US20140010702A1 - Mg-al-ca-based master alloy for mg alloys, and a production method therefor - Google Patents

Mg-al-ca-based master alloy for mg alloys, and a production method therefor Download PDF

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US20140010702A1
US20140010702A1 US14/008,081 US201214008081A US2014010702A1 US 20140010702 A1 US20140010702 A1 US 20140010702A1 US 201214008081 A US201214008081 A US 201214008081A US 2014010702 A1 US2014010702 A1 US 2014010702A1
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master alloy
weight
melted
alloy
production method
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Shae K. KIM
Hyeon Gyu Lym
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Emk Co Ltd
Korea Institute of Industrial Technology KITECH
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Korea Institute of Industrial Technology KITECH
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Publication of US20140010702A1 publication Critical patent/US20140010702A1/en
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    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C23/00—Alloys based on magnesium
    • C22C23/02—Alloys based on magnesium with aluminium as the next major constituent
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22D—CASTING OF METALS; CASTING OF OTHER SUBSTANCES BY THE SAME PROCESSES OR DEVICES
    • B22D21/00—Casting non-ferrous metals or metallic compounds so far as their metallurgical properties are of importance for the casting procedure; Selection of compositions therefor
    • B22D21/002—Castings of light metals
    • B22D21/007—Castings of light metals with low melting point, e.g. Al 659 degrees C, Mg 650 degrees C
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C1/00—Making non-ferrous alloys
    • C22C1/02—Making non-ferrous alloys by melting
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C23/00—Alloys based on magnesium

Definitions

  • the present invention relates to an Mg—Al—Ca based master alloy for Mg alloys and a production method therefor.
  • Mg alloys have a density of approximately 1.8 g/cm 3 , which is a minimum of density levels of various alloys that are commercially available up to now, and demonstrate high specific strength and modulus of elasticity.
  • Mg alloys are excellent in view of absorbing capability of vibrations or impacts, electrical and thermal conductivity, processibility, fatigue strength at high temperature, impact property, and so on.
  • Mg alloys have various advantageous properties complying with requirements for weight reduction in various fields including transportation equipment such as automobiles, airplanes, or the like, equipment for defense industry, general machinery, and so on.
  • Mg alloys are lightness in weight.
  • Currently commercially available Mg alloys have a specific weight in a range of 1.79 to 1.81, which is approximately 35% or greater lighter than Al alloys, and demonstrate excellent mechanical properties. That is to say, whereas Mg alloys are similar to Al or steel in view of the modulus of elasticity and density, they demonstrate a noticeably reducing effect of weight, compared to Al alloys or plastic material.
  • the Mg alloy Since the Mg alloy is melted at a relatively low temperature in a range of 650 to 680° C., although there is a slight difference in the melting temperature according to the kind of allying element used, a small amount of energy is consumed in recycling the Mg alloy.
  • the Mg alloy can be recycled only with a quarter of the energy required for producing an Mg alloy ingot for the first time, thereby demonstrating a very high energy saving effect.
  • the Mg alloy recovered from the field production process may be melted to be recycled, followed by removing impurities and reducing components, and the recycled Mg alloy can be reused in substantially the same state as a new Mg alloy.
  • Mg alloys are at least twice longer than Al alloys in view of the life of molds, and are higher than Al alloys in view of manufacturability. Consequently, the production cost required by each unitary part can be reduced.
  • alloying elements to be used in uniform amounts it is often the case that an alloy containing large amounts of elements to be added is separately prepared as a flux, and small pieces of the flux are added to a molten metal used as a parent material of a desired alloy to then be diluted.
  • the alloy containing large amounts of elements to be added is referred to as a master alloy.
  • the master alloy is also called an intermediate alloy.
  • Al has the most advantageous effect when it is used as an alloying element of Mg.
  • the addition of Al increases the strength and hardness of Mg alloys, improves flowability during casting and increases a solidifying range, thereby improving castability.
  • Al When Al is added in an amount of 6 wt % or less, it may turn into solid-solution in an Mg base.
  • Al when Al is added in an amount of greater than 6 wt %, it may be precipitated and cured by heat treatment.
  • the content of Al is 10 wt % or less, in which Al alloys have excellent physical properties in view of strength and elongation.
  • an Mg 17 Al 12 phase may be formed, thereby lowering crepe resistance at high temperature.
  • Ca considerably improves high temperature strength and crepe resistance of Mg—Al based Mg alloys.
  • the addition of a trace amount ( ⁇ 0.5%) of Ca to an Al containing Mg alloy forms an Al 2 Ca intermetallic compound, which is stable at high temperature, during solidification, thereby increasing the strength and heat resistance.
  • Ca is an effective element in preventing alloys from being oxidized during casting or heat treatment.
  • Ca may serve to make crystalline particles into microstructures.
  • Ca may reduce flowability of a molten metal, thereby deteriorating castability, facilitates hot tearing, and increasing viscosity with respect to a mold during die casting, thereby ultimately lowering the manufacturability. If Ca is added in an amount of 0.3 wt % or greater, cracks may be generated during welding.
  • the present invention provides a novel Mg—Al—Ca based master alloy for Mg alloys, which is different from alloying elements added for alloying to Mg or an Mg alloy or a conventional master alloy, and a production method therefor.
  • the Mg alloy produced using the master alloy according to the present invention demonstrates excellent physical properties, compared to conventional Mg alloys.
  • a balance of Mg may be added in an amount of up to 85% of the entire weight of the master alloy, based on percentage by weight.
  • an Mg—Al—Ca based master alloy for Mg alloys wherein while a Ca:Al composition ratio is maintained at between 7:3 and 1:9, based on percentages by weight in the alloy, a balance of Mg is added in an amount of up to 85% of the entire weight of the master alloy, based on percentage by weight.
  • the Ca:Al composition ratio may be maintained at between 6:4 and 2:8, based on percentages by weight.
  • the content of Al may be contained in an amount of 15% or greater of the entire weight of the Mg—Al—Ca based master alloy, based on percentage by weight.
  • Mg may be contained in an amount of 65% of the entire weight of the master alloy, based on percentage by weight.
  • a production method of an Mg—Al—Ca based master alloy for Mg alloys including preparing components of a master alloy by selecting a composition in which, while a Ca:Al composition ratio is maintained at between 7:3 and 1:9, based on percentages by weight in the alloy, there is a balance of Mg in an amount of up to 85% of the entire weight of the master alloy, based on percentage by weight, sequentially melting Mg, Al and Ca, completely melting the components by applying an adequate amount of heat, and solidifying the molten metal.
  • the solidifying of the molten metal may include rapidly cooling the molten metal.
  • the Ca:Al composition ratio may be maintained at between 6:4 and 2:8, based on percentages by weight.
  • the content of Al may be contained in an amount of 15% or greater of the entire weight of the Mg—Al—Ca based master alloy, based on percentage by weight.
  • Mg may first be melted, Al may then be melted, and Ca may finally be melted.
  • Al may first be melted, Mg may then be melted, and Ca may finally be melted.
  • Mg and Al may be melted together and Ca may then be melted.
  • Mg and Ca may be melted together and Al may then be melted.
  • the master alloy according to the present invention is used in producing Mg alloys having excellent physical properties by controlling components of alloying elements added to produce commercially available Mg alloys within composition ranges to cause Al 2 Ca phase formation. That is to say, the Al 2 Ca phase formed from the master alloy is maintained in the final Mg alloy, thereby making the Mg alloy have a microstructure and increasing yield strength and the tensile strength of the Mg alloy. In addition, formation of a ⁇ -Mg 17 Al 12 phase that is thermally unstable is suppressed, and casting defects can be greatly reduced.
  • FIG. 1 is a calculated phase diagram of Al—Ca binary alloys
  • FIG. 2 is a calculated phase diagram of Mg—Al binary alloys
  • FIG. 3 is a calculated phase diagram of Mg—Ca binary alloys
  • FIG. 4 is a graph illustrating composition ranges (region 1) according to an embodiment of the present invention on a liquid projection view of an Mg—Al—Ca ternary phase diagram indicated by weight ratios;
  • FIG. 5 is a graph illustrating composition ranges (region 2) according to another embodiment of the present invention on a liquid projection view of an Mg—Al—Ca ternary phase diagram indicated by weight ratios.
  • the present invention provides an Mg—Al—Ca based master alloy, which is different from the conventional alloying element or conventional master alloy added to Mg or an Mg alloy for alloying, and a production method therefor, in an attempt to develop Mg alloys having better physical properties than conventional Mg alloy using the master alloy according to the present invention.
  • the inputting of the alloying element using the master alloy is achieved by inputting comprises inputting an Mg—Al—Ca master alloy prepared to cause Al 2 Ca phase formation to Mg or an Mg alloy.
  • the obtained Mg alloy has better physical properties than the conventional Mg alloy obtained by adding alloying elements of the same composition.
  • Ca or Al may further be added in addition to the master alloy.
  • FIG. 1 is a calculated phase diagram of Al—Ca binary alloy. It can be confirmed that intermetallic compounds are formed in various composition ranges. Examples of the intermetallic compound may include Al 4 Ca, Al 2 Ca, Al 14 Ca 13 and Al 3 Ca 8 . Specifically, Al 2 Ca has a considerably high melting point. It is understood that Al 2 Ca, observed in the present invention for the purpose of improving physical properties, is an intermetallic compound having a high melting point.
  • a method of calculating and obtaining a phase diagram is generally known in the related art. In particular, a commercially available program, such as a CALPHAD method, may also be used in calculating and obtaining the phase diagram.
  • FIG. 2 is a calculated phase diagram of Mg—Al binary alloys. As shown in FIG. 2 , there is high solid solubility of either Mg or Al with respect to each opponent element. While Mg and Al are mixed together and melted, melting points thereof are lowered.
  • FIG. 3 is a calculated phase diagram of Mg—Ca binary alloys.
  • Mg 2 Ca exists as an intermetallic compound between the Mg—Ca binary alloys.
  • the melting point of Mg 2 Ca is positioned between melting points between pure Mg and pure Ca. That is to say, the melting point of Mg 2 Ca is higher than the melting point of pure Mg and lower than the melting point of pure Ca.
  • FIGS. 4 and 5 are liquid projection views of Mg—Al—Ca ternary phase diagrams indicated by weight ratios. Composition ranges of the master alloy developed according to the present invention and exemplary embodiments thereof are illustrated in FIGS. 4 and 5 .
  • vertexes of a triangle indicates points at which fractions of components Mg, Ca and Al are 100%, respectively, and sides of the triangle indicate binary system of two components on each of the sides.
  • the temperatures can be calculated in terms of degrees in Celsius (C) by simply subtracting 273 from temperature values indicated in terms of degrees in Kelvin (K).
  • the Mg—Al—Ca based master alloy for Mg alloys produced in the present invention maintains a Ca:Al composition ratio at between 7:3 and 1:9, based on percentages by weight.
  • the line of the Ca:Al composition ratio being 7:3 is maintained along the line ⁇ circle around (1) ⁇
  • the line of the Ca:Al composition ratio being 1:9 is maintained along the line ⁇ circle around (2) ⁇ .
  • the Ca:Al composition ratio is maintained at between 7:3 and 1:9, based on percentages by weight is that the ranges of components of the master alloy are established below the line 1 and above the line ⁇ circle around (2) ⁇ .
  • Mg is further added in an amount of up to 85% of the entire weight of the master alloy, based on percentage by weight, which is established above line ⁇ circle around (3) ⁇ .
  • the compositions for the master alloy are determined in a region established by the lines ⁇ circle around (1) ⁇ , ⁇ circle around (2) ⁇ and ⁇ circle around (3) ⁇ , indicated by a region 1. That is to say, the master alloy is produced within the composition range of the region 1 established by the lines ⁇ circle around (1) ⁇ , ⁇ circle around (2) ⁇ and ⁇ circle around (3) ⁇ .
  • the Ca:Al composition ratio is maintained at between 6:4 and 2:8, which are composition ranges formed by lines ⁇ circle around (4) ⁇ , ⁇ circle around (5) ⁇ and ⁇ circle around (3) ⁇ , as shown in FIG. 5 . That is to say, in the case where the Ca:Al composition ratio is maintained at between 6:4 and 2:8, the compositions for the master alloy are determined in a region established by the lines ⁇ circle around (4) ⁇ , ⁇ circle around (5) ⁇ and ⁇ circle around (3) ⁇ .
  • 6:4 is more preferred than 7:3 for the reason below. That is to say, when the composition range is shifted toward Al 2 Ca from the region established by Mg 2 Ca, Al 14 Ca 13 and Al 2 Ca, Al 2 Ca formation is more securely guaranteed. That is to say, since the 7:3 composition ratios exists around boundary lines between Mg 2 Ca, Al 14 Ca 13 and Al 2 Ca, there are also possibilities of forming Mg 2 Ca and Al 14 Ca 13 , rather than Al 2 Ca. However, the 6:4 composition ratios can make Al2Ca formation more securely confirmed.
  • 2:8 is more preferred than 1:9 for the reason below. That is to say, when the composition range is shifted toward Al 2 Ca from the region established by Al 2 Ca and Al 4 Ca, Al 2 Ca formation is more securely guaranteed. That is to say, since the 1:9 composition ratios exists around a boundary line between Al 2 Ca and Al 4 Ca, there is also possibility of forming Al 4 Ca, rather than Al 2 Ca. However, the 2:8 composition ratios can make Al2Ca formation more securely confirmed.
  • a feature of the present invention lies in that the content of Al is contained in an amount of 15% or greater of the entire weight of the Mg—Al—Ca based master alloy, based on percentage by weight. If the content of Al is less than 15%, an amount of Al2Ca formed is reduced. In this case, the effect of Al 2 Ca as a master alloy may become insignificant.
  • a production method of an Mg—Al—Ca based master alloy for Mg alloys includes preparing components of a master alloy by selecting a composition in which, while a Ca:Al composition ratio is maintained at between 7:3 and 1:9, based on percentages by weight in the alloy, there is a balance of Mg in an amount of up to 85% of the entire weight of the master alloy, based on percentage by weight, sequentially melting Mg, Al and Ca, completely melting the components by applying an adequate amount of heat, and solidifying the molten metal.
  • the molten metal may be rapidly cooled.
  • the rapidly cooling refers to forced cooling, which is faster than natural solidifying in a general casting process.
  • the forced cooling includes water cooling (including brine quenching) or rapid cooling by blowing air quenching.
  • the composition selected for producing the Mg—Al—Ca based master alloy is determined in the range of the region 1 shown in FIG. 4 .
  • the reason of the foregoing is briefly described. That is to say, the alloy components are completely melted by raising the temperature over the liquid phase line of the corresponding composition of the region 1, and the molten metal is then rapidly cooled, thereby maximally producing Al 2 Ca as desired in the master alloy of the present invention.
  • the Ca:Al composition ratio may be maintained at between 6:4 and 2:8, based on percentage by weight.
  • the composition selected for producing the Mg—Al—Ca based master alloy is determined in the range of the region 2 shown in FIG. 5 , established by the lines ⁇ circle around (4) ⁇ , ⁇ circle around (5) ⁇ and ⁇ circle around (3) ⁇ .
  • 6:4 is more preferred than 7:3 because when the composition range is shifted toward Al 2 Ca from the region established by Mg 2 Ca, Al 14 Ca 13 and Al 2 Ca, Al 2 Ca formation is more securely guaranteed.
  • the Ca:Al composition ratio 2:8 is more preferred than 1:9 for the reason below. That is to say, when the composition range is shifted toward Al2Ca from the region established by Al 2 Ca and Al 4 Ca, Al 2 Ca formation is more securely guaranteed. That is to say, since the 1:9 composition ratios exists around a boundary line between Al 2 Ca and Al 4 Ca, there is also possibility of forming Al 4 Ca, rather than Al 2 Ca. However, the 2:8 composition ratios can make Al 2 Ca formation more securely confirmed. More preferably, while the Ca:Al composition ratio is maintained at 4.3:5.7, Mg is contained in an amount of 65% of the entire weight of the master alloy, based on percentage by weight.
  • Al and Ca maintain the Al 2 Ca composition ratio.
  • An ideal amount of Al 2 Ca can be formed by adding Mg while maintaining the composition ratio on the Al 2 Ca line.
  • Mg is more preferably added in an amount of up to 65% of the entire weight of the master alloy, based on percentage by weight.
  • Mg—Al—Ca based master alloy according to the present invention Various components for forming the Mg—Al—Ca based master alloy according to the present invention are prepared, and Mg, Al and Ca are sequentially melted one by one. For example, Mg is melted by applying an adequate amount of heat, Al is then melted, and Ca is finally melted.
  • the melting may also be performed from Mg to Al and to Ca, Al to Ca and to Mg, or Ca to Mg and to Al in that order.
  • the molten metal can only be formed by applying a much larger amount of heat due to a high melting point of the generated intermetallic compound, which is disadvantageous. Therefore, when the respective components are melted, it is not desirable to form Al 2 Ca from the beginning by melting Al and Ca together. Therefore, the melting in the order of Al—Ca—Mg or Ca—Al—Mg is the most undesirable method.
  • Mg and Al may be melted together, or Ca and Mg may be melted together, and the rest alloying element (Ca or Al) may then be melted.
  • the rest alloying element Ca or Al
  • FIGS. 1 , 2 and 3 with regard to cases of Al and Mg, and Ca and Mg, except for a case of Al and Ca, when two metals are melted at the same time, the melting point is lowered, compared to a case when a pure metal is melted.
  • three components Mg, Al and Ca may also be melted at the same time.
  • the three components Mg, Al and Ca are put into a crucible and an adequate amount of heat for melting is applied in a protection gas atmosphere, they are melted in the crucible, thereby forming a molten metal for forming the Mg—Al—Ca based master alloy.
  • melting may be performed in the protection gas atmosphere.
  • the melting temperature for forming the molten metal is as high as a temperature in which a solid phase metal is sufficiently melted to then exist a perfect liquid phase.
  • the temperature of the molten metal may be lowered with addition of sequentially input components, it is necessary to maintain the molten metal to be in a temperature range having a sufficient margin. In metallography, it is generally often the case that the melting point is lowered according to the progress of alloying.
  • Mg or Ca may be readily evaporated in view of its characteristic, resulting in a loss of the amount of the molten metal, thereby adversely affecting final physical properties due to ignited oxides.
  • the molten metal is preferably stirred.
  • the stifling may be performed by generating an electric field by providing an apparatus for applying an electromagnetic field around a furnace containing the molten metal, thereby inducing convection of the molten metal.
  • the molten metal may be mechanically stirred from the outside.
  • Table 2 shows yield strengths of final Mg alloys obtained by inputting the master alloy produced by the present invention to Mg or Mg alloys according to composition ratios.
  • Table 3 shows measuring results of yield strengths of Mg alloys of Comparative Examples having the same composition ratios with those of Examples of the present invention by directly adding Al and/or Ca to the final Mg alloys, instead of adding the master alloy produced by the present invention. Numbers for identifying the respective examples shown in Table 2 correspond to those for identifying the respective comparative examples shown in Table 3. When Mg alloys are produced using the master alloy with Al 2 Ca formed in the present invention, they exhibited higher yield strengths than general Mg alloys having the same composition ratios.
  • Mg alloy was microstructured with the addition of the master alloy produced by the present invention. Further, it was confirmed that Mg 2 Ca or (Mg, Al) 2 Ca phases in addition to Al 2 Ca were distributed in the Mg alloy base.
  • composition ratios listed in Tables 2 and 3 indicate compositions of the final Mg alloys produced using the master alloy according to the present invention.
  • Table 4 shows comparison results of Ca yields when Mg-5Al-2Ca is produced by adding 10Mg-50Al-40Ca as the inventive master alloy to Mg, by wt %, and directly adding Ca as an alloying element to Mg or an Mg alloy. Additionally, when necessary, Al is further added to adjust the final composition to Mg-5Al-2Ca.
  • the yield means a percentile obtained by dividing the amount of finally alloyed Ca in the Mg alloy by a total input amount of Ca.
  • the Mg alloy is microstructured with the addition of the master alloy produced by the present invention with the addition of the master alloy and Mg2Ca, Al2Ca or (Mg, Al) 2 Ca phases are uniformly distributed in the Mg alloy.
  • formation of a ⁇ -Mg17Al12 phase that is thermally unstable can be suppressed, and casting defects can be greatly reduced.
  • the yield strengths of the Mg alloys were increased and the tensile strengths of the Mg alloys were also increased.
  • the Mg—Al—Ca based master alloy produced according to the present invention may be added as an alloying means to one selected from the group consisting of pure Mg, Mg alloys and equivalents thereof.
  • usable examples of the Mg alloy may include AZ91D, AM20, AM30, AM50, AM60, AZ31, AS41, AS31, AS21X, AE42, AE44, AX51, AX52, AJ50X, AJ52X, AJ62X, MRI153, MRI230, AM-HP2, Mg—Al, Mg—Al—Re, Mg—Al—Sn, Mg—Zn—Sn, Mg—Si, and Mg—Zn—Y, but aspects of the present invention are not limited thereto. Any Mg alloy that is generally used in industries may be used.

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  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
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US14/008,081 2011-03-30 2012-03-30 Mg-al-ca-based master alloy for mg alloys, and a production method therefor Abandoned US20140010702A1 (en)

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KR10-2011-0028939 2011-03-30
KR1020110028939A KR101385685B1 (ko) 2011-03-30 2011-03-30 Ｍｇ합금용 Ｍｇ-Ａｌ-Ｃａ계 모합금 및 이의 제조하는 방법
PCT/KR2012/002426 WO2012134243A2 (fr) 2011-03-30 2012-03-30 Alliage maître à base de mg-al-ca pour des alliages de mg, et procédé de production de celui-ci

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EP (1) EP2692883B1 (fr)
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US20160348217A1 (en) * 2015-05-27 2016-12-01 Honda Motor Co., Ltd. Magnesium alloy and method of manufacturing same
CN115641929A (zh) * 2022-11-04 2023-01-24 中南大学 一种多元多相合金弹性模量的计算方法及成分设计方法

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CN107245593A (zh) * 2017-06-26 2017-10-13 重庆文理学院 镁中间合金晶粒细化剂及其制备方法和应用
KR101961468B1 (ko) * 2017-09-29 2019-04-15 (주)한국주조산업 알루미늄합금용 Al-Mg-Ca 모합금 및 그 제조방법
CN111155011A (zh) * 2020-02-21 2020-05-15 江苏理工学院 一种高性能Mg-Al-Ca镁合金及其制备方法

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CN115641929A (zh) * 2022-11-04 2023-01-24 中南大学 一种多元多相合金弹性模量的计算方法及成分设计方法

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KR101385685B1 (ko) 2014-04-16
CN103502494B (zh) 2017-05-31
EP2692883A2 (fr) 2014-02-05
WO2012134243A2 (fr) 2012-10-04
WO2012134243A3 (fr) 2013-01-03
EP2692883B1 (fr) 2017-10-04
EP2692883A4 (fr) 2014-11-19
KR20120110818A (ko) 2012-10-10

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