A polyphenylene ether-polyurethane composite and a method for producing the same

Abstract

This invention relates to a polyphenylene ether-polyurethane composite material and its preparation method, belonging to the field of composite material molding technology. The preparation method of the polyphenylene ether-polyurethane composite material of this invention involves first coating a coupling agent onto a polyurethane film, then coating molten polyphenylene ether onto the polyurethane film. When the coupling agent layer on the polyurethane film comes into contact with the molten polyphenylene ether, molecular cross-linking occurs between the polyurethane film, the coupling agent layer, and the molten polyphenylene ether. During cooling, hydrogen bonds are formed. These molecular cross-linking and hydrogen bonding effects improve the bonding force between the polyurethane film and the polyphenylene ether, preventing the polyurethane film from detaching from the polyphenylene ether and extending the service life of the polyphenylene ether-polyurethane composite material. Furthermore, the preparation method of the polyphenylene ether-polyurethane composite material of this invention eliminates the need for adhesive spraying, is less affected by external factors, and produces a polyphenylene ether-polyurethane composite material with stable quality and a high product qualification rate.

Description

Technical Field

[0001] This invention relates to a polyphenylene ether-polyurethane composite material and its preparation method, belonging to the field of composite material molding technology. Background Technology

[0002] Marine lightweight filler material is a flooring material used on ship decks, providing load-bearing and flame-retardant properties. This flooring material is a polyphenylene ether-polyurethane composite material, consisting of a base plate and a coating adhered to it. The base plate is a high-strength polyphenylene ether engineering plastic, primarily serving a supporting role; the coating is a polyurethane coating, mainly used to improve wear resistance. Polyphenylene ether is a high-strength engineering plastic, chemically known as poly2,6-dimethyl-1,4-phenylene ether, abbreviated as PPO (Polyphenylene Oxide) or PPE (Polypheylene ether), also called polyphenylene oxide or polyphenylene ether. If the surface of the polyphenylene ether does not have a polyurethane coating, when heavy vehicles pass over the ship deck, the poor wear resistance of the polyphenylene ether engineering plastic causes dents or scratches on the surface, affecting the flatness and service life of the flooring material. Therefore, a polyurethane coating is required on the surface of the polyphenylene ether. To improve the adhesion between the polyurethane coating and polyphenylene oxide (PPE), an adhesive is first sprayed onto the PPE surface during the manufacturing process, followed by the application of the polyurethane coating over the adhesive. However, PPE is a difficult-to-bond material, and over time, the adhesive on the PPE will fail, leading to the detachment of the polyurethane coating.

[0003] Therefore, in order to improve the service life of flooring materials composed of polyphenylene ether and polyurethane coating, it is urgent to develop a method for preparing polyphenylene ether-polyurethane composite materials. Summary of the Invention

[0004] The purpose of this invention is to provide a method for preparing polyphenylene ether-polyurethane composite materials, which can solve the problem that the polyurethane layer is prone to peeling off when the currently prepared polyphenylene ether-polyurethane composite materials are used as flooring materials.

[0005] Another objective of this invention is to provide a polyphenylene ether-polyurethane composite material that can solve the problems of poor interfacial bonding and short product lifespan of current polyphenylene ether-polyurethane composite materials.

[0006] To achieve the above objectives, the technical solution adopted in the preparation method of the polyphenylene ether-polyurethane composite material of the present invention is as follows:

[0007] A method for preparing a polyphenylene ether-polyurethane composite material includes the following steps:

[0008] (1) A coupling agent is coated onto a polyurethane film to form a coupling agent layer. The coupling agent is a silane coupling agent, specifically KH550 and / or KH560. The surface roughness of the polyurethane film to be coated with the coupling agent is not less than 3 μm. The polyurethane film is a thermosetting polyurethane.

[0009] (2) The molten polyphenylene ether is coated onto the coupling agent layer and cooled to room temperature to obtain a polyphenylene ether-polyurethane composite material; the temperature of the molten polyphenylene ether is 235-245℃.

[0010] The preparation method of the polyphenylene ether-polyurethane composite material of the present invention involves first coating a coupling agent onto a polyurethane film with a roughness of not less than 3 μm. The reaction of the coupling agent and the surface roughness enhance the adhesion of the coupling layer to the polyurethane film. Then, molten polyphenylene ether is coated onto the polyurethane film. Upon contact between the coupling agent layer on the polyurethane film and the molten polyphenylene ether, molecular cross-linking occurs between the polyurethane film, the coupling agent layer, and the molten polyphenylene ether due to the high surface activity of the molten polyphenylene ether. During cooling, hydrogen bonds are formed. These molecular cross-linking and hydrogen bonding enhance the bonding force between the polyurethane film and the polyphenylene ether, and these effects do not degrade over time, thus preventing the polyurethane film from detaching from the polyphenylene ether and extending the service life of the polyphenylene ether-polyurethane composite material. Furthermore, the preparation method of the polyphenylene ether-polyurethane composite material of the present invention eliminates the need for adhesive spraying, is less affected by external factors, and produces a polyphenylene ether-polyurethane composite material with stable quality and a high product qualification rate.

[0011] Preferably, the thickness of the polyurethane film is 1-2 mm. If the polyurethane film is too thin, the interaction area between the molten polyphenylene ether and the polyurethane film will be too thin, reducing the bonding force between them. If the polyurethane film is too thick, the deformation difference between the heated surface (the side in contact with the molten polyphenylene ether) and the unheated surface (the side in contact with the inner wall of the mold) of the polyurethane film will be large during the lamination process, resulting in a large difference in the deformation rate of the polyurethane film in the thickness direction, thereby reducing the flatness of the polyurethane film and the bonding force between the polyphenylene ether and the polyurethane film.

[0012] In this invention, the polyurethane film is a thermosetting polyurethane, which can be prepared using a commercially available two-component polyurethane adhesive, such as HT8666 two-component polyurethane adhesive produced by Huitian New Materials. Preferably, the polyurethane film is prepared by a method comprising the following steps: mixing components A and B of the HT8666 two-component polyurethane adhesive according to a specified ratio to obtain a mixture, then pouring the mixture into a mold for curing reaction, and obtaining the polyurethane film after demolding.

[0013] Preferably, the surface roughness of the polyurethane film to be coated with the coupling agent is 3–5 μm. If the surface roughness of the polyurethane film to be coated with the coupling agent is too small, it is not conducive to the penetration of the coupling agent into the polyurethane film matrix, reducing the contact area between the polyurethane film and the coupling agent, resulting in a decrease in the bonding force between the polyphenylene ether and the polyurethane. If the surface roughness of the polyurethane film to be coated with the coupling agent is too large, it will lead to poor continuity and uniformity of the polyurethane film, resulting in a decrease in the mechanical properties of the polyurethane film, and failing to guarantee the wear resistance and service life of the polyurethane film on the polyphenylene ether.

[0014] Preferably, the thickness of the coupling agent layer is 8–12 μm.

[0015] Preferably, the coupling agent layer is prepared by a method comprising the following steps: coating a coupling agent solution onto a polyurethane film, and after the solvent evaporates, forming a coupling agent layer on the polyurethane film. Preferably, the coupling agent solution is composed of a silane coupling agent and an alcohol solvent, wherein the mass fraction of the silane coupling agent is 8-10%. Preferably, the alcohol solvent is methanol or ethanol.

[0016] This invention does not limit the molecular weight of the polyphenylene ether; both polyphenylene ether and modified polyphenylene ether are applicable. However, both polyphenylene ether and modified polyphenylene ether must meet the requirements of injection molding. The polyphenylene ether used in this invention is a commercially available product, such as ZMPPE50 polyphenylene ether produced by Dalian Zhongmu Chemical Co., Ltd., and OS10F265 polyphenylene ether produced by Handan Fengfeng Xinbao New Material Technology Co., Ltd. Preferably, the number-average molecular weight of the polyphenylene ether is 10,000 to 20,000. For example, the number-average molecular weight of the polyphenylene ether is 14,000 to 18,000.

[0017] Preferably, the temperature of the molten polyphenylene ether is 241–245°C.

[0018] Preferably, the molten polyphenylene ether is coated onto the polyurethane film by injection molding.

[0019] Preferably, the injection molding method includes the following steps: laying a polyurethane film containing a coupling agent layer flat on the bottom of a mold with the coupling agent layer facing upwards, and then injecting molten polyphenylene ether into the mold to coat the polyurethane film with the molten polyphenylene ether.

[0020] Preferably, the injection pressure during injection molding is 110–140 MPa. Injection pressure refers to the pressure applied to the molten plastic by the plunger or screw tip. Its function is to overcome the flow resistance of the molten plastic from the barrel to the mold cavity, to provide the melt with a certain filling rate, and to compact and compensate for shrinkage. During injection, the pressure is highest at the injection nozzle to overcome the flow resistance of the melt throughout its flow. Subsequently, the pressure gradually decreases along the flow length to the front end of the melt. If the mold cavity has good venting, the final pressure at the front end of the melt is atmospheric pressure. As the injection pressure increases, the filling speed of the plastic accelerates, the weld strength in the product increases, and the density of the product increases. However, the internal stress of the product also increases with the increase of injection pressure, making it prone to deformation after molding, resulting in a poorer bond between the polyurethane film and the polyphenylene ether.

[0021] Preferably, the temperature inside the mold during injection molding is 237–247°C. For example, the temperature inside the mold during injection molding is 246–247°C. Excessive mold temperature will cause oxidation, aging, and deformation of the polyurethane film, leading to a deterioration in the wear resistance and other properties of the polyurethane layer in the composite material. Conversely, excessively low mold temperature will cause the molten polyphenylene ether injected into the mold to cool down too quickly, preventing the effective formation of hydrogen bonds and macromolecular crosslinks with the polyurethane film, resulting in a reduced bonding strength between the polyphenylene ether and the polyurethane film.

[0022] Preferably, after injection molding, the holding pressure within the mold cavity is 0.5–0.8 MPa, and the holding time is 5–7 minutes. Holding pressure refers to the pressure applied to the melt within the mold for a period after the injection pressure has completed filling the mold (the cooling and solidification time after melt filling). The purpose of holding pressure is to solidify the plastic under pressure and provide sufficient melt replenishment during melt cooling and shrinkage to ensure the density and dimensional accuracy of the molded product. In production, the holding pressure is generally less than or equal to the injection pressure. Higher holding pressure results in products with higher density, lower shrinkage, higher dimensional accuracy, and better mechanical properties, but also greater residual stress after demolding, which can easily lead to overflow and flash. Insufficient holding pressure results in incomplete molding.

[0023] Preferably, the cooling rate to room temperature is 3–5 °C / min. If the cooling rate is too slow, the polyurethane film will be heated for too long, leading to oxidation or performance degradation, and resulting in low production efficiency. If the cooling rate is too fast, the interaction time between the polyphenylene ether, the coupling agent layer, and the polyurethane film will be too short, preventing the effective formation of hydrogen bonds and macromolecular crosslinking, thus weakening the bonding force between the polyphenylene ether and the polyurethane film.

[0024] It is understood that the polyphenylene ether-polyurethane composite material of the present invention includes a polyurethane layer and a polyphenylene ether layer, with a coupling agent layer between the polyurethane layer and the polyphenylene ether layer. Preferably, the thickness of the polyphenylene ether layer in the polyphenylene ether-polyurethane composite material is not less than 10 mm.

[0025] The technical solution adopted in the polyphenylene ether-polyurethane composite material of the present invention is as follows:

[0026] A polyphenylene ether-polyurethane composite material prepared by the method described above.

[0027] The polyphenylene ether-polyurethane composite material of the present invention includes polyphenylene ether and a polyurethane film composited on polyphenylene ether. A coupling agent layer is coated on the polyurethane film. There are molecular crosslinking and hydrogen bonds between the polyurethane film, the coupling agent and the polyphenylene ether. There is a high bonding force between the polyphenylene ether and the polyurethane film, which can improve the service life of the polyphenylene ether-polyurethane composite material. Attached Figure Description

[0028] Figure 1 This is a schematic flowchart of the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 of the present invention. Detailed Implementation

[0029] The technical solution of the present invention will be further described below with reference to specific embodiments. It should be noted that the purpose of this embodiment is to further illustrate the present invention and is not intended to limit the scope of protection of the present invention.

[0030] I. Specific embodiments of the preparation method of the polyphenylene ether-polyurethane composite material of the present invention are as follows:

[0031] Example 1

[0032] The preparation method of the polyphenylene ether-polyurethane composite material in this embodiment is as follows: Figure 1 As shown, the specific steps include:

[0033] (1) Preparation of coupling agent modified polyurethane film

[0034] The A and B components of the HT8666 two-component polyurethane adhesive produced by Huitian New Materials Co., Ltd. were added to a mixing tank in a specified ratio (the mass ratio of component A to component B is 7:1, and component B is the curing agent). After stirring evenly, a mixture was obtained. The mixture was then poured into a mold for curing reaction. After the reaction was completed, the polyurethane film was demolded from the mold to obtain a polyurethane film with a thickness of 1 mm (the roughness of the upper and lower surfaces of the polyurethane film is 3 μm). Then, a silane coupling agent solution (the silane coupling agent solution is composed of KH550 and ethanol, and the mass fraction of KH550 is 8%) was brushed onto the upper and lower surfaces of the polyurethane film. After brushing, the solvent evaporated, and a coupling agent layer with a thickness of 8 μm was formed on the upper and lower surfaces of the polyurethane film, thus obtaining a coupling agent modified polyurethane film.

[0035] (2) The coupling agent-modified polyurethane film is laid flat on the bottom of the polyphenylene ether injection mold (the shape and size of the coupling agent-modified polyurethane film are the same as the shape and size of the bottom surface of the mold), pressed and compacted, and then the molten polyphenylene ether is injected into the mold. After the injection molding is completed, it is cooled to room temperature and demolded to obtain polyphenylene ether-polyurethane composite material (the thickness of the polyphenylene ether layer in the polyphenylene ether-polyurethane composite material is 20cm).

[0036] In this embodiment, the polyphenylene ether is manufactured by Handan Fengfeng Xinbao New Material Technology Co., Ltd., and the product model is OS10F265. The temperature of the molten polyphenylene ether is 241°C, the injection pressure during injection molding is 120MPa, the temperature inside the mold is 246°C when the molten polyphenylene ether is injected into the mold, the holding pressure inside the mold cavity is 0.5MPa after the molten polyphenylene ether is injected, the holding time is 7min, and the cooling rate to room temperature is 5°C / min.

[0037] Example 2

[0038] The preparation method of the polyphenylene ether-polyurethane composite material in this embodiment specifically includes the following steps:

[0039] (1) Preparation of coupling agent modified polyurethane film

[0040] The A and B components of the HT8666 two-component polyurethane adhesive produced by Huitian New Materials Co., Ltd. were added to a mixing tank in a specified ratio (the mass ratio of component A to component B is 7:1, and component B is the curing agent). After stirring evenly, a mixture was obtained. The mixture was then poured into a mold for curing reaction. After the reaction was completed, the polyurethane film was demolded from the mold to obtain a polyurethane film with a thickness of 1.5 mm (the roughness of the upper and lower surfaces of the polyurethane film is 5 μm). Then, a silane coupling agent solution (the silane coupling agent solution is composed of KH550 and ethanol, and the mass fraction of KH550 is 8%) was brushed onto the upper and lower surfaces of the polyurethane film. After brushing, the solvent evaporated, and a coupling agent layer with a thickness of 12 μm was formed on each of the upper and lower surfaces of the polyurethane film, thus obtaining a coupling agent modified polyurethane film.

[0041] (2) The coupling agent-modified polyurethane film is laid flat on the bottom of the polyphenylene ether injection mold (the shape and size of the coupling agent-modified polyurethane film are the same as the shape and size of the bottom surface of the mold), pressed and compacted, and then the molten polyphenylene ether is injected into the mold. After the injection molding is completed, it is cooled to room temperature and demolded to obtain polyphenylene ether-polyurethane composite material (the thickness of the polyphenylene ether layer in the polyphenylene ether-polyurethane composite material is 20cm).

[0042] In this embodiment, the polyphenylene ether is manufactured by Dalian Zhongmu Chemical Co., Ltd., and the product model is ZMPPE50. The temperature of the molten polyphenylene ether is 245°C, the injection pressure during injection molding is 140MPa, the temperature inside the mold is 247°C when the molten polyphenylene ether is injected into the mold, the holding pressure inside the mold cavity is 0.8MPa after the molten polyphenylene ether is injected, the holding time is 7min, and the cooling rate used to cool to room temperature is 5°C / min.

[0043] Example 3

[0044] The preparation method of the polyphenylene ether-polyurethane composite material in this embodiment specifically includes the following steps:

[0045] (1) Preparation of coupling agent modified polyurethane film

[0046] The A and B components of the HT8666 two-component polyurethane adhesive produced by Huitian New Materials Co., Ltd. were added to a mixing tank in a specified ratio (the mass ratio of component A to component B is 7:1, and component B is the curing agent). After stirring evenly, a mixture was obtained. The mixture was then poured into a mold for curing reaction. After the reaction was completed, the polyurethane film was demolded from the mold to obtain a polyurethane film with a thickness of 2 mm (the roughness of the upper and lower surfaces of the polyurethane film is 4 μm). Then, a silane coupling agent solution (the silane coupling agent solution is composed of KH550 and ethanol, and the mass fraction of KH550 is 8%) was brushed onto the upper and lower surfaces of the polyurethane film. After brushing, the solvent evaporated, and a coupling agent layer with a thickness of 10 μm was formed on each of the upper and lower surfaces of the polyurethane film, thus obtaining a coupling agent modified polyurethane film.

[0047] (2) The coupling agent-modified polyurethane film is laid flat on the bottom of the polyphenylene ether injection mold (the shape and size of the coupling agent-modified polyurethane film are the same as the shape and size of the bottom surface of the mold), pressed and compacted, and then the molten polyphenylene ether is injected into the mold. After the injection molding is completed, it is cooled to room temperature and demolded to obtain polyphenylene ether-polyurethane composite material (the thickness of the polyphenylene ether layer in the polyphenylene ether-polyurethane composite material is 20cm).

[0048] In this embodiment, the polyphenylene ether is manufactured by Handan Fengfeng Xinbao New Material Technology Co., Ltd., and the product model is OS10F265. The temperature of the molten polyphenylene ether is 241°C, the injection pressure during injection molding is 110MPa, the temperature inside the mold is 246°C when the molten polyphenylene ether is injected into the mold, the holding pressure inside the mold cavity is 0.8MPa after the molten polyphenylene ether is injected, the holding time is 5min, and the cooling rate used to cool to room temperature is 3°C / min.

[0049] Comparative Example 1

[0050] The only difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the thickness of the polyurethane film used in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is 0.8 mm.

[0051] Comparative Example 2

[0052] The only difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the thickness of the polyurethane film used in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is 2.5 mm.

[0053] Comparative Example 3

[0054] The only difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the temperature of the molten polyphenylene ether in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is 260°C.

[0055] Comparative Example 4

[0056] The only difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the temperature of the molten polyphenylene ether in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is 232°C.

[0057] Comparative Example 5

[0058] The only difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the injection pressure during injection molding in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is 150 MPa.

[0059] Comparative Example 6

[0060] The only difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the injection pressure during injection molding in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is 90 MPa.

[0061] Comparative Example 7

[0062] The only difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the roughness of the upper and lower surfaces of the polyurethane film in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is 1 μm.

[0063] Comparative Example 8

[0064] The difference between the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example and the preparation method of the polyphenylene ether-polyurethane composite material in Example 1 is that the silane coupling agent solution used in the preparation method of the polyphenylene ether-polyurethane composite material in this comparative example is composed of KH560 and ethanol, and the mass fraction of KH560 is 8%.

[0065] Comparative Example 9

[0066] The preparation method of the polyphenylene ether-polyurethane composite material in this comparative example specifically includes the following steps:

[0067] Molten polyphenylene ether (PPE) was injected into a mold. After injection molding, the mixture was cooled to room temperature and demolded to obtain a PPE board (the size of the PPE board was the same as the size of the PPE layer in the PPE-polyurethane composite material prepared in Example 1). Then, a silane coupling agent solution (the same silane coupling agent solution used in Example 1) was applied to the upper and lower surfaces of the PPE board. The solvent evaporated, forming a coupling agent layer with a thickness of 8 μm on each of the upper and lower surfaces of the PPE board. Then, the mixture (the same mixture used in Example 1) was uniformly sprayed onto the upper surface of the PPE board using a cold spraying method. After curing, a polyurethane film with a thickness of 1 mm was formed on the coupling agent layer on the PPE board, thus obtaining the PPE-polyurethane composite material.

[0068] II. Specific embodiments of the polyphenylene ether-polyurethane composite material of the present invention are as follows:

[0069] The polyphenylene ether-polyurethane composite material of this embodiment was prepared by any of the preparation methods of polyphenylene ether-polyurethane composite materials in Examples 1-3, and will not be described again here.

[0070] Experimental Example

[0071] To evaluate the bonding strength between polyphenylene ether (PPE) and polyurethane film in commercially available PPE-polyurethane composites (formed by bonding polyurethane film and PPE together with an adhesive), PPE-polyurethane composites prepared in Examples 1-3 and Comparative Examples 1-9, each PPE-polyurethane composite was cut into samples of the same shape and size, and then the bonding strength between polyurethane film and PPE in each sample was tested using a universal testing machine. The test results are shown in Table 1.

[0072] Table 1. Bond strength between polyurethane film and polyphenylene ether in different polyphenylene ether-polyurethane composites

[0073]

[0074]

[0075] To test the quality stability of different polyphenylene ether-polyurethane composites, 20 commercially available polyphenylene ether-polyurethane composites of the same model and batch were randomly selected as comparisons. Then, polyphenylene ether-polyurethane composites were prepared repeatedly according to the methods of Examples 1-3 and Comparative Examples 1-9, with 20 samples prepared for each method. The bonding strength between the polyurethane film and polyphenylene ether in each sample was then tested. Finally, the bonding strength between the polyurethane film and polyphenylene ether in all samples prepared by each method was statistically analyzed, and the coefficient of variation (coefficient of variation = standard deviation / mean × 100%) was calculated. The coefficient of variation was used to evaluate the quality stability of the polyphenylene ether-polyurethane composites prepared by each method. The coefficients of variation of the bonding strength between the polyurethane film and polyphenylene ether in polyphenylene ether-polyurethane composites prepared by different methods are shown in Table 2.

[0076] Table 2. Coefficients of variation of the bonding strength between polyurethane film and polyphenylene ether in polyphenylene ether-polyurethane composites prepared by different methods.

[0077] Composite materials Coefficient of variation (%) Composite materials Coefficient of variation (%) Commercially available products 25.6 Comparative Example 4 38.7 Example 1 8.8 Comparative Example 5 11.1 Example 2 7.6 Comparative Example 6 10.9 Example 3 9.8 Comparative Example 7 9.5 Comparative Example 1 10.2 Comparative Example 8 8.6 Comparative Example 2 8.4 Comparative Example 9 29.4 Comparative Example 3 33.5 - -

Claims

1. A method for producing a polyphenylene ether-polyurethane composite material, characterized by, Includes the following steps: (1) Coating a coupling agent onto a polyurethane film to form a coupling agent layer, wherein the coupling agent is a silane coupling agent, and the silane coupling agent is KH550 and / or KH560; the surface roughness of the polyurethane film to be coated with the coupling agent is not less than 3μm; the polyurethane film is a thermosetting polyurethane. (2) Molten polyphenylene ether is coated onto the coupling agent layer by injection molding, and after cooling to room temperature, a polyphenylene ether-polyurethane composite material is obtained; the temperature of the molten polyphenylene ether is 235~245℃; the injection pressure is 110~140MPa during injection molding.

2. The method of producing a polyphenylene ether-polyurethane composite material according to claim 1, wherein The thickness of the polyurethane film is 1-2 mm; the thickness of the coupling agent layer is 8-12 μm.

3. The method of producing a polyphenylene ether-polyurethane composite material according to claim 1, wherein The surface roughness of the polyurethane film to be coated with the coupling agent is 3~5μm; the temperature of the molten polyphenylene ether is 241~245℃.

4. The method of producing a polyphenylene ether-polyurethane composite material according to any one of claims 1 to 3, characterized by, The coupling agent layer is prepared by a method comprising the following steps: coating a coupling agent solution onto a polyurethane film, and after the solvent evaporates, forming a coupling agent layer on the polyurethane film.

5. The method for preparing the polyphenylene ether-polyurethane composite material as described in claim 4, characterized in that, The coupling agent solution is composed of a silane coupling agent and an alcohol solvent, wherein the mass fraction of the silane coupling agent is 8-10%.

6. The method of producing a polyphenylene ether-polyurethane composite material according to claim 4, wherein During injection molding, the temperature inside the mold is 237~247℃.

7. The method of producing a polyphenylene ether-polyurethane composite material according to claim 6, wherein During injection molding, the temperature inside the mold is 246~247℃.

8. The method of producing a polyphenylene ether-polyurethane composite material according to claim 4, wherein After injection molding, the holding pressure in the mold cavity is 0.5~0.8MPa, and the holding time is 5~7min.

9. The method of making a polyphenylene ether-polyurethane composite of any one of claims 1-3, wherein, The cooling rate used to cool to room temperature is 3~5℃ / min.

10. A polyphenylene ether-polyurethane composite material prepared by the method for preparing polyphenylene ether-polyurethane composite materials according to any one of claims 1-9.

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