JP2007063659A - High strength magnesium alloy essentially consisting of magnesium and admixed with trace amount of copper or copper and yttrium - Google Patents
High strength magnesium alloy essentially consisting of magnesium and admixed with trace amount of copper or copper and yttrium Download PDFInfo
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- JP2007063659A JP2007063659A JP2005277896A JP2005277896A JP2007063659A JP 2007063659 A JP2007063659 A JP 2007063659A JP 2005277896 A JP2005277896 A JP 2005277896A JP 2005277896 A JP2005277896 A JP 2005277896A JP 2007063659 A JP2007063659 A JP 2007063659A
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- 239000010949 copper Substances 0.000 title claims abstract description 37
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 title claims abstract description 31
- 229910052802 copper Inorganic materials 0.000 title claims abstract description 31
- 239000011777 magnesium Substances 0.000 title claims abstract description 25
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 title claims abstract description 19
- 229910000861 Mg alloy Inorganic materials 0.000 title claims abstract description 18
- 229910052749 magnesium Inorganic materials 0.000 title claims abstract description 17
- 229910052727 yttrium Inorganic materials 0.000 title claims abstract description 17
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 title claims abstract description 17
- 229910045601 alloy Inorganic materials 0.000 claims abstract description 35
- 239000000956 alloy Substances 0.000 claims abstract description 35
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 7
- 238000001816 cooling Methods 0.000 claims description 6
- 239000000203 mixture Substances 0.000 claims description 4
- 239000000155 melt Substances 0.000 claims 2
- 238000005507 spraying Methods 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 12
- 239000013078 crystal Substances 0.000 abstract description 8
- 239000000463 material Substances 0.000 abstract description 6
- 238000002844 melting Methods 0.000 abstract description 6
- 230000008018 melting Effects 0.000 abstract description 6
- 238000010438 heat treatment Methods 0.000 abstract description 3
- 239000002244 precipitate Substances 0.000 abstract description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 abstract 2
- 229910052786 argon Inorganic materials 0.000 abstract 1
- 239000002131 composite material Substances 0.000 abstract 1
- 238000004519 manufacturing process Methods 0.000 description 12
- 239000000654 additive Substances 0.000 description 4
- 230000000996 additive effect Effects 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 4
- 239000001301 oxygen Substances 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- 229910052710 silicon Inorganic materials 0.000 description 4
- 239000010703 silicon Substances 0.000 description 4
- 229910002530 Cu-Y Inorganic materials 0.000 description 3
- 239000012535 impurity Substances 0.000 description 3
- 238000002347 injection Methods 0.000 description 3
- 239000007924 injection Substances 0.000 description 3
- 238000007578 melt-quenching technique Methods 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
- 239000002184 metal Substances 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 239000010453 quartz Substances 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
- 229910000881 Cu alloy Inorganic materials 0.000 description 2
- 229910019086 Mg-Cu Inorganic materials 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 238000010791 quenching Methods 0.000 description 2
- 230000000171 quenching effect Effects 0.000 description 2
- 238000007712 rapid solidification Methods 0.000 description 2
- 239000006104 solid solution Substances 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- 229910000946 Y alloy Inorganic materials 0.000 description 1
- OWXLRKWPEIAGAT-UHFFFAOYSA-N [Mg].[Cu] Chemical compound [Mg].[Cu] OWXLRKWPEIAGAT-UHFFFAOYSA-N 0.000 description 1
- 229910000808 amorphous metal alloy Inorganic materials 0.000 description 1
- 239000012300 argon atmosphere Substances 0.000 description 1
- 238000005266 casting Methods 0.000 description 1
- 238000009750 centrifugal casting Methods 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 230000015271 coagulation Effects 0.000 description 1
- 238000005345 coagulation Methods 0.000 description 1
- 238000009689 gas atomisation Methods 0.000 description 1
- 238000003754 machining Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
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Abstract
Description
本発明は、銅を単独またはイットリウムと共に微量添加したマグネシウムの溶融物を急冷凝固する方法を用い、銅単独の添加の場合には、結晶粒を微細化すると共に析出物を均一分散させ、銅とイットリウムの添加の場合には、結晶粒内に均一分散した微細なアモルファス相の周囲に長周期六方稠密構造を生成させ、マグネシウムの機械的強度を著しく向上させたマグネシウム合金及びその製造法に関するものである。 The present invention uses a method of rapidly solidifying magnesium melt obtained by adding a small amount of copper alone or together with yttrium. In the case of adding copper alone, the crystal grains are refined and precipitates are uniformly dispersed, In the case of addition of yttrium, it relates to a magnesium alloy in which a long-period hexagonal close-packed structure is formed around a fine amorphous phase uniformly dispersed in crystal grains, and the mechanical strength of magnesium is remarkably improved, and a manufacturing method thereof. is there.
銅はマグネシウムに対して固溶領域がほとんど存在しないことから、これまで添加元素として注目されてこなかった。このため銅を含むマグネシウム系合金として、これまで知られている物は、その多くが３元系以上の多元素系であった。増本等はＭｇ−（Ｃｕ＋Ｍ）（Ｍ＝Ｎｉ，Ｓｎ，Ｚｎ）合金について開示しているが、高強度を得るためには非晶質合金で無ければならないし、また経時と共にもろさが出るといった合金の安定性に欠けるものであった。更に、強度の高い合金を得るためには銅を含む添加元素の添加量は１０〜６０原子％とかなり多量添加する必要がある（特許文献１参照）。また増本等は、溶融急冷法を用いたＭｇ−Ｚｎ−Ｙ系合金等では、高強度のマグネシウム合金が得られることを開示しているが、５０％以上の非晶質相を有する非晶質合金を条件としている（特許文献２参照）。さらに井上等は、Ｍｇ９７Ｚｎ１Ｙ２（原子％）合金で５００ＭＰａ以上の降伏強度を報告しているが、その製造過程は、溶融急冷法を利用したガスアトマイズによって作製した粉末を、５７３Ｋで押し出し成形した後に、さらに機械加工によって成形したものを測定試料としており、複雑な製造過程を有しているため実用性に乏しいという問題点を有している（特許文献３参照）。マグネシウムへの銅とイットリウムの２種の添加について井上等は、Ｍｇ−Ｍ−Ｙの非晶質合金を報告しているが、比較的高価なイットリウム元素を１５〜３５原子％添加する必要がある上に、Ｍｇ−Ｍ−ＹのＭには銅，銀，パラジウムから２種類の元素を選択する必要があり、材料構成もより複雑である。このように、これまでの高強度マグネシウム合金では、比較的高価な添加元素を含んだものであり、多元素系の高強度マグネシウム合金の作製方法も複雑な製造過程を必要としている。従って高強度マグネシウム基合金では、より製造コストを抑えた合金の開発が求められている。また、一般的な溶融急冷法に用いられる石英製の溶融金属噴射ノズルは、マグネシウムと反応しやすく、作製されたマグネシウム合金への珪素及び酸素の混入によって、著しく合金の機械的特性を弱める。そのため、合金の溶解時に珪素や酸素等の不純物の混入を防ぐノズルの開発も求められている。 Since copper has almost no solid solution region with respect to magnesium, it has not been noted as an additive element so far. For this reason, as for the magnesium-type alloy containing copper, the thing known so far was many multielement system of the ternary system or more. Masumoto et al. Discloses an Mg- (Cu + M) (M = Ni, Sn, Zn) alloy. However, in order to obtain high strength, the alloy must be an amorphous alloy and becomes brittle over time. The lack of stability. Furthermore, in order to obtain an alloy with high strength, it is necessary to add a large amount of additive elements including copper, such as 10 to 60 atomic% (see Patent Document 1). Further, Masumoto et al. Discloses that a Mg-Zn-Y alloy using a melt quenching method can obtain a high-strength magnesium alloy, but an amorphous material having an amorphous phase of 50% or more. The condition is an alloy (see Patent Document 2). Furthermore, Inoue et al. Reported a yield strength of 500 MPa or more with an Mg 97 Zn 1 Y 2 (atomic%) alloy, but the manufacturing process was performed by extruding a powder produced by gas atomization using a melt quenching method at 573K. After molding, a sample that is molded by machining is used as a measurement sample, which has a problem of poor practicality because it has a complicated manufacturing process (see Patent Document 3). Inoue et al. Have reported Mg-MY amorphous alloys for the addition of two types of copper and yttrium to magnesium, but it is necessary to add 15 to 35 atomic percent of a relatively expensive yttrium element. Furthermore, it is necessary to select two types of elements from copper, silver, and palladium for M in Mg-MY, and the material configuration is more complicated. Thus, conventional high-strength magnesium alloys contain relatively expensive additive elements, and a method for producing a multi-element high-strength magnesium alloy also requires a complicated production process. Therefore, for high-strength magnesium-based alloys, there is a demand for the development of an alloy with a lower manufacturing cost. Further, a quartz molten metal injection nozzle used in a general melting and quenching method easily reacts with magnesium, and the mechanical properties of the alloy are significantly weakened by mixing silicon and oxygen into the produced magnesium alloy. Therefore, the development of a nozzle that prevents the entry of impurities such as silicon and oxygen during melting of the alloy is also required.
本発明ではマグネシウムに、より安価な金属を微量添加し、珪素及び酸素等の不純物が混入しない、より単純な製造方法を用いることによって、製造コストを抑えた高強度マグネシウム合金を提供することを課題としている。 It is an object of the present invention to provide a high-strength magnesium alloy with reduced manufacturing cost by adding a trace amount of a cheaper metal to magnesium and using a simpler manufacturing method in which impurities such as silicon and oxygen are not mixed. It is said.
マグネシウムに対して固溶領域をほとんど持たない銅を単独またはイットリウムと共に添加した合金を溶融状態から急冷凝固すること、さらに従来の石英製ノズルに代わるカーボン製ノズルを使用することにより、高強度のＭｇ−Ｃｕ合金およびＭｇ−Ｃｕ−Ｙ合金が得られることを見出し、本発明に至った。そのような方法にて得られるマグネシウム合金は上記問題点の解決策を与えるものである。 High-strength Mg can be obtained by rapidly solidifying an alloy in which copper, which has almost no solid solution region with respect to magnesium, alone or together with yttrium is melted, and by using a carbon nozzle instead of a conventional quartz nozzle. The inventors have found that a -Cu alloy and a Mg-Cu-Y alloy can be obtained, and have reached the present invention. The magnesium alloy obtained by such a method provides a solution to the above problems.
マグネシウムに銅を添加したＭｇ−Ｃｕ合金の場合は、加熱溶解した溶融合金を適当な方法にて急速に冷却すると、得られた合金は微細な結晶粒を有すると共に、微細な析出物が均一に分散した高強度マグネシウム合金となる。さらに、銅の濃度や急冷速度によって、結晶粒径を自由に選択できると同時に、合金の強度を任意に制御するが可能になる。マグネシウムに銅とイットリウムを共に添加したＭｇ−Ｃｕ−Ｙ合金の場合は、結晶粒内に均一に分散した微細な非晶質相を形成すると共に、その非晶質相の周囲には長周期六方稠密構造を持つ複相構造を示す。また、この溶融急冷時にカーボン製のノズルを使用することによって、合金への珪素及び酸素等の不純物の混入を防ぎ、より高強度なＭｇ基合金を作製することが可能となる。より安価な銅元素とイットリウム元素を微量に用い、単純な製造方法によって作製されるこのＭｇ−Ｃｕ合金及びＭｇ−Ｃｕ−Ｙ合金は、従来のマグネシウム合金よりも製造コストを抑えることが可能となる。 In the case of an Mg—Cu alloy in which copper is added to magnesium, when the molten alloy melted by heating is rapidly cooled by an appropriate method, the resulting alloy has fine crystal grains and uniform fine precipitates. It becomes a dispersed high strength magnesium alloy. Furthermore, the crystal grain size can be freely selected according to the copper concentration and the rapid cooling rate, and at the same time, the strength of the alloy can be arbitrarily controlled. In the case of Mg-Cu-Y alloy in which both copper and yttrium are added to magnesium, a fine amorphous phase uniformly dispersed in the crystal grains is formed, and a long-period hexagon is formed around the amorphous phase. It shows a multiphase structure with a dense structure. Further, by using a carbon nozzle at the time of melting and quenching, impurities such as silicon and oxygen can be prevented from being mixed into the alloy, and a higher strength Mg-based alloy can be produced. This Mg-Cu alloy and Mg-Cu-Y alloy produced by a simple manufacturing method using less expensive copper elements and yttrium elements can be manufactured at a lower cost than conventional magnesium alloys. .
本法のＭｇ１００−（ａ＋ｂ）ＣｕａＹｂの成分組成は、原子％で０．１≦ａ≦５％，０≦ｂ≦１０の範囲が好ましい。この合金は例えば、マグネシウムと銅およびイットリウム金属をノズル状容器内において、高周波溶解法を用い溶融した状態から、冷却速度約５０００〜１００００℃／ｓｅｃで急冷凝固することによって作製される。ノズルの材質としては石英、セラミックス、カーボンなど色々なものを使用できる。その中でもカーボン製のノズルを使用すると非常に特性的に良好な合金が得ることができる。薄帯リボンの場合は、縦に高速回転させた銅製ロールの回転表面に、溶融状態の合金を射出し、溶融合金をロール表面に接触急冷させることによって、リボン状の合金の作製が可能となる。また、インゴットの場合は、冶金型鋳造法や遠心鋳造法を用いることによって、インゴット状の合金の作製が可能になる。さらに粉末試料の場合は、粉末凝固法による作製方法も適用できる。この急冷凝固では、より高い冷却速度によって結晶粒の微細化が促進され、高強度のマグネシウム合金を得ることができる。マグネシウムへの銅の添加量は、銅５原子％までであれば、実用性を確保することが可能である。イットリウムは１０原子％までの添加が好ましい。 The component composition of Mg 100- (a + b) Cu a Y b in this method is preferably in the range of 0.1 ≦ a ≦ 5% and 0 ≦ b ≦ 10 in atomic percent. This alloy is produced, for example, by rapidly solidifying magnesium, copper, and yttrium metal in a nozzle-like container at a cooling rate of about 5000 to 10000 ° C./sec from a melted state using a high frequency melting method. Various materials such as quartz, ceramics, and carbon can be used as the nozzle material. Among them, when a carbon nozzle is used, an alloy with very good characteristics can be obtained. In the case of ribbon ribbons, a ribbon-like alloy can be produced by injecting a molten alloy onto the rotating surface of a copper roll that has been rotated at a high speed in the vertical direction and rapidly cooling the molten alloy in contact with the roll surface . In the case of an ingot, an ingot-like alloy can be produced by using a metallurgical mold casting method or a centrifugal casting method. Furthermore, in the case of a powder sample, a production method by a powder coagulation method can also be applied. In this rapid solidification, refinement of crystal grains is promoted by a higher cooling rate, and a high-strength magnesium alloy can be obtained. If the amount of copper added to magnesium is up to 5 atomic%, practicality can be ensured. Yttrium is preferably added up to 10 atomic%.
総量約３ｇのマグネシウムおよび銅のインゴットを、射出口径０．５ｍｍのカーボン製のノズルに入れ、アルゴン雰囲気中、８００℃、５分間の高周波溶解によって溶融する。その後、溶融した合金を周速度４０ｍ／ｓで回転する銅製の単ロール表面へ、０．２ＭＰａの圧力で射出することにより急速冷却し、薄帯状のマグネシウム−銅合金を作製した。得られた薄帯試料は、およそ幅１．５ｍｍ、厚さ０．４ｍｍの形状をもつ。この方法によって作製されたＭｇ９６Ｃｕ４（原子％）の薄帯試料の０．２％耐力の値は、純マグネシウムの薄帯に対して約３倍であった。（図１参照）。 A total of about 3 g of magnesium and copper ingots are placed in a carbon nozzle having an injection diameter of 0.5 mm and melted by high frequency melting at 800 ° C. for 5 minutes in an argon atmosphere. Thereafter, the molten alloy was rapidly cooled by injection at a pressure of 0.2 MPa onto the surface of a copper single roll rotating at a peripheral speed of 40 m / s, thereby producing a ribbon-like magnesium-copper alloy. The obtained ribbon sample has a shape with a width of about 1.5 mm and a thickness of 0.4 mm. The 0.2% proof stress value of the Mg 96 Cu 4 (atomic%) ribbon sample produced by this method was about three times that of the pure magnesium ribbon. (See FIG. 1).
総量約３ｇのマグネシウム、銅およびイットリウムのインゴットから、実施例１と同様の溶融状態からの急冷凝固によって薄帯試料を作製した。得られたＭｇ９８Ｃｕ２Ｙ１の薄帯試料の０．２％耐力の値は、純マグネシウムの薄帯に対して約２倍であった。 A ribbon sample was prepared from an ingot of magnesium, copper and yttrium in a total amount of about 3 g by rapid solidification from the molten state as in Example 1. The 0.2% proof stress value of the obtained Mg 98 Cu 2 Y 1 ribbon sample was about twice that of the pure magnesium ribbon.
従来のマグネシウム合金と異なり、比較的安価な銅と微量なイットリウムのみを添加元素としている点や、複雑な熱処理過程および製造工程を必要としない点、更に銅およびイットリウムの添加量と急冷速度のみによって、任意に合金強度を制御できることから、製造コストを抑えた高強度マグネシウム合金として、携帯電子機器や航空機及び自動車等の部品材料として利用される可能性を有している。 Unlike conventional magnesium alloys, only relatively inexpensive copper and a small amount of yttrium are used as additive elements, complicated heat treatment and manufacturing processes are not required, and only the addition amount of copper and yttrium and the rapid cooling rate. Since the alloy strength can be controlled arbitrarily, it has the possibility of being used as a component material for portable electronic devices, aircrafts, automobiles and the like as a high-strength magnesium alloy with reduced manufacturing costs.
Claims (3)
The high-strength magnesium alloy according to claim 1 or 2, wherein a nozzle made of carbon is used as a nozzle used for spraying the melt when rapidly cooling the alloy composition heated and melted.
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