Impact-resistant high thermal conductive polyphenylene sulfide composite material and preparation method thereof

By introducing high melt viscosity aromatic polyamide and functionalized polysulfone resin into PPS material, and combining melt spinning and solid-phase stretching processes, a PPS composite material with high thermal conductivity and high toughness was prepared. This solved the problem of insufficient thermal conductivity and toughness of PPS material in the fields of electronics, electrical appliances and power batteries, and enabled its application in the fields of national defense and aerospace.

CN121086527BActive Publication Date: 2026-05-08GOODALL MATERIALS TECHNOLOGY (CHUZHOU) CO LTD
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
GOODALL MATERIALS TECHNOLOGY (CHUZHOU) CO LTD
Filing Date
2025-10-09
Publication Date
2026-05-08

AI Technical Summary

Technical Problem

The application of existing polyphenylene sulfide (PPS) materials in the fields of electronics, electrical appliances and power batteries is limited by their low thermal conductivity and poor toughness. Furthermore, existing high thermal conductivity fillers have poor compatibility with PPS resin, which leads to the deterioration of composite material performance.

Method used

High melt viscosity and high temperature resistant aromatic polyamides are used to improve the viscoelasticity of PPS resin, and functionalized polysulfone resin compatibilizers are used to enhance interfacial compatibility. Highly oriented PPS fibers are prepared by melt spinning and solid-phase high-ratio stretching-annealing processes to form a continuous phonon transport path. Combined with injection molding process, impact-resistant and high thermal conductivity composite materials are prepared.

Benefits of technology

The thermal conductivity and impact resistance of PPS composite materials have been improved, with a thermal conductivity of up to 8.45 W/m·K and a notched impact strength of 16.38 kJ/m2 for simply supported beams, thus addressing the application needs of PPS materials in defense, aerospace and other fields.

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Abstract

The application discloses an impact-resistant high-thermal-conductivity polyphenylene sulfide composite material and a preparation method thereof, and relates to the technical field of plastic processing. The preparation method comprises the following steps: S1, preparation of a highly oriented PPS fiber insert; and S2, preparation of the impact-resistant high-thermal-conductivity PPS composite material. The application provides an impact-resistant high-thermal-conductivity PPS composite material and a preparation method thereof. Firstly, the viscoelasticity of PPS resin is improved by using high-melt-viscosity and high-temperature-resistant aromatic polyamide, the interfacial compatibility of PPS / aromatic polyamide is enhanced by using a functionalized polysulfone-based resin as a compatibilizer, so that the stretchability and the tensile orientation degree of PPS are improved; PPS composite fibers are obtained by using a melt spinning machine, and a fiber solid-phase high-multiple-stretching-annealing forming process is established, so that the high-toughness and highly oriented PPS composite fiber material is obtained.
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Description

Technical Field

[0001] This invention relates to the field of plastic processing technology, and in particular to an impact-resistant, high thermal conductivity polyphenylene sulfide composite material and its preparation method. Background Technology

[0002] Polyphenylene sulfide (PPS), a high-temperature resistant crystalline engineering plastic, is one of the thermoplastic resins with the highest thermal stability. It possesses high mechanical strength and modulus, excellent flame retardancy, corrosion resistance, and electrical insulation, making it widely used in electronics, petrochemicals, automobiles, precision machinery, aerospace, and defense. However, PPS suffers from low thermal conductivity and poor toughness, severely limiting its application in electronics, electrical appliances, and power batteries. Current research typically employs the addition of highly thermally conductive fillers to improve thermal conductivity. For example, blending magnesium oxide particles with PPS resin increases the thermal conductivity of the composite material from 0.3 W / m·K for pure PPS resin to 1.93 W / m·K. Chinese patent CN202310488007.1 introduces chopped glass fibers and graphite into a PPS resin composite system, resulting in a PPS composite material with excellent high thermal conductivity and heat dissipation performance. Chinese patent CN202011416113.1 utilizes graphite / silicon carbide / graphene and / or boron nitride composites with PPS resin; the introduction of high-content thermally conductive fillers significantly increases the thermal conductivity of the PPS composite material by 15.35 W / m·K. In summary, fillers used to improve the thermal conductivity of PPS resin are mostly inorganic fillers such as magnesium oxide, graphite, graphene, and silicon carbide. These fillers have poor compatibility with PPS resin, are prone to interfacial debonding, leading to performance degradation of the composite material and limiting its practical application. Summary of the Invention

[0003] The purpose of this invention is to address the shortcomings of existing technologies by providing an impact-resistant, high thermal conductivity polyphenylene sulfide (PPS) composite material and its preparation method. The key feature is the use of a high melt viscosity, high-temperature resistant aromatic polyamide to enhance the viscoelasticity of PPS resin, and a functionalized polysulfone-based resin as a compatibilizer to improve the interfacial compatibility of PPS / aromatic polyamide, thereby improving the stretchability and stretch orientation of PPS. PPS composite fibers are obtained using a melt spinning machine, and a high-strength stretching-annealing process is established to obtain a high-toughness and highly oriented PPS composite fiber material. The highly oriented molecular chains of the stretched PPS composite fibers form continuous phonon transport paths, reducing phonon scattering and thus achieving rapid heat exchange and dissipation. Furthermore, these oriented fibers are bundled into impact-resistant, high thermal conductivity inserts, and the impact-resistant, high thermal conductivity PPS composite material is obtained through injection molding.

[0004] Specifically, the following technical solutions are included:

[0005] In a first aspect, a method for preparing an impact-resistant and highly thermally conductive polyphenylene sulfide composite material is provided, comprising the following steps:

[0006] S1. Preparation of highly oriented PPS fiber inserts: (1) Polysulfone resin, first antioxidant, initiator and active monomer are reacted to obtain functionalized polysulfone resin compatibilizer; (2) PPS, aromatic polyamide, functionalized polysulfone resin compatibilizer and second antioxidant are mixed and melt extruded to obtain composite resin particles; (3) Composite resin particles are melt spun to obtain fiber samples; the fiber samples are subjected to solid-phase super-stretching orientation and high-temperature annealing to obtain highly oriented PPS fibers; (4) The highly oriented PPS fibers are aligned in multiple directions, bundled and then highly oriented PPS fiber inserts are obtained.

[0007] S2. Preparation of impact-resistant and high thermal conductivity PPS composite material: PPS and a third antioxidant are uniformly mixed and then injection molded with highly oriented PPS fiber inserts to obtain impact-resistant and high thermal conductivity PPS composite material.

[0008] Furthermore, in step S1, the fiber sample undergoes solid-phase super-stretching orientation with a stretching ratio of 1500%-2500%.

[0009] Furthermore, in step S1, the highly oriented PPS fiber insert is obtained by aligning 1,000-10,000 highly oriented PPS fibers in multiple directions and bundling them into a specific shape.

[0010] The shape of the highly oriented PPS fiber insert depends on the shape of the product (highly oriented PPS fiber).

[0011] Preferably, the specific shape of the highly oriented PPS fiber insert is any one or a combination of cuboid, cube, cylinder, and irregular shape.

[0012] Further, in step S1, the polysulfone-based resin is one of polyethersulfone, polyphenylsulfone, polyphenylene sulfone, and polyarylethersulfone; the first antioxidant, the second antioxidant, and the third antioxidant are all selected from pentaerythritol tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate], octadecyl β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, 2,6-di-tert-butyl-p-cresol, tris(2,4-di-tert-butylphenyl)phosphite, and bis(2,4-di-tert-butylphenyl)propionate. The initiator is selected from one of pentaerythritol diphosphite, dilauryl thiodipropionate, and N-isopropyl-N'-phenyl-p-phenylenediamine; the initiator is selected from one of azobisisobutyronitrile, benzoyl peroxide, dicumyl peroxide, diisopropyl peroxide, dicyclohexyl peroxide, di(4-tert-butylcyclohexyl) peroxide, di(2-ethylhexyl) peroxide, dimethyl peroxide, diphenyl peroxide, and azobisisobutyronitrile.

[0013] Further, in step S1, the active monomer is selected from one of hydroxyethyl acrylate, hydroxypropyl methacrylate, hydroxyethyl methacrylate, isobutyl methacrylate, n-butyl methacrylate, ethyl methacrylate, 2-ethylhexyl acrylate, methyl methacrylate, glycidyl methacrylate, ethylene glycol dimethacrylate, triethylene glycol dimethacrylate, allyl methacrylate, dimethylaminoethyl methacrylate, and siloxane methacrylate; the aromatic polyamide is selected from one of poly(hexamethylene terephthalamide), poly(hexamethylene isophthalamide / hexamethylene terephthalamide copolymer, poly(decyl terephthalamide), poly(butyl terephthalamide / hexamethylene terephthalamide copolymer, poly(hexamethylene terephthalamide), and poly(nonadiamine terephthalamide).

[0014] Further, in step S1, the functionalized polysulfone resin compatibilizer is obtained by adding 100 parts of polysulfone resin, 0.5-3 parts of the first antioxidant, 0.5-5 parts of the initiator, and 5-30 parts of the active monomer into a mixer and reacting at 300-380°C for 10-30 minutes, by weight; the composite resin particles are obtained by melting and extruding a mixture of 100 parts of PPS, 10-50 parts of aromatic polyamide, 5-30 parts of the functionalized polysulfone resin compatibilizer, and 0.5-5 parts of the second antioxidant into a twin-screw extruder, by weight.

[0015] Further, in step S1, the fiber sample is obtained by melt spinning composite resin particles using a melt spinning machine under the conditions of an extrusion temperature of 320-380℃ and a screw speed of 120-200rpm. The melt spinning temperature is 320-380℃ and the winding speed of the melt spinning is 100-200m / min. The highly oriented PPS fiber is obtained by fixing the fiber sample on a universal testing machine and performing solid-phase super-stretching orientation at 120-200℃. After the stretching ratio reaches 1500%-2500%, the stretching is stopped, and the fiber is then subjected to high-temperature annealing in an oven at 230-250℃ for 1-3 hours.

[0016] Furthermore, in step S1, the highly oriented PPS fiber insert is obtained by aligning 1,000-10,000 highly oriented PPS fibers in multiple directions and bundling them into a specific shape.

[0017] Furthermore, in step S2, the impact-resistant and high thermal conductivity PPS composite material is prepared by uniformly mixing 100 parts PPS and 0.5-5 parts of a third antioxidant by weight and then adding them to the injection molding machine barrel; the highly oriented PPS fiber insert is preheated at 160-220℃ for 20-40 minutes and then laid flat into the injection molding machine mold cavity for injection molding. The injection temperature is 330-380℃, the nozzle temperature is 310-360℃, the mold temperature is 160-220℃, and the injection time is 80-150MPa.

[0018] In a second aspect, an impact-resistant and thermally conductive polyphenylene sulfide composite material is provided, which is prepared by the method for preparing the impact-resistant and thermally conductive polyphenylene sulfide composite material described in the first aspect.

[0019] Preferably, the impact-resistant and high thermal conductivity polyphenylene sulfide composite material has a thermal conductivity of up to 8.45 W / m·K along the fiber (insertion) length and a notched impact strength of up to 16.38 kJ / m². 2 .

[0020] This invention provides an impact-resistant, high thermal conductivity polyphenylene sulfide composite material and its preparation method, with the following advantages:

[0021] (1) High melt viscosity and high temperature resistant aromatic polyamide are used to improve the viscoelasticity of PPS resin. By grafting active substances such as methacrylate onto the polysulfone resin molecular chain, the interfacial compatibility of PPS / aromatic polyamide is enhanced, thereby improving the stretchability and stretch orientation of PPS.

[0022] (2) PPS composite fibers were obtained using a melt spinning machine, and a solid-state high-stretching-annealing molding process was established to obtain high-toughness and highly oriented PPS composite fiber materials. The molecular chains of the PPS composite fibers after solid-state stretching are highly oriented, and a large number of regularly arranged fibrous nanocrystals are formed inside the fibers. These highly oriented crystalline structures can construct continuous phonon transport paths and reduce phonon scattering. Based on this, the oriented fibers are bundled into inserts, so that the inserts have good thermal conductivity along their length direction; at the same time, the highly oriented composite fibers can serve as a reinforcing structure to improve the impact resistance and toughness of the material. Furthermore, the impact-resistant and high thermal conductivity inserts are composited with PPS resin through injection molding. Since the inserts and PPS have similar molecular structures, the bonding ability between the two interfaces is strong, thus obtaining impact-resistant and high thermal conductivity PPS composite materials. Attached Figure Description

[0023] To more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings used in the following description of the embodiments will be briefly introduced. Obviously, the drawings described below are some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0024] Figure 1 This is a schematic diagram illustrating the preparation of the impact-resistant, high thermal conductivity polyphenylene sulfide composite material of Example 1 of the present invention. Detailed Implementation

[0025] The technical solutions in the embodiments of the present invention will be clearly and completely described below. Obviously, the described embodiments are only some, not all, of the embodiments of the present invention. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0026] It should be understood that, when used in this specification and the appended claims, the terms "comprising" and "including" indicate the presence of the described features, integrals, steps, operations, elements and / or components, but do not exclude the presence or addition of one or more other features, integrals, steps, operations, elements, components and / or collections thereof.

[0027] It should also be understood that the terminology used in this specification is for the purpose of describing particular embodiments only and is not intended to limit the invention. As used in this specification and the appended claims, the singular forms “a,” “an,” and “the” are intended to include the plural forms unless the context clearly indicates otherwise.

[0028] It should also be further understood that the term "and / or" as used in this specification and the appended claims refers to any combination of one or more of the associated listed items and all possible combinations, and includes such combinations.

[0029] To better understand the technical content of the present invention, the technical solution of the present invention will be further introduced and explained below with reference to specific embodiments.

[0030] Unless otherwise specified, all parts of raw materials mentioned in this invention are by weight.

[0031] The high thermal conductivity described in this invention refers to a thermal conductivity greater than 6 W / m·K.

[0032] Example 1

[0033] An impact-resistant, high thermal conductivity polyphenylene sulfide composite material is prepared by a method for preparing impact-resistant, high thermal conductivity polyphenylene sulfide composite materials. Figure 1 This is a schematic diagram illustrating the preparation of the impact-resistant, high thermal conductivity polyphenylene sulfide composite material of Example 1 of the present invention.

[0034] The preparation method of the aforementioned impact-resistant and high thermal conductivity polyphenylene sulfide composite material includes the following steps:

[0035] S1. Preparation of highly oriented PPS fiber inserts: By weight, 100 parts of polysulfone resin, 0.5 parts of the first antioxidant (pentaerythritol tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate]), 1 part of initiator (azobisisobutyronitrile), and 10 parts of active monomer (n-butyl methacrylate) were added to a mixer and reacted at 320°C for 30 min to obtain a functionalized polysulfone resin compatibilizer; (2) By weight, 100 parts of PPS, 20 parts of aromatic polyamide (poly(hexamethylene terephthalamide), 10 parts of functionalized polysulfone resin compatibilizer and 0.5 parts of the second antioxidant (pentaerythritol tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate]) were mixed and added to a twin-screw extruder. (3) The composite resin particles were melt-extruded in the machine to obtain composite resin particles; (4) Under the conditions of extrusion temperature of 340℃ and screw speed of 120rpm, the composite resin particles were melt-spun using a melt spinning machine. The melt spinning temperature was 340℃ and the winding speed of melt spinning was 100m / min to obtain fiber samples; The fiber samples were fixed on a universal material testing machine and subjected to solid-phase super-stretching orientation at 120℃. After the stretching ratio reached 1500%, the stretching was stopped, and the samples were subjected to high-temperature annealing in an oven at 230℃ for 3h to obtain highly oriented PPS fibers; (5) 1000 highly oriented PPS fibers were aligned in multiple directions, bundled into a cuboid shape, and then highly oriented PPS fiber inserts were obtained.

[0036] S2. Preparation of impact-resistant and high thermal conductivity PPS composite material: By weight, 100 parts of PPS and 0.5 parts of the third antioxidant (pentaerythritol tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate]) were uniformly mixed and added to the injection molding machine barrel; the highly oriented PPS fiber insert was preheated at 160℃ for 40 min and then laid flat into the injection molding machine mold cavity for injection molding. The injection temperature was 330℃, the nozzle temperature was 315℃, the mold temperature was 160℃, and the injection time was 80 MPa to obtain the impact-resistant and high thermal conductivity PPS composite material.

[0037] Example 2

[0038] An impact-resistant, high thermal conductivity polyphenylene sulfide composite material is prepared by a method for preparing impact-resistant, high thermal conductivity polyphenylene sulfide composite materials.

[0039] The preparation method of the aforementioned impact-resistant and high thermal conductivity polyphenylene sulfide composite material includes the following steps:

[0040] S1. Preparation of highly oriented PPS fiber inserts: By weight, 100 parts of polysulfone resin, 1.2 parts of the first antioxidant (2,6-di-tert-butyl-p-cresol), 2 parts of initiator (dimethyl peroxide dicarbonate), and 20 parts of active monomer (ethylene glycol dimethacrylate) were added to a mixer and reacted at 360°C for 20 min to obtain a functionalized polysulfone resin compatibilizer; (2) By weight, 100 parts of PPS, 30 parts of aromatic polyamide (poly(hexamethylene isophthalamide / hexamethylene terephthalamide copolymer), 15 parts of functionalized polysulfone resin compatibilizer and 1.5 parts of the second antioxidant (2,6-di-tert-butyl-p-cresol) were mixed and melt-extruded in a twin-screw extruder to obtain Composite resin particles; (3) Under the conditions of extrusion temperature of 350℃ and screw speed of 160rpm, the composite resin particles are melt-spun using a melt spinning machine. The melt spinning temperature is 345℃ and the winding speed of melt spinning is 150m / min to obtain fiber samples; The fiber samples are fixed on a universal material testing machine and subjected to solid-phase super-stretching orientation at 150℃. After the stretching ratio reaches 2000%, the stretching is stopped, and the samples are subjected to high-temperature annealing in an oven at 240℃ for 2 hours to obtain highly oriented PPS fibers; (4) 5000 highly oriented PPS fibers are aligned in multiple directions, bundled into a cuboid shape, and then highly oriented PPS fiber inserts are obtained;

[0041] S2. Preparation of impact-resistant and high thermal conductivity PPS composite material: By weight, 100 parts of PPS and 1.5 parts of third antioxidant (2,6-di-tert-butyl-p-cresol) were uniformly mixed and added to the injection molding machine barrel; the highly oriented PPS fiber insert was preheated at 180°C for 30 minutes and then laid flat into the injection molding machine mold cavity for injection molding. The injection temperature was 340°C, the nozzle temperature was 330°C, the mold temperature was 180°C, and the injection time was 110 MPa to obtain the impact-resistant and high thermal conductivity PPS composite material.

[0042] Example 3

[0043] An impact-resistant, high thermal conductivity polyphenylene sulfide composite material is prepared by a method for preparing impact-resistant, high thermal conductivity polyphenylene sulfide composite materials.

[0044] The preparation method of the aforementioned impact-resistant and high thermal conductivity polyphenylene sulfide composite material includes the following steps:

[0045] S1. Preparation of highly oriented PPS fiber inserts: By weight, 100 parts of polysulfone resin, 3 parts of the first antioxidant (tris(2,4-di-tert-butylphenyl) phosphite), 4 parts of initiator (azobisisobutyronitrile), and 30 parts of active monomer (dimethylaminoethyl methacrylate) were added to a mixer and reacted at 380°C for 15 min to obtain a functionalized polysulfone resin compatibilizer; (2) By weight, 100 parts of PPS, 50 parts of aromatic polyamide (poly(hexamethylene phthalamide), 25 parts of functionalized polysulfone resin compatibilizer and 3 parts of the second antioxidant (tris(2,4-di-tert-butylphenyl) phosphite) were mixed and added to a twin-screw extruder for melt extrusion to obtain a composite resin. (3) Under the conditions of extrusion temperature of 370℃ and screw speed of 200rpm, the composite resin particles are melt-spun using a melt spinning machine. The melt spinning temperature is 370℃ and the winding speed of melt spinning is 200m / min to obtain fiber samples. The fiber samples are fixed on a universal material testing machine and subjected to solid-phase super-stretching orientation at 200℃. After the stretching ratio reaches 2500%, the stretching is stopped, and the samples are subjected to high-temperature annealing in an oven at 250℃ for 1h to obtain highly oriented PPS fibers. (4) 10,000 highly oriented PPS fibers are aligned in multiple directions and bundled into a cuboid shape to obtain highly oriented PPS fiber inserts.

[0046] S2. Preparation of impact-resistant and high thermal conductivity PPS composite material: By weight, 100 parts of PPS and 3 parts of third antioxidant (tris(2,4-di-tert-butylphenyl) phosphite) were uniformly mixed and added to the injection molding machine barrel; the highly oriented PPS fiber insert was preheated at 220℃ for 20 min and then laid flat into the injection molding machine mold cavity for injection molding. The injection temperature was 350℃, the nozzle temperature was 335℃, the mold temperature was 220℃, and the injection time was 150 MPa to obtain the impact-resistant and high thermal conductivity PPS composite material.

[0047] Comparative Example 1

[0048] Compared with Example 3, Comparative Example 1 differs in that in step S1, 100 highly oriented PPS fibers are aligned in multiple directions, bundled into a cuboid shape, and then a highly oriented PPS fiber insert is obtained. All other conditions are the same.

[0049] Comparative Example 2

[0050] Compared with Example 3, Comparative Example 2 differs in that step S2 involves obtaining an impact-resistant and thermally conductive PPS composite material by injection molding composite resin particles; all other steps are the same.

[0051] Comparative Example 3

[0052] The difference between Comparative Example 3 and Example 3 is that no functionalized polysulfone resin compatibilizer was added during the preparation process, while all other conditions were the same.

[0053] Comparative Example 4

[0054] Compared with Example 3, Comparative Example 4 differs in that the stretching ratio of the solid phase super-stretching orientation in step S1 is 200%, while all other conditions are the same.

[0055] The impact-resistant and high thermal conductivity PPS composite materials of Examples 1-3 and Comparative Examples 1-4 were tested for thermal conductivity along the fiber (insert) length direction according to GB / T3399 1982 Thermal conductivity of plastics - heat-resistant plate method, and for notched impact strength of simply supported beams according to ISO 179 2000 Plastics - Determination of impact strength of simply supported beams. The test results are shown in Table 1.

[0056] Table 1. Thermal conductivity and notched impact strength of Examples 1-3 and Comparative Examples 1-4

[0057]

[0058] Table 1 shows that for Examples 1-3, functionalized polysulfone resin was used as a compatibilizer to enhance the interfacial compatibility of PPS / aromatic polyamide, thereby improving the stretchability and stretch orientation of PPS. PPS composite fibers were obtained using a melt spinning machine, and a high-strength stretching-annealing process was established to obtain high-toughness and highly oriented PPS composite fiber materials. The molecular chains of the stretched PPS composite fibers are highly oriented, forming continuous phonon transport paths and reducing phonon scattering. Furthermore, these oriented fibers were bundled into impact-resistant, high-thermal-conductivity inserts, and impact-resistant, high-thermal-conductivity PPS composite materials were obtained through injection molding. The impact strength of the composite material reached 13.42-16.38 kJ / m. 2 Its thermal conductivity can reach 6.66-8.45 W / m·K.

[0059] For Comparative Example 1, when only 100 highly oriented PPS fibers were bundled into a multi-directionally aligned cuboid insert, the impact strength of the composite material significantly decreased to 5.54 kJ / m². 2 The thermal conductivity significantly decreased to 0.47 W / m·K. For Comparative Example 2, PPS composite materials were obtained directly from composite resin particles via injection molding. The composite system did not contain impact-resistant, high-thermal-conductivity inserts composed of bundled oriented fibers, and there was no continuous phonon transport path in the composite system. The thermal conductivity of the composite material was only 0.41 W / m·K, and the impact strength decreased to 6.14 kJ / m. 2 For Comparative Example 3, the absence of a functionalized polysulfone resin compatibilizer resulted in weak interfacial interaction between PPS and aromatic polyamide. During the solid-state super-stretching orientation of the composite fiber, interfacial debonding occurred between PPS and aromatic polyamide, making it impossible to obtain an oriented composite fiber with a stretch ratio of 2500%. For Comparative Example 4, the solid-state stretch ratio of the fiber was only 200%, resulting in an excessively low degree of molecular orientation in the fiber inserts, making it impossible to form a continuous phonon transport path. Simultaneously, the low-oriented fiber exhibited lower impact resistance and toughness, leading to a significant decrease in the thermal conductivity of the composite resin to 0.42 W / m·K and an impact strength to 9.53 kJ / m². 2 .

[0060] In summary, this invention provides an impact-resistant, high thermal conductivity PPS composite material and its preparation method. First, a high melt viscosity, high-temperature resistant aromatic polyamide is used to enhance the viscoelasticity of PPS resin. Functionalized polysulfone-based resin is used as a compatibilizer to enhance the interfacial compatibility of PPS / aromatic polyamide, thereby improving the stretchability and stretch orientation of PPS. PPS composite fibers are obtained using a melt spinning machine, and a fiber solid-phase high-stretching-annealing molding process is established to obtain a high-toughness and highly oriented PPS composite fiber material. The highly oriented molecular chains of the stretched PPS composite fibers form continuous phonon transport paths, reducing phonon scattering and enabling rapid heat exchange and dissipation. Furthermore, these oriented fibers are bundled into impact-resistant, high thermal conductivity inserts, and the impact-resistant, high thermal conductivity PPS composite material is obtained through injection molding, showing promising application prospects in defense, aerospace, and other fields.

[0061] The above description is merely a specific embodiment of the present invention, but the scope of protection of the present invention is not limited thereto. Any person skilled in the art can easily conceive of various equivalent modifications or substitutions within the technical scope disclosed in the present invention, and these modifications or substitutions should all be covered within the scope of protection of the present invention. Therefore, the scope of protection of the present invention should be determined by the scope of the claims.

Claims

1. A method for preparing an impact-resistant and high thermal conductivity polyphenylene sulfide composite material, characterized in that, Includes the following steps: S1. Preparation of highly oriented PPS fiber inserts: (1) Polysulfone resin, first antioxidant, initiator and active monomer are reacted to obtain functionalized polysulfone resin compatibilizer; (2) PPS, aromatic polyamide, functionalized polysulfone resin compatibilizer and second antioxidant are mixed and melt extruded to obtain composite resin particles; (3) Composite resin particles are melt spun to obtain fiber samples; the fiber samples are subjected to solid-phase super-stretching orientation and high-temperature annealing to obtain highly oriented PPS fibers; (4) The highly oriented PPS fibers are aligned in multiple directions, bundled and then highly oriented PPS fiber inserts are obtained. S2. Preparation of impact-resistant and high thermal conductivity PPS composite material: PPS and third antioxidant are uniformly mixed and then injection molded with highly oriented PPS fiber inserts to obtain impact-resistant and high thermal conductivity PPS composite material. In step S1, the fiber sample undergoes solid-phase super-stretching orientation with a stretching ratio of 1500%-2500%. In step S1, the highly oriented PPS fiber insert is obtained by aligning 1,000-10,000 highly oriented PPS fibers in multiple directions and bundling them into a specific shape. The active monomer is selected from one of the following: hydroxyethyl acrylate, hydroxypropyl methacrylate, hydroxyethyl methacrylate, isobutyl methacrylate, n-butyl methacrylate, ethyl methacrylate, 2-ethylhexyl acrylate, methyl methacrylate, glycidyl methacrylate, ethylene glycol dimethacrylate, triethylene glycol dimethacrylate, allyl methacrylate, dimethylaminoethyl methacrylate, and siloxane methacrylate. The initiator is selected from one of azobisisobutyronitrile, benzoyl peroxide, dicumyl peroxide, diisopropyl peroxide, dicyclohexyl peroxide, di(4-tert-butylcyclohexyl) peroxide, di(2-ethylhexyl) peroxide, dimethyl peroxide, diphenyl peroxide, and azobisisobutyronitrile. In step S1, the functionalized polysulfone resin compatibilizer is obtained by adding 100 parts of polysulfone resin, 0.5-3 parts of the first antioxidant, 0.5-5 parts of the initiator, and 5-30 parts of the active monomer into a mixer and reacting at 300-380°C for 10-30 minutes, by weight. The composite resin particles are obtained by melting and extruding a mixture of 100 parts of PPS, 10-50 parts of aromatic polyamide, 5-30 parts of the functionalized polysulfone resin compatibilizer, and 0.5-5 parts of the second antioxidant into a twin-screw extruder, by weight. In step S2, the impact-resistant and high thermal conductivity PPS composite material is prepared by uniformly mixing 100 parts PPS and 0.5-5 parts of a third antioxidant by weight and then adding the mixture to the injection molding machine barrel. The highly oriented PPS fiber insert is preheated at 160-220℃ for 20-40 minutes and then laid flat into the injection molding machine mold cavity for injection molding. The injection temperature is 330-380℃, the nozzle temperature is 310-360℃, the mold temperature is 160-220℃, and the injection time is 80-150MPa.

2. The preparation method of the impact-resistant and high thermal conductivity polyphenylene sulfide composite material as described in claim 1, characterized in that, In step S1, the polysulfone-based resin is one of polyethersulfone, polyphenylsulfone, polyphenylene sulfone, and polyarylethersulfone; the first antioxidant, the second antioxidant, and the third antioxidant are all selected from one of pentaerythritol tetrakis[β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate], octadecyl β-(3,5-di-tert-butyl-4-hydroxyphenyl)propionate, 2,6-di-tert-butyl-p-cresol, tris(2,4-di-tert-butylphenyl) phosphite, bis(2,4-di-tert-butylphenyl) pentaerythritol diphosphite, dilauryl thiodipropionate, and N-isopropyl-N'-phenyl-p-phenylenediamine.

3. The method for preparing the impact-resistant and high thermal conductivity polyphenylene sulfide composite material as described in claim 1, characterized in that, In step S1, the aromatic polyamide is selected from one of poly(hexamethylene terephthalamide), poly(hexamethylene isophthalamide / hexamethylene terephthalamide copolymer), poly(decyl terephthalamide), poly(butyl terephthalamide / hexamethylene diamine copolymer), poly(hexamethylene phthalamide), and poly(nonadiamine terephthalamide).

4. The preparation method of the impact-resistant and high thermal conductivity polyphenylene sulfide composite material as described in claim 1, characterized in that, In step S1, the fiber sample is obtained by melt spinning composite resin particles using a melt spinning machine at an extrusion temperature of 320-380℃ and a screw speed of 120-200 rpm. The melt spinning temperature is 320-380℃ and the winding speed is 100-200 m / min. The highly oriented PPS fiber is obtained by fixing the fiber sample on a universal testing machine and performing solid-phase super-stretching orientation at 120-200℃. After the stretching ratio reaches 1500%-2500%, the stretching is stopped, and the fiber is annealed at high temperature in an oven at 230-250℃ for 1-3 hours.

5. A high-impact, high-thermal-conductivity polyphenylene sulfide composite material, characterized in that, It is prepared by the method of any one of claims 1-4 for the preparation of impact-resistant and high thermal conductivity polyphenylene sulfide composite material.

Citation Information

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