EP0062831B1 - Container for a long term storage of radioactive materials - Google Patents

Container for a long term storage of radioactive materials Download PDF

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Publication number
EP0062831B1
EP0062831B1 EP82102660A EP82102660A EP0062831B1 EP 0062831 B1 EP0062831 B1 EP 0062831B1 EP 82102660 A EP82102660 A EP 82102660A EP 82102660 A EP82102660 A EP 82102660A EP 0062831 B1 EP0062831 B1 EP 0062831B1
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EP
European Patent Office
Prior art keywords
copper
container
term storage
radioactive materials
oxide particles
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
Application number
EP82102660A
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German (de)
French (fr)
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EP0062831A1 (en
Inventor
Hartmut Dipl. Phys. Kroll
Günther Dr. Dipl. Chem. Luthardt
Horst Dr. Dipl. Chem. Vietzke
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.)
Deutsche Gesellschaft fuer Wiederaufarbeitung von Kernbrennstoffen mbH
Nukem GmbH
Original Assignee
Deutsche Gesellschaft fuer Wiederaufarbeitung von Kernbrennstoffen mbH
Nukem GmbH
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Application filed by Deutsche Gesellschaft fuer Wiederaufarbeitung von Kernbrennstoffen mbH, Nukem GmbH filed Critical Deutsche Gesellschaft fuer Wiederaufarbeitung von Kernbrennstoffen mbH
Publication of EP0062831A1 publication Critical patent/EP0062831A1/en
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Publication of EP0062831B1 publication Critical patent/EP0062831B1/en
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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
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/28—Treating solids
    • G21F9/34—Disposal of solid waste
    • G21F9/36—Disposal of solid waste by packaging; by baling
    • 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
    • G21F5/00—Transportable or portable shielded containers
    • G21F5/005—Containers for solid radioactive wastes, e.g. for ultimate disposal

Definitions

  • the invention relates to a container for long-term storage of radioactive substances, in particular radioactive fuel elements, in suitable geological formations, consisting essentially of a container body and a lid made of a copper-based alloy.
  • Irradiated, spent fuel elements are processed either immediately after temporary storage in water basins or after a limited further interim storage.
  • the nuclear fuels and broods are separated from the fission products and returned to the fuel cycle.
  • the fission products are conditioned by known methods, usually using large amounts of valuable materials, such as lead and copper, and in practical geological formations they are virtually no longer removable.
  • Containers made of alloyed and unalloyed steels, copper and corundum are proposed as packaging for radioactive materials, especially for irradiated fuel elements.
  • the containers are either not sufficiently corrosion-resistant or, like copper, are very expensive.
  • the corrosion behavior of even copper is not always sufficient.
  • Corundum containers are generally suitable, but the experience required for their manufacture is lacking.
  • the fuel elements for packaging would have to be disassembled into small corundum containers for manufacturing reasons, which is possible, but is associated with considerable costs and safety-related expenses.
  • the invention was therefore based on the object of creating a container for the long-term storage of radioactive waste, in particular spent fuel elements, in suitable geological formations, consisting essentially of a container body and a lid made of copper-based alloys, which can also be used for a long time with particularly economical use of valuable material Periods is corrosion-proof.
  • the container body and lid consist of a copper-based alloy with 2 to 20% tin or 6 to 10% aluminum, which contains dispersed oxide particles.
  • the copper-based alloy with 6 to 10% aluminum contains iron and / or nickel in addition to aluminum.
  • Processing takes place in a manner known per se, inter alia by continuous casting or centrifuging molding.
  • certain copper-based alloys e.g. B. »Tin bronze « to be deposited electrolytically on a suitable thin carrier material, which alone is not a container coating function.
  • dispersed oxide particles are, for example, tin oxide (Sn0 2 ), thorium oxide (ThO 2 ), rare earth oxides, for. B. of gadolinium and samarium, but also tungsten oxide (W0 3 ) suitable, in some cases also uranium dioxide (U0 2 ).
  • non-oxides such as e.g. B. boron carbide (B 4 C) may be included. All of these dispersed particles can, depending on the nature of the radioactive container contents, improve the shielding against radioactive radiation.
  • the dispersed oxide particles consist of uranium oxide U 3 0 8 , since this oxide because of its shielding action and because of its inert chemical behavior, but also because of its z. B. compared to »tin bronze favorable density, is ideally suited for this purpose. It is expedient to use U 3 0 8 powder which contains uranium depleted in U-235.
  • the copper-based alloys with the alloyed metals and oxide particles mentioned can contain minor amounts of impurities without increasing the corrosion rates, and for electrochemical reasons even an improvement in the corrosion behavior, e.g. B. against salt solutions, may be possible.
  • impurities can u. a. Include iron, lead, arsenic, antimony and bismuth.
  • the figure shows a container for long-term storage of radioactive substances. It consists of a container body (1) and a lid (2). The lid (2) can also be cast onto the container body (1). A copper-based alloy containing dispersed oxide particles (3) is used as the material for the container base body (1) and lid (2).
  • the container according to the invention also has sufficient mechanical stability even with thin wall thicknesses, has excellent corrosion properties with low use of recyclables and is also excellently suitable as an over-container for pre-packaged radioactive materials such as fuel assemblies, fuel rods and waste.
  • the container according to the invention can be equipped with the usual handling aids. Furthermore, the container can also be equipped with an optionally removable cooling fin jacket and with further additional auxiliary devices.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Environmental & Geological Engineering (AREA)
  • Packages (AREA)
  • Closures For Containers (AREA)
  • Details Of Rigid Or Semi-Rigid Containers (AREA)

Description

Gegenstand der Erfindung ist ein Behälter zur Langzeitlagerung von radioaktiven Stoffen, insbesondere von radioaktiven Brennelementen, in geeigneten geologischen Formationen, im wesentlichen aus einem Behältergrundkörper und einem Deckel aus einer Kupferbasislegierung bestehend.The invention relates to a container for long-term storage of radioactive substances, in particular radioactive fuel elements, in suitable geological formations, consisting essentially of a container body and a lid made of a copper-based alloy.

Bestrahlte, abgebrannte Brennelemente werden nach einer vorübergehenden Aufbewahrung in Wasserbecken entweder sofort oder nach einer begrenzten weiteren Zwischenlagerung aufgearbeitet. Dabei werden die nuklearen Brenn-und Brutstoffe von den Spaltprodukten abgetrennt und wieder dem Brennstoffkreislauf zugeführt. Die Spaltprodukte werden nach bekannten Verfahren, meist unter Verwendung großer Mengen Wertstoffe, wie zum Beispiel Blei und Kupfer, konditioniert und in geeigneten geologischen Formationen praktisch nicht mehr entnehmbar endgelagert.Irradiated, spent fuel elements are processed either immediately after temporary storage in water basins or after a limited further interim storage. The nuclear fuels and broods are separated from the fission products and returned to the fuel cycle. The fission products are conditioned by known methods, usually using large amounts of valuable materials, such as lead and copper, and in practical geological formations they are virtually no longer removable.

Darüber hinaus wird überlegt, die bestrahlten Brennelemente in absehbarer Zeit nicht aufzuarbeiten, auf die in ihnen vorhandenen Brenn- und Brutstoffe zunächst zu verzichten und die Brennelemente - nach einer angemessenen Abklingzeit in dafür vorgesehenen Lagern - gegebenenfalls wieder entnehmbar endzulagern. Die Lagerzeiten können mehrere Generationen bis zu etwa tausend Jahren betragen, wobei sich das Gefährdungspotential des radioaktiven Inventars in dieser Zeit, den bekannten physikalischen Gesetzen folgend, entsprechend seiner Zusammensetzung außerordentlich stark verringert.In addition, it is being considered not to reprocess the irradiated fuel assemblies in the foreseeable future, to initially dispense with the fuels and broods present in them and, after an appropriate decay time in the storage facilities provided for this purpose, to be disposed of again if necessary. The storage times can be several generations up to about a thousand years, whereby the risk potential of the radioactive inventory during this time, following the known physical laws, is reduced extraordinarily greatly according to its composition.

Wegen der unbestimmten Lagerdauer dieser radioaktiven Stoffe, werden an derartige, für die Langzeitlagerung geeignete Behälter, die gegenüber bekannten Transport- und Lagerbehältern eine mehrfache Betriebszeit aufweisen müssen, besondere Anforderungen gestellt, welche die an normale Transport- bzw. Lagerbehälter gestellten Anforderungen weit übersteigen und praktisch nicht vergleichbar sind. Erschwerend kommt hinzu, daß die Behälterlager schwer zugänglich sein müssen und folglich den Überwachungsmöglichkeiten Grenzen gesetzt sind.Because of the indefinite storage period of these radioactive materials, special requirements are placed on such containers suitable for long-term storage, which must have a multiple operating time compared to known transport and storage containers, which far exceed the requirements placed on normal transport or storage containers and are practical are not comparable. To make matters worse, the container storage must be difficult to access and the monitoring options are therefore limited.

Es sind teilweise sehr aufwendige Konzepte bekannt, bestrahlte Brennelemente mittels Behälter aus Metall oder Beton in Salz, Sand oder Felskavernen zu lagern.In some cases, very complex concepts are known for storing irradiated fuel elements in containers made of metal or concrete in salt, sand or rock caverns.

Als Verpackung für radioaktive Stoffe, vor allem für bestrahlte Brennelemente, werden Behälter aus legierten und unlegierten Stählen, aus Kupfer sowie aus Korund vorgeschlgen. Die Behälter sind entweder nicht genügend korrosionsbeständig oder wie solche aus Kupfer sehr teuer. Zudem ist das Korrosionsverhalten selbst von Kupfer nicht immer ausreichend. Behälter aus Korund sind zwar grundsätzlich geeignet, jedoch fehlen die für die Herstellung notwendigen Erfahrungen. Darüber hinaus müßten die Brennelemente zur Verpackung in die aus herstellungsbedingten Gründen nur kleinen Korundbehälter zerlegt werden, was zwar möglich ist, jedoch mit einem erheblichen Kosten- und sicherheitstechnischem Aufwand verbunden ist.Containers made of alloyed and unalloyed steels, copper and corundum are proposed as packaging for radioactive materials, especially for irradiated fuel elements. The containers are either not sufficiently corrosion-resistant or, like copper, are very expensive. In addition, the corrosion behavior of even copper is not always sufficient. Corundum containers are generally suitable, but the experience required for their manufacture is lacking. In addition, the fuel elements for packaging would have to be disassembled into small corundum containers for manufacturing reasons, which is possible, but is associated with considerable costs and safety-related expenses.

Solche Behälter erfüllen die Bedingungen der Langzeitlagerung, wie dichter Einschluß bei den auftretenden Bedingungen, vor allem gegenüber Korrosion, hauptsächlich durch Salzlaugen, nur zum Teil, oder sie müssen sehr dickwandig ausgebildet werden. Dieses bedeutet jedoch nachteilig den Einsatz großer Mengen immer knapper werdender Wertstoffe.Such containers only partially meet the conditions of long-term storage, such as tight containment under the conditions that arise, especially against corrosion, mainly due to brine, or they must be made very thick-walled. However, this means disadvantageously the use of large quantities of increasingly scarce resources.

Aus der EP-A-20 948 sind Behälter bekannt, die aus Kupferbasislegierungen, wie Messing oder Bronze bestehen, jedoch ebenfalls dickwandig ausgebildet sein müssen.From EP-A-20 948 containers are known which consist of copper-based alloys such as brass or bronze, but which also have to be thick-walled.

Der Erfindung lag daher die Aufgabe zugrunde, einen Behälter zur Langzeitlagerung von radioaktiven Abfällen, insbesondere von abgebrannten Brennelementen, in geeigneten geologischen Formationen zu schaffen, im wesentlichen aus einem Behältergrundkörper und einem Deckel aus Kupferbasislegierungen bestehend, der unter besonders sparsamem Einsatz von Wertstoff auch in langen Zeiträumen korrosionssicher ist.The invention was therefore based on the object of creating a container for the long-term storage of radioactive waste, in particular spent fuel elements, in suitable geological formations, consisting essentially of a container body and a lid made of copper-based alloys, which can also be used for a long time with particularly economical use of valuable material Periods is corrosion-proof.

Die Aufgabe wurde erfindungsgemäß dadurch gelöst, daß Behältergrundkörper und Dekkel aus einer Kupferbasislegierung mit 2 bis 20% Zinn oder 6 bis 10% Aluminium bestehen, die dispergierte Oxidteilchen enthält.The object was achieved in that the container body and lid consist of a copper-based alloy with 2 to 20% tin or 6 to 10% aluminum, which contains dispersed oxide particles.

Es wurde gefunden, daß Langzeitlagerbehälter, deren Wandungen und Deckel aus Kupferbasislegierungen, also aus Legierungen mit überwiegendem Kupferanteil, die 2 bis 20% Zinn oder 6 bis 10% Aluminium und zusätzlich dispergierte Oxidteilchen enthalten, gegen aggressive Flüssigkeiten, wie sie gegebenenfalls in geologischen Formationen im extremen Schadensfall vorhanden sein können, besonders korrosionsfest sind. So können in an sich gut geeigneten geologischen Salzlagerstätten in Sonderfällen Salzlösungen auftreten, deren Korrosionsangriff die genannten Kupferbasislegierungen hervorragend widerstehen. Die Korrosionsraten mit Abträgen von wenigen Zehnteln Millimetern während eines tausendjährigen permanenten Salzwasserangriffes sind deutlich geringer als vergleichsweise Kupfer, bekannte Kupferbasislegierungen und andere im Prinzip in Frage kommende Metalle. Dadurch kann der erfindungsgemäße Behälter vorteilhafterweise mit relativ dünnen Wanddicken ausgestattet werden, wobei Wanddicken zwischen 0,5 bis 10 cm besonders günstig sind. Dadurch werden auch überraschend günstige Kostenvorteile erzielt und große Menge seltener werdende Werkstoffe eingespart.It has been found that long-term storage containers, their walls and lids made of copper-based alloys, i.e. alloys with a predominant copper content, which contain 2 to 20% tin or 6 to 10% aluminum and additionally dispersed oxide particles, against aggressive liquids, as may be found in geological formations in the extreme damage can be present, are particularly corrosion-resistant. Thus, in special cases, geological salt deposits, which are well suited per se, can contain salt solutions whose corrosion attack excellently withstands the copper-based alloys mentioned. The corrosion rates with erosion of a few tenths of a millimeter during a thousand-year permanent salt water attack are significantly lower than comparatively copper, known copper-based alloys and other metals that are in principle possible. As a result, the container according to the invention can advantageously be equipped with relatively thin wall thicknesses, wall thicknesses between 0.5 and 10 cm being particularly favorable. As a result, surprisingly favorable cost advantages are achieved and large quantities of materials that are becoming less common are saved.

Es ist besonders vorteilhaft, wenn die Kupferbasislegierung mit 6 bis 10% Aluminium neben Aluminium noch Eisen und/oder Nickel enthält.It is particularly advantageous if the copper-based alloy with 6 to 10% aluminum contains iron and / or nickel in addition to aluminum.

Die Verarbeitung erfolgt auf an sich bekannte Weise, u. a. durch Strangguß oder Schleuderguß. In besonderen Fällen ist es sogar möglich, bestimmte Kupferbasislegierungen, wie z. B. »Zinnbronzen« elektrolytisch auf einem geeigneten dünnen Trägermaterial, das allein keine Behältermantelfunktion darstellt, abzuscheiden.Processing takes place in a manner known per se, inter alia by continuous casting or centrifuging molding. In special cases, it is even possible to use certain copper-based alloys, e.g. B. »Tin bronze« to be deposited electrolytically on a suitable thin carrier material, which alone is not a container coating function.

Als dispergierte Oxidteilchen sind beispielsweise Zinnoxid (Sn02), Thoriumoxid (ThO2) , Oxide der Seltenen Erden, z. B. von Gadolinium und Samarium, aber auch Wolframoxid (W03) geeignet, in einzelnen Fällen auch Urandioxid (U02). Außer Oxidteilchen können auch Nichtoxide, wie z. B. Borkarbid (B4C), enthalten sein. Alle diese dispergierten Teilchen können je nach Beschaffenheit des radioaktiven Behälterinhaltes die Abschirmung von radioaktiver Strahlung verbessern. Besonders vorteilhaft ist es, wenn die dispergierten Oxidteilchen aus dem Uranoxid U308 bestehen, da dieses Oxid wegen seiner Abschirmwirkung und wegen seines inerten chemischen Verhaltens, aber auch wegen seiner z. B. gegenüber »Zinnbronzenct günstigen Dichte, hervorragend geeignet für diesen Zweck ist. Zweckmäßig ist die Verwendung von U308-Pulver, das an U-235 abgereichertes Uran enthält.As dispersed oxide particles are, for example, tin oxide (Sn0 2 ), thorium oxide (ThO 2 ), rare earth oxides, for. B. of gadolinium and samarium, but also tungsten oxide (W0 3 ) suitable, in some cases also uranium dioxide (U0 2 ). In addition to oxide particles, non-oxides such as e.g. B. boron carbide (B 4 C) may be included. All of these dispersed particles can, depending on the nature of the radioactive container contents, improve the shielding against radioactive radiation. It is particularly advantageous if the dispersed oxide particles consist of uranium oxide U 3 0 8 , since this oxide because of its shielding action and because of its inert chemical behavior, but also because of its z. B. compared to »tin bronze favorable density, is ideally suited for this purpose. It is expedient to use U 3 0 8 powder which contains uranium depleted in U-235.

Die Kupferbasislegierungen mit den genannten zulegierten Metallen und Oxidteilchen können geringfügige Verunreinigungsanteile enthalten, ohne die Korrosionsraten zu vergrößern, wobei aus elektrochemischen Gründen sogar eine Verbesserung des Korrosionsverhaltens, z. B. gegen Salzlösungen, möglich sein kann. Zu derartigen Verunreinigungen können u. a. Eisen, Blei, Arsen, Antimon und Wismut gehören.The copper-based alloys with the alloyed metals and oxide particles mentioned can contain minor amounts of impurities without increasing the corrosion rates, and for electrochemical reasons even an improvement in the corrosion behavior, e.g. B. against salt solutions, may be possible. Such impurities can u. a. Include iron, lead, arsenic, antimony and bismuth.

Die Abbildung zeigt einen Behälter zur Langzeitlagerung von radioaktiven Stoffen. Er besteht aus einem Behältergrundkörper (1) und einem Deckel (2). Der Deckel (2) kann auf dem Behältergrundkörper (1) auch aufgegossen sein. Als Material für Behältergrundkörper (1) und Deckel (2) wird eine Kupferbasislegierung verwendet, die dispergierte Oxidteilchen (3) enthält.The figure shows a container for long-term storage of radioactive substances. It consists of a container body (1) and a lid (2). The lid (2) can also be cast onto the container body (1). A copper-based alloy containing dispersed oxide particles (3) is used as the material for the container base body (1) and lid (2).

Der erfindungsgemäße Behälter weist auch bei dünnen Wanddicken noch eine ausreichend mechanische Stabilität auf, hat hervorragende Korrosionseigenschaften bei geringem Wertstoffeinsatz und ist auch als Überbehälter für bereits vorverpackte radioaktive Stoffe, wie Brennelemente, Brennstäbe und Abfälle, ausgezeichnet geeignet.The container according to the invention also has sufficient mechanical stability even with thin wall thicknesses, has excellent corrosion properties with low use of recyclables and is also excellently suitable as an over-container for pre-packaged radioactive materials such as fuel assemblies, fuel rods and waste.

Es liegt im Rahmen der Erfindung, daß der erfindungsgemäße Behälter mit den üblichen Handhabungshilfen ausgestattet werden kann. Weiterhin ist der Behälter auch mit einem gegebenenfalls abnehmbaren Kühlrippenmantel sowie mit weiteren zusätzlichen Hilfseinrichtungen ausstattbar.It is within the scope of the invention that the container according to the invention can be equipped with the usual handling aids. Furthermore, the container can also be equipped with an optionally removable cooling fin jacket and with further additional auxiliary devices.

Claims (3)

1. A receptacle for the long-term storage of radioactive materials and more particularly of spent fuel elements in suitable geological formations, substantially consisting of a main receptacle body and a cover consisting of a copper- absed alloy, characterised in that the main receptacle bocy (1) and the cover (2) consists of a copper-based alloy having from 2 to 20% of tin or from 6 to 10% of aluminium, which alloy contains dispersed oxide particles (3).
2. A receptacle according to claim 1, characterised in that the copper-based alloy contains iron and/or nickel in addition to aluminium.
3. A receptacle according to claims 1 and 2, characterised in that the dispersed oxide particles (3) consist of U308.
EP82102660A 1981-04-11 1982-03-30 Container for a long term storage of radioactive materials Expired EP0062831B1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE3114725 1981-04-11
DE19813114725 DE3114725A1 (en) 1981-04-11 1981-04-11 CONTAINER FOR LONG-TERM STORAGE OF RADIOACTIVE SUBSTANCES (II)

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Publication Number Publication Date
EP0062831A1 EP0062831A1 (en) 1982-10-20
EP0062831B1 true EP0062831B1 (en) 1984-10-31

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EP82102660A Expired EP0062831B1 (en) 1981-04-11 1982-03-30 Container for a long term storage of radioactive materials

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EP (1) EP0062831B1 (en)
JP (1) JPS57179800A (en)
DE (2) DE3114725A1 (en)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS6077299A (en) * 1983-10-04 1985-05-01 オムロン株式会社 Line bus operation managing system
RU2671844C1 (en) * 2017-12-08 2018-11-07 Акционерное общество "АКМЭ-инжиниринг" (АО "АКМЭ-инжиниринг") Method of long-term storage of nuclear fuel and tank for cooling and storage for its implementation

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3781189A (en) * 1971-07-07 1973-12-25 Atlantic Richfield Co Spent nuclear fuel shipping casks
US4227928A (en) * 1978-05-01 1980-10-14 Kennecott Copper Corporation Copper-boron carbide composite particle and method for its production
US4292528A (en) * 1979-06-21 1981-09-29 The Carborundum Company Cask for radioactive material and method for preventing release of neutrons from radioactive material
US4253917A (en) * 1979-08-24 1981-03-03 Kennecott Copper Corporation Method for the production of copper-boron carbide composite

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DE3114725A1 (en) 1982-10-21
JPS57179800A (en) 1982-11-05
EP0062831A1 (en) 1982-10-20
DE3261104D1 (en) 1984-12-06

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