WO2022149535A1 - Ra-226の回収方法、Ra-226溶液の製造方法及びAc-225溶液の製造方法 - Google Patents
Ra-226の回収方法、Ra-226溶液の製造方法及びAc-225溶液の製造方法 Download PDFInfo
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- WO2022149535A1 WO2022149535A1 PCT/JP2021/048690 JP2021048690W WO2022149535A1 WO 2022149535 A1 WO2022149535 A1 WO 2022149535A1 JP 2021048690 W JP2021048690 W JP 2021048690W WO 2022149535 A1 WO2022149535 A1 WO 2022149535A1
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- radium
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- 238000000034 method Methods 0.000 title claims abstract description 59
- 238000011084 recovery Methods 0.000 title claims abstract description 19
- 238000004519 manufacturing process Methods 0.000 title claims description 30
- 239000000126 substance Substances 0.000 claims abstract description 50
- 239000007787 solid Substances 0.000 claims abstract description 35
- 229910001426 radium ion Inorganic materials 0.000 claims abstract description 19
- 239000007788 liquid Substances 0.000 claims description 75
- 229910052705 radium Inorganic materials 0.000 claims description 48
- HCWPIIXVSYCSAN-UHFFFAOYSA-N radium atom Chemical compound [Ra] HCWPIIXVSYCSAN-UHFFFAOYSA-N 0.000 claims description 48
- 230000005855 radiation Effects 0.000 claims description 29
- 229910052770 Uranium Inorganic materials 0.000 claims description 25
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims description 25
- 239000002253 acid Substances 0.000 claims description 19
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- 230000001678 irradiating effect Effects 0.000 claims description 9
- NBZBKCUXIYYUSX-UHFFFAOYSA-N iminodiacetic acid Chemical group OC(=O)CNCC(O)=O NBZBKCUXIYYUSX-UHFFFAOYSA-N 0.000 claims description 6
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- 238000001914 filtration Methods 0.000 description 16
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- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 12
- -1 alkali metal salt Chemical class 0.000 description 11
- 239000003957 anion exchange resin Substances 0.000 description 11
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- MXQFUMUIEZBICJ-UHFFFAOYSA-L [Ra+2].[O-]S([O-])(=O)=O Chemical compound [Ra+2].[O-]S([O-])(=O)=O MXQFUMUIEZBICJ-UHFFFAOYSA-L 0.000 description 8
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- 239000002245 particle Substances 0.000 description 7
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- KBPLFHHGFOOTCA-UHFFFAOYSA-N 1-Octanol Chemical compound CCCCCCCCO KBPLFHHGFOOTCA-UHFFFAOYSA-N 0.000 description 6
- YPWICUOZSQYGTD-UHFFFAOYSA-L [Ra+2].[O-]C([O-])=O Chemical compound [Ra+2].[O-]C([O-])=O YPWICUOZSQYGTD-UHFFFAOYSA-L 0.000 description 6
- 238000002474 experimental method Methods 0.000 description 6
- 229910000029 sodium carbonate Inorganic materials 0.000 description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 5
- 229910021529 ammonia Inorganic materials 0.000 description 5
- 238000004070 electrodeposition Methods 0.000 description 5
- 238000000605 extraction Methods 0.000 description 5
- 150000002500 ions Chemical class 0.000 description 5
- 238000007670 refining Methods 0.000 description 5
- 230000002378 acidificating effect Effects 0.000 description 4
- 229910052783 alkali metal Inorganic materials 0.000 description 4
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 4
- 150000001342 alkaline earth metals Chemical class 0.000 description 4
- 150000001875 compounds Chemical class 0.000 description 4
- ZAASRHQPRFFWCS-UHFFFAOYSA-P diazanium;oxygen(2-);uranium Chemical compound [NH4+].[NH4+].[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[U].[U] ZAASRHQPRFFWCS-UHFFFAOYSA-P 0.000 description 4
- 238000010828 elution Methods 0.000 description 4
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- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
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- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
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- 239000000872 buffer Substances 0.000 description 2
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- 229910052742 iron Inorganic materials 0.000 description 2
- 230000007935 neutral effect Effects 0.000 description 2
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- 230000005260 alpha ray Effects 0.000 description 1
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- 229910000024 caesium carbonate Inorganic materials 0.000 description 1
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- 239000010949 copper Substances 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
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- NBVXSUQYWXRMNV-UHFFFAOYSA-N fluoromethane Chemical compound FC NBVXSUQYWXRMNV-UHFFFAOYSA-N 0.000 description 1
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- JEGUKCSWCFPDGT-UHFFFAOYSA-N h2o hydrate Chemical compound O.O JEGUKCSWCFPDGT-UHFFFAOYSA-N 0.000 description 1
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- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 1
- 229910052808 lithium carbonate Inorganic materials 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
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- 125000002347 octyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 1
- 238000010979 pH adjustment Methods 0.000 description 1
- 239000008055 phosphate buffer solution Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- HWLDNSXPUQTBOD-UHFFFAOYSA-N platinum-iridium alloy Chemical compound [Ir].[Pt] HWLDNSXPUQTBOD-UHFFFAOYSA-N 0.000 description 1
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- GIKWXTHTIQCTIH-UHFFFAOYSA-L radium bromide Chemical compound [Br-].[Br-].[Ra+2] GIKWXTHTIQCTIH-UHFFFAOYSA-L 0.000 description 1
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- 239000011701 zinc Substances 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
- C22B7/005—Separation by a physical processing technique only, e.g. by mechanical breaking
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B60/00—Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
- C22B60/02—Obtaining thorium, uranium, or other actinides
- C22B60/0204—Obtaining thorium, uranium, or other actinides obtaining uranium
- C22B60/0217—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes
- C22B60/0252—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries
- C22B60/026—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries liquid-liquid extraction with or without dissolution in organic solvents
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B3/00—Extraction of metal compounds from ores or concentrates by wet processes
- C22B3/20—Treatment or purification of solutions, e.g. obtained by leaching
- C22B3/22—Treatment or purification of solutions, e.g. obtained by leaching by physical processes, e.g. by filtration, by magnetic means, or by thermal decomposition
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B3/00—Extraction of metal compounds from ores or concentrates by wet processes
- C22B3/20—Treatment or purification of solutions, e.g. obtained by leaching
- C22B3/22—Treatment or purification of solutions, e.g. obtained by leaching by physical processes, e.g. by filtration, by magnetic means, or by thermal decomposition
- C22B3/24—Treatment or purification of solutions, e.g. obtained by leaching by physical processes, e.g. by filtration, by magnetic means, or by thermal decomposition by adsorption on solid substances, e.g. by extraction with solid resins
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B3/00—Extraction of metal compounds from ores or concentrates by wet processes
- C22B3/20—Treatment or purification of solutions, e.g. obtained by leaching
- C22B3/26—Treatment or purification of solutions, e.g. obtained by leaching by liquid-liquid extraction using organic compounds
- C22B3/28—Amines
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B3/00—Extraction of metal compounds from ores or concentrates by wet processes
- C22B3/20—Treatment or purification of solutions, e.g. obtained by leaching
- C22B3/26—Treatment or purification of solutions, e.g. obtained by leaching by liquid-liquid extraction using organic compounds
- C22B3/40—Mixtures
- C22B3/402—Mixtures of acyclic or carbocyclic compounds of different types
- C22B3/404—Mixtures of acyclic or carbocyclic compounds of different types of organic acids and oximes
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B3/00—Extraction of metal compounds from ores or concentrates by wet processes
- C22B3/20—Treatment or purification of solutions, e.g. obtained by leaching
- C22B3/42—Treatment or purification of solutions, e.g. obtained by leaching by ion-exchange extraction
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B60/00—Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
- C22B60/02—Obtaining thorium, uranium, or other actinides
- C22B60/0295—Obtaining thorium, uranium, or other actinides obtaining other actinides except plutonium
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
- C22B7/04—Working-up slag
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/20—Recycling
Definitions
- One aspect of the present invention relates to a method for recovering 226 Ra, a method for producing a 226 Ra solution, or a method for producing a 225 Ac solution.
- RI internal therapy is performed in which a drug containing a radioisotope (RI) is selectively taken up into a lesion such as a tumor for treatment.
- RI radioisotope
- alpha rays have a short range, so that the effect of unnecessary exposure to surrounding normal cells is small.
- 225 Ac which is one of the alpha ray emitting nuclides, is a radionuclide having a half-life of 10 days, and is expected as a therapeutic nuclide in the treatment of cancer in recent years.
- 225 Ac is produced by the nuclear reaction of (p, 2n), for example, by irradiating the 226 Ra target with protons using an accelerator. Therefore, in order to produce 225 Ac, 226 Ra is required as a raw material for the 226 Ra target.
- 226 Ra was factory-produced from ore and processed into radium-based radiation sources for radiotherapy, but in recent years it has hardly been produced. Therefore, there is a demand for a technique for recovering 226 Ra from already produced substances containing 226 Ra such as radium radiation sources and other naturally collected materials containing 226 Ra.
- a part of the 226 Ra-containing substance is collected from the radium source, the chemical form of 226 Ra contained in the radium source is determined, and then the chemical form is used.
- a method of extracting and recovering 226 Ra by a suitable treatment method is known. For example, if the chemical form of 226 Ra is radium sulfate, it is heated in an aqueous solution of sodium carbonate to generate radium carbonate, the radium carbonate is filtered with a filter, the filter is washed, and then dissolved with acid to dissolve 226 Ra. To collect.
- Non-Patent Document 1 an attempt is made to isolate 226 Ra from solid radium sulfate, and its efficiency is evaluated.
- the above-mentioned conventional method has the following problems. -Since the operation of collecting a 226 Ra sample from a radium radiation source is difficult and complicated, the possibility of exposure was high. -It was difficult to identify the chemical form of 226 Ra, and it was sometimes not possible to select an appropriate treatment method. -The conversion efficiency from radium sulfate to radium carbonate was not 100%, and the recovery rate of 226 Ra was low because radium sulfate and radium carbonate were slightly dissolved in water. -If salt or the reagent used remains in the 226 Ra recovered product, there is a concern that the electrodeposition rate will decrease when 226 Ra is electrodeposited for the production of the 226 Ra target.
- Non-Patent Document 1 226 Ra has been successfully isolated quantitatively by several methods, but the reagent for adsorbing 226 Ra used here, particularly EDTA, needs to be dissolved in water. Therefore, a step for separating 226 Ra-EDTA from the aqueous matrix is required in the subsequent operation. In addition, since 226 Ra and EDTA strongly form a chelate bond, a step of releasing 226 Ra from EDTA is required. Therefore, there is a problem that the process becomes complicated and the possibility of radiation exposure is high.
- One aspect of the present invention provides a method for recovering 226 Ra, a method for producing a 226 Ra solution, and a method for producing a 225 Ac solution.
- One aspect of the present invention is a step of immersing a solid 226 Ra-containing substance and a carrier having a function of adsorbing 226 Ra ions in a treatment liquid, and then irradiating the treatment liquid with ultrasonic waves (A1).
- 226 Ra recovery method including.
- another aspect of the present invention is a step of immersing a solid 226 Ra-containing substance and a carrier having a function of adsorbing 226 Ra ions in a treatment liquid, and then irradiating the treatment liquid with ultrasonic waves.
- A1 a 226 Ra solution comprising a step (A2) of separating the carrier from the treatment liquid, and a step (A3) of eluting 226 Ra from the carrier separated in the step (A2) with an acid. It is a manufacturing method of.
- another aspect of the present invention includes a step of obtaining a 226 Ra solution (B1) by the method for producing a 226 Ra solution described above, and a step of producing a 225 Ac solution from the 226 Ra solution (B2). , 225 This is a method for producing an Ac solution.
- 226 Ra can be recovered efficiently and easily even if the chemical form of 226 Ra is unknown. Further, according to the method for producing a 226 Ra solution, which is one aspect of the present invention, the 226 Ra solution can be efficiently and easily produced even if the chemical form of the 226 Ra is unknown. Further, according to the method for producing a 225 Ac solution, which is one aspect of the present invention, the 225 Ac solution can be efficiently produced using the 226 Ra solution obtained by the above production method.
- the method for recovering 226 Ra (hereinafter, also referred to as “recovery method (X)”), which is one aspect of the present invention, comprises a solid 226 Ra-containing substance and a carrier having a function of adsorbing 226 Ra ions (hereinafter, “recovery method (X)”).
- the carrier (i) is included in the step (A1) of immersing the treatment liquid in the treatment liquid and then irradiating the treatment liquid with ultrasonic waves.
- Step (A1) the solid 226 Ra-containing substance and the carrier (i) are immersed in the treatment liquid, and then the treatment liquid is irradiated with ultrasonic waves.
- the conditions of the step (A1) are not particularly limited as long as the carrier (i) can adsorb 226 Ra ions, but the steps (A1) can be performed under neutral or alkaline conditions, and are preferably performed under alkaline conditions.
- Alkaline conditions are more preferably alkaline conditions in which the pH is adjusted using at least one selected from the group consisting of ammonia, alkali metal hydroxides, alkaline metal carbonates, and alkaline buffers.
- the step (A1) is carried out under alkaline conditions in which the pH is adjusted with ammonia.
- the alkali metal salt does not remain in the subsequent steps, so it can be suitably used for applications where the residual alkali metal salt may have an adverse effect, such as using the recovered solution containing 226 Ra for electrodeposition.
- the solution containing the recovered 226 Ra can be used for a wide range of purposes.
- alkali metal hydroxides include lithium hydroxide, sodium hydroxide, potassium hydroxide, rubidium hydroxide, and cesium hydroxide.
- Examples of the carbonate of the alkali metal include sodium carbonate, potassium carbonate, lithium carbonate and cesium carbonate.
- alkaline buffer solution include boric acid buffer solution, Tris buffer solution, phosphate buffer solution, and McKillbane buffer solution.
- the pH adjustment may be performed at any timing as long as it is before the treatment liquid and the carrier (i) are brought into contact with each other. That is, the solid 226 Ra-containing substance may be immersed in the treatment liquid under neutral conditions and then subjected to alkaline conditions, or the solid 226 Ra-containing substance may be immersed in the treatment liquid and then subjected to alkaline conditions. However, the solid 226 Ra-containing substance may be subjected to alkaline conditions before being immersed in the treatment liquid.
- the solid 226 Ra-containing substance is not particularly limited as long as it is a substance containing 226 Ra and is solid at 25 ° C.
- the solid state means that the 226 Ra-containing substance has no fluidity when allowed to stand on a horizontal plane at 25 ° C.
- the solid 226 Ra-containing material is preferably at least one selected from the group consisting of uranium slag and radium radiation sources.
- a radium radiation source in which 226 Ra is sealed for radiotherapy is well known.
- the structure of the radium radiation source is not particularly limited, and those having various structures can be used.
- the 226 Ra is sealed and housed in a single or double casing containing, for example, iron, titanium, platinum, platinum iridium and the like.
- the shape and size of the radium radiation source are not particularly limited, and examples of the shape include a needle shape (long rod shape), a tubular shape, a plate shape, a rugby ball shape, a spherical shape, and the like, preferably a needle shape (long rod shape). be.
- the size is preferably 1 to 50 mm in length and 0.5 to 5.0 mm in diameter.
- the chemical form of 226 Ra contained in the radium radiation source is not particularly limited, and various chemical forms can be used.
- the chemical form of 226 Ra contained in radium sources is often radium sulfate, rarely radium bromide.
- the uranium slag (also referred to as slag) is an unnecessary substance separated during the refining of uranium ore, and the composition and refining process are not particularly limited. Coarse refining of uranium ore is carried out, for example, in the following steps.
- Uranium ore is crushed and crushed, dissolved with acid or alkali, uranium is leached into a liquid, and then solid-liquid separation is performed.
- the obtained liquid is subjected to solvent extraction using an ion exchange resin to remove impurities, and uranium is concentrated to obtain a uranium purified liquid.
- the purified uranium solution is allowed to stand and precipitates, which is called yellow cake. Therefore, more specifically, the uranium slag is a combination of the solid obtained by solid-liquid separation in the above-mentioned step and the waste liquid generated in the process of obtaining yellow cake from the purified uranium liquid. That is, the uranium slag contains a solid uranium slag and a liquid uranium slag.
- Uranium ore contains 226 Ra, albeit at a very low concentration. Since 226 Ra is transferred to slag in the crude refining process, solid slag (solid obtained by solid-liquid separation) and liquid slag (waste liquid generated in the process of obtaining yellow cake from uranium refined liquid) are 226 Ra. Contains.
- the 226 Ra content of solid and liquid slag can vary depending on the type of uranium ore and the uranium crude smelting process, but solid slag is considered to be more common.
- the process of obtaining yellow cake from uranium ore is generally called crude refining, and it is performed at the factory attached to the uranium mine.
- a large amount of uranium slag is disposed of in the uranium slag dam adjacent to the factory. Therefore, recovering 226 Ra from uranium slag is significant not only because 226 Ra, which exists on the earth in a finite amount, can be used without waste, but also because environmental pollution caused by 226 Ra can be prevented.
- the carrier (i) is not particularly limited as long as it has a function of adsorbing 226 Ra ions.
- the carrier (i) is preferably a carrier that can complex with metal ions under acidic or alkaline conditions and elute the metal ions under alkaline or acidic conditions opposite to the complexed conditions. ..
- Examples of the carrier (i) include a carrier capable of exchanging 226 Ra ions, and a carrier having a group capable of exchanging 226 Ra ions is preferable.
- Specific examples of the group capable of exchanging 226 Ra ions include a carrier having an iminodiacetic acid group, a polyamine group, and a methylglycan group, and an iminodiacetic acid group is preferable.
- the carrier having a group capable of exchanging 226 Ra ions is not particularly limited as long as a solid phase carrier such as a resin holds a group capable of exchanging 226 Ra ions.
- a preferred example of a carrier having a group capable of exchanging Ra ions is a styrenedivinylbenzene copolymer having an iminodiacetic acid group.
- examples of commercially available resins having such iminodiacetic acid groups include Bio-Rad's "Chelex” series, Mitsubishi Chemical's "Diaion” series, Dow Chemical's "Amberlite” series, and the like. Specific examples thereof include “Chelex100” manufactured by Bio-Rad (particle size: 50 to 100 mesh, ionic type: Na type, Fe type).
- a carrier containing a compound represented by the following formula (B) can be mentioned.
- Examples of commercially available products of such carrier (i) include "Ln resin”, “Ln2 resin” and “Ln3 resin” manufactured by Eichrom Technologies.
- R 5 and R 6 are independently -R'or -OR'(R'is an alkyl group having 8 carbon atoms).
- the alkyl group having 8 carbon atoms in the R' may be linear or may have a branch, and preferred examples thereof include an octyl group, a 2-ethylhexyl group, and 2-methyl-4,4-. Examples include the dimethylpentyl group.
- Preferable examples of the compound represented by the formula (B) include compounds represented by the following formulas (B-1) to (B-3).
- a carrier containing 1-octanol containing a compound represented by the following formula (III) can be mentioned. Specifically, 1-octanol containing 4,4'-bis (t-butylcyclohexano) -18-crown-6 or 4,5'-bis (t-butylcyclohexano) -18-crown-6. Is a carrier containing 1-octanol containing. Examples of commercially available products of such a carrier (i) include "Sr resin" manufactured by Eichrom Technologies.
- the amount of the carrier (i) used is not particularly limited and may be determined according to the amount of the solid 226 Ra-containing substance.
- the solid 226 Ra-containing substance is a radium radiation source, for example, if the radium radiation source is 10 mg or less, about 1 mL of the carrier (i) can be used.
- the carrier (i) is preferably used by filling it in a bag or a pack.
- the bag or pack is not particularly limited as long as it can be filled with the carrier (i) and does not adsorb 226 Ra, but is preferably a mesh-shaped bag or pack made of ⁇ -olefin such as polyethylene or polypropylene. More preferably, it is a mesh-shaped bag made of at least one selected from polyethylene and polypropylene.
- the shape and size of the bag or pack are not particularly limited, but are preferably a 2 cm square bag, and more preferably a 2 cm square tetrahedron.
- the treatment liquid is a water-based liquid used for immersing the solid 226 Ra-containing substance and the carrier (i).
- the content of water in the treatment liquid is not particularly limited, but it is preferable that the content is larger because the solvent in which the 226 Ra ions are dissolved increases and the ultrasonic wave is less attenuated.
- the treatment liquid may contain a liquid other than water. Examples of liquids other than water include ethanol, methanol, glycerin and the like. Moreover, you may add a preservative or the like to these solutions.
- the treatment liquid may contain liquid slag. When the treatment liquid contains liquid slag, 226 Ra is recovered not only from the solid slag but also from the liquid slag, and as a result, the amount of 226 Ra recovered is increased, which is preferable.
- the pH of the treatment liquid is not particularly limited.
- the treatment liquid when the step (A1) is performed under alkaline conditions, the treatment liquid is preferably an alkaline aqueous solution, the pH is preferably 8 or more, and more preferably 9 or more.
- the pH is preferably adjusted using at least one selected from the group consisting of ammonia, alkali metal hydroxides or carbonates, and alkaline buffers. As a result, 226 Ra can be adsorbed on the carrier (i).
- the treatment liquid preferably does not contain alkaline earth metals. Since the alkaline earth metal is easily adsorbed on the carrier (i), if the treatment liquid does not contain the alkaline earth metal, it is easy to avoid recovering the alkaline earth metal together with 226 Ra.
- the amount of the treatment liquid is not particularly limited, but at least the amount in which the entire carrier (i) can be completely immersed in the treatment liquid is preferable.
- the carrier (i) is filled in a bag or pack, an amount that allows the entire bag or pack to be completely immersed in the treatment liquid is preferable.
- the frequency of the ultrasonic wave to be irradiated is not particularly limited as long as it is 16 kHz or more, but is preferably 16 to 120 kHz, more preferably 19 to 100 kHz, and further preferably 20 to 80 kHz.
- the frequency of the ultrasonic wave is within the above range, 226 Ra can be efficiently extracted from the solid 226 Ra-containing substance, and 226 Ra can be efficiently adsorbed on the carrier (i).
- the ultrasonic wave generator is not particularly limited, and for example, a water tank type ultrasonic cleaner, an ultrasonic crusher (also referred to as an ultrasonic disperser or an ultrasonic homogenizer) or the like can be used.
- a water tank type ultrasonic cleaner is preferable because it can irradiate ultrasonic waves without radioactively contaminating the ultrasonic generator.
- the output of the ultrasonic generator is not particularly limited, but is preferably 10 to 800 W, more preferably 20 to 600 W, and even more preferably 30 to 400 W.
- the ultrasonic wave generator may be provided with a constant temperature bath in order to suppress the temperature rise of the ultrasonic wave generator and the treatment liquid due to the irradiation of ultrasonic waves.
- the temperature of the constant temperature bath is, for example, 10 to 25 ° C.
- Ultrasound irradiation can be performed once or multiple times at appropriate intervals, eg, once or twice to five times a day, preferably once to three times a day, or two days or more. Once or twice to five times per three days, preferably once to three times per two or three days. This is done, for example, for 1 to 60 days, preferably 2 to 30 days.
- 226 Ra can be efficiently taken out from the solid 226 Ra-containing substance and adsorbed on the carrier (i).
- the ultrasonic irradiation time per irradiation is, for example, 10 seconds to 1 hour, preferably 1 minute to 45 minutes, and more preferably 15 minutes to 45 minutes.
- the total irradiation time of the ultrasonic wave is, for example, 0.1 hour or more, preferably 0.5 to 50 hours, more preferably 0.5 to 20 hours, still more preferably 0.5 to 10 hours.
- 226 Ra can be efficiently taken out from the solid 226 Ra-containing substance and adsorbed on the carrier (i).
- the carrier (i) is separated from the treatment liquid (A2), and the carrier (i) separated in the step (A2) is subjected to 226 Ra using an acid. It is preferable to include the elution step (A3).
- the carrier (i) on which 226 Ra is adsorbed in the step (A1) is separated from the treatment liquid.
- the method of separation is not particularly limited, and for example, by filtering with a membrane filter or the like, the carrier (i) on which 226 Ra is adsorbed can be collected on the filter and separated from the treatment liquid.
- the carrier (i) can be separated from the treatment liquid by lifting the bag or pack filled with the carrier (i) with tweezers or the like. ..
- 226 Ra is eluted from the carrier (i) on which 226 Ra is adsorbed using an acid.
- the 226 Ra adsorbed on the carrier (i) can be eluted by passing an acid through the carrier (i) or immersing the carrier (i) in the acid.
- the acid is not particularly limited as long as it can dissolve 226 Ra adsorbed on the carrier (i) to form an ion, but is preferably at least one selected from the group consisting of hydrochloric acid and nitric acid.
- the acid concentration is preferably 0.01 to 10 mol / L, more preferably 0.1, because 226 Ra can be efficiently eluted from the carrier and acid-derived anions can be efficiently removed in a later step. It is ⁇ 5 mol / L, more preferably 0.3 ⁇ 2 mol / L.
- the step (A2) and the step (A3) are performed after the step (A1) is repeated a plurality of times.
- 226 Ra can be efficiently recovered.
- the number of repetitions of the step (A1) is not particularly limited, but the step (A2) and the step (A3) are preferably performed after the step (A1) is performed 2 to 10 times, and the step (A1) is performed 3 to 5 times. It is more preferable to do it afterwards.
- Step (A4) Step of filtering the eluate obtained in step (A3)
- Step (A5) Step of adjusting the pH of the filtrate obtained in step (A4) and then performing filter filtration.
- the eluate containing 226 Ra obtained in the step (A3) can be filtered to remove the substance that precipitates under acidic conditions.
- Filter The filter used for filtration is not particularly limited, and examples of the material include fluorocarbon-based, cellulose-based, nylon-based, polyester-based, and hydrocarbon-based.
- the pore size of the filter can be appropriately selected according to the target cleanliness, but is preferably 1 ⁇ m or less, more preferably 0.5 ⁇ m or less.
- the filtration method may be such that the solution is passed only once, but it is more preferable to perform filtration multiple times.
- step (A5) after adjusting the pH of the filtrate containing 226 Ra obtained in the step (A4), the substance that precipitates under the pH condition different from that of the step (A3) is removed by performing filter filtration. be able to.
- Filter The filter used for filtration can be appropriately selected based on the same criteria as in step (A4).
- step (A5) it is preferable to adjust the pH of the filtrate to alkaline conditions using ammonia. This makes it possible to remove substances that precipitate under alkaline conditions.
- the steps (A1) to (A5) are repeated a plurality of times. As a result, 226 Ra can be efficiently recovered.
- the number of repetitions is not particularly limited, but the steps (A1) to (A5) are preferably performed 2 to 10 times, and more preferably 3 to 5 times.
- the recovery method (X) may include a step of washing the carrier (i) between the steps (A2) to (A5). Specifically, water may be passed through the carrier (i). By doing so, the proportion of impurities contained in the recovered solution containing 226 Ra can be reduced, and the recovery rate of 226 Ra can be increased.
- production method (Y) In the method for producing a 226 Ra solution (hereinafter, also referred to as “production method (Y)”), which is one aspect of the present invention, a solid 226 Ra-containing substance and a carrier (i) are immersed in a treatment liquid. After that, an acid is used from the step (A1) of irradiating the treatment liquid with ultrasonic waves, the step (A2) of separating the carrier (i) from the treatment liquid, and the carrier (i) separated in the step (A2). The step (A3) of leaching 226 Ra is included.
- the 226 Ra solution produced by the production method (Y) is referred to as a 226 Ra solution ( ⁇ ). Since the 226 Ra solution ( ⁇ ) contains 226 Ra in high purity, it can be used for various purposes, but it is preferably used for producing a 226 Ra target.
- Step (A4) A step of filtering the eluate obtained in the step (A3)
- Step (A5) A step of adjusting the pH of the filtrate obtained in the step (A4) and then filtering the eluate.
- the steps (A1) to (A5) in Y) can be performed in the same manner as the steps (A1) to (A5) of the manufacturing method (X) described above.
- the method for producing a 225 Ac solution includes a step (B1) of obtaining a 226 Ra solution ( ⁇ ) by the production method (Y) and a step of producing a 225 Ac solution from the 226 Ra solution ( ⁇ ) (. B2) and is included.
- the production method (Y) is performed to obtain a 226 Ra solution ( ⁇ ).
- a 225 Ac solution is produced from the 226 Ra solution ( ⁇ ).
- the method for producing the 225 Ac solution is not particularly limited, and examples thereof include the following methods.
- An electrodeposition solution is prepared using the 226 Ra solution ( ⁇ ), and the 226 Ra is electrodeposited on the substrate using the electrodeposition solution to produce a 226 Ra target.
- the 226 Ra target is irradiated with at least one selected from charged particles, photons and neutrons using an accelerator to generate 225 Ac by a nuclear reaction.
- the irradiated 226 Ra target is dissolved in an acidic solution to give a 225 Ac solution containing 225 Ac ions.
- the treatment solution in the step (B1) does not contain an alkali metal salt.
- a solid 226 Ra-containing substance and a carrier having a function of adsorbing 226 Ra ions are immersed in a treatment liquid, and then the treatment liquid is irradiated with ultrasonic waves (A1) .
- Ra recovery method [2] The method for recovering 226 Ra according to [1], wherein the solid 226 Ra-containing substance is at least one selected from the group consisting of uranium ore and a radium radiation source. [3] The method for recovering 226 Ra according to [1] or [2], wherein the carrier is capable of exchanging 226 Ra ions.
- the present invention includes a step (A2) of separating the carrier from the treatment liquid and a step (A3) of eluting 226 Ra from the carrier separated in the step (A2) using an acid. ] To [4]. The method for collecting 226 Ra according to any one of [4]. [6] The method for recovering 226 Ra according to [5], wherein the acid is at least one selected from the group consisting of hydrochloric acid and nitric acid.
- Method for producing Ra solution [8]
- a 225 Ac solution comprising a step of obtaining a 226 Ra solution (B1) by the method for producing a 226 Ra solution according to [7] and a step of producing a 225 Ac solution from the 226 Ra solution (B2). Production method.
- Example 1 All of the following work was done in the glove box.
- a radium radiation source (diameter 3 mm, length 20 mm) whose chemical form of the contained radium is unknown was cut with nippers into 5 to 6 small pieces.
- Celex-100 resin (Bio-Rad, particle size: 50-100 mesh, ionic type: Na type, usage amount: 1 mL) converted to NH 4 + type is converted into a bag (polyethylene, polypropylene mesh, shape). : 2 cm square tetrahedron) and closed.
- a bag containing Chelex-100 resin and a small piece of radium radiation source were placed in a 100 mL glass bottle, and then 0.5 mL of 14% ammonia water (manufactured by Nacalai Tesque Co., Ltd.) was added to adjust the pH to 10.
- the bottle was placed in a treatment tank (water bathtub) of a water tank type ultrasonic generator (US-610, output 110 W, frequency 44 kHz) manufactured by SND Co., Ltd., and irradiated with ultrasonic waves for 30 minutes. Ultrasound irradiation was repeated multiple times once every 2 to 3 days. The bottle after ultrasonic irradiation was allowed to stand at room temperature until the next ultrasonic irradiation.
- the bag containing the Chelex-100 resin was removed with tweezers and placed in a glass bottle containing 15 mL of 0.7 M nitric acid (first bottle). A few days later, a bag of Chelex-100 resin was removed from a glass bottle containing 15 mL of 0.7 M nitric acid with tweezers and placed in another glass bottle containing 15 mL of 0.7 M nitric acid (second bottle). ). A few days later, a bag of Chelex-100 resin was removed with tweezers from a second glass bottle containing 0.7 M nitric acid (15 mL). The eluates from the first bottle and the second bottle were combined to form a 226 Ra-containing solution (a-1). The pH was 0-2.
- the acidic precipitate was removed by filtering the 226 Ra-containing solution (a-1) with a membrane filter (ML Filter, manufactured by NMP, pore diameter 0.2 ⁇ m). This filtrate was used as a 226 Ra-containing solution (a-2).
- a-2 To the Ra-containing solution (a-2), add 14% aqueous ammonia (prepared by diluting aqueous ammonia (Nakalitesk Co., Ltd., 02512-95)) until it becomes alkaline (pH 9-11), and then a membrane filter.
- the basic precipitate was removed by filtration with. This filtrate was used as a 226 Ra-containing solution (a-3).
- a medical tube (manufactured by Hakkou Co., Ltd., 3.2 x 4.) having an inner diameter of 3.2 mm, an outer diameter of 4.4 mm, and a length of 50 cm obtained by converting Chelex 100 (usage amount: 3 mL) into NH 4 + type. It was filled in 4 ⁇ 500 mm (4 mL)).
- the anion exchange resin (Monosphere 550A) (manufactured by Fuji Film Wako Chemical Co., Ltd., particle size: 590 ⁇ 50 ⁇ m mesh, ion type: OH type, usage amount: 16 mL) was washed with water, and then the inner diameter was 3.2 mm.
- a medical tube having an outer diameter of 4.4 mm and a length of 50 cm (manufactured by Hakkou Co., Ltd., 3.2 ⁇ 4.4 ⁇ 500 mm (4 mL)) was filled, and the tube was connected next to the tube filled with Chelex 100.
- the 226 Ra-containing solution (a-3) was passed through Chelex 100 and an anion exchange resin. This passing liquid was used as waste liquid.
- 10 mL of 1 mol / L nitric acid and then 10 mL of water were passed through Chelex 100 and an anion exchange resin at a flow rate of 1 to 2 mL / min, and 20 mL of the eluted solution was used as a purified 226 Ra-containing solution (a-4).
- the radium radiation source small pieces treated once in the above step were subjected to re-extraction according to the following procedure.
- a bag containing Chelex-100 resin was added to a 100 mL glass bottle containing a small piece of radium radiation source, and ultrasonic irradiation was performed in the same manner as described above. Then, the bag containing Chelex-100 resin was taken out and placed in a glass bottle containing 15 mL of 0.7 M nitric acid (first bottle). A few days later, the bag containing Chelex-100 resin was removed from the first glass bottle containing 15 mL of 0.7 M nitric acid with tweezers and placed in another glass bottle containing 15 mL of 0.7 M nitric acid (2).
- the radioactivity of the purified 226 Ra-containing solution (a-4) was measured with a germanium semiconductor detector.
- Chelex-100 resin, radium radiation source small pieces, materials (membrane filter, anion exchange resin, plastic equipment, glass equipment), and waste liquid are also radiated with a germanium semiconductor detector to check the distribution amount of residual 226 Ra.
- the capacity was measured and the material balance of 226 Ra was calculated. The results are shown in Table 1. Since the same procedure was repeated 3 times, the measured radioactivity value is the total value for 3 times.
- Radioactivity of the radium radiation source before the start of the experiment was calculated from the following formula (1).
- Radium radiation source (calculated value) before the start of the experiment Purified 226 Ra-containing solution (a-4) + Residue in radium radiation source + Residue in Celex100 resin after elution + Residue in materials + Waste liquid ... (1) )
- the 226 Ra recovery rate (purified 226 Ra-containing solution (a-4) / radium radiation source before the start of the experiment ⁇ 100) was 99%.
- the 226 Ra loss rate (residual / purified 226 Ra-containing solution (a-4) ⁇ 100 in Celex100 resin after elution) was 1%.
- the contents of the radium radiation source that has been dug out are placed in a glass bottle, and 2 mL of 1.5 M sodium carbonate (manufactured by Nakaraitesk Co., Ltd., 3131-25, prepared by dissolving sodium carbonate in water) is added, and the temperature is 80 ° C. It was heated for 1 hour.
- the contents of the bottle were filtered with a membrane filter, and the filtrate was used as a waste liquid (b-1).
- the filter medium remaining on the filter was dissolved in 10 mL of 1 M hydrochloric acid (manufactured by Nacalai Tesque, Inc., 18429-15, prepared by diluting hydrochloric acid), but a part of the filter remained undissolved.
- This undissolved residue (which is considered to be radium sulfate) was used as a residue (b-2).
- the acid precipitate was removed by filtering the solution dissolved in 1M hydrochloric acid with a membrane filter. 14% aqueous ammonia (Nakalitesk Co., Ltd., 02512-95, prepared by diluting aqueous ammonia) is added to this filtrate until it becomes alkaline (pH 9-11), and then filtered through a membrane filter to remove the basic precipitate. A solution containing 226 Ra was obtained.
- a medical tube manufactured by Hakkou Co., Ltd., 3.2 x 4. having an inner diameter of 3.2 mm, an outer diameter of 4.4 mm, and a length of 50 cm obtained by converting Chelex 100 (usage amount: 3 mL) into NH 4 + type. It was filled in 4 ⁇ 500 mm (4 mL)).
- the anion exchange resin (Monosphere 550A) (manufactured by Fuji Film Wako Chemical Co., Ltd., particle size: 590 ⁇ 50 ⁇ m mesh, ion type: OH type, usage amount: 16 mL) was washed with water, and then the inner diameter was 3.2 mm.
- a medical tube having an outer diameter of 4.4 mm and a length of 50 cm (manufactured by Hakkou Co., Ltd., 3.2 ⁇ 4.4 ⁇ 500 mm (4 mL)) was filled, and the tube was connected next to the tube filled with Chelex 100. After removing the basic precipitate, the 226 Ra-containing solution was passed through Celex100 and an anion exchange resin.
- the radium source small pieces used once in the above step were subjected to re-extraction according to the following procedure.
- the radium source small pieces are placed in a glass bottle again, and the procedure from heating at 80 ° C. for 1 hour in 1.5 M sodium carbonate to obtaining a purified 226 Ra-containing solution (b-3) is carried out in the same manner as above. rice field.
- the re-extraction procedure was repeated 4 times.
- the radioactivity of the purified 226 Ra-containing solution (b-3) was measured with a germanium semiconductor detector.
- a germanium semiconductor detector was used to check the distribution amount of residual 226 Ra.
- the radioactivity was measured in 226 Ra and the material balance was calculated. The results are shown in Table 2. Since the same procedure was repeated 5 times, the measured radioactivity value is the total value for 5 times.
- Radioactivity of the radium radiation source before the start of the experiment was calculated from the following formula (2).
- Radium radiation source (calculated value) before the start of the experiment Residue in radium radiation source + Waste liquid (b-1) + Residue (b-2) + Purified 226 Ra-containing solution (b-3) + Residue in materials ... ⁇ (2)
- the 226 Ra recovery rate (purified 226 Ra-containing solution (b-3) / radium radiation source before the start of the experiment ⁇ 100) was 21%.
- the 226 Ra loss rate (waste liquid (b-1) + residue (b-2) / purified 226 Ra-containing solution (b-3) ⁇ 100) was 6%.
- Nippers (1/16'' stainless steel tube with old radium needles (diameter 1.6 mm, length 25 mm, including 37-74 MBq (1-2 mCi) as radioactivity of 226 Ra) of unknown chemical form of contained radium It was cut into small pieces of 5 to 6 pieces. The pieces were placed in a 50 mL glass bottle with a propylene screw cap (Duran Waiton Kimble). There, Chelex-100 resin (manufactured by Bio-Rad, particle size: 50 to 100 mesh, ionic type: Na type, usage amount: 3 mL) converted to NH 4 + type, 7 mL of water, and 28% ammonia water. Was added to adjust the pH to 10.
- the glass bottle was placed in a treatment tank (water bath) of a water tank type ultrasonic generator (US-350S manufactured by SND Co., Ltd., output 40 W, frequency 38 kHz) and irradiated with ultrasonic waves for 5 minutes. Ultrasound irradiation was performed about 1 to 3 times a day. A series of work of irradiating with ultrasonic waves and leaving it for several days was repeated for one week. The glass bottle after ultrasonic irradiation was allowed to stand at room temperature until the next ultrasonic irradiation. Empty cartridge (Bond Elut, 5mL, Agilent) inside the glass bottle It was placed on (manufactured by Technology) and the Celex-100 resin was filtered off. To this, 5 mL of 1 M hydrochloric acid and then 10 ml of purified water were added to elute 226 Ra. This eluate was used as a 226 Ra-containing solution (c-1). The pH was estimated to be 0-1.
- 226 Ra-containing solution (c-1) is passed through an anion exchange resin (Monosphere 550A) (manufactured by Fuji Film Wako Chemical Co., Ltd., particle size: 590 ⁇ 50 ⁇ m mesh, ion type: OH type, usage amount: 16 mL). Chloride ion was removed. Subsequently, 10 mL of purified water was passed to wash the anion exchange resin. This eluate was used as a purified 226 Ra-containing solution (c-1). The purified 226 Ra-containing solution (c-1) was concentrated at 130 ° C. under reduced pressure, and 226 Ra was recovered as dried hydroxide radium.
- an anion exchange resin Monosphere 550A
- the radioactivity of the purified 226 Ra-containing solution (c-1) was measured with a germanium semiconductor detector.
- a germanium semiconductor detector For Chelex-100 resin, radium needle pieces, and materials (cartridges, anion exchange resins, plastic instruments), radioactivity was measured with a germanium semiconductor detector to check the distribution of residual 226 Ra, and 226 Ra. The material balance of was calculated. The recovery rate of 226 Ra from the radium needle was about 30 to 50%.
- the filtered Chelex-100 resin was placed in a 50 mL glass bottle with a propylene screw cap, and 7 mL of water and ammonia water were added to adjust the pH. No. 10 was not irradiated with ultrasonic waves and was allowed to stand for one month. From the procedure of filtering out the Celex-100 resin using an empty cartridge, the procedure of obtaining dried hydroxide radium was carried out in the same manner as described above.
- the 226 Ra-containing solution obtained by re-extraction was designated as a purified 226 Ra-containing solution (c-2).
- the purified 226 Ra-containing solution (c-2) was combined with the purified 226 Ra-containing solution (c-1), and the radioactivity was measured with a germanium semiconductor detector. As a result, the recovery rate of 226 Ra from the radium needle was 100%.
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Abstract
Description
例えば、226Raの化学形が硫酸ラジウムであれば、炭酸ナトリウム水溶液中で加熱して炭酸ラジウムを生成させ、炭酸ラジウムをフィルターで濾過し、濾物を洗浄した後、酸で溶解して226Raを回収する。
226Raの化学形が炭酸ラジウムであれば、炭酸ラジウムをフィルターで濾過し、濾物を洗浄した後、酸で溶解させて226Raを回収する。
また、非特許文献1では、固体である硫酸ラジウムから226Raの単離を試み、その効率を評価している。
・ラジウム線源から226Raサンプルを採取する操作が困難かつ煩雑であるため、被曝の可能性が高かった。
・226Raの化学形の特定も難しく、適切な処理方法を選択できない場合があった。
・硫酸ラジウムから炭酸ラジウムへの変換効率は100%ではなく、また、硫酸ラジウム及び炭酸ラジウムは水にわずかに溶解するため、226Raの回収率が低かった。
・226Ra回収物に、塩又は使用した試薬が残存すると、226Raターゲット製造のために226Raを電着する際に電着率が低下する懸念があった。
数値範囲に関する「A~B」との記載は、特に断りがなければ、A以上B以下であることを意味する。また、%とは質量%を意味する。
本発明の一態様である226Raの回収方法(以下、「回収方法(X)」ともいう。)は、固体状の226Ra含有物質と、226Raイオンを吸着する機能を有する担体(以下「担体(i)」ともいう。)とを、処理液に浸漬させた後、該処理液に超音波を照射する工程(A1)を含む。
工程(A1)では、固体状の226Ra含有物質と、担体(i)とを、処理液に浸漬させた後、該処理液に超音波を照射する。
工程(A1)は、担体(i)が226Raイオンを吸着できれば、その条件は特に限定されないが、例えば、中性又はアルカリ条件下で行うことができ、アルカリ条件下で行うことが好ましい。アルカリ条件は、アンモニア、アルカリ金属の水酸化物、アルカリ金属の炭酸塩、及びアルカリ性緩衝液からなる群より選ばれる少なくとも1種を用いてpHを調整したアルカリ条件がより好ましい。これにより、226Ra含有物質に含まれる、アルカリ条件下で沈殿しやすい金属イオン(アルミニウム、亜鉛、鉄、鉛、銅、銀等)を沈殿させて、担体(i)に吸着されにくい状態にできる。また、226Raを担体(i)に効率的に吸着させることができる。工程(A1)は、アンモニアを用いてpHを調整したアルカリ条件下で行うことがさらに好ましい。これにより、アルカリ金属塩が以降の工程に残存しないので、回収した226Raを含む溶液を電着に用いる等、アルカリ金属塩の残存が悪影響を及ぼす可能性がある用途にも好適に用いることができ、回収した226Raを含む溶液の用途が広くなる。
固体状の226Ra含有物質は、226Raを含有する物質であって、25℃において固体状であれば、特に限定されない。固体状とは、226Ra含有物質を25℃において水平面に静置した場合に流動性を有さないことを意味する。
固体状の226Ra含有物質は、好ましくはウラン鉱滓及びラジウム線源からなる群から選ばれる少なくとも1種である。
ラジウム線源に含まれる226Raの化学形は特に制限されず、様々な化学形を用いることができる。ラジウム線源に含まれる226Raの化学形は、硫酸ラジウムであることが多く、稀に臭化ラジウムである。
ウラン鉱石の粗精錬は、例えば以下の工程で行う。
担体(i)は、226Raイオンを吸着する機能を有すれば、特に制限されない。担体(i)は、酸性条件下又はアルカリ条件下で金属イオンと錯形成し、錯形成した条件と反対のアルカリ条件下又は酸性条件下で金属イオンを溶離することができる担体であることが好ましい。担体(i)としては、例えば、226Raイオンを交換できる担体が挙げられ、好ましくは226Raイオンを交換できる基を有する担体である。226Raイオンを交換できる基としては、具体的には、イミノジ酢酸基、ポリアミン基、メチルグリカン基を有する担体が挙げられ、好ましくはイミノジ酢酸基である。226Raイオンを交換できる基を有する担体は、樹脂などの固相担体に226Raイオンを交換できる基が保持されていれば特に限定されない。226Raイオンを交換できる基を有する担体の好ましい例として、イミノジ酢酸基を保持するスチレンジビニルベンゼン共重合体が挙げられる。このようなイミノジ酢酸基を有する樹脂の市販品としては、Bio-Rad社製「Chelex」シリーズ、三菱化学社製「ダイヤイオン」シリーズ、ダウケミカル社製「アンバーライト」シリーズ等が挙げられ、より具体的にはBio-Rad社製「Chelex100」(粒径:50~100mesh、イオン型:Na型、Fe型)が挙げられる。
袋又はパックを用いることで、担体(i)を処理液から分離する工程(A2)を容易に行うことができる。また、担体(i)から226Raを溶離させた後、担体(i)を袋又はパックに充填させたまま、その他の器具及び機器等を放射能汚染させることなく、簡便に廃棄することができる。
処理液は、固体状の226Ra含有物質と、担体(i)とを浸漬するために用いる、水を溶媒とする液体である。
処理液中の水の含有量は、特に限定されないが、226Raイオンが溶解する溶媒が増え、また、超音波の減衰が少ないため、多いほど好ましい。
処理液は、水以外の液体を含んでもよい。水以外の液体としては、例えば、エタノール、メタノール、グリセリン等があげられる。また、これらの溶液に、防腐剤等を添加しても良い。
処理液は、液体状の鉱滓を含んでもよい。処理液が液体状の鉱滓を含むと、固体状の鉱滓からだけでなく、液体状の鉱滓からも226Raが回収されるので、結果として回収される226Raの量が増えるため、好ましい。
照射する超音波の周波数は、16kHz以上であれば、特に制限されないが、好ましくは16~120kHz、より好ましくは19~100kHz、さらに好ましくは20~80kHzである。超音波の周波数が上記範囲内にあると、固体状の226Ra含有物質から226Raを効率的に取り出し、226Raを担体(i)に効率的に吸着させることができる。
超音波発生装置は、超音波の照射に伴う超音波発生装置及び処理液の温度上昇を抑えるために、恒温槽を備えていてもよい。恒温槽の温度は、例えば、10~25℃である。
工程(A2)では、工程(A1)において226Raを吸着させた担体(i)を処理液から分離する。
分離する方法は特に制限されず、例えばメンブレンフィルター等で濾過することで、226Raを吸着させた担体(i)をフィルター上に捕集し、処理液から分離することができる。担体(i)が袋又はパックに充填されている場合は、担体(i)が充填された袋又はパックをピンセット等を用いて持ち上げることにより、担体(i)を処理液から分離することができる。
工程(A3)では、226Raを吸着させた担体(i)から酸を用いて226Raを溶離させる。具体的には、例えば、担体(i)に酸を通液、又は担体(i)を酸に浸漬することで、担体(i)に吸着させた226Raを溶離することができる。
226Raを担体から効率的に溶離できる点、後の工程で酸由来の陰イオンを効率的に除去できる点から、酸の濃度は好ましくは0.01~10mol/L、より好ましくは0.1~5mol/L、さらに好ましくは0.3~2mol/Lである。
工程(A1)の繰り返し回数は特に制限されないが、工程(A2)及び工程(A3)は工程(A1)を2~10回行った後に行うことが好ましく、工程(A1)を3~5回行った後に行うことがより好ましい。
工程(A4):工程(A3)で得られた溶出液を、フィルター濾過する工程
工程(A5):工程(A4)で得られた濾液のpHを調節した後に、フィルター濾過を行う工程
工程(A4)では、工程(A3)で得られた226Raを含む溶出液を、フィルター濾過することで、酸性条件下で沈殿する物質を除去することができる。
フィルター濾過に用いるフィルターは特に制限されないが、材質としては、例えば、フルオロカーボン系、セルロース系、ナイロン系、ポリエステル系、炭化水素系等が挙げられる。フィルターの孔径は、目標とする清浄度に合わせて適宜選択できるが、好ましくは1μm以下であり、より好ましくは0.5μm以下である。濾過方法は、溶液を1回のみ通過されるだけでもよいが、複数回濾過を行うことがより好ましい。
工程(A5)では、工程(A4)で得られた226Raを含む濾液のpHを調整した後に、フィルター濾過を行うことで、工程(A3)とは異なるpH条件下で沈殿する物質を除去することができる。フィルター濾過に用いるフィルターは工程(A4)と同様の基準で適宜選択できる。
工程(A5)では、アンモニアを用いて濾液のpHをアルカリ条件に調節することが好ましい。これにより、アルカリ条件下で沈殿する物質を除去することができる。
回収方法(X)において、工程(A2)~工程(A5)の各工程間に担体(i)を洗浄する工程を含んでいてもよい。具体的には、担体(i)に水を通液することが挙げられる。そうすることで、回収された226Raを含む溶液に含まれる不純物の割合を低減し、また、226Raの回収率を上げることができる。
本発明の一態様である226Ra溶液の製造方法(以下、「製造方法(Y)」ともいう。)は、固体状の226Ra含有物質と、担体(i)とを、処理液に浸漬させた後、該処理液に超音波を照射する工程(A1)、担体(i)を該処理液から分離する工程(A2)、及び工程(A2)で分離された担体(i)から酸を用いて226Raを溶離させる工程(A3)を含む。製造方法(Y)により製造される226Ra溶液を、226Ra溶液(α)と称する。
226Ra溶液(α)は、高純度で226Raを含むので、様々な用途に用いることができるが、226Raターゲットの製造に用いることが好ましい。
工程(A4):工程(A3)で得られた溶出液を、フィルター濾過する工程
工程(A5):工程(A4)で得られた濾液のpHを調節した後に、フィルター濾過を行う工程
製造方法(Y)における工程(A1)~工程(A5)は、上述した製造方法(X)の工程(A1)~工程(A5)と同様に行うことができる。
本発明の一態様である225Ac溶液の製造方法は、製造方法(Y)により226Ra溶液(α)を得る工程(B1)と、226Ra溶液(α)から225Ac溶液を製造する工程(B2)とを含む。
工程(B1)では、製造方法(Y)を行って、226Ra溶液(α)を得る。
工程(B2)では、226Ra溶液(α)から225Ac溶液を製造する。225Ac溶液を製造する方法は特に制限されないが、例えば以下の方法を挙げることができる。
226Ra溶液(α)を用いて電着液を調製する場合、工程(B1)の処理液は、アルカリ金属塩を含まないことが好ましい。
[1]固体状の226Ra含有物質と、226Raイオンを吸着する機能を有する担体とを、処理液に浸漬させた後、前記処理液に超音波を照射する工程(A1)を含む、226Raの回収方法。
[2]前記固体状の226Ra含有物質が、ウラン鉱滓及びラジウム線源からなる群から選ばれる少なくとも1種である、[1]に記載の226Raの回収方法。
[3]前記担体が、226Raイオンを交換できるものである、[1]又は[2]に記載の226Raの回収方法。
[4]前記担体が、イミノジ酢酸基を含む、[1]~[3]のいずれかに記載の226Raの回収方法。
[5]さらに、前記担体を前記処理液から分離する工程(A2)と、前記工程(A2)で分離された前記担体から酸を用いて226Raを溶離させる工程(A3)を含む、[1]~[4]のいずれかに記載の226Raの回収方法。
[6]前記酸が、塩酸及び硝酸からなる群から選ばれる少なくとも1種である、[5]に記載の226Raの回収方法。
[7]固体状の226Ra含有物質と、226Raイオンを吸着する機能を有する担体とを、処理液に浸漬させた後、前記処理液に超音波を照射する工程(A1)、
前記担体を前記処理液から分離する工程(A2)、及び
前記工程(A2)で分離された前記担体から酸を用いて226Raを溶離させる工程(A3)
を含む、226Ra溶液の製造方法。
[8][7]に記載の226Ra溶液の製造方法により226Ra溶液を得る工程(B1)と、前記226Ra溶液から225Ac溶液を製造する工程(B2)とを含む、225Ac溶液の製造方法。
[9]前記工程(A1)を複数回繰り返した後に、前記工程(A2)及び前記工程(A3)を行う、[5]又は[6]に記載の226Raの回収方法。
[10]前記工程(A3)を行った後に、下記工程(A4)及び工程(A5)を行う、[5]、[6]及び[9]のいずれかに記載の226Raの回収方法。
工程(A4):前記工程(A3)で得られた溶出液を、フィルター濾過する工程
工程(A5):前記工程(A4)で得られた濾液のpHを調節した後に、フィルター濾過を行う工程
[11]前記工程(A5)において、アンモニアを用いて濾液のpHをアルカリ条件に調節する、[10]に記載の226Raの回収方法。
以下の作業は全てグローブボックス内で行った。含まれるラジウムの化学形が不明であるラジウム線源(直径3mm、長さ20mm)をニッパーで切断し、5~6の小片にした。Chelex-100樹脂(Bio-Rad社製、粒径:50~100mesh、イオン型:Na型、使用量:1mL)をNH4 +型に変換したものを、袋(ポリエチレン、ポリプロピレン製メッシュ状、形状:2cm四方の四面体)に入れて、閉じた。100mLガラス製ボトルに、Chelex-100樹脂の入った袋及びラジウム線源小片を入れた後、14%アンモニア水(ナカライテスク株式会社製)0.5mLを添加してpH10にした。そのボトルを、水槽型超音波発生器(株式会社エスエヌディ社製、US-610、出力110W、周波数44kHz)の処理槽(水浴槽)に入れ、30分間超音波を照射した。超音波照射は、2~3日に1回、複数回繰り返した。超音波照射後のボトルは、次の超音波照射まで室温に静置した。Chelex-100樹脂の入った袋をピンセットで取り出し、0.7M硝酸15mLの入ったガラス製ボトルに入れた(1つ目のボトル)。数日後、0.7M硝酸15mLの入ったガラス製ボトルからChelex-100樹脂の入った袋をピンセットで取り出し、0.7M硝酸15mLの入った別のガラス製ボトルに入れた(2つ目のボトル)。数日後、2つ目の0.7M硝酸15mLの入ったガラス製ボトルからChelex-100樹脂の入った袋をピンセットで取り出した。1つ目のボトルと2つ目のボトルの溶出液を合わせて、226Ra含有溶液(a-1)とした。pHは0~2であった。
次に、陰イオン交換樹脂(モノスフィア550A)(富士フィルムワコーケミカル社製、粒径:590±50μm mesh、イオン型:OH形、使用量:16mL)を、水で洗浄後、内径3.2mm、外径4.4mm、長さ50cmの医療用チューブ(株式会社八光社製、3.2×4.4×500mm(4mL))に充填し、Chelex100を充填したチューブの次に接続した。226Ra含有溶液(a-3)をChelex100及び陰イオン交換樹脂に通液させた。この通過液を廃液とした。その後、1mol/Lの硝酸10mL、次いで水10mLをChelex100及び陰イオン交換樹脂に流速1~2mL/minで通液させ、溶出した液20mLを精製226Ra含有溶液(a-4)とした。
実験開始前のラジウム線源(計算値)=精製226Ra含有溶液(a-4)+ラジウム線源への残留+溶離後のChelex100樹脂への残留+資材への残留+廃液・・・(1)
以下の作業は全てグローブボックス内で行った。含まれるラジウムの化学形が不明であるラジウム線源(直径3mm、長さ20mm)をニッパーで切断し、5~6の小片にした。針を用いて、ラジウム線源小片から、中身を穿り出した。古いラジウム線源には、硫酸ラジウムが使われていることが多いことから、含まれるラジウムの化学形は、硫酸ラジウムであると予測した。そこで、炭酸ナトリウム水溶液中で加熱することにより、ラジウムを回収することにした。
実験開始前のラジウム線源(計算値)=ラジウム線源への残留+廃液(b-1)+残渣(b-2)+精製226Ra含有溶液(b-3)+資材への残留
・・・(2)
含まれるラジウムの化学形が不明である古いラジウム針(直径1.6mm、長さ25mm、226Raの放射能として37~74MBq(1~2mCi)を含む)をニッパー(1/16''ステンレスチューブ用)で切断し、5~6の小片にした。この小片をプロピレン製スクリューキャップ付きの50mLガラスボトル(Duran Wheaton Kimble社製)に入れた。そこに、Chelex-100樹脂(Bio-Rad社製、粒径:50~100mesh、イオン型:Na型、使用量:3mL)をNH4 +型に変換したもの、水7mL、及び28%アンモニア水を添加し、pHを10とした。そのガラスボトルを、水槽型超音波発生器(株式会社エスエヌディ社製、US-350S、出力40W、周波数38kHz)の処理槽(水浴槽)に入れ、5分間超音波を照射した。超音波照射は、一日1~3回程度行った。超音波照射して数日放置するという一連の作業を、1週間繰り返した。超音波照射後のガラスボトルは、次の超音波照射まで室温に静置した。ガラスボトルの中身を空のカートリッジ(Bond Elut、5mL、Agilent
Technologies社製)にのせ、Chelex-100樹脂を濾別した。そこに、1M塩酸5mL、続いて精製水10mlを添加して、226Raを溶出させた。この溶出液を226Ra含有溶液(c-1)とした。pHは0~1であると推定された。
Claims (8)
- 固体状の226Ra含有物質と、226Raイオンを吸着する機能を有する担体とを、処理液に浸漬させた後、前記処理液に超音波を照射する工程(A1)を含む、226Raの回収方法。
- 前記固体状の226Ra含有物質が、ウラン鉱滓及びラジウム線源からなる群から選ばれる少なくとも1種である、請求項1に記載の226Raの回収方法。
- 前記担体が、226Raイオンを交換できるものである、請求項1又は2に記載の226Raの回収方法。
- 前記担体が、イミノジ酢酸基を含む、請求項1~3のいずれか一項に記載の226Raの回収方法。
- さらに、前記担体を前記処理液から分離する工程(A2)と、前記工程(A2)で分離された前記担体から酸を用いて226Raを溶離させる工程(A3)を含む、請求項1~4のいずれか一項に記載の226Raの回収方法。
- 前記酸が、塩酸及び硝酸からなる群から選ばれる少なくとも1種である、請求項5に記載の226Raの回収方法。
- 固体状の226Ra含有物質と、226Raイオンを吸着する機能を有する担体とを、処理液に浸漬させた後、前記処理液に超音波を照射する工程(A1)、
前記担体を前記処理液から分離する工程(A2)、及び
前記工程(A2)で分離された前記担体から酸を用いて226Raを溶離させる工程(A3)
を含む、226Ra溶液の製造方法。 - 請求項7に記載の226Ra溶液の製造方法により226Ra溶液を得る工程(B1)と、前記226Ra溶液から225Ac溶液を製造する工程(B2)とを含む、225Ac溶液の製造方法。
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AU2021418250A AU2021418250A1 (en) | 2021-01-08 | 2021-12-27 | RECOVERY METHOD OF Ra-226, PRODUCTION METHOD OF Ra-226 SOLUTION, AND PRODUCTION METHOD OF Ac-225 SOLUTION |
US18/260,515 US20240084419A1 (en) | 2021-01-08 | 2021-12-27 | RECOVERY METHOD OF Ra-226, PRODUCTION METHOD OF Ra-226 SOLUTION, AND PRODUCTION METHOD OF Ac-225 SOLUTION |
CA3207653A CA3207653A1 (en) | 2021-01-08 | 2021-12-27 | Recovery method of ra-226, production method of ra-226 solution, and production method of ac-225 solution |
KR1020237022663A KR20230129419A (ko) | 2021-01-08 | 2021-12-27 | Ra-226의 회수 방법, Ra-226 용액의 제조 방법 및 Ac-225용액의 제조 방법 |
CN202180089085.3A CN116710581A (zh) | 2021-01-08 | 2021-12-27 | Ra-226的回收方法、Ra-226溶液的制造方法及Ac-225溶液的制造方法 |
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Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
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JP2000119765A (ja) * | 1998-10-09 | 2000-04-25 | Matsushita Electric Ind Co Ltd | リチウムの回収方法およびリチウムの回収装置 |
CN108396146A (zh) * | 2018-03-01 | 2018-08-14 | 常熟理工学院 | 稀土废渣中钍元素的吸附处理方法及装置 |
WO2021002275A1 (ja) * | 2019-07-02 | 2021-01-07 | 日本メジフィジックス株式会社 | 226Ra含有溶液の精製方法、226Raターゲットの製造方法および225Acの製造方法 |
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Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2000119765A (ja) * | 1998-10-09 | 2000-04-25 | Matsushita Electric Ind Co Ltd | リチウムの回収方法およびリチウムの回収装置 |
CN108396146A (zh) * | 2018-03-01 | 2018-08-14 | 常熟理工学院 | 稀土废渣中钍元素的吸附处理方法及装置 |
WO2021002275A1 (ja) * | 2019-07-02 | 2021-01-07 | 日本メジフィジックス株式会社 | 226Ra含有溶液の精製方法、226Raターゲットの製造方法および225Acの製造方法 |
Non-Patent Citations (1)
Title |
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JAN KOZEMPEL ET AL.: "Dissolution of [226Ra] BaSC as part of a method for recovery of Ra from aged Radium sources.", J. RADIOANAL. NUCL. CHEM., vol. 304, 2015, pages 337 - 342 |
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US20240084419A1 (en) | 2024-03-14 |
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