Method of converting waste uranium hexafluoride into uranium metal

FIELD: chemistry.

SUBSTANCE: invention relates to ecology and is aimed at preventing environmental pollution and radiation poisoning. The method of converting waste uranium hexafluoride into uranium metal and calcium fluoride involves reaction of uranium hexafluoride and calcium metal, where gaseous uranium hexafluoride is fed into molten calcium metal by bubbling, and operating temperature is kept higher than the melting point of calcium fluoride.

EFFECT: invention enables conversion of toxic radioactive uranium hexafluoride into an non-volatile compact product which is safe for storage.

1 ex


The invention relates to the field of ecology, it is aimed to prevent the possibility of pollution and poisoning of the population with radioactive substances.

The separation of uranium isotopes, resulting in two fractions: enriched with isotope235U more to 0.72 wt.% and moldboard, which contains 0.1 to 0.3 wt.%235U.

Talking uranium hexafluoride is stored in containers, mostly in open areas. This represents a significant risk to the environment and population. As a result of corrosion during long-term storage, the action of natural phenomena (storm, earthquake), as well as sabotage and bombing can disrupt the integrity of part of the container and the environment will be hexafluoride uranium is radioactive, poisonous gas, having a stifling effect that can lead to mass poisoning of the population.

A method of refining uranium hexafluoride in tetraploid uranium, [Fsatom, Damluji, Vulgarities Nuclear fuel based on enriched uranium, Atomizdat, M., 1966, p.42-47]. According to this method through the nozzle type "pipe in pipe" on the outside of the reactor is hydrogen, and then through the interior of the nozzle begin to apply a mixture of uranium hexafluoride and fluorine, and fluorine is supplied to achieve the desired temperature. The origin is W ill result in the following response:

UF6(gas)+H2(gas)→UF4(TV.)+2F(gas)ΔN329=-280 kJ/mol;

F2(gas)+H2(gas)→2F(gas)That ΔN298=-268 kJ/mol.

Excess hydrogen 100-500%, the flow rate of the fluorine 20-32 g/kg UF6, 90% received UF4settles at the bottom of the hopper, UF4carried by the gases is captured cermet filters.

The disadvantage of this method is to obtain free-flowing powdery product of relatively low density (ρ(UF4)=6.7 g/cm3), which makes its storage.

There is a method of conversion of depleted uranium hexafluoride to uranium oxide (U3O8by high-temperature pyrohydrolysis [Proven management for depleted uranium: the French reference of Cogema's defluorination plant / P.Netter, B.Dupperret, B.Le Motais. International Conferences "Decomissioning, decontamination and reutilization of commercial and government facilities". Knoxville, USA, September 12-16, 1999. - 11 R.].

The disadvantage of this method is the high energy intensity of the process and the final product in powder form, which can worsen the ecological situation in the case of damage to the packaging.

A known method of converting uranium hexafluoride in tetrafide uranium and anhydrous hydrogen fluoride and device for its implementation (patent RU No. 2188795 C2 from 23.11.2000).

The invention can be used for processing of depleted uranium hexafluoride. The method consists in collaboration the AI of uranium hexafluoride with hydrogen in hydrofluoric flame. The process is conducted in a reactor at a pressure in it 540-720 mm Hg Molar ratio of the components UF6:F2: H2=1:(0,12-0,36):(1,5-3). As a reducing agent can be used cathode gas.

The temperature of the walls of the reactor support about 480°C. Cooling of the reaction products is carried out by cooling the walls of the reactor. Powder tetrafluoride uranium auger-feeder discharge device is moved to the receiver of the finished product. Body discharge device made in the form of a vertical oval. Hydrogen fluoride from the process gases condense at the temperature (-35)-(-40)°C and (-70)-(-80)°C. Additionally remove HF sodium fluoride at temperatures of 70-80°C and 20-30°C. the Desorption of hydrogen fluoride is carried out at a temperature of 350-375°C. The invention: the degree of conversion of uranium hexafluoride in tetraploid uranium up to 99.5%. The degree of extraction of hydrogen fluoride to 99.6%.

The disadvantage of this process is that the final product is a powdery product - tetraploid uranium in the accident and pollutes the atmosphere, and hydrosphere.

A method of obtaining powder of uranium dioxide of uranium hexafluoride (patent RU 2381993 from 16.01.2008), including the filing in a pre-heated reaction zone of the reaction chamber of uranium hexafluoride and steam, feeding the second of reaction the th zone of the reaction chamber a mixture of water vapor and hydrogen transfer in this area uranylnitrate to uranium dioxide the discharge of powder from the reaction chamber dovolenkovania unreacted uranylnitrate. The resulting powder was cooled and stabilized with a mixture of air and nitrogen.

The disadvantage of this method is:

- multi-stage operations;

the end product is obtained in powder form, which complicates storage and gives the possibility of environmental pollution.

A known method of recovering uranium hexafluoride adopted for the prototype (patent RU №2204529 C2 from 28.03.2001).

The invention relates to methods for recovery of uranium hexafluoride to the lowest fluoride and uranium metal and can be used in the processing of depleted uranium hexafluoride. The result of the way: the possibility of obtaining a product of a given composition and the implementation of reduction reaction of uranium hexafluoride at a lower temperature.

Recovery UF6carry out pre-comisioane hydrogen in the chemical reactor in a mixture with a buffer gas-diluent continuous spontaneous combustion. Atomic hydrogen is produced by mixing in the flow of molecular hydrogen in excess of the molecular fluorine ignited in the burner unit, so that the excess molecules of fluorine thermally dissociates into atoms of fluorine. Recovery UF6 is carried out to uranium metal at a ratio of conc the Nations of atomic hydrogen and UF6 molecules in the mixture, fed to the reactor, 6:1, respectively. Recovery of UF6 to carry tetrafluoride uranium at a ratio of concentrations of atomic hydrogen and molecular UF6in the mixture fed to the reactor, 2:1, respectively.

The disadvantage of this method is metallic uranium is obtained in the form of fine pyrophoric powder is not suitable for storage.

The objective of the invention is the transfer of toxic radioactive uranium hexafluoride in non-volatile compact product - uranium metal ingot, not having vysokopronitsaemogo gamma activity.

A method of converting waste uranium hexafluoride to uranium metal includes the interaction of uranium hexafluoride and metallic calcium. Gaseous uranium hexafluoride is introduced into the molten metal calcium by sparging. The temperature of the process for obtaining a compact ingot uranium is supported above the melting point of calcium fluoride.

Proposed in the present invention method has several advantages: the product of the process is a compact ingot of metallic uranium, which occupies a small volume (the density of α-uranium 19,05 g/cm3). The resulting product nesius, Neleus (the boiling point of uranium metal 3813°C). In addition to uranium ingot obtained slag consisting of calcium fluoride, which you can use to acquire the Oia of fluoride.

The translation process of uranium from waste hexafluoride urn in uranium metal is proposed to carry out by bubbling gaseous uranium hexafluoride through the molten metal by the reaction of calcium

The reaction is practically irreversible, because the change in free energy of the process is more negative -1440 kJ/mol.

In the process releases a significant amount of heat (ΔH=-1520,6 kJ/mol), which will provide the course of the reaction without the supply of external heat.


In the apparatus, which is a cylindrical vessel with a lid flange is loaded metal calcium, then the device is sealed, it is pumped out the air, after which it is filled with argon. The apparatus is moved into a furnace and heated to melt the calcium. The heating is turned off, and through the pipe in the upper part of the melt of calcium is served gaseous uranium hexafluoride from heated sublimator. The number Bartiromo of uranium hexafluoride shall not exceed 95% of the stoichiometric amount for reaction with the loaded amount of calcium.

Under these conditions, the reaction products according to their densities are distributed in the following order: bottom layer - melt uranium metal, the middle layer of the molten slag (Ca 2), the upper layer of excess calcium.

After cooling and crystallization of the reaction products are extracted from the reactor and share: ingot uranium metal is deposited, the slag - receiving fluoride, metal calcium reuse.

A method of converting waste uranium hexafluoride into uranium metal and calcium fluoride, including the interaction of uranium hexafluoride and metallic calcium, and gaseous uranium hexafluoride is introduced into the molten metal calcium through sparging, the process temperature is maintained above the melting point of calcium fluoride.


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EFFECT: invention allows to enhance the process efficiency and obtain uranium hexafluoride of 99,9% purity.

1 tbl

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