JP2003239051A - HIGH-STRENGTH Zr-BASE METALLIC GLASS - Google Patents

HIGH-STRENGTH Zr-BASE METALLIC GLASS

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Publication number
JP2003239051A
JP2003239051A JP2002039149A JP2002039149A JP2003239051A JP 2003239051 A JP2003239051 A JP 2003239051A JP 2002039149 A JP2002039149 A JP 2002039149A JP 2002039149 A JP2002039149 A JP 2002039149A JP 2003239051 A JP2003239051 A JP 2003239051A
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Prior art keywords
glass
metallic glass
formula
alloy
strength
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Japanese (ja)
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JP3737056B2 (en
Inventor
Akihisa Inoue
明久 井上
To Cho
涛 張
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Japan Science and Technology Agency
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Japan Science and Technology Corp
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Abstract

<P>PROBLEM TO BE SOLVED: To obtain metallic glass which does not contain elements of high melting points, such as Nb and Ta, permits easy smelting of a base material and exhibits high strength of 2,000 MPa. <P>SOLUTION: The Zr-base metallic glass has the composition expressed by formula: Zr<SB>1-x-y</SB>Al<SB>x</SB>Co<SB>y</SB>or formula: Zr<SB>1-x-y-z</SB>Al<SB>x</SB>Co<SB>y</SB>(Fe, Ni, Cu)<SB>z</SB>[(x), (y), (z) in the formulas are atomic ratios and are respective x=15 to 25, y=20 to 30, z≤10] and has the tensile strength of 2,000 MPa. The bulk metallic glass having a glass phase of ≥3 mm in diameter or thickness is obtained by a die casting process. <P>COPYRIGHT: (C)2003,JPO

Description

【発明の詳細な説明】Detailed Description of the Invention

【０００１】[0001]

【発明の属する技術分野】本発明は、強度が高く、組織
中にガラス相を含むZr基金属ガラスに関するものであ
る。TECHNICAL FIELD The present invention relates to a Zr-based metallic glass having high strength and containing a glass phase in its structure.

【０００２】[0002]

【従来の技術】金属または合金は、溶融状態から十分に
大きな冷却速度で冷却すると、金属ガラス得られること
がわかっている。従来のガラス相形成合金はガラス相形
成の臨界冷却速度は、104 〜106 K/秒であり、このため
金属ガラスは急速冷却の可能な薄体、粉末あるいは細線
状などに限られていた。薄体や細線状だけではなく、バ
ルク状の金属ガラスが作製可能となれば、例えば高強度
や高靭性といった金属ガラスの有する優れた特性によ
り、金属ガラスの用途範囲を著しく拡大できる。2. Description of the Related Art It has been known that a metal or an alloy can be obtained by cooling a metal or alloy from a molten state at a sufficiently high cooling rate. In the conventional glass phase forming alloys, the critical cooling rate for glass phase formation is 10 4 to 10 6 K / sec. Therefore, metallic glass is limited to thin bodies, powders or fine wires that can be rapidly cooled. . If it is possible to produce not only thin metal or thin wire-shaped but also bulk-shaped metallic glass, the range of applications of metallic glass can be significantly expanded due to the excellent properties of metallic glass such as high strength and high toughness.

【０００３】金型鋳造法によりバルク状の金属ガラスが
得られるためには、103 K/秒以下の遅い冷却速度でガラ
ス相が形成する合金が必要である。1990年頃から遅い冷
却速度でガラス化する合金の研究が進み、そのような合
金として、例えば特公平7-122120号公報に示される合
金、特開平8-74010号公報、特開平8-199318号公報に示
される合金、特開2000-265252号公報、米国特許5288344
号明細書、米国特許5368659号明細書に示される各種Zr
系合金が開発されている。In order to obtain a bulk metallic glass by the die casting method, an alloy which forms a glass phase at a slow cooling rate of 10 3 K / sec or less is required. Since around 1990, research on alloys that vitrify at a slow cooling rate proceeded, and as such alloys, for example, the alloys shown in Japanese Patent Publication No. 7-122120, JP-A-8-74010, JP-A-8-199318. Alloy shown in Japanese Patent Laid-Open No. 2000-265252 and US Pat. No. 5,288,344.
Various Zr shown in US Pat. No. 5,368,659
System alloys have been developed.

【０００４】[0004]

【発明が解決しようとする課題】従来のZr基ガラス合金
は、高融点のNb、Taなどの元素を含んでいるため、これ
らの元素は、他の構成元素との融点差が大きいので、均
一な母材を溶製するのが困難である。また、Beなど毒性
の強い元素を含有している。そのため、バルク金属ガラ
スは工業用材料として応用分野が制限されている。Beを
含有していない合金では、Alの含有量は15原子％以下で
あり、2000MPa以上の高強度を有する金属ガラスが得ら
れなかった。本発明は、Nb、Taなどの高融点の元素を含
まずに、母材を溶製することが容易で、2000MPaの高強
度を示す金属ガラスを得ることを目的とする。Since the conventional Zr-based glass alloy contains elements such as Nb and Ta having a high melting point, these elements have a large melting point difference from other constituent elements, so that they are uniform. It is difficult to melt the various base materials. It also contains highly toxic elements such as Be. Therefore, the application field of the bulk metallic glass is limited as an industrial material. In the alloy containing no Be, the Al content was 15 atomic% or less, and a metallic glass having a high strength of 2000 MPa or more could not be obtained. It is an object of the present invention to obtain a metallic glass that does not contain a high melting point element such as Nb or Ta, is easy to melt the base material, and has a high strength of 2000 MPa.

【０００５】[0005]

【課題を解決するための手段】本発明者らは、上記の課
題を解決するために、高強度を示す製造しやすい、工業
材料への応用が可能であるガラス形成能を有するZr基バ
ルク金属ガラスを提供することを目的として、合金組成
について探索した。その結果、Zr-Al-Co系の合金で引張
強度2000MPa以上のガラス相を有する高強度の金属ガラ
スが得られることを見出した。In order to solve the above-mentioned problems, the present inventors have proposed a Zr-based bulk metal which has high strength, is easy to manufacture, and can be applied to industrial materials and has a glass-forming ability. An alloy composition was searched for the purpose of providing glass. As a result, they have found that a high-strength metallic glass having a glass phase with a tensile strength of 2000 MPa or more can be obtained from a Zr-Al-Co alloy.

【０００６】すなわち、本発明は、式：Zr1-ｘ-ｙAlxCo
ｙ[式中のｘ、ｙは原子比率であり、それぞれｘ＝15〜2
5、ｙ＝20〜30]で表される組成を有する引張強度2000MP
a以上のZr基金属ガラスである。That is, the present invention provides the formula: Zr 1-x-y Al x Co
y [where x and y are atomic ratios, and x = 15 to 2 respectively
5, tensile strength 2000MP having a composition represented by y = 20 to 30]
It is a Zr-based metallic glass of a or more.

【０００７】また、本発明は、式：Zr1-ｘ-ｙ-ｚAlxCo
ｙ(Fe,Ni,Cu)ｚ[式中のｘ、ｙは原子比率であり、それ
ぞれｘ＝15〜25、ｙ＝20〜30、ｚ≦10]で表される組成
を有する引張強度2000MPa以上のZr基金属ガラスであ
る。The invention also provides the formula: Zr 1-x-y-z Al x Co
y (Fe, Ni, Cu) z [where x and y are atomic ratios, and have a composition represented by x = 15 to 25, y = 20 to 30 and z ≦ 10] and a tensile strength of 2000 MPa or more. Is a Zr-based metallic glass.

【０００８】また、本発明は、式：Zr1-ｘ-ｙAlxCo
ｙ[式中のｘ、ｙは原子比率であり、それぞれｘ＝15〜2
5、ｙ＝20〜30]で表される組成を有する金型鋳造法によ
りガラス相が得られた直径または厚み3ｍｍ以上のバル
クZr基金属ガラスである。The invention also provides the formula: Zr 1-xy Al x Co
y [where x and y are atomic ratios, and x = 15 to 2 respectively
5, y = 20 to 30], which is a bulk Zr-based metallic glass having a glass phase obtained by a metal mold casting method having a composition represented by y = 20 to 30] and having a diameter or a thickness of 3 mm or more.

【０００９】また、本発明は、式：Zr1-ｘ-ｙ-ｚAlxCo
ｙ(Fe,Ni,Cu)ｚ[式中のｘ、ｙは原子比率であり、それ
ぞれｘ＝15〜25、ｙ＝20〜30、ｚ≦10]で表される組成
を有する金型鋳造法によりガラス相が得られた直径また
は厚み3ｍｍ以上のバルクZr基金属ガラスガラスであ
る。The invention also provides the formula: Zr 1-x-y-z Al x Co
y (Fe, Ni, Cu) z [where x and y are atomic ratios, and a die casting method having a composition represented by x = 15 to 25, y = 20 to 30, and z ≦ 10] It is a bulk Zr-based metallic glass having a diameter or thickness of 3 mm or more in which a glass phase is obtained.

【００１０】本発明の金属ガラスの式：Zr1-ｘ-ｙAlxCo
ｙで表される組成において、Al量が原子比率で15未満25
超、Coの量が20未満30超の組成では、ガラス遷移温度と
結晶化温度の差で定義した過冷却液体域は小さくなり、
ガラス形成能が小さくなる。よって、ガラス相を有する
直径または厚み3ｍｍ未満の合金しか得られない。上記
の組成内であれば、ガラス相を有する最大で直径または
厚み4ｍｍ程度までの合金が得られる。より好ましく
は、ｘ＋ｙは40〜50である。最大の過冷却液体域もつ組
成はZr55Al20Co25での65Kであり、この組成を中心とす
る組成で大きいガラス形成能が得られ、この組成からの
ずれによってガラス形成能が小さくなる。The formula of the metallic glass of the present invention: Zr 1-x-y Al x Co
In the composition represented by y , the Al content is less than 15 by atomic ratio 25
Ultra, the composition of the amount of Co less than 20 and more than 30, the supercooled liquid region defined by the difference between the glass transition temperature and the crystallization temperature becomes small,
Glass forming ability is reduced. Therefore, only an alloy having a glass phase and having a diameter or a thickness of less than 3 mm can be obtained. Within the above composition, an alloy having a glass phase up to a diameter or a thickness of about 4 mm can be obtained. More preferably, x + y is 40-50. The composition with the maximum supercooled liquid region is 65 K in Zr 55 Al 20 Co 25 , and a composition centering on this composition gives a large glass forming ability, and a deviation from this composition reduces the glass forming ability.

【００１１】また、本発明の金属ガラスの式：Zr
1-ｘ-ｙ-ｚAlxCoｙ(Fe,Ni,Cu)ｚで表される組成におい
て、Alの量が原子比率で15未満20超、Coの量が20未満30
超、およびFe,Ni,Cuの量が10超の場合、過冷却液体域が
小さくなり、ガラス相を有する直径または厚み3ｍｍ未
満の合金しか得られない。上記の組成内であれば、ガラ
ス相を有する最大で直径または厚み5ｍｍ程度までの合
金が得られる。より好ましくは、2＜ｚ＜6である。Fe,N
i,またはCuを含む場合は、Zr55Al20Co20Cu5を中心する
組成で最大90Kの過冷却液体域を得られ、この組成を中
心とする組成で大きいガラス形成能が得られ、この組成
からのずれによってガラス形成能が小さくなる。The metallic glass of the present invention has the formula: Zr
1-x-y-z Al x Co y (Fe, Ni, Cu) In the composition represented by z , the amount of Al is less than 15 and less than 20 in atomic ratio, and the amount of Co is less than 20 30.
When the amount is more than 10 and the amount of Fe, Ni and Cu is more than 10, the supercooled liquid region becomes small and only an alloy having a glass phase and having a diameter or a thickness of less than 3 mm can be obtained. Within the above composition, an alloy having a glass phase up to a diameter or thickness of about 5 mm can be obtained. More preferably, 2 <z <6. Fe, N
In the case of containing i, or Cu, a composition centered on Zr 55 Al 20 Co 20 Cu 5 can provide a supercooled liquid region of up to 90 K, and a composition centered on this composition can provide a large glass forming ability. The deviation from the composition reduces the glass forming ability.

【００１２】[0012]

【実施例】以下、本発明の実施例について説明する。 実施例１〜１３および比較例１〜３EXAMPLES Examples of the present invention will be described below. Examples 1-13 and Comparative Examples 1-3

【００１３】[0013]

【表１】 [Table 1]

【００１４】表１に示している合金組成からなる材料に
ついて、各合金組成になるように母合金をアーク溶解炉
で溶製し、均一な母合金が得られるように、真空中ある
いはAr、Heなどの不活性ガス雰囲気中で、高周波加熱に
より母合金を再溶解して、銅製金型鋳造法によって直径
３ｍｍ、長さ５０ｍｍの丸棒試料を作成した。Regarding the materials having the alloy compositions shown in Table 1, the master alloys are melted in an arc melting furnace so as to have the respective alloy compositions, so that a uniform master alloy can be obtained in a vacuum or Ar, He. The mother alloy was remelted by high frequency heating in an inert gas atmosphere such as, and a round bar sample having a diameter of 3 mm and a length of 50 mm was prepared by a copper mold casting method.

【００１５】図１に、各合金組成のZr-Al-Co系合金の示
差走査熱量計を用いて測定した熱分析曲線を示してい
る。ガラス遷移温度Tgと結晶化開始温度Txの温度を測定
し、過冷却液体域(Tｘ−Tg)を算出した。この丸棒試料
中に含むガラス相の体積分率（Vf%)は、DSCを用いて試
料の結晶化の際の発熱を完全ガラス化した単ロール法に
より作製したリボン試料との比較により評価した。圧縮
強度、引張強度をそれぞれ測定した。FIG. 1 shows a thermal analysis curve of a Zr-Al-Co type alloy having each alloy composition measured by using a differential scanning calorimeter. The glass transition temperature Tg and the crystallization start temperature Tx were measured, and the supercooled liquid region (Tx-Tg) was calculated. The volume fraction (Vf%) of the glass phase contained in this round bar sample was evaluated by comparison with a ribbon sample prepared by the single roll method in which the heat generated during crystallization of the sample was completely vitrified using DSC. . The compressive strength and the tensile strength were measured respectively.

【００１６】表１より明らかなように、実施例１〜１３
の銅製金型鋳造による金属ガラスは、６０K以上の過冷
却液体域を示して、ガラス相の体積分率が90％以上で、
大きなガラス形成能を有し、圧縮強度および引張強度が
2000MPa以上の値を示している。As is clear from Table 1, Examples 1 to 13
The metallic glass produced by the copper mold casting of the above shows a supercooled liquid region of 60K or more, and the volume fraction of the glass phase is 90% or more,
It has a large glass-forming ability and compressive strength and tensile strength.
The value is 2000MPa or more.

【００１７】これに対して、比較例１の合金は、直径３
ｍｍの鋳造材ではガラス相が得られず、ガラス形成能が
低い。比較例２,３の合金では、圧縮強度および引張強
度は2000MPa以下であり、機械的性質に劣ることが分か
る。On the other hand, the alloy of Comparative Example 1 has a diameter of 3
In the case of the cast material of mm, the glass phase cannot be obtained, and the glass forming ability is low. The alloys of Comparative Examples 2 and 3 have a compressive strength and a tensile strength of 2000 MPa or less, which means that they have poor mechanical properties.

【図面の簡単な説明】[Brief description of drawings]

【図１】図１は、Zr-Al-Co系金属ガラスのDSC曲線を示
すグラフである。FIG. 1 is a graph showing a DSC curve of a Zr—Al—Co based metallic glass.

Claims (4)

【特許請求の範囲】[Claims] 【請求項１】 式：Zr1-ｘ-ｙAlxCoｙ[式中のｘ、ｙは
原子比率であり、それぞれｘ＝15〜25、ｙ＝20〜30]で
表される組成を有する引張強度2000MPa以上のZr基金属
ガラス。1. A composition represented by the formula: Zr 1-xy Al x Co y [where x and y are atomic ratios, and have a composition represented by x = 15 to 25 and y = 20 to 30]. Zr-based metallic glass with a tensile strength of 2000 MPa or more. 【請求項２】 式：Zr1-ｘ-ｙ-ｚAlxCoｙ(Fe,Ni,Cu)
ｚ[式中のｘ、ｙは原子比率であり、それぞれｘ＝15〜2
5、ｙ＝20〜30、ｚ≦10]で表される組成を有する引張強
度2000MPa以上のZr基金属ガラス。2. The formula: Zr 1-x-y-z Al x Co y (Fe, Ni, Cu)
z [where x and y are atomic ratios, and x = 15 to 2 respectively
5, y = 20 to 30, z ≦ 10] Zr-based metallic glass having a tensile strength of 2000 MPa or more. 【請求項３】 式：Zr1-ｘ-ｙAlxCoｙ[式中のｘ、ｙは
原子比率であり、それぞれｘ＝15〜25、ｙ＝20〜30]で
表される組成を有する金型鋳造法によりガラス相が得ら
れた直径または厚み3ｍｍ以上のバルクZr基金属ガラ
ス。3. A composition represented by the formula: Zr 1-xy Al x Co y [where x and y are atomic ratios and have a composition represented by x = 15 to 25 and y = 20 to 30]. Bulk Zr-based metallic glass with a diameter or thickness of 3 mm or more obtained by a glass casting method. 【請求項４】 式：Zr1-ｘ-ｙ-ｚAlxCoｙ(Fe,Ni,Cu)
ｚ[式中のｘ、ｙは原子比率であり、それぞれｘ＝15〜2
5、ｙ＝20〜30、ｚ≦10]で表される組成を有する金型鋳
造法によりガラス相が得られた直径または厚み3ｍｍ以
上のバルクZr基金属ガラス。4. The formula: Zr 1-x-y-z Al x Co y (Fe, Ni, Cu)
z [where x and y are atomic ratios, and x = 15 to 2 respectively
5, y = 20 to 30, z ≦ 10] A bulk Zr-based metallic glass having a glass phase obtained by a mold casting method and having a diameter or a thickness of 3 mm or more.
JP2002039149A 2002-02-15 2002-02-15 High strength Zr-based metallic glass Expired - Fee Related JP3737056B2 (en)

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Cited By (9)

* Cited by examiner, † Cited by third party
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CN103958709A (en) * 2011-11-24 2014-07-30 萨尔布吕肯大学 Bulk metallic glass forming alloy
JP2016516893A (en) * 2013-06-07 2016-06-09 コリア インスティテュート オブ インダストリアル テクノロジーＫｏｒｅａ Ｉｎｓｔｉｔｕｔｅ Ｏｆ Ｉｎｄｕｓｔｒｉａｌ Ｔｅｃｈｎｏｌｏｇｙ Zr-based amorphous alloy composition
CN108251697A (en) * 2017-12-15 2018-07-06 昆明理工大学 A kind of low temperature resistant high-strength and high ductility alloy
CN110295293A (en) * 2019-06-28 2019-10-01 中国科学院金属研究所 A kind of amorphous alloy component and preparation method thereof
CN110923481A (en) * 2018-09-20 2020-03-27 天津大学 Amorphous film/high-entropy alloy composite material and preparation method thereof
CN111593274A (en) * 2020-05-26 2020-08-28 湖南理工学院 A series of zirconium-base amorphous alloys with special crystallization behavior
CN112063937A (en) * 2020-09-16 2020-12-11 松山湖材料实验室 Nickel-free beryllium-free zirconium-based amorphous alloy and preparation method and application thereof
CN114657480A (en) * 2022-03-28 2022-06-24 北京科技大学 High-plasticity phase-separated Zr-based amorphous alloy and preparation method and application thereof
CN115725912A (en) * 2022-12-08 2023-03-03 广州爱克科技有限公司 Zirconium-based metallic glass alloy with high strength and high plastic strain as well as preparation method and application thereof

Cited By (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN103958709A (en) * 2011-11-24 2014-07-30 萨尔布吕肯大学 Bulk metallic glass forming alloy
US9506133B2 (en) 2011-11-24 2016-11-29 Universitat Des Saarlandes Bulk metallic glass forming alloy
JP2016516893A (en) * 2013-06-07 2016-06-09 コリア インスティテュート オブ インダストリアル テクノロジーＫｏｒｅａ Ｉｎｓｔｉｔｕｔｅ Ｏｆ Ｉｎｄｕｓｔｒｉａｌ Ｔｅｃｈｎｏｌｏｇｙ Zr-based amorphous alloy composition
CN108251697A (en) * 2017-12-15 2018-07-06 昆明理工大学 A kind of low temperature resistant high-strength and high ductility alloy
CN110923481A (en) * 2018-09-20 2020-03-27 天津大学 Amorphous film/high-entropy alloy composite material and preparation method thereof
CN110295293A (en) * 2019-06-28 2019-10-01 中国科学院金属研究所 A kind of amorphous alloy component and preparation method thereof
CN111593274A (en) * 2020-05-26 2020-08-28 湖南理工学院 A series of zirconium-base amorphous alloys with special crystallization behavior
CN112063937A (en) * 2020-09-16 2020-12-11 松山湖材料实验室 Nickel-free beryllium-free zirconium-based amorphous alloy and preparation method and application thereof
CN112063937B (en) * 2020-09-16 2022-03-22 松山湖材料实验室 Nickel-free beryllium-free zirconium-based amorphous alloy and preparation method and application thereof
CN114657480A (en) * 2022-03-28 2022-06-24 北京科技大学 High-plasticity phase-separated Zr-based amorphous alloy and preparation method and application thereof
CN115725912A (en) * 2022-12-08 2023-03-03 广州爱克科技有限公司 Zirconium-based metallic glass alloy with high strength and high plastic strain as well as preparation method and application thereof

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