EP0265541A1 - Alliage à base de cuivre, du type alpha, apte à la mise en forme à l'état de mélange liquide-solide - Google Patents

Alliage à base de cuivre, du type alpha, apte à la mise en forme à l'état de mélange liquide-solide Download PDF

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Publication number
EP0265541A1
EP0265541A1 EP86114985A EP86114985A EP0265541A1 EP 0265541 A1 EP0265541 A1 EP 0265541A1 EP 86114985 A EP86114985 A EP 86114985A EP 86114985 A EP86114985 A EP 86114985A EP 0265541 A1 EP0265541 A1 EP 0265541A1
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EP
European Patent Office
Prior art keywords
alloy
matrix
semi
copper base
alloys
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EP86114985A
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German (de)
English (en)
Inventor
Sankaranarayanan Ashok
John F. Breedis
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Olin Corp
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Olin Corp
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Publication date
Priority to US06/599,107 priority Critical patent/US4569702A/en
Priority to US06/786,564 priority patent/US4642146A/en
Application filed by Olin Corp filed Critical Olin Corp
Priority to EP86114985A priority patent/EP0265541A1/fr
Publication of EP0265541A1 publication Critical patent/EP0265541A1/fr
Withdrawn legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C9/00—Alloys based on copper
    • C22C9/06—Alloys based on copper with nickel or cobalt as the next major constituent
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C9/00—Alloys based on copper
    • C22C9/01—Alloys based on copper with aluminium as the next major constituent

Definitions

  • the present invention relates to a copper base alloy which is adapted to be formed as a semi-solid metal slurry.
  • the forming operation preferably comprises press forging.
  • the alloy is precipitation hardenable in the forged state to provide desired levels of strength.
  • the alloys of this invention find particular application in articles such as cartridge cases although they may be useful in a wide variety of articles.
  • the member In the manufacture of thin walled elongated high strength members such as cartridge cases, it is highly desirable to form the member from a material having physical properties capable of achieving certain desired objectives, i.e. sufficient fracture toughness to withstand the shock associated with firing, good formability so that the member can expand during firing and contract afterwards, high strength properties to form a reusable cartridge, etc.
  • a metal or alloy composition which is suitable for forming while in the state of a semi-solid slurry having thixotropic properties generally has a microstructure comprising solid discrete particles in a surrounding matrix having a lower melting point than the particles.
  • the surrounding matrix is solid when the metal composition is fully solidified and is liquid when the metal composition comprises a semi-solid slurry made up of the solid discrete particles in the molten surrounding matrix.
  • the microstructure of the copper base alloy may be formed by any of a number of techniques.
  • One technique which is particularly preferred in accordance with the present invention involves casting the alloy while it is agitated or stirred, preferably by electromagnetic means.
  • This technique which has sometimes been referred to as "rheocasting" or "thixocasting” is exemplified in U.S. Patent Nos. 3,902,544, 3,948,650 and 3,954,455 all to Flemings et al., 3,936,298 and 3,951,651 both to Mehrabian et al., 4,106,956 to Bercovici and 4,434,837 to Winter et al.
  • the solid discrete particles comprise degenerate dendrites or nodules which are generally spheroidal in shape.
  • Roach et al. also fail to disclose the adaptability of their alloys to forming in a semi-solid state and the provision of their alloys with a microstructure suited to such a forming technique.
  • Rozenberg et al. claim an alloy including 10 to 12% nickel, 2.2 to 2.6% aluminum, .8 to 1.1% silicon and .5 to .8% chromium and the balance copper.
  • Rozenberg et al.'s alloy is not disclosed to be suited to semi-solid metal forming or to be adapted to have a microstructure as in accordance with this invention.
  • a precipitation hardenable copper base alloy which is particularly suited to forming the desired microstructure and adapting it to semi-solid metal slurry forming processes.
  • the alloy is adapted to have from about 5% to about 40% liquid phase during slurry forming.
  • the alloy consists essentially of from about 3% to about 6% by weight nickel, from about 2% to about 4.25% by weight aluminum, from about 0.25% to about 1.2% by weight silicon, from about 5% to about 15% zinc, up to about 5% iron and the balance essentially copper.
  • the alloy has a microstructure comprising discrete particles contained in a matrix having a lower melting point than the particles.
  • the discrete particles may comprise primary degenerate dendrites.
  • the particles and the matrix are comprised such that when the alloy is heated to a desired temperature the alloy forms a semi-solid slurry wherein the matrix is in a molten condition comprising from about 5% to about 40% liquid and the particles are within the liquid matrix.
  • the alloy contains from about 3% to about 6% nickel, from about 2% to about 4% aluminum, from about 0.25% to about 1% silicon, from about 8% to about 10% zinc, from about 3% to about 5% iron and the balance essentially copper.
  • the alloys in accordance with this invention provide improved properties for semi-solid metal slurry forming techniques including having a lower melting point and a good temperature differential between its liquidus and solidus.
  • the alloys also provide improved aging kinetics, electrical conductivity and reduced quench sensitivity.
  • the alloys have a microstructure in accordance with this invention comprising primary solid particles contained in a matrix having a lower melting point, they have surprising formability as compared to wrought alloys of similar composition.
  • Alloys within the broad limits of the present invention are capable of forming the desired microstructure comprising discrete particles contained in a matrix having a lower melting point than the particles by MHD casting or any other suitable stirring technique. However, when the alloys are maintained within the preferred limits they are capable of forming the desired microstructure without stirring.
  • copper base alloys are provided which are adapted to be formed as a semi-solid slurry by techniques such as press forging.
  • techniques for forming semi-solid metal slurries by casting, forging, etc. Such slurries are often referred to as “thixotropic” since within certain ranges of volume fraction of liquid they behave in a thixotropic manner. Accordingly, sometimes forging of such slurries is referred to as “thixoforging” and casting of such slurries is preferred to as “thixocasting”.
  • the desired alloy microstructure in accordance with this invention can be formed by MHD slurry casting. Such a technique is sometines referred to as "rheocasting".
  • the copper base alloy of the present invention is adapted to form a semi-solid slurry when heated to a temperature between its liquidus and solidus temperatures.
  • the alloy preferably has a microstructure comprising discrete particles within a lower melting point matrix.
  • the particles and the matrix are comprised such that when the alloy is heated to a desired temperature the alloy forms a semi-solid slurry wherein the matrix is in a molten condition comprising from about 5% to about 40% liquid and the particles are within the liquid matrix.
  • the discrete paticles preferably comprise degenerate dendrites or nodules which are generally spheroidal in shape.
  • These particles comprise primary solid particles and are made up of a single phase or a plurality of phases having an average composition different from the average compostion of the generally surrounding matrix in the fully solidified alloy.
  • the discrete particles are contained in a generally surrounding matrix which is solid when the alloy is fully solidified and which is liquid when the alloy has been heated to form a semi-solid slurry.
  • the matrix itself comprises one or more phases having a lower melting point than the discret particles.
  • solidified alloys generally have branched dendrites which develop interconnected networks as the temperature is reduced and the weight fraction of solid increases.
  • semi-solid metal slurries consist of discrete primary particles separated from each other by a liquid metal matrix.
  • the primary solid particles may be degenerate dendrites in that they are characterized by smoother surfaces and a less branched structure than normal dendrites, approaching a spheroidal configuration.
  • the surrounding solid matrix is formed during solidification of the liquid matrix subsequent to the formation of the primary solids and contains one or more phases of the type which would be obtained during solidification of the liquid alloy in a more conventional process.
  • the surrounding matrix comprises dendrites, single or multi- phased compounds, solid solution, or mixtures of dendrites, and/or compounds, and/or solid solutions.
  • surrounding matrix refers to the matrix in which the discrete particles are contained and it need not fully surround each particle. Therefore, the term “surrounding” should be read as generally surrounding.
  • Semi-solid slurries can be formed into a wide variety of possible shapes by techniques such as forging, die casting, etc.
  • the semi-solid slurries in accordance with this invention by virtue of their structure comprising discrete particles in a molten matrix avoid problems relating to the separation of solids and liquids and thereby insure that uniform properties are obtained.
  • the use of semi-solid slurries in press forging or die casting provides improved die life and reduced thermal shock effects during processing.
  • it is possible to produce thin wall parts such as cartridge cases by press forging the alloy.
  • alloys which are suited to forming in a semi-solid state must have particular combinations of properties not required for other processes such as die casting and conventional forging.
  • the alloys have a wide solidification range which comprises the temperature differential between the liquidus and solidus temperatures of the alloy.
  • the alloy should preferably have from about 10% to about 30% of nonequilibrium eutectic phase so that the volume fraction of solid can be controlled upon heating the alloy to a semi-solid condition for forging.
  • This range of volume fraction or percent of nonequilibrium eutectic phase corresponds to the range of volume percent liquid in the slurry upon heating to the semi-solid state.
  • High fluidity of the molten alloy matrix is desired in order to minimize porosity in the finished part.
  • the alloy is precipitation hardenable in order to permit high strength to be attained without the necessity of cold working the resultant forged part. It is also desirable that the alloy exhibit a low quench sensitivity from the temperature at which it is solutionized before age hardening. Lower melting points for the alloy are desired to prolong die life.
  • Improved electrical conductivity may be desired to facilitate the use of magnetohydrodynamic (MHD) stirring to form the desired cast structure.
  • MHD magnetohydrodynamic
  • thermal conductivity is advantageous for facilitating reheating to a uniform temperature before forging.
  • the alloys of the present invention provide significant improvements in a number of properties important to semi-solid slurry forming techniques while maintaining comparable strength and formability of prior copper-nickel-aluminum alloys.
  • a copper base alloy capable of having a microstructure comprising discrete particles contained within a matrix having a lower melting point than the particles.
  • the particles and the matrix are comprised such that when the alloy is heated to a desired temperature the alloy forms a semi-solid slurry wherein the matrix is in a molten condition comprising from about 5% to about 40% liquid and the particles are within the liquid matrix.
  • the alloys have a composition consisting essentially of from about 3% to about 6% nickel, from about 2% to about 4.25% aluminum, from about 0.25% to about 1.2% silicon, from about 5% to about 15% zinc, up to about 5% iron and the balance essentially copper.
  • the composition consists essentially of from about 3% to about 6% nickel, from about 2% to about 4% aluminum, from about 0.25% to about 1% silicon, from about 8% to about 10% zinc, from about 3% to about 5% iron and the balance essentially copper.
  • the alloys as above having the above noted microstructure can be formed by MHD stirring techniques as described in Winter et al. patent and Pryor et al. U.S. patent and U.S. patent application although any desired technique as is known in the art could be employed for forming the alloy with the desired microstructure.
  • the alloy of the present invention having the desired microstructure can be formed in a semi-solid condition wherein the alloy has a volume fraction of about 5% to about 40% liquid and preferably from about 10% to about 30% liquid comprising a molten metal matrix. This minimizes significant changes in the volume fraction liquid at the forging temperature as a function of small variations in temperature. It also provides better dimensional tolerance and improved die life. After forging the alloy of this invention is preferably subjected to a heat treatment to increase its strength comprising solutionizing followed by aging.
  • the forged alloy can be separately solution treated.
  • Solutionizing in accordance with this invention preferably is carried out by heating the alloy to a temperature of at least about 800°C for a time period of 5 minutes to 4 hours.
  • the alloy is heated to a temperature in the range of 800°C to about 950°C for about 5 minutes to about 2 hours.
  • solutionizing the alloy is preferably quenched in water. If the solutionizing is carried out as part of the forging operation, then the alloy is preferably quenched immediately following forging.
  • the alloy After solutionizing the alloy is preferably subjected to an aging treatment wherein it is heated to a temperature in the range of from about 350°C to about 700°C for a time period of from about 1 minute to about 10 hours and, preferably, it is heated to a temperature of from about 400°C to about 600°C for about 5 minutes to about 3 hours.
  • the alloys of the present invention are capable of achieving a tensile strength of at least about 80 ksi.
  • the alloys are formed into parts such as cartridge cases comprising thin walled elongated members.
  • the member has a cup-shaped configuration typical of a cartridge case.
  • the alloy of the present invention can be utilized to form any desired component by the techniques which have been described.
  • the volume fraction liquid when the alloy is heated to the semi-solid condition preferably should be between about 10% to about 30%.
  • This liquid comprises in the alloy of this invention a eutectic.
  • the nickel content of the alloy does not substantially affect the volume fraction of nonequilibrium eutectic or liquid phase present. However, it has a major effect on the aging characteristics of the alloy particularly the strength which can be achieved. Accordingly, the nickel range, in accordance with the present invention, has been limited to an amount between about 3% to about 6%.
  • the lower limit has been determined by the strength requirements for the alloy and the upper limit has been established by the mix value of the alloy since it is desired to minimize the expense of the resultant alloy.
  • iron is added to the alloy so that the alloy can be cast without stirring and yet be capable of forming the desired microstructure comprising discrete particles in a lower melting point matrix.
  • the ranges of the other elements in the alloy must be controlled within critical limits.
  • the iron range in accordance with the preferred embodiment has been limited to an amount between about 3% to about 5% iron.
  • less than 3% iron is included in the alloy, a columnar dendritic structure is promoted. It has been found that the addition of 2% iron produced all columnar dendritic structure in a Cu-10%Zn-4%AI-0.75%Si-5%Ni alloy.
  • iron When more than 5% iron is included in the alloy, a mixed structure results including undesirable dendrites. Maintaining the iron content within the range of 3% to about 5% should provide the desired structure.
  • the nickel content for the preferred alloy should be maintained in the range of from about 3% to about 6%. Nickel contents of 7% were found to form dendrites.
  • the nickel and iron contents are interrelated with respect to forming an alloy capable of achieving the desired mircostructure. It has been found, for example, that for a 5% nickel alloy, otherwise within the ranges of this invention, a minimum of 3% iron is required. It is believed that a ratio of iron to nickel of at least about .5 (.5:1) and, preferably, at least about .6 (.6:1) it is necessary to obtain a desired microstructure upon casting without stirring. This has been confirmed by comparison with an alloy having 7% nickel and 3% iron with all other elements within the ranges of this invention which produced an as-cast dendritic structure. However, when the iron content of the alloy was increased to 5% meeting the minimum ratio, the desired microstructure was achieved as cast.
  • the iron-nickel ratio also depends upon cooling rate in the semi-solid state.
  • the ratio set forth hereinbefore holds for cooling rates characteristic of chill castings of rods or plates less than 3/4" thick.
  • the minimum ratio should be increased to about 0.9 (.9:1) and, preferably, at least about 1 (1:1
  • the range for zinc in accordance with the preferred embodiment of the invention is from about 8% to about 10%.
  • An alloy as cast without agitation having 12% zinc and otherwise being within the ranges of this embodiment produced a mixed structure including undesirable dendrites.
  • a similar as-cast alloy at 15% zinc was columnar dendritic.
  • an alloy having 5% zinc resulted in a mostly columnar dendritic structure.
  • Aluminum in accordance with the preferred embodiment should be within the range of from about 2% to about 4%. Lower aluminum contents do not provide sufficient strength. Higher aluminum contents promote the formation of equiaxed dendrites.
  • Silicon in accordance with the preferred embodiment of this invention should be within the range of about 0.25% to about 1%. It has been found that silicon in the lower part of the range results in finer particulates in the microstructure. "Particulate” as the term is used herein comprises a discrete particle with its surrounding matrix. However, decreasing silicon results in longer aging times and slightly inferior hardness and strength.
  • the composition range for the alloys of this embodiment should most preferably consist essentially of from about 8% to about 10% zinc, from about 4% to about 6% nickel, from about 3% to about 4% aluminum, from about 0.5% to about 1% silicon, from about 3% to about 5% iron and the balance essentially copper. Decreasing the nickel, aluminum or silicon contents below the most preferred limits results in longer aging treatments and reduced hardness although the alloy would still be precipitation hardenable.
  • Forging in accordance with this invention is normally carried out in the semi-solid condition and coarsening of the particulates may occur during reheating to the semi-solid condition. This is undesirable from a forging point of view. It has surprisingly been found that no significant growth in the particulate size of the alloys of this invention results and that coring is significantly reduced by casting the alloys without stirring.
  • Table I shows the effect of zinc on the melting point and solidification range of the alloy. It is apparent from a consideration of Table I that the addition of zinc significantly decreases the solidus temperature. This decrease in solidus temperature does not occur at the expense of decreasing the solidification temperature range ⁇ T. Further the alloys of this invention show very wide solidification temperature ranges as compared to the other alloys shown in Table I.
  • one pound chill castings 1/2" thick were prepared of a series of alloys having the following composition: Cu-10%Zn-5%Ni-4%AI-0.75%Si-3 to 5%Fe.
  • the alloys as cast without stirring had a fine particulate microstructure in accordance with this invention.
  • Tensile tests were performed on these castings in the as-cast condition and after heat treatment at 550°C for 1 hour. The results are set forth in Table II.
  • the alloys of the preferred embodiment of this invention can achieve excellent mechanical properties in the aged condition which would make them suitable for applications such as cartridge cases. Further, the alloys come close to achieving the necessary properties in the as-cast condition itself.
  • an alloy in accordance with this invention having Cu-10%Zn-5%Ni-4%AI-3%Fe0.75%Si was treated as set forth in the table.
  • the alloy was aged for 1 hour and 2 hours, respectively, in the as-cast without stirring condition.
  • Other samples of the alloy were reheated to the semi-solid condition and then water quenched.
  • Still other samples were reheated to the semi-solid condition and air cooled.
  • the alloys described in the hereinbefore examples were all cast from 1200°C.
  • the alloys in accordance with the preferred embodiment exhibited the desired microstructure in the as-cast without stirring condition. It has surprisingly been found the casting temperature influences the as-cast without stirring structure with respect to alloys of the preferred embodiment.
  • alloys having Cu-10%Zn-5%Ni-4%AI-3%Fe-0.75%Si were cast from temperatures varying from 1100 to 1300°C in increment of 50°C.
  • the desired microstructure was achieved in the as-cast castings made at 1100°C, 1150°C and 1200°C.
  • the castings at 1250°C and 1300°C resulted in microstructures including undesired equiaxed dendrites. Accordingly, it is preferred in accordance with this invention to cast the alloys of the preferred embodiment at temperatures up to about 1200°C.
  • the alloys of this invention comprise predominately alpha phase alloys.
  • Alpha phase alloys have the advantage of high ductility in the as-cast and forged conditions with comparatively low strength so that additional forming operations can be performed without difficulty.
  • the alloys can be heat treated after forming to high strengths and still retain very good ductilities.
  • the alloys in accordance with this invention may include other elements which do not significantly affect their properties or their ability to form the aesired microstructure. Further, the alloys may have other elements in impurity amounts which do not materially affect their characteristics.

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EP86114985A 1984-04-11 1986-10-28 Alliage à base de cuivre, du type alpha, apte à la mise en forme à l'état de mélange liquide-solide Withdrawn EP0265541A1 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
US06/599,107 US4569702A (en) 1984-04-11 1984-04-11 Copper base alloy adapted to be formed as a semi-solid metal slurry
US06/786,564 US4642146A (en) 1984-04-11 1985-10-11 Alpha copper base alloy adapted to be formed as a semi-solid metal slurry
EP86114985A EP0265541A1 (fr) 1986-10-28 1986-10-28 Alliage à base de cuivre, du type alpha, apte à la mise en forme à l'état de mélange liquide-solide

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EP86114985A EP0265541A1 (fr) 1986-10-28 1986-10-28 Alliage à base de cuivre, du type alpha, apte à la mise en forme à l'état de mélange liquide-solide

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102013208151A1 (de) * 2013-05-03 2014-11-20 Breuckmann GmbH & Co. KG Verfahren zur Herstellung von Erzeugnissen aus Metall

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2112676A (en) * 1982-01-06 1983-07-27 Olin Corp Method and apparatus for forming a thixoforged copper base alloy cartridge casing
EP0163860A1 (fr) * 1984-04-11 1985-12-11 Olin Corporation Alliage à base de cuivre, du type bêta, apte à la mise en forme à l'état d'un mélange liquide-solide et procédé pour sa fabrication
US4569702A (en) * 1984-04-11 1986-02-11 Olin Corporation Copper base alloy adapted to be formed as a semi-solid metal slurry

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2112676A (en) * 1982-01-06 1983-07-27 Olin Corp Method and apparatus for forming a thixoforged copper base alloy cartridge casing
EP0163860A1 (fr) * 1984-04-11 1985-12-11 Olin Corporation Alliage à base de cuivre, du type bêta, apte à la mise en forme à l'état d'un mélange liquide-solide et procédé pour sa fabrication
US4569702A (en) * 1984-04-11 1986-02-11 Olin Corporation Copper base alloy adapted to be formed as a semi-solid metal slurry
US4642146A (en) * 1984-04-11 1987-02-10 Olin Corporation Alpha copper base alloy adapted to be formed as a semi-solid metal slurry

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102013208151A1 (de) * 2013-05-03 2014-11-20 Breuckmann GmbH & Co. KG Verfahren zur Herstellung von Erzeugnissen aus Metall
DE102013208151B4 (de) * 2013-05-03 2020-11-19 Breuckmann GmbH & Co. KG Verfahren zur Herstellung von Erzeugnissen aus Metall

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