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Manufacturing method of ceramic fuel pellets for fuel elements of nuclear reactor

Manufacturing method of ceramic fuel pellets for fuel elements of nuclear reactor
IPC classes for russian patent Manufacturing method of ceramic fuel pellets for fuel elements of nuclear reactor (RU 2421834):

G21C3/02 - Fuel elements
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FIELD: power industry.

SUBSTANCE: pellets are pressed in two stages; at that, first, pressing of workpiece of internal core of pellet with axial hole is performed from moulding powder of highly-enriched uranium dioxide UO2, which contains alloying additives, by using press mould of smaller diameter. Then, obtained workpiece is put into press mould of larger diameter; after that, the gap formed between workpiece and internal wall of press mould is filled with moulding powder from low-enriched uranium dioxide UO2 for creation of outer layer of pellet and the second pressing stage is performed. It is proposed to obtain moulding powder of low-enriched uranium dioxide UO2 by using water technology including preparation of uranyl nitrate solution, two-stage deposition of ammonium polyuranate with hydrogen nitride, calcination of deposit, and reduction of monoxide-oxide to uranium dioxide UO2. Size of granules of low-enriched powder of UO2 uranium dioxide shall be less than 100 mcm.

EFFECT: higher burnout degree of nuclear fuel.

4 cl, 3 dwg, 2 tbl, 2 ex

 

The present invention relates to the nuclear industry and may find use in the manufacturing of ceramic fuel pellets of uranium dioxide for fuel elements of nuclear reactors.

A known method of making pelletized fuel for fuel cells, including the preparation of press powder of uranium dioxide (UO2), enriched in uranium 235, the phasic mixture with a dry binder and powder nitrous-oxide of uranium (U3O8the pressing of tablets in the matrix, sintering the pellets in a gaseous reducing environment, the dry binder is used which does not contain metal plasticizer in an amount of 0.1%and 0.5% by weight of oxides of uranium (see RF patent №2360308, IPC G21C 3/62 BI No. 18, 2009).

There is also known a method of manufacturing a preformed nuclear fuel (see RF patent №2255386, IPC G21C 3/62), adopted as a prototype, which consists in preparing a press powder, extrusion of pellets, sintering the pellets in a reducing environment by their movement in counter-current movement of the restorative environment. According to the invention in a press powder enter the oxides of aluminum and silicon, which upon sintering the pellets to form the aluminosilicate contributing to the coarsening of grains of uranium dioxide and increases the hardness compensated plasticine is updated.

However, as we know, the quality of fuel pellets of uranium dioxide characterized by their microstructure, including the size and shape of the grain. These parameters significantly affect the performance of the tablets of the oxides of uranium and, therefore, fuel elements (cartridges). In particular, the microstructure depends what quantity of gas products is retained in the fuel, the nature of the interaction of the fuel with the shell. Therefore, to reduce outgassing seek to obtain tablets with a large grain. On the other hand, to reduce the interaction of the fuel with the shell you want finer grain.

The above methods do not allow to obtain tablets with controlled grain size on its periphery and a Central region, and there is no possibility of the radial regulating the content of the fissile isotope that is not possible to increase the degree of burn-up to 80-100 GW·d/t U.

The technical result of the invention aims to obtain a combined ceramic fuel pellets for fuel elements of a nuclear reactor having a controlled grain size and radial distribution of the fissile isotope that will allow for a greater degree of burnout.

The technical result is achieved in that in the method of manufacturing a ceramic fuel pellets for fuel elements is s nuclear reactor, including the preparation of press powder of uranium dioxide UO2in a mixture with a binder, compressing the tablets and their sintering in a reducing environment, the pressing of tablets according to the invention, is carried out in two stages, in this case, initially spend extrusion billet inner core tablets with the axial hole of the press powder of highly enriched uranium dioxide UO2containing alloying elements, using the mold of smaller diameter, then the resulting billet is placed in a mold of larger diameter, after which the gap formed between the workpiece and the inner wall of the mold, fill the press powder from discouraging uranium dioxide UO2to create the outer layer of the tablet and carry out the second stage of pressing, the pressure P1in the first stage does not exceed half of the P2- pressure in the second stage, followed by their sintering in a reducing environment.

According to claim 2, the inner core as alloying additives may contain oxides of Al, Si, Cr, Nb or Ti.

In addition, according to p.3 of the claims of the press-powder low-enriched uranium dioxide UO2offered by water technologies, including the preparation of a solution of uranyl nitrate, the two-stage deposition osakapolice ammonium ammonia, the course of annealing, recovery of nitrous oxide to uranium dioxide UO2while the deposition of paloranta ammonium in the first stage is carried out at pH16,5-6,6, and the second stage at pH29,0-9,5.

According to claim 4 of the formula of the invention the size of the granules of low-enriched powder of uranium dioxide UO2should be less than 100 microns.

This technology of ceramic fuel pellets allows you to get a secure grip of the outer layer of the tablet with its inner core. For any given density of sintered pellets within 95-96% of theoretical density, it is necessary to provide a density of compaction from 48 to 52% of theoretical density. This is achieved by two-stage pressing, the pressure of the inner core of the first stage P1does not exceed 1/2 of the molding core in General, R2.

Below are examples of implementation of the proposed method of manufacture of ceramic fuel pellets.

Example 1. For receiving the inner core of ceramic fuel pellets prepared two uranyl nitrate solution: 1st solution using commercial powder of uranium dioxide UO210%enrichment in235U, the 2nd solution using commercial powder of uranium dioxide UO2depleted by235U. Wasp is doing paloranta ammonium (PUA) was performed in two stages by the method of simultaneous draining to the buffer of two solutions: solution of uranyl nitrate and 22-25%-aqueous solution of NH 4OH. Deposition POIX from the 1st solution in the first stage was carried out at pH1of 6.8-7.0 and the second stage at pH28,0-8,2. Deposition POIX from the 2nd solution in the first stage was carried out at pH16,5-6,6 and the second phase pH29,0-9,5. PH1and pH2are optimal. The obtained precipitation was progulivali to nitrous oxide at a temperature of 650°C. Then pursued recovery of nitrous oxide to UO2hydrogen at 700°C. the uranium dioxide Powder UO2mixed with plasticizer (solution of polyvinyl alcohol (glycerol). To obtain press powder extruded briquettes (checkers) at a pressure of 1.3-1.5 t/cm2. The briquettes were crushed and rubbed through a sieve: press powder of uranium dioxide UO210%enrichment through a sieve with mesh size 400 µm, and press the powder of low-enriched uranium dioxide UO2through a sieve with a mesh size of 100 microns. Using the mold outer diameter of 8.5 mm and an inner diameter of 2.4 mm of powder 10%enrichment pre-compressed billet inner core ceramic fuel pellets at a pressure P1in the range of 1.2-1.3 t/cm2. Then pressed billet inner core ceramic fuel pellets transferred to a second mold having an external diameter of 10 mm Free space between the workpiece and the inner walls of the Oh of the mold was filled with granules of depleted uranium dioxide UO 2and made the second stage of pressing at a pressure P2equal to 2.5 t/cm2. Sintering of pellets was carried out at a temperature of 1750°C in an atmosphere of hydrogen for 3 hours. Characteristics of sintered ceramic fuel pellets are shown in table 1, which shows that the average density of the sintered pellets was of 10.73±0.02 g/cm3that meets the specifications for ceramic fuel pellets.

Figure 1 shows the microstructure (before etching) tablets UO210%enrichment with an outer layer of UO2depleted. The transition boundary from the inner core of ceramic fuel pellets to the external layer is absent, which indicates good adhesion of the outer layer with the inner core. The boundary is shown on a cut this tablet after etching, the microstructure of which is presented in figure 2.

Example 2. For receiving the inner core of ceramic fuel pellets used industrial powder of uranium dioxide UO22%enrichment for the235U made way dry conversion powder No. 1. In powder No. 1 were added oxides of Al, Si and Cr in the amount of less than 0.4 wt.%. For making the outer layer of ceramic fuel pellets used depleted uranium, which was prepared with water rest the R uranyl nitrate. Deposition of paloranta ammonium (PUA) was performed in two stages by the method of simultaneous draining to the buffer of two solutions: solution of uranyl nitrate and 22-25%-aqueous solution of NH4OH, when values of the first stage pH16,5-6,6, and the second stage pH29,0-9,5. The precipitate was probalily to nitrous oxide U3O8at a temperature of 650°C, and then restored to UO2hydrogen at 700°C, the obtained powder No. 2. Each powder of uranium dioxide UO2(No. 1 and No. 2) was mixed with the plasticizer (solution of polyvinyl alcohol (glycerol). To obtain press powder initially extruded briquettes (checkers) at a pressure of 1.3-1.5 t/cm2. The briquettes were crushed and rubbed through a sieve: uranium dioxide UO2No. 1 is through a sieve with mesh size 400 µm, and then uranium dioxide UO2No. 2 through a sieve with a mesh size of 100 microns. Using the mold with an outer diameter of 8.5 mm and an inner diameter of 2.4 mm pre-compressed from powder No. 1 billet inner core ceramic fuel pellets at a pressure P1in the range of 1.2-1.3 t/see Then the preparation was transferred to a second mold having an external diameter of 10 mm Free space between the workpiece and the inner wall of the mold filled with the granulate of depleted uranium dioxide UO2(powder No. 2) and made a second pressing at a pressure P1that is equally the m 2.5 t/cm 2. Sintering of pellets was carried out at a temperature of 1750°C in a reducing atmosphere of hydrogen for 3 hours. Characteristics of sintered pellets are shown in table 2, from which it follows that the average value of the density is 10.63±0.02 g/cm3that meets the specifications for ceramic fuel pellets.

Figure 3 presents the microstructure of the ceramic fuel pellets UO2, 2%enrichment for the235U with an outer layer of UO2,depleted by235U. the transition Boundary from the inner core of ceramic fuel pellets to the outer layer shows better adhesion of the outer layer with the inner core.

Thus, the proposed method is compared with previously known allows to obtain a composite ceramic fuel pellets for fuel elements of a nuclear reactor having a controlled grain size and radial distribution of the fissile isotope that will allow for a greater degree of burnout.

td align="center" namest="c4" nameend="c5" rowspan="1" colspan="1"> Density, g/cm3
Table 1.
No. of tablets. The external diameter, mm Internal diameter, mm Height, mm Shrinkage, %
geometric hydrostatic
1 to $ 7.91 1,9 6,89 10,28 10,71 20,90
2 to 7.93 1,9 6,89 10,36 10,75 20,70
3 7,99 1,9 6,98 10,35 a 10.74 20,10
4 to 7.93 1,9 6,99 10,31 of 10.73 20,70

Table 2.
No. tablet The external diameter, mm Internal diameter, mm Height, m the Hydrostatic density, g/cm3
1 8,0 1,9 6,92 10,65
2 of 8.06 1,9 6,95 or 10.60
3 8,04 1,9 6,93 10,63

1. A method of manufacturing a ceramic fuel pellets for fuel elements of a nuclear reactor, including the preparation of press powder of uranium dioxide UO2in a mixture with a binder, compressing the tablets and their sintering in a reducing environment, wherein the pressing of tablets is carried out in two stages, in this case, initially spend extrusion billet inner core tablets with the axial hole of the press powder of highly enriched uranium dioxide UO2containing alloying elements, using the mold of smaller diameter, then the resulting billet is placed in a mold of larger diameter, and the gap formed between the workpiece and the inner wall of the mold, fill the press powder of low-enriched dioxide from the Ana UO 2for the formation of the outer layer of the tablet and carry out the second stage of pressing, the pressure P1in the first stage does not exceed half of the P2- pressure in the second stage, followed by their sintering in a reducing environment.

2. The method according to claim 1, characterized in that the inner core as alloying additives contains oxides of Al, Si, Cr, Nb or Ti.

3. The method according to claim 1, characterized in that the press-powder low-enriched uranium dioxide UO2receive by water technologies, including the preparation of a solution of uranyl nitrate, the two-stage deposition of sediment paloranta ammonium ammonia, the course of annealing, recovery of nitrous oxide to uranium dioxide, with the deposition of paloranta ammonium in the first stage is carried out at pH16,5-6,6, and the second stage at pH29,0-9,5.

4. The method according to claim 1 or 3, characterized in that the granule size of low-enriched powder of uranium dioxide UO2is less than 100 μm.

 

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