US20040118491A1 - Alloy and tube for nuclear fuel assembly and method for making same - Google Patents

Alloy and tube for nuclear fuel assembly and method for making same Download PDF

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Publication number
US20040118491A1
US20040118491A1 US10/728,237 US72823703A US2004118491A1 US 20040118491 A1 US20040118491 A1 US 20040118491A1 US 72823703 A US72823703 A US 72823703A US 2004118491 A1 US2004118491 A1 US 2004118491A1
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ppm
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tube
tin
iron
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US10/728,237
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Jean-Paul Mardon
Jean Senevat
Daniel Charquet
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Priority claimed from FR9803970A external-priority patent/FR2776821B1/en
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C3/00—Reactor fuel elements and their assemblies; Selection of substances for use as reactor fuel elements
    • G21C3/02—Fuel elements
    • G21C3/04—Constructional details
    • G21C3/06—Casings; Jackets
    • G21C3/07—Casings; Jackets characterised by their material, e.g. alloys
    • Y—GENERAL 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
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00—Energy generation of nuclear origin
    • Y02E30/30—Nuclear fission reactors

Definitions

  • the present invention relates to tubes made from an alloy with a zirconium base intended for making all or the external part of the sheath of a nuclear fuel rod or a guide tube as well as the alloys used to make such tubes.
  • One important although not exclusive application is the manufacture of sheathing tubes for fuel rods designed for those of light water reactors and in particular pressurized water reactors in which the risks of corrosion are particularly high due to a high lithium content and/or risks of boiling.
  • a method of manufacturing tubes enabling a high resistance to corrosion and a satisfactory capacity to withstand creep has already been proposed (FR A-2 729 000 or EP 720 177), starting with an ingot of a zirconium based alloy which also contains 50 to 250 ppm of iron, 0.8 to 1.3% by weight of niobium, less than 1600 ppm of oxygen, less than 200 ppm of carbon and less than 120 ppm of silicon.
  • An object of this invention is to provide an alloy and a method of manufacturing tubes which are even more resistant to corrosion and whose composition will not hamper the rolling stages of manufacture.
  • the invention proposes in particular an alloy with a zirconium base which also contains, by weight, other than the inevitable impurities, 0.03 to 0.25% in total firstly of iron, secondly of at least one of the elements from the group comprising chromium and vanadium, with 0.8 to 1.3% of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon, the ratio between the iron content firstly and the chromium or vanadium content secondly ranging between 0.5 and 30.
  • an alloy of this type can also be used to make grill plates for a nuclear fuel assembly.
  • the invention also proposes a casing tube for a nuclear fuel rod or guide tube for a fuel assembly made from an alloy with a zirconium base, also containing, by weight, 0.03 to 0.25% in total of, firstly iron, secondly, at least one of the elements from the group comprising chromium and vanadium, 0.8 to 1.3% by weight of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon, in the recrystallized state, at least the greater part of the iron therein being in the form of Zr(Nb,Fe,Cr) 2 or Zr(Nb,Fe,v) 2 .
  • the invention also proposes a manufacturing method, comprising:
  • a bar of a zirconium based alloy which also contains, other than the inevitable impurities, 0.03 to 0.25% in total firstly of iron, secondly, of at least one of the elements from the group comprising chromium and vanadium, having 0.8 to 1.3% of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon, the ratio between firstly the iron content and secondly the chromium or vanadium content ranging between 0.5 and 30,
  • An oxygen content ranging between 1000 and 1600 ppm is of particular advantage. It may be adjusted by deliberate and controlled addition of zirconia before casting.
  • vanadium may replace some of the chromium for a high Fe/Cr ratio or even all.
  • intermetallic compounds which constitute a Laves phase, precipitate in a very fine form, with a size of between 100 and 200 nanometers. They substitute to the precipitates of phase ⁇ niobium. They significantly improve the resistance in a lithium-containing medium without significantly affecting the uniform resistance to corrosion at a temperature of 400° C., representative of the temperature prevailing in reactors.
  • Table I below illustrates how the iron content affects the corrosion behavior of a sample of zirconium alloy with 1% of niobium for different iron contents: TABLE I Mass increase (mg/dm 2 ) lithium-containing steam water with 70 ppm Li phase Fe 360° C. - 28 days 400°C. - ppm (with pre-filming) 262 days 120 2070 240 1480 1670 250 2920 315 240 4300 25 270
  • Pre-filming is an operation intended to accelerate the response and selectivity of the corrosion test; this operation makes it possible to determine the effect of additives on corrosion more rapidly.
  • the sample was manufactured by thermo-metallurgical operations comparable to those given above, i.e. not exceeding a temperature of 620° C.
  • the lithium content in the water in pressurized water reactors is not more than a few ppm. This being the case, it is of advantage to keep the tin content to less than 300 ppm. A higher content has a slightly adverse affect on resistance to uniform corrosion in water steam at about 415° C. (whereas its effect on nodular corrosion in steam at 500° C. is negligible).
  • tin in a quantity of between 300 and 2000 ppm and in particular between 1000 and 1500 ppm considerably reduces corrosion in an aqueous medium with the levels of lithium content currently used to run reactors. Above 1500 ppm, resistance in the lithium-containing medium is only slightly improved by increasing the tin content so that there would rarely be any point in going above a value of 1500 ppm of tin.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Metallurgy (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Heat Treatment Of Steel (AREA)

Abstract

The invention concerns a method for making tubes designed for a nuclear fuel pencil case or guide tube which consists in forming a bar in a zirconium based alloy containing equally 0.3 to 0.25 wt. % of the total iron, of chromium or vanadium, 0.8 to 1.3 wt. % of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 30 ppm of sulphur and less than 50 ppm of silicon. The bar is soaked in water after being heated at a temperature between 1000° C. and 1200° C. A blank is spun after being heated at a temperature between 600° C. and 800° C. The blank is cold-rolled, in at least three of four passes, to obtain a tube with intermediate heat treatments between 560° C. and 620° C. and s final heat treatment is carried out between 560° C. and 620° C. in inert atmosphere or under vacuum.

Description

  • The present invention relates to tubes made from an alloy with a zirconium base intended for making all or the external part of the sheath of a nuclear fuel rod or a guide tube as well as the alloys used to make such tubes. One important although not exclusive application is the manufacture of sheathing tubes for fuel rods designed for those of light water reactors and in particular pressurized water reactors in which the risks of corrosion are particularly high due to a high lithium content and/or risks of boiling. [0001]
  • A method of manufacturing tubes enabling a high resistance to corrosion and a satisfactory capacity to withstand creep has already been proposed (FR A-2 729 000 or EP 720 177), starting with an ingot of a zirconium based alloy which also contains 50 to 250 ppm of iron, 0.8 to 1.3% by weight of niobium, less than 1600 ppm of oxygen, less than 200 ppm of carbon and less than 120 ppm of silicon.[0002]
  • An object of this invention is to provide an alloy and a method of manufacturing tubes which are even more resistant to corrosion and whose composition will not hamper the rolling stages of manufacture. [0003]
  • To this end, the invention proposes in particular an alloy with a zirconium base which also contains, by weight, other than the inevitable impurities, 0.03 to 0.25% in total firstly of iron, secondly of at least one of the elements from the group comprising chromium and vanadium, with 0.8 to 1.3% of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon, the ratio between the iron content firstly and the chromium or vanadium content secondly ranging between 0.5 and 30. [0004]
  • If it has a low content of iron, chromium, vanadium and tin, an alloy of this type can also be used to make grill plates for a nuclear fuel assembly. [0005]
  • The invention also proposes a casing tube for a nuclear fuel rod or guide tube for a fuel assembly made from an alloy with a zirconium base, also containing, by weight, 0.03 to 0.25% in total of, firstly iron, secondly, at least one of the elements from the group comprising chromium and vanadium, 0.8 to 1.3% by weight of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon, in the recrystallized state, at least the greater part of the iron therein being in the form of Zr(Nb,Fe,Cr)[0006] 2 or Zr(Nb,Fe,v)2.
  • The invention also proposes a manufacturing method, comprising: [0007]
  • forming a bar of a zirconium based alloy which also contains, other than the inevitable impurities, 0.03 to 0.25% in total firstly of iron, secondly, of at least one of the elements from the group comprising chromium and vanadium, having 0.8 to 1.3% of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon, the ratio between firstly the iron content and secondly the chromium or vanadium content ranging between 0.5 and 30, [0008]
  • quenching the bar in water after heating to between 1000° C. and 1200° C., [0009]
  • extruding a blank after heating to a temperature of between 600° C. and 800° C., [0010]
  • cold rolling said blank in at least four passes to obtain a tube, with intermediate heat treatments between 560° C. and 620° C., and [0011]
  • applying a final heat treatment at between 560° C. and 620° C., all heat treatments being applied in an inert atmosphere or under vacuum. [0012]
  • The final heat treatment brings the tube to the recrystallized state without modifying the nature of the phases. [0013]
  • An oxygen content ranging between 1000 and 1600 ppm is of particular advantage. It may be adjusted by deliberate and controlled addition of zirconia before casting. [0014]
  • More often than not, an alloy without vanadium will be used. However, vanadium may replace some of the chromium for a high Fe/Cr ratio or even all. [0015]
  • In alloys containing approximately 1% of Nb, the presence of iron with a content in excess of 75 ppm and chromium and/or vanadium in a content in excess of 5 ppm produces iron contents of not more than 0.20% with intermetallic compounds of the type Zr(Nb, Fe, Cr)[0016] 2 or Zr(Nb,Fe,V)2. Chromium is always present to form such compounds if contained in the alloy in a quantity of more than 5 ppm. The existence of the intermetallic compound reduces the quantity of β phase niobium precipitates and also reduces the niobium content in solid solution.
  • The above-mentioned intermetallic compounds, which constitute a Laves phase, precipitate in a very fine form, with a size of between 100 and 200 nanometers. They substitute to the precipitates of phase β niobium. They significantly improve the resistance in a lithium-containing medium without significantly affecting the uniform resistance to corrosion at a temperature of 400° C., representative of the temperature prevailing in reactors. [0017]
  • It is preferable not to exceed a total Fe+(Cr and/or V) content of 2500 ppm (i.e. 0.25% by weight), even though higher contents remain beneficial in terms of resistance to corrosion in a lithium-containing medium. The reason for this is that, in addition to the Laves phase, a precipitate of the type (Zr, Nb)[0018] 4Fe2 appears, the diameter of which can be as much as 1 μm and which is detrimental from the point of view of rollability. A maximum content of 0.20% constitutes a compromise close to optimum between corrosion in a lithium-containing medium and rollability.
  • The presence of chromium in the intermetallic precipitates of type Zr (Nb, Fe, Cr)[0019] 2 does not have any marked effect on corrosion at 400° C. up to a Fe/Cr ratio of about 30 because in this range, chromium is simply substituted for iron in the intermetallic precipitates as the chromium content increases. The Fe content may be limited to 0.20% to avoid that excess iron causes too high a content in the (Zr, Nb)4Fe2 phase. Improved resistance to corrosion at 400° C. is obtained if the Fe/(Cr+V) ratio is higher than 0.5 and the sum of Fe+Cr+V is at least 0.03%.
  • Table I below illustrates how the iron content affects the corrosion behavior of a sample of zirconium alloy with 1% of niobium for different iron contents: [0020]
    TABLE I
    Mass increase (mg/dm2)
    lithium-containing steam
    water with 70 ppm Li phase
    Fe 360° C. - 28 days 400°C. -
    ppm (with pre-filming) 262 days
    120 2070 240
    1480 1670 250
    2920 315 240
    4300 25 270
  • The contents of C, Si, S, O[0021] 2 and Sn were essentially identical for all samples and were below the maximum values given above; they were less than 300 ppm for tin.
  • Pre-filming is an operation intended to accelerate the response and selectivity of the corrosion test; this operation makes it possible to determine the effect of additives on corrosion more rapidly. [0022]
  • The sample was manufactured by thermo-metallurgical operations comparable to those given above, i.e. not exceeding a temperature of 620° C. [0023]
  • The effect of the Fe/Cr ratio in the precipitates is shown in table 2 below, which gives the increase in weight of alloy samples after being kept in steam for 200 days at a temperature of 400° C. It may be noted that the variation due to change of Fe/Cr is relatively low. [0024]
    TABLE II
    Fe/Cr in the Gain in weight
    precipitates mg/dm2
    0.5 100
    1 110
    2 120
    5 110
    30 100
  • Complementary tests have shown that similar results are obtained if the chromium is replaced by vanadium. The chromium or vanadium contents are selected so as to be low enough not to cause any major difficulties during the metallurgical treatments and in particular rolling. [0025]
  • At present, the lithium content in the water in pressurized water reactors is not more than a few ppm. This being the case, it is of advantage to keep the tin content to less than 300 ppm. A higher content has a slightly adverse affect on resistance to uniform corrosion in water steam at about 415° C. (whereas its effect on nodular corrosion in steam at 500° C. is negligible). [0026]
  • On the other hand, incorporating tin in a quantity of between 300 and 2000 ppm and in particular between 1000 and 1500 ppm considerably reduces corrosion in an aqueous medium with the levels of lithium content currently used to run reactors. Above 1500 ppm, resistance in the lithium-containing medium is only slightly improved by increasing the tin content so that there would rarely be any point in going above a value of 1500 ppm of tin. [0027]
  • The effects described above are set out in Table III below: [0028]
    TABLE III
    Corrosion in autoclave
    Mass gain (mg/dm2)
    mass gain in
    water with 70
    ppm lithium
    after 28 days
    Tin Steam Steam at 360° C.,
    content 1 day 105 days with pre-heating
    as a % at 500° C. at 415° C. in steam
    0.00 37 135 2560
    0.05 43 141 2270
    0.10 43 155 1200
    0.15 42 165 580
    0.25 44 173 280
  • The tests set out in table III, the purpose of which was to ascertain the effect of tin, were conducted on an alloy with a 1% Nb content, iron, chromium and vanadium being present only as impurities. They demonstrate an unexpectedly favorable effect of tin in a lithium-containing medium without any unacceptable degradation as regards corrosion in steam. [0029]
  • The contents of C, Si, S, O[0030] 2 and Sn were substantially identical for all samples and were below the maximum values given above.

Claims (11)

1. Zirconium based alloy also containing, by weight, 0.03 to 0.25% in total firstly of iron and secondly at least one of the elements from the group comprising chromium and vanadium, 0.8% to 1.3% by weight of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon.
2. Sheathing tube for a nuclear fuel rod or guide tube for a nuclear fuel assembly, made from a zirconium based alloy also containing, by weight, 0.03 to 0.25% in total firstly of iron and secondly at least one of the elements from the group comprising chromium and vanadium, 0.8% to 1.3% by weight of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon, in the re-crystallized state, at least the greater part of the iron being in the form Zr(Nb,Fe,Cr)2 or Zr(Nb,Fe,V)2 and in which the intermetallic compounds are of a size not exceeding 200 nm.
3. Tube as claimed in claim 2, characterized in that the oxygen content is between 1000 and 1600 ppm.
4. Tube as claimed in claim 2 or 3, characterized in that the content of tin is less than 300 ppm.
5. Tube as claimed in claim 2 or 3, characterized in that the content of tin is between 300 and 1500 ppm.
6. Sheet of alloy as claimed in claim 1.
7. Method of manufacturing tubes intended for making all or the external part of a sheathing tube for a nuclear fuel rod or a guide tube for a nuclear fuel assembly, characterized in that a bar is formed of a zirconium based alloy which also contains, firstly 0.03 to 0.25% in total firstly of iron, secondly, at least one of the elements from the group comprising chromium and vanadium, 0.8 to 1.3% of niobium, less than 2000 ppm of tin, 500 to 2000 ppm of oxygen, less than 100 ppm of carbon, 5 to 35 ppm of sulfur and less than 50 ppm of silicon,
quenching the bar in water after heating to between 1000° and 1200° C.,
extruding a blank after heating to a temperature of between 600° C. and 800° C.,
cold-rolling said blank in at least four passes to obtain a tube, with intermediate heat treatments between 560° C. and 620° C., and
applying a final heat treatment at between 560° C. and 620° C., all the heat treatments being applied in an inert atmosphere or under vacuum.
8. Method as claimed in claim 7, characterized in that the alloy contains at most 0.20% of iron.
9. Method as claimed in claim 7, characterized in that the Fe/(Cr+V) ratio is between 0.5 and 30 by weight.
10. Method as claimed in claim 7, characterized in that the Fe/(Cr+V) ratio is at least 0.5 and the content of Fe+Cr+V is at least 0.03%.
11. Method as claimed in any one of claims 7 to 10, characterized in that the oxygen content is between 1000 and 1600 ppm.
US10/728,237 1998-03-31 2003-12-03 Alloy and tube for nuclear fuel assembly and method for making same Abandoned US20040118491A1 (en)

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US10/728,237 US20040118491A1 (en) 1998-03-31 2003-12-03 Alloy and tube for nuclear fuel assembly and method for making same

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
FR9803970A FR2776821B1 (en) 1998-03-31 1998-03-31 METHOD OF MANUFACTURING A TUBE FOR ASSEMBLY OF NUCLEAR FUEL
FR9803970 1998-03-31
US64733900A 2000-11-27 2000-11-27
US10/728,237 US20040118491A1 (en) 1998-03-31 2003-12-03 Alloy and tube for nuclear fuel assembly and method for making same

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20100322370A1 (en) * 2009-05-29 2010-12-23 Korea Atomic Energy Research Institute Process of manufacturing zirconium alloy for fuel guide tube and measuring tube having high strength and excellent corrosion resistance
US9284629B2 (en) 2004-03-23 2016-03-15 Westinghouse Electric Company Llc Zirconium alloys with improved corrosion/creep resistance due to final heat treatments
US10221475B2 (en) 2004-03-23 2019-03-05 Westinghouse Electric Company Llc Zirconium alloys with improved corrosion/creep resistance

Citations (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4171992A (en) * 1977-08-09 1979-10-23 Allied Chemical Corporation Preparation of zirconium alloys containing transition metal elements
US4212686A (en) * 1978-03-03 1980-07-15 Ab Atomenergi Zirconium alloys
US4584030A (en) * 1982-01-29 1986-04-22 Westinghouse Electric Corp. Zirconium alloy products and fabrication processes
US4649023A (en) * 1985-01-22 1987-03-10 Westinghouse Electric Corp. Process for fabricating a zirconium-niobium alloy and articles resulting therefrom
US4717428A (en) * 1985-08-02 1988-01-05 Westinghouse Electric Corp. Annealing of zirconium based articles by induction heating
US4981527A (en) * 1987-12-07 1991-01-01 Cezus Tube, bar, sheet or strip made from zirconium alloy resistant both to uniform and nodular corrosion
US5478419A (en) * 1993-10-11 1995-12-26 Compagnie Europeenne Du Zirconium Cezus Process for the manufacture of a flat product of zirconium alloy comprising heating in the β range with infra-red
US5832050A (en) * 1996-04-16 1998-11-03 Compagnie Europeene Du Zirconium Cezus Zirconium-based alloy, manufacturing process, and use in a nuclear reactor
US6125161A (en) * 1997-10-13 2000-09-26 Mitsubishi Materials Corporation Method for making Zr alloy nuclear reactor fuel cladding having excellent corrosion resistance and creep properties
US6863745B1 (en) * 1999-09-30 2005-03-08 Framatome Anp Zirconium based alloy and method for making a component for a nuclear fuel assembly with same

Patent Citations (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4171992A (en) * 1977-08-09 1979-10-23 Allied Chemical Corporation Preparation of zirconium alloys containing transition metal elements
US4212686A (en) * 1978-03-03 1980-07-15 Ab Atomenergi Zirconium alloys
US4584030A (en) * 1982-01-29 1986-04-22 Westinghouse Electric Corp. Zirconium alloy products and fabrication processes
US4649023A (en) * 1985-01-22 1987-03-10 Westinghouse Electric Corp. Process for fabricating a zirconium-niobium alloy and articles resulting therefrom
US4717428A (en) * 1985-08-02 1988-01-05 Westinghouse Electric Corp. Annealing of zirconium based articles by induction heating
US4981527A (en) * 1987-12-07 1991-01-01 Cezus Tube, bar, sheet or strip made from zirconium alloy resistant both to uniform and nodular corrosion
US5478419A (en) * 1993-10-11 1995-12-26 Compagnie Europeenne Du Zirconium Cezus Process for the manufacture of a flat product of zirconium alloy comprising heating in the β range with infra-red
US5832050A (en) * 1996-04-16 1998-11-03 Compagnie Europeene Du Zirconium Cezus Zirconium-based alloy, manufacturing process, and use in a nuclear reactor
US6125161A (en) * 1997-10-13 2000-09-26 Mitsubishi Materials Corporation Method for making Zr alloy nuclear reactor fuel cladding having excellent corrosion resistance and creep properties
US6863745B1 (en) * 1999-09-30 2005-03-08 Framatome Anp Zirconium based alloy and method for making a component for a nuclear fuel assembly with same

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9284629B2 (en) 2004-03-23 2016-03-15 Westinghouse Electric Company Llc Zirconium alloys with improved corrosion/creep resistance due to final heat treatments
US9725791B2 (en) 2004-03-23 2017-08-08 Westinghouse Electric Company Llc Zirconium alloys with improved corrosion/creep resistance due to final heat treatments
US10221475B2 (en) 2004-03-23 2019-03-05 Westinghouse Electric Company Llc Zirconium alloys with improved corrosion/creep resistance
US20100322370A1 (en) * 2009-05-29 2010-12-23 Korea Atomic Energy Research Institute Process of manufacturing zirconium alloy for fuel guide tube and measuring tube having high strength and excellent corrosion resistance

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