CN120114994A - A method for preparing a carrier-free 90YCl3 solution - Google Patents
A method for preparing a carrier-free 90YCl3 solution Download PDFInfo
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- CN120114994A CN120114994A CN202510267431.2A CN202510267431A CN120114994A CN 120114994 A CN120114994 A CN 120114994A CN 202510267431 A CN202510267431 A CN 202510267431A CN 120114994 A CN120114994 A CN 120114994A
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Abstract
本发明涉及一种无载体90YCl3溶液的制备方法，包括如下步骤，将预处理的90Sr‑90Y母液加载到第一色谱柱上，使90Y吸附到第一色谱柱上与大量90Sr分离，收集90Sr流出液；分别依次使用洗涤剂1和洗脱剂1淋洗第一色谱柱，收集洗涤剂1的流出液和洗脱剂1的流出液；将收集的洗脱剂1的流出液通过第二色谱柱，使其中的90Y吸附到第二色谱柱上；分别依次使用洗涤剂2和洗脱剂2淋洗第二色谱柱，收集洗涤剂2的流出液和洗脱剂2的流出液，洗脱剂2的流出液即为90YCl3溶液。与现有技术相比，本发明仅用两根萃淋树脂色谱柱就能实现90Sr和90Y的高效分离，操作简单、分离效率高、90Sr损失率低，可直接制备出药用级无载体90YCl3溶液。
The invention relates to a method for preparing a carrier-free 90 YCl 3 solution, comprising the following steps: loading a pretreated 90 Sr- 90 Y mother liquor onto a first chromatographic column, allowing 90 Y to be adsorbed onto the first chromatographic column and separated from a large amount of 90 Sr, and collecting 90 Sr effluent; using detergent 1 and eluent 1 to elute the first chromatographic column in sequence, collecting the effluent of the detergent 1 and the effluent of the eluent 1; passing the collected effluent of the eluent 1 through a second chromatographic column, allowing 90 Y therein to be adsorbed onto the second chromatographic column; using detergent 2 and eluent 2 to elute the second chromatographic column in sequence, collecting the effluent of the detergent 2 and the effluent of the eluent 2, wherein the effluent of the eluent 2 is the 90 YCl 3 solution. Compared with the prior art, the present invention can achieve efficient separation of 90 Sr and 90 Y with only two leaching resin chromatographic columns, has simple operation, high separation efficiency, and low 90 Sr loss rate, and can directly prepare a pharmaceutical-grade carrier-free 90 YCl 3 solution.
Description
Technical Field
The invention relates to the technical field of medical isotope preparation, in particular to a preparation method of a carrier-free 90YCl3 solution.
Background
Yttrium-90 (90 Y) is an important medical isotope, has short half-life (64.1 h), emits high-energy pure beta rays (up to 2.27MeV, average 0.938 MeV), has short tissue penetration distance (average range in tissue of 2.5mm, maximum range of 10.3 mm), has stable and nontoxic decay daughter 90 Zr, has good chelating chemical property and the like, and is the preferred isotope for clinically treating large-volume tumors. The carrier-free yttrium trichloride-90 (90YCl3) solution is an important raw material for preparing radiopharmaceuticals and products such as 90 Y microspheres, 90 Y labeled monoclonal antibodies, 90 Y labeled polypeptides and the like, and has wide market application prospect. The main method for obtaining the carrier-free 90YCl3 is to extract 90 Y from 90Sr-90 Y equilibrium solution, namely 90Sr-90 Y mother liquor, periodically and repeatedly by utilizing the principle of 90Sr-90 Y decay equilibrium and the difference of chemical properties of two nuclides. since 90 Sr is a strong bone-philic and highly toxic nuclide, the key of the medicinal 90YCl3 is to reduce the content of 90 Sr to below 2X 10 -5Bq/Bq 90 Y, reduce the content of Fe 3+ and other metal ions which compete with 90Y3+ for coordination, and the like (group standard T/CIRA 55-2023 yttrium trichloride [ 90 Y ] solution). Currently, methods for strontium-yttrium separation mainly include solvent extraction, electrodeposition, precipitation, column chromatography, and the like.
In 1990, the national laboratory on oak-ridge reported for the first time that 90 Y was extracted from 90Sr-90 Y mother liquor using di- (2-ethylhexyl) phosphate (HDEHP)/n-dodecane as extractant to effect separation of strontium and yttrium, and finally separated curie grade 90 Y product (Applied Radiation Isotopes,1990,41,861) by washing, back extraction, etc., which subsequently optimized the flow and filed US patent No. 5512256. Although the method can obtain a large amount of high-purity 90 Y, the defects of accumulated extractant radiation decomposition products, large amount of radioactive waste liquid, complicated operations of purifying 90 Y by combining an ion exchange resin column, evaporating concentrated acid and the like exist in the 90 Sr raw material, and the application range of the method is limited.
In 2003, the university of Qinghua reported an electrodeposition method for separating 90 Y from 90Sr-90 Y mother liquor, 90 Y was deposited on a cathode platinum electrode to achieve strontium-yttrium separation (patent CN1455023 a), and then, the content of 90 Sr in 90 Y (isotope, 2007,20,159;Nuclear Medicine and Biology,2008,35,245;CN117702190A) was reduced by two electrodeposition at the university of Qinghua, the indian baba atomic research center, the high-pass homoleptin limited company of chengdou, etc., but the method still had the problems that the mother liquor reuse needs to be adjusted in pH, the electrodeposition rate of 90 Y is low, the electrolysis process is difficult to control, mass production is impossible, etc.
In 2001, U.S. patent publication reports a method of purifying 90 Y using a Y-selective extraction resin column after separating strontium and yttrium by precipitation 90 Sr with concentrated nitric acid, and then the method applies for China patent (CN 1429391A), similarly, in 2006, U.S. patent (US 7517508B 2) reports a method of removing trace 90 Sr, zr, etc. in 90 Y using ion exchange resin after precipitating 90 Sr with concentrated nitric acid. The precipitation method is complicated in operation, and often requires the addition of a non-radioactive carrier, further purification by combining with column chromatography, and the like.
In 1992, the national laboratory of the US archery reported column chromatography for the preparation of 90 Y of high chemical and radiochemical purity, passing 90Sr-90 Y mother liquor through a three-stage Sr-selective chromatography column to effect strontium yttrium separation, and then passing 90 Y-containing stream through a first-stage Y-selective chromatography column to effect purification of 90 Y (Applied Radiation Isotopes,1992,43,1093), followed by the method being filed for US patent No. 5368736. There are patent and literature reports (CN 105478097a; journal of Chromatography A,2011,1218,6483) that resins containing crown ether (4 ',4 "(5") -di-tert-butyldicyclohexyl and 18-crown-6) or TODGA (N, N' -tetraoctyl-3-oxa-glutaramide) can be used for strontium yttrium separation, but the amount of 90 Sr contamination in the final 90 Y product is high and does not meet the pharmaceutical requirements.
Although column chromatography has the advantages of simple operation and less radioactive waste liquid, the existing method has the defects of multi-stage (> 3) chromatographic column combination, acid regulation by evaporation between chromatographic columns, no 90YCl3 form of 90 Y at last, complex treatment by 90 Sr multiplexing and the like.
Disclosure of Invention
The invention aims to provide a preparation method of a carrier-free 90YCl3 solution, which has the advantages of simple operation, high separation efficiency and low 90 Sr loss rate, can realize the high-efficiency separation of 90 Sr and 90 Y by only using two extraction resin chromatographic columns, and can directly prepare a medicinal carrier-free 90YCl3 solution.
The aim of the invention can be achieved by the following technical scheme:
A method for preparing a solution without carrier 90YCl3, comprising the steps of:
S1, loading the pretreated 90Sr-90 Y mother liquor onto a first chromatographic column, enabling 90 Y to be adsorbed onto the first chromatographic column and separated from 90 Sr, and collecting 90 Sr effluent;
s2, eluting the first chromatographic column by sequentially using a detergent 1 and an eluent 1, and collecting an effluent of the eluent 1;
S3, allowing the collected effluent of the eluent 1 to pass through a second chromatographic column, and adsorbing 90 Y in the effluent onto the second chromatographic column;
S4, sequentially eluting the second chromatographic column by using the washing agent 2 and the eluting agent 2, and collecting the effluent of the eluting agent 2 to obtain 90YCl3 solution.
Preferably, in step S1, the pre-treated 90Sr-90 Y mother liquor is 90Sr-90 Y balanced or nearly balanced HNO 3 solution of 0.05-1mol/L, and 90Sr-90 Y balanced or nearly balanced refers to that the 90 Sr solution with high purity is placed for 7-28 days.
Preferably, the height-to-diameter ratio of the first chromatographic column to the second chromatographic column is 1:1-25:1.
Preferably, the packing material in the first chromatographic column and the second chromatographic column is an extraction resin.
Further preferably, the size of the extraction resin is 5-500 μm.
Preferably, the first chromatographic column is filled with trialkyl phosphine oxide resin, and alkyl in the trialkyl phosphine oxide is one or more of C 5、C6、C7、C8、C9、C10、C11、C12 straight-chain or branched-chain alkyl.
Preferably, the second chromatographic column is filled with amide methyl phosphine oxide resin, and the amide methyl phosphine oxide resin comprises one or two of octyl (phenyl) -N, N-diisobutyl-carbamoyl methyl phosphine oxide and diphenyl-N, N-diisobutyl-carbamoyl methyl phosphine oxide.
Preferably, in the step S2, the detergent 1 is HNO 3 solution with the concentration of 0.05-1mol/L, and the eluent 1 is HNO 3 solution with the concentration of 4-10 mol/L.
Preferably, in step S4, the detergent 2 is 4-10mol/L HNO 3 solution, and the eluent 2 is HCl solution with pH value of 1-2.
Preferably, in step S1, the 90 Sr effluent is left for 7-28 days to obtain a new 90Sr-90 Y mother liquor.
Further preferably, the 90 Sr effluent liquid is placed for 14 days to obtain new 90Sr-90 Y mother liquor.
Further preferably, the preparation method of the carrier-free 90YCl3 solution comprises the steps of loading the pretreated 90Sr-90 Y mother liquor on a first chromatographic column, enabling 90 Y to be adsorbed on the first chromatographic column and separated from a large amount of 90 Sr, collecting 90 Sr effluent, standing for a period of time to obtain new 90Sr-90 Y mother liquor, eluting the first chromatographic column by using a detergent 1, collecting the effluent of the detergent 1, eluting the first chromatographic column by using the eluent 1, enabling the effluent of the eluent 1 to pass through a second chromatographic column, enabling 90 Y in the effluent to be adsorbed on the second chromatographic column, eluting the second chromatographic column by using the detergent 2, collecting the effluent of the detergent 2, eluting the second chromatographic column by using the eluent 2, and collecting the effluent of the eluent 2 to obtain 90YCl3 solution.
According to the invention, the trialkylphosphine oxide type extraction resin is adopted as a first chromatographic column to adsorb yttrium 90 (90 Y), the amidomethyl phosphine oxide type extraction resin is adopted as a second chromatographic column to remove a small amount of strontium 90 (90 Sr), wherein the selection of column materials of the first chromatographic column and the second chromatographic column is matched with the acidity of the selected detergents 1 and 2 and the eluents 1 and 2, the elution acidity of the two-stage chromatographic columns is optimized to form a continuous gradient, the two-stage chromatographic columns can be well connected, the intermediate concentration or pH adjustment step is avoided, the high-efficiency separation of 90 Sr and 90 Y can be realized, and the medical yttrium chloride 90 (90YCl3) solution is directly obtained.
Compared with the prior art, the invention has the following beneficial effects:
(1) The invention provides a preparation method of a carrier-free 90YCl3 solution, which has the advantages of simple operation, high separation efficiency and low 90 Sr loss rate, can realize the high-efficiency separation of 90 Sr and 90 Y by only using two extraction resin chromatographic columns, and can directly prepare a medicinal carrier-free 90YCl3 solution.
(2) The 90 Sr effluent collected in the preparation process can be directly reused after being placed for 7-28 days, the recovery rate is high, and the 90 Sr loss rate is low.
(3) The preparation method has the advantages of simple operation, short time consumption, repeated multiplexing of chromatographic columns, less waste liquid amount, no need of evaporation for acid regulation and other complex operations, and can directly prepare the pharmaceutical grade 90YCl3 solution, wherein the recovery rate of 90 Y is more than 70%.
(4) Compared with other methods, the method is very suitable for preparing 90Sr-90 Y generator devices or systems, is directly used in a radioactive pharmacy of a hospital or a medical company, and realizes mass production of medical 90 Y nuclide millicurie to Baicurie orders.
Drawings
FIG. 1 is a flow chart of a method for preparing carrier-free 90YCl3 from 90Sr-90 Y mother liquor by separation according to the present invention;
FIG. 2 is a diagram showing the separation effect of example 1 of the present invention.
Detailed Description
The present embodiment is implemented on the premise of the technical scheme of the present invention, and a detailed implementation manner and a specific operation process are given, but the protection scope of the present invention is not limited to the following examples.
A method for preparing a solution without carrier 90YCl3, comprising the steps of:
S1, loading the pretreated 90Sr-90 Y mother liquor onto a first chromatographic column, enabling 90 Y to be adsorbed onto the first chromatographic column and separated from 90 Sr, and collecting 90 Sr effluent;
s2, eluting the first chromatographic column by sequentially using a detergent 1 and an eluent 1, and collecting an effluent of the eluent 1;
S3, allowing the collected effluent of the eluent 1 to pass through a second chromatographic column, and adsorbing 90 Y in the effluent onto the second chromatographic column;
S4, sequentially eluting the second chromatographic column by using the washing agent 2 and the eluting agent 2, and collecting the effluent of the eluting agent 2 to obtain 90YCl3 solution.
In the following examples, 90 Sr material was 90 Sr solution obtained by extraction and purification from spent fuel post-treatment high-level waste liquid, and the index was that the alpha impurity in 90 Sr was <1×10 -8, the gamma impurity was <2×10 -4, and the chemical purity of strontium was >95%. Unless specifically indicated otherwise, the reagents, methods, apparatus and devices employed in the present invention are those conventional in the art. Reagents and materials used in the following examples are commercially available unless otherwise specified.
The invention will now be described in detail with reference to the drawings and specific examples.
Example 1
A preparation method of a carrier-free 90YCl3 solution is shown in fig. 1, and comprises the following specific steps:
(1) The acidity of 90Sr-90 Y mother liquor is regulated to be HNO 3 solution with the concentration of 0.4mol/L, and the activity of 90 Sr is regulated to be 20Ci/L;
(2) Passing 100mL of 90Sr-90 Y mother liquor in the step (1) through a first chromatographic column, wherein 50-100 mu m TOPO (tri-n-octyl phosphine oxide) extraction resin is filled in the chromatographic column, the inner diameter of the resin column is 8mm, and the volume of the resin column is 2mL, collecting 90 Sr effluent, and standing for 14 days to obtain new 90Sr-90 Y mother liquor;
(3) Eluting the first chromatographic column by using 30mL of 0.4mol/L HNO 3 solution as a detergent 1, and collecting effluent liquid;
(4) Eluting the first chromatographic column by using 15mL 7mol/L HNO 3 solution as eluent 1, and collecting effluent;
(5) Passing the eluent in (4) through a second chromatographic column, wherein the chromatographic column is filled with 50-100 mu m CMPO (octyl (phenyl) -N, N-diisobutyl-carbamoylmethylphosphine oxide) resin, the inner diameter of the resin column is 5mm, and the volume of the resin column is 1mL;
(6) Eluting the second chromatographic column by using 15mL 7mol/L HNO 3 solution as a detergent 2, and collecting effluent;
(7) And eluting the second chromatographic column by using 10mL of 0.01mol/L HCl solution as an eluent 2, and collecting effluent liquid, namely the carrier-free 90YCl3 solution.
In the above steps, the flow rate of the liquid passing through the chromatographic column was 1mL/min. The separation effect is shown in fig. 2 and table 1. In fig. 2, washing liquid 1, i.e. the effluent of the washing agent 1 flowing through the first chromatographic column, eluting liquid 1, i.e. the effluent of the washing agent 1 flowing through the first chromatographic column, washing liquid 2, i.e. the effluent of the washing agent 2 flowing through the second chromatographic column, eluting liquid 2, i.e. the effluent of the eluting agent 2 flowing through the second chromatographic column.
Example 2
A preparation method of a carrier-free 90YCl3 solution is shown in fig. 1, and comprises the following specific steps:
(1) The acidity of 90Sr-90 Y mother liquor is regulated to be HNO 3 solution with the concentration of 0.1mol/L, and the activity of 90 Sr is regulated to be 50Ci/L;
(2) Passing 100mL of 90Sr-90 Y mother liquor in the step (1) through a first chromatographic column, filling 50-100 mu m TRPO (C 6-C8 mixed trialkylphosphine oxide) resin in the chromatographic column, wherein the inner diameter of the resin column is 8mm, and the volume of the resin column is 2mL, collecting 90 Sr effluent, and standing for 14 days to obtain new 90Sr-90 Y mother liquor;
(3) 40mL of 0.1mol/L HNO 3 solution is used as a detergent 1, the first chromatographic column is leached, and effluent liquid is collected;
(4) Eluting the first chromatographic column by using 20mL 8mol/L HNO 3 solution as eluent 1, and collecting effluent;
(5) Passing the eluent in (4) through a second chromatographic column filled with 100-150 mu m CMPO resin extract, wherein the inner diameter of the resin column is 8mm, and the volume of the resin column is 2mL;
(6) Eluting the second chromatographic column by using 20mL 8mol/L HNO 3 solution as a detergent 2, and collecting effluent liquid;
(7) And eluting the second chromatographic column by using 20mL of 0.1mol/L HCl solution as an eluent 2, and collecting effluent liquid, namely the carrier-free 90YCl3 solution.
In the above steps, the flow rate of the liquid through the chromatographic column was 0.5mL/min. The separation effect is shown in Table 1.
Example 3
100ML of 90Sr-90 Y mother liquor multiplexed in example 1, namely the novel 90Sr-90 Y mother liquor obtained after the 90 Sr effluent collected in step (2) of example 1 is placed for 14 days, the activity of the novel 90Sr-90 Y mother liquor is 19.85Ci/L, and the separation effects of the other steps are shown in Table 1 as in example 1.
Example 4
The first column of example 2 was eluted with 8mol/L HNO 3 and 0.4mol/L HNO 3 and then reused, and the second column was eluted with 0.1mol/L HCl and 8mol/L HNO 3 and then reused.
50ML of 100Ci/L 90Sr-90 Y mother liquor was used, and the remaining steps were the same as in example 2, and the separation effect was shown in Table 1.
TABLE 1 evaluation of separation effect of examples 1 to 4
In conclusion, the preparation method of the carrier-free 90YCl3 solution provided by the invention has the advantages of simple operation, high separation efficiency, low 90 Sr loss rate, multiple multiplexing of chromatographic columns, realization of high-efficiency separation of 90 Sr and 90 Y by only using two extraction resin chromatographic columns, direct preparation of medicinal carrier-free 90YCl3 solution and wide application prospect.
The previous description of the embodiments is provided to facilitate a person of ordinary skill in the art in order to make and use the present invention. It will be apparent to those skilled in the art that various modifications can be readily made to these embodiments and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above-described embodiments, and those skilled in the art, based on the present disclosure, should make improvements and modifications without departing from the scope of the present invention.
Claims (10)
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