CN108385039B - Additional high-toughness zirconium-based amorphous composite material and preparation method thereof - Google Patents

Additional high-toughness zirconium-based amorphous composite material and preparation method thereof Download PDF

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CN108385039B
CN108385039B CN201810122693.XA CN201810122693A CN108385039B CN 108385039 B CN108385039 B CN 108385039B CN 201810122693 A CN201810122693 A CN 201810122693A CN 108385039 B CN108385039 B CN 108385039B
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李丹
王晶
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Ruisheng Precision Manufacturing Technology Changzhou Co ltd
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    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C45/00—Amorphous alloys
    • C22C45/10—Amorphous alloys with molybdenum, tungsten, niobium, tantalum, titanium, or zirconium or Hf as the major constituent
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
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    • 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
    • C22C1/11—Making amorphous alloys

Abstract

The invention relates to the field of materials with high mechanical properties, in particular to an additional high-toughness zirconium-based amorphous composite material and a preparation method thereof. The material is mainly made of a zirconium-based amorphous alloy and a second phase. According to the method, the second phase is added into the original amorphous alloy matrix, the second phase prevents the expansion of a single shear band in the amorphous alloy, more shear bands are induced, the bending and breaking strain of the material is improved on the premise of not reducing the breaking and bending strength of the original alloy material, the intrinsic characteristics of the material are improved from the original material end, the surface treatment and the like of the formed product are not needed, no additional process is needed except the smelting step of the master alloy, and the method is suitable for mass production.

Description

Additional high-toughness zirconium-based amorphous composite material and preparation method thereof
Technical Field
The invention relates to a material with high mechanical property in the application fields of consumer electronics, precision devices (such as robots), medical instruments, aerospace, aviation and the like, in particular to a high-toughness ultrahigh-strength zirconium-based amorphous composite material and a preparation method thereof.
Background
Amorphous alloys are distinguished from common crystalline materials by their distinct structural differences. In general, materials exist in the form of crystals, while amorphous materials are characterized by long-range disorder (short-range order), metastable state (crystallization at a certain temperature), isotropic physical properties to some extent, lack of exact melting point, glass transition temperature point, and the like. Meanwhile, the Glass has a similar structure with common Glass, has the characteristics of solid, metal and Glass, and is also called Metallic Glass (Metallic Glass). The crystal grain structure is not existed, and the atoms are randomly and uniformly distributed directly, and are connected by metal bond. Because the crystal grain structure is not existed, the crystal grain boundary and other defects and the lattice period translational symmetry and other characteristics are not existed, so that the crystal alloy material has the excellent properties which are not possessed by the traditional crystalline alloy material, such as high mechanical strength, high hardness, low elastic modulus, high wear resistance, high corrosion resistance and excellent soft magnetic property. The amorphous alloy has an internal structure formed by the super-quenching solidification of a molten mother alloy, and atoms of the amorphous alloy are not arranged in a periodic manner in the solidification process, so that a long-range disordered amorphous state is formed. After the discovery of the amorphous alloy, research and exploration of researchers are attracted for decades, and at present, amorphous alloy systems such as Zr-based, Cu-based, Al-based, Fe-based, Pd-based, Ni-based, Ti-based, Mg-based, rare earth-based systems and the like are discovered.
The research result of the Zr-based bulk amorphous alloy material is the most remarkable, and although the application of the Zr-based bulk amorphous alloy in industry is still limited by practical factors of various applications, such as high raw material cost, harsh process conditions, complex post-treatment processing and the like. The biggest limiting factor of the application is that the amorphous alloy has no plasticity, so that the feedback of the market application is always hesitant. Therefore, improving the toughness of the amorphous alloy is an urgent need for mass production of the material.
The addition of the second phase to prepare the amorphous composite material is one method for improving the toughness of the amorphous alloy, but the bonding (wettability) problem often exists between the added phase and the amorphous matrix, so that the interface strength of the second phase and the amorphous matrix is lower. In addition, the addition of the external phase often requires a large volume fraction (greater than 40%) to achieve the toughening effect, and thus the problem of uneven distribution of the external phase is easily caused. Due to the different shapes of the added phases, for the second phase which is fibrous, lamellar and three-dimensional skeleton, the amorphous composite material is often prepared by methods such as infiltration or hot pressing, and is not suitable for industrial production. Therefore, the micro-addition of the particulate second phase has been a major research point in amorphous composite materials for industrial production.
Disclosure of Invention
The invention aims to overcome the problems and provide a high-toughness zirconium-based amorphous alloy composite material. According to the method, the second phase is added into the original amorphous alloy matrix, the second phase prevents the expansion of a single shear band in the amorphous alloy, more shear bands are induced, the bending and breaking strain of the material is improved on the premise of not reducing the breaking and bending strength of the original alloy material, the intrinsic characteristics of the material are improved from the original material end, the surface treatment and the like of the formed product are not needed, no additional process is needed except the smelting step of the master alloy, and the method is suitable for mass production.
The invention also aims to provide a preparation method of the zirconium-based amorphous alloy composite material.
The object of the invention can be achieved by the following measures:
a zirconium-based amorphous alloy composite material is mainly prepared from a zirconium-based amorphous alloy and a second phase.
The alloy composite material of the invention can be prepared by only zirconium-based amorphous alloy and the second phase, and other components which do not influence the main performance of the alloy composite material can be further added to prepare the alloy composite material with other performances
The second phase is metal or nonmetal powder, and the zirconium-based amorphous composite material with excellent mechanical properties is prepared by suspension smelting and vacuum die-casting the second phase and an amorphous master alloy material.
The amount of the second phase used is 20% or less, preferably 10% or less, more preferably 5% or less, most preferably 3% or less, and still more preferably in the range of 0.5 to 3%, based on 100% by volume of the total of the zirconium-based amorphous alloy and the second phase.
The second phase of the present invention includes, but is not limited to: I. non-metal powder (e.g., carbon powder), high melting point material powder (tungsten carbide, aluminum oxide, zirconium carbide, tungsten powder, niobium powder, molybdenum powder, tantalum powder, etc.), ductile metal powder (nickel powder, zirconium powder), etc.
The addition of the second phase I of the non-metal powder is expected to react with the pickaxe elements in the pickaxe-based amorphous alloy in situ to generate a compound, the compound can prevent the expansion of a shear band in an amorphous matrix, and meanwhile, the compound generated by the in situ reaction and the amorphous matrix have better interface combination, so that the mechanical property of the product is improved on the basis of not changing the original property of the alloy.
The second phase II of the high-melting-point material is slightly dissolved in the preparation process of the amorphous composite material to form a transition interface with the amorphous matrix, the dissolved part does not react with the amorphous matrix, and the undissolved second phase prevents the shear band in the amorphous matrix from expanding by bypassing the mechanism, so that the mechanical property of the product is improved on the basis of not changing the original property of the alloy.
The ductile metal second phase III is partially dissolved in the preparation process of the amorphous composite material, the forming capacity of the amorphous matrix is not influenced by the dissolved part, the expansion of a shear band in the amorphous matrix can be prevented only by bypassing the mechanism without the dissolved second phase, and the expansion energy of the shear band can be absorbed through the self plastic deformation, so that the mechanical property of the product is improved on the basis of not changing the original property of the alloy.
The zirconium-based amorphous alloy of the present invention includes, but is not limited to, a zirconium-based amorphous alloy material i, a zirconium-based amorphous alloy material ii, and a zirconium-based amorphous alloy material iii.
As for the zirconium-based amorphous alloy material i,
the chemical components of the zirconium-based amorphous alloy material i are as follows: (Zr)aHf1-a)x(Cu1-b-c-dNibAlcLd)yNbzM100-x-y-z(ii) a Wherein: l is an element of the IIIB or IVB group, M is an element of the VIII, IB, IIIA or IVA group, x is more than or equal to 45 and less than or equal to 65, y is more than or equal to 10 and less than or equal to 45, z is more than or equal to 0 and less than or equal to 10, a is more than or equal to 0.9885 and less than or equal to 0.9894, B is more than or equal to 0.05 and less than or equal to 0.2, c is more than or equal to 0.05 and less than or equal to 0.3.
In a preferable scheme, in the zirconium-based amorphous alloy material i, L is Y, Er or Gd element, M is Fe, Co or Sn element, a is 0.989 or 0.9889, x is more than or equal to 50 and less than or equal to 60, y is more than or equal to 20 and less than or equal to 45, z is more than or equal to 1 and less than or equal to 10, b is more than or equal to 0.10 and less than or equal to 0.20, c is more than or equal to 0.10 and less than or equal to 0.35, and d is more than or equal to 0.001 and less.
With regard to the zirconium-based amorphous alloy material ii,
in the zirconium-based amorphous alloy material ii, (Zr)aMbRE100-a-b)x(AlcCu100-c)y(NidCoeFe100-d-e)1-x-y- zAgzWherein:
x is more than or equal to 0.45 and less than or equal to 0.65, y is more than or equal to 0.30 and less than or equal to 0.40, z is more than or equal to 0 and less than or equal to 0.02, a is more than or equal to 85 and less than or equal to 95, b is more than or equal to 2 and less than or equal to 10, c is more than or equal to 20 and less than or equal to 40, d is more than or equal to 60 and less than or equal to;
among them, preferred are:
x is more than or equal to 0.50 and less than or equal to 0.55, y is more than or equal to 0.30 and less than or equal to 0.40, z is more than or equal to 0 and less than or equal to 0.01, a is more than or equal to 88 and less than or equal to 93, b is more than or equal to 2 and less than or equal to 8, c is more than or equal to 25 and less than or equal to 40, d is more than or equal to 66 and less than or equal to;
more preferably:
x is more than or equal to 0.53 and less than or equal to 0.57, y is 0.35, and 1-x-y-z is 0.10; z is more than or equal to 0 and less than or equal to 0.01, a is more than or equal to 85 and less than or equal to 95, b is more than or equal to 2 and less than or equal to 10, c is 28.57, d is 70, e is 20, RE is a rare earth element, and M represents Ti or Nb.
With regard to the zirconium-based amorphous alloy material iii,
the zirconium-based amorphous alloy material iii is: the Zr-Cu-Ni-Al-Ag-Y blocky amorphous alloy comprises the following components in atomic percentage: 41-63% of Zr, 18-46% of Cu, 1.5-12.5% of Ni, 4-15% of Al, 0.01-5% of Ag and 0.01-5% of Y.
The preferable Zr-Cu-Ni-Al-Ag-Y bulk amorphous alloy comprises the following components in percentage by atom: 49-55% of Zr, 28-36% of Cu, 4-10% of Al, 2-7% of Ni, 0.02-1.45% of Ag and 0.05-3% of Y.
The zirconium-based amorphous alloy material iii may specifically adopt the material referred to in CN 201410078957.8.
Preparation method of zirconium-based amorphous alloy composite material
The invention provides a preparation method of a zirconium-based amorphous composite alloy material, which comprises the following steps: the method comprises the steps of weighing high-purity raw materials of elements of the alloy corresponding to an amorphous matrix according to a proportion, preparing an amorphous mother alloy material by adopting an arc melting method under the protection of inert gas, then preparing an amorphous composite mother alloy by carrying out suspension melting on a second phase and the amorphous mother alloy material under the protection of inert gas, and finally preparing the amorphous composite material by adopting a vacuum die casting machine.
The high-purity raw materials of the invention are metal or nonmetal materials with the purity of corresponding elements of more than 99.3 percent.
The invention provides a more specific preparation method of a zirconium-based amorphous composite material, which comprises the following steps:
1. the raw materials adopted in the invention are all high-purity raw materials, wherein the purity of Zr is 99.4%, the purity of the other elements is 99.9%, and the raw materials are accurately weighed according to the proportion of a formula;
2. preparing a round ingot-shaped amorphous mother alloy material by an arc melting method under the protection of argon;
3. preparing a round ingot-shaped amorphous composite material master alloy by a suspension smelting method under the protection of argon;
3. selecting a certain amount of master alloy material, and preparing a sample with the thickness of 2mm by using a vacuum die casting machine;
4. observing the structural morphology of the second phase and the interface with the amorphous matrix by SEM;
5. and respectively carrying out three-point bending and impact mechanical property tests on the amorphous composite material sample.
The details for each of the above steps are as follows:
in step 1, the equipment used was an analytical balance with an accuracy of 0.0001 g.
In the step 2, a plurality of methods for preparing the amorphous master alloy are provided, and the amorphous master alloy is prepared by combining the copper mold smelting and the copper mold suspension smelting of an electric arc furnace.
In step 3, the vacuum die casting machine can adopt equipment developed by the cooperation of AAC and other research units. The equipment is used for forming national standard three-point bending and impact toughness sample shapes, and the die is designed, simulated and manufactured in an AAC interior.
In step 4, SEM test is completed in an AAC analysis center, and the size specification of a specific test sample is in accordance with the AAC unified sampling standard.
In the step 5, the three-point bending and impact mechanical property tests of the sample are finished in the AAC, and the size specification of the specific test sample is in accordance with the AAC unified sampling standard.
The invention has the beneficial effects that:
according to the method, the second phase is added into the original amorphous alloy matrix, the second phase prevents the expansion of a single shear band in the amorphous alloy, more shear bands are induced, and the bending and breaking strain of the material is improved on the premise of not reducing the breaking and bending strength of the original alloy material. Limited experimental data show that the composite material can maintain the original breaking bending strength on the basis of maintaining the original breaking bending strength on a zirconium-based amorphous alloy material base material with the original breaking bending strength of 2280MPa and the breaking bending strain of 2.3 percent, and the breaking bending strain reaches 3.5 percent; the range has different improvement effects according to different materials added with the second phase material and the material base material of the amorphous alloy; the intrinsic characteristics of the material are improved from the raw material end, and the surface treatment and the like of the formed product are not needed; besides the step of smelting the master alloy, no additional working procedure is required to be introduced, and the method is suitable for mass production.
Drawings
FIG. 1 is an optical microscope photograph of an amorphous matrix in examples 1 and 3;
FIG. 2 is an SEM image of amorphous composite A1 prepared in example 1;
FIG. 3 is an SEM photograph of amorphous composite C1 prepared in example 3;
fig. 4 is a bending stress-strain curve of amorphous composite material C1 prepared in example 3.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the following detailed description is given with reference to the embodiments. However, it will be appreciated by those of ordinary skill in the art that numerous technical details are set forth in order to provide a better understanding of the present invention in its various embodiments. However, the technical solutions claimed in the claims of the present invention can be implemented without these technical details and with various changes and modifications based on the following embodiments.
The examples are summarized in the following table:
composite material Substrate 1 Substrate 2 Substrate 3(F1)
Second phase C / / Example 1-A1
Second phase W Example 2B 1 Examples 5 to E1 Example 4D 1
Second phase Ni / / Example 3C 1
Example 1
This example illustrates the preparation of a pick-based amorphous composite material a1, in which the amorphous matrix (i.e., substrate) contains Zr51.9Cu31.8Ni6Al10Ag0.1Y0.2The second phase is C powder, and the addition amount is 3 Vol%. The ZrC is expected to react with the additionally added pickaxe elements in situ to generate ZrC, the ZrC can prevent the expansion of a shear band in the amorphous matrix, and meanwhile, the ZrC generated by the in situ reaction can be well combined with the amorphous matrix, so that the mechanical property of the product is improved on the basis of not changing the original property of the alloy.
a. Formulation Zr according to chemical composition51.9Cu31.8Ni6Al10Ag0.1Y0.2Each amorphous alloy formulation required the preparation of 240g of master alloy, one master alloy prepared according to 80g, for a total of 3 master alloys. The weighed amounts were calculated as atomic mass (total weight: 80g, 3 parts in the following table). Wherein the purity of zirconium is 99.4%, which is industrial grade sponge zirconium, and the purity of the rest elements is 99.9%. Before melting, the C needed to be added and the Zr needed to react with C in situ were prepared (table below).
Zr Cu Ni Al Ag Y Zr C
51.205g 21.855g 3.809g 2.918g 0.117g 0.096g 0.8g 0.8g
b. Under the protection of argon, the raw materials are smelted by an arc smelting method to prepare the amorphous composite master alloy material, and the whole process aims at melting various elements into an alloy material. In order to ensure the uniformity of the smelted mother alloy round ingot, the mother alloy round ingot needs to be turned over for 3-4 times in the process of arc smelting the mother alloy round ingot, the temperature of the arc smelting heating is above the melting point of the mother alloy, and the vacuum degree is 10-1Pa to 10-2Pa。
c. The prepared 240g of round ingot master alloy material is put into a vacuum die casting machine, and a uniform die casting process is adopted to form 12 strip-shaped samples for testing the mechanical properties of three-point bending and impacting, wherein the size is 2mm x 10mm x 50 mm.
d. The prepared sample is subjected to three-point bending and impact mechanical property tests, and specific data are shown in table 1.
The comparative example was prepared in the same manner as above except that step b was not employed, using an amorphous alloy without the second phase as a control.
TABLE 1 sample A1 three-point bend and impact mechanical Property test data
Figure BDA0001572563050000051
As can be seen from FIG. 2, the addition of C promotes the formation of ZrC, and ZrC is uniformly distributed in the amorphous matrix.
Example 2
This example illustrates the preparation of a pick-based amorphous composite material B1, in which the amorphous matrix component is Zr56.1Hf0.6Cu15.2Ni14.0Al10.4Nb3.5Y0.2The second phase was W and the amount added was 1.75 Vol%. W is dissolved in a small amount in the process of preparing the amorphous composite material, a transition interface is formed between the W and an amorphous matrix, the dissolved part does not react with the amorphous matrix, and the undissolved second phase prevents the shear band in the amorphous matrix from expanding by bypassing a mechanism, so that the mechanical property of the product is improved on the basis of not changing the original property of the alloy.
a. Formulation Zr according to chemical composition56.1Hf0.6Cu15.2Ni14.0Al10.4Nb3.5Y0.2Each amorphous alloy formulation required the preparation of 240g of master alloy, one master alloy prepared according to 80g, for a total of 3 master alloys. The weighed amounts were calculated as atomic mass (total weight: 80g, 3 parts in the following table). Wherein the purity of zirconium is 99.4%, which is industrial grade sponge zirconium, and the purity of the rest elements is 99.9%.
b. Under the protection of argon, the raw materials are smelted by an arc smelting method to prepare the amorphous mother alloy material, and the whole process aims at melting various elements into the alloy material. In order to ensure the uniformity of the smelted mother alloy round ingot, the mother alloy round ingot needs to be turned over for 3-4 times in the process of arc smelting the mother alloy round ingot, the temperature of the arc smelting heating is above the melting point of the mother alloy, and the vacuum degree is 10-1Pa to 10-2Pa。
c. In argonUnder protection, the mother alloy and W are smelted together by a suspension smelting method to prepare the amorphous composite mother alloy material, and the whole process aims to ensure that W is uniformly distributed in the amorphous mother alloy. In order to ensure that the melted amorphous composite material master alloy is uniform, in the suspension melting process, a master alloy round ingot needs to be turned over for 4-6 times, the temperature of suspension melting and heating is 100 ℃ above the melting point of the master alloy, the total melting time is 10min, and the vacuum degree is 10-1Pa to 10-2Pa。
d. The prepared 240g of round ingot master alloy material is put into a vacuum die casting machine, and a uniform die casting process is adopted to form 12 strip-shaped samples for testing the mechanical properties of three-point bending and impacting, wherein the size is 2mm x 10mm x 50 mm.
e. The prepared sample is subjected to three-point bending mechanical property test, and specific data are shown in table 2.
The comparative example was prepared in the same manner as above except that step c was not employed, using an amorphous alloy without the second phase as a control.
TABLE 2 sample B1 three-point bend mechanical Property test data
Figure BDA0001572563050000061
Example 3
This example illustrates the preparation of a pick-based amorphous composite material C1, in which the amorphous matrix component is Zr51.9Cu31.8Ni6Al10Ag0.1Y0.2The second phase was Ni and the amount added was 3 Vol%. Ni is used as an amorphous matrix composition element, a small amount of Ni is dissolved in the preparation process of the amorphous composite material, the forming capability of the amorphous matrix is not influenced by the dissolved part, the expansion of a shear band in the amorphous matrix is prevented by bypassing a mechanism by the undissolved second phase technique, and the expansion energy of the shear band can be absorbed through self plastic deformation, so that the mechanical property of the product is improved on the basis of not changing the original property of the alloy.
The a, b, d, e steps are the same as in example 2, except that the suspension smelting process in c is different. Since Ni is magnetic and has a low melting point, it is necessary to use a master alloyFeeding materials for the second time through a charging basket after melting, firstly increasing current for melting for 4min, then reducing current for melting for 2min, and controlling the vacuum degree to be 10-1Pa to 10-2Pa。
The comparative example was prepared in the same manner as above except that step c was not employed, using an amorphous alloy without the second phase as a control.
TABLE 3 sample C1 three-Point bend and impact mechanical Property test data
Figure BDA0001572563050000071
As can be seen from fig. 3, the slight dissolution of Ni did not affect the formation of the matrix, and the undissolved Ni was uniformly distributed in the amorphous matrix. Undissolved Ni blocks the expansion of the shear band by bypassing the mechanism, absorbs the expansion energy of the shear band through self plastic deformation, promotes the formation of multiple shear bands, and improves the bending strain of the amorphous matrix (see figure 4), so that the impact toughness of the amorphous matrix exceeds 200J/cm2。
Example 4
This example illustrates the preparation of a pick-based amorphous composite material D1, in which the amorphous matrix component is Zr51.9Cu31.8Ni6Al10Ag0.1Y0.2The second phase was W and the amount added was 1.75 Vol%. The principle is the same as that of example 2. The preparation method is the same as example 2. The preparation method of the comparative example was the same as that of the comparative example except that step c was not employed, except that the second phase-free amorphous alloy was used as the comparative example.
TABLE 4 sample D1 three-point bend mechanical Property test data
Figure BDA0001572563050000072
Example 5
This example illustrates the preparation of a pick-based amorphous composite material E1, in which the amorphous matrix component is Zr50.8Ti4Y0.2Al10Cu25Ni7Co2Fe1The second phase was W and the amount added was 1.75 Vol%. Original sourceThe same procedure as in example 2 was repeated. The preparation method is the same as example 2. The preparation method of the comparative example was the same as that of the comparative example except that step c was not employed, except that the second phase-free amorphous alloy was used as the comparative example.
TABLE 5 sample E1 three-point bend mechanical Property test data
Figure BDA0001572563050000081
It will be understood by those of ordinary skill in the art that the foregoing embodiments are specific examples for carrying out the invention, and that various changes in form and details may be made therein without departing from the spirit and scope of the invention in practice.

Claims (9)

1. An additional high-toughness zirconium-based amorphous composite material is characterized in that the material is mainly prepared from a zirconium-based amorphous alloy and a second phase;
the zirconium-based amorphous alloy is selected from:
the zirconium-based amorphous alloy material ii: (Zr)aMbRE100-a-b)x(AlcCu100-c)y(NidCoeFe100-d-e)1-x-y-zAgzWherein: x is more than or equal to 0.50 and less than or equal to 0.55, y is more than or equal to 0.30 and less than or equal to 0.40, z is more than or equal to 0 and less than or equal to 0.01, a is more than or equal to 88 and less than or equal to 93, b is more than or equal to 2 and less than or equal to 8, c is more than or equal to 25 and less than or equal to 40, d is more than or equal to 66 and less than or equal to.
2. The added high toughness zirconium based amorphous composite material according to claim 1, wherein said second phase is one or more of non-metal powder, high melting point material powder or tough metal powder.
3. The added high-toughness zirconium-based amorphous composite material as claimed in claim 1 or 2, wherein the second phase is one or more of carbon powder, tungsten carbide, aluminum oxide, zirconium carbide, tungsten powder, niobium powder, molybdenum powder, tantalum powder, nickel powder and zirconium powder.
4. Additional high toughness zirconium based amorphous composite material according to claim 1 or 2, characterized in that the amount of the second phase is 20% or less based on 100% total volume of the zirconium based amorphous alloy and the second phase.
5. Additional high toughness zirconium based amorphous composite material according to claim 1 or 2, characterized in that the amount of the second phase is 10% or less based on 100% total volume of the zirconium based amorphous alloy and the second phase.
6. Additional high toughness zirconium based amorphous composite material according to claim 1 or 2, characterized in that the amount of the second phase is below 5% based on 100% of the total volume of the zirconium based amorphous alloy and the second phase.
7. Additional high toughness zirconium based amorphous composite material according to claim 1 or 2, characterized in that the amount of the second phase is 3% or less based on 100% total volume of the zirconium based amorphous alloy and the second phase.
8. The added high-toughness zirconium-based amorphous composite material according to claim 1, wherein in the zirconium-based amorphous alloy material ii, x is 0.53 ≦ 0.57, y is 0.35, and 1-x-y-z is 0.10; z is more than or equal to 0 and less than or equal to 0.01, a is more than or equal to 85 and less than or equal to 95, b is more than or equal to 2 and less than or equal to 10, c is 28.57, d is 70, e is 20, RE is a rare earth element, and M represents Ti or Nb.
9. The preparation method of the externally added high-toughness zirconium-based amorphous composite material as claimed in claim 1, characterized in that after high-purity raw materials of elements corresponding to the alloy of the amorphous matrix are weighed in proportion, an amorphous mother alloy material is prepared by arc melting under the protection of inert gas, then a second phase and the amorphous mother alloy material are suspended and melted under the protection of inert gas to prepare the amorphous composite material mother alloy, and finally, a vacuum die casting machine is adopted to prepare the amorphous composite material.
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