Insulating heat-conducting glass fiber reinforced polyphenylene sulfide composite material and preparation method thereof

Abstract

The invention discloses an insulating heat-conducting glass fiber reinforced polyphenylene sulfide composite material and a preparation method thereof. The composite material comprises the following raw material components: 30-50 parts by mass of polyphenylene sulfide, 10-20 parts by mass of glass fiber, 30-50 parts by mass of a heat-conducting filler, 5-10 parts by mass of a compatilizer and 0.3-1 part by mass of a coupling agent, and the heat-conducting filler is selected from one or more of graphite, silicon carbide, aluminum oxide, magnesium oxide, aluminum nitride and hexagonal boron nitride; the compatilizer is selected from a glycidyl methacrylate graft polymer. The polyphenylene sulfide composite material prepared by the preparation method disclosed by the invention has high insulativity, high thermal conductivity and good mechanical properties.

Description

Technical Field

[0001] The present invention relates to the technical field of polyphenylene sulfide composite materials, and in particular to an insulating and heat-conducting glass fiber reinforced polyphenylene sulfide composite material. Background Art

[0002] With the rapid development of technologies such as 5G, virtual reality, and the Internet of Things, the design and manufacturing of electronic appliances are gradually moving towards miniaturization, high power, and high integration, which also puts increasingly higher requirements on the mechanical properties, dielectric properties, heat dissipation, and thermal conductivity of electronic and electrical substrates.

[0003] Polyphenylene sulfide (PPS) is a high-performance engineering plastic widely used in electronic appliances. It has good heat resistance, chemical corrosion resistance, mechanical strength, and excellent dielectric and mechanical properties. However, its thermal conductivity is only 0.2-0.30 W / (m·K), which is poor. This significantly limits its application in areas requiring high thermal conductivity.

[0004] In order to improve the thermal conductivity of PPS, it is usually necessary to add thermal conductive fillers, such as carbon fillers or ceramic fillers. However, the addition of carbon fillers will greatly reduce the insulation performance of the material. The addition of ceramic fillers not only requires a large amount of filler, but also causes the material's fluidity to deteriorate, processing difficulties, and rapid mechanical properties.

[0005] Therefore, developing a polyphenylene sulfide composite material that has both high insulation and high thermal conductivity and good mechanical properties is a technical problem that needs to be solved urgently in this field. Summary of the Invention

[0006] In view of the defects of the prior art, the purpose of the present invention is to provide a modified polyphenylene sulfide composite material with high insulation, high thermal conductivity and good mechanical properties and a preparation method thereof. The composite material enhances the insulation and thermal conductivity of polyphenylene sulfide by using glass fiber and specific thermal conductive fillers.

[0007] The technical solutions of the present invention are as follows:

[0008] An insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material comprises the following raw material components: 30-50 parts by mass of polyphenylene sulfide, 10-20 parts by mass of glass fiber, 30-50 parts by mass of a thermally conductive filler, 5-10 parts by mass of a compatibilizer, and 0.3-1 part by mass of a coupling agent, wherein the thermally conductive filler is selected from one or more of graphite, silicon carbide, aluminum oxide, magnesium oxide, aluminum nitride, and hexagonal boron nitride; and the compatibilizer is selected from a glycidyl methacrylate graft polymer.

[0009] According to some preferred embodiments of the present invention, the invention further comprises 0.2-2 parts by mass of other auxiliary agents.

[0010] According to some preferred embodiments of the present invention, the other additives include one or more of antioxidants, lubricants, and pigments.

[0011] According to some preferred embodiments of the present invention, the compatibilizer is a ternary random copolymer of ethylene, butyl acrylate and glycidyl methacrylate.

[0012] According to some preferred embodiments of the present invention, the coupling agent is a silane coupling agent.

[0013] According to some preferred embodiments of the present invention, the glass fiber is a continuous glass fiber.

[0014] According to some preferred embodiments of the present invention, the mass flow rate of the polyphenylene sulfide is 600-1000 g / 10 min.

[0015] According to some preferred embodiments of the present invention, the thermally conductive filler is selected from alumina and hexagonal boron nitride, the glass fiber is continuous glass fiber, the compatibilizer is selected from a ternary random copolymer of ethylene, butyl acrylate and glycidyl methacrylate, the coupling agent is selected from a silane coupling agent, and the composite material further includes an antioxidant and silicone powder.

[0016] More preferably, it includes the following raw material components: 32-45 parts by mass of polyphenylene sulfide; 10-20 parts by mass of glass fiber; 35-45 parts by mass of thermal conductive filler, wherein the mass ratio of aluminum oxide to hexagonal boron nitride is 25-35:20-8; 5-6 parts by mass of compatibilizer; 1 part by mass of coupling agent; 0.3 parts by mass of antioxidant and 0.7 parts by mass of silicone powder.

[0017] The present invention further proposes a method for preparing the above insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material, which comprises:

[0018] (1) premixing polyphenylene sulfide, a compatibilizer, and a coupling agent at high speed to obtain a premix;

[0019] (2) adding the premix to the main feed port of a high-torque extruder with dual feed ports, premixing the thermal conductive filler at high speed and then adding it to the side feed port of the extruder, adding the glass fiber from the natural vent of the extruder, and co-extruding the three to obtain an extruded material strip;

[0020] (3) Cooling and cutting the extruded material strips to obtain the insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material.

[0021] According to some preferred embodiments of the present invention, step (1) further comprises adding other additives and continuing to mix after the polyphenylene sulfide, the compatibilizer and the coupling agent are premixed at high speed to obtain the premix.

[0022] According to some preferred embodiments of the present invention, the time for the high-speed premixing is 5-10 minutes.

[0023] The present invention has the following beneficial effects:

[0024] The preparation method of the present invention comprises the following steps: high-speed blending and modification of glass fiber, thermal conductive filler, compatibilizer, coupling agent and polyphenylene sulfide in a dual-feed high-torque extruder, so that the components can interact synergistically with each other to prepare a polyphenylene sulfide composite material with high insulation and excellent thermal conductivity. At the same time, the composite material maintains good mechanical properties, and its scope of application is significantly expanded.

[0025] The preparation method of the present invention has simple and easy-to-control technology, and the material has good processing performance and is suitable for batch and large-scale production. DETAILED DESCRIPTION

[0026] The technical solutions of the present invention will be further described below in conjunction with the embodiments of the present invention. The embodiments described below are only some of the embodiments of the present invention, not all of them. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without making creative efforts should fall within the scope of protection of the present invention.

[0027] Example 1

[0028] The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material is prepared by the following steps:

[0029] (1) 45 parts by mass of PPS with a mass flow rate of 800 g / 10 min, 5 parts by mass of compatibilizer AX8700, and 1 part by mass of coupling agent KH-570 were weighed and premixed in a high-speed mixer for 5-10 min, and then 0.3 parts by mass of antioxidant 1035 and 0.7 parts by mass of silicone powder were added, and the mixture was stirred and mixed in the high-speed mixer for 10-20 min to obtain a mixture;

[0030] (2) The mixed material is added to the main feeding funnel of a high-torque extruder with a double feeding port, 30 parts by mass of filler Al2O3 and 8 parts by mass of h-BN (hexagonal boron nitride) are premixed in a high-speed mixer for 5-10 minutes and then added to the side feeding funnel of the extruder, and 10 parts by mass of glass fiber are added from the natural vent of the extruder to obtain extruded material strips;

[0031] (3) Cooling the extruded material strips in a water tank, drying them with a blower, and pelletizing them with a pelletizer to obtain pellets of insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite materials.

[0032] Example 2

[0033] The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material is prepared by the following steps:

[0034] (1) 34 parts by mass of PPS with a mass flow rate of 800 g / 10 min, 6 parts by mass of compatibilizer AX8700, and 1 part by mass of coupling agent KH-570 were weighed and premixed in a high-speed mixer for 5-10 min, and then 0.3 parts by mass of antioxidant 1035 and 0.7 parts by mass of silicone powder were added, and the mixture was stirred and mixed in the high-speed mixer for 10-20 min to obtain a mixture;

[0035] (2) The mixed material is added to the main feeding funnel of a high-torque extruder with dual feeding ports, 30 parts by mass of filler Al2O3 and 8 parts by mass of h-BN (hexagonal boron nitride) are premixed in a high-speed mixer for 5-10 minutes and then added to the side feeding funnel of the extruder, and 20 parts by mass of glass fiber are added from the natural vent of the extruder to obtain extruded material strips;

[0036] (3) Cooling the extruded material strips in a water tank, drying them with a blower, and pelletizing them with a pelletizer to obtain pellets of insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite materials.

[0037] Example 3

[0038] The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material is prepared by the following steps:

[0039] (1) 32 parts by mass of PPS with a mass flow rate of 800 g / 10 min, 6 parts by mass of compatibilizer AX8700, and 1 part by mass of coupling agent KH-570 were weighed and premixed in a high-speed mixer for 5-10 min, and then 0.3 parts by mass of antioxidant 1035 and 0.7 parts by mass of silicone powder were added, and the mixture was stirred and mixed in the high-speed mixer for 10-20 min to obtain a mixture;

[0040] (2) The mixed material was added to the main feeding funnel of a high-torque extruder with dual feeding ports, 35 parts by mass of filler Al2O3 and 10 parts by mass of h-BN (hexagonal boron nitride) were premixed in a high-speed mixer for 5-10 minutes and then added to the side feeding funnel of the extruder, and 15 parts by mass of glass fiber was added from the natural vent of the extruder to obtain extruded material strips;

[0041] (3) Cooling the extruded material strips in a water tank, drying them with a blower, and pelletizing them with a pelletizer to obtain pellets of insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite materials.

[0042] Example 4

[0043] The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material is prepared by the following steps:

[0044] (1) 32 parts by mass of PPS with a mass flow rate of 800 g / 10 min, 6 parts by mass of compatibilizer AX8700, and 1 part by mass of coupling agent KH-570 were weighed and premixed in a high-speed mixer for 5-10 min, and then 0.3 parts by mass of antioxidant 1035 and 0.7 parts by mass of silicone powder were added, and the mixture was stirred and mixed in the high-speed mixer for 10-20 min to obtain a mixture;

[0045] (2) The mixed material was added to the main feeding funnel of a high-torque extruder with dual feeding ports, 25 parts by mass of filler Al2O3 and 20 parts by mass of h-BN (hexagonal boron nitride) were premixed in a high-speed mixer for 5-10 minutes and then added to the side feeding funnel of the extruder, and 15 parts by mass of glass fiber was added from the natural vent of the extruder to obtain extruded material strips;

[0046] (3) Cooling the extruded material strips in a water tank, drying them with a blower, and pelletizing them with a pelletizer to obtain pellets of insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite materials.

[0047] Comparative Example 1

[0048] The reinforced polyphenylene sulfide composite material was prepared by the following steps:

[0049] (1) 32 parts by mass of PPS with a mass flow rate of 800 g / 10 min, 6 parts by mass of compatibilizer AX8700, and 1 part by mass of coupling agent KH-570 were weighed and premixed in a high-speed mixer for 5-10 min, and then 0.3 parts by mass of antioxidant 1035, 0.7 parts by mass of silicone powder, 35 parts by mass of filler Al2O3, and 10 parts by mass of h-BN (hexagonal boron nitride) were added, and the mixture was stirred and mixed in the high-speed mixer for 10-20 min to obtain a mixture;

[0050] (2) adding the mixed material into the main feeding funnel of a high torque extruder with dual feeding ports, and adding 15 parts by weight of glass fiber from the natural vent of the extruder to obtain an extruded material strip;

[0051] (3) Cooling the extruded material strips in a water tank, drying them with a blower, and pelletizing them with a pelletizer to obtain pellets of reinforced polyphenylene sulfide composite materials.

[0052] Comparative Example 2

[0053] The strong polyphenylene sulfide composite material was prepared by the following steps:

[0054] (1) 45 parts by mass of PPS with a mass flow rate of 800 g / 10 min, 5 parts by mass of compatibilizer AX8700, and 1 part by mass of coupling agent KH-570 were weighed and premixed in a high-speed mixer for 5-10 min, and then 0.3 parts by mass of antioxidant 1035, 0.7 parts by mass of silicone powder, and 8 parts by mass of high thermal conductivity carbon fiber were added, and the mixture was stirred and mixed in the high-speed mixer for 10-20 min to obtain a mixture;

[0055] (2) adding the mixed material into the main feeding funnel of a high torque extruder with dual feeding ports, adding 30 parts by mass of Al2O3 filler into the side feeding funnel of the extruder, and adding 10 parts by mass of glass fiber from the natural vent of the extruder to obtain extruded material strips;

[0056] (3) Cooling the extruded material strips in a water tank, drying them with a blower, and pelletizing them with a pelletizer to obtain pellets of reinforced polyphenylene sulfide composite materials.

[0057] The reinforced polyphenylene sulfide composite materials prepared in Examples 1-4 and Comparative Examples 1-2 were subjected to performance tests, with tensile strength, flexural strength, flexural modulus, notched impact strength, thermal conductivity and volume resistivity as test indicators. The results are shown in Table 1 below:

[0058] Table 1 Performance test results of reinforced polyphenylene sulfide composite materials

[0059]

[0060] As can be seen from Table 1, compared with Comparative Examples 1 and 2, the thermal conductivity of the composite materials prepared in Examples 1-4 is significantly improved, and at the same time has high insulation and good mechanical properties, which can meet the high-end use requirements of insulating and thermally conductive PPS composite materials.

[0061] It should be noted that the above description is merely a preferred embodiment of the present invention and is not intended to limit the scope of protection of the technical solutions of the present invention. Any modifications to the technical solutions described in the aforementioned embodiments, or equivalent replacements of technical features made by persons of ordinary skill in the art that fall within the spirit and principles of the present invention, shall be included within the scope of protection of the present invention.

Claims

1. An insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material, characterized in that: The invention comprises the following raw material components: 30-50 parts by mass of polyphenylene sulfide, 10-20 parts by mass of glass fiber, 30-50 parts by mass of thermal conductive filler, 5-10 parts by mass of compatibilizer and 0.3-1 part by mass of coupling agent, wherein the thermal conductive filler is selected from one or more of graphite, silicon carbide, aluminum oxide, magnesium oxide, aluminum nitride and hexagonal boron nitride; and the compatibilizer is selected from glycidyl methacrylate graft polymer.

2. The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material according to claim 1, characterized in that: It also includes 0.2-2 parts by mass of other auxiliary agents.

3. The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material according to claim 2, characterized in that: The other additives include one or more of antioxidants, lubricants, and pigments.

4. The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material according to claim 1, characterized in that: in, The compatibilizer is a ternary random copolymer of ethylene, butyl acrylate and glycidyl methacrylate; and / or the coupling agent is a silane coupling agent; and / or the glass fiber is a continuous glass fiber.

5. The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material according to claim 1, characterized in that: The mass flow rate of the polyphenylene sulfide is 600-1000 g / 10 min.

6. The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material according to claim 1, characterized in that: The thermal conductive filler is selected from alumina and hexagonal boron nitride, the glass fiber is continuous glass fiber, the compatibilizer is selected from a ternary random copolymer of ethylene, butyl acrylate and glycidyl methacrylate, the coupling agent is selected from a silane coupling agent, and the composite material also includes an antioxidant and silicone powder.

7. The insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material according to claim 6, characterized in that: The invention comprises the following raw material components: 32-45 parts by mass of polyphenylene sulfide; 10-20 parts by mass of glass fiber; 35-45 parts by mass of thermal conductive filler, wherein the mass ratio of aluminum oxide to hexagonal boron nitride is 25-35:20-8; 5-6 parts by mass of compatibilizer; 1 part by mass of coupling agent; 0.3 part by mass of antioxidant and 0.7 part by mass of silicone powder.

8. The method for preparing the insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material according to any one of claims 1 to 7, characterized in that: It includes: (1) premixing polyphenylene sulfide, a compatibilizer, and a coupling agent at high speed to obtain a premix; (2) adding the premix to the main feed port of a high-torque extruder with dual feed ports, premixing the thermal conductive filler at high speed and then adding it to the side feed port of the extruder, adding the glass fiber from the natural vent of the extruder, and co-extruding the three to obtain an extruded material strip; (3) Cooling and cutting the extruded material strips to obtain the insulating and thermally conductive glass fiber reinforced polyphenylene sulfide composite material.

9. The preparation method according to claim 7, characterized in that Step (1) further comprises adding other additives and continuing to mix after the polyphenylene sulfide, the compatibilizer and the coupling agent are premixed at high speed to obtain the premix.

10. The preparation method according to claim 7, characterized in that The time of the high-speed premixing is 5-10 minutes.

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