A polyetheretherketone composite material and preparation method thereof

Abstract

The invention discloses a polyetheretherketone composite material and a preparation method thereof, belonging to the technical field of polymer composite materials. The raw materials of the invention include 5%-30% of reinforcing material fiber, 0.1%-3% of macromolecular silane coupling agent, and the balance is polyetheretherketone. Compared with small molecule silane coupling agent, the invention adopts macromolecular silane coupling agent to improve the mechanical properties of composite material more; the thermal properties and crystallization properties of fiber / polyetheretherketone composite material treated with macromolecular silane coupling agent of the invention are better.

Description

Technical Field

[0001] The invention relates to the technical field of polymer composite materials, in particular to a polyetheretherketone composite material and a preparation method thereof. Background Art

[0002] PEEK-based composites have been studied for many years at home and abroad, but due to the structural characteristics of PEEK resin itself, there are still problems such as poor solubility, high processing temperature and high melt viscosity. Due to the high melt viscosity of PEEK, it is difficult to evenly infiltrate the reinforcing filler to form a well-impregnated composite material, and due to the polarity difference and molecular chain inertness of PEEK and reinforcing materials, the two have poor compatibility, it is difficult to form chemical bonds, the interface bonding strength is low, and effective reinforcement cannot be achieved. Debonding between fibers and matrix has been proven to be one of the main failure mechanisms of PEEK composites.

[0003] At present, the coupling agents used in polyetheretherketone-based composite materials are mainly small molecule silane coupling agents. Although a certain reinforcement effect can be achieved after modifying the surface of the reinforcement material, due to compatibility issues, the interaction efficiency between the fiber and the matrix resin is low, so the reinforcement effect is also very limited. Compared with small molecule coupling agents, macromolecular coupling agents have relatively long molecular chains. When used to modify polyetheretherketone-based composite materials, they can produce stronger physical entanglement with the polymer matrix to achieve effective reinforcement; and the structure and composition of the synthesized macromolecular coupling agents can be changed by design to control and improve the performance of the material.

[0004] Therefore, providing a method for preparing a polyetheretherketone composite material using a macromolecular silane coupling agent is a technical problem that those skilled in the art urgently need to solve. Summary of the invention

[0005] In view of this, the present invention is based on the actual needs and future development of polyetheretherketone composite materials, and solves the problem that the existing small molecule silane coupling agent has weak interaction with PEEK resin and the reinforcement effect of the composite material is not ideal. It is used to modify the fiber to prepare a polyetheretherketone-based composite material, improve its physical and mechanical properties and processing performance, and obtain a high-performance fiber / polyetheretherketone composite material.

[0006] To achieve the above object, the present invention adopts the following technical solution:

[0007] A polyetheretherketone composite material comprises the following raw materials in percentage by mass: 5%-30% of reinforcing material fiber, 0.1%-3% of a macromolecular silane coupling agent, and the balance being polyetheretherketone.

[0008] Furthermore, the macromolecular silane coupling agent is any one of the following general formulas (I) to (III):

[0009]

[0010] (I);

[0011]

[0012] (II);

[0013]

[0014] (III);

[0015] In general formula (I) to general formula (III), 3≤n≤20, X is a C1-C18 linear or branched saturated alkyl group, or a branched or branched alkane with a heteroatom; Y is a C1-C18 linear or branched saturated alkyl group.

[0016] The preparation method of the above-mentioned macromolecular silane coupling agent is as follows: raw material A and raw material B are added to an organic solvent under anhydrous and oxygen-free conditions for mixed reaction, the reaction product is added to methanol to precipitate a precipitate, the precipitate is washed and dried, and then mixed with raw material C, added to tetrahydrofuran for reaction and end-capping to prepare the macromolecular silane coupling agent;

[0017] The raw material A is a compound containing bisphenol hydroxyl group, the raw material B is a ketone compound containing difluoride, and C is a silane coupling agent whose terminal group is an isocyanate group.

[0018] Furthermore, the compound containing bisphenol hydroxyl groups is any one of resorcinol, 2-methylhydroquinone and 3,3',5,5'-tetramethyl-4,4'-dihydroxybiphenyl.

[0019] Furthermore, the difluoro-containing ketone compound is 4,4'-difluorobenzophenone.

[0020] Preferably, the molar ratio of the compound containing bisphenol hydroxyl group to the difluoro ketone compound is 1:1.1-1.5.

[0021] Furthermore, the organic solvent is N,N-dimethylformamide or N-methylpyrrolidone.

[0022] Furthermore, the reaction temperature of the raw material A and the raw material B is 60-220° C., and the reaction time is 5-8 hours.

[0023] Furthermore, the reaction temperature of the precipitated precipitate and the raw material C is 60-220° C., and the reaction time is 2-5 h.

[0024] Furthermore, the reaction of raw material A and raw material B also includes removing water and adding a catalyst;

[0025] The dehydration is azeotropic dehydration with toluene, and the catalyst is potassium carbonate.

[0026] Furthermore, the reaction of the precipitated precipitate with the raw material C further comprises adding a catalyst;

[0027] The catalyst is dibutyltin dilaurate.

[0028] Preferably, the preparation steps of the macromolecular silane coupling agent are:

[0029] (1) Under room temperature, a compound containing bisphenol hydroxyl groups was added into a four-necked flask equipped with a Dean-Stark apparatus, a condenser, and a nitrogen inlet and outlet, with N-methylpyrrolidone as solvent and anhydrous potassium carbonate as catalyst; the reaction mixture was refluxed at high temperature for 4 h with toluene as an azeotropic agent to dehydrate the system;

[0030] (2) After dehydration and removal of toluene, the temperature was lowered and a difluoroketone compound was added to the flask to increase the reaction temperature. The reaction was heated for 6 h. The reaction product was cooled to room temperature and then poured into anhydrous methanol to form a precipitate. The solid was collected by centrifugation and dried in a vacuum oven at 120 °C for 24 h to obtain a hydroxyl-terminated polyetheretherketone oligomer.

[0031] (3) Add the hydroxyl-terminated polyetheretherketone oligomer into a four-necked flask, add dry tetrahydrofuran as a solvent, add the catalyst dibutyltin dilaurate (DBTDL), and add the silane coupling agent with an isocyanate terminal group dropwise through a separatory funnel under a nitrogen atmosphere. After the addition is completed, continue heating and reacting for 4 hours with continuous stirring. After the reaction is completed, cool to room temperature, precipitate with anhydrous ethanol, centrifuge the precipitate, wash with anhydrous ethanol, and dry in a vacuum drying oven to obtain a macromolecular silane coupling agent.

[0032] Furthermore, the reinforcing material fibers are carbon fibers or glass fibers.

[0033] The present invention also provides a method for preparing the polyetheretherketone composite material, comprising the following steps:

[0034] (1) Add the reinforcing material fiber and the macromolecular silane coupling agent into an organic solvent to obtain an organic solution, then add water and stir to react. After the reaction is completed, filter and collect the fiber, wash it with a cold organic reagent, and dry it for storage;

[0035] (2) adding the fiber prepared in step (1) into an extruder, and then melting the polyetheretherketone in the front section of the extruder, mixing the fiber and the polyetheretherketone in the mixing section under the action of a twin screw, and distributing the fiber in the molten polyetheretherketone and being driven by the screw to the end of the extruder;

[0036] (3) A twin-screw extruder is used for extrusion granulation to obtain a fiber-reinforced polyetheretherketone composite material.

[0037] Furthermore, the organic solvent in step (1) is N,N-dimethylformamide or N-methylpyrrolidone, and the amount of water added is 1-3% of the mass of the organic solution.

[0038] Furthermore, the reaction temperature in step (1) is 60-100°C, and the reaction time is 12-24h.

[0039] Furthermore, the extrusion granulation temperature in step (3) is 360-400°C.

[0040] Preferably, the temperatures of each section of the twin-screw extruder are 360°C, 380°C, 380°C, 380°C, 370°C, 365°C, 360°C, and 360°C.

[0041] Further, the preparation method of the macromolecular silane coupling agent is:

[0042] A compound containing bisphenol hydroxyl group and a ketone compound containing difluoride are added to N, N-dimethylformamide or N-methylpyrrolidone under anhydrous and oxygen-free conditions, mixed and reacted at 60-220° C. for 5-8 hours, the reaction product is added to methanol to precipitate a precipitate, the precipitate is washed and dried, and then mixed with a silane coupling agent having an isocyanate terminal group, added to tetrahydrofuran, reacted at 60-220° C. for 2-5 hours, and the end-capping is performed to prepare a macromolecular silane coupling agent;

[0043] Furthermore, the compound containing bisphenol hydroxyl group is any one of resorcinol, 2-methylhydroquinone and 3,3',5,5'-tetramethyl-4,4'-dihydroxybiphenyl; and the ketone compound containing difluoride is 4,4'-difluorobenzophenone.

[0044] The beneficial effects of the present invention are:

[0045] The fiber-reinforced polyetheretherketone composite material prepared by the present invention using the macromolecular silane coupling agent has a maximum tensile strength and flexural strength of 131.2MPa and 170.1MPa. After being treated with KH550, the tensile and flexural strengths are 114.7MPa and 155.9MPa. Compared with the small molecule silane coupling agent, the macromolecular silane coupling agent has a greater improvement in the mechanical properties of the composite material.

[0046] The fiber-reinforced polyetheretherketone composite material using macromolecular silane coupling agent still has good thermal stability above 500°C, which meets the use temperature of polyetheretherketone composite materials. The crystallinity of fiber-reinforced polyetheretherketone composite materials using macromolecular silane coupling agent can reach 29.92%, and the crystallinity performance is improved. The crystallinity of polyetheretherketone treated with small molecule silane coupling agent is 26.11%. Although the crystallinity of the fiber is enhanced after being treated with small molecule silane coupling agent, the effect is limited. The crystallinity and crystallinity performance of carbon fiber polyetheretherketone composite materials treated with macromolecular silane coupling agent increase more significantly. BRIEF DESCRIPTION OF THE DRAWINGS

[0047] Figure 1 Figure 1 is a cross-sectional scan of a carbon fiber material that has been treated differently in an embodiment of the present invention, wherein Figure (a) is untreated, Figure (b) is a treatment diagram of a small molecule silane coupling agent KH901, Figure (c) is a treatment diagram of a macromolecular silane coupling agent R-DFBP-KH901, Figure (d) is a treatment diagram of a macromolecular silane coupling agent MeHQ-DFBP-KH901, and Figure (e) is a treatment diagram of a macromolecular silane coupling agent TMDHB-DFBP-KH901;

[0048] Figure 2 The mechanical properties of carbon fiber reinforced polyetheretherketone composite materials treated with different coupling agents in the embodiments of the present invention;

[0049] Figure 3 The DSC graphs of carbon fiber reinforced polyetheretherketone composite materials treated with different coupling agents in the embodiments of the present invention;

[0050] Figure 4 TG graphs of carbon fiber reinforced polyetheretherketone composite materials treated with different coupling agents in an embodiment of the present invention;

[0051] Figure 5 Infrared spectra of R-DFBP-KH901, MeHQ-DFBP-KH901 and TMDHB-DFBP-KH901 prepared in the examples of the present invention;

[0052] Figure 6 H NMR spectra of R-DFBP-KH901, MeHQ-DFBP-KH901 and TMDHB-DFBP-KH901 prepared in the examples of the present invention;

[0053] Figure 7 XPS structural characterization diagrams of R-DFBP-KH901, MeHQ-DFBP-KH901, and TMDHB-DFBP-KH901 prepared in the embodiments of the present invention; wherein (a) is R-DFBP-KH901, (b) is MeHQ-DFBP-KH901, and (c) is TMDHB-DFBP-KH901;

[0054] Figure 8 TG and DTG graphs of R-DFBP-KH901, MeHQ-DFBP-KH901, and TMDHB-DFBP-KH901 prepared in the embodiments of the present invention; wherein (a) is R-DFBP-KH901, (b) is MeHQ-DFBP-KH901, and (c) is TMDHB-DFBP-KH901. DETAILED DESCRIPTION

[0055] The following will be combined with the drawings in the embodiments of the present invention to clearly and completely describe the technical solutions in the embodiments of the present invention. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.

[0056] Example 1

[0057] A method for preparing a 10% 3mm carbon fiber / polyetheretherketone composite material, the steps are as follows:

[0058] (1) Weigh the reinforcing materials carbon fiber 10%, macromolecular silane coupling agent 2%, and polyetheretherketone 88% by mass.

[0059] (2) Clean the surface of the carbon fiber, soak the carbon fiber in anhydrous ethanol solution for 24 hours, ultrasonically treat it for 30 minutes, and vacuum dry it. Then treat the dried carbon fiber with nitric acid in a 60°C water bath; after treatment, wash it with distilled water until it is neutral, and dry it in a vacuum drying oven at 60°C.

[0060] (3) Add the treated carbon fiber to the NMP solution of the macromolecular silane coupling agent, then slowly add 2% water, heat the mixture to 80°C with stirring, and react for 12 hours. Collect the fibers by filtration, wash with cold NMP, and dry in a vacuum oven at 120°C for 48 hours.

[0061] The structure of the macromolecular silane coupling agent (R-DFBP-KH901) used is as follows:

[0062] ;

[0063] (4) Turn on the power of the extruder and connect the cooling water. First, add the dried polyetheretherketone matrix into the barrel and run the machine. Then, add the corresponding treated carbon fiber from the side forced feeding port at the fourth section of the extruder. After the polyetheretherketone is melted in the first two sections of the extruder, it is evenly mixed with the fibers added from the side when it reaches the fourth section under the action of the twin screw. The fibers are distributed in the molten polyetheretherketone and are driven to the end of the extrusion by the screw. The temperature of each section of the twin-screw extruder was controlled at 360°C, 380°C, 380°C, 380°C, 370°C, 365°C, 360°C, and 360°C, and the extrusion temperature was 360°C to obtain fiber-reinforced PEEK composite filament strips. After extrusion, the strips were transported by a conveyor belt and entered into a water-cooled, and after cooling, they were pulled into a roller cutter pelletizer to obtain cylindrical particles with a diameter of 2-4 mm and a length of 4-6 mm, i.e., carbon fiber reinforced polyetheretherketone composite pellets with a fiber mass percentage of 10% were obtained.

[0064] (5) The carbon fiber reinforced polyetheretherketone composite pellets prepared above were dried at 150 °C for 3 h to remove moisture. A high-temperature release agent was sprayed in the mold, and the release agent was evenly applied to all corners of the mold with a wire brush to facilitate smooth demolding after molding. 10 g and 5 g of the dried pellets were respectively placed in the dumbbell mold and the long strip mold of the high-temperature molding machine, and pre-pressed for 30 s to squeeze out some of the air remaining in the mold before the mold was heated. The mold temperature was set to 380 °C, and then the mold began to heat. When the pellets were melted and plasticized, the following pressurization and depressurization methods were used: the pressure was increased to 25 T and maintained for 1 min, and then the pressure was released; the pressure was increased to 25 T and maintained for 1 min, and then the pressure was released; finally, the pressure was increased to 25 T again and maintained for 30 min. Some splashing occurred during this period, which is normal. After 30 minutes of heat preservation and pressure holding, the molded product will be cooled at a rate of 40℃ / h and continue to maintain pressure. When the system temperature drops below 300℃, the pressure will be reduced until the product temperature is below 150℃ for demolding. After cooling to room temperature, the edges and corners of the spline will be further polished and corrected with a file.

[0065] The macromolecular silane coupling agent (R-DFBP-KH901) for the polyetheretherketone composite material in Example 1 has the following structural formula:

[0066] , where n=10.

[0067] The specific preparation steps are:

[0068] 12.10 g (0.11 mol) of resorcinol and 16.56 g (0.11 mol) of anhydrous potassium carbonate were added to a four-necked flask equipped with a Dean-Stark apparatus, a condenser, and a nitrogen inlet. 30 ml of NMP was used as a solvent and 25 ml of toluene was used as an azeotropic agent. The mixture was refluxed at 140°C for 4 h, then the temperature was reduced to 100°C, 21.82 g (0.10 mol) of 4,4'-difluorobenzophenone was added to the flask to raise the reaction temperature to 170°C, and maintained at this temperature for another 6 h. The reaction mixture was cooled to room temperature. The resulting mixture was then poured into anhydrous methanol to form a precipitate, and the solid was collected by centrifugal filtration and dried in a vacuum oven at 120°C for 24 h to obtain a reddish-brown solid, which was recorded as R-DFBP.

[0069] R-DFBP (0.485 mmol) was added to a four-necked flask, and then 30 ml of dry tetrahydrofuran was added as a solvent, and a catalyst dibutyltin dilaurate (DBTDL) (0.5% of the reactant mass) was added. Under a nitrogen atmosphere, 3-isocyanate propyltrimethoxysilane (KH901) (0.3 g, 1.456 mmol) was added dropwise through a separatory funnel at a ratio of 1 / 1.5 to the functional group. After the addition was completed, the reaction was continued at 70°C for 4 hours with continuous stirring. After the reaction was completed, it was cooled to room temperature, precipitated with anhydrous ethanol, centrifuged, washed with anhydrous ethanol, dried in a vacuum drying oven, sealed and stored, and the product was labeled R-DFBP-KH901.

[0070] Example 2

[0071] The difference from Example 1 is that the structure of the macromolecular silane coupling agent (MeHQ-DFBP-KH901) used is as follows:

[0072] , where n=10.

[0073] The specific preparation steps are:

[0074] 13.64 g (0.11 mol) of MeHQ and 16.56 g (0.11 mol) of anhydrous potassium carbonate were added to a four-necked flask equipped with a Dean-Stark apparatus, a condenser, and a nitrogen inlet and outlet. 30 ml of NMP was used as a solvent and 25 ml of toluene was used as an azeotropic agent. The mixture was refluxed at 160°C for 4 h to dehydrate the system. After dehydration and removal of toluene, the temperature was lowered to 100°C, and 21.82 g (0.10 mol) of DFBP was added to the flask to raise the reaction temperature to 200°C and maintained for 3 h. The reaction mixture was cooled to room temperature. The resulting mixture was then poured into anhydrous methanol to form a precipitate, which was collected by filtration. The product was a tan solid and was recorded as MeHQ-DFBP.

[0075] The synthesized MeHQ-DFBP (0.485 mmol) was added to a four-necked flask, 30 ml of dry tetrahydrofuran was added as a solvent, and the catalyst dibutyltin dilaurate (DBTDL) (0.5% of the reactant mass) was added. Under a nitrogen atmosphere, 3-isocyanate propyltrimethoxysilane (KH901) (0.3 g, 1.456 mmol) was added dropwise through a separatory funnel at a ratio of 1 / 1.5 to the functional group. After the addition was completed, the reaction was continued at 70°C for 4 hours with continuous stirring. After the reaction was completed, it was cooled to room temperature, precipitated with anhydrous ethanol, centrifuged, washed with anhydrous ethanol, dried in a vacuum drying oven, and sealed for storage. The product was recorded as MeHQ-DFBP-KH901.

[0076] Example 3

[0077] The difference from Example 1 is that the structure of the macromolecular silane coupling agent (TMDHB-DFBP-KH901) used is as follows:

[0078] , where n=10.

[0079] The specific preparation steps are:

[0080] 26.62 g (0.11 mol) of 3,3',5,5'-tetramethyl-4,4'-dihydroxybiphenyl (excess) and 16.56 g (0.12 mol) of anhydrous potassium carbonate were added to a four-necked flask equipped with a Dean-Stark apparatus, a condenser, and a nitrogen inlet and outlet. 30 ml of NMP was used as a solvent and 25 ml of toluene was used as an azeotropic agent. The mixture was refluxed at 160°C for 4 h to dehydrate the system. After dehydration and removal of toluene, the temperature was reduced to 100°C, and 21.82 g (0.10 mol) of DFBP was added to the flask to increase the reaction temperature to 220°C and maintained for 6 h. The reaction mixture was cooled to room temperature. The resulting mixture was then poured into anhydrous methanol to form a precipitate, which was collected by filtration. The product was an amorphous brown solid, recorded as TMDHB-DFBP.

[0081] The synthesized TMDHB-DFBP (0.485 mmol) was added to a four-necked flask, 30 ml of dry tetrahydrofuran was added as a solvent, and the catalyst dibutyltin dilaurate (DBTDL) (0.5% of the reactant mass) was added. Under a nitrogen atmosphere, 3-isocyanate propyltrimethoxysilane (KH901) (0.3 g, 1.456 mmol) was added dropwise through a separatory funnel at a ratio of 1 / 1.5 to the functional group. After the addition was completed, the reaction was carried out at a temperature of 70°C for 4 hours with continuous stirring. After the reaction was completed, it was cooled to room temperature, precipitated with anhydrous ethanol, centrifuged, washed with anhydrous ethanol, dried in a vacuum drying oven, sealed and stored, and the products were marked as TMDHB-DFBP-KH901.

[0082] Comparative Example 1

[0083] The difference from Example 1 is that the reinforcing material carbon fiber is not treated with a coupling agent, and the other steps are completely the same.

[0084] Comparative Example 2

[0085] The difference from Example 1 is that the reinforcing material carbon fiber is treated with a small molecule coupling agent KH901, and the other steps are completely the same.

[0086] The performance of the reviewed materials obtained in Examples 1-3 and Comparative Examples 1-2 was tested and analyzed:

[0087] like Figure 1As shown in the figure, the prepared specimens were subjected to tensile and three-point bending tests by a universal testing machine, and the width and thickness of the sample to be tested were measured using a vernier caliper. In the three-point bending test, the span was set to 64 mm, and the experiment was carried out at a rate of 2 mm / min, and the force and displacement data when the sample broke were recorded. The results show that the tensile and flexural strengths of carbon fiber reinforced polyetheretherketone composites without coupling agent treatment are 113.5MPa and 149.9MPa, the tensile and flexural strengths after treatment with KH901 are 114.7MPa and 155.9MPa, the tensile and flexural strengths after treatment with R-DFBP-KH901 macromolecular silane coupling agent are 128.5MPa and 166.3MPa, the tensile and flexural strengths after treatment with MeHQ-DFBP-KH901 macromolecular silane coupling agent are 131.2MPa and 170.1MPa, and the tensile and flexural strengths after treatment with TMDHB-DFBP-KH901 macromolecular silane coupling agent are 128.8MPa and 161.7MPa. Compared with small molecular silane coupling agents, macromolecular silane coupling agents have a greater improvement in the mechanical properties of composites.

[0088] like Figure 2 As shown, there is no PEEK matrix entangled on the carbon fiber surface and the grooved surface structure of the carbon fiber itself is observed. The cross-section of the carbon fiber / PEEK composite material treated with the small molecule silane coupling agent KH901 has partial PEEK matrix adhesion on the carbon fiber surface, and the adhesion uniformity is poor. The cross-section of the carbon fiber / PEEK composite material treated with the three macromolecular silane coupling agents is tightly wrapped by the PEEK matrix, the original surface groove structure of the carbon fiber has been completely covered, and the PEEK wrapping on the fiber surface is uniform and not exposed.

[0089] like Figure 3 As shown in the figure, the Tc values ​​of fiber / PEEK composites treated with three macromolecular silane coupling agents are the highest, R-DFBP-KH901 can increase Tc to 288.07℃, MeHQ-DFBP-KH901 can increase Tc to 290.58℃, and TMDHB-DFBP-KH901 can increase Tc to 286.79℃, which shows that when the macromolecular silane coupling agent is grafted onto the fiber surface, the macromolecular silane coupling agent has a PEEK-like segment, which is similar to the molecular structure of the PEEK matrix, so that the fiber and the PEEK matrix have good compatibility. The similar and compatible properties of the two not only optimize the interface structure and play a entanglement connection effect, but also cause a lubrication effect, making the molecular mobility of the polymer matrix easier. Therefore, the Tc of the fiber-filled PEEK composite material treated with the macromolecular silane coupling agent is improved. This shows that the addition of the macromolecular silane coupling agent improves the interface bonding effect between the interface fiber and the matrix and improves the crystallization performance.

[0090] like Figure 4 As shown in the figure, after the fiber is treated with a macromolecular silane coupling agent, the composite material decomposes slightly slower at high temperature. This is because the macromolecular silane coupling agent has a PEEK structural segment similar to the matrix, which improves the compatibility between the fiber and the matrix, enhances the interface bonding effect between the fiber and the PEEK matrix, and increases the thermal stability of the material. The 5% thermal weight loss temperature of the composite material is above 500°C, and it has excellent thermal stability.

[0091] Although the embodiments of the present invention have been shown and described above, it is to be understood that the above embodiments are exemplary and are not to be construed as limitations of the present invention. A person skilled in the art may change, modify, replace and vary the above embodiments within the scope of the present invention.

Claims

1. A polyetheretherketone composite material, characterized in that: The invention is composed of the following raw materials in percentage by weight: 5%-30% of reinforcing material fiber, 0.1%-3% of macromolecular silane coupling agent, and the balance of polyetheretherketone; The macromolecular silane coupling agent is any one of the following general formulas (I) to (III): In general formula (I) to general formula (III), 3≤n≤20, X is a C1-C18 linear or branched saturated alkylene group; Y is a C1-C18 linear or branched saturated alkyl group; the reinforcing material fiber is a carbon fiber or a glass fiber; The preparation method of the polyetheretherketone composite material is: (1) adding reinforcing material fibers and a macromolecular silane coupling agent into an organic solvent to obtain an organic solution, then adding water and stirring to react, filtering and collecting the fibers after the reaction is completed, washing with a cold organic reagent, and drying and storing; (2) adding the fiber prepared in step (1) into an extruder, and then melting the polyetheretherketone in the front section of the extruder, mixing the fiber and the polyetheretherketone in the mixing section under the action of a twin screw, and distributing the fiber in the molten polyetheretherketone and being driven by the screw to the extrusion end; (3) using a twin-screw extruder to extrude and granulate to obtain a fiber-reinforced polyetheretherketone composite material; The preparation method of the macromolecular silane coupling agent is: A compound containing bisphenol hydroxyl group and a ketone compound containing difluoride are added to N, N-dimethylformamide or N-methylpyrrolidone under anhydrous and oxygen-free conditions, mixed and reacted at 60-220° C. for 5-8 hours, the reaction product is added to methanol to precipitate a precipitate, the precipitate is washed and dried, and then mixed with a silane coupling agent having an isocyanate terminal group, added to tetrahydrofuran, reacted at 60-220° C. for 2-5 hours, and capped to prepare a macromolecular silane coupling agent; the compound containing bisphenol hydroxyl group is any one of resorcinol, 2-methylhydroquinone and 3,3',5,5'-tetramethyl-4,4'-dihydroxybiphenyl; the ketone compound containing difluoride is 4,4'-difluorobenzophenone.

2. A polyetheretherketone composite material according to claim 1, characterized in that: The organic solvent in step (1) is N,N-dimethylformamide or N-methylpyrrolidone, and the amount of water added is 1-3% of the mass of the organic solution.

3. A polyetheretherketone composite material according to claim 1, characterized in that: The reaction temperature in step (1) is 60-100° C. and the reaction time is 12-24 h.

4. The polyetheretherketone composite material according to claim 1, characterized in that: The extrusion granulation temperature in step (3) is 360-400°C.

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