Solid polymer sorbent for separation of fission molybdenum-99 from irradiated by neutrons uranylacetate solution and method thereof

 

(57) Abstract:

The invention can be used in nuclear industry for separation of fission molybdenum-99 from the uranyl sulfate solution (UO2SO43H2O) for medical purposes. The essence of the invention: sorbent has the following structural formula:

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where R is styrene, Piracicaba acid or vinyl acetate; X - HOC6H4OH, HOC2H4C2H4OH, H2N(CH2)NH2, HOCH2CH(OH)CH2OH, HOC2H4OH. Sorbent joint is obtained by polycondensation of a copolymer of maleic anhydride, a bifunctional organic compounds (hydroquinone, diethylene glycol, diamine, glycerol, etc. and benzoyloxy in molar ratios 1: (0,25-5):(0,75-0,5) when heated in a polar solvent. The sorbent has a high selectivity, thermal and radiologically. 2 S. and 2 C.p. f-crystals, 1 Il. 4 table.

The invention relates to sorbents, in particular solid polymeric sorbent, and methods for their preparation to extract radioactive isotopes and can be used in the nuclear industry to obtain fragmentation of Mo-99 from uranylacetate solution (UO2SO43H2O) homogeneous R is hochetsja more than 50% of the annual production of radionuclides. They are mostly used for early disease diagnosis and therapy. One of the main applications of radionuclides in medicine is a reduction in the dose load on the patient, which is achieved by using short-lived radionuclides. However, a small half-life of the nuclide cause difficulties during transportation and storage of isotope production. Therefore, the preferred radionuclides that dominates Mo-99 with a half-life of 6.02 h and convenient to register energy-radiation 140 Kev. Currently, more than 70% of diagnostic tests is carried out with the help of this radionuclide.

Known as a sorbent for separation of fission molybdenum-99 from irradiated solutions-benzoyloxy (-"BO"), having the following structural formula

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[C. F. Hillebrand and other Practical guide for inorganic analysis M. : State. scientific and technical publishing house of the chemical literature, 1967, S. 325-339].

Used the ratio of the deposition reaction is

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"BO" is that it is of sulfuric acid is not enough: Ag, Pb, Hg, Bi, Cu, Cd, As, Sb, Sn, Al, Fe, Ti, Zr, Cr(III), V(IV), Ce, U, Ni, Co, Mg and Zn, and Se, Te, Re, Ru, Ro, Os, Ir and Pt are not deposited, when they n is complex-BO," Mo-99, low sorption rate and low radiation resistance under neutron irradiation, -, -, and-rays.

The technical result of the invention to provide a sorbent with high sorption selectivity of Mo-99, the absence of almost sorption of uranium, with high thermal stability and radiation resistance.

The technical result is achieved by the fact that for the first time synthesized solid polymer sorbent (BOX 2) to highlight the fragmentation of Mo-99 from uranylacetate solution of the General structural formula:

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where R is styrene, an ester of acrylic acid or vinyl acetate;

X = HOCH2CH(OH)CH2OH.

Theoretically and experimentally certain content in the sorbent Boxing-2 C105H97O24N3(M+1783) C, H and N are given in table. 1.

The sorbent obtained by the esterification reaction of a copolymer of maleic anhydride with mesonoxian according to the following scheme:

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Also proposed is a method of obtaining the specified sorbent, consisting in joint polycondensation of a copolymer of maleic anhydride (CMA), a bifunctional organic compounds (BOS) (hydroquinone diethylene glycol, diamine, glycerol, etc. and benzoyloxy (BO) in moorland or toluene) at 90 - 95oC with constant stirring for 1 to 2 hours, subsequent deposition of the sorbent with water and cooled to a temperature of 20 - 25oC, the processing of 3 - to 5-fold excess of cold water, evaporation and grinding the resulting product, the selection of particles with a diameter of 1 to 2 mm. Examples are given in table. 4.

The IR spectrum of the obtained sorbent BOX 2 contains absorption bands characteristic of functional groups: - OH, CH, C=O, COOR, C=N and substituted benzene rings in the areas: 3500 - 3300, 2960 - 2880, 1715, 1650 and 650 cm-1(respectively), which confirms the structure of the obtained compounds.

Sorption by the sorbent elements of uranylacetate solution was determined through the distribution coefficient (Kd). Determination of Kd Mo-99, Tc-C and U-235 were carried out in static conditions. Sorption of elements was carried out under continuous mechanical stirring with the mixer the mixer CB-1 (3000 vibrations/min) at room temperature for 15 minutes During this time of the contact phase sorption of Mo-99 was 93 - 98%.

The number of radioactive elements in the solid phase was determined by the difference between the listed amounts of radioisotopes in the aqueous phase (initial solution) and the remaining number in the aqueous phase after sorption.

The Kd of the items on the sorbent BOXING-2 equals: KdMo= 1048 (BOXING-2P - 134), KdTc=628, KdU=0 (PL. 2), i.e. the output of the Mo-99 is 99,7%, and U-235 is not sorbed.

Extracting Mo-99 on the sorbent BOXING-2 under dynamic conditions was performed in the extraction-chromatographic column. Sorption of Mo was carried out without pressure (gravity). The yield of Mo-99 was 99.7%, Tc-99 was sorbirovtsa by 60.4%, U-235 was not sorbirovtsa (not less than 99.99% remains in solution) (see tab. 2, 3 and drawing).

To determine the radiation resistance BOX 2 was irradiated with three different doses of radiation. Irradiation was performed on Co-source HERE-20 with a capacity of 500 SV/C. it is Established that the maximum dose BOXING-2 should not greatly exceed 9 Mrad.

For violations of the above conditions after deposition of the sorbent with water and cooled to 20-25oC precipitation in the form of a gel, i.e., the reaction of formation of the sorbent is not until the end, resulting in a solid polymer sorbent, claimed as the invention is not formed.

1. Solid polymer sorbent for separation frag Mo 99 from irradiated by neutrons uranylacetate solution based on a complex ester of the copolymer malacetic;

X - HOC6H4OH, HOC2H4C2H4OH, H2N(CH2)NH2, HOCH2CH(OH)CH2OH, HOC2H4OH. 2. A method of producing a sorbent under item 1 joint polycondensation of a copolymer of maleic anhydride, a bifunctional organic compounds and benzoyloxy in molar ratios 1 : (0,25 - 0,5) : (0,75 - 0,5) when heated in a polar solvent at 90 - 95oC with constant stirring for 1 to 2 h, followed by precipitation of the sorbent and cooled to 20 to 25oC, treatment with a 3 - to 5-fold excess of cold water, evaporation and grinding the resulting product, the selection of particles with a diameter of 1 - 2 mm

3. The method according to p. 2, characterized in that as a bifunctional organic compounds using hydroquinone, diethylene glycol or hexamethylenediamine were.

4. The method according to p. 2, characterized in that the polar solvent used dioxane, dimethylformamide or toluene.

 

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