Hybrid hetero-fiber filler constructs high-performance GW&CF@PEEK composite material and preparation method thereof

Abstract

The application provides a kind of hybrid heterogeneous fiber filler constructs high-performance GW&CF@PEEK composite material and preparation method thereof.The hybrid heterogeneous fiber filler constructs high-performance GW&CF@PEEK composite material of the application, comprising the following steps: heat treatment of carbon fiber, add the heat-treated carbon fiber to the solution containing nickel sulfate, nickel chloride, boric acid and sodium dodecyl sulfate, nickel plating to obtain nickel-plated carbon fiber;Nickel-plated carbon fiber is added to benzoxazine / acetone solution, then graphene and carbon nanotube are added and stirred, and finally the micro-wet state is obtained by vacuum filtration and transferred to an oven for heat curing;After curing, a hybrid filler is obtained;After mixing the hybrid filler and polyether ether ketone, hot compression molding is carried out to obtain GW&CF@PEEK composite material.The application solves the problem of agglomeration of nanofiller in polymer, and improves the problem of insufficient thermal conductivity and electrical conductivity of carbon fiber, and prepares a high-performance material with excellent performance of thermal conductivity, electrical conductivity, EMI shielding, electrical heating and mechanical properties.

Description

TECHNICAL FIELD

[0001] The present application relates to the field of materials, in particular to a kind of hybrid hetero fiber filler constructs high-performance GW&CF@PEEK composite material and preparation method thereof. BACKGROUND

[0002] With its outstanding specific strength, high corrosion resistance and unique design flexibility, carbon fiber reinforced polymer composites (CFRP) have received great enthusiasm in aerospace, transportation, energy, electronic devices and sports fields, which are very eager to reduce weight without sacrificing performance. In recent decades, with the development of advanced manufacturing technology, advanced composites have been rapidly developed. Among them, carbon fiber reinforced polymer (CFRP) composites have been widely used in aerospace applications due to their light weight, excellent mechanical properties, fatigue resistance and corrosion resistance. The weight percentage of CFRP composites in civil aircraft has become an important indicator to evaluate the progress of the aircraft. The weight percentage of new generation civil aircraft such as Boeing 787 and Airbus A350 has exceeded 50%. In particular, CFRP composites are mainly used for large main load-bearing structures such as fuselage and wings. The large-scale use of high-strength lightweight CFRP composites on civil aircraft can effectively improve passenger capacity and fuel efficiency. However, as a semiconductor material, CFRP composites are more susceptible to accidental lightning strikes compared to metal materials, which can cause some harmful problems such as electromagnetic interference (EMI) and direct damage to CFRP composites by lightning. Over the years, the aviation industry has increasingly adopted carbon fiber reinforced polymer (CFRP) composites to reduce weight and improve mechanical properties. However, there have been many major problems that have hindered the widespread use of CFRP composites. Among these problems, the need to significantly improve electrical conductivity and thermal conductivity is crucial. This defect poses a significant threat to flight safety, especially in extreme weather conditions such as lightning and icing. Although carbon fibers have excellent intrinsic electrical conductivity, the insulating properties of the resin matrix can compromise the overall electrical conductivity during lightning strikes, leading to devastating consequences such as acoustic shock waves, resin pyrolysis, fiber sublimation, and even composite combustion. In addition, the electromagnetic pulses generated by lightning pose a serious risk to electronic devices, further endangering flight safety. With an average of one lightning strike every 3000 flight hours, combined with frequent icing, there is an urgent need to develop an innovative CFRP composite material with enhanced electrical conductivity, effective electromagnetic interference (EMI) shielding and electrical heating (E-heating) capabilities.

[0003] Another potential risk to flight safety comes from electromagnetic interference, which can interfere with precision electronic instruments in the aircraft, such as airborne radars or navigation systems, due to the low impedance mismatch between the CFRP skin and the air environment. Therefore, considering issues related to lightning strike protection (LSP) and electromagnetic interference (EMI) shielding is extremely important to meet the protection requirements for flight safety, especially for modern aircraft that use CFRP on a large scale. Carbon fiber reinforced polymers (CFRP) have also received extensive attention in aerospace applications due to their high specific strength, light weight, easy processing, low thermal expansion, and ablation resistance, among other characteristics

[0004] Traditionally, researchers have focused on a single aspect of CFRP, such as improving its mechanical properties, its electrically conductive composite, enhancing EMI shielding operation, or developing electronic heating solutions. The consequences of neglecting EMI shielding and electronic heating capabilities are evident in historical aviation accidents, emphasizing the need for a comprehensive study of electrical conductivity, EMI shielding, and electronic heating performance to ensure flight safety. Recent studies have shown that improving electrical conductivity and optimizing material structure can effectively mitigate the effects of electromagnetic interference. Given the link between electronic heating and electrical pathways, creating a complex conductive network in the design structure not only promises to improve electrical conductivity but also to mitigate electromagnetic interference (EMI) shielding and attribute to electronic heating capabilities.

[0005] Compared to metal fillers, simple carbon fibers dispersed in polymers generally provide a good balance between mechanical and electrical properties. It is generally believed that both electrical conductivity and electromagnetic shielding effectiveness will improve as the percentage of conductive carbon fibers increases. At very low filler concentrations, electrical conductivity remains close to that of pure polymer because the distance between conductive elements is too large to form a conductive network, and electrical current only passes through the electrical conductivity between conductive elements. These sparsely distributed elements interact with electromagnetic waves and provide little shielding. When the filler concentration reaches the percolation threshold, a conductive network is formed. This results in a rapid increase in electrical conductivity by several orders of magnitude within a very narrow range of fiber concentrations. With further addition of conductive filler, electrical conductivity tends to be stable. However, after reaching the percolation threshold, electromagnetic shielding effectiveness increases more significantly. Composites with a newly formed conductive network have some perforations through which electromagnetic energy can leak. Adding more conductive particles means that the conductive network becomes denser, resulting in a closed structure of the network that is not affected by electromagnetic leakage. The electromagnetic shielding effectiveness in this structure tends to increase slightly with frequency. As the wavelength decreases and approaches the size of the optical fiber, electromagnetic waves are more likely to encounter fibers in the polymer, and the optical fiber is more likely to absorb or reflect electromagnetic waves. At very high carbon fiber concentrations, weak frequency dependence is attributed to enhanced reflection from multiple coherent scatterers.

[0006] One of the problems with using pure discontinuous carbon fibers as conductive fillers is that relatively large amounts of carbon fibers are usually required to achieve high levels of shielding. But one of the problems with carbon fibers as conductive fillers is that large amounts of carbon fibers are usually required to achieve desirable properties, increasing the weight and cost of the composite, and also causing problems of dispersion. Below the percolation threshold of the filler, the electrical conductivity remains close to that of the pure polymer because the distance between the conductive fillers is too large to form a conductive network.

[0007] However, high filler content creates difficulties for common manufacturing techniques such as extrusion or injection molding due to significant decreases in toughness and rheological properties. Large amounts of carbon fibers increase the weight and cost of the composite, and can also cause difficulties in uniform dispersion. One of the solutions is to add a thin layer of metal to the surface of the carbon fiber, enhancing electron transport in the conductive network, improving electrical conductivity, dielectric polarization, magnetic loss performance, and interfacial interactions. Although this method is promising, metals also present challenges such as excessive weight, corrosion, and poor flexibility. In summary, non-metallic carbon-based nanomaterials, while lightweight and corrosion-resistant, face challenges related to cost and safety, and another key issue is the mechanical performance impairment caused by the metallization of carbon fibers, which weakens the interfacial adhesion between the fibers and the matrix.

[0008] To solve these difficulties, different strategies have been explored, including the incorporation of highly conductive nanofillers such as carbon nanotubes and graphene onto the surface of carbon fibers through chemical grafting, sizing technology, chemical vapor deposition (CVD), electrophoretic deposition (EPD), and layer-by-layer (LbL) attachment. In addition, electroplating and spraying techniques have also been used to introduce metal particles onto the surface of CFs and show potential for enhancing electrical conductivity. SUMMARY

[0009] In view of this, the present application proposes a hybrid heterogeneous fiber filler for constructing high-performance GW&CF@PEEK composites and a preparation method thereof.

[0010] The technical scheme of the present application is implemented as follows:

[0011] A preparation method of a hybrid heterogeneous fiber filler for constructing high-performance GW&CF@PEEK composites, comprising the following steps:

[0012] S1, heat-treating carbon fibers, adding the heat-treated carbon fibers to a solution containing nickel sulfate, nickel chloride, boric acid, and sodium dodecyl sulfate, and plating nickel to obtain nickel-plated carbon fibers;

[0013] S2, adding the nickel-plated carbon fibers to a benzoxazine / acetone solution, then adding graphene and carbon nanotubes and stirring, and finally transferring to an oven for heat curing after vacuum filtration to obtain a slightly wet state; obtaining a hybrid filler after curing;

[0014] S3, after mixing the hybrid filler and the polyether ether ketone, hot compression molding is performed to obtain the GW&CF@PEEK composite material.

[0015] Further, in step S1, when plating the nickel, the pH value of the plating solution is 7.5-8.5, the temperature of the plating solution is 60-70℃, the current density is 1.2-1.7A / dm 2 , and the time is 3-8min.

[0016] Further, in step S1, the preparation of the nickel-plated carbon fiber comprises the following steps: before electroplating, the carbon fiber is first heat treated in an air atmosphere at 440-460℃ for 20-40min; then the pretreated carbon fiber is added into a solution containing 190-210g / L nickel sulfate, 55-65g / L nickel chloride, 45-55g / L boric acid and 0.08-0.12g / L sodium dodecyl sulfate; when plating the nickel, the pH value of the plating solution is maintained at 7.8-8.2, the temperature of the plating solution is 60-70℃, the current density is 1.4-1.6A / dm 2 , and the time is 4-6min, to obtain the nickel-plated carbon fiber.

[0017] Further, in step S1, the preparation of the nickel-plated carbon fiber comprises the following steps: before electroplating, the carbon fiber is first heat treated in an air atmosphere at 450℃ for 30min; then the pretreated carbon fiber is added into a solution containing 200g / L nickel sulfate hexahydrate, 60g / L nickel chloride hexahydrate, 40g / L boric acid and 0.1g / L sodium dodecyl sulfate; when plating the nickel, the pH value of the plating solution is maintained at 8.0, the temperature of the plating solution is 65℃, the current density is 1.5A / dm 2 , and the time is 5min, to obtain the nickel-plated carbon fiber.

[0018] Further, in step S2, the preparation of the hybrid filler comprises the following steps: the nickel-plated carbon fiber is added into a 0.8-1.2wt% benzoxazine / acetone solution, then graphene and carbon nanotubes are added and stirred for 5-7h, the total mass of the graphene and the carbon nanotubes is 0.95-1.05 times the mass of the nickel-plated carbon fiber, the mass ratio of the graphene and the carbon nanotubes is 7-9:1.5-2.5, and finally the hybrid filler in a slightly wet state is obtained by vacuum suction filtration and then transferred to an oven for heat curing; the heat curing procedure is as follows: first heat curing at 145-155℃ for 1.5-2.5h, then heat curing at 175-185℃ for 1.5-2.5h, and finally heat curing at 205-215℃ for 1.5-2.5h; the hybrid filler is obtained after curing.

[0019] Further, step S2, the preparation of the hybrid filler includes the following steps: adding nickel-plated carbon fibers into a 1wt% benzoxazine / acetone solution, then adding graphene and carbon nanotubes and stirring for 6h, the total mass of graphene and carbon nanotubes is the same as the mass of nickel-plated carbon fibers, the mass ratio of graphene and carbon nanotubes is 8:2, and finally transferring to an oven for heat curing after obtaining a slightly wet state through vacuum filtration; the heat curing procedure is: first heat curing at 150℃ for 2h, then heat curing at 180℃ for 2h, and finally heat curing at 210℃ for 2h; and the hybrid filler is obtained after curing.

[0020] Further, step S3, the temperature of the hot compression molding is 375-385℃, preferably 380℃.

[0021] Further, step S3, the volume fraction of the filler in the composite material is 1.8%-35%, preferably 34.15%.

[0022] Compared with the prior art, the present application has the following beneficial effects:

[0023] The present application constructs a hybrid heterogeneous fiber filler, which is a sub-millimeter fiber filler, and can solve the problem of agglomeration of nanofillers in polymers, and improve the problems of insufficient thermal conductivity and electrical conductivity of carbon fibers.

[0024] The present application constructs a unique three-core-shell filler network structure based on carbon fibers (CF), combines metals and nanomaterials, and prepares high-performance-price-ratio materials with excellent properties such as thermal conductivity, electrical conductivity, EMI shielding, electrical heating, and mechanical properties. The present application first plates nickel on the surface of carbon fibers to enhance electron transmission in the conductive network, then anchors the interconnected graphene / carbon nanotube (GnPs&MWCNTs) hybrid network on the surface of Ni-CF through the heat curing effect of benzoxazine, and constructs a mixed three-dimensional arrangement of thermal conductive network on the surface of nickel-plated carbon fibers. These multi-scale carbon-based fillers with special 3D structure are proved to be excellent candidates for improving the overall layer thermal conductivity of CF / PEEK composite materials. BRIEF DESCRIPTION OF DRAWINGS

[0025] Figure 1 : Schematic diagram of the preparation method of the GW&Ni-CF@PEEK composite material of the present application embodiment;

[0026] Figure 2 : Scanning electron microscope image of carbon fibers;

[0027] Figure 3 : Scanning electron microscope image of nickel-plated carbon fibers;

[0028] Figure 4 : Scanning electron microscope image of the hybrid heterogeneous fiber filler;

[0029] Figure 5 Elemental mapping of hybrid hetero-fiber filler

[0030] Figure 6 Comparison of thermal conductivity of PEEK composites doped with hybrid hetero-fiber filler and hybrid filler

[0031] Figure 7 Comparison of electromagnetic shielding performance of PEEK composites doped with hybrid hetero-fiber filler and hybrid filler

[0032] Figure 8 Comparison of electrical conductivity of PEEK composites doped with hybrid hetero-fiber filler and hybrid filler

[0033] In the figure,

[0034] Thermal Conductivity: Thermal conductivity

[0035] EMI SE T Electromagnetic shielding performance

[0036] Elecrical conductivity: Electrical conductivity

[0037] Filler Content (vol%): Volume fraction of filler DETAILED DESCRIPTION

[0038] In order to better understand the technical content of the present application, the following specific examples are provided to further illustrate the present application.

[0039] The experimental methods used in the embodiments of the present application are all conventional methods unless otherwise specified.

[0040] The materials, reagents, etc. used in the embodiments of the present application can be obtained from commercial channels unless otherwise specified.

[0041] Table 1 Sources of some raw materials (manufacturer / brand)

[0042] Serial number Raw material Factory / brand 1 Carbon fiber (CF) Cangzhou Carbon Fiber Factory, Hebei 2 Benzoxazine Chengdu Keyi High Polymer Technology Co., Ltd. 3 Acetone National Pharmaceutical Group Chemical Reagent Co., Ltd. 4 nickel sulfate hexahydrate (NiS04-6H20) National Pharmaceutical Group Chemical Reagent Co., Ltd. 5 nickel chloride hexahydrate (NiCl2-6H2O) National Pharmaceutical Group Chemical Reagent Co., Ltd. 6 boric acid (H3BO3) National Pharmaceutical Group Chemical Reagent Co., Ltd. 7 Sodium dodecylbenzenesulfonate (C12H 25 SO4Na) Shanghai Maikelin Biochemical Technology Co., Ltd. 8 Polyether ether ketone (PEEK) Changchun Jida Special Plastics Engineering Research Co., Ltd.

[0043] Table 2 English Chinese meaning

[0044] Serial number English Chinese 1 CF, Carbon Fiber Carbon fiber 2 Ni-CF Nickel-coated carbon fiber 3 GnPs Graphene 4 MWCNTs Carbon nanotube 5 PEEK Polyether ether ketone

[0045] EMBODIMENT

[0046] S1, electroplating method was used to plate nickel on the surface of carbon fiber: before electroplating, the carbon fiber (CF) was first heat treated in an air atmosphere at 450°C for 30 minutes to remove the sizing agent. Then the pretreated CF was added to a solution containing NiSO4·6H2O (200 g / L), NiCl2·6H2O (60 g / L), H3BO3 (40 g / L) and C12H 25 SO4Na (0.1 g / L). When plating Ni, the pH value of the plating solution was kept at 8.0, the plating solution temperature was 65°C, the current density was 1.5 A / dm 2 , and the time was 5 min to obtain plated nickel carbon fiber (Ni-CF).

[0047] S2, preparation of hybrid heterogeneous fiber filler. The plated nickel carbon fiber prepared in step S1 was added to a 1wt% benzoxazine / acetone solution, then 8:2 mass ratio of graphene (GnPs) and carbon nanotubes (MWCNTs) were added and stirred for 6 hours, the total mass of graphene and carbon nanotubes was the same as the mass of plated nickel carbon fiber, and finally the slightly wet state was obtained by vacuum filtration and transferred to an oven for heat curing. The heat curing procedure was: 150°C / 2h + 180°C / 1h + 210°C / 1h. After curing, a mixed graphene and carbon nanotube thermal conduction network was finally deposited on the surface of the plated nickel carbon fiber, and the hybrid filler was recorded as GW&Ni-CF.

[0048] For comparison, a mixed graphene and carbon nanotube thermal conduction network was prepared on the surface of carbon fiber, recorded as GW&CF (comparison group). The specific preparation method was as follows: carbon fiber CF was added to a 1wt% benzoxazine / acetone solution, then 8:2 mass ratio of graphene (GnPs) and carbon nanotubes (MWCNTs) were added and stirred for 6 hours, and finally the slightly wet state was obtained by vacuum filtration and transferred to an oven for heat curing. The heat curing procedure was: 150°C / 2h + 180°C / 1h + 210°C / 1h. After curing, a mixed graphene and carbon nanotube thermal conduction network was finally deposited on the surface of the carbon fiber, and the hybrid filler was recorded as GW&CF.

[0049] S3, preparation of PEEK composite material: the schematic diagram of preparation of composite materials with different structures is shown in Figure 1 .

[0050] The hybrid heterogeneous fiber filler GW&Ni-CF prepared in step S2 and polyether ether ketone (PEEK) particles were mixed in a certain mass ratio, then hot compression molding was carried out at 380°C using a flat vulcanizing instrument to obtain a series of composite materials with hybrid heterogeneous filler volume fractions of 1.81%, 3.76%, 8.07%, 13.09%, 18.98%, 26.00%, and 34.15%, recorded as GW&Ni-CF@PEEK composite material.

[0051] For comparison, a series of graphene, carbon nanotubes and plated nickel carbon fiber (the same total amount of graphene and carbon nanotubes and the mass of plated nickel carbon fiber, the mass ratio of graphene and carbon nanotubes is 8:2) and PEEK random mixed composite materials were prepared, the total content of fillers (by volume percentage) is 1.81%, 3.76%, 8.07%, 13.09%, 18.98%, 26.00%, 34.15%, denoted as GnPs / MWCNTs / Ni-CF / PEEK composite materials. As a comparison group.

[0052] The results show that the application successfully prepares a new type of fiber filler, which can reduce the accumulation of graphene and carbon nanotube nanofillers, and form a micron-sized filler connected network in the composite material. Compared with the composite material with random dispersion of fillers, the composite material prepared by the application has higher thermal conductivity, electromagnetic shielding and electrical conductivity.

[0053] Figure 1 It is a preparation process of a new type of hybrid heterogeneous fiber and composite material.

[0054] Figure 2 It is the surface morphology of the original CF, and the surface is smooth.

[0055] Figure 3 Compared with Figure 2 , the plated nickel carbon fiber surface exists a layer of nickel metal particles, which indicates that the nickel is successfully plated on the smooth CF surface.

[0056] Figure 4 It is a hybrid heterogeneous fiber filler constructed by fixing graphene and carbon nanotubes on the plated nickel carbon fiber surface using thermosetting benzoxazine. In the figure, the obvious adhesion of graphene and carbon nanotubes can be seen, which confirms the successful preparation of the new hybrid heterogeneous fiber.

[0057] Figure 5 It is an element distribution map of the hybrid heterogeneous fiber filler, which further confirms the composition of the hybrid heterogeneous fiber. Ni is mainly provided by plated nickel carbon fiber, C is provided by graphene, carbon nanotubes, plated nickel carbon fiber and a small amount of benzoxazine, and N element is provided by benzoxazine.

[0058] Figure 6 It is the thermal conductivity performance of the PEEK composite material doped with hybrid heterogeneous fiber filler and mixed filler. The comparison results show that the use of hybrid heterogeneous fiber filler in the application is beneficial to the construction of thermal conduction path and the improvement of thermal conductivity performance.

[0059] Figure 7 It is the electromagnetic shielding performance of the PEEK composite material doped with hybrid heterogeneous fiber filler and mixed filler. The comparison results show that the use of hybrid heterogeneous fiber filler in the application strengthens the multiple reflection and absorption of electromagnetic waves, and improves the electromagnetic shielding performance.

[0060] Figure 8 The conductive performance of the PEEK composite material doped with the hybrid heterogeneous fiber filler and the mixed filler is compared, and the result shows that the hybrid heterogeneous fiber filler used in the application strengthens the construction of the conductive network and improves the conductive performance.

[0061] The above merely describes the preferred embodiments of the present application and is not used to limit the present application, and any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present application shall be included in the protection scope of the present application.

Claims

1. A method for preparing a high-performance GW&CF@PEEK composite material using hybrid heterogeneous fiber fillers, characterized in that: The following steps are involved: S1, heat-treating the carbon fiber, adding the heat-treated carbon fiber to a solution containing nickel sulfate, nickel chloride, boric acid, and sodium lauryl sulfate, and plating the carbon fiber with nickel to obtain nickel-plated carbon fiber; S2, adding the nickel-coated carbon fiber to a benzoxazine / acetone solution, then adding graphene and carbon nanotubes and stirring, finally vacuum filtering to a slightly moist state, and then transferring to an oven for thermal curing; after curing, a hybrid filler is obtained; S3. Mixing the hybrid filler and polyetheretherketone, and then performing hot compression molding to obtain a GW&CF@PEEK composite material.

2. The method for preparing the GW&CF@PEEK composite material according to claim 1, characterized in that: Step S1: During nickel plating, the pH value of the plating solution is 7.5-8.5, the plating solution temperature is 60-90°C, and the current density is 1.2-1.7A / dm 2 , time is 3-8 minutes.

3. The method for preparing the GW&CF@PEEK composite material according to claim 1, characterized in that: Step S1, the preparation of the nickel-plated carbon fiber includes the following specific steps: before electroplating, first placing the carbon fiber in an air atmosphere at 440-460°C for heat treatment for 20-40 minutes; then adding the pretreated carbon fiber to a solution containing 190-210g / L nickel sulfate, 55-65g / L nickel chloride, 45-55g / L boric acid and 0.08-0.12g / L sodium dodecyl sulfate; during nickel plating, the pH value of the plating solution is maintained at 7.8-8.2, the plating solution temperature is 60-70°C, and the current density is 1.4-1.6A / dm 2 , time is 4-6min, and nickel-plated carbon fiber is obtained.

4. The method for preparing the GW&CF@PEEK composite material according to claim 3, characterized in that: Step S1, the preparation of the nickel-plated carbon fiber comprises the following specific steps: before electroplating, firstly, heat-treating the carbon fiber in an air atmosphere at 450°C for 30 minutes; then, adding the pretreated carbon fiber to a solution containing 200 g / L nickel sulfate hexahydrate, 60 g / L nickel chloride hexahydrate, 40 g / L boric acid and 0.1 g / L sodium dodecyl sulfate; during nickel plating, the pH value of the plating solution is maintained at 8.0, the plating solution temperature is 65°C, and the current density is 1.5 A / dm 2 , time is 5min, and nickel-plated carbon fiber is obtained.

5. The method for preparing the GW&CF@PEEK composite material according to claim 1, characterized in that: Step S2, the preparation of the hybrid filler includes the following specific steps: adding nickel-plated carbon fiber to a 0.8-1.2wt% benzoxazine / acetone solution, then adding graphene and carbon nanotubes and stirring for 5-7h, the total mass of graphene and carbon nanotubes is 0.95-1.05 times the mass of the nickel-plated carbon fiber, and the mass ratio of graphene to carbon nanotubes is 7-9:1.5-2.5; finally, vacuum filtration is performed to obtain a slightly moist state and then transferred to an oven for thermal curing; the thermal curing procedure is: first thermal curing at 145-155°C for 1.5-2.5h, then thermal curing at 175-185°C for 1.5-2.5h, and finally thermal curing at 205-215°C for 1.5-2.5h; after curing, the hybrid filler is obtained.

6. The method for preparing the GW&CF@PEEK composite material according to claim 5, characterized in that: Step S2, the preparation of the hybrid filler includes the following specific steps: adding nickel-plated carbon fiber to a 1wt% benzoxazine / acetone solution, then adding graphene and carbon nanotubes and stirring for 6 hours, the total mass of graphene and carbon nanotubes is the same as the mass of the nickel-plated carbon fiber, and the mass ratio of graphene to carbon nanotubes is 8:2; finally, vacuum filtration is performed to obtain a slightly moist state and then transferred to an oven for thermal curing; the thermal curing procedure is: first thermal curing at 150°C for 2 hours, then thermal curing at 180°C for 2 hours, and finally thermal curing at 210°C for 2 hours; after curing, the hybrid filler is obtained.

7. The method for preparing the GW&CF@PEEK composite material according to claim 1, characterized in that: Step S3: The temperature of the hot compression molding is 375-385°C.

8. The method for preparing the GW&CF@PEEK composite material according to claim 1, characterized in that: Step S3: The volume fraction of the filler in the composite material is 1.8% to 35%.

9. The method for preparing the GW&CF@PEEK composite material according to claim 8, characterized in that: Step S3: The volume fraction of the filler in the composite material is 34.15%.

10. A high-performance GW&CF@PEEK composite material constructed with hybrid heterogeneous fiber fillers, characterized in that: Prepared by the preparation method according to any one of claims 1 to 9.

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