CN1958831A - Copper-zirconium based amorphous alloy, and preparation method - Google Patents

Copper-zirconium based amorphous alloy, and preparation method Download PDF

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CN1958831A
CN1958831A CN 200510117160 CN200510117160A CN1958831A CN 1958831 A CN1958831 A CN 1958831A CN 200510117160 CN200510117160 CN 200510117160 CN 200510117160 A CN200510117160 A CN 200510117160A CN 1958831 A CN1958831 A CN 1958831A
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copper
zirconium
alloy
amorphous alloy
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CN100445413C (en
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汤美波
余鹏
赵德乾
潘明祥
汪卫华
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Institute of Physics of CAS
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Abstract

This invention relates to a Cu-Zr-based amorphous alloy, whose general formula is (Cu1-xZrx)aAlbMc, where, x is 0.40-0.60; a is 80-100; b is 0-14; c is 0-20; a + b + c is 100; M is Y, La, Ce, Pr, Nd, Gd, Tb, Dy, Ho, Er, Ti, Ag, Ga, Hf, Ta, Nb, Ni, Co or Fe. The preparation method comprises: (1) mixing Cu, Zr, Al and M according to the ratio in Ti-adsorbed Ar atmosphere in an arc furnace, smelting and cooling to obtain mother alloy ingot; (2) re-melting the mother alloy ingot in air, and casting into a water-cooling metal mold to obtain the Cu-Zr-based amorphous alloy. The alloy has high glass formation ability, high crystallization inhibition and large size at a very low cooling speed.

Description

A kind of copper-zirconium-base amorphous alloy and preparation method thereof
Technical field
The invention belongs to non-crystaline amorphous metal or metallic glass field, specifically relate to a kind of copper-zirconium-base amorphous alloy, and preparation method thereof.
Background technology
Non-crystaline amorphous metal or metallic glass normally metal alloy from the liquid cooled to the glass transformation temperature below, before forming core and crystallization, solidify formation.Yet be subjected to the restriction of metal alloy amorphous formation ability, obtain large-sized amorphous bulk, sufficiently high speed of cooling must be arranged.Can obtain high rate of cooling by molten metal or alloy are sprayed onto on the extraordinary conductive substrate of heat conduction, but adopt this method can only obtain strip or powder.
Nearly more than ten years, improvement by alloying constituent optimization design and technology of preparing, people have broken through the restriction of high speed cooling conditions, a series of non-crystaline amorphous metals have been found with stronger inhibition crystallizing power, promptly under low rate of cooling, by the bulk amorphous alloy or the metallic glass of the multiple alloy systems of preparation such as ordinary process method such as die cast, shrend, containment heterogeneous nucleation, directional freeze, powder metallurgy, spray to cast shaping, compaction moulding.Compare with traditional crystal alloy material, bulk amorphous alloys has excellent mechanical property, good processing properties, excellent in chemical activity and magnetic performance, thereby has been applied in many fields such as civilian and military affairs.
In the bulk amorphous alloys that has been found that system, mainly be multicomponent alloy system, and the preparation of relevant compound basic alloy system and research are gone back seldom based on single-element.Bulk amorphous alloys has excellent performances such as higher intensity mostly, for example in copper base or zirconium base, reach more than the 1500MPa, much larger than the intensity of ordinary steel, and be used in very soon on golf club panel, other precision optical instrument parts, corrosion-resistant vessel, bullet or the armour piercing shot bullet core.But the shortcoming of bulk amorphous alloys maximum does not have plastic deformation exactly, does not more have the work hardening characteristic.This performance shortcomings has limited too the piece non-crystaline amorphous metal widely in application in engineering.We wish by appropriate design of alloy, make the inhibition crystallization begin required critical cooling rate and further reduce, thereby obtain larger sized amorphous bulk, satisfy the needs of industrial application.
Summary of the invention
It is low to the objective of the invention is to overcome the inhibition crystallizing power that has non-crystaline amorphous metal now, the very little defective of non-crystaline amorphous metal size of using prior art to obtain, thus providing a kind of has high glass forming ability, suppress crystallizing power strong, can under very low rate of cooling, make larger sized, have super-high-plasticity and a very high-intensity copper-zirconium-base amorphous alloy.
Another object of the present invention is to provide the preparation method of described copper-zirconium-base amorphous alloy.
The objective of the invention is to realize by the following technical solutions:
The invention provides a kind of copper-zirconium-base amorphous alloy, is to be main component with copper and zirconium, and other metallic element is as alloying element, and it forms available following formulate:
(Cu 1-xZr x) aAl bM c
Wherein, 0.40≤x≤0.60,80≤a≤100,0≤b≤14,0≤c≤20, and a+b+c=100;
Metallic element M is Y, La, Ce, Pr, Nd, Gd, Tb, Dy, Ho, Er, Ti, Ag, Ga, Hf, Ta, Nb, Ni, Co or Fe.
Described copper zirconium base large amorphous alloy comprises the amorphous phase that is not less than 70% volume percent, and the ratio of this amorphous phase is determined by calculating heat content.
The invention provides a kind of preparation method of above-mentioned copper-zirconium-base amorphous alloy, comprise following step:
1) batching: according to general formula (Cu 1-xZr x) aAl bM cNeeded ratio is with the Cu in the said components, Zr, Al and metallic element M batching;
2) ingot casting: in the electric arc furnace of the argon atmospher that titanium adsorbs, each component batching in the step 1) is mixed, melting obtains mother alloy ingot after the cooling;
3) suction casting: use conventional permanent mold casting method, with step 2) the mother alloy ingot refuse that makes utilizes the absorbing and casting device in the electric arc furnace, and the melt suction water-cooled metal mould with mother alloy obtains copper-zirconium-base amorphous alloy (Cu 1-xZr x) aAl bM c
The purity of each element Cu, Zr, Al and M raw material all is not less than 99.9wt% (weight percent) in the described step 1).
Above-mentioned copper zirconium base large amorphous alloy provided by the invention has high glass forming ability, and its crystallization temperature is at 660～783K, and glass transformation temperature is at 629～706K, and the width of supercooling liquid phase region is at 30～86K.This alloy has excellent mechanical property and super-high-plasticity, and its intensity can reach 2265MPa, has the characteristics of work hardening and 18% plastic deformation simultaneously.
Copper zirconium base large amorphous alloy provided by the invention and existing non-crystaline amorphous metal, its advantage is:
1, copper-zirconium-base amorphous alloy of the present invention has excellent mechanical property, in the plastic deformation that room temperature has superelevation, and work hardening and very high performances such as intensity.Therefore copper-zirconium-base amorphous alloy has the potential application prospect.
2, copper zirconium base large amorphous alloy of the present invention has higher glass forming ability and thermostability, and its glass transformation temperature is at 629～739K, and crystallization temperature is at 660～783K, and the width of supercooling liquid phase region is at 30～87K.
3, the required critical cooling rate of copper zirconium base large amorphous alloy of the present invention's formation is low, and it is stronger to suppress crystallizing power, is easy to form large-sized non-crystaline amorphous metal, and its size is not less than 1 millimeter in each dimension, and the critical diameter size is not less than 1 millimeter.
4, copper zirconium base large amorphous alloy of the present invention has high glass transformation temperature and crystallization temperature, and corresponding high thermostability helps it and is applied in wideer temperature range.
5, preparing the required raw copper of copper zirconium base large amorphous alloy of the present invention or the purity of zirconium is 99.9wt%, can be industrial starting material, and the Mineral resources of copper or zirconium are quite abundant, thereby the alloy phase ratio of its cost and other precious metal-based, want cheap a lot, so development copper zirconium base large amorphous alloy is very suitable for the china natural resources characteristics.
Description of drawings
Fig. 1 is the Cu of the embodiment of the invention 1 preparation 55Zr 45The X-ray diffractogram of non-crystaline amorphous metal;
Fig. 2 is the Cu of the embodiment of the invention 1 preparation 55Zr 45Differential scanning calorimetry of bulk amorphous alloys (DSC) and differential thermal analysis (DTA) graphic representation (heating rate is 10K/min);
Fig. 3 is that the diameter of the embodiment of the invention 4 to 7 preparations all is 8 millimeters (Cu 0.5Zr 0.5) aAl 7Gd 93-a(a=92; 91; 90; 88) X-ray diffractogram of copper-zirconium-base amorphous alloy;
Fig. 4 is that the diameter of the embodiment of the invention 4 to 8 preparations all is 8 millimeters (Cu 0.5Zr 0.5) aAl 7Gd 93-a(a=92; 91; 90; 88; 86) the DSC graphic representation of copper zirconium base large amorphous alloy (heating rate is 20K/min);
Fig. 5 is the embodiment of the invention 11 preparation (Cu 0.5Zr 0.5) 90Ti 10The X-ray diffractogram of copper-zirconium-base amorphous alloy;
Fig. 6 is the embodiment of the invention 11 preparation (Cu 0.5Zr 0.5) 90Ti 10The DSC graphic representation of copper zirconium base large amorphous alloy (heating rate is 20K/min);
Fig. 7 is that the diameter of the embodiment of the invention 2 preparations is 2 millimeters (Cu 0.5Zr 0.5) 95Al 5And Cu 50Zr 50Copper-zirconium-base amorphous alloy is 8 * 10 in strain rate -4s -1Stress-strain(ed) curve.
Embodiment
Embodiment 1, preparation Cu 55Zr 45Bulk amorphous alloys
With the purity of raw material be the Cu of 99.9% (weight percent) and Zr component by the molar weight ratio be prepare at 55: 45 after, in the electric arc furnace of the argon atmospher of titanium absorption, mix and melting, obtain Cu after the cooling 55Zr 45The mother alloy ingot of binary alloy; Use conventional metal mould cast method then, with this ingot casting refuse, utilize the absorbing and casting device in the electric arc furnace, the mother alloy melt is sucked water cooled copper mould, can obtain composition is Cu 55Zr 45, diameter is 1 millimeter a block amorphous alloy.
Can prove Cu from X-ray diffraction (XRD) as shown in Figure 1 55Zr 45Alloy is an amorphous alloy completely.Fig. 2 is Cu 55Zr 45The heat analysis of bulk amorphous alloys (DSC and DTA) figure, as can be seen from the figure: its second-order transition temperature (T g), crystallization begins temperature (T x), fusing beginning temperature (T m) and width (the Δ T=T that crosses the cold-zone liquid phase x-T g) be respectively 689K, 725K, 1151K and 36K.In addition, this alloy also has higher reduction glass temperature (T Rg) and vitrifying index (γ), they are respectively 0.58 and 0.386.T RgUsually can be used for judging the glass forming ability of non-crystaline amorphous metal with the γ value, therefore visible Cu 55Zr 45Non-crystaline amorphous metal has bigger glass forming ability.
The copper zirconium base large amorphous alloy of embodiment 2～34, the various proportionings of preparation
Prepare the copper zirconium base large amorphous alloy of various proportionings by the method for embodiment 1, it is formed and thermal physical property parameter is listed in the table 1.
The composition and the hot rerum natura of table l, copper zirconium base large amorphous alloy of the present invention
Embodiment Alloying constituent D (mm) T g (K) T x (K) T l (K) ΔT (K) T rg γ R (K/min)
l 2 3 4 5 6 7 8 9 10 11 12 Cu 55Zr 45 (Cu 0.5Zr 0.5) 95Al 5 (Cu 0.5Zr 0.5) 88Al 12 (Cu 0.5Zr 0.5) 92Al 7Gd 1 (Cu 0.5Zr 0.5) 91Al 7Gd 2 (Cu 0.5Zr 0.5) 90Al 7Gd 3 (Cu 0.5Zr 0.5) 88Al 7Gd 5 (Cu 0.5Zr 0.5) 86Al 7Gd 7 (Cu 0.5Zr 0.5) 91Al 7Y 2 (Cu 0.55Zr 0.45) 86Al 7Y 7 (Cu 0.5Zr 0.5) 90Ti 10 (Cu 0.5Zr 0.5) 86Al 7Er 7 1 5 3 8 8 8 5 5 5 5 3 3 689 695 708 696 687 679 673 671 693 681 629 69l 725 760 771 771 766 765 754 744 770 768 660 753 1187 1176 ll56 1151 1149 1145 1139 1130 l143 1131 1191 1145 36 65 63 75 79 86 71 73 77 87 30 62 0.58 0.59 0.6l 0.60 0.60 0.59 0.59 0.59 0.61 0.60 0.53 0.60 0.39 0.41 0.41 0.42 0.42 0.42 0.42 0.41 0.42 0.42 0.36 0.41 10 20 20 20 20 20 20 20 20 20 20 20
13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 (Cu 0.5Zr 0.5) 86Al 7Ho 7 (Cu 0.5Zr 0.5) 86Al 7Tb 7 (Cu 0.5Zr 0.5) 86Al 7Dy 7 (Cu 0.5Zr 0.5) 86Al 7Nd 7 (Cu 0.5Zr 0.5) 86Al 7Pr 7 (Cu 0.5Zr 0.5) 86Al 7Ce 7 (Cu 0.5Zr 0.5) 86Al 7La 7 (Cu 0.5Zr 0.5) 86Al 7Ag 7 (Cu 0.5Zr 0.5) 80Ag 20 (Cu 0.54Zr 0.46) 92.5Al 5Ti 2.5 (Cu 0.55Zr 0.45) 95Ga 5 (Cu 0.6Zr 0.4) 95Ta 5 (Cu 0.6Zr 0.4) 95Nb 5 (Cu 0.42Zr 0.58) 86Al 14 (Cu 0.4Zr 0.6) 90Al 10 (Cu 0.53Zr 0.47) 95Al 5 (Cu 0.47Zr 0.53) 95Al 5 (Cu 0.6Zr 0.4) 90Al 10 (Cu 0.53Zr 0.47) 95Hf 5 (Cu 0.5Zr 0.5) 94Al 5Ni 1 (Cu 0.5Zr 0.5) 94Al 5Co 1 (Cu 0.5Zr 0.5) 94Al 5 Fe 1 3 3 2 2 1 1 8 1 4 2 1 1 5 5 5 3 2 1 2 2 2 687 676 680 659 661 659 664 722 739 700 733 709 705 724 698 714 701 723 725 698 699 697 749 742 748 729 725 721 723 794 796 746 777 765 761 771 763 764 773 797 794 757 754 759 1142 1138 1135 1120 1115 1114 1119 1125 1148 1161 1187 1195 1188 1188 1176 1185 1157 1163 1189 1178 1175 1177 62 66 68 70 64 61 59 72 57 64 44 56 56 47 65 50 72 74 69 59 55 62 0.60 0.59 0.60 0.59 0.59 0.59 0.59 0.64 0.64 0.60 0.62 0.59 0.59 0.61 0.59 0.60 0.61 0.62 0.61 0.59 0.59 0.59 0.41 0.41 0.41 0.41 0.41 0.41 0.41 0.43 0.42 0.40 0.40 0.40 0.40 0.40 0.41 0.40 0.42 0.42 0.41 0.40 0.40 0.41 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20 20
Annotate: 1) the symbol implication is as follows in the table: the critical diameter size under D---this experiment condition; T g---second-order transition temperature; T x---crystallization begins temperature; T l---the fusing end temp; Δ T=T x-T g---cross the width of cold-zone liquid phase; T Rg---the reduction glass temperature; γ---vitrifying index; R---used heating rate during each composition sample measurement.
2)T rg＝T g/T l；γ＝T x/(T g+T l)。

Claims (3)

1, a kind of copper-zirconium-base amorphous alloy is to be main component with copper and zirconium, and it is formed and uses following formulate:
(Cu 1-xZr x) aAl bM c
Wherein, 0.40≤x≤0.60,80≤a≤100,0≤b≤14,0≤c≤20, and a+b+c=100;
Metallic element M is Y, La, Ce, Pr, Nd, Gd, Tb, Dy, Ho, Er, Ti, Ag, Ga, Hf, Ta, Nb, Ni, Co or Fe.
2, the preparation method of the described copper-zirconium-base amorphous alloy of a kind of claim 1 comprises following step:
1) batching: according to general formula (Cu 1-xZr x) aAl bM cNeeded ratio is with the Cu in the said components, Zr, Al and metallic element M batching;
2) ingot casting: in the electric arc furnace of the argon atmospher that titanium adsorbs, each component batching in the step 1) is mixed, melting obtains mother alloy ingot after the cooling;
3) suction casting: use conventional permanent mold casting method, with step 2) the mother alloy ingot refuse that makes utilizes the absorbing and casting device in the electric arc furnace, and the melt suction water-cooled metal mould with mother alloy obtains copper-zirconium-base amorphous alloy (Cu of the present invention 1-xZr x) aAl bM c
3, the preparation method of copper-zirconium-base amorphous alloy as claimed in claim 2 is characterized in that: the purity of each element Cu, Zr, Al and M raw material all is not less than 99.9wt% in the described step 1).
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CN107829046B (en) * 2017-11-08 2020-01-31 湖南理工学院 Fe-containing copper-based bulk amorphous alloy and preparation process thereof
CN109943785A (en) * 2019-02-27 2019-06-28 山东融金粉末科技股份有限公司 A kind of amorphous alloy matrix composite and preparation method thereof
CN109722559A (en) * 2019-03-14 2019-05-07 北京科技大学 A kind of copper zirconium/hafnium base noncrystal alloy of oxygen alloy and preparation method thereof
CN114381674A (en) * 2021-12-24 2022-04-22 盘星新型合金材料(常州)有限公司 ZrCu-based amorphous alloy powder and preparation method thereof
CN114561604A (en) * 2022-01-18 2022-05-31 中国人民解放军陆军装甲兵学院 Copper-zirconium-based amorphous powder for repairing multiple damages, coating and preparation method
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
CN115386812A (en) * 2022-08-31 2022-11-25 东莞市逸昊金属材料科技有限公司 Block amorphous alloy for casting light component and processing method thereof
CN116254488A (en) * 2022-12-08 2023-06-13 广州爱克科技有限公司 High-ductility zirconium-based metallic glass alloy with work hardening characteristics and preparation method and application thereof

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