CN117126489A - Oriented crystal and multidimensional filler synergistic heat conduction composite material and preparation method and application thereof - Google Patents
Oriented crystal and multidimensional filler synergistic heat conduction composite material and preparation method and application thereof Download PDFInfo
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- CN117126489A CN117126489A CN202311023464.XA CN202311023464A CN117126489A CN 117126489 A CN117126489 A CN 117126489A CN 202311023464 A CN202311023464 A CN 202311023464A CN 117126489 A CN117126489 A CN 117126489A
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- 239000000945 filler Substances 0.000 title claims abstract description 65
- 239000002131 composite material Substances 0.000 title claims abstract description 51
- 239000013078 crystal Substances 0.000 title claims abstract description 30
- 230000002195 synergetic effect Effects 0.000 title claims abstract description 25
- 238000002360 preparation method Methods 0.000 title claims abstract description 13
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims abstract description 26
- 229910052582 BN Inorganic materials 0.000 claims abstract description 25
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 22
- 229920000642 polymer Polymers 0.000 claims abstract description 22
- 239000002041 carbon nanotube Substances 0.000 claims abstract description 17
- 229910021393 carbon nanotube Inorganic materials 0.000 claims abstract description 16
- 238000000034 method Methods 0.000 claims abstract description 13
- 238000002156 mixing Methods 0.000 claims abstract description 8
- 238000002844 melting Methods 0.000 claims abstract description 7
- 230000008018 melting Effects 0.000 claims abstract description 7
- 229910021389 graphene Inorganic materials 0.000 claims abstract description 6
- 239000000835 fiber Substances 0.000 claims abstract description 3
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims abstract description 3
- 229910010271 silicon carbide Inorganic materials 0.000 claims abstract description 3
- 229920001903 high density polyethylene Polymers 0.000 claims description 15
- 239000004700 high-density polyethylene Substances 0.000 claims description 15
- 239000000463 material Substances 0.000 claims description 11
- 239000002245 particle Substances 0.000 claims description 9
- 239000004743 Polypropylene Substances 0.000 claims description 4
- 229920000747 poly(lactic acid) Polymers 0.000 claims description 4
- 239000004626 polylactic acid Substances 0.000 claims description 4
- -1 polypropylene Polymers 0.000 claims description 4
- 229920001155 polypropylene Polymers 0.000 claims description 4
- 238000010008 shearing Methods 0.000 abstract description 13
- 101100453790 Drosophila melanogaster Kebab gene Proteins 0.000 abstract description 4
- 235000015231 kebab Nutrition 0.000 abstract description 4
- 239000002861 polymer material Substances 0.000 abstract description 4
- 239000004020 conductor Substances 0.000 abstract description 3
- 230000006872 improvement Effects 0.000 abstract description 3
- 230000008569 process Effects 0.000 abstract description 3
- 230000000052 comparative effect Effects 0.000 description 12
- 238000004519 manufacturing process Methods 0.000 description 5
- 230000006835 compression Effects 0.000 description 4
- 238000007906 compression Methods 0.000 description 4
- 230000007246 mechanism Effects 0.000 description 4
- 230000004048 modification Effects 0.000 description 4
- 238000012986 modification Methods 0.000 description 4
- 238000003723 Smelting Methods 0.000 description 3
- 238000011068 loading method Methods 0.000 description 3
- 230000009471 action Effects 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 239000011231 conductive filler Substances 0.000 description 2
- 229920001940 conductive polymer Polymers 0.000 description 2
- 238000000280 densification Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000008187 granular material Substances 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- LNKJESSHRFPVPE-UHFFFAOYSA-N 5-(diethylamino)pentyl 3,4,5-trimethoxybenzoate;hydrochloride Chemical compound Cl.CCN(CC)CCCCCOC(=O)C1=CC(OC)=C(OC)C(OC)=C1 LNKJESSHRFPVPE-UHFFFAOYSA-N 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000002322 conducting polymer Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 230000003014 reinforcing effect Effects 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/02—Elements
- C08K3/04—Carbon
- C08K3/041—Carbon nanotubes
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/02—Elements
- C08K3/04—Carbon
- C08K3/042—Graphene or derivatives, e.g. graphene oxides
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/38—Boron-containing compounds
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K3/00—Use of inorganic substances as compounding ingredients
- C08K3/38—Boron-containing compounds
- C08K2003/382—Boron-containing compounds and nitrogen
- C08K2003/385—Binary compounds of nitrogen with boron
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K2201/00—Specific properties of additives
- C08K2201/011—Nanostructured additives
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2203/00—Applications
- C08L2203/20—Applications use in electrical or conductive gadgets
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2207/00—Properties characterising the ingredient of the composition
- C08L2207/06—Properties of polyethylene
- C08L2207/062—HDPE
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- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
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- Engineering & Computer Science (AREA)
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- Nanotechnology (AREA)
- Compositions Of Macromolecular Compounds (AREA)
- Processing And Handling Of Plastics And Other Materials For Molding In General (AREA)
Abstract
The invention belongs to the field of high polymer materials, and particularly relates to an oriented crystal and multidimensional filler synergistic heat conduction composite material, a preparation method and application thereof; the preparation method comprises the steps of uniformly mixing a crystalline polymer and a heat conducting filler accounting for 1-40wt% of the mass of the crystalline polymer in a melting way, and then applying a circumferential shearing field to obtain the heat conducting material; the heat-conducting filler comprises a one-dimensional filler and a two-dimensional filler, the one-dimensional filler comprises carbon nanotubes or silicon carbide fibers, and the two-dimensional filler comprises hexagonal boron nitride or graphene. According to the invention, a unique shish-kebab serial crystal structure is constructed for the composite material, a double-filler system is dispersed and oriented in a fixed manner, the ternary synergistic effect among the one-dimensional filler, the two-dimensional filler and the oriented crystal effectively reduces the threshold value of heat conductivity improvement, the mechanical property and heat conductivity of the composite material in the shish and kebab directions are improved, and the process is simple and easy to popularize.
Description
Technical Field
The invention belongs to the field of high polymer materials, and particularly relates to an oriented crystal and multidimensional filler synergistic heat conduction composite material, a preparation method and application thereof.
Background
With the development of the electronic information field, the high-heat-conductivity composite material becomes an important medium for fast heat dissipation of electronic devices. Typically, the intrinsic polymer has a Thermal Conductivity (TC) of less than 0.4W/(mK), which cannot meet the application requirements in the field of electronic devices. A common method of reinforcing TC is to incorporate a large amount of thermally conductive fillers, such as ceramic fillers, graphene, metal fillers, and the like, into the polymer matrix. Although this approach increases thermal conductivity to some extent, randomly dispersed fillers are hindered and isolated by the polymer chains, forming islands-in-the-sea structures. This creates a thermal barrier for the directional transport of phonons, making the high thermal conductivity inherent in the filler underutilized. At the same time, large loadings of thermally conductive filler tend to significantly reduce the mechanical properties of the composite, which will reduce the length of service of the material and increase the iteration frequency.
As such, the production of polymer composites having both excellent thermal conductivity and mechanical properties remains a challenge due to the need to trade off between high filler content and strength loss.
Chinese patent No. 113045813a discloses a heat conductive polymer composite material, in which a material having a shish-kebab serial crystal structure is first prepared from a crystalline polymer and a two-dimensional filler, and then the obtained material is subjected to thermal compression along the kebab direction to increase the degree of densification of the crystal and further orientation of the two-dimensional filler, thereby realizing simultaneous improvement of mechanical properties and thermal conductivity, but in general, the composite material has a complicated process and insufficient thermal conductivity, and is limited in use in high-end manufacture.
Disclosure of Invention
The invention aims to overcome the defects and provide the synergistic heat conduction composite material of the oriented crystal and the multidimensional filler, so that the effect of further improving the heat conductivity is realized on the basis of ensuring the mechanical strength of the material.
The aim of the invention is realized by the following technical scheme:
a preparation method of oriented crystal and multidimensional filler synergistic heat conduction composite material comprises the steps of evenly mixing crystalline polymer and heat conduction filler accounting for 1-40wt% of the crystalline polymer in a melting way, and then applying a circumferential shear field to obtain the material;
the heat-conducting filler comprises a one-dimensional filler and a two-dimensional filler, the one-dimensional filler comprises carbon nanotubes or silicon carbide fibers, and the two-dimensional filler comprises hexagonal boron nitride or graphene.
Further, after the crystalline polymer and the heat conducting filler accounting for 1-25wt% of the mass of the crystalline polymer are melted and mixed uniformly, the mixture is subjected to circumferential shearing field to obtain the heat conducting material.
Further, the one-dimensional filler accounts for 0.5 to 5 weight percent of the crystalline polymer mass, and the two-dimensional filler accounts for 0.5 to 20 weight percent of the crystalline polymer mass.
Further, the crystalline polymer includes high density polyethylene, polypropylene or polylactic acid.
Further, the average length of the one-dimensional filler is 20-50 mu m, and the average diameter is 5-20nm.
Further, the particle size of the two-dimensional filler is 100nm-10 μm.
Further, the melt mixing is carried out by a double screw extruder, and the temperature of the extruder is controlled to be 160-235 ℃.
Further, the circumferential shearing field is applied by a rotary shearing device, which is a rotary pipe making device disclosed in patent application number 2019110377859, and comprises an extruder, a motor, an upper die, a lower die, a core rod, a rotary conductive mechanism, a cooling mechanism and an electric box. Wherein the screw speed of the extruder is 6-15Hz, the holding pressure is 3-8MPa, the die temperature is 140-180 ℃, the rotating speed of the core rod is 2-15rpm, and the shearing time of the core rod is 2-8min.
The method can lead the composite material to form a serial crystal structure, and is favorable for fully dispersing and regulating orientation distribution of the multi-dimensional heat conducting material.
The invention also provides the oriented crystal and multidimensional filler synergistic heat conduction composite material obtained by the preparation method.
Further, the composite material has a shish-kebab serial crystal structure.
The invention also provides application of the oriented crystal and multidimensional filler synergistic heat conduction composite material in electronic devices.
The beneficial effects of the invention are as follows:
1. according to the invention, a unique shish-kebab serial crystal structure is constructed for the composite material, a double-filler system is dispersed and oriented in a fixed manner, and the ternary synergistic effect among the one-dimensional filler, the two-dimensional filler and the oriented crystal effectively reduces the threshold value of heat conductivity improvement, so that the mechanical property and heat conductivity of the composite material in the shish and kebab directions are improved;
2. compared with the patent CN113045813A, the composite material provided by the invention has higher heat conductivity while ensuring mechanical strength, and in the preparation method, the process is simplified due to the omission of thermal compression of the material, and the composite material is easier to popularize.
Drawings
FIG. 1 is a schematic diagram of the mechanism of the enhancement of mechanical properties and thermal conductivity of the composite material of the present invention.
Detailed Description
The technical solution of the present invention will be described in further detail with reference to the accompanying drawings, but the scope of the present invention is not limited to the following description.
Example 1
A preparation method of a synergistic heat-conducting composite material of oriented crystals and multidimensional fillers comprises the steps of uniformly melting and mixing polypropylene (purchased from Shanxi institute of fine chemical industry, brand TMB-5) with 1wt% of carbon nano tubes and 5wt% of hexagonal boron nitride of polypropylene by mass at about 200 ℃ through a double screw extruder, granulating, and then applying an annular shearing field with the rotating speed of 8rpm to the obtained particles by adopting a rotary pipe making device disclosed in patent application number 2019110377859 to obtain the composite material.
Wherein the average length of the carbon nano tube is 35-50 mu m, the average diameter is 15-20nm, the particle size of the hexagonal boron nitride is 1-10 mu m, and the temperature of the upper die and the lower die of the rotary pipe making device is 150 ℃.
Example 2
A preparation method of a synergistic heat-conducting composite material of oriented crystals and multidimensional fillers comprises the steps of uniformly melting and mixing polylactic acid (purchased from NeQIWok under the brand 4032D) with carbon nano tubes of 20 weight percent and graphene of 20 weight percent of the mass of the polylactic acid at about 200 ℃ through a double screw extruder, granulating, and then applying an annular shearing field with the rotating speed of 8rpm to the obtained granules by adopting a rotary pipe making device disclosed in patent application number 2019110377859 to obtain the composite material.
Wherein the average length of the carbon nano tube is 20-35 mu m, the average diameter is 5-10nm, the particle size of the graphene is 100nm-1 mu m, and the temperature of an upper die and a lower die of the rotary pipe making device is 150 ℃.
Example 3
A preparation method of a synergistic heat-conducting composite material of oriented crystals and multidimensional fillers comprises the steps of uniformly melting and mixing high-density polyethylene (purchased from Jilin petrochemical industry, JHMGC 100S) with 5 weight percent of carbon nano tubes and 20 weight percent of hexagonal boron nitride by mass of the high-density polyethylene at about 200 ℃ through a double-screw extruder, granulating, and then applying an annular shearing field with the rotating speed of 8rpm to the obtained particles by adopting a rotary pipe making device disclosed in patent application number 2019110377859 to obtain the composite material.
Wherein the average length of the carbon nano tube is 35-50 mu m, the average diameter is 15-20nm, the particle size of the hexagonal boron nitride is 1-10 mu m, and the temperature of the upper die and the lower die of the rotary pipe making device is 150 ℃.
Comparative example 1
A process for preparing high-molecular material includes such steps as smelting high-density polyethylene by twin-screw extruder at 200 deg.C, granulating, and applying 8rpm shearing field to obtain composite material.
The difference between comparative example 1 and example 4, in which the upper and lower molds of the rotary pipe making apparatus had a temperature of 150 ℃, is that no filler was added to the polymer material.
Comparative example 2
A process for preparing high-molecular composite material includes such steps as smelting high-density polyethylene and hexagonal boron nitride (20 wt.%) by mass of high-density polyethylene at 200 deg.C, granulating, and applying 8rpm shearing field to obtain composite material.
Wherein the particle size of the hexagonal boron nitride is 1-10 mu m, the temperature of the upper die and the lower die of the rotary pipe making device is 150 ℃, and the difference between the comparative example 2 and the example 4 is that one-dimensional filler is not added into the composite material.
Comparative example 3
A process for preparing high-molecular composite material includes such steps as smelting high-density polyethylene and carbon nanotubes (5 wt.%) by mass of high-density polyethylene at 200 deg.C, granulating, and applying a shearing field at 8rpm to obtain composite material.
Wherein the average length of the carbon nano tube is 35-50 mu m, the average diameter is 15-20nm, the temperature of the upper die and the lower die of the rotary pipe making device is 150 ℃, and the difference between the comparative example 3 and the example 4 is that no two-dimensional filler is added into the composite material.
Comparative example 4
A preparation method of a polymer composite material comprises the steps of uniformly melting and mixing high-density polyethylene, carbon Nano Tubes (CNT) accounting for 5wt% of the mass of the high-density polyethylene and hexagonal Boron Nitride (BN) accounting for 20wt% of the mass of the high-density polyethylene at about 200 ℃ through a double-screw extruder, granulating, and then putting the obtained granules into a rotary pipe making device disclosed in the patent application number 2019110377859 without applying a circumferential shearing field to obtain the composite material.
Wherein the average length of the carbon nanotubes is 35-50 μm, the average diameter is 15-20nm, the particle size of the hexagonal boron nitride is 1-10 μm, the upper and lower mold temperatures of the rotary pipe making device are 150 ℃, and the comparative example 4 is different from the example 4 in that the comparative example 4 does not apply a circumferential shear field to the material.
Comparative example 5
A polymer composite is prepared by the method described in patent CN 113045813A.
The method comprises the following steps: preparing a material with a shish-kebab serial crystal structure from high-density polyethylene and hexagonal boron nitride accounting for 20wt% of the mass of the high-density polyethylene, and then carrying out thermal compression treatment on the obtained material along the kebab direction to obtain the heat-conducting polymer composite material.
The polymer materials prepared in the above examples and comparative examples were subjected to mechanical properties and thermal conductivity tests, and the test results are shown in table 1 below.
TABLE 1
According to the analysis of the table 1, the composite material obtained by the invention has the advantages of greatly improving the heat conductivity, maintaining excellent mechanical properties and having remarkable benefit compared with the prior art.
The mechanism of the invention is shown in figure 1, and under the action of the circumferential shear field, entangled polymer chains are oriented along the shear field and form an interlocked 'sh-kebab' structure after stretching. With the loading of the BN plate, the enhanced heat conduction network is provided with BN and a 'hash-kebab' structure which are arranged in an oriented way under the shearing modification effect. In particular, the oriented BN is considered as a connection anchor between adjacent "sh-kebab" structures, forming a thermal path of "aligned BN" - "sh-kebab" - "aligned BN" during thermal conduction. Based on the above thermal network, further loading CNTs acts as a thermal bridge, connecting not only the interlocked "sh-kebab" structure, but also the aligned BN plates. The in-plane heat conduction path becomes "aligned BN" - "sh-kebab" - "elongated CNT" or "aligned BN" - "elongated CNT" - "aligned BN", and the ternary synergistic effect is combined to greatly increase the thermal conductivity.
For comparative example 5, only single-component boron nitride is added into high-density polyethylene, a heat conduction network of a sh-kebab and an oriented crystal of an oriented BN and single boron nitride is formed under the action of a rotary shear field, and the thermal compression treatment is used for enhancing the degree of crystal densification and the degree of orientation of the boron nitride, and belongs to a binary synergistic heat conduction path of the sh-kebab and the BN.
The foregoing is merely a preferred embodiment of the invention, and it is to be understood that the invention is not limited to the form disclosed herein but is not to be construed as excluding other embodiments, but is capable of numerous other combinations, modifications and environments and is capable of modifications within the scope of the inventive concept, either as taught or as a matter of routine skill or knowledge in the relevant art. And that modifications and variations which do not depart from the spirit and scope of the invention are intended to be within the scope of the appended claims.
Claims (9)
1. A preparation method of an oriented crystal and multidimensional filler synergistic heat conduction composite material is characterized in that a crystalline polymer and a heat conduction filler accounting for 1-40wt% of the mass of the crystalline polymer are melted and mixed uniformly, and then a circumferential shear field is applied to obtain the material;
the heat-conducting filler comprises a one-dimensional filler and a two-dimensional filler, the one-dimensional filler comprises carbon nanotubes or silicon carbide fibers, and the two-dimensional filler comprises hexagonal boron nitride or graphene.
2. The method for preparing the oriented crystal and multidimensional filler synergistic heat conduction composite material according to claim 1, wherein the oriented crystal and multidimensional filler synergistic heat conduction composite material is obtained by evenly melting and mixing a crystalline polymer and a heat conduction filler accounting for 1-25wt% of the crystalline polymer, and then applying a circumferential shear field.
3. The method for preparing the oriented crystal and multidimensional filler synergistic heat conduction composite material according to claim 2, wherein the one-dimensional filler accounts for 0.5-5wt% of the crystalline high molecular mass, and the two-dimensional filler accounts for 0.5-20wt% of the crystalline high molecular mass.
4. The method for preparing the oriented crystal and multidimensional filler synergistic heat conduction composite material according to claim 1, wherein the crystalline polymer comprises high-density polyethylene, polypropylene or polylactic acid.
5. The method for preparing the oriented crystal and multidimensional filler synergistic heat conduction composite material according to claim 1, wherein the average length of the one-dimensional filler is 20-50 μm, and the average diameter is 5-20nm.
6. The method for preparing the oriented crystal and multidimensional filler synergistic heat conduction composite material according to claim 1, wherein the particle size of the two-dimensional filler is 100nm-10 μm.
7. An oriented crystalline and multidimensional filler synergistic thermally conductive composite material obtained by the method of any one of claims 1-6.
8. An oriented crystalline and multidimensional filler synergistic thermally conductive composite material as claimed in claim 7, characterized in that the composite material has a shish-kebab string crystal structure.
9. Use of an oriented crystalline and multidimensional filler synergistic thermally conductive composite material according to claim 7 or 8 in an electronic device.
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| Application Number | Priority Date | Filing Date | Title |
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| CN202311023464.XA CN117126489A (en) | 2023-08-15 | 2023-08-15 | Oriented crystal and multidimensional filler synergistic heat conduction composite material and preparation method and application thereof |
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| Application Number | Priority Date | Filing Date | Title |
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| CN202311023464.XA CN117126489A (en) | 2023-08-15 | 2023-08-15 | Oriented crystal and multidimensional filler synergistic heat conduction composite material and preparation method and application thereof |
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