WO2024019449A1 - Système d'élimination de dioxyde de carbone de gaz d'échappement - Google Patents

Système d'élimination de dioxyde de carbone de gaz d'échappement Download PDF

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Publication number
WO2024019449A1
WO2024019449A1 PCT/KR2023/010175 KR2023010175W WO2024019449A1 WO 2024019449 A1 WO2024019449 A1 WO 2024019449A1 KR 2023010175 W KR2023010175 W KR 2023010175W WO 2024019449 A1 WO2024019449 A1 WO 2024019449A1
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Prior art keywords
carbon dioxide
exhaust gas
receives
tank
clause
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PCT/KR2023/010175
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English (en)
Korean (ko)
Inventor
홍원방
박무신
홍정환
장인영
박성수
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홍원방
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Publication of WO2024019449A1 publication Critical patent/WO2024019449A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D21/00—Separation of suspended solid particles from liquids by sedimentation
    • B01D21/01—Separation of suspended solid particles from liquids by sedimentation using flocculating agents
    • 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
    • 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
    • B01D53/14—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 absorption
    • 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
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
    • C01F11/00—Compounds of calcium, strontium, or barium
    • C01F11/18—Carbonates
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/52—Treatment of water, waste water, or sewage by flocculation or precipitation of suspended impurities
    • 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

Definitions

  • the present invention relates to a system that can remove carbon dioxide from exhaust gases of power plants, etc. and provide high purity calcium carbonate.
  • the exhaust gas after combustion contains a large amount of CO 2 .
  • NOx generation due to the high-temperature combustion process is removed using a denitrification facility (SCR or SNCR), and even excluding the case of relatively expensive LNG power generation, sulfur in the fuel is first removed depending on the type of fossil fuel used as fuel. SOx is generated after combustion due to the components, and dust containing ash and heavy metals is removed with an electrostatic precipitator (EP).
  • EP electrostatic precipitator
  • the present invention was developed to solve the above problems, and aims to provide a system that can efficiently remove not only sulfur oxides but also carbon dioxide from exhaust gases and produce high-purity calcium carbonate as a result.
  • system of the present invention to achieve the above object is a dust collection system that receives exhaust gas discharged from an exhaust gas source and removes dust from the exhaust gas.
  • a carbon dioxide absorption tank that receives the exhaust gas that has passed through the dust collector, removes carbon dioxide and sulfur oxides from the exhaust gas by reacting with a carbon dioxide absorbent containing an aqueous sodium hydroxide solution, and discharges treated gas
  • a primary sedimentation tank that receives the reaction solution from the carbon dioxide absorption tank and precipitates foreign substances through a coagulation reaction with a coagulant
  • secondary precipitation tank that receives the reaction solution from the primary precipitation tank and reacts it with calcium oxide to recover calcium carbonate.
  • the front end of the dust collector further includes a nitrogen oxide removal unit that receives exhaust gas discharged from an exhaust gas source, removes nitrogen oxides from the exhaust gas, and discharges the nitrogen oxides.
  • the process gas discharged through the carbon dioxide absorption tank is discharged to the outside through a heat exchanger.
  • the carbon dioxide absorbent includes illite extract.
  • One example is characterized in that sodium tetraborate is further included.
  • One example is characterized in that water glass is further included.
  • One example is that hydrogen peroxide is further included.
  • the present invention has the advantage of being able to efficiently operate the system without a desulfurization facility or without a load on the desulfurization facility by using a carbon dioxide absorbent that can simultaneously process carbon dioxide and sulfur oxides.
  • the captured carbon dioxide to be recovered as high-purity calcium carbonate without impurities, it has the advantage of being able to be used across industries such as papermaking, construction, and steelmaking without restrictions on demand.
  • FIG. 1 is a block diagram showing the system of the present invention
  • Figure 2 is a diagram showing the carbon dioxide absorption mechanism of the carbon dioxide absorbent applied to the present invention
  • Figure 3 is a graph showing the results of an experiment on the removal of sulfur oxides
  • Figure 4 is a graph showing experimental results regarding the removal of carbon dioxide.
  • the system 1 of the present invention includes a dust collector 4 that receives exhaust gas discharged from an exhaust gas discharge source 2 and removes dust from the exhaust gas; a carbon dioxide absorption tank (7) that receives the exhaust gas that has passed through the dust collector (4), removes carbon dioxide and sulfur oxides from the exhaust gas by reacting with a carbon dioxide absorbent containing an aqueous sodium hydroxide solution, and discharges treated gas; a primary sedimentation tank (8) that receives the reaction solution from the carbon dioxide absorption tank (7) and precipitates foreign substances through a coagulation reaction with a coagulant; It is characterized in that it includes a secondary precipitation tank (9) that receives the reaction solution from the primary precipitation tank (8) and reacts it with calcium oxide to recover calcium carbonate.
  • the front end of the dust collector (4) further includes a nitrogen oxide removal unit (3) that receives exhaust gas discharged from the exhaust gas discharge source (2), removes nitrogen oxides from the exhaust gas, and discharges the nitrogen oxides.
  • the emission source 2 is a concept that refers to places and facilities that emit exhaust gas mixed with various pollutants such as power plants, nitrogen oxides, sulfur oxides, and carbon dioxide.
  • the nitrogen oxide removal unit 3 is configured to remove nitrogen oxides from the exhaust gas discharged from the emission source 2.
  • the nitrogen oxide removal unit 3 removes nitrogen oxides from the exhaust gas by applying various known technologies. In order to discharge it, for example, SCR denitrification technology can be applied.
  • the dust collector 4 is a device that receives the exhaust gas that has passed through the nitrogen oxide removal unit 3 and removes dust from the exhaust gas, and removes dust from the exhaust gas by electric dust collection.
  • the dust is a concept that includes particulate contaminants, ash, heavy metals, etc.
  • the desulfurization unit 5 shown in FIG. 1 is configured to remove sulfur oxides from the exhaust gas, and in the system 1 of the present invention, simultaneous removal of sulfur oxides and carbon dioxide is possible in the carbon dioxide absorption tank 7 described below.
  • the desulfurization unit 5 can be selectively bypassed, thereby simplifying the system and controlling the load on the desulfurization unit 5.
  • the heat exchanger (6) allows heat exchange while passing the processed gas through the desulfurization unit (5) or the carbon dioxide absorption tank (7).
  • the carbon dioxide absorption tank (7) receives the exhaust gas that has passed through the dust collector (4), removes carbon dioxide and sulfur oxides from the exhaust gas by reacting with a carbon dioxide absorbent containing an aqueous sodium hydroxide solution, and returns the exhaust gas to the heat exchanger (6). It corresponds to a configuration that discharges process gas.
  • the carbon dioxide absorption tank 7 is capable of allowing exhaust gas without passing through the desulfurization unit 5 to flow in as shown in the drawing by applying a carbon dioxide absorbent that simultaneously removes carbon dioxide and sulfur oxides. Although this has not been done, the reaction can be achieved by introducing exhaust gas that has passed through the desulfurization unit (5).
  • the carbon dioxide absorbent is characterized in that it contains an aqueous sodium hydroxide solution and an illite extract.
  • the sodium hydroxide aqueous solution is characterized in that mixed gas containing high temperature and high concentration of carbon dioxide and COS (hydrocarbon, O 2 , SOx) can be simultaneously removed. In other words, it absorbs not only sulfur oxides (SOx) but also carbon dioxide from power plant exhaust gases.
  • the illite is a mineral found to be buried in large quantities in the Yeongdong region of Korea, expressed as ⁇ K 0.75 [Al 1.75 (Mg ⁇ Fe 2+ ) 0.25 ](Si 3.50 Al 0.50 )O 10 (OH) 2 ⁇ .
  • the layer charge is lower than that of muscovite, and the charge is due to the reduction of isomorphic substitution of Al 3+ and Si 4+ of the tetrahedral plate. Some isomorphic substitutions occur in the octahedral plate.
  • Illite is non-expandable due to the strong bonding force caused by K+ that exists between layers, and the layer spacing is 10 ⁇ . Therefore, it is a mineral that is extracted from the liquid phase, has a full cationic charge, and is easily converted into a chelation compound. In the present invention, it is appropriate to use micronized illite to facilitate extraction of such metal foreign substances.
  • the extract extracted from illite is an extract containing several types of metal oxides such as potassium oxide, and serves as a reaction enhancer by providing minerals that are easily converted into chelation compounds in the liquid phase. That is, in the absorption of carbon dioxide including SOx in the sodium hydroxide aqueous solution, more illite extract is added to increase the absorption efficiency.
  • reaction formula of sodium hydroxide of illite extract as a reaction enhancer is as shown below. Only the main components of illite are described, and oxides of other minor components such as Ca, Fe, Mg, Mn, Ti, and P 2 O 5 also contribute greatly to forming a stable metal chelation compound in the liquid phase.
  • the illite extract is prepared by adding illite powder to water heated to 40 to 100°C and stirring. That is, it can be obtained by adding illite powder to heated water, stirring to precipitate solids, and separating and filtering the supernatant.
  • the present invention provides an example in which the carbon dioxide absorbent further includes sodium tetraborate (Na 2 B 4 O 7 ⁇ 10H 2 O) and water glass (Na 2 SiO 3 ).
  • the aqueous sodium hydroxide solution contains sodium tetraborate and water glass in addition to the illite extract. As more sodium tetraborate and water glass are added, the carbon dioxide and the absorbent component react directly, so the reaction rate is much faster and the mass transfer coefficient increases.
  • the present invention presents an example in which hydrogen peroxide (H 2 O 2 ) is further added as a reaction-promoting additive.
  • reaction equation of sodium tetraborate and hydrogen peroxide in aqueous sodium hydroxide solution is as follows.
  • the primary sedimentation tank (8) receives the reaction solution from the carbon dioxide absorption tank (7) and precipitates foreign substances through a coagulation reaction with a coagulant, thereby removing foreign substances such as heavy metals, ash, and SS from the reaction solution by coagulation. This is to increase the purity of calcium carbonate obtained in the secondary precipitation tank 9 at the rear, and although not shown in the drawing, it is intended to ensure that a regenerated carbon dioxide absorbent without impurities is regenerated when regenerating the reaction solution.
  • the type of coagulant is not limited, and for example, calcium hydroxide (Ca(OH) 2 ) may be applied.
  • the secondary precipitation tank (9) receives the reaction solution from the primary precipitation tank (8) and reacts it with calcium oxide to recover calcium carbonate.
  • the reaction solution from which foreign substances as well as captured carbon dioxide are removed as it passes through the first sedimentation tank 8 and the second sedimentation tank 9 can be reused as a regenerated carbon dioxide absorbent.
  • the cost of the carbon dioxide absorbent provided according to the present invention is that it has a mechanism for recovering the absorption power by precipitating it again as calcium carbonate after the chemical absorption reaction of carbon dioxide, and although not shown in the drawing, a small amount of carbon dioxide absorbent is used in the pipe and absorption tower through the circulation system.
  • the temperature of the filtrate is maintained above 60°C after calcium carbonate precipitation due to the dilution heat generated when CaO is added in the secondary precipitation tank 9, so an exothermic reaction develops with almost no loss of heat energy.
  • calcium carbonate has almost no solubility in alkaline water even at high temperatures above 60°C, and it only affects the size and crystal form of the precipitate depending on the temperature.
  • a portion of the calcium carbonate obtained in the secondary precipitation tank 9 can be sent to the desulfurization unit 5 and used to remove sulfur oxides.
  • the calcium carbonate obtained in this way Because it has a very high purity without impurities, it can be used on its own without restrictions across industries such as papermaking, construction, and steelmaking, and it can be recycled as resources by producing high-purity carbon dioxide and slaked lime through the sintering process.
  • pure calcium carbonate like this is a pollution-free resource that is not affected by the natural world and can at least be used for reclaiming abandoned mines.
  • the system (1) of the present invention does not directly collect carbon dioxide and then store or recycle it. It does not require large-scale facilities, generates little or no wastewater, and quickly produces calcium carbonate of very low solubility through a 1:1 reaction with carbonic acid. As the entire amount is deposited at a rapid rate, heat energy is obtained through the exothermic reaction of calcium carbonate, rather than reducing conversion energy costs in a small-scale sedimentation tank. Although not shown in the drawing, operating costs such as additional chemical costs are expected to be minimized through the circulation of carbon dioxide absorbents with restored performance. It is done. As a conversion product, high purity precipitated calcium carbonate can be expected to have high added value in terms of market size and price.
  • 1,350 g of yellow illite ground to 1,000 mesh was added to 15 L of RO water heated to 60°C and stirred for 30 minutes. Next, add 150g of sodium tetraborate and stir for 10 minutes to dissolve it well (temperature drop of about 10°C), then slowly add 300g of sodium hydroxide and stir. When the temperature of the reaction solution reaches 70°C due to the heat of dilution, add 300g of water glass and stir for 1 hour. It was stirred.
  • reaction solution naturally decreased and was stirred until it reached room temperature. Stirring was stopped at room temperature, left to stand overnight, and the supernatant was filtered to prepare an adsorbent.
  • NOVA 9K (MRU Emission Monitoring System, Germany) was used, and the sensor, measurement range, and resolution for each measurement target are as shown below.
  • Electrochemical sensor Electrochemical sensor
  • NDIR Non-dispersive infrared sensor
  • Ignition coal was put into the Meseta Harry wood stove and ignited, and after 5 minutes, 1kg of lignite was added to start combustion. After about 15 minutes, 100 g of the liquid desulfurization catalyst prepared in Example 1 was evenly sprayed with 3 kg of lignite, and combustion began in earnest.
  • the experimental results are shown in FIG. 3.
  • the first downward curve on the graph indicates that CO 2 is being reduced due to the injection of Example 2, and the rising curve while CO 2 is being reduced is when the lid of the reactor is opened to allow outside air.
  • a regenerated absorbent obtained by regenerating the previously used absorbent of Example 2 although not mentioned in the present invention, was added. As a result, it can be seen that CO 2 was reduced again.

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Abstract

La présente invention concerne un système pour l'élimination de dioxyde de carbone à partir de gaz d'échappement, le système comprenant : un collecteur de poussière qui reçoit un gaz d'échappement émis par une source de gaz d'échappement et élimine la poussière du gaz d'échappement ; un réservoir d'absorption de dioxyde de carbone qui reçoit le gaz d'échappement passant à travers le collecteur de poussière, réagit avec un absorbant de dioxyde de carbone contenant une solution d'hydroxyde de sodium pour éliminer le dioxyde de carbone et les oxydes de soufre des gaz d'échappement et évacue le gaz traité ; un réservoir de décantation principal qui reçoit le liquide de réaction provenant du réservoir d'absorption de dioxyde de carbone et précipite les impuretés par une réaction de coagulation avec un coagulant ; et un réservoir de décantation auxiliaire qui reçoit le liquide de réaction provenant du réservoir de décantation principal et réagit avec l'oxyde de calcium pour récupérer le carbonate de calcium.
PCT/KR2023/010175 2022-07-19 2023-07-17 Système d'élimination de dioxyde de carbone de gaz d'échappement WO2024019449A1 (fr)

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KR10-2022-0089156 2022-07-19

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