EP0171684A1 - Process for stabilizing the corrosion resistance of a zirconium alloy cladding tube for nuclear-fuel rods - Google Patents

Process for stabilizing the corrosion resistance of a zirconium alloy cladding tube for nuclear-fuel rods Download PDF

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Publication number
EP0171684A1
EP0171684A1 EP85109390A EP85109390A EP0171684A1 EP 0171684 A1 EP0171684 A1 EP 0171684A1 EP 85109390 A EP85109390 A EP 85109390A EP 85109390 A EP85109390 A EP 85109390A EP 0171684 A1 EP0171684 A1 EP 0171684A1
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Prior art keywords
cladding tube
tube
coolant
zirconium alloy
quenching
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EP85109390A
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German (de)
French (fr)
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Eckard Dipl.-Ing. Steinberg (Fh)
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Kraftwerk Union AG
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Kraftwerk Union AG
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22F—CHANGING THE PHYSICAL STRUCTURE OF NON-FERROUS METALS AND NON-FERROUS ALLOYS
    • C22F1/00—Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working
    • C22F1/16—Changing the physical structure of non-ferrous metals or alloys by heat treatment or by hot or cold working of other metals or alloys based thereon
    • C22F1/18—High-melting or refractory metals or alloys based thereon
    • C22F1/186—High-melting or refractory metals or alloys based thereon of zirconium or alloys based thereon

Definitions

  • the invention relates to a method for stabilizing the corrosion resistance of a cladding tube made of a zirconium alloy for a nuclear reactor fuel rod by moving an annealing zone in the longitudinal direction through the cladding tube and subsequent quenching with a coolant.
  • the increased surface corrosion leads to the formation of local oxide pustules on the shell tube of the nuclear reactor fuel rod, on which the cladding tube of the nuclear reactor fuel rod can finally corrode in extreme cases.
  • the " ⁇ -quenching" dissolves the secondary deposits, and in the subsequent quenching only very small and finely divided secondary deposits are formed, which are no longer the starting cells for nodular corrosion.
  • the invention has for its object to avoid such breaks and coarsening of the secondary excretions in the finished cladding tube.
  • the method of the type mentioned at the outset is characterized according to the invention in that the cladding tube is rotated around the tube axis during annealing and quenching and is held in a straight line with the longitudinal axis aligned on both sides of the annealing zone.
  • This cladding tube 2 is held in a straight line by two pairs of inclined drive rollers 3; 4 and 5; 6 with an exactly aligned longitudinal axis. With these pairs of inclined drive rollers 3.4; and 5; 6 the cladding tube 2 is further rotated about its longitudinal axis and also in the direction of this longitudinal axis i.e. moved in the direction of arrow 7.
  • a quartz tube 8 is arranged between the pairs of inclined drive rollers 3; 4 and 5; 6, through which the cladding tube 2 is guided coaxially and which is flushed on the inside with argon or helium, so that the zirconium alloy of the cladding tube cannot absorb atmospheric nitrogen.
  • annular nozzle 9 which is coaxial with the quartz tube 8 and the cladding tube 2 and has nozzle openings on the inner circumferential surface facing the cladding tube 2.
  • the cladding tube 2 is moved at a feed rate of 1 to 10 mm per second through the quartz cylinder 8 in the direction of its longitudinal axis. At the same time, the cladding tube 2 makes one revolution about its longitudinal axis with a rotational speed in the range from 200 to 2000 revolutions per minute.
  • the cladding tube 2 emerging from the quartz cylinder 8 is sprayed by the nozzle ring 9 with a coolant, which can be water containing hydrogen peroxide, for example. With the hydrogen peroxide on the outside Cladding tube 2 produces a gas-tight, oxidic surface coating.
  • An inert gas containing oxygen for example oxygen-containing argon or helium, can also be used as the coolant if the cooling rate of the cladding tube 2 emerging from the quartz cylinder 8 should not be too high.
  • the feed rate of the cladding tube 2 in the range of 1 to 10 mm per second in the direction of the arrow 7 means that the annealing zone generated with the induction coil 10 in the cladding tube 2 is moved into the cladding tube 2 with the same feed rate.
  • a uniform temperature distribution in the cladding tube 2 is achieved at the annealing zone, which is moreover held in a straight line with the aligned longitudinal axis by the pairs of inclined drive rollers 3; 4 and 5; 6, so that the cladding tube 2 when it has finally left the device shown in the drawing, is not only stabilized against corrosion, but also has no deformations ie is straight and has a circular inner and outer cross section.

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  • Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Heat Treatment Of Articles (AREA)
  • Chemically Coating (AREA)
  • Laminated Bodies (AREA)

Abstract

The cladding tube (2) is set in rotation about the tube axis during annealing by moving it through an annealing zone and subsequent quenching with a coolant; in this way, a cladding tube is obtained which shows no fractures in the tube wall, no coarsened secondary precipitations and no distortions. <IMAGE>

Description

Die Erfindung betrifft ein Verfahren zum Stabilisieren der Korrosionsfestigkeit eines Hüllrohres aus einer Zirkoniumlegierung für einen Kernreaktorbrennstab durch Bewegen einer Glühzone in Längarichtung durch das Hüllrohr und nachfolgendes Abschrecken mit einem Kühlmittel.The invention relates to a method for stabilizing the corrosion resistance of a cladding tube made of a zirconium alloy for a nuclear reactor fuel rod by moving an annealing zone in the longitudinal direction through the cladding tube and subsequent quenching with a coolant.

Dieses Verfahren ist als sogenanntes "β - Quenchen" bekannt. In der Zirkoniumlegierung sind nach dem Ziehen oder Pilgern des Hüllrohres Sekundärausacheidungen mit Legierungsbestandteilen wie z.B. Eisen, Chrom und/oder Nickel vorhanden, die Partikel in der Matrix der Zirkoniumlegierung bilden, einen verhältnismäßig großen mittleren Durchmesser im Bereich von 0.01 bis 0.05 /um haben, die technologischen Eigenschaften der Zirkoniumlegierung wie z.B. ihre Härte und Festigkeit beeinflussen und ein anderes Korrosionsverhalten als die Matrix der Zirkoniumlegierung zeigen. Diese Partikel können die Keimzellen für örtlich erhöhte Oberflächenkorrosion, der sogenannten Nodularkorrosion am Hüllrohr eines in einen Kernreaktor eingesetzten Kernreaktorbrennstabes sein. Die erhöhte Oberflächenkorrosion führt zur Ausbildung von örtlichen Oxidpusteln am Hüllrohr des Kernreaktorbrennstabes, an denen schlieBlich in Extremfall das Hüllrohr des Kernreaktorbrennstabes durchkorrodieren kann. In der Glühzone werden beim "β - Quenchen" die Sekundärausscheidungen aufgelöst, und beim nachfolgenden-Abschrecken bilden sich nur sehr kleine und fein verteilte Sekundärausscheidungen, die nicht mehr Ausgangszellen für Nodularkorrosion sind.This process is known as "beta quenching". In the zirconium alloy, secondary pullings with alloy components such as iron, chromium and / or nickel, which form particles in the matrix of the zirconium alloy, have a relatively large average diameter in the range from 0.01 to 0.05 / um, after pulling or pilgriming the cladding tube influence the technological properties of the zirconium alloy such as its hardness and strength and show a different corrosion behavior than the matrix of the zirconium alloy. These particles can be the germ cells for locally increased surface corrosion, the so-called nodular corrosion on the cladding tube of a nuclear reactor fuel rod used in a nuclear reactor. The increased surface corrosion leads to the formation of local oxide pustules on the shell tube of the nuclear reactor fuel rod, on which the cladding tube of the nuclear reactor fuel rod can finally corrode in extreme cases. In the annealing zone, the "β-quenching" dissolves the secondary deposits, and in the subsequent quenching only very small and finely divided secondary deposits are formed, which are no longer the starting cells for nodular corrosion.

Das "β - Quenchen" führt jedoch zu Verwerfungen (Dimensionsveränderungen) des Hüllrohres, die für die Fertigung von Kernreaktorbrennstäben unzulässig sind. Das "ß - Quenchen* konnte daher nicht am Fertigrohr durchgeführt werden, sondern mußte in eine Zwischenstufe bei der Rohrherstellung gelegt werden. Beim notwendigerweise nachfolgenden Verformen des Rohres durch Ziehen oder Pilgern konnten dann aber Brüche der Rohrwand auftreten. Auch begünstigt dieses nachfolgende Verformen wieder die Bildung von gröberen lokalen Sekundärausscheidungen in der Zirkoniumlegierung des fertigen Hüllrohres.However, "β-quenching" leads to distortions (dimensional changes) of the cladding tube, which are not permitted for the production of nuclear reactor fuel rods. The "ß - quenching * could therefore not be carried out on the finished pipe, but had to be placed in an intermediate stage in pipe production. However, when the pipe was subsequently deformed by pulling or pilgrimage, breaks in the pipe wall could occur. This subsequent deformation also favors the Formation of coarser local secondary deposits in the zirconium alloy of the finished cladding tube.

Der Erfindung liegt die Aufgabe zugrunde, solche Brüche und Vergröberungen der Sekundärausscheidungen im fertigen Hüllrohr zu vermeiden.The invention has for its object to avoid such breaks and coarsening of the secondary excretions in the finished cladding tube.

Zur Lösung dieser Aufgabe ist das Verfahren der eingangs erwähnten Art erfindungsgemäß dadurch gekennzeichnet, daB das Hüllrohr beim Glühen und Abschrecken in Umdrehung um die Rohrachse versetzt und beiderseits der Glühzone geradlinig mit fluchtender Längsachse gehalten wird.To achieve this object, the method of the type mentioned at the outset is characterized according to the invention in that the cladding tube is rotated around the tube axis during annealing and quenching and is held in a straight line with the longitudinal axis aligned on both sides of the annealing zone.

Es wurde gefunden, daB auf diese Weise Verwerfungen des Hüllrohres vermieden werden, so daß das "ß - Quenchen" nicht mehr in Zwischenstufen der Hüllrohrfertigung gelegt zu werden braucht, sondern an fertigen Hüllrohr durchgeführt werden kann.It has been found that warping of the cladding tube is avoided in this way, so that the "β-quenching" no longer has to be carried out in intermediate stages of cladding tube production, but can instead be carried out on finished cladding tube.

Es ist günstig, wenn beim Abschrecken mit dem Kühlmittel auf der Hüllrohraußenfläche ein gasdicht abschließender oxidischer Oberflächenüberzug erzeugt wird. Dadurch wird die Außenoberfläche des Hüllrohres zusätzlich gegen Korrosion in einem Kernreaktor geschützt.It is expedient for a gas-tight, oxidic surface coating to be produced on the outer tube surface during quenching with the coolant. This additionally protects the outer surface of the cladding tube against corrosion in a nuclear reactor.

Die Erfindung und ihre Vorteile seien anhand der Zeichnung in einem Ausführungsbeispiel näher erläutert:

  • In der Zeichnung ist schematisch eine Einrichtung zum Stabilisieren der Korrosionsfestigkeit eines Hüllrohres 2 dargestellt, das aus einer mit Zircaloy 2 bezeichneten Zirkoniumlegierung besteht, die 1.2 bis 1.7 Gew. % Zinn, 0.07 bis 0.2 Gew. % Eisen, 0.05 bis 0.15 Gew. % Chrom,. 0.03 bis 0.08 Gew. % Nickel, 0.07 bis 0.15 Gew. % Sauerstoff und den Rest Zirkonium enthält.
The invention and its advantages are explained in more detail with reference to the drawing in an exemplary embodiment:
  • In the drawing, a device for stabilizing the corrosion resistance of a cladding tube 2 is shown schematically, which consists of a zirconium alloy designated Zircaloy 2, which contains 1.2 to 1.7 wt.% Tin, 0.07 to 0.2 wt.% Iron, 0.05 to 0.15 wt.% Chromium ,. Contains 0.03 to 0.08% by weight of nickel, 0.07 to 0.15% by weight of oxygen and the rest of zirconium.

Dieses Hüllrohr 2 wird durch zwei Paare schräggestellter Antriebsrollen 3;4 und 5;6 geradlinig mit genau fluchtender Längsachse gehalten. Mit diesen Paaren schräggestellter Antriebsrollen 3,4; und 5;6 wird das Hüllrohr 2 ferner in Umdrehung um seine Längsachse versetzt und außerdem in Richtung dieser Längsachse d.h. in Richtung des Pfeiles 7 vorbewegt.This cladding tube 2 is held in a straight line by two pairs of inclined drive rollers 3; 4 and 5; 6 with an exactly aligned longitudinal axis. With these pairs of inclined drive rollers 3.4; and 5; 6 the cladding tube 2 is further rotated about its longitudinal axis and also in the direction of this longitudinal axis i.e. moved in the direction of arrow 7.

Zwischen den Paaren schräggestellter Antriebsrollen 3;4 und 5;6 ist ein Quarzrohr 8 angeordnet, durch das das Hüllrohr 2 koaxial geführt ist und das innen mit Argon oder Helium gespült wird, so daB die Zirkoniumlegierung des Hüllrohres keinen Luftstickstoff aufnehmen kann. Außen auf dem Quarzrohr 8 befindet sich eine koaxiale Induktionsheizspule, die an einem
elektrischen Hochfrequenzgenerator angeschlossen ist und mit der im Hüllrohr 2 innerhalb des Quarzrohres 8 eine GlUhzone erzeugt wird, in der die Zirkoniumlegierung eine Temperatur im Bereich von 900 bis 1200°C hat.A quartz tube 8 is arranged between the pairs of inclined drive rollers 3; 4 and 5; 6, through which the cladding tube 2 is guided coaxially and which is flushed on the inside with argon or helium, so that the zirconium alloy of the cladding tube cannot absorb atmospheric nitrogen. On the outside of the quartz tube 8 there is a coaxial induction heating coil which is attached to one
electrical high-frequency generator is connected and with which a glow zone is generated in the cladding tube 2 within the quartz tube 8, in which the zirconium alloy has a temperature in the range from 900 to 1200 ° C.

An Ende des Quarzrohres 8, an dem das Hüllrohr 2 aus dem Quarzrohr 8 austritt, ist eine zum Quarzrohr 8 und zum Hüllrohr 2 koaxiale Ringdüse 9 angebracht, die auf der inneren Mantelfläche dem Hüllrohr 2 zugewandte Düsenöffnungen aufweist.At the end of the quartz tube 8, at which the cladding tube 2 emerges from the quartz tube 8, there is an annular nozzle 9 which is coaxial with the quartz tube 8 and the cladding tube 2 and has nozzle openings on the inner circumferential surface facing the cladding tube 2.

Das Hüllrohr 2 wird mit einer Vorschubgeschwindigkeit von 1 bis 10 mm pro Sekunde durch den Quarzzylinder 8 hindurch in Richtung seiner Längsachse bewegt. Zugleich vollführt das Hüllrohr 2 um seine Längsachse eine Umdrehung mit einer Umdrehungsgeschwindigkeit im Bereich von 200 bis 2000 Umdrehungen pro Minute. Das aus den Quarzzylinder 8 austretende Hüllrohr 2 wird vom Düsenring 9 mit einem Kühlmittel besprüht, das beispielsweise Wasserstoffperoxid enthaltendes Wasser sein kann. Mit dem Wasserstoffperoxid wird außen auf dem Hüllrohr 2 ein gasdicht abschließender oxidischer Oberflächenüberzug erzeugt. Als Kühlmittel kann auch Sauerstoff enthaltendes Inertgas, z.B. Sauerstoff enthaltendes Argon oder Helium verwendet werden, wenn die AbkUhlgeschwindigkeit des aus den Quarzzylinder 8 austretenden Hüllrohres 2 nicht zu hoch gewählt sein soll.The cladding tube 2 is moved at a feed rate of 1 to 10 mm per second through the quartz cylinder 8 in the direction of its longitudinal axis. At the same time, the cladding tube 2 makes one revolution about its longitudinal axis with a rotational speed in the range from 200 to 2000 revolutions per minute. The cladding tube 2 emerging from the quartz cylinder 8 is sprayed by the nozzle ring 9 with a coolant, which can be water containing hydrogen peroxide, for example. With the hydrogen peroxide on the outside Cladding tube 2 produces a gas-tight, oxidic surface coating. An inert gas containing oxygen, for example oxygen-containing argon or helium, can also be used as the coolant if the cooling rate of the cladding tube 2 emerging from the quartz cylinder 8 should not be too high.

Die Vorschubgeschwindigkeit des Hüllrohres 2 im Bereich von 1 bis 10 mm pro Sekunde in Richtung des Pfeiles 7 bedeutet, daB die mit der Induktionsspule 10 im Hüllrohr 2 erzeugte Glühzone mit der gleichen Vorschubgeschwindigkeit duroh in das Hüllrohr 2 bewegt wird. Durch die Umdrehung des Hüllrohres 2 um seine Längsachse wird an der Glühzone eine über dem Rohrumfang gleichmäßige Tenperaturverteilung im Hüllrohr 2 erzielt, das überdies durch die Paare schräggestellter Antriebsrollen 3;4 und 5;6 geradlinig mit fluchtender Längsachse gehalten ist, so daß das Hüllrohr 2, wenn es schließlich die in der Zeichnung dargestellte Einrichtung verlassen hat,nicht nur gegen Korrosion stabilisiert ist, sondern auch keine Deformationen aufweist d.h. geradlinig ist und einen kreisrunden Innen- und Außenquerschnitt aufweist.The feed rate of the cladding tube 2 in the range of 1 to 10 mm per second in the direction of the arrow 7 means that the annealing zone generated with the induction coil 10 in the cladding tube 2 is moved into the cladding tube 2 with the same feed rate. By rotating the cladding tube 2 about its longitudinal axis, a uniform temperature distribution in the cladding tube 2 is achieved at the annealing zone, which is moreover held in a straight line with the aligned longitudinal axis by the pairs of inclined drive rollers 3; 4 and 5; 6, so that the cladding tube 2 when it has finally left the device shown in the drawing, is not only stabilized against corrosion, but also has no deformations ie is straight and has a circular inner and outer cross section.

Claims (5)

1. Verfahren zum Stabilisieren der Korrosionsfestigkeit eines Hüllrohres aus einer Zirkoniumlegierung für einen Kernreaktorbrennstab durch Bewegen einer Glühzone in Längsrichtung durch das Hüllrohr und nachfolgendes Abschrecken mit einen Kühlmittel, dadurch gekennzeichnet, daß das Hüllrohr (2) beim Glühen und Abschrecken in Umdrehung um die Rohrachse versetzt und beiderseits der GlUhzone geradlinig mit fluchtender Längsachse gehalten wird.1. A method for stabilizing the corrosion resistance of a cladding tube made of a zirconium alloy for a nuclear reactor fuel rod by moving a glow zone in the longitudinal direction through the cladding tube and subsequent quenching with a coolant, characterized in that the cladding tube (2) rotates around the tube axis during annealing and quenching and is held in a straight line on both sides of the glow zone with the longitudinal axis aligned. 2. Verfahren nach Anspruch 1, dadurch ge- kennzeichnet, daß beim Abschrecken mit dem Kühlmittel auf der Hüllrohraußeafläche ein gasdicht abschließender oxidischer Oberflächenüberzug erzeugt wird.2. The method according to claim 1, character- ized in that a gas-tight final oxidic surface coating is generated on the outer tube surface during quenching with the coolant. 3. Verfahren nach Anspruch 2, dadurch ge- kennzeichnet, daB als Kühlmittel Wasserstoffperoxid enthaltendes Wasser verwendet wird.3. The method according to claim 2, characterized in that water containing hydrogen peroxide is used as the coolant. 4. Verfahren nach Anspruch 2, dadurch ge- kennzeichnet, daß als Kühlmittel Sauerstoff enthaltendes Inertgas verwendet wird.4. The method according to claim 2, characterized in that oxygen-containing inert gas is used as the coolant. 5. Verfahren nach Anspruch 1, dadurch ge- kennzeichnet, daß eine Vorschubgeschwindigkeit der GlUhzone im Bereich von 1 bis 10 mm/Sekunde und eine Umdrehungsgeschwindigkeit des Hüllrohres im Bereich von 200 bis 2000 Umdrehungen pro Minute gewählt wird.5. The method according to claim 1, character- ized in that a feed speed of the glow zone in the range of 1 to 10 mm / second and a rotational speed of the cladding tube in the range of 200 to 2000 revolutions per minute is selected.
EP85109390A 1984-08-10 1985-07-26 Process for stabilizing the corrosion resistance of a zirconium alloy cladding tube for nuclear-fuel rods Withdrawn EP0171684A1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE3429567 1984-08-10
DE19843429567 DE3429567A1 (en) 1984-08-10 1984-08-10 METHOD FOR STABILIZING THE CORROSION RESISTANCE OF A PIPE PIPE MADE OF A ZIRCONIUM ALLOY FOR A CORE REACTOR FUEL

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EP0171684A1 true EP0171684A1 (en) 1986-02-19

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EP85109390A Withdrawn EP0171684A1 (en) 1984-08-10 1985-07-26 Process for stabilizing the corrosion resistance of a zirconium alloy cladding tube for nuclear-fuel rods

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19944509A1 (en) * 1999-09-16 2001-04-19 Siemens Ag Component made of zirconium alloy comprises first layer with further layer which reduces diffusion speed of oxygen atoms and/or electrons through the layers

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3826124A (en) * 1972-10-25 1974-07-30 Zirconium Technology Corp Manufacture of tubes with improved metallic yield strength and elongation properties
US4065328A (en) * 1975-05-06 1977-12-27 Atomic Energy Of Canada Limited High strength Sn-Mo-Nb-Zr alloy tubes and method of making same
US4238251A (en) * 1977-11-18 1980-12-09 General Electric Company Zirconium alloy heat treatment process and product
US4360389A (en) * 1975-11-17 1982-11-23 General Electric Company Zirconium alloy heat treatment process
FR2509509A1 (en) * 1981-07-07 1983-01-14 Asea Atom Ab METHOD FOR MANUFACTURING COATING TUBES IN A ZIRCONIUM-BASED ALLOY FOR FUEL BARS FOR NUCLEAR REACTORS

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3826124A (en) * 1972-10-25 1974-07-30 Zirconium Technology Corp Manufacture of tubes with improved metallic yield strength and elongation properties
US4065328A (en) * 1975-05-06 1977-12-27 Atomic Energy Of Canada Limited High strength Sn-Mo-Nb-Zr alloy tubes and method of making same
US4360389A (en) * 1975-11-17 1982-11-23 General Electric Company Zirconium alloy heat treatment process
US4238251A (en) * 1977-11-18 1980-12-09 General Electric Company Zirconium alloy heat treatment process and product
FR2509509A1 (en) * 1981-07-07 1983-01-14 Asea Atom Ab METHOD FOR MANUFACTURING COATING TUBES IN A ZIRCONIUM-BASED ALLOY FOR FUEL BARS FOR NUCLEAR REACTORS

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19944509A1 (en) * 1999-09-16 2001-04-19 Siemens Ag Component made of zirconium alloy comprises first layer with further layer which reduces diffusion speed of oxygen atoms and/or electrons through the layers

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DE3429567A1 (en) 1986-02-20
JPS6148560A (en) 1986-03-10

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