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WO1995008827A1 - Corps fritte de combustible nucleaire et son procede de production - Google Patents

Corps fritte de combustible nucleaire et son procede de production Download PDF

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Publication number
WO1995008827A1
WO1995008827A1 PCT/EP1994/003060 EP9403060W WO9508827A1 WO 1995008827 A1 WO1995008827 A1 WO 1995008827A1 EP 9403060 W EP9403060 W EP 9403060W WO 9508827 A1 WO9508827 A1 WO 9508827A1
Authority
WO
WIPO (PCT)
Prior art keywords
nuclear fuel
sintered body
surface film
boron
particles
Prior art date
Application number
PCT/EP1994/003060
Other languages
German (de)
English (en)
Inventor
Gerhard Gradel
Alfons Roppelt
Martin Peehs
Harald Cura
Klaus Koebke
Erhard Ortlieb
Richard A. Perkins
Original Assignee
Siemens Aktiengesellschaft
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Siemens Aktiengesellschaft filed Critical Siemens Aktiengesellschaft
Priority to JP7509538A priority Critical patent/JPH09503858A/ja
Priority to EP94926937A priority patent/EP0720766A1/fr
Publication of WO1995008827A1 publication Critical patent/WO1995008827A1/fr
Priority to KR1019960701486A priority patent/KR960705324A/ko

Links

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
    • 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
    • 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
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S376/00—Induced nuclear reactions: processes, systems, and elements
    • Y10S376/90—Particular material or material shapes for fission reactors
    • Y10S376/901—Fuel

Definitions

  • the invention relates to a nuclear fuel sintered body according to claim 1, a nuclear reactor fuel element according to claim 13 and a method for producing a nuclear fuel sintered body according to claim 14.
  • EP-A1-0 239 843 discloses a nuclear fuel sintered body made of U ⁇ 2 (U, Pu) ⁇ 2 and (U, Th) ⁇ 2.
  • This known nuclear fuel sintered body is obtained by producing a mixture of uranium oxide powder or uranium mixed oxide powder with uranium boride or boron carbide powder and pressing it into compacts, which are then sintered in a sintering furnace in a reducing sintering atmosphere to form nuclear fuel sintered bodies.
  • the boron is thus distributed uniformly everywhere in the sintered matrix.
  • Boron in uranium-containing nuclear fuel sintered bodies is a neutron absorber that can be burned off in terms of physical physics and, after a certain period of use, these nuclear fuel sintered bodies lose their property as an absorber for thermal neutrons in a nuclear reactor.
  • Nuclear reactor fuel elements with fuel rods which contain uranium-containing nuclear fuel sintered bodies are used in the nuclear reactor, for example, during four successive, generally equally long fuel element cycles. At the end of a fuel element cycle, some of the nuclear reactor fuel elements in the nuclear reactor are replaced by fresh, unirradiated nuclear reactor fuel elements.
  • the fresh, unirradiated nuclear reactor fuel elements would bring about a relatively high reactivity in the nuclear reactor compared to the already irradiated nuclear reactor fuel elements.
  • the boron in the nuclear fuel sintered bodies of these fresh, unirradiated nuclear reactor fuel elements initially dampens the reactivity brought about by these nuclear reactor fuel elements by initially absorbing thermal neutrons.
  • the nuclear fuel of fresh and unirradiated nuclear reactor fuel elements gradually burns off in the nuclear reactor by nuclear fission, but at the same time a combustible neutron absorber present in this nuclear fuel gradually burns off neutron physically, so that this neutron absorber finally has little or no thermal energy Neutrons absorb. That is why even freshly inserted unirradiated nuclear reactor fuel elements in the nuclear reactor can have about the same reactivity in the nuclear reactor during their entire service life in the nuclear reactor as the nuclear reactor fuel elements that have already undergone a fuel element cycle in the nuclear reactor.
  • Boron as a neutron absorber in the nuclear fuel is compared to other combustible neutron absorbers such as rare earths
  • the fuel element cycles are relatively long, e.g. are longer than 12 months, since boron prevents heat build-up in the nuclear fuel.
  • the invention is based on the object of developing the known nuclear fuel sintered body so that there is no increase in reactivity which is too rapid and too high when starting up a nuclear reactor if this nuclear fuel sintered body is freshly introduced into this nuclear reactor in the unirradiated state .
  • the particles of boron or a chemical boron compound with a are provided surface film that holds back boron, this boron cannot escape from the nuclear fuel sintered body according to the invention. This ensures an increase in reactivity which is damped with regard to its speed and height.
  • the surface film advantageously contains no boron at all.
  • Claims 2 to 12 are directed to advantageous further developments of the nuclear fuel sintered body according to claim 1.
  • the further development according to claim 9 ensures good retention of boron
  • the further development according to claim 10 ensures a largely uniform distribution of the particles of boron or chemical boron compound in the sintered matrix of the nuclear fuel sintered body enables.
  • Claim 13 relates to a nuclear reactor fuel element with a fuel rod which contains such a nuclear fuel sintered body in a cladding tube.
  • the method according to claim 14 allows a relatively simple production of a nuclear fuel sintered body which contains particles of boron and / or a chemical boron compound provided with the surface film.
  • Claims 14 and 15 are directed to advantageous developments of this method.
  • UO2 powder is used as the powdered starting oxide and is obtained, for example, in accordance with the ammonium uranyl carbonate or AUC process (for example, Gemelin Handbook of Inorganic Chemistry, Uranium, Supplement Volume A3, 1981, pplOl to 104).
  • This U ⁇ 2 "powder has an average particle diameter of 15 to 20 .mu.m.
  • the U ⁇ 2 ⁇ powder can also by another method, such as the ammonium diuranate (ADU) process (e.g.
  • crystalline boron powder 300 ppm of crystalline boron powder, the average particle diameter of which is 20 to 25 ⁇ m, is added to the U ⁇ 2 ⁇ powder.
  • the particles of this crystalline boron powder have a surface film made of metallic molybdenum, the film thickness of which is approximately 5 ⁇ m. This surface film is in a sputtering device (e.g. E. Lang, "Coatings For High Temperature
  • the sputtering device has an electrically conductive anode body, for example made of aluminum, on which crystalline boron powder was located. Furthermore, a cathode body is made of The crystalline starting boron powder with a mean starting particle size of about 15 ⁇ m is treated between anode and cathode body in a argon atmosphere at a direct electrical voltage of about 2000 V during a sputtering time of about 2.
  • the crystalline boron powder rolls again and again during this sputtering on an inclined plane from the anode body, so that a uniformly thick, firmly adhering and all-round dense surface film of molybdenum is achieved on the boron powder particles.
  • the surface film can also consist of at least one of the metals, ruthenium, tungsten and chromium or of at least one of the alloys molybdenum-based alloy, ruthenium-based alloy, tungsten-based alloy and chromium-based alloy. It is favorable if this surface film from a
  • Chromium-nickel alloy or a molybdenum-niobium alloy exists.
  • the metals of these two alloys all have one relatively small capture cross section for thermal neutrons.
  • the metals rhenium, rhodium and hafnium and the base alloys of these metals are also suitable for the surface film, since these metals have a large initial cross section for thermal neutrons, but do not burn out neutron physically as quickly as boron Therefore, in conjunction with boron, particularly long fuel element cycles are possible.
  • the surface film can also consist of at least one of the non-metals tantalum carbide, niobium carbide, titanium carbide, tantalum carbide, niobium carbide, titanium carbide, zirconium carbide, chro carbide, vanadium carbide, tungsten carbide, molybdenum carbide, tantalum nitride, niobium nitride, titanium nitride, zirconium nitride, zirconium nitride Vanadium silicide, tungsten silicide, molybdenum silicide, zirconium silicide, magnesium oxide, beryllium oxide, chromium oxide, calcium oxide, cerium oxide and zirconium oxide exist.
  • the surface film consists of at least one of the substances silicon carbide and silicon nitride, preferably Si3N4.
  • the capture cross section for thermal neutrons of these non-metals is particularly small.
  • These non-metals are advantageously applied in the form of a surface film to the boron powder particles by precipitating the reaction product of a chemical gas phase reaction of chemical compounds which contain the components of the surface film (for example chemical vapor deposition (CVD) processes according to E. Lang , “Coating For High Temperature Applications", 1983, Applied Science Publishers, London and New York, pp.33 to 78). In this way, however, a metallic surface film can also be applied to the boron powder particles.
  • CVD chemical vapor deposition
  • 0.2% by weight of powdered zinc stearate is also added to the UO2 powder with the added crystalline boron powder as a pressing aid.
  • powdered aluminum distearate can also be used as a pressing aid.
  • the UO2 powder with the added boron powder and the added pressing aid is then mixed intimately in a tumbling mixer for 15 minutes.
  • about 5% powdered U3O3 can be added to the powder in the tumble mixer as a pore former.
  • compacts are pressed from the mixture obtained by intimate mixing, which are sintered in a hydrogen atmosphere at a sintering temperature of 1750 ° C. for three hours.
  • the nuclear fuel sintered bodies After cooling, the nuclear fuel sintered bodies have a specific density of approximately 10.30 g / cm 3 to 10.55 g / cm 3 while the specific density of the boron particles in the sintered matrix is 7 to 9 g / cm 3 , that is to say in the favorable range of 5 g / cm 3 to 10 g / cm 3 .
  • Boron analysis of the nuclear fuel sintered bodies after sintering shows a boron concentration of 295 ppm, that is to say only a very small boron loss within the measuring accuracy.
  • the equivalent diameter of the boron particles (diameter of a sphere whose spherical volume is equal to the boron particle volume) in the sintered matrix is in the favorable range from 5 ⁇ m to 300 ⁇ m.
  • the thickness of the surface film on these boron particles, which consists of a different material than the sinter matrix and the boron particles is in the favorable range from 0.3 ⁇ m to 30 ⁇ m.
  • Such boron particles show practically no tendency to segregate, in particular in UO2 powder which has been obtained by the processes indicated above. No boron escapes from them during sintering.
  • the boron concentration in the sinter matrix of the nuclear fuel sintered body is in the range from 100 ppm to 10,000 ppm; because on the one hand a strong damping of the speed and amount of the increase in reactivity can be achieved in a nuclear reactor into which such nuclear fuel sintered bodies are introduced as part of a fresh nuclear reactor fuel element, but on the other hand the formation of cracks in the sintered matrix of the nuclear fuel sintered body is avoided.
  • the isotope B] _Q in the boron in the boron or in the boron-containing chemical compounds used is enriched compared to the natural isotope composition of boron. This can be achieved in a known manner, for example by cyclotron, diffusion or separation nozzle enrichment. This isotope B I _ Q practically absorbs the thermal neutrons. Due to its accumulation in the boron, which is located in the sintered matrix of the nuclear fuel sintered body, the concentration of this boron can be chosen to be relatively low.
  • a nuclear reactor fuel element for a nuclear reactor.
  • a nuclear reactor fuel element is advantageously provided for a light water nuclear reactor, in particular for a pressurized water nuclear reactor or a boiling water nuclear reactor.

Landscapes

  • 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)
  • Powder Metallurgy (AREA)
  • Monitoring And Testing Of Nuclear Reactors (AREA)

Abstract

L'invention concerne un corps fritté de combustible nucléaire, constitué d'UO2 ou d'un des oxydes mixtes suivants: (U, Pu)O2, (U, Th)O2, (U, RE)O2, (U, Pu, RE)O2 et (U, Pu, Th, RE)O2 (RE = terre rare) qui contient dans la matrice frittée, des particules de bore et/ou d'un composé bore chimique. Pour retenir le bore, ces particules sont recouvertes d'un film superficiel réalisé dans un matériau différent de celui qui constitue la matrice frittée et les particules. Un élément combustible nucléaire comporte une barre combustible qui contient un corps de combustible fritté de ce type dans un tube de gainage.
PCT/EP1994/003060 1993-09-22 1994-09-13 Corps fritte de combustible nucleaire et son procede de production WO1995008827A1 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
JP7509538A JPH09503858A (ja) 1993-09-22 1994-09-13 核燃料焼結体、核燃料焼結体を有する原子炉燃料要素及び核燃料焼結体の製造方法
EP94926937A EP0720766A1 (fr) 1993-09-22 1994-09-13 Corps fritte de combustible nucleaire et son procede de production
KR1019960701486A KR960705324A (ko) 1993-09-22 1996-03-22 핵연료 소결체 및 그 제조 방법(nuclear fuel sintered body and process for producing it)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
EP93115342 1993-09-22
EP93115342.3 1993-09-22

Publications (1)

Publication Number Publication Date
WO1995008827A1 true WO1995008827A1 (fr) 1995-03-30

Family

ID=8213295

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/EP1994/003060 WO1995008827A1 (fr) 1993-09-22 1994-09-13 Corps fritte de combustible nucleaire et son procede de production

Country Status (5)

Country Link
EP (1) EP0720766A1 (fr)
JP (1) JPH09503858A (fr)
KR (1) KR960705324A (fr)
TW (1) TW257869B (fr)
WO (1) WO1995008827A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2814584A1 (fr) * 2000-09-27 2002-03-29 Commissariat Energie Atomique Combustible nucleaire comprenant un poison consommable et son procede de fabrication
KR100746800B1 (ko) 2002-03-11 2007-08-06 우렌코 네덜란드 비.브이. 핵 연료의 제공방법, 및 그 방법으로 얻어진 핵 연료가 제공된 연료 성분

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2787370B1 (fr) * 1998-12-22 2001-03-16 Franco Belge Combustibles Procede de liaison de deux pieces tubulaires coaxiales, outil pour realiser cette liaison et utilisation
KR100331483B1 (ko) * 1999-06-02 2002-04-03 장인순 중성자 흡수물질을 함유한 산화물 핵연료 소결체의 제조방법
KR101436499B1 (ko) * 2012-11-05 2014-09-01 한국원자력연구원 급속소결을 통한 가연성 흡수 핵연료 소결체의 제조방법 및 이에 따라 제조된 가연성 흡수 핵연료 소결체

Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1414598A (fr) * 1963-11-25 1965-10-15 Int Research & Dev Co Ltd Perfectionnements apportés aux matériaux contenant du bore et aux procédés pour leur élaboration
US3917768A (en) * 1969-02-25 1975-11-04 Fiat Spa Sintered nuclear fuel and method of preparing same
US4671927A (en) * 1984-12-03 1987-06-09 Westinghouse Electric Corp. Nuclear fuel rod containing a hybrid gadolinium oxide, boron carbide burnable absorber
EP0239843A1 (fr) * 1986-03-24 1987-10-07 Siemens Aktiengesellschaft Combustible nucléaire fritté et son procédé de fabrication
ES2002719A6 (es) * 1986-07-22 1988-10-01 Westinghouse Electric Corp Una pastilla de combustible para un reactor nuclear
JPH01155294A (ja) * 1987-12-14 1989-06-19 Toshiba Corp 中性子吸収体
EP0418578A1 (fr) * 1989-09-18 1991-03-27 General Electric Company Composition de combustible nucléaire par fission

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1414598A (fr) * 1963-11-25 1965-10-15 Int Research & Dev Co Ltd Perfectionnements apportés aux matériaux contenant du bore et aux procédés pour leur élaboration
US3917768A (en) * 1969-02-25 1975-11-04 Fiat Spa Sintered nuclear fuel and method of preparing same
US4671927A (en) * 1984-12-03 1987-06-09 Westinghouse Electric Corp. Nuclear fuel rod containing a hybrid gadolinium oxide, boron carbide burnable absorber
EP0239843A1 (fr) * 1986-03-24 1987-10-07 Siemens Aktiengesellschaft Combustible nucléaire fritté et son procédé de fabrication
ES2002719A6 (es) * 1986-07-22 1988-10-01 Westinghouse Electric Corp Una pastilla de combustible para un reactor nuclear
JPH01155294A (ja) * 1987-12-14 1989-06-19 Toshiba Corp 中性子吸収体
EP0418578A1 (fr) * 1989-09-18 1991-03-27 General Electric Company Composition de combustible nucléaire par fission

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
DATABASE WPI Section Ch Week 8929, Derwent World Patents Index; Class E32, AN 89-208673 *
DATABASE WPI Section Ch Week 8930, Derwent World Patents Index; Class K05, AN 89-217108 *

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2814584A1 (fr) * 2000-09-27 2002-03-29 Commissariat Energie Atomique Combustible nucleaire comprenant un poison consommable et son procede de fabrication
EP1193717A1 (fr) * 2000-09-27 2002-04-03 Commissariat A L'energie Atomique Combustible nucleaire comprenant un poison consommable et son procédé de fabrication
KR100746800B1 (ko) 2002-03-11 2007-08-06 우렌코 네덜란드 비.브이. 핵 연료의 제공방법, 및 그 방법으로 얻어진 핵 연료가 제공된 연료 성분

Also Published As

Publication number Publication date
TW257869B (fr) 1995-09-21
EP0720766A1 (fr) 1996-07-10
JPH09503858A (ja) 1997-04-15
KR960705324A (ko) 1996-10-09

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