CN107293345B - The preparation method of -68 radioactive source source core of germanium - Google Patents

The preparation method of -68 radioactive source source core of germanium Download PDF

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CN107293345B
CN107293345B CN201710410662.XA CN201710410662A CN107293345B CN 107293345 B CN107293345 B CN 107293345B CN 201710410662 A CN201710410662 A CN 201710410662A CN 107293345 B CN107293345 B CN 107293345B
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germanium
radioactive
zirconium silicate
source
radioactive source
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CN107293345A (en
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阎尓坤
孙勇林
朱辉
李佳
白红升
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Tianjin Co Ltd Of Saden Medicine Research Academy
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Tianjin Co Ltd Of Saden Medicine Research Academy
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    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21GCONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G4/00Radioactive sources
    • G21G4/04Radioactive sources other than neutron sources

Abstract

The invention discloses a kind of preparation methods of -68 radioactive source source core of germanium, include the following steps: in reaction vessel, it is put into zirconium silicate particles after processing, aqueous hydrochloric acid solution, germanium saline solution and -68 saline solution of germanium is added to be uniformly mixed, supernatant is abandoned in oscillating reactions, it is cleaned with deionized water, washes of absolute alcohol is used again, is dried at room temperature to get -68 radioactive source source core of germanium is arrived.- 68 radioactive source source core radioactive activity of germanium of preparation of the invention is evenly distributed, and -68 utilization rate of germanium is high, and the radioactive liquid waste of generation is few.The method reaction time of the invention is short, and operational sequence is simple and easy to control, high production efficiency, while using low-concentration hcl, and staff's safe operation and dose of radiation are low.Chemical reagent used in method of the invention is conventional commercial reagent, and conveniently, cheap, production cost is low for nontoxic, buying.Zirconium silicate has high radiation resistance, and particle is uniform, and adsorption effect is good, is easy to load, it is good to load uniformity.

Description

The preparation method of -68 radioactive source source core of germanium
Technical field
The invention belongs to nuclear technology fields, specifically being related to a kind of preparation method of -68 radioactive source source core of germanium.
Background technique
Position emission tomography (PET), also referred to as molecular imaging or biochemical imaging are that nuclear medicine develops One new technology is the new technology of the present age state-of-the-art non-invasive high-quality diagnostic imaging, is high-level nuclear medicine diagnostic Mark.PET is widely using the clinical diagnosis of various diseases and research of preclinical medicine etc..Since detector is inconsistent Property, isotope decay, tissue severely impact the picture quality of PET to isotope absorption, random error and scattering error And diagnosis effect, often there is image fault phenomenon.One of an important factor for correction for attenuation is influence PET image quality, every time It is imaged using PET, it is necessary to be corrected, to guarantee imaging quality and diagnosis effect.
The most frequently used radioactive source for PET correction for attenuation is germanium -68 and cesium-137 radioactive source.It is generated since germanium -68 decays The transmitting of daughter gallium-68 positive electron energy and intracorporal positive electron energy coincidence, attenuation coefficient (ACF) closest to true value, It being not required to correct again, the half-life period of germanium -68 is 271d, is up to 1 year or more using the time, it is easy to use, it needs to regularly replace, therefore The scanning that penetrates of -68 sealed radioactive source of germanium is the most-often used correction for attenuation side of classical transmission attenuation correction mode and PET Formula, widely application specific PET and PET-CT.
- 68 radioactive source of germanium is the source core that will be adsorbed with radioactivity germanium -68, is packed into stainless steel tube, both ends sealing, after sealing Stainless steel tube setting reassembled on pedestal in casing, that is, be made a kind of germanium [68Ge] sealed radioactive source.
The technology of preparing of -68 radioactive source source core of germanium is the key technology of -68 radioactive source of germanium, and uniformity and stability can be straight The quality of -68 radioactive source of influence germanium is connect, and then influences the effect of correction for attenuation.The source core production of -68 sealed radioactive source of germanium is usual Using galvanoplastic, colloid method and absorption method.Galvanoplastic be in the dilute alkaline soln containing cyanide, with68GeCu3Alloy plating in Nickel metal foil.Advantage is that source core uniformity is good, the disadvantage is that complex process, it is difficult to control, high production cost, while also generate a large amount of Radioactive liquid waste, germanium [68Ge] utilization rate it is low, about 60%.Colloid method prepare source core be by68GeCl4Solution, gelatin or Carbow-1450 is uniformly mixed at 40~50 DEG C, solidification sealing preparation PET calibration source in injection container.Its advantage gelinite Fusing point it is lower (generally below 50 DEG C), gelinite after a period of use, can be melted and supplement appropriate activity by -68 source of germanium68Ge is reused, and manufacture craft is simple.Disadvantage must be stirred quickly avoid colloid solidification in the production process, and manufacturing process is difficult It controls, temperature is higher in preparation process will cause the volatilization of germanium -68, and colloid is easy adhesion during filling and pollutes on wall With the loss of germanium -68.It is that adsorbent prepares -68 source core of germanium, advantage manufacture craft that absorption method, which is with anion-cation exchange resin, Relatively simple, easy to control, cost is relatively low, and the utilization rate of germanium -68 is 90% or so.The disadvantage is that ion exchange resin radiation-resistant property Poor, resin can cause the line uniformity of radioactive source to become larger agent because of aging or broken in long-time use process, and school is not achieved Effect is tested, thus the distortion for imaging PET image.Chinese patent ZL 2,009 1 0069323.5 discloses a kind of using resistance to spoke The silica penetrated be adsorbent prepared under high-concentration sulfuric acid solution germanium [68Ge] radioactive source source core method, overcome above-mentioned skill The shortcomings that art, but there are still deficiency, be that there are security risks to operator in operation for high-concentration sulfuric acid, reacted Heat is generated in journey and increases reaction temperature, is caused a small amount of germanium -68 to volatilize, is needed to be centrifugated after reaction, source core is cleaned into Property needed for cleaning solution volume it is big, generate waste liquid amount it is big, increase waste processing cost.
Summary of the invention
The purpose of the present invention is overcoming deficiency in the prior art, provide a kind of safe operation, simple for production, radiation resistance and Load the preparation method of easy -68 radioactive source source core of germanium.
Technical solution of the present invention is summarized as follows:
A kind of preparation method of -68 radioactive source source core of germanium, includes the following steps: in reaction vessel, is put into after processing 1-5g partial size be 10-100 μm of zirconium silicate particles, be added 5-20mL 0.5-2M aqueous hydrochloric acid solution, 0-2mL 0-1.5M germanium salt water Solution and -68 saline solution of 0.1-3mL 0.5-10mCi/mL germanium are uniformly mixed, and oscillating reactions 10-40min abandons supernatant, spends Ionized water cleaning, then use washes of absolute alcohol, dry at room temperature to get arrive -68 radioactive source source core of germanium.
Zirconium silicate particles processing method is to impregnate zirconium silicate particles 5-20min with 1-2M aqueous hydrochloric acid solution, uses deionized water It is washed till neutrality, is dried at 200-300 DEG C.
Preferably, the volume of germanium saline solution is 0.5-1.5mL, and the concentration of germanium saline solution is 0.05-1.3M.
Germanium salt is preferably germanium chloride or nitric acid germanium.
- 68 salt of germanium is preferably germanium chloride -68 or nitric acid germanium -68.
Advantages of the present invention
1. the reaction system that method of the invention is formed using low concentration of salt aqueous acid and carrier germanium saline solution, with silicon Sour zirconium particle is adsorbent, and -68 radioactive source source core radioactive activity of germanium of preparation is evenly distributed, and -68 utilization rate of germanium is high, generation Radioactive liquid waste is few.
2. the method reaction time of the invention is short, operational sequence is simple and easy to control, high production efficiency, while using low concentration of salt Acid, staff's safe operation and dose of radiation are low.
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.
4, zirconium silicate has high radiation resistance, and particle is uniform, and adsorption effect is good, is easy to load, it is good to load uniformity.
Specific embodiment
The present invention is further illustrated combined with specific embodiments below.
Chemical reagent used in all embodiments is that analysis is pure.
Embodiment 1
A kind of preparation method of -68 radioactive source source core of germanium, includes the following steps:
In reaction vessel, the 1g partial size being put into after processing is 20 μm of zirconium silicate particles, and it is water-soluble that 5mL 2M hydrochloric acid is added Liquid, 1.5mL 0.5M germanium chloride aqueous solution and -68 aqueous solution of 3mL 0.5mCi/mL germanium chloride are uniformly mixed, oscillating reactions 40min abandons supernatant, is cleaned 2 times with deionized water, then with washes of absolute alcohol 1 time, dries radiate to get to germanium -68 at room temperature Core in a steady stream.
Zirconium silicate particles processing method be with 1M aqueous hydrochloric acid solution impregnate zirconium silicate particles 20min, be washed with deionized water to Neutrality, in an oven 200 DEG C of drying.
- 68 utilization rate of radioactivity germanium=(- 68 activity of radioactivity germanium/- 68 activity of investment radioactivity germanium in 1- supernatant) × 100%
- 68 activity of radioactivity germanium is 0.03mCi in supernatant, and investment -68 activity of radioactivity germanium is 1.5mCi, radioactivity - 68 utilization rate of germanium is 98%.
Embodiment 2
A kind of preparation method of -68 radioactive source source core of germanium, includes the following steps:
In reaction vessel, the 1.5g partial size being put into after processing is 10 μm of zirconium silicate particles, and 10mL 0.5M hydrochloric acid is added Aqueous solution, 0.5mL 0.05M germanium chloride aqueous solution and -68 aqueous solution of 0.1mL 10mCi/mL germanium chloride are uniformly mixed, and oscillation is anti- 10min is answered, supernatant is abandoned, is cleaned 2 times with deionized water, then with washes of absolute alcohol 1 time, dry put to get to germanium -68 at room temperature Penetrate core in a steady stream.
Zirconium silicate particles processing method be with 1.5M aqueous hydrochloric acid solution impregnate zirconium silicate particles 5min, be washed with deionized water to Neutrality, in an oven 250 DEG C of drying.
- 68 activity of radioactivity germanium is 0.025mCi in supernatant, and investment -68 activity of radioactivity germanium is 1.0mCi, radioactivity - 68 utilization rate of germanium is 97.5%.
Embodiment 3
A kind of preparation method of -68 radioactive source source core of germanium, includes the following steps:
In reaction vessel, the 5g partial size being put into after processing is 80 μm of zirconium silicate particles, and 20mL 1.5M hydrochloric acid water is added Solution, 2mL 1.5M germanium chloride aqueous solution and -68 aqueous solution of 3.0mL 5mCi/mL germanium chloride are uniformly mixed, oscillating reactions 30min abandons supernatant, is cleaned 2 times with deionized water, then with washes of absolute alcohol 1 time, dries radiate to get to germanium -68 at room temperature Core in a steady stream.
Zirconium silicate particles processing method be with 2M aqueous hydrochloric acid solution impregnate zirconium silicate particles 15min, be washed with deionized water to Neutrality, in an oven 300 DEG C of drying.
- 68 activity of radioactivity germanium is 0.113mCi in supernatant, and investment -68 activity of radioactivity germanium is 7.5mCi, radioactivity - 68 utilization rate of germanium is 98.5%.
Embodiment 4
A kind of preparation method of -68 radioactive source source core of germanium, includes the following steps:
In reaction vessel, the 2.5g partial size being put into after processing is 100 μm of zirconium silicate particles, and 15mL 1M hydrochloric acid is added Aqueous solution, 1.5mL 1.3M nitric acid germanium aqueous solution and -68 aqueous solution of 2.5mL 10mCi/mL nitric acid germanium are uniformly mixed, oscillating reactions 15min abandons supernatant, is cleaned 2 times with deionized water, then with washes of absolute alcohol 1 time, dries radiate to get to germanium -68 at room temperature Core in a steady stream.
Zirconium silicate particles processing method is to impregnate zirconium silicate particles 18min with 1.5M aqueous hydrochloric acid solution, is washed with deionized water To neutrality, in an oven 250 DEG C of drying.
- 68 activity of radioactivity germanium is 0.875mCi in supernatant, and investment -68 activity of radioactivity germanium is 25mCi, radioactivity - 68 utilization rate of germanium is 96.5%.
Embodiment 5
A kind of preparation method of -68 radioactive source source core of germanium, includes the following steps:
In reaction vessel, the 2.5g partial size being put into after processing is 100 μm of zirconium silicate particles, and 12mL 1.3M salt is added Aqueous acid, 1.5mL 0.5M germanium chloride aqueous solution and -68 aqueous solution of 2.0mL 8mCi/mL germanium chloride are uniformly mixed, and oscillation is anti- 30min is answered, supernatant is abandoned, is cleaned 2 times with deionized water, then with washes of absolute alcohol 1 time, dry put to get to germanium -68 at room temperature Penetrate core in a steady stream.
Zirconium silicate particles processing method be with 1M aqueous hydrochloric acid solution impregnate zirconium silicate particles 10min, be washed with deionized water to Neutrality, in an oven 220 DEG C of drying.
- 68 activity of radioactivity germanium is 0.400mCi in supernatant, and investment -68 activity of radioactivity germanium is 16mCi, radioactivity - 68 utilization rate of germanium is 97.5%.
Embodiment 6
A kind of preparation method of -68 radioactive source source core of germanium, includes the following steps:
In reaction vessel, the 1.5g partial size being put into after processing is 30 μm of zirconium silicate particles, and 8mL 1.2M hydrochloric acid is added Aqueous solution, -68 saline solution of 1.5mL 4mCi/mL nitric acid germanium are uniformly mixed, and oscillating reactions 25min abandons supernatant, uses deionized water Cleaning 2 times, then with washes of absolute alcohol 1 time, dried at room temperature to get -68 radioactive source source core of germanium is arrived.
Zirconium silicate particles processing method be with 1M aqueous hydrochloric acid solution impregnate zirconium silicate particles 10min, be washed with deionized water to Neutrality, in an oven 250 DEG C of drying.
- 68 activity of radioactivity germanium is 0.096mCi in supernatant, and investment -68 activity of radioactivity germanium is 6mCi, radioactivity germanium - 68 utilization rates are 98.3%.
According to -68 radioactive source of germanium and U.S. SANDERS company of 1 method of embodiment preparation in GE Discovery ST PET-C has carried out 3D sweep test, reads radiocounting every 2cm, calculates the uniformity of -68 radioactive source of radioactivity germanium, experiment It the results are shown in Table 1.
The radioactive source of the product preparation of 1 embodiment 1 of table is compared with U.S. SANDERS Products uniformity

Claims (5)

1. a kind of preparation method of -68 radioactive source source core of germanium, it is characterized in that include the following steps: in reaction vessel, be put into through Treated, and 1-5g partial size is 10-100 μm of zirconium silicate particles, and 5-20mL 0.5-2M aqueous hydrochloric acid solution, 0-2mL 0-1.5M is added Germanium saline solution and -68 saline solution of 0.1-3mL 0.5-10mCi/mL germanium are uniformly mixed, oscillating reactions 10-40min, in abandoning Clearly, it is cleaned, then with washes of absolute alcohol, is dried at room temperature to get to -68 radioactive source source core of germanium with deionized water.
2. according to the method described in claim 1, it is characterized in that the zirconium silicate particles processing method is with 1-2M hydrochloric acid water Solution impregnates zirconium silicate particles 5-20min, is washed with deionized water to neutrality, dries at 200-300 DEG C.
3. according to the method described in claim 1, it is characterized in that the volume of germanium saline solution is 0.5-1.5mL, germanium saline solution Concentration be 0.05-1.3M.
4. method according to claim 1 or 3, it is characterized in that the germanium salt is germanium chloride or nitric acid germanium.
5. according to the method described in claim 1, it is characterized in that -68 salt of germanium is germanium chloride -68 or nitric acid germanium -68.
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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
TW436814B (en) * 2000-05-04 2001-05-28 Inst Of Nuclear Energy Res Roc A novel method for fabrication of germanium-68 sealed sources
CN101593567A (en) * 2009-06-18 2009-12-02 天津赛德生物制药有限公司 68The preparation method of Ge sealed radioactive source
CN101777399A (en) * 2010-02-03 2010-07-14 中国原子能科学研究院 PET attenuation correction method68Preparation process of Ge line source
CN102382994A (en) * 2011-07-18 2012-03-21 原子高科股份有限公司 Radioactivity68Preparation method of Ge solution
CN105308687A (en) * 2013-06-27 2016-02-03 马林克罗特有限公司 Process of generating germanium

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP6052681B2 (en) * 2011-10-21 2016-12-27 国立大学法人 長崎大学 68Ge-68Ga generator and method for producing 68Ga-containing liquid using the same

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
TW436814B (en) * 2000-05-04 2001-05-28 Inst Of Nuclear Energy Res Roc A novel method for fabrication of germanium-68 sealed sources
CN101593567A (en) * 2009-06-18 2009-12-02 天津赛德生物制药有限公司 68The preparation method of Ge sealed radioactive source
CN101777399A (en) * 2010-02-03 2010-07-14 中国原子能科学研究院 PET attenuation correction method68Preparation process of Ge line source
CN102382994A (en) * 2011-07-18 2012-03-21 原子高科股份有限公司 Radioactivity68Preparation method of Ge solution
CN105308687A (en) * 2013-06-27 2016-02-03 马林克罗特有限公司 Process of generating germanium

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