EP1026269A1 - Superlegierung mit hoher Schmelztemperatur und Verfahren zu ihrer Herstellung - Google Patents

Superlegierung mit hoher Schmelztemperatur und Verfahren zu ihrer Herstellung Download PDF

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Publication number
EP1026269A1
EP1026269A1 EP00300755A EP00300755A EP1026269A1 EP 1026269 A1 EP1026269 A1 EP 1026269A1 EP 00300755 A EP00300755 A EP 00300755A EP 00300755 A EP00300755 A EP 00300755A EP 1026269 A1 EP1026269 A1 EP 1026269A1
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Prior art keywords
superalloy
phase
atomic
base
iridium
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French (fr)
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EP1026269B1 (de
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Yoko Mitarai
Yuefeng Gu
Shizuo Nakazawa
Xihong Yu
Yoshikazu Ro
Hiroshi Harada
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National Research Institute for Metals
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National Research Institute for Metals
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C19/00—Alloys based on nickel or cobalt
    • C22C19/03—Alloys based on nickel or cobalt based on nickel
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C5/00—Alloys based on noble metals
    • C22C5/04—Alloys based on a platinum group metal

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  • the present invention relates to a high-melting superalloy. More specifically, the invention relates to a new high-melting superalloy having an excellent high-temperature strength and a good ductility, which is useful as a material for high-temperature instruments such as a gas turbine for electric power generation, a jet engine, a rocket engine, etc.
  • Turbine blades and turbine vanes used for high-temperature instruments such as a gas turbine for electric power generation, a jet engine, a rocket engine, etc., are used under high-temperature and high-stress conditions. Hitherto, for theses turbine blades and turbine vanes, Ni-base superalloys having a high heat resistance and an excellent high-temperature strength have been used but the use temperature have become severe year by year. This is because the increase of a combustion gas temperature is the most effective correspondence to further increase the output and the heat efficiency of high-temperature instruments.
  • the improvement in the high-temperature strength has been desired, wich means, in other words, that the improvement in the high-temperature strength of materials used for turbine blades and turbine vanes is indispensable.
  • the durable temperature of Ni-base superalloys capable of having a substantial, strength is about 1,100°C. If a new material, which can be used at a temperature higher than the temperature and can be realized at a relatively low cost, can be developed, it is very useful for practical use.
  • Ni-base superalloys having superior high-temperature strength various investigations have hitherto been made in order to improve an acid resistance, a corrosion resistance, etc.
  • the present inventors have proposed to improve the high-temperature strength and the high-temperature corrosion resistance by solid-solution strengthenedNi-basesuperalloys in which from 0.1 to 5 atomic % of iridium (Ir) is added, whereby iridium is subjected to solid solution in a ⁇ -phase and a ⁇ '-phase (see Japanese Patent Laid-Open No. 183281/1998).
  • the present inventors have also already proposed high-melting alloys having two crystal structures, i.e., an FCC structure and an LI 2 structure, in which iridium, rhodium or a mixture thereof is added with niobium, tantalum, titanium, aluminum, etc., as alloys having excellent high-temperature strength characteristics and oxidation resistance characteristics (see Japanese Patent Laid-Open No. 311584/1996).
  • Ni-base heat-resistant superalloys are lowered in ductility with an improvement in the strength and are trou lesome as practically useful heat-resistant materials.
  • the prior above iridium-base alloys or rhodium base alloys are high in cost of the raw materials and involve disadvantages in general-purpose properties. In this sense, the Ni-base superalloys which are relatively cheap and can be easily handled are advantageous.
  • Ni-base heat-resistant superalloys can not used at the temperature condition of above 1,300°C as a melting point.
  • the present invention has been made in view of the circumstances as described above, and the invention relates to a new high-melting superalloy which can further improve the output arid the heat efficiency of high-temperature instruments, has the characteristics better in not only high-temperature strength but also ductility than the related art Ni-base superalloys, and can be realized at a relatively low cost.
  • the present inventors have discovered that by compounding or mixing an iridium-base alloy (melting point: 2,447°C) or a rhodium-base alloy (meltpoint: 1,960°C) having a high-melting point and a high strength at a high temperature and being excellent in the oxidation resistance with nickel or a nickel-base alloy (density: 8.9 g/cm 3 (cf., density of an iridium-base superalloy: 22.4 g/cm 3 , density of a rhodium-base superalloy: 12.44 g/cm 3 )), which is light-weight, is excellent in ductility, and is inexpensive as compared with the above-described "superalloys, followed by ingoting, a superalloy wherein both phases of an fcc phase and an LI 2 phase are formed in the texture, and a deposit having an LI 2 structure in the matrix phase having an fcc structure is conformity-
  • a first aspect of the present invention is to provide a high-melting superalloy comprising (A) from 5 to 65 atomic % of nickel and (B) from 5 to 20 atomic % of at least one metal selected from the group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum, with (C) from 30 to 75 atomic % of iridium or rhodium, or a mixture thereof, wherein a LI 2 phase is precipitated in a fcc phase of the matrix phase, and an amount of the LI 2 phase is from 20 to 80% by volume.
  • a second aspect of the invention is to provide the high-melting superalloy according to the first aspect, wherein an atomic ratio of sum of (A) and (B) is from 20 to 70%.
  • a third aspect of the invention is to provide the high-melting superalloy according to the first or second aspect, wherein, in case that the metal (c) is iridium, an atomic ratio of (A) to (B) is from 0.3;1 to 8:1.
  • a fourth aspect of the invention is to provide the high-melting superalloy according to the first or second aspect, wherein, in case that the method (C) is rhodium, the atomic ratio of (A) to (B) is from 0.25:1 to 12:1.
  • a fifth aspect of the invention is to provide the high-melting superalloy comprising (A) from 4 to 86 atomic % of nickel, (B) from 0.5 to 20 atomic % of at least one metal selected from the group consisting of titanium, zirconium, habrium, vanadium, niobium, and tantalum, and (C) from 4 to 86 atomic % of iridium or rhodium, or a mixture thereof, with (D) from 0.4 to 20 atomic % of aluminum, wherein a LI 2 phase is precipitated in a fcc phase of the matrix phase, and an amount of the LI 2 phase is from 20 to 80% by volume.
  • the sixth aspect of the invention is to provide the high-melting superalloy according to fifth aspect, wherein the sum of atomic % of (A) and (C), and (B) and (D) are set as follows; (A) + (C) ⁇ 75 atomic % (B) + (D) ⁇ 25 atomic %
  • a seventh aspect of the invention is to provide a method of producing a high-melting superalloy as set forth in any of the first to fourth aspects, which comprises compounding at least one of an iridium-base superalloy made of iridium as a base added with at least one metal selected from the metal group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum and a rhodium-base superalloy made of rhodium as a base added with at least one metal selected from the above-described metal group, with nickel, followed by ingoting to produce a high-melting superalloy.
  • An eighth aspect of the invention is to provide a method of producing a high-melting superalloy as set forth in any of the first to sixth aspects, which comprises compounding at least one of an iridium-base superalloy made of iridium as a base added with at least one metal selected from the metal group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum and a rhodium-base superalloy made of rhodium as base added with at least one metal selected from the above-d scribed metal group, with a nickel-base alloy made of nickel a a base added with at least one metal selected from the above-described metal group, or aluminum, followed by ingoting t produce a high-melting superalloy.
  • the high-melting superalloy according to the invention comprises (A) from 5 to 73 atomic % of nickel and (B) from 2 to 22 atomic % of at least one metal selected from the group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum, with (C) a balance of iridium or rhodium, or a mixture thereof, wherein an fcc phase and a LI2 phase are formed in a texture thereof and the LI2 phase is precipitated in a fcc phase of the matrix phase, and an amount of the LI 2 phase is from 20 to 80% by volume.
  • a proportion of the component (C), i.e., iridium or rhodium, or a mixture thereof, to be contained as a balance is substantially from 30 to 75 atomic %.
  • a sum of atomic % of (A) and (B) is from 20 to 70% and that, in case of iridium as metal (C), an atomic ratio of the component (A) to the component (B) is from 0.3:1 to 8:1. It is further preferred that, in case of rhodium as metal (C), the atomic ratio of the component (A) to the component (B) is from 0.25:1 to 12:1.
  • titanium zirconium, hafnium, vanadium, niobium, and tantalum as the component (C) are particularly preferred niobium, tantalum and titanium.
  • These high-melting superalloys are produced by mixing the alloy-constituting element materials so as to obtain a specified composition, followed by ingoting, and more actually, by compounding at least one of an iridium-base superalloy made of iridium as a base added with at least one metal selected from the metal group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum and a rhodium-base superalloy made of rhodium as a base added with at least one metal selected from the above-described metal group, with nickel, followed by ingoting.
  • an iridium-base superalloy made of iridium as a base added with at least one metal selected from the metal group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum
  • a rhodium-base superalloy made of rhodium as a base added with at least
  • these high-melting superalloys are produced by mixing at least one of an iridium-base superalloy made of iridium as a base added with at least one metal selected from the metal group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum and a rhodium-base superalloy made of rhodium as a base added with at least one metal selected from the above-described metal group, with a nickel-base alloy made of nickel as a base added with at least one metal selected from the above-described metal group, followed by ingoting.
  • an iridium-base superalloy made of iridium as a base added with at least one metal selected from the metal group consisting of titanium, zirconium, hafnium, vanadium, niobium, and tantalum and a rhodium-base superalloy made of rhodium as a base added with at least one metal selected from the above
  • the high-melting superalloy of the present invention comprises
  • Ni-Al nickel-aluminum alloys which are presently used as heat i resisting materials for high-temperature instruments are useful as the above-described nickel-base alloy.
  • the high-melting superalloys of this invention produced by these production methods each has both phase of the fcc phase and the LI 2 phase in the texture.
  • the composition ratio of the metal components on the superalloy is an important factor
  • a two-phase conformity texture wherein a deposit having an LI 2 structure, is conformity-deposited in the matrix phase having an fcc structure, is formed.
  • the two-phase conformity texture means a texture wherein a row of adjacent crystal lattices is continued without being broken.
  • the strength is more increased than the superalloy simply made of two phases of the fcc phase and the LI2 phase. This is considered to be caused by that the conformity interface between the matrix phase and the deposit disturbs the transfer of the dislocation.
  • Such a two-phase conformity texture is surely formed in the case where at least one of the iridium-base superalloy and the rhodium-base superalloy, and the nickel-base alloy are used as the raw materials in the above-described production method, and each alloy has a two-phase conformity texture having an fcc phase and an LI2 phase.
  • the fcc phase and the LI 2 phase each exists as one kind regarding the kind of constituting substances. Because the high-melting superalloy of the invention is the multi-component alloy as described above, it is possible that plural kinds of the fcc phases and LI 2 phases each having a different existing concentration exist together.
  • an amount of the LI 2 phase is from 20 to 80% by volume.
  • the amount of the LI 2 phase is less than the lower limit, the strength is lowered.
  • the LI 2 phase may exceeds the upper limit but the preparation of such a superalloy becomes considerably difficult.
  • the high-melting superalloy of the invention can independently show the characteristics of the iridium-base superalloy or the rhodium-base superalloy and nickel or the nickel alloy, in the above-described production method. That is, the high-melting superalloy'of the invention shows all the high melting point, the high-temperature high strength, and the excellent oxidation resistance of the iridium-base superalloy or the rhodium-base superalloy and also the right-weight and the excellent ductility of nickel or the nickel-base alloy. Also, by the existence of nickel or the nickel-base alloy, the high-melting superalloy of this invention becomes relatively inexpensive.
  • the high-melting superalloy containing 50 atomic % and below of the iridium-base superalloy or the rhodium-base superalloy of itself or in terms of them is light-weight and is considered to be effective as the rotary members of turbine blades, etc., and on the other hand, when the content of the iridium-base superalloy or the rhodium-base superalloy is larger than the above-described content, as 50 % and above, the application of the high-melting superalloy of the invention to the members used at a higher temperature is expected to be useful.
  • test piece having a height of 6 mm and a diameter of 3 mm was cut and subjected to an aging treatment in a vacuum furnace of 5 ⁇ 10 -7 Torr at 1,300°C for one week. Also, the phase formed in each test piece was determined by an X-ray diffraction analysis (XRD) and an energy dispersion type X-ray analyzer (EDAX).
  • XRD X-ray diffraction analysis
  • EDAX energy dispersion type X-ray analyzer
  • the superalloys A and B of Table 1 had the textures composed of only two phases of the fcc phase and the LI 2 phase.
  • a two-phase conformity texture that the precipitation having the LI 2 structure was conformity-precipitated in the matrix phase having the fcc structure was formed.
  • the fcc phase was made of Ir and the LI 2 phase was made of Ir 3 Nb.
  • Ni formed a solid solution with the phase.
  • Figs. 1a to 1d each is an optical microphotograph of each test piece.
  • a dendrite texture (Fig. 1a) was formed and in the superalloys B, C, and D, fine textures (Figs. 1b, 1c, and 1d) were formed. Also, it was confirmed that with the increase of the compounding amount of Ni, the texture became thicker and rougher.
  • the compression strength of superalloy A was about 2 times that of Ir-15Nb at room temperature and was almost same as that of Ir-15Nb at 1,200°C.
  • the compression strengths of superalloys B, C, and D were lower than the compression strength of Ir-15Nb at both room temperature and 1,200°C.
  • the compression strengths of each of the above superalloys are higher than that of an N -base superalloy used for high-temperature instruments.
  • the ductility is improved by the addition of Ni.
  • the ductility is about 13%, which is far higher than that of Ir-15Nb
  • the utility of the superalloys is higher than the Ir-15Nb alloy.
  • the Ir amount of the superalloys can be reduced, which lowers the cost of the alloys. thus, in the point, the high utility of the superalloys is also confirmed.
  • an iridium-20 niobium (Ir-20Nb) alloy and an iridium-20 tantalum (Ir-20Ta) alloy were selected and, as the nickel-base alloy, a nickel-16.8 aluminum (Ni-16-8Al) alloy was selected.
  • Example 1 About these 6 kinds of the quaternary alloys, the phase determination and the texture observation as in Example 1 were carried out.
  • the two-phase conformity textures composed of the fcc phase ((Ir, Ni)) and 2 kinds of LI 2 phases ((Ni, Ir) 3 (Al, Ir) and (Ir, Ni) 3 (Nb, Al), or (Ni, Ir), (Ni, Ta) and (Ir, Ni) 3 (Ta, Al)) were formed.
  • composition formulae for example, (Ni, Ir) 3 (Al, Nb) means Ni 3 Al containing Ir and Nb, wherein a part of Ni is replaced with Ir and a part of Al is replaced with Nb.
  • Other composition formulae also employ the same expression system as above.
  • Figs. 3a, 3b, and 3c are the secondary electron images showing the textures of Ir-Nb-Ni-Al superalloys belongings to group A, group B, and group C, respectively.
  • the fcc phase and the first LI 2 phase of Ni 3 Al containing Ir and Nb were observed.
  • larger LI 2 phases were deposited.
  • the B2 phase was observed in the superalloy B only as described above.
  • a small second LI 2 phase of Ir 3 Nb containing Ni and Al was found in the fcc matrix phase.
  • the alloys prepared were subjected to an aging treatment in vacuo at 1,300°C and 1,400°C for one week and the textures were observed again.
  • Each of the quaternary alloys shows the high compression resistance as compared with an Ni-base superalloy applied to high-temperature instruments.
  • the compression strengths of these quaternary alloys are lower than that of Ir-Nb.
  • the ductility of each alloy is, by mixing of the nickel-base alloy, 18% at the lowest and is improved as 89% is obtained at the highest. Thus, it is admitted that the utility of the alloys is higher than Ir-15Nb.
  • each superalloy was observed by a scanning electron microscope (SEM) and a transmission electron microscope (TEM).
  • SEM scanning electron microscope
  • TEM transmission electron microscope
  • the test piece observed by the scanning electron microscope was electron-polished with an ethyl alcohol solution of 5% HCl.
  • the crystal structures and the phase compositions of the superalloys after the heat treatment Were determined by an X-ray diffraction analysis (XRD) and n energy dispersion type X-ray analyzer (EDAX).
  • Fig. 6 is the microphotographs of the superalloys heat-treated for 100 hours at 1,200°C.
  • Fig. 7 is a correlation diagram showing the compression strength and the ductility of the Rh 85-x Nb 15 Ni x superalloys in the relation of the content of nickel.
  • the data of the Rh-15 atomic % Nb alloy are shown together for comparisons
  • each of the superalloys with Ni added showy a high compression strength as compared with the Rh-Nb two-phase alloy.
  • the compression strength of each of the superalloy$ is higher than that of Ni-base superalloys which have hitherto been applied to high-temperature instruments.
  • Example 2 By following the same procedure as Example 2 except that rhodium was used as the component of constituting the superalloys in place of iridium, superalloys were prepared. The compression strength and the ductility of each superalloy were measured together with the determination of each phase and the observation of each texture. Each of the superalloys obtained shows a high compression strength and an improved ductility almost the same as those of Example 2 using iridium, as compared with the Ni-base superalloys which have hitherto been used for high-temperature instruments.
  • Fig. 9 and Fig. 10 are the photographs observing the rupture cross-sections of the alloys and the photographs showing the alloy textures of them, and the alloys are as follows: a: Rh 75 Nb 15 Ni 10 b: Rh 50 Ir 25 Nb 15 Ni 10 c: Rh 25 Ir 50 Nb 15 Ni 10 d: Ir 75 Nb 15 Ni 10
  • the invention is not limited to the above-described examples. That is, about the compositions, the compounding ratios, the preparation methods, etc., of the superalloys, various modifications are possible.
  • new high-melting superalloys which have the characteristics better than Ni-base superalloys in related art and can be realized at a relatively low cost are provided. Also, by the invention, the more improvements in the output and the heat efficiency of high-temperature instruments can be realized.

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EP00300755A 1999-02-02 2000-02-01 Superlegierung mit hoher Schmelztemperatur und Verfahren zu ihrer Herstellung Expired - Lifetime EP1026269B1 (de)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1983067A1 (de) * 2006-02-09 2008-10-22 Japan Science and Technology Agency Legierung auf iridiumbasis mit hoher hitzeresistenz und hoher festigkeit sowie herstellungsverfahren dafür
US20130216846A1 (en) * 2010-09-09 2013-08-22 Zebin Bao Alloy material for high temperature having excellent oxidation resistant properties and method for producing the same
EP3124630A4 (de) * 2014-03-28 2017-11-29 Tanaka Kikinzoku Kogyo K.K. Ni-ir-basierte hitzebeständige legierung und verfahren zur herstellung davon
CN113249608A (zh) * 2016-01-29 2021-08-13 德林爵-内股份有限公司 钯基合金
CN114107722A (zh) * 2021-11-08 2022-03-01 昆明理工大学 超强抗氧化耐腐蚀Pt基多组元合金及其制备方法

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US6982122B2 (en) * 2003-12-15 2006-01-03 Ut-Battelle, Llc Ir-based alloys for ultra-high temperature applications
US20060039820A1 (en) * 2004-08-20 2006-02-23 General Electric Company Stable, high-temperature nickel-base superalloy and single-crystal articles utilizing the superalloy
JP5226846B2 (ja) 2011-11-04 2013-07-03 田中貴金属工業株式会社 高耐熱性、高強度Ｒｈ基合金及びその製造方法
US9828658B2 (en) 2013-08-13 2017-11-28 Rolls-Royce Corporation Composite niobium-bearing superalloys
US9938610B2 (en) 2013-09-20 2018-04-10 Rolls-Royce Corporation High temperature niobium-bearing superalloys
US10029935B2 (en) * 2014-09-04 2018-07-24 Canon Kabushiki Kaisha Amorphous alloy molding die and method for forming optical element

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Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1983067A1 (de) * 2006-02-09 2008-10-22 Japan Science and Technology Agency Legierung auf iridiumbasis mit hoher hitzeresistenz und hoher festigkeit sowie herstellungsverfahren dafür
EP1983067A4 (de) * 2006-02-09 2012-11-07 Japan Science & Tech Agency Legierung auf iridiumbasis mit hoher hitzeresistenz und hoher festigkeit sowie herstellungsverfahren dafür
US20130216846A1 (en) * 2010-09-09 2013-08-22 Zebin Bao Alloy material for high temperature having excellent oxidation resistant properties and method for producing the same
EP3124630A4 (de) * 2014-03-28 2017-11-29 Tanaka Kikinzoku Kogyo K.K. Ni-ir-basierte hitzebeständige legierung und verfahren zur herstellung davon
US10094012B2 (en) 2014-03-28 2018-10-09 Tanaka Kikinzoku Kogyo K.K. Ni-Ir-based heat-resistant alloy and process for producing same
CN113249608A (zh) * 2016-01-29 2021-08-13 德林爵-内股份有限公司 钯基合金
CN114107722A (zh) * 2021-11-08 2022-03-01 昆明理工大学 超强抗氧化耐腐蚀Pt基多组元合金及其制备方法
CN114107722B (zh) * 2021-11-08 2023-02-28 昆明理工大学 超强抗氧化耐腐蚀Pt基多组元合金及其制备方法

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US20040211492A1 (en) 2004-10-28
EP1026269B1 (de) 2004-12-01
ZA200000456B (en) 2001-04-04
US20030136478A1 (en) 2003-07-24

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