CN116656985B - Preparation method of diamond/aluminum composite material - Google Patents
Preparation method of diamond/aluminum composite material Download PDFInfo
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- CN116656985B CN116656985B CN202310468582.5A CN202310468582A CN116656985B CN 116656985 B CN116656985 B CN 116656985B CN 202310468582 A CN202310468582 A CN 202310468582A CN 116656985 B CN116656985 B CN 116656985B
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- 229910003460 diamond Inorganic materials 0.000 title claims abstract description 128
- 239000010432 diamond Substances 0.000 title claims abstract description 128
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 title claims abstract description 63
- 239000002131 composite material Substances 0.000 title claims abstract description 58
- 229910052782 aluminium Inorganic materials 0.000 title claims abstract description 55
- 238000002360 preparation method Methods 0.000 title abstract description 8
- 239000000843 powder Substances 0.000 claims abstract description 55
- 238000005245 sintering Methods 0.000 claims abstract description 26
- 239000000463 material Substances 0.000 claims abstract description 23
- 238000000034 method Methods 0.000 claims abstract description 22
- 238000007731 hot pressing Methods 0.000 claims abstract description 20
- 239000011159 matrix material Substances 0.000 claims abstract description 19
- 229910000676 Si alloy Inorganic materials 0.000 claims abstract description 17
- 238000000498 ball milling Methods 0.000 claims abstract description 17
- 239000000203 mixture Substances 0.000 claims abstract description 17
- 238000010438 heat treatment Methods 0.000 claims abstract description 14
- 238000011049 filling Methods 0.000 claims abstract description 12
- 239000011863 silicon-based powder Substances 0.000 claims abstract description 12
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 10
- 238000002156 mixing Methods 0.000 claims abstract description 10
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 5
- 238000001816 cooling Methods 0.000 claims abstract description 4
- 238000011010 flushing procedure Methods 0.000 claims abstract description 4
- 238000003825 pressing Methods 0.000 claims abstract description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 16
- 230000008569 process Effects 0.000 claims description 10
- 229910052786 argon Inorganic materials 0.000 claims description 8
- 238000006073 displacement reaction Methods 0.000 claims description 3
- 238000012544 monitoring process Methods 0.000 claims description 3
- 239000004615 ingredient Substances 0.000 claims description 2
- 239000002245 particle Substances 0.000 abstract description 53
- 229910052751 metal Inorganic materials 0.000 abstract description 8
- 239000002184 metal Substances 0.000 abstract description 8
- 230000008595 infiltration Effects 0.000 abstract description 4
- 238000001764 infiltration Methods 0.000 abstract description 4
- 238000012545 processing Methods 0.000 abstract description 4
- 238000005516 engineering process Methods 0.000 abstract description 3
- 239000006185 dispersion Substances 0.000 abstract description 2
- 229910010271 silicon carbide Inorganic materials 0.000 description 24
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 22
- 230000002902 bimodal effect Effects 0.000 description 10
- CSDREXVUYHZDNP-UHFFFAOYSA-N alumanylidynesilicon Chemical compound [Al].[Si] CSDREXVUYHZDNP-UHFFFAOYSA-N 0.000 description 7
- 239000011156 metal matrix composite Substances 0.000 description 6
- 239000007788 liquid Substances 0.000 description 5
- 238000002844 melting Methods 0.000 description 5
- 230000008018 melting Effects 0.000 description 5
- 239000012071 phase Substances 0.000 description 5
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 238000012856 packing Methods 0.000 description 4
- 230000002787 reinforcement Effects 0.000 description 4
- 230000035882 stress Effects 0.000 description 4
- 230000015572 biosynthetic process Effects 0.000 description 3
- 239000011248 coating agent Substances 0.000 description 3
- 238000000576 coating method Methods 0.000 description 3
- 239000013078 crystal Substances 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 230000007246 mechanism Effects 0.000 description 3
- 229910052710 silicon Inorganic materials 0.000 description 3
- 239000010703 silicon Substances 0.000 description 3
- 239000000758 substrate Substances 0.000 description 3
- 229910045601 alloy Inorganic materials 0.000 description 2
- 239000000956 alloy Substances 0.000 description 2
- CAVCGVPGBKGDTG-UHFFFAOYSA-N alumanylidynemethyl(alumanylidynemethylalumanylidenemethylidene)alumane Chemical compound [Al]#C[Al]=C=[Al]C#[Al] CAVCGVPGBKGDTG-UHFFFAOYSA-N 0.000 description 2
- 238000012512 characterization method Methods 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 229910052755 nonmetal Inorganic materials 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 238000006467 substitution reaction Methods 0.000 description 2
- 230000008646 thermal stress Effects 0.000 description 2
- 229910021364 Al-Si alloy Inorganic materials 0.000 description 1
- 238000007088 Archimedes method Methods 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 230000001186 cumulative effect Effects 0.000 description 1
- 230000001419 dependent effect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000005496 eutectics Effects 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 229910001338 liquidmetal Inorganic materials 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- 238000003801 milling Methods 0.000 description 1
- 238000004806 packaging method and process Methods 0.000 description 1
- 238000010587 phase diagram Methods 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 230000003014 reinforcing effect Effects 0.000 description 1
- 239000012763 reinforcing filler Substances 0.000 description 1
- 238000005070 sampling Methods 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 229920002994 synthetic fiber Polymers 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
- 230000000007 visual effect Effects 0.000 description 1
- 238000012800 visualization Methods 0.000 description 1
- 239000011800 void material Substances 0.000 description 1
Classifications
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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
- C22C1/04—Making non-ferrous alloys by powder metallurgy
- C22C1/05—Mixtures of metal powder with non-metallic powder
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F3/00—Manufacture of workpieces or articles from metallic powder characterised by the manner of compacting or sintering; Apparatus specially adapted therefor ; Presses and furnaces
- B22F3/12—Both compacting and sintering
- B22F3/14—Both compacting and sintering simultaneously
-
- 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
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C26/00—Alloys containing diamond or cubic or wurtzitic boron nitride, fullerenes or carbon nanotubes
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/25—Process efficiency
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Manufacturing & Machinery (AREA)
- Manufacture Of Alloys Or Alloy Compounds (AREA)
Abstract
The invention relates to a preparation method of a diamond/aluminum composite material, which comprises the following steps: selecting Ib type artificial diamond micro powder and IMS-15 diamond as filling materials, and selecting pure aluminum powder, A1-8mass% Si alloy powder and Si powder as matrix materials; placing the filling powder and the matrix material into a container for swinging and vibrating mixing, and then ball milling to obtain a powder mixture; pressing the powder mixture, and then vacuumizing for hot-pressing sintering; sintering from room temperature to 480-520 ℃, preserving heat at the temperature for 2-4 minutes, then heating to 590-620 ℃ and preserving heat at the temperature for 1-3 minutes; and (3) closing the heating system under the vacuum state, naturally cooling to below 100 ℃, flushing high-purity nitrogen into the sintering furnace cavity, and opening the cavity after the pressure inside and outside the cavity is equal to the pressure. The method can effectively solve the problems of high processing temperature, reduced heat conductivity caused by direct contact of diamond particles and molten Al in the preparation of the diamond/aluminum composite material by a metal infiltration technology, and uneven dispersion of the diamond particles in the composite material.
Description
Technical Field
The invention relates to the technical field of composite materials, in particular to a preparation method of a high-heat-conductivity diamond/aluminum composite material.
Background
High performance thermal management materials should have high thermal conductivity and low Coefficient of Thermal Expansion (CTE) to maximize heat dissipation and minimize thermal stress and deformation, which are critical issues in microprocessors, power semiconductors, high power laser diodes, light emitting diodes, and microelectromechanical system packages. Thermal stress and warpage are caused by CTE differences, which becomes important in advanced electronic devices because of the high heat generated when using high power laser diodes or high integration ICs, for example. To ensure that these electronic devices have ideal or desired performance and sufficient lifetime, halasz suggests that it is necessary to reduce the junction temperature between the two components to a temperature below 473K (200 ℃) (corresponding to a discrete power semiconductor); 398K (125 ℃) (logic devices for military and automotive); 343K (70 ℃) for some commercial logic devices. In the case of high power density devices, the allowable temperature range of the package base and chip connection thermal resistance is limited. In any event, the development of thermal management materials is of great importance in the electronics field.
The traditional packaging substrate is a Cu-W, alN, beO and Al/SiC composite material, and the thermal conductivity k is close to 200W/m.k. The highest thermal conductivity material is high quality diamond, a naturally occurring material with nitrogen content below 100ppm and thermal conductivity of about 2000W/m.k. Johnson WB, sonuparlak B. And Chen N, pan XF, gu MY two groups prepared highly thermally conductive composites, which used metal infiltration techniques to prepare diamond particle dispersed aluminum based composites. In their studies, the composites were fabricated at a temperature above the melting point of the Al matrix (which melting point is tm=933k, thermal conductivity is k=210W/m·k). The high processing temperatures in these infiltration techniques are believed to have drawbacks, such as reduced thermal conductivity due to structural changes that occur as a result of direct contact of the diamond particles with the molten Al. Furthermore, when using this technique, it is practically difficult to uniformly disperse diamond particles in the composite material. This is especially true when the composite contains a relatively low volume fraction of diamond, for example less than 50% by volume, due to the large difference in mass density between diamond and Al; when the volume ratio of diamond is about 75%, the thermal conductivity can reach more than eight hundred percent, but the tensile strength and the bending strength of the material in the state are reduced, and the processability and the application occasions are limited.
Disclosure of Invention
The invention aims to provide a preparation method of a diamond/aluminum composite material, which can effectively solve the problems of high processing temperature, reduced heat conductivity caused by direct contact of diamond particles and molten Al and uneven dispersion of the diamond particles in the composite material in the preparation of the diamond/aluminum composite material by a metal infiltration technology.
In order to solve the technical problems, the invention adopts the following technical scheme:
a method for preparing a diamond/aluminum composite material, comprising the following steps:
(1) Mixing the ingredients: selecting Ib type artificial diamond micro powder and IMS-15 diamond as filling materials, and selecting pure aluminum powder, al-8mass% Si alloy powder and Si powder as matrix materials; placing the filling powder and the matrix material into a container for swinging and vibrating mixing, then performing ball milling, vacuumizing a ball milling environment, and pouring high-purity argon into the ball milling environment, so as to obtain a powder mixture after ball milling;
(2) Hot pressing and sintering: pressing the powder mixture, and then vacuumizing for hot-pressing sintering; wherein the conditions of hot press sintering are as follows: sintering from room temperature to 480-520 ℃, preserving heat at the temperature for 2-4 minutes, then heating to 590-620 ℃ and preserving heat at the temperature for 1-3 minutes; and (3) closing the heating system under the vacuum state, naturally cooling to below 100 ℃, flushing high-purity nitrogen into the sintering furnace cavity, and opening the cavity after the pressure inside and outside the cavity is equal to the pressure, thus obtaining the diamond/aluminum composite material.
Wherein, the average grain diameter of the Ib type artificial diamond micro powder in the filling material is 300 mu m, and the IMS-15 diamond adopts IMM diamond with the average grain diameter of 30 mu m; the grain size of the pure aluminum powder in the matrix material was 200 mesh, the average grain size of the Al-8mass% Si alloy powder was 60 μm, and the average grain size of the Si powder was 50. Mu.m.
Wherein the amount of pure aluminum powder in the base material is 88 to 90vol%, the amount of Al-8mass% Si alloy powder is 8 to 10vol%, and the amount of Si powder is 2vol%.
Wherein the shape of the Ib type artificial diamond micro powder, the IMS-15 diamond, the pure aluminum and the Al-8mass%Si alloy powder are respectively regular dodecahedron, parallelepipedal, teardrop and spherical.
Wherein the time for mixing the filling powder and the matrix material in a container in a swinging and vibrating way is 1-2 hours, and then the vacuum ball milling tank is vacuumized to 10 -2 Pa postflushBall milling is carried out by high-purity argon, the pressure of the argon is controlled to be 0.2 MPa-0.5 MPa, and the ball milling time is 4-6 hours.
Wherein, the conditions of hot press sintering are: firstly, sintering from room temperature to 502 ℃ at a heating rate of 0.6K/s-0.9K/s, and preserving heat at the temperature for 2-4 minutes; then heating to 612 ℃ at a rate of 0.03K/s-0.07K/s, and preserving heat for 1-3 minutes after reaching the temperature; in addition, visualization of the relative bulk density change of the composite material during the HP process is achieved by monitoring the longitudinal displacement between the punches during sintering.
In order to prepare a high performance thermal management material having ultra-high thermal conductivity and low CTE, the present invention prepares a metal matrix composite with diamond particles dispersed by a Hot Pressing (HP) process. Specifically, an aluminum-based composite material in which diamond particles are dispersed is prepared in a continuous solid-liquid coexisting state by a Hot Pressing (HP) process, and the composite material has a relatively high relative bulk density and good bonding between aluminum and diamond particles. The results showed that at a diamond volume fraction of 50vol%, the thermal conductivity was 583W/mK. In an embodiment, a bimodal diamond particle composite material is selected and a percentage of aluminum silicon powder, pure silicon powder, is added in order to achieve a continuous solid-liquid coexisting state below the melting point temperature of aluminum during Hot Pressing (HP) and to form a discrete aluminum/silicon carbide/diamond interface that achieves minimal thermal resistance.
According to the invention, by improving the diamond/aluminum interface components and the structure, low interface thermal resistance is obtained, and the diamond/aluminum composite material with the thermal conductivity more than 520W/m.K can be obtained in a low component ratio state that the diamond volume ratio is about 50%; the maximum tensile strength (UTS) of the diamond/aluminum composite material can reach 350MPa; a Coefficient of Thermal Expansion (CTE) of less than 10/K; the volume ratio of diamond can be continuously adjusted within the range of 50-74% to obtain diamond/aluminum composite materials with different components matched with the thermal expansion Coefficient (CTE) of the contact surface of the power device; the lower hot press sintering temperature (about 600K) avoids damaging the thermal property of the diamond micro powder.
Drawings
FIG. 1 is a schematic diagram of a diamond/aluminum composite interface structure;
FIG. 2 is a schematic view of HP hot press sintering device and microstructure of synthetic material;
FIG. 3 is an aluminum-silicon alloy phase diagram;
FIG. 4 is a schematic diagram of a through-wafer break;
figure 5 is an XRD characterization result of the diamond/aluminum composite material.
Detailed Description
The present invention will be specifically described with reference to examples below in order to make the objects and advantages of the present invention more apparent. It should be understood that the following text is intended to describe only one or more specific embodiments of the invention and does not limit the scope of the invention strictly as claimed.
According to the three-dimensional euclidean space, if the diamond particles are spherical and uniform in size, the maximum volume fraction of diamond particles in the aluminum-based composite is desirably about 74vol%. Because of some experimental limitations, aluminum-based composites typically contain about 50vol% diamond when using diamond particles of substantially a single size.
In the present invention, two sizes of type Ib artificial diamond micropowder (average particle diameter of about 300 μm) and IMS-15 diamond (IMM diamond having average particle diameter of about 30 μm) were used as heat conduction reinforcing filler, and the thermal conductivity of the selected synthetic diamond micropowder was about 1800W/m·k. Two kinds of metal powder and one kind of non-metal powder were used as the base material, and pure aluminum (Al) powder (200 mesh), al-8mass% Si alloy powder (60 μm) and Si powder (50 μm) having a purity of 99.9% were used. The large diamond, the small diamond, the pure Al and the Al-8mass% Si alloy powder used in the present invention have the shape of a regular dodecahedron, a parallel octahedron, a teardrop and a sphere, respectively.
In the present invention, the aluminum-silicon alloy powder is important for generating two phases of aluminum (solid phase) and aluminum-silicon (liquid phase) coexisting in a short time during Hot Pressing (HP) process sintering. The present invention exploits a unique HP manufacturing technique that can manufacture metal matrix composites with or without dispersed diamond particles. The characteristic is that the use of Al-Si alloy eutectic temperature below the melting point of aluminum creates a quasi-continuous solid-liquid coexistence state of the metal powder mixture during HP process. In addition, the micro-silicon powder is added to form part of the diamond interface of aluminum/silicon carbide (/ beta-silicon carbide, cubic structure, with higher unit surface area than alpha type) to reduce the grain boundary thermal resistance.
It should be noted that since the thermal conductivity of the Al-8mass% Si alloy powder is low (140W/mK), and since it is necessary to avoid a sharp decrease in the thermal conductivity of the Al matrix, an Al-based powder mixture composed of 88 to 90vol% pure Al powder, 8 to 10vol% Al-8mass% Si alloy powder and 2vol% Si powder is selected as the matrix material in the present invention. The silicon micropowder is filled mainly in consideration of poor wettability between aluminum and diamond, even under the high-temperature condition, the wettability of aluminum to diamond is still poor, and the interface pattern shown in the b of fig. 1 is formed by filling a small amount of silicon micropowder, so that the tensile strength of the composite material is enhanced, and the interface thermal resistance between diamond and aluminum is reduced. In bimodal diamond particle mixtures, the mixing ratio of the large and small diamond particles is important to achieve a high bulk density of the diamond particle containing aluminum matrix composite. The theory of geometric random packing and void fraction of polydisperse particles suggests that bimodal packing can be converted to a continuous particle size distribution of the power law type. It follows that when the exponentially distributed modulus of the power law function is zero, the maximum packing fraction of particles can be obtained, that is, the cumulative fine particle size is a logarithmic function of the particle size. For maximum geometric packing consisting of sieve grade or discrete size particles, the distribution modulus is positive, typically 0 to 0.37. In the present invention, the optimum mixing ratio is determined as follows. When the bimodal powder mixture is placed in a container and tapped, the Furnas model can be used to evaluate the porosity of the bimodal powder mixture as described in the present invention.
Assuming that (a) the large particles are much larger in diameter than the small particles, (b) the mass density of the large particles is equal to that of the small particles, and (c) the small particles fill the gaps between the large particles, the porosity ε of the bimodal powder mixture can be calculated by the following formula:
wherein ε is 1 Is the porosity, v, of the large particles when packed into a container 1 Is the volume fraction of large particles in a bimodal powder mixture consisting of large particles and small particles;
when the volume fraction of large diamond particles in the bimodal diamond powder is 75%, the porosity of the bimodal diamond powder is minimal, 12.5%. In this example, a high relative bulk density of the diamond-containing aluminum-based composite material can be achieved using a bimodal diamond powder mixture consisting of 75vol% large diamond particles and 25vol% small diamond particles. The relative bulk density is defined as the ratio of experimentally measured material density to material density assuming no porosity.
The preparation method comprises the following steps:
1) Alloy mixing is carried out through a ball mill. The type Ib artificial diamond micropowder (namely, the average grain diameter is about 300 mu m) and the IMS-15 diamond (IMM diamond with the average grain diameter of about 30 mu m) are selected as heat conduction reinforcing filling materials, and the heat conductivity of the selected synthetic diamond micropowder is about 1800W/m.K. Two kinds of metal powder and one kind of non-metal powder were used as the base material, and pure aluminum (Al) powder (200 mesh), al-8mass% Si alloy powder (60 μm) and Si powder (50 μm) having a purity of 99.9% were used. The large diamond, the small diamond, the pure Al and the Al-8mass% Si alloy powder used in the present invention have the shape of a regular dodecahedron, a parallel octahedron, a teardrop and a sphere, respectively. Placing the powder according to the stoichiometric ratio into a related container, shaking and mixing for 1-2 hours, then placing into a vacuum ball milling tank, and vacuumizing to 10 -2 And (3) after Pa, high-purity argon is filled, the argon pressure is controlled to be 0.2-0.5 MPa, and then a ball milling tank is fixed on a station of a planetary ball mill for ball milling for 4-6 hours.
2) Hot pressing and sintering: first, a lower punch is inserted into a die from one end thereof, and then a powder mixture containing diamond particles is poured. Then, the upper punch was placed on the powder mixture. The powder mixture is pressed by an upper punch and a lower punch under the pressure of 60MPa to 80MPa, and then is sintered by hot pressing after being vacuumized to 1.5 Pa. Firstly sintering from room temperature to 775K at a heating rate of 0.6K/s-0.9K/s, preserving heat at the temperature for 2-4 minutes, then heating to 885K at a heating rate of 0.03K/s-0.07K/s, preserving heat for 1-3 minutes after reaching the temperature, and realizing the change of the relative bulk density of the composite material in the visual HP process by monitoring the longitudinal displacement between the punches in the sintering process. At the same time, the process parameters are set based on ensuring the formation of beta-cubic silicon carbide in the composite material phase and the absence of aluminum carbide phase (fig. 5). And (3) closing the heating system under the vacuum state, naturally cooling to below 100 ℃, flushing high-purity nitrogen into the sintering furnace cavity, and opening the cavity for sampling after the pressure inside and outside the cavity is equal.
In the embodiment, the diamond-containing aluminum-based composite material disc is subjected to gold plating, and the German relaxation resistance LFA467 thermal constant analyzer is adopted to measure the thermal diffusivity by a laser flash technology; bulk density of the fabricated composite discs was measured using archimedes method; measuring the heat capacity of the composite material by DSC; the coefficient of thermal expansion was measured using a German relaxation-resistant DIL 402Expedis Classic thermal expansion instrument. As can be seen from the characterization results of FIG. 5, aluminum has a face-centered cubic structure, a lattice constant of about 0.4049nm, a beta-cubic silicon carbide lattice constant of 0.4359nm, and a spectrum clearly shows the beta-cubic silicon carbide phase, and no aluminum carbide phase is present. The diamond/aluminum composite material of the present example has a thermal conductivity of 520W/mK or higher, a tensile strength (UTS) of 350MPa or higher, and a Coefficient of Thermal Expansion (CTE) of 10/K or lower in a low-component-ratio state in which the diamond volume ratio is about 50%.
The thermal conductivity of the diamond/aluminum composite material changes along with the change of the interface layer thickness, and as the thickness of the SiC interface layer increases, the thermal conductivity of the diamond/aluminum composite material increases and then decreases, and the relationship between the thermal conductivity of the diamond/aluminum composite material and the interface layer thickness can be explained by the following reasons:
the addition of low silicon will result in direct contact between the diamond and the aluminum, forming a discontinuous interface. Defects or voids at the interface increase the interfacial thermal resistance and significantly reduce the thermal conductivity of the diamond/aluminum composite. As the thickness of the interfacial layer increases to a certain thickness coverage, there is little exposed surface on the diamond (approximately alternating arrangement of aluminum and silicon carbide). The interface layer connects the diamond to the substrate. As SiC interface layers continue to increase, the thermal conductivity of diamond/aluminum composites begins to decrease. This can be explained by the low intrinsic thermal conductivity of SiC relative to diamond, and the increase in interface layer thickness increases the interface thermal resistance. Therefore, in designing a low thermal resistance interface, the interface layer thickness should be considered as the minimum thickness when the diamond surface is free of bare defects.
The proportion of the metal matrix powder components firstly ensures that a solid-liquid mixed state with a certain proportion can be generated below the melting point of aluminum, but forms a beta-cubic silicon carbide structural layer which is approximately uniformly distributed and equally spaced on the surface of the diamond micro powder so as to reduce interface thermal resistance and enhance the tensile strength of the composite material. Specifically, the reduction in thermal resistance is based on the following mechanism:
the interfacial thermal resistance for a complete aluminum-diamond interface can be illustrated by the following analytical formula:
aluminum-diamond interface
Aluminum-silicon carbide-diamond interface
The material interfaces formed in this embodiment are an alternating arrangement of the two interfaces described above. For the interface formed by the alternation of the aluminum-diamond interface and the aluminum-silicon carbide-diamond interface, the total thermal resistance is obtained by connecting the two thermal resistances in parallel, and the total thermal resistance is smaller than that of any interface.
Description of tensile strength enhancement of diamond/aluminum composite material in this example: the thermal expansion coefficient of aluminum is about 23.2/K, the thermal expansion coefficient of diamond is 1.2-4.5/K, the large stress is caused by large difference, the tensile strength of the material is greatly reduced, the thermal expansion coefficient of beta-silicon carbide corresponds to the operating temperature point of a power device to be about 6.6/K, meanwhile, the interface area of aluminum-silicon carbide is increased relative to the interface area of aluminum-diamond due to the formation of a silicon carbide interface layer, so that stress relaxation is facilitated, and the total unit solid angle binding force is increased.
The diamond reinforced metal matrix composite has three main fracture modes: when the interfacial bond strength is weak, cracks tend to initiate and propagate at the interface, resulting in interface debonding. Bare smooth diamond surfaces were observed in the fractured tissue. As the interfacial bond strength increases, crack propagation resistance increases. Cracks tend to fracture at the sides of the substrate. In the broken structure, adhesion of the metal to the diamond surface can be observed. The interface bonding strength is further improved, and the diamond particles undergo crystal-through fracture due to the existence of stress concentration in the process of crack propagation (after dislocation in the crystal grains is sharply increased, roughness and resident slip bands are greatly formed, the strength of the crystal grains is reduced, and cracks are easy to initiate from the inside of the crystal grains to become crystal-through fracture. Impact of diamond particle size (50-500 μm) on microstructure, flexural strength, density, fracture toughness and thermal conductivity of diamond/SiC composites. The thermal conductivity of the composite material can be improved by using large-sized diamond particles, but as the particle size of the diamond increases, the density of the diamond/SiC composite material increases, the mechanical properties of the composite material are reduced, and the fracture mechanism of the composite material is changed into interfacial debonding by the crystal-through fracture of the diamond particles.
The prior art describes that forming SiC on the diamond surface effectively enhances the adhesion and thermal conductivity of the diamond/aluminum interface. In this example, the optimal processing temperature and pressure to form SiC on diamond is given for application to the diamond/Al composite coating of SiC coating to improve interfacial adhesion and thermal conductivity. The treatment temperature has a great influence on the formation of SiC on the diamond surface, and the coverage of the SiC coating on the diamond increases with increasing treatment temperature.
In metal matrix composites, the transfer of operating stresses from the matrix to the reinforcement is largely dependent on the interface structure and strength between the ceramic reinforcement and the matrix.
The invention aims to provide the effect result of interface structure and strength on SiC particle reinforced aluminum 6061 metal matrix composite material fracture behavior. Interface variation is obtained by adding as-received or heat-treated SiC particles to a melt region where solid and liquid coexist. Heat treating the particles achieves good wettability of the particles with the liquid metal alloy and a uniform distribution of SiC particles, whereas agglomeration of the particles is observed for composites produced from the received particles. SEM observations of the fracture surface showed that both particle fracture and debonding occurred at the stronger reinforcement/matrix interface, but only particle debonding occurred at the weaker interface with little change in ductility. These observations are consistent with the fracture mechanism in which the interface structure and strength between the matrix and reinforcement play a dominant role in determining the fracture behavior of the particle-reinforced metal-matrix composite.
While the embodiments of the present invention have been described in detail with reference to the drawings, the present invention is not limited to the above embodiments, and it will be apparent to those skilled in the art that various equivalent changes and substitutions can be made therein without departing from the principles of the present invention, and such equivalent changes and substitutions should also be considered to be within the scope of the present invention.
Claims (6)
1. A method for preparing a diamond/aluminum composite material, which is characterized by comprising the following steps:
(1) Mixing the ingredients: selecting Ib type artificial diamond micro powder and IMS-15 diamond as filling materials, and selecting pure aluminum powder, al-8mass% Si alloy powder and Si powder as matrix materials, wherein the dosage of the pure aluminum powder in the matrix materials is 88-90 vol%, the dosage of the Al-8mass% Si alloy powder is 8-10 vol%, and the dosage of the Si powder is 2vol%; placing the filling material and the matrix material into a container for swinging and vibrating mixing, then performing ball milling, vacuumizing a ball milling environment, and pouring high-purity argon into the ball milling environment, so as to obtain a powder mixture after ball milling;
(2) Hot pressing and sintering: pressing the powder mixture, and then vacuumizing for hot-pressing sintering; wherein the conditions of hot press sintering are as follows: sintering from room temperature to 480-520 ℃, preserving heat at the room temperature for 2-4 minutes, then heating to 590-620 ℃, and preserving heat at the room temperature for 1-3 minutes; and (3) closing the heating system under the vacuum state, naturally cooling to below 100 ℃, flushing high-purity nitrogen into the sintering furnace cavity, and opening the cavity after the pressure inside and outside the cavity is equal to the pressure, thus obtaining the diamond/aluminum composite material.
2. The method of preparing a diamond/aluminum composite material according to claim 1, wherein: the average grain diameter of the Ib type artificial diamond micro powder in the filling material is 300 mu m, and IMM diamond with the average grain diameter of 30 mu m is selected as IMS-15 diamond; the grain size of the pure aluminum powder in the base material was 200 mesh, the average grain size of the Al-8mass% Si alloy powder was 60 μm, and the average grain size of the Si powder was 50. Mu.m.
3. The method of preparing a diamond/aluminum composite material according to claim 1, wherein: the shape of the Ib type artificial diamond micro powder, the IMS-15 diamond, the pure aluminum and the Al-8mass% Si alloy powder are respectively regular dodecahedron, parallelepipedal, teardrop and spherical.
4. The method of preparing a diamond/aluminum composite material according to claim 1, wherein: the filling material and the matrix material are mixed in a container in a swinging and vibrating way for 1-2 hours, and then vacuumized to 10 in a vacuum ball milling tank -2 And (3) after Pa, high-purity argon is filled for ball milling, wherein the argon pressure is controlled to be 0.2-0.5 MPa, and the ball milling time is 4-6 hours.
5. The method of preparing a diamond/aluminum composite material according to claim 1, wherein the hot press sintering conditions are: firstly, sintering from room temperature to 502 ℃ at a heating rate of 0.6K/s-0.9K/s, and preserving heat at the temperature for 2-4 minutes; then heating to 612 ℃ at a rate of 0.03K/s-0.07K/s, and preserving heat for 1-3 minutes after reaching the temperature.
6. The method of preparing a diamond/aluminum composite material according to claim 5, wherein: the relative bulk density of the composite material during the HP process was visualized by monitoring the longitudinal displacement between the punches during sintering.
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| CN101728279A (en) * | 2009-11-27 | 2010-06-09 | 北京科技大学 | Preparation method of high-performance diamond reinforced Al-matrix electronic packaging composite material |
| CN102534331A (en) * | 2012-01-10 | 2012-07-04 | 上海交通大学 | Method for preparing high conductivity diamond/aluminum composite material |
| CN111730054A (en) * | 2020-06-30 | 2020-10-02 | 湖南大学 | Low-temperature synthesis method and application of silicon carbide coated diamond composite powder |
| CN114086016A (en) * | 2021-11-05 | 2022-02-25 | 长飞光纤光缆股份有限公司 | Aluminum-based diamond composite material with high finish and preparation method thereof |
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| CN101728279A (en) * | 2009-11-27 | 2010-06-09 | 北京科技大学 | Preparation method of high-performance diamond reinforced Al-matrix electronic packaging composite material |
| CN102534331A (en) * | 2012-01-10 | 2012-07-04 | 上海交通大学 | Method for preparing high conductivity diamond/aluminum composite material |
| CN111730054A (en) * | 2020-06-30 | 2020-10-02 | 湖南大学 | Low-temperature synthesis method and application of silicon carbide coated diamond composite powder |
| CN114086016A (en) * | 2021-11-05 | 2022-02-25 | 长飞光纤光缆股份有限公司 | Aluminum-based diamond composite material with high finish and preparation method thereof |
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