EP1087408B1 - Procédé de production d'un revêtement qui absorbe des neutrons - Google Patents

Procédé de production d'un revêtement qui absorbe des neutrons Download PDF

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Publication number
EP1087408B1
EP1087408B1 EP99118989A EP99118989A EP1087408B1 EP 1087408 B1 EP1087408 B1 EP 1087408B1 EP 99118989 A EP99118989 A EP 99118989A EP 99118989 A EP99118989 A EP 99118989A EP 1087408 B1 EP1087408 B1 EP 1087408B1
Authority
EP
European Patent Office
Prior art keywords
neutron capture
capture section
produced
high neutron
coating
Prior art date
Legal status (The legal status 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 status listed.)
Expired - Lifetime
Application number
EP99118989A
Other languages
German (de)
English (en)
Other versions
EP1087408A1 (fr
Inventor
Leo Wilbuer Klaus
Patzelt Matthias
Methling Dieter
Stelzer Hermann
Diersch Rudolph
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
GNS Gesellschaft fuer Nuklearservice mbH
Metallveredlung GmbH and Co KG
Original Assignee
GNS Gesellschaft fuer Nuklearservice mbH
Metallveredlung GmbH and Co KG
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 GNS Gesellschaft fuer Nuklearservice mbH, Metallveredlung GmbH and Co KG filed Critical GNS Gesellschaft fuer Nuklearservice mbH
Priority to DE59914334T priority Critical patent/DE59914334D1/de
Priority to PCT/EP1999/007166 priority patent/WO2001024198A1/fr
Priority to EP99118989A priority patent/EP1087408B1/fr
Priority to AT99118989T priority patent/ATE362181T1/de
Priority to ES99118989T priority patent/ES2287998T3/es
Publication of EP1087408A1 publication Critical patent/EP1087408A1/fr
Application granted granted Critical
Publication of EP1087408B1 publication Critical patent/EP1087408B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F1/00—Shielding characterised by the composition of the materials
    • G21F1/02—Selection of uniform shielding materials
    • G21F1/08—Metals; Alloys; Cermets, i.e. sintered mixtures of ceramics and metals

Definitions

  • the invention relates to a method for producing a coating for absorbing the neutrons produced in the nuclear reaction of radioactive materials.
  • the invention also relates to an absorber element produced by the process.
  • EP 0 385 187 A1 discloses a fuel element storage rack in which absorber sheets form a number of ducts which surround the fuel elements over their entire length.
  • These absorber elements are manholes or tubes made of a neutron-absorbing material, for example boron steel, a stainless steel with a boron content of 1 to 2%.
  • boron steel for example boron steel
  • stainless steel with a boron content of 1 to 2%.
  • these absorber elements are extremely expensive and the efficiency is limited because of the limited - boron content.
  • the deposition of a boron-nickel alloy was checked. Although the proportion of boron can be increased to up to 8%, the costs increase by a factor of about 10, so that an economical use of such pipes can not be considered.
  • US Pat. No. 4,218,622 describes a composite absorber element which has a thin carrier foil or a thin carrier plate onto which a polymer matrix in which boron carbide particles have been incorporated is applied.
  • the material of the carrier film or of the carrier sheet is preferably glass fiber-reinforced polymer.
  • the boron carbide particles are uniformly distributed on the surface of the polymer matrix, with a boron concentration of up to 0.1 g / cm 2 .
  • this absorber element has a thickness of up to 7 mm, is configured in the form of a foil or sheet, and suspended between an inner wall and an outer wall.
  • EP 0 016 252 A1 describes a method for producing a neutron-absorbing absorber element.
  • boron carbide is applied to a substrate together with a metallic substance by means of plasma spraying, the boron carbide being incorporated into a matrix of a metallic substance.
  • the process also takes place in such a way that oxidation of the boron is avoided.
  • the absorber element thus produced should be stable to a liquid medium, as it is present for example in a fuel storage pool.
  • the thickness of the plasma sprayed metal and boron carbide layer is at least 500 ⁇ m.
  • the proportion of boron carbide is about 50% by volume.
  • the substrate containing the same metallic substance as the sprayed layer.
  • a relatively thick layer of boron carbide is required, in particular, the thickness of the layer is 3 to 6 mm.
  • DE-AS 1 037 302 and DE 2 361 363 it is known to provide pipes, in particular cans, on their outer surface by electrolytic means with absorber material for protection against radioactive radiation.
  • absorber material for protection against radioactive radiation.
  • no information can be taken from DE-AS-1 037 302 and DE 2 361 363.
  • EP 0 055 679 A2 discloses processes for the production of shielding elements, boron carbide being applied to the surface of the shielding element either in a plasma coating process, or according to a electrolytic or chemical Vorvernickelung of the shielding element boron carbide scattered as a powder on the surface and the shielding element is then electrolyzed or chemically nachvernickelt.
  • these methods only small quantities of boron carbide in the order of 20 wt.% With respect to nickel are applied to the surface. It therefore requires very strong layers, so that these prior art methods are uneconomical. In practice, these methods were not used, since they are not technically feasible in terms of process engineering.
  • the application of a powder to a surface in the sense of spreading is not a measure that ensures a secure industrial production.
  • a fuel assembly for nuclear reactors which comprises a fuel tube having an inner surface coated with a support metal having a low neutron capture section in which layer combustible reactant cages are incorporated. Boron compounds can serve as reactant compounds.
  • boron steel is very expensive.
  • the steel is melted and boron is enriched by complex processes up to the 10 valence and mixed with the molten steel. This results in a boron steel with 1.1 to 1.4 wt .-% boron.
  • This steel can be very bad work, is extremely brittle and can be poorly welded. Shielding elements made of this have an extremely high weight with average absorption properties.
  • the present invention has the object to improve a method for producing a coating or by shielding the absorption of the produced during the nuclear reaction of radioactive materials neutron further, which is economical and easy to use, the effectiveness of the absorption increases, with respect to the base materials and shape of the shielding allows greater variability, is technically well controlled and in particular allows the production of lighter absorber elements with at least the same absorption qualities.
  • Elements with a high neutron capture range include elements from the group boron, also in elemental form or boron carbide, gadolinium, cadmium, samarium, europium or dysprosium.
  • the high neutron capture section represents the size of the capture cross section for neutrons of the respective element.
  • conductive compounds in particular metallic compounds have proven to be particularly useful. These include metal borides such as iron boride, nickel boride and the like. The list is exemplary and extensible in relation to the named elements.
  • the conductivity stands for the good electrolytic controllability, so that the process can be performed under less demanding conditions with high reliability and reproducibility.
  • electrolytically or autocatalytically depositable metallic element are in particular nickel, cadmium or copper.
  • the high neutron capture section element or its compounds are incorporated in this metal matrix with the corresponding effect.
  • isotopes of the respective elements which have an enlarged neutron capture section.
  • 11 B signifies a neutron capture section of 0.005 barn
  • isotope 10 B signifies 3837 barn. This results in the possible lower layer thicknesses.
  • the absorption layers are in the order of magnitude of up to 800 ⁇ m.
  • a special advantage is the independence of the process from the base material.
  • inorganic base material is to be used, for example steel, stainless steel, boron steel, titanium, aluminum, copper, nickel and the like, including corresponding alloys.
  • carbon fiber material may be considered as the base material. Carbon fiber material has the particular advantage of galvanotechnical manufacturability of the absorption element.
  • the absorber element in the finished state or in individual parts. Due to the independence of the base material very easy machinable materials can be used. On the other hand, even very complicated forms of absorber elements, containers, baskets and the like, can be completely prefabricated and then coated according to the invention.
  • the shield is extremely effective so that the layers can be extremely thin.
  • weight savings of up to 50% are possible with respect to shielding elements which can be produced by conventional methods.
  • the currently used in the container program for fuel storage storage containers (baskets) of previously about 10 t can be after the process according to the invention now produce in the order of 4 to 6 tons.
  • the base material can be prefabricated as a finished part or item, so that can be formed from the items finished absorber elements.
  • the assembly of the absorber elements or the parts of absorber elements to complete bearings or baskets can be made by positive and / or positive connections.
  • the invention also enables the coating of complete storage racks and baskets. The coating in the dispersion bath is carried out either chemically or electrolytically.
  • the relative movement between the surface to be coated and the dispersion bath can be effected, for example, by a movement of the element to be coated in the dispersion bath.
  • elements such as boron and the like are such that circulating or circulating the dispersion is practically not economically possible. Any circulating or pumping unit would be worn out in no time. Nevertheless, on the one hand a further good mixing or repeated mixing of the dispersion is to be achieved by the relative movement, on the other hand a directional supply of the dispersion to the surface to be coated.
  • a directional supply of the dispersion to the surface to be coated In addition to the movement of the element itself and the entire coating system for the purpose of generating the relative movement can be moved. For example, the implementation of the coating in a kind of drum is conceivable.
  • the relative movement can also be effected by mechanical movement of the bath, blowing gas, in particular air, ultrasound support and combinations thereof.
  • the invention proposes that the surface to be coated is arranged in the dispersion bath pointing upwards. This means that the surface to be coated in such Disperse bath is arranged that due to gravity, the particles in the dispersion fall to the surface.
  • This arrangement according to the invention in particular in combination with the temporary generation of a relative movement between the surface and the dispersion bath, favors excellent coating results.
  • the coating process is carried out in a ceramic or glass pan. This ensures a special purity of the dispersion bath.
  • the invention also relates to absorber elements produced by the process described in claims 1-13. These are characterized by having a coating formed of a high neutron capture section element and nickel having a proportion of the element or its high neutron capture section compound of up to 60% by volume and 40% by volume, respectively.
  • the layer thickness is 350 to 500 microns to 800 microns, wherein the layer is formed on an inorganic base material such as steel, titanium, copper or the like. Layer thicknesses up to 2000 ⁇ m can be realized.
  • the training takes place chemically or electrolytically.
  • the shielding element may have been coated in finished form or composed of individual coated individual parts. As the electrolyte come, for example, in question without electroless nickel-phosphorus or electrolytic nickel.

Landscapes

  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Metallurgy (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Other Surface Treatments For Metallic Materials (AREA)
  • Paints Or Removers (AREA)

Claims (14)

  1. Procédé de fabrication d'un revêtement pour l'absorption des neutrons produits lors de la réaction nucléaire de matériaux radioactifs, dans lequel une partie au moins d'un élément composé d'un matériau de base est dotée sur ses surfaces prévues à cette fin, dans un bain de dispersion, d'un revêtement composé d'un élément à grande section efficace de capture des neutrons et d'un élément métallique pouvant être déposé par électrolyse ou autocatalyse, dans lequel un mouvement relatif est produit pendant l'opération de revêtement, au moins par intermittences, entre la surface à revêtir et le bain de dispersion, et dans lequel l'élément à grande section efficace de capture des neutrons utilisé est au moins un élément du groupe comprenant le bore, le gadolinium, le cadmium, le samarium, l'europium ou le dysprosium, caractérisé en ce que l'élément à grande section efficace de capture des neutrons est présent dans le bain de dispersion dans un composé électriquement conducteur et est déposé dans une proportion de plus de 20 % en volume dans le revêtement.
  2. Procédé selon la revendication 1, caractérisé en ce que l'élément métallique pouvant être déposé par électrolyse ou autocatalyse utilisé est l'un des éléments du groupe comprenant le nickel, le cadmium ou le cuivre.
  3. Procédé selon l'une des revendications précédentes, caractérisé en ce que le composé conducteur de l'élément à grande section efficace de capture des neutrons utilisé est un composé métallique.
  4. Procédé selon l'une des revendications précédentes, caractérisé en ce que le composé conducteur de l'élément à grande section efficace de capture des neutrons utilisé est un borure métallique.
  5. Procédé selon l'une des revendications précédentes, caractérisé en ce que l'élément à grande section efficace de capture des neutrons est utilisé sous la forme d'un isotope à section efficace de capture des neutrons augmentée.
  6. Procédé selon l'une des revendications précédentes, caractérisé en ce que le mouvement relatif est produit par le déplacement de l'élément à revêtir.
  7. Procédé selon l'une des revendications 1 à 5, caractérisé en ce que le mouvement relatif est produit par injection de gaz et/ou application d'ultrasons.
  8. Procédé selon l'une des revendications précédentes, caractérisé en ce que la formation du revêtement est réalisée par voie chimique.
  9. Procédé selon l'une des revendications 1 à 7, caractérisé en ce que la formation du revêtement est réalisée par voie électrolytique.
  10. Procédé selon l'une des revendications précédentes, caractérisé en ce qu'un revêtement d'une épaisseur de 800 µm au maximum est produit.
  11. Procédé selon l'une des revendications précédentes, caractérisé en ce que l'élément à grande section efficace de capture des neutrons ou ses composés sont intégrés jusqu'à 60 % en volume dans la matrice métallique.
  12. Procédé selon l'une des revendications précédentes, caractérisé en ce que le bain de dispersion est brassé au moins par intermittences pendant l'opération de revêtement.
  13. Procédé selon l'une des revendications précédentes, caractérisé en ce que le procédé est réalisé dans un bac en céramique ou en verre.
  14. Unité d'absorbeur fabriquée par le procédé selon l'une au moins des revendications 1 à 13.
EP99118989A 1999-09-27 1999-09-27 Procédé de production d'un revêtement qui absorbe des neutrons Expired - Lifetime EP1087408B1 (fr)

Priority Applications (5)

Application Number Priority Date Filing Date Title
DE59914334T DE59914334D1 (de) 1999-09-27 1999-09-27 Verfahren zur Herstellung einer Beschichtung zur Absorption der bei der Kernreaktion radioaktiver Materialien entstehenden Neutronen
PCT/EP1999/007166 WO2001024198A1 (fr) 1999-09-27 1999-09-27 Procede de fabrication d'un revetement pour l'absorption de neutrons prenant naissance lors de la reaction nucleaire de materiaux radioactifs
EP99118989A EP1087408B1 (fr) 1999-09-27 1999-09-27 Procédé de production d'un revêtement qui absorbe des neutrons
AT99118989T ATE362181T1 (de) 1999-09-27 1999-09-27 Verfahren zur herstellung einer beschichtung zur absorption der bei der kernreaktion radioaktiver materialien entstehenden neutronen
ES99118989T ES2287998T3 (es) 1999-09-27 1999-09-27 Procedimiento de fabricacion de un revestimiento para la absorcion de los neutrones producidos por la reaccion nuclear de materiales radioactivos.

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
PCT/EP1999/007166 WO2001024198A1 (fr) 1999-09-27 1999-09-27 Procede de fabrication d'un revetement pour l'absorption de neutrons prenant naissance lors de la reaction nucleaire de materiaux radioactifs
EP99118989A EP1087408B1 (fr) 1999-09-27 1999-09-27 Procédé de production d'un revêtement qui absorbe des neutrons

Publications (2)

Publication Number Publication Date
EP1087408A1 EP1087408A1 (fr) 2001-03-28
EP1087408B1 true EP1087408B1 (fr) 2007-05-09

Family

ID=26070383

Family Applications (1)

Application Number Title Priority Date Filing Date
EP99118989A Expired - Lifetime EP1087408B1 (fr) 1999-09-27 1999-09-27 Procédé de production d'un revêtement qui absorbe des neutrons

Country Status (5)

Country Link
EP (1) EP1087408B1 (fr)
AT (1) ATE362181T1 (fr)
DE (1) DE59914334D1 (fr)
ES (1) ES2287998T3 (fr)
WO (1) WO2001024198A1 (fr)

Family Cites Families (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3625821A (en) * 1968-06-26 1971-12-07 Westinghouse Electric Corp Fuel-element coating containing burnable poison
US4227928A (en) * 1978-05-01 1980-10-14 Kennecott Copper Corporation Copper-boron carbide composite particle and method for its production
US4238299A (en) * 1979-08-24 1980-12-09 Kennecott Copper Corporation Tubing with copper-boron carbide composite facing and methods for its production
YU305181A (en) * 1980-12-31 1986-04-30 Farmatome Sa Method of making housings for the subaqueous storing of radiated fuel assemblies
JPS59102953A (ja) * 1982-12-03 1984-06-14 Rin Kagaku Kogyo Kk 導電性の合成樹脂組成物
JPS60235096A (ja) * 1984-05-07 1985-11-21 三菱マテリアル株式会社 中性子遮蔽吸収用材料の製法
US4880597A (en) * 1987-08-05 1989-11-14 Combustion Engineering, Inc. Alloy coated fuel cladding
US4824634A (en) * 1987-08-05 1989-04-25 Combustion Engineering, Inc. Element with burnable poison coating
WO1996036972A1 (fr) * 1995-05-16 1996-11-21 Metallveredlung Gmbh & Co. Kg Procede de production d'elements de blindage pour absorber les neutrons produits lors de la reaction nucleaire de materiaux radioactifs
EP0996953B1 (fr) * 1997-06-24 2005-05-18 Metallveredlung GmbH & Co. KG Procede de production d'un revetement qui absorbe des neutrons

Also Published As

Publication number Publication date
ATE362181T1 (de) 2007-06-15
DE59914334D1 (de) 2007-06-21
WO2001024198A1 (fr) 2001-04-05
ES2287998T3 (es) 2007-12-16
EP1087408A1 (fr) 2001-03-28

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