An end group functionalized polyphenylene ether modified epoxy resin and a method for preparing the same

Abstract

The application provides an end group functionalized polyphenyl ether modified epoxy resin and a preparation method thereof. The end group functionalized polyphenyl ether modified epoxy resin comprises the following raw material components: an epoxy resin, SA9000, a curing agent, a catalyst and an initiator; wherein the amount of the methyl acryloyl polyphenyl ether is 5-30 wt% of the epoxy resin; the amount of the curing agent is 60-90 wt% of the epoxy resin; the amount of the catalyst is 0.5-3 wt% of the epoxy resin; and the amount of the initiator is 0.5-3 wt% of the methyl acryloyl polyphenyl ether. The method comprises the following steps: S1, reacting SA90 with MeAc in the presence of toluene and triethylamine to obtain SA9000; S2, heating and melting the epoxy resin and SA9000 to obtain a mixed glue solution; adding the curing agent, the catalyst and the initiator into the mixed glue solution, and then performing heating, stirring, reaction and vacuum degassing; and then pouring the obtained mixed solution into a mold, and then performing curing, temperature reduction and demolding to obtain the end group functionalized polyphenyl ether modified epoxy resin.

Description

Technical Field

[0001] This invention belongs to the field of functional composite materials technology, and particularly relates to an end-functionalized polyphenylene ether modified epoxy resin and its preparation method. Background Technology

[0002] Epoxy resins possess excellent mechanical properties, electrical insulation, adhesion, and processing performance, making them widely used in electronic packaging, aerospace materials, and other fields. However, cured epoxy resins suffer from problems such as high brittleness, low impact strength, and insufficient heat resistance. Furthermore, their dielectric constant and dielectric loss are insufficient to meet the demands of high-speed, high-frequency electronic applications. These shortcomings limit their application in high-end electronic packaging and advanced composite materials.

[0003] Polyphenylene oxide (PPO) possesses extremely low dielectric constant and dielectric loss, high glass transition temperature, and excellent dimensional stability, making it an ideal modifier for improving the dielectric properties and heat resistance of epoxy resins. However, the ends of PPO molecular chains are typically inert methyl groups, resulting in poor compatibility with epoxy resins. Furthermore, it lacks reactive functional groups, hindering effective chemical interactions with the epoxy resin matrix. Therefore, traditional methods often involve physically blending PPO into epoxy resin systems. However, this simple physical mixing tends to leave PPO in a "sea-like" form outside the epoxy crosslinking network, limiting its performance enhancement.

[0004] To improve interfacial compatibility, researchers have attempted to modify polyphenylene ethers (PPO) by end-group functionalization. For example, in the paper "Synthesis Study of Low Molecular Weight Dihydroxyl-Terminated Polyphenylene Ethers" published in Volume 49, Issue 1, 2021 of *Plastics Industry*, dihydroxyl-terminated polyphenylene ethers (PPO-OH) were successfully prepared using 2,6-dimethylphenol and tetramethylbisphenol A as copolymer monomers. However, the reactivity of hydroxyl groups with epoxy groups is limited, making it difficult to achieve sufficient chemical bonding in conventional epoxy curing systems, thus limiting the improvement on the overall performance of epoxy resins. Summary of the Invention

[0005] To address the aforementioned technical problems, this invention provides a method for preparing epoxy resin modified with end-functionalized polyphenylene ether, which improves the heat resistance and mechanical properties of epoxy resin composites while reducing their dielectric properties.

[0006] To achieve the above objectives, the present invention provides the following technical solution: This invention provides an epoxy resin modified with end-functionalized polyphenylene ether, comprising the following raw material components: epoxy resin, methacrylonitrile polyphenylene ether (SA9000), curing agent, catalyst, and initiator; wherein the amount of methacrylonitrile polyphenylene ether is 5-30 wt% of the epoxy resin; the amount of curing agent is 60-90 wt% of the epoxy resin; the amount of catalyst is 0.5-3 wt% of the epoxy resin; and the amount of initiator is 0.5-3 wt% of the methacrylonitrile polyphenylene ether.

[0007] Furthermore, the epoxy resin is preferably a bisphenol A type epoxy resin; the curing agent is at least one of methyltetrahydrophthalic anhydride (MTHPA), methylhexahydrophthalic anhydride (MHHPA), and methylnadic anhydride (MNA); the catalyst is 2,4,6-tris(dimethylaminomethyl)phenol (DMP-30) or benzyl dimethylamine (BDMA); and the initiator is benzoyl peroxide or azobisisobutyronitrile.

[0008] The present invention also provides a method for preparing the above-mentioned end-functionalized polyphenylene ether modified epoxy resin, the method comprising: S1, using toluene as a solvent, reacting phenolic hydroxyl polyphenylene ether (SA90) with methacryloyl chloride in the presence of triethylamine to obtain methacryloyl polyphenylene ether; S2, heating and melting the epoxy resin and methacryloyl polyphenylene ether to obtain an epoxy resin solution; sequentially adding a curing agent, a catalyst and an initiator to the epoxy resin solution, heating and stirring to react and degassing under vacuum, and after the obtained system is cured, obtaining the end-functionalized polyphenylene ether modified epoxy resin.

[0009] Further, S1 specifically includes: S11, dissolving phenolic hydroxyl polyphenylene ether and toluene by stirring to obtain a phenolic hydroxyl polyphenylene ether-toluene mixture; S12, adding triethylamine dropwise to the phenolic hydroxyl polyphenylene ether-toluene mixture, stirring and reacting at a certain temperature to obtain a first mixture; S13, dissolving methacryloyl chloride (MeAc) in toluene to obtain a methacryloyl chloride-toluene mixture; adding the methacryloyl chloride-toluene mixture dropwise to the first mixture, reacting at a certain temperature to obtain a second mixture; slowly adding the second mixture to anhydrous ethanol, stirring thoroughly until the solid is completely precipitated, filtering under reduced pressure, soaking the obtained solid in deionized water, filtering under reduced pressure, washing with anhydrous ethanol, and then vacuum drying to obtain methacryloyl polyphenylene ether.

[0010] Further, the following dosage ratios are used: S11 specifically includes: dissolving 7.5–15 g of phenolic hydroxyl polyphenylene ether in 50–100 mL of toluene at room temperature and stirring at 200–500 r / min for 0.5–1 h; S12 specifically includes: adding 6.5–13.0 mL of triethylamine, reacting at 60–80 °C for 1–2 h.

[0011] Furthermore, S13 specifically includes: dissolving 3.3–6.5 mL of methacryloyl chloride in 15–30 mL of toluene, reacting at a temperature of 60–80 °C for 6–12 h; using 375–750 mL of anhydrous ethanol; soaking in deionized water for 30–60 min; and drying under vacuum at 40–50 °C for 6–12 h.

[0012] Furthermore, S2 specifically includes: after adding the curing agent, reacting with magnetic stirring at 300-600 r / min at 60-90 ℃ for 10-30 min, followed by degassing at -0.085--0.095 MPa and 70-80 ℃ for 10-20 min; after adding the catalyst, reacting with magnetic stirring at 300-600 r / min at 60-90 ℃ for 3-8 min, followed by degassing at -0.085--0.095 MPa and 70-80 ℃ for 5-15 min; after adding the initiator, reacting with magnetic stirring at 600-1000 r / min at 50-80 ℃ for 5-15 min, followed by degassing at -0.085--0.095 MPa and 60-70 ℃ for 10-20 min.

[0013] Furthermore, S2 also includes: after heating, stirring, reacting, and vacuum degassing, casting the resulting system into a mold, curing, cooling, and demolding to obtain the end-functionalized polyphenylene ether modified epoxy resin.

[0014] Furthermore, the curing process specifically includes: degassing and curing at -0.085 to -0.095 MPa and 70 to 80 °C for 1 to 2 hours, followed by curing at 110 to 120 °C for 1 to 2 hours, then curing at 160 °C for 2 to 3 hours, and finally curing at 180 to 200 °C for 2 to 3 hours.

[0015] This invention also provides the application of the above-mentioned end-functionalized polyphenylene ether modified epoxy resin in the fields of high-frequency and high-speed electronic packaging and advanced aerospace composite materials.

[0016] Compared with the prior art, the beneficial effects of the present invention are as follows: (1) This invention innovatively prepares methacryloyl-terminated polyphenylene ether, namely SA9000, by using MeAc as an acylation reagent to undergo an esterification reaction with SA90. Using epoxy resin as the matrix and SA9000 as the modifier, under the action of a synergistic curing system composed of curing agent, catalyst and initiator, a class of epoxy resins modified with end-functionalized polyphenylene ether with strong interfacial bonding is prepared through chemical bonding and dual curing mechanism.

[0017] (2) Compared with the traditional "physical blending" or "single curing" polyphenylene ether modification methods, the present invention enables polyphenylene ether to be chemically integrated into the epoxy network through molecular design, which fundamentally solves the problem of poor interfacial compatibility, thereby synergistically improving the mechanical properties, heat resistance and dielectric properties of the material.

[0018] (3) The preparation method provided by the present invention has a clear molecular design concept and strong process controllability. The resulting composite material has excellent properties such as high glass transition temperature, low dielectric constant and loss, and has important application value in the fields of high frequency and high speed electronic packaging and advanced aerospace composite materials.

[0019] The resulting composite material exhibits a glass transition temperature of 176 °C, which is 22.4% higher than that of pure epoxy resin. This invention features mild operating conditions, a short process flow, low energy consumption, and suitability for large-scale production, providing innovative ideas and effective strategies for the development of high-performance epoxy resin encapsulation materials. Attached Figure Description

[0020] Figure 1 The reaction formula for the reaction of SA90 with MeAc to generate SA9000 in the embodiments of the present invention; Figure 2 Infrared spectra of SA90 and SA9000 according to embodiments of the present invention; Figure 3 The NMR spectra of SA90 and SA9000 in this embodiment of the invention; Figure 4 The mechanical loss of epoxy resin and the mechanical loss of Examples 1-4 of the present invention varies with temperature. Detailed Implementation

[0021] The inventors discovered that the methacryloyl group is a functional group containing an active carbon-carbon double bond, which can undergo efficient polymerization in the presence of a free radical initiator. Introducing the methacryloyl group into the polymer chain end via esterification can endow the material with free radical polymerization properties. If the polyphenylene ether end is modified to a methacryloyl group and combined with a suitable epoxy resin curing system, it is expected to participate in the curing and crosslinking network of the epoxy resin through free radical polymerization, constructing a synergistically cured composite material. This would enhance the interfacial bonding between the two phases, thereby significantly improving the overall performance of the epoxy resin-based composite material.

[0022] Based on this, the present invention provides a method for preparing end-functionalized polyphenylene ether modified epoxy resin, such as... Figure 1 As shown, the method includes: S1, using toluene as a solvent, reacting SA90 with MeAc in the presence of triethylamine to obtain end-functionalized SA9000; S2, heating and melting epoxy resin and SA9000 to obtain epoxy resin solution; sequentially adding curing agent, catalyst and initiator to the epoxy resin solution, heating and stirring to react and then degassing under vacuum, casting the resulting mixture into a mold, curing, cooling and demolding to obtain the end-functionalized polyphenylene ether modified epoxy resin.

[0023] Preferably, the end-functionalized polyphenylene ether modified epoxy resin uses SA9000 as a reactive modifier, and its technical route is as follows: Using epoxy resin as the matrix, SA9000 is introduced, and the material structure is constructed through a stepwise curing mechanism under the synergistic effect of anhydride curing agent, catalyst, and initiator. Specifically, SA9000 undergoes free radical polymerization under the action of the initiator to form polyphenylene ether-based segments or micronetworks. Simultaneously, the epoxy resin undergoes ring-opening polymerization under the action of the curing agent and catalyst to form a three-dimensional cross-linked network. During the curing process, the two interpenetrate and intertwine, ultimately forming a stable interpenetrating or semi-interpenetrating polymer network structure. After vacuum degassing and programmed curing, an end-functionalized polyphenylene ether modified epoxy resin with excellent dielectric properties, high heat resistance, and good mechanical properties is obtained. In this invention, SA9000 has good solubility in epoxy resin, the system viscosity is suitable, it is easy to vacuum degas and process, the overall process conditions are mild, and it has the potential for large-scale production. The composite material provided by this invention has low dielectric loss, high glass transition temperature, excellent interface stability and molding processability. It is an ideal candidate system for high-frequency / high-speed printed circuit board substrates, advanced semiconductor packaging molding materials, and high-performance structural adhesives and composite materials in the aerospace field. It provides an innovative and feasible technical strategy for the development of next-generation high-performance electronic packaging and insulation materials.

[0024] The present invention will now be described in detail with reference to specific embodiments. The embodiments given in this section are merely illustrative and should not be construed as limiting the scope of protection of the present invention. All other embodiments obtained by those skilled in the art based on the embodiments of the present invention without inventive effort are within the scope of protection of the present invention.

[0025] In this invention, unless otherwise specified, all equipment and raw materials are commercially available or commonly used in the industry. The methods described in the following embodiments are conventional methods in the art, unless otherwise specified.

[0026] The epoxy resin used in this embodiment of the invention is preferably a bisphenol A type epoxy resin, and more specifically, the selected bisphenol A type epoxy resin is E51. The curing agent used in this embodiment of the invention is at least one of MHHPA, MTHPA, and MNA, and the catalyst used is DMP-30 or BDMA.

[0027] Preferably, the method for preparing SA9000 according to embodiments of the present invention includes: sequentially adding 7.5–15 g SA90 and 50–100 mL toluene to a three-necked flask, stirring at 200–500 r / min for 0.5–1 h at room temperature until the solid is completely dissolved; then, under nitrogen protection, adding 6.5–13.0 mL triethylamine dropwise to the mixture, reacting at 60–80 °C for 1–2 h; dissolving 3.3–6.5 mL MeAc in 15–30 mL toluene, and adding this solution dropwise to an alkaline mixture, then adding the mixture dropwise to the three-necked flask; subsequently, continuing the reaction at 60–80 °C for 6–12 h; cooling the mixture to room temperature, and then slowly adding the mixture to 375–750 mL anhydrous ethanol with rapid stirring; after the solid has completely precipitated, filtering under reduced pressure. The solid was transferred to a beaker, soaked in an appropriate amount of deionized water for 30-60 min, filtered under reduced pressure, soaked in an appropriate amount of deionized water for another 30-60 min, filtered under reduced pressure again, and washed with anhydrous ethanol 2-3 times. The product was then dried under vacuum at 40-50 °C for 6-12 h to obtain a dry solid, thus obtaining SA9000.

[0028] Example 1 Add 20 g of epoxy resin to the reaction flask, preheat to 80 °C until it reaches a fluid state, then raise the temperature to 100 °C and add 1.0 g of SA9000 powder. Turn on the magnetic stirrer and set the speed to 400–500 r / min, stirring for 3–4 h until the polyphenylene ether is completely melted and the system is homogeneous and transparent. Cool down to 80 °C, add 17 g of curing agent MHHPA and 0.2 g of catalyst DMP-30, maintain the speed at 400–500 r / min, and stir for 15 min. Then, place the mixture in an 80 °C vacuum drying oven and degas at -0.085–-0.095 MPa for 10–15 min. The temperature was lowered to 60 °C, and 0.01 g of benzoyl peroxide was added. The mixture was stirred at 700–800 r / min for 10 min, and then placed in a vacuum drying oven at 60 °C for degassing at -0.085–-0.095 MPa for 10 min. The mixture was poured into a stainless steel mold preheated to 80 °C, and pre-cured at 80 °C and -0.085–-0.095 MPa for 1 h. Then, the temperature was raised to 120 °C and cured at normal pressure for 1 h, then raised to 160 °C and cured for 2 h. Finally, the temperature was raised to 210 °C and cured for 2 h. After naturally cooling to room temperature, the fully cured end-functionalized polyphenylene ether modified epoxy resin was demolded, denoted as S1.

[0029] Example 2 Add 10 g of epoxy resin to the reaction flask, preheat to 80 °C until it reaches a fluid state, then raise the temperature to 100 °C and add 1.0 g of SA9000 powder. Turn on the magnetic stirrer and set the speed to 400–500 r / min, stirring for 3–4 h until the polyphenylene ether is completely melted and the system is homogeneous and transparent. Cool down to 80 °C, add 8.5 g of curing agent MHHPA and 0.1 g of catalyst DMP-30, maintain the speed at 400–500 r / min, and stir for 15 min. Then, place the mixture in an 80 °C vacuum drying oven and degas at -0.085–-0.095 MPa for 10–15 min. The temperature was lowered to 60 °C, and 0.01 g of benzoyl peroxide was added. The mixture was stirred at 700–800 r / min for 10 min, and then placed in a vacuum drying oven at 60 °C for degassing at -0.085–-0.095 MPa for 10 min. The mixture was poured into a stainless steel mold preheated to 80 °C, and pre-cured at 80 °C and -0.085–-0.095 MPa for 1 h. Then, the temperature was raised to 120 °C and cured at normal pressure for 1 h, then raised to 160 °C and cured for 2 h, and finally raised to 210 °C and cured for 2 h. After naturally cooling to room temperature, the fully cured end-functionalized polyphenylene ether modified epoxy resin was demolded, denoted as S2.

[0030] Example 3 The difference between Example 3 and Example 2 is that the amount of SA9000 added is 2.0 g, and the amount of benzoyl peroxide added is 0.02 g. The remaining steps are the same as in Example 2, and the resulting product is denoted as S3.

[0031] Example 4 The difference between Example 4 and Example 2 is that the amount of SA9000 added is 3.0 g, and the amount of benzoyl peroxide added is 0.03 g. The remaining steps are the same as in Example 2, and the resulting product is denoted as S4.

[0032] The SA9000 sample underwent structural and compositional analysis, and the test results are shown below.

[0033] Figure 1 This is the design and synthesis reaction formula for Example SA9000; Figure 2 The infrared spectra of SA90 and Example SA9000 are shown in the figure. As can be seen from the figure, after methacryloyl substitution, the infrared spectrum of SA90 at 3300 cm⁻¹ is significantly higher. -1 ~3630 cm -1 The characteristic stretching vibrations of the hydroxyl groups, which have lower intensity and larger width at 1745 cm, disappear, while at 1745 cm... -1 A new absorption peak appears at 1140 cm⁻¹, attributed to the stretching vibration of the C=O bond. -1 The appearance of a stretching vibration peak of the CO bond indicates that the methacryloyl group has successfully substituted the terminal hydrogen atom of SA90. Figure 3 The NMR spectra of SA90 and SA9000 in this embodiment of the invention are obtained from... Figure 3 As can be seen from point a: the disappearance of the hydrogen peak on the benzene ring at 6.7-6.8 ppm in the product indicates that the reactants have reacted completely; Figure 3 The presence of double-bonded hydrogen atom signals at 5.80 ppm and 6.36 ppm in sample b indicates successful preparation of SA9000. The flexural mechanical properties and dielectric properties of the epoxy resin and Examples 1 to 4 were tested, and the results are shown below.

[0034] Table 1. Test results of flexural mechanical properties and dielectric properties of epoxy resin and Examples 1-4

[0035] The test results above show that the flexural strength and flexural modulus of the samples in Examples 1-4 first increased and then slightly decreased with the increase of SA9000 addition; the dielectric constant and dielectric loss of Examples 1-4 showed a trend of first decreasing and then slightly increasing, but were always lower than those of pure epoxy resin.

[0036] Glass transition temperature of resin materials ( T g) can be characterized by dynamic thermomechanical analysis, often using the mechanical loss peak ( tanδ The corresponding temperature is used to represent it. T g . Figure 4 The results are dynamic thermomechanical analysis of epoxy resin and Examples 1-4. A single cantilever mode was used during testing to accurately record the length, width, and thickness of the sample. The testing frequency was 1 Hz, the temperature range was 50~230 ℃, and the heating rate was 5 K / min. Based on... Figure 4 As the temperature rises, the losses in Examples 1 to 4 continuously increase, reaching a peak ( T g After that, the glass transition temperature (Tg) began to decrease. Compared with epoxy resin, the glass transition temperature of Examples 1 to 4 was significantly increased, and the dynamic thermomechanical analysis (DMA) curves of Examples 2 to 4 showed a double peak. The possible reason is that the methacryloyl group at the end of SA9000 can undergo free radical polymerization under the initiation of benzoyl peroxide (BPO) to form PPO segments. These segments form interpenetrating or semi-interpenetrating networks with the epoxy network. At the same time, the rigid PPO segments restrict the movement of epoxy segments, resulting in an increase in Tg of Examples 1 to 4. In addition, when the amount of SA9000 added is low, its compatibility with the epoxy matrix is ​​good, and no obvious phase separation occurs. The DMA curve is still a single peak. When the amount of SA9000 added reaches 10%, a double peak begins to appear. This is because after the content of SA9000 increases, the PPO segments formed by its self-polymerization tend to aggregate, forming SA9000-rich microregions. The molecular movement at the interface between these microregions and the epoxy matrix is ​​restricted, resulting in a second loss peak.

[0037] The above description is only a preferred embodiment of the present invention. It should be noted that for those skilled in the art, several improvements and modifications can be made without departing from the principle of the present invention, and the above technical features can be combined in an appropriate manner. These improvements, modifications and combinations should all be considered within the scope of protection of the present invention.

Claims

1. An epoxy resin modified with end-functionalized polyphenylene ether, characterized in that, It includes the following raw material components: epoxy resin, methacrylamide polyphenylene ether, curing agent, catalyst and initiator; The amount of the methacryloyl polyphenylene ether used is 5-30 wt% of the epoxy resin. The amount of curing agent used is 60-90 wt% of the epoxy resin; The catalyst is used in an amount of 0.5–3 wt% of the epoxy resin. The amount of the initiator is 0.5 to 3 wt% of methacryloyl polyphenylene ether.

2. The epoxy resin modified with end-functionalized polyphenylene ether according to claim 1, characterized in that, The curing agent is at least one of methyltetrahydrophthalic anhydride, methylhexahydrophthalic anhydride, and methylnadic anhydride; The catalyst is 2,4,6-tris(dimethylaminomethyl)phenol or benzyldimethylamine; The initiator is benzoyl peroxide or azobisisobutyronitrile.

3. A method for preparing an end-functionalized polyphenylene ether-modified epoxy resin according to claim 1 or 2, characterized in that, The method includes: S1. Using toluene as a solvent, phenolic hydroxy polyphenylene ether reacts with methacrylamide chloride in the presence of triethylamine to obtain methacrylamide polyphenylene ether. S2. Epoxy resin and methacrylamide polyphenylene ether are heated and melt-blended to obtain epoxy resin solution; curing agent, catalyst and initiator are added to the epoxy resin solution in sequence, heated and stirred to react and vacuum degassing are performed. After the obtained system is cured, the end-functionalized polyphenylene ether modified epoxy resin is obtained.

4. The method for preparing end-functionalized polyphenylene ether modified epoxy resin according to claim 3, characterized in that, S1 specifically includes: S11. Stir and dissolve phenolic hydroxyl polyphenylene ether and toluene to obtain a phenolic hydroxyl polyphenylene ether-toluene mixture; S12. Triethylamine is added dropwise to the phenolic hydroxy polyphenylene ether-toluene mixture, and the mixture is stirred at a certain temperature to obtain the first mixture. S13. Dissolve methacryloyl chloride in toluene to obtain a methacryloyl chloride-toluene mixture; add the methacryloyl chloride-toluene mixture dropwise to the first mixture and react at a certain temperature to obtain a second mixture; slowly add the second mixture to anhydrous ethanol, stir thoroughly until the solid is completely precipitated, filter under reduced pressure, soak the obtained solid in deionized water, filter under reduced pressure, wash with anhydrous ethanol, and dry under vacuum to obtain methacryloyl polyphenylene ether.

5. The method for preparing the end-functionalized polyphenylene ether modified epoxy resin according to claim 4, characterized in that, The following dosage ratio shall be used, specifically S11: at room temperature, 7.5-15 g of phenolic hydroxyl polyphenylene ether shall be dissolved in 50-100 mL of toluene and stirred at 200-500 r / min for 0.5-1 h; S12 specifically includes: adding 6.5–13.0 mL of triethylamine, reacting at 60–80 °C, and for 1–2 h.

6. The method for preparing the end-functionalized polyphenylene ether modified epoxy resin according to claim 5, characterized in that, S13 specifically includes: dissolving 3.3–6.5 mL of methacryloyl chloride in 15–30 mL of toluene, reacting at a temperature of 60–80 °C for 6–12 h; using 375–750 mL of anhydrous ethanol; soaking in deionized water for 30–60 min; and drying under vacuum at 40–50 °C for 6–12 h.

7. The method for preparing the end-functionalized polyphenylene ether modified epoxy resin according to claim 3, characterized in that, S2 specifically includes: after adding the curing agent, reacting with magnetic stirring at 300-600 r / min at 60-90 ℃ for 10-30 min, and then degassing at -0.085--0.095 MPa and 70-80 ℃ for 10-20 min; After adding the catalyst, the reaction was carried out at 60–90 °C with magnetic stirring at 300–600 r / min for 3–8 min, followed by degassing at -0.085–-0.095 MPa and 70–80 °C for 5–15 min. After adding the initiator, the reaction is carried out at 50–80 °C with magnetic stirring at 600–1000 r / min for 5–15 min, followed by degassing at -0.085–-0.095 MPa and 60–70 °C for 10–20 min.

8. The method for preparing end-functionalized polyphenylene ether modified epoxy resin according to claim 3, characterized in that, S2 also includes: after heating, stirring and reacting and vacuum degassing, casting the resulting system into a mold, curing, cooling and demolding to obtain the end-functionalized polyphenylene ether modified epoxy resin.

9. The method for preparing the end-functionalized polyphenylene ether modified epoxy resin according to claim 3, characterized in that, The curing process specifically includes: degassing and curing at -0.085 to -0.095 MPa and 70 to 80 ℃ for 1 to 2 hours, followed by curing at 110 to 120 ℃ for 1 to 2 hours, then curing at 160 ℃ for 2 to 3 hours, and finally curing at 180 to 200 ℃ for 2 to 3 hours.

10. The application of an end-functionalized polyphenylene ether modified epoxy resin according to claim 1 or 2 in the fields of high-frequency and high-speed electronic packaging and advanced aerospace composite materials.

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