CN106540282B - A kind of preparation method of -103 sealed seed source source core of palladium - Google Patents

A kind of preparation method of -103 sealed seed source source core of palladium Download PDF

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CN106540282B
CN106540282B CN201510591213.0A CN201510591213A CN106540282B CN 106540282 B CN106540282 B CN 106540282B CN 201510591213 A CN201510591213 A CN 201510591213A CN 106540282 B CN106540282 B CN 106540282B
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palladium
sealed seed
source
preparation
seed source
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CN106540282A (en
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阎尔坤
白红升
张兴福
朱辉
李佳
崔贝
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TIANJIN SAIDE BIOLOGICAL PHARMACEUTICAL CO Ltd
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TIANJIN SAIDE BIOLOGICAL PHARMACEUTICAL CO Ltd
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Abstract

The invention discloses a kind of preparation methods of -103 sealed seed source source core of palladium, it is made of following steps: in reaction vessel, it is put into 100 silver-colored sticks in proportion, saline citrate, soluble palladium saline solution and sodium hydrate aqueous solution, mixing is added, reaction, then -103 aqueous solution of radioactivity palladium chloride and aqueous thiosulfate is added, supernatant is abandoned in the oscillating reactions under pH=6~11, it is cleaned with acetone, deionized water or ethyl alcohol to get -103 sealed seed source source core of palladium is arrived.Method reaction system of the invention is stablized, -103 sealed seed source source core dose uniformity of palladium of preparation, securely and fine and close, palladium -103 utilization rate height.Reaction time is short, and whole preparation process at most needs 60min, and one-step method is completed at room temperature, and operational sequence is simple and easy to control, improves production efficiency, reduces labor intensity and dose of radiation.Used chemical reagent is conventional commercial, and nontoxic, cheap, production cost is low.

Description

A kind of preparation method of -103 sealed seed source source core of palladium
Technical field
The invention belongs to the medicinal preparation technical fields containing radioactive substance, specifically it is close to be related to a kind of palladium -103 Seal the preparation method of seed core in a steady stream.
Background technique
Radioactive particle Implantation in Treating tumour be by art or using implanting device percutaneous puncture by radioactivity grain Around sub (radioactive sealed seed source) implantation tumour or tumour, the low-energyγ-ray or X-ray released using radionuclide Tumour cell is killed, achieve the purpose that treatment and alleviates disease.The technology is adapted to the implanted treatment of various entity tumors, as before Column gland cancer, breast cancer, liver cancer, incidence tumor, cancer of pancreas and oophoroma etc. achieve identical as surgical operation, fluconazole ear drops Therapeutic effect, there is Small side effects, recurrence rate are low and wound is small etc..The most common radioactive particle of the technology is iodo- at present - 103 sealed seed source of 125 sealed seed sources and palladium, wherein iodine-125 sealed seed source is suitable for growing slow tumor implantation therapy;Palladium- 103 sealed seed sources are suitable for growing fast tumor implantation therapy.
Compared with other radionuclides, radionuclide palladium -103 have good nulcear properties, palladium [103Pd] do not have and waves Hair property, therefore can effectively avoid the pollution to operating environment around and personnel;Secondly, palladium [103Pd] energy is low, and only 21 The characteristic X-ray of~23KeV, easily shields, and the lead of 0.06 millimeters thick is being organized it is prevented that 97% or more ray passes through In partly subtract layer be 1 centimetre, therefore protect it is more convenient, exposure dose suffered by normal tissue and surrounding population is small;Third, palladium [103Pd] half-life short, 16.96 days half-life period can make the predose of implantation high, and doses remaining is small, for inhibiting quick The tumour of growth has good therapeutic effect.
- 103 sealed seed source of palladium is support rod (also referred to as -103 source core of radioactivity palladium) the loading titanium tube that will be adsorbed with palladium -103 Or in stainless steel tube, sealing both ends and it is manufactured.
Be used to prepare -103 sealed seed source of palladium support rod be resin microsphere, ceramic rod or microballoon, inorganic adsorbent microballoon and Metal bar (gold, silver, copper etc.) generally selects support rod of the silver as fixed palladium -103, since the ductility of metallic silver is easy to add Work, price is low, and is the marker of x-ray, convenient for -103 sealed seed source of palladium is accurately positioned and is controlled when implanted treatment Treat the estimation of dosage.Different tumor implantation therapies are used for according to -103 sealed seed source of palladium, the length of silver-colored stick to be 3.0mm, and diameter is 0.1~0.7mm of Φ, the technology (also referred to as -103 source core technology of preparing of palladium) that radionuclide palladium -103 is fixed on silver-colored stick is palladium -103 The key technology of sealed seed source manufacture, usually there is absorption method, galvanoplastic and electroless plating method.Compared with other two kinds, chemical plating tool Have that process flow is simple, palladium -103 utilization rate is high, equipment easily obtains, preparation process has controlled and easy large-scale production.Such as United States Patent (USP) US4702228 discloses a kind of absorption method, for Adsorption of Radioactive palladium -103 such as aluminum oxide micro-spheres, after absorption Two microballoons are packed into titanium tube, silver-colored stick are placed between two microballoons as x-ray marker, the palladium -103 of this method preparation seals seed The active region in source is at the both ends of sealed seed source, it is difficult to ensure that dosage distributing homogeneity, process is not easy to control, while increasing palladium -103 The difficulty of sealed seed source assembling, is not easy large-scale production, while dosage distribution changes because of two moving for microballoon, to facing Bed therapeutic effect generation does not utilize influence, is difficult to realize the accurate treatment of tumour.Chinese patent Zl01105243.0 discloses one Kind electroless plating method, with palladium chloride, ammonium chloride, ammonium hydroxide and sodium hypophosphite for main plating solution composition, reaction 1 is small at pH=10 and 35 DEG C When, so that silver-colored stick surface is covered upper one layer of palladium -103, obtains -103 source core of palladium.This method is using ammonium chloride as stabilizer, but chlorine Reaction rate can be reduced while stablizing plating solution by changing ammonium, and in addition the concentration of required reducing agent sodium hypophosphite is higher, be unfavorable for The stability of plating solution.In another example Chinese patent ZL101880873A discloses a kind of two-step method electroless plating method, the stick activation of (1) silver: First silver-colored stick is impregnated in palladium chloride aqueous solution, taking-up washes with water, and then impregnates, washes with water in the alkaline ammonium hydroxide of hydrazine; (2) the silver-colored stick after activation -103 chemical plating of palladium: is placed in the mixed of palladium chloride, sodium ethylene diamine tetracetate, ammonium hydroxide and hydrazine composition It closes in solution, 30~90min is stirred to react under condition of water bath heating, that is, is prepared into -103 source core of palladium.This method reaction system phase It is complicated for operation to stabilization, it needs to heat, there is ammonia release in reaction process.
Summary of the invention
The purpose of the present invention is overcome the deficiencies of the prior art and provide a kind of at low cost, easily-controllable, quick, easy palladium- The preparation method of 103 sealed seed source source cores.
Technical solution of the present invention is summarized as follows:
A kind of preparation method of -103 sealed seed source source core of palladium, is made of following steps:
In reaction vessel, it is put into the silver-colored stick that 100 diameters are 0.1~0.7mm, length is 2.0~3.5mm in proportion, The saline citrate that 0.01~2mL concentration is 0.01~2mol/L is added, 0.1~2mL concentration is 0.003~0.06mol/ L soluble palladium saline solution and 0.01~1mL concentration are 0.02~2mol/L sodium hydrate aqueous solution, and mixing reacts 1~5 point Clock, then addition 0.1~1mL concentration is -103 aqueous solution of 100-1000mCi/mL radioactivity palladium chloride and 0.1~2mL concentration is 0.05mol/L~1.0mol/L aqueous thiosulfate, 20~60min of oscillating reactions under pH=6~11 abandon supernatant, use Acetone, deionized water or ethyl alcohol clean 2~4 times to get -103 sealed seed source source core of palladium is arrived.
Citrate optimization citric acid sodium or potassium citrate.
The preferred palladium bromide of soluble palladium salt, fluorination palladium or palladium chloride.
The preferred sodium thiosulfate of thiosulfate or potassium thiosulfate.
Advantages of the present invention:
1. the soluble palladium saline solution that method of the invention uses, saline citrate, sodium hydrate aqueous solution and The reaction system of aqueous thiosulfate composition, reaction system are stablized, -103 sealed seed source source core dose uniformity of palladium of preparation, Securely and fine and close, -103 utilization rate of palladium is high.
2. the method reaction time of the invention is short, whole preparation process at most needs 60min, at room temperature one-step method It completes, operational sequence is simple and easy to control, substantially increases production efficiency, reduces the labor intensity and dose of radiation of staff.
3. chemical reagent used in method of the invention is conventional commercial reagent, conveniently, price is just for nontoxic, buying Preferably, production cost is low.
Detailed description of the invention
Fig. 1 is -103 sealed seed source structural schematic diagram of palladium.
1 is titanium tube in figure, and 2 be -103 sealed seed source source core of palladium.
Specific embodiment
Below with reference to specific implementation, the present invention is further illustrated.
Chemical reagent used in all embodiments is that analysis is pure.
Embodiment 1
A kind of preparation method of -103 sealed seed source source core of palladium, is made of following steps:
100 silver-colored sticks (0.3 × 3mm of Φ) are packed into the reaction flask of 15mL, 0.2mL 0.1mol/L sodium citrate water is added 2min is reacted in solution, 0.3mL0.02mol/L palladium chloride aqueous solution and 0.5mL0.04mol/L sodium hydrate aqueous solution, mixing, - 103 aqueous solution of 1mL 100mCi/mL radioactivity palladium chloride and 0.1mL 1.0mol/L sodium thiosulfate solution are added, is adjusted PH=10 is saved, oscillating reactions 30 minutes, supernatant is abandoned, is cleaned 3 times with deionized water, is dried to get -103 sealed seed source source of palladium is arrived Core.Then the source core made is packed into the titanium tube of Φ 0.5mm, with laser welder sealing, sees Fig. 1.
The activity of palladium -103 is 0.4mCi in solution after reaction, and the utilization rate of palladium -103 is 99.6%, -103 source core of palladium Mean radio activity is 0.730mCi.
The utilization rate of palladium -103=[(activity of palladium -103 in solution after activity-reaction of investment palladium -103) ÷ investment The activity of palladium -103] × 100%.
Embodiment 2
A kind of preparation method of -103 sealed seed source source core of palladium, is made of following steps:
100 silver-colored sticks (0.5 × 3mm of Φ) are packed into the reaction flask of 15mL, it is water-soluble that 0.01mL 2mol/L sodium citrate is added 1min is reacted in liquid, 0.1mL 0.06mol/L palladium chloride aqueous solution and 0.01mL 2mol/L sodium hydrate aqueous solution, mixing, then - 103 aqueous solution of 0.1mL 1000mCi/mL radioactivity palladium chloride and 0.1mL 1.0mol/L sodium thiosulfate solution is added, adjusts PH=6 is saved, oscillating reactions 60 minutes, supernatant is abandoned, is cleaned 2 times with acetone, is dried to get -103 sealed seed source source core of palladium is arrived.So The source core made is packed into afterwards in the titanium tube of Φ 0.8mm, with laser welder sealing.
The activity of palladium -103 is 0.75mCi in solution after reaction, and the utilization rate of palladium -103 is 99.25%, -103 source core of palladium Mean radio activity be 0.65mCi.
Embodiment 3
A kind of preparation method of -103 sealed seed source source core of palladium, is made of following steps:
100 silver-colored sticks (0.7 × 2mm of Φ) are packed into the rectangular quartzy bottle of 15mL, 2mL 0.01mol/L potassium citrate is added 5min is reacted in aqueous solution, 2mL0.003mol/L palladium chloride aqueous solution and 1mL 0.02mol/L sodium hydrate aqueous solution, mixing, - 103 aqueous solution of 1mL 180mCi/mL radioactivity palladium chloride and 2mL 0.05mol/L thiosulfuric acid aqueous solutions of potassium are added, is adjusted PH=11 oscillating reactions 40 minutes, abandons supernatant, is cleaned 2 times with ethyl alcohol, dries to get -103 sealed seed source source core of palladium is arrived.Then The source core made is packed into the titanium tube of Φ 1.0mm, with laser welder sealing.
The activity of palladium -103 is 0.70mCi in solution after reaction, and the utilization rate of palladium -103 is 99.61%, -103 source core of palladium Mean radio activity be 1.05mCi.
Embodiment 4
A kind of preparation method of -103 sealed seed source source core of palladium, is made of following steps:
100 silver-colored sticks (0.1 × 3.5mm of Φ) are packed into the rectangular quartzy bottle of 15mL, 0.4mL 0.05mol/L lemon is added Sour aqueous solutions of potassium, 0.4mL0.015mol/L fluorination aqueous palladium and 0.4mL 0.05mol/L sodium hydrate aqueous solution, mixing, instead 4min is answered, -103 aqueous solution of 0.5mL 200mCi/mL radioactivity palladium chloride and 0.4mL 0.25mol/L potassium thiosulfate are added Aqueous solution adjusts pH=11, oscillating reactions 20 minutes, abandons supernatant, cleaned 4 times with deionized water, dries to get close to palladium -103 Seal seed core in a steady stream.Then the source core made is packed into the titanium tube of 0.3mm (Φ 0.3mm), with laser welder sealing.
The activity of palladium -103 is 0.8mCi in solution after reaction, and the utilization rate of palladium -103 is 99.2%, -103 source core of palladium Mean radio activity is 0.625mCi.
Embodiment 5
A kind of preparation method of -103 sealed seed source source core of palladium, is made of following steps:
100 silver-colored sticks (0.7 × 3.5mm of Φ) are packed into the rectangular quartzy bottle of 15mL, 0.4mL 0.05mol/L lemon is added Sour aqueous solutions of potassium, 0.4mL0.015mol/L bromination aqueous palladium and 0.4mL 0.05mol/L sodium hydrate aqueous solution, mixing, instead 4min is answered, -103 aqueous solution of 0.5mL 100mCi/mL radioactivity palladium chloride and 0.4mL 0.25mol/L sodium thiosulfate are added Aqueous solution adjusts pH=10, oscillating reactions 35 minutes, abandons supernatant, cleaned 3 times with deionized water, dries to get close to palladium -103 Seal seed core in a steady stream.Then the source core made is packed into the titanium tube of 1.0mm (Φ 1.0mm), with laser welder sealing.
The activity of palladium -103 is 0.25mCi in solution after reaction, and the utilization rate of palladium -103 is 99.5%, -103 source core of palladium Mean radio activity is 0.41mCi.
The above content is combine the embodiment of optimization to illustrate the implementation, and it cannot be said that of the invention to what the present invention was done Mode only these existing explanations.For the different technologies personnel of the technical field of the invention, present inventive concept is not being departed from Under the premise of, several simple deductions and transformation can also be made, all shall be regarded as belonging in protection scope of the present invention.

Claims (4)

1. a kind of preparation method of -103 sealed seed source source core of palladium, it is characterized in that being made of following steps:
In reaction vessel, it is put into the silver-colored stick that 100 diameters are 0.1~0.7mm, length is 2.0~3.5mm in proportion, is added Saline citrate that 0.01~2mL concentration is 0.01~2mol/L, 0.1~2mL concentration are that 0.003~0.06mol/L can Dissolubility palladium salt aqueous solution and 0.01~1mL concentration are 0.02~2mol/L sodium hydrate aqueous solution, and mixing is reacted 1~5 minute, Then addition 0.1~1mL concentration is -103 aqueous solution of 100-1000mCi/mL radioactivity palladium chloride and 0.1~2mL concentration is 0.05mol/L~1.0mol/L aqueous thiosulfate, 20~60min of oscillating reactions under pH=6~11 abandon supernatant, use Acetone, deionized water or ethyl alcohol clean 2~4 times to get -103 sealed seed source source core of palladium is arrived.
2. the preparation method of -103 sealed seed source source core of a kind of palladium according to claim 1, it is characterized in that the citric acid Salt is sodium citrate or potassium citrate.
3. the preparation method of -103 sealed seed source source core of a kind of palladium according to claim 1, it is characterized in that the solubility Palladium salt is palladium bromide, fluorination palladium or palladium chloride.
4. the preparation method of -103 sealed seed source source core of a kind of palladium according to claim 1, it is characterized in that the thio sulphur Hydrochlorate is sodium thiosulfate or potassium thiosulfate.
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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101469420A (en) * 2007-04-16 2009-07-01 上村工业株式会社 Electroless gold-plating method and electronic component
CN101709462A (en) * 2009-12-23 2010-05-19 长沙理工大学 Chemical palladium plating solution
CN101880873A (en) * 2010-06-30 2010-11-10 中国原子能科学研究院 103Preparation process of Pd sealed seed source core
CN104561943A (en) * 2014-12-27 2015-04-29 广东致卓精密金属科技有限公司 Chemical nickel-palladium alloy plating process for circuit boards

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101469420A (en) * 2007-04-16 2009-07-01 上村工业株式会社 Electroless gold-plating method and electronic component
CN101709462A (en) * 2009-12-23 2010-05-19 长沙理工大学 Chemical palladium plating solution
CN101880873A (en) * 2010-06-30 2010-11-10 中国原子能科学研究院 103Preparation process of Pd sealed seed source core
CN104561943A (en) * 2014-12-27 2015-04-29 广东致卓精密金属科技有限公司 Chemical nickel-palladium alloy plating process for circuit boards

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