CN117095848B - 99Mo-99mTc color layer generator99mPreparation method of Tc isotope - Google Patents
99Mo-99mTc color layer generator99mPreparation method of Tc isotope Download PDFInfo
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- 238000000034 method Methods 0.000 title claims description 23
- 238000000926 separation method Methods 0.000 claims abstract description 79
- 230000000694 effects Effects 0.000 claims abstract description 49
- 239000007788 liquid Substances 0.000 claims abstract description 45
- WAKHLWOJMHVUJC-SQFISAMPSA-N (2z)-2-hydroxyimino-1,2-diphenylethanol Chemical compound C=1C=CC=CC=1C(=N/O)/C(O)C1=CC=CC=C1 WAKHLWOJMHVUJC-SQFISAMPSA-N 0.000 claims abstract description 27
- 238000002386 leaching Methods 0.000 claims abstract description 24
- 238000012856 packing Methods 0.000 claims abstract description 18
- 238000001179 sorption measurement Methods 0.000 claims abstract description 13
- 230000005855 radiation Effects 0.000 claims abstract description 12
- 230000002285 radioactive effect Effects 0.000 claims abstract description 11
- 239000003480 eluent Substances 0.000 claims abstract description 10
- 230000004224 protection Effects 0.000 claims abstract description 9
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 24
- 239000000243 solution Substances 0.000 claims description 19
- 239000002244 precipitate Substances 0.000 claims description 15
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 14
- 229910017604 nitric acid Inorganic materials 0.000 claims description 14
- 230000002378 acidificating effect Effects 0.000 claims description 12
- 239000002504 physiological saline solution Substances 0.000 claims description 12
- 239000000463 material Substances 0.000 claims description 7
- QXYJCZRRLLQGCR-UHFFFAOYSA-N molybdenum(IV) oxide Inorganic materials O=[Mo]=O QXYJCZRRLLQGCR-UHFFFAOYSA-N 0.000 claims description 7
- 239000013077 target material Substances 0.000 claims description 7
- 239000012670 alkaline solution Substances 0.000 claims description 6
- 239000012074 organic phase Substances 0.000 claims description 6
- 239000012527 feed solution Substances 0.000 claims description 5
- 238000011068 loading method Methods 0.000 claims description 5
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 claims description 2
- 238000002360 preparation method Methods 0.000 abstract description 17
- 239000002994 raw material Substances 0.000 abstract description 6
- 230000007547 defect Effects 0.000 abstract description 3
- 239000002901 radioactive waste Substances 0.000 abstract description 3
- 238000000605 extraction Methods 0.000 abstract description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 10
- 239000000741 silica gel Substances 0.000 description 9
- 229910002027 silica gel Inorganic materials 0.000 description 9
- 239000011521 glass Substances 0.000 description 6
- 238000010586 diagram Methods 0.000 description 4
- 238000010828 elution Methods 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- 229910015667 MoO4 Inorganic materials 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000003513 alkali Substances 0.000 description 3
- 230000004992 fission Effects 0.000 description 3
- 239000000499 gel Substances 0.000 description 3
- 229920001296 polysiloxane Polymers 0.000 description 3
- 239000013049 sediment Substances 0.000 description 3
- 239000011734 sodium Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
- 229910021641 deionized water Inorganic materials 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000003384 imaging method Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
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- 229910052750 molybdenum Inorganic materials 0.000 description 2
- 239000011733 molybdenum Substances 0.000 description 2
- 239000011824 nuclear material Substances 0.000 description 2
- 239000002699 waste material Substances 0.000 description 2
- WAKHLWOJMHVUJC-FYWRMAATSA-N (2e)-2-hydroxyimino-1,2-diphenylethanol Chemical compound C=1C=CC=CC=1C(=N/O)\C(O)C1=CC=CC=C1 WAKHLWOJMHVUJC-FYWRMAATSA-N 0.000 description 1
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 235000011114 ammonium hydroxide Nutrition 0.000 description 1
- 239000003957 anion exchange resin Substances 0.000 description 1
- WAKHLWOJMHVUJC-UHFFFAOYSA-N benzoin alpha-oxime Natural products C=1C=CC=CC=1C(=NO)C(O)C1=CC=CC=C1 WAKHLWOJMHVUJC-UHFFFAOYSA-N 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 238000004587 chromatography analysis Methods 0.000 description 1
- 239000000084 colloidal system Substances 0.000 description 1
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- 238000006731 degradation reaction Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000000706 filtrate Substances 0.000 description 1
- 230000004907 flux Effects 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 description 1
- 150000002484 inorganic compounds Chemical class 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- MEFBJEMVZONFCJ-UHFFFAOYSA-N molybdate Chemical compound [O-][Mo]([O-])(=O)=O MEFBJEMVZONFCJ-UHFFFAOYSA-N 0.000 description 1
- JKQOBWVOAYFWKG-UHFFFAOYSA-N molybdenum trioxide Inorganic materials O=[Mo](=O)=O JKQOBWVOAYFWKG-UHFFFAOYSA-N 0.000 description 1
- 230000003472 neutralizing effect Effects 0.000 description 1
- 125000003544 oxime group Chemical group 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 230000035515 penetration Effects 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000000941 radioactive substance Substances 0.000 description 1
- 239000000700 radioactive tracer Substances 0.000 description 1
- 230000001950 radioprotection Effects 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000002791 soaking Methods 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 238000004659 sterilization and disinfection Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000000967 suction filtration Methods 0.000 description 1
- 229910021512 zirconium (IV) hydroxide Inorganic materials 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/04—Treating liquids
- G21F9/06—Processing
- G21F9/12—Processing by absorption; by adsorption; by ion-exchange
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/007—Recovery of isotopes from radioactive waste, e.g. fission products
-
- 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
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- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Abstract
The invention provides a 99Mo-99m Tc color layer generator and a 99m Tc isotope preparation method, which can be applied to the preparation of medical radioactive isotope 99m Tc. The generator includes: the leaching unit is used for respectively conveying 99 Mo feed liquid and leaching liquid to the separation unit and leaching column packing in the separation unit; a separation unit for adsorbing 99Mo、99 Mo and separating daughter nuclide 99m Tc; a collection unit for collecting 99m Tc eluents; and the radiation protection unit is used for protecting the generator from radiation. The generator adopts alpha-benzoin oxime and Al 2O3 as column packing of the 99Mo-99m Tc generator together, and the adsorption quantity of 99 Mo is obviously increased, so that the preparation of the high-activity 99Mo-99m Tc generator by taking low-specific-activity 99 Mo feed liquid as a raw material is realized, the defects that the generator prepared by the low-specific-activity 99 Mo feed liquid at present has large volume, complex operation, more radioactive waste liquid and the like can be overcome, and the generator has the advantages of simplicity in operation, low cost and the like. The enriched 98 Mo or 100 Mo target may also be recovered by extraction after 99 Mo has sufficiently decayed.
Description
Technical Field
The invention relates to the field of radioisotope preparation, in particular to a preparation method for preparing a high-activity 99Mo-99m Tc color layer generator and a 99m Tc isotope by using 99 Mo with low specific activity.
Background
99m Tc is a very important medical isotope, and medical 99m Tc is currently all derived from 99Mo-99m Tc generators. Due to the influence of various factors, supply shortage of fissionable 99 Mo has occurred, and non-fissionable 99 Mo production technology has been actively advanced internationally in recent years.
The non-fissile 99 Mo preparation method with commercial application prospect mainly comprises the steps that reactor irradiation 98 Mo is produced through nuclear reaction 98Mo(n,γ)99 Mo, or accelerator irradiation 100 Mo is produced through 100Mo(p,pn)99 Mo and 100Mo(γ,n)99 Mo, and 99 Mo obtained by the methods is low in specific activity. High activity medical 99Mo-99m Tc color layer generators cannot be prepared with low specific activity 99 Mo.
Disclosure of Invention
In view of the above problems, the invention provides a preparation method for preparing a high-activity 99Mo-99m Tc color layer generator and a 99m Tc isotope by using low-specific-activity 99 Mo, which can solve the technical problem that the high-activity medical 99Mo-99m Tc generator cannot be prepared by using the low-specific-activity 99 Mo at present, and simultaneously, the cost is reduced by recycling the enriched target material.
According to a first aspect of the present invention there is provided a 99Mo-99m Tc colour layer generator comprising:
The liquid outlet end of the leaching unit is connected with the liquid inlet end of the separation unit and is used for respectively conveying leaching liquid and 99 Mo feed liquid to the separation unit and leaching column packing in the separation unit;
the separation unit comprises a column packing in the separation unit from a liquid inlet end to a liquid outlet end, wherein the liquid outlet end of the separation unit is connected with the liquid inlet end of the elution unit, and the separation unit is used for generating 99MoO2(α-BzO)2 sediment by reacting the alpha-benzoin oxime with 99 Mo, adsorbing 99 Mo by Al 2O3 and realizing separation of 99 Mo and 99m Tc;
The collecting unit is used for collecting 99m Tc eluent, and the eluent is liquid discharged after the column packing is leached.
The radiation protection unit is used for radiation protection of radionuclides 99 Mo and 99m Tc.
According to an embodiment of the disclosure, the 99 Mo feed liquid has a specific activity greater than 4×10 10 Bq/gMo.
According to embodiments of the present disclosure, the acidic alumina has a particle size of 100 to 200 mesh.
According to an embodiment of the present disclosure, a support is further provided below the acidic alumina, the support being for preventing the acidic alumina from falling off.
The second aspect of the invention provides a method for preparing a high activity 99m Tc isotope, comprising:
wet loading acidic alumina into a separation unit;
Tiling alpha-benzoin oxime onto the alumina in the separation unit;
Injecting a pre-formulated 99 Mo feed solution into the separation unit to soak the α -benzoin oxime to obtain a 99MoO2(α-BzO)2 precipitate;
eluting the column packing in the separation unit by using normal saline to obtain 99m Tc isotopes.
According to an embodiment of the present invention, after 99 Mo in the generator decays completely, it further includes:
Dissolving the non-radioactive MoO 2(α-BzO)2 precipitate into an alkaline solution;
Adding a polar organic phase to extract the alpha-benzoin oxime in the non-radioactive MoO 2(α-BzO)2 precipitate to the organic phase, and separating 98 Mo or 100 Mo target material.
According to an embodiment of the invention, before said tiling of α -benzoin oxime on said alumina in said separation unit, comprises:
A nitric acid solution is added to the separation unit to pre-equilibrate with the nitric acid solution.
According to an embodiment of the present invention, after loading 99 Mo into a separation unit, eluting column packing in the separation unit with physiological saline to obtain 99m Tc isotope, the method includes:
The 99 Mo remaining in the separation unit was rinsed with dilute nitric acid solution.
According to an embodiment of the present invention, before dissolving the MoO 2(α-BzO)2 precipitate into an alkaline solution, the method comprises:
The residual 99 Tc in the separation unit was rinsed with physiological saline, and the 99 Tc was decayed from the 99m Tc.
According to the embodiment of the invention, the specific activity of 99 Mo feed liquid is greater than 4 multiplied by 10 10 Bq/gMo.
According to the 99Mo-99m Tc color layer generator and the 99m Tc isotope preparation method provided by the invention, alpha-benzoin oxime and Al 2O3 are used as column packing of the 99Mo-99m Tc color layer generator together, so that the adsorption quantity of 99 Mo is obviously increased, and the preparation of the high-activity 99Mo-99m Tc color layer generator by taking low-specific-activity 99 Mo feed liquid as a raw material is realized. Meanwhile, based on the characteristic that MoO 2(α-BzO)2 precipitate is soluble in alkali liquor, expensive 98 Mo or 100 Mo target materials can be effectively recovered.
Drawings
The foregoing and other objects, features and advantages of the invention will be apparent from the following description of embodiments of the invention with reference to the accompanying drawings, in which:
FIG. 1 schematically illustrates a schematic diagram of a 99Mo-99m Tc color layer generator according to an embodiment of the invention;
Fig. 2 schematically shows a flow diagram of 99m Tc isotope production in accordance with an embodiment of the present invention.
Detailed Description
Hereinafter, embodiments of the present invention will be described with reference to the accompanying drawings. It should be understood that the description is only illustrative and is not intended to limit the scope of the invention. In the following detailed description, for purposes of explanation, numerous specific details are set forth in order to provide a thorough understanding of the embodiments of the invention. It may be evident, however, that one or more embodiments may be practiced without these specific details. In addition, in the following description, descriptions of well-known structures and techniques are omitted so as not to unnecessarily obscure the concepts of the present disclosure.
The terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. The terms "comprises," "comprising," and/or the like, as used herein, specify the presence of stated features, steps, operations, and/or components, but do not preclude the presence or addition of one or more other features, steps, operations, or components.
All terms (including technical and scientific terms) used herein have the same meaning as commonly understood by one of ordinary skill in the art unless otherwise defined. It should be noted that the terms used herein should be construed to have meanings consistent with the context of the present specification and should not be construed in an idealized or overly formal manner.
The existing main commercial 99Mo-99m Tc chromatographic generator is prepared by taking high-specific activity fission 99 Mo as a raw material and aluminum oxide as an adsorption material. The generator is characterized in that a certain amount of acidic alumina is filled into a glass column, after disinfection, high specific activity (up to 10 14 Bq/g) is fissionally 99 Mo is loaded onto an alumina chromatographic column, and the generator can be conveniently eluted by physiological saline according to clinical needs by hospital staff, and 99m Tc generated by 99 Mo decay in the generator is eluted, so that the generator has the advantages of high 99m Tc concentration, high 99m Tc eluting efficiency, good 99m Tc imaging quality and the like. However, the production of fissile 99 Mo requires the use of nuclear material 235 U, is complex in preparation process, consumes large energy and generates a large amount of radioactive fissile waste, which is not friendly to the environment.
Still another medical 99Mo-99m Tc generator is gel type, and the specific preparation method is as follows: the method comprises the steps of placing a natural MoO 3 or enriched 98MoO3 target with pure spectrum in a reactor for irradiation to generate (n, gamma) reaction, obtaining a supported heap 99 Mo (with the specific activity of about 10 10 Bq/g), dissolving the supported heap 99 Mo in alkali liquor, neutralizing the supported heap with nitric acid, mixing the supported heap 99 Mo with hydrous zirconia to react to generate molybdate colloid, and carrying out suction filtration, drying, cracking and rinsing to prepare the gel 99Mo-99m Tc generator. As 99 Mo raw material contains a large amount of carrier Mo and has low specific activity, the generator has the defect of large column volume, and has low 99m Tc concentration in eluent, low 99m Tc leaching efficiency, wide leaching peak and poor 99m Tc imaging quality, thereby seriously affecting the clinical application.
In addition, in order to solve the problem of preparing a high-activity 99Mo-99m Tc color layer generator by using 99 Mo with low specific activity, the separation processes of ARSII, tcMM are developed successively based on the technology of activated carbon, anion exchange resin and alumina, and although the leaching efficiency of 99m Tc can reach 90%, the generator has the advantages of more use procedures, complex operation (difficult operation of non-professional hospital staff), large generator volume and more generated radioactive waste.
For a medical 99Mo-99m Tc color layer generator, 99Mo/99m Tc separated column material is a critical component. When the adsorption capacity of the generator adsorption material to Mo is low, only high specific activity 99 Mo (such as fission 99 Mo with specific activity of 10 14 Bq/g) can be used for preparing the high-activity generator (more than 37 GBq); for example, using a heap of 99 Mo with a specific activity of about 10 10 Bq/g, only low activity (less than 3.7 GBq) generators can be produced. Low activity generators are almost unusable for hospitals. When the adsorption capacity of the generator adsorption material to Mo is large, 99 Mo with high and low specific activities can be used for preparing the high-activity generator.
Fig. 1 schematically shows a schematic diagram of a 99Mo-99m Tc generator according to an embodiment of the invention.
As shown in fig. 1, the 99Mo-99m Tc generator includes a rinsing unit 10, a separating unit 20, and a collecting unit 30. The liquid outlet end of the leaching unit 10 is connected with the liquid inlet end of the separation unit 20, and the leaching unit 10 is used for respectively conveying leaching liquid and 99 Mo feed liquid to the separation unit 20 and leaching column packing in the separation unit 20. The column packing in the separation unit 20 comprises alpha-benzoin oxime and acidic alumina 22 in sequence from the liquid inlet end to the liquid outlet end, the liquid outlet end of the separation unit 30 is connected with the liquid inlet end of the elution unit 30, and the separation unit 20 is used for generating 99MoO2(α-BzO)2 a precipitate 21 and separating 99 Mo from daughter nuclide 99m Tc. The collection unit 30 is used to collect the eluate to obtain 99m Tc isotopes.
In one embodiment, the eluting unit 10, the separating unit 20 and the eluting unit 30 are all communicated through silica gel pipes.
In one embodiment, plugs for connecting silicone tubes are provided on both the liquid inlet and liquid outlet ends of the separation unit 20. The silica gel tube is used for connecting the leaching unit 10 and the separation unit 20, one end of the silica gel tube is connected with a plug at the liquid inlet end of the separation unit 20, the other end of the silica gel tube is connected with a double needle, the double needle is inserted into the leaching unit 10, and leaching liquid in the diversion leaching unit 10 flows into the separation unit 20 through the silica gel tube. The silica gel tube is used for connecting the separation unit 20 and the collection unit 30, one end of the silica gel tube is connected with the plug of the liquid outlet end of the separation unit 20, the other end of the silica gel tube is connected with a single needle, the single needle is inserted into the elution unit 30, and liquid in the diversion separation unit 20 flows into the collection unit 30 through the silica gel tube.
In one embodiment of the present invention, the separation unit 20 may be a glass bottle, which may be cylindrical or other shape, and for example, the glass bottle may have a height in the range of 5 to 10 cm and a diameter of about 1 em.
It should be noted that, the separation unit 20 and the collection unit 30 are respectively installed in the radiation protection unit 40 with a radioprotection function, and the radiation protection unit 40 includes a lead shielding body of the separation unit 20 and a lead tank outside a vacuum bottle containing 99m Tc eluted from the separation column, for radiation protection of radionuclides 99 Mo and 99m Tc. The radiation protection unit 40 may be made of lead material, or may be made of other materials having the same function, which is not limited in the present invention.
In an embodiment of the invention, a support 23 is also provided under the acidic alumina, which support 23 is used to prevent the acidic alumina and the benzoin oxime from falling off. Such as glass sand cores and the like.
Alumina (Al 2O3) is an inorganic compound, is an amorphous porous structural substance composed of hydrate, has good irradiation tolerance, can be used for separating high-activity radioactive substances, has good selectivity to 99 Mo, but has an adsorption capacity of only 20-40 mg Mo/g Al 2O3 to molybdenum, and is equivalent to fissile 99 Mo capable of adsorbing 2000-4000 GBq per gram of Al 2O3 and heap irradiation 99 Mo of 0.2-0.4 GBq. At an alumina level of 1 gram (limited by the size of the generator), high specific activity fissile 99 Mo must be used to produce a high activity generator.
In the embodiment of the invention, the specific activity of the 99 Mo feed liquid may be a low specific activity 99 Mo feed liquid. The low specific activity 99 Mo can be carrier 99Mo(99 Mo which is produced by a reactor or an accelerator irradiation molybdenum target through 98Mo(n,γ)99Mo、100Mo(p,pn)99 Mo, 100Mo(γ,n)99 Mo and other ways, and the specific activity of the carrier is lower than 10 11 Bq/g Mo.
Compared with 1g Al 2O3 for adsorbing 20-40 mg 99 Mo, the invention can be specifically and quantitatively combined with 99 Mo in an acidic environment to generate a precipitate 99MoO2(α-BzO)2 by adopting alpha-benzoin oxime (alpha-BzO), and 1g alpha-benzoin oxime can be combined with 210mg 99 Mo, so that the adsorption capacity of 99 Mo is obviously improved. And alpha-BzO does not adsorb 99 Mo daughter nuclide 99m Tc, so that the 99m Tc elution efficiency of the generator can be ensured. In addition, the radiation resistance of the alpha-BzO is good, when the accumulated radiation dose is lower than 550kGy, the alpha-BzO hardly undergoes radiolytic degradation, and when 99 Mo in each 99Mo-99m Tc generator is generally 37-185 GBq and 99 Mo decays for 10 half-lives, the absorption dose of the alpha-BzO is only 0.007-0.035 Gy.
The method utilizes the characteristic that 99 Mo can quantitatively coordinate with oxime groups, adopts alpha-BzO and Al 2O3 together as column packing of the 99Mo-99m Tc color layer generator, and remarkably increases the adsorption quantity of 99 Mo, thereby realizing the preparation of the high specific activity 99Mo-99m Tc color layer generator by taking low specific activity 99 Mo feed liquid as a raw material. Meanwhile, based on the characteristic that MoO 2(α-BzO)2 is soluble in alkali liquor, 98 Mo or 100 Mo target material can be effectively recovered.
Fig. 2 schematically shows a flow diagram of a method of preparing 99m Tc isotopes according to an embodiment of the present disclosure.
The preparation method of 99m Tc isotopes provided in this embodiment can be implemented using a 99Mo-99m Tc generator as shown in fig. 1.
As shown in FIG. 2, the preparation method of 99m Tc isotope is operated from S210 to S240.
In operation S210, acidic alumina is wet-charged into the separation unit.
In operation S220, alpha-benzoin oxime is tiled onto the alumina in the separation unit.
In operation S230, a pre-formulated 99 Mo feed solution is injected into the separation unit to soak the α -benzoin oxime, resulting in 99MoO2(α-BzO)2 precipitate.
In operation S240, the column packing in the separation unit is rinsed with physiological saline to obtain 99m Tc isotopes.
In one embodiment of the present invention, after leaching the separation unit with 0.9% physiological saline to obtain 99m Tc isotopes in operation S240, the method further includes: dissolving the non-radioactive MoO 2(α-BzO)2 precipitate into an alkaline solution; adding a polar organic phase to extract alpha-BzO in the non-radioactive MoO 2(α-BzO)2 precipitate into the organic phase, and separating 98 Mo or 100 Mo target materials. 98 Mo or 100 Mo target material is recovered from the used generator, so that the production cost is further saved, and the resource utilization rate is high.
In one embodiment of the invention, prior to tiling the α -benzoin oxime on the alumina in the separation unit in operation S220, comprising: a nitric acid solution is added to the separation unit to pre-equilibrate with the nitric acid solution.
In one embodiment of the present invention, before eluting the column packing in the separation unit with physiological saline to obtain 99m mTc isotopes in operation S240, the method comprises: the 99 Mo remaining in the separation unit was rinsed with dilute nitric acid solution.
In an embodiment of the present invention, before the foregoing dissolving the MoO 2(α-BzO)2 precipitate into the alkaline solution, the method includes: the residual 99 Tc in the separation unit was rinsed with physiological saline, and the 99 Tc was decayed from the 99m Tc.
Example 1
The target 98 Mo is obtained by theoretical calculation by using 98 Mo target to irradiate for 7 days under the condition of the neutron flux rate of 2X 10 14n/s·cm2 in a reactor, so that about 37GBq 99 Mo is generated, and the dosage of the target 98 Mo is 0.28g.
1. 1.0G of alumina for chromatography is taken, immersed overnight in a 1mol/L nitric acid solution, rinsed with deionized water to neutrality. Then 1mol/L ammonia water is used for soaking overnight, and deionized water is used for rinsing to neutrality. After loading the pretreated alumina into a glass column by a wet method, the column was pre-equilibrated with a 1mol/L nitric acid solution.
2. 1.4G of alpha-benzoin oxime was tiled on top of alumina in a glass column. Plugs connected with a silicone tube are arranged at two ends of the separation column, and the other end of the silicone tube is connected with a needle head. The separation column is encased in a lead shield.
3. 0.6G of Na 2MoO4 (containing 0.28g of Mo, which is equivalent to a carrier 99 Mo with an activity of 37GBq, and 99 Mo with a specific activity of 132GBq/g Mo in a generator) is weighed and dissolved in 40mL of 1mol/L nitric acid to prepare Na 2MoO4 solution, a certain volume of 99 Mo tracer solution is taken and added into the Na 2MoO4 solution, and the mixture is uniformly mixed. Loading the mixed solution on a separation column, and reacting for 5min to generate 99MoO2(α-BzO)2 sediment. The separation column was rinsed with a suitable volume of dilute nitric acid solution.
4. 10ML of 0.9% physiological saline is taken to wash the generator, and the test is conducted. After 24 hours, the generator was rinsed with 10ml of 0.9% physiological saline and the eluate was collected in a vacuum flask. The radionuclide composition in the eluent was analyzed by a high-purity germanium gamma spectrometer, no 99 Mo component with an energy peak of 739keV was present in the eluent, and only 99m Tc with 140keV was present, indicating that the adsorption rate of 99 Mo on the separation column was 100%, and no 99 Mo penetration was present in the eluent.
5. After 99 Mo in the generator decays fully, the sediment in the generator is dissolved in 60mL of 2mol/L sodium hydroxide solution, the solution is filtered by a 0.2 mu m filter membrane, an equal volume of ethyl acetate is added into the filtrate, and after extraction and separation, water phase is collected and evaporated to dryness, and then the MoO 3 powder is obtained by burning at 500 ℃.
The 99Mo-99m Tc color layer generator and the 99m Tc isotope preparation provided by the invention have high adsorption capacity to 99 Mo, can solve the problems of large chromatographic column volume, large radioactive waste liquid volume and the like in the preparation of the chromatographic 99Mo-99m Tc generator by taking 99 Mo with low specific activity as a raw material, overcome the defects of large column volume, wide leaching peak, low 99m Tc leaching efficiency, low 99m Tc radioactive concentration and the like of a gel generator, and simultaneously provide a target recovery method for enriching 98 Mo and 100 Mo, and avoid the problems of using a nuclear material 235 U and generating a large amount of radioactive fission waste. Has the advantages of low cost, similar structure to the existing generator, convenient operation of hospital staff, and the like.
Those skilled in the art will appreciate that the features recited in the various embodiments of the invention and/or in the claims may be combined in various combinations and/or combinations, even if such combinations or combinations are not explicitly recited in the invention. In particular, the features recited in the various embodiments of the invention and/or in the claims can be combined in various combinations and/or combinations without departing from the spirit and teachings of the invention. All such combinations and/or combinations fall within the scope of the invention.
The embodiments of the present invention are described above. These examples are for illustrative purposes only and are not intended to limit the scope of the present invention. Although the embodiments are described above separately, this does not mean that the measures in the embodiments cannot be used advantageously in combination. The scope of the invention is defined by the appended claims and equivalents thereof. Various alternatives and modifications can be made by those skilled in the art without departing from the scope of the invention, and such alternatives and modifications are intended to fall within the scope of the invention.
Claims (8)
1. A method for preparing a high activity 99Mo-99m Tc color layer generator from low specific activity 99 Mo comprising:
the leaching unit comprises 99 Mo feed liquid bottle, a liquid storage bottle filled with 5-10 mL of 0.9% physiological saline, a pipeline connected with the separation unit and a needle head fixed on the pipeline, wherein the liquid outlet end of the leaching unit is connected with the liquid inlet end of the separation unit and is used for respectively conveying 99 Mo feed liquid and leaching liquid to the separation unit and leaching column packing in the separation unit;
The separation unit comprises a separation column, an adsorption material and plugs at two ends of the separation column, wherein a support piece is fixed at the bottom of the separation column, column packing in the separation unit sequentially comprises alpha-benzoin oxime and acidic alumina from a liquid inlet end to a liquid outlet end, the liquid outlet end of the separation unit is connected with the liquid inlet end of the collection unit, and the separation unit is used for reacting the alpha-benzoin oxime with 99 Mo, adsorbing 99 Mo by Al 2O3 and realizing separation of 99 Mo and 99m Tc;
The collecting unit comprises a vacuum bottle, a pipeline connected with the separating unit and a needle head fixed on the pipeline, and is used for collecting 99m Tc eluent, wherein the eluent is 99m Tc-containing solution collected after the column packing is leached;
The radiation protection unit comprises a lead shielding body of the separation unit and a lead tank outside a 99m Tc vacuum bottle which is eluted from the separation column and is used for radiation protection of radionuclides 99 Mo and 99m Tc.
2. The method of claim 1, wherein the specific activity of the 99 Mo solution is greater than 4 x 10 10 Bq/g Mo.
3. A method of preparing a 99m Tc isotope for a high activity 99Mo-99m Tc color layer generator from low specific activity 99 Mo according to claim 1 or 2, comprising:
wet loading acidic alumina into a separation unit;
Tiling alpha-benzoin oxime onto the alumina in the separation unit;
injecting a pre-configured 99 Mo feed solution into the separation unit to soak the α -benzoin oxime to obtain a 99MoO2(α-BzO)2 precipitate;
Eluting column packing in the separation unit with normal saline at regular intervals, and collecting eluent to obtain 99m Tc isotopes.
4. A method of preparing 99m Tc isotopes according to claim 3, wherein after decay of 99 Mo in the unit to be separated, further comprising:
Dissolving the non-radioactive MoO 2(α-BzO)2 precipitate into an alkaline solution;
Adding a polar organic phase to extract the alpha-benzoin oxime in the non-radioactive MoO 2(α-BzO)2 precipitate into the organic phase, and separating and recovering 98 Mo or 100 Mo target materials.
5. A method of preparing 99m Tc isotopes according to claim 3, characterised in that prior to tiling α -benzoin oxime on the alumina in the separation unit, it comprises:
A nitric acid solution is added to the separation unit to pre-equilibrate with the nitric acid solution.
6. A method of preparing 99m Tc isotopes according to claim 3, wherein said injecting a pre-configured 99 Mo feed solution into said separation unit, prior to eluting column packing in said separation unit with physiological saline, comprises:
The 99 Mo remaining in the separation unit was rinsed with dilute nitric acid solution.
7. The method of claim 4, wherein prior to dissolving the non-radioactive MoO 2(α-BzO)2 precipitate in the alkaline solution, comprising:
The residual 99 Tc in the separation unit was rinsed with physiological saline, and the 99 Tc was obtained by decay of the 99m Tc.
8. The method of claim 6, wherein the 99 Mo feed solution has a specific activity greater than 4 x 10 10 Bq/g Mo.
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