EP0060765A1 - Neutron absorbing material, method to produce the same and application of this material to the manufacture of storage containers - Google Patents

Neutron absorbing material, method to produce the same and application of this material to the manufacture of storage containers Download PDF

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Publication number
EP0060765A1
EP0060765A1 EP82400401A EP82400401A EP0060765A1 EP 0060765 A1 EP0060765 A1 EP 0060765A1 EP 82400401 A EP82400401 A EP 82400401A EP 82400401 A EP82400401 A EP 82400401A EP 0060765 A1 EP0060765 A1 EP 0060765A1
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EP
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Prior art keywords
boron carbide
product
product according
neutron absorbing
polyethylene
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Application number
EP82400401A
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German (de)
French (fr)
Inventor
Pierre Cals
Roger Conche
Gérard Fraize
Lucien Hayet
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Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
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Commissariat a lEnergie Atomique CEA
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    • 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
    • G21F1/04—Concretes; Other hydraulic hardening materials
    • G21F1/042—Concretes combined with other materials dispersed in the carrier
    • G21F1/045—Concretes combined with other materials dispersed in the carrier with organic substances

Definitions

  • the subject of the present invention is a product capable of absorbing neutrons as well as a process for manufacturing this product.
  • the materials produced so far include substances rich in hydrogen to slow down fast neutrons (this is the case with polyethylene) and substances capable of absorbing slowed down neutrons like boron compounds.
  • French patent 1,534,032 belonging to the applicant, describes a material capable of absorbing neutrons consisting of polyethylene, plaster, water and boric acid. If such a product has good absorbent qualities, its manufacture causes a certain number of difficulties. This was how we noted a poor amalgamation of the components and a rise in the surface of the polyethylene beads during the solidification phase of the product; moreover this last stage always required a fairly long time.
  • the object of the present invention is precisely a neutron absorbing material which overcomes these drawbacks by using thixotropic concrete.
  • the product which is the subject of the invention, it comprises a thixotropic concrete in which are incorporated 30 to 40% by weight of high density polyethylene beads and 1 to 5 ⁇ by weight of boron carbide grains.
  • the polyethylene balls have a diameter of the order of 2 to 5 mm and the grains of boron carbide have dimensions of the order of 300 to 500 ⁇ m.
  • the invention also relates to an application of this product to the production of storage castles of the type comprising an internal wall and an external wall between which there is a neutron absorbing product.
  • the internal face of the external wall is covered with a paint based on boron carbide and the product according to the invention is poured between the internal and external walls of the castle.
  • the product is poured into the container for which it is intended, for example between the walls of a storage castle, while agitating the latter using a vibrating system which can be in the form pneumatic vibrating needles. Thanks to this last precaution, the product remains liquid until the end of the operation, which ensures good homogeneity, homogeneity all the better as the product solidifies quickly once the vibrations have stopped, which avoids disadvantages of the prior art.
  • Test tubes are hermetically sealed to keep the moisture content of the compound constant.
  • curve 2 is clearly below curve 1 while curve 3 is very close to curve 2: a very low content of boron carbide is therefore sufficient to appreciably reduce the dose rate. neutron.
  • the material which is the subject of the invention has numerous advantages, in particular with regard to its preparation process.
  • the use of thixotropic concrete makes it possible to keep the liquid product while the mixing is carried out in the concrete mixer and while it is poured into the storage castle since it is set in motion by vibrating needles .
  • a very homogeneous product is obtained. since solidification takes place quickly once the vibrations have ceased.
  • this product has good mechanical strength, good fire resistance and a low cost price since it can be produced from materials readily available on the market.
  • the procedure is as follows: first cover the internal face of the external wall with a base paint boron carbide, the product according to the invention is then poured between the walls of the castle while keeping it in vibration and the vibrations are stopped to allow the product to harden.

Abstract

The product comprises a thixotropic concrete in which there are incorporated 30 to 40% by weight of high-density polyethylene beads with a diameter of the order of 2 to 5 mm and 0.1 to 0.5% by weight of boron carbide particles of the order of approximately from 300 to 500 mu m in size. Application to the storage and transport of radioactive products.

Description

La présente invention a pour objet un produit capable d'absorber les neutrons ainsi qu'un procédé de fabrication de ce produit.The subject of the present invention is a product capable of absorbing neutrons as well as a process for manufacturing this product.

Plus précisément, elle a pour objet un matériau absorbant les neutrons et plus spécialement les neutrons rapides et thermiques d'énergie comprise entre 0,1 et 14 MeV, utilisable dans les châteaux de transport et de stockage de produits radioactifs.More specifically, it relates to a material absorbing neutrons and more particularly fast and thermal neutrons with an energy of between 0.1 and 14 MeV, usable in transport and storage châteaux of radioactive products.

On sait que, contrairement aux rayons gamma qui nécessitent pour leur absorption des matériaux lourds (fer, plomb, tungstène, uranium), l'absorption des neutrons est en majeure partie obtenue après ralentissement par des atomes légers (hydrogène, carbone).We know that, unlike gamma rays which require heavy materials (iron, lead, tungsten, uranium) for their absorption, the absorption of neutrons is mainly obtained after slowing down by light atoms (hydrogen, carbon).

C'est pourquoi les matériaux réalisés jusqu' ici comportent des substances riches en hydrogène pour ralentir les neutrons rapides (c'est le cas du polyéthylène) et des substances capables d'absorber les neutrons ralentis comme les composés de bore. Par exemple, le brevet français 1 534 032, appartenant au déposant, décrit un matériau capable d'absorber les neutrons consitué par du polyéthylène, du plâtre, de l'eau et de l'acide borique. Si un tel produit présente de bonnes qualités absorbantes, sa fabrication entraîne un certain nombre de difficultés. C'est ainsi qu'on a pu noter un mauvais amalgame des composants et une remontée en surface des billes de polyéthylène pendant la phase de solidification du produit ; de plus cette dernière étape exigeait toujours un temps assez long.This is why the materials produced so far include substances rich in hydrogen to slow down fast neutrons (this is the case with polyethylene) and substances capable of absorbing slowed down neutrons like boron compounds. For example, French patent 1,534,032, belonging to the applicant, describes a material capable of absorbing neutrons consisting of polyethylene, plaster, water and boric acid. If such a product has good absorbent qualities, its manufacture causes a certain number of difficulties. This was how we noted a poor amalgamation of the components and a rise in the surface of the polyethylene beads during the solidification phase of the product; moreover this last stage always required a fairly long time.

La présente invention a justement pour objet un matériau absorbant les neutrons qui supprime ces inconvénients grâce à la mise en oeuvre d'un béton thixotropique.The object of the present invention is precisely a neutron absorbing material which overcomes these drawbacks by using thixotropic concrete.

Selon la principale caractéristique du produit objet de l'invention, celui-ci comprend un béton thixotropique dans lequel sont incorporés 30 à 40 % en poids de billes de polyéthylène haute densité et 1 à 5 ‰ en poids de grains de carbure de bore.According to the main characteristic of the product which is the subject of the invention, it comprises a thixotropic concrete in which are incorporated 30 to 40% by weight of high density polyethylene beads and 1 to 5 ‰ by weight of boron carbide grains.

Selon un mode de réalisation préféré, les billes de polyéthylène ont un diamètre de l'ordre de 2 à 5 mm et les grains de carbure de bore ont des dimensions de l'ordre de 300 à 500 um.According to a preferred embodiment, the polyethylene balls have a diameter of the order of 2 to 5 mm and the grains of boron carbide have dimensions of the order of 300 to 500 μm.

L'invention a également pour objet un procédé de fabrication de ce produit. Selon la principale caractéristique de ce procédé, celui-ci comprend les étapes suivantes :

  • - on mélange intimement le polyéthylène avec des constituants aptes à former un béton thixotropique,
  • - on ajoute le carbure de bore,
  • - on ajoute de l'eau,
  • - on verse le mélange dans le récipient auquel il est destiné tout en maintenant celui-ci en vibration, et
  • - on laisse durcir le mélange.
The invention also relates to a method of manufacturing this product. According to the main characteristic of this process, it comprises the following steps:
  • the polyethylene is intimately mixed with constituents capable of forming a thixotropic concrete,
  • - the boron carbide is added,
  • - we add water,
  • the mixture is poured into the container for which it is intended while keeping it in vibration, and
  • - the mixture is allowed to harden.

Si l'on retrouve le polyéthylène, dont le rôle est de ralentir les neutrons rapides, et le carbure de bore, dont le rôle est de les absorber, l'utilisation d'un béton thixotropique comme liant favorise la préparation et le coulage du matériau et confère la qualité de matériau incombustible. En effet, un tel béton reste liquide tant qu'on l'agite et se solidifie rapidement lorsqu'on le laisse au repos. Ainsi, le produit reste liquide quand on réalise le mélange puisque celui-ci se fait obligatoirement sous agitation permanente des divers constituants.If we find polyethylene, whose role is to slow fast neutrons, and boron carbide, whose role is to absorb them, the use of a thixotropic concrete as a binder promotes the preparation and casting of the material and gives the quality of non-combustible material. Indeed, such concrete remains liquid as long as it is agitated and solidifies quickly when it is left to stand. Thus, the product remains liquid when the mixture is produced since it is necessarily done with permanent stirring of the various constituents.

Enfin, lorsque l'agitation cesse, le produit se prend en masse rapidement, ce qui empêche la remontée en surface des billes de polyéthylène et conduit à un matériau plus homogène.Finally, when the agitation ceases, the product solidifies rapidly, which prevents the polyethylene balls from rising to the surface and leads to a more homogeneous material.

L'invention a encore pour objet une application de ce produit à la réalisation de châteaux de stockage du type comprenant une paroi interne et une paroi externe entre lesquelles se trouve un produit absorbant les neutrons. Pour cela, on recouvre la face interne de la paroi externe d'une peinture à base de carbure de bore et on coule le produit selon l'invention entre les parois interne et externe du château.The invention also relates to an application of this product to the production of storage castles of the type comprising an internal wall and an external wall between which there is a neutron absorbing product. For this, the internal face of the external wall is covered with a paint based on boron carbide and the product according to the invention is poured between the internal and external walls of the castle.

D'autres caractéristiques et avantages de l'invention apparaîtront à la lecture de la description qui va suivre d'un exemple de réalisation, donnée à titre purement illustratif et nullement limitatif , en référence aux dessins annexés dans lesquels :

  • - la figure 1 représente un ensemble de courbes donnant le débit de dose neutron d'un échantillon de produit selon l'invention, en millirem par heure et par microgramme de californium 252, en fonction de l'épaisseur de l'échantillon et de sa teneur en carbure de bore, et
  • - la figure 2 représente un ensemble de courbes donnant le débit de dose gamma d'un échantillon, en millirad par heure et par microgramme de californium 252, en fonction de l'épaisseur de l'échantillon et de sa teneur en carbure de bore.
Other characteristics and advantages of the invention will appear on reading the following description of an exemplary embodiment, given purely by way of illustration and in no way limiting, with reference to the appended drawings in which:
  • - Figure 1 shows a set of curves giving the neutron dose rate of a sample of product according to the invention, in millirem per hour and per microgram of californium 252, depending on the thickness of the sample and its boron carbide content, and
  • - Figure 2 shows a set of curves giving the gamma dose rate of a sample, in millirad per hour and per microgram of californium 252, depending on the thickness of the sample and its boron carbide content.

A titre d'essai, on a réalisé un produit conforme à l'invention dont la composition était la suivante, les proportions étant calculées pour 1 dm3 de produit

  • Polyéthylène : 0,448 kg
  • Béton thixotropique : 0, 845 kg
  • Eau : 0,134 litre
  • Carbure de bore : 1,5 g
As a test, a product in accordance with the invention was produced, the composition of which was as follows, the proportions being calculated for 1 dm 3 of product
  • Polyethylene: 0.448 kg
  • Thixotropic concrete: 0.845 kg
  • Water: 0.134 liter
  • Boron carbide: 1.5 g

La préparation du produit a été réalisée selon le processus suivant :

  • - dans une bétonnière en marche, on met en place d'abord les billes de polyéthylène, puis le béton et on réalise le mélange à sec jusqu'à ce que les billes prennent une couleur grise,
  • - on ajoute ensuite le carbure de bore et on laisse tourner la bétonnière jusqu'à obtention d'un mélange homogène,
  • - on ajoute l'eau et on attend que le mélange prenne une apparence relativement sèche de couleur gris/noir.
The preparation of the product was carried out according to the following process:
  • - in a running concrete mixer, first place the polyethylene balls, then the concrete and dry mix until the balls take on a gray color,
  • - the boron carbide is then added and the concrete mixer is left to rotate until a homogeneous mixture is obtained,
  • - add the water and wait until the mixture takes on a relatively dry appearance of gray / black color.

Ensuite, on coule le produit dans le récipient auquel il est destiné, par exemple entre les parois d'un château de stockage, tout en agitant ce dernier à l'aide d'un système de mise en vibration qui peut se présenter sous la forme d'aiguilles vibrantes pneumatiques. Grâce à cette dernière précaution, le produit reste liquide jusqu'à la fin de l'opération, ce qui assure une bonne homogénéité, homogénéité d'autant meilleure que le produit se solidifie rapidement une fois que les vibrations ont cessé, ce qui évite les inconvénients de l'art antérieur.Then, the product is poured into the container for which it is intended, for example between the walls of a storage castle, while agitating the latter using a vibrating system which can be in the form pneumatic vibrating needles. Thanks to this last precaution, the product remains liquid until the end of the operation, which ensures good homogeneity, homogeneity all the better as the product solidifies quickly once the vibrations have stopped, which avoids disadvantages of the prior art.

Des essais de résistance au feu effectués sur une éprouvette en acier de diamètre 100 mm, longueur 300 mm, épaisseur 3 mm, fermée à chaque extrémité par une tôle d'acier de même épaisseur et remplie du produit objet de l'invention ont montré que celui-ci présentait une bonne tenue au feu, sans déformation mécanique de l'éprouvette après un séjour de 30 minutes dans un four à 800°C.Fire resistance tests carried out on a steel test tube with a diameter of 100 mm, length 300 mm, thickness 3 mm, closed at each end by a steel sheet of the same thickness and filled with the product which is the subject of the invention have shown that this exhibited good fire resistance, without mechanical deformation of the test piece after a stay of 30 minutes in an oven at 800 ° C.

Une autre série d'essais avait pour but d'étudier l'influence de la teneur en carbure de bore sur le pouvoir absorbant du matériau.Another series of tests aimed to study the influence of the boron carbide content on the absorbency of the material.

Pour cela, on a réalisé 21 éprouvettes en acier de diamètre 80 mm, d'épaisseur 3 mm, de longueur variable (150 ou 300 mm) obturées à chacune de leurs extrémités par une plaque d'acier d'épaisseur 3 mm.For this, 21 steel test tubes of 80 mm diameter, 3 mm thick, of variable length (150 or 300 mm) were made closed at each of their ends by a steel plate 3 mm thick.

L'intérieur de ces tubes est rempli du produit objet de l'invention auquel on incorpore du carbure de bore en quantité variable. Les éprouvettes sont hermétiquement closes afin de maintenir constante la teneur en humidité du composé.The interior of these tubes is filled with the product which is the subject of the invention, to which boron carbide is incorporated in variable quantities. Test tubes are hermetically sealed to keep the moisture content of the compound constant.

Les trois courbes de la figure 1 (débit de dose neutron) correspondent à trois teneurs différentes en carbure de bore, à savoir :

  • Courbe 1 : 0 kg/m3
  • Courbe 2 : 3 kg/m 3
  • Courbe 3 : 20 kg/m 3
The three curves in FIG. 1 (neutron dose rate) correspond to three different boron carbide contents, namely:
  • Curve 1: 0 kg / m 3
  • Curve 2: 3 k g / m 3
  • Curve 3: 20 k g / m 3

On voit que la courbe 2 se situe nettement en dessous de la courbe 1 alors que la courbe 3 est très voisine de la courbe 2 : il suffit donc d'une très faible teneur en carbure de bore pour diminuer de façon appréciable le débit de dose neutron.We see that curve 2 is clearly below curve 1 while curve 3 is very close to curve 2: a very low content of boron carbide is therefore sufficient to appreciably reduce the dose rate. neutron.

Les trois courbes de la figure 2 (débit de dose gamma) correspondent aux teneurs suivantes en carbure de bore :

  • Courbe 4 : 0 kg/m 3
  • Courbe 5 : 3 kg/m3
  • Courbe 6 : 8 kg/m 3
The three curves in Figure 2 (gamma dose rate) correspond to the following boron carbide contents:
  • Curve 4: 0 k g / m 3
  • Curve 5: 3 kg / m 3
  • Curve 6: 8 k g / m 3

On peut voir à la lecture de la figure 2 que le débit de dose gamma diminue régulièrement à mesure que l'on augmente la teneur en carbure de bore. De plus, la comparaison des figures 2 et 3 montre que le débit de dose neutron est toujours très supérieur au débit de dose gamma. C'est pourquoi on choisira une teneur en carbure de bore comprise entre 3 et 5 kg/m3 et de préférence plus proche de 3 kg/m3.It can be seen from reading Figure 2 that the gamma dose rate decreases regularly as the boron carbide content is increased. In addition, the comparison of Figures 2 and 3 shows that the neutron dose rate is always much higher than the gamma dose rate. This is why a boron carbide content of between 3 and 5 kg / m 3 and preferably closer to 3 kg / m 3 will be chosen.

Le matériau objet de l'invention présente de nombreux avantages, notamment en ce qui concerne son procédé de préparation. L'utilisation d'un béton thixotropique permet de garder le produit liquide pendant qu'on réalise le mélange dans la bétonnière et pendant qu'on le verse dans le château de stockage puisque celui-ci est mis en mouvement au moyen d'aiguilles vibrantes. De plus, on obtient un produit très homogène puisque la solidification se fait rapidement une fois que les vibrations ont cessé.The material which is the subject of the invention has numerous advantages, in particular with regard to its preparation process. The use of thixotropic concrete makes it possible to keep the liquid product while the mixing is carried out in the concrete mixer and while it is poured into the storage castle since it is set in motion by vibrating needles . In addition, a very homogeneous product is obtained. since solidification takes place quickly once the vibrations have ceased.

De plus, ce produit présente une bonne tenue mécanique, une bonne tenue au feu et un prix de revient peu élevé puisqu'on peut le réaliser à partir de matériaux facilement disponibles dans le commerce.In addition, this product has good mechanical strength, good fire resistance and a low cost price since it can be produced from materials readily available on the market.

Quant aux applications possibles, elles couvrent tous les cas où l'on a besoin d'un bon écran contre les radiations et plus spécialement les flux de neutrons rapides ; c'est ainsi que le produit selon l'invention trouve une application particulièrement intéressante comme écran neutronique dans la réalisation d'emballages pour le transport et le stockage de produits radioactifs.As for the possible applications, they cover all the cases where a good screen against radiation is needed and more particularly the fast neutron fluxes; this is how the product according to the invention finds a particularly advantageous application as a neutron screen in the production of packaging for the transport and storage of radioactive products.

Dans le cas des châteaux de stockage comprenant une paroi interne et une paroi externe entre lesquelles se trouve un produit absorbant les neutrons, on procède de la manière suivante : on recouvre d'abord la face interne de la paroi externe d'une peinture à base de carbure de bore, on coule ensuite le produit selon l'invention entre les parois du château tout en maintenant celui-ci en vibration et on arrête les vibrations pour laisser durcir le produit.In the case of storage castles comprising an internal wall and an external wall between which there is a neutron absorbing product, the procedure is as follows: first cover the internal face of the external wall with a base paint boron carbide, the product according to the invention is then poured between the walls of the castle while keeping it in vibration and the vibrations are stopped to allow the product to harden.

Claims (5)

1. Produit absorbant les neutrons caractérisé en ce qu'il comprend un béton thixotropique dans lequel sont incorporés 30 à 40% en poids de billes de polyéthylène haute densité et 1 à 5 ‰ en poids de grains de carbure de bore.1. Neutron absorbing product characterized in that it comprises a thixotropic concrete in which are incorporated 30 to 40% by weight of high density polyethylene beads and 1 to 5 ‰ by weight of boron carbide grains. 2. Produit selon la revendication 1, caractérisé en ce que les billes de polyéthylène ont un diamètre de l'ordre de 2 à 5 mm.2. Product according to claim 1, characterized in that the polyethylene balls have a diameter of the order of 2 to 5 mm. 3. Produit selon l'une quelconque des revendications 1 ou 2, caractérisé en ce que les grains de carbure de bore ont des dimensions de l'ordre de 300 à 500 um.3. Product according to any one of claims 1 or 2, characterized in that the boron carbide grains have dimensions of the order of 300 to 500 µm. 4. Procédé de préparation du produit selon l'une quelconque des revendications 1 à 3, caractérisé en ce qu'il comprend les étapes suivantes : - on mélange intimement le polyéthylène avec des constituants aptes à former un béton thixotropique, - on ajoute le carbure de bore, - on ajoute de l'eau, - on verse le mélange dans le récipient auquel il est destiné tout en maintenant celui-ci en vibration, et - on laisse durcir le mélange. 4. Method for preparing the product according to any one of claims 1 to 3, characterized in that it comprises the following steps: - the polyethylene is intimately mixed with constituents capable of forming a thixotropic concrete, - the boron carbide is added, - we add water, the mixture is poured into the container for which it is intended while keeping it in vibration, and - the mixture is allowed to harden. 5. Application du produit selon l'une quelconque des revendications 1 à 3 à la réalisation de châteaux de stockage ayant une paroi interne et une paroi externe entre lesquelles se trouve un produit absorbant les neutrons, caractérisée en ce qu'on recouvre la face interne de la paroi externe d'une peinture à base de carbure de bore, puis on coule le produit selon l'une quelconque des revendications 1 à 3 entre la paroi interne et la paroi externe dudit château de stockage.5. Application of the product according to any one of claims 1 to 3 to the production of storage castles having an internal wall and an external wall between which there is a neutron absorbing product, characterized in that the internal face is covered of the external wall of a paint based on boron carbide, then the product according to any one of claims 1 to 3 is poured between the internal wall and the external wall of said storage castle.
EP82400401A 1981-03-13 1982-03-08 Neutron absorbing material, method to produce the same and application of this material to the manufacture of storage containers Withdrawn EP0060765A1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR8105057 1981-03-13
FR8105057A FR2501895A1 (en) 1981-03-13 1981-03-13 PRODUCT ABSORBING NEUTRONS, METHOD FOR MANUFACTURING THE SAME, AND APPLICATION OF SAID PRODUCT TO STORAGE CASTLES

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DE3225788A1 (en) * 1982-05-07 1984-01-12 Selim Dipl.-Ing. 8000 München Mourad Building material and process for the manufacture thereof
WO1999066512A2 (en) * 1998-06-15 1999-12-23 Kurnosov Vladimir Aleksandrovi Protection structure against radioactive substances, and method and material for realising said structure
WO2002037906A2 (en) * 2000-11-01 2002-05-10 Axcelis Technologies, Inc. Mechanism for containment of neutron radiation in ion implanter beamline

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Cited By (5)

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Publication number Priority date Publication date Assignee Title
DE3225788A1 (en) * 1982-05-07 1984-01-12 Selim Dipl.-Ing. 8000 München Mourad Building material and process for the manufacture thereof
WO1999066512A2 (en) * 1998-06-15 1999-12-23 Kurnosov Vladimir Aleksandrovi Protection structure against radioactive substances, and method and material for realising said structure
WO1999066512A3 (en) * 1998-06-15 2000-01-27 Vladimir Aleksandrovi Kurnosov Protection structure against radioactive substances, and method and material for realising said structure
WO2002037906A2 (en) * 2000-11-01 2002-05-10 Axcelis Technologies, Inc. Mechanism for containment of neutron radiation in ion implanter beamline
WO2002037906A3 (en) * 2000-11-01 2002-09-06 Axcelis Tech Inc Mechanism for containment of neutron radiation in ion implanter beamline

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JPS57170857A (en) 1982-10-21

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