A high thermal conductivity aluminum-based composite material with adjustable thermal expansion coefficient and preparation method thereof
Through the hybrid reinforcement design of negative thermal expansion reinforcements and high thermal conductivity reinforcements, combined with solid-phase sintering technology, precise control of the volume fraction of reinforcements in aluminum-based composite materials is achieved, and high thermal conductivity aluminum-based composite materials with adjustable thermal expansion coefficient are prepared. This solves the problem of difficult precise control of the volume fraction of reinforcements in existing technologies, and obtains materials with excellent comprehensive performance.
Patent Information
- Application Number
- CN202411193673.3
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2024-08-28
- Publication Date
- 2025-09-23
- Estimated Expiration
- 2044-08-28
AI Technical Summary
It is difficult to achieve precise control of the volume fraction of reinforcements in the preparation process of existing aluminum-based composites, especially in mixed reinforcement composites with low expansion coefficient and high thermal conductivity. The liquid phase infiltration method is difficult to achieve precise control of low volume fractions, and there is little research on the solid phase sintering process, which cannot meet the requirements of comprehensive performance.
A hybrid reinforcement design of negative thermal expansion reinforcements and high thermal conductivity reinforcements is adopted. Through solid-phase sintering technology, the volume fraction of the reinforcements is regulated to prepare a high thermal conductivity aluminum-based composite material with adjustable thermal expansion coefficient. The total volume content of the negative thermal expansion reinforcements and the high thermal conductivity reinforcements is 10~70vol.%, of which the negative thermal expansion reinforcements are 5~65vol.%, the high thermal conductivity reinforcements are 5~65vol.%, and the balance is aluminum matrix. The solid-phase sintering method is carried out in vacuum or protective atmosphere to control the volume fraction of the reinforcements and the interface reaction.
The precise control of the volume fraction of the reinforcement in aluminum-based composite materials with low thermal conductivity and high thermal conductivity is achieved, and a composite material with excellent comprehensive performance is obtained, which solves the problem in the existing technology that it is difficult to achieve both high thermal conductivity and low thermal conductivity. The method is simple, fast and easy to apply in engineering.
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Abstract
Description
Technical Field
[0001] The invention relates to a high-thermal-conductivity aluminum-based composite material with an adjustable thermal expansion coefficient and a preparation method thereof, and belongs to the technical field of composite materials. Background Art
[0002] With the advent of the 5G era and the continuous advancement of microelectronics technology, electronic devices are rapidly developing towards high integration, high power, and lightweight, placing higher demands on the overall performance of electronic packaging materials. Research on materials that match the thermal expansion coefficient of semiconductor components while exhibiting high thermal conductivity, low density, and good mechanical properties is becoming increasingly widespread.
[0003] Currently, fourth-generation electronic packaging materials, such as Si / Al and SiC / Al aluminum-based composites, boast low thermal expansion coefficients, high thermal conductivity, low density, and excellent mechanical properties, finding widespread application in electronic packaging, aerospace, and rail transportation. However, to match semiconductor materials like Si and GaAs, the Si or SiC reinforcement content in Si / Al and SiC / Al aluminum-based composites must be as high as 70 vol.% or higher to meet the low thermal expansion coefficient requirement. However, this high ceramic content results in virtually no plasticity in the composite material as a whole, leading to increased brittleness, difficulty in processing, and poor welding performance.
[0004] Compared to low thermal expansion materials like Si or SiC, the discovery of negative thermal expansion materials offers a solution for manipulating the thermal expansion coefficient of composite materials from negative to positive over a wide temperature range. However, due to their extremely low intrinsic thermal conductivity, the use of AM2O8-based negative thermal expansion materials alone in composite materials can easily result in low overall thermal conductivity.
[0005] To address these issues, hybrid reinforcement is an effective approach for designing and preparing aluminum-based composites with low thermal expansion coefficients and high thermal conductivity. It can leverage the properties of different reinforcements to achieve composites with excellent overall performance. Currently, the main challenges in preparing aluminum-based composites hybridly reinforced with negative thermal expansion reinforcements and other reinforcements are as follows: 1) Most existing hybrid aluminum-based composites hybridized with negative thermal expansion reinforcements and other reinforcements are prepared using liquid-phase infiltration, which makes it difficult to prepare composites with low volume fractions (e.g., less than 30-40 vol.%) and precisely control the volume fraction. For example, patent document CN114231783B successfully achieves improved composite strength while maintaining low thermal expansion properties by co-introducing high-strength ceramic particles and ZrW2O8 particles into an aluminum matrix. However, this patent indicates that the liquid-phase infiltration method is only suitable for preparing hybrid-reinforced composites with high volume fractions (above 60 vol.%) of reinforcements. Patent document CN110846597B proposes a silicon carbide nanowire hybrid reinforced zirconium tungstate / aluminum composite material and its preparation method. Zirconium tungstate particles and silicon carbide nanowires are evenly mixed, and then the composite material is prepared by pressure infiltration (liquid phase infiltration). The thermal expansion coefficient of the prepared silicon carbide nanowire hybrid reinforced zirconium tungstate / aluminum composite material can reach a minimum of 2×10 -6 K -1 , and the mechanical properties of the composite materials prepared compared to single zirconium tungstate are improved, solving the problem of poor mechanical properties of existing zirconium tungstate / aluminum composite materials. The volume fraction of the zirconium tungstate reinforcements reinforced by silicon carbide nanowires reaches 30-60%. As can be seen from the above two patents, the volume fraction of the reinforcements in the liquid phase infiltration process cannot be lower than 30%, and it cannot get rid of the inherent process defects of liquid phase infiltration, such as the difficulty in accurately controlling the volume fraction. In addition, both patents are based on hybrid reinforcement designs made to improve the strength of the composite materials, rather than hybrid reinforcement designs based on the comprehensive thermophysical properties of the composite materials. 2) Compared with liquid phase infiltration or pressure infiltration, the use of solid phase sintering for low expansion aluminum-based composite materials is more conducive to controlling the low volume fraction and accuracy of the reinforcements. However, there are currently few research reports on the solid phase sintering process of low expansion aluminum-based composite materials, which cannot meet the technical requirements. For example, patent documents CN105886823A and CN115870504A both use spark plasma sintering to prepare zirconium tungstate / aluminum composite materials, but only focus on the sintering of a single zirconium tungstate negative thermal expansion reinforcement and an aluminum-based composite material, and the volume fraction of the zirconium tungstate reinforcement is above 50 vol.%. There are no reports on the solid-phase sintering of aluminum-based composite materials with low volume fraction and / or negative thermal expansion reinforcements and other reinforcements.
[0006] Therefore, when using a variety of reinforcements to prepare aluminum-based composite materials with low expansion coefficient and high thermal conductivity, how to achieve precise control of the reinforcement volume fraction from low to high becomes a technical problem that needs to be solved. Summary of the Invention
[0007] The present invention aims to achieve precise control of the volume fraction of reinforcements from low to high when using multiple reinforcements to prepare aluminum-based composite materials with low thermal expansion coefficient and high thermal conductivity, and proposes a high thermal conductivity aluminum-based composite material with adjustable thermal expansion coefficient and a preparation method.
[0008] The present invention provides a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient, comprising: a negative thermal expansion reinforcement, a high thermal conductivity reinforcement, and an aluminum matrix, wherein the total volume content of the negative thermal expansion reinforcement and the high thermal conductivity reinforcement is 10 to 70 vol.%, wherein the volume content of the negative thermal expansion reinforcement is 5 to 65 vol.%, the volume content of the high thermal conductivity reinforcement is 5 to 65 vol.%, and the balance is the aluminum matrix;
[0009] The negative thermal expansion reinforcement is one or a combination of two or more ceramic materials, intermetallic compounds, and alloys whose average linear expansion coefficient or volume expansion coefficient is negative at t°C, -100°C < t < 300°C; the high thermal conductivity reinforcement is one or a combination of two or more inorganic non-metallic materials whose thermal conductivity is higher than that of the aluminum matrix; the aluminum matrix is one or a combination of two or more aluminum alloys or pure aluminum with an aluminum mass percentage of more than 50wt%, and the purity of the pure aluminum is more than 99.0wt%.
[0010] Optionally, the ceramic material is selected from at least one of the following chemical formulas: chemical formula aα2O8, wherein a represents one or more chemical elements of Zr, Hf, Sn, Ti, Eu, Er, and Yb, and α represents one or more chemical elements of W, Mo, and V; chemical formula bβ2O7, wherein b represents one or more chemical elements of Zr, Th, and Ce, and β represents one or more chemical elements of P, Mo, and V; chemical formula c2γ3O 12 , where c represents one or more of the chemical elements Sc, Dy, Y, Er, Yb, and Lu, and γ represents one or more of the chemical elements W and Mo; the chemical formula is dδO5, where d represents one or more of the chemical elements Nb and Ta, and δ represents one or more of the chemical elements V and P; the chemical formula is eε2P3O 12, where e represents one or more of the chemical elements Na, K, Nb, Rb, and Cs, and ε represents one or more of the chemical elements Zr, Ti, and Hf; chemical formula f2ζ2O7, where f represents one or more of the chemical elements Cu, Mn, Fe, Co, Ni, Mg, and Zn, and ζ represents one or more of the chemical elements P and V; chemical formula g2O(PO4)2, where g represents one or more of the chemical elements U and Th; chemical formula hθF6, where h represents one or more of the chemical elements Ca, Mn, Fe, Zn, Co, Ni, Mg, Yb, and Ti, and θ represents one or more of the chemical elements Zr, Hf, and Nb; chemical formula i(CN)2, where i represents one or more of the chemical elements Zn and Cd; chemical formula j B(CN)4, where j represents one or more of the chemical elements Cu and Ag; chemical formula kτ(CN)6, where k represents one or more of the chemical elements Y, Fe, Ga, Sc, Ti, La, Sm, Ho, Lu, Er, Cs, Rb, Cd, Mn, Co, Ni, and Zn, and τ represents one or more of the chemical elements Fe, Co, Pt, Cd, Ni, Cu, and Zn; chemical formula Mn3lN, where l represents one or more of Zn, Cu, Ga, Sn, Ge, Si, Ge, and Fe, and compounds formed by partial replacement of Mn in the chemical formula Mn3lN by any one or two of V, Cr, Fe, Co, Ni, Cu, and Zn; Zn[Ag(CN)2]2, CaZr4P6O 24 , Si(NCN)2, ReO3, SiO2, Cu2O, Ag2O, ScF3;
[0011] The intermetallic compound is selected from at least one of the following chemical formulas: Zr y Nb 1-y Fe2、Hf y Nb 1-y Fe2、Hf 1- y Ta y Fe2、Sc 1-y Ti y Fe2、CrTe y Se 1-y 、LaFe 13-x Si x 、LaFe 13-x Al x , Mn3Ge, Mn-Co-Ge series, Fe-Mn-Ga series, Ni-Mn-Ga series, RCo2, R2Fe 14 B. R2Fe 17 、RCo3、RFe 12 、R3Fe 29, in the chemical formula, y is any value from 0 to 1, x is any value from 0 to 13, and R is one or more rare earth elements; and an intermetallic compound formed by partial substitution of the Fe, Co, or Mn positions in the above chemical formula by any one or two elements selected from Si, Al, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Hf, and Ta;
[0012] The alloy is selected from at least one of the following element combinations: Fe-Ni, Fe-Pt, Cr-Fe, Ni-Ti, Ti-Nb.
[0013] Optionally, the inorganic non-metallic material is selected from at least one of SiC, Si3N4, AlN, graphite, carbon fiber, graphene, and diamond.
[0014] Optionally, the aluminum alloy is selected from at least one of Al-Si alloy, Al-Cu alloy, Al-Mg alloy, Al-Zn alloy, and Al-Mn alloy.
[0015] The present invention also provides a method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient, comprising the following steps:
[0016] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0017] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0018] Step S3: put the composite powder of step S2 into a sintering mold and move it into a furnace, adjust the furnace environment, keep it warm or keep it warm and pressurize it for solid phase sintering, cool it with the furnace, and take it out at room temperature to obtain an aluminum-based composite material.
[0019] Optionally, in step S1, the negative thermal expansion reinforcement powder is one or a combination of two or more of a ceramic powder, an intermetallic compound powder, and an alloy powder, whose average linear expansion coefficient or volume expansion coefficient is negative at t°C, -100°C < t < 300°C, and the average particle size of the negative thermal expansion reinforcement powder is 0.1-500 μm;
[0020] The high thermal conductivity reinforcement powder is one or a combination of two or more inorganic non-metallic powders having a thermal conductivity higher than that of the aluminum matrix, and the average particle size of the high thermal conductivity reinforcement powder is 0.1 to 500 μm;
[0021] The aluminum matrix powder is one or a combination of two or more of aluminum alloy powder or pure aluminum powder with an aluminum mass percentage of more than 50wt%, the purity of pure aluminum is more than 99.0wt%, and the average particle size of the aluminum matrix powder is 0.1~500μm.
[0022] Optionally, in step S3, solid phase sintering is performed in any one of a vacuum sintering furnace, an atmosphere sintering furnace, a hot pressing sintering furnace, a hot isostatic pressing furnace or a spark plasma sintering furnace.
[0023] Optionally, in vacuum sintering furnace, atmosphere sintering furnace, hot pressing sintering furnace, hot isostatic pressing furnace, the furnace environment is 1×10 -2 ~50Pa vacuum environment or pressure of 1~1×10 3 A protective gas among nitrogen, argon and helium with a sintering temperature of 0.15 MPa is used. The sintering mold used is a cylindrical graphite or steel mold, which is axially compressible. The inner diameter of the sintering mold is 6 to 300 mm. The pressure applied during the sintering process is 0 to 200 MPa, the temperature is 400 to 720 ° C, and the holding time is 30 to 120 min.
[0024] Optionally, in a spark plasma sintering furnace, the furnace environment is 1×10 -4 A vacuum environment of ~100Pa or a pressure of 10~1×10 3 A protective gas among nitrogen, argon and helium with a sintering temperature of 10000 Pa. The sintering mold used is a cylindrical graphite or steel mold, which is axially compressible. The inner diameter of the sintering mold is 6 to 150 mm. The pressure applied during the sintering process is 30 to 200 MPa, the temperature is 400 to 640 ° C, and the holding time is 5 to 100 min.
[0025] Optionally, in a spark plasma sintering furnace, a pressure of 70-200 MPa, a temperature of 400-470° C., and a holding time of 10-100 min are applied during the sintering process.
[0026] Compared with the prior art, the advantages of the present invention are:
[0027] 1. The advantage of the present invention is that it uses a negative thermal expansion reinforcement and a high thermal conductivity reinforcement to jointly reinforce the aluminum-based composite material. Compared with a composite material prepared with a single negative thermal expansion reinforcement, the material of the present invention maintains a low thermal expansion coefficient while having high thermal conductivity, and has better overall performance.
[0028] 2. Compared with the aluminum matrix reinforced with a single high thermal conductivity or negative thermal expansion ceramic reinforcement, the present invention can achieve full play of the high thermal conductivity, low density and other characteristics of the aluminum matrix under the premise of relatively low total reinforcement content through the synergistic effect of two reinforcements with different properties, thereby obtaining a composite material with better performance.
[0029] 3. The present invention adopts solid phase sintering technology, which avoids interfacial reaction by regulating the sintering process and obtains a denser composite material, and more accurately controls the volume fraction.
[0030] 4. The present invention provides a hybrid reinforced aluminum-based composite material with high thermal conductivity and adjustable thermal expansion coefficient and a preparation method thereof. The method is simple, fast, highly operational, and easy to implement in engineering applications, solving the problem that existing electronic packaging materials are difficult to maintain low thermal expansion and high thermal conductivity. BRIEF DESCRIPTION OF THE DRAWINGS
[0031] In order to more clearly illustrate the technical solutions in the embodiments of the present invention, the following briefly introduces the drawings required for use in the description of the embodiments. Obviously, the drawings described below are only some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on these drawings without creative work.
[0032] Figure 1 This is the microstructure diagram of the aluminum-based composite material of Example 4;
[0033] Figure 2 is a thermal expansion curve diagram of the Al-Si alloy and aluminum-based composite material of Example 4;
[0034] In the figure, 1 is the high thermal conductivity reinforcement SiC; 2 is the negative thermal expansion reinforcement ZrW2O8; and 3 is the Al-Si alloy matrix. DETAILED DESCRIPTION
[0035] In order to make the invention purpose, technical solution and beneficial technical effect of the present invention clearer, the present invention is described in detail below with reference to specific embodiments. It should be understood that the embodiments described in this specification are only for explaining the present invention and are not intended to limit the present invention.
[0036] The present invention provides a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient. The material has a low expansion coefficient and high thermal conductivity, and includes a negative thermal expansion reinforcement, a high thermal conductivity reinforcement and an aluminum matrix. The total volume content of the negative thermal expansion reinforcement and the high thermal conductivity reinforcement is 10-70 vol.%, of which the volume content of the negative expansion reinforcement is 5-65 vol.%, the volume content of the high thermal conductivity reinforcement is 5-65 vol.%, and the balance is the aluminum matrix.
[0037] The negative thermal expansion reinforcement is one or a combination of two or more of a ceramic material, an intermetallic compound, and an alloy whose average linear expansion coefficient or volume expansion coefficient is negative at t°C, -100°C < t < 300°C.
[0038] Specifically, the negative thermal expansion reinforcement is selected from: (1) ceramic materials: chemical formula aα2O8, wherein a represents one or more chemical elements of Zr, Hf, Sn, Ti, Eu, Er, Yb, and α represents one or more chemical elements of W, Mo, and V; chemical formula bβ2O7, wherein b represents one or more chemical elements of Zr, Th, and Ce, and β represents one or more chemical elements of P, Mo, and V; chemical formula c2γ3O 12 , where c represents one or more of the chemical elements Sc, Dy, Y, Er, Yb, and Lu, and γ represents one or more of the chemical elements W and Mo; the chemical formula is dδO5, where d represents one or more of the chemical elements Nb and Ta, and δ represents one or more of the chemical elements V and P; the chemical formula is eε2P3O 12 , where e represents one or more of the chemical elements Na, K, Nb, Rb, and Cs, and ε represents one or more of the chemical elements Zr, Ti, and Hf; chemical formula f2ζ2O7, where f represents one or more of the chemical elements Cu, Mn, Fe, Co, Ni, Mg, and Zn, and ζ represents one or more of the chemical elements P and V; chemical formula g2O(PO4)2, where g represents one or more of the chemical elements U and Th; chemical formula hθF6, where h represents one or more of the chemical elements Ca, Mn, Fe, Zn, Co, Ni, Mg, Yb, and Ti, and θ represents one or more of the chemical elements Zr, Hf, and Nb; chemical formula i(CN)2, where i represents one or more of the chemical elements Zn and Cd; chemical formula j B(CN)4, where j represents one or more of the chemical elements Cu and Ag; chemical formula kτ(CN)6, where k represents one or more of the chemical elements Y, Fe, Ga, Sc, Ti, La, Sm, Ho, Lu, Er, Cs, Rb, Cd, Mn, Co, Ni, and Zn, and τ represents one or more of the chemical elements Fe, Co, Pt, Cd, Ni, Cu, and Zn; chemical formula Mn3lN, where l represents one or more of Zn, Cu, Ga, Sn, Ge, Si, Ge, and Fe, and compounds formed by partial replacement of Mn in the chemical formula Mn3lN by any one or two of V, Cr, Fe, Co, Ni, Cu, and Zn; Zn[Ag(CN)2]2, CaZr4P6O 24 , Si(NCN)2, ReO3, SiO2, Cu2O, Ag2O, ScF3, ZrW2O8, ZrMo2O8, ZrV2O8, Cu2P2O7, Cu2V2O7, etc.
[0039] (2) Intermetallic compound selected from: Zr y Nb 1-y Fe2、Hf y Nb1-y Fe2、Hf 1-y Ta y Fe2、Sc 1-y Ti y Fe2、CrTe y Se 1-y 、LaFe 13-x Si x 、LaFe 13-x Al x , Mn3Ge, Mn-Co-Ge series, Fe-Mn-Ga series, Ni-Mn-Ga series, RCo2, R2Fe 14 B. R2Fe 17 、RCo3、RFe 12 、R3Fe 29 etc., wherein y is any value from 0 to 1, x is any value from 0 to 13, and R is one or more rare earth elements, such as rare earth elements La, Ce, Dy, Ho, Yb, etc.; and intermetallic compounds formed by partial substitution of the Fe position, Co position or Mn position in the above intermetallic compounds by any one or two elements selected from Si, Al, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Hf, and Ta.
[0040] (3) The alloy is selected from: Fe-Ni, Fe-Pt, Cr-Fe, Ni-Ti, Ti-Nb, etc.
[0041] The high thermal conductivity reinforcement is one or a combination of two or more inorganic non-metallic materials having a thermal conductivity higher than that of the aluminum matrix, such as one or a combination of two or more of SiC, Si3N4, AlN, graphite, carbon fiber, graphene, and diamond;
[0042] The aluminum matrix is an aluminum alloy or pure aluminum having an aluminum mass percentage of more than 50wt%, such as an Al-Si alloy, an Al-Cu alloy, an Al-Mg alloy, an Al-Zn alloy, an Al-Mn alloy, or a combination of more than two kinds of pure aluminum, and the purity of the pure aluminum is more than 99.0wt%.
[0043] It should be noted that the negative thermal expansion reinforcement exhibits the property of "heat shrinkage and cold expansion" within the operating temperature range of electronic components. Within this temperature range, the average linear expansion coefficient and the volume expansion coefficient are both negative. The negative thermal expansion material is compounded with other positive thermal expansion materials in the aluminum-based composite material to prepare a material with a controllable thermal expansion coefficient, such as a zero expansion material. The material of the high thermal conductivity reinforcement is a material with higher thermal conductivity. The high thermal conductivity reinforcement is compounded with other materials with lower thermal conductivity in the aluminum-based composite material to prepare a material with higher thermal conductivity. Within the allowable range of the volume content of the above-mentioned negative thermal expansion reinforcement and high thermal conductivity reinforcement, by adjusting their volume ratio, an aluminum-based composite material with different thermal expansion coefficients and thermal conductivities that meets the use conditions is obtained, such as 10vol% ZrW2O8+10vol% SiC+80vol% Al-Si alloy matrix, whose thermal conductivity is 147.1W / mK and thermal expansion coefficient is 12.6ppm / ℃; 10vol% ZrW2O8 +40vol%SiC+50vol%Al-Si alloy matrix, its thermal conductivity is 131.1W / mK, thermal expansion coefficient is 9.7ppm / ℃; 40vol%ZrW2O8+10vol%SiC+50vol%Al-Si alloy matrix, its thermal conductivity is 63.1W / mK, thermal expansion coefficient is 6.2ppm / ℃; 30vol%ZrW2O8+20vol%SiC+50vol%Al-Si alloy matrix, its The thermal conductivity is 87.2W / mK and the thermal expansion coefficient is 7.6ppm / ℃; the thermal conductivity of 30vol%ZrW2O8+30vol%SiC+40vol%Al-Si alloy matrix is 68.7W / mK and the thermal expansion coefficient is 5.1ppm / ℃; the thermal conductivity of 20vol%Cu2P2O7+30vol%SiC+50vol%Al-Si alloy matrix is 54.2W / mK and the thermal expansion coefficient is 7.6ppm / ℃.
[0044] The present invention also provides a method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient, comprising the following steps:
[0045] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0046] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0047] Step S3, loading the composite powder of step S2 into a sintering mold and moving it into a furnace, adjusting the furnace environment, maintaining heat or maintaining heat and applying pressure to perform solid-phase sintering, cooling with the furnace, and taking it out at room temperature to obtain an aluminum-based composite material;
[0048] Specifically, in step S1, first, the total volume is calculated according to the size of the aluminum-based composite material to be prepared; then, the respective volumes of the negative expansion reinforcement, the high thermal conductivity reinforcement, and the aluminum matrix are calculated according to the volume fraction; finally, the weight of each material is calculated based on the volume and true density of the negative expansion reinforcement, the high thermal conductivity reinforcement, and the aluminum matrix.
[0049] The negative thermal expansion reinforcement powder is one or a combination of two or more of a ceramic powder, an intermetallic compound powder, and an alloy powder, whose average linear expansion coefficient or volume expansion coefficient is negative at t°C, -100°C < t < 300°C, and the average particle size of the negative thermal expansion reinforcement powder is 0.1~500μm. Specifically, the negative thermal expansion reinforcement powder is selected from: (1) ceramic powder: chemical formula aα2O8, wherein a represents one or more chemical elements of Zr, Hf, Sn, Ti, Eu, Er, Yb, and α represents one or more chemical elements of W, Mo, and V; chemical formula bβ2O7, wherein b represents one or more chemical elements of Zr, Th, and Ce, and β represents one or more chemical elements of P, Mo, and V; chemical formula c2γ3O 12 , where c represents one or more of the chemical elements Sc, Dy, Y, Er, Yb, and Lu, and γ represents one or more of the chemical elements W and Mo; the chemical formula is dδO5, where d represents one or more of the chemical elements Nb and Ta, and δ represents one or more of the chemical elements V and P; the chemical formula is eε2P3O 12, where e represents one or more of the chemical elements Na, K, Nb, Rb, and Cs, and ε represents one or more of the chemical elements Zr, Ti, and Hf; chemical formula f2ζ2O7, where f represents one or more of the chemical elements Cu, Mn, Fe, Co, Ni, Mg, and Zn, and ζ represents one or more of the chemical elements P and V; chemical formula g2O(PO4)2, where g represents one or more of the chemical elements U and Th; chemical formula hθF6, where h represents one or more of the chemical elements Ca, Mn, Fe, Zn, Co, Ni, Mg, Yb, and Ti, and θ represents one or more of the chemical elements Zr, Hf, and Nb; chemical formula i(CN)2, where i represents one or more of the chemical elements Zn and Cd; chemical formula j B(CN)4, where j represents one or more of the chemical elements Cu and Ag; chemical formula kτ(CN)6, where k represents one or more of the chemical elements Y, Fe, Ga, Sc, Ti, La, Sm, Ho, Lu, Er, Cs, Rb, Cd, Mn, Co, Ni, and Zn, and τ represents one or more of the chemical elements Fe, Co, Pt, Cd, Ni, Cu, and Zn; chemical formula Mn3lN, where l represents one or more of Zn, Cu, Ga, Sn, Ge, Si, Ge, and Fe, and compounds formed by partial replacement of Mn in the chemical formula Mn3lN by any one or two of V, Cr, Fe, Co, Ni, Cu, and Zn; Zn[Ag(CN)2]2, CaZr4P6O 24 、Si(NCN)2、ReO3、SiO2、Cu2O、Ag2O、ScF3、ZrW2O8、ZrMo2O8、ZrV2O8、Cu2P2O7、Cu2V2O7, etc.;(2)Intermetallic compound powder is selected from: Zr y Nb 1-y Fe2、Hf y Nb 1- y Fe2、Hf 1-y Ta y Fe2、Sc 1-y Ti y Fe2、CrTe y Se 1-y 、LaFe 13-x Si x 、LaFe 13-x Al x , Mn3Ge, Mn-Co-Ge series, Fe-Mn-Ga series, Ni-Mn-Ga series, RCo2, R2Fe 14 B. R2Fe 17 、RCo3、RFe 12 、R3Fe 29etc., wherein y is any value from 0 to 1, x is any value from 0 to 13, and R is one or more rare earth elements, such as rare earth elements La, Ce, Dy, Ho, Yb, etc.; and intermetallic compounds formed by partial substitution of the Fe position, Co position or Mn position in the above intermetallic compounds by any one or two elements selected from Si, Al, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Hf, and Ta; (3) alloy powders selected from: Fe-Ni, Fe-Pt, Cr-Fe, Ni-Ti, Ti-Nb, etc.
[0050] The high thermal conductivity reinforcement powder is one or a combination of two or more inorganic non-metallic powders having a thermal conductivity higher than that of the aluminum matrix, such as one or a combination of two or more of SiC, Si3N4, AlN, graphite, carbon fiber, graphene, and diamond, and the average particle size of the powder is 0.1~500μm.
[0051] The aluminum matrix powder is an aluminum alloy powder or a combination of one or more of pure aluminum powders with an aluminum mass percentage of more than 50wt%, such as one or more of Al-Si alloy, Al-Cu alloy, Al-Mg alloy, Al-Zn alloy, Al-Mn alloy, and pure aluminum, the purity of pure aluminum is more than 99.0wt%, and the average particle size of the aluminum matrix powder is 0.1~500μm.
[0052] Specifically, in step S3, the solid phase sintering is performed in any one of a vacuum sintering furnace, an atmosphere sintering furnace, a hot pressing sintering furnace, a hot isostatic pressing furnace or a spark plasma sintering furnace.
[0053] In vacuum sintering furnace, atmosphere sintering furnace, hot pressing sintering furnace and hot isostatic pressing furnace, the furnace environment is 1×10 -2 ~50Pa vacuum environment or pressure of 1~1×10 3 A protective gas among nitrogen, argon and helium with a sintering temperature of 0.15 MPa is used. The sintering mold used is a cylindrical graphite or steel mold, which is axially compressible. The inner diameter of the sintering mold is 6 to 300 mm. The pressure applied during the sintering process is 0 to 200 MPa, the temperature is 400 to 720 ° C, and the holding time is 30 to 120 min.
[0054] In the spark plasma sintering furnace, the furnace environment is 1×10 -4 A vacuum environment of ~100Pa or a pressure of 10~1×10 3Pa of nitrogen, argon, helium, the sintering mold used is a cylindrical graphite or steel mold, axially compressible, the inner diameter of the sintering mold is 6 ~ 150mm, the pressure applied during the sintering process is 30 ~ 200MPa, the temperature is 400 ~ 640℃, and the holding time is 5 ~ 100min; if the pressure is 70 ~ 200MPa, the temperature is 400 ~ 470℃, and the holding time is 10 ~ 100min.
[0055] First, the hybrid reinforcement preparation method of the present invention can achieve flexible matching of the two thermophysical properties of thermal conductivity and thermal expansion coefficient of aluminum-based composite materials; second, the solid-phase sintering method of the present invention can prepare aluminum-based composite materials with low volume fraction reinforcement and can control the accuracy of the volume fraction.
[0056] Example 1
[0057] A high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient includes a negative thermal expansion reinforcement ZrW2O8, a high thermal conductivity reinforcement SiC and an Al-Si alloy matrix. The total volume content of the negative thermal expansion reinforcement ZrW2O8 and the high thermal conductivity reinforcement SiC is 20 vol.%, of which the volume content of the negative thermal expansion reinforcement ZrW2O8 is 10 vol.%, the volume content of the high thermal conductivity reinforcement SiC is 10 vol.%, and the balance is the Al-Si alloy matrix.
[0058] A method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient comprises the following steps:
[0059] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0060] Prefabricated aluminum matrix composite material volume 3.14cm 3 Weigh 1.60g of ZrW2O8 powder (negative expansion reinforcement), 1.01g of SiC powder (high thermal conductivity reinforcement), and 6.74g of Al-Si alloy powder (aluminum matrix). The average particle size of the ZrW2O8 powder, the average particle size of the SiC powder, and the average particle size of the Al-Si alloy powder are 0.1μm.
[0061] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0062] Step S3, loading the composite powder from step S2 into a sintering mold and moving it into a furnace, adjusting the furnace environment, maintaining heat and applying pressure for solid-phase sintering, cooling with the furnace, and taking it out at room temperature to obtain an aluminum-based composite material;
[0063] Solid-phase sintering is carried out in a discharge plasma furnace in a vacuum environment of 10 Pa. The sintering mold used is a cylindrical graphite; the inner diameter of the sintering mold is 20 mm, the pressure applied during the sintering process is 30 MPa, the temperature during the sintering process is 500°C, and the holding time is 10 min.
[0064] The thermal conductivity of the prepared aluminum-based composite material was tested by a thermal conductivity meter, and the thermal expansion coefficient of the prepared aluminum-based composite material was tested by a linear thermal expansion meter. The test results are shown in Table 1.
[0065] Example 2
[0066] A high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient includes a negative thermal expansion reinforcement ZrW2O8, a high thermal conductivity reinforcement SiC and an Al-Si alloy matrix. The total volume content of the negative thermal expansion reinforcement ZrW2O8 and the high thermal conductivity reinforcement SiC is 50 vol.%, of which the volume content of the negative thermal expansion reinforcement ZrW2O8 is 10 vol.%, the volume content of the high thermal conductivity reinforcement SiC is 40 vol.%, and the balance is the Al-Si alloy matrix.
[0067] A method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient comprises the following steps:
[0068] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0069] Prefabricated aluminum matrix composite volume 678.58cm 3 Weigh 346.08g of ZrW2O8 powder (negative expansion reinforcement), 871.30g of SiC powder (high thermal conductivity reinforcement), and 909.30g of Al-Si alloy powder. The average particle size of the ZrW2O8 powder is 100μm, the average particle size of the SiC powder is 5μm, and the average particle size of the Al-Si alloy powder is 500μm.
[0070] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0071] Step S3, loading the composite powder from step S2 into a sintering mold and moving it into a furnace, adjusting the furnace environment, maintaining heat and applying pressure for solid-phase sintering, cooling with the furnace, and taking it out at room temperature to obtain an aluminum-based composite material;
[0072] Solid phase sintering is carried out in a spark plasma furnace with an internal atmosphere of 1×10 -1Pa vacuum environment, the sintering mold used is cylindrical graphite; the inner diameter of the sintering mold is 120 mm, the pressure applied during the sintering process is 80 MPa, the temperature during the sintering process is 550 ° C, and the holding time is 100 min.
[0073] The thermal conductivity of the prepared aluminum-based composite material was tested by a thermal conductivity meter, and the thermal expansion coefficient of the prepared aluminum-based composite material was tested by a linear thermal expansion meter. The test results are shown in Table 1.
[0074] Example 3
[0075] A high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient includes a negative thermal expansion reinforcement ZrW2O8, a high thermal conductivity reinforcement SiC and an Al-Si alloy matrix. The total volume content of the negative thermal expansion reinforcement ZrW2O8 and the high thermal conductivity reinforcement SiC is 50 vol.%, of which the volume content of the negative thermal expansion reinforcement ZrW2O8 is 40 vol.%, the volume content of the high thermal conductivity reinforcement SiC is 10 vol.%, and the balance is the Al-Si alloy matrix.
[0076] A method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient comprises the following steps:
[0077] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0078] Prefabricated aluminum matrix composite volume 201.06cm 3 Weigh 410.17g of ZrW2O8 powder (negative expansion reinforcement), 64.54g of SiC powder (high thermal conductivity reinforcement), and 269.42g of Al-Si alloy powder. The average particle size of the ZrW2O8 powder is 5μm, the average particle size of the SiC powder is 80μm, and the average particle size of the Al-Si alloy powder is 250μm.
[0079] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0080] Step S3, loading the composite powder from step S2 into a sintering mold and moving it into a furnace, adjusting the furnace environment, maintaining heat and applying pressure for solid-phase sintering, cooling with the furnace, and taking it out at room temperature to obtain an aluminum-based composite material;
[0081] Solid phase sintering is carried out in a spark plasma furnace with an internal atmosphere of 1×10 -1 Pa vacuum environment, the sintering mold used is cylindrical graphite, axially compressible, the inner diameter of the sintering mold is 80mm, the pressure applied during the sintering process is 50MPa, the temperature is 550℃, and the holding time is 40min.
[0082] The thermal conductivity of the prepared aluminum-based composite material was tested by a thermal conductivity meter, and the thermal expansion coefficient of the prepared aluminum-based composite material was tested by a linear thermal expansion meter. The test results are shown in Table 1.
[0083] Example 4
[0084] A high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient includes a negative thermal expansion reinforcement ZrW2O8, a high thermal conductivity reinforcement SiC and an Al-Si alloy matrix. The total volume content of the negative thermal expansion reinforcement ZrW2O8 and the high thermal conductivity reinforcement SiC is 50 vol.%, of which the volume content of the negative thermal expansion reinforcement ZrW2O8 is 30 vol.%, the volume content of the high thermal conductivity reinforcement SiC is 20 vol.%, and the balance is the Al-Si alloy matrix.
[0085] A method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient comprises the following steps:
[0086] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0087] Prefabricated aluminum matrix composite material volume 0.39cm 3 Weigh 60g of ZrW2O8 powder (negative expansion reinforcement), 0.25g of SiC powder (high thermal conductivity reinforcement), and 0.52g of Al-Si alloy powder. The average particle size of the ZrW2O8 powder is 70μm, the average particle size of the SiC powder is 0.1μm, and the average particle size of the Al-Si alloy powder is 500μm.
[0088] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0089] Step S3, loading the composite powder from step S2 into a sintering mold and moving it into a furnace, adjusting the furnace environment, maintaining heat and applying pressure for solid-phase sintering, cooling with the furnace, and taking it out at room temperature to obtain an aluminum-based composite material;
[0090] Solid phase sintering is carried out in a spark plasma furnace with an internal atmosphere of 1×10 -4 Pa vacuum environment, the sintering mold used is cylindrical graphite; the inner diameter of the sintering mold is 10 mm, the pressure applied during the sintering process is 40 MPa, the temperature during the sintering process is 500°C, and the holding time is 5 min.
[0091] The thermal conductivity of the prepared aluminum-based composite material was tested by a thermal conductivity meter, and the thermal expansion coefficient of the prepared aluminum-based composite material was tested by a linear thermal expansion meter. The test results are shown in Table 1.
[0092] Figure 1This is the microstructure diagram of the aluminum-based composite material of Example 4, where mark 1 is the high thermal conductivity reinforcement SiC, mark 2 is the negative thermal expansion reinforcement ZrW2O8, and mark 3 is the Al-Si alloy matrix. Figure 2 The thermal expansion curves of the Al-Si alloy and the aluminum-based composite material in Example 4 show that the thermal expansion coefficient of the Al-Si alloy is 21.0 ppm / °C in the range of -100°C to 50°C, and the thermal expansion coefficient of the aluminum-based composite material is 7.6 ppm / °C. It can be seen that the addition of the negative thermal expansion reinforcement ZrW2O8 to the Al-Si alloy reduces the thermal expansion coefficient of the composite material.
[0093] Example 5
[0094] A high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient includes a negative thermal expansion reinforcement ZrW2O8, a high thermal conductivity reinforcement SiC and an Al-Si alloy matrix. The total volume content of the negative thermal expansion reinforcement ZrW2O8 and the high thermal conductivity reinforcement SiC is 60 vol.%, of which the volume content of the negative thermal expansion reinforcement ZrW2O8 is 30 vol.%, the volume content of the high thermal conductivity reinforcement SiC is 30 vol.%, and the balance is the Al-Si alloy matrix.
[0095] A method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient comprises the following steps:
[0096] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0097] Prefabricated aluminum matrix composite material volume 25.13cm 3 Weigh 38.45g of ZrW2O8 powder, a negative expansion reinforcement, 24.20g of SiC powder, a high thermal conductivity reinforcement, and 26.94g of Al-Si alloy powder. The average particle size of the ZrW2O8 powder is 8μm, the average particle size of the SiC powder is 70μm, and the average particle size of the Al-Si alloy powder is 250μm.
[0098] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0099] Step S3, loading the composite powder from step S2 into a sintering mold and moving it into a furnace, adjusting the furnace environment, maintaining heat and applying pressure for solid-phase sintering, cooling with the furnace, and taking it out at room temperature to obtain an aluminum-based composite material;
[0100] Solid phase sintering is carried out in a spark plasma furnace with an internal atmosphere of 1×10 -3Pa vacuum environment, the sintering mold used is cylindrical graphite; the inner diameter of the sintering mold is 40 mm, the pressure applied during the sintering process is 50 MPa, the temperature during the sintering process is 500 ° C, and the holding time is 20 min.
[0101] The thermal conductivity of the prepared aluminum-based composite material was tested by a thermal conductivity meter, and the thermal expansion coefficient of the prepared aluminum-based composite material was tested by a linear thermal expansion meter. The test results are shown in Table 1.
[0102] Example 6
[0103] A high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient comprises a negative thermal expansion reinforcement Cu2P2O7, a high thermal conductivity reinforcement SiC and an Al-Si alloy matrix, wherein the total volume content of the negative thermal expansion reinforcement Cu2P2O7 and the high thermal conductivity reinforcement SiC is 50 vol.%, of which the volume content of the negative thermal expansion reinforcement Cu2P2O7 is 20 vol.%, the volume content of the high thermal conductivity reinforcement SiC is 30 vol.%, and the balance is the Al-Si alloy matrix.
[0104] A method for preparing a high thermal conductivity aluminum-based composite material with an adjustable thermal expansion coefficient comprises the following steps:
[0105] Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight;
[0106] Prefabricated aluminum matrix composite volume 392.70cm 3 Weigh 471.24g of Cu2P2O7 powder (negative expansion reinforcement), 252.11g of SiC powder (high thermal conductivity reinforcement), and 526.22g of Al-Si alloy powder. The average particle size of the Cu2P2O7 powder is 70μm, the average particle size of the SiC powder is 3μm, and the average particle size of the Al-Si alloy powder is 400μm.
[0107] Step S2, mixing the three powders weighed in step S1 to obtain a composite powder;
[0108] Step S3, loading the composite powder from step S2 into a sintering mold and moving it into a furnace, adjusting the furnace environment, maintaining heat and applying pressure for solid-phase sintering, cooling with the furnace, and taking it out at room temperature to obtain an aluminum-based composite material;
[0109] Solid phase sintering is carried out in a spark plasma furnace with an internal atmosphere of 1×10 -1 Pa vacuum environment, the sintering mold used is cylindrical graphite; the inner diameter of the sintering mold is 100 mm, the pressure applied during the sintering process is 30 MPa, the temperature during the sintering process is 550 ° C, and the holding time is 50 min.
[0110] The thermal conductivity of the prepared aluminum-based composite material was tested by a thermal conductivity meter, and the thermal expansion coefficient of the prepared aluminum-based composite material was tested by a linear thermal expansion meter. The test results are shown in Table 1.
[0111] Table 1 Thermophysical properties of aluminum-based composite materials of Examples 1 to 6
[0112]
[0113] As shown in Examples 1-6, by selecting different materials and volume ratios of negative expansion reinforcements, high thermal conductivity reinforcements, and aluminum matrices, aluminum-based composite materials with thermal conductivities ranging from 54.2 to 147.1 W / mK and thermal expansion coefficients ranging from 5.1 to 12.6 ppm / °C can be obtained. This patent demonstrates that the hybrid reinforcement design significantly improves the thermal conductivity of aluminum-based composite materials while simultaneously achieving a low thermal expansion coefficient. Specifically, in Example 4, a low thermal expansion coefficient of 7.6 ppm / °C is maintained while achieving a high thermal conductivity of 87.2 W / mK.
[0114] The foregoing description is merely a specific embodiment of the present invention, and the scope of protection of the present invention is not limited thereto. Any person skilled in the art will readily conceive of various equivalent modifications or substitutions within the technical scope disclosed herein, and such modifications or substitutions are intended to be encompassed within the scope of protection of the present invention. Therefore, the scope of protection of the present invention shall be subject to the scope of protection defined in the claims.
Claims
1. A high thermal conductivity, low volume fraction reinforced aluminum matrix composite material with adjustable thermal expansion coefficient, characterized in that: The material includes a negative thermal expansion reinforcement, a high thermal conductivity reinforcement and an aluminum matrix, wherein the total volume content of the negative thermal expansion reinforcement and the high thermal conductivity reinforcement is 10 to 20 vol.%, wherein the volume content of the negative thermal expansion reinforcement is 5 to 10 vol.%, the volume content of the high thermal conductivity reinforcement is 5 to 10 vol.%, and the balance is the aluminum matrix; The negative thermal expansion reinforcement is one or a combination of two or more ceramic materials, intermetallic compounds, and alloys whose average linear expansion coefficient or volume expansion coefficient is negative at t°C, -100°C < t < 300°C; the high thermal conductivity reinforcement is one or a combination of two or more inorganic non-metallic materials whose thermal conductivity is higher than that of the aluminum matrix; the aluminum matrix is one or a combination of two or more aluminum alloys or pure aluminum having an aluminum mass percentage of 50 wt% or more, and the purity of the pure aluminum is above 99.0 wt%; The ceramic material is selected from at least one of the following chemical formulas: chemical formula aα2O8, wherein a represents one or more chemical elements of Zr, Hf, Sn, Ti, Eu, Er, and Yb, and α represents one or more chemical elements of W, Mo, and V; chemical formula bβ2O7, wherein b represents one or more chemical elements of Zr, Th, and Ce, and β represents one or more chemical elements of P, Mo, and V; chemical formula c2γ3O 12 , where c represents one or more of the chemical elements Sc, Dy, Y, Er, Yb, and Lu, and γ represents one or more of the chemical elements W and Mo; the chemical formula is dδO5, where d represents one or more of the chemical elements Nb and Ta, and δ represents one or more of the chemical elements V and P; the chemical formula is eε2P3O 12 , where e represents one or more of the chemical elements Na, K, Nb, Rb, and Cs, and ε represents one or more of the chemical elements Zr, Ti, and Hf; chemical formula f2ζ2O7, where f represents one or more of the chemical elements Cu, Mn, Fe, Co, Ni, Mg, and Zn, and ζ represents one or more of the chemical elements P and V; chemical formula g2O(PO4)2, where g represents one or more of the chemical elements U and Th; chemical formula hθF6, where h represents one or more of the chemical elements Ca, Mn, Fe, Zn, Co, Ni, Mg, Yb, and Ti, and θ represents one or more of the chemical elements Zr, Hf, and Nb; chemical formula i(CN)2, where i represents one or more of the chemical elements Zn and Cd; chemical formula j B(CN)4, where j represents one or more of the chemical elements Cu and Ag; chemical formula kτ(CN)6, where k represents one or more of the chemical elements Y, Fe, Ga, Sc, Ti, La, Sm, Ho, Lu, Er, Cs, Rb, Cd, Mn, Co, Ni, and Zn, and τ represents one or more of the chemical elements Fe, Co, Pt, Cd, Ni, Cu, and Zn; chemical formula Mn3lN, where l represents one or more of Zn, Cu, Ga, Sn, Ge, Si, Ge, and Fe, and compounds formed by partial replacement of Mn in the chemical formula Mn3lN by any one or two of V, Cr, Fe, Co, Ni, Cu, and Zn; Zn[Ag(CN)2]2, CaZr4P6O 24 , Si(NCN)2, ReO3, SiO2, Cu2O, Ag2O, ScF3; The method for preparing the material comprises the following steps: Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight; Step S2, mixing the three powders weighed in step S1 to obtain a composite powder; Step S3: Load the composite powder from step S2 into a sintering mold and move it into a furnace, adjust the furnace environment, keep it warm or apply heat and pressure to perform solid-phase sintering, cool it with the furnace, and take it out at room temperature to obtain an aluminum-based composite material; the solid-phase sintering is spark plasma sintering.
2. The material according to claim 1, characterized in that The intermetallic compound is selected from at least one of the following chemical formulas: Zr y Nb 1-y Fe2、Hf y Nb 1-y Fe2、Hf 1-y Ta y Fe2、Sc 1-y Ti y Fe2、CrTe y Se 1-y 、LaFe 13-x Si x 、LaFe 13-x Al x , Mn3Ge, Mn-Co-Ge series, Fe-Mn-Ga series, Ni-Mn-Ga series, RCo2, R2Fe 14 B. R2Fe 17 、RCo3、RFe 12 、R3Fe 29 , in the chemical formula, y is any value from 0 to 1, x is any value from 0 to 13, and R is one or more rare earth elements; and intermetallic compounds formed by partial substitution of the Fe, Co, or Mn positions in the above chemical formula by any one or two elements selected from Si, Al, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Hf, and Ta; The alloy is selected from at least one of the following element combinations: Fe-Ni, Fe-Pt, Cr-Fe, Ni-Ti, and Ti-Nb.
3. The material according to claim 1, characterized in that The inorganic non-metallic material is selected from at least one of SiC, Si3N4, AlN, graphite, carbon fiber, graphene, and diamond.
4. The material according to claim 1, characterized in that The aluminum alloy is selected from at least one of Al-Si alloy, Al-Cu alloy, Al-Mg alloy, Al-Zn alloy and Al-Mn alloy.
5. A method for preparing a high thermal conductivity aluminum-based composite material with adjustable thermal expansion coefficient, characterized in that: The method is used to prepare the material according to any one of claims 1 to 4, and the method comprises the following steps: Step S1: weighing negative expansion reinforcement powder, high thermal conductivity reinforcement powder, and aluminum matrix powder according to the volume fraction of the aluminum-based composite material to be prepared, converted into weight; Step S2, mixing the three powders weighed in step S1 to obtain a composite powder; Step S3: Load the composite powder from step S2 into a sintering mold and move it into a furnace, adjust the furnace environment, keep it warm or apply heat and pressure to perform solid-phase sintering, cool it with the furnace, and take it out at room temperature to obtain an aluminum-based composite material; the solid-phase sintering is spark plasma sintering.
6. The method according to claim 5, characterized in that In step S1, the negative thermal expansion reinforcement powder is one or a combination of two or more of a ceramic powder, an intermetallic compound powder, and an alloy powder, the average linear expansion coefficient or volume expansion coefficient of which is negative at t°C, -100°C < t < 300°C, and the average particle size of the negative thermal expansion reinforcement powder is 0.1 to 500 μm; The high thermal conductivity reinforcement powder is one or a combination of two or more inorganic non-metallic powders having a thermal conductivity higher than that of the aluminum matrix, and the average particle size of the high thermal conductivity reinforcement powder is 0.1 to 500 μm; The aluminum matrix powder is one or a combination of two or more of aluminum alloy powder or pure aluminum powder with an aluminum mass percentage of more than 50wt%, the purity of pure aluminum is more than 99.0wt%, and the average particle size of the aluminum matrix powder is 0.1-500μm.
7. The method according to claim 5, characterized in that In the step S3, the solid phase sintering is performed in a spark plasma sintering furnace.
8. The method according to claim 7, characterized in that In the spark plasma sintering furnace, the furnace environment is 1×10 -4 A vacuum environment of 100 Pa or a pressure of 10 to 1×10 3 A protective gas among nitrogen, argon and helium with a sintering temperature of 10000 Pa is used. The sintering mold used is a cylindrical graphite or steel mold, which is axially compressible. The inner diameter of the sintering mold is 6 to 150 mm. The pressure applied during the sintering process is 30 to 200 MPa, the temperature is 400 to 640 ° C, and the holding time is 5 to 100 minutes.
9. The method according to claim 8, characterized in that During the sintering process, the pressure applied is 70-200 MPa, the temperature is 400-470° C., and the heat preservation time is 10-100 minutes.
Citation Information
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