US20060081313A1 - Method for the production of a semi-finished product made of zirconium alloy for the production of a flat product and use thereof - Google Patents
Method for the production of a semi-finished product made of zirconium alloy for the production of a flat product and use thereof Download PDFInfo
- Publication number
- US20060081313A1 US20060081313A1 US10/541,262 US54126205A US2006081313A1 US 20060081313 A1 US20060081313 A1 US 20060081313A1 US 54126205 A US54126205 A US 54126205A US 2006081313 A1 US2006081313 A1 US 2006081313A1
- Authority
- US
- United States
- Prior art keywords
- production
- alloy
- zirconium alloy
- zirconium
- ingot
- 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.)
- Abandoned
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Classifications
-
- 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
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C16/00—Alloys based on zirconium
-
- 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 the production of a semi-finished product made of zirconium alloy intended for the production of a flat product used for the manufacture of fuel assembly elements.
- Fuel assemblies in nuclear reactors cooled by light water for example pressurized water reactors (PWR) and boiling water reactors (BWR), or fuel assemblies of CANDU reactors, contain elements comprising a zirconium alloy with the property of low neutron absorption in the heart of the nuclear reactor.
- PWR pressurized water reactors
- BWR boiling water reactors
- CANDU reactors fuel assemblies of CANDU reactors
- the jacket tubes for the fuel rods and the plates used for production of the spacer grids for the fuel assembly can be made of zirconium alloy, in particular zirconium alloy containing tin and iron such as the alloys Zircaloy 2 or Zircaloy 4.
- the parallelepipedic housings of the fuel assemblies for BWR reactors are also generally produced from flat products of zirconium alloys such as Zircaloy 2 or Zircaloy 4.
- alloys such as the alloy known under the commercial name M5, which essentially comprises zirconium and niobium, are also used for the production of fuel assembly elements in the form of flat or tubular products.
- the zirconium alloys used for the production of fuel assembly elements comprise at least 97% zirconium by weight, the remainder of the composition which represents at most 3% by weight, with the exception of impurities due to the production of the alloy, can comprise various elements and in particlar iron, tin or niobium.
- Zirconium alloys meeting these conditions in relation to their composition, depending on the temperature and the heat treatment to which they are subjected, can take one or the other of the two allotropic forms of zirconium i.e. the alpha phase, which is the phase of zirconium stable at low temperature with a compact hexagonal structure, or the beta phase, which is the phase stable at high temperature with a cubic structure.
- the alpha phase which is the phase of zirconium stable at low temperature with a compact hexagonal structure
- beta phase which is the phase stable at high temperature with a cubic structure.
- zirconium alloys such as the technical alloys used for the production of fuel assembly elements defined above can have a mixed alpha+beta structure.
- Flat products of zirconium alloy are generally produced by numerous successive stages of hot and cold forming and heat treatment.
- the starting product is usually a very large ingot obtained by casting an alloy set to the required composition.
- an ingot is cast with a diameter for example between 400 and 800 mm, and a length between 2 m and 3 m.
- the ingot then undergoes forging operations in a temperature range in which it can be in the ⁇ , ⁇ or ⁇ + ⁇ phase (EP-0.085.552 and U.S. Pat. No. 5,674,330).
- the ingot is heated so that the alloy is in the beta phase, then a first forging stage is performed on the heated ingot in the beta phase.
- the ingot can be heated to 1050° C. for ten hours before forging.
- the product resulting from the forging is quenched from the beta phase.
- the resulting product which constitutes the semi-finished product of the process for producing a flat product is a slab which can have a thickness of the order of 100 mm.
- the slab is then subjected to various hot rolling and cold rolling operations to obtain a flat end product such as a strip with a thickness of 0.2 to 4 mm.
- the heat treatments of quenching and annealing are performed between at least certain of the forming operations of the flat end product.
- the transformation process which has just been described comprises numerous phases of successive treatments and in particular several quenchings from the beta phase to obtain the semi-finished product such as a slab which is hot formed, and the second intermediate product which is cold formed.
- the zirconium alloy product comes into contact with humid air and/or water so that it absorbs hydrogen which fixes in the material in the form of hydrides.
- Hydrides are generally precipitated in a temperature range from 220° C. to 100° C. during the cooling of the product, and the hydrides form in a quantity which is larger and in a form which is coarser as the material absorbs more hydrogen.
- French patent 2,334,763 proposes a process of heat treatment and/or thermomechanical treatment of a zirconium alloy containing over 150 ppm carbon in a temperature range between 830° C. and 950° C. in order to solubilise at least part of the carbon, no subsequent heat treatment being performed at a temperature greater than 950° C.
- the heat treatment or thermomechanical treatment in the temperature range of 830° C. to 950° C., which corresponds to the range in which the alpha and beta phases are present in the alloy, is only performed after a first forging of an ingot in the beta phase followed by quenching in water.
- the objective of the present invention is to propose a method for production of a zirconium alloy semi-finished product containing by weight at least 97% zirconium and intended for the production of flat products, in which a large ingot is produced by casting the zirconium alloy, then by forging the large ingot a semi-finished product intended to be hot rolled then cold rolled to obtain the flat product is produced, heat treatments of quenching and annealing being interspersed between at least certain of the forming operations, where this method simplifies and reduces the cost of production of the product, and limits to low levels the presence of hydrides which have a harmful effect on the formability and corrosion resistance of the zirconium alloy product.
- the semi-finished product is produced from the large cast ingot by a single forging operation at a temperature at which the zirconium alloy is in a state comprising the crystalline ⁇ and ⁇ phases of the zirconium alloy.
- the invention also relates to the use of the method for production of a slab intended for production of a flat product of a thickness between 0.2 mm and 4 mm for the manufacture of a nuclear fuel assembly element such as a plate of a spacer grid for the fuel assembly of a PWR reactor or a wall of a fuel assembly housing for a BWR reactor or again a fuel assembly element for a CANDU reactor.
- a nuclear fuel assembly element such as a plate of a spacer grid for the fuel assembly of a PWR reactor or a wall of a fuel assembly housing for a BWR reactor or again a fuel assembly element for a CANDU reactor.
- FIG. 1 is a diagram showing in a symbolic manner the various stages of the production method of the prior art.
- FIG. 2 is a diagrammatic representation similar to that in FIG. 1 of the production method according to the invention serving to produce the semi-finished product.
- FIG. 1 shows a cast ingot 1 which can be a large ingot, the diameter of which can be between 400 mm and 800 mm and the length between 2 m and 3 m, which is obtained by casting a zirconium alloy used for the production of flat products for the manufacture of fuel assembly elements.
- the zirconium alloy can be for example a Zircaloy 2 alloy comprising in weight from 1.2% to 1.7% tin, 0.07% to 0.20% iron, 0.05% to 0.15% chromium, 0.03% to 0.08% nickel, at most 120 ppm silicon and 150 ppm carbon, the remainder of the alloy being constituted by zirconium with the exception of the usual impurities.
- the alloy for production of the flat product can be also a Zircaloy 4 comprising by weight 1.2% to 1.7% tin, 0.18% to 0.24% iron, 0.07% to 0.13% chromium, at most 150 ppm carbon, the remainder of the alloy being constituted by zirconium and impurities.
- the alloy is cast as a large ingot 1 which is then brought to a temperature higher than 1000° C. and for example a temperature of 1050° C. for ten hours so that the alloy of the ingot is entirely in the beta cubic phase, stable at high temperature.
- the cast ingot is then forged at a temperature in the beta range of the alloy and for example at a temperature close to 1000° C. in the form of a flat product of substantial thickness known as a slab, as shown by stage 2 on FIG. 1 .
- the thick slab 3 then undergoes quenching in water or humid air as shown symbolically by the arrows representing a third stage 4 of the production process.
- the thick slab 3 is forged at a temperature in the alpha range of the zirconium alloy, for example at a temperature of the order of 800° C.
- the initial forging of the ingot 1 in the beta phase must be followed by quenching in the beta phase (stage 2 of the process) as the metal, which cools during forging, can contain an external zone in the alpha+beta phase leading to the formation of segregations of alphagenic elements such as tin and oxygen and betagenic elements such as iron, chromium, nickel or niobium, depending on the elements contained in the alloy.
- alphagenic elements such as tin and oxygen
- betagenic elements such as iron, chromium, nickel or niobium
- Quenching in the beta phase entails the slab 3 coming into contact with a quenching environment constituted by water or humid air, i.e. an environment containing hydrogen.
- Hydrogen is absorbed by the slab at the time of heat treatment and fixes inside the alloy in the form of hydrides.
- the large cast ingot 1 of zirconium alloy is subjected to a single forging operation 7 in the ⁇ + ⁇ phase to obtain the slab 8 substantially similar to the slab 3 obtained by the complex forging process in the ⁇ phase, quenching from the ⁇ phase and forging in the ⁇ phase.
- the method according to the invention thus comprises replacing the three first stages 2, 4 and 5 of the process of the prior art, i.e. stage 2 of forging in the beta phase (above 1000° C.) followed by stage 4 of quenching the slab 3 ′ from the beta phase and forging in the alpha phase at a temperature below 800° C., with a single stage 7 of forging in the alpha+beta phase, for example in the case of alloys Zircaloy 2 and 4, at a temperature between 850° C. and 950° C. and for example at a temperature of the order of 900° C.
- the temperature for the ⁇ + ⁇ phase forging is selected so that the volume proportion of the ⁇ phase in the ingot alloy is between 10% and 90%, the remainder of the alloy being in the ⁇ phase.
- the ingot 1 is forged to give a slab 8 of thickness which can be of the order of 100 mm and which constitutes the semi-finished product that will then be subjected to the operations of hot rolling and cold rolling as described above, separated by stages of quenching and annealing as heat treatment.
- the quantity of hydrides contained in the alloy obtained by the process according to the invention is substantially smaller than the quantity of hydrides contained in a product according to the prior art.
- the hydrides precipitated in the product according to the invention are also of a size generally smaller than the hydrides precipitated in a flat product according to the prior art.
- one of the advantages of the method according to the invention is to simplify considerably the process of production of the semi-finished product. This therefore leads to a substantial reduction in cost and duration in the implementation of the process.
- the product is only brought to a temperature in the ⁇ and ⁇ range, i.e. a temperature markedly lower than the sustained temperature in the ⁇ phase of the process in the prior art.
- the forging of the ingot 1 in the ⁇ + ⁇ phase is performed in a temperature interval ranging from 850° C. to 950° C. and for example at 900° C.
- the transition to the ⁇ + ⁇ phase of the alloy, to perform the forging of the method according to the invention can lead to the formation of tin segregations.
- the forging temperature in the ⁇ + ⁇ phase can be substantially lower than 900° C. taking into account however the malleability properties of the alloy at the forging temperature.
- zirconium alloys other than Zircaloy or to niobium alloys can be considered.
- These alloys generally contain at most 3% in weight of additive elements comprising at least one of the additive elements tin, iron, chromium, nickel, oxygen, niobium, vanadium and silicon, the remainder of the alloy being constituted by zirconium and the inevitable impurities.
- the invention applies in particular to the production of a flat product of zirconium alloy for the manufacture of fuel assembly elements such as plates for the manufacture of spacer grids for assemblies for PWR-type nuclear reactors or housing walls for assemblies for BWR reactors or for fuel assembly elements for CANDU reactors.
- the temperature for forging in the ⁇ + ⁇ phase depends on the composition of the zirconium alloy.
- the forging operations can be performed using the normal means for forging in the ⁇ phase or ⁇ phase of the process of the prior art or other means adapted to ⁇ + ⁇ phase forging in a single operation to obtain a slab.
- the invention applies generally to any technical zirconium alloy product defined by the composition limits given above.
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Crystallography & Structural Chemistry (AREA)
- Forging (AREA)
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
FR0300316 | 2003-01-13 | ||
FR0300316A FR2849865B1 (fr) | 2003-01-13 | 2003-01-13 | Procede de fabrication d'un demi-produit en alliage de zirconium pour l'elaboration d'un produit plat et utilisation |
PCT/FR2004/000036 WO2004072318A1 (fr) | 2003-01-13 | 2004-01-09 | Procede de fabrication d’un demi-produit en alliage de zirconium pour l’elaboration d’un produit plat et utilisation |
Publications (1)
Publication Number | Publication Date |
---|---|
US20060081313A1 true US20060081313A1 (en) | 2006-04-20 |
Family
ID=32524867
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US10/541,262 Abandoned US20060081313A1 (en) | 2003-01-13 | 2004-01-09 | Method for the production of a semi-finished product made of zirconium alloy for the production of a flat product and use thereof |
Country Status (8)
Country | Link |
---|---|
US (1) | US20060081313A1 (fr) |
EP (1) | EP1585841A1 (fr) |
JP (1) | JP2006520430A (fr) |
KR (1) | KR20050090456A (fr) |
CN (1) | CN100529148C (fr) |
FR (1) | FR2849865B1 (fr) |
RU (1) | RU2337177C2 (fr) |
WO (1) | WO2004072318A1 (fr) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US10119181B2 (en) | 2013-01-11 | 2018-11-06 | Areva Np | Treatment process for a zirconium alloy, zirconium alloy resulting from this process and parts of nuclear reactors made of this alloy |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US8116422B2 (en) * | 2005-12-29 | 2012-02-14 | General Electric Company | LWR flow channel with reduced susceptibility to deformation and control blade interference under exposure to neutron radiation and corrosion fields |
JP2014077152A (ja) * | 2012-10-09 | 2014-05-01 | Tohoku Univ | Zr合金及びその製造方法 |
Citations (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3645800A (en) * | 1965-12-17 | 1972-02-29 | Westinghouse Electric Corp | Method for producing wrought zirconium alloys |
US5674330A (en) * | 1994-08-30 | 1997-10-07 | Compagnie Europeene Du Zirconium Cezus | Process for the production of zirconium alloy sheet metal having good resistance to nodular corrosion and to deformation under irradiation |
US5844959A (en) * | 1997-08-01 | 1998-12-01 | Siemens Power Corporation | Zirconium niobium tin alloys for nuclear fuel rods and structural parts for high burnup |
US5854818A (en) * | 1997-08-28 | 1998-12-29 | Siemens Power Corporation | Zirconium tin iron alloys for nuclear fuel rods and structural parts for high burnup |
US20060090821A1 (en) * | 2003-01-13 | 2006-05-04 | Pierre Barberis | Method of producing a zirconium alloy semi-finished product for the production of elongated product and use thereof |
US20060215806A1 (en) * | 2003-07-31 | 2006-09-28 | Pierre Barberis | Method for making a flat zirconium alloy product, resulting flat product and fuel, assembly component for nuclear power plant reactor made from said flat product |
US20070053476A1 (en) * | 2003-10-08 | 2007-03-08 | Pierre Barberis | Method of producing a flat zirconium alloy product, flat product thus obtained and a nuclear plant reactor grid which is made from said flat product |
US20080080660A1 (en) * | 2004-08-04 | 2008-04-03 | Pierre Barberis | Method Of Manufacturing A Fuel Cladding Tube For A Nuclear Reactor, And A Tube Obtained Thereby |
Family Cites Families (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR2334763A1 (fr) * | 1975-12-12 | 1977-07-08 | Ugine Aciers | Procede permettant d'ameliorer la tenue a chaud du zirconium et de ses alliages |
ZA8383B (en) * | 1982-01-29 | 1983-12-28 | Westinghouse Electric Corp | High energy beam thermal processing of alpha zirconium alloys and the resulting articles |
CA1214978A (fr) * | 1982-01-29 | 1986-12-09 | Samuel G. Mcdonald | Produits en alliage de zirconium et procedes de fabrication connexes |
JPH059688A (ja) * | 1991-07-06 | 1993-01-19 | Kobe Steel Ltd | 加工性に優れたZr合金圧延材の製造方法 |
FR2801323B1 (fr) * | 1999-11-23 | 2002-02-01 | Cezus Cie Europ Du Zirconium | Alliage a base de zirconium a forte resistance a la corrosion et a l'hydruration par l'eau et la vapeur d'eau et procede de transformation thermomecanique de l'alliage |
KR100441562B1 (ko) * | 2001-05-07 | 2004-07-23 | 한국수력원자력 주식회사 | 우수한 내식성과 기계적 특성을 갖는 지르코늄 합금핵연료 피복관 및 그 제조 방법 |
-
2003
- 2003-01-13 FR FR0300316A patent/FR2849865B1/fr not_active Expired - Fee Related
-
2004
- 2004-01-09 WO PCT/FR2004/000036 patent/WO2004072318A1/fr active Application Filing
- 2004-01-09 US US10/541,262 patent/US20060081313A1/en not_active Abandoned
- 2004-01-09 RU RU2005125715/02A patent/RU2337177C2/ru not_active IP Right Cessation
- 2004-01-09 EP EP04701028A patent/EP1585841A1/fr not_active Withdrawn
- 2004-01-09 CN CNB200480002113XA patent/CN100529148C/zh not_active Expired - Fee Related
- 2004-01-09 KR KR1020057012999A patent/KR20050090456A/ko not_active Application Discontinuation
- 2004-01-09 JP JP2006502091A patent/JP2006520430A/ja active Pending
Patent Citations (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3645800A (en) * | 1965-12-17 | 1972-02-29 | Westinghouse Electric Corp | Method for producing wrought zirconium alloys |
US5674330A (en) * | 1994-08-30 | 1997-10-07 | Compagnie Europeene Du Zirconium Cezus | Process for the production of zirconium alloy sheet metal having good resistance to nodular corrosion and to deformation under irradiation |
US5844959A (en) * | 1997-08-01 | 1998-12-01 | Siemens Power Corporation | Zirconium niobium tin alloys for nuclear fuel rods and structural parts for high burnup |
US5854818A (en) * | 1997-08-28 | 1998-12-29 | Siemens Power Corporation | Zirconium tin iron alloys for nuclear fuel rods and structural parts for high burnup |
US20060090821A1 (en) * | 2003-01-13 | 2006-05-04 | Pierre Barberis | Method of producing a zirconium alloy semi-finished product for the production of elongated product and use thereof |
US20060215806A1 (en) * | 2003-07-31 | 2006-09-28 | Pierre Barberis | Method for making a flat zirconium alloy product, resulting flat product and fuel, assembly component for nuclear power plant reactor made from said flat product |
US20070053476A1 (en) * | 2003-10-08 | 2007-03-08 | Pierre Barberis | Method of producing a flat zirconium alloy product, flat product thus obtained and a nuclear plant reactor grid which is made from said flat product |
US20080080660A1 (en) * | 2004-08-04 | 2008-04-03 | Pierre Barberis | Method Of Manufacturing A Fuel Cladding Tube For A Nuclear Reactor, And A Tube Obtained Thereby |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US10119181B2 (en) | 2013-01-11 | 2018-11-06 | Areva Np | Treatment process for a zirconium alloy, zirconium alloy resulting from this process and parts of nuclear reactors made of this alloy |
Also Published As
Publication number | Publication date |
---|---|
WO2004072318B1 (fr) | 2004-10-28 |
CN100529148C (zh) | 2009-08-19 |
WO2004072318A1 (fr) | 2004-08-26 |
RU2337177C2 (ru) | 2008-10-27 |
RU2005125715A (ru) | 2006-02-10 |
CN1735705A (zh) | 2006-02-15 |
FR2849865B1 (fr) | 2006-01-21 |
FR2849865A1 (fr) | 2004-07-16 |
EP1585841A1 (fr) | 2005-10-19 |
KR20050090456A (ko) | 2005-09-13 |
JP2006520430A (ja) | 2006-09-07 |
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Owner name: COMPAGNIE EUROPEENNE DU ZIRCONIUM-CEZUS, FRANCE Free format text: ASSIGNMENT OF ASSIGNORS INTEREST;ASSIGNORS:BARBERIS, PIERRE;RIZZI, JOSEPH NOEL;ROBBE, XAVIER;REEL/FRAME:017414/0309;SIGNING DATES FROM 20050613 TO 20050620 |
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STCB | Information on status: application discontinuation |
Free format text: ABANDONED -- FAILURE TO RESPOND TO AN OFFICE ACTION |