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CN110835432A - Polymer-based heat-conducting composite material and preparation method and application thereof - Google Patents

Polymer-based heat-conducting composite material and preparation method and application thereof Download PDF

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CN110835432A
CN110835432A CN201911206797.XA CN201911206797A CN110835432A CN 110835432 A CN110835432 A CN 110835432A CN 201911206797 A CN201911206797 A CN 201911206797A CN 110835432 A CN110835432 A CN 110835432A
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conducting
heat
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composite material
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邹华维
李生钊
李瑶
周生态
陈洋
梁梅
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Sichuan University
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    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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Abstract

The invention provides a polymer-based heat-conducting composite material and a preparation method and application thereof. The composite material is prepared from the following raw materials in volume fraction: 5-30% of metal-based heat-conducting and electric-conducting filler, 5-30% of ceramic-based heat-conducting and electric-insulating filler and 40-90% of matrix. The composite material takes the compounding of copper and heat-conducting insulating filler silicon carbide or boron nitride as the filler, and the heat-conducting property of the polymer material is obviously improved. The composite material has excellent comprehensive performance, utilizes the metal material with high heat conductivity and high resistivity, can be applied to thermal diffusion in occasions with high requirements on electrical insulation performance and other occasions requiring thermal diffusion management, and has good market prospect in the fields of microelectronics, electrician electricity, light emitting diodes, heat exchange engineering, solar energy, lithium batteries, automobiles, aerospace and the like when preparing heat-conducting and heat-radiating materials. In addition, the composite material has simple preparation process and excellent processing performance, and can be applied to large-scale practical application.

Description

Polymer-based heat-conducting composite material and preparation method and application thereof
Technical Field
The invention belongs to the field of composite materials, and particularly relates to a polymer-based heat-conducting composite material and a preparation method and application thereof.
Background
Currently, leading-edge technologies such as big data, cloud computing, internet of things and mobility are changing the world deeply, and the blossoming electronics and electrical industry is a cornerstone of the growth promotion science and technology progress. Numerous electronic products, such as mobile phones, computers, household appliances, new energy vehicles and the like, are advancing towards intellectualization and integration, which requires higher packaging density and higher power density of circuit components in electronic equipment. However, a large amount of heat is generated in the operation process of the electronic equipment, the internal temperature rises rapidly during the operation process due to heat accumulation, the high temperature is a large enemy of an integrated circuit, the equipment is unstable in operation and short in service life, and certain parts can be disabled even serious life and property losses can be caused. Therefore, how to dissipate heat in time and ensure the normal temperature of the electronic component is a current research hotspot.
Although metal and ceramic materials have excellent heat-conducting property, the metal materials are not resistant to chemical corrosion and poor in electrical insulation property and cannot be used in occasions of electrical insulation and chemical corrosion, and the ceramic materials are high in processing cost and poor in impact resistance and cannot meet the requirements of industrial and scientific development at present. Although the polymer material has light weight, good formability and processability, good electrical insulation performance and excellent corrosion resistance, the polymer material has low intrinsic thermal conductivity and is not beneficial to heat conduction and heat dissipation.
The heat conduction filler has a wide variety of types and can be generally divided into three types, namely metal filler, ceramic filler and carbon-based filler, the heat conductivity of the filler depends on the internal heat conduction mechanism of the filler, generally, the filler mainly based on phonon heat conduction has low heat conductivity, for example, the metal oxide α -aluminum oxide has a heat conductivity coefficient of 30W/(m.K) even though the ceramic filler with high heat conductivity, such as boron nitride and aluminum nitride, has a heat conductivity coefficient of only 300W/(m.K) while the heat conductivity of the filler is generally limited by 100W/(m.K), the heat conduction metal and carbon-based material with free electron motion has more excellent heat conductivity, and in order to construct a channel network structure in the composite material, the additive amount of the filler has more than 100W/(m.K), the heat conduction metal and carbon-based filler has more important influence on the heat conduction performance of the heat conduction and insulation of the composite material, and the electrical and the heat conduction dielectric materials have more important influence on the comprehensive heat conduction performance of the heat conduction and the heat conduction of the aerospace engineering, the electrical and the electrical insulation of the composite material.
Disclosure of Invention
In order to solve the problems in the background art, the invention provides a polymer-based heat-conducting composite material, and a preparation method and application thereof.
The invention provides a polymer-based heat-conducting composite material, which is prepared from the following raw materials in volume fraction: 5-30% of metal-based heat-conducting and electric-conducting filler, 5-30% of ceramic-based heat-conducting and electric-insulating filler and 40-90% of matrix.
Further, the polymer-based heat-conducting composite material is prepared from the following raw materials in volume fraction: 7.5-22.5% of metal-based heat-conducting and electric-conducting filler, 7.5-22.5% of ceramic-based heat-conducting and insulating filler and 70% of matrix;
preferably, the material is prepared from the following raw materials in volume fraction: 7.5% of metal-based heat and electricity conducting filler, 22.5% of ceramic-based heat and electricity conducting and insulating filler and 70% of matrix.
Further, the metal-based heat and electricity conducting filler is copper, silver, gold, aluminum, tungsten, nickel or iron; the ceramic-based heat-conducting insulating filler is aluminum nitride, beryllium oxide, SiC whiskers or boron nitride; the matrix is thermoplastic plastic, rubber or thermosetting plastic;
preferably, the copper is copper powder; the thermoplastic plastic is nylon, polyformaldehyde, polyphenylene sulfide or high-density polyethylene; the rubber is natural rubber, ethylene propylene diene monomer or silicone rubber; the thermosetting plastic is epoxy resin or polyester.
Further, the physical property parameters of the SiC whisker are as follows: the diameter is 1-30 mu m, the length-diameter ratio is more than 20, the SiC content is more than 96%, and the axial thermal conductivity is 100-500W/(m.K);
the boron nitride is hexagonal boron nitride, and the particle size of the hexagonal boron nitride is 5-50 microns;
the copper powder is atomized copper powder, and the atomized copper powder is sieved by a 325-mesh sieve;
the high-density polyethylene is 5000S high-density polyethylene;
preferably, the hexagonal boron nitride has a particle size of 30 μm or 5 μm.
Further, the preparation method of the polymer-based heat-conducting composite material comprises the following steps:
placing the high-density polyethylene granules in a preheated double-roller open mill until the high-density polyethylene granules are completely melted and wrapped, adding copper and heat-conducting insulating filler, mixing, thinly passing to obtain a blend, and forming the blend to obtain the polyethylene heat-conducting heat-insulating.
Further, the air conditioner is provided with a fan,
the temperature of a double roller in the double-roller open mill is 100-350 ℃;
and/or the preheating time is 1-10 min;
and/or the mixing is carried out for 3-10 times at a roll spacing of 0.5-2 mm;
and/or the thin passing is performed 3-10 times at a roll gap of 0.5-2 mm;
and/or, the molding is compression molding by a flat vulcanizing machine;
preferably, the first and second electrodes are formed of a metal,
the temperature of a double roller in the double-roller open mill is 150-230 ℃;
more preferably still, the first and second liquid crystal compositions are,
the temperature of the double rollers in the double-roller open mill is 160 +/-10 ℃;
and/or the preheating time is 3 min;
and/or the mixing is carried out for 6 times at a roll spacing of 1.2 mm;
and/or the thin passing is performed 6 times at a roll spacing of 0.8 mm;
and/or the pressure of the die pressing is set to be 10MPa, the die pressing temperature is 190 ℃, and the time is 5 min.
The invention also provides a method for preparing the polymer-based heat-conducting composite material, which comprises the following steps:
placing the high-density polyethylene granules in a preheated double-roller open mill until the high-density polyethylene granules are completely melted and wrapped, adding copper and heat-conducting insulating filler, mixing, thinly passing to obtain a blend, and forming the blend to obtain the polyethylene heat-conducting heat-insulating.
Further, the air conditioner is provided with a fan,
the temperature of a double roller in the double-roller open mill is 100-350 ℃;
and/or the preheating time is 1-10 min;
and/or the mixing is carried out for 3-10 times at a roll spacing of 0.5-2 mm;
and/or the thin passing is performed 3-10 times at a roll gap of 0.5-2 mm;
and/or, the molding is compression molding by a flat vulcanizing machine;
preferably, the first and second electrodes are formed of a metal,
the temperature of a double roller in the double-roller open mill is 150-230 ℃;
more preferably still, the first and second liquid crystal compositions are,
the temperature of the double rollers in the double-roller open mill is 160 +/-10 ℃;
and/or the preheating time is 3 min;
and/or the mixing is carried out for 6 times at a roll spacing of 1.2 mm;
and/or the thin passing is performed 6 times at a roll spacing of 0.8 mm;
and/or the pressure of the die pressing is set to be 10MPa, the die pressing temperature is 190 ℃, and the time is 5 min.
The invention also provides the application of the polymer-based heat-conducting composite material in preparing heat-conducting materials; preferably, the heat conducting material is an insulating heat conducting material.
Furthermore, the insulating heat conduction material is applied to the fields of microelectronics, electrician electricity, light emitting diodes, heat exchange engineering, solar energy, lithium batteries, automobiles and aerospace.
The polymer-based heat-conducting composite material disclosed by the invention takes copper and heat-conducting insulating filler silicon carbide or boron nitride as a filler in a compounding manner, so that the heat-conducting property of the polymer material is obviously improved. Particularly, copper and the heat-conducting insulating filler are compounded in a specific proportion, so that the heat conductivity of the prepared high-density polyethylene composite material is obviously improved, the heat-conducting property is better than that of the high-density polyethylene composite material enhanced by singly using copper, and the synergistic effect is reflected. Meanwhile, the polymer-based heat-conducting composite material disclosed by the invention is excellent in comprehensive performance and high in resistivity, can be applied to heat diffusion in occasions with higher requirements on electrical insulation performance and other occasions requiring heat diffusion management, and has good market prospect in the fields of preparing heat-conducting and heat-dissipating materials, microelectronic, electrical and electronic, light-emitting diodes, heat exchange engineering, solar energy, lithium batteries, automobiles, aerospace and the like. In addition, the polymer-based heat-conducting composite material disclosed by the invention is simple in preparation process, excellent in processing performance and capable of being practically applied in a large scale.
Obviously, many modifications, substitutions, and variations are possible in light of the above teachings of the invention, without departing from the basic technical spirit of the invention, as defined by the following claims.
The present invention will be described in further detail with reference to the following examples. This should not be understood as limiting the scope of the above-described subject matter of the present invention to the following examples. All the technologies realized based on the above contents of the present invention belong to the scope of the present invention.
Drawings
FIG. 1 shows the thermal conductivity of the polymer-based thermally conductive composite materials prepared in examples 1 to 8.
FIG. 2 shows the thermal conductivity of the polymer-based thermally conductive composite materials prepared in examples 9 to 13.
FIG. 3 is a graph showing the volume resistivity of the polymer-based thermally conductive composite materials prepared in examples 14 to 23.
Detailed Description
The raw materials and equipment used in the embodiment of the present invention are known products and obtained by purchasing commercially available products.
The information of the main raw materials used in the experiment is shown in table 1.
TABLE 1 information on the main raw materials used in the experiments
Figure BDA0002297099010000041
The physical properties of the SiC whiskers are shown in Table 2.
TABLE 2 SiC whisker physical Property parameters
The main equipment and instruments used in the experiment are shown in table 3.
TABLE 3 Main Equipment and instruments used in the experiment
Figure BDA0002297099010000043
Examples 1-13 preparation of Polymer-based thermally conductive composites of the invention
In the embodiments 1-13 of the invention, a silicon carbide/Cu compound reinforced polymer-based heat-conducting composite material is used. The invention uses a two-roll mill for melt mixing. And washing the purchased atomized copper powder in absolute ethyl alcohol and drying for later use.
The preparation method comprises the following steps: the HDPE pellets are preheated for 3min in a double-roll open mill at the temperature of 160 +/-10 ℃, then are completely melted and coated with rolls, Cu powder and SiC whiskers are added according to the formula, the mixture is mixed for six times at the roll spacing of 1.2mm, then is thinly passed for 6 times at the roll spacing of 0.8mm, and then the mixture is subjected to compression molding by a flat-plate vulcanizing machine at the pressure of 10MPa and the compression molding temperature of 190 ℃ for 5 min. The formulations of the polymer-based heat-conducting composite materials of embodiments 1 to 13 of the present invention are shown in table 4. Cu powder and SiC whisker are used as fillers, and HDPE is used as a polymer matrix.
TABLE 4 formulation of Polymer-based thermally conductive composites of the invention
Figure BDA0002297099010000051
Examples 14 to 18 preparation of Polymer-based thermally conductive composite Material of the present invention
In the embodiments 14-18 of the invention, a boron nitride/Cu compound reinforced polymer-based heat-conducting composite material is used. The particle size of the boron nitride was 5 μm. The invention uses a two-roll mill for melt mixing. And washing the purchased atomized copper powder in absolute ethyl alcohol and drying for later use.
The preparation method comprises the following steps: preheating HDPE granules in a double-roll open mill for 3min at the double-roll temperature of 160 +/-10 ℃, then completely melting and roll-wrapping the HDPE granules, adding Cu powder and h-BN powder (h-BN05) with the particle size of 5 mu m according to the formula, mixing for six times at a roll spacing of 1.2mm, then thinly passing for 6 times at a roll spacing of 0.8mm, then carrying out compression molding on the blend by using a flat-plate vulcanizer, setting the pressure to be 10MPa, and setting the compression molding temperature to be 190 ℃ for 5 min. The formulations of the polymer-based heat-conducting composite materials of the embodiments 14 to 18 of the present invention are shown in table 5. Cu powder and h-BN are used as fillers, and HDPE is used as a polymer matrix.
TABLE 5 formulation of Polymer-based thermally conductive composites of the invention
Figure BDA0002297099010000052
Figure BDA0002297099010000061
Examples 19 to 23 preparation of Polymer-based thermally conductive composite Material of the present invention
In the embodiments 19-23 of the invention, a boron nitride/Cu compound reinforced polymer-based heat-conducting composite material is used. The particle size of the boron nitride was 30 μm. The invention uses a two-roll mill for melt mixing. And washing the purchased atomized copper powder in absolute ethyl alcohol and drying for later use.
The preparation method comprises the following steps: the HDPE pellets are preheated for 3min in a double-roll open mill at the preheating temperature of 160 +/-10 ℃, then are completely melted and coated with rolls, Cu powder and h-BN powder (h-BN30) with the particle size of 30 mu m are added according to the formula, the mixture is mixed for six times at the roll spacing of 1.2mm, then the mixture is thinly passed for 6 times at the roll spacing of 0.8mm, then the mixture is molded by a flat-plate vulcanizer, the pressure is set to be 10MPa, the mold pressing temperature is 190 ℃, and the time is 5 min. The formulations of the polymer-based heat-conducting composite materials in the embodiments 19 to 23 of the present invention are shown in table 6. Cu powder and h-BN are used as fillers, and HDPE is used as a polymer matrix.
TABLE 6 formulation of Polymer-based thermally conductive composites of the present invention
Comparative example 1 preparation of Cu-reinforced Polymer-based thermally conductive composite
The invention uses a two-roll mill for melt mixing. And washing the purchased atomized Cu powder in absolute ethyl alcohol and drying for later use.
The formula is as follows: the volume fraction of Cu was 30 vol%, and the volume fraction of HDPE was 70 vol%.
The preparation method comprises the following steps: preheating HDPE granules in a double-roll open mill for 3min at the double-roll temperature of 160 +/-10 ℃, completely melting the HDPE granules, wrapping the HDPE granules with rolls, adding Cu powder according to a formula, mixing for six times at a roll spacing of 1.2mm, thinly passing for 6 times at a roll spacing of 0.8mm, and then carrying out compression molding on the blend by using a flat-plate vulcanizing machine at the pressure of 10MPa and the compression molding temperature of 190 ℃ for 5 min.
Comparative example 2 preparation of Small particle size boron nitride reinforced Polymer-based thermally conductive composite
The particle size of the boron nitride was 5 μm. The invention uses a two-roll mill for melt mixing.
The formula is as follows: the volume fraction of boron nitride was 30 vol%, and the volume fraction of HDPE was 70 vol%.
The preparation method comprises the following steps: the HDPE pellets are preheated for 3min in a double-roll open mill at the temperature of 160 +/-10 ℃, then are completely melted and coated with rolls, h-BN powder (h-BN05) with the particle size of 5 mu m is added according to the formula, the mixture is mixed for six times at the roll spacing of 1.2mm, then is subjected to thin passing for 6 times at the roll spacing of 0.8mm, and then the mixture is subjected to compression molding by a flat-plate vulcanizing machine, the pressure is set to be 10MPa, the compression molding temperature is 190 ℃, and the time is 5 min.
Comparative example 3 preparation of Large particle size boron nitride reinforced Polymer-based thermally conductive composite
The particle size of the boron nitride was 30 μm. The invention uses a two-roll mill for melt mixing.
The formula is as follows: the volume fraction of boron nitride was 30 vol%, and the volume fraction of HDPE was 70 vol%.
The preparation method comprises the following steps: the HDPE pellets are preheated for 3min in a double-roll open mill at the temperature of 160 +/-10 ℃, then are completely melted and coated with rolls, h-BN powder (h-BN30) with the particle size of 30 mu m is added according to the formula, the mixture is mixed for six times at the roll spacing of 1.2mm, then is subjected to thin passing for 6 times at the roll spacing of 0.8mm, and then the mixture is subjected to compression molding by a flat-plate vulcanizing machine, the pressure is set to be 10MPa, the compression molding temperature is 190 ℃, and the time is 5 min.
The advantageous effects of the present invention are demonstrated by specific test examples below.
Test example 1, Performance test of silicon carbide/Cu composite reinforced Polymer-based thermally conductive composite
First, test method
1. Test of Heat conductivity
A test instrument Hot disk 2500-OT thermal constant analyzer based on the transient method principle is adopted to measure the thermal conductivity coefficient of an experimental sample (pure HDPE, the polymer-based heat-conducting composite material prepared in comparative example 1 and examples 1-13), the diameter of a probe is 3.189mm, the thickness of the tested sample is larger than 4mm, the surface of the tested sample is polished smoothly, and good contact with the probe is guaranteed.
2. Volume resistivity test
The electrical resistivity of a sample (the polymer-based heat-conducting composite material prepared in comparative example 1 and examples 9 to 13) was measured by a ZC36 high-resistivity meter, and the volume resistivity of the material was calculated by formula 1, with a test voltage of 10V.
Wherein:
ρv-insulation resistance (Ω · cm) of the material to be measured,
Rx-the insulation resistance test result (Ω),
s-inner electrode cylindrical surface area 21.237cm2
t-average thickness of the material sample to be tested.
Second, test results
1. The heat-conducting property of the polymer-based heat-conducting composite material
FIG. 1 shows the results of the thermal conductivity tests of the polymer-based thermal conductive composites of examples 1 to 8. As can be seen from fig. 1: the thermal conductivity of the composite material prepared in example 8 was the highest at 1.488W/(m.K), followed by a thermal conductivity of 1.371W/(m.K) for the composite material prepared in example 4. The lowest thermal conductivity was the composite prepared in example 7, which had a thermal conductivity of 0.5089W/(m.K). The volume fraction of the filler is 30 vol%, and the prepared polymer-based heat-conducting composite material has the optimal heat-conducting property.
FIG. 2 shows the results of thermal conductivity tests on pure HDPE (PE in FIG. 2), comparative example 1, and examples 9-13. The volume fraction of the filler (Cu and SiC whisker) was fixed at 30 vol%, and the volume fraction ratios of SiC whisker and Cu were 1:3, 1:2, 1:1, 2:1, and 3:1, respectively. As can be seen from fig. 2: when the volume fraction ratio of the SiC whiskers to the Cu is 1:3, the thermal conductivity of the composite material is 1.663W/(m.K), and compared with that of a comparative example 1 (the volume fraction of Cu is 30 vol%, the SiC whiskers are not contained, and the thermal conductivity is 1.416W/(m.K)), the thermal conductivity of a sample is improved by 17.44%; compared with example 8 (the volume fraction of Cu is 24 vol%, the volume fraction of SiC whisker is 6 vol%, and the thermal conductivity is 1.488W/(m.K)), the thermal conductivity of the sample is improved by 11.76%. When the volume fraction ratio of the SiC whiskers to the Cu reaches 3:1 (example 13), the thermal conductivity of the composite material reaches 1.921W/(m.K), and compared with pure HDPE, the thermal conductivity of the sample is improved by 380%; the thermal conductivity of the sample was 35.7% higher than that of comparative example 1.
The results of the test pieces show that: the heat-conducting property of HDPE can be improved by compounding the SiC whiskers and the Cu. Particularly, the SiC whisker and the Cu are compounded in a specific proportion (the volume fraction ratio of the SiC whisker to the Cu is 3:1), the thermal conductivity of the prepared HDPE composite material is obviously improved, the thermal conductivity is better than that of the HDPE composite material enhanced by singly using the copper, and the synergistic effect is reflected.
2. The volume resistivity of the polymer-based heat-conducting composite material of the invention
Table 7 shows the volume resistivity of the polymer-based heat-conducting composite materials (examples 9-13 and comparative example 1) prepared by compounding SiC whiskers and Cu with different volume fraction ratios. As can be seen from Table 7: along with the increase of the volume fraction of the SiC whiskers, the volume resistivity of the composite material is gradually improved, and the resistivity is 1014The thickness is more than omega cm, and the application requirements of the fields of electronics and electricity and the like on the insulating and heat conducting materials are met.
TABLE 7 volume resistivity of polymer-based heat-conducting composite materials prepared by compounding SiC whiskers and Cu with different volume fraction ratios
Figure BDA0002297099010000081
Test example 2 Performance test of boron nitride/Cu composite reinforced Polymer-based thermally conductive composite
First, test method
1. Test of Heat conductivity
The heat conductivity of each composite material was tested by the method of test example 1 "and heat conductivity test" using the polymer-based heat conductive composite materials prepared in comparative example 1 and examples 14 to 23.
2. Volume resistivity test
The volume resistivity of each composite material was tested according to the method of test example 1, 2, volume resistivity test, using the polymer-based heat-conductive composite materials prepared in comparative examples 2 to 3 and examples 14 to 23.
Second, test results
1. The heat-conducting property of the polymer-based heat-conducting composite material
Table 8 shows the thermal conductivity (thermal conductivity) of the polymer-based thermally conductive composite material prepared with the boron nitride particle size of 5 μm (examples 14 to 18), and Table 9 shows the thermal conductivity (thermal conductivity) of the polymer-based thermally conductive composite material prepared with the boron nitride particle size of 30 μm (examples 19 to 23).
TABLE 8 thermal conductivity of Polymer-based thermally conductive composites of the present invention (h-BN05)
Figure BDA0002297099010000091
TABLE 9 thermal conductivity of Polymer-based thermally conductive composites of the invention (h-BN30)
Figure BDA0002297099010000092
From the test results, it can be seen that, with h-BN: the increase of the Cu ratio leads the thermal conductivity of the material to show an upward trend, and the thermal conductivity is improved. When the filler is Cu powder with the volume fraction of 30% (comparative example 1), the thermal conductivity of the prepared composite material is 1.416W/(m.K), the thermal conductivity of the composite material prepared by compounding boron nitride with different particle sizes and Cu as the filler is obviously higher than that of the composite material prepared by the comparative example 1, and the synergistic effect is shown.
Meanwhile, the sheet diameter of the h-BN has certain influence on the heat conductivity of the composite system. When the ratio of BN to Cu is less than or equal to 1, the thermal conductivity of the h-BN30/Cu system is higher than that of h-BN 05/Cu; in contrast, when BN: Cu > 1, the ratio is h-BN30 with respect to the major diameter. In conclusion, the small-sheet-diameter h-BN05 contributes to the thermal conductivity of the composite system more obviously.
The results of the test pieces show that: the heat conductivity of HDPE can be improved by compounding boron nitride and Cu. Particularly, boron nitride and Cu are compounded in a specific ratio (the volume fraction ratio of boron nitride to Cu is 3:1), the thermal conductivity of the prepared HDPE composite material is remarkably improved, the thermal conductivity is better than that of the HDPE composite material enhanced by singly using copper, a synergistic effect is reflected, and at the moment, the boron nitride with small particle size is more beneficial to the improvement of the thermal conductivity.
2. The volume resistivity of the polymer-based heat-conducting composite material of the invention
FIG. 3 shows the results of the volume resistivity of HDPE obtained by compounding Cu powder with h-BN, wherein the volume fractions of the Cu powder and the h-BN are 30%. As can be seen from FIG. 3, the volume resistivity of each sample was maintained at 1014Omega cm or more; along with the increase of the volume fraction of boron nitride substituted Cu particles in a compound system, the volume resistivity of the compound system is gradually improved, and the application requirements of the fields of electronics, electricity and the like on the insulating and heat conducting materials are met.
In conclusion, the polymer-based heat-conducting composite material disclosed by the invention takes copper and heat-conducting insulating filler silicon carbide or boron nitride as a filler, so that the heat-conducting property of the polymer material is obviously improved. Particularly, copper and the heat-conducting insulating filler are compounded in a specific proportion, so that the heat conductivity of the prepared high-density polyethylene composite material is obviously improved, the heat-conducting property is better than that of the high-density polyethylene composite material enhanced by singly using copper, and the synergistic effect is reflected. Meanwhile, the polymer-based heat-conducting composite material disclosed by the invention is excellent in comprehensive performance and high in resistivity, can be applied to heat diffusion in occasions with higher requirements on electrical insulation performance and other occasions requiring heat diffusion management, and has good market prospect in the fields of preparing heat-conducting and heat-dissipating materials, microelectronic, electrical and electronic, light-emitting diodes, heat exchange engineering, solar energy, lithium batteries, automobiles, aerospace and the like. In addition, the polymer-based heat-conducting composite material disclosed by the invention is simple in preparation process, excellent in processing performance and capable of being practically applied in a large scale.

Claims (10)

1. A polymer-based thermally conductive composite characterized by: the material is prepared from the following raw materials in percentage by volume: 5-30% of metal-based heat-conducting and electric-conducting filler, 5-30% of ceramic-based heat-conducting and electric-insulating filler and 40-90% of matrix.
2. The polymer-based thermally conductive composite of claim 1, wherein: the material is prepared from the following raw materials in percentage by volume: 7.5-22.5% of metal-based heat-conducting and electric-conducting filler, 7.5-22.5% of ceramic-based heat-conducting and insulating filler and 70% of matrix;
preferably, the material is prepared from the following raw materials in volume fraction: 7.5% of metal-based heat and electricity conducting filler, 22.5% of ceramic-based heat and electricity conducting and insulating filler and 70% of matrix.
3. The polymer-based thermally conductive composite of claim 2, wherein: the metal-based heat-conducting and electric-conducting filler is copper, silver, gold, aluminum, tungsten, nickel or iron; the ceramic-based heat-conducting insulating filler is aluminum nitride, beryllium oxide, SiC whiskers or boron nitride; the matrix is thermoplastic plastic, rubber or thermosetting plastic;
preferably, the copper is copper powder; the thermoplastic plastic is nylon, polyformaldehyde, polyphenylene sulfide or high-density polyethylene; the rubber is natural rubber, ethylene propylene diene monomer or silicone rubber; the thermosetting plastic is epoxy resin or polyester.
4. The polymer-based thermally conductive composite of claim 3, wherein: the physical property parameters of the SiC whisker are as follows: the diameter is 1-30 mu m, the length-diameter ratio is more than 20, the SiC content is more than 96%, and the axial thermal conductivity is 100-500W/(m.K);
the boron nitride is hexagonal boron nitride, and the particle size of the hexagonal boron nitride is 5-50 microns;
the copper powder is atomized copper powder, and the atomized copper powder is sieved by a 325-mesh sieve;
the high-density polyethylene is 5000S high-density polyethylene;
preferably, the hexagonal boron nitride has a particle size of 30 μm or 5 μm.
5. The polymer-based thermally conductive composite material according to any one of claims 1 to 4, wherein: the preparation method of the polymer-based heat-conducting composite material comprises the following steps:
placing the high-density polyethylene granules in a preheated double-roller open mill until the high-density polyethylene granules are completely melted and wrapped, adding copper and heat-conducting insulating filler, mixing, thinly passing to obtain a blend, and forming the blend to obtain the polyethylene heat-conducting heat-insulating.
6. The polymer-based thermally conductive composite of claim 5, wherein:
the temperature of a double roller in the double-roller open mill is 100-350 ℃;
and/or the preheating time is 1-10 min;
and/or the mixing is carried out for 3-10 times at a roll spacing of 0.5-2 mm;
and/or the thin passing is performed 3-10 times at a roll gap of 0.5-2 mm;
and/or, the molding is compression molding by a flat vulcanizing machine;
preferably, the first and second electrodes are formed of a metal,
the temperature of a double roller in the double-roller open mill is 150-230 ℃;
more preferably still, the first and second liquid crystal compositions are,
the temperature of the double rollers in the double-roller open mill is 160 +/-10 ℃;
and/or the preheating time is 3 min;
and/or the mixing is carried out for 6 times at a roll spacing of 1.2 mm;
and/or the thin passing is performed 6 times at a roll spacing of 0.8 mm;
and/or the pressure of the die pressing is set to be 10MPa, the die pressing temperature is 190 ℃, and the time is 5 min.
7. A method for preparing the polymer-based heat-conducting composite material as claimed in any one of claims 1 to 6, wherein: it comprises the following steps:
placing the high-density polyethylene granules in a preheated double-roller open mill until the high-density polyethylene granules are completely melted and wrapped, adding copper and heat-conducting insulating filler, mixing, thinly passing to obtain a blend, and forming the blend to obtain the polyethylene heat-conducting heat-insulating.
8. The method of claim 7, wherein:
the temperature of a double roller in the double-roller open mill is 100-350 ℃;
and/or the preheating time is 1-10 min;
and/or the mixing is carried out for 3-10 times at a roll spacing of 0.5-2 mm;
and/or the thin passing is performed 3-10 times at a roll gap of 0.5-2 mm;
and/or, the molding is compression molding by a flat vulcanizing machine;
preferably, the first and second electrodes are formed of a metal,
the temperature of a double roller in the double-roller open mill is 150-230 ℃;
more preferably still, the first and second liquid crystal compositions are,
the temperature of the double rollers in the double-roller open mill is 160 +/-10 ℃;
and/or the preheating time is 3 min;
and/or the mixing is carried out for 6 times at a roll spacing of 1.2 mm;
and/or the thin passing is performed 6 times at a roll spacing of 0.8 mm;
and/or the pressure of the die pressing is set to be 10MPa, the die pressing temperature is 190 ℃, and the time is 5 min.
9. Use of the polymer-based thermally conductive composite material according to any one of claims 1 to 6 for the preparation of a thermally conductive material; preferably, the heat conducting material is an insulating heat conducting material.
10. Use according to claim 9, characterized in that: the insulating heat conduction material is applied to the fields of microelectronics, electrician electricity, light emitting diodes, heat exchange engineering, solar energy, lithium batteries, automobiles and aerospace.
CN201911206797.XA 2019-11-29 2019-11-29 Polymer-based heat-conducting composite material and preparation method and application thereof Pending CN110835432A (en)

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