EP1205567B1 - Production de structure de grains ultrafins dans les alliages d'aluminium bruts de coulée - Google Patents

Production de structure de grains ultrafins dans les alliages d'aluminium bruts de coulée Download PDF

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Publication number
EP1205567B1
EP1205567B1 EP20010126694 EP01126694A EP1205567B1 EP 1205567 B1 EP1205567 B1 EP 1205567B1 EP 20010126694 EP20010126694 EP 20010126694 EP 01126694 A EP01126694 A EP 01126694A EP 1205567 B1 EP1205567 B1 EP 1205567B1
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EP
European Patent Office
Prior art keywords
melt
alloy
grain
grain refiner
molten
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Revoked
Application number
EP20010126694
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German (de)
English (en)
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EP1205567A2 (fr
EP1205567A3 (fr
Inventor
Men Glenn Chu
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Howmet Aerospace Inc
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Alcoa Inc
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Publication of EP1205567A3 publication Critical patent/EP1205567A3/fr
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    • 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
    • C22C1/03—Making non-ferrous alloys by melting using master alloys
    • 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
    • C22C1/026—Alloys based on aluminium
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C21/00—Alloys based on aluminium

Definitions

  • This invention relates to production of as-cast aluminum alloys with ultra-fine grain structure. More particularly, it relates to methods of adding a grain refiner to a molten aluminum alloy at levels which reduce the grain size to less than about 200 microns.
  • the size and shape of grains in as-cast aluminum alloy impacts properties of wrought or cast products. Casting with large grains, particularly dendritic grains, is highly prone to cracking during casting and reduce ductility, fracture toughness and fatigue properties. Reduction of the size as well as the form of the grains may be accomplished by mechanical or electromagnetic stirring to break up the grains. Grain size may also be controlled metallurgically by adding a grain refiner to the aluminum alloy melt.
  • a typical grain refiner used for aluminum alloys is cither an Al-Ti-B alloy or an Al-Ti-C alloy in the form of a rod or waffle.
  • a grnin refiner consists of numerous fine boride or carbide particles in an aluminum matrix.
  • grain refiners When these grain refiners are added to the aluminum alloy melt, the boride or carbide particles are dispersed into the melt and serve as nucleating sites for grains during solidification.
  • Commercially available grain refiners include alloys containing about 3-5 wt, % Ti and about 0.15-1 wt. % B or C and the balance Al. According to this practice, a residual amount of Ti is present in or is added to the aluminum melt (e.g. less than 0.015wt. %), and a controlled amount of the grain refiner is added thereto which increases the total Ti concentration in the final melt by about 0.001-0.003 wt. %. In this manner, the amount of B or C added to the melt via the grain refiner is about 0.0001-0.001 wt. %.
  • the addition of grain refiners at these conventional levels can control the size of dendritic grains to be about 250-1000 microns. For certain cast or wrought aluminum products, such a grain structure is sufficiently fine and cracking or other mechanical problems
  • ultra-fine grain size may be achieved by supersaturating a molten alloy with dispersoid-forming elements such as Zr, Mn, Cr, V, Ti, Sc and Hf as disclosed in U.S. Patent No. 6,004,506. That process requires the addition of a specialized, pre-alloyed ribbon of material containing the dispersoid-forming elements into a pool of molten metal formed during ingot casting. Accordingly, a need remains for a method of producing aluminum alloys with ultra-fine grain structure using readily available additives.
  • a method of producing fine grain aluminum having the steps of providing a molten aluminum alloy selected from 1XXX, 2XXX, 3XXX, 5XXX, 6XXX, 7XXX and 8XXX alloys, adding, 0.015-0.030 wt.% Ti to the molten alloy and adding a grain refiner to the molten alloy containing the said titanium to form a melt, wherein the grain refiner includes Ti and B or C, and solidifying the melt, wherein the grain refiner is added in an amount such that the concentration in the melt of B or C from the grain refiner is 0.003-0.010 wt.% and the grains in the solidified melt are 100 microns or less in size.
  • the element is Sc at a concentration of about 0.030-0.10 wt. % in the molten aluminum alloy.
  • the alloy is preferably an alloy of the 2XXX or 7XXX AA series.
  • Particularly preferred wrought alloys are 7055 and 7050 alloys.
  • the present invention includes a method of controlling the grain size in oast aluminum alloys to about 200 microns or less.
  • an alloying element is added to a molten aluminum alloy.
  • Preferred added alloying elements are Ti, Sc, Hf, Nb and Y, more preferably Ti and Sc when Ti is added, the concentration of the alloying element Ti in the molten aluminum alloy is about 0.015-0.030 wt. %.
  • the alloying element is Sc
  • a preferred concentration of residual Sc in the molten aluminum alloy is about 0.030-0.1 wt, %.
  • the alloying element is Hf, Nb or Y, the preferred concentration thereof is on the order of the preferred concentrations of Ti and Sc.
  • a grain refiner is added to the molten aluminum alloy containing the residual alloying element to form a melt.
  • Commercially available grain refiners are alloys consisting of Ti and B or C with the balance aluminum. Typical concentrations in the grain refiner are about 3-5 wt. % Ti and about 0.15-1 wt. % B or C. The final concentration of B or C in the melt from the grain refiner is about 0.003-0.010 wt. %.
  • Suitable commercially available grain refiners have compositions such as 3 wt. % Ti, 1 wt. % B and balance Al (referred to as Al-3%Ti-1%B), Al-5%Ti-1%B, Al-3%Ti-0.2%B, Al-5%Ti-0.2%B, Al-3%Ti-0.15%C, or Al-3%Ti-0.3%C.
  • These grain refiners typically are provided in the form of a rod or waffle.
  • the ratio of B or C to Ti in the grain refiner is normally fixed; hence, the amount of grain refiner added to the melt controls the final amount of Ti present in the melt. For example, in order to achieve a concentration of B of about 0.003-0.010 wt.
  • the present invention may be used to control grain size in wrought and cast alloys.
  • Suitable alloys include Aluminum Association (AA) wrought alloys of the 1XXX, 2XXX, 3XXX, 5XXX, 6XXX, 7XXX and 8XXX series.
  • AA Aluminum Association
  • Alloys of the AA 2XXX and 7XXX series are particularly suited to treatment according to the present invention.
  • As-cast aluminum alloy produced according to the present invention has globular grains which are about 200 microns or less in size, typically about 80 microns in size.
  • conventional grain refining practice of adding a grain refiner of Al-3%Ti-1%B such that the concentration of B in the melt is 0.001 wt. % produces dendritic grains sized about 1000 microns. These large dendritic grains interlock with each other and render the cast alloy rigid and prone to cracking, whereas the small, globular grains formed by the method of the present invention reduce crack initiation during casting and improve formability during deformation.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Continuous Casting (AREA)
  • Manufacture And Refinement Of Metals (AREA)

Claims (6)

  1. Une méthode pour produire de l'aluminium à grain fin qui comprend les pas de
    (a) fournir un alliage aluminium fondu qui appartient à la série 1XXX, 2XXX, 3XXX, 5XXX, 6XXX, 7XXX ou 8XXX, et ajouter audit alliage fondu un élément d'alliage sélectionné du groupe constitué de Sc, Hf, Nb et Y;
    (b) ajouter un affinant à l'alliage d'aluminium fondu contenant ledit élément d'alliage pour former un bain de fusion, l'affinant comprenant (i) du Ti et (ii) du B ou du C dans une telle quantité que la concentration en B ou en C de l'affinant dans le bain de fusion est 0.003-0.010 % en poids; et
    (c) solidifier le bain de fusion pour former un lingot dont la taille de grains est au plus 200 microns.
  2. La méthode selon la revendication 1, caractérisé en ce que l'élément d'alliage est le Sc et la concentration en Sc dans l'alliage aluminium fondu est 0.030-0.10 % en poids.
  3. La méthode selon l'une quelconque des revendications précédentes, dans laquelle l'alliage appartient à la série 2XXX ou 7XXX.
  4. La méthode selon la revendication 3, caractérisé en ce que l'alliage appartient à la série 7055 ou 7050.
  5. La méthode selon l'une quelconque des revendications 1-4, caractérisée en ce que la taille de grains du lingot est au plus 100 microns.
  6. Une méthode pour produire de l'aluminium à grain fin qui comprend les pas de fournir un alliage d'aluminium fondu sélectionné des séries 1XXX, 2XXX, 3XXX, 5XXX, 6XXX, 7XXX et 8XXX, l'addition de 0.015-0.030 % en poids Ti à l'alliage fondu et l'addition d'un affinant à l'alliage fondu qui contient ledit titane pour former un bain de fusion, l'affinant comprenant Ti et B ou C ; et solidifier le bain de fusion, l'affinant étant ajouté dans une quantité telle que la concentration en B ou C due à l'affinant dans le bain de fusion est 0.003-0.010 % en poids et la taille de grains dans le bain solidifié est au plus 100 microns.
EP20010126694 2000-11-10 2001-11-08 Production de structure de grains ultrafins dans les alliages d'aluminium bruts de coulée Revoked EP1205567B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US710175 1985-03-11
US71017500A 2000-11-10 2000-11-10

Publications (3)

Publication Number Publication Date
EP1205567A2 EP1205567A2 (fr) 2002-05-15
EP1205567A3 EP1205567A3 (fr) 2002-06-05
EP1205567B1 true EP1205567B1 (fr) 2005-05-04

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ID=24852923

Family Applications (1)

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EP20010126694 Revoked EP1205567B1 (fr) 2000-11-10 2001-11-08 Production de structure de grains ultrafins dans les alliages d'aluminium bruts de coulée

Country Status (3)

Country Link
EP (1) EP1205567B1 (fr)
CA (1) CA2361484A1 (fr)
DE (1) DE60110523D1 (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8083871B2 (en) 2005-10-28 2011-12-27 Automotive Casting Technology, Inc. High crashworthiness Al-Si-Mg alloy and methods for producing automotive casting
CN103060584A (zh) * 2012-12-21 2013-04-24 佛山市深达美特种铝合金有限公司 一种超细晶6061铝合金及其制备方法
CN103614581A (zh) * 2013-12-20 2014-03-05 西南铝业（集团）有限责任公司 一种1系铝合金铸锭的生产工艺

Families Citing this family (25)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6783730B2 (en) * 2001-12-21 2004-08-31 Alcoa Inc. Al-Ni-Mn casting alloy for automotive and aerospace structural components
FR2875815B1 (fr) * 2004-09-24 2006-12-01 Pechiney Rhenalu Sa Produits en alliage d'aluminium a haute tenacite et procede d'elaboration
US8157932B2 (en) 2005-05-25 2012-04-17 Alcoa Inc. Al-Zn-Mg-Cu-Sc high strength alloy for aerospace and automotive castings
CN100402681C (zh) * 2006-09-05 2008-07-16 中国铝业股份有限公司 一种Al-Ti-C中间合金的制备方法
US8349462B2 (en) 2009-01-16 2013-01-08 Alcoa Inc. Aluminum alloys, aluminum alloy products and methods for making the same
CN101838783B (zh) * 2010-02-05 2012-01-04 新星化工冶金材料(深圳)有限公司 通过控制压缩比来控制铝钛碳合金晶粒细化能力的变化量的方法
CN101871052B (zh) * 2010-06-28 2012-06-13 江阴新仁科技有限公司 一种净化铝及铝合金熔体的方法
CN101994045B (zh) * 2010-12-10 2012-07-11 西南铝业（集团）有限责任公司 一种铝锆中间合金的制备方法
GB201102849D0 (en) 2011-02-18 2011-04-06 Univ Brunel Method of refining metal alloys
CN102212725B (zh) * 2011-06-10 2012-10-10 深圳市新星轻合金材料股份有限公司 铝-锆-钛-碳中间合金在镁及镁合金变形加工中的应用
CN102225464B (zh) * 2011-06-10 2013-07-10 深圳市新星轻合金材料股份有限公司 镁及镁合金用铝-锆-钛-碳晶粒细化剂及其制备方法
CN102206777B (zh) * 2011-06-10 2013-07-10 深圳市新星轻合金材料股份有限公司 铝-锆-钛-碳中间合金的制备方法
CN102220525B (zh) * 2011-07-29 2012-10-17 哈尔滨中飞新技术股份有限公司 一种铝合金熔炼净化装置及熔炼净化方法
CN102268620A (zh) * 2011-08-01 2011-12-07 南昌大学 一种Al3Ti颗粒增强Al-Zn-Mg-Cu基铝合金的固溶处理方法
CN102212710B (zh) * 2011-08-02 2013-02-13 江苏中欧材料研究院有限公司 一种原位亚微米多元颗粒增强铝基复合新体系及材料
CN102329993A (zh) * 2011-09-07 2012-01-25 山东大学 一种高硼高碳铝基中间合金及其制备方法
CN102268621B (zh) * 2011-09-09 2013-03-20 西南铝业（集团）有限责任公司 一种铝合金棒材生产方法
CN102433454B (zh) * 2011-09-22 2013-01-16 郑州大学 一种热膨胀系数可控的金属基陶瓷材料Al-Zr2P2WO12的烧结合成方法
CN102409270A (zh) * 2011-11-07 2012-04-11 内蒙古北方重工业集团有限公司 一种大型铝合金环件轧制和电炉固溶处理方法
CN102703738A (zh) * 2012-05-17 2012-10-03 上海交通大学 Al－Ti－B－C四元晶粒细化剂的制备方法
EP3117018A4 (fr) * 2014-03-11 2017-12-13 Sapa Extrusions, Inc. Alliages d'aluminium à haute résistance
CN105624481A (zh) * 2016-03-28 2016-06-01 福建省科源新型材料有限公司 一种降低成本及能耗的铝制品制备工艺
CN108251675B (zh) * 2017-12-26 2020-04-03 上海大学 一种铸造铝硅合金用Al-Ti-Nb-B细化剂及其制备方法及应用
CN109385542B (zh) * 2018-09-17 2020-11-24 上海大学 用于晶粒细化的铝铌硼合金杆的制备方法
CN110983213B (zh) * 2019-11-12 2021-06-04 上交大(徐州)新材料研究院有限公司 一种超细结构高强韧薄带铝的制备方法

Family Cites Families (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS5810455B2 (ja) * 1979-11-20 1983-02-25 昭和軽金属株式会社 圧延用アルミニウム合金
US5100488A (en) * 1988-03-07 1992-03-31 Kb Alloys, Inc. Third element additions to aluminum-titanium master alloys
WO1996010099A1 (fr) * 1994-09-26 1996-04-04 Ashurst Technology Corporation (Ireland) Limited Alliages de fonderie d'aluminium a haute resistance pour applications structurelles
NO990813L (no) * 1999-02-19 2000-08-21 Hydelko Ks Forlegering for kornforfining av aluminiumslegeringer
US6368427B1 (en) * 1999-09-10 2002-04-09 Geoffrey K. Sigworth Method for grain refinement of high strength aluminum casting alloys

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8083871B2 (en) 2005-10-28 2011-12-27 Automotive Casting Technology, Inc. High crashworthiness Al-Si-Mg alloy and methods for producing automotive casting
US8721811B2 (en) 2005-10-28 2014-05-13 Automotive Casting Technology, Inc. Method of creating a cast automotive product having an improved critical fracture strain
US9353430B2 (en) 2005-10-28 2016-05-31 Shipston Aluminum Technologies (Michigan), Inc. Lightweight, crash-sensitive automotive component
CN103060584A (zh) * 2012-12-21 2013-04-24 佛山市深达美特种铝合金有限公司 一种超细晶6061铝合金及其制备方法
CN103060584B (zh) * 2012-12-21 2015-05-20 佛山市深达美特种铝合金有限公司 一种超细晶6061铝合金及其制备方法
CN103614581A (zh) * 2013-12-20 2014-03-05 西南铝业（集团）有限责任公司 一种1系铝合金铸锭的生产工艺

Also Published As

Publication number Publication date
EP1205567A2 (fr) 2002-05-15
EP1205567A3 (fr) 2002-06-05
DE60110523D1 (de) 2005-06-09
CA2361484A1 (fr) 2002-05-10

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