein [Fe 3+ ]=0.05mol / L,[L n- ] / [Fe 3+ ]=1.4:1,[Na + ]=0.4mol / L, NaHCO3 and Na2CO3 are used as buffers;
[0077] The H2S-containing gas produced in step (2) is introduced into the iron (III) chelate solution at a flow rate of 300 mL / min to carry out a redox reaction, and an elemental sulfur precipitate is obtained by filtration; the elemental sulfur precipitate is washed with distilled water and dried at 100°C for 24 hours. The obtained elemental sulfur can be returned to step (1) as a reducing agent for Na2SO4.
[0078] By using the formula: Carbon fixation capacity = carbon dioxide absorbed by the slurry (mg) / reduction product mainly composed of Na2S (g), the carbon fixation capacity of the reduction product obtained by reduction with Na2SO4 is calculated to be 439mg CO2 / g when the carbon fixation time is 85min, and a gas with an H2S concentration of 1.1% (v%) is produced. After treatment, elemental sulfur is obtained, which can be used as a reducing agent.
[0079] The present invention provides a method and approach for comprehensive utilization of calcium / magnesium / sodium-based desulfurization product resources, which can not only turn waste into treasure, but also reduce pollution to the environment, achieve economic benefits, and greatly improve environmental benefits.
[0080] The above is only a preferred embodiment of the present invention. It should be pointed out that for ordinary technicians in this technical field, several improvements and modifications can be made without departing from the principle of the present invention. These improvements and modifications should also be regarded as the scope of protection of the present invention.
Claims
1. A method for capturing and mineralizing CO2 by metal-based desulfurization products and coupling sulfur resource regeneration and recycling, comprising the following steps: The metal-based desulfurization product and sulfur are mixed and subjected to a reduction reaction to obtain a metal sulfide; mixing the metal sulfide and water to obtain a slurry; A gas containing CO2 is introduced into the slurry to capture the mineralized CO2 and obtain a gas containing H2S and carbonate; The H2S-containing gas is introduced into an iron (III) chelate solution to undergo an oxidation-reduction reaction to obtain elemental sulfur; and the elemental sulfur is reused in the reduction reaction.
2. The method according to claim 1, characterized in that: The metal-based desulfurization product includes one or more of calcium sulfate, magnesium sulfate and sodium sulfate.
3. The method according to claim 1 or 2, characterized in that: The mixing of the metal-based desulfurization product and sulfur comprises: drying the metal-based desulfurization product to obtain a pretreated metal-based desulfurization product; and mixing the pretreated metal-based desulfurization product and sulfur.
4. The method according to claim 3, characterized in that The drying temperature is 100-200° C., and the drying time is 0.5-1.5 hours.
5. The method according to claim 1, characterized in that: The metal-based desulfurization product is SO4 2- The sulfur is calculated as S, and the molar ratio of the metal-based desulfurization product to sulfur is 1:1-5.
6. The method according to claim 1, characterized in that The temperature of the reduction reaction is 500-1150° C., and the insulation time is 0.5-4 hours.
7. The method according to claim 1, characterized in that The mass ratio of the metal sulfide to water is 1:10-200.
8. The method according to claim 1, characterized in that The temperature of capturing mineralized CO2 is 25-60°C.
9. The method according to claim 1, characterized in that: The raw materials for preparing the iron (III) chelate solution include trivalent iron salt, organic acid, NaHCO3, Na2CO3 and water.
10. The method according to claim 1 or 9, characterized in that: The Fe(III) chelate solution 3+ The concentration is 0.05~3mol / L.