WO2018028642A1

WO2018028642A1 - Medical iodine-131 carbon microsphere and method for fabrication thereof

Info

Publication number: WO2018028642A1
Application number: PCT/CN2017/096890
Authority: WO
Inventors: 李茂良; 蔡继鸣
Original assignee: 成都纽瑞特医疗科技有限公司
Priority date: 2016-08-11
Filing date: 2017-08-10
Publication date: 2018-02-15
Also published as: CN106178006A; CN106178006B

Abstract

Provided are a medical iodine-131 carbon microsphere and method for fabrication thereof, used for tumor radiotherapy or tumor early-imaging diagnosis. The medical iodine-131 carbon microsphere is formed by using a carbon microsphere to adsorb molecular iodine (I₂) generated by reacting a medical Na¹³¹I solution with oxidants such as hydrogen peroxide and then curing, or cured by using a AgNO₃ solution to process a carbon microsphere and then reacting with a medical Na¹³¹I solution to generate Ag¹³¹I and depositing same on the interior of the carbon microsphere.

Description

Medical iodine-131 carbon microsphere and preparation method thereof

Technical field

The invention relates to a tumor radiotherapy and tumor radiography diagnostic medicine and a preparation process thereof, in particular to a medical iodine-131 carbon microsphere and a preparation process thereof.

Background technique

Radioactive microspheres have a certain history as radiotherapy for tumors in the human body. The 钇-90 (90Y) glass microspheres have been approved by the US FDA for many years and are widely used in the United States, Canada, Europe and Asia. 钇-90(90Y) Resin microspheres have been approved for marketing in Australia [Bruno Sangro, Mercedes Inarrairaegui, Jose I. Bilbao. Radioembolization for hepatocellular carcinoma. Journal of Hepatology 2012; 56: 464-473], Phosphorus-32 (32P) glass microspheres have been developed in China. For many years, there have been many reports in clinical research [Zheng Guangyong, Wang Dazhang. A new anticancer therapy-radioactive glass microspheres through intra-arterial infusion irradiation therapy. Journal of Oral and Maxillofacial Surgery 1991;1(1):52- 55. Wang Dazhang, Sun Wenhao, et al. Experimental and clinical application of anti-cancer effect of phosphorus-32 glass microspheres. Chinese Journal of Stomatology 1991; 9(1): 7-10. Wang Dazhang, Li Maoliang, et al. Preliminary evaluation of the application of arterial infusion of phosphorus-32 glass microspheres in the treatment of oral cancer. West China Journal of Stomatology 1991; 9 (2): 138-141], has a significant effect on cancer such as liver cancer, and has received international recognition. The medical profession attaches great importance to it. However, both 钇-90 ( ⁹⁰ Y) glass microspheres and phosphorus-32 ( ³² P) glass microspheres must be placed in high-throughput nuclear reactors with neutron irradiation in non-radioactive strontium glass microspheres or phosphorus glass microspheres. Acquired, due to the limited number of high-throughput nuclear reactors in the world, the timely production of 钇-90 ( ⁹⁰ Y) glass microspheres and phosphorus-32 ( ³² P) glass microspheres was limited, which affected the promotion and application.钇-90 ( ⁹⁰ Y) resin microspheres are prepared by cation-removing microspheres adsorbed by 锶-90/钇-90 separation device and prepared by curing. Due to the limited exchange capacity of cationic resin, 钇- The specific activity of 90( ⁹⁰ Y) resin microspheres is relatively low, and the promotion and application are also limited. Therefore, it is very necessary to develop a new type of medical radioactive microsphere which is easier to prepare and more easily applied.

Iodine -131 ⁽¹³¹ I) is the most common diagnostic nuclear medicine, radionuclide therapy for hyperthyroidism, diagnosis and treatment of thyroid cancer. ¹³¹ I emits β-rays and γ-rays. After ¹³¹ I enters the living organism, external images distributed in the body can be observed by γ camera. Therefore, ¹³¹ I microspheres can be used for tumor radiotherapy embolization and the therapeutic effect can be evaluated. In addition, ¹³¹ I microspheres do not require neutron activation before use, which is convenient for clinical applications.

Summary of the invention

The object of the present invention is to provide a medical iodine-131 carbon microsphere with simple process, high nuclide adsorption rate and low release rate and a preparation process thereof.

In order to achieve the above object, the present invention adopts the following technical solutions:

Iodine-131 is the most commonly used diagnostic and therapeutic nuclides in nuclear medicine for the diagnosis and treatment of hyperthyroidism and nail cancer. The invention utilizes carbon microspheres as a carrier to adsorb or deposit ¹³¹ I nuclide in medical Na ¹³¹ I solution in carbon microspheres by oxidation reaction or precipitation reaction, and then solidified to prepare medical iodine-131 carbon. Microspheres. The adsorption efficiency of carbon microspheres for iodine-131 is higher than 99%. After curing, the iodine-131 release rate of medical iodine-131 carbon microspheres is less than 0.01%, which can be used for embolization and radiotherapy of solid tumors containing blood vessels such as liver cancer. By dissolving the injection of radiation to treat other solid tumors, or for lymphatic cancer treatment and lymphatic metastasis treatment or lymphoma imaging, medical iodine-131 carbon microspheres containing certain tumor-like functional groups can also be used for other solid tumor treatment or diagnosis.

Specifically:

A medical iodine-131 carbon microsphere consisting of carbon microspheres and a radionuclide ¹³¹ I adsorbed or deposited in carbon microspheres.

The medical iodine-131 carbon microspheres are prepared by the following method: after the oxidation of the medical Na ¹³¹ I solution, the radionuclide ¹³¹ I is adsorbed or deposited in the carbon microspheres, and then solidified.

The oxidation reaction is a reaction of a medical Na ¹³¹ I solution with an oxidant to form molecular iodine.

Further, the oxidation reaction is to soak the carbon microspheres with a medical Na ¹³¹ I solution having a radioactivity of 0.185-11.1 GBq (5-300 mCi), and adjust the pH of the solution to 1-2 with a dilute nitric acid solution, and then add the oxidizing agent solution. The carbon microsphere mixture was prepared by shaking at 40-50 ° C for 40-60 minutes.

Further, it is also required to cure the carbon microsphere mixture: the AgNO ₃ solution is used to precipitate a small amount of negative iodide ions which are not precipitated and solidified in the solidified carbon microspheres and remove residual negative iodide ions in the solution. The carbon microspheres were soaked in physiological saline to convert the excess Ag ⁺ ions in the carbon microspheres into AgCl precipitates and solidified in the carbon microspheres, and the residual Ag ⁺ ions in the solution were changed into AgCl precipitates to be removed. The specific method is:

After the carbon microsphere mixture is separated by solid-liquid separation, the ¹³¹ I carbon microspheres are soaked with Ag(NO ₃ ) solution, shaken for 10-30 minutes, and then separated by HNO ₃ solution after repeated solid-liquid separation. After the solid-liquid separation, the Ag ⁺ ions in the solution are removed, and then immersed in medical physiological saline, and after solid-liquid separation, medical iodine-131 carbon microspheres are obtained.

The oxidizing agent is selected from one of hydrogen peroxide, potassium iodate, potassium dichromate, and potassium permanganate.

Further, the oxidizing agent is hydrogen peroxide.

The medical iodine-131 carbon microspheres can also be prepared by the following method: after the precipitation of the medical Na ¹³¹ I solution, the radionuclide ¹³¹ I is deposited in the carbon microspheres and then solidified.

The precipitation reaction is a reaction between ¹³¹ I ^- ions and Ag ⁺ ions in carbon microspheres to form a silver iodide precipitate.

Further, the precipitation reaction is:

(1) soaking carbon microspheres with HNO ₃ solution for 10 minutes, after solid-liquid separation, the carbon microspheres have a pH of 1-2;

(2) soak the carbon microspheres with AgNO ₃ solution, shake at 40-50 ° C for 40-60 minutes, adsorb Ag ⁺ ions in the carbon microspheres, and then separate the solid and liquid;

(3) soaking and cleaning the carbon microspheres with HNO ₃ solution, after solid-liquid separation, repeatedly washing, then immersing and cleaning the carbon microspheres with purified water, and separating and removing the Ag ⁺ ions not adsorbed by the carbon microspheres after solid-liquid separation. ;

(4) Add a medical Na ¹³¹ I solution with a radioactivity of 0.185-11.1 GBq (5-300 mCi) to the cleaned carbon microspheres, and vortex at 40-50 ° C for 40-60 minutes to form Ag ¹³¹ inside the carbon microspheres. I precipitates, so that ¹³¹ I ^- ions are solidified in the carbon microspheres, and then solid-liquid separation;

(5) and then soaked in physiological saline carbon microspheres that are not adsorbed carbon microballoons I ^- fully cured ions Ag ⁺ ions and Cl ^- ions generated AgCl precipitation, solid-liquid separation again, iodine-131 to obtain a medical Carbon microspheres.

The 2-3 mL medical Na ¹³¹ I solution contained 10-20 mg of the NaI carrier.

The medical Na ¹³¹ I solution has a nuclear purity of ¹³¹ I of not less than 99.9%, a radiochemical purity of not less than 95%, and a concentration of radioactivity per ml of not less than 185 MBq.

When the purity of the carbon microspheres is insufficient, the carbon microspheres need to be further purified. Specifically, the carbon microspheres are soaked with ethyl acetate, acetone or ethanol to remove the fat, and the sodium hydroxide solution is used to soak the alkali-soluble impurities. Rinse thoroughly with purified water until weakly alkaline, then soak the acid-soluble impurities with nitric acid, and rinse with purified water until the pH is 1-2.

The carbon microspheres used in the present invention refer to microspheres prepared by carbon-rich organic materials (such as artificial organic polymers, natural organic materials such as sucrose, and carbonaceous materials such as asphalt), which are carbonized at a high temperature, and then degreased and alkali washed. Pickling and other impurities are removed by pickling, and spherical particles which are non-toxic and biocompatible are prepared.

Self-made or commercially available carbon microspheres should meet the quality standards of carbon microspheres for their respective applications. First, the biocompatibility of carbon microspheres must meet the requirements of in vivo and intravascular administration. The size and particle size distribution of microspheres should be consistent with Requirements for use, in addition to meet the purity requirements, meet the requirements of bacterial and endotoxin content restrictions, specific requirements see relevant quality standards.

In the present invention, the particle size of the carbon microspheres for treating tumors is determined according to the use: the medical iodine-131 carbon microspheres having a particle diameter of 20-30 μm are mainly used for arterial perfusion embolization and radiotherapy for liver cancer, and the particle diameter of 30 μm-100 μm can be used. Blood vessel-rich tumors such as lung cancer, kidney cancer, tongue cancer, breast cancer, and cervical cancer can also be used for direct dispersion injection into other tumors; radioactive implantation therapy for tumors with a particle size of 100 μm or more; particle size of 100 -150nm medical iodine-131 carbon microspheres are mainly used for the treatment of lymphoma. The medical iodine-131 carbon microspheres with a particle size of 10-100nm have tumor-like properties and can be used for tumor targeted therapy.

The carbon microspheres have a diameter of 20-30 μm.

The carbon microspheres have a diameter of 30 to 100 μm.

The carbon microspheres have a diameter greater than 100 μm.

The carbon microspheres have a diameter of 10 to 100 nm.

The carbon microspheres have a diameter of 100 to 150 nm.

The adsorption rate of the ¹³¹ I nuclide by the carbon microspheres in the medical iodine-131 carbon microspheres is higher than 99%.

The release rate of ¹³¹ I nuclide in the medical iodine-131 carbon microspheres is less than 0.01%.

The medical iodine-131 carbon microspheres have an Ag ⁺ ion concentration of less than 20 ng/L in their suspension (eg, physiological saline).

A preparation for use in in vivo tumor radiotherapy or early tumor imaging diagnosis prepared from the medical iodine-131 carbon microspheres.

The radioactivity of iodine-131 in the preparation for tumor treatment is 1.85-11.1 GBq (50-300 mCi), and the particle size of the carbon microspheres depends on the use.

The medical iodine-131 carbon microspheres in the preparation for early diagnosis of tumor imaging have a radioactivity of 0.185-0.37 GBq (5-10 mCi), and the particle size of the carbon microspheres depends on the use.

Use of the medical iodine-131 carbon microspheres for the treatment of a medicament for a mammal having a medical condition, wherein the medical iodine-131 carbon microspheres are administered by an interventional catheter, a syringe or an in vivo implantation.

The beneficial effects of the invention are:

1. The method is simple, the introduction of impurities is small, and the product purity is high.

2. The high utilization rate of iodine-131 produces less radioactive waste and is conducive to environmental protection.

3. The release rate of iodine-131 is low and the safety is good.

4. The radioactivity of medical iodine-131 carbon microspheres can be adjusted according to individual needs, and can meet the individualized precise treatment requirements at any time.

5. Iodine-131 is easily obtained from multiple sources. The normal production of medical iodine-131 carbon microspheres is not affected by the supply of raw materials, and can meet the annual production and supply requirements.

6. Medical iodine-131 carbon microspheres have low production cost and good curative effect, and are convenient for popularization and application.

detailed description

Chemical Oxidation Adsorption: The negative iodine ions ( ¹³¹ I ^- and I ^- ) in Na ¹³¹ I solution are oxidized to iodine molecules ( ¹³¹ I ₂ and I ₂ ) by a suitable oxidizing agent, which is then adsorbed by carbon microspheres, solid-liquid separation After centrifugation or filtration, the carbon microspheres are soaked with AgNO ₃ solution, and the negative iodide ions ( ¹³¹ I ^- and I ^- ) which have not been completely oxidized in the carbon microspheres are reacted with Ag ⁺ ions to form silver iodide (Ag ¹³¹ I and AgI) is precipitated and solidified in medical carbon microspheres; after solid-liquid separation, a small amount of negative iodide ions ( ¹³¹ I ^- and I ^- ) in the solution that have not been completely oxidized are reacted with Ag ⁺ ions to form silver iodide (Ag ¹³¹ I And AgI) precipitate removal, and then soak the carbon microspheres with physiological saline to change the excess Ag ⁺ ions in the carbon microspheres into AgCl precipitates and solidify in the carbon microspheres, and the residual Ag ⁺ ions in the solution become AgCl precipitates. It was removed to prepare the desired iodine-131 carbon microspheres.

as well as

Chemical precipitation method: using the principle of very low solubility of AgI, the ¹³¹ I ^- ions in the Na ¹³¹ I solution and the Ag ⁺ ions in the AgNO ₃ solution form a very low solubility Ag ¹³¹ I precipitate in the carbon microspheres, thereby ¹³¹ I ^- ions are solidified in carbon microspheres.

Example 1

(1) Purification of carbon microspheres: soaking the fat with an organic solvent such as ethyl acetate, acetone or ethanol; soaking the alkali-soluble impurities with a dilute sodium hydroxide solution (0.1-0.5 mol/L), and then repeatedly washing to a weak base (pH 8-10); then dilute the acid-soluble impurities with dilute nitric acid (0.1mol/L-0.5mol/L) and wash to a pH of 1-2.

(2) Soaking 1-3 g of the purified carbon microspheres with 5 mL of HNO ₃ solution having a pH of 1, and separating the solid carbon particles (centrifugation or filtration) to make the soaked carbon microspheres have a pH of 1-2.

(3) Add 1-2 mL of Na ¹³¹ I solution (containing 10-20 mg of I ^- ion carrier) containing the required activity (such as 0.185-11.1 GBq (5-300 mCi)), and add HNO ₃ solution with pH 1 Soak 1-3 g of carbon microspheres to 8 mL.

(4) Add 2 mL (concentration of 30% (mL/mL)) H ₂ O ₂ solution, shake at 45 ° C for 50 minutes, oxidize negative iodide ions (including ¹³¹ I ^- ions and non-radioactive I ^- ions) into iodine The molecule (H ₂ O ₂ +2H ⁺ +2I ^- =I ₂ +2H ₂ O) is adsorbed by medical carbon microspheres (the adsorption efficiency of ¹³¹ I is higher than 99%), after solid-liquid separation (centrifugation or filtration), The curing treatment is carried out: a small amount of negative iodide ions which are not precipitated and solidified in the solidified carbon microspheres are precipitated by the AgNO ₃ solution, and residual negative iodide ions in the solution are removed. The carbon microspheres were soaked in physiological saline to convert the excess Ag ⁺ ions in the carbon microspheres into AgCl precipitates and solidified in the carbon microspheres, and the residual Ag ⁺ ions in the solution were changed into AgCl precipitates to be removed. The specific method is:

1 Soak the medical carbon microspheres with iodine-131 nuclide (including stable carrier iodine) in 10 mL of 12 mg/mL AgNO ₃ solution, and fluorinate for 20 minutes at 45 ° C to form silver iodide precipitated solid negative iodide ions inside the medical carbon microspheres. Precipitation removes residual negative iodide ions from the solution and separates them by solid-liquid separation (centrifugation or filtration).

2 The medical carbon microspheres were immersed in a 10 mL solution of 0.1 mol/L HNO ₃ solution, and after solid-liquid separation (centrifugation or filtration), excess Ag ⁺ ions were removed and repeatedly immersed and washed.

3 After soaking the carbon microspheres with 10 mL of physiological saline, the Ag ⁺ ions adsorbed by the carbon microspheres and not completely solidified by I ^- ions and the Ag ^- ions formed by the Cl ^- ions are precipitated and solidified in the carbon microspheres, and the residual Ag ^{+ in the} solution The ions and Cl ^- ions form AgCl precipitate, and after solid-liquid separation (centrifugation or filtration), the residual Ag ⁺ ions are removed, and the I-131 release rate of the cured medical iodine-131 carbon microspheres is less than 0.01%, physiological The concentration of Ag ⁺ ions in the saline suspension is less than 20 ng/L, thereby obtaining the medical iodine-131 carbon microspheres having the purity requirements and safety required for the administration in human body.

The medical iodine-131 carbon microspheres prepared by the above process are autoclaved and sterilized in an autoclave for 20 minutes, and the prepared medical iodine-131 carbon microspheres meet the requirements of sterility and endotoxin limit, and can be used for intratumoral radiotherapy or tumor. Radiographic imaging.

Example 2

(1) 1-3 g of carbon microspheres were treated in the same manner as in the steps (1) and (2) in Example 1, so that the carbon microspheres had a pH of 1-2.

(2) Add 1-2 mL of the desired activity (for example, 0.185-11.1 GBq (5-300 mCi) of Na ¹³¹ I solution (containing 10 to 20 mg of I ^- ionophore).

(3) Add 2 mL of 0.10 mol/L KIO ₃ solution and shake at 45 ° C for 50 minutes to oxidize negative iodide ions (including ¹³¹ I ^- ions and non-radioactive I ^- ions) into iodine molecules.

While being adsorbed by medical carbon microspheres (the adsorption efficiency of ¹³¹ I is higher than 99%), after solid-liquid separation (centrifugation or filtration), the oxidized adsorption iodine is treated according to the curing treatment method in the step (4) in the first embodiment. After the medical iodine-131 carbon microspheres, the release rate of iodine-131 is less than 0.01%, and the Ag ⁺ ion concentration is lower than 20 ng/L, thereby obtaining the purity requirement and safety of the medical iodine-131 required for human administration. Carbon microspheres.

Example 3

(2) Add 1-2 mL of the desired activity (for example, 0.185-11.1 GBq (5 mCi-300 mCi) of Na ¹³¹ I solution (containing 10 to 20 mg of I ^- ionophore).

(3) Adding 0.10 mol/L KMnO ₄ solution is preferably 2 mL, and then adding 25% H ₂ SO ₄ 2.0 mL to control the acidity of the reaction liquid. Oxidation of negative iodide ions (including ¹³¹ I ^- ions and non-radioactive I ^- ions) to iodine molecules by shaking at 45 ° C for 50 minutes

Example 4

(2) adding the required radioactivity [e.g. 0.185-11.1GBq (5-300mCi)] of Na ¹³¹ I solution (containing I ^- ionophore 10-20mg) 1-2mL. An additional 20% H ₂ SO ₄ 2.0 mL was added to control the acidity of the reaction solution.

(3) Add ₂ mL of 0.10 mol/L K ₂ Cr ₂ O ₇ solution, shake at 45 ° C for 50 minutes, and oxidize negative iodide ions (including ¹³¹ I ^- ions and non-radioactive I ^- ions) into iodine molecules (Cr ₂ 0 ₇ ^2- +6 I ^- +14 H ⁺ =2 Cr ³⁺ +3 I ₂ +7 H ₂ O) is adsorbed by medical carbon microspheres (adsorption efficiency of ¹³¹ I is higher than 99%), solid-liquid separation (centrifugation) Or after filtration, the medical iodine-131 carbon microspheres after oxidative adsorption of iodine are treated according to the curing treatment method in the step (4) in the embodiment 1, and the release rate of the iodine-131 is less than 0.01%, and the Ag ⁺ ion The concentration is less than 20 ng/L, thereby obtaining the medical iodine-131 carbon microspheres having the purity requirement and safety required for administration in human body.

Example 5

Using the principle of very low solubility of AgI, the ¹³¹ I ^- ions in the Na ¹³¹ I solution and the Ag ⁺ ions in the AgNO ₃ solution form a very low solubility silver iodide precipitate in the carbon microspheres, thereby solidifying the ¹³¹ I ^- ions. Medical carbon microspheres. The specific preparation method is as follows:

(1) Immerse 1-3 g of medical carbon microspheres with 10 mL of a 0.1 mol/L HNO ₃ solution for 10 minutes, and then solid-liquid separation (centrifugation or filtration) to make the medical carbon microspheres have a pH of 1-2.

(2) Soak the medical carbon microspheres with 10 mL of 12 mg/mL AgNO ₃ solution, shake at 45 ° C for 50 minutes, and then separate the solid and liquid (centrifugation or filtration).

(3) Soak the carbon microspheres with 10mL of 0.1mol/L HNO ₃ solution, solid-liquid separation (centrifugation or filtration), repeat the cleaning, then rinse the medical carbon microspheres with ultrapure water, solid-liquid separation (centrifugation or After filtration, the Ag ⁺ ions not adsorbed by the carbon microspheres are removed by washing.

(4) Add 10 mL of the required radioactivity [such as 0.185-11.1 GBq (5-300 mCi)] of Na ¹³¹ I solution (containing 10-20 mg of I ^- ion carrier) to the cleaned carbon microspheres at 45 ° C. After shaking for 50 minutes, a silver iodide precipitate was formed inside the carbon microspheres, so that ¹³¹ I ^- ions were solidified in the carbon microspheres, and then solid-liquid separation (centrifugation or filtration).

(5) saline and then soaked in 10mL of carbon microspheres medical without being adsorbed carbon microspheres I ^- fully cured ions Ag ⁺ ions and Cl ^- ion AgCl precipitate formed, such as a medical preparation 131I carbon microspheres The iodine-131 release rate is extremely low (less than 0.01%), and the Ag ⁺ ion concentration is lower than 20 ng/L, ensuring the purity and safety of the prepared medical iodine-131 carbon microspheres.

Claims

A medical iodine-131 carbon microsphere, characterized in that the medical iodine-131 carbon microsphere is composed of carbon microspheres and a radionuclide 131 I adsorbed or deposited in carbon microspheres.
The medical iodine-131 carbon microsphere according to claim 1, wherein the medical iodine-131 carbon microsphere is obtained by the following method: the medical Na 131 I solution is adsorbed by the radionuclide 131 I after oxidation reaction It is prepared by curing in carbon microspheres.
The medical iodine-131 carbon microsphere according to claim 2, wherein the oxidation reaction is a reaction of a medical Na 131 I solution with an oxidant to form molecular iodine.
The medical iodine-131 carbon microsphere according to claim 3, wherein the oxidation reaction is to soak carbon microspheres with a medical Na 131 I solution having a radioactivity of 0.185-11.1 GBq (5-300 mCi), and use a thinner The nitric acid solution adjusts the pH of the solution to 1-2, and then adds the oxidizing agent solution, and shakes at 40-50 ° C for 40-60 minutes to prepare a carbon microsphere mixture.
The medical iodine-131 carbon microsphere according to claim 4, wherein the carbon microsphere mixture is further cured: the carbon microsphere mixture is separated by solid-liquid separation, and then immersed in an Ag(NO 3 ) solution. 131 I carbon microspheres have been adsorbed and shaken for 10-30 minutes. After solid-liquid separation, the HNO 3 solution is repeatedly washed. After solid-liquid separation, the Ag + ions in the solution are removed, and then soaked with medical saline. After solid-liquid separation, medical iodine-131 carbon microspheres were prepared.
The medical iodine-131 carbon microsphere according to claim 4, wherein the oxidizing agent is one selected from the group consisting of hydrogen peroxide, potassium iodate, potassium dichromate, and potassium permanganate.
The medical iodine-131 carbon microsphere according to claim 6, wherein the oxidizing agent is hydrogen peroxide.
The medical iodine-131 carbon microsphere according to claim 1, wherein the medical iodine-131 carbon microsphere is prepared by the following method: a medical Na 131 I solution is deposited by a precipitation reaction to deposit a radionuclide 131 I It is prepared by curing in carbon microspheres.
The medical iodine-131 carbon microsphere according to claim 8, wherein the precipitation reaction is a reaction of 131 I - ions and Ag + ions in carbon microspheres to form an Ag 131 I precipitate.
The medical iodine-131 carbon microsphere according to claim 9, wherein the precipitation reaction is:

(1) soaking carbon microspheres with HNO 3 solution for 10 minutes, after solid-liquid separation, the carbon microspheres have a pH of 1-2;

(2) soaking the carbon microspheres with AgNO 3 solution, shaking at 40-50 ° C for 40-60 minutes, adsorbing Ag + ions in the carbon microspheres, and separating the solid and liquid again;

(3) soaking and cleaning the carbon microspheres with HNO 3 solution, after solid-liquid separation, repeatedly washing, then immersing and cleaning the carbon microspheres with purified water, and separating and removing the Ag + ions not adsorbed by the carbon microspheres after solid-liquid separation. ;

(4) Add a medical Na 131 I solution with a radioactivity of 0.185-11.1 GBq (5-300 mCi) to the cleaned carbon microspheres, and vortex at 40-50 ° C for 40-60 minutes to form Ag 131 inside the carbon microspheres. I precipitates, so that 131 I - ions are solidified in the carbon microspheres, and then solid-liquid separation;

(5) and then soaked in physiological saline carbon microspheres that are not adsorbed carbon microballoons I - fully cured ions Ag + ions and Cl - ions generated AgCl precipitation, solid-liquid separation again, iodine-131 to obtain a medical Carbon microspheres.
The medical iodine-131 carbon microsphere according to any one of claims 2, 3, 4, 8, or 10, wherein the 2-3 mL medical Na 131 I solution contains 10-20 mg of a NaI carrier.
The medical iodine-131 carbon microsphere according to any one of claims 2, 3, 4, 8, or 10, wherein the medical Na 131 I solution has a nuclear purity of 131 I of not less than 99.9%, and radiochemistry The purity is not less than 95%, and the concentration of radioactivity per ml is not less than 185 MBq.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 10, wherein the preparation method of the medical iodine-131 carbon microsphere further comprises a purification process of carbon microspheres, specifically: carbon The microspheres are soaked with ethyl acetate, acetone or ethanol to remove the fat, soaked with sodium hydroxide solution to remove alkali-soluble impurities, and repeatedly washed with purified water to weakly alkaline, then soaked with acid nitrate to remove acid-soluble impurities, and washed with purified water to pH. The value is 1-2 and is reserved.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 10, wherein the carbon microsphere refers to a microsphere prepared by carbon-rich organic material, which is carbonized at a high temperature, and then degreased and alkali. Washing, pickling, etc. to remove various impurities, to prepare spherical particles that are non-toxic and biocompatible to the human body.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 10, wherein the carbon microspheres have a diameter of 20 to 30 μm.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 10, wherein the carbon microspheres have a diameter of 30 to 100 μm.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 10, wherein the carbon microspheres have a diameter of more than 100 μm.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 10, wherein the carbon microspheres have a diameter of 10 to 100 nm.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 10, wherein the carbon microspheres have a diameter of 100 to 150 nm.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 19, wherein the adsorption rate of the 131 I nuclide by the carbon microspheres in the medical iodine-131 carbon microsphere is higher than 99%.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 19, wherein the 131 I nuclides release rate of the medical iodine-131 carbon microspheres is less than 0.01%.
The medical iodine-131 carbon microsphere according to any one of claims 1 to 19, wherein the medical iodine-131 carbon microsphere has an Ag + ion concentration of less than 20 ng/L in its suspension.
A preparation for use in in vivo tumor radiotherapy or early tumor imaging diagnosis, prepared by the medical iodine-131 carbon microsphere of any one of claims 1-19.
The preparation for use in in vivo tumor radiotherapy or early tumor imaging diagnosis according to claim 23, wherein the activity of iodine-131 in the preparation for tumor treatment is 1.85-11.1 GBq (50-300 mCi) The size of the carbon microspheres depends on the application.
The preparation for use in in vivo tumor radiotherapy or early tumor imaging diagnosis according to claim 23, wherein the medical iodine-131 carbon microsphere has a radioactivity of 0.185 in a preparation for early diagnosis of tumor imaging. -0.37 GBq (5-10 mCi), the particle size of the carbon microspheres depends on the application.
Use of the medical iodine-131 carbon microsphere of any of claims 1-19 for the treatment of a medicament for a mammal having a medical condition.
The use of claim 26, wherein said medical iodine-131 carbon microspheres are administered by means of an interventional catheter, syringe or in vivo implantation.