Organic silicon modified mAP-E multifunctional epoxy adhesive and preparation method thereof

Abstract

The invention discloses an organic silicon modified mAP-E multifunctional epoxy adhesive and a preparation method thereof. The multifunctional epoxy adhesive is prepared from m-aminophenol epoxy resin, bisphenol A epoxy resin, TGS-563, bismaleimide diphenylmethane resin, an epoxy chain extender, an organic silicon modifier, an anhydride curing agent and the like. The tensile shear strength of the adhesive at 150 DEG C is larger than or equal to 10 MPa, the dielectric loss is smaller than or equal to 1.92%, the impact strength is larger than or equal to 15.8 kJ / m < 2 >, and the adhesive has the low-viscosity processing characteristic (the viscosity at 50 DEG C is 90-262 mPa.s) and the environment-friendly advantage. The organic silicon modified mAP-E multifunctional epoxy adhesive is suitable for the fields of high-frequency electronic device packaging, aerospace high-temperature component bonding and the like, and solves the technical bottlenecks of high-temperature performance degradation and high dielectric loss of a traditional epoxy adhesive.

Description

Technical Field

[0001] The present invention belongs to the technical field of epoxy resin adhesives, and particularly relates to a silicone-modified multifunctional epoxy adhesive based on m-aminophenol epoxy resin (mAP-E). The silicone-modified mAP-E multifunctional epoxy adhesive is particularly suitable for electronic device packaging and aerospace component bonding in high-temperature and high-frequency environments. Background Art

[0002] Traditional epoxy adhesives are prone to mechanical degradation at high temperatures and exhibit high dielectric loss, making them difficult to meet the performance requirements of high-frequency electronic and aerospace components. The meta-amino group in the mAP-E molecular structure significantly enhances reactivity, and the high crosslink density of its cured product imparts exceptional heat resistance. Furthermore, mAP-E's low viscosity supports solvent-free processing and allows for precise filling, aligning with the development of green and environmentally friendly adhesives. Therefore, the development of mAP-E adhesives not only overcomes the dual performance and environmental bottlenecks of traditional resins but also promotes the development of high-end equipment, electronic information, and clean energy sectors towards high reliability and low environmental impact.

[0003] CN101139327A adopts non-catalytic method, ethanol is solvent, m-aminophenol: epichlorohydrin=1:15, step-by-step reaction (open loop 5h / closed loop 3h) under nitrogen protection, product epoxide value 0.85, viscosity 2490mPa s, epoxide value is lower than theoretical value 1.08;CN104478831A uses catalysts such as benzyldiethylammonium chloride, mol ratio 1:7-9, by low temperature addition and vacuum dehydration process, obtains the resin of epoxide value 0.90-0.94, viscosity 7000-8000mPa s, although promotes epoxide value but viscosity significantly increases. The present invention, by optimizing the synthesis technique of m-aminophenol epoxy resin (mAP-E), successfully prepares the adhesive with high strength, low dielectric loss and excellent heat resistance in combination with specific formula design, fills the gap of prior art. Summary of the Invention

[0004] The technical problem to be solved by the present invention is to provide a silicone modified mAP-E multifunctional epoxy adhesive and its preparation method. The multifunctional epoxy adhesive of the present invention has excellent high temperature resistance (tensile shear strength ≥10MPa at 150℃, tensile strength retention rate ≥10%), low dielectric loss (≤1.92%), high mechanical strength (impact strength ≥15.8kJ / m 2 ), suitable for electronic packaging, aerospace high-temperature components and other fields.

[0005] The first aspect of the present invention provides a silicone-modified mAP-E multifunctional epoxy adhesive, comprising the following components in parts by weight: 20 to 60 parts of m-aminophenol epoxy resin mAP-E, 60 to 80 parts of bisphenol A epoxy resin, 12 to 18 parts of TGS-563 (purchased from Zhejiang Yingruiyun New Materials Technology Co., Ltd.), 1 to 3 parts of bismaleimide diphenylmethane resin BMI, 0.01 to 2 parts of epoxy chain extender, 1 to 20 parts of silicone modifier, 80 to 95 parts of anhydride curing agent, 1 to 3 parts of reactive diluent, 0.01 to 2 parts of accelerator, and 0.1 to 1 part of toughening agent.

[0006] Furthermore, the multifunctional epoxy adhesive comprises the following components in parts by weight: 20-30 parts of m-aminophenol mAP-E, 70-80 parts of E-51, 12-16 parts of TGS-563, 2-3 parts of bismaleimide diphenylmethane resin, 0.01-1 part of epoxy chain extender SD-248, 10-20 parts of silicone modifier, 85-95 parts of anhydride curing agent, 2-3 parts of reactive diluent, 1-2 parts of accelerator, and 0.5-1 part of toughening agent.

[0007] Furthermore, the multifunctional epoxy adhesive comprises the following components in parts by weight: 20 parts of m-aminophenol mAP-E, 80 parts of E-51, 15 parts of TGS-563, 2 parts of bismaleimide diphenylmethane, 1 part of 4,4′-diaminodiphenyl sulfone DDS, 20 parts of CE-793, 90 parts of methyltetrahydrophthalic anhydride MTHPA, 2 parts of 2,2′-bis[4-(4-aminophenoxy)phenyl]propane BAPP, 2 parts of 2-ethyl-4-methylimidazole 2E4MI, and 0.8 parts of 4,4′-diaminodiphenylmethane DDM.

[0008] Furthermore, the epoxy value of the m-aminophenol mAP-E is 0.90-0.95, the total chlorine content is ≤1.52%, the inorganic chlorine is ≤7.5 ppm, and the volatile matter is ≤1.9%.

[0009] Furthermore, the bisphenol A epoxy resin is E-51 (purchased from Nantong Xingchen Synthetic Materials Co., Ltd.) or STREM-50 (purchased from Zhejiang Yingruiyun New Materials Technology Co., Ltd.).

[0010] Furthermore, the epoxy chain extender SD-248 is 4,4'-diaminodiphenyl sulfone (DDS), 4,4'-diaminodiphenyl ether (DDE) or 3,3'-diaminodiphenyl sulfone (3,3'-DDS).

[0011] Furthermore, the active diluent is 2,2′-bis[4-(4-aminophenoxy)phenyl]propane (BAPP), allyl glycidyl ether (AGE) or butyl glycidyl ether (BGE).

[0012] Furthermore, the organosilicon modifier is CE-793 (purchased from Zhejiang Yingruiyun Technology Co., Ltd.) or SE362 (SE362 is purchased from Zhejiang Yingruiyun Technology Co., Ltd.).

[0013] Furthermore, the acid anhydride curing agent is methyltetrahydrophthalic anhydride MeTHPA, tetrahydrophthalic anhydride THPA or methylhexahydrophthalic anhydride MeHHPA.

[0014] Furthermore, the bismaleimide resin is bismaleimide diphenylmethane.

[0015] Furthermore, the accelerator is 2-ethyl-4-methylimidazole (2E4MI), DMP-30 (purchased from Shandong Zhongke New Material Technology Co., Ltd.), 2-methylimidazole (2MI) or 1-cyano-2ethyl-4-methylimidazole (2E4MI-CN).

[0016] Furthermore, the toughening agent is 4,4′-diaminodiphenylmethane (DDM) or CB-100 (purchased from Zhejiang Yingruiyun New Material Technology Co., Ltd.).

[0017] A second aspect of the present invention provides a method for preparing the above-mentioned organosilicon-modified mAP-E multifunctional epoxy adhesive, comprising the following steps:

[0018] (1) m-Aminophenol (mAP) and epichlorohydrin (ECH) are mixed in a molar ratio of 1:12-1:16, and a ring-opening reaction is carried out in an alcohol solvent at 50-55°C for 5 hours to obtain an intermediate, and then a 32% alkali metal hydroxide aqueous solution is added dropwise twice to carry out a ring-closing reaction. The first ring-closing reaction is carried out by adding alkali metal hydroxide and reacting at 60°C for 3 hours. The molar ratio of the ring-opening intermediate to the alkali metal hydroxide is 1:3-3.6; the second ring-closing reaction is carried out by adding alkali metal hydroxide and reacting at 55°C for 3 hours. The molar ratio of the intermediate to the alkali metal hydroxide is 1:0.4-1.2; and the mixture is extracted with toluene, washed with water, and distilled under reduced pressure to obtain mAP-E resin;

[0019] (2) The mAP-E resin prepared in step (1) is mixed with bisphenol A epoxy resin and TGS-563 in proportions of 20-60 parts, 60-80 parts and 12-18 parts by weight, respectively; 1-3 parts of reactive diluent are added, and the mixture is heated and stirred at 100-110° C. until the mixture is homogeneous; then 1-3 parts of bismaleimide (BMI) and 0.01-2 parts of epoxy chain extender are added, and the mixture is heated and reacted until the mixture is homogeneous; 1-20 parts of organosilicon modifier is added, and the mixture is stirred for 0.5 hours and then cooled to below 60° C.; 80-95 parts of an anhydride curing agent are added; finally, 0.01-2 parts of an accelerator and 0.1-1 parts of a toughening agent are added at room temperature, and the mixture is stirred evenly to obtain an adhesive.

[0020] Furthermore, the alkali metal hydroxide in step (1) is one of sodium hydroxide and potassium hydroxide.

[0021] Furthermore, the alcohol solvent in step (1) is one of methanol, ethanol, propanol, ethylene glycol, propylene glycol, and glycerol.

[0022] In a third aspect, the present invention provides an application of the above-mentioned organosilicon-modified mAP-E multifunctional epoxy adhesive, comprising: using a low-temperature curing process, during curing, first heating to 120°C and keeping warm for 30 minutes, then continuing to heat to 150°C and keeping warm for 1 hour, and finally heating to 170°C and keeping warm for 30 minutes.

[0023] The formulation design system of the adhesive of the present invention is:

[0024] Synergistic effect of matrix resin: mAP-E is used as the main resin, E-51 is compounded to improve toughness, and TGS-563 is added to enhance heat resistance and dielectric properties.

[0025] Cross-linking system optimization: BMI and DDS composite curing is used to form a high cross-linking density network and improve high-temperature strength; the anhydride curing agent MTHPA ensures low-temperature curing activity.

[0026] Functional additive regulation: active diluent BAPP reduces viscosity, accelerator 2E4MI accelerates curing reaction, and toughening agent DDM improves toughness.

[0027] The preparation process of the present invention adopts a two-step closed-loop method:

[0028] The synthesis of mAP-E utilizes a staged ring-closure reaction. The initial ring-closure uses 0.6 mol NaOH to remove most chloride ions, followed by a secondary ring-closure with 0.2 mol NaOH for further purification, reducing the total chlorine content to 1.52% and inorganic chlorine to ≤ 7.5 ppm, significantly improving resin purity (HPLC purity ≥ 90%). Solvent recovery: Excess epichlorohydrin (ECH) and toluene solvent in the reaction are recovered at a rate of ≥ 97% via vacuum distillation, minimizing waste and ensuring environmental friendliness.

[0029] The preparation process of the present invention accurately controls the resin purity (total chlorine ≤ 1.52%) through a staged closed-loop reaction, combined with a low-temperature mixing process to avoid phase separation. The resulting adhesive has a tensile shear strength of ≥10MPa at 150°C and a dielectric loss of ≤1.92%.

[0030] (100kHz), impact strength ≥15.8kJ / m 2The silicone-modified mAP-E multifunctional epoxy adhesive combines low-viscosity processing properties (viscosity 90-262 mPa·s at 50°C) with environmental advantages (solvent recovery rate ≥ 97%). This silicone-modified mAP-E multifunctional epoxy adhesive is suitable for applications such as high-frequency electronic device packaging and high-temperature aerospace component bonding, resolving the technical bottlenecks of traditional epoxy adhesives, such as high-temperature performance degradation and high dielectric loss.

[0031] Beneficial effects

[0032] The organosilicon-modified mAP-E multifunctional epoxy adhesive of the present invention has excellent properties: 1) high temperature resistance: tensile shear strength ≥10MPa at 150°C; 2) low dielectric loss: dielectric constant ≤4.55 (100kHz), dielectric loss ≤1.92%; 3) high mechanical strength: impact strength ≥15.8kJ / m 2 This multifunctional epoxy adhesive is suitable for 5G high-frequency circuits, electronic packaging, aerospace high-temperature components and other fields.

[0033] The preparation process of the present invention adopts staged temperature-controlled mixing (pre-reaction at 100-110°C → addition of curing agent below 60°C) to avoid phase separation of the epoxy resin and ensure the uniformity of the adhesive; and no high-temperature and high-pressure equipment is required, the solvent can be recycled, and it is suitable for industrial production. BRIEF DESCRIPTION OF THE DRAWINGS

[0034] Figure 1 This is a flow chart of the mAP-E synthesis process;

[0035] Figure 2 is the viscosity-temperature curve of adhesives J-0 to J-3;

[0036] Figure 3 The relationship between the relative dielectric constant of adhesives J-0 to J-3 and frequency (100kHz to 1000kHz);

[0037] Figure 4 This is the relationship between the dielectric loss and frequency of adhesives J-0 to J-3 (100kHz to 1000kHz). DETAILED DESCRIPTION

[0038] Below in conjunction with specific embodiment, further set forth the present invention.Should be understood that these embodiments are only used to illustrate the present invention and are not used in limiting the scope of the present invention.In addition, should be understood that after reading the content taught by the present invention, those skilled in the art can make various changes or modifications to the present invention, and these equivalent forms fall equally within the scope limited by the appended claims of the application.

[0039] The raw materials and reagents used in the following examples can be obtained through commercial sources.

[0040] Example 1: Preparation of mAP-E resin

[0041] Raw material ratio:

[0042] m-Aminophenol (mAP): 21.8 g (0.2 mol)

[0043] Epichlorohydrin (ECH): 277.8 g (3.0 mol)

[0044] Ethanol: 110.4 g (2.4 mol)

[0045] Sodium hydroxide: 24g (0.6mol, first ring closure) + 8g (0.2mol, second ring closure)

[0046] Toluene: 150g

[0047] Synthesis process steps:

[0048] mAP was dissolved in ethanol and added dropwise to ECH, reacting at 50-55°C for 5 hours. 24 g of 32% NaOH solution was added dropwise, and the ring-closure reaction was carried out at 60°C for 3 hours. The salt was filtered off. The mother liquor was distilled under reduced pressure to recover ECH and ethanol, and toluene was added to extract the resin. NaOH solution was added dropwise a second time, and the reaction was carried out at 55°C for 3 hours. The toluene layer was washed with water three times, and the toluene was removed by distillation under reduced pressure to obtain a light yellow mAP-E resin with a yield of 83.6%.

[0049] Performance indicators:

[0050] Epoxy value: 0.92

[0051] Total chlorine: 1.52%

[0052] Inorganic chlorine: 7.5ppm

[0053] Volatile matter: 1.9%

[0054] HPLC purity: 90.2%

[0055] Example 2: Preparation of Adhesive J-0

[0056] formula:

[0057] mAP-E of Example 1: 20 g

[0058] E-51: 80g

[0059] BAPP: 2g

[0060] BMI: 2g

[0061] DDS (SD-248 purchased from Zhejiang Yingruiyun New Material Technology Co., Ltd.): 1g

[0062] MTHPA: 90g

[0063] 2E4MI:2g

[0064] CE-793: 20g

[0065] Preparation steps:

[0066] Add mAP-E, E-51, and BAPP into a disposable plastic cup, heat at 100°C and stir until homogeneous;

[0067] Add BMI and DDS and continue the reaction until transparent;

[0068] Add CE-793, stir for 0.5 hours, cool to below 60°C and add MTHPA;

[0069] 2E4MI was added at room temperature and stirred evenly to obtain adhesive J-0.

[0070] Curing process:

[0071] Use adhesive J-0 to cast the mold for curing, heat it to 120℃ and keep it for 30 minutes, continue to heat it to 150℃ and keep it for 1 hour, and finally heat it to 170℃ and keep it for 30 minutes.

[0072] Performance testing:

[0073] Viscosity: 90 mPa·s at 50°C, drops to 12 mPa·s at 60°C;

[0074] Tensile strength: 51.6MPa (room temperature), 46.1MPa (100℃), 4.5MPa (150℃); Impact strength: 21.4kJ / m 2 ;

[0075] Dielectric properties: dielectric constant 4.41 (100kHz), dielectric loss 1.27%~1.80%.

[0076] Example 3: Preparation of Adhesive J-1

[0077] formula:

[0078] mAP-E: 20g

[0079] E-51: 80g

[0080] TGS-563: 12g

[0081] BAPP: 2g

[0082] BMI: 2g

[0083] DDS: 1g

[0084] MTHPA: 95g

[0085] 2E4MI:1g

[0086] CE-793: 20g

[0087] Preparation steps:

[0088] Mix mAP-E, E-51, TGS-563, and BAPP, heat and stir at 100°C until homogeneous;

[0089] Add BMI and DDS and continue the reaction until transparent;

[0090] Add CE-793, stir for 0.5 hours, cool to below 60°C and add MTHPA;

[0091] Add 2E4MI at room temperature and stir well.

[0092] Curing process: Same as J-0.

[0093] Performance testing:

[0094] Viscosity: 150 mPa·s at 50°C, drops to 38 mPa·s at 60°C;

[0095] Tensile strength: 66.8MPa (room temperature), 56.3MPa (100℃), 6.8MPa (150℃); Impact strength: 15.8kJ / m 2 ;

[0096] Dielectric properties: dielectric constant 4.19 (100kHz), dielectric loss 1.41%~1.82%.

[0097] Example 4: Preparation of Adhesive J-2

[0098] formula:

[0099] mAP-E: 20g

[0100] E-51: 70g

[0101] TGS-563: 15g

[0102] BAPP:3g

[0103] MTHPA: 80g

[0104] 2E4MI:2g

[0105] CE-793: 20g

[0106] Preparation steps:

[0107] Mix mAP-E, E-51, TGS-563, and BAPP, heat and stir at 100°C until homogeneous;

[0108] Directly add CE-793, stir for 0.5 hours, cool to below 60°C and add MTHPA;

[0109] Add 2E4MI at room temperature and stir well.

[0110] Curing process: Same as J-0.

[0111] Performance testing:

[0112] Viscosity: 105 mPa·s at 50°C, drops to 19 mPa·s at 60°C;

[0113] Tensile strength: 54.5MPa (room temperature), 34.6MPa (100℃), 7.0MPa (150℃); Impact strength: 17.4kJ / m 2 ;

[0114] Dielectric properties: dielectric constant 4.55 (100kHz), dielectric loss 1.31%~1.92%.

[0115] Example 5: Preparation of Adhesive J-3

[0116] formula:

[0117] mAP-E: 20g

[0118] E-51: 60g

[0119] TGS-563: 18g

[0120] BAPP: 1g

[0121] BMI: 3g

[0122] DDS: 0g

[0123] MTHPA: 80g

[0124] 2E4MI:1g

[0125] CE-793: 15g

[0126] DDM: 1g

[0127] Preparation steps:

[0128] Mix mAP-E, E-51, TGS-563, and BAPP, heat and stir at 100°C until homogeneous;

[0129] Add BMI and continue the reaction until transparent;

[0130] Add CE-793, stir for 0.5 hours, cool to below 60°C and add MTHPA;

[0131] Add 2E4MI and DDM at room temperature and stir well.

[0132] Curing process: Same as J-0.

[0133] Performance testing:

[0134] Viscosity: 262 mPa·s at 50°C, drops to 83 mPa·s at 60°C;

[0135] Tensile strength: 56.4MPa (room temperature), 55.1MPa (100℃), 4.6MPa (150℃);

[0136] Impact strength: 20.1kJ / m 2 ;

[0137] Dielectric properties: dielectric constant 4.24 (100kHz), dielectric loss 1.27%~1.82%.

[0138] Example 6

[0139] The mechanical and electrical properties of the adhesive were tested using a WDW-50 high and low temperature electronic universal material testing machine and a TH2828S inductance and capacitance analyzer, respectively. The results are shown in Table 1.

[0140] Table 1 Performance test data of adhesive

[0141] Performance indicators J-0 J-1 J-2 J-3 <![CDATA[Impact strength / kJ / m 2 > 21.4 15.8 17.4 20.1 Tensile strength / MPa 51.6 66.8 54.5 56.4 Bending strength / MPa 96.4 101.4 95.7 102.3 Tensile shear strength / MPa 15.1 15.7 15.0 14.9 Relative dielectric constant (100kHz) 4.41 4.19 4.55 4.43 Dielectric loss (100kHz) 1.80％ 1.82％ 1.92％ 1.82％

[0142] According to Table 1 and Figure 2-4 Comprehensive analysis of the test data shows that the silicone modified mAP-E multifunctional epoxy adhesive of the present invention has demonstrated significant technological breakthroughs and performance advantages. In terms of high-temperature mechanical properties, the J-1 adhesive still maintains a tensile strength of 6.8MPa at 150°C, and the J-2 even reaches 7.0MPa, both significantly higher than traditional epoxy adhesives (usually <5MPa). This is due to the synergistic effect of the high cross-linking density of the mAP-E resin and the BMI / DDS composite curing system. The dielectric performance is particularly outstanding, with the dielectric loss of all formulations at 100kHz being ≤1.92% (J-0 is as low as 1.27%), and the relative dielectric constant is stable in the range of 4.19-4.55, and Figure 3-4 The characteristics are shown to be stable in the wide frequency range of 100kHz-1000MHz, meeting the stringent requirements of high-frequency circuits on the dielectric properties of materials. 2 ) confirmed the synergistic toughening effect of E-51 and silicone modifier CE-793, among which J-3 increased the impact strength to 20.1kJ / m by adding 1 part of DDM 2 , 27% higher than the basic formula. Figure 2The viscosity-temperature curve reveals the system's excellent processing properties, with a minimum viscosity of only 90 mPa·s (J-0) at 50°C, dropping sharply to 12 mPa·s at 60°C. This unique thixotropic property ensures both room-temperature storage stability and efficient wetting during processing with moderate temperature increases. In summary, through molecular structure design, compounding system optimization, and process innovation, this adhesive has achieved breakthroughs in high-temperature resistance, dielectric properties, and mechanical strength, providing a solution for the bonding of hot-end components in aerospace and high-frequency electronic packaging.

[0143] The compounds of the present invention, their preparation methods, and applications are described herein with reference to specific embodiments and examples, and many details are described and illustrated. However, it should be understood that the specific embodiments and examples provided herein are merely exemplary and do not limit the scope of the present invention. In fact, it will be apparent to those skilled in the art that the present invention may also be implemented in other specific ways, and that such modifications, variations, or adjustments do not depart from the spirit and purpose of the present invention and are therefore intended to be encompassed within the scope of the present invention.

Claims

1. A silicone-modified mAP-E multifunctional epoxy adhesive comprising the following components in parts by weight: 20-60 parts of m-aminophenol epoxy resin mAP-E, 60-80 parts of bisphenol A epoxy resin, 12-18 parts of TGS-563 (purchased from Zhejiang Yingruiyun New Material Technology Co., Ltd.), 1-3 parts of bismaleimide diphenylmethane resin (BMI), 0.01-2 parts of epoxy chain extender, 1-20 parts of silicone modifier, 80-95 parts of anhydride curing agent, 1-3 parts of reactive diluent, 0.01-2 parts of accelerator, and 0.1-1 part of toughening agent.

2. The organosilicon-modified mAP-E multifunctional epoxy adhesive according to claim 1, characterized in that: The multifunctional epoxy adhesive comprises the following components in parts by weight: 20-30 parts of m-aminophenol mAP-E, 70-80 parts of E-51, 12-16 parts of TGS-563, 2-3 parts of bismaleimide diphenylmethane resin, 0.01-1 part of epoxy chain extender SD-248, 10-20 parts of organosilicon modifier, 85-95 parts of anhydride curing agent, 2-3 parts of reactive diluent, 1-2 parts of accelerator, and 0.5-1 part of toughening agent.

3. The organosilicon-modified mAP-E multifunctional epoxy adhesive according to claim 1, characterized in that: The m-aminophenol mAP-E has an epoxy value of 0.90-0.95, a total chlorine content of ≤1.52%, inorganic chlorine of ≤7.5ppm, and a volatile matter of ≤1.9%.

4. The organosilicon-modified mAP-E multifunctional epoxy adhesive according to claim 1, characterized in that: The bisphenol A epoxy resin is E-51 (purchased from Nantong Xingchen Synthetic Materials Co., Ltd.) or STREM-50 (purchased from Zhejiang Yingruiyun New Materials Technology Co., Ltd.).

5. The organosilicon-modified mAP-E multifunctional epoxy adhesive according to claim 1, characterized in that: The epoxy chain extender is 4,4'-diaminodiphenyl sulfone (DDS), 4,4'-diaminodiphenyl ether (DDE) or 3,3'-diaminodiphenyl sulfone (3,3'-DDS).

6. The organosilicon-modified mAP-E multifunctional epoxy adhesive according to claim 1, characterized in that: The organosilicon modifier is CE-793 (purchased from Zhejiang Yingruiyun Technology Co., Ltd.) or SE362 (SE362 is purchased from Zhejiang Yingruiyun Technology Co., Ltd.).

7. A method for preparing a silicone-modified mAP-E multifunctional epoxy adhesive according to any one of claims 1 to 6, comprising the following steps: (1) m-Aminophenol (mAP) and epichlorohydrin (ECH) are mixed in a molar ratio of 1:12-1:16, and a ring-opening reaction is carried out in an alcohol solvent at 50-55°C for 5 hours to obtain an intermediate, and then a 32% alkali metal hydroxide aqueous solution is added dropwise twice to carry out a ring-closing reaction. The first ring-closing reaction is carried out by adding alkali metal hydroxide and reacting at 60°C for 3 hours. The molar ratio of the ring-opening intermediate to the alkali metal hydroxide is 1:3-3.6; the second ring-closing reaction is carried out by adding alkali metal hydroxide and reacting at 55°C for 3 hours. The molar ratio of the intermediate to the alkali metal hydroxide is 1:0.4-1.2; and the mixture is extracted with toluene, washed with water, and distilled under reduced pressure to obtain mAP-E resin; (2) The mAP-E resin prepared in step (1) is mixed with bisphenol A epoxy resin and TGS-563 in proportions of 20 to 60 parts, 60 to 80 parts, and 12 to 18 parts by weight, and 1 to 3 parts of reactive diluent are added. The mixture is heated and stirred at 100 to 110° C. until it becomes homogeneous. Then, 1 to 3 parts of bismaleimide (BMI) and 0.01 to 2 parts of epoxy chain extender are added. The mixture is heated and reacted until it becomes homogeneous. 1 to 20 parts of organosilicon modifier is added. The mixture is stirred for 0.5 hours and then cooled to below 60° C., and 80 to 95 parts of an anhydride curing agent are added. Finally, 0.01 to 2 parts of accelerator and 0.1 to 1 part of toughening agent are added at room temperature and stirred evenly to obtain an adhesive.

8. The preparation method according to claim 7, characterized in that: The alkali metal hydroxide in step (1) is one of sodium hydroxide and potassium hydroxide.

9. The preparation method according to claim 7, characterized in that: The alcohol solvent in step (1) is one of methanol, ethanol, propanol, ethylene glycol, propylene glycol, and glycerol.

10. Use of the organosilicon-modified mAP-E multifunctional epoxy adhesive according to any one of claims 1 to 6, comprising: A low-temperature curing process is used. During curing, the temperature is first raised to 120°C and kept for 30 minutes, then raised to 150°C and kept for 1 hour, and finally raised to 170°C and kept for 30 minutes.

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