CN115678253A - Polyurethane composite material and preparation method thereof - Google Patents
Polyurethane composite material and preparation method thereof Download PDFInfo
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- CN115678253A CN115678253A CN202211436990.4A CN202211436990A CN115678253A CN 115678253 A CN115678253 A CN 115678253A CN 202211436990 A CN202211436990 A CN 202211436990A CN 115678253 A CN115678253 A CN 115678253A
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- 229920002635 polyurethane Polymers 0.000 title claims abstract description 42
- 239000004814 polyurethane Substances 0.000 title claims abstract description 42
- 239000002131 composite material Substances 0.000 title claims abstract description 39
- 238000002360 preparation method Methods 0.000 title claims abstract description 12
- 239000000945 filler Substances 0.000 claims abstract description 39
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 claims abstract description 21
- 239000003063 flame retardant Substances 0.000 claims abstract description 21
- 239000003365 glass fiber Substances 0.000 claims abstract description 21
- 239000002002 slurry Substances 0.000 claims abstract description 16
- 239000011159 matrix material Substances 0.000 claims abstract description 13
- 229920005749 polyurethane resin Polymers 0.000 claims abstract description 10
- 239000000919 ceramic Substances 0.000 claims abstract description 8
- 238000007598 dipping method Methods 0.000 claims abstract description 7
- 239000000463 material Substances 0.000 claims abstract description 7
- 238000013329 compounding Methods 0.000 claims abstract description 4
- 238000004537 pulping Methods 0.000 claims abstract description 4
- 238000001035 drying Methods 0.000 claims description 10
- 238000000034 method Methods 0.000 claims description 10
- 239000003607 modifier Substances 0.000 claims description 9
- 239000004433 Thermoplastic polyurethane Substances 0.000 claims description 6
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 6
- 239000007822 coupling agent Substances 0.000 claims description 6
- QIQXTHQIDYTFRH-UHFFFAOYSA-N octadecanoic acid Chemical compound CCCCCCCCCCCCCCCCCC(O)=O QIQXTHQIDYTFRH-UHFFFAOYSA-N 0.000 claims description 6
- 229920002803 thermoplastic polyurethane Polymers 0.000 claims description 6
- 239000004114 Ammonium polyphosphate Substances 0.000 claims description 5
- 229910052582 BN Inorganic materials 0.000 claims description 5
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims description 5
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 claims description 5
- 235000019826 ammonium polyphosphate Nutrition 0.000 claims description 5
- 229920001276 ammonium polyphosphate Polymers 0.000 claims description 5
- 238000002791 soaking Methods 0.000 claims description 5
- 239000002202 Polyethylene glycol Substances 0.000 claims description 4
- 239000006087 Silane Coupling Agent Substances 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 4
- VTHJTEIRLNZDEV-UHFFFAOYSA-L magnesium dihydroxide Chemical compound [OH-].[OH-].[Mg+2] VTHJTEIRLNZDEV-UHFFFAOYSA-L 0.000 claims description 4
- 239000000347 magnesium hydroxide Substances 0.000 claims description 4
- 229910001862 magnesium hydroxide Inorganic materials 0.000 claims description 4
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 4
- 229920001223 polyethylene glycol Polymers 0.000 claims description 4
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims description 4
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 4
- 239000007787 solid Substances 0.000 claims description 4
- 238000001291 vacuum drying Methods 0.000 claims description 4
- WRIDQFICGBMAFQ-UHFFFAOYSA-N (E)-8-Octadecenoic acid Natural products CCCCCCCCCC=CCCCCCCC(O)=O WRIDQFICGBMAFQ-UHFFFAOYSA-N 0.000 claims description 3
- LQJBNNIYVWPHFW-UHFFFAOYSA-N 20:1omega9c fatty acid Natural products CCCCCCCCCCC=CCCCCCCCC(O)=O LQJBNNIYVWPHFW-UHFFFAOYSA-N 0.000 claims description 3
- QSBYPNXLFMSGKH-UHFFFAOYSA-N 9-Heptadecensaeure Natural products CCCCCCCC=CCCCCCCCC(O)=O QSBYPNXLFMSGKH-UHFFFAOYSA-N 0.000 claims description 3
- ZQPPMHVWECSIRJ-UHFFFAOYSA-N Oleic acid Natural products CCCCCCCCC=CCCCCCCCC(O)=O ZQPPMHVWECSIRJ-UHFFFAOYSA-N 0.000 claims description 3
- 239000005642 Oleic acid Substances 0.000 claims description 3
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims description 3
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 3
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 3
- 235000021355 Stearic acid Nutrition 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- 238000007605 air drying Methods 0.000 claims description 3
- 150000004645 aluminates Chemical class 0.000 claims description 3
- 229910001593 boehmite Inorganic materials 0.000 claims description 3
- GUJOJGAPFQRJSV-UHFFFAOYSA-N dialuminum;dioxosilane;oxygen(2-);hydrate Chemical compound O.[O-2].[O-2].[O-2].[Al+3].[Al+3].O=[Si]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O GUJOJGAPFQRJSV-UHFFFAOYSA-N 0.000 claims description 3
- GVGUFUZHNYFZLC-UHFFFAOYSA-N dodecyl benzenesulfonate;sodium Chemical compound [Na].CCCCCCCCCCCCOS(=O)(=O)C1=CC=CC=C1 GVGUFUZHNYFZLC-UHFFFAOYSA-N 0.000 claims description 3
- 239000000839 emulsion Substances 0.000 claims description 3
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 claims description 3
- QXJSBBXBKPUZAA-UHFFFAOYSA-N isooleic acid Natural products CCCCCCCC=CCCCCCCCCC(O)=O QXJSBBXBKPUZAA-UHFFFAOYSA-N 0.000 claims description 3
- 239000000395 magnesium oxide Substances 0.000 claims description 3
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims description 3
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- 229910052901 montmorillonite Inorganic materials 0.000 claims description 3
- OQCDKBAXFALNLD-UHFFFAOYSA-N octadecanoic acid Natural products CCCCCCCC(C)CCCCCCCCC(O)=O OQCDKBAXFALNLD-UHFFFAOYSA-N 0.000 claims description 3
- ZQPPMHVWECSIRJ-KTKRTIGZSA-N oleic acid Chemical compound CCCCCCCC\C=C/CCCCCCCC(O)=O ZQPPMHVWECSIRJ-KTKRTIGZSA-N 0.000 claims description 3
- 239000003960 organic solvent Substances 0.000 claims description 3
- 239000002245 particle Substances 0.000 claims description 3
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 3
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims description 3
- 229940080264 sodium dodecylbenzenesulfonate Drugs 0.000 claims description 3
- 239000008117 stearic acid Substances 0.000 claims description 3
- 238000003756 stirring Methods 0.000 claims description 3
- 239000011787 zinc oxide Substances 0.000 claims description 3
- 230000017525 heat dissipation Effects 0.000 abstract description 5
- 239000012776 electronic material Substances 0.000 abstract description 3
- 238000011031 large-scale manufacturing process Methods 0.000 abstract description 3
- 238000009413 insulation Methods 0.000 abstract description 2
- 229920000642 polymer Polymers 0.000 description 4
- 239000011810 insulating material Substances 0.000 description 3
- 238000011161 development Methods 0.000 description 2
- 238000010292 electrical insulation Methods 0.000 description 2
- 238000005979 thermal decomposition reaction Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 239000002322 conducting polymer Substances 0.000 description 1
- 229920001940 conductive polymer Polymers 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 229910003471 inorganic composite material Inorganic materials 0.000 description 1
- 239000012774 insulation material Substances 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002861 polymer material Substances 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000002787 reinforcement Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
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- Compositions Of Macromolecular Compounds (AREA)
Abstract
The invention discloses a polyurethane composite material and a preparation method thereof, wherein the composite material is mainly formed by compounding a polyurethane resin matrix, a ceramic heat-conducting filler, a flame-retardant filler and glass fibers, and the thickness of the composite material is less than or equal to 5mm. The preparation method of the polyurethane composite material comprises the following steps: pulping; (2) dipping; and (3) forming. According to the invention, the heat-conducting filler, the flame-retardant filler, the reticular glass fiber and the like are simultaneously added into the polyurethane base material, so that the polyurethane composite material with excellent comprehensive performance is obtained, and the polyurethane composite material can be applied to the heat management of electronic materials and has the functions of heat conduction, heat dissipation, insulation, flame retardance, mechanical property enhancement and the like. The invention can flexibly adjust the formula of the slurry and also can flexibly adjust the size of the material through the die to obtain a series of products. The preparation process of the polyurethane-based composite material is short in flow, low in cost and has a large-scale production prospect.
Description
Technical Field
The invention belongs to the technical field of organic-inorganic composite materials, and particularly relates to a polyurethane composite material and a preparation method thereof.
Background
With the development of high power, integration and volume miniaturization of LEDs and electronic devices, the related power devices generate more and more heat, and therefore the first problem to be solved is heat dissipation. If the heat generated by these materials cannot be dissipated in time, the junction temperature of the device will rise, and the working stability and service life of the device will be seriously affected. The polymer-based heat conduction and insulation material can be applied between a heating device and a heat dissipation device and is one of key components of heat management.
Polyurethane is applied in various fields, and has the main advantages of good elasticity, good insulating property and good water resistance on the aspect of being used as a matrix of a heat-conducting insulating material. But its intrinsic thermal conductivity is small, which is not good for heat dissipation. And the polyurethane has low thermal decomposition temperature and is flammable, so that the polyurethane is not suitable for being used in a high-temperature environment. Therefore, when polyurethane is used for power type heat-conducting and insulating materials, it is necessary to improve heat-conducting efficiency, thermal stability, mechanical properties and flame retardant properties, and to maintain excellent electrical insulation properties.
Disclosure of Invention
In order to overcome the defects in the prior art, the invention provides the polyurethane composite material with high heat conduction efficiency, strong thermal stability, good mechanical property, good flame retardant property and excellent electrical insulation property and the preparation method thereof.
In order to solve the technical problems, the invention adopts the following technical scheme: a polyurethane composite material is mainly formed by compounding a polyurethane resin matrix, a ceramic heat-conducting filler, a flame-retardant filler and glass fibers, and the thickness of the composite material is less than or equal to 5mm.
The polyurethane resin matrix is thermoplastic polyurethane, and the solid content of the thermoplastic polyurethane is 10-60%; the ceramic heat-conducting filler is: one or more of aluminum oxide, boron nitride, silicon carbide, silicon nitride, zinc oxide and magnesium oxide, and the grain diameter of the heat-conducting filler is 5-120 mu m; the flame-retardant filler is one or more of ammonium polyphosphate, aluminum hydroxide, magnesium hydroxide, boehmite, red phosphorus and montmorillonite, and the particle size of the flame-retardant filler is 1-80 mu m; the glass fiber is continuous glass fiber and is woven into a net shape, the size of the net is 0.05-0.5 mm, and the thickness is less than or equal to 0.5mm.
A preparation method of a polyurethane composite material comprises the following steps: pulping; (2) dipping; and (3) forming.
The polyurethane resin matrix adopts water-soluble polyurethane or organic solvent type polyurethane emulsion, heat-conducting filler, flame-retardant filler and proper modifier are added, and the mixture is stirred at high speed, the rotating speed is 1000-10000 r/min, and the stirring time is 0.5-24 h, so that the slurry is prepared.
The prepared slurry contains 10-80% of heat-conducting filler and 5-60% of flame-retardant filler by mass; the modifier is one or more of silane coupling agent, sodium dodecyl benzene sulfonate, titanate coupling agent, aluminate coupling agent, polyethylene glycol, polyvinyl alcohol, stearic acid, stearate, oleic acid and the like, and the mass fraction of the addition amount of the modifier is 0.5-10%.
The step (2) is specifically as follows: and (3) soaking the glass fiber woven into a net shape into the slurry to enable the slurry to be uniformly and fully adhered to the glass fiber, and drying to obtain the film.
The temperature of the dipping procedure in the step (2) is 10-80 ℃, and the time is 0.5-24 h; the drying mode is one of natural drying, vacuum drying or forced air drying.
The step (3) is specifically as follows: the multilayer films are stacked together, placed in a mold, and heated and pressurized to obtain a composite material.
The pressure applied in the step (3) is 0.1-50 MPa, the heating temperature is 100-200 ℃, and the forming time is 0.5-24 h.
By adopting the technical scheme, researches show that the ceramic heat-conducting filler comprising aluminum oxide, boron nitride, silicon carbide and the like can not only increase the heat-conducting property of a polymer matrix, but also effectively improve the thermal stability of the polymer matrix, and has better application in heat-conducting polymer composite materials; the flame-retardant filler comprises aluminum hydroxide, magnesium hydroxide, ammonium polyphosphate and the like, can improve the heat resistance and flame retardance of the polymer, and prevent fire caused by high temperature; the continuous glass fiber is compounded with the polymer material after being woven, so that the mechanical property and the thermal stability of the material can be greatly improved. According to the invention, the heat-conducting filler, the flame-retardant filler, the reticular glass fiber and the like are simultaneously added into the polyurethane base material, so that the polyurethane composite material with excellent comprehensive performance is obtained, and the polyurethane composite material can be applied to the heat management of electronic materials and has the functions of heat conduction, heat dissipation, insulation, flame retardance, mechanical property enhancement and the like. The invention can flexibly adjust the formula of the slurry and also can flexibly adjust the size of the material through the die to obtain a series of products.
The technical characteristics of the invention are as follows: 1. according to the working characteristics of the power type electronic material, the polyurethane-based composite material with glass fiber reinforcement, high heat conduction and flame retardance has the advantages that all components are tightly combined, and the effects of various fillers can be well exerted. 2. The preparation process of the polyurethane-based composite material is short in flow, low in cost and has a large-scale production prospect.
The economy of the invention is as follows: with the rapid development of the fields of electronic technology, automobiles, aerospace and the like, integrated and high-power electronic devices are applied more and more, and the heat management of the electronic devices is particularly important, so that the heat-conducting insulating material has a huge market prospect. The composite material has the advantages of good comprehensive performance, simple preparation process and low cost, and is convenient for large-scale production and practical application.
Detailed Description
The polyurethane composite material is mainly formed by compounding a polyurethane resin matrix, a ceramic heat-conducting filler, a flame-retardant filler and glass fibers, and the thickness of the composite material is less than or equal to 5mm.
The polyurethane resin matrix is thermoplastic polyurethane, and the solid content of the thermoplastic polyurethane is 10-60%; the ceramic heat-conducting filler is as follows: one or more of aluminum oxide, boron nitride, silicon carbide, silicon nitride, zinc oxide and magnesium oxide, and the grain diameter of the heat-conducting filler is 5-120 mu m; the flame-retardant filler is one or more of ammonium polyphosphate, aluminum hydroxide, magnesium hydroxide, boehmite, red phosphorus and montmorillonite, and the particle size of the flame-retardant filler is 1-80 mu m; the glass fiber is continuous glass fiber and is woven into a net shape, the size of the net is 0.05-0.5 mm, and the thickness is less than or equal to 0.5mm.
A preparation method of a polyurethane composite material comprises the following steps: pulping; (2) dipping; and (3) forming.
The polyurethane resin matrix adopts water-soluble polyurethane or organic solvent polyurethane emulsion, heat-conducting filler, flame-retardant filler and proper modifier are added, and the mixture is stirred at high speed, the rotating speed is 1000-10000 r/min, and the stirring time is 0.5-24 h, so that slurry is prepared.
The prepared slurry contains 10-80% of heat-conducting filler and 5-60% of flame-retardant filler by mass; the modifier is one or more of silane coupling agent, sodium dodecyl benzene sulfonate, titanate coupling agent, aluminate coupling agent, polyethylene glycol, polyvinyl alcohol, stearic acid, stearate, oleic acid and the like, and the mass fraction of the addition amount of the modifier is 0.5-10%.
The step (2) is specifically as follows: and (3) soaking the glass fiber woven into a net shape into the slurry to enable the slurry to be uniformly and fully adhered to the glass fiber, and drying to obtain the film.
The temperature of the dipping procedure in the step (2) is 10-80 ℃, and the time is 0.5-24 h; the drying mode is one of natural drying, vacuum drying or forced air drying.
The step (3) is specifically as follows: the multilayer films are stacked together, placed in a mold, and heated and pressurized to obtain a composite material.
The pressure applied in the step (3) is 0.1 to 50MPa, the heating temperature is 100 to 200 ℃, and the forming time is 0.5 to 24 hours.
Experiments for preparing polyurethane composites were carried out in the laboratory, and the specific examples are as follows:
100 parts of waterborne polyurethane and 30% of solid content of polyurethane are added, 40 parts of boron nitride, 20 parts of ammonium polyphosphate, 10 parts of aluminum hydroxide, 3 parts of silane coupling agent and 3 parts of polyethylene glycol are stirred and blended for 2 hours, and the rotating speed is 4000r/min, so that viscous slurry is obtained. And (3) soaking the woven glass fiber net into the slurry, preserving the heat of a water bath kettle at 50 ℃, soaking for 10h, taking out, and drying in a vacuum drying oven to obtain the composite material film. Laminating 6 layers of films, paving the films into a mould for pressing, keeping the pressure at 0.2MPa and the temperature at 130 ℃ for 1h to obtain a smooth composite material film, wherein the thickness of the film is about 2mm, and testing: the thermal conductivity is 1.5W/mK, the tensile strength is improved by 50 percent compared with pure polyurethane, the initial thermal decomposition temperature is improved to 210 ℃ from 180 ℃, and the flame retardance reaches V-0 level.
Although the present invention has been described in detail with reference to the foregoing embodiments, it will be apparent to those skilled in the art that modifications may be made to the embodiments or portions thereof without departing from the spirit and scope of the invention.
Claims (9)
1. A polyurethane composite characterized by: the composite material is mainly formed by compounding a polyurethane resin matrix, a ceramic heat-conducting filler, a flame-retardant filler and glass fibers, and the thickness of the material is less than or equal to 5mm.
2. A polyurethane composite according to claim 1, wherein: the polyurethane resin matrix is thermoplastic polyurethane, and the solid content of the thermoplastic polyurethane is 10-60%; the ceramic heat-conducting filler is: one or more of aluminum oxide, boron nitride, silicon carbide, silicon nitride, zinc oxide and magnesium oxide, and the grain diameter of the heat-conducting filler is 5-120 mu m; the flame-retardant filler is one or more of ammonium polyphosphate, aluminum hydroxide, magnesium hydroxide, boehmite, red phosphorus and montmorillonite, and the particle size of the flame-retardant filler is 1-80 mu m; the glass fiber is continuous glass fiber and is woven into a net shape, the size of the net is 0.05-0.5 mm, and the thickness is less than or equal to 0.5mm.
3. The method for preparing a polyurethane composite material according to claim 2, wherein: the method comprises the following steps: pulping; (2) dipping; and (3) forming.
4. A preparation method of a polyurethane composite material is characterized by comprising the following steps: the step (1) is specifically as follows: the polyurethane resin matrix adopts water-soluble polyurethane or organic solvent type polyurethane emulsion, heat-conducting filler, flame-retardant filler and proper modifier are added, and the mixture is stirred at high speed, the rotating speed is 1000-10000 r/min, and the stirring time is 0.5-24 h, so that the slurry is prepared.
5. The method for preparing a polyurethane composite material according to claim 4, wherein: the prepared slurry contains 10-80% of heat-conducting filler and 5-60% of flame-retardant filler by mass; the modifier is one or more of silane coupling agent, sodium dodecyl benzene sulfonate, titanate coupling agent, aluminate coupling agent, polyethylene glycol, polyvinyl alcohol, stearic acid, stearate, oleic acid and the like, and the mass fraction of the addition amount of the modifier is 0.5-10%.
6. The method for preparing a polyurethane composite material according to claim 5, wherein: the step (2) is specifically as follows: and (3) soaking the glass fiber woven into a net shape into the slurry to enable the slurry to be uniformly and fully adhered to the glass fiber, and drying to obtain the film.
7. The method for preparing a polyurethane composite material according to claim 6, wherein: the temperature of the dipping procedure in the step (2) is 10-80 ℃, and the time is 0.5-24 h; the drying mode is one of natural drying, vacuum drying or forced air drying.
8. The method for preparing a polyurethane composite material according to claim 7, wherein: the step (3) is specifically as follows: the multilayer films are stacked together, placed in a mold, and heated and pressurized to obtain a composite material.
9. The method of claim 8, wherein the polyurethane composite is prepared by the following steps: the pressure applied in the step (3) is 0.1-50 MPa, the heating temperature is 100-200 ℃, and the forming time is 0.5-24 h.
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| CN202211436990.4A CN115678253A (en) | 2022-11-16 | 2022-11-16 | Polyurethane composite material and preparation method thereof |
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| CN202211436990.4A CN115678253A (en) | 2022-11-16 | 2022-11-16 | Polyurethane composite material and preparation method thereof |
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