阅读说明：本技术 一种钼锝分离柱及钼锝分离方法 (Molybdenum-technetium separation column and molybdenum-technetium separation method ) 是由 周赛 李龙 黄勇 陈林 李杨 雷嗣烦 于 2020-04-10 设计创作，主要内容包括：本申请提供了一种钼锝分离柱及钼锝分离方法,涉及放射性核素分离技术领域,分离柱由双水相分离树脂制成,双水相分离树脂包括亲水基团和疏水基质,在分离钼锝过程中不需要使用有机溶剂,最终锝溶液中无有机物残留,更适用于核医学诊断。(The application provides a molybdenum-technetium separation column and a molybdenum-technetium separation method, which relate to the technical field of radionuclide separation.)

1. A molybdenum-technetium separation column, which is obtained by stacking irradiation⁹⁹Mo and^99mtc, characterized by: the separation column is made of a two aqueous phase separation resin comprising a hydrophilic group and a hydrophobic matrix.

2. The technetium-molybdenum separation column of claim 1, wherein: the hydrophilic group includes one or more of polyethylene glycol having a molecular weight of 500-.

3. The technetium-molybdenum separation column of claim 2, wherein: the hydrophilic group includes one or more of polyethylene glycol having a molecular weight of 5000-.

4. The technetium-molybdenum separation column of claim 1, wherein: the hydrophobic matrix comprises one or more of chloromethyl polystyrene, polystyrene and graphene oxide.

5. A method for separating molybdenum and technetium, which is obtained by stacking irradiation⁹⁹Mo and^99mtc, characterized by: the separation steps are as follows:

s1, dissolving molybdenum-technetium by using alkali liquor with hydroxide ion concentration of more than 0.5 mol/L;

s2, separating the molybdenum-technetium in the solution prepared in the step S1 by using the molybdenum-technetium separation column as claimed in any one of claims 1 to 4 through a dynamic method or a static method;

s3, leaching the molybdenum on the molybdenum-technetium separation column by using leacheate;

s4, eluting technetium on the molybdenum-technetium separation column by using an eluent.

6. The molybdenum-technetium separation method of claim 5, wherein: the alkali is sodium hydroxide or potassium hydroxide, and the concentration of hydroxide ions is 2-5 mol/L.

7. The molybdenum-technetium separation method of claim 5, wherein: in the S2 step, when molybdenum-technetium is separated by the dynamic method, the solution prepared in the S1 step is passed through a molybdenum-technetium separation column at a flow rate of 0.01-10000 mL/min.

8. The molybdenum-technetium separation method of claim 5, wherein: in the step S3, the leacheate is a hydroxide solution, and the specific operations are as follows:

s3.1, leaching the molybdenum-technetium separation column by using hydroxide radical solution with the concentration of 0.5-10 mol/L;

s3.2, leaching the molybdenum-technetium separation column by using hydroxide radical solution with the concentration of 0.1-0.5 mol/L.

9. The molybdenum-technetium separation method of claim 5, wherein: in the step S4, the eluent is a solution of carbonate ions, bicarbonate ions, and chloride ions in any ratio.

10. The molybdenum-technetium separation method of claim 9, wherein: the eluent is 0.9% sodium chloride solution.

Technical Field

The application relates to the technical field of radionuclide separation, in particular to a molybdenum-technetium separation column and a molybdenum-technetium separation method.

Background

^99mTc is due to the presence of gamma rays of suitable energy (140keV) and half-life (T)_1/26.02h) and is widely applied to nuclear medicine single photon emission computed tomography. Worldwide every year^99mThe Tc marker drug has more than thirty million times of nuclear medicine diagnosis, more than 80 percent of the nuclear medicine diagnosis, and has wide market prospect.

Conventional^99mThe main production modes of Tc are: high or low concentration in reactor²³⁵U fission generation⁹⁹Mo，⁹⁹Decay of Mo to produce^99mTc, then using molybdenum technetium separation technology to obtain the product meeting medical requirements^99mTc. Produced by 6 international reactors⁹⁹Mo accounts for more than 95% of the total amount of the whole world. However, due to extended maintenance times and unexpected shutdowns caused by these reactor ages, nuclear nonproliferation regulations, etc., many times have appeared in the world in recent years⁹⁹Mo and^99ma shortage of Tc.

Accordingly, non-fission has been developed in many countries and regions of the world⁹⁹Mo production^99mTc technical study, in which a pile-up photograph is used⁹⁹Mo production^99mTc technology is widely studied. However, because of⁹⁹The specific activity of Mo is very low, and the secondary fission cannot be adopted⁹⁹Separation and extraction of Mo^99mMethod for obtaining Tc^99mTc, and therefore, how to reduce specific activity⁹⁹High-efficiency separation and extraction of Mo^99mTc is a problem to be solved.

At present, from low specific activity⁹⁹Mo separation and extraction^99mThe methods for Tc are mainly: solvent extraction, sublimation, electrochemical processes, and column chromatography, often using organic solvents as extractants, resulting in the final^99mThe Tc solution contains a small amount of organic solvent, which poses certain risks for clinical use; in the sublimation method, technetium needs to be sublimated under the high-temperature condition so as to be collected, on one hand, the operation is relatively complex, and on the other hand, the recovery rate of the technetium is low; the operation of the electrochemical method is more complex, and the preparation cost is higher; the key of the column chromatography is to use a solid phase material to contain⁹⁹Mo and^99madsorption in Tc solution^99mTc, without or with little adsorption⁹⁹Mo, thereby achieving separation of molybdenum and technetium. The method has the characteristics of easy automation realization, stability and reliability, and the column chromatography becomes a research hotspot, in the prior art, the Dowex resin is adopted as a separation column to separate molybdenum and technetium, and the operation needs to be carried out by using an organic solvent or perchloric acid for leachingThe technetium is desorbed from the solid phase material, which presents a risk for clinical use.

Content of application

The first objective of the present application is to provide a separation column of molybdenum-technetium, which is made of two aqueous phase separation resin, and no organic solvent is needed in the process of separating molybdenum-technetium, and finally no organic matter remains in the technetium solution, and is more suitable for nuclear medicine diagnosis.

The second purpose of the application is to provide a molybdenum-technetium separation method, which adopts the molybdenum-technetium separation column to separate molybdenum from technetium, wherein the technetium elution efficiency is as high as more than 90%, the recovery rate of raw material molybdenum is as high as more than 85%, the operation is simple, and the whole process only needs about 90 minutes.

The embodiment of the application is realized by the following technical scheme:

a molybdenum-technetium separation column, which is obtained by stacking irradiation⁹⁹Mo and^99mtc, said separation column being made of an aqueous two-phase separation resin comprising hydrophilic groups and a hydrophobic matrix.

Further, the hydrophilic group comprises one or more of polyethylene glycol having a molecular weight of 500-20000 and polypropylene glycol having a molecular weight of 400-10000.

Further, the hydrophilic group comprises one or more of polyethylene glycol with the molecular weight of 5000-10000 and polypropylene glycol with the molecular weight of 3000-7000.

Further, the hydrophobic matrix comprises one or more of chloromethyl polystyrene, polystyrene and graphene oxide.

A method for separating molybdenum and technetium, which is obtained by stacking irradiation⁹⁹Mo and^99mtc, the separation steps are as follows:

s1, dissolving molybdenum-technetium by using alkali liquor with hydroxide ion concentration of more than 0.5 mol/L;

s2, separating the molybdenum-technetium in the solution prepared in the step S1 by using the molybdenum-technetium separation column as claimed in any one of claims 1 to 4 through a dynamic method or a static method;

s3, leaching the molybdenum on the molybdenum-technetium separation column by using leacheate;

s4, eluting technetium on the molybdenum-technetium separation column by using an eluent.

Preferably, the alkali is sodium hydroxide or potassium hydroxide, and the concentration of hydroxide ions is 2-5 mol/L.

Further, in the S2 step, when molybdenum-technetium is separated by the dynamic method, the solution prepared in the S1 step is passed through a molybdenum-technetium separation column at a flow rate of 0.01-10000 mL/min.

Further, in the step S3, the leacheate is a hydroxide solution, and the specific operations are as follows:

s3.1, leaching the molybdenum-technetium separation column by using hydroxide radical solution with the concentration of 0.5-10 mol/L;

s3.2, leaching the molybdenum-technetium separation column by using hydroxide radical solution with the concentration of 0.1-0.5 mol/L.

Further, in the step S4, the eluent is a solution of carbonate ions, bicarbonate ions, and chloride ions in any ratio.

Preferably, the eluent is a 0.9% sodium chloride solution.

The technical scheme of the embodiment of the application has at least the following advantages and beneficial effects:

the molybdenum-technetium separation column provided by the application is made of aqueous two-phase separation resin, an organic solvent is not needed in the molybdenum-technetium separation process, and finally, no organic matter remains in a technetium solution, so that the molybdenum-technetium separation column is more suitable for nuclear medicine diagnosis.

The molybdenum-technetium separation column is used for molybdenum-technetium separation, technetium elution efficiency is stabilized to be more than 90%, the recovery rate of raw material molybdenum is up to more than 85%, operation is simple, and the whole process only needs about 90 minutes.

Detailed Description

In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below. The examples, in which specific conditions are not specified, were conducted under conventional conditions or conditions recommended by the manufacturer. The reagents or instruments used are not indicated by the manufacturer, and are all conventional products available commercially.

The following provides a detailed description of the separation column and method for molybdenum-technetium.

A molybdenum-technetium separating column, which is obtained by stacking irradiation of molybdenum and technetium⁹⁹Mo and^99mtc, the separation column is made of a two-aqueous phase separation resin comprising a hydrophilic group and a hydrophobic matrix, wherein the hydrophilic group comprises one or more of polyethylene glycol with molecular weight of 500-20000 (e.g. polyethylene glycol with molecular weight of 500, polyethylene glycol with molecular weight of 5000, polyethylene glycol with molecular weight of 10000, polyethylene glycol with molecular weight of 20000, etc.) and polypropylene glycol with molecular weight of 400-10000 (e.g. polypropylene glycol with molecular weight of 400, polypropylene glycol with molecular weight of 3000, polypropylene glycol with molecular weight of 7000, polypropylene glycol with molecular weight of 10000, etc.); the hydrophobic matrix comprises one or more of chloromethyl polystyrene, polystyrene and graphene oxide.

A method for separating molybdenum and technetium, which is obtained by stacking molybdenum⁹⁹Mo and^99mtc, molybdenum can be molybdenum in various chemical forms, can be natural or highly enriched molybdenum, and the separation steps are as follows:

s1, dissolving molybdenum-technetium by using alkali liquor with hydroxide ion concentration of more than 0.5 mol/L;

the alkali solution may be any strong alkali such as sodium hydroxide, potassium hydroxide, etc., and the hydroxide ion concentration is preferably 2 to 5mol/L, for example, the hydroxide ion concentration may be 2mol/L, 3mol/L, 4mol/L, 5mol/L, etc.

S2, separating the molybdenum-technetium in the solution prepared in the step S1 by using the molybdenum-technetium separation column through a dynamic method or a static method;

the molybdenum-technetium separation column has high technetium adsorption efficiency, almost all technetium is adsorbed, molybdenum is hardly adsorbed, molybdenum flows out along with the solution, and the recovery rate of molybdenum is as high as more than 85%.

When the dynamic method is used, the solution obtained in the step S1 is passed through a molybdenum-technetium separation column at a flow rate of 0.01-10000 mL/min.

S3, leaching the molybdenum on the molybdenum-technetium separation column by using leacheate;

optionally, the leacheate is a hydroxide solution, and the molybdenum can be selectively eluted by gradient elution with the leacheate without eluting technetium, and specifically, the method comprises the following steps:

s3.1, leaching the molybdenum-technetium separation column by using hydroxide radical solution with the concentration of 0.5-10 mol/L;

s3.2, leaching the molybdenum-technetium separation column by using hydroxide radical solution with the concentration of 0.1-0.5 mol/L;

s4, eluting technetium on the molybdenum-technetium separation column by using an eluent;

the eluent is a solution of carbonate ions, bicarbonate ions and chloride ions in any proportion, and is 0.9 percent of sodium chloride solution for more convenient use in nuclear medicine labeling.

The method has at least the following advantages: firstly, the elution efficiency of technetium is stabilized to be more than 90 percent; ② the recovery rate of the raw material molybdenum is up to more than 85 percent; thirdly, 0.9 percent sodium chloride solution or deionized water is used as eluent, so that the method can be more conveniently used for nuclear medicine marking; organic solvent is not used in the whole process, and finally, the technetium solution has no organic matter residue, so that the method is more suitable for nuclear medicine diagnosis. The method is simple to operate, and the whole process only needs about 90 minutes.

The above description is only a preferred embodiment of the present application and is not intended to limit the present application, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, improvement and the like made within the spirit and principle of the present application shall be included in the protection scope of the present application.