Method of making chromatographic generator of technetium-99m from neutron-irradiated molybdenum-98

FIELD: chemistry.

SUBSTANCE: method of making a chromatographic technetium-99m generator from neutron-irradiated molybdenum-98 involves depositing a predetermined mass of molybdenum into a chromatographic column with aluminium oxide. For this purpose, eluate output of technetium-99m from the generators with different adsorbed molybdenum mass is determined. Through extrapolation from the obtained calibration curve, the mass of molybdenum which corresponds to maximum output of technetium-99m from the generator Be=1 is found as mi=exp[(1-a)/b], where a and b are coefficients of the calibration curve Bi=a+b·ln mi, where Bi is the eluate output of technetium-99m from the generator for the adsorbed mass of molybdenum mi.

EFFECT: obtaining a generator based on neutron-irradiated molybdenum-98 with a narrow eluate profile for extracting technetium-99m.

1 cl, 3 dwg

 

The invention relates to the field of radiochemistry, in particular a process for the production of technetium-99m for medicine.

Short-lived radionuclide technetium-99m is a subsidiary product of the β-decay of the isotope99Mo. For rapid separation from the99Mo and subsequent medical use are most commonly used small-sized device - chromatographic technetium generators [patent RU No. 2171512 C2, 27.07.2001]. They represent a small chromatographic column Packed with a sorbent (aluminium oxide Al2O3), which cause the molybdenum-99. All this together with inlet and outlet needles communication is placed in a protective container and transported to medical facilities, where the elution of technetium-99m from generator carried out with 0.9% sodium chloride (saline) in the form of finished product for intravenous sodium pertechnitat,99mTc.

For "charging" of generators required99Mo with high specific activity. In the world, including in Russia, it is separated from fission products of uranium-235. This method produced a large number of related long-lived radioactive waste, which is high environmental hazard and require further processing and recycling. An alternative and practical, metthods the second method of obtaining 99Mo is the neutron irradiation of the reactor molybdenum targets, the reaction98Mo(n,γ)99Mo. With an average thermal neutron flux of 1·1014n/cm2·enriched targets can be obtained specific activity99Mo 6-8 CI/g, which, in principle, sufficient to produce chromatographic generators.

This technology was introduced in the USSR in the reactor INP EN Uz SSR in the early 90-ies, and in 2003 in Russia on the reactor IRT-T Institute of nuclear physics at Tomsk Polytechnic University, where for increasing the specific activity99Mo for the reaction98Mo(n,γ)99Mo was used channels of the reactor with a high content in the neutron spectrum of resonance neutrons [Ryabchikov A.I, Skuridin V.S., A. Nesterov, Chibisov E.V., Golovkov V.M. Obtaining Molybdenum-99 in Research Reactor IR-T With Using Resonance Neutrons // Nuclear Instruments and Methods in Phys. Res., 2004, 213, p.364-368].

In the irradiated molybdenum targets for each nuclide formed99Mo has about 104-10-5atoms of stable molybdenum-98 - media. Therefore, for the manufacture of such materials generator with a nominal activity of technetium-99m 0,5 Ki Of 18.5 GBq) and more on the column of the generator it is necessary to adsorb about 200 mg of molybdenum, which requires the use of columns larger sizes.

A known method of manufacturing a generator of technetium-99m from (n,γ)99M is [Mikheev NB, Volkov, D., Rumer IA and other Generator technetium-99m. // Radiochemistry, 1971, v.13, №4.-s-633], which solves the problem of applying the column with oxide of Al2O3a large amount of molybdenum through the use of as sorbed form solution limit phosphomolybdate. The method allows you to absorb more than 670 mg molybdenum (metal) on a column with a mass of oxide of Al2O3more than 10, however, as shown by our study and as noted in several works [for example, Steigman J. Chemistry of the Alumina Column // Int. J. Apl. Radiat. Isot, 1982, V.33, p.829-834], the presence of stable molybdenum significantly affects the magnitude of the output of technetium-99m from generator. In addition, the use of columns of large size leads to increased lacienega profile generator. The latter means that for a full selection of technetium-99m from generator column requires several times more saline than other generators on the basis of a fission product of uranium-235. Correspondingly decreases and the volume activity of the drug, which is also a disadvantage of this method.

A known method of making chromatographic generator technetium-99m from neutron-irradiated molybdenum-98 authors of this application, selected as a prototype [RF patent N 2276102, priority 29.11.04, bull. No. 13, 2006], which solves the problem of determining it is possible and sufficient mass of molybdenum, providing the desired activity of technetium-99m allocated from the generator. In accordance with this method, the aluminum oxide is applied molybdenum with known specific activity99Mo and in such quantity that the specified activity technetium-99m is achieved in the complete elution of the generator some limiting displacement of saline, which further increases do not lead to increased activity of the secreted radionuclide. In this case the obtained value of the volumetric activity of the drug is defined as the ratio of allocated activity of technetium-99m to the total volume of saline, passed through a column of the generator. One of the possible ways to increase the volume activity for the given dimensions of the chromatographic column is narrowing its lacienega profile. However, such a possibility in the method prototype is not considered that determines his fault.

Thus, to date remains unresolved the problem of obtaining the highest possible volumetric activity of the preparation of technetium-99m allocated from the generator with a large adsorbed mass of molybdenum.

The technical result of the invention consists in obtaining a generator on the basis of neutron-irradiated molybdenum-98 with narrow aluation profile excretion of technetium-99m.

The goal of the project resh which is as follows. In the same way as in the known method, chromatographic column filled with alumina put a predefined mass of molybdenum. In contrast, define eduational output of technetium-99m from generator with different adsorbed mass of molybdenum, then obtained from the calibration based extrapolation find a lot of molybdenum, corresponding to the maximum output of technetium-99m from generatorE=1, as mI=exp[(1-a)/V], where a and b are coefficients of the calibration dependence of Bi=a+b·lnmiwhere Bi- eduational output of technetium-99m from generator when the adsorbed mass of molybdenum mi.

The invention is illustrated by drawings, on which:

figure 1 - change release of technetium-99m depending on the volume of saline, passed through a column of generators with different adsorbed mass of molybdenum: 70 mg (curve 1) and 150 mg (curve 2);

figure 2 - dependence of changes in the output of technetium-99m InEfrom the logarithm of the mass of molybdenum mMo;

figure 3 - luiziana curve generator with adsorbed mass of molybdenum mI=0,235,

As an example, figure 1 shows aluation curves changes the output of technetium-99m depending on the volume of saline, passed through a column of generators with different adsorbed mass of molybdenum: 70 mg (curve 1) and 150 mg (distorting the I 2). The columns have the same volume of 7.3 cm3. As adsorbent was used acidic oxide Al2O3for column chromatography (0,063-0,200 mm) of the firm Merck, pre-treated with hydrochloric acid and washed with water to pH 3. Weight of oxide in the columns was 8.1,

Presented aluation curves, it follows that with increasing adsorbed mass of molybdenum eduational profile generator is reduced. So, if in the first case, for a full selection of technetium-99m required volume of saline solution 20 ml, in the second - 14 ml. it is Explained in the following. As is known, the adsorption of molybdenum is carried out on the active centres of aluminum oxide. When they are incomplete filling molybdenum remaining vacant centers have a "braking" effect on the rate of leaching of technetium-99m from generator, which leads to the expansion of its lacienega profile. In accordance with this, the problem arises in determining the required mass of molybdenum, which guarantees the most narrow profile generator and, as a consequence, the maximum yield of technetium-99m in the optimal volume of saline. This volume may be recommended in the Instruction manual of the generator. For example, generators, made on the basis of99Mo, a fission product of uranium-235 with a standard column 2.8 cm3- featured is the volume of eluent is 5 ml. As for the generator, made of neutron-irradiated molybdenum-98 with column more than 10 cm3this amount may be equal to 70 ml [Molinski V.J. A Review of99mTc Generator Technology // Int. J. Appl. Radiat. Isot. - 1982. - v.33. - p.811-819].

Table 1 shows the values of the volumetric activity of the drug, calculated from the dependency figure 1 for different volumes of saline, passed through the generator column. The initial activity of technetium-99m generators was 20 GBq.

From table 1 it follows that, despite the differences aluation profiles, in both cases, the highest specific activity of the eluate is achieved in the volume of 7-10 ml of Here as best may be selected volume of 8.5 ml Next, the mass of molybdenum, providing the maximum yield of technetium-99m in this volume are from the calibration curve of the output of technetium-99m BIfrom the adsorbed mass of molybdenum for the limiting case BE=1.

The invention is illustrated by specific example.

Sample enriched up to 98.6% of molybdenum-98 mass of 1.2 g irradiated in the channel reactor neutron flux of 1.1·1014n/cm2·within 100 hours After the "cooling" of the target for 10 h, it was dissolved in 5 ml of 5 M NaOH solution with the addition of 0.5 ml of hydrogen peroxide, and then transferred to polymolybdates with pH 3 by introducing into the resulting solution of 18.5 ml of 1 M rastvoritelei acid. Specific activity99Mo in solution is 7.2 CI/g (266.5 Azerbaijani GBq/g), the concentration of molybdenum CMo=1,2/24=0,050 g/ml.

On pre-prepared 4 chromatographic column with a volume of 7.3 cm3aluminum oxide mass of 8.1 g, treated with hydrochloric acid and washed with water to pH 3, put 2,0; 2,6; 3.0 and 3.4 ml polymolybdates, which corresponds to the adsorbed mass of molybdenum 0,10; 0,13; of 0.15 and 0.17, After exposure of generators for 22 h - time equilibrium accumulation of technetium-99m spend their elution successively with two portions of saline solution with a volume of 8.5 and 11.5 ml of calculation, that the total volume reached total allocation of technetium-99m from the speakers. Then measure the activity of the obtained eluates using daskalopetra. The results of the measurements are presented in table 2. In her last column shows the values of the output of technetium-99m Bi1 flushing, calculated from the ratio of the activity 1 flush to the total activity of 1 and 2 swabs. According to table 2, we build the dependence of changes in the output of technetium-99m Bifrom the logarithm of the mass of molybdenum miwhich is presented in figure 2. The dependence is described by the linear relation:

where a and b - some coefficients of the calibration dependence, which for the case in question, respectively 1,482 and of 0.333.

E. strapline curve 2 to the value of B I=1, we find that this ultimate case corresponds lnmMo=of-1.45. Hence the mass of molybdenum, which guarantees maximum eduational output of technetium-99m in a given volume of saline solution of 8.5 ml, is 0,235, In analytical form, this result can be obtained from equation (1) by equating it to 1. In accordance with this: ln mI=(1-a)/C. Hence:

mI=exp[(1-a)/]=exp[(1-1,482)/0,333]=0,235.

Confirmation of the proposed provisions is luiziana curve generator with adsorbed mass of molybdenum mI=0,235 g presented on figure 3. It follows that the volume of 8.5 ml is reached the output 0,99 when the total width lacienega profile generator 9 ml.

The proposed method allows to determine the adsorbed mass of molybdenum, providing the maximum yield of technetium-99m from generator.

Table 1
mMo, g/v, mlSurround activity, GBq/ml
3578,510121416180,0700,731,11,331,421,451,411,311,21,11,0
0,1501,391,91to 2.062,00to 1.861,631,42

Table 2
No. generatormigActivity99mTc, HBRBi
1 wash (8.5 oz)2 erosion (11.5 ml)
10,1013,35,20,72
20,1319,2 4,80,80
30,1523,54,20,85
40,1727,82,60,89

The method of making chromatographic generator technetium-99m from neutron-irradiated molybdenum-98, including the application of a predetermined weight of molybdenum on a chromatographic column filled with alumina, wherein define eduational output of technetium-99m from generator with different adsorbed mass of molybdenum, then obtained from the calibration based extrapolation find a lot of molybdenum mIcorresponding to the maximum LaCinema output of technetium-99m from generatorE=1, as mI=exp[(1-a)/b], where a and b are coefficients of the calibration dependence of Bi=a+b·ln miwhere Bi- eduational output of technetium-99m from generator when the adsorbed mass of molybdenum mi.



 

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