WO2007097607A1 - Procédé de production de combustible d'uranium-erbium céramique nucléaire - Google Patents

Procédé de production de combustible d'uranium-erbium céramique nucléaire Download PDF

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Publication number
WO2007097607A1
WO2007097607A1 PCT/KZ2006/000014 KZ2006000014W WO2007097607A1 WO 2007097607 A1 WO2007097607 A1 WO 2007097607A1 KZ 2006000014 W KZ2006000014 W KZ 2006000014W WO 2007097607 A1 WO2007097607 A1 WO 2007097607A1
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WO
WIPO (PCT)
Prior art keywords
erbium
uranium
fuel
uranium dioxide
nuclear
Prior art date
Application number
PCT/KZ2006/000014
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English (en)
Russian (ru)
Inventor
Sergei Vladimirovich Bezhetskiy
Anatoliy Andreevich Kuchkovskiy
Igor Vladimirovich Korobeinikov
Anton Vladimirovich Manych
Natalya Aleksandrovna Marakhovets
Andrey Yurievich Rufin
Elena Fedorovna Stolbova
Galina Mikhaylovna Shevchenko
Original Assignee
Ulba Metallurgical Plant Joint-Stock Company
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Publication date
Application filed by Ulba Metallurgical Plant Joint-Stock Company filed Critical Ulba Metallurgical Plant Joint-Stock Company
Publication of WO2007097607A1 publication Critical patent/WO2007097607A1/fr

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Classifications

    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42—Selection of substances for use as reactor fuel
    • G21C3/58—Solid reactor fuel Pellets made of fissile material
    • G21C3/62—Ceramic fuel
    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/42—Selection of substances for use as reactor fuel
    • G21C3/58—Solid reactor fuel Pellets made of fissile material
    • G21C3/62—Ceramic fuel
    • G21C3/623—Oxide fuels
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00—Energy generation of nuclear origin
    • Y02E30/30—Nuclear fission reactors

Definitions

  • the invention relates to nuclear engineering, in particular, to the production of fuel elements for power reactors that use nuclear fuel based on uranium dioxide with the addition of erbium as a burnable absorber.
  • the active zones of water-cooled nuclear reactors are formed from fuel assemblies containing fuel of various compositions with the addition of a burnable absorber, which makes it possible to compensate for reactivity, equalize energy release over the core volume and maintain the temperature coefficient of reactivity at a given level.
  • RBMK reactors use erbium, which is introduced as an erbium oxide powder directly in the manufacture of fuel pellets.
  • uranium-erbium fuel Another problem of uranium-erbium fuel is that the presence of erbium, mechanically mixed with uranium dioxide powder, negatively affects the properties of the fuel itself, this manifests itself in a decrease in density, an increase in open porosity, and a decrease in
  • a method of manufacturing nuclear fuel is that. in a mixer, in particular a blade type, a two-component mixture of uranium dioxide and oxide is prepared
  • the uniform distribution of erbium in uranium is determined by the particle size of the powders, the size of which varies from a few to hundreds of microns);
  • the objective of the present invention is to increase the uniformity of the distribution of erbium in the fuel tablet at the macro and micro levels.
  • the technical result consists in improving the operational properties and characteristics of nuclear fuel (density, porosity, grain size), the possibility of expanding the range of erbium content in it.
  • the essence of the invention lies in the fact that, in contrast to the known method for producing nuclear ceramic uranium-erbium fuel, which consists in the standard technology for producing uranium dioxide powder by the ADU process, namely, the precipitation of ammonium diuranate, its drying, thermal decomposition, recovery , and preparing 25 a two-component mixture of uranium dioxide with erbium oxide by mechanical mixing of the components in a predetermined ratio, pressing and sintering the resulting mixture, in the proposed method before precipitation of diures erbium nitrate or another water-soluble salt of erbium is introduced into a solution of uranyl nitrate, and erso, a bi-containing powder of uranium dioxide, is pressed and sintered.
  • the proposed method of mixing uranium and erb> iy allows to obtain a highly homogeneous mixture of two components. Given the likeness the properties of uranyl and erbium ions (close ionic radii and densities of solutions, complete ionization and solubility at pH ⁇ 3), the homogenization of erbium and uranyl ions in a solution occurs rather quickly when the solution is mixed or pumped. After stirring at
  • the uranium dioxide powder is not broken, all the characteristics of the fuel pellet obtained by technology without the addition of erbium are preserved.
  • the inventive method allows to obtain tablets of nuclear fuel having a density, average grain size, uniformity in the distribution of grain size is at least the same as a tablet without the addition of erbium.
  • a solution of any erbium salt can be used to introduce erbium into a solution of uranyl nitrate, the anions of which decompose without heat and do not pollute uranium dioxide with limited impurities.
  • These salts may be, for example, nitrates, citrates, acetates, etc.
  • the range of erbium content in nuclear fuel can be expanded to be from 0.02 to 3 wt.% Without deterioration of fuel characteristics, while in the prototype the range is limited from 0.46 to 0.64 wt.% For erbium.
  • the labor costs for implementing the method significantly increase, namely, the number of stages of intermediate mixing increases.
  • Erbium was introduced into a uranyl nitrate solution (industrial reextract) with a uranium concentration of 74.5 g / L as an erbium nitrate solution with an erbium concentration of 9.79 g / L (20.8 g / L by erbium nitrate).
  • the calculation of the volume of the erbium solution was carried out to obtain the erbium content in uranium dioxide of 0.02 + 0.002 wt.%.
  • the composition of the resulting solution U - 74.5 g / l, Er - 0.017 g / l.
  • the erbium-containing ammonium polyuranate was calcined at a temperature of 650 ° C.
  • the uranium dioxide powder after hydrogen reduction with uranium oxide contained 0.019 wt.% Erbium.
  • Erbium was introduced into an industrial re-extract with a uranium concentration of 70 g / l in the form of a solution of erbium acetate with a concentration of 10 g / l (20.5 g / l for erbium acetate).
  • the calculation of the volume of the erbium solution was carried out to obtain the erbium content in uranium dioxide - 0.60 ⁇ 0.03 wt.%.
  • the composition of the obtained f ⁇ solution L) - 67 g / l, Er - 0.46 g / l.
  • the precipitation of ammonium polyuranate and its calcination was carried out analogously to example 1.
  • the uranium dioxide powder after reduction with hydrogen of uranium oxide-uranium contained 0.58 wt.% Erbium.
  • uranium dioxide powder containing erbium was subjected to 15 compaction in a vibration mill together with a modifying additive: uranium oxide oxide powder containing 0.60 wt.% Erbium, in terms of uranium dioxide in an amount of 5%. Plasticizer was not administered.
  • the characteristics of the obtained fuel pellets and the erbium content in them are shown in table 1.
  • Erbium was introduced into a uranyl nitrate solution (industrial re-extract) with a uranium concentration of 74.5 g / l as an erbium nitrate solution with an erbium concentration of 45 g / l (95.7 g / l by erbium nitrate).
  • the calculation of the volume of the erbium solution was carried out to obtain the erbium content in uranium dioxide - 2.8 ⁇ 0.2%.
  • the composition of the resulting solution U - 70.8 g / l, Er - 2.26 g / l.
  • uranium dioxide powder contained 2.75 wt.% Erbium.
  • a two-component mixture of uranium dioxide and erbium oxide powders was prepared in a laboratory drum mixer from 5 kg of uranium dioxide and 34.31 g of erbium oxide. Averaging time ZOmin. Before mixing, a “rich” mixture was prepared manually, containing all erbium oxide and 1, 67 kg of uranium dioxide. Then a press powder was prepared by compacting the mixture in a vibrating mill, mixing with plasticizer and granulation. Spent pressing and sintering of the compacts. Sintered tablets were ground and characteristics were determined: density, open porosity, grain size and erbium content. The results are presented in table 1.
  • a press powder was prepared from powder 15 of uranium dioxide without the addition of erbium. Spent pressing and sintering of the compacts. Sintered tablets were ground and their characteristics were determined: density, open porosity, grain size. The results are presented in table 1.
  • the fuel pellets 20 obtained by the present method have a more uniform grain structure, lower porosity and higher density compared to the prototype.
  • the introduction of erbium into uranium dioxide powder in the form of Er 2 O 3 powder by mechanical means led to the appearance of an uneven grain structure.
  • clusters of small 25 grains 1-3 microns in size are clearly distinguished.
  • Preparation of uranium-erbium fuel in accordance with the claimed method helps reduce the cost of 10-15%, the acquisition and maintenance of equipment portion preparation press ⁇ powders and tablets, to reduce the energy and labor costs.
  • the number of rejects and i production turns will decrease.
  • Patent RU Ns2141693. The fuel assembly of a water-cooled nuclear reactor. IPC G21C 3 / 02.3 / 62.3 / 64, 1998.
  • Patent RU Ns2142170 Nuclear Fuel Tablet, IPC G21C ; 3/02.3 / 62.3 / 64.1998.
  • Patent RU N ° 2157568 Nuclear fuel tablet, IPC G21C 3/62, 0 3/02, 1999.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Chemical & Material Sciences (AREA)
  • Ceramic Engineering (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)

Abstract

La présente invention relève du domaine des techniques nucléaires et concerne en particulier la production d'éléments combustibles pour des réacteurs de puissance dans lesquels on utilise un combustible nucléaire à base de dioxyde d'uranium dont l'absorbeur consommable se présente sous la forme d'oxyde d'erbium. L'absorbeur consommable est traditionnellement ajouté par mélange mécanique de poudres de dioxyde d'uranium et d'oxyde d'erbium. Ce procédé se caractérise en ce que de l'erbium est ajouté à la poudre de dioxyde d'uranium par voie chimique, autrement dit lors de la production de la poudre de dioxyde d'uranium, une quantité donnée de solution de nitrate d'erbium ou d'une autre solution de sel d'erbium hydrosoluble étant ajoutée à une solution de nitrate d'uranyle avant le dépôt de diuranate d'ammonium. Une poudre de dioxyde d'uranium contenant de l'uranium et de l'erbium, pouvant être utilisée pour produire des pastilles combustibles, est ensuite obtenue au moyen d'une technique connue. Le procédé de cette invention permet d'exclure l'opération de mélange mécanique des poudres d'oxydes de deux composants, de garantir une parfaite homogénéité de la répartition des composants les uns dans les autres, et d'améliorer les caractéristiques des pastilles combustibles, telles que la densité, le calibre moyen des grains et l'uniformité de la répartition des grains par taille. Les caractéristiques du combustible d'uranium-erbium nucléaire pouvant être produit par ce procédé permettent d'obtenir de meilleures valeurs (libération de gaz réduite, taux de combustion plus élevé, etc.) pendant son exploitation dans des réacteurs nucléaires, tels que les réacteurs RBMK.
PCT/KZ2006/000014 2006-02-20 2006-11-09 Procédé de production de combustible d'uranium-erbium céramique nucléaire WO2007097607A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KZ20060196 2006-02-20
KZ2006/0196.1 2006-02-20

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WO2007097607A1 true WO2007097607A1 (fr) 2007-08-30

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB847013A (en) * 1957-06-04 1960-09-07 Us Of America Atomic Energy Co Fuel element composition and process of making same
EP0076680A1 (fr) * 1981-10-02 1983-04-13 Westinghouse Electric Corporation Procédé de production de pastilles stables de combustible de bioxyde d'uranium
RU2157568C1 (ru) * 1999-11-26 2000-10-10 Открытое акционерное общество "Машиностроительный завод" Таблетка ядерного топлива

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB847013A (en) * 1957-06-04 1960-09-07 Us Of America Atomic Energy Co Fuel element composition and process of making same
EP0076680A1 (fr) * 1981-10-02 1983-04-13 Westinghouse Electric Corporation Procédé de production de pastilles stables de combustible de bioxyde d'uranium
RU2157568C1 (ru) * 1999-11-26 2000-10-10 Открытое акционерное общество "Машиностроительный завод" Таблетка ядерного топлива

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