WO2022030338A1 - 二酸化炭素固体回収材及びその製造方法 - Google Patents

二酸化炭素固体回収材及びその製造方法 Download PDF

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Publication number
WO2022030338A1
WO2022030338A1 PCT/JP2021/027994 JP2021027994W WO2022030338A1 WO 2022030338 A1 WO2022030338 A1 WO 2022030338A1 JP 2021027994 W JP2021027994 W JP 2021027994W WO 2022030338 A1 WO2022030338 A1 WO 2022030338A1
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Prior art keywords
carbon dioxide
weight
solid
recovery material
sodium
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PCT/JP2021/027994
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English (en)
French (fr)
Japanese (ja)
Inventor
宗由 坂本
伸哉 志茂
栄一 栗田
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Toda Kogyo Corp
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Toda Kogyo Corp
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Priority to US18/040,393 priority Critical patent/US12502637B2/en
Priority to CN202180057894.6A priority patent/CN116234625B/zh
Priority to KR1020237005860A priority patent/KR20230044243A/ko
Priority to EP21852264.7A priority patent/EP4194083A4/en
Priority to JP2022541476A priority patent/JP7771957B2/ja
Publication of WO2022030338A1 publication Critical patent/WO2022030338A1/ja
Anticipated expiration legal-status Critical
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    • B01D53/04—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography with stationary adsorbents
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Definitions

  • the present invention has been made in view of the above problems, and an object thereof is that carbon dioxide can be fixed in a low temperature range such as room temperature to 200 ° C., and carbon dioxide can be recovered and fixed by heating at 50 to 200 ° C. It is an object of the present invention to provide a solid carbon dioxide recovery material having excellent recovery performance and a method for producing the same.
  • carbon dioxide is fixed in a temperature range from room temperature to 200 ° C. by supporting sodium ferrite on a porous material or granulating with the porous material under predetermined conditions. Then, carbon dioxide fixed by heating at 50 to 200 ° C. can be recovered with high efficiency.
  • the carbon dioxide solid recovery material according to the present invention is a carbon dioxide solid recovery material containing 1% by weight to 99% by weight of sodium ferrite and 1% by weight to 99% by weight of a porous material.
  • the average particle size is 1 mm to 10 mm
  • the specific surface area is 5 m 2 / g to 1500 m 2 / g
  • the axial ratio of the average major axis diameter to the average minor axis diameter of the sodium ferrite primary particles is 1 to 2. It is characterized by being.
  • the solid carbon dioxide recovery material according to the present invention carbon dioxide can be fixed in a temperature range from room temperature to 200 ° C. and recovered by heating at 50 to 200 ° C., and has excellent fixed recovery performance.
  • the solid carbon dioxide recovery material according to the present invention contains the sodium ferrite in an amount of 1% by weight to 70% by weight, the porous material in an amount of 30% by weight to 99% by weight, and has a specific surface area of 100 m 2 / g to 1500 m 2 /. It is preferably g.
  • the hardness is 5 kgf / mm 2 to 35 kgf / mm 2 and the bulk density is 0.3 g / mL to 0.8 g / mL.
  • the porous material can promote the aggregation of sodium ferrite particles to form a molded product containing a high concentration of sodium ferrite. Therefore, the solid carbon dioxide recovery material according to the present invention containing sodium ferrite and a porous material has an excellent property of adsorbing carbon dioxide in a gas, confining it in the solid, and releasing carbon dioxide by heating. Can be done. Further, when granulating sodium ferrite exceeding 70% by weight and 99% by weight or less using a porous material of 1% by weight or more and less than 30% by weight, if the specific surface area is less than 5 m 2 / g, it is contained in the gas. If the specific surface area exceeds 500 m 2 / g, industrial production becomes difficult due to difficulty in contact with carbon dioxide, which reduces the fixed recovery performance of carbon dioxide.
  • the hardness is preferably 3 kgf / mm 2 to 30 kgf / mm 2
  • the sphericity is preferably 1 to 2.
  • the solid recovery material for carbon dioxide according to the present invention is basic, it becomes easy to catch carbon dioxide which is weakly acidic.
  • a solid and a solid are mixed and the element is moved and reacted without a solvent, so that a solvent as a reaction mother liquor is not used, so that a liquid phase reaction can be carried out. It is possible to suppress waste such as a solvent when used. In particular, in the case of a solid-phase reaction at a low temperature, an extremely high concentration reaction can occur, so that the energy cost can be kept low. Therefore, according to the method for producing a solid carbon dioxide recovery material according to the present invention, carbon dioxide can be fixed in a temperature range of room temperature to 200 ° C., and the fixed carbon dioxide can be recovered by heating at 50 to 200 ° C. with high efficiency. It is possible to produce a carbon dioxide recovery material having excellent fixed recovery performance.
  • the solid carbon dioxide recovery material according to the present embodiment contains 1% by weight to 70% by weight of sodium ferrite and 30% by weight to 99% by weight of a porous material. In the range of the weight%, sodium ferrite can be stably supported on the porous material while maintaining the fixed recovery performance of carbon dioxide originally possessed by sodium ferrite.
  • the carbon dioxide solid recovery material according to the present embodiment has an average particle size of 1 mm to 10 mm and a specific surface area of 100 m 2 / g to 1500 m 2 / g.
  • the average particle size of the solid carbon dioxide recovery material is preferably 2 mm to 8 mm.
  • the specific surface area of the solid recovery material for carbon dioxide is preferably 300 m 2 / g to 1000 m 2 / g.
  • the carbon dioxide solid recovery material according to the present embodiment has an axial ratio (average major axis diameter / average minor axis diameter) of the average major axis diameter to the average minor axis diameter of the primary particles of sodium ferrite being 1 to 2.
  • the axial ratio exceeds 2, the primary particles tend to aggregate with each other, and it becomes difficult to maintain a state in which the dispersibility of sodium ferrite is high.
  • the axial ratio cannot be less than 1.
  • the axial ratio of the primary particles of the solid recovery material of carbon dioxide is preferably 1.1 to 1.9.
  • the carbon dioxide solid recovery material according to the present embodiment preferably has a hardness of 5 kgf / mm 2 to 35 kgf / mm 2 and a bulk density of 0.3 g / mL to 0.8 g / mL.
  • the hardness and bulk density are in the above ranges, when the adsorption tower or the like is filled, it is difficult to break due to gravity or friction due to the flow of exhaust gas, and the gas such as exhaust gas easily flows.
  • the hardness is 6 kgf / mm 2 to 33 kgf / mm 2
  • the bulk density is 0.35 g / mL to 0.70 g / mL.
  • the carbon dioxide solid recovery material according to this embodiment preferably has a powder pH value of 8 to 14.
  • the powder pH value is 8 to 14
  • the solid carbon dioxide recovery material according to the present embodiment is basic, it is easy to catch weakly acidic carbon dioxide.
  • a more preferable powder pH value is 9 to 14.
  • the porous material according to the present embodiment is a porous material selected from activated carbon, porous clay minerals such as zeolite, porous silica and activated alumina.
  • porous clay minerals such as smectite, sepiolite, imogolite, barigolite, kaolin, montmorillonite, bentonite, attapargite, acidic clay, cordierite, and limonite can be used. Since the porous material has excellent adsorptivity, it is possible to support a large amount of sodium ferrite and improve the fixed recovery ability of carbon dioxide.
  • activated carbon has a strong adsorptive power because it has a small pore diameter. Therefore, activated carbon is preferable because it can support a large amount of sodium ferrite and improve the fixed recovery ability of carbon dioxide.
  • the porous material preferably has a porosity of more than 50% and 70% or less.
  • the porosity is 50% or less, the specific surface area of the solid recovery material of carbon dioxide, that is, the contact area with carbon dioxide becomes small, and the absorption rate of carbon dioxide may decrease.
  • the porosity exceeds 70%, the volume ratio of sodium ferrite decreases, and the fixed recovery performance of carbon dioxide deteriorates.
  • the solid carbon dioxide recovery material according to this embodiment can selectively adsorb carbon dioxide from a gas containing carbon dioxide and can be fixed.
  • the adsorption temperature is about 10 ° C. to 200 ° C., which is the room temperature to the exhaust gas outlet temperature. Since no additional heating from the outside is required, the energy cost for adsorption can be kept low (the above is the carbon dioxide fixation process).
  • the solid carbon dioxide recovery material according to the present embodiment desorbs carbon dioxide taken in by the above-mentioned carbon dioxide fixing step at a temperature of 50 to 200 ° C. in a carbon dioxide-free gas atmosphere to release carbon dioxide. It is preferable to collect it. Since the desorption temperature is as low as 200 ° C. or lower, the energy cost for desorption can be kept low (above, carbon dioxide recovery step).
  • the solid carbon dioxide recovery material according to the present embodiment can be obtained by reacting a material containing iron oxide with an alkaline compound containing sodium in the presence of a porous material (support).
  • the compound containing sodium is not particularly limited, but for example, sodium nitrite, sodium sulfate, sodium carbonate, sodium hydrogen carbonate, sodium hydroxide and the like can be used. However, considering industrial use, sodium nitrite, sodium sulfate, etc., which may generate toxic nitrite gas, sulfurous acid gas, etc. during manufacturing should be avoided.
  • the solid-phase reaction is a synthetic method in which a solid and a solid are mixed and the elements are moved and reacted without a solvent. Since no solvent is used as the reaction mother liquor, waste such as the solvent when used for the liquid phase reaction can be suppressed. Further, in the case of a solid-phase reaction at a low temperature, which is also a feature of the present invention, an extremely high concentration reaction can occur, so that the energy cost can be suppressed to a low level. Moreover, since the high reaction concentration and the need for washing are not required, a high yield of the product can be expected.
  • the solid carbon dioxide recovery material according to the present embodiment contains sodium ferrite in an amount of more than 70% by weight and 99% by weight or less, and a porous material of 1% by weight or more and less than 30% by weight.
  • the solid carbon dioxide recovery material according to the present embodiment is a molded product containing a high concentration of sodium ferrite while maintaining the fixed recovery performance of carbon dioxide originally possessed by sodium ferrite. Can be formed.
  • the carbon dioxide solid recovery material according to the present embodiment has an average particle size of 1 mm to 10 mm and a specific surface area of 5 m 2 / g to 500 m 2 / g.
  • the average particle size of the solid carbon dioxide recovery material is preferably 2 mm to 8 mm.
  • the specific surface area of the solid recovery material for carbon dioxide is preferably 30 m 2 / g to 300 m 2 / g.
  • the carbon dioxide solid recovery material according to the present embodiment has an axial ratio (average major axis diameter / average minor axis diameter) of the average major axis diameter to the average minor axis diameter of the primary particles of sodium ferrite being 1 to 2.
  • the axial ratio exceeds 2, the primary particles tend to aggregate with each other, and it becomes difficult to maintain a state in which the dispersibility of sodium ferrite is high.
  • the axial ratio cannot be less than 1.
  • the axial ratio of the primary particles of the solid recovery material of carbon dioxide is preferably 1.1 to 1.9.
  • the carbon dioxide solid recovery material according to the present embodiment preferably has an average primary particle diameter of 0.05 ⁇ m to 1.0 ⁇ m as the primary particles of sodium ferrite. If it is less than 0.05 ⁇ m, industrial production becomes difficult. Further, if it exceeds 1.0 ⁇ m, the carbon dioxide absorption performance becomes low. It is more preferably 0.1 ⁇ m to 0.7 ⁇ m.
  • the carbon dioxide solid recovery material according to the present embodiment preferably has a hardness of 3 kgf / mm 2 to 30 kgf / mm 2 and a sphericity of 1 to 2.
  • a hardness of 3 kgf / mm 2 to 30 kgf / mm 2 and a sphericity of 1 to 2.
  • the shape of the solid recovery material for carbon dioxide is not particularly limited, but a spindle shape, a rectangular parallelepiped shape, a dice shape, a columnar shape, or the like is preferable in addition to the spherical shape.
  • the carbon dioxide solid recovery material according to this embodiment preferably has a powder pH value of 8 to 14.
  • the powder pH value is 8 to 14
  • the solid carbon dioxide recovery material according to the present embodiment becomes basic, and it is easy to catch weakly acidic carbon dioxide.
  • the carbon dioxide solid recovery material according to this embodiment preferably has a molar ratio of Na / Fe of sodium ferrite of 0.7 to 1.3. In the range of the molar ratio, a large amount of sodium ferrite crystal phase can be contained, and the fixed recovery performance of carbon dioxide becomes good.
  • the porous material according to the present embodiment is preferably a porous material selected from activated carbon, aluminosilicate, hydrotalcite, porous clay mineral, porous silica and activated alumina.
  • a porous clay mineral zeolite, smectite, sepiolite, imogolite, varigorskite, kaolin, montmorillonite, bentonite, attapargit, acidic clay, cordierite, limonite and the like can be used. Since the porous material has excellent adsorptivity, it is possible to form a molded product containing a high concentration of sodium ferrite, and it is possible to improve the fixed recovery ability of carbon dioxide.
  • the porous material preferably has a porosity of more than 50% and 70% or less.
  • the porosity is 50% or less, the specific surface area of the solid recovery material of carbon dioxide, that is, the contact area with carbon dioxide becomes small, and the absorption rate of carbon dioxide may decrease.
  • the porosity exceeds 70%, the volume ratio of sodium ferrite decreases, and the fixed recovery performance of carbon dioxide deteriorates.
  • iron oxide and sodium source powder are mixed and pulverized, and calcined to obtain sodium ferrite particle powder, and then the obtained sodium ferrite particle powder and a porous material are mixed.
  • Granulation is performed using a granulator such as a rolling granulator. Then, by firing, a solid recovery material of carbon dioxide can be obtained.
  • steam heating, microwave heating, ultrasonic heating, or the like may be performed for firing.
  • a porous material selected from activated carbon, aluminosilicate, hydrotalcite, porous clay minerals such as zeolite, porous silica and activated alumina can be used.
  • porous clay minerals such as smectite, sepiolite, imogolite, barigolite, kaolin, montmorillonite, bentonite, attapargite, acidic clay, cordierite, and limonite can be used.
  • the content of the porous material is preferably 1% by weight or more and less than 30% by weight. This is because, as described above, the formation of a molded product containing a high concentration of sodium ferrite improves the fixed recovery ability of carbon dioxide.
  • the material containing iron oxide is not particularly limited, but for example, hematite, magnetite, maghemite, goethite and the like can be used.
  • the compound containing sodium is not particularly limited, but for example, sodium nitrite, sodium hydroxide, sodium oxide, sodium carbonate and the like can be used. However, considering industrial use, sodium nitrite, sodium sulfate, etc., which may generate toxic nitrite gas, sulfurous acid gas, etc. during manufacturing should be avoided.
  • the solid-phase reaction is a synthetic method in which a solid and a solid are mixed and the elements are moved and reacted without a solvent. Since no solvent is used as the reaction mother liquor, waste such as the solvent when used for the liquid phase reaction can be suppressed. Further, in the case of a solid-phase reaction at a low temperature, which is also a feature of the present invention, an extremely high concentration reaction can occur, so that the energy cost can be suppressed to a low level. Moreover, since there is no need for the high-concentration reaction or washing, a high yield of the product can be expected.
  • Typical embodiments of the present invention are as follows.
  • composition of the solid carbon dioxide recovery material according to the present invention was identified by the fully automatic multipurpose X-ray diffractometer D8 ADVANCE manufactured by BRUKER after crushing the solid carbon dioxide recovery material in a dairy pot and pelletizing it. It was identified as a ferrite and a porous material.
  • the content of sodium ferrite and the porous material contained in the solid recovery material of carbon dioxide according to the present invention is determined by crushing the solid recovery material of carbon dioxide in a dairy pot, pelletizing it, and then analyzing it by scanning fluorescent X-rays manufactured by Rigaku. Elemental analysis (excluding oxygen) was performed with the apparatus ZSX PrimusII and quantified.
  • the BET specific surface area of the solid carbon dioxide recovery material according to the present invention was measured by the BET method using nitrogen using Multisorb-16 manufactured by QUANTA CHROME.
  • the average value of the crushing hardness of 80 grains was taken as the hardness by the digital force gauge ZP-500N manufactured by Imada.
  • the bulk density of the solid carbon dioxide recovery material according to the present invention was measured according to JISZ2504.
  • the determination of the bulk density of the solid carbon dioxide recovery material according to the present invention was evaluated in the following four stages.
  • the sphericity of the solid carbon dioxide recovery material according to the present invention was evaluated in the following two stages by calculating the ratio of the major axis to the minor axis.
  • ⁇ Sphericity of 1 or more and less than 2
  • ⁇ Sphericity of 2 or more
  • the pH value of the solid carbon dioxide recovery material according to the present invention is determined by weighing 5 g of a sample in a 300 ml Erlenmeyer flask, adding 100 ml of boiled pure water, heating and holding the boiled state for about 5 minutes, and then plugging. Allow to cool to room temperature, add water equivalent to weight loss, plug again, shake for 1 minute, allow to stand for 5 minutes, and then measure the pH of the obtained supernatant according to JIS Z8802-7 to obtain. The value was taken as the pH value.
  • the molar ratio of Na / Fe of sodium ferrite contained in the solid recovery material of carbon dioxide according to the present invention is determined by crushing the solid recovery material of carbon dioxide in a dairy pot, pelletizing it, and then using a scanning fluorescent X-ray analyzer manufactured by Rigaku. Elemental analysis (excluding oxygen) was performed with ZSX PrimusII and quantified.
  • the axial ratio of sodium ferrite contained in the carbon dioxide recovery material according to the present invention is the average major axis diameter and average minor axis of the particle diameter of 350 primary particles shown in the micrograph by the Hitachi High-Tech scanning electron microscope S-4800. The diameters were measured and shown as the ratio of the average major axis diameter to the average minor axis diameter (average major axis diameter / average minor axis diameter).
  • the average primary particle size of the sodium ferrite particle powder contained in the carbon dioxide recovery material according to the present invention is shown as the average value of the average minor axis diameter of the average major axis diameter.
  • Example 1 9.0 parts by weight of ferrous chloride tetrahydrate is dissolved in 900 parts by weight of pure water, and granulated activated carbon (Kuraray Kuraraycol 4GG, 4x6 mesh) 10.0 is used as a porous support. A portion by weight was added and immersed for 1 hour. To this, 27 parts by weight of urea dissolved in 100 parts by weight of pure water was added, the temperature was raised to 90 ° C., the mixture was stirred for 3 hours, and then the mixture was stirred for 10 hours while allowing to cool.
  • Kuraray Kuraraycol 4GG, 4x6 mesh granulated activated carbon
  • iron oxide-supported activated carbon was obtained.
  • the obtained iron oxide-supported activated carbon and 1.80 parts by weight of sodium hydroxide were mixed in a solid state, placed in a crucible, and subjected to a solid-phase reaction at 400 ° C. in a nitrogen stream for 16 hours. Then, it was cooled to room temperature and used as a solid recovery material for carbon dioxide.
  • the obtained solid recovery material of carbon dioxide was pulverized and qualitatively determined by X-ray diffraction. As a result, it was sodium ferrite and amorphous carbon.
  • the hardness of the obtained solid recovery material of carbon dioxide was 20 kgf / mm 2 , and the bulk density was 0.48 g / mL. From these results, it is clear that when the carbon dioxide recovery material according to Example 1 is filled in a carbon dioxide adsorption tower or the like, it is not easily broken due to gravity or friction due to the distribution of exhaust gas, and gas such as exhaust gas is easily distributed. be.
  • the hardness of the obtained carbon dioxide recovery material was evaluated in the following three stages. ⁇ : Crushing hardness of 10 kgf / mm 2 or more ⁇ : Crushing hardness of 5 to 10 kgf / mm less than 2 ⁇ : Crushing hardness of less than 5 kgf / mm 2
  • the molar ratio of Na / Fe of sodium ferrite contained in the obtained solid recovery material of carbon dioxide was 1.0, which was almost the same as the charging ratio of the raw materials.
  • FIG. 1 shows a measurement chart with the horizontal axis as the sample temperature.
  • the TG curve was the weight% of the residual sample at each temperature when the initial value was 100% by weight, and the decrease in the sample was considered to be due to the emission of carbon dioxide.
  • the DTG curve is a differential curve of the TG curve, and the temperature at which the maximum value of the DTG curve is taken is regarded as the carbon dioxide desorption temperature.
  • the DTA curve showed a downwardly convex curve, and it was found that the endothermic reaction was carried out at around 114 ° C.
  • the desorption temperature of carbon dioxide was 114 ° C.
  • the desorption amount of carbon dioxide was 10% by weight with respect to the sample solid content, which was excellent fixation of carbon dioxide. It became clear that there was recovery performance.
  • Examples 2-8 The solid recovery materials according to Examples 2 to 8 were obtained in the same manner as in Example 1 except that the types and amounts of the iron raw material and the support were variously changed.
  • Comparative Example 1 9.0 parts by weight of ferrous chloride tetrahydrate was dissolved in 900 parts by weight of pure water and stirred for 1 hour. To this, 27 parts by weight of urea dissolved in 100 parts by weight of pure water was added, the temperature was raised to 90 ° C., the mixture was stirred for 3 hours, then stirred for 10 hours while allowing to cool, washed with filtered water, and washed at 80 ° C. The mixture was dried for 12 hours to obtain iron oxide fine particles. The obtained iron oxide fine particles and 1.80 parts by weight of sodium hydroxide were mixed in a solid state, placed in a crucible, and subjected to a solid phase reaction at 400 ° C. in a nitrogen stream for 16 hours.
  • the obtained powder was pulverized and X-ray diffraction revealed that it was sodium ferrite.
  • fluorescent X-rays revealed that the content of sodium ferrite was 90% by weight.
  • the remaining 10% by weight was maghemite.
  • the obtained powder was suspended in 100 parts by weight of pure water, 10 parts by weight of activated carbon was added thereto as a porous support, and the mixture was stirred for 16 hours, and then water was distilled off while rotating with an evaporator.
  • As a solid recovery material for carbon dioxide As a solid recovery material for carbon dioxide. When the obtained solid recovery material was pulverized and qualitized by X-ray diffraction, it was found to be maghemite, sodium ferrite and amorphous carbon.
  • the average major axis diameter was 0.7 ⁇ m
  • the average minor axis diameter was 0.4 ⁇ m
  • the average primary particle diameter was 0.57 ⁇ m
  • the axial ratio was 1.6. ..
  • the powder pH was relatively high at 13.8. 100 parts by weight of the obtained sodium ferrite particle powder is mixed with 5 parts by weight of powdered activated carbon as a porous material, and tumbled and granulated at 40 rpm with a rolling granulator to obtain a spherical granule having a particle size of 5 mm. Obtained. This was placed in a crucible and sintered in a nitrogen stream at 400 ° C. for 16 hours.
  • the obtained solid recovery material of carbon dioxide was pulverized and qualitatively determined by X-ray diffraction. As a result, it was sodium ferrite and amorphous carbon. In addition, fluorescent X-rays revealed that the content of sodium ferrite was 95%. The porous material was 5%.
  • the BET specific surface area of this solid carbon dioxide recovery material was 54 m 2 / g. The minor axis was 5 mm, the major axis was 5 mm, and the average particle size was 5 mm.
  • the powder pH was 13.
  • the hardness of the obtained solid recovery material of carbon dioxide was 10 kgf / mm 2 , and the sphericity was 1.0. From these results, it is clear that when the carbon dioxide recovery material according to Example 9 is filled in a carbon dioxide adsorption tower or the like, it is not easily broken due to gravity or friction due to the distribution of exhaust gas, and gas such as exhaust gas is easily distributed. be.
  • the hardness of the obtained carbon dioxide recovery material was evaluated in the following three stages. ⁇ : Crushing hardness of 10 kgf / mm 2 or more ⁇ : Crushing hardness of 3 kgf / mm 2 or more and less than 10 kgf / mm 2 ⁇ : Crushing hardness of less than 3 kgf / mm 2
  • the molar ratio of Na / Fe of sodium ferrite contained in the obtained solid recovery material of carbon dioxide was 1.0, which was almost the same as the charging ratio of the raw materials.
  • FIG. 2 shows a measurement chart with the horizontal axis as the sample temperature.
  • the TG curve was the weight% of the residual sample at each temperature when the initial value was 100% by weight, and the decrease in the sample was considered to be due to the emission of carbon dioxide.
  • the DTG curve is a differential curve of the TG curve, and the temperature at which the maximum value of the DTG curve is taken is regarded as the carbon dioxide desorption temperature.

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JP7248202B1 (ja) * 2022-10-18 2023-03-29 住友電気工業株式会社 二酸化炭素吸収モジュール、二酸化炭素吸収塔、二酸化炭素吸収装置及び二酸化炭素吸収方法
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JP2024003311A (ja) * 2022-06-27 2024-01-15 鹿島道路株式会社 路盤材
EP4541770A4 (en) * 2022-06-14 2026-02-11 Toda Kogyo Corp COMPOSITE IRON OXIDE PARTICLE POWDER AND ITS MANUFACTURING PROCESS

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