EP0865652A1 - Container with a radioactive body - Google Patents

Container with a radioactive body

Info

Publication number
EP0865652A1
EP0865652A1 EP96939924A EP96939924A EP0865652A1 EP 0865652 A1 EP0865652 A1 EP 0865652A1 EP 96939924 A EP96939924 A EP 96939924A EP 96939924 A EP96939924 A EP 96939924A EP 0865652 A1 EP0865652 A1 EP 0865652A1
Authority
EP
European Patent Office
Prior art keywords
container
activated carbon
zeolite
bed
zeoiith
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.)
Granted
Application number
EP96939924A
Other languages
German (de)
French (fr)
Other versions
EP0865652B1 (en
Inventor
Volker Dannert
Joachim Banck
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.)
Siemens AG
Original Assignee
Siemens AG
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 AG filed Critical Siemens AG
Publication of EP0865652A1 publication Critical patent/EP0865652A1/en
Application granted granted Critical
Publication of EP0865652B1 publication Critical patent/EP0865652B1/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Classifications

    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21FPROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F1/00Shielding characterised by the composition of the materials
    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21FPROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F5/00Transportable or portable shielded containers
    • G21F5/005Containers for solid radioactive wastes, e.g. for ultimate disposal
    • YGENERAL 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
    • Y10TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10STECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10S422/00Chemical apparatus and process disinfecting, deodorizing, preserving, or sterilizing
    • Y10S422/903Radioactive material apparatus

Definitions

  • the object of the invention is to improve the retention capacity of the barriers thus formed for radioactive emitters (radionuclides).
  • a container according to the invention in which a capsule which contains a radioactive substance is embedded in a bed of zeolite and / or activated carbon.
  • zeolite and activated carbon absorb or adsorb non-volatile or highly volatile radionuclides and thus offer the possibility of drastically reducing the radioactivity released in the event of a leak in the cap. This applies in particular to radioactive iodine, cesium and strontium. Zeoiith and activated carbon thus relieve the barrier function of the container for radioactive emitters (radionuclides).
  • the bed of Zeoiith and / or activated carbon in the container also leaves enough empty space to hold free NEN noble gases, so that no high internal pressure can develop in the container.Nevertheless, the fill of zeolite and / or activated carbon has sufficient thermal conductivity to dissipate decay heat from the capsule. In addition, the filling represents an additional heat capacity in the container
  • the debris especially if it contains activated carbon, also has a good moderating effect on neutrons and therefore reduces the hardness of neutron radiation that can emanate from the radioactive substance in the capsule. It can also be used to shield gamma radiation emanating from the capsule Contribute to the bulk material
  • the bulk material also represents a mechanical puff for the capsule stored in the container. The bulk material is additionally protected by the bulk material from damage during transport or when handling the container. Radionuclides absorbed by the bulk material are in equilibrium due to chemical laws and thereby lose their tendency to migrate, so that the rubble reliably ensures long-term storage of the capsule.
  • FIG. 1 schematically shows a cross section through a transport and / or storage container with an irradiated nuclear reactor fuel element
  • FIG. 2 shows a schematic cross section of the storage container according to FIG. 1 in a repository
  • This nuclear reactor fuel element 3 has capsules, especially fuel rod 4, and guide tubes 5.
  • the fuel rods 4 are filled with spent nuclear fuel, for example U0 2 and / or U / Pu0 2 , which contains radionuclides.
  • This nuclear fuel is located in a cladding tube of the fuel rods 4, for example made of a zirconium alloy, each of which has a stopper at the two tube ends Zirconium alloy is closed. These zirconium alloy plugs are welded gas-tight to the cladding tube.
  • the guide tubes 5 were used to guide control rods and are open on at least one tube end. They contain no radionuclides.
  • the storage container 2 is filled with a bed 6 of granules of a zeolite. This bed 6 need not be compressed, and the fuel rods 4 and inevitably the guide tubes 5 of the nuclear reactor fuel element 3 are also backfilled with it.
  • the container 2 is made of steel and is gas-tightly welded to a steel plate at both ends.
  • the container 2 which contains the nuclear reactor fuel element 3 with the spent fuel rods, is inserted into a bore which is located, for example, in a salt dome of a repository.
  • a bore which is located, for example, in a salt dome of a repository.
  • another fill 7 on the outside of the container 2 which is also granulate of a zeolite.
  • the container 2 is completely embedded in this fill 7.
  • Activated carbon can also be added to the beds 6 and 7 made of Zeoiith in FIGS. 1 and 2.
  • Zeo ⁇ iith of type A preferably at least one of the substances MgA, CaA and SrA, is particularly suitable for the fillings 6 and 7.
  • Such a type A zeolite can also be doped with silver, so that it contains radioactive iodine particularly well holds back, which possibly emerges from a leak in the cladding tube of a fuel rod 4, but is then already retained in front of the wall of the container 2, the retention effect of which is thus reinforced by the zeolite of the bed 6 in the container 2.
  • Chabazite and mordenite are also well suited for zeolite fillings.
  • Zeolites with the trade name "Zeolon Molecular Sieves" of the 400 Series, 500 Series, 700 Series and 900 Series, which bind Cs and Sr via ion exchange, are particularly well suited.

Abstract

The invention relates to a container (2) in which there is a capsule (4) which contains a radioactive substance and is intended to improve the restraining capacity of the barriers formed for radioactive radiating elements (radionuclides). Said capsule is embedded in a layer (6) of zeolite and/or activated carbon.

Description

Beschreibungdescription
Behälter mit einem radioaktiven KörperContainer with a radioactive body
Es ist bekannt, ein abgebranntes Kernreaktorbrennelement mit Brennstäben, die radioaktiven Kernbrennstoff in einem eine dichtverschlossene Kapsel darstellenden Hüllrohr enthalten, mit Kupfergranulat zwischen den Brennstäben zu verfüllen und anschließend um das Kernreaktorbrennelement bei hohen Tempe- raturen und hohem Druck einen gasdicht verschlossenen Behäl¬ ter aus Kupferblech anzubringen. Dieser gasdicht verschlosse¬ ne Behälter wird in einem Endlager in ein Bohrloch einge¬ bracht, das sich in Granit befindet und das mit Bentonit-Lehm als Barriere gegen radioaktive Strahler (Radionuklide) zuge- füllt wird. Das Kupfergranulat in dem Behälter aus Kupfer¬ blech soll diesem Behälter mechanische Stabilität verleihen.It is known to fill a spent nuclear reactor fuel element with fuel rods, which contain radioactive nuclear fuel in a cladding tube which represents a tightly sealed capsule, with copper granulate between the fuel rods and then around the nuclear reactor fuel element at high temperatures and high pressure, a gas-tightly closed container made of copper sheet to attach. This gas-tightly closed container is placed in a repository in a borehole which is located in granite and which is filled with bentonite clay as a barrier against radioactive emitters (radionuclides). The copper granulate in the copper sheet container is said to give this container mechanical stability.
Der Erfindung liegt die Aufgabe zugrunde, das Rückhaltevermö¬ gen der auf diese Weise für radioaktive Strahler (Radionuklide) gebildeten Barrieren zu verbessern.The object of the invention is to improve the retention capacity of the barriers thus formed for radioactive emitters (radionuclides).
Diese Aufgabe löst ein erfindungsgemäßer Behälter, in dem ei¬ ne Kapsel, die eine radioaktive Substanz enthält, in einer Schüttung aus Zeoiith und/oder Aktivkohle eingebettet ist.This object is achieved by a container according to the invention in which a capsule which contains a radioactive substance is embedded in a bed of zeolite and / or activated carbon.
Zeoiith und Aktivkohle ab- bzw. adsorbieren - abgesehen von Edelgasen - nicht- bzw. leichtflüchtige Radionuklide und bie¬ ten damit die Möglichkeit zu drastischer Reduzierung freige¬ setzter Radioaktivität im Falle einer Undichtigkeit der Kap- sei. Dies gilt insbesondere auch für radioaktives Jod, Cäsium und Strontium. Zeoiith und Aktivkohle entlasten also die Bar¬ rierenfunktion des Behälters für radioaktive Strahler (Radionuklide) .Apart from noble gases, zeolite and activated carbon absorb or adsorb non-volatile or highly volatile radionuclides and thus offer the possibility of drastically reducing the radioactivity released in the event of a leak in the cap. This applies in particular to radioactive iodine, cesium and strontium. Zeoiith and activated carbon thus relieve the barrier function of the container for radioactive emitters (radionuclides).
Die Schüttung aus Zeoiith und/oder Aktivkohle im Behälter läßt auch genügend Leervolumen zur Aufnahme von freigeworde- nen Edelgasen, so daß sich im Behalter kein hoher Innendruck ausbilden kann Trotzdem hat die Schuttung aus Zeoiith und/oder Aktivkohle genügend Wärmeleitfähigkeit zum Abfuhren von Nachzerfallswarme von der Kapsel Außerdem stellt die Schuttung eine zusätzliche Wärmekapazität im Behalter darThe bed of Zeoiith and / or activated carbon in the container also leaves enough empty space to hold free NEN noble gases, so that no high internal pressure can develop in the container.Nevertheless, the fill of zeolite and / or activated carbon has sufficient thermal conductivity to dissipate decay heat from the capsule. In addition, the filling represents an additional heat capacity in the container
Die Schuttung, insbesondere wenn sie Aktivkohle enthalt, hat ferner eine gute Moderationswirkung auf Neutronen und verrin¬ gert deshalb die Harte von Neutronenstrahlung, die von der radioaktiven Substanz m der Kapsel ausgehen kann Auch zur Abschirmung von Gammastrahlung, die von der Kapsel ausgeht, kann die Schuttung beitragen Schließlich stellt die Schut¬ tung auch noch einen mechanischen Puffei für die im Behalter eingelagerte Kapsel dar Letztere wird durch die Schuttung vor Beschädigung beim Transport oder bei der Handhabung αes Behälters zusatzlich geschützt Von der Schuttung absorbierte Radionuklide begeben sich aufgrund chemischer Gesetze in Gleichgewichte und verlieren dadurch ihre Neigung zur Migra¬ tion, so daß die Schuttung eine Langzeitlagerung der Kapsel sicher gewährleistet.The debris, especially if it contains activated carbon, also has a good moderating effect on neutrons and therefore reduces the hardness of neutron radiation that can emanate from the radioactive substance in the capsule. It can also be used to shield gamma radiation emanating from the capsule Contribute to the bulk material Finally, the bulk material also represents a mechanical puff for the capsule stored in the container. The bulk material is additionally protected by the bulk material from damage during transport or when handling the container. Radionuclides absorbed by the bulk material are in equilibrium due to chemical laws and thereby lose their tendency to migrate, so that the rubble reliably ensures long-term storage of the capsule.
Gegenstand der Patentansprüche 2 bis 11 sind vorteilhafte Weiterbildungen des Behälters nach Patentanspruch 1The subject of claims 2 to 11 are advantageous developments of the container according to claim 1
Die Erfindung und ihre Vorteile seien anhand der Zeichnung an zwei Ausführungsbeispielen näher erläutert:The invention and its advantages are explained in more detail with reference to the drawing using two exemplary embodiments:
Figur 1 zeigt schematisiert einen Querschnitt durch einen Transport- und/oder Lagerbehalter mit einem be¬ strahlten Kernreaktorbrennelement,FIG. 1 schematically shows a cross section through a transport and / or storage container with an irradiated nuclear reactor fuel element,
Figur 2 zeigt schematisiert im Querschnitt den Lagerbehal¬ ter nach Fig 1 m einem EndlagerFIG. 2 shows a schematic cross section of the storage container according to FIG. 1 in a repository
Im langgestreckten Lagerbehalter 2 nach Fig. l befindet sich ein Kernreaktorbrennelement 3, dessen quadratischer Umriß ge¬ strichelt angedeutet ist Dieses Kernreaktorbrennelement 3 weist Kapseln, speziell Brennstabe 4, und Fuhrungsrohre 5 auf. Die Brennstäbe 4 sind mit abgebranntem Kernbrennstoff, z.B. U02 und/oder U/Pu02 gefüllt, der Radionuklide enthält Dieser Kernbrennstoff befindet sich m einem Hüllrohr der Brennstäbe 4, z.B aus einer Zirkoniumlegierung, das an bei¬ den Rohrenden jeweils mit einem Stopfen aus Zirkoniumlegie¬ rung verschlossen ist. Diese Stopfen aus Zirkoniumlegierung sind mit dem Hüllrohr gasdicht verschweißt. Die Fuhrungsrohre 5 dienten zum Fuhren von Steuerstäben und sind an mindestens einem Rohrende offen Sie enthalten keine Radionuklide.In the elongated storage container 2 according to FIG. 1 there is a nuclear reactor fuel element 3, the square outline of which is indicated by dashed lines. This nuclear reactor fuel element 3 has capsules, especially fuel rod 4, and guide tubes 5. The fuel rods 4 are filled with spent nuclear fuel, for example U0 2 and / or U / Pu0 2 , which contains radionuclides. This nuclear fuel is located in a cladding tube of the fuel rods 4, for example made of a zirconium alloy, each of which has a stopper at the two tube ends Zirconium alloy is closed. These zirconium alloy plugs are welded gas-tight to the cladding tube. The guide tubes 5 were used to guide control rods and are open on at least one tube end. They contain no radionuclides.
Der Lagerbehälter 2 ist mit einer Schüttung 6 aus Granulat eines Zeoliths aufgefüllt. Diese Schüttung 6 braucht nicht zusammengepreßt zu sein, und mit ihr sind auch die Brennstäbe 4 und zwangsläufig die Führungsrohre 5 des Kernreaktorbren¬ nelements 3 hinterfüllt. Der Behälter 2 besteht aus Stahl und ist an beiden Enden mit einer Stahlplatte gasdicht ver¬ schweißt .The storage container 2 is filled with a bed 6 of granules of a zeolite. This bed 6 need not be compressed, and the fuel rods 4 and inevitably the guide tubes 5 of the nuclear reactor fuel element 3 are also backfilled with it. The container 2 is made of steel and is gas-tightly welded to a steel plate at both ends.
In Figur 2 ist der Behälter 2, der das Kernreaktorbrenneie- ment 3 mit den abgebrannten Brennstäben enthalt, in eine Boh¬ rung eingesetzt, die sich beispielsweise m einem Salzstock eines Endlagers befindet. In dieser Bohrung befindet sich auf der Außenseite des Behälters 2 eine weitere Schuttung 7, die ebenfalls Granulat eines Zeoliths ist. In dieser Schuttung 7 ist der Behälter 2 vollständig eingebettet .In FIG. 2, the container 2, which contains the nuclear reactor fuel element 3 with the spent fuel rods, is inserted into a bore which is located, for example, in a salt dome of a repository. In this hole there is another fill 7 on the outside of the container 2, which is also granulate of a zeolite. The container 2 is completely embedded in this fill 7.
Den Schüttungen 6 und 7 aus Zeoiith m den Figuren 1 und 2 kann auch Aktivkohle beigemischt sein. Zu Zeolithen wira auf Ulimanns "Enzyklopädie der Technischen Chemie", Band 24, Sei¬ ten 575 bis 578, 1983, und auf Ullmanns "Enzyklopädie αer Technischen Chemie", Band 17, Seiten 9 bis 17, 1979 verwie¬ sen. Besonders geeignet ist für die Schuttungen 6 und 7 Zeo¬ iith vom Typ A, vorzugsweise mindestens einer der Stoffe MgA, CaA und SrA. Em solches Zeoiith vom Typ A kann auch mi: Sil¬ ber dotiert sein, so daß es besonders gut radioaktives Jod zurückhält, das möglicherweise aus einem Leck im Hüllrohr ei¬ nes Brennstabs 4 austritt, dann aber schon vor der Wand des Behälters 2 zurückgehalten wird, deren Rückhaltewirkung durch das Zeoiith der Schüttung 6 im Behälter 2 also noch verstärkt ist. Gut geeignet für Zeolithschüttungen sind auch Chabazit und Mordenit. Besonders gut geeignet sind beispielsweise Zeo- lithe mit der Handelsbezeichnung "Zeolon Molecular Sieves" der 400 Series, 500 Series, 700 Series und 900 Series, die über Ionenaustausch Cs und Sr binden.Activated carbon can also be added to the beds 6 and 7 made of Zeoiith in FIGS. 1 and 2. For zeolites we refer to Ulimann's "Encyclopedia of Technical Chemistry", volume 24, pages 575 to 578, 1983, and to Ullmanns "Encyclopedia of Technical Chemistry", volume 17, pages 9 to 17, 1979. Zeo¬ iith of type A, preferably at least one of the substances MgA, CaA and SrA, is particularly suitable for the fillings 6 and 7. Such a type A zeolite can also be doped with silver, so that it contains radioactive iodine particularly well holds back, which possibly emerges from a leak in the cladding tube of a fuel rod 4, but is then already retained in front of the wall of the container 2, the retention effect of which is thus reinforced by the zeolite of the bed 6 in the container 2. Chabazite and mordenite are also well suited for zeolite fillings. Zeolites with the trade name "Zeolon Molecular Sieves" of the 400 Series, 500 Series, 700 Series and 900 Series, which bind Cs and Sr via ion exchange, are particularly well suited.
Partikel aus mindestens einem der Stoffe Metallgrieß, Mn02, Al203, MgO, Su02, Zr02 und Silikat, die mindestens einer der Schüttungen 6 und 7 beigemischt werden, erhöhen die Wärme¬ leitfähigkeit dieser Schüttungen 6 und 7 zum Abführen von Nachzerfallswärme von den Brennstäben 4. Particles of at least one of the materials metal grit, Mn0 2 , Al 2 0 3 , MgO, Su0 2 , Zr0 2 and silicate, which are added to at least one of the beds 6 and 7, increase the thermal conductivity of these beds 6 and 7 for the removal of Post-decay heat from the fuel rods 4.

Claims

Patentansprüche claims
1. Behälter (2) , in dem eine Kapsel (4) , die eine radioaktive Substanz enthält, in einer Schüttung (6) aus Zeoiith und/oder Aktivkohle eingebettet ist.1. Container (2) in which a capsule (4) containing a radioactive substance is embedded in a bed (6) made of zeolite and / or activated carbon.
2. Behälter (2) nach Anspruch 1, in dem die die radioaktive Substanz enthaltende Kapsel (4) ein mit Kernbrennstoff gefüllter Brennstab ist.2. Container (2) according to claim 1, in which the capsule (4) containing the radioactive substance is a fuel rod filled with nuclear fuel.
3. Behälter (2) nach Anspruch 2, in dem der Brennstab zu ei¬ nem Kernreaktorbrennelement (3) gehört, das m der Schüttung3. A container (2) according to claim 2, in which the fuel rod belongs to a nuclear reactor fuel element (3), the m of the bed
(6) aus Zeoiith und/oder der Aktivkohle eingebettet ist.(6) is embedded from Zeoiith and / or the activated carbon.
4. Behälter (2) nach einem der Ansprüche 1 bis 3, der in einer auf seiner Außenseite befindlichen weiteren Schüttung4. Container (2) according to any one of claims 1 to 3, in a further bed located on its outside
(7) aus Zeoiith und/oder Aktivkohle eingebettet ist.(7) is embedded from Zeoiith and / or activated carbon.
5. Behälter (2) nach einem der Ansprüche 1 bis 4 mit einer Schüttung (6) , die Granulat des Zeoliths und/oder der5. Container (2) according to one of claims 1 to 4 with a bed (6), the granules of the zeolite and / or
Aktivkohle ist.Activated carbon is.
6. Behälter (2) nach Anspruch 4 mit der weiteren Schüttung (7) auf seiner Außenseite, die ein Granulat des Zeoliths und/oder der Aktivkohle ist.6. Container (2) according to claim 4 with the further bed (7) on its outside, which is a granulate of the zeolite and / or the activated carbon.
7. Behälter (2) nach einem der Ansprüche 1 bis 5 mit Zeoiith, das vom Typ A ist .7. Container (2) according to one of claims 1 to 5 with Zeoiith, which is of type A.
8. Behälter (2) nach Anspruch 7 mit Zeoiith vom Typ A, daε mindestens einer der Stoffe MgA, CaA und SrA ist.8. Container (2) according to claim 7 with Zeoiith of type A, that is at least one of the substances MgA, CaA and SrA.
9. Behälter (2) nach Anspruch 7 mit Zeoiith vom Typ A, das mit Silber dotiert ist. 9. container (2) according to claim 7 with Zeoiith of type A, which is doped with silver.
10. Behälter (2) nach einem der Ansprüche 1 bis 5 mit Zeoiith, das mindestens einer der Stoffe Chabazit und Mordenit ist .10. Container (2) according to one of claims 1 to 5 with zeolite, which is at least one of the substances chabazite and mordenite.
11. Behälter (2) nach einem der Ansprüche 1 bis 10 mit einer Schüttung (6) und/oder einer weiteren Schüttung (7) aus Zeoiith und/oder Aktivkohle, die beigemischt Partikel aus mindestens einem der Stoffe Metallgrieß, Mn02, A120, , MgO, Sno2, Zr02 und Silikat enthalten. 11. Container (2) according to one of claims 1 to 10 with a bed (6) and / or a further bed (7) made of zeolite and / or activated carbon, which is mixed with particles of at least one of the materials metal grit, Mn0 2 , A1 2nd 0,, MgO, Sno 2 , Zr0 2 and silicate included.
EP96939924A 1995-12-07 1996-11-25 Container with a radioactive body Expired - Lifetime EP0865652B1 (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE19545761A DE19545761A1 (en) 1995-12-07 1995-12-07 Containers with a radioactive body
DE19545761 1995-12-07
PCT/EP1996/005205 WO1997021227A1 (en) 1995-12-07 1996-11-25 Container with a radioactive body

Publications (2)

Publication Number Publication Date
EP0865652A1 true EP0865652A1 (en) 1998-09-23
EP0865652B1 EP0865652B1 (en) 1999-06-02

Family

ID=7779513

Family Applications (1)

Application Number Title Priority Date Filing Date
EP96939924A Expired - Lifetime EP0865652B1 (en) 1995-12-07 1996-11-25 Container with a radioactive body

Country Status (5)

Country Link
US (1) US6699439B1 (en)
EP (1) EP0865652B1 (en)
DE (2) DE19545761A1 (en)
ES (1) ES2133198T3 (en)
WO (1) WO1997021227A1 (en)

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DE202011102838U1 (en) * 2011-07-02 2011-12-27 Ewald von Hagen Radiation protection offset for the prevention and discharge of radioactive radiation in mining
WO2018064572A1 (en) * 2016-09-29 2018-04-05 Elysium Industries Ltd. Silver chloride waste form and apparatus
US10878972B2 (en) 2019-02-21 2020-12-29 Deep Isolation, Inc. Hazardous material repository systems and methods

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Also Published As

Publication number Publication date
EP0865652B1 (en) 1999-06-02
DE59602126D1 (en) 1999-07-08
ES2133198T3 (en) 1999-09-01
US6699439B1 (en) 2004-03-02
DE19545761A1 (en) 1997-06-12
WO1997021227A1 (en) 1997-06-12

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