CN107293345A - The preparation method of the radioactive source source core of germanium 68 - Google Patents

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

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CN107293345A
CN107293345A CN201710410662.XA CN201710410662A CN107293345A CN 107293345 A CN107293345 A CN 107293345A CN 201710410662 A CN201710410662 A CN 201710410662A CN 107293345 A CN107293345 A CN 107293345A
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germanium
source
radioactive
zirconium silicate
radioactive source
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CN107293345B (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

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  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
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Abstract

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

Description

The preparation method of the radioactive source source core of germanium -68
Technical field
The invention belongs to nuclear technology field, specifically being related to a kind of preparation method of the radioactive source of germanium -68 source core.
Background technology
Position emission tomography (PET), also referred to as molecular imaging or biochemical imaging, are nuclear medicine development One new technology, is the new technology of contemporary state-of-the-art non-invasive high-quality diagnostic imaging, is high-level nuclear medicine diagnostic Mark.PET has widely applied the clinical diagnosis of various diseases and the research of preclinical medicine etc..Because detector is inconsistent Property, isotope decay, tissue severely impact PET picture quality to isotope absorption, random error and scattering error And diagnosis effect, often there is image fault phenomenon.Correction for attenuation is to influence one of key factor of PET image qualities, every time Imaged using PET, it is necessary to be corrected, to ensure imaging quality and diagnosis effect.
The most frequently used radioactive source for PET correction for attenuations is germanium -68 and cesium-137 radioactive source.Generated because germanium -68 decays The transmitting of daughter gallium-68 positive electron energy and internal positive electron energy coincidence, attenuation coefficient (ACF) closest to actual value, It is not required to correct again, the half-life period of germanium -68 is 271d, and use time is up to more than 1 year, easy to use, it is necessary to regularly replace, therefore The scanning that penetrates of the sealed radioactive source of germanium germanium -68 is classical transmission attenuation correction mode, is also the most-often used correction for attenuations of PET Mode, widely application specific PET and PET-CT.
The radioactive source of germanium -68 is will to be adsorbed with the source core of radioactivity germanium -68, is loaded in stainless steel tube, two ends sealing, after sealing Stainless steel tube be arranged in sleeve pipe and reassemble on base, that is, be made a kind of germanium [68Ge] sealed radioactive source.
The technology of preparing of the radioactive source source core of germanium -68 is the key technology of the radioactive source of germanium germanium -68, its uniformity and stability meeting The quality of the radioactive source of germanium -68 is directly affected, and then influences the effect of correction for attenuation.The source core of the sealed radioactive source of germanium -68 makes logical Frequently with 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, has the disadvantage complex process, it is difficult to control, and production cost is high, while also producing big The radioactive liquid waste of amount, germanium [68Ge] utilization rate it is low, about 60%.Colloid method prepare source core be by68GeCl4Solution, gelatin Or Carbow-1450 is well mixed at 40~50 DEG C, solidification sealing prepares PET calibration sources in injection container.Its advantage gel The fusing point of body is relatively low (generally below 50 DEG C), and the source of germanium -68 was used after a period of time, gelinite melting can be supplemented into appropriate activity 's68Ge is reused, and manufacture craft is simple.Shortcoming must quickly stir in manufacturing process and avoid colloid solidification, manufacturing process Temperature is higher in hardly possible control, preparation process can cause germanium -68 to volatilize, and easily adhesion causes dirt to colloid on wall during filling The loss of dye and germanium -68.It with anion-cation exchange resin is that adsorbent prepares the source core of germanium -68 that absorption method, which is, and its advantage makes work Skill is simpler, easy to control, and cost is relatively low, and the utilization rate of germanium -68 is 90% or so.It has the disadvantage ion exchange resin radioresistance Can be poor, resin can cause the line uniformity of radioactive source to become big agent because of aging or broken during long-time use, and not reach Effect is verified, so that the distortion of PET image imaging.Chinese patent ZL 2,009 1 0069323.5 discloses a kind of using resistance to The silica of radiation be adsorbent prepared under high-concentration sulfuric acid solution germanium [68Ge] radioactive source source core method, overcome above-mentioned The shortcoming of technology, but deficiency is still suffered from, it is that high-concentration sulfuric acid has potential safety hazard to operating personnel in operation, reaction During produce heat but reaction temperature is raised, cause a small amount of germanium -68 to volatilize, need to centrifuge after reaction, source core clean to Neutral required cleaning fluid volume is big, produces waste liquid amount greatly, increases waste processing cost.
The content of the invention
The purpose of the present invention is to overcome of the prior art not enough there is provided a kind of safe operation, simple for production, resistance to irradiation and Load the preparation method of the easy radioactive source source core of germanium -68.
Technical scheme is summarized as follows:
A kind of preparation method of the radioactive source of germanium -68 source core, comprises the following steps:In reaction vessel, it is put into after processing 1-5g particle diameters be 10-100 μm of zirconium silicate particles, add 5-20mL 0.5-2M aqueous hydrochloric acid solutions, 0-2mL 0-1.5M germanium salt solution Solution and the saline solution of 0.1-3mL 0.5-10mCi/mL germanium -68 are well mixed, and oscillating reactions 10-40min abandons supernatant, spent Ionized water is cleaned, then with washes of absolute alcohol, is dried at room temperature, that is, obtains the radioactive source source core of germanium -68.
Zirconium silicate particles processing method is, with 1-2M aqueous hydrochloric acid solutions immersion zirconium silicate particles 5-20min, to use deionized water Neutrality is washed till, in 200-300 DEG C of drying.
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.
The salt of germanium -68 is preferably germanium chloride -68 or nitric acid germanium -68.
Advantages of the present invention
1. the reaction system that the method for the present invention is constituted using low concentration of salt aqueous acid and carrier germanium saline solution, with silicon Sour zirconium particle is adsorbent, and the radioactive source source core radioactive activity of germanium -68 of preparation is evenly distributed, and the utilization rate of germanium -68 is high, generation Radioactive liquid waste is few.
2. the method reaction time of the present invention is short, operational sequence is simple and easy to control, and production efficiency is high, while using low concentration of salt Acid, staff's safe operation and dose of radiation are low.
3. chemical reagent used in the method for the present invention is conventional commercial reagent, nontoxic, buying is convenient, and price is just Preferably, production cost is low.
4th, zirconium silicate has high radiation resistance, and particle is uniform, and advantages of good adsorption effect is easily loaded, and loads uniformity good.
Embodiment
With reference to specific embodiment, the present invention is further illustrated.
The chemical reagent used in all embodiments is that analysis is pure.
Embodiment 1
A kind of preparation method of the radioactive source of germanium -68 source core, comprises the following steps:
In reaction vessel, it is 20 μm of zirconium silicate particles to be put into the 1g particle diameters after processing, adds 5mL 2M hydrochloric acid water-soluble Liquid, the 1.5mL 0.5M germanium chlorides aqueous solution and the aqueous solution of 3mL 0.5mCi/mL germanium chlorides -68 are well mixed, oscillating reactions 40min, abandons supernatant, is cleaned with deionized water 2 times, then with washes of absolute alcohol 1 time, dries at room temperature, that is, obtains the radiation of germanium -68 Core in a steady stream.
Zirconium silicate particles processing method be with 1M aqueous hydrochloric acid solutions immersion zirconium silicate particles 20min, be washed with deionized water to Neutrality, in an oven 200 DEG C of drying.
The utilization rate of radioactivity germanium -68=(- 68 activity of radioactivity germanium/activity of input radioactivity germanium -68 in 1- supernatants) × 100%
The activity of radioactivity germanium -68 is 0.03mCi in supernatant, and the activity of input radioactivity germanium -68 is 1.5mCi, radioactivity The utilization rate of germanium -68 is 98%.
Embodiment 2
A kind of preparation method of the radioactive source of germanium -68 source core, comprises the following steps:
In reaction vessel, it is 10 μm of zirconium silicate particles to be put into the 1.5g particle diameters after processing, adds 10mL 0.5M hydrochloric acid The aqueous solution, the 0.5mL 0.05M germanium chlorides aqueous solution and the aqueous solution of 0.1mL 10mCi/mL germanium chlorides -68 are well mixed, and vibration is anti- 10min is answered, supernatant is abandoned, is cleaned with deionized water 2 times, then with washes of absolute alcohol 1 time, dries at room temperature, that is, obtains germanium -68 and put Penetrate core in a steady stream.
Zirconium silicate particles processing method be with 1.5M aqueous hydrochloric acid solutions immersion zirconium silicate particles 5min, be washed with deionized water to Neutrality, in an oven 250 DEG C of drying.
The activity of radioactivity germanium -68 is 0.025mCi in supernatant, and the activity of input radioactivity germanium -68 is 1.0mCi, radioactivity The utilization rate of germanium -68 is 97.5%.
Embodiment 3
A kind of preparation method of the radioactive source of germanium -68 source core, comprises the following steps:
In reaction vessel, it is 80 μm of zirconium silicate particles to be put into the 5g particle diameters after processing, adds 20mL 1.5M hydrochloric acid waters Solution, the 2mL 1.5M germanium chlorides aqueous solution and the aqueous solution of 3.0mL 5mCi/mL germanium chlorides -68 are well mixed, oscillating reactions 30min, abandons supernatant, is cleaned with deionized water 2 times, then with washes of absolute alcohol 1 time, dries at room temperature, that is, obtains the radiation of germanium -68 Core in a steady stream.
Zirconium silicate particles processing method be with 2M aqueous hydrochloric acid solutions immersion zirconium silicate particles 15min, be washed with deionized water to Neutrality, in an oven 300 DEG C of drying.
The activity of radioactivity germanium -68 is 0.113mCi in supernatant, and the activity of input radioactivity germanium -68 is 7.5mCi, radioactivity The utilization rate of germanium -68 is 98.5%.
Embodiment 4
A kind of preparation method of the radioactive source of germanium -68 source core, comprises the following steps:
In reaction vessel, it is 100 μm of zirconium silicate particles to be put into the 2.5g particle diameters after processing, adds 15mL 1M hydrochloric acid The aqueous solution, the 1.5mL 1.3M nitric acid germanium aqueous solution and the aqueous solution of 2.5mL 10mCi/mL nitric acid germanium -68 are well mixed, oscillating reactions 15min, abandons supernatant, is cleaned with deionized water 2 times, then with washes of absolute alcohol 1 time, dries at room temperature, that is, obtains the radiation of germanium -68 Core in a steady stream.
Zirconium silicate particles processing method is, with 1.5M aqueous hydrochloric acid solutions immersion zirconium silicate particles 18min, to be washed with deionized water To neutral, 250 DEG C of drying in an oven.
The activity of radioactivity germanium -68 is 0.875mCi in supernatant, and the activity of input radioactivity germanium -68 is 25mCi, radioactivity The utilization rate of germanium -68 is 96.5%.
Embodiment 5
A kind of preparation method of the radioactive source of germanium -68 source core, comprises the following steps:
In reaction vessel, it is 100 μm of zirconium silicate particles to be put into the 2.5g particle diameters after processing, adds 12mL 1.3M salt Aqueous acid, the 1.5mL 0.5M germanium chlorides aqueous solution and the aqueous solution of 2.0mL 8mCi/mL germanium chlorides -68 are well mixed, and vibration is anti- 30min is answered, supernatant is abandoned, is cleaned with deionized water 2 times, then with washes of absolute alcohol 1 time, dries at room temperature, that is, obtains germanium -68 and put Penetrate core in a steady stream.
Zirconium silicate particles processing method be with 1M aqueous hydrochloric acid solutions immersion zirconium silicate particles 10min, be washed with deionized water to Neutrality, in an oven 220 DEG C of drying.
The activity of radioactivity germanium -68 is 0.400mCi in supernatant, and the activity of input radioactivity germanium -68 is 16mCi, radioactivity The utilization rate of germanium -68 is 97.5%.
Embodiment 6
A kind of preparation method of the radioactive source of germanium -68 source core, comprises the following steps:
In reaction vessel, it is 30 μm of zirconium silicate particles to be put into the 1.5g particle diameters after processing, adds 8mL 1.2M hydrochloric acid The aqueous solution, the saline solution of 1.5mL 4mCi/mL nitric acid germanium -68 are well mixed, and oscillating reactions 25min abandons supernatant, uses deionized water Cleaning 2 times, then with washes of absolute alcohol 1 time, dry at room temperature, that is, obtain the radioactive source source core of germanium -68.
Zirconium silicate particles processing method be with 1M aqueous hydrochloric acid solutions immersion zirconium silicate particles 10min, be washed with deionized water to Neutrality, in an oven 250 DEG C of drying.
The activity of radioactivity germanium -68 is 0.096mCi in supernatant, puts into the activity of radioactivity germanium -68 for 6mCi, radioactivity germanium - 68 utilization rates are 98.3%.
The radioactive source of germanium -68 prepared according to the method for embodiment 1 is with SANDERS companies of the U.S. in GE Discovery ST PET-C has carried out 3D sweep tests, and radiocounting is read every 2cm, calculates the uniformity of the radioactive source of radioactivity germanium -68, experiment It the results are shown in Table 1.
Radioactive source prepared by the product of the embodiment 1 of table 1 is compared with U.S. SANDERS Products uniformities

Claims (5)

1. a kind of preparation method of the radioactive source of germanium -68 source core, it is characterized in that comprising the following steps:In reaction vessel, be put into through 1-5g particle diameters after processing are 10-100 μm of zirconium silicate particles, add 5-20mL 0.5-2M aqueous hydrochloric acid solutions, 0-2mL 0-1.5M Germanium saline solution and the saline solution of 0.1-3mL 0.5-10mCi/mL germanium -68 are well mixed, and oscillating reactions 10-40min is abandoned Clearly, cleaned, then with washes of absolute alcohol, dried at room temperature with deionized water, that is, obtain the radioactive source source core of germanium -68.
2. according to the method described in claim 1, it is characterized in that described zirconium silicate particles processing method is to use 1-2M hydrochloric acid waters Solution soaks zirconium silicate particles 5-20min, is washed with deionized water to neutrality, in 200-300 DEG C of drying.
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. the 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 the described salt of germanium -68 is germanium chloride -68 or nitric acid germanium -68.
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Citations (6)

* 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
US20140263074A1 (en) * 2011-10-21 2014-09-18 Nagasaki University GE ADSORBENT FOR 68Ge-68Ga GENERATOR
CN105308687A (en) * 2013-06-27 2016-02-03 马林克罗特有限公司 Process of generating germanium

Patent Citations (6)

* 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
US20140263074A1 (en) * 2011-10-21 2014-09-18 Nagasaki University GE ADSORBENT FOR 68Ge-68Ga GENERATOR
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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