CN115612868A - Purification process for separating actinium 225 from thorium, actinium and radium - Google Patents
Purification process for separating actinium 225 from thorium, actinium and radium Download PDFInfo
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- CN115612868A CN115612868A CN202211149724.3A CN202211149724A CN115612868A CN 115612868 A CN115612868 A CN 115612868A CN 202211149724 A CN202211149724 A CN 202211149724A CN 115612868 A CN115612868 A CN 115612868A
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- 229910052776 Thorium Inorganic materials 0.000 title claims abstract description 34
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 title claims abstract description 31
- QQINRWTZWGJFDB-YPZZEJLDSA-N actinium-225 Chemical compound [225Ac] QQINRWTZWGJFDB-YPZZEJLDSA-N 0.000 title claims abstract description 30
- 229940125666 actinium-225 Drugs 0.000 title claims abstract description 30
- 229910052767 actinium Inorganic materials 0.000 title claims abstract description 28
- 229910052705 radium Inorganic materials 0.000 title claims abstract description 27
- QQINRWTZWGJFDB-UHFFFAOYSA-N actinium atom Chemical compound [Ac] QQINRWTZWGJFDB-UHFFFAOYSA-N 0.000 title claims abstract description 26
- HCWPIIXVSYCSAN-UHFFFAOYSA-N radium atom Chemical compound [Ra] HCWPIIXVSYCSAN-UHFFFAOYSA-N 0.000 title claims abstract description 24
- 238000000746 purification Methods 0.000 title claims abstract description 23
- 239000011347 resin Substances 0.000 claims abstract description 102
- 229920005989 resin Polymers 0.000 claims abstract description 102
- 238000001179 sorption measurement Methods 0.000 claims abstract description 66
- 239000003480 eluent Substances 0.000 claims abstract description 10
- 238000004519 manufacturing process Methods 0.000 claims abstract description 9
- 239000002253 acid Substances 0.000 claims abstract description 8
- 238000005303 weighing Methods 0.000 claims abstract description 8
- 238000000034 method Methods 0.000 claims abstract description 5
- 238000000926 separation method Methods 0.000 claims description 15
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 6
- 239000012498 ultrapure water Substances 0.000 claims description 6
- 239000002245 particle Substances 0.000 claims description 5
- 229920000742 Cotton Polymers 0.000 claims description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 2
- 229910017604 nitric acid Inorganic materials 0.000 claims description 2
- 238000012856 packing Methods 0.000 claims description 2
- 238000011084 recovery Methods 0.000 claims description 2
- 239000000741 silica gel Substances 0.000 claims description 2
- 229910002027 silica gel Inorganic materials 0.000 claims description 2
- 239000000725 suspension Substances 0.000 claims description 2
- 229910052768 actinide Inorganic materials 0.000 claims 2
- 150000001255 actinides Chemical class 0.000 claims 2
- 239000000243 solution Substances 0.000 description 53
- 150000002500 ions Chemical class 0.000 description 8
- 230000000694 effects Effects 0.000 description 6
- 206010028980 Neoplasm Diseases 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 238000002560 therapeutic procedure Methods 0.000 description 3
- 238000013459 approach Methods 0.000 description 2
- 230000006378 damage Effects 0.000 description 2
- 238000000605 extraction Methods 0.000 description 2
- 238000001727 in vivo Methods 0.000 description 2
- 230000001225 therapeutic effect Effects 0.000 description 2
- 102000008394 Immunoglobulin Fragments Human genes 0.000 description 1
- 108010021625 Immunoglobulin Fragments Proteins 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 201000011510 cancer Diseases 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 238000005429 filling process Methods 0.000 description 1
- 230000004992 fission Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000003384 imaging method Methods 0.000 description 1
- 238000011835 investigation Methods 0.000 description 1
- 229910052747 lanthanoid Inorganic materials 0.000 description 1
- 150000002602 lanthanoids Chemical class 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000011259 mixed solution Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000009206 nuclear medicine Methods 0.000 description 1
- -1 on the other hand Chemical compound 0.000 description 1
- 230000035515 penetration Effects 0.000 description 1
- 229920001184 polypeptide Polymers 0.000 description 1
- 102000004196 processed proteins & peptides Human genes 0.000 description 1
- 108090000765 processed proteins & peptides Proteins 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000002285 radioactive effect Effects 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 230000008685 targeting Effects 0.000 description 1
- 238000011287 therapeutic dose Methods 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
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- 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
- 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
- C22B3/38—Treatment or purification of solutions, e.g. obtained by leaching by liquid-liquid extraction using organic compounds containing phosphorus
- C22B3/384—Pentavalent phosphorus oxyacids, esters thereof
- C22B3/3846—Phosphoric acid, e.g. (O)P(OH)3
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- Life Sciences & Earth Sciences (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Environmental & Geological Engineering (AREA)
- Materials Engineering (AREA)
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Abstract
The invention relates to the field and discloses a purification process for separating actinium 225 from thorium, actinium and radium, which comprises the following steps of S1, preparing an adsorption resin column, respectively weighing appropriate LN series resin and P204 resin, and manufacturing the resin adsorption column; s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant-temperature oscillator, reacting for a period of time, and taking out the LN series resin adsorption column to obtain a solution A; s3, adding a proper amount of acid liquor into the solution A obtained in the step S2, adding a P204 resin adsorption column, putting the centrifugal tube into a constant-temperature oscillator for reaction for a period of time, and taking out the P204 resin adsorption column to obtain a solution C; and S4, treating the P204 resin adsorption column in the step S3 by taking a proper amount of eluent to obtain the purified actinium 225 solution, wherein the actinium 225 can be efficiently separated from the thorium and the radium by the process provided by the invention, so that the actinium 225 is purified.
Description
Technical Field
The invention relates to the field, in particular to a purification process for separating actinium 225 from thorium, actinium and radium.
Background
Nuclear medicine has great application value in both diagnostic and therapeutic applications, where radionuclides for diagnostic or therapeutic use are usually attached to selective biomolecules (polypeptides, antibody fragments or whole antibodies) to deliver imaging or therapeutic doses to targets (tumors or other tissues) in vivo, targeted Alpha Therapy (TAT) is a rapidly developing field that utilizes alpha radionuclides to selectively deliver radiation doses that kill cells to the tumor site, where low penetration ranges (50-90 μm) and high linear mass transfer of alpha particles (tens to hundreds of keV/μm) can maximize destruction of cancer cells with minimal damage to surrounding healthy tissues.
Actinium-0225 has significant potential as a TAT nuclide because of its favorable half-life and decay cascade including multiple short-lived alpha nuclides, which when combined with a biological targeting vector can be used directly for therapy, or as a parent for the daughter nuclide 213Bi (t 1/2=45.6 min), which can also be chelated or complexed for use in vivo.
At the present time, it is known that, 225 the main source of Ac is the parent 229 Th(t 1/2 =7340 a), early stage from 233 U is obtained in reactors as fuel, now produced globally by decay 225 The supply of Ac does not exceed 63GBq (1.7 Ci) [9 ] per year]To is aligned with 225 The Ac demand exceeds the raw material 229 Th can be provided, therefore, in recent years, a different group including the Los Alamos National Laboratory (LANL) has been paired with production 225 Alternative approaches to Ac have been investigated, and one of the most promising approaches is thought to be via intermediate energy (C) ((R))>70 MeV) proton activation 232 Th occur 232 Th (p, x) nuclear reaction, data obtained from LANL, showed proton pairs with energies of 100MeV, 250 μ A 232 Th producing 73.2GBq (1.98 Ci) after 10 days of irradiation 225 Ac, the number of which exceeds that of each research department worldwide 229 Obtained from Th 225 Accumulation of Ac.
Albeit from 232 The Th (p, x) nuclear reaction can produce appreciable quantities 225 Ac, but separation of actinium and radium from irradiated thorium targets is a difficult problem, the irradiation mainly contains three elements Th, ra and Ac, and also generates a series of radioactive isotopes, fission products and a large excess of thorium must be separated from actinium, the separation of thorium and actinium is more difficult, on one hand, the metals thorium and actinium are very different in quality because of the relationship between decay parent and daughter generation, the concentration difference is several orders of magnitude, namely, trace actinium and radium are enriched and separated from a large amount of thorium, on the other hand, thorium and actinium which are both actinium have similar chemical propertiesBecause it is difficult to directly separate Ac from Th due to the interference of high-concentration Th, gradual separation is needed, namely, chemical treatment is carried out on irradiated thorium target through a series of ion separation and extraction chromatographic columns, so that a high-efficiency and rapid chemical separation and purification method of thorium, actinium and radium is sought, which provides a foundation for the research and development of Targeted Alpha Therapy (TAT) and has important significance for the development of radionuclide drugs.
Disclosure of Invention
The invention aims to provide a purification process for separating actinium 225 from thorium, actinium and radium aiming at the defects of the prior art.
The technical purpose of the invention is realized by the following technical scheme: a purification process for separating actinium 225 from thorium, actinium and radium comprises the following steps:
s1, preparing an adsorption resin column, namely respectively weighing appropriate LN series resin and P204 resin, and manufacturing the resin adsorption column;
s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant-temperature oscillator, reacting for a period of time, and taking out the LN series resin adsorption column to obtain a solution A;
s3, adding a proper amount of acid liquor into the solution A obtained in the step S2, adding a P204 resin adsorption column, putting the centrifugal tube into a constant-temperature oscillator for reaction for a period of time, and taking out the P204 resin adsorption column to obtain a solution C;
and S4, treating the P204 resin adsorption column in the step S3 by using a proper amount of eluent to obtain the purified actinium 225 solution.
Further, the resin in the step S1 is filled into a column by adopting a wet method, and the resin is put into a beaker filled with ultrapure water to prepare a suspension.
Furthermore, before the resin column filling in the step S1, cotton needs to be plugged at the bottom of the column, silica gel needs to be laid on the cotton, and ultrapure water needs to be used for repeated washing in the resin column filling process.
Further, the step S3 is to add an appropriate amount of nitric acid solution to the solution a until the PH of the solution a is 3.
Further, the step S2 and the step S3 are respectively put into a constant temperature oscillator for reaction for 10-20h.
Further, the LN series resin of step S1 has a particle size of 0.315 to 0.515mm.
Further, the eluent for the P204 resin adsorption column treatment in step S3 in step S4 may be ultrapure water.
Further, the LN series resin adsorption column of step S2 and the solution C of step S3 are subjected to a recovery treatment.
Compared with the prior art, the scheme of the invention has the following beneficial effects: the invention separates the solution by a resin adsorption column prepared by wet column packing, thereby realizing the purification process of actinium 225, wherein, LN series resin with smaller granularity is adopted to adsorb thorium in the solution, and then the solution is adjusted to PH 3, ra and Ra are mixed by a P204 resin adsorption column 225 In the mixed solution of Ac 225 Ac purification and purification process is efficient, and the obtained product 225 The Ac purity is high.
Drawings
FIG. 1 shows the ion concentrations of the solutions after treatment with LN series resin adsorption column of example 1 of the present invention;
FIG. 2 shows the ion concentrations of the solutions after the LN series resin adsorption column treatment in example 2 of the present invention;
FIG. 3 shows the ion concentrations of the solutions after the treatment of the P204 resin adsorption column in example 3 of the present invention;
FIG. 4 shows the ion concentrations of the solutions after the treatment of the P204 resin adsorption column in example 4 of the present invention.
Detailed Description
The invention provides a purification process for separating actinium 225 from thorium, actinium and radium, which comprises the following steps:
s1, preparing an adsorption resin column, namely respectively weighing appropriate LN series resin and P204 resin, and manufacturing the resin adsorption column;
s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant temperature oscillator for reaction for a period of time, and taking out the LN series resin adsorption column to obtain a solution A;
step S3, adding a proper amount of acid liquor into the solution A obtained in the step S2, adding a P204 resin adsorption column, putting the centrifugal tube into a constant-temperature oscillator for reacting for a period of time, and taking out the P204 resin adsorption column to obtain a solution C;
and S4, treating the P204 resin adsorption column in the step S3 by taking a proper amount of eluent to obtain the purified actinium 225 solution.
Because it is difficult to directly separate Ac from Th under the interference of high-concentration Th, it is still necessary to separate it step by step, i.e. the irradiated thorium target is chemically treated by a series of extraction chromatographic columns, and it is found by investigation that commercial series LN resin has excellent separation effect on rare earth elements and lanthanide elements, while P204 resin can selectively separate Sr and Y, so it may also have separation effect on Ac and Ra in the same main group. Therefore, the present invention uses these two resins to separate three ions, th, ac and Ra.
Example 1
A purification process for separating actinium 225 from thorium, actinium and radium comprises the following steps:
s1, preparing an adsorption resin column, namely respectively weighing appropriate LN series resin with the granularity of 0.515mm and P204 resin, and manufacturing the resin adsorption column;
s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant-temperature oscillator, reacting for a period of time, and taking out the LN series resin adsorption column to obtain a solution A;
s3, adding a proper amount of acid liquor into the solution A in the step S2 to enable the pH value of the solution to be 5, adding a P204 resin adsorption column, putting the centrifugal tube into a constant-temperature oscillator for reaction for a period of time, taking out the P204 resin adsorption column, and obtaining a solution C;
and S4, treating the P204 resin adsorption column in the step S3 by taking a proper amount of eluent to obtain the purified actinium 225 solution.
Example 2
A purification process for separating actinium 225 from thorium, actinium and radium comprises the following steps:
s1, preparing an adsorption resin column, namely respectively weighing appropriate LN series resin with the granularity of 0.315mm and appropriate P204 resin, and manufacturing the resin adsorption column;
s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant-temperature oscillator, reacting for a period of time, and taking out the LN series resin adsorption column to obtain a solution A;
step S3, adding a proper amount of acid liquor into the solution A obtained in the step S2 to enable the pH value of the solution to be 4, adding a P204 resin adsorption column, placing the centrifugal tube into a constant-temperature oscillator to react for a period of time, taking out the P204 resin adsorption column, and obtaining a solution C;
and S4, treating the P204 resin adsorption column in the step S3 by taking a proper amount of eluent to obtain the purified actinium 225 solution.
Example 3
A purification process for separating actinium 225 from thorium, actinium and radium comprises the following steps:
s1, preparing an adsorption resin column, namely respectively weighing appropriate LN series resin with the granularity of 0.515mm and P204 resin, and manufacturing the resin adsorption column;
s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant temperature oscillator for reaction for a period of time, and taking out the LN series resin adsorption column to obtain a solution A;
step S3, adding a proper amount of acid liquor into the solution A obtained in the step S2 to enable the pH value of the solution to be 5, adding a P204 resin adsorption column, placing the centrifugal tube into a constant-temperature oscillator to react for a period of time, taking out the P204 resin adsorption column, and obtaining a solution C;
and S4, treating the P204 resin adsorption column in the step S3 by using a proper amount of eluent to obtain the purified actinium 225 solution.
Example 4
A purification process for separating actinium 225 from thorium, actinium and radium comprises the following steps:
s1, preparing an adsorption resin column, namely respectively weighing an appropriate amount of LN series resin with the granularity of 0.315 and P204 resin, and manufacturing the resin adsorption column;
s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant temperature oscillator for reaction for a period of time, and taking out the LN series resin adsorption column to obtain a solution A;
s3, adding a proper amount of acid liquor into the solution A in the step S2 to enable the pH value of the solution to be 3, adding a P204 resin adsorption column, putting the centrifugal tube into a constant-temperature oscillator for reaction for a period of time, taking out the P204 resin adsorption column, and obtaining a solution C;
and S4, treating the P204 resin adsorption column in the step S3 by taking a proper amount of eluent to obtain the purified actinium 225 solution.
Each of the solutions of examples 1 to 4 was individually taken, and the effluent of each solution was measured for Th, ra, and, 225 Ac ion concentration is shown in FIGS. 1-4, where the triangular symbol curve represents thorium, the circular curve represents actinium 225, and the rectangular curve represents radium, and it can be seen from FIGS. 1-4 that the LN series resin has different concentration ratios of Th, ra, and, 225 Three ions of Ac have good separation effect; however, the LN resin having a large particle size at a high concentration ratio had a poor separation effect, while the LN resin having a small particle size still had a good separation effect, and the P204 resin had a pH =3-5 in the range of Ra, 225 Ac was excellent in separation effect, and was most preferable at pH = 3.
The present embodiment is only for explaining the present invention, and it is not limited to the present invention, and those skilled in the art can make modifications without inventive contribution to the present embodiment as required after reading the present specification, but all of them are protected by patent law within the scope of the present invention.
Claims (8)
1. A purification process for separating actinium 225 from thorium, actinium and radium is characterized by comprising the following steps:
s1, preparing an adsorption resin column, namely respectively weighing appropriate LN series resin and P204 resin, and manufacturing the resin adsorption column;
s2, removing a proper amount of solution to be separated, injecting the solution into a centrifuge tube, adding an LN series resin adsorption column, putting the centrifuge tube into a constant-temperature oscillator, reacting for a period of time, and taking out the LN series resin adsorption column to obtain a solution A;
s3, adding a proper amount of acid liquor into the solution A obtained in the step S2, adding a P204 resin adsorption column, putting the centrifugal tube into a constant-temperature oscillator for reaction for a period of time, and taking out the P204 resin adsorption column to obtain a solution C;
and S4, treating the P204 resin adsorption column in the step S3 by taking a proper amount of eluent to obtain the purified actinium 225 solution.
2. The purification process for separating actinium 225 from thorium, actinium and radium as claimed in claim 1, wherein the resin of step S1 is packed into a column by a wet method, and the resin is put into a beaker filled with ultrapure water to prepare a suspension.
3. The purification process for separating actinium 225 from thorium, actinium and radium as claimed in claim 2, wherein the cotton is packed at the bottom of the resin column and is paved with silica gel before the resin column is packed in the step S1, and the resin column is repeatedly washed by using ultrapure water during the resin column packing process.
4. A purification process for the separation of actinium 225 from thorium, actinium and radium according to claim 1, characterized in that the step S3 consists in adding a suitable amount of nitric acid solution to solution A until the pH of solution A is 3.
5. The purification process for separation of actinium 225 from thorium, actinium and radium according to claim 1, characterized in that the steps S2 and S3 respectively put the centrifuge tube into a constant temperature oscillator for reaction for 10-20h.
6. A purification process for the separation of actinium 225 from thorium, actinium and radium according to claim 1, characterised in that the particle size of the LN series resin of step S1 is 0.315-0.515mm.
7. The purification process for separating actinium 225 from thorium, actinium and radium as claimed in claim 1, wherein the eluent used in the step S4 for the treatment of the P204 resin adsorption column of the step S3 can be ultrapure water.
8. A purification process for the separation of actinides 225 from thorium, actinides and radium according to claim 1, characterized in that: the LN series resin adsorption column of step S2 and the solution C of step S3 are also subjected to a recovery treatment.
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