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WO2025142649A1 - Procédé et système de capture et d'élimination de dioxyde de carbone atmosphérique - Google Patents

Procédé et système de capture et d'élimination de dioxyde de carbone atmosphérique Download PDF

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Publication number
WO2025142649A1
WO2025142649A1 PCT/JP2024/044657 JP2024044657W WO2025142649A1 WO 2025142649 A1 WO2025142649 A1 WO 2025142649A1 JP 2024044657 W JP2024044657 W JP 2024044657W WO 2025142649 A1 WO2025142649 A1 WO 2025142649A1
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WIPO (PCT)
Prior art keywords
aqueous solution
carbon dioxide
sodium carbonate
naoh
medium
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PCT/JP2024/044657
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English (en)
Japanese (ja)
Inventor
和弘 佐山
由也 小西
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National Institute of Advanced Industrial Science and Technology AIST
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National Institute of Advanced Industrial Science and Technology AIST
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    • 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
    • B01D53/14—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
    • B01D53/18—Absorbing units; Liquid distributors therefor

Definitions

  • Non-Patent Document 1 a method has been devised in which the taken-in air is simply bubbled in an alkaline aqueous solution or sprayed against a moving alkaline aqueous solution to bring the air into contact and absorb it.
  • Patent Document 2 a method has been devised in which the taken-in air is simply sprayed with an alkaline aqueous solution to bring the air into contact and absorb it.
  • the air collector's liquid delivery pump also consumes a relatively large amount of energy.
  • the installation cost of the absorption tower is also high.
  • the blower and liquid delivery pump consume a certain amount of energy even in the gas-liquid contact method using blowing or bubbling air taken into the air collector and spraying alkaline aqueous solution.
  • Patent Document 3 In the technology disclosed in Patent Document 3, the alkaline aqueous solution exposed to the airflow maintained in a laminar or near-laminar state completely covers the smooth or roughened surface of the plate, and moves by flowing over the surface of the plate. In this case, the airflow comes into gas-liquid contact with the liquid surface of the alkaline aqueous solution covering the entire surface of the plate, and the contact area is at most the apparent surface area of the plate, which is not efficient. Even if the plate surface is roughened to increase the surface area, the airflow that comes into contact with it will then transition from laminar to turbulent due to the roughening, resulting in increased pressure loss.
  • Patent Document 4 uses NaOH generated from an electrochemical reaction device such as electrolysis, but does not disclose a method for efficiently recovering and removing carbon dioxide from dilute atmospheric air.
  • the objective of the present invention is to provide a method and system for capturing and removing atmospheric carbon dioxide, which utilizes an aqueous NaOH solution produced by an electrochemical reaction with sodium salt to efficiently and directly reduce dilute atmospheric carbon dioxide, as a measure to prevent global warming using electricity from renewable energy sources, etc.
  • the inventors have examined various factors involved in capturing low concentrations of carbon dioxide in the atmosphere as a measure against climate change, and have invented a method and system for capturing and removing carbon dioxide from the atmosphere.
  • the problem is to efficiently capture and remove carbon dioxide in the air and fix it in a process in which an acidic aqueous solution and an aqueous solution of NaOH are produced by electrolysis or electrodialysis, and then carbon dioxide in the air is brought into contact with the aqueous solution of NaOH to produce carbonate.
  • a fourth step of washing the medium with water by supplying water that dissolves the sodium carbonate adhering to the medium, and discharging the aqueous solution of sodium carbonate from the medium and collecting the aqueous solution in a storage tank.
  • [2] The method for recovering and removing carbon dioxide from the atmosphere according to [1], further comprising a fifth step (5) of reusing the medium that has been washed with water.
  • [3] The method for capturing and removing carbon dioxide in the atmosphere according to [1] or [2], characterized in that in the fourth step, the sodium carbonate is extracted from the aqueous solution of sodium carbonate accumulated in the storage tank and stored on land in a location with no inflow of water.
  • [4] The method for recovering and removing carbon dioxide from the atmosphere according to any one of [1] to [3], characterized in that in the third step, the CO 2 /Na ratio of the solid or aqueous solution of sodium carbonate, and the pH of the aqueous solution of sodium carbonate are measured to control the water content in the step.
  • [5] The method for recovering and removing carbon dioxide in the atmosphere according to any one of [1] to [4], wherein in the second step, the carbon dioxide in the atmosphere comes into contact with the NaOH deposit layer by natural wind.
  • the power used can be reduced to the same level as the oxygen reduction type electrolysis device.
  • the current density is lower than that of the electrolysis device, but this can be overcome by improving the membrane.
  • Bipolar membranes and ion exchange membranes are mainly hydrocarbon-based, and costs can be significantly reduced by mass production of membranes.
  • the current density is 5 to 500 mA/cm 2 , preferably 10 to 50 mA/cm 2 .
  • the medium according to this embodiment preferably further has base resistance and durability.
  • the base resistance is preferably long-term durability against high-concentration NaOH.
  • examples of such a medium include organic substances such as cellulose and rayon that have hydroxyl groups (OH groups) or carboxyl groups on the surface, and hydrophilic polymers such as surface-treated polyalkanes.
  • examples of such a medium include inorganic substances such as aluminum silicate, zirconia, alumina, silicate, titania, glass wool, asbestos material, and basalt fiber. These have surface hydroxyl groups and are hydrophilic. The presence or absence of hydrophilicity can be judged by whether dropped water penetrates and spreads or whether the contact angle is 90 degrees or less.
  • the hydrophilic material may be compounded with a stable resin such as nylon or PPS (polyphenylene sulfide).
  • the medium according to the present embodiment may be a composite containing at least one hydrophilic substance and another substance.
  • a hydrophilic porous substance may be coated on another substance, or a hydrophilic substance may be coated on another porous substance.
  • specific examples thereof include a composite in which a mixture of zirconium oxide and a polymer is coated on a PPS mesh, such as a membrane for water electrolysis, and a composite of nylon and an ion exchange membrane (anion exchange membrane and cation exchange membrane).
  • strong base resistance is required for the parts that come into contact with NaOH, but strong base resistance is not required in areas where carbonation progresses and the pH drops.
  • the NaOH adhesion layer that comes into contact with carbon dioxide in the atmosphere may be in a dry or semi-dry state, or may be in a wet state containing an aqueous solution of NaOH. It is preferable that the layer be as dry or semi-dry as possible. It is preferred that the atmospheric carbon dioxide comes into contact with the NaOH deposit by natural wind. In addition, when the carbon dioxide in the atmosphere comes into contact with the NaOH adhesion layer by natural wind, the NaOH adhesion layer that the carbon dioxide in the atmosphere comes into contact with by the natural wind may be in an air-dried state or in a wet state containing an aqueous solution of NaOH. It is preferable that the adhesion layer is in an air-dried state as much as possible.
  • Air-drying refers to the state in which the moisture contained in a material evaporates as it dries.
  • the salt of Na2CO3 that is produced can be anhydrous or hydrated. When carrying out outdoors where there is a lot of precipitation, it is advisable to put up a roof so that rain does not directly hit the media or the storage tank. Also, promoting drying with sunlight will promote the reaction with CO2 . If the media deteriorates due to sunlight, measures should be taken to increase the light resistance of the media or to block the light.
  • a pipe may be laid around the medium, and a hole, a mist shower, and an automatic opening and closing valve may be provided on the pipe.
  • moisture for wetting can be supplied from upstream to downstream by gravity, but moisture can also be supplied by capillary action.
  • the presence of the medium contributes to the water retention effect due to its hydrophilicity and porosity, and to the increase in the actual surface area of the salt particles due to the large area of porosity.
  • Carbonates are hydrophilic, just like NaOH. If they were hydrophobic, they would likely form large clumps rather than spreading through the medium.
  • Figure 4 shows an example where the wetting water is supplied by capillary action.
  • the lower part of the medium 10 may be fixed to the bottom of the storage tank 20, and formed as a protrusion that stands upright so that the part above the liquid level of the water in the storage tank 20 comes into contact with the air. It is possible to form the medium 10 into a cylindrical shape (cylinder, square tube, etc.) and fix the lower part to the bottom surface of the storage tank 20, protruding from the liquid level into the air like a pile, so that it comes into contact with the water below the liquid level and comes into contact with the air above the liquid level.
  • the solution contains a lot of Na 2 CO 3 salt and its hydrated salts, but as carbon dioxide from the atmosphere is absorbed, crystal growth of sodium sesquicarbonate (Na 2 CO 3.NaHCO 3.2H 2 O) progresses, resulting in a state in which sodium sesquicarbonate is abundant, and the average CO 2 /Na ratio of the solid salt and aqueous solution can increase from around 0.5 to around 0.67.
  • the crystal growth of sodium sesquicarbonate is preferably carried out by contacting with liquid water and causing dissolution and reprecipitation, rather than supplying water only in the gas phase of water vapor.
  • the water when water is added onto the medium, the water does not have to be pure water.
  • a part of the carbonate aqueous solution in the reservoir can be returned to the medium to keep it moist.
  • the wetting switch point By varying the flow rate or flow rate of the aqueous solution, the wetting switch point can be changed.
  • the CO2 /Na ratio can be measured by analyzing the salt composition using Raman spectroscopy or XRD analysis, or calculated from the CO2 content using solid TOC analysis.
  • Raman spectroscopy can be used to measure online. It would be desirable to be able to monitor and measure the carbonate in its solid form, but by sampling a portion of the carbonate and adding water to dissolve it, various measurements can be made using the resulting aqueous solution.
  • an aqueous solution it can be measured using a pH meter, a Na+ ion meter, electrical conductivity, liquid TOC, gas chromatograph, ion chromatograph, ICP analysis, titration device, etc.
  • pH meters, sodium ion meters, electrical conductivity, etc. can be measured online.
  • the CO 2 /Na ratio can be monitored by creating a calibration curve by combining multiple solution state measurements based on different principles. pH measurement is particularly important. For example, if a calibration curve is created by combining a pH meter (with temperature compensation) and a Na+ ion meter, the CO 2 /Na ratio can be measured simply by measuring a small amount of salt water solution with these two measuring instruments. By combining these two measuring instruments with a device for adding a small amount of water to the sensor, even small amounts of solid samples can be measured online.
  • a step of washing the sodium carbonate adhering to the medium with water by supplying water that dissolves the sodium carbonate, causing it to flow out of the medium and be collected in a storage tank will be described. Washing involves applying a larger amount of water than wetting to wash the carbonates out of the media. This water washing makes the media reusable. The media is again wetted with an aqueous NaOH solution to absorb CO2 . When water is supplied to carbonates containing sodium sesquicarbonate or NaHCO3 on the medium, the carbonates downstream dissolve from the medium and are collected in the storage tank.
  • the storage tank according to this embodiment may be an open type storage tank or a closed type treatment tank.
  • CO 2 absorption from the atmosphere can continue to proceed within the tank.
  • a high temperature is preferable when the CO 2 /Na ratio is 0.5 to 0.67, and a low temperature is preferable when the CO 2 /Na ratio is 0.67 or more.
  • a sealed treatment tank can be applied to the recovery of high-concentration CO2 gas, etc. By slanting the storage tank, treatment tank, or piping, the aqueous solution can be collected by gravity.
  • the water used for washing does not need to be pure water. Impurities such as NaCl may be present. It is not necessary to wash away all the salt.
  • the water may be circulated and discharged using an aqueous carbonate solution in a storage tank.
  • the storage tanks in the fourth step are, for example, storage tanks 20.
  • the sodium carbonate is extracted from the aqueous solution of sodium carbonate accumulated in the storage tank, and ultimately stored on land in a location free from water inflow.
  • the carbon dioxide recovery and removal method of this embodiment can produce carbonate solids containing sodium sesquicarbonate with a CO2 /Na ratio of about 0.67 or more. When the CO2 /Na ratio is greater than 0.67, a high proportion of NaHCO3 salt can be mixed and produced. Unlike conventional CCS, which stores CO2 gas deep underground, the carbonate produced is solid and can be stored on land. Storage conditions vary depending on the type of carbonate, but generally it is best to store it in a place that is not susceptible to water inflow.
  • NaHCO3 is relatively stable when humidity is low, but when it comes into contact with water, it gradually decomposes in the air, so it must be stored in an environment that does not come into contact with water. Even if water is present, it can be stored stably in cold conditions or in an environment with a high CO2 concentration.
  • Sodium sesquicarbonate is more stable than NaHCO3 and is stable when in contact with water for short periods of time, but becomes unstable over long periods of time and at high temperatures. It is preferable to store NaHCO3 or sodium sesquicarbonate in a warehouse, tent, or cave where rainwater and groundwater cannot get in. In the case of sodium sesquicarbonate, it is sufficient to bury the carbonate in an open-cut hole and cover it with soil.
  • Na2CO3 , MgCO3 , CaCO3 , and basic magnesium carbonate are quite stable even when in contact with water. It is advisable to avoid contact with running water.
  • sodium sesquicarbonate or NaHCO3 decomposes significantly at 70°C, so it is best to store it in a location below that temperature, preferably below 50°C, and more preferably below 10°C.
  • Methods for extracting the solid salt from the carbonate aqueous solution accumulated in the water tank include natural drying in air, drying by heating, etc. It is preferable to evaporate the aqueous solution slowly while avoiding high temperatures.
  • the medium may be present if it is desired to proceed with the carbonation of CO2 during the removal and drying process, but may not be present if the subsequent process of separating the medium from the carbonate becomes complicated.
  • low-temperature distillation using a temperature difference in a sealed container, desiccant dehydration using a dehydrating agent, and reverse osmosis membrane separation using pressure can be used.
  • Silica gel dehydrating agents can be dehydrated at relatively low temperatures and can be regenerated by drying in the sun, etc.
  • the CO2 passes through the membrane, so the CO2 /Na ratio temporarily decreases, but high-concentration CO2 gas is obtained, so after dehydration, the high-concentration CO2 can be used to produce solid salt with a high CO2 /Na ratio.
  • the fourth step may include a salting-out step in which the aqueous solution of sodium carbonate accumulated in the storage tank is cooled or NaCl or Na 2 SO 4 is added to the aqueous solution to precipitate and separate a solid salt of a second carbonate.
  • the carbonate obtained in the fourth step may contain impurities, so there is a great advantage in being able to effectively use natural rock salt or salt derived from brine water.
  • impurities such as sodium sesquicarbonate
  • solid salts with a large CO2 /Na ratio can be preferentially precipitated. The higher the concentration and the lower the temperature , the greater the effect.
  • the fourth step may include a step of removing the liquid phase from the aqueous solution of sodium carbonate accumulated in the storage tank, which is in a liquid-solid phase mixture state in which a solid salt containing sodium sesquicarbonate and a saturated aqueous solution are mixed, returning the liquid phase to the medium, and separating carbonates having a CO2 /Na ratio in the solid phase greater than that of sodium sesquicarbonate.
  • the aqueous solution of sodium carbonate accumulated in the storage tank is evaporated and concentrated to a certain extent to produce a liquid-solid mixture of solid salts including sodium sesquicarbonate and a saturated aqueous solution, and then, by utilizing the difference in solubility between Na2CO3 and NaHCO3 , carbonates having a higher CO2 /Na ratio than sodium sesquicarbonate, that is, carbonates having a high proportion of NaHCO3 (which may contain some sesquisalt), can be separated.
  • the temperature of the aqueous solution is preferably 5°C or higher, and more preferably in the range of room temperature (20°C to 40°C).
  • the molar solubility of Na 2 CO 3 and NaHCO 3 differs greatly at room temperature from 20°C to around 40°C, and the difference is particularly large around 40°C. It is preferable to carry out this liquid-solid separation operation when the air temperature or water temperature is closest to 40°C, such as under sunlight during the day.
  • room temperature (20°C) to 40°C if a liquid-solid mixed state in which a solid salt containing sodium sesquicarbonate and a saturated aqueous solution are mixed is maintained, the concentration of Na 2 CO 3 will be high in the liquid phase and the ratio of NaHCO 3 will be high in the solid phase, so the CO 2 /Na ratio can be improved by removing the precipitate in the solid phase.
  • Examples of the method for generating the CO2 gas include a method of thermally decomposing the aqueous solution of the carbonate, a method of introducing an acidic aqueous solution generated by the electrolysis or electrodialysis into the aqueous solution of the carbonate, and a method of introducing an acidic substance such as a waste material into the aqueous solution of the carbonate.
  • the method of adding the acidic aqueous solution produced by electrolysis or electrodialysis to the aqueous carbonate solution is preferred, as this method can extract high concentration CO2 gas.
  • the high concentration CO2 gas thus generated can also be utilized.
  • Example 2 "Drying experiment using dehydrating agent in closed treatment tank" When an aqueous carbonate solution with a CO 2 /Na ratio of 0.67 was mixed with dehydrated silica gel in a closed treatment tank, a solid salt with a CO 2 /Na ratio of 0.65 was precipitated.
  • silica gel as a desiccant, dehydration was possible even at 60°C, confirming that the material can be regenerated by drying in the sun, etc.
  • the CO2 concentration was about 6000 ppm
  • the pH and CO2 /Na ratio of the liquid obtained after 159 hours were 8.8 and 1.0, respectively, which were equivalent to those of an aqueous NaHCO3 solution.
  • Example 12 As a method for easily determining the CO 2 /Na ratio, a pH meter (HORIBA, F-2000) and an electrical conductivity meter (HORIBA, LAQUAtwin, EC-33B) were used to create a two-dimensional calibration curve with different ratios and concentrations of NaOH-Na 2 CO 3 -NaHCO 3. An aqueous carbonate solution of unknown concentration was synthesized by reacting an aqueous NaOH solution with atmospheric CO 2 , and the results of this two-dimensional calibration curve were compared with the results of a TOC measurement (total Na content known), and it was found that they were consistent.
  • HORIBA pH meter
  • HORIBA electrical conductivity meter
  • the present invention provides a method for capturing and removing carbon dioxide gas that can directly reduce carbon dioxide in the atmosphere on a large scale.
  • Implementing certain methods shown in the present invention can contribute to negative emissions. It is a technology that suppresses global warming caused by carbon dioxide and promotes the realization of a low-carbon society.
  • medium 20 storage tank 30-1, 30-2: nozzles 40-1, 40-2: piping 50: inclined surface 60: pole

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Treating Waste Gases (AREA)

Abstract

L'invention concerne un procédé et un système de capture et d'élimination de dioxyde de carbone atmosphérique, le procédé et le système étant capables de réduire efficacement et directement le dioxyde de carbone atmosphérique à faible concentration. Un procédé de capture et d'élimination de dioxyde de carbone atmosphérique selon la présente invention comprend des étapes de génération d'un carbonate de sodium à l'aide d'une solution de NaOH générée par électrolyse ou électrodialyse et mise en contact de celui-ci avec du dioxyde de carbone atmosphérique. Le procédé comprend les première à quatrième étapes suivantes. (1) Une première étape consistant à étaler la solution de NaOH sur un milieu hydrophile et poreux afin de mouiller celui-ci. (2) Une seconde étape consistant à générer du carbonate de sodium en amenant le dioxyde de carbone atmosphérique à entrer en contact avec le NaOH. (3) Une troisième étape consistant à ajouter de l'eau pour maintenir un état humide dans lequel de l'eau est présente dans une phase liquide et pour ainsi augmenter le rapport CO2/Na dans le carbonate de sodium. (4) Une quatrième étape consistant à égoutter une solution du carbonate de sodium du milieu et à collecter celui-ci dans un réservoir de stockage.
PCT/JP2024/044657 2023-12-25 2024-12-17 Procédé et système de capture et d'élimination de dioxyde de carbone atmosphérique Pending WO2025142649A1 (fr)

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JP2023-218078 2023-12-25
JP2023218078 2023-12-25

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008510600A (ja) * 2004-08-20 2008-04-10 グローバル リサーチ テクノロジーズ，エルエルシー 空気中からの二酸化炭素の除去
JP2022105973A (ja) * 2021-01-05 2022-07-15 健司 反町 二酸化炭素固定装置
WO2022241049A1 (fr) * 2021-05-11 2022-11-17 Carbon Engineering Ltd. Contacteur gaz-liquide avec garnissage pour capturer du dioxyde de carbone
WO2023107578A1 (fr) * 2021-12-07 2023-06-15 Carbon Engineering Ltd. Capture de dioxyde de carbone

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008510600A (ja) * 2004-08-20 2008-04-10 グローバル リサーチ テクノロジーズ，エルエルシー 空気中からの二酸化炭素の除去
JP2022105973A (ja) * 2021-01-05 2022-07-15 健司 反町 二酸化炭素固定装置
WO2022241049A1 (fr) * 2021-05-11 2022-11-17 Carbon Engineering Ltd. Contacteur gaz-liquide avec garnissage pour capturer du dioxyde de carbone
WO2023107578A1 (fr) * 2021-12-07 2023-06-15 Carbon Engineering Ltd. Capture de dioxyde de carbone

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