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

FIELD: chemistry.

SUBSTANCE: limiting specific weight of acid mLA, required for complete termination of its reaction with aluminium oxide is determined. The amount of acid mHCl required for treating aluminium oxide with mass mox is calculated using the relationship: mHCl=mLA·mOX. After making the corresponding calculations, aluminium oxide is treated with acid, put into a chromatographic column and a molybdenum solution is added.

EFFECT: more reliable operation of a technetium-99m generator in terms of prevention molybdenum from falling into the eluate owing to achieving maximum sorption capacity of the oxide used.

3 dwg, 1 ex

 

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 (99mTc) is a subsidiary product of the β-decay of the isotope molybdenum-99 (99Mo). For rapid separation from Mo and subsequent medical use are most commonly used small-sized device - chromatographic technetium generators [e.g., Patent RU No. 2171512 C2, 27.07.2001]. They represent a small chromatographic column Packed with a sorbent (aluminum oxide), which is applied to 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. Alternative and almost b is zachodnie way to obtain 99Mo is the neutron irradiation of the reactor molybdenum targets of natural or enriched molybdenum-98, 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 high activity of technetium-99m 0,5 Ki Of 18.5 GBq) and more on the column of the generator it is necessary to adsorb large amounts of molybdenum of about 200 mg.

The quantity of molybdenum, which can be applied to the column generator is, is determined by the product of the sorption capacity of the oxide to molybdenum W on its mass mOX. The increase in the mass of the oxide in the column, and hence its size, is highly undesirable, as it leads to increase in width lacienega profile generator and, ultimately, to reduce the volume activity of the preparation of technetium-99m. In this regard, in practice, the goal of improving the adsorbed mass of molybdenum often be solved by selection of a suitable sorbent and its preparation for adsorption. Typically, such training is in the acid treatment of aluminum oxide Al2O3, resulting in activation of their surface with the formation of active centers for adsorption, which depending on the pH of the medium created heterocomplexes different number of atoms of molybdenum. Despite the importance of this operation, up to the present time there are no criteria that would accurately determine required for processing the selected oxide amount of acid, which would provide the maximum sorption capacity. In the known methods oxides zachisliaut in a fairly wide pH ranges from 6 to 1. For example, in the method according to GB No. 1365405 (A), IPC G21G 56/00. in 1974, the Generator of radioactive isotopes and the retrieval method for the activation of the sorbent through the column pass hydrochloric or nitric acid is a pH of between 1.6 to 1.7, and then "locking" solution of acetic acid or acetate with a pH in the range of 2.8 to 7.0.

According to the method proposed by Abrashkin, S., Heller-Grossman L., Schafferman A., Davis M.A. 99mTc Generators: the Influence of the Radiation Dose on the Elution Yield // Int. J. Appl. Radiat. Isot. - 1978. - No 29. - P.395, neutral alumina (Fluka S) washed with 1 M and 0.1 M solutions of hydrochloric acid until pH=4. Also known way [Molinski V.J. A Review of99mTc Generator Technology // Int. J. Appl. Radiat. Isot. - 1982. -v.33. - p.811-819], according to which the alumina prior to the adsorption of molybdenum treated with 0.1 M solution of HCl or HNO3to pH 1-2. After charging generator solution polymolybdates with pH 3±0,5 additional column was washed with 100 ml of 0.1 M HCl solution and carry out the elution of the generator 75 ml of saline. At the last stage of the generators, which is found to have "breakthrough" of molybdenum in the eluate is excluded. The disadvantage of this method as well as all of the above analogues, is that it does not guarantee reliable binding of molybdenum on the sorbent due to the uncertainty of the final state of the oxide after treatment with acid.

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 from 29.11.04, bull. N 13, 2006], which solves the problem of determining the mass of molybdenum is, providing the desired activity of technetium-99m allocated from the generator. In accordance with this method the whole lot alumina before it is loaded on column and holding adsorption of molybdenum is treated with hydrochloric acid and washed with water to pH=3 wash water. In this way there is no justification of the choice of the amount of acid that determines his fault.

Thus, to date remains unresolved the problem of determining necessary and sufficient acid treatment of the alumina prior to the adsorption of molybdenum, which would ensure the maximum sorption capacity of the selected oxide.

The technical result of the invention is to increase the reliability of the generator in order to prevent the leakage of molybdenum in the eluate by maximum sorption capacity of the oxide used.

The technical problem is solved as follows. As in the known method prototype manufacturing chromatographic generator technetium-99m from neutron-irradiated molybdenum-98, treated aluminum oxide, acid, contribute a portion of the alumina chromatographic column and put on him the solution of molybdenum. Unlike the prototype of the pre-defined limit odelin the th mass of acid m pTorequired for a complete cessation of its interaction with alumina, and then handle all the aluminum oxide acid based

mHCl=mpTo·mOX,

where mHClthe amount of acid required for the processing of aluminum oxide with a mass mOX.

The implementation of the claimed method let us consider a specific example. Chromatographic alumina (Al2O3for column chromatography (0,063-0,200 mm) firm Merck in the number of mOX=8,155 g contribute to column generator. Then through the column portions by volume of 5-6 ml miss 0,05-0,06 M HCl solution (pH=1,28) with subsequent measurement of the pH of the past solutions for the determination of the amount of unreacted acid. Mass absorbed by the oxide acid for each of the missed portions of the solution calculated from the equation

where C0and CK- acid concentration of HCl in the solution before and after passing it through a column of oxide respectively; Vi- volume missed the first portion of the solution.

Based on these data build dependency changes absorbed by the oxide amount of acid from the total introduced quantity, which determines the maximum weight of acid per 1 g of oxide required for a complete cessation of its interaction with oxide is.

Figure 1 shows the dependence of a change in the pH of the eluates from the amount of the missed acids, and figure 2 - estimates the dependence of the absorbed oxide amount of acid from the total quantity entered.

Curve 1 is a plot of an abrupt change in pH from 4 to 1.28. This plot is based on figure 2 corresponds to the region of change of the absorbed amount of acid from the mp0=3,2·10-4to mpTo=3,95·10-4mol per 1 g of the oxide, where the first value corresponds to the beginning of the slow response and the second is its complete cessation. Our studies showed that these distinctive areas with the spike at pH=4 is observed when acid treatment of any chromatographic oxides of both domestic and foreign firms.

Subsequent investigation of the magnitude of adsorption of molybdenum oxide treated with various amounts of acid before slowing its absorption in the range of mp0to mpToshowed that the maximum adsorption is reached when the mass of the acid corresponding to mpTo. At the same time, decreasing the amount of acid to mp0in the lower region, begins to experience a "breakthrough" of molybdenum in the eluate at any adsorbed mass. Hence it was concluded that the starting point of the deceleration of the reaction (m p0) begin to form some new active centers, which is stable chemisorption of molybdenum instead of the less stable physical, is caused by the van-der-Waals forces.

To confirm the expressed provisions the following are the results of experimental determination of sorption capacity under consideration oxide on the number of absorbed them acid. From figure 3 it follows that the maximum adsorption is reached when mpTo=3,95·10-4mol/g, followed by an exponential decrease as approaching mp0=3,2·10-4mol/g Then there is an even sharper decline, which confirms the claimed position.

To obtain this dependence hanging oxides weighing 10 g were directly processed in separate cups to 0.055 m solution of Hcl. The volumes of the solutions were selected with the expectation that they contained the specified amount of acid: 2,6; 3,2; 3,4; 3,7 and 3.95·10-4mol per 1 g of oxide. For sub-samples of 10 g of the total quantity of hydrochloric acid mHClaccordingly accounted for 26; 32; 34; 37 and 3.95·10-4mol, and the volumes of solutions VHCl=mHCl/0,055: 47,3; 58,2; 61,8; 67,3 and 71,8 ml.

Monitoring the progress of the reaction of interaction from its beginning until the cessation was performed using a pH meter. The process is considered complete when the pH of the solution above about what led has reached the value of 4 (1·10 -4mol/l). After that, the solution was filtered, and the oxides were dried at 110°C for 2 h and Then weighed oxides mass 7, 8 g were placed in a chromatographic column prepared and conducted their "charge", passing through them, the portions of 0.2 ml solution polymolybdates,99Mo (pH=3) with the concentration of molybdenum 0.3 g/ml until breakthrough99Mo through the column. After the column was rinsed with water to 20 ml and saline 15 ml

The value of sorption capacity W was calculated by the equation

where A0and AP- volumetric activity99Mo in the original solution polymolybdates and lavage, respectively; V1- the volume passed through the column of solution polymolybdates; V2- the volume of wash water.

Subsequent elution of the resulting generators saline solution with a volume of 20 ml showed that the molybdenum content in the product is isolated from the generator with a maximum adsorption capacity of alumina reached when processing mHCl=3,95·10-4mol per 1 g of the oxide is 0.1 mcg/ml at the rate of 0.2 µg/ml, and if mHCl=3,210-4mol per 1 g of the oxide - 2.7 µg/ml.

The proposed method allows to optimize conditions for the preparation of sorbents and to prevent leakage of molybdenum in the eluate.

The method of making chromatographic generator those who ecia-99m from neutron-irradiated molybdenum-98, including processing of alumina acid, making hanging alumina chromatographic column and the subsequent application of a solution of molybdenum, wherein the pre-determined limit of the specific gravity of the acid mptorequired for a complete cessation of its interaction with alumina, and then handle all the aluminum oxide acid of calculation:
mHCl=mpto·mOX,
where mHClthe amount of acid required for the processing of aluminum oxide with a mass mOX.



 

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